Instantaneous Radiative Forcing Research Articles

The ozone radiative forcing of nitrogen oxide emissions from aviation can be estimated using a probabilistic approach

Reliable prediction of aviation’s environmental impact, including the effect of nitrogen oxides on ozone, is vital for effective mitigation against its contribution to global warming. Estimating this climate impact however, in terms of the short-term ozone instantaneous radiative forcing, requires computationally-expensive chemistry-climate model simulations that limit practical applications such as climate-optimised planning. Existing surrogates neglect the large uncertainties in their predictions due to unknown environmental conditions and missing features. Relative to these surrogates, we propose a high-accuracy probabilistic surrogate that not only provides mean predictions but also quantifies heteroscedastic uncertainties in climate impact estimates. Our model is trained on one of the most comprehensive chemistry-climate model datasets for aviation-induced nitrogen oxide impacts on ozone. Leveraging feature selection techniques, we identify essential predictors that are readily available from weather forecasts to facilitate the implementation therein. We show that our surrogate model is more accurate than homoscedastic models and easily outperforms existing linear surrogates. We then predict the climate impact of a frequently-flown flight in the European Union, and discuss limitations of our approach.

Adjustments to Climate Perturbations—Mechanisms, Implications, Observational Constraints

AbstractSince the 5th Assessment Report of the Intergovernmental Panel on Climate Change (AR5) an extended concept of the energetic analysis of climate change including forcings, feedbacks and adjustment processes has become widely adopted. Adjustments are defined as processes that occur in response to the introduction of a climate forcing agent, but that are independent of global‐mean surface temperature changes. Most considered are the adjustments that impact the Earth energy budget and strengthen or weaken the instantaneous radiative forcing due to the forcing agent. Some adjustment mechanisms also impact other aspects of climate not related to the Earth radiation budget. Since AR5 and a following description by Sherwood et al. (2015, https://doi.org/10.1175/bams‐d‐13‐00167.1), much research on adjustments has been performed and is reviewed here. We classify the adjustment mechanisms into six main categories, and discuss methods of quantifying these adjustments in terms of their potentials, shortcomings and practicality. We furthermore describe aspects of adjustments that act beyond the energetic framework, and we propose new ideas to observe adjustments or to make use of observations to constrain their representation in models. Altogether, the problem of adjustments is now on a robust scientific footing, and better quantification and observational constraint is possible. This allows for improvements in understanding and quantifying climate change.

Compensating atmospheric adjustments reduce the volcanic forcing from Hunga stratospheric water vapor enhancement.

The 2022 eruption of the Hunga submarine volcano injected an unprecedented volume of water vapor into the stratosphere, presenting a unique, natural experiment for ascertaining the influence of stratospheric water vapor within the global radiation budget. This study examines the radiative forcings of the Hunga stratospheric water vapor enhancement, comparing stratosphere-adjusted radiative forcing derived from offline methods to an effective radiative forcing derived from Earth System Model simulations. Assuming a uniform 2 parts per million mass mixing ratio increase of water vapor in the Southern Hemisphere stratosphere, we estimated the instantaneous, stratosphere-adjusted, and overall effective radiative forcing to be -0.04, 0.08, and 0.05 W m-2, respectively. The lower magnitude of the positive volcanic stratospheric water vapor effective radiative forcing is due to compensating effects from atmospheric adjustments. Ensemble simulations of a coupled atmosphere-ocean model suggest a surface warming of 0.05 K, affirming a limited influence on global mean surface temperature from the volcanic stratospheric water vapor injection.

