Direct Radiative Effect Research Articles

The radiative impact of biomass burning aerosols on dust emissions over Namibia and the long-range transport of smoke observed during the Aerosols, Radiation and Clouds in southern Africa (AEROCLO-sA) campaign

Abstract. The radiative effects of biomass burning aerosols (BBAs) on low-level atmospheric circulation over southern Africa are investigated on 5 September 2017 during the Aerosols, Radiation and Clouds in southern Africa (AEROCLO-sA) field campaign. This is conducted using a variety of in situ and remote sensing observations, as well as two 5 d ensemble simulations made with the Meso-NH mesoscale model, one including the direct and semi-direct radiative effects of aerosols and one in which these effects are not included. We show that the radiative impact of BBA building up over a period of 5 d in the Meso-NH simulations can lead to significantly different circulations at low and middle levels, thereby affecting dust emissions over southern Namibia and northwestern South Africa as well as the transport of BBA in a so-called “river of smoke”. While most of the regional-scale dynamics, thermodynamics and composition features are convincingly represented in the simulation with BBA radiative effects, neglecting the radiative impact of BBA leads to unrealistic representations of (i) the low-level jet (LLJ) over the plateau, which is the main low-level dynamic feature fostering dust emission, and (ii) the mid-level dynamics pertaining to the transport of BBA from the fire-prone regions in the tropics to the mid-latitudes. For instance, when the BBA radiative impacts are not included, the LLJ is too weak and not well established over night, and the developing convective planetary boundary layer (PBL) is too deep compared to observations. The deeper convective PBL over Etosha and surrounding areas is related to the enhanced anomalous upward motion caused by the eastern displacement of the river of smoke. This eastern displacement is, in turn, related to the weaker southerly African easterly jet. Both ensemble simulations provide clear evidence that the enhanced near-surface extinction coefficient values detected from observations over Etosha are related to the downward mixing of BBA in the developing convective boundary layer rather than dust being emitted as a result of the LLJ breakdown after sunrise. This study suggests that the radiative effect of BBAs needs to be taken into account to properly forecast dust emissions in Namibia.

Sensitivity of global direct aerosol shortwave radiative forcing to uncertainties in aerosol optical properties

Abstract. New satellite missions promise global reductions in the uncertainties in aerosol optical properties, but it is unclear how those reductions will propagate to uncertainties in the shortwave (SW) direct aerosol radiative effect (DARE) and direct aerosol radiative forcing (DARF), which are currently large, on the order of at least 20 %. In this work, we build a Monte Carlo framework to calculate the impact of uncertainties in aerosol optical depth (AOD), single scattering albedo (SSA), and the asymmetry parameter on the uncertainty in shortwave DARE and DARF. This framework uses the results of over 2.3 million radiative transfer simulations to calculate global clear-sky DARE and DARF based on a range of uncertainties in present-day and pre-industrial aerosol optical properties, representative of existing and future global observing systems. We find the 1σ uncertainty varies between ±0.23 and ±1.91 W m−2 (5 % and 42 %) for the top-of-atmosphere (TOA) clear-sky DARE and between ±0.08 and ±0.47 W m−2 (9 % and 52 %) for the TOA DARF. At the TOA, AOD uncertainty is the main contributor to overall uncertainty except over bright surfaces where SSA uncertainty contributes most. We apply regionally varying uncertainties to represent current measurement uncertainties and find that aerosol optical property uncertainties represent 24 % of TOA DARE and DARF. Reducing regionally varying optical property uncertainties by a factor of 2 would reduce their contributions to TOA DARE and DARF uncertainty proportionally. Applying a simple scaling to all-sky conditions, aerosol optical property uncertainty contributes to about 25 % total uncertainty in TOA, all-sky SW DARE, and DARF. Compared to previous studies which considered uncertainties in non-aerosol variables, our results suggest that the aerosol optical property uncertainty accounts for one-third to half of the total direct SW uncertainty. Recent and future progress in constraining aerosol optical properties using ground-based or satellite retrievals could be translated into DARE and DARF uncertainty using our freely available framework.

