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General circulation models' (GCMs) estimates of the liquid water path adjustment to anthropogenic aerosol emissions differ in sign from other lines of evidence. This reduces confidence in estimates of the effective radiative forcing of the climate by aerosol–cloud interactions (ERFaci). The discrepancy is thought to stem in part from GCMs' inability to represent the turbulence–microphysics interactions in cloud-top entrainment, a mechanism that leads to a reduction in liquid water in response to an anthropogenic increase in aerosols. In the real atmosphere, enhanced cloud-top entrainment is thought to be the dominant adjustment mechanism for liquid water path, weakening the overall ERFaci. We show that the latest generation of GCMs includes models that produce a negative correlation between the present-day cloud droplet number and liquid water path, a key piece of observational evidence supporting liquid water path reduction by anthropogenic aerosols and one that earlier-generation GCMs could not reproduce. However, even in GCMs with this negative correlation, the increase in anthropogenic aerosols from preindustrial to present-day values still leads to an increase in the simulated liquid water path due to the parameterized precipitation suppression mechanism. This adds to the evidence that correlations in the present-day climate are not necessarily causal. We investigate sources of confounding to explain the noncausal correlation between liquid water path and droplet number. These results are a reminder that assessments of climate parameters based on multiple lines of evidence must carefully consider the complementary strengths of different lines when the lines disagree.

Brown carbon (BrC) is an absorbing organic aerosol (OA), primarily emitted through biomass burning (BB), which exhibits light absorption unique to both black carbon (BC) and other organic aerosols. Despite many field and laboratory studies seeking to constrain BrC properties, the radiative forcing (RF) of BrC is still highly uncertain. To better understand its climate impact, we introduced BrC to the One-Moment Aerosol (OMA) module of the GISS ModelE Earth system model (ESM). We assessed ModelE sensitivity to primary BrC processed through a novel chemical aging scheme and to secondary BrC formed from biogenic volatile organic compounds (BVOCs). Initial results show that BrC typically contributes a top-of-the-atmosphere (TOA) radiative effect of 0.04 W m−2. Sensitivity tests indicate that explicitly simulating BrC (separating it from other OAs), including secondary BrC, and simulating chemical bleaching of BrC contribute distinguishable radiative effects and should be accounted for in BrC schemes. This addition of prognostic BrC to ModelE allows greater physical and chemical complexity in OA representation with no apparent trade-off in model performance, as the evaluation of ModelE aerosol optical depth against Aerosol Robotic Network (AERONET) and Moderate Resolution Imaging Spectroradiometer (MODIS) retrieval data, with and without the BrC scheme, reveals similar skill in both cases. Thus, BrC should be explicitly simulated to allow more physically based chemical composition, which is crucial for more detailed OA studies like comparisons to in situ measurement campaigns. We include a summary of best practices for BrC representation within ModelE at the end of this paper.

The composition of soil dust aerosols derives from the mineral abundances in the parent soils that vary across dust source regions. Nonetheless, Earth system models (ESMs) have traditionally represented mineral dust as a globally homogeneous species. The growing interest in modeling dust mineralogy, facilitated by the recognized sensitivity of the dust climate impacts to composition, has motivated state-of-the-art ESMs to incorporate the mineral speciation of dust along with its effect upon the dust direct radiative effect (DRE). In this work, we enable the NASA Goddard Institute for Space Studies ModelE2.1 to calculate the shortwave (SW) DRE accounting for the regionally varying soil mineralogy. Mineral–radiation interaction at solar wavelengths is calculated according to two alternative coupling schemes: (1) external mixing of three mineral components that are optically distinguished, one of which contains embedded iron oxides; (2) a single internal mixture of all dust minerals with a dynamic fraction of iron oxides that varies regionally and temporally. We link dust absorption to the fractional mass of iron oxides based on recent chamber measurements using natural dust aerosol samples. We show that coupled mineralogy overall enhances the scattering by dust, and thus the global cooling, compared to our control run with globally uniform composition. According to the external mixing scheme, the SW DRE at the top of atmosphere (TOA) changes from −0.25 to -0.30Wm-2, corresponding to a change in the net DRE, including the longwave effect, from −0.08 to -0.12Wm-2. The cooling increase is accentuated when the internal mixing scheme is configured: the SW DRE at the TOA becomes -0.34Wm-2 with a net DRE of -0.15Wm-2. The varying composition modifies the regional distribution of single scattering albedo (SSA), whose variations in specific regions can be remarkable (above 0.03) and significantly modify the regional SW DRE. Evaluation against the AErosol RObotic NETwork (AERONET) shows that explicit representation of soil mineralogy and its regional variations reduces the low bias of model dust SSA while improving the range of variability across stations and calendar months. Despite these improvements, the moderate spatiotemporal correlation with AERONET reveals remaining modeling challenges and the need for more accurate measurements of mineral fractions in soils.

