Light absorption properties and implications of particulate
brown carbon in Chongqing

Abstract

Abstract: Aerosol samples were collected at urban and rural sites in Chongqing, China, from December 2015 to July 2017, and then the spatial and seasonal variations of light absorption properties and implications of brown carbon (BrC) in aerosols in this area were systematically investigated, and the radiative forcing of BrC was evaluated. The results show that the average light absorption coefficient b405,BrC, contribution to aerosol light absorption, and mass absorption efficiency of BrC at 405 nm in winter were (13.0±9.0) Mm−1, (24.5±6.1)% and (0.9±0.2) m2·g−1 respectively, about 11.3, 2.9 and 3.4 times of those in summer. The average b405,BrC at urban site (YB) in summer and winter were 2.8 and 1.8 times of those at rural site (JY) respectively. However, the absorption Ångstrom ¨ exponent (E =1.2±0.1) and the contribution to aerosol light absorption of BrC at 405 nm (16.7±5.9)% at YB were significantly lower than those at JY ((1.6±0.2) and (32.3±6.3)%, respectively). The relationships between b405,BrC and the indicators of pollution sources indicated that the light absorption properties of BrC were mainly affected by the formation of secondary organic aerosols (SOA) in summer, while mainly affected by biomass burning, coal burning and the formation of SOA in winter. Compared with those in summer (p > 0.1), the significant correlation between b405,BrC and NH4+ concentrations (p < 0.001), as well as the significant correlations between E and the mass fractions of NO3− and NH4+, were observed in winter. The shape of fit line between E values and φ in winter was similar to that of combustion chamber results of biomass burning, indicating that BrC light absorption was mainly affected by biomass burning and the aged BrC produced from the reactions of organic compounds with NO3− and NH4+ during winter. The fractional contribution of radiation absorbed by BrC was (29.1±5.8)% in 405∼980 nm and (60.8±13.7)% in 405∼445 nm in winter, about 2.9 and 3.2 times those in summer, indicating that the radiation absorbed by BrC was the main contributor affecting the radiative balance during winter, especially at short wavelengths.

Key words: brown carbon aerosol, light absorption properties, influential factors, Chongqing

CLC Number:

X513
X-1

PENG Chao, CHEN Yang∗, YANG Fumo, TIAN Mi, ZHAI Chongzhi, . Light absorption properties and implications of particulate brown carbon in Chongqing[J]. Journal of Atmospheric and Environmental Optics, 2022, 17(1): 135-147.

