Source Quantification of South Asian Black Carbon Aerosols with Isotopes and Modeling.
ABSTRACT: Black carbon (BC) aerosols perturb climate and impoverish air quality/human health-affecting ?1.5 billion people in South Asia. However, the lack of source-diagnostic observations of BC is hindering the evaluation of uncertain bottom-up emission inventories (EIs) and thereby also models/policies. Here, we present dual-isotope-based (?14C/?13C) fingerprinting of wintertime BC at two receptor sites of the continental outflow. Our results show a remarkable similarity in contributions of biomass and fossil combustion, both from the site capturing the highly populated highly polluted Indo-Gangetic Plain footprint (IGP; ?14C-fbiomass = 50 ± 3%) and the second site in the N. Indian Ocean representing a wider South Asian footprint (52 ± 6%). Yet, both sites reflect distinct ?13C-fingerprints, indicating a distinguishable contribution of C4-biomass burning from peninsular India (PI). Tailored-model-predicted season-averaged BC concentrations (700 ± 440 ng m-3) match observations (740 ± 250 ng m-3), however, unveiling a systematically increasing model-observation bias (+19% to -53%) through winter. Inclusion of BC from open burning alone does not reconcile predictions (fbiomass = 44 ± 8%) with observations. Direct source-segregated comparison reveals regional offsets in anthropogenic emission fluxes in EIs, overestimated fossil-BC in the IGP, and underestimated biomass-BC in PI, which contributes to the model-observation bias. This ground-truthing pinpoints uncertainties in BC emission sources, which benefit both climate/air-quality modeling and mitigation policies in South Asia.
Project description:A majority of black carbon (BC) emitted to the atmosphere in the Indo-Gangetic Plain (IGP) region is from burning biomass fuel used in traditional, open-design cookstoves. However, BC and particulate matter (PM) household emissions are not well characterized. Household emission information is needed to develop emission profiles to validate regional climate change models and serve as a baseline for assessing the impact of adopting improved stove technology. This paper presents field-based household PM and BC exfiltration (amount exiting) estimates from village homes in rural Nepal that utilize traditional, open-design cookstoves. Use of these stoves resulted in a 26% mean PM exfiltration, ranging from 6% to 58%. This is a significant departure from an 80% estimate cited in previous reports. Furthermore, having a window/door resulted in an 11% increase in exfiltration when an opening was present, while fuel type had a marginally significant impact on emission. Air-exchange rates (AER) were determined with average (95% CI) AER of 12 (10-14) per hour, consistent with previous studies. In addition, BC to PM2.5 mass-ratio composition during cooking was ascertained, with an average (95% CI) of 31% (24-39), agreeing with previous biomass fuel emission composition literature.
Project description:Black carbon (BC) contributes to Arctic climate warming, yet source attributions are inaccurate due to lacking observational constraints and uncertainties in emission inventories. Year-round, isotope-constrained observations reveal strong seasonal variations in BC sources with a consistent and synchronous pattern at all Arctic sites. These sources were dominated by emissions from fossil fuel combustion in the winter and by biomass burning in the summer. The annual mean source of BC to the circum-Arctic was 39 ± 10% from biomass burning. Comparison of transport-model predictions with the observations showed good agreement for BC concentrations, with larger discrepancies for (fossil/biomass burning) sources. The accuracy of simulated BC concentration, but not of origin, points to misallocations of emissions in the emission inventories. The consistency in seasonal source contributions of BC throughout the Arctic provides strong justification for targeted emission reductions to limit the impact of BC on climate warming in the Arctic and beyond.
Project description:Black carbon (BC) not only warms the atmosphere but also affects human health. The nationwide lockdown due to the Coronavirus Disease 2019 (COVID-19) pandemic led to a major reduction in human activity during the past 30 years. Here, the concentration of BC in the urban, urban-industry, suburb, and rural areas of a megacity Hangzhou were monitored using a multiwavelength Aethalometer to estimate the impact of the COVID-19 lockdown on BC emissions. The citywide BC decreased by 44% from 2.30 to 1.29 ?g/m<sup>3</sup> following the COVID-19 lockdown period. The source apportionment based on the Aethalometer model shows that vehicle emission reduction responded to BC decline in the urban area and biomass burning in rural areas around the megacity had a regional contribution of BC. We highlight that the emission controls of vehicles in urban areas and biomass burning in rural areas should be more efficient in reducing BC in the megacity Hangzhou.