Updating the radiation infrastructure in MESSy (based on MESSy version 2.55)

Abstract. The calculation of the radiative transfer is a key component of global circulation models. In this article, we describe the most recent updates of the radiation infrastructure in the Modular Earth Submodel System (MESSy). These updates include the implementation of the PSrad radiation scheme within the RAD submodel. Furthermore, the radiation-related submodels CLOUDOPT (for the calculation of cloud optical properties) and AEROPT (for the calculation of aerosol optical properties) have been updated and are now more flexible in order to deal with different sets of shortwave and longwave bands of radiation schemes. In the wake of these updates, a new submodel (ALBEDO), which features solar-zenith-angle-dependent albedos and a new satellite-based background (white sky) albedo, was created. All of these developments are backward compatible, and previous features of the MESSy radiation infrastructure remain available. Moreover, these developments mark an important step in the use of the ECHAM/MESSy Atmospheric Chemistry (EMAC) model, as the update of the radiation scheme was a key aspect in the development of the sixth generation of the European Centre for Medium-Range Weather Forecasts – HAMburg (ECHAM6) model from ECHAM5. The developments presented here are also aimed towards using the MESSy infrastructure with the ICOsahedral Non-hydrostatic (ICON) model as a base model. The improved infrastructure will also aid in the implementation of additional radiation schemes once this should be needed. We have optimized the set of free parameters for two general circulation model-type (GCM-type) setups for pre-industrial and present-day conditions: one with the radiation scheme that was used to date (i.e. the radiation scheme of ECHAM5) and one with the newly implemented PSrad radiation scheme. After this parameter optimization, we performed four model simulations and evaluated the corresponding model results using reanalysis and observational data. The most apparent improvements related to the updated radiation scheme are the reduced cold biases in the tropical upper troposphere and lower stratosphere and the extratropical lower stratosphere and a strengthened polar vortex. The former is also related to improved stratospheric humidity and its variability if the new radiation scheme is employed. Using the multiple radiation call capability of MESSy, we have applied the two model configurations to calculate instantaneous and stratospheric-adjusted radiative forcings related to changes in greenhouse gases. Overall, we find that for many forcing experiments the simulations with the new radiation scheme show improved radiative forcing values. This is in particular the case for methane radiative forcings, which are considerably higher when assessed with the new radiation scheme and thus in better agreement with reference values.

Changes in the Direct Climate Effect of Black Carbon Aerosols in East Asia Under the “Dual Carbon” Goal of China

AbstractIn the context of China's “dual carbon” goal, emissions of air pollutants are expected to significantly decrease in the future. Thus, the direct climate effects of black carbon (BC) aerosols in East Asia are investigated under this goal using an updated regional climate and chemistry model. The simulated annual average BC concentration over East Asia is approximately 1.29 μg/m3 in the last decade. Compared to those in 2010–2020, both the BC column burden and instantaneous direct radiative forcing in East Asia decrease by more than 55% and 80%, respectively, in the carbon peak year (2030s) and the carbon neutrality year (2060s). Conversely, the BC effective radiative forcing (ERF) and regional climate responses to BC exhibit substantial nonlinearity to emission reduction, possibly resulting from different adjustments of thermal‐dynamic fields and clouds from BC‐radiation interactions. The regional mean BC ERF at the tropopause over East Asia is approximately +1.11 W/m2 in 2010–2020 while negative in the 2060s. BC‐radiation interactions in the present‐day impose a significant annual mean cooling of −0.2 to −0.5 K in central China but warming +0.3 K in the Tibetan Plateau. As China's BC emissions decline, surface temperature responses show a mixed picture compared to 2010–2020, with more cooling in eastern China and Tibet of −0.2 to −0.3 K in the 2030s, but more warming in central China of approximately +0.3 K by the 2060s. The Indian BC might play a more important role in East Asian climate with reduction of BC emissions in China.

Sponge iron-coupled biochar solution can achieve the synergistic augmentation of carbon sequestration, carbon sink capacity, and denitrification in ecological ditches