References 49

[1]	Bond T C, Doherty S J, Fahey D W, et al. Bounding the role of black carbon in the climate system: A scientific assessment [J].
	Journal of Geophysical Research: Atmospheres, 2013, 118(11): 5380-5552.
[2]	Laskin A, Laskin J, Nizkorodov S A. Chemistry of atmospheric brown carbon [J]. Chemical Reviews, 2015, 115(10): 4335-
	4382.
[3]	Andreae M O, Gelencser A. Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols [J]. ´ Atmospheric Chemistry and Physics, 2006, 6(10): 3131-3148.
[4]	Bond T C, Bergstrom R W. Light absorption by carbonaceous particles: An investigative review [J]. Aerosol Science and
	Technology, 2006, 40(1): 27-67.
[5]	Chung C E, Ramanathan V, Decremer D. Observationally constrained estimates of carbonaceous aerosol radiative forcing [J].
	Proceedings of the National Academy of Sciences of the United States of America, 2012, 109(29): 11624-11629.
[6]	Feng Y, Ramanathan V, Kotamarthi V R. Brown carbon: A significant atmospheric absorber of solar radiation? [J]. Atmospheric
	Chemistry and Physics, 2013, 13(17): 8607-8621.
[7]	Jo D S, Park R J, Lee S, et al. A global simulation of brown carbon: Implications for photochemistry and direct radiative effect
[J]	Atmospheric Chemistry and Physics, 2016, 16(5): 3413-3432.
[8]	Huang R J, Yang L, Cao J J, et al. Brown carbon aerosol in urban Xi′an, Northwest China: The composition and light absorption
	properties [J]. Environmental Science & Technology, 2018, 52(12): 6825-6833.
[9]	Wu C, Wang G H, Li J, et al. The characteristics of atmospheric brown carbon in Xi′an, inland China: Sources, size distributions
	and optical properties [J]. Atmospheric Chemistry and Physics, 2020, 20(4): 2017-2030.
[10]	Liu J M, Lin P, Laskin A, et al. Optical properties and aging of light-absorbing secondary organic aerosol [J]. Atmospheric
	Chemistry and Physics, 2016, 16(19): 12815-12827.
[11]	Monod A, Liu Y. Aerosol formation and heterogeneous chemistry in the atmosphere [J]. EPJ Web of Conferences, 2011, 18:
04	002.
[12]	Flores J M, Washenfelder R A, Adler G, et al. Complex refractive indices in the near-ultraviolet spectral region of biogenic
	secondary organic aerosol aged with ammonia [J]. Physical Chemistry Chemical Physics, 2014, 16(22): 10629-10642.
[13]	Lin P, Laskin J, Nizkorodov S A, et al. Revealing brown carbon chromophores produced in reactions of methylglyoxal with
	ammonium sulfate [J]. Environmental Science & Technology, 2015, 49(24): 14257-14266.
[14]	Chen L W A, Chow J C, Wang X L, et al. Multi-wavelength optical measurement to enhance thermal/optical analysis for
	carbonaceous aerosol [J]. Atmospheric Measurement Techniques, 2015, 8(1): 451-461.
[15]	Chow J C, Watson J G, Green M C, et al. Separation of brown carbon from black carbon for IMPROVE and Chemical
	Speciation Network PM2.5 samples [J]. Journal of the Air & Waste Management Association, 2018, 68(5): 494-510.
[16]	Zhao Z Z, Cao J J, Chow J C, et al. Multi-wavelength light absorption of black and brown carbon at a high-altitude site on the
	Southeastern margin of the Tibetan Plateau, China [J]. Atmospheric Environment, 2019, 212: 54-64.
[17]	Peng C, Tian M, Wang X L, et al. Light absorption of brown carbon in PM2.5 in the Three Gorges Reservoir region, southwestern China: Implications of biomass burning and secondary formation [J]. Atmospheric Environment, 2020, 229: 117409.
[18]	Li S, Zhu M, Yang W Q, et al. Filter-based measurement of light absorption by brown carbon in PM2.5 in a megacity in South
	China [J]. Science of the Total Environment, 2018, 633: 1360-1369.
[19]	Kirillova E N, Andersson A, Han J, et al. Sources and light absorption of water-soluble organic carbon aerosols in the outflow
	from Northern China [J]. Atmospheric Chemistry and Physics, 2014, 14(3): 1413-1422.
[20]	Chen D, Zhao Y, Lyu R T, et al. Seasonal and spatial variations of optical properties of light absorbing carbon and its influencing
	factors in a typical polluted city in Yangtze River Delta, China [J]. Atmospheric Environment, 2019, 199: 45-54.
[21]	Qin Y M, Tan H B, Li Y J, et al. Chemical characteristics of brown carbon in atmospheric particles at a suburban site near
	Guangzhou, China [J]. Atmospheric Chemistry and Physics, 2018, 18(22): 16409-16418.
[22]	Peng C, Yang F M, Tian M, et al. Brown carbon aerosol in two megacities in the Sichuan Basin of southwestern China: Light
	absorption properties and implications [J]. Science of the Total Environment, 2020, 719: 137483.
[23]	Chen Y, Wenger J C, Yang F M, et al. Source characterization of urban particles from meat smoking activities in Chongqing,
	China using single particle aerosol mass spectrometry [J]. Environmental Pollution, 2017, 228: 92-101.
[24]	Tian M, Liu Y, Yang F M, et al. Increasing importance of nitrate formation for heavy aerosol pollution in two megacities in
	Sichuan Basin, southwest China [J]. Environmental Pollution, 2019, 250: 898-905.
[25]	Lack D A, Langridge J M. On the attribution of black and brown carbon light absorption using the Ångstrom exponent [J]. ¨
	Atmospheric Chemistry and Physics, 2013, 13(20): 10535-10543.
[26]	Tian J, Wang Q Y, Ni H Y, et al. Emission characteristics of primary brown carbon absorption from biomass and coal burning:
	Development of an optical emission inventory for China [J]. Journal of Geophysical Research: Atmospheres, 2019, 124(3):
18	79-1893.
