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Light absorption potential of water-soluble organic aerosols in the two polluted urban locations in the central Indo-Gangetic Plain
2022
Rajeev, Pradhi | Choudhary, Vikram | Chakraborty, Abhishek | Singh, Gyanesh Kumar | Gupta, Tarun
PM₂.₅ (particulate matter having aerodynamic diameter ≤2.5 μm) samples were collected during wintertime from two polluted urban sites (Allahabad and Kanpur) in the central Indo-Gangetic Plain (IGP) to comprehend the sources and atmospheric transformations of light-absorbing water-soluble organic aerosol (WSOA). The aqueous extract of each filter was atomized and analyzed in a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Water-soluble organic carbon (WSOC) and WSOA concentrations at Kanpur were ∼1.2 and ∼1.5 times higher than that at Allahabad. The fractions of WSOC and secondary organic carbon (SOC) to total organic carbon (OC) were also significantly higher ∼53% and 38%, respectively at Kanpur compared to Allahabad. This indicates a higher abundance of oxidized WSOA at Kanpur. The absorption coefficient (bₐbₛ₋₃₆₅) of light-absorbing WSOA measured at 365 nm was 46.5 ± 15.5 Mm⁻¹ and 73.2 ± 21.6 Mm⁻¹ in Allahabad and Kanpur, respectively, indicating the dominance of more light-absorbing fractions in WSOC at Kanpur. The absorption properties such as mass absorption efficiency (MAE₃₆₅) and imaginary component of refractive index (kₐbₛ₋₃₆₅) at 365 nm at Kanpur were also comparatively higher than Allahabad. The absorption forcing efficiency (Abs SFE; indicates warming effect) of WSOA at Kanpur was ∼1.4 times higher than Allahabad. Enhancement in light absorption capacity was observed with the increase in f44/f43 (fraction of m/z 44 (f44) to 43 (f43) in organic mass spectra) and O/C (oxygen to carbon) ratio of WSOA at Kanpur while no such trend was observed for the Allahabad site. Moreover, the correlation between carbon fractions and light absorption properties suggested the influence of low-volatile organic compounds (OC3 + OC4 fraction obtained from thermal/optical carbon analyzer) in increasing the light absorption capacity of WSOA in Kanpur.
显示更多 [+] 显示较少 [-]Brown carbon light absorption over an urban environment in northern peninsular Southeast Asia
2021
Pani, Shantanu Kumar | Lin, Neng-Huei | Griffith, Stephen M. | Chantara, Somporn | Lee, Chung-Te | Thepnuan, Duangduean | Tsai, Ying I.
Light-absorbing organic carbon (or brown carbon, BrC) has been recognized as a critical driver in regional-to-global climate change on account of its significant contribution to light absorption. BrC sources vary from primary combustion processes (burning of biomass, biofuel, and fossil fuel) to secondary formation in the atmosphere. This paper investigated the light-absorbing properties of BrC such as site-specific mass absorption cross-section (MACBᵣC), absorption Ångström exponent (AAEBᵣC), and the absorbing component of the refractive index (kBᵣC) by using light absorption measurements from a 7-wavelength aethalometer over an urban environment of Chiang Mai, Thailand in northern peninsular Southeast Asia (PSEA), from March to April 2016. The contribution of BrC to total aerosol absorption (mean ± SD) was 46 ± 9%, 29 ± 7%, 24 ± 6%, 20 ± 4%, and 15 ± 3% at 370, 470, 520, 590, and 660 nm, respectively, highlighting the significant influence of BrC absorption on the radiative imbalance over northern PSEA. Strong and significant associations between BrC light absorption and biomass-burning (BB) organic tracers highlighted the influence of primary BB emissions. The median MACBᵣC and kBᵣC values at 370 nm were 2.4 m² g⁻¹ and 0.12, respectively. The fractional contribution of solar radiation absorbed by BrC relative to BC (mean ± SD) in the 370–950 nm range was estimated to be 34 ± 7%, which can significantly influence the regional radiation budget and consequently atmospheric photochemistry. This study provides valuable information to understand BrC absorption over northern PSEA and can be used in model simulations to reassess the regional climatic impact with greater accuracy.