Carbon dioxide (CO2) is a more powerful greenhouse gas due to its enhanced instantaneous radiative forcing. Since agricultural ecological ditches (eco-ditches) controlling agricultural non-point source pollution are potential CO2 hotspots, carbon capture technologies must be deployed immediately to sequester carbon and combat climate change. Zero-waste biochar, a negative-carbon technology, remains contentious regarding C sequestration. Iron (Fe) enhances long-term organic carbon (OC) preservation, but the cascading effects of Fe-biochar interactions on the promotion of C accumulation are unclear in eco-ditches. In this paper, we fill these research gaps and employ sponge iron (s-ZVI) and biochar coupling (Fe-C) to enhance the iron gate C protection in eco-ditches. The results reveal that Myriophyllum aquaticum(M.A.)-derived biochar prepared by low-temperature pyrolysis (Biochar_M.A.) enjoys the highest FI, the lowest SUVA254 and SUVA280 and moderate dissolution stability. The coupling of s-ZVI and environmentally compatible Biochar_M.A. achieve a triple benefit situation of C sequestration, C sink, and pollutant removal. Overall carbon gain is jointly determined by abiotic controls and biotic controls. The carbon burial effects of biochar-amended eco-ditches are mainly controlled by the trade-offs between Fe-bound OC mineralization via the biochar-induced prime effect and preservation of OC derived from microbial biomass. The unique Fe-C boosts the rusty sink and yields a negative priming as a result of the dominance of Fe-OC. The upregulated β-glucosidase activity and new-formed Fe-OC indirectly and directly contribute to overall C gain in Fe-C-filled eco-ditches, respectively. These findings provide novel insights into the coupled biotic-abiotic contribution mechanisms underlying the iron gate and reverse enzyme latch phenomenon and advance more robust and prospective theoretical knowledge of C dynamics that are not restricted to eco-ditches, soil, constructed wetlands C storage.

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.

Impacts of a double-moment bulk cloud microphysics scheme (NDW6-G23) on aerosol fields in NICAM.19 with a global 14 km grid resolution

Abstract. In accordance with progression in current capabilities towards high-resolution approaches, applying a convective-permitting resolution to global aerosol models helps comprehend how complex cloud–precipitation systems interact with aerosols. This study investigates the impacts of a double-moment bulk cloud microphysics scheme, i.e., NICAM Double-moment bulk Water 6 developed in this study (NDW6-G23), on the spatiotemporal distribution of aerosols in the Nonhydrostatic ICosahedral Atmospheric Model as part of the version-19 series (NICAM.19) with 14 km grid spacing. The mass concentrations and optical thickness of the NICAM-simulated aerosols are generally comparable to those obtained from in situ measurements. However, for some aerosol species, especially dust and sulfate, the differences between experiments of NDW6 and of the NICAM single-moment bulk module with six water categories (NSW6) were larger than those between experiments with different horizontal resolutions (14 and 56 km grid spacing), as shown in a previous study. The simulated aerosol burdens using NDW6 are generally lower than those using NSW6; the net instantaneous radiative forcing due to aerosol–radiation interaction (IRFari) is estimated to be −1.36 W m−2 (NDW6) and −1.62 W m−2 (NSW6) in the global annual mean values at the top of the atmosphere (TOA). The net effective radiative forcing due to anthropogenic aerosol–radiation interaction (ERFari) is estimated to be −0.19 W m−2 (NDW6) and −0.23 W m−2 (NSW6) in the global annual mean values at the TOA. This difference among the experiments using different cloud microphysics modules, i.e., 0.26 W m−2 or 16 % difference in IRFari values and 0.04 W m−2 or 16 % difference in ERFari values, is attributed to a different ratio of column precipitation to the sum of the column precipitation and column liquid cloud water, which strongly determines the magnitude of wet deposition in the simulated aerosols. Since the simulated ratios in the NDW6 experiment are larger than those of the NSW6 result, the scavenging effect of the simulated aerosols in the NDW6 experiment is larger than that in the NSW6 experiment. A large difference between the experiments is also found in the aerosol indirect effect (AIE), i.e., the net effective radiative forcing due to aerosol–cloud interaction (ERFaci) from the present to preindustrial days, which is estimated to be −1.28 W m−2 (NDW6) and −0.73 W m−2 (NSW6) in global annual mean values. The magnitude of the ERFaci value in the NDW6 experiment is larger than that in the NSW6 result due to the differences in both the Twomey effect and the susceptibility of the simulated cloud water to the simulated aerosols between NDW6 and NSW6. Therefore, this study shows the importance of the impacts of the cloud microphysics module on aerosol distributions through both aerosol wet deposition and the AIE.

