Interactive comment on “Light absorption of brown carbon in eastern China based on 3-year multi-wavelength aerosol optical property observations at the SORPES station and an improved Absorption Ångstrom exponent segregation method” by Jiaping Wang et

2018 ◽  
Author(s):  
Anonymous
2018 ◽  
Author(s):  
Jiaping Wang ◽  
Wei Nie ◽  
Yafang Cheng ◽  
Yicheng Shen ◽  
Xuguang Chi ◽  
...  

Abstract. Brown carbon (BrC), a certain group of organic carbon (OC) with strong absorption from the visible to ultraviolet (UV) wavelengths, makes considerable contribution to light absorption on both global and regional scales. High concentration and proportion of OC has been reported in China, but studies of BrC absorption based on long-term observations are rather limited in this region. In this study, we reported 3-year results of light absorption of BrC based on continuous measurement at the Station for Observation Regional Processes of the Earth System (SORPES) in the Yangtze River Delta, China combined with Mie-theory calculation. Light absorption of BrC was obtained using an improved Absorption Ångstrom exponent (AAE) segregation method to calculate AAE of pure and non-absorbing coated black carbon (BC) at each time step based on Mie-theory simulation and measurement of multi-wavelength aerosol light absorption. By using this improved method, the variation of AAE over time is taken into consideration, making it applicable for long-term analysis. The yearly average light absorption of BrC (babs_BrC) at 370 nm was 4.3 Mm−1 at the SORPES station. The contribution of BrC to total aerosol absorption (PBrC) at 370 nm ranged from 6 % to 18 % (10th and 90th percentiles, respectively), and reached up to ~ 28 % in biomass burning-dominant season and winter. Both babs_BrC and PBrC exhibited clear seasonal cycles with two peaks in later spring/early summer (May–June, babs_BrC ~ 4 Mm−1, PBrC ~ 11 %) and winter (December, babs_BrC ~ 12 Mm−1, PBrC ~ 17 %), respectively. Lagrangian modeling and chemical signature observed at the site suggested that open biomass burning and residential emissions were the dominate sources influencing BrC in the two seasons.


2013 ◽  
Vol 13 (6) ◽  
pp. 15493-15515 ◽  
Author(s):  
D. A. Lack ◽  
J. M. Langridge

Abstract. The absorption Ångström exponent (åAbs) of black carbon (BC), or BC internally mixed with non-absorbing material (BCInt), is often used to differentiate the contribution of black carbon, dust and brown carbon to light absorption at low-visible wavelengths. This attribution method contains assumptions with uncertainties that have not been formally assessed. We show that the potential range of åAbs for BC (or BCInt) in the atmosphere can reasonably lead to +7% to −22% uncertainty in BC (or BCInt) absorption at 404nm derived from measurements made at 658 nm. These uncertainties propagate to errors in the attributed absorption and mass absorption efficiency (MAE) of brown carbon (BrC). For data collected during a biomass-burning event, the mean uncertainty in MAE at 404 nm attributed to BrC using the åAbs method was found to be 34%. In order to yield attributed BrC absorption uncertainties of ±33%, 23% to 41% of total absorption must be sourced from BrC. In light of the potential for introducing significant and poorly constrained errors, we caution against the universal application of the åAbs attribution method.


2018 ◽  
Vol 18 (12) ◽  
pp. 9061-9074 ◽  
Author(s):  
Jiaping Wang ◽  
Wei Nie ◽  
Yafang Cheng ◽  
Yicheng Shen ◽  
Xuguang Chi ◽  
...  

Abstract. Brown carbon (BrC), a certain group of organic carbon (OC) with strong absorption from the visible (VIS) to ultraviolet (UV) wavelengths, makes a considerable contribution to light absorption on both global and regional scales. A high concentration and proportion of OC has been reported in China, but studies of BrC absorption based on long-term observations are rather limited in this region. In this study, we reported 3-year results of light absorption of BrC based on continuous measurement at the Station for Observing Regional Processes of the Earth System (SORPES) in the Yangtze River Delta, China, combined with Mie theory calculation. Light absorption of BrC was obtained using an improved absorption Ångström exponent (AAE) segregation method. The AAE of non-absorbing coated black carbon (BC) at each time step is calculated based on Mie theory simulation, together with single particle soot photometer (SP2) and aethalometer observations. By using this improved method, the variation of the AAE over time is taken into consideration, making it applicable for long-term analysis. The annual average light absorption coefficient of BrC (babs_BrC) at 370 nm was 6.3 Mm−1 at the SORPES station. The contribution of BrC to total aerosol absorption (PBrC) at 370 nm ranged from 10.4 to 23.9 % (10th and 90th percentiles, respectively), and reached up to ∼ 33 % in the open-biomass-burning-dominant season and winter. Both babs_BrC and PBrC exhibited clear seasonal cycles with two peaks in later spring/early summer (May–June, babs_BrC ∼ 6 Mm−1, PBrC ∼ 17 %) and winter (December, babs_BrC ∼ 15 Mm−1, PBrC ∼ 22 %), respectively. Lagrangian modeling and the chemical signature observed at the site suggested that open biomass burning and residential coal/biofuel burning were the dominant sources influencing BrC in the two seasons, respectively.


