Articles | Volume 21, issue 15
https://doi.org/10.5194/acp-21-11637-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-11637-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
05 Aug 2021
Research article |
| 05 Aug 2021
| 05 Aug 2021
A predictive model for salt nanoparticle formation using heterodimer stability calculations
Sabrina Chee
Department of Chemistry, University of California, Irvine, CA, USA
Kelley Barsanti
Department of Chemical & Environmental Engineering, University of California, Riverside, CA, USA
Department of Chemistry, University of California, Irvine, CA, USA
Department of Chemistry, University of California, Irvine, CA, USA
Department of Chemistry, University of Jyväskylä, Jyväskylä, Finland
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James D. A. Butler, Afsara Tasnia, Deep Sengupta, Nathan Kreisberg, Kelley C. Barsanti, Allen H. Goldstein, Chelsea V. Preble, Rebecca A. Sugrue, and Thomas W. Kirchstetter
EGUsphere, https://doi.org/10.5194/egusphere-2025-2295, https://doi.org/10.5194/egusphere-2025-2295, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Prescribed burns are controlled fires used to prevent wildfires. Smoke emissions were measured to characterize emission factors and optical properties of black and brown soot particles. Brown particles were emitted at 7–14 times that of black particles and contributed 82 % of atmospheric absorption by particles for ultraviolet light and 23 % for total solar radiation. These findings will improve inventories and climate models for prescribed burns.
William P. L. Carter, Jia Jiang, Zhizhao Wang, and Kelley C. Barsanti
EGUsphere, https://doi.org/10.5194/egusphere-2025-1183, https://doi.org/10.5194/egusphere-2025-1183, 2025
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The SAPRC Atmospheric Chemical Mechanism Generation System (MechGen) generates explicit chemical reaction mechanisms for organic compounds. MechGen has been used for decades in the development of the widely-used SAPRC mechanisms. This manuscript, detailing the software system, and a companion manuscript, detailing the chemical basis, represent the first complete documentation of MechGen. This manuscript includes examples and instructions for generating explicit and reduced mechanisms.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
Atmos. Chem. Phys., 25, 4313–4331, https://doi.org/10.5194/acp-25-4313-2025, https://doi.org/10.5194/acp-25-4313-2025, 2025
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We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants that may influence future approaches to modelling climate.
Ida Karppinen, Dominika Pasik, Emelda Ahongshangbam, and Nanna Myllys
Aerosol Research, 3, 175–183, https://doi.org/10.5194/ar-3-175-2025, https://doi.org/10.5194/ar-3-175-2025, 2025
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Acyl peroxy radicals can act as atmospheric oxidants of unsaturated hydrocarbons if their 1) unimolecular reactions are slow and 2) bimolecular accretion reactions are fast. Using theoretical tools, we show which acyl peroxy radicals should be considered oxidants in the atmosphere.
Adam E. Thomas, Hayley S. Glicker, Alex B. Guenther, Roger Seco, Oscar Vega Bustillos, Julio Tota, Rodrigo A. F. Souza, and James N. Smith
Atmos. Chem. Phys., 25, 959–977, https://doi.org/10.5194/acp-25-959-2025, https://doi.org/10.5194/acp-25-959-2025, 2025
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We present measurements of the organic composition of ultrafine particles collected from the eastern Amazon, an understudied region that is subjected to increasing human influence. We find that while isoprene chemistry is likely significant for ultrafine-particle growth throughout the year, compounds related to other sources, such as biological-spore emissions and biomass burning, exhibit striking seasonal differences, implying extensive variation in regional ultrafine-particle sources.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
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This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
Samiha Binte Shahid, Forrest G. Lacey, Christine Wiedinmyer, Robert J. Yokelson, and Kelley C. Barsanti
Geosci. Model Dev., 17, 7679–7711, https://doi.org/10.5194/gmd-17-7679-2024, https://doi.org/10.5194/gmd-17-7679-2024, 2024
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The Next-generation Emissions InVentory expansion of Akagi (NEIVA) v.1.0 is a comprehensive biomass burning emissions database that allows integration of new data and flexible querying. Data are stored in connected datasets, including recommended averages of ~1500 constituents for 14 globally relevant fire types. Individual compounds were mapped to common model species to allow better attribution of emissions in modeling studies that predict the effects of fires on air quality and climate.
