Articles | Volume 24, issue 9
https://doi.org/10.5194/acp-24-5235-2024
© Author(s) 2024. 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-24-5235-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Technical note: Characterization of a single-beam gradient force aerosol optical tweezer for droplet trapping, phase transition monitoring, and morphology studies
Xiangyu Pei
Zhejiang Provincial Key Laboratory of Organic Pollution Process and Control, MOE Key Laboratory of Environment Remediation and Ecological Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China
Yikan Meng
Zhejiang Provincial Key Laboratory of Organic Pollution Process and Control, MOE Key Laboratory of Environment Remediation and Ecological Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China
Yueling Chen
Zhejiang Provincial Key Laboratory of Organic Pollution Process and Control, MOE Key Laboratory of Environment Remediation and Ecological Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China
Huichao Liu
Zhejiang Provincial Key Laboratory of Organic Pollution Process and Control, MOE Key Laboratory of Environment Remediation and Ecological Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China
Yao Song
Zhejiang Provincial Key Laboratory of Organic Pollution Process and Control, MOE Key Laboratory of Environment Remediation and Ecological Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China
Zhengning Xu
Zhejiang Provincial Key Laboratory of Organic Pollution Process and Control, MOE Key Laboratory of Environment Remediation and Ecological Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China
Fei Zhang
Zhejiang Provincial Key Laboratory of Organic Pollution Process and Control, MOE Key Laboratory of Environment Remediation and Ecological Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China
Thomas C. Preston
Department of Atmospheric and Oceanic Sciences and Department of Chemistry, McGill University, 805 Sherbrooke Street West, Montréal, Quebec H3A 0B9, Canada
Zhibin Wang
CORRESPONDING AUTHOR
Zhejiang Provincial Key Laboratory of Organic Pollution Process and Control, MOE Key Laboratory of Environment Remediation and Ecological Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China
ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou 311215, China
Related authors
Jing Wei, Jin-Mei Ding, Yao Song, Xiao-Yuan Wang, Xiang-Yu Pei, Sheng-Chen Xu, Fei Zhang, Zheng-Ning Xu, Xu-Dong Tian, Bing-Ye Xu, and Zhi-Bin Wang
EGUsphere, https://doi.org/10.5194/egusphere-2025-2844, https://doi.org/10.5194/egusphere-2025-2844, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Black carbon (BC) is a light-absorbing particle that contributes to atmospheric warming, but its radiative impact remains highly uncertain. We conducted field measurements in Hangzhou, China, to examine how mass ratio (coating-to-BC) and morphology influence light absorption. Our results show that widely used optical models overestimate absorption especially under clean conditions. A new morphology-based method improves model accuracy and reduces this uncertainty.
Yao Song, Jing Wei, Wenlong Zhao, Jinmei Ding, Xiangyu Pei, Fei Zhang, Zhengning Xu, Ruifang Shi, Ya Wei, Lu Zhang, Lingling Jin, and Zhibin Wang
Atmos. Chem. Phys., 25, 4755–4766, https://doi.org/10.5194/acp-25-4755-2025, https://doi.org/10.5194/acp-25-4755-2025, 2025
Short summary
Short summary
This study investigates the size-resolved effective density (ρeff) of aerosol particles in Hangzhou using a tandem aerodynamic aerosol classifier and scanning mobility particle sizer system. The ρeff values ranged from 1.47 to 1.63 g cm-3, increasing with particle diameter. The relationship between ρeff and the particle diameter varies due to differences in the chemical composition of the particles. A new method to derive the size-resolved chemical composition of particles from ρeff is proposed.
Junyue Yang, Zhengning Xu, Zheng Xia, Xiangyu Pei, Yunye Yang, Botian Qiu, Shuang Zhao, Yuzhong Zhang, and Zhibin Wang
Atmos. Chem. Phys., 25, 4571–4585, https://doi.org/10.5194/acp-25-4571-2025, https://doi.org/10.5194/acp-25-4571-2025, 2025
Short summary
Short summary
Mobile CH4 measurements were conducted at a wastewater treatment plant in Hangzhou in the summer and winter of 2023. A multi-source Gaussian plume model, combined with a genetic algorithm inversion framework, was used to locate major CH4 sources at the plant and quantify emissions. Results indicate that the summer CH4 emissions (603.33 ± 152.66 t a-1) were 2.8 times as high as inventory values, and winter values (418.95 ± 187.59 t a-1) were twice as high. The main sources were the screen and primary clarifier.