Source-specific light absorption and radiative effects decreases and indications due to the lockdown

The ‘extreme’ emission abatement during the lockdown (from the end of 2019 to the early 2020) provided an experimental period to investigate the corresponding source-specific effects of aerosol. In this study, the variations of source-specific light absorption (babs) and direct radiative effect (DRE) were obtained during and after the lockdown period by using the artificial neural network (ANN) and source apportionment environmental receptor model. The results showed that the babs decreased for all sources during the two periods. The most reductions were observed with ∼90% for traffic-related emissions (during the lockdown) and ∼85% for coal combustion (after the lockdown), respectively. Heightened babs (370 nm) values were obtained for coal and biomass burning during the lockdown, which was attributed to the enhanced atmospheric oxidization capacity. Nevertheless, the variations of babs (880 nm) after the lockdown was mainly due to the weakening of oxidation and reduced emissions of secondary precursors. The present study indicated that the large-scale emission reduction can promote both reductions of babs (370 nm) and DRE (34–68%) during the lockdown. The primary emissions decrease (e.g., Traffic emission) may enhance atmosphere oxidation, increase the ultraviolet wavelength light absorption and DRE efficiencies. The source-specific emission reduction may be contributed to various radiation effects, which is beneficial for the adopting of control strategies.

Accumulation of absorbing aerosols over the Indian Sector of Southern Ocean during the austral summer: Role of thermal inversions

Optical properties of aerosols and their direct radiative effect were analyzed from columnar Aerosol Optical Depth (AOD) and ambient Black Carbon (BC) mass concentration (MB) estimated during Indian Southern Ocean Expeditions (SOEs), conducted in the austral summers of 2016–17 (SOE-IX) and 2017–18 (SOE-X). The aforementioned observations were supplemented with concurrent vertical soundings of the lower atmosphere. Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) data aided in investigating the vertical distribution of aerosols up to 10 km altitude. The relative contribution of BC aerosols emanating from fossil fuel combustion and biomass burning showed the former to be predominant, as the latter is larger and preferentially scavenged during long-range transport to remote marine regions. The highest values of AOD at 500 nm (AOD500; 0.156 ± 0.026) and MB (90.78 ± 40.11 ng m−3) were encountered in the region between 50 and 60°S. Consequently, the atmospheric clear-sky Aerosol Direct Radiative Effect (ADRE; +3.10 ± 0.38 W m−2) and heating rate (HR; 0.087 ± 0.011 K day−1) were also observed to be the highest in the region. Multiple atmospheric inversions were detected between 40 and 69°S. Although a much lower AOD500 (0.070 ± 0.017) prevailed between 60 and 69°S, the average clear-sky ADRE (+1.56 ± 0.49 W m−2) and HR (0.044 ± 0.014 K day−1) were fairly high. The mean MB in the region was high (68.81 ± 28.40 ng m−3) for the pristine ice-covered region. Low-lying inversions prevented the vertical ventilation and dispersal of BC therein. Simulations of BC-induced atmospheric heating rates at three locations in the coastal Antarctic waters indicated a ≈ 3–5-fold increase, corresponding to an increase in ambient BC from 50 to 300 ng m−3.

Seasonal characteristics of emission, distribution, and radiative effect of marine organic aerosols over the western Pacific Ocean: an investigation with a coupled regional climate aerosol model

Abstract. Organic aerosols from marine sources over the western Pacific Ocean of East Asia were investigated using an online coupled regional chemistry–climate model RIEMS-Chem for the entire year 2014. Model evaluation against a wide variety of observations from research cruises and in situ measurements demonstrated a good skill of the model in simulating temporal variation and spatial distribution of particulate matter with aerodynamic diameter less than 2.5 and 10 µm (PM2.5 and PM10), black carbon (BC), organic carbon (OC), sodium, and aerosol optical depth (AOD) in the marine atmosphere. The inclusion of marine organic aerosols improved model performance on OC concentration by reducing model biases of up to 20 %. The regional and annual mean near-surface marine organic aerosol (MOA) concentration was estimated to be 0.27 µg m−3, with the maximum in spring and the minimum in winter, and contributed 26 % of the total organic aerosol concentration on average over the western Pacific. Marine primary organic aerosol (MPOA) accounted for the majority of marine organic aerosol (MOA) mass, and the MPOA concentration exhibited the maximum in autumn and the minimum in summer, whereas marine secondary organic aerosol (MSOA) was approximately 1–2 orders of magnitude lower than MPOA, having a distinct summer maximum and a winter minimum. MOA induced a direct radiative effect (DREMOA) of −0.27 W m−2 and an indirect radiative effect (IREMOA) of −0.66 W m−2 at the top of the atmosphere (TOA) in terms of annual and oceanic average over the western Pacific, with the highest seasonal mean IREMOA up to −0.94 W m−2 in spring. IREMOA was stronger than, but in a similar magnitude to, the IRE due to sea salt aerosol on average, and it was approximately 9 % of the IRE due to anthropogenic aerosols in terms of annual mean over the western Pacific. This ratio increased to 19 % in the northern parts of the western Pacific in autumn. This study reveals an important role of MOA in perturbing cloud properties and shortwave radiation fluxes in the western Pacific of East Asia.

