scholarly journals Simulations of black carbon over the Indian region: improvements and implications of diurnality in emissions

2019 ◽  
Vol 19 (12) ◽  
pp. 8229-8241 ◽  
Author(s):  
Gaurav Govardhan ◽  
Sreedharan Krishnakumari Satheesh ◽  
Krishnaswamy Krishna Moorthy ◽  
Ravi Nanjundiah
Keyword(s):  
Boundary Layer ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Regional Scale ◽  
Early Morning ◽  
Temporal Variations ◽  
Indian Region ◽  
Near Surface ◽  
Aerosol Radiative Forcing ◽  
Convective Mixing

Abstract. With a view to improving the performance of WRF-Chem over the Indian region in simulating BC (black carbon) mass concentrations as well as its short-term variations, especially on a diurnal scale, a region-specific diurnal variation scheme has been introduced in the model emissions and the performance of the modified simulations has been evaluated against high-resolution measurements carried out over eight ARFI (Aerosol Radiative Forcing over India) network observatories spread across India for distinct seasons: pre-monsoon (represented by May), post-monsoon (represented by October) and winter (represented by December). In addition to an overall improvement in the simulated concentrations and their temporal variations, we have also found that the effects of prescribing diurnally varying emissions on the simulated near-surface concentrations largely depend on the boundary layer turbulence. The effects are perceived quickly (within about 2–3 h) during the evening–early morning hours when the atmospheric boundary layer is shallow and convective mixing is weak, while they are delayed, taking as much as about 5–6 h, during periods when the boundary layer is deep and convective mixing is strong. This information would also serve as an important input for agencies concerned with urban planning and pollution mitigation. Despite these improvements in the near-surface concentrations, the simulated columnar aerosol optical depth (AOD) still remains largely underestimated vis-à-vis the satellite-retrieved products. These modifications will serve as a guideline for further model-improvement initiatives at a regional scale.

scholarly journals Simulations of Black Carbon Over Indian Region: Improvements and Implications of Diurnality in Emissions

2019 ◽  
Author(s):  
Gaurav Govardhan ◽  
Sreedharan Krishnakumari Satheesh ◽  
Krishnaswamy Krishna Moorthy ◽  
Ravi Nanjundiah
Keyword(s):  
Boundary Layer ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Regional Scale ◽  
Early Morning ◽  
Temporal Variations ◽  
Indian Region ◽  
Near Surface ◽  
Aerosol Radiative Forcing ◽  
Convective Mixing

Abstract. With a view to improving the performance of WRF-Chem over the Indian region in simulating BC (black Carbon) mass concentrations as well as its short-term variations, especially on diurnal scale, a region-specific diurnal variation scheme has been introduced in the model emissios and the performance of the modified simulations has been evaluated against high-resolution measurements carried out over 8 ARFI (Aerosol Radiative Forcing over India) network observatories spread across India for distinct seasons; pre-monsoon (represented by May), post-monsoon (represented by October) and winter (represented by December). In addition to an overall improvement in the simulated concentrations and their temporal variations, it has also been found that the effects of prescribing diurnally varying emissions on the simulated near-surface concentrations largely depend on the boundary layer turbulence. The effects are perceived fast (within about 2–3 hours) during the evening–early morning hours when the atmospheric boundary layer is shallow and convective mixing is weak, while they are delayed, taking as much as about 5–6 hours, during periods when the boundary layer is deep and convective mixing is strong. This information would also serve as an important input for agencies concerned with urban planning and pollution mitigation. Despite these improvements in the near-surface concentrations, the simulated columnar aerosol optical depth (AOD) still remains largely underestimated vis-a-vis the satellite retrieved products. These modifications will serve as a guideline for further model-improvement initiatives at regional scale.

scholarly journals The surface aerosol optical properties in urban areas of Nanjing, west Yangtze River Delta of China

2016 ◽  
Author(s):  
B. L. Zhuang ◽  
T. J. Wang ◽  
J. Liu ◽  
S. Li ◽  
M. Xie ◽  
...  
Keyword(s):  
Optical Properties ◽  
Urban Areas ◽  
Radiative Forcing ◽  
Early Morning ◽  
Single Scattering ◽  
Temporal Variations ◽  
Yangtze River Delta ◽  
Aerosol Optical Properties ◽  
Growth Trend ◽  
Near Surface

