Articles | Volume 18, issue 16
https://doi.org/10.5194/amt-18-4045-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-18-4045-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Numerical quantitation on the effect of coating materials on the mixing state retrieval accuracy of fractal black carbon based on single particle soot photometer
Department of Atmospheric and Oceanic Sciences and Institutes of Atmospheric Sciences, Fudan University, Shanghai 200438, China
Engineering Research Center of Zero-carbon Energy Buildings and Measurement Techniques, Ministry of Education, Hebei University, Baoding 071002, China
China Meteorological Administration Xiong'an Atmospheric Boundary Layer Key Laboratory, Baoding 071800, China
Donghui Zhou
Engineering Research Center of Zero-carbon Energy Buildings and Measurement Techniques, Ministry of Education, Hebei University, Baoding 071002, China
China Meteorological Administration Xiong'an Atmospheric Boundary Layer Key Laboratory, Baoding 071800, China
Guangya Wang
Engineering Research Center of Zero-carbon Energy Buildings and Measurement Techniques, Ministry of Education, Hebei University, Baoding 071002, China
China Meteorological Administration Xiong'an Atmospheric Boundary Layer Key Laboratory, Baoding 071800, China
Cancan Zhu
Engineering Research Center of Zero-carbon Energy Buildings and Measurement Techniques, Ministry of Education, Hebei University, Baoding 071002, China
China Meteorological Administration Xiong'an Atmospheric Boundary Layer Key Laboratory, Baoding 071800, China
Xuehai Zhang
School of Information Science and Engineering, Henan University of Technology, Zhengzhou 450001, China
Related authors
Jia Liu, Cancan Zhu, Donghui Zhou, and Jinbao Han
Atmos. Chem. Phys., 24, 12341–12354, https://doi.org/10.5194/acp-24-12341-2024, https://doi.org/10.5194/acp-24-12341-2024, 2024
Short summary
Short summary
The hydrophilic coatings of aged black carbon (BC) particles absorb moisture during the hygroscopic growth process, but it is difficult to characterize how much water is absorbed under different relative humidities (RHs). In this study, we propose a method to obtain the water content in the coatings based on the equivalent complex refractive index retrieved from optical properties. This method is verified from a theoretical perspective, and it performs well for thickly coated BC at high RHs.
Jia Liu, Guangya Wang, Cancan Zhu, Donghui Zhou, and Lin Wang
Atmos. Meas. Tech., 16, 4961–4974, https://doi.org/10.5194/amt-16-4961-2023, https://doi.org/10.5194/amt-16-4961-2023, 2023
Short summary
Short summary
Single-particle soot photometer (SP2) employs the core-shell model to represent coated BC particles, which introduces retrieval errors in the mixing state (Dp/Dc) of BC. We construct fractal models to represent thinly and thickly coated BC particles, and the retrieval errors of the mixing state are investigated from the numerical aspect. We find that errors in Dp/Dc are noteworthy, and the errors in Dp/Dc can further affect the evaluation accuracy of the radiative forcing of BC.
Jia Liu, Cancan Zhu, Donghui Zhou, and Jinbao Han
Atmos. Chem. Phys., 24, 12341–12354, https://doi.org/10.5194/acp-24-12341-2024, https://doi.org/10.5194/acp-24-12341-2024, 2024
Short summary
Short summary
The hydrophilic coatings of aged black carbon (BC) particles absorb moisture during the hygroscopic growth process, but it is difficult to characterize how much water is absorbed under different relative humidities (RHs). In this study, we propose a method to obtain the water content in the coatings based on the equivalent complex refractive index retrieved from optical properties. This method is verified from a theoretical perspective, and it performs well for thickly coated BC at high RHs.
Jia Liu, Guangya Wang, Cancan Zhu, Donghui Zhou, and Lin Wang
Atmos. Meas. Tech., 16, 4961–4974, https://doi.org/10.5194/amt-16-4961-2023, https://doi.org/10.5194/amt-16-4961-2023, 2023
Short summary
Short summary
Single-particle soot photometer (SP2) employs the core-shell model to represent coated BC particles, which introduces retrieval errors in the mixing state (Dp/Dc) of BC. We construct fractal models to represent thinly and thickly coated BC particles, and the retrieval errors of the mixing state are investigated from the numerical aspect. We find that errors in Dp/Dc are noteworthy, and the errors in Dp/Dc can further affect the evaluation accuracy of the radiative forcing of BC.
