Brown carbon (BrC) has been recognized as an important light-absorbing carbonaceous aerosol, yet understanding of its influence on regional climate and air quality has been lacking, mainly due to the ignorance of regional coupled meteorology-chemistry models. Besides, assumptions about its emissions in previous explorations might cause large uncertainties in estimates. Here, we implemented a BrC module into the WRF-Chem model that considers source-dependent absorption and avoids uncertainties caused by assumptions about emission intensities. To our best knowledge, we made the first effort to consider BrC in a regional coupled model. We then applied the developed model to explore the impacts of BrC absorption on radiative forcing, regional climate, and air quality in East Asia. We found notable increases in aerosol absorption optical depth (AAOD) in areas with high OC concentrations. The most intense forcing of BrC absorption occurs in autumn over Southeast Asia, and values could reach around 4 W m(-2). The intensified atmospheric absorption modified surface energy balance, resulting in subsequent declines in surface temperature, heat flux, boundary layer height, and turbulence exchanging rates. These changes in meteorological variables additionally modified near-surface dispersion and photochemical conditions, leading to changes of PM2.5 and O-3 concentrations. These findings indicate that BrC could exert important influence in specific regions and time periods. A more in-depth understanding could be achieved later with the developed model.
It is increasingly recognized that light-absorbing impurities (LAI) deposited on snow and ice affect their albedo and facilitate melting processes leading to various feedback loops, such as the ice albedo feedback mechanism. Black carbon (BC) is often considered the most important LAI, but some areas can be more impacted by high dust emissions. Iceland is one of the most important high latitude sources for the Arctic due to high emissions and the volcanic nature of the dust. We studied optical properties of volcanic dust from Iceland and Chile to understand how it interacts with the Sun's radiation and affects areas of deposition as LAI. Optical properties of dust samples were measured at the laboratory of the Finnish Geospatial Research Institute (FGI) using the latest setup of the FGI's goniospectrometer. We found that, depending on the particle size, the albedo of dry volcanic dust on the visible spectrum is as low as 0.03, similar to that of BC, and the albedo decreases with increasing particle size. Wet dust reduces its albedo by 66% compared to dry sample. This supports the comparability of their albedo reducing effects to BC as LAIs, and highlights their significant role in albedo reduction of snow and ice areas. The potential use of the results from our measurements is diverse, including their use as a ground truth reference for Earth Observation and remote sensing studies, estimating climate change over time, as well as measuring other ecological effects caused by changes in atmospheric composition or land cover.
China is an important emitter of light-absorbing carbonaceous aerosols (LACs), including black carbon (BC) and brown carbon (BrC). Currently, there are large uncertainties in model-estimated direct radiative forcing (DRF) of LACs, partially due to the poor understanding of the emissions and optical properties of LACs. In this study, we estimated the DRF of LACs over China during the implementation of the Air Pollution Prevention and Control Action Plan (APPCAP) using the global chemical transport model (GEOS-Chem) coupled with the Rapid Radiative Transfer Model of GCMs (RRTMG). We updated the refractive index of BC, includedbiomass burning (BB) sources, biofuel (BF) and coal combustion (CC) sources in the residential sector as BrC emission sources and the optical properties were updated, which were not fully considered in the previous model studies. Our results showed that model could reasonably capture the spatial and temporal variations of LACs in China with the correlation coefficients between model simulated and Aerosol Robotic Network (AERONET) observed daily absorption aerosol optical depth (AAOD) of LACs at 440 nm above 0.63 and the corresponding values of the normalized mean bias within +/- 30%. The simulated annual mean LACs AAOD at 440 nm in China was 0.016 (0.021) in 2017 (2014) and BrC contributed about 20% (21%). The estimated annual mean clear-sky LACs DRF at the top of the atmosphere in China was 1.02 W m(-2) in 2017 and 1.38 W m(-2) in 2014, and the contribution of BrC was about 10% and 11%, respectively, which was dominated by the BF sources (46% in 2017 and 44% in 2014) and the BB sources (38% in 2017 and 43% in 2014), with CC sources being low (16% in 2017 and 13% in 2014). The annual mean AAOD and DRF of LACs in China decreased by 0.005 and 0.36 W m(-2) from 2014 to 2017, which were largely attributed to the reductions of anthropogenic emissions during the implementation of APPCAP. Our results would improve the understanding of the light absorption capacity and climate effects of LACs in China.