显示更多 [+] 显示较少 [-]Influence of chemical aging on physico-chemical properties of mineral dust particles: A case study of 2016 dust storms over Delhi
2020
Goel, Vikas | Mishra, Sumit K. | Pal, Prabir | Ahlawat, Ajit | Vijayan, Narayanasamy | Jain, Srishti | Sharma, C. (Chhemendra)
The physico-chemical properties of dust particles collected During Dust Storm (DDS) and After Dust Storm (ADS) events were studied using Scanning Electron Microscope coupled with Energy Dispersive X-ray Spectroscopy (SEM-EDS), X-ray Fluorescence Spectroscopy (XRF) and X-ray Photoelectron Spectroscopy (XPS). Morphological and compositional change in dust particles were observed as they react with the anthropogenic pollutants present in the urban environment. The calcite rich particles were observed to transform into calcium chloride, calcium nitrate, and calcium sulfate on reacting with the chlorides, nitrates, and sulfates present in the urban atmosphere. The frequency distributions of Aspect Ratio (AR) for the DDS and ADS particles were observed to be bimodal (mode peaks at 1.2 and 1.5) and monomodal (mode peak at 1.1), respectively. The highly irregular shaped solid dust particles were observed to transform into nearly spherical semisolid particles in the urban environment. XPS analysis confirms the high concentration of oxides, nitrates, and chlorides at the surface of ADS samples which show the signatures of mineral dust particles aging. Species with a high value of imaginary part of refractive index (like Cr metal, Fe metal, Cr₂O₃, FeO, Fe₂O₃) were observed at the surface of dust particles. At 550 nm wavelength, the light-absorbing potential of the observed species along with black carbon (BC) was found to vary in the order; Cr metal > Fe metal > Cr₂O₃> FeO > BC > Fe₂O₃> FeOOH. The presence of the aforementioned species on the surface of ADS particles will tremendously affect the particle optical and radiative properties compared to that of DDS particles. The present work could reduce the uncertainty in the radiation budget estimations of mineral dust and assessment of their climatic impacts over Delhi.
显示更多 [+] 显示较少 [-]Columnar aerosol properties and radiative effects over Dushanbe, Tajikistan in Central Asia
2020
Rupakheti, Dipesh | Rupakheti, Maheswar | Abdullaev, Sabur F. | Yin, Xiufeng | Kang, Shichang
This paper presents the results of the study on columnar aerosol optical and physical properties and radiative effects directly observed over Dushanbe, the capital city of Tajikistan, a NASA AERONET site (equipped with a CIMEL sunphotometer) in Central Asia. The average aerosol optical depth (AOD) and Ångström exponent (AE) during the observation period from July 2010 to April 2018 were found to be 0.28 ± 0.20 and 0.82 ± 0.40, respectively. The highest seasonal AOD (0.32 ± 0.24), accompanied by the lowest average AE (0.61 ± 0.25) and fine-mode fraction in AOD (0.39), was observed during summer due to the influence of coarse particles like dust from arid regions. Fine particles were found in significant amounts during winter. The ‘mixed aerosol’ was identified as the dominant aerosol type with presence of ‘dust aerosol’ during summer and autumn seasons. Aerosol properties like volume size distribution, single scattering albedo, asymmetry parameter and refractive index suggested the influence of coarse particles (during summer and autumn). Most of the air masses reaching this site transported local and regional emissions, including from beyond Central Asia, explaining the presence of various aerosol types in Dushanbe’s atmosphere. The seasonal aerosol radiative forcing efficiency (ARFE) in the atmosphere was found high (>100 Wm⁻²) and consistent throughout the year. Consequently, this resulted in similar seasonally coherent high atmospheric solar heating rate (HR) of 1.5 K day⁻¹ during summer-autumn-winter, and ca. 0.9 K day⁻¹ during spring season. High ARFE and HR values indicate that atmospheric aerosols could exert significant implications to regional air quality, climate and cryosphere over the central Asian region and downwind Tianshan and Himalaya-Tibetan Plateau mountain regions with sensitive ecosystems.