An observation-constrained estimation of brown carbon aerosol direct radiative effects

Abstract. Brown carbon (BrC) is an organic carbon component with noticeable absorption in the ultraviolet and short visible wavelengths, which influences the global radiative balance. However, assessing BrC radiative effects remains a challenging task owing to the scarcity of direct BrC observations and the uncertainties regarding their chemical and optical properties. This study proposes an efficient method for estimating BrC radiative effects based on the available observational data. The light-absorbing properties of BrC obtained from aethalometer measurements and an optical separation method were combined with simulated BrC optical properties to determine mass concentrations. An optical closure study was conducted to constrain the total and other aerosol contents. Subsequently, we estimated the aerosol optical properties and concentrations. Such a state-of-the-art combination of measurements and numerical models provides primary variables for simulating radiative transfer to estimate BrC radiative effects. We used observations conducted over 4 months (from 1 July to 18 November 2021) in Nanjing (a megacity in east China) as an example. During the observational period, BrC absorption constituted 8.7 %–34.1 % of the total aerosol absorption at 370 nm. In the atmosphere, BrC plays a warming role, with its average instantaneous radiative forcing (RF) and standard deviation of 4.0 ± 2.3 W m−2 corresponding to 15 ± 4.2 % of the black carbon (BC) RF. At the surface, the BrC-induced actinic flux (AF) attenuation is comparable to that caused by BC, accounting for over 55 % of the BC effects in the UV range and almost 20 % in the visible range. The photosynthetically active radiation (PAR) attenuated by BrC is approximately 33.5 ± 9.4 % of that attenuated by BC. Furthermore, we quantified the influences of several BC and BrC microphysical and optical properties on their radiative effects. These findings provide valuable insights for understanding BrC radiative effects. Moreover, they highlight the importance of and necessity for improved observation and modeling of BrC properties.

The direct and indirect radiative effects of sea salt aerosols over the western Pacific using an online-coupled regional chemistry-climate model with a developed sea salt emission scheme

The direct and indirect radiative effects of sea salt aerosols (SSA) over the western Pacific Ocean of East Asia for the year 2014 are investigated by using an online-coupled regional chemistry-climate model (RIEMS-Chem) with a developed sea salt emission scheme (G03SSTRH) by considering the effects of sea surface temperature (SST) and relative humidity (RH) on sea salt generation. Model comparison with observations at coastal and island sites demonstrates the G03SSTRH scheme apparently improve model simulation for sea salt concentration, with the overall model-observation bias for PM10 concentration reduced from 29% to 16% and more evident improvement at northern sites of the western Pacific. It is noteworthy that compared to the experiment with the old SSA emission scheme (G03), the G03SSTRH experiment substantially alters the spatial distribution of mass concentration and radiative effects of sea salt, shifting the maximum value center from the ocean northeast of Japan to the southern parts of the western Pacific with the maximum value increasing to some extent. SSA exerts a negative radiative effect at the top of atmosphere (TOA), in which direct radiative effect (DRESSA) dominates over indirect radiative effect (IRESSA) in the western Pacific. The oceanic and annual mean DRESSA, IRESSA, and total radiative effect (TRESSA) are estimated to be −1.22 W/m2, −0.46 W/m2, and −1.65 W/m2, respectively, from the G03SSTRH experiment, which are 16%, 5%, and 12% stronger than those from the G03 experiment, and the seasonal mean DRESSA in G03SSTRH are approximately 45% and 32% higher than those in G03 in summer and autumn. Distinct seasonality of SSA radiative effects is revealed in the G03SSTRH experiment, showing stronger DRESSA and IRESSA in summer and autumn than those in spring and winter, in marked contrast to the little seasonality in the G03 experiment. This study provides a comprehensive regional estimation of radiative effects induced by SSA and reveals the significant effect of different SSA emission schemes on both mass concentration, radiative effects and seasonal variation of SSA over the western Pacific.