Snow-covered regions are the main source of reflection of incident shortwave radiation on the Earth's surface. The deposition of light-absorbing particles on these regions increases the capacity of snow to absorb radiation and decreases surface snow albedo, which intensifies the radiative forcing, leading to accelerated snowmelt and modifications of the hydrologic cycle. In this work, the changes in surface snow albedo and radiative forcing were investigated, induced by light-absorbing particles in the Upper Aconcagua River Basin (Chilean Central Andes) using remote sensing satellite data (MODIS), in situ spectral snow albedo measurements, and the incident shortwave radiation during the austral winter months (May to August) for the 2004-2016 period. To estimate the changes in snow albedo and radiative forcing, two spectral ranges were defined: (i) an enclosed range between 841 and 876 nm, which isolates the effects of black carbon, an important light-absorbing particle derived from anthropogenic activities, and (ii) a broadband range between 300 and 2500 nm. The results indicate that percent variations in snow albedo in the enclosed range are higher than in the broadband range, regardless of the total amount of radiation received, which may be attributed to the presence of light-absorbing particles, as these particles have a greater impact on surface snow albedo at wavelengths in the enclosed band than in the broadband band.
This article investigates the snow albedo changes in Colombian tropical glaciers, namely, Sierra Nevada de Santa Marta (SNSM), Sierra Nevada del Cocuy (NSC), Nevado del Ruiz (NDR), Nevado Santa Isabel (NDS), Nevado del Tolima (NDT), and Nevado del Huila (NDH). They are associated with the possible mineral dust deposition from the Sahara Desert during the June and July months using snow albedo (SA), snow cover (SC), and land surface temperature (LST) from the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard NASA's Terra and Aqua satellites. And mineral dust (MD) from The Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2), both of them during 2000-2020. Results show the largest snow albedo reductions were observed at 39.39%, 32.1%, and 30.58% in SNC, SNSM, and NDR, respectively. Meanwhile, a multiple correlation showed that the glaciers where MD contributed the most to SA behavior were 35.4%, 24%, and 21.4% in NDS, NDC, and NDR. Results also display an increasing trend of dust deposition on Colombian tropical glaciers between 2.81 x 10-3 & mu;g & BULL;m-2 & BULL;year-1 and 6.58 x 10-3 & mu;g & BULL;m-2 & BULL;year-1. The results may help recognize the influence of Saharan dust on reducing snow albedo in tropical glaciers in Colombia. The findings from this study also have the potential to be utilized as input for both regional and global climate models. This could enhance our comprehension of how tropical glaciers are impacted by climate change.
Duringthe summer and winter periods of 2019-2020, we conductedsampling of fine mode ambient aerosols in the western Himalayan glacialregion (WHR; Thajiwas glacier, 2799 m asl), central Himalayan glacialregion (CHR; Gomukh glacier, 3415 m asl), and eastern Himalayan glacialregion (EHR; Zemu glacier, 2700 m asl). We evaluated the aerosol opticalproperties, which included the mass absorption coefficient, mass absorptionefficiency, mass scattering efficiency, absorption angstrom exponent,single scattering albedo, as well as their simple radiative forcingefficiencies. We observed the highest absorption in the near ultraviolet-visiblewavelength range (200-400 nm), with CHR showing the highestabsorption compared to the other two sites, WHR and EHR, respectively.Across the wavelength range of 200-1100 nm, the overall contributionof black carbon to light attenuation was greater than that of browncarbon. However, brown carbon dominated the absorption in the nearUV-visible wavelengths, providing evidence of its non-trivialpresence over the Himalayan region. Additionally, we observed a positiveradiative forcing (W/g), which leads to net warming at these sites.The findings of this ground-based study contribute to our understandingof the light-absorbing nature of carbonaceous aerosols and their impacton the Himalayan glacier regions.
