Effects Of Aerosols Research Articles

Stratus and Stratocumulus Cloud Microphysics and Drizzle Relationships With CCN Modality

AbstractHigh resolution extended‐range cloud condensation nuclei (CCN) spectral comparisons with cloud microphysics and drizzle of the Physics of Stratocumulus Tops (POST) field experiment confirmed results in the Marine Stratus/Stratocumulus Experiment (MASE). Both of these stratus cloud projects demonstrated that bimodal CCN spectra typically caused by cloud processing were associated with clouds that exhibited higher concentrations of smaller droplets with narrower distributions and less drizzle than clouds associated with unimodal CCN spectra. Resulting brighter clouds and increased cloudiness could enhance both indirect aerosol effects (IAE). These stratus findings are opposite of analogous measurements in two cumulus cloud projects, which showed bimodal CCN associated with fewer larger droplets more broadly distributed and with more drizzle than clouds associated with unimodal CCN. Resulting reduced cumulus brightness and cloudiness could reduce both IAE. Physics of Stratocumulus Tops (POST) flights in air masses with higher CCN concentrations, NCCN, showed more extremes of the stratus characteristics. However, POST flights with lower NCCN showed opposite droplet characteristics similar to the cumulus clouds, yet still showed less drizzle in clouds associated with bimodal CCN, but not as much less as the flights with higher NCCN. Since all MASE clouds were in polluted air masses, while the two cumulus projects were in clean air masses we deduce from these four projects that both the dynamic stratus/cumulus differences (vertical wind) and NCCN are responsible for the microphysics and drizzle differences among these projects. This is because the clean POST characteristics are a hybrid between MASE/POST high NCCN and the two cumulus projects.

Intrinsic Chemical Drivers of Organic Aerosol Volatility: From Experimental Insights to Model Predictions

AbstractAccurately predicting the volatilities of molecules in aerosols is challenging but crucial for understanding the atmospheric effects of aerosols. We used negative and positive ion electrospray ionization Fourier‐transform ion cyclotron resonance mass spectrometry (FT‐ICR MS) to identify differences in the molecular compositions of gas and particle phase samples from urban atmosphere. We aimed to identify intrinsic chemical parameters that determine and predict the organic aerosol volatility. We found higher average molecular weights, carbon mass percentages, and double bond equivalents (DBE) but lower average O/C ratios and oxygen mass percentages in the particle phase than the gas phase. We identified DBE, which display a significant negative correlation with volatility, as a key parameter. We proposed to improve the previous model for predicting organic aerosol volatility by incorporating DBE as a new variant; and the result showed that this subsequently improved the accuracy of the model, particularly for compounds with minimal or no heteroatoms (0–2) such as hydrocarbons (CH). The revised model offers insights into the contributions of DBE, carbon, nitrogen, oxygen, and sulfur atoms to the volatilities of diverse organic molecules in aerosols and could be applied to improve our understanding of the phase distributions of volatile organic compounds in the ambient air.

Effect of Regional Anthropogenic Aerosols on Tropical Cyclone Frequency of Occurrence

AbstractPrevious studies have highlighted the distinct impacts of anthropogenic aerosols from the Western and Eastern Hemispheres on past multi‐decadal changes in tropical cyclone frequency of occurrence (TCF). However, the detailed effect of subregional aerosol variations remained unclear. Using idealized simulations with a dynamical climate model, this study reveals that reduced aerosol emissions from Europe and the U.S. since 1980 may have equally contributed to increased TCF over the North Atlantic, with Europe playing a major role in the decreased TCF in the South Indian Ocean and the U.S. contributing to the decrease in TCF in the South Pacific. Additionally, increased aerosol emissions from India since 1980 may have played a major role in decreasing TCF over the western North Pacific compared to increased emissions from China. TCFs are projected to decrease for most global tropics toward the end of this century due to the dominant effect of increasing greenhouse gases.