Abstract. Observational studies of aerosol optical properties are useful to reducing uncertainties in estimating aerosol radiative forcing and forecasting visibility. In this study, the observed near-surface aerosol optical properties in urban Nanjing are analyzed from Mar 2014 to Feb 2016. Results show that near-surface urban aerosols in Nanjing are mainly from local emissions and the regions around. They have lower loadings but are more scattering than in most cities in China. The annual mean aerosol extinction coefficient (EC), single scattering albedo (SSA) and asymmetry parameter (ASP) at 550 nm are 381.96 Mm−1, 0.9 and 0.57, respectively. The aerosol absorption coefficient (AAC) is about one order of magnitude smaller than its scattering coefficient (SC). However, the absorbing aerosol has larger Ångström exponent (AAE) value, 1.58 at 470/660 nm, about 0.2 larger than the scattering aerosols' (SAE). All the aerosol optical properties followed a near unimodal pattern, the ranges around their averages accounting for more than 60 % of the total samplings. Additionally, they have substantial seasonality and diurnal variations. High levels of SC and AAC all appear in winter due to higher aerosol and trace gas emissions. AAE (ASP) is the smallest (largest) in summer because of high relative humidity (RH) which also causes considerably larger SC and smaller SAE, although intensive gas-to-particle transformation could produce a large number of finer scattering aerosols in this season. Seasonality of EC is different from the columnar aerosol optical depth. Larger AACs appear at the rush hours of the day while SC and Bsp only peak in the early morning. Aerosols are fresher at daytime than at nighttime, leading to their larger AE and smaller ASP. Different temporal variations between AAC and SC cause the aerosols more absorbing (smaller SSA) in autumn and around rush hours. ASP has a good quasi-LogNormal growth trend with increasing SC when RH is below 60 %. The correlation between AAC and SC at the site is close but a little smaller than that in suburban Nanjing in spring. Atmospheric visibility decreases exponentially with increasing EC or SC, more sharply in spring and summer. It could be further deteriorated with increasing SSA and ASP.

Aerosol radiative forcing due to enhanced black carbon at an urban site in India

2002 ◽  
Vol 29 (18) ◽  
pp. 27-1-27-4 ◽  
Author(s):  
S. Suresh Babu ◽  
S. K. Satheesh ◽  
K. Krishna Moorthy
Keyword(s):  
Black Carbon ◽  
Radiative Forcing ◽  
Urban Site ◽  
Aerosol Radiative Forcing ◽  
Aerosol Radiative

scholarly journals Dome effect of black carbon and its key influencing factors: A one-dimensional modelling study

2017 ◽  
Author(s):  
Zilin Wang ◽  
Xin Huang ◽  
Aijun Ding
Keyword(s):  
Boundary Layer ◽  
Air Pollution ◽  
Black Carbon ◽  
Rural Areas ◽  
Land Surface ◽  
Critical Role ◽  
Aerosol Layer ◽  
Near Surface ◽  
Haze Pollution ◽  
The Impact

Abstract. Black carbon (BC) has been identified to play a critical role in aerosol-planet boundary layer (PBL) interaction and further deterioration of near-surface air pollution in megacities, which has been named as its dome effect. However, the impacts of key factors that influence this effect, such as the vertical distribution and aging processes of BC, and also the underlying land surface, have not been quantitatively explored yet. Here, based on available in-situ measurements of meteorology and atmospheric aerosols together with the meteorology-chemistry online coupled model, WRF-Chem, we conduct a set of parallel simulations to quantify the roles of these factors in influencing the BC's dome effect and surface haze pollution, and discuss the main implications of the results to air pollution mitigation in China. We found that the impact of BC on PBL is very sensitive to the altitude of aerosol layer. The upper level BC, especially those near the capping inversion, is more essential in suppressing the PBL height and weakening the turbulence mixing. The dome effect of BC tends to be significantly intensified as BC aerosol mixed with scattering aerosols during winter haze events, resulting in a decrease of PBL height by more than 25 %. In addition, the dome effect is more substantial (up to 15 %) in rural areas than that in the urban areas with the same BC loading, indicating an unexpected regional impact of such kind of effect to air quality in countryside. This study suggests that China's regional air pollution would greatly benefit from BC emission reductions, especially those from the elevated sources from the chimneys and also the domestic combustions in rural areas, through weakening the aerosol-boundary layer interactions that triggered by BC.

scholarly journals Impact of topography on black carbon transport to the southern Tibetan Plateau during the pre-monsoon season and its climatic implication