Zhengning Xu, Jian Gao, Zhuanghao Xu, Michel Attoui, Xiangyu Pei, Mario Amo-González, Kewei Zhang, and Zhibin Wang
Atmos. Meas. Tech., 16, 5995–6006, https://doi.org/10.5194/amt-16-5995-2023, https://doi.org/10.5194/amt-16-5995-2023, 2023
Short summary
Short summary
Planar differential mobility analyzers (DMAs) have higher ion transmission efficiency and sizing resolution compared to cylindrical DMAs and are more suitable for use with mass spectrometers (MSs). Performance of the latest planar DMA (P5) was characterized. Sizing resolution and ion transmission efficiency were 5–16 times and ∼10 times higher than cylindrical DMAs. Sulfuric acid clusters were measured by DMA(P5)-MSs. This technique can be applied for natural products and biomolecule analysis.
Yueling Chen, Xiangyu Pei, Huichao Liu, Yikan Meng, Zhengning Xu, Fei Zhang, Chun Xiong, Thomas C. Preston, and Zhibin Wang
Atmos. Chem. Phys., 23, 10255–10265, https://doi.org/10.5194/acp-23-10255-2023, https://doi.org/10.5194/acp-23-10255-2023, 2023
Short summary
Short summary
The impact of acidity on the phase transition behavior of levitated aerosol particles was examined. Our results revealed that lower acidity decreases the separation relative humidity of aerosol droplets mixed with ammonium sulfate and secondary organic aerosol proxy. Our research suggests that in real atmospheric conditions, with the high acidity found in many ambient aerosol particles, droplets encounter heightened impediments to phase separation and tend to display a homogeneous structure.
Chun Xiong, Binyu Kuang, Fei Zhang, Xiangyu Pei, Zhengning Xu, and Zhibin Wang
Atmos. Chem. Phys., 23, 8979–8991, https://doi.org/10.5194/acp-23-8979-2023, https://doi.org/10.5194/acp-23-8979-2023, 2023
Short summary
Short summary
In hydration, an apparent water diffusion hindrance by an organic surfactant shell was confirmed, raising the inorganic deliquescence relative humidity (RH) to a nearly saturated condition. In dehydration, phase separations were observed for inorganic surfactant systems, showing a strong dependence on the organic molecular
oxygen-to-carbon ratio. Our results could improve fundamental knowledge about aerosol mixing states and decrease uncertainty in model estimations of global radiative effects.
Chun Xiong, Xueyan Chen, Xiaolei Ding, Binyu Kuang, Xiangyu Pei, Zhengning Xu, Shikuan Yang, Huan Hu, and Zhibin Wang
Atmos. Chem. Phys., 22, 16123–16135, https://doi.org/10.5194/acp-22-16123-2022, https://doi.org/10.5194/acp-22-16123-2022, 2022
Short summary
Short summary
Water surface tension is applied widely in current aerosol–cloud models but could be inappropriate in the presence of atmospheric surfactants. With cloud condensation nuclei (CCN) activity and atomic force microscopy (AFM) measurement results of mixed inorganic salt and dicarboxylic acid particles, we concluded that surface tension reduction and phase state should be carefully considered in aerosol–cloud interactions. Our results could help to decease uncertainties in climate models.
Yao Song, Xiangyu Pei, Huichao Liu, Jiajia Zhou, and Zhibin Wang
Atmos. Meas. Tech., 15, 3513–3526, https://doi.org/10.5194/amt-15-3513-2022, https://doi.org/10.5194/amt-15-3513-2022, 2022
Short summary
Short summary
Accurate particle classification is very important in aerosol studies. Differential mobility analyzers (DMAs), centrifugal particle mass analyzers (CPMAs), aerodynamic aerosol classifiers (AACs) and their tandem systems are commonly used. We demonstrated that DMA–CPMA is more susceptible to the multiple charging effect than DMA–AAC. It is not suggested to reduce the resolutions of the instruments, especially when selecting small-size soot particles.