Quantifying the Role of Model Internal Year-to-Year Variability in Estimating Anthropogenic Aerosol Radiative Effects

The model internal year-to-year variability (hereafter, internal variability) is a significant source of uncertainty when estimating anthropogenic aerosol effective radiative forcing (ERF). In this study, we investigate the impact of internal variability using large ensemble simulations (600 years in total) with the same climate model under prescribed anthropogenic aerosol forcings. A comparison of the magnitudes (i.e., standard deviation, Std) of these influences confirms that internal variability has negligible impacts on the instantaneous radiative forcing (RF) diagnosed by double radiation calls but has considerable impacts on estimating ERF through rapid adjustments (ADJ). Approximately half of the model grids exhibit a strong internal variability influence on ERF (Std > 5 W m−2). These strong internal variabilities lead to a 50% probability that the 30-year linear change can reach 2 W m−2 and the 10-year linear change can reach 4 W m−2. A 50-year simulation can provide a relatively stable annual mean map of ERF (ERF = ADJ + RF), but it fails for ADJ. The statistically significant areas in the annual mean maps of both ERF and ADJ from a 10-year simulation exhibit instability with evident chaotic features. The insights derived from our analysis aid in assessing the stability of modeled ERF and contribute to the design of comparative experiments.

Combined effect of algae and dust on snow spectral and broadband albedo

The optical properties of snow can be strongly modified by the presence of a variety of impurities including mineral dust and snow algae. We made use of measured concentration of snow algae and mineral dust to parameterize the BioSNICAR radiative transfer model. Surficial snow samples were gathered during a field campaign on 7th July 2020 at the Presena glacier (Rhaetian Alps). We collected 18 samples of surface snow containing different amount of snow algae and mineral dust. Through radiative transfer simulations we estimated an average broadband albedo reduction of 7.4 ± 6.1 % and 35.3 ± 7.4 % compared to clean snow, caused by snow algae and mineral dust presence, respectively. When we considered the combined effect of snow algae and dust, we estimated a broadband albedo reduction equal to 40.8 ± 8.4 %. We estimated an average instantaneous radiative forcing induced by snow algae, mineral dust and both impurities equals to 42.3 (± 36.1) W/m2, 203.7 (±45.5) W/m2, and 211.8 (±45.9) W/m2, respectively.Using BioSNICAR simulations, we also tested a series of narrowband spectral indices to determine the concentration of mineral dust and snow algae from multi- and hyper-spectral data. Results showed that most spectral indices used for snow algae mapping are correlated also with mineral dust concentration. We found that only an index correlates uniquely with snow algae: the scaled band integral at 680 nm. A new spectral index, namely the Green Blue Normalized Index, is therefore proposed to discriminate mineral dust from snow algae when both impurities are present. The high spectral resolution of current (e.g. PRISMA, EnMAP) and future (e.g. CHIME, SBG) hyperspectral satellite missions will be fundamental to decouple the effect of mineral dust and snow algae on the optical properties of snow. In fact, from those data it is possible to calculate all narrowband indices presented in this study.

Greenhouse Gas Forcing and Climate Feedback Signatures Identified in Hyperspectral Infrared Satellite Observations

AbstractGlobal greenhouse gas forcing and feedbacks are the primary causes of climate change but have limited direct observations. Here we show that continuous, stable, global, hyperspectral infrared satellite measurements (2003–2021) display decreases in outgoing longwave radiation (OLR) in the CO2, CH4, and N2O absorption bands and increases in OLR in the window band and H2O absorption bands. By conducting global line‐by‐line radiative transfer simulations with 2003–2021 meteorological conditions, we show that increases in CO2, CH4, and N2O concentrations caused an instantaneous radiative forcing and stratospheric cooling adjustment that decreased OLR. The climate response, comprising surface and atmospheric feedbacks to radiative forcings and unforced variability, increased OLR. The spectral trends predicted by our climate change experiments using our general circulation model identify three bedrock principles of the physics of climate change in the satellite record: an increasing greenhouse effect, stratospheric cooling, and surface‐tropospheric warming.