Future photovoltaic potential in India: navigating the interplay between air pollution control and climate change mitigation

Abstract India has set ambitious solar energy targets to meet its climate commitments. However, climate change, already evident in the country, poses significant challenges to solar power generation. Therefore, assessing the impact of climate change on future photovoltaic potential in India is essential. This study evaluates the mid-century (2041-2050) solar photovoltaic potential across Indian power grids using CMIP6 models under two scenarios: SSP2-4.5 (moderate climate action with intermediate air pollution) and SSP5-8.5 (weak climate action with strong air pollution control). The results indicate that the nationally averaged photovoltaic potential is projected to decrease by -2.3±0.6% (SSP5-8.5) to -3.3±0.9% (SSP2-4.5) compared to the 1985-2014 baseline, primarily due to reduced radiation and increased temperatures. Additionally, cell temperatures are expected to rise by 1.5±0.13°C (SSP2-4.5) to 2±0.11°C (SSP5-8.5), leading to efficiency losses and additional 18±5 days under SSP2-4.5 (26±3 days under SSP5-8.5) of efficiency de-rating, particularly in solar-rich regions. This translates to a loss of 600±160 GWh under SSP2-4.5 and 840±100 GWh under SSP5-8.5, based on the solar generation status of 2023-24. Overall, SSP5-8.5 projects a smaller reduction in photovoltaic potential, it also predicts greater temperature-induced efficiency losses compared to SSP2-4.5, due to aerosol direct effect and weak climate action. Finally, this assessment highlights the need for combined climate and pollution mitigation efforts to boost India’s photovoltaic potential and secure a sustainable, resilient energy future.

The spatiotemporal and dependency analysis of selected meteorological parameters and normalized difference vegetation index with aerosol optical depth over east Africa

The unprecedented rise in atmospheric aerosols, coupled with their intricate interactions with the environment through a wide array of physical, chemical, and biological processes, has profoundly impacted global climate. Their presence in the atmosphere scatters and absorbs solar radiation, thus altering the amount of sunlight reaching the Earth's surface. These direct effects, along with the indirect effects of aerosols, have significantly altered atmospheric temperatures, land surface processes, global surface temperature, hydrological cycle, and ecosystems. Understanding the complex interplay between aerosols and climatic variables necessitates a multidisciplinary approach, such as dependency modeling. Addressing these challenges, the current study conducts a spatiotemporal correlational analysis of selected key meteorological parameters with aerosol optical depth over East Africa (EA) using multisensory data from Moderate-resolution Imaging Spectroradiometer (MODIS), Modern-Era Retrospective analysis for Research and Application (MERRA-2) model, and Tropical Rainfall Measurement Mission (TRMM). Employing a weighted least squares regression (WLS) model, the study quantifies trends in the time series of climatic variables and Normalized Difference Vegetation Index (NDVI), further utilizing a statistical dependency modeling technique for correlational analysis. The trend analysis reveals a significant decreasing trend in surface wind speed (SWS) in most months, with sporadic positive trends attributed to anthropogenic activities, notably biomass burning, observed in January. Spatial trend analysis of Precipitation Rate (PR) displays heterogeneity, with significant negative trends in January and March, and positive trends in February, April, November, and December. Negative trends during May to August are attributed to increased anthropogenic activities, while enhanced positive trends in May correlate with low aerosol optical depth (AOD) during this period. Surface air temperature (SAT) exhibits diverse variations across the region, with dry months recording higher averages and trends than wet months. The study notes heterogeneous correlations in NDVI over the study area, with positive and negative correlations observed in different regions. Specifically, positive correlations are noted along the coastal and Lake Victoria regions, attributed to improved PR enhancing vegetation cover in these areas.

Random Forest Spatial-Temporal and State Space Models to Assess the Impact of Bushfire-Induced Aerosol Events on Ozone Depletion in Australia

Serious concerns exist that the increasing frequency of fires may delay the recovery of ozone given increasing temperatures due to climate change. Australian bushfires from September 2019 to February 2020 were catastrophic. A random forest spatial-temporal (RF sp) analysis using satellite data to detect an association between Australian bushfires and stratosphere ozone on the local depletion of ozone in the vicinity of fires in three regions of Australia (Pacific Ocean, Victoria, NSW) has shown a significant reduction in ozone attributable to aerosols from fires. By intervention analysis, increases in aerosols in all three regions were shown to have a significant and ongoing impact 1–5 days later on reducing ozone (p < 0.0001). Intervention analysis also gave similar periods of aerosol exceedance to those found by Hidden Markov models (HMMs). HMMs established a significant and quantifiable decline in ozone due to bushfire-induced aerosols, with significant lags of 10–25 days between times of aerosol exceedance and subsequent ozone level decline in all three regions.

