Articles | Volume 16, issue 14
https://doi.org/10.5194/acp-16-8729-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-8729-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
18 Jul 2016
Research article |
| 18 Jul 2016
Model–measurement comparison of functional group abundance in α-pinene and 1,3,5-trimethylbenzene secondary organic aerosol formation
Giulia Ruggeri
ENAC/IIE Swiss Federal Institute of Technology Lausanne (EPFL), Lausanne, Switzerland
Fabian A. Bernhard
ENAC/IIE Swiss Federal Institute of Technology Lausanne (EPFL), Lausanne, Switzerland
Barron H. Henderson
Department of Environmental Engineering Sciences, University of Florida, Gainesville, FL, USA
Satoshi Takahama
CORRESPONDING AUTHOR
ENAC/IIE Swiss Federal Institute of Technology Lausanne (EPFL), Lausanne, Switzerland
Related authors
Satoshi Takahama and Giulia Ruggeri
Atmos. Chem. Phys., 17, 4433–4450, https://doi.org/10.5194/acp-17-4433-2017, https://doi.org/10.5194/acp-17-4433-2017, 2017
Short summary
Short summary
We formalize a method for classifying carbon atoms in organic aerosols according to their functionalization. This conceptual approach allows estimation of carbon mass from functional group measurements, which previously required a series of assumptions that were not well constrained. We describe how the proposed strategy can lead to better comparisons among functional group measurements, chemically explicit model simulations, and other measurements.
Satoshi Takahama, Giulia Ruggeri, and Ann M. Dillner
Atmos. Meas. Tech., 9, 3429–3454, https://doi.org/10.5194/amt-9-3429-2016, https://doi.org/10.5194/amt-9-3429-2016, 2016
Short summary
Short summary
We introduce the application of statistical algorithms that allow us to associate various dimensions of aerosol composition to vibrational modes measured by infrared absorption spectroscopy. We demonstrate their use on four organic functional groups for which absorption bands are known and extend the application to interpret bands associated with ambient organic carbon and elemental carbon quantified by an independent measurement technique that is widely used in aerosol monitoring networks.
Giulia Ruggeri and Satoshi Takahama
Atmos. Chem. Phys., 16, 4401–4422, https://doi.org/10.5194/acp-16-4401-2016, https://doi.org/10.5194/acp-16-4401-2016, 2016
Short summary
Short summary
We present a set of tools for mapping molecular information to functional group composition. This allows us to reduce the complexity of representing the organic aerosol composition, as it consists of hundreds of thousands of different compounds. We describe the tools and methods for validation, and demonstrate several applications in which this tool can facilitate measurement intercomparisons and chemical modeling of aerosol chemistry.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
Short summary
Short summary
We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
Short summary
Short summary
Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Emily Y. Li, Amir Yazdani, Ann M. Dillner, Guofeng Shen, Wyatt M. Champion, James J. Jetter, William T. Preston, Lynn M. Russell, Michael D. Hays, and Satoshi Takahama
Atmos. Meas. Tech., 17, 2401–2413, https://doi.org/10.5194/amt-17-2401-2024, https://doi.org/10.5194/amt-17-2401-2024, 2024
Short summary
Short summary
Infrared spectroscopy is a cost-effective measurement technique to characterize the chemical composition of organic aerosol emissions. This technique differentiates the organic matter emission factor from different fuel sources by their characteristic functional groups. Comparison with collocated measurements suggests that polycyclic aromatic hydrocarbon concentrations in emissions estimated by conventional chromatography may be substantially underestimated.
T. Nash Skipper, Christian Hogrefe, Barron H. Henderson, Rohit Mathur, Kristen M. Foley, and Armistead G. Russell
EGUsphere, https://doi.org/10.5194/egusphere-2024-554, https://doi.org/10.5194/egusphere-2024-554, 2024
Short summary
Short summary
Chemical transport model simulations are combined with ozone observations to estimate the bias in ozone attributable to US anthropogenic sources as well as several individual sources of US background ozone: natural sources, non-US anthropogenic sources, and stratospheric ozone. Results indicate a positive bias correlated with US anthropogenic emissions during summer in the eastern US and a negative bias correlated with stratospheric ozone during spring.
Kelvin H. Bates, Mathew J. Evans, Barron H. Henderson, and Daniel J. Jacob
Geosci. Model Dev., 17, 1511–1524, https://doi.org/10.5194/gmd-17-1511-2024, https://doi.org/10.5194/gmd-17-1511-2024, 2024
Short summary
Short summary
Accurate representation of rates and products of chemical reactions in atmospheric models is crucial for simulating concentrations of pollutants and climate forcers. We update the widely used GEOS-Chem atmospheric chemistry model with reaction parameters from recent compilations of experimental data and demonstrate the implications for key atmospheric chemical species. The updates decrease tropospheric CO mixing ratios and increase stratospheric nitrogen oxide mixing ratios, among other changes.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
Short summary
Short summary
We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Marife B. Anunciado, Miranda De Boskey, Laura Haines, Katarina Lindskog, Tracy Dombek, Satoshi Takahama, and Ann M. Dillner
Atmos. Meas. Tech., 16, 3515–3529, https://doi.org/10.5194/amt-16-3515-2023, https://doi.org/10.5194/amt-16-3515-2023, 2023
Short summary
Short summary
Organic sulfur compounds are used to identify sources and atmospheric processing of aerosol. Our paper evaluates the potential of using a non-destructive measurement technique to measure organic sulfur compounds in filter samples by assessing their chemical stability over time. Some were stable, but some evaporated or changed chemically. Future work includes evaluating the stability and potential interference of multiple organic sulfur compounds in laboratory mixtures and ambient aerosol.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
Short summary
Short summary
Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Monica Crippa, Diego Guizzardi, Tim Butler, Terry Keating, Rosa Wu, Jacek Kaminski, Jeroen Kuenen, Junichi Kurokawa, Satoru Chatani, Tazuko Morikawa, George Pouliot, Jacinthe Racine, Michael D. Moran, Zbigniew Klimont, Patrick M. Manseau, Rabab Mashayekhi, Barron H. Henderson, Steven J. Smith, Harrison Suchyta, Marilena Muntean, Efisio Solazzo, Manjola Banja, Edwin Schaaf, Federico Pagani, Jung-Hun Woo, Jinseok Kim, Fabio Monforti-Ferrario, Enrico Pisoni, Junhua Zhang, David Niemi, Mourad Sassi, Tabish Ansari, and Kristen Foley
Earth Syst. Sci. Data, 15, 2667–2694, https://doi.org/10.5194/essd-15-2667-2023, https://doi.org/10.5194/essd-15-2667-2023, 2023
Short summary
Short summary
This study responds to the global and regional atmospheric modelling community's need for a mosaic of air pollutant emissions with global coverage, long time series, spatially distributed data at a high time resolution, and a high sectoral resolution in order to enhance the understanding of transboundary air pollution. The mosaic approach to integrating official regional emission inventories with a global inventory based on a consistent methodology ensures policy-relevant results.
Qian Shu, Sergey L. Napelenok, William T. Hutzell, Kirk R. Baker, Barron H. Henderson, Benjamin N. Murphy, and Christian Hogrefe
Geosci. Model Dev., 16, 2303–2322, https://doi.org/10.5194/gmd-16-2303-2023, https://doi.org/10.5194/gmd-16-2303-2023, 2023
Short summary
Short summary
Source attribution methods are generally used to determine culpability of precursor emission sources to ambient pollutant concentrations. However, source attribution of secondarily formed pollutants such as ozone and its precursors cannot be explicitly measured, making evaluation of source apportionment methods challenging. In this study, multiple apportionment approach comparisons show common features but still reveal wide variations in predicted sector contribution and species dependency.
James D. East, Barron H. Henderson, Sergey L. Napelenok, Shannon N. Koplitz, Golam Sarwar, Robert Gilliam, Allen Lenzen, Daniel Q. Tong, R. Bradley Pierce, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 22, 15981–16001, https://doi.org/10.5194/acp-22-15981-2022, https://doi.org/10.5194/acp-22-15981-2022, 2022
Short summary
Short summary
We present a framework that uses a computer model of air quality, along with air pollution data from satellite instruments, to estimate emissions of nitrogen oxides (NOx) across the Northern Hemisphere. The framework, which advances current methods to infer emissions from satellite observations, provides observationally constrained NOx estimates, including in regions of the world where emissions are highly uncertain, and can improve simulations of air pollutants relevant for health and policy.
Nikunj Dudani and Satoshi Takahama
Atmos. Meas. Tech., 15, 4693–4707, https://doi.org/10.5194/amt-15-4693-2022, https://doi.org/10.5194/amt-15-4693-2022, 2022
Short summary
Short summary
We designed and fabricated an aerosol collector with high collection efficiency that enables quantitative infrared spectroscopy analysis. By collecting particles on optical windows, typical substrate interferences are eliminated. New methods for fabricating aerosol devices using 3D printing with post-treatment to reduce the time and cost of prototyping are described.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2857–2874, https://doi.org/10.5194/amt-15-2857-2022, https://doi.org/10.5194/amt-15-2857-2022, 2022
Short summary
Short summary
While the aerosol mass spectrometer provides high-time-resolution characterization of the overall extent of oxidation, the extensive fragmentation of molecules and specificity of the technique have posed challenges toward deeper understanding of molecular structures in aerosols. This work demonstrates how functional group information can be extracted from a suite of commonly measured mass fragments using collocated infrared spectroscopy measurements.
Bruno Debus, Andrew T. Weakley, Satoshi Takahama, Kathryn M. George, Anahita Amiri-Farahani, Bret Schichtel, Scott Copeland, Anthony S. Wexler, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2685–2702, https://doi.org/10.5194/amt-15-2685-2022, https://doi.org/10.5194/amt-15-2685-2022, 2022
Short summary
Short summary
In the US, routine particulate matter composition is measured on samples collected on three types of filter media and analyzed using several techniques. We propose an alternate approach that uses one analytical technique, Fourier transform-infrared spectroscopy (FT-IR), and one filter type to measure the chemical composition of particulate matter in a major US monitoring network. This method could be used to add low-cost sites to the network, fill-in missing data, or for quality control.
Mária Lbadaoui-Darvas, Satoshi Takahama, and Athanasios Nenes
Atmos. Chem. Phys., 21, 17687–17714, https://doi.org/10.5194/acp-21-17687-2021, https://doi.org/10.5194/acp-21-17687-2021, 2021
Short summary
Short summary
Aerosol–cloud interactions constitute the most uncertain contribution to climate change. The uptake kinetics of water by aerosol is a central process of cloud droplet formation, yet its molecular-scale mechanism is unknown. We use molecular simulations to study this process for phase-separated organic particles. Our results explain the increased cloud condensation activity of such particles and can be generalized over various compositions, thus possibly serving as a basis for future models.
Amir Yazdani, Ann M. Dillner, and Satoshi Takahama
Atmos. Meas. Tech., 14, 4805–4827, https://doi.org/10.5194/amt-14-4805-2021, https://doi.org/10.5194/amt-14-4805-2021, 2021
Short summary
Short summary
We propose a spectroscopic method for estimating several mixture-averaged molecular properties (carbon number and molecular weight) in particulate matter relevant for understanding its chemical origins. This estimation is enabled by calibration models built and tested using laboratory standards containing molecules with known structure, and can be applied to filter samples of PM2.5 currently collected in existing air pollution monitoring networks and field campaigns.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys., 21, 10273–10293, https://doi.org/10.5194/acp-21-10273-2021, https://doi.org/10.5194/acp-21-10273-2021, 2021
Short summary
Short summary
Functional group compositions of primary and aged aerosols from wood burning and coal combustion sources from chamber experiments are interpreted through compounds present in the fuels and known gas-phase oxidation products. Infrared spectra of aged wood burning in the chamber and ambient biomass burning samples reveal striking similarities, and a new method for identifying burning-impacted samples in monitoring network measurements is presented.
