DOI: https://doi.org/10.1038/s41612-024-00610-8
تاريخ النشر: 2024-03-08
الخصائص الميكروفزيائية للسخام الجوي والجسيمات العضوية: القياسات، النمذجة، والتأثيرات
الملخص
السخام الجوي والجزيئات العضوية الناتجة عن احتراق الوقود الأحفوري وحرق الكتلة الحيوية تعدل مناخ الأرض من خلال تفاعلاتها مع الإشعاع الشمسي ومن خلال تعديل خصائص السحب من خلال عملها كنوى تكثف السحب وجزيئات نواة الجليد. أدت التقدمات الأخيرة في فهم خصائصها الفردية وتركيبها المجهري إلى زيادة الاهتمام بخصائصها الميكروفزيائية. تقدم هذه المقالة الاستعراضية لمحة عامة عن القياسات المجهرية المتقدمة الحالية وتقدم رؤى حول السبل المستقبلية لدراسة الخصائص الميكروفزيائية لهذه الجزيئات. لت quantifying شكل السخام وعمره، بُعد الفراكتال
تظل الهباءات العضوية نقاط بحث محورية بسبب أدوارها المهمة ومساهماتها المحتملة في عدم اليقين في نظام المناخ الجوي.
تظهر الخلائط أيضًا خصائص امتصاص ضوء ملحوظة، والتي تم تسميتها بشكل جماعي بالكربون البني (BrC).
ما الذي يحدد آليات الشيخوخة الرئيسية لمجموعات الجسيمات المكونة من السخام والمكونات العضوية؟ كيف تغير عمليات الشيخوخة الجوية هيكل الخلط لجسيمات السخام-العضوية في الهواء الملوث؟
كيف يؤثر الماء الجوي على الطور وهيكل الخلط لمخاليط الجسيمات السخام-العضوية؟ إلى أي مدى تؤثر المكونات غير العضوية على خصائص الطور والخلط للجسيمات؟
كيف تحول هياكل الخلط للسخام والعضويات الشكل والخصائص البصرية للجسيمات، مما يؤثر على تأثيرها على ديناميات المناخ وصحة الإنسان؟
المنهجيات لملاحظات الجسيمات المفصلة لمخاليط السخام-العضوية

الظروف والتعرض لإشعاع شعاع الإلكترون (كما يتضح من المكون الغني بالكبريت في الشكل 2 ج)، خاصة في حالة المكونات العضوية وغير العضوية المختلطة
الخصائص الميكروفزيائية لجزيئات السخام

مونومر، و
يفترض أن نوع مصدر الاحتراق لجزيئات السخام يؤثر بشكل ملحوظ على الشكل الكسري لجزيئات السخام. وقد أكدت الدراسات الحديثة على الفروق في المعلمات الشكلية لجزيئات السخام المنبعثة حديثًا من مصادر احتراق مختلفة، لا سيما بالنسبة للأحجام الدقيقة والخشنة لجزيئات السخام.

مستمد من NanoSIMS يظهر
الخصائص الميكروفزيائية للجسيمات العضوية
خلط الهيكل وحالة الطور. الأخيرة تصف ما إذا كانت الجسيمات سائلة أو لزجة أو شبه صلبة أو مواد زجاجية غير متبلورة. يتعلق هيكل خلط الهباء العضوي بكيفية خلط المادة العضوية داخليًا مع المكونات غير العضوية (كما هو موضح في الأشكال 3 و4a وb).

تم جمع (SEM) في الهواء الضاحي. توزيعات حجم جزيئات كرات القطران المجمعة في حرائق الغابات

الهياكل المختلطة المطلية بـ SOA والمتماثلة بـ SOA
التأثيرات الجوية للجسيمات المكونة من السخام والمخاليط العضوية

المراجع.
خصائص. على وجه التحديد، يمكن أن تكون مقاطع التشتت لهذه الجسيمات أكبر بنسبة تصل إلى 50% مقارنة بتلك الخاصة بالجسيمات المختلطة بشكل متجانس، في حين قد يتم تقليل مقاطع الامتصاص بنسبة تصل إلى
آثار على القوة الإشعاعية
آثار على السحب


غيوم
آثار أخرى محتملة
العلاقة المعقدة بين ترسبات الهباء الجوي الممتص للضوء (مثل السخام، الكربون العضوي الأسود، والغبار المعدني) في تقليل البياض الثلجي. الثلج يعكس ضوء الشمس بشكل قوي، بينما يعتمد مدى الانعكاس بشكل كبير على عوامل مثل حجم حبيبات الثلج وشكلها وحالة خلط السخام مع مصفوفة الثلج. على الرغم من أن هناك تقارير قليلة تناولت هياكل خلط جزيئات السخام في الغلاف الجوي للثلوج الجليدية.
ملخص وآفاق المستقبل
امتصاص السخام وBrC. (3) بالإضافة إلى الخصائص الميكروفزيائية للجسيمات الممتصة للضوء، فإن تركيبها الكيميائي، وخاصة BrC، يخضع لتغيرات مستمرة بسبب شيخوخة الغلاف الجوي أو التغيرات الناجمة عن مسارات التكوين المختلفة والمصادر. (4) هناك حاجة إلى نماذج بصرية محسّنة لهياكل الخلط الواقعية للتنبؤ بدقة بالخصائص البصرية للسخام العضوي والجسيمات العضوية المتقدمة، وخاصة تلك التي تظهر هياكل مختلطة معقدة وأشكال. يمكن أن يؤدي تنفيذ هذه التقنيات المتقدمة إلى تقليل وقت الحساب بشكل كبير وتسهيل إنشاء قاعدة بيانات بصرية واسعة لنماذج المناخ.
تم النشر عبر الإنترنت: 08 مارس 2024
References
- Riemer, N., Ault, A. P., West, M., Craig, R. L. & Curtis, J. H. Aerosol mixing state: measurements, modeling, and impacts. Rev. Geophys. 57 https://doi.org/10.1029/2018RG000615 (2019).
- Li, W. et al. A review of single aerosol particle studies in the atmosphere of East Asia: morphology, mixing state, source, and heterogeneous reactions. J. Clean. Prod. 112, 1330-1349 (2016).
- Bond, T. C. et al. Bounding the role of black carbon in the climate system: a scientific assessment. J. Geophys. Res. 118, 5380-5552 (2013).
- Li, J. et al. Scattering and absorbing aerosols in the climate system. Nat. Rev. Earth Environ. https://doi.org/10.1038/s43017-022-00296-7 (2022).
- Coppola, A. I. et al. The black carbon cycle and its role in the Earth system. Nat. Rev. Earth Environ. https://doi.org/10.1038/s43017-022-00316-6 (2022).
- Laskin, A., Laskin, J. & Nizkorodov, S. A. Chemistry of atmospheric brown carbon. Chem. Rev. 115, 4355-4382 (2015).
- Wang, Q. et al. Review of brown carbon aerosols in China: pollution level, optical properties, and emissions. J. Geophys. Res. 127, e2021JD035473 (2022).
- Yue, S. et al. Brown carbon from biomass burning imposes strong circum-Arctic warming. One Earth 5, 293-304 (2022).
- Freedman, M. A. Liquid-liquid phase separation in supermicrometer and submicrometer aerosol particles. Acc. Chem. Res. 53, 1102-1110 (2020).
- Laskin, A., Moffet, R. C. & Gilles, M. K. Chemical imaging of atmospheric particles. Acc. Chem. Res. 52, 3419-3431 (2019).
- Reid, J. P. et al. The viscosity of atmospherically relevant organic particles. Nat. Commun. 9, 956 (2018).
- Shrivastava, M. et al. Recent advances in understanding secondary organic aerosol: implications for global climate forcing. Rev. Geophys. 55, 509-559 (2017).
- Wang, Y. et al. Nonlinear enhancement of radiative absorption by black carbon in response to particle mixing structure. Geophys. Res. Lett. 48, e2021GL096437 (2021).
- Fierce, L. et al. Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition. Proc. Natl Acad. Sci. USA 117, 5196-5203 (2020).
- Wang, J. et al. Unified theoretical framework for black carbon mixing state allows greater accuracy of climate effect estimation. Nat. Commun. 14, 2703 (2023).
- Kanakidou, M. et al. Organic aerosol and global climate modelling: a review. Atmos. Chem. Phys. 5, 1053-1123 (2005).
- Chen, Q. et al. Mass spectral characterization of submicron biogenic organic particles in the Amazon Basin. Geophys. Res. Lett. 36 https://doi.org/10.1029/2009gl039880 (2009).
- Petzold, A. et al. Recommendations for reporting “black carbon” measurements. Atmos. Chem. Phys. 13, 8365-8379 (2013).
- Buseck, P. R., Adachi, K., Gelencsér, A., Tompa, É. & Pósfai, M. Nssoot: a material-based term for strongly light-absorbing carbonaceous particles. Aerosp. Sci. Technol. 48, 777-788 (2014).
- IPCC. in Climate Change 2021: The Physical Science Basis (eds Masson-Delmotte, V. et al.) 817-922 (Cambridge University Press, 2022).
- Cao, J.-J. et al. Black carbon relationships with emissions and meteorology in Xi’an, China. Atmos. Res. 94, 194-202 (2009).
- Metcalf, A. R. et al. Black carbon aerosol over the Los Angeles Basin during CalNex. J. Geophys. Res. 117, D00V13 (2012).
- Sharma, S. Long-term trends of the black carbon concentrations in the Canadian Arctic. J. Geophys. Res. 109 https://doi.org/10.1029/ 2003jd004331 (2004).
- Dai, M. et al. Long-term variation and source apportionment of black carbon at Mt. Waliguan, China. J. Geophys. Res. 126, e2021JD035273 (2021).
- Cappa, C. D. et al. Radiative absorption enhancements due to the mixing state of atmospheric black carbon. Science 337, 1078-1081 (2012).
- Adachi, K., Chung, S. H. & Buseck, P. R. Shapes of soot aerosol particles and implications for their effects on climate. J. Geophys. Res. 115 https://doi.org/10.1029/2009JD012868 (2010).