Synoptic Scale Controls and Aerosol Effects on Fog and Low Stratus Life Cycle Processes in the Po Valley, Italy

AbstractFog and low stratus clouds (FLS) form as a result of complex interactions of multiple factors in the atmosphere and at the land surface and impact both the anthropogenic and natural environments. Here, we analyze the role of synoptic conditions and aerosol loading on FLS occurrence and persistence in the Po valley in northern Italy. By applying k‐means clustering to reanalysis data, we find that FLS formation in the Po valley is either based on radiative processes or moisture advection from the Mediterranean sea. Satellite‐based data on FLS persistence shows longer persistence of radiatively formed FLS events, likely due to air mass stagnation and a temperature inversion. Ground‐based aerosol optical depth observations further reveal that FLS event duration is significantly higher under high aerosol loading. The results underline the combined effect of topography, moisture advection and aerosol loading on the FLS life cycle in the Po valley.

Can satellite products monitor solar brightening in Europe?

Satellite products provide the best way to monitor the solar radiation reaching the Earth’s surface on a global scale. However, their capability to monitor solar radiation trends needs to be constantly evaluated. This depends on their temporal stability and the accurate representation of all processes driving solar radiation. This study evaluates these aspects by comparing and cross-comparing different solar radiation products (ERA5, CAMS-RAD 4.6, SARAH-3, CLARA-A3, CERES-EBAF 4.2) against in-situ measurements over Europe.All products show a moderate positive bias over Europe but strong differences in their root mean squared deviation (RMSD) related to their different cloud transmittance models. Geostationary-based products (SARAH-3, CAMS-RAD 4.6) provide the smallest RMSD closely followed by CLARA-A3, whereas ERA5 shows a large RMSD due to random errors in cloud transmittance.All products show an increase in surface solar radiation, or brightening, over the last 40 years over Europe, but the magnitude of the trends and their spatiotemporal variability differ between products. Despite finding temporal inhomogeneities in some products, the different trends are mostly due to different aerosol modeling approaches implemented by each product. Both SARAH-3 (+2.3 W/m2/decade, 2001–22) and CERES-EBAF 4.2 (+2.2 W/m2/decade, 2001–22) provide the most consistent trends compared to in-situ data, showing that after stabilizing in the late 2000s, brightening is particularly recovering in Western Europe. In-situ measurements show a reduction of aerosol optical depth from 2001 to 2022 that has been accentuated in the last 10 years, particularly in Western Europe. This would be consistent with the hypothesis that brightening recovery is driven by an aerosol reduction, though other analyses suggest that clouds also play a role in this recovery. More work is needed to understand the contribution of aerosols to solar radiation trends and the exact aerosol effects represented by each solar radiation product.

Interaction of Cooking-Generated Aerosols on the Human Nervous System and the Impact of Caloric Restriction Post-Exposure

Background: The inhalation of cooking-generated aerosols could lead to translocation to the brain and impact its function; therefore, the effects of cooking-generated aerosols on healthy adults were investigated using an electroencephalograph (EEG) during the 2 h period post-exposure. Methods: To explore any changes from the impact of exposure to cooking-generated aerosols on the human brain due to the absence of food intake during exposure, we divided the study participants into three groups: (A) no food intake for 2 h (2 h-zero calorie intake), (B) non-zero calorie intake, and (C) control group (simulated cooking). Results: The ultrafine particle concentrations increased from 9.0 × 103 particles/cm3 at the background level to approximately 8.74 × 104 particles/cm3 during cooking. EEGs were recorded before cooking (step 1), 60 min after cooking (step 2), 90 min after cooking (step 3), and 120 min after cooking (step 4). Comparing the non-zero calorie group with the control group, it was concluded that exposure to cooking-generated aerosols resulted in a 12.82% increase in the alpha band two hours post-exposure, compared to pre-exposure. The results revealed that zero calorie intake after exposure mitigated the impacts of cooking-generated aerosols for the alpha, beta3, theta, and delta bands, while it exacerbated effects on the whole brain for the beta1 and beta2 bands. Conclusions: While these are short-term studies, long-term exposure to cooking-generated ultrafine particles can be established through successive short-term exposures. These results underscore the need for further research into the health impacts of cooking-generated aerosols and the importance of implementing strategies to mitigate exposure.

