Explore the vast range of titles available.

The radiative impact of organic aerosols (OA) is a large source of uncertainty in estimating the global direct radiative effect (DRE) of aerosols. This radiative impact includes not only light scattering but also light absorption from a subclass of OA referred to as brown carbon (BrC). However, the absorption properties of BrC are poorly understood, leading to large uncertainties in modeling studies. To obtain observational constraints from measurements, a simple absorption Ångström exponent (AAE) method is often used to separate the contribution of BrC absorption from that of black carbon (BC). However, this attribution method is based on assumptions regarding the spectral dependence of BC that are often violated in the ambient atmosphere. Here we develop a new AAE method which improves upon previous approaches by using the information from the wavelength-dependent measurements themselves and by allowing for an atmospherically relevant range of BC properties, rather than fixing these at a single assumed value. We note that constraints on BC optical properties and mixing state would help further improve this method. We apply this method to multiwavelength absorption aerosol optical depth (AAOD) measurements at AERONET sites worldwide and surface aerosol absorption measurements at multiple ambient sites. We estimate that BrC globally contributes up to 40 % of the seasonally averaged absorption at 440 nm. We find that the mass absorption coefficient of OA (OA-MAC) is positively correlated with the BC ∕ OA mass ratio. Based on the variability in BC properties and BC ∕ OA emission ratio, we estimate a range of 0.05–1.5 m2 g−1 for OA-MAC at 440 nm. Using the combination of AERONET and OMI UV absorption observations we estimate that the AAE388∕440 nm for BrC is generally  ∼ 4 worldwide, with a smaller value in Europe (< 2). Our analyses of observations at two surface sites (Cape Cod, to the southeast of Boston, and the GoAmazon2014/5 T3 site, to the west of Manaus, Brazil) reveal no significant relationship between BrC absorptivity and photochemical aging in urban-influenced conditions. However, the absorption of BrC measured during the biomass burning season near Manaus is found to decrease with photochemical aging with a lifetime of  ∼ 1 day. This lifetime is comparable to previous observations within a biomass burning plume but much slower than estimated from laboratory studies. Given the large uncertainties associated with AERONET retrievals of AAOD, the most challenging aspect of our analysis is that an accurate, globally distributed, multiple-wavelength aerosol absorption measurement dataset is unavailable at present. Thus, achieving a better understanding of the properties, evolution, and impacts of global BrC will rely on the future deployment of accurate multiple-wavelength absorption measurements to which AAE methods, such as the approach developed here, can be applied.

Knowledge of aerosol radiative effects in the Tibetan Plateau (TP) is limited due to the lack of reliable aerosol optical properties, especially the single scattering albedo (SSA). We firstly reported in situ measurement of SSA in Lhasa using a cavity enhanced albedometer (CEA) at λ = 532 nm from 22nd May to 11th June 2021. Unexpected strong aerosol absorbing ability was observed with an average SSA of 0.69. Based on spectral absorptions measured by Aethalometer (AE33), black carbon (BC) was found to be the dominated absorbing species, accounting for about 83% at λ = 370 nm, followed by primary and secondary brown carbon (BrCpri and BrCsec). The average direct aerosol radiative forcing at the top of atmosphere (DARFTOA) was 2.83 W/m2, indicating aerosol warming effect on the Earth‐atmosphere system. Even though aerosol loading is low, aerosol heating effect plays a significant role on TP warming due to strong absorbing ability. Plain Language Summary The Tibetan Plateau (TP) has experienced rapid warming over the past decades, but the key factors affecting TP climate change haven't yet been clearly understood. Aerosol single scattering albedo (SSA) is a key optical parameter determining aerosol warming or cooling effect; however, reliable SSA measurement is scarce in TP. This study firstly reported in situ measurement of SSA in Lhasa and explored the direct radiative effect of aerosol on TP warming. Strong aerosol absorption, mainly contributed by black carbon (BC), was observed with an average SSA value of 0.69 in this city. Besides Lhasa, other sites over TP were also reported with low SSA (≤0.77) from surface measurement. The strong aerosol absorption could cause heating effect on the Earth‐atmosphere system. To relieve TP warming, reasonable pollutant emission control strategies should be taken urgently to weaken aerosol absorbing ability. Key Points Unexpected low aerosol single scattering albedo was observed in Lhasa via in situ measurement of multiple optical parameters simultaneously Black carbon was the dominant contributor (∼83%) to aerosol absorption at 370 nm, followed by primary and secondary brown carbon The strong absorption in Lhasa exerted positive direct aerosol radiative forcing (warming effect) at the top of atmosphere