Alexandra J. Boris, Satoshi Takahama, Andrew T. Weakley, Bruno M. Debus, Stephanie L. Shaw, Eric S. Edgerton, Taekyu Joo, Nga L. Ng, and Ann M. Dillner
Atmos. Meas. Tech., 14, 4355–4374, https://doi.org/10.5194/amt-14-4355-2021, https://doi.org/10.5194/amt-14-4355-2021, 2021
Short summary
Short summary
Infrared spectrometry can be applied in routine monitoring of atmospheric particles to give comprehensive characterization of the organic material by bond rather than species. Using this technique, the concentrations of particle organic material were found to decrease 2011–2016 in the southeastern US, driven by a decline in highly aged material, concurrent with declining anthropogenic emissions. However, an increase was observed in the fraction of more moderately aged organic matter.
Qian Shu, Benjamin Murphy, Jonathan E. Pleim, Donna Schwede, Barron H. Henderson, Havala O.T. Pye, Keith Wyat Appel, Tanvir R. Khan, and Judith A. Perlinger
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-129, https://doi.org/10.5194/gmd-2021-129, 2021
Preprint withdrawn
Short summary
Short summary
We have bridged the gap between dry deposition measurement and modeling by rigorous use of box and regional transport models and field measurements, but more efforts are needed. This study highlights that deviation among deposition schemes is most pronounced for small and large particles. This study better links model predictions to available real-world observations and incrementally reduces uncertainties in the magnitude of loss processes important for the lifecycle of air pollutants.
Amy E. Christiansen, Annmarie G. Carlton, and Barron H. Henderson
Atmos. Chem. Phys., 20, 11607–11624, https://doi.org/10.5194/acp-20-11607-2020, https://doi.org/10.5194/acp-20-11607-2020, 2020
Short summary
Short summary
We quantify differences in surface-level fine particle mass (PM2.5) chemical composition in relation to satellite-derived cloud flags and find significant differences between clear-sky and cloud days. The work suggests that future analysis in this area is warranted.
Eirini Boleti, Christoph Hueglin, Stuart K. Grange, André S. H. Prévôt, and Satoshi Takahama
Atmos. Chem. Phys., 20, 9051–9066, https://doi.org/10.5194/acp-20-9051-2020, https://doi.org/10.5194/acp-20-9051-2020, 2020
Short summary
Short summary
Long-term temporal evolution of ozone concentrations between 2000 and 2015 in Europe was estimated using a signal decomposition technique. The seasonal cycles are correlated with local climate conditions and vary according to geographic region, while ozone levels are indicative of distance to emission sources. The site's environment plays a key role in ozone trends, with the most polluted environments showing the least reduction in ozone, while in less polluted areas ozone has decreased.
Charlotte Bürki, Matteo Reggente, Ann M. Dillner, Jenny L. Hand, Stephanie L. Shaw, and Satoshi Takahama
Atmos. Meas. Tech., 13, 1517–1538, https://doi.org/10.5194/amt-13-1517-2020, https://doi.org/10.5194/amt-13-1517-2020, 2020
Short summary
Short summary
Infrared spectroscopy is a chemically informative method for particulate matter characterization. However, recent work has demonstrated that predictions depend heavily on the choice of calibration model parameters. We propose a means for managing parameter uncertainties by combining available data from laboratory standards, molecular databases, and collocated ambient measurements to provide useful characterization of atmospheric organic matter on a large scale.
Alexandra J. Boris, Satoshi Takahama, Andrew T. Weakley, Bruno M. Debus, Carley D. Fredrickson, Martin Esparza-Sanchez, Charlotte Burki, Matteo Reggente, Stephanie L. Shaw, Eric S. Edgerton, and Ann M. Dillner
Atmos. Meas. Tech., 12, 5391–5415, https://doi.org/10.5194/amt-12-5391-2019, https://doi.org/10.5194/amt-12-5391-2019, 2019
Short summary
Short summary
Organic species are abundant in atmospheric particle-phase (aerosol) pollution and originate from a variety of biogenic and anthropogenic sources. Infrared spectrometry of filter-based atmospheric particle samples can afford a direct measurement of the particulate organic matter concentration and a characterization of its composition. This work discusses recent method improvements and compositions measured in samples from the SouthEastern Aerosol Research and Characterization (SEARCH) network.
Matteo Reggente, Ann M. Dillner, and Satoshi Takahama
Atmos. Meas. Tech., 12, 2287–2312, https://doi.org/10.5194/amt-12-2287-2019, https://doi.org/10.5194/amt-12-2287-2019, 2019
Short summary
Short summary
We compare state-of-the-art models for predicting functional group composition in atmospheric particulate matter across urban and rural samples collected in a US monitoring network. While trends across models are consistent, absolute abundances can be sensitive to selection of calibration standards, spectral processing procedures, and calibration algorithms. Recommendations for further method development for reducing uncertainties are outlined.
Matteo Reggente, Rudolf Höhn, and Satoshi Takahama
Atmos. Meas. Tech., 12, 2313–2329, https://doi.org/10.5194/amt-12-2313-2019, https://doi.org/10.5194/amt-12-2313-2019, 2019
Short summary
Short summary
The infrared spectra of atmospheric particles are rich in chemical information but require sophisticated statistical methods to extract information on account of their complex absorption profiles. We present an open software suite which makes current algorithms used for analysis of such spectra available to the community, with a browser-based interface for general users and modular architecture that facilitates addition of new methods by developers.
Satoshi Takahama, Ann M. Dillner, Andrew T. Weakley, Matteo Reggente, Charlotte Bürki, Mária Lbadaoui-Darvas, Bruno Debus, Adele Kuzmiakova, and Anthony S. Wexler
Atmos. Meas. Tech., 12, 525–567, https://doi.org/10.5194/amt-12-525-2019, https://doi.org/10.5194/amt-12-525-2019, 2019
Short summary
Short summary
Mid-infrared spectra of particulate matter (PM) samples are complex but chemically informative and present an opportunity for cost-effective measurement of PM provided that quantitative calibration models can be built. We review an emerging strategy for building statistical calibration models using collocated measurements, interpreting the physical bases for such models and evaluating the suitability of existing calibration models to new samples.
Satoshi Takahama and Giulia Ruggeri
Atmos. Chem. Phys., 17, 4433–4450, https://doi.org/10.5194/acp-17-4433-2017, https://doi.org/10.5194/acp-17-4433-2017, 2017
Short summary
Short summary
We formalize a method for classifying carbon atoms in organic aerosols according to their functionalization. This conceptual approach allows estimation of carbon mass from functional group measurements, which previously required a series of assumptions that were not well constrained. We describe how the proposed strategy can lead to better comparisons among functional group measurements, chemically explicit model simulations, and other measurements.
Rob L. Modini and Satoshi Takahama
Atmos. Meas. Tech., 9, 3337–3354, https://doi.org/10.5194/amt-9-3337-2016, https://doi.org/10.5194/amt-9-3337-2016, 2016
Short summary
Short summary
Aerosol measurement techniques with high detection limits often result in poorly time-resolved measurements. We investigated sampling strategies and post-processing methods for constructing hourly resolved aerosol concentration time series from samples collected for 4 to 8 h. We show that this is an effective way to increase measurement time resolution, and that under realistic experimental conditions, simple methods can perform as well as more sophisticated methods.
Satoshi Takahama, Giulia Ruggeri, and Ann M. Dillner
Atmos. Meas. Tech., 9, 3429–3454, https://doi.org/10.5194/amt-9-3429-2016, https://doi.org/10.5194/amt-9-3429-2016, 2016
Short summary
Short summary
We introduce the application of statistical algorithms that allow us to associate various dimensions of aerosol composition to vibrational modes measured by infrared absorption spectroscopy. We demonstrate their use on four organic functional groups for which absorption bands are known and extend the application to interpret bands associated with ambient organic carbon and elemental carbon quantified by an independent measurement technique that is widely used in aerosol monitoring networks.
Adele Kuzmiakova, Ann M. Dillner, and Satoshi Takahama
Atmos. Meas. Tech., 9, 2615–2631, https://doi.org/10.5194/amt-9-2615-2016, https://doi.org/10.5194/amt-9-2615-2016, 2016
Short summary
Short summary
We describe a new method for removing Teflon substrate interference from ambient aerosol infrared spectra such that functional group quantification and spectral clustering (for source classification) can be applied. We demonstrate that this technique produces similar results to a more labor-intensive method used in many field campaigns over the past several years, but is simpler and better constrained by physical criteria that we impose, leading to the possibility of widespread adoption.
Giulia Ruggeri and Satoshi Takahama
Atmos. Chem. Phys., 16, 4401–4422, https://doi.org/10.5194/acp-16-4401-2016, https://doi.org/10.5194/acp-16-4401-2016, 2016
Short summary
Short summary
We present a set of tools for mapping molecular information to functional group composition. This allows us to reduce the complexity of representing the organic aerosol composition, as it consists of hundreds of thousands of different compounds. We describe the tools and methods for validation, and demonstrate several applications in which this tool can facilitate measurement intercomparisons and chemical modeling of aerosol chemistry.
Matteo Reggente, Ann M. Dillner, and Satoshi Takahama
Atmos. Meas. Tech., 9, 441–454, https://doi.org/10.5194/amt-9-441-2016, https://doi.org/10.5194/amt-9-441-2016, 2016
Short summary
Short summary
Organic carbon and elemental carbon are major components of atmospheric PM. Typically they are measured using destructive and relatively expensive methods (e.g., TOR). We aim to reduce the operating costs of large air quality monitoring networks using FT-IR spectra of ambient PTFE filters and PLS regression. We achieve accurate predictions for models (calibrated in 2011) that use samples collected at the same or different sites of the calibration data set and in a different year (2013).
B. R. Ayres, H. M. Allen, D. C. Draper, S. S. Brown, R. J. Wild, J. L. Jimenez, D. A. Day, P. Campuzano-Jost, W. Hu, J. de Gouw, A. Koss, R. C. Cohen, K. C. Duffey, P. Romer, K. Baumann, E. Edgerton, S. Takahama, J. A. Thornton, B. H. Lee, F. D. Lopez-Hilfiker, C. Mohr, P. O. Wennberg, T. B. Nguyen, A. Teng, A. H. Goldstein, K. Olson, and J. L. Fry
Atmos. Chem. Phys., 15, 13377–13392, https://doi.org/10.5194/acp-15-13377-2015, https://doi.org/10.5194/acp-15-13377-2015, 2015
Short summary
Short summary
This paper reports atmospheric gas- and aerosol-phase field measurements from the southeastern United States in summer 2013 to demonstrate that the oxidation of biogenic volatile organic compounds by nitrate radical produces a substantial amount of secondary organic aerosol in this region. This process, driven largely by monoterpenes, results in a comparable aerosol nitrate production rate to inorganic nitrate formation by heterogeneous uptake of HNO3 onto dust particles.
A. M. Dillner and S. Takahama
Atmos. Meas. Tech., 8, 4013–4023, https://doi.org/10.5194/amt-8-4013-2015, https://doi.org/10.5194/amt-8-4013-2015, 2015
Short summary
Short summary
Elemental carbon (EC), a constituent of atmospheric particulate matter (PM), adversely affects climate, visibility and human health. EC is measured in PM monitoring networks world-wide but the method is expensive and destructive to the samples. Here, methods are presented to accurately predict EC using Fourier transform infrared (FT-IR) analysis which is inexpensive and non-destructive. This method complements measurements of organic carbon and organic functional groups made using FT-IR.