How the extreme 2019–2020 Australian wildfires affected global circulation and adjustments

Abstract. Wildfires are a significant source of absorbing aerosols in the atmosphere. Extreme fires in particular, such as those during the 2019–2020 Australian wildfire season (Black Summer fires), can have considerable large-scale effects. In this context, the climate impact of extreme wildfires unfolds not only because of the emitted carbon dioxide but also due to smoke aerosol released up to an altitude of 17 km. The overall aerosol effects depend on a variety of factors, such as the amount emitted, the injection height, and the composition of the burned material, and is therefore subject to considerable uncertainty. In the present study, we address the global impact caused by the exceptionally strong and high-reaching smoke emissions from the Australian wildfires using simulations with a global aerosol–climate model. We show that the absorption of solar radiation by the black carbon contained in the emitted smoke led to a shortwave radiative forcing of more than +5 W m−2 in the southern mid-latitudes of the lower stratosphere. Subsequent adjustment processes in the stratosphere slowed down the diabatically driven meridional circulation, thus redistributing the heating perturbation on a global scale. As a result of these stratospheric adjustments, a positive temperature perturbation developed in both hemispheres, leading to additional longwave radiation emitted back to space. According to the model results, this adjustment occurred in the stratosphere within the first 2 months after the event. At the top of the atmosphere (TOA), the net effective radiative forcing (ERF) averaged over the Southern Hemisphere was initially dominated by the instantaneous positive radiative forcing of about +0.5 W m−2, for which the positive sign resulted mainly from the presence of clouds above the Southern Ocean. The longwave adjustments led to a compensation of the initially net positive TOA ERF, which is seen in the Southern Hemisphere, the tropics, and the northern mid-latitudes. The simulated changes in the lower stratosphere also affected the upper troposphere through a thermodynamic downward coupling. Subsequently, increased temperatures were also obtained in the upper troposphere, causing a global decrease in relative humidity, cirrus amount, and the ice water path of about 0.2 %. As a result, surface precipitation also decreased by a similar amount, which was accompanied by a weakening of the tropospheric circulation due to the given energetic constraints. In general, it appears that the radiative effects of smoke from single extreme wildfire events can lead to global impacts that affect the interplay of tropospheric and stratospheric budgets in complex ways. This emphasizes that future changes in extreme wildfires need to be included in projections of aerosol radiative forcing.

An emerging Asian aerosol dipole pattern reshapes the Asian summer monsoon and exacerbates northern hemisphere warming

Since the early 2010s, anthropogenic aerosols have started decreasing in East Asia (EA) while have continued to increase in South Asia (SA). Yet the climate impacts of this Asian aerosol dipole (AAD) pattern remain largely unknown. Using a state-of-the-art climate model, we demonstrate that the climate response is distinctly different between the SA aerosol increases and EA aerosol decreases. The SA aerosol increases lead to ~2.7 times stronger land summer precipitation change within the forced regions than the EA aerosol decreases. Contrastingly, the SA aerosol increases, within the tropical monsoon regime, produce weak and tropically confined responses, while the EA aerosol decreases yield a pronounced northern hemisphere warming aided by extratropical mean westerly and positive air-sea feedbacks over the western North Pacific. By scaling the observed instantaneous shortwave radiative forcing, we reveal that the recent AAD induces a pronounced northern hemisphere extratropical (beyond 30°N) warming (0.024 ± 0.010 °C decade−1), particularly over Europe (0.049 ± 0.009 °C decade−1). These findings highlight the importance of the pattern effect of forcings in driving global climate and have important implications for decadal prediction.