Brown carbon (BrC) in China is of great interest to the regional and global climate due to its strong absorption of sunlight. However, the contribution of BrC to total carbonaceous aerosol light absorption and its direct radiative effects (DRE) in China remains largely uncertain. To better assess its climate impact in China, we develop an explicit BrC scheme and implement it in a global climate model, which includes optical parameters of primary BrC derived from local measurements, secondary BrC absorption, and a photobleaching parameterization of BrC. By comparing with multi‐type observational data, we find that with the implementation of this scheme, the model captures the seasonal variations of BrC light absorption well in China. The model estimates that BrC contributes 19% and 12% to the total light absorption of carbonaceous aerosol in China in winter and summer, resulting in 0.110 and 0.205 W m−2 of DRE, respectively. Plain Language Summary While the existing research on the direct radiative effects (DRE) of brown carbon (BrC) predominantly focuses on biomass‐burning sources, little attention has been given to BrC originating from anthropogenic sources. Coal combustion and residential fuels used for cooking and heating release many brown carbon aerosols in China. Source of BrC in China is different from that in Europe and North America. Therefore, studying the light‐absorbing properties and climate effects of BrC in China is of great scientific significance. Here, we introduce local optical parameters of primary BrC based on observations in China, secondary BrC absorption, and chemical bleaching of BrC in a global climate model (GCM). We find that the model can simulate the strong seasonal variations of BrC absorption observed in China. With the help of the model and multi‐type measurement data, we estimate the contribution of BrC to the total carbonaceous aerosol absorption and the DRE of BrC in China in different seasons. This study is the first attempt to introduce an explicit BrC scheme in a GCM to estimate the DRE of BrC in China. Key Points An explicit brown carbon (BrC) scheme is introduced in a climate model together with observations to constrain light absorption of BrC BrC contributes 19% and 12% of total carbonaceous aerosol absorption in China in winter and summer, respectively Simulated direct radiative effects due to BrC absorption over China are 0.110 and 0.205 W m2 in the winter and summer seasons

Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between July and August 2019 aboard the NASA DC-8 research aircraft during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated, highly spectrally resolved light absorption in solvent (water and methanol) extracts of particles collected on filters and in situ bulk aerosol particle light absorption measured at three wavelengths (405, 532 and 664 nm) with a photoacoustic spectrometer (PAS). A light-absorption closure analysis for wavelengths between 300 and 700 nm was performed. The combined light absorption of particle pure black carbon material, including enhancements due to internally mixed materials, plus soluble BrC and a Mie-predicted factor for conversion of soluble BrC to aerosol particle BrC, was compared to absorption spectra from a power law fit to the three PAS wavelengths. For the various parameters used, at a wavelength of roughly 400 nm they agreed, at lower wavelengths the individual component-predicted particle light absorption significantly exceeded the PAS and at higher wavelengths the PAS absorption was consistently higher but more variable. Limitations with extrapolation of PAS data to wavelengths below 405 nm and missing BrC species of low solubility that more strongly absorb at higher wavelengths may account for the differences. Based on measurements closest to fires, the emission ratio of PAS-measured BrC at 405 nm relative to carbon monoxide (CO) was on average 0.13 Mm−1 ppbv−1; emission ratios for soluble BrC are also provided. As the smoke moved away from the burning regions, the evolution over time of BrC was observed to be highly complex; BrC enhancement, depletion or constant levels with age were all observed in the first 8 h after emission in different plumes. Within 8 h following emissions, 4-nitrocatechol, a well-characterized BrC chromophore commonly found in smoke particles, was largely depleted relative to the bulk BrC. In a descending plume where temperature increased by 15 K, 4-nitrocatechol dropped, possibly due to temperature-driven evaporation, but bulk BrC remained largely unchanged. Evidence was found for reactions with ozone, or related species, as a pathway for secondary formation of BrC under both low and high oxides of nitrogen (NOx) conditions, while BrC was also observed to be bleached in regions of higher ozone and low NOx, consistent with complex behaviors of BrC observed in laboratory studies. Although the evolution of smoke in the first hours following emission is highly variable, a limited number of measurements of more aged smoke (15 to 30 h) indicate a net loss of BrC. It is yet to be determined how the near-field BrC evolution in smoke affects the characteristics of smoke over longer timescales and spatial scales, where its environmental impacts are likely to be greater.