2020 ◽  
Vol 20 (10) ◽  
pp. 5923-5943 ◽  
Author(s):  
Meixin Zhang ◽  
Chun Zhao ◽  
Zhiyuan Cong ◽  
Qiuyan Du ◽  
Mingyue Xu ◽  
...  
Keyword(s):  
Tibetan Plateau ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Monsoon Season ◽  
Radiative Heating ◽  
The Tibetan Plateau ◽  
Complex Topography ◽  
Meridional Transport ◽  
Near Surface ◽  
Mass Volume

Abstract. Most previous modeling studies about black carbon (BC) transport and its impact over the Tibetan Plateau (TP) conducted simulations with horizontal resolutions coarser than 20 km that may not be able to resolve the complex topography of the Himalayas well. In this study, the two experiments covering all of the Himalayas with the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) at the horizontal resolution of 4 km but with two different topography datasets (4 km complex topography and 20 km smooth topography) are conducted for pre-monsoon season (April 2016) to investigate the impacts of topography on modeling the transport and distribution of BC over the TP. Both experiments show the evident accumulation of aerosols near the southern Himalayas during the pre-monsoon season, consistent with the satellite retrievals. The observed episode of high surface BC concentration at the station near Mt. Everest due to heavy biomass burning near the southern Himalayas is well captured by the simulations. The simulations indicate that the prevailing upflow across the Himalayas driven by the large-scale westerly and small-scale southerly circulations during the daytime is the dominant transport mechanism of southern Asian BC into the TP, and it is much stronger than that during the nighttime. The simulation with the 4 km topography resolves more valleys and mountain ridges and shows that the BC transport across the Himalayas can overcome the majority of mountain ridges, but the valley transport is more efficient. The complex topography results in stronger overall cross-Himalayan transport during the simulation period primarily due to the strengthened efficiency of near-surface meridional transport towards the TP, enhanced wind speed at some valleys and deeper valley channels associated with larger transported BC mass volume. This results in 50 % higher transport flux of BC across the Himalayas and 30 %–50 % stronger BC radiative heating in the atmosphere up to 10 km over the TP from the simulation with the 4 km complex topography than that with the 20 km smoother topography. The different topography also leads to different distributions of snow cover and BC forcing in snow. This study implies that the relatively smooth topography used by the models with resolutions coarser than 20 km may introduce significant negative biases in estimating light-absorbing aerosol radiative forcing over the TP during the pre-monsoon season. Highlights. The black carbon (BC) transport across the Himalayas can overcome the majority of mountain ridges, but the valley transport is much more efficient during the pre-monsoon season. The complex topography results in stronger overall cross-Himalayan transport during the study period primarily due to the strengthened efficiency of near-surface meridional transport towards the TP, enhanced wind speed at some valleys and deeper valley channels associated with larger transported BC mass volume. The complex topography generates 50 % higher transport flux of BC across the Himalayas and 30 %–50 % stronger BC radiative heating in the atmosphere up to 10 km over the Tibetan Plateau (TP) than the smoother topography, which implies that the smooth topography used by the models with relatively coarse resolution may introduce significant negative biases in estimating BC radiative forcing over the TP during the pre-monsoon season. The different topography also leads to different distributions of snow cover and BC forcing in snow over the TP.

scholarly journals Role of black carbon mass size distribution in the direct aerosol radiative forcing

2019 ◽  
Vol 19 (20) ◽  
pp. 13175-13188 ◽  
Author(s):  
Gang Zhao ◽  
Jiangchuan Tao ◽  
Ye Kuang ◽  
Chuanyang Shen ◽  
Yingli Yu ◽  
...  
Keyword(s):  
Size Distribution ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Climate Models ◽  
Radiative Effects ◽  
Aerosol Radiative Forcing ◽  
Mass Size Distribution ◽  
Mass Size ◽  
Mixing States ◽  
Aerosol Radiative