H. M. Allen, D. C. Draper, B. R. Ayres, A. Ault, A. Bondy, S. Takahama, R. L. Modini, K. Baumann, E. Edgerton, C. Knote, A. Laskin, B. Wang, and J. L. Fry
Atmos. Chem. Phys., 15, 10669–10685, https://doi.org/10.5194/acp-15-10669-2015, https://doi.org/10.5194/acp-15-10669-2015, 2015
Short summary
Short summary
We report ion chromatographic measurements of gas- and aerosol-phase inorganic species at the SOAS 2013 field study. Our particular focus is on inorganic nitrate aerosol formation via HNO3 uptake onto coarse-mode dust and sea salt particles, which we find to be the dominant source of episodic inorganic nitrate at this site, due to the high acidity of the particles preventing formation of NH4NO3. We calculate a production rate of inorganic nitrate aerosol.
K. M. Seltzer, W. Vizuete, and B. H. Henderson
Atmos. Chem. Phys., 15, 5973–5986, https://doi.org/10.5194/acp-15-5973-2015, https://doi.org/10.5194/acp-15-5973-2015, 2015
A. M. Dillner and S. Takahama
Atmos. Meas. Tech., 8, 1097–1109, https://doi.org/10.5194/amt-8-1097-2015, https://doi.org/10.5194/amt-8-1097-2015, 2015
Short summary
Short summary
We demonstrate the feasibility of using FT-IR spectra of aerosols and a multivariate calibration to estimate organic carbon (OC) from thermal-optical reflectance analysis. Using 800 IMPROVE samples, we establish that prediction error can be explained by differences in distributions of OC and aerosol composition between calibration and test set. This work is an initial step in proposing a non-destructive analysis method that can reduce the operating costs of large air quality monitoring networks.
W. Tang, D. S. Cohan, A. Pour-Biazar, L. N. Lamsal, A. T. White, X. Xiao, W. Zhou, B. H. Henderson, and B. F. Lash
Atmos. Chem. Phys., 15, 1601–1619, https://doi.org/10.5194/acp-15-1601-2015, https://doi.org/10.5194/acp-15-1601-2015, 2015
Short summary
Short summary
A joint application of multiple satellite-derived model inputs to improve Texas O3 SIP modeling is demonstrated in this study. The GOES-retrieved clouds are applied to correct the modeled photolysis rates, and the DKF inversion approach is incorporated into the CAMx-DDM model to adjust NOx emissions using OMI NO2. Using both GOES-derived photolysis rates and OMI-constrained NOx emissions together improves O3 simulations and makes O3 more sensitive to NOx emissions in the O3 non-attainment areas.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
Short summary
Short summary
Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
A. L. Corrigan, L. M. Russell, S. Takahama, M. Äijälä, M. Ehn, H. Junninen, J. Rinne, T. Petäjä, M. Kulmala, A. L. Vogel, T. Hoffmann, C. J. Ebben, F. M. Geiger, P. Chhabra, J. H. Seinfeld, D. R. Worsnop, W. Song, J. Auld, and J. Williams
Atmos. Chem. Phys., 13, 12233–12256, https://doi.org/10.5194/acp-13-12233-2013, https://doi.org/10.5194/acp-13-12233-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods
Nocturnal atmospheric synergistic oxidation reduces the formation of low-volatility organic compounds from biogenic emissions
The interplay between aqueous replacement reaction and the phase state of internally mixed organic/ammonium aerosols
Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers
Enhanced Sulfate Formation in Mixed Biomass Burning and Sea-salt Particles Mediated by Photosensitization: Effects of Chloride and Nitrogen-containing Compounds
Characterization of the particle size distribution, mineralogy, and Fe mode of occurrence of dust-emitting sediments from the Mojave Desert, California, USA
Heterogeneous formation and light absorption of secondary organic aerosols from acetone photooxidation: Remarkably enhancing effects of seeds and ammonia
Atmospheric oxidation of 1,3-butadiene: influence of acidity and relative humidity on SOA composition and air toxic compounds
Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China
Probing Iceland's dust-emitting sediments: particle size distribution, mineralogy, cohesion, Fe mode of occurrence, and reflectance spectra signatures
Photoenhanced sulfate formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
Comparison of water-soluble and water-insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Technical note: High-resolution analyses of concentrations and sizes of black carbon particles deposited on northwest Greenland over the past 350 years – Part 1. Continuous flow analysis of the SIGMA-D ice core using a Wide-Range Single-Particle Soot Photometer and a high-efficiency nebulizer
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
The impact of nanostructure on hygroscopicity and reactivity of fatty acid atmospheric aerosol proxies
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Temperature-dependent aqueous OH kinetics of C2–C10 linear and terpenoid alcohols and diols: new rate coefficients, structure–activity relationship, and atmospheric lifetimes
A possible unaccounted source of nitrogen-containing compound formation in aerosols: amines reacting with secondary ozonides
Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles
Variability in sediment particle size, mineralogy, and Fe mode of occurrence across dust-source inland drainage basins: the case of the lower Drâa Valley, Morocco
Gas–particle partitioning of toluene oxidation products: an experimental and modeling study
Chemically speciated air pollutant emissions from open burning of household solid waste from South Africa
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Volatile oxidation products and secondary organosiloxane aerosol from D5 + OH at varying OH exposures
Molecular fingerprints and health risks of smoke from home-use incense burning
High enrichment of heavy metals in fine particulate matter through dust aerosol generation
Production of ice-nucleating particles (INPs) by fast-growing phytoplankton
Technical note: In situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a quartz crystal microbalance with dissipation monitoring (QCM-D)
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
Quantifying the seasonal variations in and regional transport of PM2.5 in the Yangtze River Delta region, China: characteristics, sources, and health risks
Opinion: Atmospheric multiphase chemistry – past, present, and future
Distinct photochemistry in glycine particles mixed with different atmospheric nitrate salts
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Characterization of gas and particle emissions from open burning of household solid waste from South Africa
Chemically distinct particle-phase emissions from highly controlled pyrolysis of three wood types
Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles
Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic
Large differences of highly oxygenated organic molecules (HOMs) and low-volatile species in secondary organic aerosols (SOAs) formed from ozonolysis of β-pinene and limonene
Impact of fossil and non-fossil fuel sources on the molecular compositions of water-soluble humic-like substances in PM2.5 at a suburban site of Yangtze River Delta, China
Technical note: Improved synthetic routes to cis- and trans-(2-methyloxirane-2,3-diyl)dimethanol (cis- and trans-β-isoprene epoxydiol)
Technical note: Intercomparison study of the elemental carbon radiocarbon analysis methods using synthetic known samples
Julia Pikmann, Frank Drewnick, Friederike Fachinger, and Stephan Borrmann
Atmos. Chem. Phys., 24, 12295–12321, https://doi.org/10.5194/acp-24-12295-2024, https://doi.org/10.5194/acp-24-12295-2024, 2024
Short summary
Short summary
Cooking activities can contribute substantially to indoor and ambient aerosol. We performed a comprehensive study with laboratory measurements cooking 19 different dishes and ambient measurements at two Christmas markets measuring various particle properties and trace gases of emissions in real time. Similar emission characteristics were observed for dishes with the same preparation method, mainly due to similar cooking temperature and use of oil, with barbecuing as an especially strong source.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
Short summary
Short summary
Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 24, 11619–11635, https://doi.org/10.5194/acp-24-11619-2024, https://doi.org/10.5194/acp-24-11619-2024, 2024
Short summary
Short summary
Atmospheric secondary aerosols, composed of organic and inorganic components, undergo complex reactions that impact their phase state. Using molecular spectroscopy, we showed that ammonium-promoted aqueous replacement reaction, unique to these aerosols, is closely linked to phase behavior. The interplay between reactions and aerosol phase state can cause atypical phase transition and irreversible changes in aerosol composition during hygroscopic cycles, further impacting atmospheric processes.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
Short summary
Short summary
Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2633, https://doi.org/10.5194/egusphere-2024-2633, 2024
Short summary
Short summary
This study provided laboratory evidence that the photosensitizers in biomass burning extracts can enhance the sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air, with less contribution of direct photosensitization via triplets.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Melani Hernández-Chiriboga, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert Green, Paul Ginoux, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 9155–9176, https://doi.org/10.5194/acp-24-9155-2024, https://doi.org/10.5194/acp-24-9155-2024, 2024
Short summary
Short summary
In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understanding the effect of dust upon climate. We found two different playa lakes according to the groundwater regime, which implies differences in crusts' cohesion state and mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
Si Zhang, Xinbei Xu, Luyao Chen, Can Wu, Zheng Li, Rongjie Li, Binyu Xiao, Xiaodi Liu, Rui Li, Fan Zhang, and Gehui Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2119, https://doi.org/10.5194/egusphere-2024-2119, 2024
Short summary
Short summary
SOA from acetone photooxidation can be formed more readily on neutral aerosols than on acidic aerosols, while heterogeneous reaction of carbonyl with ammonium is only active on acidic aerosols in the presence of NH3, which produces light-absorbing N-containing compounds. Our work suggested that the heterogeneous oxidation of highly volatile VOC, for example acetone, is an importance source of SOA in the atmosphere, which should be accounted for in the future model studies.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof Rudzinski, Michael Lewandowski, Tadeusz Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
EGUsphere, https://doi.org/10.5194/egusphere-2024-2032, https://doi.org/10.5194/egusphere-2024-2032, 2024
Short summary
Short summary
Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications to urban air quality. Health effects studies have focused on whole particulate matter but compounds responsible for adverse health effects remain uncertain. This study provides the effect of relative humidity and acidity on the chemical composition of aerosol formed from 13BD photooxidation.
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, and Xinming Wang
Atmos. Chem. Phys., 24, 7575–7589, https://doi.org/10.5194/acp-24-7575-2024, https://doi.org/10.5194/acp-24-7575-2024, 2024
Short summary
Short summary
The present research unveiled that acidity dominates while transition metal ions harmonize with the light absorption properties of humic-like substances (HULIS). Cu2+ has quenching effects on HULIS by complexation, hydrogen substitution, or electrostatic adsorption, with aromatic structures of HULIS. Such effects are less pronounced if from Mn2+, Ni2+, Zn2+, and Cu2+. Oxidized HULIS might contain electron-donating groups, whereas N-containing compounds might contain electron-withdrawing groups.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert O. Green, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 6883–6910, https://doi.org/10.5194/acp-24-6883-2024, https://doi.org/10.5194/acp-24-6883-2024, 2024
Short summary
Short summary
The knowledge of properties from dust emitted in high latitudes such as in Iceland is scarce. This study focuses on the particle size, mineralogy, cohesion, and iron mode of occurrence and reflectance spectra of dust-emitting sediments. Icelandic top sediments have lower cohesion state, coarser particle size, distinctive mineralogy, and 3-fold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
Wangjin Yang, Jiawei Ma, Hongxing Yang, Fu Li, and Chong Han
Atmos. Chem. Phys., 24, 6757–6768, https://doi.org/10.5194/acp-24-6757-2024, https://doi.org/10.5194/acp-24-6757-2024, 2024
Short summary
Short summary
We provide evidence that light enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where triplet states of SO2 (3SO2) can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. The SO2 photochemistry on non-photoactive mineral dust contributes to sulfates, highlighting previously unknown pathways to better explain the missing sources of atmospheric sulfates.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
Atmos. Chem. Phys., 24, 6323–6337, https://doi.org/10.5194/acp-24-6323-2024, https://doi.org/10.5194/acp-24-6323-2024, 2024
Short summary
Short summary
Brown carbon (BrC) is related to radiative forcing and climate change. The BrC fraction from residential coal and biomass burning emissions, which were the major source of BrC, was characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coal. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, and such information could be used for source appointment.