Project description:WRF-Chem and a modified version of the ECLIPSE 5a emission inventory were used to investigate the sources impacting black carbon (BC) deposition to the Himalaya, Karakoram, and Hindu Kush (HKHK) region. This work extends previous studies by simulating deposition to the HKHK region not only under current conditions, but also in the 2040-2050 period under two realistic emission scenarios and in three different phases of the El Niño-Southern Oscillation (ENSO). Under current conditions, sources from outside our South Asian modelling domain have a similar impact on total BC deposition to the HKHK region (35-87%, varying with month) as South Asian anthropogenic sources (13-62%). Industry (primarily brick kilns) and residential solid fuel burning combined account for 45-66% of the in-domain anthropogenic BC deposition to the HKHK region. Under a no further control emission scenario for 2040-2050, the relative contributions to BC deposition in the HKHK region are more skewed toward in-domain anthropogenic sources (45-65%) relative to sources outside the domain (26-52%). The in-domain anthropogenic BC deposition has significant contributions from industry (32-42%), solid fuel burning (17-28%), and diesel fuel burning (17-27%). Under a scenario in which emissions in South Asia are mitigated, the relative cotribution from South Asian anthropogenic sources is significantly reduced to 11-34%. The changes due to phase of ENSO do not seem to follow consistent patterns with ENSO. Future work will use the high-resolution deposition maps developed here to determine the impact of different sources of BC on glacier melt and water availability in the region.
Project description:Although elevated surface ozone (O3) concentrations are observed in many areas within southern Africa, few studies have investigated the regional atmospheric chemistry and dominant atmospheric processes driving surface O3 formation in this region. Therefore, an assessment of comprehensive continuous surface O3 measurements performed at four sites in continental South Africa was conducted. The regional O3 problem was evident, with O3 concentrations regularly exceeding the South African air quality standard limit, while O3 levels were higher compared to other background sites in the Southern Hemisphere. The temporal O3 patterns observed at the four sites resembled typical trends for O3 in continental South Africa, with O3 concentrations peaking in late winter and early spring. Increased O3 concentrations in winter were indicative of increased emissions of O3 precursors from household combustion and other low-level sources, while a spring maximum observed at all the sites was attributed to increased regional biomass burning. Source area maps of O3 and CO indicated significantly higher O3 and CO concentrations associated with air masses passing over a region with increased seasonal open biomass burning, which indicated CO associated with open biomass burning as a major source of O3 in continental South Africa. A strong correlation between O3 on CO was observed, while O3 levels remained relatively constant or decreased with increasing NO x , which supports a VOC-limited regime. The instantaneous production rate of O3 calculated at Welgegund indicated that ~ 40 % of O3 production occurred in the VOC-limited regime. The relationship between O3 and precursor species suggests that continental South Africa can be considered VOC limited, which can be attributed to high anthropogenic emissions of NO x in the interior of South Africa. The study indicated that the most effective emission control strategy to reduce O3 levels in continental South Africa should be CO and VOC reduction, mainly associated with household combustion and regional open biomass burning.
Project description:A nationwide lockdown was imposed in India due to COVID-19 pandemic in five phases from 25th March to May 31, 2020. The lockdown restricted major anthropogenic activities, primarily vehicular and industrial, thereby reducing the particulate matter concentration. This work investigates the variation in Black Carbon (BC) concentration and its sources (primarily Fossil Fuel (ff) burning and Biomass Burning (bb)) over Delhi from 18th February to July 31, 2020, covering one month of pre-lockdown phase, all the lockdown phases, and two months of successive lockdown relaxations. The daily average BC concentration varied from 0.22 to 16.92 μg/m<sup>3</sup>, with a mean value of 3.62 ± 2.93 μg/m<sup>3</sup>. During Pre-Lockdown (PL, 18th Feb-24th March 2020), Lockdown-1 (L1, 25th March-14th April 2020), Lockdown-2 (L2, 15th April-3rd May 2020), Lockdown-3 (L3, 4th-17th May 2020), Lockdown-4 (L4, 18th-31st May 2020), Unlock-1 (UN1, June 2020), and Unlock-2 (UN2, July 2020) the average BC concentrations were 7.93, 1.73, 2.59, 3.76, 3.26, 2.07, and 2.70 μg/m<sup>3</sup>, respectively. During the lockdown and unlock phases, BC decreased up to 78% compared to the PL period. The BC source apportionment studies show that fossil fuel burning was the dominant BC source during the entire sampling period. From L1 to UN2 an increasing trend in BC<sub>ff</sub> contribution was observed (except L3) due to the successive relaxations given to anthropogenic activities. BC<sub>ff</sub> contribution dipped briefly during L3 due to the intensive crop residue burning events in neighboring states. CWT analysis showed that local emission sources were the dominant contributors to BC concentration over Delhi.
