Global Aerosol Radiative Forcing Research Articles

The worldwide COVID-19 lockdown impacts on global secondary inorganic aerosols and radiative budget.

Global lockdown measures to prevent the spread of the coronavirus disease 2019 (COVID-19) led to air pollutant emission reductions. While the COVID-19 lockdown impacts on both trace gas and total particulate pollutants have been widely investigated, secondary aerosol formation from trace gases remains unclear. To that end, we quantify the COVID-19 lockdown impacts on NOx and SO2 emissions and sulfate-nitrate-ammonium aerosols using multiconstituent satellite data assimilation and model simulations. We find that anthropogenic emissions over major polluted regions were reduced by 19 to 25% for NOx and 14 to 20% for SO2 during April 2020. These emission reductions led to 8 to 21% decreases in sulfate and nitrate aerosols over highly polluted areas, corresponding to >34% of the observed aerosol optical depth declines and a global aerosol radiative forcing of +0.14 watts per square meter relative to business-as-usual scenario. These results point to the critical importance of secondary aerosol pollutants in quantifying climate impacts of future mitigation measures.

Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing

Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway and the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and, hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions, based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden and the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg S (+29 %) and 582 Gg S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is −0.11 W m−2. The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2, with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms the sensitivity of aerosol IRF to the PI aerosol loading and the need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes.

Radiative effects of reduced aerosol emissions during the COVID-19 pandemic and the future recovery

The pandemic in 2020 caused an abrupt change in the emission of anthropogenic aerosols and their precursors. We estimate the associated change in the aerosol radiative forcing at the top of the atmosphere and the surface. To that end, we perform new simulations with the CMIP6 global climate model EC-Earth3. The simulations use the here newly created data for the anthropogenic aerosol optical properties and an associated effect on clouds from the simple plumes parameterization (MACv2-SP), based on revised SO2 and NH3 emission scenarios. Our results highlight the small impact of the pandemic on the global aerosol radiative forcing in 2020 compared to the CMIP6 scenario SSP2-4.5 of the order of +0.04Wm−2, which is small compared to the natural year-to-year variability in the radiation budget. Natural variability also limits the ability to detect a meaningful regional difference in the anthropogenic aerosol radiative effects. We identify the best chances to find a significant change in radiation at the surface during cloud-free conditions for regions that were strongly polluted in the past years. The post-pandemic recovery scenarios indicate a spread in the aerosol forcing of −0.68 to −0.38Wm−2 for 2050 relative to the pre-industrial, which translates to a difference of +0.05 to −0.25Wm−2 compared to the 2050 baseline from SSP2-4.5. This spread falls within the present-day uncertainty in aerosol radiative forcing and the CMIP6 spread in aerosol forcing at the end of the 21st century. We release the new MACv2-SP data for studies on the climate response to the pandemic and the recovery scenarios. Our 2050 forcing estimates suggest that sustained aerosol emission reductions during the post-pandemic recovery cause a stronger climate response than in 2020, i.e., there is a delayed influence of the pandemic on climate.

Historical (1850–2014) Aerosol Evolution and Role on Climate Forcing Using the GISS ModelE2.1 Contribution to CMIP6

AbstractThe Earth's climate is rapidly changing. Over the past centuries, aerosols, via their ability to absorb or scatter solar radiation and alter clouds, played an important role in counterbalancing some of the greenhouse gas (GHG) caused global warming. The multicentury anthropogenic aerosol cooling effect prevented present‐day climate from reaching even higher surface air temperatures and subsequent more dramatic climate impacts. Trends in aerosol concentrations and optical depth show that in many polluted regions such as Europe and the United States, aerosol precursor emissions decreased back to levels of the 1950s. More recent polluting countries such as China may have reached a turning point in recent years as well, while India still follows an upward trend. Here we study aerosol trends in the Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations of the GISS ModelE2.1 climate model using a fully coupled atmosphere composition configuration, including interactive gas‐phase chemistry and either an aerosol microphysical (MATRIX) or a mass‐based (One‐Moment Aerosol, OMA) aerosol module. Results show that whether global aerosol radiative forcing is already declining depends on the aerosol scheme used. Using the aerosol microphysical scheme, where the aerosol system reacts more strongly to the trend in sulfur dioxide (SO2) emissions, global peak direct aerosol forcing was reached in the 1980s, whereas the mass‐based scheme simulates peak direct aerosol forcing around 2010.