Drought is a hydroclimatic extreme that causes perturbations to the terrestrial biosphere and acts as a stressor on vegetation, affecting emissions patterns. During severe drought, isoprene emissions are reduced. In this paper, we focus on capturing this reduction signal by implementing a new percentile isoprene drought stress (yd) algorithm in NASA GISS ModelE based on the MEGAN3 (Model of Emissions of Gases and Aerosols from Nature Version 3) approach as a function of a photosynthetic parameter (Vc,max) and water stress (β). Four global transient simulations from 2003–2013 are used to demonstrate the effect without yd (Default_ModelE) and with online yd (DroughtStress_ModelE). DroughtStress_ModelE is evaluated against the observed isoprene measurements at the Missouri Ozarks AmeriFlux (MOFLUX) site during the 2012 severe drought where improvements in the correlation coefficient indicate it is a suitable drought stress parameterization to capture the reduction signal during severe drought. The application of yd globally leads to a decadal average reduction of ∼2.7 %, which is equivalent to ∼14.6 Tg yr−1 of isoprene. The changes have larger impacts in regions such as the southeastern US. DroughtStress_ModelE is validated using the satellite ΩHCHO column from the Ozone Monitoring Instrument (OMI) and surface O3 observations across regions of the US to examine the effect of drought on atmospheric composition. It was found that the inclusion of isoprene drought stress reduced the overestimation of ΩHCHO in Default_ModelE during the 2007 and 2011 southeastern US droughts and led to improvements in simulated O3 during drought periods. We conclude that isoprene drought stress should be tuned on a model-by-model basis because the variables used in the parameterization responses are relative to the land surface model hydrology scheme (LSM) and the effects of yd application could be larger than seen here due to ModelE not having large biases of isoprene during severe drought.

Global models are widely used to simulate biomass burning aerosol (BBA). Exhaustive evaluations on model representation of aerosol distributions and properties are fundamental to assess health and climate impacts of BBA. Here we conducted a comprehensive comparison of Aerosol Comparisons between Observations and Models (AeroCom) project model simulations with satellite observations. A total of 59 runs by 18 models from three AeroCom Phase-III experiments (i.e., biomass burning emissions, CTRL16, and CTRL19) and 14 satellite products of aerosols were used in the study. Aerosol optical depth (AOD) at 550 nm was investigated during the fire season over three key fire regions reflecting different fire dynamics (i.e., deforestation-dominated Amazon, Southern Hemisphere Africa where savannas are the key source of emissions, and boreal forest burning in boreal North America). The 14 satellite products were first evaluated against AErosol RObotic NETwork (AERONET) observations, with large uncertainties found. But these uncertainties had small impacts on the model evaluation that was dominated by modeling bias. Through a comparison with Polarization and Directionality of the Earth’s Reflectances measurements with the Generalized Retrieval of Aerosol and Surface Properties algorithm (POLDER-GRASP), we found that the modeled AOD values were biased by −93 % to 152 %, with most models showing significant underestimations even for the state-of-the-art aerosol modeling techniques (i.e., CTRL19). By scaling up BBA emissions, the negative biases in modeled AOD were significantly mitigated, although it yielded only negligible improvements in the correlation between models and observations, and the spatial and temporal variations in AOD biases did not change much. For models in CTRL16 and CTRL19, the large diversity in modeled AOD was in almost equal measures caused by diversity in emissions, lifetime, and the mass extinction coefficient (MEC). We found that in the AeroCom ensemble, BBA lifetime correlated significantly with particle deposition (as expected) and in turn correlated strongly with precipitation. Additional analysis based on Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) aerosol profiles suggested that the altitude of the aerosol layer in the current models was generally too low, which also contributed to the bias in modeled lifetime. Modeled MECs exhibited significant correlations with the Ångström exponent (AE, an indicator of particle size). Comparisons with the POLDER-GRASP-observed AE suggested that the models tended to overestimate the AE (underestimated particle size), indicating a possible underestimation of MECs in models. The hygroscopic growth in most models generally agreed with observations and might not explain the overall underestimation of modeled AOD. Our results imply that current global models contain biases in important aerosol processes for BBA (e.g., emissions, removal, and optical properties) that remain to be addressed in future research.