Vignesh Vasudevan-Geetha, Lee Tiszenkel, Zhizhao Wang, Robin Russo, Daniel Bryant, Julia Lee-Taylor, Kelley Barsanti, and Shan-Hu Lee
EGUsphere, https://doi.org/10.5194/egusphere-2024-2454, https://doi.org/10.5194/egusphere-2024-2454, 2024
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Our laboratory experiments using two high-resolution mass spectrometers show that these OOMs can also form within the particle phase, in addition to gas-to-particle conversion processes. Our results demonstrate that particle-phase formation processes can contribute to the formation and growth of new particles in biogenic environments.
Xiaoxiao Li, Yijing Chen, Yuyang Li, Runlong Cai, Yiran Li, Chenjuan Deng, Jin Wu, Chao Yan, Hairong Cheng, Yongchun Liu, Markku Kulmala, Jiming Hao, James N. Smith, and Jingkun Jiang
Atmos. Chem. Phys., 23, 14801–14812, https://doi.org/10.5194/acp-23-14801-2023, https://doi.org/10.5194/acp-23-14801-2023, 2023
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Near-continuous measurements show the composition, sources, and seasonal variations of ultrafine particles (UFPs) in urban Beijing. Vehicle and cooking emissions and new particle formation are the main sources of UFPs, and aqueous/heterogeneous processes increase UFP mode diameters. UFPs are the highest in winter due to the highest primary particle emission rates and new particle formation rates, and CHO fractions are the highest in summer due to the strongest photooxidation.
Christine Wiedinmyer, Yosuke Kimura, Elena C. McDonald-Buller, Louisa K. Emmons, Rebecca R. Buchholz, Wenfu Tang, Keenan Seto, Maxwell B. Joseph, Kelley C. Barsanti, Annmarie G. Carlton, and Robert Yokelson
Geosci. Model Dev., 16, 3873–3891, https://doi.org/10.5194/gmd-16-3873-2023, https://doi.org/10.5194/gmd-16-3873-2023, 2023
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The Fire INventory from NCAR (FINN) provides daily global estimates of emissions from open fires based on satellite detections of hot spots. This version has been updated to apply MODIS and VIIRS satellite fire detection and better represents both large and small fires. FINNv2.5 generates more emissions than FINNv1 and is in general agreement with other fire emissions inventories. The new estimates are consistent with satellite observations, but uncertainties remain regionally and by pollutant.
Deanna C. Myers, Saewung Kim, Steven Sjostedt, Alex B. Guenther, Roger Seco, Oscar Vega Bustillos, Julio Tota, Rodrigo A. F. Souza, and James N. Smith
Atmos. Chem. Phys., 22, 10061–10076, https://doi.org/10.5194/acp-22-10061-2022, https://doi.org/10.5194/acp-22-10061-2022, 2022
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We present the first measurements of gas-phase sulfuric acid from the Amazon basin and evaluate the efficacy of existing sulfuric acid parameterizations in this understudied region. Sulfuric acid is produced during the daytime and nighttime, though current proxies underestimate nighttime production. These results illustrate the need for better parameterizations of sulfuric acid and its precursors that are informed by measurements across a broad range of locations.
Yutong Liang, Christos Stamatis, Edward C. Fortner, Rebecca A. Wernis, Paul Van Rooy, Francesca Majluf, Tara I. Yacovitch, Conner Daube, Scott C. Herndon, Nathan M. Kreisberg, Kelley C. Barsanti, and Allen H. Goldstein
Atmos. Chem. Phys., 22, 9877–9893, https://doi.org/10.5194/acp-22-9877-2022, https://doi.org/10.5194/acp-22-9877-2022, 2022
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This article reports the measurements of organic compounds emitted from western US wildfires. We identified and quantified 240 particle-phase compounds and 72 gas-phase compounds emitted in wildfire and related the emissions to the modified combustion efficiency. Higher emissions of diterpenoids and monoterpenes were observed, likely due to distillation from unburned heated vegetation. Our results can benefit future source apportionment and modeling studies as well as exposure assessments.