Kumiko Goto-Azuma, Remi Dallmayr, Yoshimi Ogawa-Tsukagawa, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Motohiro Hirabayashi, Jun Ogata, Kyotaro Kitamura, Kenji Kawamura, Koji Fujita, Sumito Matoba, Naoko Nagatsuka, Akane Tsushima, Kaori Fukuda, and Teruo Aoki
EGUsphere, https://doi.org/10.5194/egusphere-2024-1496, https://doi.org/10.5194/egusphere-2024-1496, 2024
Short summary
Short summary
We developed a continuous flow analysis system to analyse an ice core from northwest Greenland, and coupled it with an improved BC measurement technique. This coupling allowed accurate high-resolution analyses of BC particles' size distributions and concentrations with diameters between 70 nm and 4 μm for the past 350 years. Our results provide crucial insights into BC's climatic effects. We also found that previous ice core studies substantially underestimated the BC mass concentrations.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
Short summary
Short summary
Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
Short summary
Short summary
We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
Short summary
Short summary
We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Adam Milsom, Adam M. Squires, Ben Laurence, Ben Wōden, Andrew J. Smith, Andrew D. Ward, and Christian Pfrang
EGUsphere, https://doi.org/10.5194/egusphere-2024-905, https://doi.org/10.5194/egusphere-2024-905, 2024
Short summary
Short summary
We followed nano-structural changes in mixtures found in urban organic aerosol emissions (oleic acid, sodium oleate & fructose) during humidity change & ozone exposure. We demonstrate that self-assembly of fatty acid nanostructures can impact on water uptake & chemical reactivity affecting atmospheric lifetimes, urban air quality (protecting harmful emissions from degradation and enabling their long-range transport) & climate (affecting cloud formation) with implications for human health.
Xingjun Fan, Ao Cheng, Xufang Yu, Tao Cao, Dan Chen, Wenchao Ji, Yongbing Cai, Fande Meng, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 24, 3769–3783, https://doi.org/10.5194/acp-24-3769-2024, https://doi.org/10.5194/acp-24-3769-2024, 2024
Short summary
Short summary
Molecular-level characteristics of high molecular weight (HMW) and low MW (LMW) humic-like substances (HULIS) were comprehensively investigated, where HMW HULIS had larger chromophores and larger molecular size than LMW HULIS and exhibited higher aromaticity and humification. Electrospray ionization high-resolution mass spectrometry revealed more aromatic molecules in HMW HULIS. HMW HULIS had more CHON compounds, while LMW HULIS had more CHO compounds.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
Short summary
Short summary
The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
Short summary
Short summary
We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
Short summary
Short summary
Secondary organic aerosol (SOA) from gasoline vehicles can be a significant source of particulate matter in urban areas. Here the chemical composition of secondary volatile organic compounds and SOA produced by photo-oxidation of Euro 5 gasoline vehicle emissions was studied. The volatility of the SOA formed was calculated. Except for the temperature and the concentration of the aerosol, additional parameters may play a role in the gas-to-particle partitioning.
András Hoffer, Aida Meiramova, Ádám Tóth, Beatrix Jancsek-Turóczi, Gyula Kiss, Ágnes Rostási, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 24, 1659–1671, https://doi.org/10.5194/acp-24-1659-2024, https://doi.org/10.5194/acp-24-1659-2024, 2024
Short summary
Short summary
Specific tracer compounds identified previously in controlled test burnings of different waste types in the laboratory were detected and quantified in ambient PM10 samples collected in five Hungarian and four Romanian settlements. Back-of-the-envelope calculations based on the relative emission factors of individual tracers suggested that the contribution of solid waste burning particulate emissions to ambient PM10 mass concentrations may be as high as a few percent.
Xiao-San Luo, Weijie Huang, Guofeng Shen, Yuting Pang, Mingwei Tang, Weijun Li, Zhen Zhao, Hanhan Li, Yaqian Wei, Longjiao Xie, and Tariq Mehmood
Atmos. Chem. Phys., 24, 1345–1360, https://doi.org/10.5194/acp-24-1345-2024, https://doi.org/10.5194/acp-24-1345-2024, 2024
Short summary
Short summary
PM2.5 are air pollutants threatening health globally, but they are a mixture of chemical compositions from many sources and result in unequal toxicity. Which composition from which source of PM2.5 as the most hazardous object is a question hindering effective pollution control policy-making. With chemical and toxicity experiments, we found automobile exhaust and coal combustion to be priority emissions with higher toxic compositions for precise air pollution control, ensuring public health.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
Short summary
Short summary
The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Ryan J. Patnaude, Kathryn A. Moore, Russell J. Perkins, Thomas C. J. Hill, Paul J. DeMott, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 24, 911–928, https://doi.org/10.5194/acp-24-911-2024, https://doi.org/10.5194/acp-24-911-2024, 2024
Short summary
Short summary
In this study we examined the effect of atmospheric aging on sea spray aerosols (SSAs) to form ice and how newly formed secondary marine aerosols (SMAs) may freeze at cirrus temperatures (< −38 °C). Results show that SSAs freeze at different relative humidities (RHs) depending on the temperature and that the ice-nucleating ability of SSA was not hindered by atmospheric aging. SMAs are shown to freeze at high RHs and are likely inefficient at forming ice at cirrus temperatures.
Bartłomiej Witkowski, Priyanka Jain, Beata Wileńska, and Tomasz Gierczak
Atmos. Chem. Phys., 24, 663–688, https://doi.org/10.5194/acp-24-663-2024, https://doi.org/10.5194/acp-24-663-2024, 2024
Short summary
Short summary
This article reports the results of the kinetic measurements for the aqueous oxidation of the 29 aliphatic alcohols by hydroxyl radical (OH) at different temperatures. The data acquired and the literature data were used to optimize a model for predicting the aqueous OH reactivity of alcohols and carboxylic acids and to estimate the atmospheric lifetimes of five terpenoic alcohols. The kinetic data provided new insights into the mechanism of aqueous oxidation of aliphatic molecules by the OH.
Junting Qiu, Xinlin Shen, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 155–166, https://doi.org/10.5194/acp-24-155-2024, https://doi.org/10.5194/acp-24-155-2024, 2024
Short summary
Short summary
We studied reactions of secondary ozonides (SOZs) with amines. SOZs formed from ozonolysis of β-caryophyllene and α-humulene are found to be reactive to ethylamine and methylamine. Products from SOZs with various conformations reacting with the same amine had different functional groups. Our findings indicate that interaction of SOZs with amines in the atmosphere is very complicated, which is potentially a hitherto unrecognized source of N-containing compound formation.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
Short summary
Short summary
We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Cristina Reche, Patricia Córdoba, Natalia Moreno, Andres Alastuey, Konrad Kandler, Martina Klose, Clarissa Baldo, Roger N. Clark, Zongbo Shi, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 15815–15834, https://doi.org/10.5194/acp-23-15815-2023, https://doi.org/10.5194/acp-23-15815-2023, 2023
Short summary
Short summary
The effect of dust emitted from desertic surfaces upon climate and ecosystems depends on size and mineralogy, but data from soil mineral atlases of desert soils are scarce. We performed particle-size distribution, mineralogy, and Fe speciation in southern Morocco. Results show coarser particles with high quartz proportion are near the elevated areas, while in depressed areas, sizes are finer, and proportions of clays and nano-Fe oxides are higher. This difference is important for dust modelling.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
Short summary
Short summary
Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Steven Sai Hang Ho, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 15375–15393, https://doi.org/10.5194/acp-23-15375-2023, https://doi.org/10.5194/acp-23-15375-2023, 2023
Short summary
Short summary
Open burning of municipal solid waste emits chemicals that are harmful to the environment. This paper reports source profiles and emission factors for PM2.5 species and acidic/alkali gases from laboratory combustion of 10 waste categories (including plastics and biomass) that represent open burning in South Africa. Results will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
Short summary
Short summary
We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
Short summary
Short summary
D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
Kai Song, Rongzhi Tang, Jingshun Zhang, Zichao Wan, Yuan Zhang, Kun Hu, Yuanzheng Gong, Daqi Lv, Sihua Lu, Yu Tan, Ruifeng Zhang, Ang Li, Shuyuan Yan, Shichao Yan, Baoming Fan, Wenfei Zhu, Chak K. Chan, Maosheng Yao, and Song Guo
Atmos. Chem. Phys., 23, 13585–13595, https://doi.org/10.5194/acp-23-13585-2023, https://doi.org/10.5194/acp-23-13585-2023, 2023
Short summary
Short summary
Incense burning is common in Asia, posing threats to human health and air quality. However, less is known about its emissions and health risks. Full-volatility organic species from incense-burning smoke are detected and quantified. Intermediate-volatility volatile organic compounds (IVOCs) are crucial organics accounting for 19.2 % of the total emission factors (EFs) and 40.0 % of the secondary organic aerosol (SOA) estimation, highlighting the importance of incorporating IVOCs into SOA models.
Qianqian Gao, Shengqiang Zhu, Kaili Zhou, Jinghao Zhai, Shaodong Chen, Qihuang Wang, Shurong Wang, Jin Han, Xiaohui Lu, Hong Chen, Liwu Zhang, Lin Wang, Zimeng Wang, Xin Yang, Qi Ying, Hongliang Zhang, Jianmin Chen, and Xiaofei Wang
Atmos. Chem. Phys., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
Short summary
Short summary
Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Dust aerosols are mainly generated by wind erosion, which may have some chemical selectivity. Mn, Cd and Pb were found to be highly enriched in fine-dust (PM2.5) aerosols. In addition, estimation of heavy metal emissions from dust generation by air quality models may have errors without using proper dust profiles.
Daniel C. O. Thornton, Sarah D. Brooks, Elise K. Wilbourn, Jessica Mirrielees, Alyssa N. Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana McFadden
Atmos. Chem. Phys., 23, 12707–12729, https://doi.org/10.5194/acp-23-12707-2023, https://doi.org/10.5194/acp-23-12707-2023, 2023
Short summary
Short summary
A major uncertainty in our understanding of clouds and climate is the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast-growing marine phytoplankton was a source of ice-nucleating particles (INPs). INPs facilitate freezing of ice crystals at warmer temperatures than otherwise possible and therefore change cloud formation and properties. Our results show that ecosystem processes and the properties of sea spray aerosol are linked.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 2023
Short summary
Short summary
Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
Atmos. Chem. Phys., 23, 10809–10822, https://doi.org/10.5194/acp-23-10809-2023, https://doi.org/10.5194/acp-23-10809-2023, 2023
Short summary
Short summary
In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene). We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content in aerosol formation and inform ongoing research on particle environmental effects and applications in models.
Yangzhihao Zhan, Min Xie, Wei Zhao, Tijian Wang, Da Gao, Pulong Chen, Jun Tian, Kuanguang Zhu, Shu Li, Bingliang Zhuang, Mengmeng Li, Yi Luo, and Runqi Zhao
Atmos. Chem. Phys., 23, 9837–9852, https://doi.org/10.5194/acp-23-9837-2023, https://doi.org/10.5194/acp-23-9837-2023, 2023
Short summary
Short summary
Although the main source contribution of pollution is secondary inorganic aerosols in Nanjing, health risks mainly come from industry sources and vehicle emissions. Therefore, the development of megacities should pay more attention to the health burden of vehicle emissions, coal combustion, and industrial processes. This study provides new insight into assessing the relationship between source apportionment and health risks and can provide valuable insight into air pollution strategies.
Jonathan P. D. Abbatt and A. R. Ravishankara
Atmos. Chem. Phys., 23, 9765–9785, https://doi.org/10.5194/acp-23-9765-2023, https://doi.org/10.5194/acp-23-9765-2023, 2023
Short summary
Short summary
With important climate and air quality impacts, atmospheric multiphase chemistry involves gas interactions with aerosol particles and cloud droplets. We summarize the status of the field and discuss potential directions for future growth. We highlight the importance of a molecular-level understanding of the chemistry, along with atmospheric field studies and modeling, and emphasize the necessity for atmospheric multiphase chemists to interact widely with scientists from neighboring disciplines.