Impact of Saharan dust outbreaks on short‐range weather forecast errors in Europe

AbstractMineral dust, the most abundant atmospheric aerosol by mass, interacts with radiation directly and alters cloud properties indirectly. Many operational numerical weather prediction models account for aerosol direct effects by using climatological mean concentrations and neglect indirect effects. This simplification may lead to shortcomings in model forecasts during outbreaks of Saharan dust towards Europe, when climatological mean dust concentrations deviate strongly from actual concentrations. This study investigates errors in model analyses and short‐range forecasts during such events. We investigate a pronounced dust event in March 2021 using the pre‐operational ICOsahedral Nonhydrostatic weather and climate model with Aerosols and Reactive Trace gases (ICON‐ART) with prognostic calculation of dust and the operational European Centre for Medium‐Range Weather Forecasts (ECMWF) Integrated Forecasting System (IFS) model, which deploys a dust climatology. We compare model analysis and forecast with measurements from satellite and in situ instruments. We find that inclusion of prognostic aerosol and direct radiative effects from dust improves forecasts of surface radiation during clear‐sky conditions. However, dust‐induced cirrus clouds are strongly underestimated, highlighting the importance of representing indirect effects adequately. These findings are corroborated by systematic quantification of forecast errors against satellite measurements. For this we construct an event catalogue with 49 dust days over Central Europe between January 2018 and March 2022. We classify model cells by simulated and observed cloudiness and simulated dustiness in the total atmospheric column. We find significant overestimations of brightness temperature for cases with dust compared with cases without dust. For surface shortwave radiation, we find median overestimations of 6.2% during cloudy conditions with dust optical depth greater than 0.1, however these are not significant compared with cloudy conditions without dust. Our findings show that the pre‐operational ICON‐ART and the operational IFS model still do not reproduce cloudiness adequately during events with Saharan dust over Central Europe. Missing implementations of prognostic dust, particularly of indirect effects on cloud formation, lead to significant underestimations of cloudiness and potentially overestimations of surface radiation.

Cyclogenesis in the Tropical Atlantic: First Scientific Highlights from the Clouds–Atmospheric Dynamics–Dust Interactions in West Africa (CADDIWA) Field Campaign

Abstract During the boreal summer, mesoscale convective systems generated over West Africa propagate westward and interact with African easterly waves, and dust plumes transported from the Sahel and Sahara by the African easterly jet. Once off West Africa, the vortices in the wake of these mesoscale convective systems evolve in a complex environment sometimes leading to the development of tropical storms and hurricanes, especially in September when sea surface temperatures are high. Numerical weather predictions of cyclogenesis downstream of West Africa remains a key challenge due to the incomplete understanding of the clouds–atmospheric dynamics–dust interactions that limit predictability. The primary objective of the Clouds–Atmospheric Dynamics–Dust Interactions in West Africa (CADDIWA) project is to improve our understanding of the relative contributions of the direct, semidirect, and indirect radiative effects of dust on the dynamics of tropical waves as well as the intensification of vortices in the wake of offshore mesoscale convective systems and their evolution into tropical storms over the North Atlantic. Airborne observations relevant to the assessment of such interactions (active remote sensing, in situ microphysics probes, among others) were made from 8 to 21 September 2021 in the tropical environment of Sal Island, Cape Verde. The environments of several tropical cyclones, including Tropical Storm Rose, were monitored and probed. The airborne measurements also serve the purpose of regional model evaluation and the validation of spaceborne wind, aerosol and cloud products pertaining to satellite missions of the European Space Agency and EUMETSAT (including the Aeolus, EarthCARE, and IASI missions).

