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The study aimed to understand the optical properties of Black Carbon (BC) and radiative forcing over a data deficient Himalayan region focusing on critical zone observatory employing ground-based measurements by Aethalometer for BC and satellite retrieval techniques for optical properties during mid-May-June 2022 and January-May 2023. BC mass concentration ranged from 0.18 to 4.43 mu gm- 3, exhibit a mean of 1.47 +/- 0.83 mu gm- 3 with higher summer concentration (1.51 +/- 0.94 mu gm- 3) than winter (1.39 +/- 0.61 mu gm- 3). The average Absorption & Aring;ngstrom Exponent observed to be significantly higher than unity (1.77 +/- 0.31) over the studied high-altitude Himalayan region, suggesting the dominance of biomass-burning aerosol. Higher aethalometer derived compensation parameter (K) in winter suggesting locally originated BC while, lower K value in summer suggesting aged BC transported from Indo-Gangetic Plains. Optical properties calculated from Optical Properties of Aerosol and Cloud (OPAC) model are used in the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model to calculate the aerosol Direct Radiative Force (DRF). The entire studied period is characterized by the predominance of absorbing aerosols, particularly BC, increasing Aerosol Optical Depth, Asymmetric Parameters and decreasing Single Scattering Albedo, leading to a considerable increase in atmospheric radiative forcing (+0.9 Wm-2, top of atmosphere) and Heating Rate (0.36 KDay- 1). The mean radiative forcing within atmosphere during summer was higher (+14.29 Wm-2) relative to the winter (+12.00 Wm-2), emphasizing the impact of absorbing aerosols on regional warming and potential glacier melting in the Himalayas at a faster rate. Urgent policy consideration for the reduction of absorbing aerosols is highlighted, recognizing the critical roles of Black Carbon in the changing behaviour of Critical Zone observatory. The study's data serve as a valuable resource to understanding and addressing uncertainties in climate models, aiding effective policy implementation for Black Carbon reduction.

2024-07-10 Web of Science

The emission of black carbon (BC) particles, which cause atmospheric warming by affecting radiation budget in the atmosphere, is the result of an incomplete combustion process of organic materials. The recent wildfire event during the summer 2019-2020 in south-eastern Australia was unprecedented in scale. The wildfires lasted for nearly 3 months over large areas of the two most populated states of New South Wales and Victoria. This study on the emission and dispersion of BC emitted from the biomass burnings of the wildfires using the Weather Research Forecast-Chemistry (WRF-Chem) model aims to determine the extent of BC spatial dispersion and ground concentration distribution and the effect of BC on air quality and radiative transfer at the top of the atmosphere, the atmosphere and on the ground. The predicted aerosol concentration and AOD are compared with the observed data using the New South Wales Department of Planning and Environment (DPE) aethalometer and air quality network and remote sensing data. The BC concentration as predicted from the WRF-Chem model, is in general, less than the observed data as measured using the aethalometer monitoring network, but the spatial pattern corresponds well, and the correlation is relatively high. The total BC emission into the atmosphere during the event and the effect on radiation budget were also estimated. This study shows that the summer 2019-2020 wildfires affect not only the air quality and health impact on the east coast of Australia but also short-term weather in the region via aerosol interactions with radiation and clouds.

2023-04-01 Web of Science

The role of atmospheric aerosols in earth's radiative balance is crucial. A thorough knowledge about the spectral optical properties of various types of aerosols is necessary to quantify the net radiative forcing produced by aerosol-light interactions. In this study, we exploited an open-source inverse algorithm based on the Python-PyMieScatt survey iteration method, to retrieve the wavelength dependent Mie-equivalent complex refractive indices of ambient aerosols. This method was verified by obtaining the broadband complex refractive indices of monodisperse polystyrene latex spheres and polydisperse common salt aerosols, using laboratory data collected with a supercontinuum broadband cavity enhanced extinction spectrometer operating in the 420-540 nm wavelength range. Field measurements of ambient aerosol were conducted using a similar cavity enhanced extinction spectrometer (IBBCEES) operating in the wavelength range of 400-550 nm, a multi-wavelength aethalometer, and a scanning mobility particle sizer, in Changzhou city, People's Republic of China. The absorption coefficients for the entire wavelength range were retrieved using the absorption Angstrom exponents calculated from a pair of measured absorption coefficients at known wavelengths. The survey iteration method takes scattering and absorption coefficients, wavelength, and size distributions as inputs; and it calculates the Mie-equivalent wavelength dependent complex refractive index (RI = n +/- ik) and estimated errors. The retrieved field RI values ranged from 1.66 <= n <= 1.80 to 1.65 <= n <= 1.86 and from 0.036 <= k <= 0.038 to 0.062 <= k <= 0.067 in the wavelength range (400-550 nm), for low and high aerosol loading conditions, respectively. Additionally, we derived the spectral dependencies of scattering and absorption coefficients along with the n and k Angstrom exponents (AE). The nAE and kAE estimated values suggest a stronger wavelength dependence for aerosol light scattering compared to absorption, and a decreasing trend for the spectrally dependent single scattering albedo during both loading conditions. The extremum of errors in the retrieved n and k values were quantified by considering (a) uncertainties in input parameters in the broad spectral region (400-550 nm), (b) using CAPS extinction values at 530 nm and (c) an estimated size distribution incorporating the coarse particles (at 530 nm).

