Assessing the consequences of including aerosol absorption in potential Stratospheric Aerosol Injection Climate Intervention Strategies

Theoretical Stratospheric Aerosol Intervention (SAI) strategies model the deliberate injection of aerosols or their precursors into the stratosphere thereby reflecting incident sunlight back to space and counterbalancing a fraction of the warming due to increased concentrations of greenhouse gases. This cooling mechanism is known to be relatively robust through analogues from explosive volcanic eruptions which have been documented to cool the climate of the Earth. However, a practical difficulty of SAI strategies is how to deliver the injection high enough to ensure dispersal of the aerosol within the stratosphere on a global scale. Recently, it has been suggested that including a small amount of absorbing material in a dedicated 10-day intensive deployment might enable aerosols or precursor gases to be injected at significantly lower, more technologically-feasible altitudes. The material then absorbs sunlight causing a localised heating and ‘lofting’ of the particles, enabling them to penetrate into the stratosphere. Such self-lofting has recently been observed following the intensive wildfires in 2019–2020 in south east Australia, where the resulting absorbing aerosol penetrated into the stratosphere and was monitored by satellite instrumentation for many months subsequent to emission. This study uses the fully coupled UKESM1 climate model simulations performed for the Geoengineering Model Intercomparison Project (GeoMIP) and new simulations where the aerosol optical properties have been adjusted to include a moderate degree of absorption. The results indicate that partially absorbing aerosols i) reduce the cooling efficiency per unit mass of aerosol injected, ii) increase deficits in global precipitation iii) delay the recovery of the stratospheric ozone hole, iv) disrupt the Quasi Biennial Oscillation when global mean temperatures are reduced by as little as 0.1 K, v) enhance the positive phase of the wintertime North Atlantic Oscillation which is associated with floods in Northern Europe and droughts in Southern Europe. While these results are dependent upon the exact details of the injection strategies and our simulations use ten times the ratio of black carbon to sulfate that is considered in the recent intensive deployment studies, they demonstrate some of the potential pitfalls of injecting an absorbing aerosol into the stratosphere to combat the global warming problem.

Influence of Aerosols on Atmospheric Gravity Waves at an Urban Tropical Location

The elevated layer of heat-absorbing pollutant aerosols causes temperature perturbations in the pre-monsoon period above the boundary layer height (1.6-4 km) as observed over a polluted tropical urban location Kolkata (22°34' N, 88°22' E) during 2007-2016. Satellite observations of different types of aerosols show an increase in aerosol extinction coefficient around 1.6-4 km altitude, enhancing the perturbations in both temperature and wind profiles at that height. The opposing air mass movement within and above the boundary layer, which is strengthened by elevated heat-absorbing aerosols, is illustrated by height profiles of atmospheric vorticity and divergence. This results in higher Brunt-Vaisala frequencies indicating increased atmospheric oscillations. Consequently, atmospheric gravity waves, which manifest the temperature and wind profile perturbations, have enhanced energy in the upper troposphere (6-10 km). Based on multi- technique observations consisting of radiosonde, space-borne lidar and model data, this study reveals the interactions between aerosol and other atmospheric processes such as temperature variations and wind perturbations, which affect the atmospheric instability and increase gravity wave activities during the pre-monsoon period over a tropical metropolis.

Interaction between aerosol and thermodynamic stability within the PBL during the wintertime over the North China Plain: Aircraft observation and WRF-Chem simulation