Zhancong Liang, Zhihao Cheng, Ruifeng Zhang, Yiming Qin, and Chak K. Chan
Atmos. Chem. Phys., 23, 9585–9595, https://doi.org/10.5194/acp-23-9585-2023, https://doi.org/10.5194/acp-23-9585-2023, 2023
Short summary
Short summary
In this study, we found that the photolysis of sodium nitrate leads to a much quicker decay of free amino acids (FAAs, with glycine as an example) in the particle phase than ammonium nitrate photolysis, which is likely due to the molecular interactions between FAAs and different nitrate salts. Since sodium nitrate likely co-exists with FAAs in the coarse-mode particles, particulate nitrate photolysis can possibly contribute to a rapid decay of FAAs and affect atmospheric nitrogen cycling.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
Short summary
Short summary
Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 8921–8937, https://doi.org/10.5194/acp-23-8921-2023, https://doi.org/10.5194/acp-23-8921-2023, 2023
Short summary
Short summary
Open burning of household and municipal solid waste is a common practice in developing countries and is a significant source of air pollution. However, few studies have measured emissions from open burning of waste. This study determined gas and particulate emissions from open burning of 10 types of household solid-waste materials. These results can improve emission inventories, air quality management, and assessment of the health and climate effects of open burning of household waste.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
Short summary
Short summary
Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
Short summary
Short summary
Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
Short summary
Short summary
Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Dandan Liu, Yun Zhang, Shujun Zhong, Shuang Chen, Qiaorong Xie, Donghuan Zhang, Qiang Zhang, Wei Hu, Junjun Deng, Libin Wu, Chao Ma, Haijie Tong, and Pingqing Fu
Atmos. Chem. Phys., 23, 8383–8402, https://doi.org/10.5194/acp-23-8383-2023, https://doi.org/10.5194/acp-23-8383-2023, 2023
Short summary
Short summary
Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) exhibit higher yield at high ozone concentration, while limonene oxidation-derived HOMs exhibit higher yield at moderate ozone concentration. The distinct molecular response of HOMs and low-volatile species in different biogenic secondary organic aerosols to ozone concentrations provides a new clue for more accurate air quality prediction and management.
Mengying Bao, Yan-Lin Zhang, Fang Cao, Yihang Hong, Yu-Chi Lin, Mingyuan Yu, Hongxing Jiang, Zhineng Cheng, Rongshuang Xu, and Xiaoying Yang
Atmos. Chem. Phys., 23, 8305–8324, https://doi.org/10.5194/acp-23-8305-2023, https://doi.org/10.5194/acp-23-8305-2023, 2023
Short summary
Short summary
The interaction between the sources and molecular compositions of humic-like substances (HULIS) at Nanjing, China, was explored. Significant fossil fuel source contributions to HULIS were found in the 14C results from biomass burnng and traffic emissions. Increasing biogenic secondary organic aerosol (SOA) products and anthropogenic aromatic compounds were detected in summer and winter, respectively.
Molly Frauenheim, Jason D. Surratt, Zhenfa Zhang, and Avram Gold
Atmos. Chem. Phys., 23, 7859–7866, https://doi.org/10.5194/acp-23-7859-2023, https://doi.org/10.5194/acp-23-7859-2023, 2023
Short summary
Short summary
We report synthesis of the isoprene-derived photochemical oxidation products trans- and cis-β-epoxydiols in high overall yields from inexpensive, readily available starting compounds. Protection/deprotection steps or time-consuming purification is not required, and the reactions can be scaled up to gram quantities. The procedures provide accessibility of these important compounds to atmospheric chemistry laboratories with only basic capabilities in organic synthesis.
Xiangyun Zhang, Jun Li, Sanyuan Zhu, Junwen Liu, Ping Ding, Shutao Gao, Chongguo Tian, Yingjun Chen, Ping'an Peng, and Gan Zhang
Atmos. Chem. Phys., 23, 7495–7502, https://doi.org/10.5194/acp-23-7495-2023, https://doi.org/10.5194/acp-23-7495-2023, 2023
Short summary
Short summary
The results show that 14C elemental carbon (EC) was not only related to the isolation method but also to the types and proportions of the biomass sources in the sample. The hydropyrolysis (Hypy) method, which can be used to isolate a highly stable portion of ECHypy and avoid charring, is a more effective and stable approach for the matrix-independent 14C quantification of EC in aerosols, and the 13C–ECHypy and non-fossil ECHypy values of SRM1649b were –24.9 ‰ and 11 %, respectively.
Cited articles
Aimanant, S. and Ziemann, P. J.: Development of Spectrophotometric Methods for the Analysis of Functional Groups in Oxidized Organic Aerosol, Aerosol Sci. Tech., 47, 581–591, https://doi.org/10.1080/02786826.2013.773579, 2013.
Allen, D. T., Palen, E. J., Haimov, M. I., Hering, S. V., and Young, J. R.: Fourier-transform Infrared-spectroscopy of Aerosol Collected In A Low-pressure Impactor (LPI/FTIR) – Method Development and Field Calibration, Aerosol Sci. Tech., 21, 325–342, https://doi.org/10.1080/02786829408959719, 1994.
Aschmann, S. M., Atkinson, R., and Arey, J.: Products of reaction of OH radicals with α-pinene, J. Geophys. Res.-Atmos., 107, ACH 6-1–ACH 6-7, https://doi.org/10.1029/2001JD001098, 2002.
Aumont, B., Szopa, S., and Madronich, S.: Modelling the evolution of organic carbon during its gas-phase tropospheric oxidation: development of an explicit model based on a self generating approach, Atmos. Chem. Phys., 5, 2497–2517, https://doi.org/10.5194/acp-5-2497-2005, 2005.
Aumont, B., Valorso, R., Mouchel-Vallon, C., Camredon, M., Lee-Taylor, J., and Madronich, S.: Modeling SOA formation from the oxidation of intermediate volatility n-alkanes, Atmos. Chem. Phys., 12, 7577–7589, https://doi.org/10.5194/acp-12-7577-2012, 2012.
Barley, M. H., Topping, D., Lowe, D., Utembe, S., and McFiggans, G.: The sensitivity of secondary organic aerosol (SOA) component partitioning to the predictions of component properties – Part 3: Investigation of condensed compounds generated by a near-explicit model of VOC oxidation, Atmos. Chem. Phys., 11, 13145–13159, https://doi.org/10.5194/acp-11-13145-2011, 2011.
Bloss, C., Wagner, V., Jenkin, M. E., Volkamer, R., Bloss, W. J., Lee, J. D., Heard, D. E., Wirtz, K., Martin-Reviejo, M., Rea, G., Wenger, J. C., and Pilling, M. J.: Development of a detailed chemical mechanism (MCMv3.1) for the atmospheric oxidation of aromatic hydrocarbons, Atmos. Chem. Phys., 5, 641–664, https://doi.org/10.5194/acp-5-641-2005, 2005.
Bonn, B., von Kuhlmann, R., and Lawrence, M. G.: High contribution of biogenic hydroperoxides to secondary organic aerosol formation, Geophys. Res. Lett., 31, L10108, https://doi.org/10.1029/2003GL019172, 2004.
Capouet, M., Mueller, J. F., Ceulemans, K., Compernolle, S., Vereecken, L., and Peeters, J.: Modeling aerosol formation in alpha-pinene photo-oxidation experiments, J. Geophys. Res.-Atmos., 113, D02308, https://doi.org/10.1029/2007JD008995, 2008.
Cappa, C. D.: A model of aerosol evaporation kinetics in a thermodenuder, Atmos. Meas. Tech., 3, 579–592, https://doi.org/10.5194/amt-3-579-2010, 2010.
Cappa, C. D. and Wilson, K. R.: Multi-generation gas-phase oxidation, equilibrium partitioning, and the formation and evolution of secondary organic aerosol, Atmos. Chem. Phys., 12, 9505–9528, https://doi.org/10.5194/acp-12-9505-2012, 2012.
Cappa, C. D., Jathar, S. H., Kleeman, M. J., Docherty, K. S., Jimenez, J. L., Seinfeld, J. H., and Wexler, A. S.: Simulating secondary organic aerosol in a regional air quality model using the statistical oxidation model – Part 2: Assessing the influence of vapor wall losses, Atmos. Chem. Phys., 16, 3041–3059, https://doi.org/10.5194/acp-16-3041-2016,, 2016.
Chameides, W., Lindsay, R., Richardson, J., and Kiang, C.: The role of biogenic hydrocarbons in urban photochemical smog: Atlanta as a case study, Science, 241, 1473–1475, https://doi.org/10.1126/science.3420404, 1988.
Chang, E. I. and Pankow, J. F.: Organic particulate matter formation at varying relative humidity using surrogate secondary and primary organic compounds with activity corrections in the condensed phase obtained using a method based on the Wilson equation, Atmos. Chem. Phys., 10, 5475–5490, https://doi.org/10.5194/acp-10-5475-2010, 2010.
Chen, Q., Liu, Y., Donahue, N. M., Shilling, J. E., and Martin, S. T.: Particle-phase chemistry of secondary organic material: modeled compared to measured O:C and H:C elemental ratios provide constraints, Environ. Sci. Technol., 45, 4763–4770, https://doi.org/10.1021/es104398s, 2011.
Chhabra, P. S., Ng, N. L., Canagaratna, M. R., Corrigan, A. L., Russell, L. M., Worsnop, D. R., Flagan, R. C., and Seinfeld, J. H.: Elemental composition and oxidation of chamber organic aerosol, Atmos. Chem. Phys., 11, 8827–8845, https://doi.org/10.5194/acp-11-8827-2011, 2011.
Cleveland, M. J., Ziemba, L. D., Griffin, R. J., Dibb, J. E., Anderson, C. H., Lefer, B., and Rappenglück, B.: Characterization of urban aerosol using aerosol mass spectrometry and proton nuclear magnetic resonance spectroscopy, Atmos. Environ., 54, 511–518, https://doi.org/10.1016/j.atmosenv.2012.02.074, 2012.
Cocker, D. R., Clegg, S. L., Flagan, R. C., and Seinfeld, J. H.: The effect of water on gas-particle partitioning of secondary organic aerosol. Part I: alpha-pinene/ozone system, Atmos. Environ., 35, 6049–6072, https://doi.org/10.1016/S1352-2310(01)00404-6, 2001.
Compernolle, S., Ceulemans, K., and Muller, J. F.: EVAPORATION: a new vapour pressure estimation methodfor organic molecules including non-additivity and intramolecular interactions, Atmos. Chem. Phys., 11, 9431–9450, https://doi.org/10.5194/acp-11-9431-2011, 2011.
Coury, C. and Dillner, A. M.: A method to quantify organic functional groups and inorganic compounds in ambient aerosols using attenuated total reflectance FTIR spectroscopy and multivariate chemometric techniques, Atmos. Environ., 42, 5923–5932, https://doi.org/10.1016/j.atmosenv.2008.03.026, 2008.
Damian, V., Sandu, A., Damian, M., Potra, F., and Carmichael, G. R.: The kinetic preprocessor KPP-a software environment for solving chemical kinetics, Comput. Chem. Eng., 26, 1567–1579, https://doi.org/10.1016/S0098-1354(02)00128-X, 2002.
Day, D. A., Liu, S., Russell, L. M., and Ziemann, P. J.: Organonitrate group concentrations in submicron particles with high nitrate and organic fractions in coastal southern California, Atmos. Environ., 44, 1970–1979, https://doi.org/10.1016/j.atmosenv.2010.02.045, 2010.