Cuiqi Zhang, Zhijun Wu, Jingchuan Chen, Jie Chen, Lizi Tang, Wenfei Zhu, Xiangyu Pei, Shiyi Chen, Ping Tian, Song Guo, Limin Zeng, Min Hu, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 7539–7556, https://doi.org/10.5194/acp-22-7539-2022, https://doi.org/10.5194/acp-22-7539-2022, 2022
Short summary
Short summary
The immersion ice nucleation effectiveness of aerosols from multiple sources in the urban environment remains elusive. In this study, we demonstrate that the immersion ice-nucleating particle (INP) concentration increased dramatically during a dust event in an urban atmosphere. Pollutant aerosols, including inorganic salts formed through secondary transformation (SIA) and black carbon (BC), might not act as effective INPs under mixed-phase cloud conditions.
Jing Wei, Jin-Mei Ding, Yao Song, Xiao-Yuan Wang, Xiang-Yu Pei, Sheng-Chen Xu, Fei Zhang, Zheng-Ning Xu, Xu-Dong Tian, Bing-Ye Xu, and Zhi-Bin Wang
EGUsphere, https://doi.org/10.5194/egusphere-2025-2844, https://doi.org/10.5194/egusphere-2025-2844, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Black carbon (BC) is a light-absorbing particle that contributes to atmospheric warming, but its radiative impact remains highly uncertain. We conducted field measurements in Hangzhou, China, to examine how mass ratio (coating-to-BC) and morphology influence light absorption. Our results show that widely used optical models overestimate absorption especially under clean conditions. A new morphology-based method improves model accuracy and reduces this uncertainty.
Vahid Shahabadi, Cassandra Lefort, Hoi Tang Law, Man Nin Chan, and Thomas C. Preston
EGUsphere, https://doi.org/10.5194/egusphere-2025-2170, https://doi.org/10.5194/egusphere-2025-2170, 2025
Short summary
Short summary
This research explores how organosulfate surfactants affect aerosol particles and their response to changes in relative humidity in the atmosphere. Using optical trapping and strong electric fields to investigate single particles, it is found that these surfactants can significantly lower surface tension, even in very small amounts. These findings are important for understanding how such particles influence cloud formation and properties like brightness.
Yao Song, Jing Wei, Wenlong Zhao, Jinmei Ding, Xiangyu Pei, Fei Zhang, Zhengning Xu, Ruifang Shi, Ya Wei, Lu Zhang, Lingling Jin, and Zhibin Wang
Atmos. Chem. Phys., 25, 4755–4766, https://doi.org/10.5194/acp-25-4755-2025, https://doi.org/10.5194/acp-25-4755-2025, 2025
Short summary
Short summary
This study investigates the size-resolved effective density (ρeff) of aerosol particles in Hangzhou using a tandem aerodynamic aerosol classifier and scanning mobility particle sizer system. The ρeff values ranged from 1.47 to 1.63 g cm-3, increasing with particle diameter. The relationship between ρeff and the particle diameter varies due to differences in the chemical composition of the particles. A new method to derive the size-resolved chemical composition of particles from ρeff is proposed.
Junyue Yang, Zhengning Xu, Zheng Xia, Xiangyu Pei, Yunye Yang, Botian Qiu, Shuang Zhao, Yuzhong Zhang, and Zhibin Wang
Atmos. Chem. Phys., 25, 4571–4585, https://doi.org/10.5194/acp-25-4571-2025, https://doi.org/10.5194/acp-25-4571-2025, 2025
Short summary
Short summary
Mobile CH4 measurements were conducted at a wastewater treatment plant in Hangzhou in the summer and winter of 2023. A multi-source Gaussian plume model, combined with a genetic algorithm inversion framework, was used to locate major CH4 sources at the plant and quantify emissions. Results indicate that the summer CH4 emissions (603.33 ± 152.66 t a-1) were 2.8 times as high as inventory values, and winter values (418.95 ± 187.59 t a-1) were twice as high. The main sources were the screen and primary clarifier.
Zhengning Xu, Jian Gao, Zhuanghao Xu, Michel Attoui, Xiangyu Pei, Mario Amo-González, Kewei Zhang, and Zhibin Wang
Atmos. Meas. Tech., 16, 5995–6006, https://doi.org/10.5194/amt-16-5995-2023, https://doi.org/10.5194/amt-16-5995-2023, 2023
Short summary
Short summary
Planar differential mobility analyzers (DMAs) have higher ion transmission efficiency and sizing resolution compared to cylindrical DMAs and are more suitable for use with mass spectrometers (MSs). Performance of the latest planar DMA (P5) was characterized. Sizing resolution and ion transmission efficiency were 5–16 times and ∼10 times higher than cylindrical DMAs. Sulfuric acid clusters were measured by DMA(P5)-MSs. This technique can be applied for natural products and biomolecule analysis.