2013 ◽  
Vol 13 (20) ◽  
pp. 10535-10543 ◽  
Author(s):  
D. A. Lack ◽  
J. M. Langridge

Abstract. The absorption Ångström exponent (AAE) of externally mixed black carbon (BCExt), or BC internally mixed with non-absorbing material (BCInt), is often used to determine the contribution of brown carbon (BrC) light absorption at short visible wavelengths. This attribution method contains assumptions with uncertainties that have not been formally assessed. We show that the potential range of AAE for BCExt (or BCInt) in the atmosphere can reasonably lead to +7% to −22% uncertainty in BCExt (or BCInt) absorption at short wavelengths derived from measurements made at longer wavelengths, where BrC is assumed not to absorb light. These uncertainties propagate to errors in the attributed absorption of BrC. For uncertainty in attributed BrC absorption to be ≤ ± 33%, 23% to 41% of total absorption must be sourced from BrC. These uncertainties would be larger if absorption by dust were also to be considered due to additional AAE assumptions. For data collected during a biomass-burning event, the mean difference between measured and AAE attributed BrC absorption was found to be 34% – an additional uncertainty in addition to the theoretical uncertainties presented. In light of the potential for introducing significant and poorly constrained errors, we caution against the universal application of the AAE method for attributing BrC absorption.


2018 ◽  
Vol 18 (1) ◽  
pp. 405-425 ◽  
Author(s):  
Huizheng Che ◽  
Bing Qi ◽  
Hujia Zhao ◽  
Xiangao Xia ◽  
Thomas F. Eck ◽  
...  

Abstract. Aerosol pollution in eastern China is an unfortunate consequence of the region's rapid economic and industrial growth. Here, sun photometer measurements from seven sites in the Yangtze River Delta (YRD) from 2011 to 2015 were used to characterize the climatology of aerosol microphysical and optical properties, calculate direct aerosol radiative forcing (DARF) and classify the aerosols based on size and absorption. Bimodal size distributions were found throughout the year, but larger volumes and effective radii of fine-mode particles occurred in June and September due to hygroscopic growth and/or cloud processing. Increases in the fine-mode particles in June and September caused AOD440 nm > 1.00 at most sites, and annual mean AOD440 nm values of 0.71–0.76 were found at the urban sites and 0.68 at the rural site. Unlike northern China, the AOD440 nm was lower in July and August (∼ 0.40–0.60) than in January and February (0.71–0.89) due to particle dispersion associated with subtropical anticyclones in summer. Low volumes and large bandwidths of both fine-mode and coarse-mode aerosol size distributions occurred in July and August because of biomass burning. Single-scattering albedos at 440 nm (SSA440 nm) from 0.91 to 0.94 indicated particles with relatively strong to moderate absorption. Strongly absorbing particles from biomass burning with a significant SSA wavelength dependence were found in July and August at most sites, while coarse particles in March to May were mineral dust. Absorbing aerosols were distributed more or less homogeneously throughout the region with absorption aerosol optical depths at 440 nm ∼ 0.04–0.06, but inter-site differences in the absorption Angström exponent indicate a degree of spatial heterogeneity in particle composition. The annual mean DARF was −93 ± 44 to −79 ± 39 W m−2 at the Earth's surface and ∼ −40 W m−2 at the top of the atmosphere (for the solar zenith angle range of 50 to 80∘) under cloud-free conditions. The fine mode composed a major contribution of the absorbing particles in the classification scheme based on SSA, fine-mode fraction and extinction Angström exponent. This study contributes to our understanding of aerosols and regional climate/air quality, and the results will be useful for validating satellite retrievals and for improving climate models and remote sensing algorithms.