Overview of the NOAA/ESRL Federated Aerosol Network

AbstractTo estimate global aerosol radiative forcing, measurements of aerosol optical properties are made by the National Oceanic and Atmospheric Administration (NOAA) Earth System Research Laboratory (ESRL)’s Global Monitoring Division (GMD) and their collaborators at 30 monitoring locations around the world. Many of the sites are located in regions influenced by specific aerosol types (Asian and Saharan desert dust, Asian pollution, biomass burning, etc.). This network of monitoring stations is a shared endeavor of NOAA and many collaborating organizations, including the World Meteorological Organization (WMO)’s Global Atmosphere Watch (GAW) program, the U.S. Department of Energy (DOE), several U.S. and foreign universities, and foreign science organizations. The result is a long-term cooperative program making atmospheric measurements that are directly comparable with those from all the other network stations and with shared data access. The protocols and software developed to support the program facilitate participation in GAW’s atmospheric observation strategy, and the sites in the NOAA/ESRL network make up a substantial subset of the GAW aerosol observations. This paper describes the history of the NOAA/ESRL Federated Aerosol Network, details about measurements and operations, and some recent findings from the network measurements.

The Effects of the Spatial Distribution of Direct Anthropogenic Aerosols Radiative Forcing on Atmospheric Circulation

The large uncertainty in estimating the global aerosol radiative forcing (ARF) is one of the major challenges the climate community faces for climate projection. While the global-mean ARF may affect global quantities such as surface temperature, its spatial distribution may result in local thermodynamical and, thus, dynamical changes. Future changes in aerosol emissions distribution could further modulate the atmospheric circulation. Here, the effects of the spatial distribution of the direct anthropogenic ARF are studied using an idealized global circulation model, forced by a range of estimated-ARF amplitudes, based on the Copernicus Atmosphere Monitoring Service data. The spatial distribution of the estimated-ARF is globally decomposed, and the effects of the different modes on the circulation are studied. The most dominant spatial distribution feature is the cooling of the Northern Hemisphere in comparison to the Southern Hemisphere. This induces a negative meridional temperature gradient around the equator, which modulates the mean fields in the tropics. The ITCZ weakens and shifts southward, and the Northern (Southern) Hemisphere Hadley cell strengthens (weakens). The localization of the ARF in the Northern Hemisphere midlatitudes shifts the subtropical jet poleward and strengthens both the eddy-driven jet and Ferrel cell, because of the weakening of high-latitude eddy fluxes. Finally, the larger aerosol concentration in Asia compared to North America results in an equatorial superrotating jet. Understanding the effects of the different modes on the general circulation may help elucidate the circulation’s future response to the projected changes in ARF distribution.

Evidence for pyrazine-based chromophores in cloud water mimics containing methylglyoxal and ammonium sulfate

Abstract. Simulating aqueous brown carbon (aqBrC) formation from small molecule amines and aldehydes in cloud water mimics provides insight into potential humic-like substance (HULIS) contributors and their effect on local and global aerosol radiative forcing. Previous work has shown that these (Maillard type) reactions generate products that are chemically, physically, and optically similar to atmospheric HULIS in many significant ways, including in their complexity. Despite numerous characterization studies, attribution of the intense brown color of many aqBrC systems to specific compounds remains incomplete. In this work, we present evidence of novel pyrazine-based chromophores (PBCs) in the product mixture of aqueous solutions containing methylglyoxal and ammonium sulfate. PBCs observed here include 2,5-dimethyl pyrazine (DMP) and products of methylglyoxal addition to the pyrazine ring. This finding is significant as the literature of Maillard reactions in food chemistry tightly links the formation of pyrazine (and related compounds) to browning in foods. We investigated the roles of both cloud processing (by bulk evaporation) and pH in absorptivity and product distribution in microliter samples to understand the contribution of these PBCs to aqBrC properties. In agreement with previous work, we observed elevated absorptivity across the entire UV–visible spectrum following simulated cloud processing as well as higher absorptivity in more basic samples. Absorptivity of the pH 2 sample, following evaporation over a period of days, exceeded that of the unevaporated pH 9 sample. In addition, mixtures of ammonium sulfate and methylglyoxal at pH 5 that were dried in under 1 h and analyzed 24 h later were as absorptive as pH 9 samples allowed to react for 7 days, indicating that evaporation occurring during cloud processing may provide a reaction pathway favorable for carbonyl–ammonia chemistry even under acidic conditions of aerosol and cloud water. The fraction of pyrazine compounds in the product mixture increased by up to a factor of 4 in response to drying with a maximum observed contribution of 16 % at pH 5. Therefore, cloud processing under acidic conditions may produce PBCs at the expense of imine- and imidazole-derived compounds. This finding has implications for further BrC reactivity and degradation pathways.