Abstract. Large uncertainties exist when estimating radiative effects of ambient black carbon (BC) aerosol. Previous studies about the BC aerosol radiative forcing mainly focus on the BC aerosols' mass concentrations and mixing states, while the effects of BC mass size distribution (BCMSD) were not well considered. In this paper, we developed a method of measuring the BCMSD by using a differential mobility analyzer in tandem with an Aethalometer. A comprehensive method of multiple charging corrections was proposed and implemented in measuring the BCMSD. Good agreement was obtained between the BC mass concentration integrated from this system and that measured in the bulk phase, demonstrating the reliability of our proposed method. Characteristics of the BCMSD and corresponding radiative effects were studied based on a field measurement campaign conducted in the North China Plain by using our own measurement system. Results showed that the BCMSD had two modes and the mean peak diameters of the modes were 150 and 503 nm. The BCMSD of the coarser mode varied significantly under different pollution conditions with peak diameter varying between 430 and 580 nm, which gave rise to significant variation in aerosol bulk optical properties. The direct aerosol radiative forcing was estimated to vary by 8.45 % for different measured BCMSDs of the coarser mode, which shared the same magnitude with the variation associated with assuming different aerosol mixing states (10.5 %). Our study reveals that the BCMSD as well as its mixing state in estimating the direct aerosol radiative forcing matters. Knowledge of the BCMSD should be fully considered in climate models.

scholarly journals Assessing the formation and evolution mechanisms of severe haze pollution in Beijing−Tianjin−Hebei region by using process analysis

2019 ◽  
Author(s):  
Lei Chen ◽  
Jia Zhu ◽  
Hong Liao ◽  
Yi Gao ◽  
Yulu Qiu ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Process Analysis ◽  
Vertical Mixing ◽  
Mixing Process ◽  
Aerosol Chemistry ◽  
Near Surface ◽  
Aerosol Radiative Forcing ◽  
Local Emission ◽  
Aerosol Radiative ◽  
Pm2.5 Concentration

Abstract. Fine–particle pollution associated with haze threatens human health, especially in the North China Plain, where extremely high PM2.5 concentrations were frequently observed during winter. In this study, the WRF–Chem model coupled with an improved integrated process analysis scheme was used to investigate the formation and evolution mechanisms of a haze event happened over Beijing–Tianjin–Hebei (BTH) in December 2015, including examining the contributions of local emission and outside transport to the absolute PM2.5 concentration in BTH, and the contributions of each detailed physical or chemical process to the variations in the PM2.5 concentration. The influence mechanisms of aerosol radiative forcing (including aerosol direct and indirect effects) were also examined by using the process analysis. During the aerosol accumulation stage (December 20–22, Stage_1), the average near–surface PM2.5 concentration in BTH was 250.0 µg m−3, which was contributed by local emission of 42.3 % and outside transport of 36.6 %. During the aerosol dispersion stage (December 23–27, Stage_2), the average concentration of PM2.5 was 107.9 µg m−3. The contribution of local emission increased to 50.9 %, while the contribution of outside transport decreased to 24.3 %. The 24–h change (23:00LST minus 00:00LST) in the near–surface PM2.5 concentration was +50.4 µg m−3 during Stage_1 and −41.5 µg m−3 during Stage_2. Contributions of aerosol chemistry process and vertical mixing process to the 24–h change were +43.8 (+17.9) µg m−3 and −161.6 (−221.6) µg m−3 for Stage_1 (Stage_2), respectively. Small differences in contributions from other processes were found between Stage_1 and Stage_2, such as advection process, cloud chemistry process, and so on. Therefore, the PM2.5 increase over BTH during haze formation stage (Stage_1) was mainly attributed to strong production by aerosol chemistry process and weak removal by vertical mixing process. When aerosol radiative feedback was considered, the 24–h PM2.5 increase was enhanced by 9.6 µg m−3 during Stage_1, which could be mainly attributed to the contributions of vertical mixing process (+39.8 µg m−3), advection process (−38.6 µg m−3) and aerosol chemistry process (+5.1 µg m−3). The restrained vertical mixing could be the primary reason for the enhancement in near–surface PM2.5 increase when aerosol radiative forcing was considered.

scholarly journals Impact of the isoprene photochemical cascade on tropical ozone

2012 ◽  
Vol 12 (3) ◽  
pp. 1307-1325 ◽  
Author(s):  
F. Paulot ◽  
D. K. Henze ◽  
P. O. Wennberg
Keyword(s):  
Boundary Layer ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Regional Scale ◽  
Oxidative Capacity ◽  
Adjoint Sensitivity ◽  
Tropical Regions ◽  
Isoprene Nitrates ◽  
Near Shore ◽  
Considerable Work