Yueling Chen, Xiangyu Pei, Huichao Liu, Yikan Meng, Zhengning Xu, Fei Zhang, Chun Xiong, Thomas C. Preston, and Zhibin Wang
Atmos. Chem. Phys., 23, 10255–10265, https://doi.org/10.5194/acp-23-10255-2023, https://doi.org/10.5194/acp-23-10255-2023, 2023
Short summary
Short summary
The impact of acidity on the phase transition behavior of levitated aerosol particles was examined. Our results revealed that lower acidity decreases the separation relative humidity of aerosol droplets mixed with ammonium sulfate and secondary organic aerosol proxy. Our research suggests that in real atmospheric conditions, with the high acidity found in many ambient aerosol particles, droplets encounter heightened impediments to phase separation and tend to display a homogeneous structure.
Chun Xiong, Binyu Kuang, Fei Zhang, Xiangyu Pei, Zhengning Xu, and Zhibin Wang
Atmos. Chem. Phys., 23, 8979–8991, https://doi.org/10.5194/acp-23-8979-2023, https://doi.org/10.5194/acp-23-8979-2023, 2023
Short summary
Short summary
In hydration, an apparent water diffusion hindrance by an organic surfactant shell was confirmed, raising the inorganic deliquescence relative humidity (RH) to a nearly saturated condition. In dehydration, phase separations were observed for inorganic surfactant systems, showing a strong dependence on the organic molecular
oxygen-to-carbon ratio. Our results could improve fundamental knowledge about aerosol mixing states and decrease uncertainty in model estimations of global radiative effects.
Juan Hong, Min Tang, Qiaoqiao Wang, Nan Ma, Shaowen Zhu, Shaobin Zhang, Xihao Pan, Linhong Xie, Guo Li, Uwe Kuhn, Chao Yan, Jiangchuan Tao, Ye Kuang, Yao He, Wanyun Xu, Runlong Cai, Yaqing Zhou, Zhibin Wang, Guangsheng Zhou, Bin Yuan, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 23, 5699–5713, https://doi.org/10.5194/acp-23-5699-2023, https://doi.org/10.5194/acp-23-5699-2023, 2023
Short summary
Short summary
A comprehensive investigation of the characteristics of new particle formation (NPF) events was conducted at a rural site on the North China Plain (NCP), China, during the wintertime of 2018 by covering the particle number size distribution down to sub–3 nm. Potential mechanisms for NPF under the current environment were explored, followed by a further discussion on the factors governing the occurrence of NPF at this rural site compared with other regions (e.g., urban areas) in the NCP region.
Chun Xiong, Xueyan Chen, Xiaolei Ding, Binyu Kuang, Xiangyu Pei, Zhengning Xu, Shikuan Yang, Huan Hu, and Zhibin Wang
Atmos. Chem. Phys., 22, 16123–16135, https://doi.org/10.5194/acp-22-16123-2022, https://doi.org/10.5194/acp-22-16123-2022, 2022
Short summary
Short summary
Water surface tension is applied widely in current aerosol–cloud models but could be inappropriate in the presence of atmospheric surfactants. With cloud condensation nuclei (CCN) activity and atomic force microscopy (AFM) measurement results of mixed inorganic salt and dicarboxylic acid particles, we concluded that surface tension reduction and phase state should be carefully considered in aerosol–cloud interactions. Our results could help to decease uncertainties in climate models.
Rui Zhang, Yuying Wang, Zhanqing Li, Zhibin Wang, Russell R. Dickerson, Xinrong Ren, Hao He, Fei Wang, Ying Gao, Xi Chen, Jialu Xu, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 14879–14891, https://doi.org/10.5194/acp-22-14879-2022, https://doi.org/10.5194/acp-22-14879-2022, 2022
Short summary
Short summary
Factors of cloud condensation nuclei number concentration (NCCN) profiles determined in the North China Plain include air mass sources, temperature structure, anthropogenic emissions, and terrain distribution. Cloud condensation nuclei (CCN) spectra suggest that the ability of aerosol activation into CCN is stronger in southeasterly than in northwesterly air masses and stronger in the free atmosphere than near the surface. A good method to parameterize NCCN from aerosol optical data is found.