Improving Estimates of Dynamic Global Marine DMS and Implications for Aerosol Radiative Effect

AbstractDimethyl sulfide (DMS) is the predominant natural sulfur source and plays a pivotal role in regulating global climate. However, the current method for estimating seawater DMS concentrations has limitations, and the existing DMS‐induced radiative effect heavily relies on bottom‐up DMS climatologies. This study aims to improve the method for estimating seawater DMS concentrations as well as to evaluate its induced aerosol direct radiative effect (DRE) and indirect radiative effect (IRE) using a state‐of‐the‐art aerosol microphysics scheme integrated with a chemical transport model. The predicted seawater DMS concentrations based on data‐driven methods were verified with multi‐year in situ measurements, revealing a marked reduction in mean bias by over 80%. Results show that our estimates generally indicate lower seawater DMS concentrations (1.48–1.88 μmol/m3) compared to previous seawater DMS climatologies, with differences ranging from −37% to 11%, and that interannual variability in DMS concentrations is varies significantly, particularly in polar regions. The DRE and cloud‐albedo IRE induced by DMS were −0.06 and −0.19 W/m2, respectively, representing a cooling effect on radiative effect that was weaker by 31.4% and 27.0% of those derived from the commonly used bottom‐up DMS climatology. The comprehensive evaluation of the model's performance of atmospheric DMS prediction based on global‐scale observations shows a significant improvement after using our estimates. Thus, we conclude that the global DMS fluxes provided in the past are overestimated, including its resulting DMS radiative effect, which highlights the need for refining the estimation of global aerosol radiative effect to enhance the accuracy of assessing aerosol‐induced climate impacts.

A novel methodology for calculating the aerosol direct radiative effect using a non-uniform five-dimensional lookup table

ABSTRACT The quantification of aerosol direct radiative effects (ADREs) under clear sky conditions is essential for understanding the influence of aerosols on climate. This paper introduces a novel approach, the non-uniform five-dimensional lookup table (NU-5D-LUT) method, for calculating the ADREs under clear sky conditions. The NU-5D-LUT method considers key parameters such as aerosol optical thickness, single scattering albedo, asymmetry factor, surface albedo, and solar zenith angle. Validation against the SBDART model shows strong agreement, with correlation coefficients of 0.97 and 0.99 for TOA and BOA ADREs, respectively. Global comparisons demonstrate consistent ADRE distributions, with relative errors below 5.8% for TOA ADRE and 4.4% for BOA ADRE. The NU-5D-LUT method significantly reduces computation time, offering a practical solution for large-scale simulations and climate model evaluations in aerosol research.

High contributions of fossil fuel sources to char-EC/soot-EC at a high-altitude site: Direct radiative effects and transport pathway

Char-EC and soot-EC in the atmosphere produced from different fuel combustion have distinct optical properties which lead to different radiative forcing. Pollutants transported into high-altitude environment could have a long-lasting radiative effect due to being free of deposition. In this study, the mass absorption cross-section (MAC), the sources, transport pathways and the direct radiative effects (DREs) of soot-EC and char-EC were investigated at a peak of Mountain Hua (Mt. Hua) in China. The measurement results showed that soot-EC and char-EC account for 15.7 % and 84.3 % of EC, respectively. The mean MAC (λ = 633 nm) of soot-EC (13.7 ± 3.8 m2/g) was much higher than that of char-EC (5.4 ± 2.5 m2/g), indicating a stronger light absorption ability for soot-EC. During the study period, 62.1 % char-EC was from anthracite chunk coal, 24.3 % of it from liquid fuel combustion. By contrast, 59.0 % soot-EC from liquid fuel combustion and 36.6 % of it from anthracite chunk coal. EC (both char-EC and soot-EC) produced from anthracite chunk coal reached the peak of the Mt. Hua primarily through the raising of the planetary boundary layer (PBL), while the EC produced from liquid fuel arrived the peak mainly by the regional transport above the PBL of the site. Although soot-EC has a stronger ability (2.8 times higher) to absorb the light compared with char-EC, its DRE (5.7 ± 3.9 W m−2) was lower than that of char-EC (11.6 ± 6.9 W m−2) due to the smaller mass quantity. Liquid fuel consumption contributed 3.5 ± 2.9 W m−2 DRE of soot-EC, while the combustion of anthracite chunk coal contributed 7.5 ± 5.7 W m−2 DRE of char-EC. This study highlights the differences in DREs of soot-EC and char-EC from fossil fuel combustion and the DRE mass efficiency of soot-EC and char-EC. The results emphasize the divergent climate warming effects caused by the combustion of different fossil fuels and imply that setting path to a green transition of energy use would benefit reducing the EC perturbation to the radiation balance of earth-atmosphere.