Cited articles
Bhandari, J., China, S., Girotto, G., Scarnato, B. V., Gorkowski, K., Aiken, A. C., Dubey, M. K., and Mazzoleni, C.: Optical properties and radiative forcing of fractal-like tar ball aggregates from biomass burning, J. Quant. Spectrosc. Ra., 230, 65–74, https://doi.org/10.1016/j.jqsrt.2019.01.032, 2019.
Bond, T. C. and Bergstrom, R. W.: Light absorption by carbonaceous particles: An investigative review, Aerosol Sci. Tech., 40, 27–67, https://doi.org/10.1080/02786820500421521, 2006.
Bond, T. C., Doherty, S. J., Fahey, D. W., Forster, P. M., Berntsen, T., DeAngelo, B. J., Flanner, M. G., Ghan, S., Kärcher, B., Koch, D., Kinne, S., Kondo, Y., Quinn, P. K., Sarofim, M. C., Schultz, M. G., Schulz, M., Venkataraman, C., Zhang, H., Zhang, S., Bellouin, N., Guttikunda, S. K., Hopke, P. K., Jacobson, M. Z., Kaiser, J. W., Klimont, Z., Lohmann, U., Schwarz, J. P., Shindell, D., Storelvmo, T., Warren, S. G., and Zender, C. S.: Bounding the role of black carbon in the climate system: A scientific assessment, J. Geophys. Res.-Atmos., 118, 5380–5552, https://doi.org/10.1002/jgrd.50171, 2013.
Ceolato, R., Paulien, L., Maughan, J. B., Sorensen, C. M., and Berg, M. J.: Radiative properties of soot fractal superaggregates including backscattering and depolarization, J. Quant. Spectrosc. Ra., 247, https://doi.org/10.1016/j.jqsrt.2020.106940, 2020.
China, S., Mazzoleni, C., Gorkowski, K., Aiken, A. C., and Dubey, M. K.: Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles, Nat. Commun., 4, https://doi.org/10.1038/ncomms3122, 2013.
Cui, X., Wang, X., Yang, L., Chen, B., Chen, J., Andersson, A., and Gustafsson, Ö.: Radiative absorption enhancement from coatings on black carbon aerosols, Sci. Total Environ., 551, 51–56, 2016.
Ding, A. J., Huang, X., Nie, W., Sun, J. N., Kerminen, V. M., Petäjä, T., Su, H., Cheng, Y. F., Yang, X. Q., Wang, M. H., Chi, X. G., Wang, J. P., Virkkula, A., Guo, W. D., Yuan, J., Wang, S. Y., Zhang, R. J., Wu, Y. F., Song, Y., Zhu, T., Zilitinkevich, S., Kulmala, M., and Fu, C. B.: Enhanced haze pollution by black carbon in megacities in China, Geophys. Res. Lett., 43, 2873–2879, https://doi.org/10.1002/2016gl067745, 2016.
Gao, R. S., Schwarz, J. P., Kelly, K. K., Fahey, D. W., Watts, L. A., Thompson, T. L., Spackman, J. R., Slowik, J. G., Cross, E. S., Han, J. H., Davidovits, P., Onasch, T. B., and Worsnop, D. R.: A novel method for estimating light-scattering properties of soot aerosols using a modified single-particle soot photometer, Aerosol Sci. Tech., 41, 125–135, https://doi.org/10.1080/02786820601118398, 2007.
Kahnert, M. and Kanngiesser, F.: Modelling optical properties of atmospheric black carbon aerosols, J. Quant. Spectrosc. Ra., 244, https://doi.org/10.1016/j.jqsrt.2020.106849, 2020.