Yao Song, Xiangyu Pei, Huichao Liu, Jiajia Zhou, and Zhibin Wang
Atmos. Meas. Tech., 15, 3513–3526, https://doi.org/10.5194/amt-15-3513-2022, https://doi.org/10.5194/amt-15-3513-2022, 2022
Short summary
Short summary
Accurate particle classification is very important in aerosol studies. Differential mobility analyzers (DMAs), centrifugal particle mass analyzers (CPMAs), aerodynamic aerosol classifiers (AACs) and their tandem systems are commonly used. We demonstrated that DMA–CPMA is more susceptible to the multiple charging effect than DMA–AAC. It is not suggested to reduce the resolutions of the instruments, especially when selecting small-size soot particles.
Cuiqi Zhang, Zhijun Wu, Jingchuan Chen, Jie Chen, Lizi Tang, Wenfei Zhu, Xiangyu Pei, Shiyi Chen, Ping Tian, Song Guo, Limin Zeng, Min Hu, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 7539–7556, https://doi.org/10.5194/acp-22-7539-2022, https://doi.org/10.5194/acp-22-7539-2022, 2022
Short summary
Short summary
The immersion ice nucleation effectiveness of aerosols from multiple sources in the urban environment remains elusive. In this study, we demonstrate that the immersion ice-nucleating particle (INP) concentration increased dramatically during a dust event in an urban atmosphere. Pollutant aerosols, including inorganic salts formed through secondary transformation (SIA) and black carbon (BC), might not act as effective INPs under mixed-phase cloud conditions.
Yaqing Zhou, Nan Ma, Qiaoqiao Wang, Zhibin Wang, Chunrong Chen, Jiangchuan Tao, Juan Hong, Long Peng, Yao He, Linhong Xie, Shaowen Zhu, Yuxuan Zhang, Guo Li, Wanyun Xu, Peng Cheng, Uwe Kuhn, Guangsheng Zhou, Pingqing Fu, Qiang Zhang, Hang Su, and Yafang Cheng
Atmos. Chem. Phys., 22, 2029–2047, https://doi.org/10.5194/acp-22-2029-2022, https://doi.org/10.5194/acp-22-2029-2022, 2022
Short summary
Short summary
This study characterizes size-resolved particle effective densities and their evolution associated with emissions and aging processes in a rural area of the North China Plain. Particle effective density exhibits a high-frequency bimodal distribution, and two density modes exhibit opposite trends with increasing particle size. SIA and BC mass fractions are key factors of particle effective density, and a value of 0.6 g cm−3 is appropriate to represent BC effective density in bulk particles.
Hang Yin, Jing Dou, Liviana Klein, Ulrich K. Krieger, Alison Bain, Brandon J. Wallace, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 22, 973–1013, https://doi.org/10.5194/acp-22-973-2022, https://doi.org/10.5194/acp-22-973-2022, 2022
Short summary
Short summary
Iodine and carbonate species are important components in marine and dust aerosols, respectively. We introduce an extended version of the AIOMFAC thermodynamic mixing model, which includes the ions I−, IO3−, HCO3−, CO32−, OH−, and CO2(aq) as new species, and we discuss two methods for solving the carbonate dissociation equilibria numerically. We also present new experimental water activity data for aqueous iodide and iodate systems.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys., 21, 14789–14814, https://doi.org/10.5194/acp-21-14789-2021, https://doi.org/10.5194/acp-21-14789-2021, 2021
Short summary
Short summary
Oxygenated organic molecules (OOMs) are crucial intermediates linking volatile organic compounds to secondary organic aerosols. Using nitrate time-of-flight chemical ionization mass spectrometry in eastern China, we performed positive matrix factorization (PMF) on binned OOM mass spectra. We reconstructed over 1000 molecules from 14 derived PMF factors and identified about 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of NOx in OOM formation in populated areas.
Ting Lei, Nan Ma, Juan Hong, Thomas Tuch, Xin Wang, Zhibin Wang, Mira Pöhlker, Maofa Ge, Weigang Wang, Eugene Mikhailov, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Alfred Wiedensohler, and Yafang Cheng
Atmos. Meas. Tech., 13, 5551–5567, https://doi.org/10.5194/amt-13-5551-2020, https://doi.org/10.5194/amt-13-5551-2020, 2020
Short summary
Short summary
We present the design of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. We further introduce comprehensive methods for system calibration and validation of the performance of the system. We then study the size dependence of the deliquescence and the efflorescence of aerosol nanoparticles for sizes down to 6 nm.