2022-03-01 Web of Science

Accurate estimation of black carbon (BC) from the widely used optical attenuation technique is important for the reliable assessment of their climatic impact. The optical instruments use Mass Absorption Cross- (MAC) for converting light attenuation records to BC mass concentrations and Aethalometer is a widely used optical instrument for BC estimation. Several studies have shown large variability in MAC values. It is thus necessary to examine the accuracy and consistency of MAC values obtained using Aethalometer over distinct geographic locations and seasons. In the present study, MAC values are derived using simultaneous observations (2014-2017) from an EC-OC analyzer and an Aethalometer (AE-42) over a high altitude central Himalayan site at Nainital (29.4(o)N, 79.5(o)E, 1958 a.m.s.l). The observations reveal that the annual mean value of MAC (5.03 +/- 0.03 m(2)g(- 1) at 880nm) is significantly lower than the constant value used by the manufacturer (16.6 m(2)g(- 1) at 880nm). The estimated MAC values also showed significant seasonal variation, spanning over a range from 3.7 to 6.6 m(2)g(- 1). It is found that the seasonal variability of elemental carbon (EC), air mass variation and meteorological parameters play an important role in the changes in MAC values over this region. Multi-wavelength determination of MAC shows the contribution of absorption by species other than EC at shorter wavelengths. MAC does not show a clear diurnal variation, unlike EC and absorption coefficient. The slope of EC vs. corrected equivalent black carbon (eBC) showed a significant improvement during all seasons when compared with uncorrected eBC. This lends credibility to the fact that the use of site-specific MAC leads to more reliable estimates of eBC over the central Himalayan region. It is found that, instead of using the site specific MAC value, had we used the one supplied by the instrument, we would have underestimated the radiative forcing by about 7.8Wm(- 2) which amounts to a reduction by 24 %.

2022-02-01 Web of Science

Portable aethalometers are commonly used for online measurements of light-absorbing carbonaceous particles (LAC). However, they require strict calibration. In this study, the performance of a micro-aethalometer (MA200 with polytetrafluoroethylene filter) in charactering brown carbon aerosol (BrC) absorption was evaluated in comparison with reference materials and techniques that included bulk solution absorbance and Mie-theory based particle extinction retrieval via broadband cavity enhanced spectrometer (BBCES). Continuous-wavelength resolved (300-650 nm) imaginary refractive index (k(BrC)) was derived with these methods for various BrC proxies and standard materials representing a wide range of sources and absorbing abilities, including the strongly absorbing nigrosin, pahokee peat fluvic acid (PPFA), tar aerosol from wood pyrolysis, humic-like substance (HULIS) separated from wood smoldering burning emissions, and secondary organic aerosols (SOA) from photochemical oxidation of indole and naphthalene in the presence of NOx. The BrC and nigrosin optical results by bulk solution absorption are comparable with the properties retrieved from BBCES. The MA200 raw measurements provide reliable absorption Angstrom exponent (AAE) but overestimate kBrC largely. The parameterized overestimates against reference methods depend on light absorption strength, so that the MA200 overestimates more for the less absorbing BrC. The correction factor for MA200 can be expressed well as an exponential function of kBrC or particle single scattering albedo (SSA), and also as a power-law function of the MA200 raw results derived BrC mass absorption efficiency (MAE). The ensemble correction factor regressed for all these BrC and nigrosin is 2.8 based on bulk absorption and 2.7 using BBCES result as reference. Simple radiative forcing (SRF) calculations for different scenarios using the correction for MA200, show consistent SRF when using the aethalometer results after the k(BrC)-dependent correction. (C) 2021 Elsevier B.V. All rights reserved.