Global climate forcing of aerosols embodied in international trade

International trade separates regions consuming goods and services from regions where goods and related aerosol pollution are produced. Yet the role of trade in aerosol climate forcing attributed to different regions has never been quantified. Here, we contrast the direct radiative forcing of aerosols related to regions’ consumption of goods and services against the forcing due to emissions produced in each region. Aerosols assessed include black carbon, primary organic aerosol, and secondary inorganic aerosols, including sulfate, nitrate and ammonium. We find that global aerosol radiative forcing due to emissions produced in East Asia is much stronger than the forcing related to goods and services ultimately consumed in that region because of its large net export of emissions-intensive goods. The opposite is true for net importers such as Western Europe and North America: global radiative forcing related to consumption is much greater than the forcing due to emissions produced in these regions. Overall, trade is associated with a shift of radiative forcing from net importing to net exporting regions. Compared to greenhouse gases such as carbon dioxide, the short atmospheric lifetimes of aerosols cause large localized differences between consumption- and production-related radiative forcing. International efforts to reduce emissions in the exporting countries will help alleviate trade-related climate and health impacts of aerosols while lowering global emissions.

Attribution of the Present-Day Aerosol Direct Radiative Forcing to Anthropogenic Emission Sectors

In this study, a general circulation model cou- pled with a gas-phase module and an aerosol chemistry module was employed to investigate the impacts of an- thropogenic emission sectors on aerosol direct radiative forcing at the top of atmosphere (TOA) in the present-day climate. The predictions were based on the emission in- ventories developed in support of the Intergovernmental Panel on Climate Change (IPCC) Fifth Assessment Re- port (AR5). Six emission sectors—agriculture, open bio- mass burning, domestic activities, industry, energy gen- eration, and transport—were considered, with a special focus on nitrate aerosol that shows large uncertainties in current models. The results show that the energy sector accounts for the largest contribution (−222 mW m −2 ) to global aerosol radiative forcing, with substantial negative forcing from sulfate. Inclusion of nitrate results in the transport sector yielding a global nitrate radiative forcing of −92 mW m −2 and an internally mixed aerosol radiative forcing of −85 mW m −2 , which is opposite to the positive radiative forcing predicted in the past, indicating that the transport emissions could not be a potential control target to counteract climate warming as expected before. The maximum change in nitrate burden is found to be associ- ated with agricultural emissions, which accounts for about 75% of global ammonia gas (NH3) emissions. Agricul- tural emissions account for global nitrate radiative forcing of −186 mW m −2 and internally mixed aerosols direct radiative forcing of −149 mW m −2 . Such agricultural ra- diative forcing exceeds the radiative forcing of the indus- trial sector and is responsible for a large portion of nega- tive radiative forcing over the Northern Hemisphere.  Keywords: anthropogenic aerosols, radiative forcing, emission sector Citation: Chang, W.-Y., 2013: Attribution of the pre- sent-day aerosol direct radiative forcing to anthropogenic emission sectors, Atmos. Oceanic Sci. Lett., 6, 369-374,

The 1985 Biomass Burning Season in South America: Satellite Remote Sensing of Fires, Smoke, and Regional Radiative Energy Budgets

Using satellite imagery, more than five million square kilometers of the forest and cerrado regions over South America are extensively studied to monitor fires and smoke during the 1985 biomass burning season. The results are characterized for four major ecosystems, namely, 1) tropical rain forest, 2) tropical broadleaf seasonal, 3) savanna/grass and seasonal woods (SGW), and 4) mild/warm/hot grass/shrub (MGS). The spatial and temporal distribution of fires are examined from two different methods using the multispectral Advanced Very High Resolution Radiometer Local Area Coverage data. Using collocated measurements from the instantaneous scanner Earth Radiation Budget Experiment data, the direct regional radiative forcing of biomass burning aerosols is computed. The results show that more than 70% of the fires occur in the MGS and SGW ecosystems due to agricultural practices. The smoke generated from biomass burning has negative instantaneous net radiative forcing values for all four major ecosystems within South America. The smoke found directly over the fires has mean net radiative forcing values ranging from 225.6 to 233.9 W m22. These results confirm that the regional net radiative impact of biomass burning is one of cooling. The spectral and broadband properties for clear-sky and smoke regions are also presented that could be used as input and/or validation for other studies attempting to model the impact of aerosols on the earth‐atmosphere system. These results have important applications for future instruments from the Earth Observing System (EOS) program. Specifically, the combination of the Visible Infrared Scanner and Clouds and the Earth’s Radiant Energy System (CERES) instruments from the Tropical Rainfall Measuring Mission and the combination of Moderate Resolution Imaging Spectrometer and CERES instruments from the EOS morning crossing mission could provide reliable estimates of the direct radiative forcing of aerosols on a global scale, thereby reducing the uncertainties in current global aerosol radiative forcing values.