Albedo change from snow algae blooms can contribute substantially to snow melt in the North Cascades, USA

Snow algae are ubiquitous in the Pacific Northwest cryosphere in the summer where snowmelt is an important contribution to regional watersheds. However, less attention has been given to biological impurities as drivers of snowmelt compared to inorganic light-absorbing particles. Here we map snow algae near Mt. Baker with a multispectral camera on an uncrewed aerial vehicle using (1) principal components and (2) spectral indexing. The two approaches are tested under differing bloom states and verified with coincident algal pigment and cell count data. During high bloom intensity we found an average instantaneous radiative forcing of 237 W m−2 with a maximum of 360 W m−2. This translated to 1,508 ± 536 m3 of melted snow water equivalent in the 0.1 km2 basin. These results demonstrate snow algae contribute to snowmelt at mid-latitudes and the potential for uncrewed autonomous vehicles to map snow algae over expansive areas of the cryosphere.

Observations of microphysical properties and radiative effects of a contrail cirrus outbreak over the North Atlantic

Abstract. Contrail cirrus constitute the largest radiative forcing (RF) component to the total aviation effect on climate. However, the microphysical properties and radiative effects of contrail cirrus and natural cirrus clouds in the same meteorological conditions are still not completely resolved. Motivated by these uncertainties, we investigate an extended cirrus region perturbed by aviation in the North Atlantic region (NAR) on 26 March 2014 during the Midlatitude Cirrus (ML-CIRRUS) experiment. On that day, high air traffic density in the NAR combined with large scale cold and humid ambient conditions favored the formation of a contrail cirrus outbreak situation. In addition, low coverage by low-level water clouds and the homogeneous oceanic albedo increased the sensitivity for retrieving cirrus properties and their radiative effect from satellite remote sensing. This allowed us to extend the current knowledge on contrail cirrus by combining airborne in situ, lidar and satellite observations. In the synoptic context of a ridge cirrus, an extended thin ice cloud with many persistent contrails and contrail cirrus has been observed for many hours with the geostationary Meteosat Second Generation (MSG)/Spinning Enhanced Visible and InfraRed Imager (SEVIRI) from the early morning hours until dissipation after noon. Airborne lidar observations aboard the German High Altitude and LOng Range Research Aircraft (HALO) suggest that this cirrus has a significant anthropogenic contribution from aviation. A new method based on in situ measurements was used to distinguish between contrails, contrail cirrus and natural cirrus based on ice number and gas phase NO concentrations. Results show that contrail effective radii (Reff) reach at most 11 µm, while contrail cirrus Reff can be as large as 51 µm. Contrail and contrail cirrus mean Reff is 18 % smaller than that of natural cirrus. We find that a difference in Reff between contrail cirrus and natural cirrus survives in this contrail cirrus outbreak event. As for radiative effects, a new method to estimate top-of-atmosphere instantaneous RF in the solar and thermal range is developed based on radiative transfer model simulations exploiting in situ and lidar measurements, satellite observations and ERA5 reanalysis data for both cirrus and cirrus-free regions. Broadband irradiances estimated from our simulations compare well with satellite observations from MSG, indicating that our method provides a good representation of the real atmosphere and can thus be used to determine the RF of ice clouds. For a larger spatial area around the flight path, we find that the contrail cirrus outbreak is warming in the early morning and cooling during the day. The methods presented here and the results will be valuable for future research to constrain uncertainties in the assessment of radiative impacts of contrail cirrus and natural cirrus and for the formulation and evaluation of contrail mitigation options.

Reconstructing volcanic radiative forcing since 1990, using a comprehensive emission inventory and spatially resolved sulfur injections from satellite data in a chemistry-climate model