显示更多 [+] 显示较少 [-]The climatology of aerosol optical thickness and radiative effects in Southeast Asia from 18-years of ground-based observations
2019
Khan, Rehana | Kumar, Kanike Raghavendra | Zhao, Tianliang
The present study utilizes 18 years of long-term (2001–2018) data collected from six active AERONET sites over the Indo-Gangetic Plain (IGP) and the North China Plain (NCP) areas in Southeast Asia. The annual mean (±SD) aerosol optical thickness at 440 nm (AOT₄₄₀) was found high at XiangHe (0.92 ± 0.69) and Taihu (0.90 ± 0.51) followed by Beijing (0.81 ± 0.69), Lahore (0.81 ± 0.43), and Kanpur (0.73 ± 0.35) and low at Karachi (0.52 ± 0.23). Seasonally, high AOT₄₄₀ with corresponding high Ångström exponent (ANG₄₄₀₋₈₇₀) noticed during JJA for all sites, except Kanpur, suggesting the dominance of fine-mode particles, generally associated with large anthropogenic emissions. Climatologically, an increasing (decreasing) trend was observed over IGP (NCP) sites, with the highest (lowest) percentage of departures in AOT₄₄₀ found over Beijing (Karachi). We further identified major aerosol types which showed the dominance of biomass burning, urban-industrial followed by the mixed type of aerosols. In addition, single scattering albedo (SSA), asymmetry parameter (ASP), volume size distribution (VSD), and complex aerosol refractive index (RI) showed significant temporal and spectral changes, illustrating the complexity of aerosol types. At last, the annual mean direct aerosol radiative forcing at the top, bottom, and within the atmosphere for all sites were found in the range from −17.36 ± 3.75 to −45.17 ± 4.87 W m⁻², -64.6 ± 4.86 to −93.7 ± 10.27 W m⁻², and 40.5 ± 6.43 to 68.25 ± 7.26 W m⁻², respectively, with an averaged atmospheric heating rate of 0.9–2.3 K day⁻¹. A large amount of anthropogenic aerosols showed a significant effect of heating (cooling) on the atmosphere (surface) results obviously, due to an increased rate of atmospheric heating. Therefore, the thermodynamic effects of anthropogenic aerosols on the atmospheric circulation and its structure should be taken into consideration for future study over the experimental sites.
显示更多 [+] 显示较少 [-]Changes in column aerosol optical properties during extreme haze-fog episodes in January 2013 over urban Beijing
2016
Yu, Xingna | Kumar, K Raghavendra | Lu, Rui | Ma, Jia
Several dense haze-fog (HF) episodes were occurred in the North China Plain (NCP), especially over Beijing in January 2013 characterized by a long duration, a large influential region, and an extremely high PM2.5 values (>500 μg m−3). In this study, we present the characteristics of aerosol optical properties and radiative forcing using Cimel sun-sky radiometer measurements during HF and no haze-fog (NHF) episodes occurred over Beijing during 1–31 January, 2013. The respective maximum values of daily mean aerosol optical depth at 440 nm (AOD440) were observed to be 1.21, 1.43, 1.52, and 2.21 occurred on 12, 14 19, and 28 January. It was found that the Ångström exponent (AE) values were almost higher than 1.0 during all the days with its maximum on 26 January (1.53), suggests the dominance of fine-mode particles. The maximum (minimum) aerosol volume size distributions occurred during dense HF (NHF) days with larger particle volumes of fine-mode. The single scattering albedo, asymmetry parameter, and complex refractive index values during HF events suggest the abundance of fine-mode particles from anthropogenic (absorbing) activities mixed with scattering dust particles. The average shortwave direct aerosol radiative forcing (DARF) values at the bottom-of-atmosphere (BOA) during HF and NHF days were estimated to be 112.29 ± 42.18 W m−2 and −58.61 ± 13.09 W m−2, while at the top-of-atmosphere (TOA) the forcing values were −45.78 ± 22.17 W m−2 and −18.64 ± 5.84 W m−2, with the corresponding heating rate of 1.61 ± 0.48 K day−1 and 1.12 ± 0.31 K day−1, respectively. The DARF values retrieved from the AERONET were in good agreement with the SBDART computed both at the TOA (r = 0.95) and the BOA (r = 0.97) over Beijing in January 2013.