Long-range transport of air pollutants increases the concentration of hazardous components of PM2.5 in northern South America

Abstract. Long-range transport (LRT) of air pollutants from a range of sources can substantially enhance background pollution levels, especially in urbanized regions, which can exacerbate high-pollution episodes. In the Aburrá Valley (AV), Colombia, and other cities in northern South America, biomass burning (BB), dust, and volcanic degassing have been identified as sources of long-range aerosol transport. However, the impact of these sources on air quality and the characterization of these sources have yet to be thoroughly studied. This work investigates the influence of these sources on the chemical composition of PM2.5 during annual and intra-annual high-load aerosol events in the AV. We identified, tracked, and meteorologically characterized LRT events and evaluated their influence on PM2.5 concentration and chemical composition. We found that the LRT of aerosols from BB, dust, and volcanic degassing influenced approximately 13 %, 8 %, and 13 % of days in the year, respectively. We applied the positive-matrix-factorization (PMF) statistical model to quantify PM2.5 concentrations and chemical compositions for the different LRT event types (e.g., BB). For BB events, we identified large contributions from organic carbon (OC1 and OC2), F−, and secondary aerosol tracers (SO42- and NO3-). For dust LRT events, crustal mineral components, along with Ti and Ca, were the primary contributors to aerosol composition, while SO42-, Na, Al, and Ca were the primary contributors during volcanic events. The concentrations of some ions and toxic heavy metals (Cr, Mn, Cd, and Ni) were also elevated during BB and volcanic-degassing events. BB contributed the most to PM2.5 levels during the LRT events (∼11 µg m−3), while contributions from aerosols arising from dust and volcanic events were also substantial (<7 µg m−3). Our study identifies the Orinoco and the Middle Magdalena Valley as sizable sources of BB aerosols and Nevado del Ruiz as a source of volcanic aerosols. Additionally, we found that African dust reached the Andean region via the Caribbean route. As a result, we identify the need for future chemical-transport modeling studies in the region and new support strategies to manage internal and external pollution sources that degrade air quality in the AV and the surrounding region.

The Transition from Aerosol- to Updraft-Limited Susceptibility Regime in Large-Eddy Simulations with Bulk Microphysics

Large-eddy simulation (LES) is often used as a benchmark simulation in climate science and is suggested as a fundamental tool to examine, e.g., marine cloud brightening. Therefore, it is necessary to critically evaluate if these high-resolution models can skillfully simulate expected physical phenomena. This study focuses on the first indirect aerosol effect in warm stratocumulus clouds. We investigate if an LES code with explicit aerosol-cloud interactions and a widely used two-moment bulk microphysical scheme can reproduce well-known cloud droplet number susceptibility regimes previously identified by observations and supported by detailed parcel model simulations—the updraft-limited regime (typically occurring at high aerosol number concentrations and low updraft speeds) and the aerosol-limited regime (typically occurring at low aerosol number concentrations and high updraft speeds). Our simulations show that the LES in its default configuration cannot reproduce the two regimes if the initial droplet radius of newly activated droplets (rid) is estimated by integrating the wet aerosol size distribution. The main reason is related to the relatively coarse (but commonly used) time step in the model (Δt ≈ 1s), which is too long to resolve relevant microphysical processes adequately at high aerosol concentrations. A regime transition does occur if the timestep is decreased to Δt ≈ 0.1s and if a renormalization procedure is applied, which limits the number of activated droplets so that the water mass of the newly activated droplets cannot exceed the available amount of supersaturated water vapor. Another way to obtain a regime transition is to increase rid to values >1 µm. However, a clear recommendation for the choice of rid cannot be made upon physical arguments. An alternative solution could be to introduce a sub-time-stepping or adaptive time-stepping algorithm to calculate droplet formation and growth, particularly for updraft-limited conditions. Our study highlights the importance of critically evaluating LES results to guarantee that relevant physical processes are properly represented.