- Jacobson, M. Z. Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols. Nature 409, 695-697 (2001).
- Poschl, U. Atmospheric aerosols: composition, transformation, climate and health effects. Angew. Chem. Int. Ed. 44, 7520-7540 (2005).
- Jo, D. S., Park, R. J., Lee, S., Kim, S. W. & Zhang, X. A global simulation of brown carbon: implications for photochemistry and direct radiative effect. Atmos. Chem. Phys. 16, 3413-3432 (2016).
- Chakrabarty, R. K. et al. Shortwave absorption by wildfire smoke dominated by dark brown carbon. Nat. Geosci. 16, 683-688 (2023).
- Corbin, J. C. et al. Infrared-absorbing carbonaceous tar can dominate light absorption by marine-engine exhaust. npj Clim. Atmos. Sci. 2 https://doi.org/10.1038/s41612-019-0069-5 (2019).
- Ault, A. P. & Axson, J. L. Atmospheric aerosol chemistry: spectroscopic and microscopic advances. Anal. Chem. 89, 430-452 (2017).
- Shao, L. et al. A review of atmospheric individual particle analyses: methodologies and applications in environmental research. Gondwana Res. 110, 347-369 (2022).
- Liu, C., Xu, X., Yin, Y., Schnaiter, M. & Yung, Y. L. Black carbon aggregates: a database for optical properties. J. Quant. Spectrosc. Radiat. Transf. 222-223, 170-179 (2019).
- Smith, A. J. A. & Grainger, R. G. Simplifying the calculation of light scattering properties for black carbon fractal aggregates. Atmos. Chem. Phys. 14, 7825-7836 (2014).
- Romshoo, B. et al. Optical properties of coated black carbon aggregates: numerical simulations, radiative forcing estimates, and size-resolved parameterization scheme. Atmos. Chem. Phys. 21, 12989-13010 (2021).
- Mackowski, D. W. & Mishchenko, M. I. A multiple sphere T-matrix Fortran code for use on parallel computer clusters. J. Quant. Spectrosc. Radiat. Transf. 112, 2182-2192 (2011).
- Wang, Y. et al. Constructing shapes and mixing structures of black carbon particles with applications to optical calculations. J. Geophys. Res. 126, e2021JD034620 (2021).
- Hu, K. et al. Measurements of the diversity of shape and mixing state for ambient black carbon particles. Geophys. Res. Lett. 48, e2021GL094522 (2021).
- Slowik, J. G. et al. Measurements of morphology changes of fractal soot particles using coating and denuding experiments: implications for optical absorption and atmospheric lifetime. Aerosp. Sci. Technol. 41, 734-750 (2007).
- Schnitzler, E. G., Dutt, A., Charbonneau, A. M., Olfert, J. S. & Jäger, W. Soot aggregate restructuring due to coatings of secondary organic aerosol derived from aromatic precursors. Environ. Sci. Technol. 48, 14309-14316 (2014).
- Sedlacek, A. J. III, Lewis, E. R., Kleinman, L., Xu, J. & Zhang, Q. Determination of and evidence for non-core-shell structure of particles containing black carbon using the single-particle soot photometer (SP2). Geophys. Res. Lett. 39, L06802 (2012).
- Zhang, Y. et al. Extremely low-volatility organic coating leads to underestimation of black carbon climate impact. One Earth 6, 158-166 (2023).
- Naseri, A., Sipkens, T. A., Rogak, S. N. & Olfert, J. S. An improved inversion method for determining two-dimensional mass distributions of non-refractory materials on refractory black carbon. Aerosp. Sci. Technol. 55, 104-118 (2020).
- Liu, D. et al. Black-carbon absorption enhancement in the atmosphere determined by particle mixing state. Nat. Geosci. 10, 184-188 (2017).
- Zhai, J. et al. Absorption enhancement of black carbon aerosols constrained by mixing-state heterogeneity. Environ. Sci. Technol. 56, 1586-1593 (2022).
- Schwarz, J. P. et al. Coatings and their enhancement of black carbon light absorption in the tropical atmosphere. J. Geophys. Res. 113 https://doi.org/10.1029/2007jd009042 (2008).
- Pratt, K. A. & Prather, K. A. Mass spectrometry of atmospheric aerosols -recent developments and applications. Part II: on-line mass spectrometry techniques. Mass Spectrom. Rev. 31, 17-48 (2012).
- Zelenyuk, A. & Imre, D. Beyond single particle mass spectrometry: multidimensional characterisation of individual aerosol particles. Annu. Rev. Phys. Chem. 28, 309-358 (2009).
- Canagaratna, M. R. et al. Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer. Mass Spectrom. Rev. 26, 185-222 (2007).
- Virtanen, A. et al. An amorphous solid state of biogenic secondary organic aerosol particles. Nature 467, 824-827 (2010).
- China, S., Mazzoleni, C., Gorkowski, K., Aiken, A. C. & Dubey, M. K. Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles. Nat. Commun. 4, 2122 (2013).
- Shi, Z. B., Zhang, D. Z., Ji, H. Z., Hasegawa, S. & Hayashi, M. Modification of soot by volatile species in an urban atmosphere. Sci. Total Environ. 389, 195-201 (2008).
- Geng, H., Ryu, J. Y., Maskey, S., Jung, H. J. & Ro, C. U. Characterisation of individual aerosol particles collected during a haze episode in Incheon, Korea using the quantitative ED-EPMA technique. Atmos. Chem. Phys. 11, 1327-1337 (2011).
- Ebert, M., Weinbruch, S., Hoffmann, P. & Ortner, H. M. The chemical composition and complex refractive index of rural and urban influenced aerosols determined by individual particle analysis. Atmos. Environ. 38, 6531-6545 (2004).
- Wang, Y. et al. Fractal dimensions and mixing structures of soot particles during atmospheric processing. Environ. Sci. Tech. Let. 4, 487-493 (2017).
- Ueda, S. et al. Morphological features and mixing states of sootcontaining particles in the marine boundary layer over the Indian and Southern oceans. Atmos. Chem. Phys. 18, 9207-9224 (2018).
- Li, W. et al. A conceptual framework for mixing structures in individual aerosol particles. J. Geophys. Res. 121, 13,784-713,798 (2016).
- Pöhlker, C. et al. Biogenic potassium salt particles as seeds for secondary organic aerosol in the Amazon. Science 337, 1075-1078 (2012).
- Li, W. et al. Microscopic evidence for phase separation of organic species and inorganic salts in fine ambient aerosol particles. Environ. Sci. Technol. 55, 2234-2242 (2021).
- O’Brien, R. E. et al. Liquid-liquid phase separation in aerosol particles: imaging at the nanometer scale. Environ. Sci. Technol. 49, 4995-5002 (2015).
- Laskina, O., Young, M. A., Kleiber, P. D. & Grassian, V. H. Infrared extinction spectroscopy and micro-Raman spectroscopy of select components of mineral dust mixed with organic compounds. J. Geophys. Res. 118, 6593-6606 (2013).
- Takahama, S., Liu, S. & Russell, L. M. Coatings and clusters of carboxylic acids in carbon-containing atmospheric particles from spectromicroscopy and their implications for cloud-nucleating and optical properties. J. Geophys. Res. 115 https://doi.org/10.1029/ 2009jd012622 (2010).
- Wang, M., Zheng, N., Zhao, D., Shang, J. & Zhu, T. Using microRaman spectroscopy to investigate chemical composition, mixing states, and heterogeneous reactions of individual atmospheric particles. Environ. Sci. Technol. 55, 10243-10254 (2021).
- Li, X., Gupta, D., Lee, J., Park, G. & Ro, C.-U. Real-time investigation of chemical compositions and hygroscopic properties of aerosols generated from NaCl and malonic acid mixture solutions using in situ Raman microspectrometry. Environ. Sci. Technol. 51, 263-270 (2017).
- Li, W. et al. Organic coating reduces hygroscopic growth of phaseseparated aerosol particles. Environ. Sci. Technol. 55, 16339-16346 (2021).
- Ott, E. J. E., Tackman, E. C. & Freedman, M. A. Effects of sucrose on phase transitions of organic/inorganic aerosols. ACS Earth Space Chem. 4, 591-601 (2020).
- Kucinski, T. M., Dawson, J. N. & Freedman, M. A. Size-dependent liquid-liquid phase separation in atmospherically relevant complex systems. J. Phys. Chem. Lett. 10, 6915-6920 (2019).
- Zhang, J. et al. Liquid-liquid phase separation reduces radiative absorption by aged black carbon aerosols. Commun. Earth Environ. 3, 128 (2022).
- Veghte, D. P., Altaf, M. B. & Freedman, M. A. Size dependence of the structure of organic aerosol. J. Am. Chem. Soc. 135, 16046-16049 (2013).
- Pang, Y. et al. Quantifying the fractal dimension and morphology of individual atmospheric soot aggregates. J. Geophys. Res. 127, e2021JD036055 (2022).
- Chakrabarty, R. K., Moosmüller, H., Arnott, W. P., Garro, M. A. & Walker, J. Structural and fractal properties of particles emitted from spark ignition engines. Environ. Sci. Technol. 40, 6647-6654 (2006).
- Brasil, A. M., Farias, T. L. & Carvalho, M. G. A recipe for image characterization of fractal-like aggregates. J. Aerosol Sci. 30, 1379-1389 (1999).
- Adachi, K., Chung, S. H., Friedrich, H. & Buseck, P. R. Fractal parameters of individual soot particles determined using electron tomography: implications for optical properties. J. Geophys. Res. 112, D14202 (2007).
- Sipkens, T. A. et al. Overview of methods to characterize the mass, size, and morphology of soot. J. Aerosol Sci. 173, 106211 (2023).
- Haffner-Staton, E., Avanzini, L., La Rocca, A., Pfau, S. A. & Cairns, A. Automated particle recognition for engine soot nanoparticles. J. Microsc. 288, 28-39 (2022).