2021-07-10 Web of Science

Biomass burnings either due to Hazards Reduction Burnings (HRBs) in late autumn and early winter or bushfires during summer periods in various part of the world (e.g., CA, USA or New South Wales, Australia) emit large amount of gaseous pollutants and aerosols. The emissions, under favourable meteorological conditions, can cause elevated atmospheric particulate concentrations in metropolitan areas and beyond. One of the pollutants of concern is black carbon (BC), which is a component of aerosol particles. BC is harmful to health and acts as a radiative forcing agent in increasing the global warming due to its light absorption properties. Remote sensing data from satellites have becoming increasingly available for research, and these provide rich datasets available on global and local scale as well as in situ aethalometer measurements allow researchers to study the emission and dispersion pattern of BC from anthropogenic and natural sources. The Department of Planning, Industry and Environment (DPIE) in New South Wales (NSW) has installed recently from 2014 to 2019 a total of nine aethalometers to measure BC in its state-wide air quality network to determine the source contribution of BC and PM2.5(particulate Matter less than 2.5 mu m in diameter) in ambient air from biomass burning and anthropogenic combustion sources. This study analysed the characteristics of spatial and temporal patterns of black carbon (BC) in New South Wales and in the Greater Metropolitan Region (GMR) of Sydney, Australia, by using these data sources as well as the trajectory HYSPLIT (Hybrid Single Particle Lagrangian Integrated Trajectory) modelling tool to determine the source of high BC concentration detected at these sites. The emission characteristics of BC in relation to PM(2.5)is dependent on the emission source and is analysed using regression analysis of BC with PM(2.5)time series at the receptor site for winter and summer periods. The results show that, during the winter, correlation between BC and PM(2.5)is found at nearly all sites while little or no correlation is detected during the summer period. Traffic vehicle emission is the main BC emission source identified in the urban areas but was less so in the regional sites where biomass burnings/wood heating is the dominant source in winter. The BC diurnal patterns at all sites were strongly influenced by meteorology.

2020-06-01 Web of Science

Black carbon (BC) is an essential climate forcer in the atmosphere. Large uncertainties remain in BC's radiative forcing estimation by models, partially due to the limited measurements of BC vertical distributions near the surface layer. We conducted time-resolved vertical profiling of BC using a 356-m meteorological tower in Shenzhen, China. Five micro-aethalometers were deployed at different heights (2, 50, 100, 200, and 350 m) to explore the temporal dynamics of BC vertical profile in the highly urbanized areas. During the observation period (December 6-15, 2017), the average equivalent BC (eBC) concentrations were 6.6 +/- 3.6, 5.4 +/- 3.3, 5.9 +/- 2.8, 5.2 +/- 1.8, and 4.9 +/- 1.4 mu g m(-3), from 2 to 350 m, respectively. eBC temporal variations at different heights were well correlated. eBC concentrations generally decreased with height. At all five heights, eBC diurnal variations exhibited a bimodal pattern, with peaks appearing at 09:00-10:00 and 19:00-21:00. The magnitudes of these diurnal peaks decreased with height, and the decrease was more pronounced for the evening peak. eBC episodes were largely initiated by low wind speeds, implying that wind speed played a key role in the observed eBC concentrations. eBC wind-rose analysis suggested that elevated eBC events at different heights originate from different directions, which suggested contributions from local primary emission plumes. Air masses from central China exhibited much higher eBC levels than the other three backward trajectory clusters found herein. The absorption angstrom ngstrom exponent (AAE(375-880)) showed clear diurnal variations at 350 m and increased slightly with height.