Measurement report: In situ vertical profiles of below-cloud aerosol over the central Greenland Ice Sheet

Abstract. Surface radiative cooling in polar regions can generate persistent stability in the atmospheric boundary layer. Stable layers below clouds can decouple the cloud layer from the near-surface environment. Under these conditions, surface aerosol measurements are not necessarily representative of the near-cloud or intra-cloud aerosol populations. To better understand the variability in the vertical structure of aerosol properties over the central Greenland Ice Sheet, in situ measurements of aerosol particle size distributions up to cloud base were made at Summit Station in July and August 2023. These measurements identified distinct vertical aerosol layers between the surface- and cloud-base-associated thermodynamic decoupling layers. Such decoupling layers occur 49 % of the time during the summer in central Greenland, suggesting that surface aerosol measurements are insufficient for describing the cloud-relevant aerosol population half of the time. Experience during this first measurement season demonstrated the ability of a tethered-balloon platform to operate effectively under icing conditions and at low surface pressure (< 680 hPa). The results presented here illustrate the value of vertically resolved in situ measurements of aerosol properties in developing a nuanced understanding of the aerosol effects on cloud properties in polar regions.

Emerging signals of climate change from the equator to the poles: new insights into a warming world

The reality of human-induced climate change is unequivocal and exerts an ever-increasing global impact. Access to the latest scientific information on current climate change and projection of future trends is important for planning adaptation measures and for informing international efforts to reduce emissions of greenhouse gases (GHGs). Identification of hazards and risks may be used to assess vulnerability, determine limits to adaptation, and enhance resilience to climate change. This article highlights how recent research programs are continuing to elucidate current processes and advance projections across major climate systems and identifies remaining knowledge gaps. Key findings include projected future increases in monsoon rainfall, resulting from a changing balance between the rainfall-reducing effect of aerosols and rainfall-increasing GHGs; a strengthening of the storm track in the North Atlantic; an increase in the fraction of precipitation that falls as rain at both poles; an increase in the frequency and severity of El Niño Southern Oscillation (ENSO) events, along with changes in ENSO teleconnections to North America and Europe; and an increase in the frequency of hazardous hot-humid extremes. These changes have the potential to increase risks to both human and natural systems. Nevertheless, these risks may be reduced via urgent, science-led adaptation and resilience measures and by reductions in GHGs.

Toward Fine Horizontal Resolution Global Simulations of Aerosol Sectional Microphysics: Advances Enabled by GCHP‐TOMAS

AbstractGlobal modeling of aerosol‐particle number and size is important for understanding aerosol effects on Earth's climate and air quality. Fine‐resolution global models are desirable for representing nonlinear aerosol‐microphysical processes, their nonlinear interactions with dynamics and chemistry, and spatial heterogeneity. However, aerosol‐microphysical simulations are computationally demanding, which can limit the achievable global horizontal resolution. Here, we present the first coupling of the TwO‐Moment Aerosol Sectional (TOMAS) microphysics scheme with the High‐Performance configuration of the GEOS‐Chem model of atmospheric composition (GCHP), a coupling termed GCHP‐TOMAS. GCHP's architecture allows massively parallel GCHP‐TOMAS simulations including on the cloud, using hundreds of computing cores, faster runtimes, more memory, and finer global horizontal resolution (e.g., 25 km × 25 km, 7.8 × 105 model columns) versus the previous single‐node capability of GEOS‐Chem‐TOMAS (tens of cores, 200 km × 250 km, 1.3 × 104 model columns). GCHP‐TOMAS runtimes have near‐ideal scalability with computing‐core number. Simulated global‐mean number concentrations increase (dominated by free‐tropospheric over‐ocean sub‐10‐nm‐diameter particles) toward finer GCHP‐TOMAS horizontal resolution. Increasing the horizontal resolution from 200 km × 200–50 km × 50 km increases the global monthly mean free‐tropospheric total particle number by 18.5%, and over‐ocean sub‐10‐nm‐diameter particles by 39.8% at 4‐km altitude. With a cascade of contributing factors, free‐tropospheric particle‐precursor concentrations increase (32.6% at 4‐km altitude) with resolution, promoting new‐particle formation and growth that outweigh coagulation changes. These nonlinear effects have the potential to revise current understanding of processes controlling global aerosol number and aerosol impacts on Earth's climate and air quality.