- Pang, Y. et al. Morphology and fractal dimension of size-resolved soot particles emitted from combustion sources. J. Geophys. Res. 128, e2022JD037711 (2023).
- Niu, H., Shao, L. & Zhang, D. Soot particles at an elevated site in eastern China during the passage of a strong cyclone. Sci. Total Environ. 430, 217-222 (2012).
- China, S., Salvadori, N. & Mazzoleni, C. Effect of traffic and driving characteristics on morphology of atmospheric soot particles at freeway on-ramps. Environ. Sci. Technol. 48, 3128-3135 (2014).
- Chen, C. et al. An unexpected restructuring of combustion soot aggregates by subnanometer coatings of polycyclic aromatic hydrocarbons. Geophys. Res. Lett. 43, 11,080-011,088 (2016).
- Zhang, J. et al. Structural collapse and coating composition changes of soot particles during long-range transport. J. Geophys. Res. 128, e2023JD038871 (2023).
- Enekwizu, O. Y., Hasani, A. & Khalizov, A. F. Vapor condensation and coating evaporation are both responsible for soot aggregate restructuring. Environ. Sci. Technol. 55, 8622-8630 (2021).
- Corbin, J. C., Modini, R. L. & Gysel-Beer, M. Mechanisms of sootaggregate restructuring and compaction. Aerosol Sci. Technol. 57, 89-111 (2023).
- Zhang, R. Y. et al. Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing. Proc. Natl Acad. Sci. USA 105, 10291-10296 (2008).
- Ma, X., Zangmeister, C. D., Gigault, J., Mulholland, G. W. & Zachariah, M. R. Soot aggregate restructuring during water processing. J. Aerosol Sci. 66, 209-219 (2013).
- Bhandari, J. et al. Extensive soot compaction by cloud processing from laboratory and field observations. Sci. Rep. 9, 11824 (2019).
- Chen, X . et al. Quantifying evolution of soot mixing state from transboundary transport of biomass burning emissions. IScience 26, 108125 (2023).
- Wu, Z. et al. Aerosol liquid water driven by anthropogenic inorganic salts: implying its key role in haze formation over the North China Plain. Environ. Sci. Technol. Lett. 5, 160-166 (2018).
- Peckhaus, A., Grass, S., Treuel, L. & Zellner, R. Deliquescence and efflorescence behavior of ternary inorganic/Organic/water aerosol particles. J. Phys. Chem. A 116, 6199-6210 (2012).
- Freney, E. J., Adachi, K. & Buseck, P. R. Internally mixed atmospheric aerosol particles: hygroscopic growth and light scattering. J. Geophys. Res. 115 https://doi.org/10.1029/ 2009jd013558 (2010).
- Kuang, Y. et al. Deliquescent phenomena of ambient aerosols on the North China Plain. Geophys. Res. Lett. 43, 8744-8750 (2016).
- Posfai, M. et al. Atmospheric tar balls: particles from biomass and biofuel burning. J. Geophys. Res. 109 https://doi.org/10.1029/ 2003JD004169 (2004).
- Wang, B. et al. Airborne soil organic particles generated by precipitation. Nat. Geosci. 9, 433-437 (2016).
- Sedlacek lii, A. J. et al. Formation and evolution of tar balls from northwestern US wildfires. Atmos. Chem. Phys. 18, 11289-11301 (2018).
- Adachi, K. et al. Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomassburning smoke. Proc. Natl Acad. Sci. USA 116, 19336-19341 (2019).
- Liu, L. et al. Persistent residential burning-related primary organic particles during wintertime hazes in North China: insights into their aging and optical changes. Atmos. Chem. Phys. 21, 2251-2265 (2021).
- Li, C. et al. Dynamic changes in optical and chemical properties of tar ball aerosols by atmospheric photochemical aging. Atmos. Chem. Phys. 19, 139-163 (2019).
- Corbin, J. C. & Gysel-Beer, M. Detection of tar brown carbon with a single particle soot photometer (SP2). Atmos. Chem. Phys. 19, 15673-15690 (2019).
- You, Y. et al. Images reveal that atmospheric particles can undergo liquid-liquid phase separations. Proc. Natl Acad. Sci. USA 109, 13188-13193 (2012).
- Kirpes, R. M. et al. Solid organic-coated ammonium sulfate particles at high relative humidity in the summertime Arctic atmosphere. Proc. Natl Acad. Sci. USA 119, e2104496119 (2022).
- Shiraiwa, M. et al. Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation. Proc. Natl Acad. Sci. USA 110, 11746-11750 (2013).
- Pajunoja, A. et al. Phase state of ambient aerosol linked with water uptake and chemical aging in the southeastern US. Atmos. Chem. Phys. 16, 11163-11176 (2016).
- Fu, Y. et al. Impact of cloud process in the mixing state and microphysical properties of soot particles: implications in light absorption enhancement. J. Geophys. Res. 127, e2022JD037169 (2022).
- Wu, Y. et al. Light absorption enhancement of black carbon aerosol constrained by particle morphology. Environ. Sci. Technol. 52, 6912-6919 (2018).
- Yuan, Q. et al. Evidence for large amounts of brown carbonaceous tarballs in the Himalayan atmosphere. Environ. Sci. Technol. Lett. 8, 16-23 (2021).
- Hoffer, A., Tóth, A., Nyirő-Kósa, I., Pósfai, M. & Gelencsér, A. Light absorption properties of laboratory-generated tar ball particles. Atmos. Chem. Phys. 16, 239-246 (2016).
- Jimenez, J. L. et al. Evolution of organic aerosols in the atmosphere. Science 326, 1525-1529 (2009).
- Fierce, L., Bond, T. C., Bauer, S. E., Mena, F. & Riemer, N. Black carbon absorption at the global scale is affected by particle-scale diversity in composition. Nat. Commun. 7, 12361 (2016).
- Peng, J. et al. Markedly enhanced absorption and direct radiative forcing of black carbon under polluted urban environments. Proc. Natl Acad. Sci. USA 113, 4266-4267 (2016).
- Farias, T. L., Köylü, Ü. Ö. & Carvalho, M. G. Range of validity of the Rayleigh-Debye-Gans theory for optics of fractal aggregates. Appl. Opt. 35, 6560-6567, (1996).
- Kelesidis, G. A., Neubauer, D., Fan, L. S., Lohmann, U. & Pratsinis, S. E. Enhanced light absorption and radiative forcing by black carbon agglomerates. Environ. Sci. Technol. 56, 8610-8618 (2022).
- Draine, B. T. & Flatau, P. J. Discrete-dipole approximation for scattering calculations. J. Opt. Soc. Am. A 11, 1491-1499, (1994).
- Liu, C., Chung, C. E., Yin, Y. & Schnaiter, M. The absorption Ångström exponent of black carbon: from numerical aspects. Atmos. Chem. Phys. 18, 6259-6273 (2018).
- Zaveri, R. A., Easter, R. C., Fast, J. D. & Peters, L. K. Model for simulating aerosol interactions and chemistry (MOSAIC). J. Geophys. Res. 113 https://doi.org/10.1029/2007JD008782 (2008).
- Curtis, J. H., Riemer, N. & West, M. A single-column particleresolved model for simulating the vertical distribution of aerosol mixing state: WRF-PartMC-MOSAIC-SCM v1.0. Geosci. Model Dev. 10, 4057-4079 (2017).
- Liu, X. et al. Toward a minimal representation of aerosols in climate models: description and evaluation in the Community Atmosphere Model CAM5. Geosci. Model Dev. 5, 709-739 (2012).
- Liu, X. et al. Description and evaluation of a new four-mode version of the Modal Aerosol Module (MAM4) within version 5.3 of the Community Atmosphere Model. Geosci. Model Dev. 9, 505-522 (2016).
- Collow, A. B. et al. Benchmarking GOCART-2G in the Goddard Earth Observing System (GEOS). Geosci. Model Dev. Discuss. 2023, 1-47 (2023).
- Matsui, H., Koike, M., Kondo, Y., Fast, J. D. & Takigawa, M. Development of an aerosol microphysical module: aerosol twodimensional bin module for formation and aging simulation (ATRAS). Atmos. Chem. Phys. 14, 10315-10331 (2014).
- Kaiser, J. C. et al. The MESSy aerosol submodel MADE3 (v2.0b): description and a box model test. Geosci. Model Dev. 7, 1137-1157 (2014).
- Grandey, B. S. et al. Effective radiative forcing in the aerosol-climate model CAM5.3-MARC-ARG. Atmos. Chem. Phys. 18, 15783-15810 (2018).
- Chen, G. et al. An aerosol optical module with observationconstrained black carbon properties for global climate models. J. Adv. Model Earth Syst. 15 https://doi.org/10.1029/ 2022 ms 003501 (2023).
- Andersson, E. & Kahnert, M. Coupling aerosol optics to the MATCH (v5.5.0) chemical transport model and the SALSA (v1) aerosol microphysics module. Geosci. Model Dev. 9, 1803-1826 (2016).
- Kahnert, M. & Kanngießer, F. Modelling optical properties of atmospheric black carbon aerosols. J. Quant. Spectrosc. Radiat. Transf. 244, 106849 (2020).
- Chakrabarty, R. K. & Heinson, W. R. Scaling laws for light absorption enhancement due to nonrefractory coating of atmospheric black carbon aerosol. Phys. Rev. Lett. 121, 218701 (2018).
- Zhang, X., Mao, M., Yin, Y. & Tang, S. The absorption Ångstrom exponent of black carbon with brown coatings: effects of aerosol microphysics and parameterization. Atmos. Chem. Phys. 20, 9701-9711 (2020).
- Cappa, C. D. et al. Light absorption by ambient black and brown carbon and its dependence on black carbon coating state for two California, USA, cities in winter and summer. J. Geophys. Res. 124, 1550-1577 (2019).
- Liu, S. et al. Enhanced light absorption by mixed source black and brown carbon particles in UK winter. Nat. Commun. 6, 8435 (2015).
- Radney, J. G. et al. Dependence of soot optical properties on particle morphology: measurements and model comparisons. Environ. Sci. Technol. 48, 3169-3176 (2014).