[27]	Peng C, Tian M, Chen Y, et al. Characteristics, formation mechanisms and potential transport pathways of PM2.5 at a rural
	background site in Chongqing, southwest China [J]. Aerosol and Air Quality Research, 2019, 19(9): 1980-1992.
[28]	Li H M, Wang Q G, Yang M, et al. Chemical characterization and source apportionment of PM2.5 aerosols in a megacity of
	Southeast China [J]. Atmospheric Research, 2016, 181: 288-299.
[29]	Yudovich Y E, Ketris M P. Chlorine in coal: A review [J]. International Journal of Coal Geology, 2006, 67(1/2): 127-144.
[30]	Tao J, Zhang L M, Zhang R J, et al. Uncertainty assessment of source attribution of PM2.5 and its water-soluble organic carbon
	content using different biomass burning tracers in positive matrix factorization analysis-a case study in Beijing, China [J].
	Science of the Total Environment, 2016, 543: 326-335.
[31]	Castro L M, Pio C A, Harrison R M, et al. Carbonaceous aerosol in urban and rural European atmospheres: Estimation of
	secondary organic carbon concentrations [J]. Atmospheric Environment, 1999, 33(17): 2771-2781.
[32]	Cao J J, Wu F, Chow J C, et al. Characterization and source apportionment of atmospheric organic and elemental carbon during
	fall and winter of 2003 in Xi′an, China [J]. Atmospheric Chemistry and Physics, 2005, 5(11): 3127-3137.
[33]	Zhang Q, Shen Z X, Lei Y L, et al. Variations of particle size distribution, black carbon, and brown carbon during a severe
	winter pollution event over Xi′an, China [J]. Aerosol and Air Quality Research, 2018, 18(6): 1419-1430.
[34]	Zhu C S, Cao J J, Hu T F, et al. Spectral dependence of aerosol light absorption at an urban and a remote site over the Tibetan
	Plateau [J]. Science of the Total Environment, 2017, 590/591: 14-21.
[35]	Yuan J F, Huang X F, Cao L M, et al. Light absorption of brown carbon aerosol in the PRD region of China [J]. Atmospheric
	Chemistry and Physics, 2016, 16(3): 1433-1443.
[36]	Chen Y F, Ge X L, Chen H, et al. Seasonal light absorption properties of water-soluble brown carbon in atmospheric fine
	particles in Nanjing, China [J]. Atmospheric Environment, 2018, 187: 230-240.
[37]	Wang J P, Nie W, Cheng Y F, et al. Light absorption of brown carbon in Eastern China based on 3-year multi-wavelength
	aerosol optical property observations and an improved absorption Ångstrom exponent segregation method [J]. ¨ Atmospheric
	Chemistry and Physics, 2018, 18(12): 9061-9074.
[38]	Olson M R, Victoria G M, Robinson M A, et al. Investigation of black and brown carbon multiple-wavelength-dependent light
	absorption from biomass and fossil fuel combustion source emissions [J]. Journal of Geophysical Research: Atmospheres,
20	15, 120(13): 6682-6697.
[39]	Teich M, Van P D, Wang M, et al. Contributions of nitrated aromatic compounds to the light absorption of water-soluble
	and particulate brown carbon in different atmospheric environments in Germany and China [J]. Atmospheric Chemistry and
	Physics, 2017, 17(3): 1653-1672.
[40]	Hecobian A, Zhang X, Zheng M, et al. Water-soluble organic aerosol material and the light-absorption characteristics of
	aqueous extracts measured over the Southeastern United States [J]. Atmospheric Chemistry and Physics, 2010, 10(13): 5965-
	5977.
[41]	Peng C. Characteristics and Optical Properties of Brown Carbon in PM2.5 in Chongqing [D]. Chongqing: University of Chinese
	Academy of Sciences (Chongqing Institute of Green and Intelligent Technology, Chinese Academy of Sciences), 2020.
	彭超. 重庆 PM2.5 中棕色碳的污染特征和光学特性研究 [D]. 重庆: 中国科学院大学 (中国科学院重庆绿色智能技术研
究院)	, 2020.
[42]	Zeng Y L, Shen Z X, Takahama S, et al. Molecular absorption and evolution mechanisms of PM2.5 brown carbon revealed by
	electrospray ionization Fourier transform-ion cyclotron resonance mass spectrometry during a severe winter pollution episode
	in Xi′an, China [J]. Geophysical Research Letters, 2020, 47(10): e2020GL087977.
[43]	Bones D L, Henricksen D K, Mang S A, et al. Appearance of strong absorbers and fluorophores in limonene-O3 secondary organic aerosol due to NH4+-mediated chemical aging over long time scales [J]. Journal of Geophysical Research: Atmospheres,
20	10, 115(D5): D05203.
[44]	Lu Z F, Streets D G, Winijkul E, et al. Light absorption properties and radiative effects of primary organic aerosol emissions
[J]	Environmental Science & Technology, 2015, 49(8): 4868-4877.
[45]	Saleh R, Robinson E S, Tkacik D S, et al. Brownness of organics in aerosols from biomass burning linked to their black carbon
	content [J]. Nature Geoscience, 2014, 7(9): 647-650.
[46]	Saleh R, Hennigan C J, McMeeking G R, et al. Absorptivity of brown carbon in fresh and photo-chemically aged biomassburning emissions [J]. Atmospheric Chemistry and Physics, 2013, 13(15): 7683-7693.
[47]	Zeng Y L, Ning Y L, Shen Z X, et al. The roles of N, S, and O in molecular absorption features of brown carbon in PM2.5
	in a typical semi-arid megacity in Northwestern China [J]. Journal of Geophysical Research: Atmospheres, 2021, 126(16):
	e2021JD034791.
[48]	Levinson R, Akbari H, Berdahl P. Measuring solar reflectance-Part I: Defining a metric that accurately predicts solar heat gain
[J]	Solar Energy, 2010, 84(9): 1717-1744.
[49]	Hammer M S, Martin R V, Van D A, 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 [J].
	Atmospheric Chemistry and Physics, 2016, 16(4): 2507-2523.

Light absorption properties and implications of particulate brown carbon in Chongqing

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