Light-absorbing particles (LAPs) deposited on snow can significantly reduce surface albedo and contribute to positive radiative forcing. This study firstly estimated and attributed the spatio-temporal variability in the radiative forcing (RF) of LAPs in snow over the northern hemisphere during the snow-covered period 2003-2018 by employing Moderate Resolution Imaging Spectroradiometer (MODIS) data, coupled with snow and atmospheric radiative transfer modelling. In general, the RF for the northern hemisphere shows a large spatial variability over the whole snow-covered areas and periods, with the highest value (12.7 W m(-2)) in northeastern China (NEC) and the lowest (1.9 W m(-2)) in Greenland (GRL). The concentration of LAPs in snow is the dominant contributor to spatial variability in RF in spring (similar to 73%) while the joint spatial contributions of snow water equivalent (SWE) and solar irradiance (SI) are the most important (>50%) in winter. The average northern hemisphere RF gradually increases from 2.1 W m(-2) in December to 4.1 W m(-2) in May and the high-value area shifts gradually northwards from mid-altitude to high-latitude over the same period, which is primarily due to the seasonal variability of SI (similar to 58%). More interestingly, our data reveal a significant decrease in RF over high-latitude Eurasia (HEUA) of -0.04 W m(-2) a(-1) and northeastern China (NEC) of -0.14 W m(-2) a(-1) from 2003 to 2018. By employing a sensitivity test, we find the concurrent decline in the concentration of LAPs in snow accounted for the primary responsibility for the decrease in RF over these two areas, which is further confirmed by in situ observations.
This study employs a fully coupled meteorology-chemistry-snow model to investigate the impacts of light-absorbing particles (LAPs) on snow darkening in the Sierra Nevada. After comprehensive evaluation with spatially and temporally complete satellite retrievals, the model shows that LAPs in snow reduce snow albedo by 0.013 (0-0.045) in the Sierra Nevada during the ablation season (April-July), producing a midday mean radiative forcing of 4.5 W m(-2) which increases to 15-22 W m(-2) in July. LAPs in snow accelerate snow aging processes and reduce snow cover fraction, which doubles the albedo change and radiative forcing caused by LAPs. The impurity-induced snow darkening effects decrease snow water equivalent and snow depth by 20 and 70 mm in June in the Sierra Nevada bighorn sheep habitat. The earlier snowmelt reduces root-zone soil water content by 20%, deteriorating the forage productivity and playing a negative role in the survival of bighorn sheep.
This study reports for the first time the content of trace elements and light-absorbing particles (LAPs) in snow samples collected from a Peruvian glacier (Huaytapallana). The sampling campaign was carried out monthly from November 2015 to March 2019. The trace elements content was quantified by inductively coupled plasma mass spectrometry, while LAPs were analyzed using the light absorption heating method. The chemical composition dataset was assessed by descriptive statistics and t-test for assessing dry season and wet season differences. In addition, enrichment factor (EF) and hierarchical cluster analysis (HCA) were employed to identify possible emission sources. The snow, ice, and aerosol radiative (SNICAR) model was used to measure the effect of LAPs on snow albedo and radiative forcing (RF). Based on analysis of EF and HCA, it was shown that Al, Ti, Si, Co, Ce, Sr, Mn, Mg, Ba and Na have mainly natural sources; K, Ca, Fe, Cu, Pb and As have a mixture of natural and anthropogenic sources, and Zn has anthropogenic source. SNICAR model results indicated that LAPs reduced the snow albedo by up 4.5 % in the dry season with RF values as high as 33 W/m(2). Therefore, we conclude that the presence of these particles substantially increases melt or sublimation rates of Peruvian glaciers.
Light-absorbing impurities (LAIs) in surface snow and snow pits together with LAIs' concentrations and their impacts on albedo reduction and sequent radiative forcing (RF) have been investigated in the past. Here, we focused on temporal-spatial distributions of LAIs, especially on the albedo reduction and radiative forcing caused by the LAIs in Urumqi Glacier No.1. Various snow samples, including fresh snow, aged snow, and granular ice were collected between 3,770 and 4,105 m a.s.l of Urumqi Glacier No.1 during the snowmelt season of 2015. For the surface snow samples, BC and OC concentrations were 582 and 1,590 ng g(-1), respectively. Mineral dust (MD) concentrations were 110 mu g g(-1). Due to the different ablation status of the glacier surface, LAIs accumulate at the lower altitude of the glacier. The estimation by the Snow, Ice, and Aerosol Radiative (SNICAR) model indicated that BC and MD could reduce the albedo by 12.8 and 10.3% in fresh snow, aged snow by 23.3 and 5.9%, and granular ice by 22.4 and 26.7%, respectively. The RF of MD was higher than that of BC in fresh snow and granular ice, whereas the RF of BC exceeded MD in aged snow. These findings suggested that BC was the main forcing factor in snow melting and dust was the main forcing factor in accelerating glacier melt.