- Moffet, R. C. & Prather, K. A. In-situ measurements of the mixing state and optical properties of soot with implications for radiative forcing estimates. Proc. Natl Acad. Sci. USA 106, 11872-11877 (2009).
- Schnaiter, M. et al. Absorption amplification of black carbon internally mixed with secondary organic aerosol. J. Geophys. Res. 110, D19204 (2005).
- Luo, J. et al. Optical modeling of black carbon with different coating materials: the effect of coating configurations. J. Geophys. Res. 124, 13230-13253 (2019).
- Zeng, L. et al. Overestimation of black carbon light absorption due to mixing state heterogeneity. npj Clim. Atmos. Sci. 7 https://doi.org/ 10.1038/s41612-023-00535-8 (2024).
- Fard, M. M., Krieger, U. K. & Peter, T. Shortwave radiative impact of liquid-liquid phase separation in brown carbon aerosols. Atmos. Chem. Phys. 18, 13511-13530 (2018).
- Huang, X. F. et al. Microphysical complexity of black carbon particles restricts their warming potential. One Earth https://doi.org/10.1016/ j.oneear.2023.12.004 (2023).
- Lohmann, U. et al. Future warming exacerbated by aged-soot effect on cloud formation. Nat. Geosci. 13, 674-680 (2020).
- Christensen, M. W. et al. Opportunistic experiments to constrain aerosol effective radiative forcing. Atmos. Chem. Phys. 22, 641-674 (2022).
- Myhre, G. et al. Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations. Atmos. Chem. Phys. 13, 1853-1877 (2013).
- Thornhill, G. D. et al. Effective radiative forcing from emissions of reactive gases and aerosols-a multi-model comparison. Atmos. Chem. Phys. 21, 853-874 (2021).
- Wang, X. et al. Exploiting simultaneous observational constraints on mass and absorption to estimate the global direct radiative forcing of black carbon and brown carbon. Atmos. Chem. Phys. 14, 10989-11010 (2014).
- Samset, B. H. et al. Modelled black carbon radiative forcing and atmospheric lifetime in AeroCom Phase II constrained by aircraft observations. Atmos. Chem. Phys. 14, 12465-12477 (2014).
- Kipling, Z. et al. Constraints on aerosol processes in climate models from vertically-resolved aircraft observations of black carbon. Atmos. Chem. Phys. 13, 5969-5986 (2013).
- Matsui, H., Hamilton, D. S. & Mahowald, N. M. Black carbon radiative effects highly sensitive to emitted particle size when resolving mixing-state diversity. Nat. Commun. 9, 3446 (2018).
- Ramanathan, V. & Carmichael, G. Global and regional climate changes due to black carbon. Nat. Geosci. 1, 221-227 (2008).
- Feng, Y., Ramanathan, V. & Kotamarthi, V. R. Brown carbon: a significant atmospheric absorber of solar radiation? Atmos. Chem. Phys. 13, 8607-8621 (2013).
- Wang, R. et al. Estimation of global black carbon direct radiative forcing and its uncertainty constrained by observations. J. Geophys. Res. 121, 5948-5971 (2016).
- Saleh, R. et al. Contribution of brown carbon and lensing to the direct radiative effect of carbonaceous aerosols from biomass and biofuel burning emissions. J. Geophys. Res. 120, 2015JD023697 (2015).
- Lin, G., Sillman, S., Penner, J. E. & Ito, A. Global modeling of SOA: the use of different mechanisms for aqueous-phase formation. Atmos. Chem. Phys. 14, 5451-5475 (2014).
- Hammer, M. S. et al. Interpreting the ultraviolet aerosol index observed with the OMI satellite instrument to understand absorption by organic aerosols: implications for atmospheric oxidation and direct radiative effects. Atmos. Chem. Phys. 16, 2507-2523 (2016).
- Drugé, T. et al. Modeling radiative and climatic effects of brown carbon aerosols with the ARPEGE-Climat global climate model. Atmos. Chem. Phys. 22, 12167-12205 (2022).
- Bellouin, N. et al. Bounding global aerosol radiative forcing of climate change. Rev. Geophys. 58, e2019RG000660 (2020).
- Schill, G. P. et al. The contribution of black carbon to global ice nucleating particle concentrations relevant to mixed-phase clouds. Proc. Natl. Acad. Sci. USA 117, 202001674 (2020).
- Jesús et al. Is black carbon an unimportant ice-nucleating particle in mixed-phase clouds? J. Geophys. Res. 123, 4273-4283 (2018).
- Levin, E. J. T. et al. Ice-nucleating particle emissions from biomass combustion and the potential importance of soot aerosol. J. Geophys. Res. 121, 5888-5903 (2016).
- Friedman, B. et al. Ice nucleation and droplet formation by bare and coated soot particles. J. Geophys. Res. 116, D17203 (2011).
- Kupiszewski, P. et al. Ice residual properties in mixed-phase clouds at the high-alpine Jungfraujoch site. J. Geophys. Res. 121, 12,343-312,362 (2016).
- Kulkarni, G. et al. Ice nucleation activity of diesel soot particles at cirrus relevant temperature conditions: effects of hydration, secondary organics coating, soot morphology, and coagulation. Geophys. Res. Lett. 43, 3580-3588 (2016).
- Cozic, J. et al. Black carbon enrichment in atmospheric ice particle residuals observed in lower tropospheric mixed phase clouds. J. Geophys. Res. 113, D15209 (2008).
- Twohy, C. H., Anderson, J. R. & Crozier, P. A. Nitrogenated organic aerosols as cloud condensation nuclei. Geophy. Res. Lett. 32 https://doi.org/10.1029/2005GL023605 (2005).
- Koch, D. et al. Soot microphysical effects on liquid clouds, a multimodel investigation. Atmos. Chem. Phys. 11, 1051-1064 (2011).
- McNeill, V. F., Sareen, N. & Schwier, A. Topics in Current Chemistry Ch. 404, 1-59 (Springer, 2013).
- Wang, J. et al. Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility. Atmos. Chem. Phys. 19, 941-954 (2019).
- Wokosin, K. A., Schell, E. L. & Faust, J. A. Surfactants, films, and coatings on atmospheric aerosol particles: a review. Environ. Sci. Atmos. https://doi.org/10.1039/D2EA00003B (2022).
- Knopf, D. A. et al. Microspectroscopic imaging and characterization of individually identified ice nucleating particles from a case field study. J. Geophys. Res. 119, 2014JD021866 (2014).
- Dong, Z. et al. Variability in individual particle structure and mixing states between the glacier-snowpack and atmosphere in the northeastern Tibetan Plateau. Cryosphere 12, 3877-3890 (2018).
- He, C. et al. Impact of grain shape and multiple black carbon internal mixing on snow albedo: parameterization and radiative effect analysis. J. Geophys. Res. 123, 1253-1268 (2018).
- Johansson, K. O., Head-Gordon, M. P., Schrader, P. E., Wilson, K. R. & Michelsen, H. A. Resonance-stabilized hydrocarbon-radical chain reactions may explain soot inception and growth. Science 361, 997-1000 (2018).
- Ching, J., Kajino, M. & Matsui, H. Resolving aerosol mixing state increases accuracy of black carbon respiratory deposition estimates. One Earth 3, 763-776 (2020).
- Zheng, Z. et al. Estimating submicron aerosol mixing state at the global scale with machine learning and earth system modeling. Earth Space Sci. 8 https://doi.org/10.1029/2020ea001500 (2021).
- Luo, J., Zhang, Y., Wang, F., Wang, J. & Zhang, Q. Applying machine learning to estimate the optical properties of black carbon fractal aggregates. J. Quant. Spectrosc. Radiat. Transf. 215, 1-8 (2018).
- Lamb, K. D. & Gentine, P. Zero-shot learning of aerosol optical properties with graph neural networks. Sci. Rep. 13, 18777 (2023).
- Wang, X., Bi, L., Han, W. & Zhang, X. Single-scattering properties of encapsulated fractal black carbon particles computed using the invariant imbedding T-matrix method and deep learning approaches. J. Geophys. Res. 128, e2023JD039568 (2023).
- Shen, W. et al. Improving BC mixing state and CCN activity representation with machine learning in the Community Atmosphere Model Version 6 (CAM6). J. Adv. Model Earth Syst. 16 https://doi. org/10.1029/2023ms003889 (2024).
- Gorkowski, K., Donahue, N. M. & Sullivan, R. C. Aerosol optical tweezers constrain the morphology evolution of liquid-liquid phaseseparated atmospheric particles. Chem 6, 204-220 (2020).
- Dazzi, A. & Prater, C. B. AFM-IR: technology and applications in nanoscale infrared spectroscopy and chemical imaging. Chem. Rev. 117, 5146-5173 (2017).
- Yuan, Q. et al. Mixing state and fractal dimension of soot particles at a remote site in the Southeastern Tibetan plateau. Environ. Sci. Technol. 53, 8227-8234 (2019).
- Raatikainen, T. et al. Size-selected black carbon mass distributions and mixing state in polluted and clean environments of northern India. Atmos. Chem. Phys. 17, 371-383 (2017).
- Fraund, M. et al. Elemental mixing state of aerosol particles collected in Central Amazonia during GoAmazon2014/15. Atmosphere 8, 173 (2017).
- Ljungman, P. L. S. et al. Long-term exposure to particulate air pollution, black carbon, and their source components in relation to ischemic heart disease and stroke. Environ. Health Perspect. 127, 107012 (2019).
- Zhu, S., Zhang, H., Zhou, C., Wei, X. & Liu, Y. Optical properties of mixed black and brown carbon aerosols. Opt. Express 30, 33588-33602 (2022).