Michelia Dam, Danielle C. Draper, Andrey Marsavin, Juliane L. Fry, and James N. Smith
Atmos. Chem. Phys., 22, 9017–9031, https://doi.org/10.5194/acp-22-9017-2022, https://doi.org/10.5194/acp-22-9017-2022, 2022
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We performed chamber experiments to measure the composition of the gas-phase reaction products of nitrate-radical-initiated oxidation of four monoterpenes. The total organic yield, effective oxygen-to-carbon ratio, and dimer-to-monomer ratio were correlated with the observed particle formation for the monoterpene systems with some exceptions. The Δ-carene system produced the most particles, followed by β-pinene, with the α-pinene and α-thujene systems producing no particles.
Christos Stamatis and Kelley Claire Barsanti
Atmos. Meas. Tech., 15, 2591–2606, https://doi.org/10.5194/amt-15-2591-2022, https://doi.org/10.5194/amt-15-2591-2022, 2022
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Building on the identification of hundreds of gas-phase chemicals in smoke samples from laboratory and field studies, an algorithm was developed that successfully identified chemical patterns that were consistent among types of trees and unique between types of trees that are common fuels in western coniferous forests. The algorithm is a promising approach for selecting chemical speciation profiles for air quality modeling using a highly reduced suite of measured compounds.
Qi Li, Jia Jiang, Isaac K. Afreh, Kelley C. Barsanti, and David R. Cocker III
Atmos. Chem. Phys., 22, 3131–3147, https://doi.org/10.5194/acp-22-3131-2022, https://doi.org/10.5194/acp-22-3131-2022, 2022
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Chamber-derived secondary organic aerosol (SOA) yields from camphene are reported for the first time. The role of peroxy radicals (RO2) was investigated using chemically detailed box models. We observed higher SOA yields (up to 64 %) in the experiments with added NOx than without due to the formation of highly oxygenated organic molecules (HOMs) when
NOx is present. This work can improve the representation of camphene in air quality models and provide insights into other monoterpene studies.
Dina Alfaouri, Monica Passananti, Tommaso Zanca, Lauri Ahonen, Juha Kangasluoma, Jakub Kubečka, Nanna Myllys, and Hanna Vehkamäki
Atmos. Meas. Tech., 15, 11–19, https://doi.org/10.5194/amt-15-11-2022, https://doi.org/10.5194/amt-15-11-2022, 2022
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To study what is happening in the atmosphere, it is important to be able to measure the molecules and clusters present in it. In our work, we studied an artifact that happens inside a mass spectrometer, in particular the fragmentation of clusters. We were able to quantify the fragmentation and retrieve the correct concentration and composition of the clusters using our dual (experimental and theoretical) approach.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Isaac Kwadjo Afreh, Bernard Aumont, Marie Camredon, and Kelley Claire Barsanti
Atmos. Chem. Phys., 21, 11467–11487, https://doi.org/10.5194/acp-21-11467-2021, https://doi.org/10.5194/acp-21-11467-2021, 2021
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This is the first mechanistic modeling study of secondary organic aerosol (SOA) from the understudied monoterpene, camphene. The semi-explicit chemical model GECKO-A predicted camphene SOA yields that were ~2 times α-pinene. Using 50/50 α-pinene + limonene as a surrogate for camphene increased predicted SOA mass from biomass burning fuels by up to ~100 %. The accurate representation of camphene in air quality models can improve predictions of SOA when camphene is a dominant monoterpene.
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Short summary
We explored molecular properties affecting atmospheric particle formation efficiency and derived a parameterization between particle formation rate and heterodimer concentration, which showed good agreement to previously reported experimental data. Considering the simplicity of calculating heterodimer concentration, this approach has potential to improve estimates of global cloud condensation nuclei in models that are limited by the computational expense of calculating particle formation rate.
We explored molecular properties affecting atmospheric particle formation efficiency and derived...
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