Kholghy, M., Saffaripour, M., Yip, C., and Thomson, M. J.: The evolution of soot morphology in a laminar coflow diffusion flame of a surrogate for Jet A-1, Combust. Flame, 160, 2119–2130, https://doi.org/10.1016/j.combustflame.2013.04.008, 2013.
Lack, D. A. and Cappa, C. D.: Impact of brown and clear carbon on light absorption enhancement, single scatter albedo and absorption wavelength dependence of black carbon, Atmos. Chem. Phys., 10, 4207–4220, https://doi.org/10.5194/acp-10-4207-2010, 2010.
Li, Y., Kang, S. C., Chen, J. Z., Hu, Z. F., Wang, K., Paudyal, R., Liu, J. S., Wang, X. X., Qin, X., and Sillanpää, M.: Black carbon in a glacier and snow cover on the northeastern Tibetan Plateau: Concentrations, radiative forcing and potential source from local topsoil, Sci. Total Environ., 686, 1030–1038, https://doi.org/10.1016/j.scitotenv.2019.05.469, 2019.
Liu, D., Allan, J. D., Young, D. E., Coe, H., Beddows, D., Fleming, Z. L., Flynn, M. J., Gallagher, M. W., Harrison, R. M., Lee, J., Prevot, A. S. H., Taylor, J. W., Yin, J., Williams, P. I., and Zotter, P.: Size distribution, mixing state and source apportionment of black carbon aerosol in London during wintertime, Atmos. Chem. Phys., 14, 10061–10084, https://doi.org/10.5194/acp-14-10061-2014, 2014.
Liu, H., Pan, X., Liu, D., Liu, X., Chen, X., Tian, Y., Sun, Y., Fu, P., and Wang, Z.: Mixing characteristics of refractory black carbon aerosols at an urban site in Beijing, Atmos. Chem. Phys., 20, 5771–5785, https://doi.org/10.5194/acp-20-5771-2020, 2020a.
Liu, H., Pan, X., Wang, D., Liu, X., Tian, Y., Yao, W., Lei, S., Zhang, Y., Li, J., Lei, L., Xie, C., Fu, P., Sun, Y., and Wang, Z.: Mixing characteristics of black carbon aerosols in a coastal city using the CPMA-SP2 system, Atmos. Res., 265, https://doi.org/10.1016/j.atmosres.2021.105867, 2022.
Liu, J., Zhang, Q., Wang, J., and Zhang, Y.: Light scattering matrix for soot aerosol: Comparisons between experimental measurements and numerical simulations, J. Quant. Spectrosc. Ra., 246, 106946, https://doi.org/10.1016/j.jqsrt.2020.106946, 2020b.
Liu, J., Wang, L., Wang, G. Y., and Zhang, X. H.: Numerical investigation on the accuracy of size information of fractal soot aerosols retrieved by lidar: Optical property, morphology effect, and parameterization scheme, J. Quant. Spectrosc. Ra., 295, https://doi.org/10.1016/j.jqsrt.2022.108435, 2023a.
Liu, J., Wang, G., Zhu, C., Zhou, D., and Wang, L.: Numerical investigation on retrieval errors of mixing states of fractal black carbon aerosols using single-particle soot photometer based on Mie scattering and the effects on radiative forcing estimation, Atmos. Meas. Tech., 16, 4961–4974, https://doi.org/10.5194/amt-16-4961-2023, 2023b.
Liu, J., Zhou, D. H., Zhu, C. C., Han, J. B., and Yin, B.: Optical and radiative properties of coated black carbon during hygroscopic growth and retrieval errors of mixing state using single-particle soot photometer, Particuology, 97, 183–192, https://doi.org/10.1016/j.partic.2024.12.010, 2025a.
Liu, J., Zhou, D., Wang, G., Zhu, C., and Zhang, X.: DpDc retrieval of soot with different coatings using SP2, ResearchGate [data set], https://doi.org/10.13140/RG.2.2.10735.14249, 2025b.
Luo, J., Zhang, Y., and Zhang, Q.: Effects of black carbon morphology on brown carbon absorption estimation: from numerical aspects, Geosci. Model Dev., 14, 2113–2126, https://doi.org/10.5194/gmd-14-2113-2021, 2021.