Simulations by six Coupled Model Intercomparison Project Phase 6 (CMIP6) Earth system models indicate that the seasonal cycle of baseline tropospheric ozone at northern midlatitudes has been shifting since the mid-20th century. Beginning in ∼ 1940, the magnitude of the seasonal cycle increased by ∼10 ppb (measured from seasonal minimum to maximum), and the seasonal maximum shifted to later in the year by about 3 weeks. This shift maximized in the mid-1980s, followed by a reversal – the seasonal cycle decreased in amplitude and the maximum shifted back to earlier in the year. Similar changes are seen in measurements collected from the 1970s to the present. The timing of the seasonal cycle changes is generally concurrent with the rise and fall of anthropogenic emissions that followed industrialization and the subsequent implementation of air quality emission controls. A quantitative comparison of the temporal changes in the ozone seasonal cycle at sites in both Europe and North America with the temporal changes in ozone precursor emissions across the northern midlatitudes found a high degree of similarity between these two temporal patterns. We hypothesize that changing precursor emissions are responsible for the shift in the ozone seasonal cycle; this is supported by the absence of such seasonal shifts in southern midlatitudes where anthropogenic emissions are much smaller. We also suggest a mechanism by which changing emissions drive the changing seasonal cycle: increasing emissions of NOx allow summertime photochemical production of ozone to become more important than ozone transported from the stratosphere, and increasing volatile organic compounds (VOCs) lead to progressively greater photochemical ozone production in the summer months, thereby increasing the amplitude of the seasonal ozone cycle. Decreasing emissions of both precursor classes then reverse these changes. The quantitative parameter values that characterize the seasonal shifts provide useful benchmarks for evaluating model simulations, both against observations and between models.

We examined daily level-3 satellite retrievals of Atmospheric Infrared Sounder (AIRS) CO, Ozone Monitoring Instrument (OMI) SO2 and NO2, and Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth (AOD) over eastern China to understand how COVID-19 lockdowns affected atmospheric composition. Changes in 2020 were strongly dependent on the choice of background period since 2005 and whether trends in atmospheric composition were accounted for. Over central east China during the 23 January–8 April lockdown window, CO in 2020 was between 3 % and 12 % lower than average depending on the background period. The 2020 CO was not consistently less than expected from trends beginning between 2005 and 2016 and ending in 2019 but was 3 %–4 % lower than the background mean during the 2017–2019 period when CO changes had flattened. Similarly for AOD, 2020 was between 14 % and 30 % lower than averages beginning in 2005 and 14 %–17 % lower compared to different background means beginning in 2016. NO2 in 2020 was between 30 % and 43 % lower than the mean over different background periods and between 17 % and 33 % lower than what would be expected for trends beginning later than 2011. Relative to the 2016–2019 period when NO2 had flattened, 2020 was 30 %–33 % lower. Over southern China, 2020 NO2 was between 23 % and 27 % lower than different background means beginning in 2013, the beginning of a period of persistently lower NO2. CO over southern China was significantly higher in 2020 than what would be expected, which we suggest was partly because of an active fire season in neighboring countries. Over central east and southern China, 2020 SO2 was higher than expected, but this depended strongly on how daily regional values were calculated from individual retrievals and reflects background values approaching the retrieval detection limit. Future work over China, or other regions, needs to take into account the sensitivity of differences in 2020 to different background periods and trends in order to separate the effects of COVID-19 on air quality from previously occurring changes or from variability in other sources.

Atmospheric ammonia (NH3) is a precursor to fine particulate matter and a source of nitrogen (N) deposition that can adversely affect ecosystem health. The main sources of NH3 – agriculture and biomass burning – are undergoing are or expected to undergo substantial changes in Africa. Although evidence of increasing NH3 over parts of Africa has been observed, the mechanisms behind these trends are not well understood. Here we use observations of atmospheric NH3 vertical column densities (VCDs) from the Infrared Atmospheric Sounding Interferometer (IASI) along with other satellite observations of the land surface and atmosphere to evaluate how NH3 concentrations have changed over Africa from 2008 through 2018, and what has caused those changes. In West Africa NH3 VCDs are observed to increase during the late dry season, with increases of over 6 % yr−1 in Nigeria during February and March (p<0.01). These positive trends are associated with increasing burned area and CO trends during these months, likely related to agricultural preparation. Increases are also observed in the Lake Victoria basin region, where they are associated with expanding agricultural area. In contrast, NH3 VCDs declined over the Sudd wetlands in South Sudan by over 1.5 % yr−1, though not significantly (p=0.28). Annual maxima in NH3 VCDs in South Sudan occur during February through May and are associated with the drying of temporarily flooded wetland soils, which favor emissions of NH3. The change in mean NH3 VCDs over the Sudd is strongly correlated with variation in wetland extent in the Sudd: in years when more area remained flooded during the dry season, NH3 VCDs were lower (r=0.64, p<0.05). Relationships between biomass burning and NH3 may be observed when evaluating national-scale statistics: countries with the highest rates of increasing NH3 VCDs also had high rates of growth in CO VCDs; burned area displayed a similar pattern, though not significantly. Livestock numbers were also higher in countries with intermediate or high rates of NH3 VCD growth. Fertilizer use in Africa is currently low but growing; implementing practices that can limit NH3 losses from fertilizer as agriculture is intensified may help mitigate impacts on health and ecosystems.