Elevation-dependence of warming due to aerosol-induced snow darkening over the Himalayan-Tibetan region

Temperature trends over the high-altitude mountains depict an increase with elevation during recent years. These stratified warming trends observed over the Himalayan-Tibetan (HT) regions are higher than the mean warming trends observed over low-elevation regions of South and East Asia, which is attributed to several factors including snow albedo feedback, clouds and water vapor feedback. In this study, we demonstrate the effects of deposition of absorbing aerosols like black carbon and dust on snow albedo and its implications for elevation-dependent warming (EDW). Though the aerosol concentration decreases with elevation, warming due to aerosol-induced snow darkening increases with elevation. Further, surface cooling due to the direct radiative effects (DRE) of aerosols is found to decrease with elevation, which also favors higher warming at high altitudes. The effects of both the deposition of absorbing aerosols on snow albedo and the surface cooling due to the DRE of atmospheric aerosols could strengthen EDW. This study clearly shows the potential of albedo feedback due to aerosol-cryosphere interaction as one of the physical mechanisms contributing to the observed EDW over the HT region.

Ozonolysis can produce long-lived greenhouse gases from commercial refrigerants.

Hydrofluoroolefins are being adopted as sustainable alternatives to long-lived fluorine- and chlorine-containing gases and are finding current or potential mass-market applications as refrigerants, among a myriad of other uses. Their olefinic bond affords relatively rapid reaction with hydroxyl radicals present in the atmosphere, leading to short lifetimes and proportionally small global warming potentials. However, this type of functionality also allows reaction with ozone, and whilst these reactions are slow, we show that the products of these reactions can be extremely long-lived. Our chamber measurements show that several industrially important hydrofluoroolefins produce CHF3 (fluoroform, HFC-23), a potent, long-lived greenhouse gas. When this process is accounted for in atmospheric chemical and transport modeling simulations, we find that the total radiative effect of certain compounds can be several times that of the direct radiative effect currently recommended by the World Meteorological Organization. Our supporting quantum chemical calculations indicate that a large range of exothermicity is exhibited in the initial stages of ozonolysis, which has a powerful influence on the CHF3 yield. Furthermore, we identify certain molecular configurations that preclude the formation of long-lived greenhouse gases. This demonstrates the importance of product quantification and ozonolysis kinetics in determining the overall environmental impact of hydrofluoroolefin emissions.

Columnar optical-radiative properties and components of aerosols in the Arctic summer from long-term AERONET measurements

Aerosols as an external factor have an important role in the amplification of Arctic warming, yet the geography of this harsh region has led to a paucity of observations, which has limited our understanding of the Arctic climate. We synthesized the latest decade (2010–2021) of data on the microphysical–optical–radiative properties of aerosols and their multi-component evolution during the Arctic summer, taking into consideration the important role of wildfire burning. Our results are based on continuous observations from eight AERONET sites across the Arctic region, together with a meteorological reanalysis dataset and satellite observations of fires, and utilize a back-trajectory model to track the source of the aerosols. The summer climatological characteristics within the Arctic Circle showed that the aerosols are mainly fine-mode aerosols (fraction >0.95) with a radius of 0.15–0.20 μm, a slight extinction ability (aerosol optical depth ∼ 0.11) with strong scattering (single scattering albedo ∼0.95) and dominant forward scattering (asymmetry factor ∼ 0.68). These optical properties result in significant cooling at the Earth's surface (∼−13 W m−2) and a weak cooling effect at the top of the atmosphere (∼−5 W m−2). Further, we found that Arctic region is severely impacted by wildfire burning events in July and August, which primarily occur in central and eastern Siberia and followed in subpolar North America. The plumes from wildfire transport aerosols to the Arctic atmosphere with the westerly circulation, leading to an increase in fine-mode aerosols containing large amounts of organic carbon, with fraction as high as 97–98 %. Absorptive carbonaceous aerosols also increase synergistically, which could convert the instantaneous direct aerosol radiative effect into a heating effect on the Earth–atmosphere system. This study provides insights into the complex sources of aerosol loading in the Arctic atmosphere in summer and emphasizes the important impacts of the increasingly frequent occurrence of wildfire burning events in recent years.

Threefold reduction of modeled uncertainty in direct radiative effects over biomass burning regions by constraining absorbing aerosols.