Brown carbon (BrC) contributes significantly to aerosol light absorption and thus can affect the Earth's radiation balance and atmospheric photochemical processes. In this study, we examined the light absorption properties and molecular compositions of water-soluble (WS-BrC) and water-insoluble (WI-BrC) BrC in PM2.5 collected from a rural site in the Guanzhong Basin – a highly polluted region in northwest China. Both WS-BrC and WI-BrC showed elevated light absorption coefficients (Abs) in winter (4–7 times those in summer) mainly attributed to enhanced emissions from residential biomass burning (BB) for heating of homes. While the average mass absorption coefficients (MACs) at 365 nm (MAC365) of WS-BrC were similar between daytime and nighttime in summer (0.99±0.17 and 1.01±0.18 m2 g−1, respectively), the average MAC365 of WI-BrC was more than a factor of 2 higher during daytime (2.45±1.14 m2 g−1) than at night (1.18±0.36 m2 g−1). This difference was partly attributed to enhanced photochemical formation of WI-BrC species, such as oxygenated polycyclic aromatic hydrocarbons (OPAHs). In contrast, the MACs of WS-BrC and WI-BrC were generally similar in winter and both showed few diel differences. The Abs of wintertime WS-BrC correlated strongly with relative humidity, sulfate and NO2, suggesting that aqueous-phase reaction is an important pathway for secondary BrC formation during the winter season in northwest China. Nitrophenols on average contributed 2.44±1.78 % of the Abs of WS-BrC in winter but only 0.12±0.03 % in summer due to faster photodegradation reactions. WS-BrC and WI-BrC were estimated to account for 0.83±0.23 % and 0.53±0.33 %, respectively, of the total down-welling solar radiation in the ultraviolet (UV) range in summer, and 1.67±0.72 % and 2.07±1.24 %, respectively, in winter. The total absorption by BrC in the UV region was about 55 %–79 % relative to the elemental carbon (EC) absorption.

Chromophores represent an important portion of light-absorbing species, i.e., brown carbon. Yet knowledge of what and how chromophores contribute to aerosol light absorption is still sparse. To address this problem, we examined soluble independent chromophores in a set of year-round aerosol samples from Bangkok. The water-soluble fluorescent chromophores identified via excitation–emission matrix (EEM) spectroscopy and follow-up parallel factor analysis could be mainly assigned as humic-like substances and protein-like substances, which differed in their EEM pattern from that of the methanol-soluble fraction. The emission wavelength of fluorescent chromophores in environmental samples tended to increase compared with that of the primary combustion emission, which could be attributed to secondary formation or the aging process. Fluorescent indices inferred that these light-absorbing chromophores were not significantly humified and comprised a mixture of organic matter of terrestrial and microbial origin, which exhibited a different characteristic from primary biomass burning and coal-combustion results. A multiple linear regression analysis revealed that larger fluorescent chromophores that were oxygen-rich and highly aromatic with high molecular weights were the key contributors of light absorption, preferably at longer emission wavelengths (λmax⁡ > 500 nm). Positive matrix factorization analysis further suggested that up to 50 % of these responsible chromophores originated from biomass burning emissions.

We investigated long-term changes using a harmonised 22-year data set of aerosol light absorption measurements, in conjunction with air mass history and aerosol source analysis. The measurements were performed at Zeppelin Observatory, Svalbard, from 2002 to 2023. We report a statistically significant decreasing long-term trend for the light absorption coefficient. However, the last 8 years of 2016–2023 showed a slight increase in the magnitude of the light absorption coefficient for the Arctic haze season. In addition, we observed an increasing trend in the single-scattering albedo from 2002 to 2023. Five distinct source regions, representing different transport pathways, were identified. The trends involving air masses from the five regions showed decreasing absorption coefficients, except for the air masses from Eurasia. We show that the changes in the occurrences of each transport pathway cannot explain the reductions in the absorption coefficient observed at the Zeppelin station. An increase in contributions of air masses from more marine regions, with lower absorption coefficients, is compensated for by an influence from high-emission regions. The proportion of air masses en route to Zeppelin, which have been influenced by active fires, has undergone a noticeable increase starting in 2015. However, this increase has not impacted the long-term trends in the concentration of light-absorbing aerosol. Along with aerosol optical properties, we also show an increasing trend in accumulated surface precipitation experienced by air masses en route to the Zeppelin Observatory. We argue that the increase in precipitation, as experienced by air masses arriving at the station, can explain a quarter of the long-term reduction in the light absorption coefficient. We emphasise that meteorological conditions en route to the Zeppelin Observatory are critical for understanding the observed trends.