الشكر والتقدير
مساهمات المؤلفين
المصالح المتنافسة
معلومات إضافية
© المؤلفون 2024
المختبر الرئيسي لبيانات الجيولوجيا الكبيرة والموارد العميقة في مقاطعة تشجيانغ، قسم علوم الغلاف الجوي، كلية علوم الأرض، جامعة تشجيانغ، هانغتشو 310027، الصين. قسم المناخ والأرصاد الجوية وعلوم الغلاف الجوي، جامعة إلينوي في أوربانا-شامبين، أوربانا، إلينوي، الولايات المتحدة الأمريكية. كلية العلوم، جامعة جيلينغ الصينية، هانغتشو 310018، الصين. قسم أبحاث نمذجة الغلاف الجوي والمحيط ونظام الأرض، معهد الأرصاد الجوية، تسوكوبا، اليابان. كلية الجغرافيا وعلوم الأرض والبيئة، جامعة برمنغهام، برمنغهام B15 2TT، المملكة المتحدة. كلية العلوم البيئية والتعايش، جامعة كوماتسو الحكومية، كوماتسو 862-8502، اليابان. قسم علوم الأرض والبيئة، جامعة مانشستر، مانشستر، المملكة المتحدة. قسم الكيمياء، جامعة بوردو، ويست لافاييت، IN 47907، الولايات المتحدة الأمريكية. قسم علوم الأرض والغلاف الجوي والعلوم الكوكبية، جامعة بوردو، ويست لافاييت، IN 47907، الولايات المتحدة الأمريكية. البريد الإلكتروني: liweijun@zju.edu.cn; alaskin@purdue.edu
DOI: https://doi.org/10.1038/s41612-024-00610-8
Publication Date: 2024-03-08
Microphysical properties of atmospheric soot and organic particles: measurements, modeling, and impacts
Abstract
Atmospheric soot and organic particles from fossil fuel combustion and biomass burning modify Earth’s climate through their interactions with solar radiation and through modifications of cloud properties by acting as cloud condensation nuclei and ice nucleating particles. Recent advancements in understanding their individual properties and microscopic composition have led to heightened interest in their microphysical properties. This review article provides an overview of current advanced microscopic measurements and offers insights into future avenues for studying microphysical properties of these particles. To quantify soot morphology and ageing, fractal dimension
organic aerosols remain focal research points due to their significant roles and their potential contributions to uncertainty in the atmospheric climate system
mixtures also exhibit significant light absorbing properties, which have been collectively termed as brown carbon ( BrC
What underlines the primary ageing mechanisms of particle ensembles composed of soot and organic components? How do atmospheric ageing processes alter the mixing structure of the soot-organic particles in polluted air?
How does atmospheric water affect the phase and mixing structure of the soot-organic particle mixtures? To what extent do inorganic constituents impact the phase and mixing characteristics of particles?
How does mixing structures of soot and organics transform the morphology and optical properties of particles, influencing their impact on climate dynamics and human health?
Methodologies for the particle-resolved observations of soot-organic mixtures

conditions and exposure to the electron beam irradiation (as exemplified by the S-rich component in Fig. 2c), especially in the case of mixed organic and inorganic components
Microphysical properties of soot particles

monomer, and
assumed that the type of combustion source soot particles exerts discernible impacts on soot particles’ fractal morphology. Recent studies have underscored the differences in morphological parameters of freshly emitted soot particles originating from different combustion sources, in particular for finer and coarser sizes of soot particles

derived from NanoSIMS showing
Microphysical properties of organic particles
mixing structure and phase state. The latter describes if the particles are liquid, viscous, semi-solids, and amorphous glassy solids. The mixing structure of organic aerosols pertains to how organic matter is internally mixed with inorganic components (as portrayed in Figs. 3 and 4a, b).

(SEM) collected in suburban air. e Size distributions of tar ball particles collected in wildfires

the SOA-coated and SOA-homogeneous mixing structures
Atmospheric effects of particles composed of soot and organic mixtures

refs.
properties. Specifically, the scattering cross sections of these particles can be up to 50% larger compared to those of homogenously mixed particles while their absorption cross sections may be reduced by up to
Impacts on radiative forcing
Impacts on clouds


clouds
Other possible effects
intricate relationship between deposits of the light-absorbing aerosols (e.g., soot, BrC , and mineral dust) in the snow albedo reduction. Snow strongly reflects sunlight, while the reflection extent depends strongly on factors such as the snow grain size and morphology and the mixing state of soot with the snow matrix. Although few reports considered mixing structures of soot particles in the glacier-snowpack atmosphere
Summary and future perspectives
absorption of soot and BrC. (3) Beyond the microphysical property of lightabsorbing particles, their chemical composition, particularly BrC undergoes continuous changes due to atmospheric ageing or variations arising from different formation pathways and sources. (4) Improved optical models of realistic mixing structures are required to accurately predict the optical properties of aged soot and organic particles, particularly those exhibiting complex mixing structures and morphologies. The implementation of these advanced techniques can significantly decrease the computation time and facilitate the creation of extensive optical database for climate models
Published online: 08 March 2024
References
- Riemer, N., Ault, A. P., West, M., Craig, R. L. & Curtis, J. H. Aerosol mixing state: measurements, modeling, and impacts. Rev. Geophys. 57 https://doi.org/10.1029/2018RG000615 (2019).
- Li, W. et al. A review of single aerosol particle studies in the atmosphere of East Asia: morphology, mixing state, source, and heterogeneous reactions. J. Clean. Prod. 112, 1330-1349 (2016).
- Bond, T. C. et al. Bounding the role of black carbon in the climate system: a scientific assessment. J. Geophys. Res. 118, 5380-5552 (2013).
- Li, J. et al. Scattering and absorbing aerosols in the climate system. Nat. Rev. Earth Environ. https://doi.org/10.1038/s43017-022-00296-7 (2022).
- Coppola, A. I. et al. The black carbon cycle and its role in the Earth system. Nat. Rev. Earth Environ. https://doi.org/10.1038/s43017-022-00316-6 (2022).
- Laskin, A., Laskin, J. & Nizkorodov, S. A. Chemistry of atmospheric brown carbon. Chem. Rev. 115, 4355-4382 (2015).
- Wang, Q. et al. Review of brown carbon aerosols in China: pollution level, optical properties, and emissions. J. Geophys. Res. 127, e2021JD035473 (2022).
- Yue, S. et al. Brown carbon from biomass burning imposes strong circum-Arctic warming. One Earth 5, 293-304 (2022).
- Freedman, M. A. Liquid-liquid phase separation in supermicrometer and submicrometer aerosol particles. Acc. Chem. Res. 53, 1102-1110 (2020).
- Laskin, A., Moffet, R. C. & Gilles, M. K. Chemical imaging of atmospheric particles. Acc. Chem. Res. 52, 3419-3431 (2019).
- Reid, J. P. et al. The viscosity of atmospherically relevant organic particles. Nat. Commun. 9, 956 (2018).
- Shrivastava, M. et al. Recent advances in understanding secondary organic aerosol: implications for global climate forcing. Rev. Geophys. 55, 509-559 (2017).
- Wang, Y. et al. Nonlinear enhancement of radiative absorption by black carbon in response to particle mixing structure. Geophys. Res. Lett. 48, e2021GL096437 (2021).
- Fierce, L. et al. Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition. Proc. Natl Acad. Sci. USA 117, 5196-5203 (2020).
- Wang, J. et al. Unified theoretical framework for black carbon mixing state allows greater accuracy of climate effect estimation. Nat. Commun. 14, 2703 (2023).
- Kanakidou, M. et al. Organic aerosol and global climate modelling: a review. Atmos. Chem. Phys. 5, 1053-1123 (2005).
- Chen, Q. et al. Mass spectral characterization of submicron biogenic organic particles in the Amazon Basin. Geophys. Res. Lett. 36 https://doi.org/10.1029/2009gl039880 (2009).
- Petzold, A. et al. Recommendations for reporting “black carbon” measurements. Atmos. Chem. Phys. 13, 8365-8379 (2013).
- Buseck, P. R., Adachi, K., Gelencsér, A., Tompa, É. & Pósfai, M. Nssoot: a material-based term for strongly light-absorbing carbonaceous particles. Aerosp. Sci. Technol. 48, 777-788 (2014).
- IPCC. in Climate Change 2021: The Physical Science Basis (eds Masson-Delmotte, V. et al.) 817-922 (Cambridge University Press, 2022).
- Cao, J.-J. et al. Black carbon relationships with emissions and meteorology in Xi’an, China. Atmos. Res. 94, 194-202 (2009).
- Metcalf, A. R. et al. Black carbon aerosol over the Los Angeles Basin during CalNex. J. Geophys. Res. 117, D00V13 (2012).
- Sharma, S. Long-term trends of the black carbon concentrations in the Canadian Arctic. J. Geophys. Res. 109 https://doi.org/10.1029/ 2003jd004331 (2004).
- Dai, M. et al. Long-term variation and source apportionment of black carbon at Mt. Waliguan, China. J. Geophys. Res. 126, e2021JD035273 (2021).
- Cappa, C. D. et al. Radiative absorption enhancements due to the mixing state of atmospheric black carbon. Science 337, 1078-1081 (2012).
- Adachi, K., Chung, S. H. & Buseck, P. R. Shapes of soot aerosol particles and implications for their effects on climate. J. Geophys. Res. 115 https://doi.org/10.1029/2009JD012868 (2010).
- Jacobson, M. Z. Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols. Nature 409, 695-697 (2001).
- Poschl, U. Atmospheric aerosols: composition, transformation, climate and health effects. Angew. Chem. Int. Ed. 44, 7520-7540 (2005).
- Jo, D. S., Park, R. J., Lee, S., Kim, S. W. & Zhang, X. A global simulation of brown carbon: implications for photochemistry and direct radiative effect. Atmos. Chem. Phys. 16, 3413-3432 (2016).
- Chakrabarty, R. K. et al. Shortwave absorption by wildfire smoke dominated by dark brown carbon. Nat. Geosci. 16, 683-688 (2023).
- Corbin, J. C. et al. Infrared-absorbing carbonaceous tar can dominate light absorption by marine-engine exhaust. npj Clim. Atmos. Sci. 2 https://doi.org/10.1038/s41612-019-0069-5 (2019).