Absorbing aerosols emitted from biomass burning (BB) greatly affect the radiation balance, cloudiness, and circulation over tropical regions. Assessments of these impacts rely heavily on the modeled aerosol absorption from poorly constrained global models and thus exhibit large uncertainties. By combining the AeroCom model ensemble with satellite and in situ observations, we provide constraints on the aerosol absorption optical depth (AAOD) over the Amazon and Africa. Our approach enables identification of error contributions from emission, lifetime, and MAC (mass absorption coefficient) per model, with MAC and emission dominating the AAOD errors over Amazon and Africa, respectively. In addition to primary emissions, our analysis suggests substantial formation of secondary organic aerosols over the Amazon but not over Africa. Furthermore, we find that differences in direct aerosol radiative effects between models decrease by threefold over the BB source and outflow regions after correcting the identified errors. This highlights the potential to greatly reduce the uncertainty in the most uncertain radiative forcing agent.

Aerosol absorption using in situ filter-based photometers and ground-based sun photometry in the Po Valley urban atmosphere

Abstract. Light-absorbing aerosols (LAAs) are short-lived climate forcers with a significant impact on Earth's radiative balance. LAAs include dust aerosols, black carbon (BC) and organic light-absorbing carbonaceous aerosol (collectively termed brown carbon, BrC), which have also been proven to be highly toxic. In this study, aerosol absorption at five wavelengths (ranging from ultraviolet to infrared) was monitored continuously using filter-based photometers during two winter seasons in 2020 and 2021 in the city of Modena (southern central Po Valley, northern Italy), at two regulatory air quality monitoring sites, along with other pollutants (coarse particulate matter, PM10; fine particulate matter, PM2.5; O3; NO; NO2; and C6H6) and the vehicular traffic rate. The aerosol optical depth (AOD) and other column aerosol optical properties were concurrently monitored at four wavelengths by an AErosol RObotic NETwork (AERONET) sun photometer under urban background conditions within Modena. In situ absorption levels were apportioned to both sources (fossil fuel and biomass burning) and species (BC and BrC), while columnar absorption was apportioned to BC, BrC and mineral dust. The combined analysis of the atmospheric aerosol and gas measurements and of the meteorological conditions (in situ and from the ERA5 reanalysis) identified the location of potential urban sources of BC and BrC, most likely related to traffic and biomass burning. In situ data show different diurnal/weekly patterns for BrC from biomass burning and BC from traffic, with minor differences between the background and the urban traffic conditions. AERONET version 3 absorption aerosol optical depth (AAOD) retrievals at four wavelengths allowed the estimation of the absorptive direct radiative effect due to LAAs over the same period under the reasonable assumption that the AOD signal is concentrated within the mixing layer. AERONET retrievals showed a modest correlation of columnar absorption with planetary boundary layer (PBL)-scaled in situ observations, although the correlation improved significantly during a desert dust transport event that affected both in situ aerosol and columnar absorption, particularly in the blue spectrum range. A low correlation occurred between the contribution of BrC to aerosol absorption for the in situ and the columnar observations, with the BrC contribution being generally larger for in situ observations. Finally, evidence of a highly layered atmosphere during the study period, featuring significant spatial mixing and modest vertical mixing, was shown by ERA5-based atmospheric temperature profiles and by the large correlation of concurrent AERONET AOD retrievals in Modena and in Ispra (on the northwestern side of the Po Valley, ca. 225 km from Modena).

The Surface Atmosphere Integrated Field Laboratory (SAIL) Campaign

Abstract The science of mountainous hydrology spans the atmosphere through the bedrock and inherently crosses physical and disciplinary boundaries: land–atmosphere interactions in complex terrain enhance clouds and precipitation, while watersheds retain and release water over a large range of spatial and temporal scales. Limited observations in complex terrain challenge efforts to improve predictive models of the hydrology in the face of rapid changes. The Upper Colorado River exemplifies these challenges, especially with ongoing mismatches between precipitation, snowpack, and discharge. Consequently, the U.S. Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) user facility has deployed an observatory to the East River Watershed near Crested Butte, Colorado, between September 2021 and June 2023 to measure the main atmospheric drivers of water resources, including precipitation, clouds, winds, aerosols, radiation, temperature, and humidity. This effort, called the Surface Atmosphere Integrated Field Laboratory (SAIL), is also working in tandem with DOE-sponsored surface and subsurface hydrologists and other federal, state, and local partners. SAIL data can be benchmarks for model development by producing a wide range of observational information on precipitation and its associated processes, including those processes that impact snowpack sublimation and redistribution, aerosol direct radiative effects in the atmosphere and in the snowpack, aerosol impacts on clouds and precipitation, and processes controlling surface fluxes of energy and mass. Preliminary data from SAIL’s first year showcase the rich information content in SAIL’s many datastreams and support testing hypotheses that will ultimately improve scientific understanding and predictability of Upper Colorado River hydrology in 2023 and beyond.