Aerosol-planetary boundary layer (PBL) interaction has been proposed as a key mechanism for stabilizing the atmosphere and exacerbating surface air pollution. Although the understanding of this process has progressed enormously, its magnitude and impact remain uncertain and vary widely concerning aerosol types, vertical distributions, synoptic conditions, etc. In this study, our primary interest is to distinguish the aerosol-PBL interaction of absorbing and scattering aerosols under contrasting synoptic patterns and aerosol vertical distributions. Detailed in-situ aircraft (KingAir-350) measurements and online coupled model Weather Research and Forecasting with Chemistry (WRF-Chem) simulations are explored over the North China Plain (NCP). Furthermore, a long-term PBL stability trend from 1980 to 2020 over the NCP is also investigated. The aircraft measurements and surface observations show that the surface air pollution over the Baoding City on 3 January is heavier than that on 4 January, 2020. In addition, the aerosols are restricted to the low layer on 3 January, whereas the aerosols mix more homogeneous upwards on 4 January. Thereupon, we focus on the two days with distinct synoptic circumstances, PBL stability, and aerosol vertical distributions over the NCP. According to the WRF-Chem modelling, the synoptic pattern over the Baoding City differs between the two days. The prevailing wind direction is opposite with a southwest wind on 3 January and a northeast wind on 4 January. The results indicate that the synoptic condition may affect the PBL thermal structure, thus affecting the aerosol vertical distribution. Additionally, the sensitive numerical experiments reveal that the light-absorbing and light-scattering aerosols have different effects on altering the PBL thermal structure. The inhibition effect of scattering aerosols on the PBL appears to be independent of the aerosol height distribution and solely depends on its concentration. However, aerosol-PBL feedback of absorbing aerosols is highly dependent on its vertical distribution. Our analysis highlights that we should principally concentrate on controlling the emissions of scattering aerosols under the stable stratification while cooperating to control the emissions of scattering and absorbing aerosols in an unstable stratification. Moreover, the long-term inter-annual variation in PBL stability shows a strong correlation with the East Asian Winter Monsoon, which seems to be valuable in determining which pollutants to target in different monsoon years and attaining more precise air pollution control. Based on the numerical simulations and observational constraints, a concept scheme description has been concluded to deepen our recognition of the interactions between thermodynamic stability and aerosols within the PBL over the NCP region.

Rethinking the correction for absorbing aerosols in the OMI- and TROPOMI-like surface UV algorithms

Satellite estimates of surface UV irradiance have been available since 1978 from the TOMS UV spectrometer and have continued with significantly improved ground resolution using the Ozone Monitoring Instrument (OMI 2004–current) and Sentinel 5 Precursor (S5P 2017–current). The surface UV retrieval algorithm remains essentially the same: it first estimates the clear-sky UV irradiance based on measured ozone and then accounts for the attenuation by clouds and aerosols, applying two consecutive correction factors. When estimating the total aerosol effect in surface UV irradiance, there are two major classes of aerosols to be considered: (1) aerosols that only scatter UV radiation and (2) aerosols that both scatter and absorb UV radiation. The former effect is implicitly included in the measured effective Lambertian-equivalent scene reflectivity (LER), so the scattering aerosol influence is estimated through cloud correction factor. Aerosols that absorb UV radiation attenuate the surface UV radiation more strongly than non-absorbing aerosols of the same extinction optical depth. Moreover, since these aerosols also attenuate the outgoing satellite-measured radiance, the cloud correction factor that treats these aerosols as purely scattering underestimates their aerosol optical depth (AOD), causing underestimation of LER and overestimation of surface UV irradiance. Therefore, for correction of aerosol absorption, additional information is needed, such as a model-based monthly climatology of aerosol absorption optical depth (AAOD). A correction for absorbing aerosols was proposed almost a decade ago and later implemented in the operational OMI and TROPOMI UV algorithms. In this study, however, we show that there is still room for improvement to better account for the solar zenith angle (SZA) dependence and nonlinearity in the absorbing aerosol attenuation, and as a result we propose an improved correction scheme. There are two main differences between the new proposed correction and the one that is currently operational in OMI and TROPOMI UV algorithms. First, the currently operational correction for absorbing aerosols is a function of AAOD only, while the new correction additionally takes the solar zenith angle dependence into account. Second, the second-order polynomial of the new correction takes the nonlinearity in the correction as a function of AAOD better into account, if compared to the currently operational one, and thus better describes the effect by absorbing aerosols over a larger range of AAOD. To illustrate the potential impact of the new correction in the global UV estimates, we applied the current and new proposed correction for global fields of AAOD from the aerosol climatology currently used in OMI UV algorithm, showing a typical differences of ±5 %. This new correction is easy to implement operationally using information of solar zenith angle and existing AAOD climatology.

On the contribution of fast and slow responses to precipitation changes caused by aerosol perturbations