- Ault, A. P. & Axson, J. L. Atmospheric aerosol chemistry: spectroscopic and microscopic advances. Anal. Chem. 89, 430-452 (2017).
- Shao, L. et al. A review of atmospheric individual particle analyses: methodologies and applications in environmental research. Gondwana Res. 110, 347-369 (2022).
- Liu, C., Xu, X., Yin, Y., Schnaiter, M. & Yung, Y. L. Black carbon aggregates: a database for optical properties. J. Quant. Spectrosc. Radiat. Transf. 222-223, 170-179 (2019).
- Smith, A. J. A. & Grainger, R. G. Simplifying the calculation of light scattering properties for black carbon fractal aggregates. Atmos. Chem. Phys. 14, 7825-7836 (2014).
- Romshoo, B. et al. Optical properties of coated black carbon aggregates: numerical simulations, radiative forcing estimates, and size-resolved parameterization scheme. Atmos. Chem. Phys. 21, 12989-13010 (2021).
- Mackowski, D. W. & Mishchenko, M. I. A multiple sphere T-matrix Fortran code for use on parallel computer clusters. J. Quant. Spectrosc. Radiat. Transf. 112, 2182-2192 (2011).
- Wang, Y. et al. Constructing shapes and mixing structures of black carbon particles with applications to optical calculations. J. Geophys. Res. 126, e2021JD034620 (2021).
- Hu, K. et al. Measurements of the diversity of shape and mixing state for ambient black carbon particles. Geophys. Res. Lett. 48, e2021GL094522 (2021).
- Slowik, J. G. et al. Measurements of morphology changes of fractal soot particles using coating and denuding experiments: implications for optical absorption and atmospheric lifetime. Aerosp. Sci. Technol. 41, 734-750 (2007).
- Schnitzler, E. G., Dutt, A., Charbonneau, A. M., Olfert, J. S. & Jäger, W. Soot aggregate restructuring due to coatings of secondary organic aerosol derived from aromatic precursors. Environ. Sci. Technol. 48, 14309-14316 (2014).
- Sedlacek, A. J. III, Lewis, E. R., Kleinman, L., Xu, J. & Zhang, Q. Determination of and evidence for non-core-shell structure of particles containing black carbon using the single-particle soot photometer (SP2). Geophys. Res. Lett. 39, L06802 (2012).
- Zhang, Y. et al. Extremely low-volatility organic coating leads to underestimation of black carbon climate impact. One Earth 6, 158-166 (2023).
- Naseri, A., Sipkens, T. A., Rogak, S. N. & Olfert, J. S. An improved inversion method for determining two-dimensional mass distributions of non-refractory materials on refractory black carbon. Aerosp. Sci. Technol. 55, 104-118 (2020).
- Liu, D. et al. Black-carbon absorption enhancement in the atmosphere determined by particle mixing state. Nat. Geosci. 10, 184-188 (2017).
- Zhai, J. et al. Absorption enhancement of black carbon aerosols constrained by mixing-state heterogeneity. Environ. Sci. Technol. 56, 1586-1593 (2022).
- Schwarz, J. P. et al. Coatings and their enhancement of black carbon light absorption in the tropical atmosphere. J. Geophys. Res. 113 https://doi.org/10.1029/2007jd009042 (2008).
- Pratt, K. A. & Prather, K. A. Mass spectrometry of atmospheric aerosols -recent developments and applications. Part II: on-line mass spectrometry techniques. Mass Spectrom. Rev. 31, 17-48 (2012).
- Zelenyuk, A. & Imre, D. Beyond single particle mass spectrometry: multidimensional characterisation of individual aerosol particles. Annu. Rev. Phys. Chem. 28, 309-358 (2009).
- Canagaratna, M. R. et al. Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer. Mass Spectrom. Rev. 26, 185-222 (2007).
- Virtanen, A. et al. An amorphous solid state of biogenic secondary organic aerosol particles. Nature 467, 824-827 (2010).
- China, S., Mazzoleni, C., Gorkowski, K., Aiken, A. C. & Dubey, M. K. Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles. Nat. Commun. 4, 2122 (2013).
- Shi, Z. B., Zhang, D. Z., Ji, H. Z., Hasegawa, S. & Hayashi, M. Modification of soot by volatile species in an urban atmosphere. Sci. Total Environ. 389, 195-201 (2008).
- Geng, H., Ryu, J. Y., Maskey, S., Jung, H. J. & Ro, C. U. Characterisation of individual aerosol particles collected during a haze episode in Incheon, Korea using the quantitative ED-EPMA technique. Atmos. Chem. Phys. 11, 1327-1337 (2011).
- Ebert, M., Weinbruch, S., Hoffmann, P. & Ortner, H. M. The chemical composition and complex refractive index of rural and urban influenced aerosols determined by individual particle analysis. Atmos. Environ. 38, 6531-6545 (2004).
- Wang, Y. et al. Fractal dimensions and mixing structures of soot particles during atmospheric processing. Environ. Sci. Tech. Let. 4, 487-493 (2017).
- Ueda, S. et al. Morphological features and mixing states of sootcontaining particles in the marine boundary layer over the Indian and Southern oceans. Atmos. Chem. Phys. 18, 9207-9224 (2018).
- Li, W. et al. A conceptual framework for mixing structures in individual aerosol particles. J. Geophys. Res. 121, 13,784-713,798 (2016).
- Pöhlker, C. et al. Biogenic potassium salt particles as seeds for secondary organic aerosol in the Amazon. Science 337, 1075-1078 (2012).
- Li, W. et al. Microscopic evidence for phase separation of organic species and inorganic salts in fine ambient aerosol particles. Environ. Sci. Technol. 55, 2234-2242 (2021).
- O’Brien, R. E. et al. Liquid-liquid phase separation in aerosol particles: imaging at the nanometer scale. Environ. Sci. Technol. 49, 4995-5002 (2015).
- Laskina, O., Young, M. A., Kleiber, P. D. & Grassian, V. H. Infrared extinction spectroscopy and micro-Raman spectroscopy of select components of mineral dust mixed with organic compounds. J. Geophys. Res. 118, 6593-6606 (2013).
- Takahama, S., Liu, S. & Russell, L. M. Coatings and clusters of carboxylic acids in carbon-containing atmospheric particles from spectromicroscopy and their implications for cloud-nucleating and optical properties. J. Geophys. Res. 115 https://doi.org/10.1029/ 2009jd012622 (2010).
- Wang, M., Zheng, N., Zhao, D., Shang, J. & Zhu, T. Using microRaman spectroscopy to investigate chemical composition, mixing states, and heterogeneous reactions of individual atmospheric particles. Environ. Sci. Technol. 55, 10243-10254 (2021).
- Li, X., Gupta, D., Lee, J., Park, G. & Ro, C.-U. Real-time investigation of chemical compositions and hygroscopic properties of aerosols generated from NaCl and malonic acid mixture solutions using in situ Raman microspectrometry. Environ. Sci. Technol. 51, 263-270 (2017).
- Li, W. et al. Organic coating reduces hygroscopic growth of phaseseparated aerosol particles. Environ. Sci. Technol. 55, 16339-16346 (2021).
- Ott, E. J. E., Tackman, E. C. & Freedman, M. A. Effects of sucrose on phase transitions of organic/inorganic aerosols. ACS Earth Space Chem. 4, 591-601 (2020).
- Kucinski, T. M., Dawson, J. N. & Freedman, M. A. Size-dependent liquid-liquid phase separation in atmospherically relevant complex systems. J. Phys. Chem. Lett. 10, 6915-6920 (2019).
- Zhang, J. et al. Liquid-liquid phase separation reduces radiative absorption by aged black carbon aerosols. Commun. Earth Environ. 3, 128 (2022).
- Veghte, D. P., Altaf, M. B. & Freedman, M. A. Size dependence of the structure of organic aerosol. J. Am. Chem. Soc. 135, 16046-16049 (2013).
- Pang, Y. et al. Quantifying the fractal dimension and morphology of individual atmospheric soot aggregates. J. Geophys. Res. 127, e2021JD036055 (2022).
- Chakrabarty, R. K., Moosmüller, H., Arnott, W. P., Garro, M. A. & Walker, J. Structural and fractal properties of particles emitted from spark ignition engines. Environ. Sci. Technol. 40, 6647-6654 (2006).
- Brasil, A. M., Farias, T. L. & Carvalho, M. G. A recipe for image characterization of fractal-like aggregates. J. Aerosol Sci. 30, 1379-1389 (1999).
- Adachi, K., Chung, S. H., Friedrich, H. & Buseck, P. R. Fractal parameters of individual soot particles determined using electron tomography: implications for optical properties. J. Geophys. Res. 112, D14202 (2007).
- Sipkens, T. A. et al. Overview of methods to characterize the mass, size, and morphology of soot. J. Aerosol Sci. 173, 106211 (2023).
- Haffner-Staton, E., Avanzini, L., La Rocca, A., Pfau, S. A. & Cairns, A. Automated particle recognition for engine soot nanoparticles. J. Microsc. 288, 28-39 (2022).
- Pang, Y. et al. Morphology and fractal dimension of size-resolved soot particles emitted from combustion sources. J. Geophys. Res. 128, e2022JD037711 (2023).
- Niu, H., Shao, L. & Zhang, D. Soot particles at an elevated site in eastern China during the passage of a strong cyclone. Sci. Total Environ. 430, 217-222 (2012).
- China, S., Salvadori, N. & Mazzoleni, C. Effect of traffic and driving characteristics on morphology of atmospheric soot particles at freeway on-ramps. Environ. Sci. Technol. 48, 3128-3135 (2014).
- Chen, C. et al. An unexpected restructuring of combustion soot aggregates by subnanometer coatings of polycyclic aromatic hydrocarbons. Geophys. Res. Lett. 43, 11,080-011,088 (2016).
- Zhang, J. et al. Structural collapse and coating composition changes of soot particles during long-range transport. J. Geophys. Res. 128, e2023JD038871 (2023).