Mackowski, D. W. and Mishchenko, M. I.: A multiple sphere T-matrix Fortran code for use on parallel computer clusters, J. Quant. Spectrosc. Ra., 112, 2182–2192, 2011.
Mackowski, D. W. and Mishchenko, M. I.: The multiple-sphere T-matrix code, GitHub [code], https://github.com/dmckwski/MSTM (last access: 26 August 2025), 2023.
Mishchenko, M. I., Travis, L. D., and Lacis, A. A.: Scattering, absorption, and emission of light by small particles, Cambridge university press, ISBN 9780521782524, 2002.
Murphy, D. M., Froyd, K. D., Schwarz, J. P., and Wilson, J. C.: Observations of the chemical composition of stratospheric aerosol particles, Q. J. Roy. Meteor. Soc., 140, 1269–1278, https://doi.org/10.1002/qj.2213, 2014.
Peng, H. Y., Wang, Y. S., Wang, Y. L., Chen, Y. K., Li, D., and Xue, H.: Characteristics of emission and light-absorption of size-segregated carbonaceous aerosol emitted from four types of coal combustion at different combustion temperatures, Atmos. Pollut. Res., 13, https://doi.org/10.1016/j.apr.2021.101265, 2022.
Qin, Z. H., Zhang, Q. X., Luo, J., and Zhang, Y. M.: Optical properties of soot aggregates with different monomer shapes, Environ. Res., 214, https://doi.org/10.1016/j.envres.2022.113895, 2022.
Santoso, M., Lestiani, D. D., Kurniawati, S., Damastuti, E., Kusmartini, I., Atmodjo, D. P. D., Sari, D. K., Hopke, P. K., Mukhtar, R., Muhtarom, T., Tjahyadi, A., Parian, S., Kholik, N., Sutrisno, D. A., Wahyudi, D., Sitorus, T. D., Djamilus, J., Riadi, A., Supriyanto, J., Dahyar, N., Sondakh, S., Hogendorp, K., Wahyuni, N., Bejawan, I. G., and Suprayadi, L. S.: Assessment of Urban Air Quality in Indonesia, Aerosol Air Qual. Res., 20, 2142–2158, https://doi.org/10.4209/aaqr.2019.09.0451, 2020.
Schwarz, J. P.: Extrapolation of single particle soot photometer incandescent signal data, Aerosol Sci. Tech., 53, 911–920, https://doi.org/10.1080/02786826.2019.1610154, 2019.
Schwarz, J. P., Gao, R. S., Fahey, D. W., Thomson, D. S., Watts, L. A., Wilson, J. C., Reeves, J. M., Darbeheshti, M., Baumgardner, D. G., Kok, G. L., Chung, S. H., Schulz, M., Hendricks, J., Lauer, A., Kärcher, B., Slowik, J. G., Rosenlof, K. H., Thompson, T. L., Langford, A. O., Loewenstein, M., and Aikin, K. C.: Single-particle measurements of midlatitude black carbon and light-scattering aerosols from the boundary layer to the lower stratosphere, J. Geophys. Res.-Atmos., 111, https://doi.org/10.1029/2006jd007076, 2006.
Schwarz, J. P., Gao, R., Spackman, J., Watts, L., Thomson, D., Fahey, D., Ryerson, T., Peischl, J., Holloway, J., and Trainer, M.: Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions, Geophys. Res. Lett., 35, https://doi.org/10.1029/2008GL033968, 2008a.
Schwarz, J. P., Spackman, J. R., Fahey, D. W., Gao, R. S., Lohmann, U., Stier, P., Watts, L. A., Thomson, D. S., Lack, D. A., Pfister, L., Mahoney, M. J., Baumgardner, D., Wilson, J. C., and Reeves, J. M.: Coatings and their enhancement of black carbon light absorption in the tropical atmosphere, J. Geophys. Res.-Atmos., 113, https://doi.org/10.1029/2007jd009042, 2008b.