Century‐Long Variations in Surface Incident Solar Radiation Over Japan——Characterized by Observations and Reanalyses

ABSTRACTSurface incident solar radiation (Rs) is of great importance in determining the energy balance in the Earth system. In this study, we use century‐long homogenized observations over Japan to constrain five 20th century reanalyses to explore their performance in reproducing Rs variation on different time scales (high‐frequency components [HFCs], for signals with cycles less than 10 years; low‐frequency components [LFCs], for signals with cycles more than 10 years) by ensemble empirical mode decomposition (EEMD) method and to quantify the impact factors on the Rs estimations by the sum of tree (SOT) model. It is found that ERA20C, ERA20CM and CERA20C overestimated Rs by 0.48–1.49 W/m−2, while 20CRv2c and 20CRv3 underestimated Rs by −0.63 and −1.18 W/m−2, respectively for 1931–2010. Poor correlation coefficient (R) was found to be 0.10 for ERA20CM and 0.22 for 20CRv2c. 20CRv2c failed for 1931–1960 but improved considerably for 1961–2010. 20CRv3 uses an upgraded model and assimilates more observations compared with its predecessor 20CRv2c; however, only the original components and HFCs in Rs were improved, with nearly no improvement in the LFCs. In general, CERA20C Rs, with small biases and higher R of 0.73 for original signals, 0.83 for HFCs and LFCs, is superior to other reanalyses. No obvious trend in clear sky Rs demonstrated that reanalysed Rs are insensitive to the aerosol forcings. Therefore, cloud cover and water vapour maybe the main factors influenced reanalysed Rs. Most of time, Rs is more sensitive to cloud cover than vapour pressure for all reanalyses except original signals (with contribution ratio of 0.29 for cloud cover and 0.71 for vapour pressure) and LFCs (with contribution ratio of 0.41 for cloud cover and 0.59 for vapour pressure) in CERA20C, and original signals (with contribution ratio of 0.37 for cloud cover and 0.63 for vapour pressure) in ERA20C. This work pointed out that aerosol related processes such as aerosol forcings or aerosol radiative effect in reanalyses should be improved in the future, which will ultimately improve the interaction between aerosol and cloud in Rs simulations.

Do Subsampling Strategies Reduce the Confounding Effect of Errors in Bispectral Retrievals on Estimates of Aerosol Cloud Interactions?

AbstractBi‐spectral retrievals of droplet effective radius and cloud optical depth are widely utilized to estimate aerosol cloud interactions (ACI) in warm clouds in the marine boundary layer. Here, we assess the effect of retrieval errors due to the neglect of 3D radiative transfer during the retrieval process on this analysis of ACI. We use an ensemble of stochastically‐modeled cloud fields and 3D radiative transfer simulations to study the retrieval errors at a solar zenith angle of 30°. Simulated retrieval biases in droplet number concentration (Nd) for all three MODIS channels vary systematically from +35% to −80% as cloud heterogeneity increases. Pixel‐level errors can be much larger. Commonly utilized subsampling strategies do not reduce the systematic variation in retrieval error. Negative error correlations between optical depth and droplet effective radius produce spuriously negative slopes between the logarithm of liquid water path and Nd (−1.0 to −0.3). Pixels at the center of (8 km)2 patches that are not overcast have a relative bias in Nd of −50%. The relative frequency of these biased pixels varies linearly with the clear fraction in MODIS data and form the basis for a simple parameterization of Nd bias that varies with cloud fraction (CF). Using this parameterization, synthetic data experiments indicate that estimates of the first indirect effect in the tropical ocean can be overestimated by up to 30%, and the effect of aerosol on CF is overestimated by 50%, due to neglecting the correlation between retrieval errors and cloud microphysics.

Characteristics of light absorption and environmental effects of Brown carbon aerosol in Chongqing during summer and winter based on online measurement: Implications of secondary formation