- Enekwizu, O. Y., Hasani, A. & Khalizov, A. F. Vapor condensation and coating evaporation are both responsible for soot aggregate restructuring. Environ. Sci. Technol. 55, 8622-8630 (2021).
- Corbin, J. C., Modini, R. L. & Gysel-Beer, M. Mechanisms of sootaggregate restructuring and compaction. Aerosol Sci. Technol. 57, 89-111 (2023).
- Zhang, R. Y. et al. Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing. Proc. Natl Acad. Sci. USA 105, 10291-10296 (2008).
- Ma, X., Zangmeister, C. D., Gigault, J., Mulholland, G. W. & Zachariah, M. R. Soot aggregate restructuring during water processing. J. Aerosol Sci. 66, 209-219 (2013).
- Bhandari, J. et al. Extensive soot compaction by cloud processing from laboratory and field observations. Sci. Rep. 9, 11824 (2019).
- Chen, X . et al. Quantifying evolution of soot mixing state from transboundary transport of biomass burning emissions. IScience 26, 108125 (2023).
- Wu, Z. et al. Aerosol liquid water driven by anthropogenic inorganic salts: implying its key role in haze formation over the North China Plain. Environ. Sci. Technol. Lett. 5, 160-166 (2018).
- Peckhaus, A., Grass, S., Treuel, L. & Zellner, R. Deliquescence and efflorescence behavior of ternary inorganic/Organic/water aerosol particles. J. Phys. Chem. A 116, 6199-6210 (2012).
- Freney, E. J., Adachi, K. & Buseck, P. R. Internally mixed atmospheric aerosol particles: hygroscopic growth and light scattering. J. Geophys. Res. 115 https://doi.org/10.1029/ 2009jd013558 (2010).
- Kuang, Y. et al. Deliquescent phenomena of ambient aerosols on the North China Plain. Geophys. Res. Lett. 43, 8744-8750 (2016).
- Posfai, M. et al. Atmospheric tar balls: particles from biomass and biofuel burning. J. Geophys. Res. 109 https://doi.org/10.1029/ 2003JD004169 (2004).
- Wang, B. et al. Airborne soil organic particles generated by precipitation. Nat. Geosci. 9, 433-437 (2016).
- Sedlacek lii, A. J. et al. Formation and evolution of tar balls from northwestern US wildfires. Atmos. Chem. Phys. 18, 11289-11301 (2018).
- Adachi, K. et al. Spherical tarball particles form through rapid chemical and physical changes of organic matter in biomassburning smoke. Proc. Natl Acad. Sci. USA 116, 19336-19341 (2019).
- Liu, L. et al. Persistent residential burning-related primary organic particles during wintertime hazes in North China: insights into their aging and optical changes. Atmos. Chem. Phys. 21, 2251-2265 (2021).
- Li, C. et al. Dynamic changes in optical and chemical properties of tar ball aerosols by atmospheric photochemical aging. Atmos. Chem. Phys. 19, 139-163 (2019).
- Corbin, J. C. & Gysel-Beer, M. Detection of tar brown carbon with a single particle soot photometer (SP2). Atmos. Chem. Phys. 19, 15673-15690 (2019).
- You, Y. et al. Images reveal that atmospheric particles can undergo liquid-liquid phase separations. Proc. Natl Acad. Sci. USA 109, 13188-13193 (2012).
- Kirpes, R. M. et al. Solid organic-coated ammonium sulfate particles at high relative humidity in the summertime Arctic atmosphere. Proc. Natl Acad. Sci. USA 119, e2104496119 (2022).
- Shiraiwa, M. et al. Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation. Proc. Natl Acad. Sci. USA 110, 11746-11750 (2013).
- Pajunoja, A. et al. Phase state of ambient aerosol linked with water uptake and chemical aging in the southeastern US. Atmos. Chem. Phys. 16, 11163-11176 (2016).
- Fu, Y. et al. Impact of cloud process in the mixing state and microphysical properties of soot particles: implications in light absorption enhancement. J. Geophys. Res. 127, e2022JD037169 (2022).
- Wu, Y. et al. Light absorption enhancement of black carbon aerosol constrained by particle morphology. Environ. Sci. Technol. 52, 6912-6919 (2018).
- Yuan, Q. et al. Evidence for large amounts of brown carbonaceous tarballs in the Himalayan atmosphere. Environ. Sci. Technol. Lett. 8, 16-23 (2021).
- Hoffer, A., Tóth, A., Nyirő-Kósa, I., Pósfai, M. & Gelencsér, A. Light absorption properties of laboratory-generated tar ball particles. Atmos. Chem. Phys. 16, 239-246 (2016).
- Jimenez, J. L. et al. Evolution of organic aerosols in the atmosphere. Science 326, 1525-1529 (2009).
- Fierce, L., Bond, T. C., Bauer, S. E., Mena, F. & Riemer, N. Black carbon absorption at the global scale is affected by particle-scale diversity in composition. Nat. Commun. 7, 12361 (2016).
- Peng, J. et al. Markedly enhanced absorption and direct radiative forcing of black carbon under polluted urban environments. Proc. Natl Acad. Sci. USA 113, 4266-4267 (2016).
- Farias, T. L., Köylü, Ü. Ö. & Carvalho, M. G. Range of validity of the Rayleigh-Debye-Gans theory for optics of fractal aggregates. Appl. Opt. 35, 6560-6567, (1996).
- Kelesidis, G. A., Neubauer, D., Fan, L. S., Lohmann, U. & Pratsinis, S. E. Enhanced light absorption and radiative forcing by black carbon agglomerates. Environ. Sci. Technol. 56, 8610-8618 (2022).
- Draine, B. T. & Flatau, P. J. Discrete-dipole approximation for scattering calculations. J. Opt. Soc. Am. A 11, 1491-1499, (1994).
- Liu, C., Chung, C. E., Yin, Y. & Schnaiter, M. The absorption Ångström exponent of black carbon: from numerical aspects. Atmos. Chem. Phys. 18, 6259-6273 (2018).
- Zaveri, R. A., Easter, R. C., Fast, J. D. & Peters, L. K. Model for simulating aerosol interactions and chemistry (MOSAIC). J. Geophys. Res. 113 https://doi.org/10.1029/2007JD008782 (2008).
- Curtis, J. H., Riemer, N. & West, M. A single-column particleresolved model for simulating the vertical distribution of aerosol mixing state: WRF-PartMC-MOSAIC-SCM v1.0. Geosci. Model Dev. 10, 4057-4079 (2017).
- Liu, X. et al. Toward a minimal representation of aerosols in climate models: description and evaluation in the Community Atmosphere Model CAM5. Geosci. Model Dev. 5, 709-739 (2012).
- Liu, X. et al. Description and evaluation of a new four-mode version of the Modal Aerosol Module (MAM4) within version 5.3 of the Community Atmosphere Model. Geosci. Model Dev. 9, 505-522 (2016).
- Collow, A. B. et al. Benchmarking GOCART-2G in the Goddard Earth Observing System (GEOS). Geosci. Model Dev. Discuss. 2023, 1-47 (2023).
- Matsui, H., Koike, M., Kondo, Y., Fast, J. D. & Takigawa, M. Development of an aerosol microphysical module: aerosol twodimensional bin module for formation and aging simulation (ATRAS). Atmos. Chem. Phys. 14, 10315-10331 (2014).
- Kaiser, J. C. et al. The MESSy aerosol submodel MADE3 (v2.0b): description and a box model test. Geosci. Model Dev. 7, 1137-1157 (2014).
- Grandey, B. S. et al. Effective radiative forcing in the aerosol-climate model CAM5.3-MARC-ARG. Atmos. Chem. Phys. 18, 15783-15810 (2018).
- Chen, G. et al. An aerosol optical module with observationconstrained black carbon properties for global climate models. J. Adv. Model Earth Syst. 15 https://doi.org/10.1029/ 2022 ms 003501 (2023).
- Andersson, E. & Kahnert, M. Coupling aerosol optics to the MATCH (v5.5.0) chemical transport model and the SALSA (v1) aerosol microphysics module. Geosci. Model Dev. 9, 1803-1826 (2016).
- Kahnert, M. & Kanngießer, F. Modelling optical properties of atmospheric black carbon aerosols. J. Quant. Spectrosc. Radiat. Transf. 244, 106849 (2020).
- Chakrabarty, R. K. & Heinson, W. R. Scaling laws for light absorption enhancement due to nonrefractory coating of atmospheric black carbon aerosol. Phys. Rev. Lett. 121, 218701 (2018).
- Zhang, X., Mao, M., Yin, Y. & Tang, S. The absorption Ångstrom exponent of black carbon with brown coatings: effects of aerosol microphysics and parameterization. Atmos. Chem. Phys. 20, 9701-9711 (2020).
- Cappa, C. D. et al. Light absorption by ambient black and brown carbon and its dependence on black carbon coating state for two California, USA, cities in winter and summer. J. Geophys. Res. 124, 1550-1577 (2019).
- Liu, S. et al. Enhanced light absorption by mixed source black and brown carbon particles in UK winter. Nat. Commun. 6, 8435 (2015).
- Radney, J. G. et al. Dependence of soot optical properties on particle morphology: measurements and model comparisons. Environ. Sci. Technol. 48, 3169-3176 (2014).
- Moffet, R. C. & Prather, K. A. In-situ measurements of the mixing state and optical properties of soot with implications for radiative forcing estimates. Proc. Natl Acad. Sci. USA 106, 11872-11877 (2009).
- Schnaiter, M. et al. Absorption amplification of black carbon internally mixed with secondary organic aerosol. J. Geophys. Res. 110, D19204 (2005).
- Luo, J. et al. Optical modeling of black carbon with different coating materials: the effect of coating configurations. J. Geophys. Res. 124, 13230-13253 (2019).
- Zeng, L. et al. Overestimation of black carbon light absorption due to mixing state heterogeneity. npj Clim. Atmos. Sci. 7 https://doi.org/ 10.1038/s41612-023-00535-8 (2024).