Abstract. This paper presents model simulations of stratospheric aerosols with a focus on explosive volcanic eruptions. Using various (occultation and limb-based) satellite instruments, providing vertical profiles of sulfur dioxide (SO2) and aerosol extinction, we characterized the chemical and radiative influence of volcanic aerosols for the period between 1990 and 2019. We established an improved and extended volcanic SO2 emission inventory that includes more than 500 explosive volcanic eruptions reaching the upper troposphere and the stratosphere. Each perturbation identified was derived from the satellite data and incorporated as a three-dimensional SO2 plume into a chemistry-climate model without the need for additional assumptions about altitude distribution and eruption duration as needed for a “point source” approach. The simultaneous measurements of SO2 and aerosol extinction by up to four satellite instruments enabled a reliable conversion of extinction measurements into injected SO2. In the chemistry-climate model, the SO2 from each individual plume was converted into aerosol particles and their optical properties were determined. Furthermore, the aerosol optical depth (AOD) and the instantaneous radiative forcing on climate were calculated online. Combined with model improvements, the results of the simulations are consistent with the observations of the various satellites. Slight deviations between the observations and model simulations were found for the large volcanic eruption of Pinatubo in 1991 and cases where simultaneous satellite observations were not unique or too sparse. Weak- and medium-strength volcanic eruptions captured in satellite data and the Smithsonian database typically inject about 10 to 50 kt SO2 directly into the upper troposphere/lower stratosphere (UTLS) region or the sulfur species are transported via convection and advection. Our results confirm that these relatively minor eruptions, which occur quite frequently, can nevertheless contribute to the stratospheric aerosol layer and are relevant for the Earth's radiation budget. These minor eruptions cause a total global instantaneous radiative forcing of the order of −0.1 W m−2 at the top of the atmosphere (TOA) compared to a background stratospheric aerosol forcing of about −0.04 W m−2. Medium-strength eruptions injecting about 400 kt SO2 into the stratosphere or accumulation of consecutive smaller eruptions can lead to a total instantaneous forcing of about −0.3 W m−2. We show that it is critical to include the contribution of the extratropical lowermost stratospheric aerosol in the forcing calculations.

Multi-angular polarimetric remote sensing to pinpoint global aerosol absorption and direct radiative forcing

Quantitative estimations of atmospheric aerosol absorption are rather uncertain due to the lack of reliable information about the global distribution. Because the information about aerosol properties is commonly provided by single-viewing photometric satellite sensors that are not sensitive to aerosol absorption. Consequently, the uncertainty in aerosol radiative forcing remains one of the largest in the Assessment Reports of the Intergovernmental Panel on Climate Change (IPCC AR5 and AR6). Here, we use multi-angular polarimeters (MAP) to provide constraints on emission of absorbing aerosol species and estimate global aerosol absorption optical depth (AAOD) and its climate effect. Our estimate of modern-era mid-visible AAOD is 0.0070 that is higher than IPCC by a factor of 1.3-1.8. The black carbon instantaneous direct radiative forcing (BC DRF) is +0.33 W/m2 [+0.17, +0.54]. The MAP constraint narrows the 95% confidence interval of BC DRF by a factor of 2 and boosts confidence in its spatial distribution.

Radiative impact of improved global parameterisations of oceanic dry deposition of ozone and lightning-generated NOx

Abstract. We investigated the radiative impact of recent process-based improvements to oceanic ozone (O3) dry deposition parameterisation and empirical improvements to lightning-generated oxides of nitrogen (LNOx) parameterisation by conducting a 5-year simulation of the Australian Community Climate and Earth System Simulator – United Kingdom Chemistry and Aerosol (ACCESS-UKCA) global chemistry–climate model, with radiative effects of O3, methane (CH4) and aerosol included. Compared to the base parameterisations, the global consequences of the two improved parameterisations on atmospheric composition are dominated by the LNOx change (which increases the LNOx production from 4.8 to 6.9 Tg N yr−1) and include (a) an increase in the O3 column of 3.75 DU, and this O3 change is centred on the tropical upper troposphere where O3 is most effective as a radiative forcer; (b) a decrease of 0.64 years in the atmospheric lifetime of CH4 due to an increase in hydroxyl radical, which corresponds to a decrease of 0.31 years in the CH4 lifetime per Tg N yr−1 change in LNOx; (c) an increase of 6.7 % in the column integrated condensation nuclei concentration; and (d) a slight increase in high-level cloud cover. The two combined parameterisation changes cause an increase of 86.3 mW m−2 in the globally-averaged all-sky net downward top-of-atmosphere (TOA) radiative flux (which is akin to instantaneous radiative forcing), and only 5 % of which is due to the dry deposition parameterisation change. Other global radiative changes from the use of the two parameterisations together include an increase in the downward longwave radiation and a decrease in the downward shortwave radiation at the earth's surface. The indirect effect of LNOx on aerosol and cloud cover can at least partly explain the differences in the downward shortwave flux at the surface. It is demonstrated that although the total global LNOx production may be the same, how LNOx is distributed spatially makes a difference to radiative transfer. We estimate that for a reported uncertainty range of 5±3 Tg N yr−1 in global estimates of LNOx, the uncertainty in the net downward TOA radiation is ±119 mW m−2. The corresponding uncertainly in the atmospheric methane lifetime is ±0.92 years. Thus, the value of LNOx used within a model will influence the effective radiative forcing (ERF) and global warming potential (GWP) of anthropogenic CH4, and influence the results of climate scenario modelling.