显示更多 [+] 显示较少 [-]Absorption properties and forcing efficiency of light-absorbing water-soluble organic aerosols: Seasonal and spatial variability
2021
Choudhary, Vikram | Rajput, Prashant | Gupta, Tarun
Light-absorbing organic aerosols, also known as brown carbon (BrC), enhance the warming effect of the Earth’s atmosphere. The seasonal and spatial variability of BrC absorption properties is poorly constrained and accounted for in the climate models resulting in a substantial underestimation of their radiative forcing estimates. This study reports seasonal and spatial variability of absorption properties and simple forcing efficiency of light-absorbing water-soluble organic carbon (WSOC, SFEWSOC) by utilizing current and previous field-based measurements reported mostly from Asia along with a few observations from Europe, the USA, and the Amazon rainforest. The absorption coefficient of WSOC at 365 nm (bₐbₛ₋₃₆₅) and the concentrations of carbonaceous species at Kanpur were about an order of magnitude higher during winter than in the monsoon season owing to differences in the boundary layer height, active sources and their strengths, and amount of seasonal wet precipitation. The WSOC aerosols during winter exhibited ∼1.6 times higher light absorption capacity than in the monsoon season at Kanpur site. The assessment of spatial variability of the imaginary component of the refractive index spectrum (kλ) across South Asia has revealed that it varies from ∼1 to 2 orders of magnitude and light absorption capacity of WSOC ranges from 3 to 21 W/g. The light absorption capacity of WSOC aerosols exhibited less spatial variability across East Asia (5–13 W/g) when compared to that in the South Asia. The photochemical aging of WSOC aerosols, indicated by the enhancement in WSOC/OC ratio, was linked to degradation in their light absorption capacity, whereas the absorption Ångström exponent (AAE) remained unaffected. This study recommends the adoption of refined climate models where sampling regime specific absorption properties are calculated separately, such that these inputs can better constrain the model estimates of the global effects of BrC.
显示更多 [+] 显示较少 [-]Variation in gravimetric correction factors for nephelometer-derived estimates of personal exposure to PM2.5
2019
Tryner, Jessica | Good, Nicholas | Wilson, Ander | Clark, Maggie L. | Peel, Jennifer L. | Volckens, John
Many portable monitors for quantifying mass concentrations of particulate matter air pollution rely on aerosol light scattering as the measurement method; however, the relationship between scattered light (what is measured) and aerosol mass concentration (the metric of interest) is a complex function of the refractive index, size distribution, and shape of the particles. In this study, we compared 33-h personal PM2.5 concentrations measured simultaneously using nephelometry (personal DataRAM pDR-1200) and gravimetric filter sampling for working adults (44 participants, 249 samples). Nephelometer- and filter-derived 33-h average PM2.5 concentrations were correlated (Spearman's ρ = 0.77); however, the nephelometer-derived concentration was within 20% of the filter-derived concentration for only 13% of samples. The nephelometer/filter ratio, which is used to correct light-scattering measurements to a gravimetric sample, had a median value of 0.52 and varied by over a factor of three (10th percentile = 0.35, 90th percentile = 1.1). When 33-h samples with >50% of 10-s average nephelometer readings below the nephelometer limit of detection were removed from the dataset during sensitivity analyses, the fraction of nephelometer-derived concentrations that were within 20% of the filter-derived concentration increased to 25%. We also evaluated how much the accuracy of nephelometer-derived concentrations improved after applying: (1) a median correction factor derived from a subset of 44 gravimetric samples, (2) participant-specific correction factors derived from one same from each subject, and (3) correction factors predicted using linear models based on other variables recorded during the study. Each approach independently increased the fraction of nephelometer-derived concentrations that were within 20% of the filter-derived concentration to approximately 45%. These results illustrate the challenges with using light scattering (without correction to a concurrent gravimetric sample) to estimate personal exposure to PM2.5 mass among mobile adults exposed to low daily average concentrations (median = 8 μg m−3 in this study).