Cited articles
Ashkin, A. and Dziedzic, J. M.: Observation of optical resonances of dielectric spheres by light scattering, Appl. Optics, 20, 1803–1814, https://doi.org/10.1364/AO.20.001803, 1981.
Boyer, H. C., Gorkowski, K., and Sullivan, R. C.: In situ pH measurements of individual levitated microdroplets using aerosol optical tweezers, Anal. Chem., 92, 1089–1096, https://doi.org/10.1021/acs.analchem.9b04152, 2020.
Buajarern, J., Mitchem, L., and Reid, J. P.: Characterizing multiphase organic/inorganic/aqueous aerosol droplets, J. Phys. Chem. A, 111, 9054–9061, https://doi.org/10.1021/jp074366a, 2007.
Cai, C., Stewart, D. J., Reid, J. P., Zhang, Y.-H., Ohm, P., Dutcher, C. S., and Clegg, S. L.: Organic component vapor pressures and hygroscopicities of aqueous aerosol measured by optical tweezers, J. Phys. Chem. A., 119, 704–718, https://doi.org/10.1021/jp510525r, 2015.
Chan, M. N., Choi, M. Y., Ng, N. L., and Chan, C. K.: Hygroscopicity of water-soluble organic compounds in atmospheric aerosols: amino acids and biomass burning derived organic species, Environ. Sci. Technol., 39, 1555–1562, https://doi.org/10.1021/es049584l, 2005.
Chen, X. and Hopke, P. K.: A chamber study of secondary organic aerosol formation by limonene ozonolysis, Indoor Air, 20, 320–328, https://doi.org/10.1111/j.1600-0668.2010.00656.x, 2010.
Combe, N. A. and Donaldson, D. J.: Water evaporation from acoustically levitated aqueous solution droplets, J. Phys. Chem. A, 121, 7197–7204, https://doi.org/10.1021/acs.jpca.7b08050, 2017.
Cremer, J. W., Thaler, K. M., Haisch, C., and Signorell, R.: Photoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics, Nat. Commun., 7, 10941, https://doi.org/10.1038/ncomms10941, 2016.
Davies, J. F.: Mass, charge, and radius of droplets in a linear quadrupole electrodynamic balance, Aerosol Sci. Tech., 53, 309–320, https://doi.org/10.1080/02786826.2018.1559921, 2019.
Davies, J. F., Haddrell, A. E., Rickards, A. M. J., and Reid, J. P.: Simultaneous analysis of the equilibrium hygroscopicity and water transport kinetics of liquid aerosol, Anal. Chem., 85, 5819–5826, https://doi.org/10.1021/ac4005502, 2013.
Freedman, M. A.: Liquid–liquid phase separation in supermicrometer and submicrometer aerosol particles, Acc. Chem. Res., 53, 1102–1110, https://doi.org/10.1021/acs.accounts.0c00093, 2020.
Freedman, M. A., Ott, E.-J. E., and Marak, K. E.: Role of pH in aerosol processes and measurement challenges, J. Phys. Chem. A, 123, 1275–1284, https://doi.org/10.1021/acs.jpca.8b10676, 2019.
Gómez Castaño, J. A., Boussekey, L., Verwaerde, J. P., Moreau, M., and Tobón, Y. A.: Enhancing double-beam laser tweezers Raman spectroscopy (LTRS) for the photochemical study of individual airborne microdroplets, Molecules, 24, 3325, https://doi.org/10.3390/molecules24183325, 2019.
Gong, Y., Chen, Z., and Li, H.: The oxidation regime and SOA composition in limonene ozonolysis: roles of different double bonds, radicals, and water, Atmos. Chem. Phys., 18, 15105–15123, https://doi.org/10.5194/acp-18-15105-2018, 2018.
Gong, Z., Pan, Y.-L., Videen, G., and Wang, C.: Optical trapping and manipulation of single particles in air: Principles, technical details, and applications, J. Quant. Spectrosc. Ra., 214, 94–119, https://doi.org/10.1016/j.jqsrt.2018.04.027, 2018.