Abstract. Tropical tropospheric ozone affects Earth's radiative forcing and the oxidative capacity of the atmosphere. Considerable work has been devoted to the study of the processes controlling its budget. Yet, large discrepancies between simulated and observed tropical tropospheric ozone remain. Here, we characterize some of the mechanisms by which the photochemistry of isoprene impacts the budget of tropical ozone. At the regional scale, we use forward sensitivity simulation to explore the sensitivity to the representation of isoprene nitrates. We find that isoprene nitrates can account for up to 70% of the local NOx = NO+NO2 sink. The resulting modulation of ozone can be well characterized by their net modulation of NOx. We use adjoint sensitivity simulations to demonstrate that the oxidation of isoprene can affect ozone outside of continental regions through the transport of NOx over near-shore regions (e.g., South Atlantic) and the oxidation of isoprene outside of the boundary layer far from its emissions regions. The latter mechanism is promoted by the simulated low boundary-layer oxidative conditions. In our simulation, ~20% of the isoprene is oxidized above the boundary layer in the tropics. Changes in the interplay between regional and global effect are discussed in light of the forecasted increase in anthropogenic emissions in tropical regions.

Experimental evidence of the lensing effect suppression for atmospheric black carbon containing brown coatings

2020 ◽  
Author(s):  
Vaios Moschos ◽  
Martin Gysel-Beer ◽  
Robin L. Modini ◽  
Joel C. Corbin ◽  
Dario Massabò ◽  
...  
Keyword(s):  
Black Carbon ◽  
Radiative Forcing ◽  
Wavelength Dependence ◽  
Chem Phys ◽  
Absorption Enhancement ◽  
Visible Spectroscopy ◽  
Scanning Mobility Particle Sizer ◽  
Absorption Data ◽  
Brown Carbon ◽  
Aerosol Radiative Forcing

<p>Accounting for the wavelength- and source-dependent optical absorption properties of the abundant light-absorbing organic (brown) carbon (BrC) and the mixing state of atmospheric black carbon (BC) are essential to reduce the large uncertainty in aerosol radiative forcing. Estimation of BrC absorption online by subtraction is highly uncertain and may be biased if not decoupled from the potential BC absorption enhancement (lensing) due to non-refractory (organic and inorganic) coating acquisition.</p><p>Here, the reported total particulate absorption is based on long-term, filter-based seven-wavelength Aethalometer (AE33 model) data, corrected for multiple scattering effects with Multi-Wavelength Absorbance Analyzer (5λ MWAA) measurements. Using ultraviolet-visible spectroscopy absorbance measurements along with particle size distributions obtained by a scanning mobility particle sizer, we have conducted Mie calculations to assess the importance of source-specific extractable particulate BrC (Moschos et al., 2018) versus BC absorption.</p><p>For the species-specific optical closure, the wavelength dependence of bare BC absorption is estimated using MWAA measurements upon successive filter extractions to remove the influence of BrC/coatings. The lensing contribution, supported by observations from field-emission scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy, is estimated at longer wavelengths using a refined proxy for the BC coating thickness. The approach is validated independently by applying a novel positive matrix factorization-based approach on the calibrated total AE33 absorption data.</p><p>Based on the observational constraints established in this study, we demonstrate for various distinct case studies that the interplay between lensing and BrC absorption results in lower than expected BC absorption at shorter wavelengths. This indicates that the volume additivity assumption is not valid for particulate absorption by internally mixed heterogeneous atmospheric aerosol populations. These comprehensive experimental analyses verify the BC lensing suppression predicted for simplified core-shell structures containing moderately absorbing BrC (Lack & Cappa, 2010). The implications discussed in this work are relevant for co-emitted species from biomass burning or aged plumes with high BrC to BC mass/absorption ratio.</p><p> </p><p><strong>References</strong></p><p>Moschos, V., Kumar, N. K., Daellenbach, K. R., Baltensperger, U., Prévôt, A. S. H., and El Haddad, I.: Source apportionment of brown carbon absorption by coupling ultraviolet-visible spectroscopy with aerosol mass spectrometry, Environ. Sci. Tech. Lett., 5, 302-308, https://doi.org/10.1021/acs.estlett.8b00118, 2018.</p><p>Lack, D. A. and Cappa, C. D.: Impact of brown and clear carbon on light absorption enhancement, single scatter albedo and absorption wavelength dependence of black carbon, Atmos. Chem. Phys., 10, 4207–4220, https://doi.org/10.5194/acp-10-4207-2010, 2010.</p>

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