Distributions and Direct Radiative Effects of Different Aerosol Types in North China

Different aerosol types exhibit distinct radiative effects in different regions, attributed to their unique optical characteristics and regional distributions. This study focuses on North China, which is impacted by both natural and anthropogenic aerosols with high concentrations and a variety of aerosol types. While many studies on aerosol direct radiative effects have been conducted in this region, the majority have focused on a specific type of aerosol or overall aerosol, leaving limited research on the direct radiative effects and contributions of different aerosol types. In this study, we use CALIPSO satellite data from 2011 to 2020 to investigate concentrations and distributions of different aerosol types. The results reveal that dust, polluted dust, polluted continental/smoke, and elevated smoke are the dominant aerosol types in North China. Based on the radiative closure experiment, we systematically calculate the radiative effects of different aerosol types and their corresponding contributions to the energy budget by combining satellite data with the Fu–Liou radiative transfer model. The annual average net aerosol direct radiative effect (ADRE) of North China is −6.1 and −13.43 W m−2 at the TOA and surface, respectively, causing a net warming effect of 7.33 W m−2 in the atmosphere. For each main aerosol type, dust contributes 93% to the shortwave ADRE in the western dust source region, while polluted dust mainly contributes 31% and 45% of the total ADRE, in Northwest China and North China Plain, respectively. Anthropogenic pollutant aerosols account for 58% of the total ADRE in Northeast China. This study holds great significance in elucidating the dominant aerosol types and their concentrations in North China, comprehending the impacts of different aerosol types on the local energy balance.

Impacts of vertical distribution of Southeast Asian biomass burning emissions on aerosol distributions and direct radiative effects over East Asia

The impacts of vertical distribution of biomass burning (BB) emissions on aerosol distributions and direct radiative effects over the BB source regions of Mainland Southeast Asia (MSEA) and downwind East Asian regions during spring (March to May) 2019 were investigated by applying an online coupled regional chemistry-aerosol-climate model (RIEMS-Chem). Model validation against a variety of observations demonstrated a generally good skill of the model in simulating aerosol chemical components, aerosol optical depth (AOD), and vertical distribution of aerosol extinction coefficient (EXT) when BB emissions were included. Four methods were adopted to represent injection height of BB emissions, including (1) a physical process-based parameterization (BB_param), (2) satellite-based prescribed profiles (BB_prof), (3) temporal-spatial varied injection profiles from the GFAS (Global Fire Assimilation System) dataset (BB_GFAS), and (4) BB emissions released at a fixed altitude (BB_high). The BB_param experiment generally produced better statistics compared to observations. Different BB injection height treatments considerably affected concentrations and distributions of BB aerosols, aerosol optical properties, direct radiative effects of BB aerosols (DREBB), atmospheric heating rate, and cloud fractions. The simulated sub-regional (100–120°E and 19–26°N, including major BB source and downwind areas) and seasonal mean DREBB at the top of the atmosphere (TOA) were +1.7 W m−2, +1.3 W m−2, +1.2 W m−2, and +1.7 W m−2 in the BB_param, BB_prof, BB_GFAS, and BB_high experiments, respectively, while the corresponding mean DREBB at the surface were −30.3 W m−2, -19.1 W m−2, -19.0 W m−2, and -22.1 W m−2. It is noticed that the DREBB at TOA and at the surface in BB_GFAS were just 68% and 63% of the values in BB_param, and the different injection height treatment had larger influences on DREBB at the surface than at TOA. The BB aerosol-induced atmospheric heating rate was up to 0.8–1.2 K/day in BB_param, which was larger than those in other experiments. Low cloud was enhanced while middle and high clouds were reduced by BB aerosols over northern MSEA. The BB aerosol-induced changes in cloud fractions in the BB_param experiment (up to 0.15 for low cloud and −0.05 for middle and high cloud) were approximately twice those in the other experiments. This study demonstrates the importance and necessity of properly representing the injection height of BB emissions in model estimation of radiative and climatic effects of BB aerosols.