Brown carbon (BrC) is a fraction of organic aerosol (OA) that absorbs radiation in the ultraviolet and short visible wavelengths. Its contribution to radiative forcing is uncertain due to limited knowledge of its imaginary refractive index (k). This study investigates the variability of k for OA from wildfires, residential, shipping, and traffic emission sources over Europe. The Multiscale Online Nonhydrostatic Atmosphere Chemistry (MONARCH) model simulated OA concentrations and source contributions, feeding an offline optical tool to constrain k values at 370 nm. The model was evaluated against OA mass concentrations from aerosol chemical speciation monitors (ACSMs) and filter sample measurements, as well as aerosol light absorption measurements at 370 nm derived from an Aethalometer™ from 12 sites across Europe. Results show that MONARCH captures the OA temporal variability across environments (regional, suburban, and urban background). Residential emissions are a major OA source in colder months, while secondary organic aerosol (SOA) dominates in warmer periods. Traffic is a minor primary OA contributor. Biomass and coal combustion significantly influence OA absorption, with shipping emissions also notable near harbors. Optimizing k values at 370 nm revealed significant variability in OA light absorption, influenced by emission sources and environmental conditions. Derived k values for biomass burning (0.03 to 0.13), residential (0.008 to 0.13), shipping (0.005 to 0.08), and traffic (0.005 to 0.07) sources improved model representation of OA absorption compared to a constant k. Introducing such emission source-specific constraints is an innovative approach to enhance OA absorption in atmospheric models.

Scientific knowledge about light absorption by aerosols is extremely limited at the eastern slope of the Tibetan Plateau (ESTP). We conducted the first aerosol field experiment at six sites (Chengdu, Sanbacun, Wenchuan, Lixian, Maerkang, Hongyuan) along the ESTP, ranging in elevation from 500 to 3500 m. The fraction of light absorption by brown carbon (BrC) to total carbon increases from 20 % to 50 % with altitude, and the mass absorption efficiency (MAE) of BrC over the Tibetan Plateau (TP) is 2–3 times higher than that inside the Sichuan Basin (SCB), especially in winter. In contrast, the MAE of elemental carbon (EC) in winter decreases with altitude. The contrasting variation of EC and BrC MAE with altitude is mainly attributed to source differences between the TP and SCB. Emissions from the more urban sources (motor vehicles, industries, etc.) inside the SCB fail to be transported to the TP due to the stable air in winter inside the basin, which is also favourable for aerosol ageing to enhance absorption efficiency. The radiative forcing of BrC relative to EC varies from 0.10 to 0.42 as altitude increases with the higher organic carbon (OC) to EC ratio over the TP than SCB. Thus, the reason for the enhanced relative BrC to EC radiative forcing from polluted SCB to pristine TP is that the BrC concentration decreases more slowly than the EC concentration with altitude. This study contributes to the understanding of the difference in light absorption by EC and BrC with altitude, from polluted lower-altitude basins to the pristine TP, and provides a data set for regional climate model validation.

Light‐absorbing carbonaceous aerosols that dominate atmospheric aerosol warming over India remain poorly characterized. Here, we delve into UV‐visible‐IR spectral aerosol absorption properties at nine PAN‐India COALESCE network sites (Venkataraman et al., 2020, https://doi.org/10.1175/bams‐d‐19‐0030.1). Absorption properties were estimated from aerosol‐laden polytetrafluoroethylene filters using a well‐constrained technique incorporating filter‐to‐particle correction factors. The measurements revealed spatiotemporal heterogeneity in spectral intrinsic and extrinsic absorption properties. Absorption analysis at near‐UV wavelengths from carbonaceous aerosols at these regional sites revealed large near‐ultraviolet brown carbon absorption contributions from 21% to 68%—emphasizing the need to include these particles in climate models. Further, satellite‐retrieved column‐integrated absorption was dominated by surface absorption, which opens possibilities of using satellite measurements to model surface‐layer optical properties (limited to specific sites) at a higher spatial resolution. Both the satellite‐modeled and direct in‐situ absorption measurements can aid in validating and constraining climate modeling efforts that suffer from absorption underestimations and high uncertainties in radiative forcing estimates. Plain Language Summary Particulate pollution in the atmosphere scatter and absorb incoming solar energy, thus cooling or warming Earth's atmosphere. In developing countries and especially in India, one of the most polluted regions of the world, the extent to which particles can absorb solar energy and warm the atmosphere is not well understood. Here, for the first time, we measure particle absorption simultaneously at nine ground sites across India, in diverse geographical regions with different levels and types of particulate pollution. We find that organic carbon particles exert large absorption at near‐ultraviolet wavelengths, which contain significant solar energy. These light absorbing organic carbon particles, called brown carbon, are emitted in large quantities from biomass burning (e.g., burning crop residue and cooking on wood‐fired stoves). Comparing ground measurements of absorption with satellite‐retrieved measurements that are representative of the entire atmospheric column, we find that near‐surface atmospheric particles can exert significant warming. This study highlights the need to improve climate model simulations of particulate pollution's impact on the climate by incorporating spatiotemporal surface‐level absorption measurements, including absorption by brown carbon particles. Key Points Measurements at nine regional PAN‐India sites reveal several regions with large aerosol absorption strength Brown carbon contributes significantly (21%–68%) to near‐ultraviolet absorption, indicating its importance in shortwave light absorption Strong correlations observed between satellite data and surface absorption indicate future potential in modeling surface absorption