Gorkowski, K., Beydoun, H., Aboff, M., Walker, J. S., Reid, J. P., and Sullivan, R. C.: Advanced aerosol optical tweezers chamber design to facilitate phase-separation and equilibration timescale experiments on complex droplets, Aerosol Sci. Tech., 50, 1327–1341, https://doi.org/10.1080/02786826.2016.1224317, 2016.
Gorkowski K., Donahue N. M., and Sullivan R. C.: Emulsified and liquid-liquid phase-separated states of α-pinene secondary organic aerosol determined using aerosol optical tweezers, Environ. Sci. Technol., 51, 12154–12163, https://doi.org/10.1021/acs.est.7b03250, 2017.
Gorkowski, K., Donahue, N. M., and Sullivan, R. C.: Aerosol optical tweezers constrain the morphology evolution of liquid-liquid phase-separated atmospheric particles, Chem., 6, 204–220, https://doi.org/10.1016/j.chempr.2019.10.018, 2020.
Kolb, C. E. and Worsnop, D. R.: Chemistry and composition of atmospheric aerosol particles, Annu. Rev. Phys. Chem., 63, 471–491, https://doi.org/10.1146/annurev-physchem-032511-143706, 2012.
Krieger, U. K., Marcolli, C., and Reid, J. P.: Exploring the complexity of aerosol particle properties and processes using single particle techniques, Chem. Soc. Rev., 41, 6631–6662, https://doi.org/10.1039/C2CS35082C, 2012.
Mitchem, L., Buajarern, J., Ward, A. D., and Reid, J. P.: A strategy for characterizing the mixing state of immiscible aerosol components and the formation of multiphase aerosol particles through coagulation, J. Phys. Chem., 110, 13700–13703, https://doi.org/10.1021/jp062874z, 2006.
Mülmenstädt, J., Sourdeval, O., Delanoë, J., and Quaas, J.: Frequency of occurrence of rain from liquid-, mixed-, and ice-phase clouds derived from A-Train satellite retrievals, Geophys. Res. Lett., 42, 6502–6509, https://doi.org/10.1002/2015GL064604, 2015.
Mutzel, A., Zhang, Y., Böge, O., Rodigast, M., Kolodziejczyk, A., Wang, X., and Herrmann, H.: Importance of secondary organic aerosol formation of α-pinene, limonene, and m-cresol comparing day- and nighttime radical chemistry, Atmos. Chem. Phys., 21, 8479–8498, https://doi.org/10.5194/acp-21-8479-2021, 2021.
O'Haver, T. C.: A pragmatic introduction to signal processing with applications in scientific measurement, Kindle Direct 402 Publishing, ISBN 9798611266687, 2022.
Pei, X., Hallquist, M., Eriksson, A. C., Pagels, J., Donahue, N. M., Mentel, T., Svenningsson, B., Brune, W., and Pathak, R. K.: Morphological transformation of soot: investigation of microphysical processes during the condensation of sulfuric acid and limonene ozonolysis product vapors, Atmos. Chem. Phys., 18, 9845–9860, https://doi.org/10.5194/acp-18-9845-2018, 2018.
Pöschl, U.: Atmospheric Aerosols: Composition, Transformation, Climate and health effects, Angew. Chem. Int. Ed., 44, 7520–7540, https://doi.org/10.1002/anie.200501122, 2005.
Preston, T. C. and Reid, J. P.: Accurate and efficient determination of the radius, refractive index, and dispersion of weakly absorbing spherical particle using whispering gallery modes, J. Opt. Soc. Am. B, 30, 2113–2122, https://doi.org/10.1364/JOSAB.30.002113, 2013.
Preston, T. C. and Reid, J. P.: Determining the size and refractive index of microspheres using the mode assignments from Mie resonances, J. Opt. Soc. Am. A, 32, 2210–2217, https://doi.org/10.1364/JOSAA.32.002210, 2015.
Reid, J. P., Meresman, H., Mitchem, L., and Symes, R.: Spectroscopic studies of the size and composition of single aerosol droplets, Int. Rev. Phys. Chem., 26, 139–192, https://doi.org/10.1080/01442350601081899, 2007.
Rickards, A. M. J., Miles, R. E. H., Davies, J. F., Marshall, F. H., and Reid, J. P.: Measurements of the sensitivity of aerosol hygroscopicity and the κ parameter to the O C ratio, J. Phys. Chem. A., 117, 14120–14131, https://doi.org/10.1021/jp407991n, 2013.