DAYLIGHT Chemical Information Systems, I.: SMARTS – A Language for Describing Molecular Patterns, http://www.daylight.com/dayhtml/doc/theory/theory.smarts.html, last access: 30 September 2015.
Decesari, S., Mircea, M., Cavalli, F., Fuzzi, S., Moretti, F., Tagliavini, E., and Facchini, M. C.: Source attribution of water-soluble organic aerosol by nuclear magnetic resonance spectroscopy, Environ. Sci. Technol., 41, 2479–2484, https://doi.org/10.1021/es061711l, 2007.
Derwent, R. G., Jenkin, M., and Saunders, S.: Photochemical ozone creation potentials for a large number of reactive hydrocarbons under European conditions, Atmos. Environ., 30, 181–199, https://doi.org/10.1016/1352-2310(95)00303-G, 1996.
Derwent, R. G., Jenkin, M. E., Saunders, S. M., and Pilling, M. J.: Photochemical ozone creation potentials for organic compounds in northwest Europe calculated with a master chemical mechanism, Atmos. Environ., 32, 2429–2441, https://doi.org/10.1016/S1352-2310(98)00053-3, 1998.
Docherty, K. S., Wu, W., Lim, Y. B., and Ziemann, P. J.: Contributions of organic peroxides to secondary aerosol formed from reactions of monoterpenes with O3, Environ. Sci. Technol., 39, 4049–4059, https://doi.org/10.1021/es050228s, 2005.
Donahue, N. M., Kroll, J. H., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set – Part 2: Diagnostics of organic-aerosol evolution, Atmos. Chem. Phys., 12, 615–634, https://doi.org/10.5194/acp-12-615-2012, 2012.
Donahue, N. M., Chuang, W., Epstein, S. A., Kroll, J. H., Worsnop, D. R., Robinson, A. L., Adams, P. J., and Pandis, S. N.: Why do organic aerosols exist? Understanding aerosol lifetimes using the two-dimensional volatility basis set, Environ. Chem., 10, 151–157, https://doi.org/10.1071/EN13022, 2013.
Dron, J., El Haddad, I., Temime-Roussel, B., Jaffrezo, J.-L., Wortham, H., and Marchand, N.: Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry, Atmos. Chem. Phys., 10, 7041–7055, https://doi.org/10.5194/acp-10-7041-2010, 2010.
Eddingsaas, N. C., Loza, C. L., Yee, L. D., Seinfeld, J. H., and Wennberg, P. O.: alpha-pinene photooxidation under controlled chemical conditions – Part 1: Gas-phase composition in low- and high-NOx environments, Atmos. Chem. Phys., 12, 6489–6504, https://doi.org/10.5194/acp-12-6489-2012, 2012.
Ehn, M., Thornton, J. A., Kleist, E., Sipilä, M., Junninen, H., Pullinen, I., Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F., Andres, S., Acir, I.-H., Rissanen, M., Jokinen, T., Schobesberger, S., Kangasluoma, J., Kontkanen, J., Nieminen, T., Kurtén, T., Nielsen, L. B., Jorgensen, S., Kjaergaard, H. G., Canagaratna, M., Maso, M. D., Berndt, T., Petäjä, T., Wahner, A., Kerminen, V.-M., Kulmala, M., Worsnop, D. R., Wildt, J., and Mentel, T. F.: A large source of low-volatility secondary organic aerosol, Nature, 506, 476–479, https://doi.org/10.1038/nature13032, 2014.
Epstein, S. A. and Donahue, N. M.: Ozonolysis of Cyclic Alkenes as Surrogates for Biogenic Terpenes: Primary Ozonide Formation and Decomposition, J. Phys. Chem. A, 114, 7509–7515, https://doi.org/10.1021/jp102177v, 2010.
Epstein, S. A., Blair, S. L., and Nizkorodov, S. A.: Direct Photolysis of α-Pinene Ozonolysis Secondary Organic Aerosol: Effect on Particle Mass and Peroxide Content, Environ. Sci. Technol., 48, 11251–11258, https://doi.org/10.1021/es502350u, 2014.
Fehsenfeld, F., Calvert, J., Fall, R., Goldan, P., Guenther, A. B., Hewitt, C. N., Lamb, B., Liu, S., Trainer, M., Westberg, H., and Zimmerman, P.: Emissions of volatile organic compounds from vegetation and the implications for atmospheric chemistry, Global Biogeochem. Cy., 6, 389–430, https://doi.org/10.1029/92GB02125, 1992.
Fuentes, J. D., Gu, L., Lerdau, M., Atkinson, R., Baldocchi, D., Bottenheim, J. W., Ciccioli, P., Lamb, B., Geron, C., Guenther, A., Sharkey, T. D., and Stockwell, W.: Biogenic Hydrocarbons in the Atmospheric Boundary Layer: A Review, B. Am. Meteorol. Soc., 81, 1537–1575, https://doi.org/10.1175/1520-0477(2000)081<1537:BHITAB>2.3.CO;2, 2000.
Gao, C. W., Allen, J. W., Green, W. H., and West, R. H.: Reaction Mechanism Generator: Automatic construction of chemical kinetic mechanisms, Comput. Phys. Commun., 203, 212–225, https://doi.org/10.1016/j.cpc.2016.02.013, 2016.
Gao, S., Keywood, M., Ng, N. L., Surratt, J., Varutbangkul, V., Bahreini, R., Flagan, R. C., and Seinfeld, J. H.: Low-molecular-weight and oligomeric components in secondary organic aerosol from the ozonolysis of cycloalkenes and alpha-pinene, J. Phys. Chem. A, 108, 10147–10164, https://doi.org/10.1021/jp047466e, 2004.
Grieshop, A. P., Miracolo, M. A., Donahue, N. M., and Robinson, A. L.: Constraining the Volatility Distribution and Gas-Particle Partitioning of Combustion Aerosols Using Isothermal Dilution and Thermodenuder Measurements, Environ. Sci. Technol., 43, 4750–4756, https://doi.org/10.1021/es8032378, 2009.
Griffin, R. J., Nguyen, K., Dabdub, D., and Seinfeld, J. H.: A coupled hydrophobic-hydrophilic model for predicting secondary organic aerosol formation, J. Atmos. Chem., 44, 171–190, https://doi.org/10.1023/A:1022436813699, 2003.
Hall, W. A. and Johnston, M. V.: Oligomer Content of alpha-Pinene Secondary Organic Aerosol, Aerosol Sci. Tech., 45, 37–45, https://doi.org/10.1080/02786826.2010.517580, 2011.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, T. F., Monod, A., Prevot, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
Hamilton, J. F., Webb, P. J., Lewis, A. C., Hopkins, J. R., Smith, S., and Davy, P.: Partially oxidised organic components in urban aerosol using GCXGC-TOF/MS, Atmos. Chem. Phys., 4, 1279–1290, https://doi.org/10.5194/acp-4-1279-2004, 2004.
Hayman, G. D.: Effects of Pollution Control on UV Exposure, AEA Technology Final Report (Reference AEA/RCEC/22522001/R/002 ISSUE1) prepared for the Department of Health on Contract 121/6377, Tech. rep., AEA Technology, Oxfordshire, UK, 1997.
Hemming, B. L. and Seinfeld, J. H.: On the Hygroscopic Behavior of Atmospheric Organic Aerosols, Indust. Eng. Chem. Res., 40, 4162–4171, https://doi.org/10.1021/ie000790l, 2001.
Henderson, B. H.: Python-based Environment for Reaction Mechanisms/Mathematics (PERMM), https://doi.org/10.5281/zenodo.44396, 2015.
Henderson, B. H.: Kinetic Pre-Processor with updates to allow working with MCM, https://doi.org/10.5281/zenodo.44682, 2016.
Henderson, B. H., Pinder, R. W., Crooks, J., Cohen, R. C., Hutzell, W. T., Sarwar, G., Goliff, W. S., Stockwell, W. R., Fahr, A., Mathur, R., Carlton, A. G., and Vizuete, W.: Evaluation of simulated photochemical partitioning of oxidized nitrogen in the upper troposphere, Atmos. Chem. Phys., 11, 275–291, https://doi.org/10.5194/acp-11-275-2011, 2011.
Holes, A., Eusebi, A., Grosjean, D., and Allen, D. T.: FTIR analysis of aerosol formed in the photooxidation of 1,3,5-trimethylbenzene, Aerosol Sci. Tech., 26, 516–526, https://doi.org/10.1080/02786829708965450, 1997.
Im, Y., Jang, M., and Beardsley, R. L.: Simulation of aromatic SOA formation using the lumping model integrated with explicit gas-phase kinetic mechanisms and aerosol-phase reactions, Atmos. Chem. Phys., 14, 4013–4027, https://doi.org/10.5194/acp-14-4013-2014, 2014.
Jang, M. S. and Kamens, R. M.: Characterization of secondary aerosol from the photooxidation of toluene in the presence of NOx and 1-propene, Environ. Sci. Technol., 35, 3626–3639, https://doi.org/10.1021/es010676+, 2001.
Jathar, S. H., Cappa, C. D., Wexler, A. S., Seinfeld, J. H., and Kleeman, M. J.: Multi-generational oxidation model to simulate secondary organic aerosol in a 3-D air quality model, Geosci. Model Dev., 8, 2553–2567, https://doi.org/10.5194/gmd-8-2553-2015, 2015.
Jayne, J. T., Leard, D. C., Zhang, X. F., Davidovits, P., Smith, K. A., Kolb, C. E., and Worsnop, D. R.: Development of an aerosol mass spectrometer for size and composition analysis of submicron particles, Aerosol Sci. Tech., 33, 49–70, https://doi.org/10.1080/027868200410840, 2000.
Jeffries, H. E. and Tonnesen, S.: A comparison of two photochemical reaction mechanisms using mass balance and process analysis, Atmos. Environ., 28, 2991–3003, https://doi.org/10.1016/1352-2310(94)90345-X, 1994.
Jenkin, M. E.: Modelling the formation and composition of secondary organic aerosol from alpha- and beta-pinene ozonolysis using MCM v3, Atmos. Chem. Phys., 4, 1741–1757, https://doi.org/10.5194/acp-4-1741-2004, 2004.
Jenkin, M. E., Saunders, S. M., and Pilling, M. J.: The tropospheric degradation of volatile organic compounds: a protocol for mechanism development, Atmos. Environ., 31, 81–104, https://doi.org/10.1016/S1352-2310(96)00105-7, 1997.
Jenkin, M. E., Saunders, S. M., Wagner, V., and Pilling, M. J.: Protocol for the development of the Master Chemical Mechanism, MCM v3 (Part B): tropospheric degradation of aromatic volatile organic compounds, Atmos. Chem. Phys., 3, 181–193, https://doi.org/10.5194/acp-3-181-2003, 2003.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang, Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken, A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L., Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y. L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara, P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J., Dunlea, E. J., Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P. I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of Organic Aerosols in the Atmosphere, Science, 326, 1525–1529, https://doi.org/10.1126/science.1180353, 2009.
Kalberer, M., Paulsen, D., Sax, M., Steinbacher, M., Dommen, J., Prevot, A. S. H., Fisseha, R., Weingartner, E., Frankevich, V., Zenobi, R., and Baltensperger, U.: Identification of polymers as major components of atmospheric organic aerosols, Science, 303, 1659–1662, https://doi.org/10.1126/science.1092185, 2004.
Kalberer, M., Sax, M., and Samburova, V.: Molecular size evolution of oligomers in organic aerosols collected in urban atmospheres and generated in a smog chamber, Environ. Sci. Technol., 40, 5917–5922, https://doi.org/10.1021/es0525760, 2006.