2020 ◽  
Vol 20 (16) ◽  
pp. 9701-9711 ◽  
Author(s):  
Xiaolin Zhang ◽  
Mao Mao ◽  
Yan Yin ◽  
Shihao Tang

Abstract. The aerosol absorption Ångstrom exponent (AAE) is a crucial optical parameter for apportionment and characterization. Due to considerable inconsistences associated with observations, numerical research is a powerful means to give a better understanding of the AAE of aged black carbon (BC) aerosols. Numerical studies of the AAE of polydisperse BC aggregates with brown coatings using the exact multiple-sphere T-matrix method (MSTM) are performed. The objective of the study is to thoroughly assess the AAE of coated BC influenced by their observation-based detailed microphysics and then provide a new AAE parameterization for application. At odds with our expectations, more large-sized BC particles coated by thin brown carbon can have an AAE smaller than 1.0, indicating that BC aerosols internally mixing with brown carbon can even show lower AAE than pure BC particles. The AAE of BC with brown coatings is highly sensitive to the absorbing volume fraction of the coating, coated volume fraction of BC, shell ∕ core ratio, and particle size distribution with a wide variation, whereas the impacts of BC geometry and BC position within the coating are negligible. The AAE of BC with brown coatings can be larger than 3.0 if there are plenty of small-sized coated BC particles, heavy coating, or a large amount of brown carbon. However, the AAE of BC with non-absorbing coating appears to be weakly sensitive to particle microphysics with values around 1.0 (i.e., 0.7–1.4), suggesting the substantial role of the absorbing volume fraction of the coating in AAE determination. With more realistic BC geometries, our study also indicates that the occurrence of brown carbon may not be confidently determined unless AAE > 1.4. The currently popular core–shell Mie model reasonably approximates the AAE of fully coated BC by brown carbon, whereas it underestimates the AAE of partially coated or externally attached BC and underestimates more for a lower coated volume fraction of BC. In addition, we present a parameterization of the AAE of coated BC with a size distribution on the basis of numerical results, which can act as a guide for the AAE response to the absorbing volume fraction of the coating, coated volume fraction of BC, and shell ∕ core ratio. The proposed parameterization of coated BC AAE generates a decent prediction for moderate BC microphysics, whereas caution should be taken in applying it for extreme cases, such as externally attached coated BC morphology. Our findings could improve the understanding and application of the AAE of BC with brown coatings.


2012 ◽  
Vol 12 (4) ◽  
pp. 2229-2244 ◽  
Author(s):  
L. Mona ◽  
A. Amodeo ◽  
G. D'Amico ◽  
A. Giunta ◽  
F. Madonna ◽  
...  

Abstract. During the eruption of Eyjafjallajökull in April–May 2010 multi-wavelength Raman lidar measurements were performed at the CNR-IMAA Atmospheric Observatory (CIAO), whenever weather conditions permitted observations. A methodology both for volcanic layer identification and accurate aerosol typing has been developed. This methodology relies on the multi-wavelength Raman lidar measurements and the support of long-term lidar measurements performed at CIAO since 2000. The aerosol mask for lidar measurements performed at CIAO during the 2010 Eyjafjallajökull eruption has been obtained. Volcanic aerosol layers were observed in different periods: 19–22 April, 27–29 April, 8–9 May, 13–14 May and 18–19 May. A maximum aerosol optical depth of about 0.12–0.13 was observed on 20 April, 22:00 UTC and 13 May, 20:30 UTC. Volcanic particles were detected at low altitudes, in the free troposphere and in the upper troposphere. Occurrences of volcanic particles within the PBL were detected on 21–22 April and 13 May. A Saharan dust event was observed on 13–14 May: dust and volcanic particles were simultaneously detected at CIAO at separated different altitudes as well as mixed within the same layer. Lidar ratios at 355 and 532 nm, the Ångström exponent at 355/532 nm, the backscatter-related Ångström exponent at 532/1064 nm and the particle linear depolarization ratio at 532 nm measured inside the detected volcanic layers are discussed. The dependence of these quantities on relative humidity has been investigated by using co-located microwave profiler measurements. The measured values of these intensive parameters indicate the presence of volcanic sulfates/continental mixed aerosol in the volcanic aerosol layers observed at CIAO. In correspondence of the maxima observed in the volcanic aerosol load on 19–20 April and 13 May, different values of intensive parameters were observed. Apart from the occurrence of sulfate aerosol, these values indicate also the presence of some ash which is affected by the aging during transport over Europe.


Sign in / Sign up

Export Citation Format

Share Document