Methane's Solar Radiative Forcing

AbstractMethane (CH4) has significant absorption bands at wavelengths of 1.7, 2.3, 3.3 and 7.6 μm which absorb incoming solar ‘shortwave’ (SW) radiation and contribute to radiative forcing (RF). A comprehensive quantification of CH4 SW RF is presented using a narrow‐band radiative transfer model to calculate spatially and monthly resolved estimates of CH4 SW RF and its impact on longwave (LW) stratospheric temperature adjusted RF (SARF). These new calculations include satellite measurements of CH4 distribution and spectrally varying surface albedo, and include absorption of solar mid‐infrared radiation by methane's 7.6 μm band. These factors substantially influence methane's SW effect. For a 750–1,800 ppb perturbation, the all‐sky top‐of‐atmosphere SW instantaneous RF is 0.082 W m−2; at the tropopause it is 0.002 W m−2, considerably smaller than previous estimates. Including the impact of SW absorption on stratospheric temperature increases tropopause SARF by 0.039 W m−2 (or 7%) compared to the LW‐only SARF.

Important role of stratospheric injection height for the distribution and radiative forcing of smoke aerosol from the 2019–2020 Australian wildfires

Abstract. More than 1 Tg smoke aerosol was emitted into the atmosphere by the exceptional 2019–2020 southeastern Australian wildfires. Triggered by the extreme fire heat, several deep pyroconvective events carried the smoke directly into the stratosphere. Once there, smoke aerosol remained airborne considerably longer than in lower atmospheric layers. The thick plumes traveled eastward, thereby being distributed across the high and mid-latitudes in the Southern Hemisphere, enhancing the atmospheric opacity. Due to the increased atmospheric lifetime of the smoke plume, its radiative effect increased compared to smoke that remains in lower altitudes. Global models describing aerosol-climate impacts lack adequate descriptions of the emission height of aerosols from intense wildfires. Here, we demonstrate, by a combination of aerosol-climate modeling and lidar observations, the importance of the representation of those high-altitude fire smoke layers for estimating the atmospheric energy budget. Through observation-based input into the simulations, the Australian wildfire emissions by pyroconvection are explicitly prescribed to the lower stratosphere in different scenarios. Based on our simulations, the 2019–2020 Australian fires caused a significant top-of-atmosphere (TOA) hemispheric instantaneous direct radiative forcing signal that reached a magnitude comparable to the radiative forcing induced by anthropogenic absorbing aerosol. Up to +0.50 W m−2 instantaneous direct radiative forcing was modeled at TOA, averaged for the Southern Hemisphere (+0.25 W m−2 globally) from January to March 2020 under all-sky conditions. At the surface, on the other hand, an instantaneous solar radiative forcing of up to −0.81 W m−2 was found for clear-sky conditions, with the respective estimates depending on the model configuration and subject to the model uncertainties in the smoke optical properties. Since extreme wildfires are expected to occur more frequently in the rapidly changing climate, our findings suggest that high-altitude wildfire plumes must be adequately considered in climate projections in order to obtain reasonable estimates of atmospheric energy budget changes.