Kroll, J. H. and Seinfeld, J. H.: Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere, Atmos. Environ., 42, 3593–3624, https://doi.org/10.1016/j.atmosenv.2008.01.003, 2008.
Kroll, J. H., Donahue, N. M., Jimenez, J. L., Kessler, S. H., Canagaratna, M. R., Wilson, K. R., Altieri, K. E., Mazzoleni, L. R., Wozniak, A. S., Bluhm, H., Mysak, E. R., Smith, J. D., Kolb, C. E., and Worsnop, D. R.: Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol, Nat. Chem., 3, 133–139, https://doi.org/10.1038/nchem.948, 2011.
La, Y. S., Camredon, M., Ziemann, P. J., Valorso, R., Matsunaga, A., Lannuque, V., Lee-Taylor, J., Hodzic, A., Madronich, S., and Aumont, B.: Impact of chamber wall loss of gaseous organic compounds on secondary organic aerosol formation: explicit modeling of SOA formation from alkane and alkene oxidation, Atmos. Chem. Phys., 16, 1417–1431, https://doi.org/10.5194/acp-16-1417-2016, 2016.
Lamb, B., Gay, D., Westberg, H., and Pierce, T.: A biogenic hydrocarbon emission inventory for the U.S.A. using a simple forest canopy model, Atmos. Environ. A, 27, 1673–1690, https://doi.org/10.1016/0960-1686(93)90230-V, 1993.
Lee, A. K. and Chan, C. K.: Single particle Raman spectroscopy for investigating atmospheric heterogeneous reactions of organic aerosols, Atmos. Environ., 41, 4611–4621, https://doi.org/10.1016/j.atmosenv.2007.03.040, 2007.
Liu, S., Shilling, J. E., Song, C., Hiranuma, N., Zaveri, R. A., and Russell, L. M.: Hydrolysis of Organonitrate Functional Groups in Aerosol Particles, Aerosol Sci. Tech., 46, 1359–1369, https://doi.org/10.1080/02786826.2012.716175, 2012.
Loza, C. L., Chan, A. W. H., Galloway, M. M., Keutsch, F. N., Flagan, R. C., and Seinfeld, J. H.: Characterization of Vapor Wall Loss in Laboratory Chambers, Environ. Sci. Technol., 44, 5074–5078, https://doi.org/10.1021/es100727v, 2010.
Matsunaga, A. and Ziemann, P. J.: Gas-Wall Partitioning of Organic Compounds in a Teflon Film Chamber and Potential Effects on Reaction Product and Aerosol Yield Measurements, Aerosol Sci. Tech., 44, 881–892, https://doi.org/10.1080/02786826.2010.501044, 2010.
McFiggans, G., Topping, D. O., and Barley, M. H.: The sensitivity of secondary organic aerosol component partitioning to the predictions of component properties – Part 1: A systematic evaluation of some available estimation techniques, Atmos. Chem. Phys., 10, 10255–10272, https://doi.org/10.5194/acp-10-10255-2010, 2010.
McVay, R. C., Zhang, X., Aumont, B., Valorso, R., Camredon, M., La, Y. S., Wennberg, P. O., and Seinfeld, J. H.: SOA formation from the photooxidation of α-pinene: systematic exploration of the simulation of chamber data, Atmos. Chem. Phys., 16, 2785–2802, https://doi.org/10.5194/acp-16-2785-2016, 2016.
Mertes, P., Pfaffenberger, L., Dommen, J., Kalberer, M., and Baltensperger, U.: Development of a sensitive long path absorption photometer to quantify peroxides in aerosol particles (Peroxide-LOPAP), Atmos. Meas. Tech., 5, 2339–2348, https://doi.org/10.5194/amt-5-2339-2012, 2012.
Metzger, A., Dommen, J., Gaeggeler, K., Duplissy, J., Prevot, A. S. H., Kleffmann, J., Elshorbany, Y., Wisthaler, A., and Baltensperger, U.: Evaluation of 1,3,5 trimethylbenzene degradation in the detailed tropospheric chemistry mechanism, MCMv3.1, using environmental chamber data, Atmos. Chem. Phys., 8, 6453–6468, https://doi.org/10.5194/acp-8-6453-2008, 2008.
Ming, Y. and Russell, L. M.: Thermodynamic equilibrium of organic-electrolyte mixtures in aerosol particles, Aiche J., 48, 1331–1348, 2002.
Mozurkewich, M. and Benson, S. W.: Self-Reaction of HO2 and DO2: Negative temperature dependence and pressure effects, Int. J. Chem. Kinet., 17, 787–807, https://doi.org/10.1002/kin.550170802, 1985.
Murphy, B. N., Donahue, N. M., Fountoukis, C., and Pandis, S. N.: Simulating the oxygen content of ambient organic aerosol with the 2D volatility basis set, Atmos. Chem. Phys., 11, 7859–7873, https://doi.org/10.5194/acp-11-7859-2011, 2011.
Myrdal, P. B. and Yalkowsky, S. H.: Estimating pure component vapor pressures of complex organic molecules, Indust. Eng. Chem. Res., 36, 2494–2499, https://doi.org/10.1021/ie950242l, 1997.
Nannoolal, Y., Rarey, J., and Ramjugernath, D.: Estimation of pure component properties – Part 3. Estimation of the vapor pressure of non-electrolyte organic compounds via group contributions and group interactions, Fluid Phase Equil., 269, 117–133, https://doi.org/10.1016/j.fluid.2008.04.020, 2008.
Ng, N. L., Chhabra, P. S., Chan, A. W. H., Surratt, J. D., Kroll, J. H., Kwan, A. J., McCabe, D. C., Wennberg, P. O., Sorooshian, A., Murphy, S. M., Dalleska, N. F., Flagan, R. C., and Seinfeld, J. H.: Effect of NOx level on secondary organic aerosol (SOA) formation from the photooxidation of terpenes, Atmos. Chem. Phys., 7, 5159–5174, https://doi.org/10.5194/acp-7-5159-2007, 2007.
Nizkorodov, S. A., Laskin, J., and Laskin, A.: Molecular chemistry of organic aerosols through the application of high resolution mass spectrometry, Phys. Chem. Chem. Phys., 13, 3612–3629, https://doi.org/10.1039/c0cp02032j, 2011.
Noziere, B., Barnes, I., and Becker, K. H.: Product study and mechanisms of the reactions of alpha-pinene and of pinonaldehyde with OH radicals, J. Geophys. Res.-Atmos., 104, 23645–23656, https://doi.org/10.1029/1999JD900778, 1999.
Nozière, B., Kalberer, M., Claeys, M., Allan, J., D'Anna, B., Decesari, S., Finessi, E., Glasius, M., Grgić, I., Hamilton, J. F., Hoffmann, T., Iinuma, Y., Jaoui, M., Kahnt, A., Kampf, C. J., Kourtchev, I., Maenhaut, W., Marsden, N., Saarikoski, S., Schnelle-Kreis, J., Surratt, J. D., Szidat, S., Szmigielski, R., and Wisthaler, A.: The Molecular Identification of Organic Compounds in the Atmosphere: State of the Art and Challenges, Chem. Rev., 115, 3919–3983, https://doi.org/10.1021/cr5003485, 2015.
O'Boyle, N. M., Morley, C., and Hutchison, G. R.: Pybel: a Python wrapper for the OpenBabel cheminformatics toolkit, Chem. Cent. J., 2, 1–7, https://doi.org/10.1186/1752-153X-2-5, 2008.
O'Boyle, N. M., Banck, M., James, C. A., Morley, C., Vandermeersch, T., and Hutchison, G. R.: Open Babel: An open chemical toolbox, J. Cheminf., 3, 1–14, https://doi.org/10.1186/1758-2946-3-33, 2011.
Orlan, E. S. and Boris, J. P.: Numerical Simulation of Reactive Flow, 2nd Edn., Cambridge University Press, Cambridge, UK, New York, NY, 2000.
Pankow, J. F.: An absorption model of gas/particle partitioning of organic compounds in the atmosphere, Atmos. Environ., 28, 185–188, https://doi.org/10.1016/1352-2310(94)90093-0, 1994.
Pankow, J. F.: A consideration of the role of gas/particle partitioning in the deposition of nicotine and other tobacco smoke compounds in the respiratory tract, Chem. Res. Toxicol., 14, 1465–1481, https://doi.org/10.1021/tx0100901, 2001.
Pankow, J. F. and Asher, W. E.: SIMPOL.1: a simple group contribution method for predicting vapor pressures and enthalpies of vaporization of multifunctional organic compounds, Atmos. Chem. Phys., 8, 2773–2796, https://doi.org/10.5194/acp-8-2773-2008, 2008.
Pavia, D., Lampman, G., and Kriz, G.: Introduction to Spectroscopy, Brooks/Cole Pub Co., Belmont, CA, 2008.
Pinho, P. G., Pio, C. A., Carter, W. P. L., and Jenkin, M. E.: Evaluation of alpha- and beta-pinene degradation in the detailed tropospheric chemistry mechanism, MCM v3.1, using environmental chamber data, J. Atmos. Chem., 57, 171–202, https://doi.org/10.1007/s10874-007-9071-0, 2007.
Presto, A. A. and Donahue, N. M.: Investigation of alpha-pinene plus ozone secondary organic aerosol formation at low total aerosol mass, Environ. Sci. Technol., 40, 3536–3543, https://doi.org/10.1021/es052203z, 2006.
Presto, A. A., Hartz, K. E. H., and Donahue, N. M.: Secondary organic aerosol production from terpene ozonolysis. 2. Effect of NOx concentration, Environ. Sci. Technol., 39, 7046–7054, https://doi.org/10.1021/es050400s, 2005.
Pun, B. K., Griffin, R. J., Seigneur, C., and Seinfeld, J. H.: Secondary organic aerosol – 2. Thermodynamic model for gas/particle partitioning of molecular constituents, J. Geophys. Res.-Atmos., 107, 4333, https://doi.org/10.1029/2001JD000542, 2002.
Radhakrishnan, K. and Hindmarsh, A. C.: Description and use of LSODE, the Livermore solver for ordinary differential equations, Tech. Rep. UCRL-ID-113855, NASA Reference Publication 1327, Lawrence Livermore National Laboratory, Washington, D.C., USA, 1993.
Ranney, A. P. and Ziemann, P. J.: Microscale Spectrophotometric Methods for Quantification of Functional Groups in Oxidized Organic Aerosol, Aerosol Sci. Tech., 50, 881–892, https://doi.org/10.1080/02786826.2016.1201197, 2016.
Reff, A., Turpin, B. J., Offenberg, J. H., Weisel, C. P., Zhang, J., Morandi, M., Stock, T., Colome, S., and Winer, A.: A functional group characterization of organic PM2.5 exposure: Results from the RIOPA study RID C-3787-2009, Atmos. Environ., 41, 4585–4598, https://doi.org/10.1016/j.atmosenv.2007.03.054, 2007.
Rickard, A. R., Wyche, K. P., Metzger, A., Monks, P. S., Ellis, A. M., Dommen, J., Baltensperger, U., Jenkin, M. E., and Pilling, M. J.: Gas phase precursors to anthropogenic secondary organic aerosol Using the Master Chemical Mechanism to probe detailed observations of 1,3,5-trimethylbenzene photo-oxidation, Atmos. Environ., 44, 5423–5433, https://doi.org/10.1016/j.atmosenv.2009.09.043, 2010.
Robinson, A. L., Donahue, N. M., Shrivastava, M. K., Weitkamp, E. A., Sage, A. M., Grieshop, A. P., Lane, T. E., Pierce, J. R., and Pandis, S. N.: Rethinking organic aerosols: Semivolatile emissions and photochemical aging, Science, 315, 1259–1262, https://doi.org/10.1126/science.1133061, 2007.