- Fard, M. M., Krieger, U. K. & Peter, T. Shortwave radiative impact of liquid-liquid phase separation in brown carbon aerosols. Atmos. Chem. Phys. 18, 13511-13530 (2018).
- Huang, X. F. et al. Microphysical complexity of black carbon particles restricts their warming potential. One Earth https://doi.org/10.1016/ j.oneear.2023.12.004 (2023).
- Lohmann, U. et al. Future warming exacerbated by aged-soot effect on cloud formation. Nat. Geosci. 13, 674-680 (2020).
- Christensen, M. W. et al. Opportunistic experiments to constrain aerosol effective radiative forcing. Atmos. Chem. Phys. 22, 641-674 (2022).
- Myhre, G. et al. Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations. Atmos. Chem. Phys. 13, 1853-1877 (2013).
- Thornhill, G. D. et al. Effective radiative forcing from emissions of reactive gases and aerosols-a multi-model comparison. Atmos. Chem. Phys. 21, 853-874 (2021).
- Wang, X. et al. Exploiting simultaneous observational constraints on mass and absorption to estimate the global direct radiative forcing of black carbon and brown carbon. Atmos. Chem. Phys. 14, 10989-11010 (2014).
- Samset, B. H. et al. Modelled black carbon radiative forcing and atmospheric lifetime in AeroCom Phase II constrained by aircraft observations. Atmos. Chem. Phys. 14, 12465-12477 (2014).
- Kipling, Z. et al. Constraints on aerosol processes in climate models from vertically-resolved aircraft observations of black carbon. Atmos. Chem. Phys. 13, 5969-5986 (2013).
- Matsui, H., Hamilton, D. S. & Mahowald, N. M. Black carbon radiative effects highly sensitive to emitted particle size when resolving mixing-state diversity. Nat. Commun. 9, 3446 (2018).
- Ramanathan, V. & Carmichael, G. Global and regional climate changes due to black carbon. Nat. Geosci. 1, 221-227 (2008).
- Feng, Y., Ramanathan, V. & Kotamarthi, V. R. Brown carbon: a significant atmospheric absorber of solar radiation? Atmos. Chem. Phys. 13, 8607-8621 (2013).
- Wang, R. et al. Estimation of global black carbon direct radiative forcing and its uncertainty constrained by observations. J. Geophys. Res. 121, 5948-5971 (2016).
- Saleh, R. et al. Contribution of brown carbon and lensing to the direct radiative effect of carbonaceous aerosols from biomass and biofuel burning emissions. J. Geophys. Res. 120, 2015JD023697 (2015).
- Lin, G., Sillman, S., Penner, J. E. & Ito, A. Global modeling of SOA: the use of different mechanisms for aqueous-phase formation. Atmos. Chem. Phys. 14, 5451-5475 (2014).
- Hammer, M. S. et al. Interpreting the ultraviolet aerosol index observed with the OMI satellite instrument to understand absorption by organic aerosols: implications for atmospheric oxidation and direct radiative effects. Atmos. Chem. Phys. 16, 2507-2523 (2016).
- Drugé, T. et al. Modeling radiative and climatic effects of brown carbon aerosols with the ARPEGE-Climat global climate model. Atmos. Chem. Phys. 22, 12167-12205 (2022).
- Bellouin, N. et al. Bounding global aerosol radiative forcing of climate change. Rev. Geophys. 58, e2019RG000660 (2020).
- Schill, G. P. et al. The contribution of black carbon to global ice nucleating particle concentrations relevant to mixed-phase clouds. Proc. Natl. Acad. Sci. USA 117, 202001674 (2020).
- Jesús et al. Is black carbon an unimportant ice-nucleating particle in mixed-phase clouds? J. Geophys. Res. 123, 4273-4283 (2018).
- Levin, E. J. T. et al. Ice-nucleating particle emissions from biomass combustion and the potential importance of soot aerosol. J. Geophys. Res. 121, 5888-5903 (2016).
- Friedman, B. et al. Ice nucleation and droplet formation by bare and coated soot particles. J. Geophys. Res. 116, D17203 (2011).
- Kupiszewski, P. et al. Ice residual properties in mixed-phase clouds at the high-alpine Jungfraujoch site. J. Geophys. Res. 121, 12,343-312,362 (2016).
- Kulkarni, G. et al. Ice nucleation activity of diesel soot particles at cirrus relevant temperature conditions: effects of hydration, secondary organics coating, soot morphology, and coagulation. Geophys. Res. Lett. 43, 3580-3588 (2016).
- Cozic, J. et al. Black carbon enrichment in atmospheric ice particle residuals observed in lower tropospheric mixed phase clouds. J. Geophys. Res. 113, D15209 (2008).
- Twohy, C. H., Anderson, J. R. & Crozier, P. A. Nitrogenated organic aerosols as cloud condensation nuclei. Geophy. Res. Lett. 32 https://doi.org/10.1029/2005GL023605 (2005).
- Koch, D. et al. Soot microphysical effects on liquid clouds, a multimodel investigation. Atmos. Chem. Phys. 11, 1051-1064 (2011).
- McNeill, V. F., Sareen, N. & Schwier, A. Topics in Current Chemistry Ch. 404, 1-59 (Springer, 2013).
- Wang, J. et al. Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility. Atmos. Chem. Phys. 19, 941-954 (2019).
- Wokosin, K. A., Schell, E. L. & Faust, J. A. Surfactants, films, and coatings on atmospheric aerosol particles: a review. Environ. Sci. Atmos. https://doi.org/10.1039/D2EA00003B (2022).
- Knopf, D. A. et al. Microspectroscopic imaging and characterization of individually identified ice nucleating particles from a case field study. J. Geophys. Res. 119, 2014JD021866 (2014).
- Dong, Z. et al. Variability in individual particle structure and mixing states between the glacier-snowpack and atmosphere in the northeastern Tibetan Plateau. Cryosphere 12, 3877-3890 (2018).
- He, C. et al. Impact of grain shape and multiple black carbon internal mixing on snow albedo: parameterization and radiative effect analysis. J. Geophys. Res. 123, 1253-1268 (2018).
- Johansson, K. O., Head-Gordon, M. P., Schrader, P. E., Wilson, K. R. & Michelsen, H. A. Resonance-stabilized hydrocarbon-radical chain reactions may explain soot inception and growth. Science 361, 997-1000 (2018).
- Ching, J., Kajino, M. & Matsui, H. Resolving aerosol mixing state increases accuracy of black carbon respiratory deposition estimates. One Earth 3, 763-776 (2020).
- Zheng, Z. et al. Estimating submicron aerosol mixing state at the global scale with machine learning and earth system modeling. Earth Space Sci. 8 https://doi.org/10.1029/2020ea001500 (2021).
- Luo, J., Zhang, Y., Wang, F., Wang, J. & Zhang, Q. Applying machine learning to estimate the optical properties of black carbon fractal aggregates. J. Quant. Spectrosc. Radiat. Transf. 215, 1-8 (2018).
- Lamb, K. D. & Gentine, P. Zero-shot learning of aerosol optical properties with graph neural networks. Sci. Rep. 13, 18777 (2023).
- Wang, X., Bi, L., Han, W. & Zhang, X. Single-scattering properties of encapsulated fractal black carbon particles computed using the invariant imbedding T-matrix method and deep learning approaches. J. Geophys. Res. 128, e2023JD039568 (2023).
- Shen, W. et al. Improving BC mixing state and CCN activity representation with machine learning in the Community Atmosphere Model Version 6 (CAM6). J. Adv. Model Earth Syst. 16 https://doi. org/10.1029/2023ms003889 (2024).
- Gorkowski, K., Donahue, N. M. & Sullivan, R. C. Aerosol optical tweezers constrain the morphology evolution of liquid-liquid phaseseparated atmospheric particles. Chem 6, 204-220 (2020).
- Dazzi, A. & Prater, C. B. AFM-IR: technology and applications in nanoscale infrared spectroscopy and chemical imaging. Chem. Rev. 117, 5146-5173 (2017).
- Yuan, Q. et al. Mixing state and fractal dimension of soot particles at a remote site in the Southeastern Tibetan plateau. Environ. Sci. Technol. 53, 8227-8234 (2019).
- Raatikainen, T. et al. Size-selected black carbon mass distributions and mixing state in polluted and clean environments of northern India. Atmos. Chem. Phys. 17, 371-383 (2017).
- Fraund, M. et al. Elemental mixing state of aerosol particles collected in Central Amazonia during GoAmazon2014/15. Atmosphere 8, 173 (2017).
- Ljungman, P. L. S. et al. Long-term exposure to particulate air pollution, black carbon, and their source components in relation to ischemic heart disease and stroke. Environ. Health Perspect. 127, 107012 (2019).
- Zhu, S., Zhang, H., Zhou, C., Wei, X. & Liu, Y. Optical properties of mixed black and brown carbon aerosols. Opt. Express 30, 33588-33602 (2022).
Acknowledgements
Author contributions
Competing interests
Additional information
© The Author(s) 2024
Key Laboratory of Geoscience Big Data and Deep Resource of Zhejiang Province, Department of Atmospheric Sciences, School of Earth Sciences, Zhejiang University, Hangzhou 310027, China. Department of Climate, Meteorology, and Atmospheric Sciences, University of Illinois at Urbana-Champaign, Urbana, IL, USA. College of Sciences, China Jiliang University, Hangzhou 310018, China. Department of Atmosphere, Ocean, and Earth System Modeling Research, Meteorological Research Institute, Tsukuba, Japan. School of Geography, Earth and Environmental Sciences, University of Birmingham, Birmingham B15 2TT, UK. Faculty of Environmental and Symbiotic Sciences, Prefectural University of Kumamoto, Kumamoto 862-8502, Japan. Department of Earth and Environmental Sciences, The University of Manchester, Manchester, UK. Department of Chemistry, Purdue University, West Lafayette, IN 47907, USA. Department of Earth Atmospheric and Planetary Sciences, Purdue University, West Lafayette, IN 47907, USA. e-mail: liweijun@zju.edu.cn; alaskin@purdue.edu