Saathoff, H., Naumann, K.-H., Möhler, O., Jonsson, Å. M., Hallquist, M., Kiendler-Scharr, A., Mentel, Th. F., Tillmann, R., and Schurath, U.: Temperature dependence of yields of secondary organic aerosols from the ozonolysis of α-pinene and limonene, Atmos. Chem. Phys., 9, 1551–1577, https://doi.org/10.5194/acp-9-1551-2009, 2009.
Shrivastava, M., Cappa, C. D., Fan, J., Goldstein, A. H., Guenther, A. B., Jimenez, J. L., Kuang, C., Laskin, A., Martin, S. T., Ng, N. L., Petaja, T., Pierce, J. R., Rasch, P. J., Roldin, P., Seinfeld, J. H., Shilling, J., Smith, J. N., Thornton, J. A., Volkamer, R., Wang, J., Worsnop, D. R., Zaveri, R. A., Zelenyuk, A., and Zhang, Q.: Recent advances in understanding secondary organic aerosol: implications for global climate forcing, Rev. Geophys., 55, 509–559, https://doi.org/10.1002/2016RG000540, 2017.
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.: Liquid-liquid phase separation and morphology of internally mixed dicarboxylic acids/ammonium sulfate/water particles, Atmos. Chem. Phys., 12, 2691–2712, https://doi.org/10.5194/acp-12-2691-2012, 2012.
Song, M., Marcolli, C., Krieger, U. K., Lienhard, D. M., and Peter, T.: Morphologies of mixed organic/inorganic/aqueous aerosol droplets, Faraday Discuss., 165, 289–316, https://doi.org/10.1039/c3fd00049d, 2013.
Stewart, D. J., Cai, C., Nayler, J., Preston, T. C., Reid, J. P., Krieger, U. K., Marcolli, C., and Zhang, Y. H.: Liquid-liquid phase separation in mixed organic/inorganic single aqueous aerosol droplets, J. Phys. Chem. A, 119, 4177–4190, https://doi.org/10.1021/acs.jpca.5b01658, 2015.
Sullivan, R. C., Gorkowski, K., and Jahn, L.: Chapter 12 – Characterization of individual aerosol particles, in: Physical chemistry of gas-liquid interfaces, edited by: Faust, J. A. and House, J. E., Elsevier, 353–402, https://doi.org/10.1016/B978-0-12-813641-6.00012-1, 2018.
Sullivan, R. C., Boyer-Chelmo, H., Gorkowski, K., and Beydoun, H.: Aerosol optical tweezers elucidate the chemistry, acidity, phase separations, and morphology of atmospheric microdroplets, Acc. Chem. Res., 53, 2498–2509, https://doi.org/10.1021/acs.accounts.0c00407, 2020.
Takeuchi, M., Berkemeier, T., Eris, G., and Ng, N. L.: Non-linear effects of secondary organic aerosol formation and properties in multi-precursor systems, Nat. Commun., 13, 7883, https://doi.org/10.1038/s41467-022-35546-1, 2022.
Veghte, D. P., Altaf, M. B., and Freedman, M. A.: Size dependence of the structure of organic aerosol, J. Am. Chem. Soc., 135, 16046–16049, https://doi.org/10.1021/ja408903g, 2013.
Vennes, B. and Preston, T. C.: Calculating and fitting morphology-dependent resonances of a spherical particle with a concentric spherical shell, J. Opt. Soc. Am. A. Opt. Image. Sci. Vis., 36, 2089–2103, https://doi.org/10.1364/JOSAA.36.002089, 2019.
Zuend, A. and Seinfeld, J. H.: Modeling the gas-particle partitioning of secondary organic aerosol: the importance of liquid-liquid phase separation, Atmos. Chem. Phys., 12, 3857–3882, https://doi.org/10.5194/acp-12-3857-2012, 2012.
Short summary
An aerosol optical tweezer (AOT) Raman spectroscopy system is developed to capture a single aerosol droplet for phase transition monitoring and morphology studies. Rapid droplet capture is achieved and accurate droplet size and refractive index are retrieved. Results indicate that mixed inorganic/organic droplets are more inclined to form core–shell morphology when RH decreases. The phase transitions of secondary mixed organic aerosol/inorganic droplets vary with their precursors.
An aerosol optical tweezer (AOT) Raman spectroscopy system is developed to capture a single...
Altmetrics
Final-revised paper
Preprint