Ruggeri, G. and Takahama, S.: Technical Note: Development of chemoinformatic tools to enumerate functional groups in molecules for organic aerosol characterization, Atmos. Chem. Phys., 16, 4401–4422, https://doi.org/10.5194/acp-16-4401-2016, 2016.
Ruppert, L., Becker, K. H., Noziere, B., and Spittler, M.: Development Of Monoterpene Oxidation Mechanisms: Results From Laboratory And Smog Chamber Studies, in: Proceedings of EUROTRAC Symposium '98, vol. 35 of WIT Transactions on Ecology and the Environment, p. 6, http://www.witpress.com/elibrary/wit-transactions-on-ecology-and-the-environment/35/5190 (last access: July 2016), 1999.
Russell, L. M.: Aerosol organic-mass-to-organic-carbon ratio measurements, Environ. Sci. Technol., 37, 2982–2987, https://doi.org/10.1021/es026123w, 2003.
Russell, L. M., Bahadur, R., Hawkins, L. N., Allan, J., Baumgardner, D., Quinn, P. K., and Bates, T. S.: Organic aerosol characterization by complementary measurements of chemical bonds and molecular fragments, Atmos. Environ., 43, 6100–6105, https://doi.org/10.1016/j.atmosenv.2009.09.036, 2009.
Ruthenburg, T. C., Perlin, P. C., Liu, V., McDade, C. E., and Dillner, A. M.: Determination of organic matter and organic matter to organic carbon ratios by infrared spectroscopy with application to selected sites in the IMPROVE network, Atmos. Environ., 86, 47–57, https://doi.org/10.1016/j.atmosenv.2013.12.034, 2014.
Sandu, A. and Sander, R.: Technical note: Simulating chemical systems in Fortran90 and Matlab with the Kinetic PreProcessor KPP-2.1, Atmos. Chem. Phys., 6, 187–195, https://doi.org/10.5194/acp-6-187-2006, 2006.
Sato, K., Takami, A., Kato, Y., Seta, T., Fujitani, Y., Hikida, T., Shimono, A., and Imamura, T.: AMS and LC/MS analyses of SOA from the photooxidation of benzene and 1,3,5-trimethylbenzene in the presence of NOx: effects of chemical structure on SOA aging, Atmos. Chem. Phys., 12, 4667–4682, https://doi.org/10.5194/acp-12-4667-2012, 2012.
Saunders, S. M., Jenkin, M. E., Derwent, R. G., and Pilling, M. J.: Protocol for the development of the Master Chemical Mechanism, MCM v3 (Part A): tropospheric degradation of non-aromatic volatile organic compounds, Atmos. Chem. Phys., 3, 161–180, https://doi.org/10.5194/acp-3-161-2003, 2003.
Sax, M., Zenobi, R., Baltensperger, U., and Kalberer, M.: Time resolved infrared spectroscopic analysis of aerosol formed by photo-oxidation of 1,3,5-trimethylbenzene and alpha-pinene, Aerosol Sci. Tech., 39, 822–830, https://doi.org/10.1080/02786820500257859, 2005.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: From Air Pollution to Climate Change, 2nd Edn., John Wiley & Sons, New York, 2006.
Seinfeld, J. H., Erdakos, G. B., Asher, W. E., and Pankow, J. F.: Modeling the formation of secondary organic aerosol (SOA). 2. The predicted effects of relative humidity on aerosol formation in the alpha-pinene-, beta-pinene-, sabinene-, Delta(3)-Carene-, and cyclohexene-ozone systems, Environ. Sci. Technol., 35, 1806–1817, https://doi.org/10.1021/es001765+, 2001.
Shiraiwa, M., Berkemeier, T., Schilling-Fahnestock, K. A., Seinfeld, J. H., and Pöschl, U.: Molecular corridors and kinetic regimes in the multiphase chemical evolution of secondary organic aerosol, Atmos. Chem. Phys., 14, 8323–8341, https://doi.org/10.5194/acp-14-8323-2014, 2014.
Sindelarova, K., Granier, C., Bouarar, I., Guenther, A., Tilmes, S., Stavrakou, T., Müller, J.-F., Kuhn, U., Stefani, P., and Knorr, W.: Global data set of biogenic VOC emissions calculated by the MEGAN model over the last 30 years, Atmos. Chem. Phys., 14, 9317–9341, https://doi.org/10.5194/acp-14-9317-2014, 2014.
Subramanian, R., Khlystov, A. Y., Cabada, J. C., and Robinson, A. L.: Positive and negative artifacts in particulate organic carbon measurements with denuded and undenuded sampler configurations, Aerosol Sci. Tech., 38, 27–48, https://doi.org/10.1080/02786820390229354, 2004.
Suda, S. R., Petters, M. D., Yeh, G. K., Strollo, C., Matsunaga, A., Faulhaber, A., Ziemann, P. J., Prenni, A. J., Carrico, C. M., Sullivan, R. C., and Kreidenweis, S. M.: Influence of Functional Groups on Organic Aerosol Cloud Condensation Nucleus Activity, Environ. Sci. Technol., 48, 10182–10190, https://doi.org/10.1021/es502147y, 2014.
Takahama, S.: APRL Substructure Search Program, https://doi.org/10.5281/zenodo.34975, 2015.
Takahama, S. and Dillner, A. M.: Model selection for partial least squares calibration and implications for analysis of atmospheric organic aerosol samples with mid-infrared spectroscopy, J. Chemometr., 29, 659–668, https://doi.org/10.1002/cem.2761, 2015.
Takahama, S., Johnson, A., and Russell, L. M.: Quantification of Carboxylic and Carbonyl Functional Groups in Organic Aerosol Infrared Absorbance Spectra, Aerosol Sci. Tech., 47, 310–325, https://doi.org/10.1080/02786826.2012.752065, 2013.
Tanaka, K., Kim, H.-J., Saito, K., Takahashi, H. G., Watanabe, M., Yokohata, T., Kimoto, M., Takata, K., and Yasunari, T.: How have both cultivation and warming influenced annual global isoprene and monoterpene emissions since the preindustrial era?, Atmos. Chem. Phys., 12, 9703–9718, https://doi.org/10.5194/acp-12-9703-2012, 2012.
Tolocka, M. P., Jang, M., Ginter, J. M., Cox, F. J., Kamens, R. M., and Johnston, M. V.: Formation of oligomers in secondary organic aerosol, Environ. Sci. Technol., 38, 1428–1434, https://doi.org/10.1021/es035030r, 2004.
Topping, D., Barley, M., Bane, M. K., Higham, N., Aumont, B., Dingle, N., and McFiggans, G.: UManSysProp v1.0: an online and open-source facility for molecular property prediction and atmospheric aerosol calculations, Geosci. Model Dev., 9, 899–914, https://doi.org/10.5194/gmd-9-899-2016, 2016.
Vayenas, D. V., Takahama, S., Davidson, C. I., and Pandis, S. N.: Simulation of the thermodynamics and removal processes in the sulfate-ammonia-nitric acid system during winter: Implications for PM2.5 control strategies, J. Geophys. Res.-Atmos., 110, D07S14, https://doi.org/10.1029/2004JD005038, 2005.
Wang, Y., Kim, H., and Paulson, S. E.: Hydrogen peroxide generation from α- and β-pinene and toluene secondary organic aerosols, Atmos. Environ., 45, 3149–3156, https://doi.org/10.1016/j.atmosenv.2011.02.060, 2011.
Wyche, K. P., Monks, P. S., Ellis, A. M., Cordell, R. L., Parker, A. E., Whyte, C., Metzger, A., Dommen, J., Duplissy, J., Prevot, A. S. H., Baltensperger, U., Rickard, A. R., and Wulfert, F.: Gas phase precursors to anthropogenic secondary organic aerosol: detailed observations of 1,3,5-trimethylbenzene photooxidation, Atmos. Chem. Phys., 9, 635–665, https://doi.org/10.5194/acp-9-635-2009, 2009.
Yanenko, N. N.: The Method of Fractional Steps: The Solution of Problems of Mathematical Physics in Several Variables, 1st Edn., Springer, Berlin, Germany, 1971.
Yeh, G. K. and Ziemann, P. J.: Gas-Wall Partitioning of Oxygenated Organic Compounds: Measurements, Structure-Activity Relationships, and Correlation with Gas Chromatographic Retention Factor, Aerosol Sci. Tech., 49, 727–738, https://doi.org/10.1080/02786826.2015.1068427, 2015.
Yu, J. Z., Cocker, D. R., Griffin, R. J., Flagan, R. C., and Seinfeld, J. H.: Gas-phase ozone oxidation of monoterpenes: Gaseous and particulate products, J. Atmos. Chem., 34, 207–258, https://doi.org/10.1023/A:1006254930583, 1999.
Zeng, G., Holladay, S., Langlois, D., Zhang, Y., and Liu, Y.: Kinetics of Heterogeneous Reaction of Ozone with Linoleic Acid and its Dependence on Temperature, Physical State, RH, and Ozone Concentration, J. Phys. Chem. A, 117, 1963–1974, https://doi.org/10.1021/jp308304n, 2013.
Zhang, X. and McMurry, P.: Theoretical analysis of evaporative losses from impactor and filter deposits, Atmos. Environ., 21, 1779–1789, https://doi.org/10.1016/0004-6981(87)90118-1, 1987.
Zhang, X. and Seinfeld, J. H.: A functional group oxidation model (FGOM) for SOA formation and aging, Atmos. Chem. Phys., 13, 5907–5926, https://doi.org/10.5194/acp-13-5907-2013, 2013.
Zhang, X., Cappa, C. D., Jathar, S. H., McVay, R. C., Ensberg, J. J., Kleeman, M. J., and Seinfeld, J. H.: Influence of vapor wall loss in laboratory chambers on yields of secondary organic aerosol, P. Natl. Acad. Sci. USA, 111, 5802–5807, https://doi.org/10.1073/pnas.1404727111, 2014a.
Zhang, X., Schwantes, R. H., Coggon, M. M., Loza, C. L., Schilling, K. A., Flagan, R. C., and Seinfeld, J. H.: Role of ozone in SOA formation from alkane photooxidation, Atmos. Chem. Phys., 14, 1733–1753, https://doi.org/10.5194/acp-14-1733-2014, 2014b.
Zhang, X., McVay, R. C., Huang, D. D., Dalleska, N. F., Aumont, B., Flagan, R. C., and Seinfeld, J. H.: Formation and evolution of molecular products in α-pinene secondary organic aerosol, P. Natl. Acad. Sci. USA, 112, 14168–14173, https://doi.org/10.1073/pnas.1517742112, 2015.
Ziemann, P. J. and Atkinson, R.: Kinetics, products, and mechanisms of secondary organic aerosol formation, Chem. Soc. Rev., 41, 6582–6605, https://doi.org/10.1039/c2cs35122f, 2012.
Zuend, A., Marcolli, C., Booth, A. M., Lienhard, D. M., Soonsin, V., Krieger, U. K., Topping, D. O., McFiggans, G., Peter, T., and Seinfeld, J. H.: New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups, Atmos. Chem. Phys., 11, 9155–9206, https://doi.org/10.5194/acp-11-9155-2011, 2011.
Download
- Article
(4717 KB) - Full-text XML
Short summary
Functional groups provide an intermediate level of chemical resolution between full molecular speciation and elemental composition for describing complex mixtures and can be a useful metric in model–measurement comparison of reaction kinetics and secondary organic aerosol formation. We introduce tools to facilitate such comparisons and demonstrate its application in study of the photooxidation of two precursor volatile organic compounds and the gas–particle partitioning of their products.
Functional groups provide an intermediate level of chemical resolution between full molecular...
Altmetrics
Final-revised paper
Preprint