显示更多 [+] 显示较少 [-]Celebration-induced air quality over a tropical urban station, Pune, India
2015
Devara, Panuganti C.S. | Vijayakumar, Katta | Safai, Pramod D. | Made, P Raju | Rao, Pasumarti S.P.
In this paper, we studied the regional aerosol and air quality over an urban location, Pune, India during the period from 8 to 18 November 2012, encompassing a major Indian celebration, namely, Diwali Festival (12–14 November 2012) and also a clean (control) day (9 November 2012). A suit of ground–based measurements, employing solar radiometers (Microtops II and Cimel Sun–sky radiometer), Nephelometer, and satellite observations carried out over the study region have been applied for these investigations. The study revealed many interesting results which include (i) almost four–fold enhancement in AOD and fine mode dominated aerosol size distribution (ASD) during Diwali compared to clean day conditions; (ii) higher columnar water vapor (H2O), nitrogen dioxide (NO2), and lower ozone (O3) during Diwali period; (iii) higher cooling at bottom (–117W m−2) and top of the atmosphere (–33W m−2) and warming (+82W m−2) in the atmosphere during the festival period, (iv) abundance of fine mode anthropogenic scattering particles associated with greater real part and smaller imaginary part of refractive index, and higher single scattering albedo, (v) higher backscattering coefficient revealing intrusion of more aerosol particles, higher depolarization ratio indicating particles of non–spherical nature, presence of water–phase particles, more polluted smoke and dust particles, (vi) greater attenuation and poor horizontal/vertical visibility, and (vii) dominance of urban industrial/biomass burning aerosols among other aerosol types. These results have been compared with concurrent satellite products and found to be consistent. The results have been further explained with local meteorology, back–trajectory analysis and satellite rapid response images.
显示更多 [+] 显示较少 [-]The impact of seismic air gun exposure on the haemolymph physiology and nutritional condition of spiny lobster, Jasus edwardsii
2017
Fitzgibbon, Quinn P. | Day, Ryan D. | McCauley, Robert D. | Simon, Cedric J. | Semmens, Jayson M.
There is a critical knowledge gap regarding the impacts of seismic air gun signals on the physiology of adult crustaceans. We conducted four controlled field experiments to examine the impact of seismic acoustic signals on spiny lobster, Jasus edwardsii. Seismic air gun exposure suppressed total haemocyte count (THC) for up to 120days post-exposure, suggesting a chronic negative impact of immune competency. THC levels after 365days post-exposure, were elevated two fold, potentially indicating an immune response to infection. Haemolymph refractive index was reduced after 120days post exposure in one experiment, suggesting a chronic impairment of nutritional condition. There was no effect of air gun exposure on 24 haemolymph biochemical parameters, hepatopancreas index or survival. Collectively these results indicate that the biochemical haematological homeostasis of J. edwardsii is reasonably resilient to seismic acoustic signals, however, air gun exposure may negatively influence the lobster's nutritional condition and immunological capacity.
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