Project description:Carbonaceous aerosols, which are emitted from biomass burning, significantly contribute to the Earth's radiation balance. Radiative forcing caused by biomass burning has been poorly qualified, which is largely attributed to uncertain absorption enhancement values (E<sub>abs</sub>) of black carbon (BC) aerosols. Laboratory measurements and theoretical modelling indicate a significant value of E<sub>abs</sub>; but this enhancement is observed to be negligible in the ambient environment, implying that models may overestimate global warming due to BC. Here, we present an aggregate model integrating BC aerosol ensembles with different morphologies and mixing states and report a quantitative analysis of the BC E<sub>abs</sub> from different combustion states during biomass burning. We show that the BC E<sub>abs</sub> produced by flaming combustion may be up to two times more than those produced by smouldering combustion, suggesting that the particle morphology and mixing state of freshly emitted BC aerosols is an important source of the contrasting values of E<sub>abs</sub>. The particle morphology of freshly emitted BC aerosols is widely assumed to be bare in models, which is rare in the ambient environment and leads to small estimates of E<sub>abs</sub> by field observations. We conclude that the exact description of freshly emitted carbonaceous aerosols plays an important role in constraining aerosol radiative forcing.
Project description:Fine particulate matter (PM2.5, aerodynamic diameter ?2.5?µm) impacts the climate, reduces visibility and severely influences human health. The Indo-Gangetic Plain (IGP), home to about one-seventh of the world's total population and a hotspot of aerosol loading, observes strong enhancements in the PM2.5 concentrations towards winter. We performed high-resolution (12?km × 12?km) atmospheric chemical transport modeling (WRF-Chem) for the post-monsoon to winter transition to unravel the underlying dynamics and influences of regional emissions over the region. Model, capturing the observed variations to an extent, reveals that the spatial distribution of PM2.5 having patches of enhanced concentrations (?100 µgm-3) during post-monsoon, evolves dramatically into a widespread enhancement across the IGP region during winter. A sensitivity simulation, supported by satellite observations of fires, shows that biomass-burning emissions over the northwest IGP play a crucial role during post-monsoon. Whereas, in contrast, towards winter, a large-scale decline in the air temperature, significantly shallower atmospheric boundary layer, and weaker winds lead to stagnant conditions (ventilation coefficient lower by a factor of ~4) thereby confining the anthropogenic influences closer to the surface. Such changes in the controlling processes from post-monsoon to winter transition profoundly affect the composition of the fine aerosols over the IGP region. The study highlights the need to critically consider the distinct meteorological processes of west-to-east IGP and changes in dominant sources from post-monsoon to winter in the formulation of future pollution mitigation policies.
Project description:Biomass burning aerosols mainly consist of black carbon (BC) and organic aerosols (OAs), and some of OAs are brown carbon (BrC). This study simulates the colors of BrC, BC and their mixture with scattering OAs in the ambient atmosphere by using a combination of light scattering simulations, a two-stream radiative transfer model and a RGB (Red, Green, Blue) color model. We find that both BCs and tar balls (a class of BrC) appear brownish at small particle sizes and blackish at large sizes. This is because the aerosol absorption Ångström exponent (AAE) largely controls the color and larger particles give smaller AAE values. At realistic size distributions, BCs look more blackish than tar balls, but still exhibit some brown color. However, when the absorptance of aerosol layer at green wavelength becomes larger than approximately 0.8, all biomass burning aerosols look blackish. The colors for mixture of purely scattering and absorptive carbonaceous aerosol layers in the atmosphere are also investigated. We suggest that the brownishness of biomass burning aerosols indicates the amount of BC/BrC as well as the ratio of BC to BrC.
Project description:A present challenge in fire ecology is to optimize management techniques so that ecological services are maximized and C emissions minimized. Here, we modeled the effects of different prescribed-burning rotation intervals and wildfires on carbon emissions (present and future) in British moorlands. Biomass-accumulation curves from four Calluna-dominated ecosystems along a north-south gradient in Great Britain were calculated and used within a matrix-model based on Markov Chains to calculate above-ground biomass-loads and annual C emissions under different prescribed-burning rotation intervals. Additionally, we assessed the interaction of these parameters with a decreasing wildfire return intervals. We observed that litter accumulation patterns varied between sites. Northern sites (colder and wetter) accumulated lower amounts of litter with time than southern sites (hotter and drier). The accumulation patterns of the living vegetation dominated by Calluna were determined by site-specific conditions. The optimal prescribed-burning rotation interval for minimizing annual carbon emissions also differed between sites: the optimal rotation interval for northern sites was between 30 and 50 years, whereas for southern sites a hump-backed relationship was found with the optimal interval either between 8 to 10 years or between 30 to 50 years. Increasing wildfire frequency interacted with prescribed-burning rotation intervals by both increasing C emissions and modifying the optimum prescribed-burning interval for minimum C emission. This highlights the importance of studying site-specific biomass accumulation patterns with respect to environmental conditions for identifying suitable fire-rotation intervals to minimize C emissions.