Sorensen, C. M. and Roberts G. C.: The Prefactor of Fractal Aggregates, J. Colloid Interf. Sci., 186, 447–452, https://doi.org/10.1006/jcis.1996.4664, 1997.
Wang, S. R., Zhou, K. L., Lu, X. H., Chen, H., Yang, F., Li, Q., Yang, X., and Wang, X. F.: Measurement of Density and Shape for Single Black Carbon Aerosols in a Heavily Polluted Urban Area, Aerosol Air Qual. Res., 21, https://doi.org/10.4209/aaqr.210162, 2021a.
Wang, Y. Y., Li, W. J., Huang, J., Liu, L., Pang, Y. E., He, C. L., Liu, F. S., Liu, D. T., Bi, L., Zhang, X. Y., and Shi, Z. B.: Nonlinear Enhancement of Radiative Absorption by Black Carbon in Response to Particle Mixing Structure, Geophys. Res. Lett., 48, https://doi.org/10.1029/2021gl096437, 2021b.
Wozniak, M., Onofri, F. R. A., Barbosa, S., Yon, J., and Mroczka, J.: Comparison of methods to derive morphological parameters of multi-fractal samples of particle aggregates from TEM images, J. Aerosol. Sci., 47, 12–26, https://doi.org/10.1016/j.jaerosci.2011.12.008, 2012.
Yu, F. and Luo, G.: Simulation of particle size distribution with a global aerosol model: contribution of nucleation to aerosol and CCN number concentrations, Atmos. Chem. Phys., 9, 7691–7710, https://doi.org/10.5194/acp-9-7691-2009, 2009.
Zeng, C., Liu, C., Li, J. N., Zhu, B., Yin, Y., and Wang, Y.: Optical Properties and Radiative Forcing of Aged BC due to Hygroscopic Growth: Effects of the Aggregate Structure, J. Geophys. Res.-Atmos., 124, 4620–4633, https://doi.org/10.1029/2018jd029809, 2019.
Zhang, K., O'Donnell, D., Kazil, J., Stier, P., Kinne, S., Lohmann, U., Ferrachat, S., Croft, B., Quaas, J., Wan, H., Rast, S., and Feichter, J.: The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations, Atmos. Chem. Phys., 12, 8911–8949, https://doi.org/10.5194/acp-12-8911-2012, 2012.
Zhang, X. L., Wang, Y. Z., Zhou, Y., Wang, J. Y., and Mao, M.: Significance of Absorbing Fraction of Coating on Absorption Enhancement of Partially Coated Black Carbon Aerosols, Atmosphere, 12, https://doi.org/10.3390/atmos12111422, 2021.
Zhang, Y. T., Liu, H., Lei, S. D., Du, A. D., Yao, W. J., Tian, Y., Sun, Y. L., Xin, J. Y., Li, J., Cao, J. J., Wang, Z. F., and Pan, X. L.: Size-resolved mixing state of ambient refractory black carbon aerosols in Beijing during the XXIV Olympic winter games, Atmos. Environ., 301, https://doi.org/10.1016/j.atmosenv.2023.119672, 2023.
Zhang, Y., Li, M., Cheng, Y., Geng, G., Hong, C., Li, H., Li, X., Tong, D., Wu, N., Zhang, X., Zheng, B., Zheng, Y., Bo, Y., Su, H., and Zhang, Q.: Modeling the aging process of black carbon during atmospheric transport using a new approach: a case study in Beijing, Atmos. Chem. Phys., 19, 9663–9680, https://doi.org/10.5194/acp-19-9663-2019, 2019.
Short summary
Single-particle soot photometer (SP2) measures the mixing state (Dp/Dc) of coated black carbon (BC) using core-shell Mie theory and coating refractive index is set to 1.50+0i. The retrieved Dp/Dc contains error due to the non-sphericity of BC and coatings with various refractive indices. We reveal the remarkable effects of coatings on the Dp/Dc retrieval accuracy of SP2 based on optical simulation of fractal BC aerosols, and further evaluate the simple radiative forcing efficiency of coated BC.
Single-particle soot photometer (SP2) measures the mixing state (Dp/Dc) of coated black carbon...