2020-05-01 Web of Science

While brown carbon (BrC) might play a substantially important role in radiative forcing, an estimation of its light absorption contribution with high-time resolution is still challenging. In this study, a multi-wavelength (370-950 nm) Aethalometer was applied to obtain the wavelength dependent light absorption coefficient (sigma(abs)) of aerosols both before and after being heated to 250 degrees C. An improved absorption angstrom ngstrom exponent (AAE)-based method was developed to evaluate the contribution of BrC to light absorption at a wavelength of 370 nm (sigma(abs,BrC)/sigma(abs,370nm)). The sigma(abs,BC) at 370 nm was determined from the field measured AAE values for the wavelengths from 880 to 950 nm with a one-hour resolution. The simultaneous measurements of heated aerosols help confirm the negligible influence of BrC on the sigma(abs) values across the range of 880-950 nm. Meanwhile, sigma(abs,BrC)/sigma(abs,370nm) was also estimated with previously reported methods by assuming that the AAE was equal to 1 (Method I) as well as a new approach based on the light absorption enhancement (Method II). While the estimated sigma(abs,BrC)/sigma(abs,370nm) based on our developed method and Method I is highly correlated (r(2) = 0.78), the difference could be as large as > 20% on average. The obtained mean sigma(abs,BrC)/sigma(abs,370nm) was negative with Method II, a indicating the net production of BrC when the aerosols were heated. The difference between the values for sigma(abs,BrC)/sigma(abs,370nm) obtained by our developed method and by Method II was similar to 40% on average and much higher (> 50%) during the noon hour, when secondary organic aerosols and sulfate were abundant. We propose that it is more suitable to use an AAE around 0.7 for pure BC to evaluate the contribution of BrC to light absorption in the PRD region. The developed method thus helps improve our understanding of the light absorption and climate forcing of BrC.

2019-01-01 Web of Science

In this study, real-time absorption coefficients of carbonaceous species in PM2.5 was observed using a dual-spot 7-wavelength Aethalometer between November 1, 2016 and December 31, 2017 at an urban site of Gwangju. In addition, 24-hr integrated PM2.5 samples were simultaneously collected at the same site and analyzed for organic carbon and elemental carbon (OC and EC) using the thermal-optical transmittance protocol. A main objective of this study was to estimate mass absorption cross (MAC) values of black carbon (BC) particles at the study site using the linear regression between aethalometer-based absorption coefficient and filter-based EC concentration. BC particles observed at 880 nm is mainly emitted from combustion of fossil fuels, and their concentration is typically reported as equivalent BC concentration (eBC). eBC concentration calculated using MAC value of 7.77 m(2)/g at wavelength of 880 nm, which was proposed by a manufacturer, ranged from 0.3 to 7.4 mu g/m(3) with an average value of 1.9 +/- 1.2 mu g/m(3), accounting for 7.3% (1.5 similar to 20.9%) of PM2.5. The relationship between aerosol absorption coefficients at 880 nm and EC concentrations provided BC MAC value of 15.2 m(2)/g, ranging from 11.4 to 16.2 m(2)/g. The eBC concentrations calculated using the estimated MAC of 15.2 m(2)/g were significantly lower than those reported originally from aethalometer, and ranged from 0.2 to 3.8 mu g/m(3), with an average of 1.0 +/- 0.6 mu g/m(3), accounting for 3.7% of PM2.5 (0.8 similar to 10.7%). Result from this study suggests that if the MAC value recommended by the manufacturer is applied to calculate the equivalent BC concentration and radiative forcing due to BC absorption, they would result in significant errors, implying investigation of an unique MAC value of BC particles at a study site.

2018-10-01 Web of Science

Black carbon (BC) is a primary aerosol emitted directly into the atmosphere from incomplete combustion. It absorbs incoming solar radiation and outgoing terrestrial radiation, which has significant implications to aerosol radiative forcing. Aethalometer employs optical attenuation technique to measure real-time BC mass concentrations. BC mass concentration measured using a single spot aethalometer (AE31) can be significantly uncertain due to filter loading effect. A modified version of AE31, namely, a dual spot aethalometer (AE33), uses a real-time loading effect compensation algorithm and measures BC mass concentrations. BC mass concentrations measured using single and dual spot aethalometers over an urban location are analysed. BC mass concentration from AE33 is higher (11%) than BC measured by post processed loading effect compensated AE31 data. Daily averaged BC mass concentration measured by AE31 and AE33 shows a very good linear agreement (coefficient of determination (0.98), and a small zero offset (0.22)). Aerosol absorption coefficients show an average difference of 28.5% between the two aethalometers. Aerosol absorption coefficient is utilised with nephelometer measured aerosol scattering coefficients to compute single scattering albedo (SSA). SSA (550 nm) estimated from the AE33 is always higher (similar to 8%) than AE31. Estimates of aerosol radiative forcing show that when SSA changes from 0.65 to 0.70 over urban regions the atmospheric warming changes by 10%, while when SSA changes from 0.85 to 0.90 the atmospheric warming changes by 25%. This study highlights the non-linear relation between SSA and aerosol forcing, and reveals how crucial it is to determine single scattering albedo accurately in order to reduce the uncertainty in aerosol radiative forcing estimate.

2018-05-01 Web of Science
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