Light-absorbing organic carbon (i.e., brown carbon, BrC) significantly contributes to light absorption and radiative forcing in the atmospheric particles. However, the secondary formation of BrC and optical properties of secondary BrC are poorly understood. In this study, we analyzed and evaluated the light absorption and environmental effects of BrC and secondary BrC from July 1st to 31st, 2022 (summer) and January 20th to February 20th, 2023 (winter) in Chongqing. BrC and secondary BrC light absorption were estimated via a seven-wavelength aethalometer and the statistical approach. The average values of secondary BrC light absorption (AbsBrC,sec,λ) accounted for 46.2–56.5% of AbsBrC. AbsBrC,370 and AbsBrC,sec,370 were significantly higher during winter (26.2 ± 13.2 and 9.1 ± 5.2 Mm−1 respectively) than that during summer (7.2 ± 4.1 and 5.2 ± 3.5 Mm−1 respectively) (p < 0.001), suggesting secondary formation played an essential role in BrC. A diurnal cycle of AbsBrC,sec,370 was explained by the photobleaching of light-absorbing chromophores under the oxidizing conditions in the daytime, and the formation of chromophores via aqueous reactions with NH4+ and NOx after sunset during winter. PSCF analysis showed that transport of anthropogenic emissions from the northeastern and southeastern areas of Chongqing was the important source of the secondary BrC in PP during winter. During winter, the average values of SFEBrC and SFEBrC,sec were 31.9 and 27.4 W g−1 lower than that during summer (64.7 and 44.5 W g−1), respectively. In contrast, J[NO2] values of SFEBrC and SFEBrC,sec decreased by 23.3% and 8.7% during winter higher than that during summer (19.9% and 5.6%), indicating that BrC and secondary BrC cause substantial radiative effects and atmospheric photochemistry. Overall, this study is helpful in understanding the characterization and secondary formation of BrC and accurately evaluating the environmental effects of BrC in Chongqing.

Increasing aerosol direct effect despite declining global emissions in MPI-ESM1.2

Abstract. Anthropogenic aerosol particles partially mask global warming driven by greenhouse gases, both directly by reflecting sunlight back to space and indirectly by increasing cloud reflectivity. In recent decades, emissions of anthropogenic aerosols have declined globally and at the same time shifted from the North American and European regions, foremost to Southeast Asia. Using simulations with the Max Planck Institute Earth System Model version 1.2 (MPI-ESM1.2), we find that the direct effect of aerosols has continued to increase despite declining emissions. Concurrently, the indirect effect has diminished in approximate proportion to the emissions. In this model, which employs parameterized aerosol effects with constant regional direct effect efficiency, the enhanced efficiency of aerosol radiative forcing in emissions is associated with less cloud masking, longer atmospheric residence times, and differences in aerosol optical properties.

The impact of coupled 3D shortwave radiative transfer on surface radiation and cumulus clouds over land

Abstract. Radiative transfer is a 3D process, but most atmospheric models consider radiation only in the vertical direction for computational efficiency. This results in inaccurate surface radiation fields, as the horizontal transport of radiation is neglected. Previous work on 3D radiative effects mainly used 3D radiative transfer uncoupled from the flow solver. In contrast, our current work uses 3D radiative transfer coupled to the flow solver to study its impact on the development of clouds and the resulting impact on the domain-averaged surface solar irradiance. To this end, we performed a series of realistic large-eddy simulations with MicroHH. To improve the level of realism of our radiation, we first included the direct effect of aerosols using aerosol data from the Copernicus Atmosphere Monitoring Service (CAMS) global reanalysis. Next, we performed simulations with 1D radiative transfer and with a coupled ray tracer for 12 d on which shallow cumulus clouds formed over Cabauw, the Netherlands. In general, simulations with the coupled ray tracer have a higher domain-averaged liquid water path, larger clouds, and similar cloud cover compared to simulations with 1D radiative transfer. Furthermore, the domain-averaged direct radiation is decreased with 3D radiative transfer, and the diffuse radiation is increased. However, the average difference in global radiation is less than 1 W m−2, as the increase in global radiation from uncoupled 3D radiative transfer is counterbalanced by a decrease in global radiation caused by changes in cloud properties.

Surface albedo regulates aerosol direct climate effect

Aerosols and Surface Albedo (SA) are critical in balancing Earth’s energy budget. With the changes of surface types and corresponding SA in recent years, an intriguing yet unresolved question emerges: how does Aerosol Direct Radiative Effect (ADRE) and its warming effect (AWE) change with varying SA? Here we investigate the critical SA marking ADRE shift from negative to positive under varying aerosol properties, along with the impact of SA on the ADRE. Results show that AWE often occurs in mid-high latitudes or regions with high-absorptivity aerosols, with critical SA ranging from 0.18 to 0.96. Thinner and/or more absorptive aerosols more readily cause AWE statistically. In regions where the SA trend is significant, SA has decreased at −0.012/decade, causing a −0.2 ± 0.17 W/m²/decade ADRE change, with the most pronounced changes in the Northern Hemisphere during June-July. As SA declines, we highlight enhanced ADRE cooling or reduced AWE, indicating aerosols’ stronger cooling, partly countering the energy rise from SA reduction.