Changes in global-mean precipitation are strongly constrained by global radiative cooling, while regional rainfall changes are less constrained because energy can be transported. Absorbing and non-absorbing aerosols have different effects on both global-mean and regional precipitation, due to the distinct effects on energetics. This study analyses the precipitation responses to large perturbations in black carbon (BC) and sulfate (SUL) by examining the changes in atmospheric energy budget terms on global and regional scales, in terms of fast (independent of changes in sea surface temperature, SST) and slow responses (mediated by changes in SST). Changes in atmospheric radiative cooling/heating are further decomposed into contributions from clouds, aerosols, and clear–clean sky (without clouds or aerosols). Both cases show a decrease in global-mean precipitation, which is dominated by fast responses in the BC case and slow responses in the SUL case. The geographical patterns are distinct too. The intertropical convergence zone (ITCZ), accompanied by tropical rainfall, shifts northward in the BC case, while it shifts southward in the SUL case. For both cases, energy transport terms from the slow response dominate the changes in tropical rainfall, which are associated with the northward (southward) shift of the Hadley cell in response to the enhanced southward (northward) cross-equatorial energy flux caused by increased BC (SUL) emission. The extra-tropical precipitation decreases in both cases. For the BC case, fast responses to increased atmospheric radiative heating contribute most to the reduced rainfall, in which absorbing aerosols directly heat the mid-troposphere, stabilise the column, and suppress precipitation. Unlike BC, non-absorbing aerosols decrease surface temperatures through slow processes, cool the whole atmospheric column, and reduce specific humidity, which leads to decreased radiative cooling from the clear–clean sky, which is consistent with the reduced rainfall. Examining the changes in large-scale circulation and local thermodynamics qualitatively explains the responses of precipitation to aerosol perturbations, whereas the energetic perspective provides a method to quantify their contributions.

Satellite-Based Aerosol Classification for Capital Cities in Asia Using a Random Forest Model

Aerosol types in Asian capital cities were classified using a random forest (RF) satellite-based aerosol classification model during 2018–2020 in an investigation of the contributions of aerosol types, with or without Aerosol Robotic Network (AERONET) observations. In this study, we used the recently developed RF aerosol classification model to detect and classify aerosols into four types: pure dust, dust-dominated aerosols, strongly absorbing aerosols, and non-absorbing aerosols. Aerosol optical and microphysical properties for each aerosol type detected by the RF model were found to be reasonably consistent with those for typical aerosol types. In Asian capital cities, pollution-sourced aerosols, especially non-absorbing aerosols, were found to predominate, although Asian cities also tend to be seasonally affected by natural dust aerosols, particularly in East Asia (March–May) and South Asia (March–August). No specific seasonal effects on aerosol type were detected in Southeast Asia, where there was a predominance of non-absorbing aerosols. The aerosol types detected by the RF model were compared with those identified by other aerosol classification models. This study indicates that the satellite-based RF model may be used as an alternative in the absence of AERONET sites or observations.

Rapid transformation of ambient absorbing aerosols from West African biomass burning

Seasonal biomass burning (BB) over West Africa is a globally significant source of carbonaceous particles in the atmosphere, which have important climate impacts but are poorly constrained. Here, the evolution of smoke aerosols emitted from flaming-controlled burning of agricultural waste and wooded savannah in the Senegal region was characterized over a timescale of half-day advection from the source during the MOYA-2017 (Methane Observation Yearly Assessment-2017) aircraft campaign. Plumes from such fire types are rich in black carbon (BC) emissions. Concurrent measurements of chemical composition, organic aerosol (OA) oxidation state, bulk aerosol size and BC mixing state reveal that emitted BB submicron aerosols changed dramatically with time. Various aerosol optical properties (e.g. absorption Ångström exponent – AAE – and mass absorption coefficients – MACs) also evolved with ageing. In this study, brown carbon (BrC) was a minor fractional component of the freshly emitted BB aerosols (< 0.5 h), but the increasing AAE with particle age indicates that BrC formation dominated over any loss process over the first ∼ 12 h of plume transport. Using different methods, the fractional contribution of BrC to total aerosol absorption showed an increasing trend with time and was ∼ 18 %–31 % at the optical wavelength of 405 nm after half-day transport. The generated BrC was found to be positively correlated with oxygenated and low-volatility OA, likely from the oxidation of evaporated primary OA and secondary OA formation. We found that the evolution of BrC with particle age was different in this region compared with previous BB field studies that mainly focused on emissions from smouldering fires, which have shown a high contribution from BrC at the source and BrC net loss upon ageing. This study suggests an initial stage of BrC absorption enhancement during the evolution of BB smoke. Secondary processing is the dominant contributor to BrC production in this BB region, in contrast to the primary emission of BrC previously reported in other BB studies. The total aerosol absorption normalized to BC mass (MACmeas-BC) was also enhanced with ageing due to the lensing effect of increasingly thick coatings on BC and the absorption by BrC. The effect of ageing on aerosol absorption, represented by the absorption enhancement (EAbs-MAC), was estimated over timescales of hours. MOYA-2017 provides novel field results. The comparisons between MOYA-2017 and previous field studies imply that the evolution of absorbing aerosols (BC and BrC) after emission varies with source combustion conditions. Different treatments of absorbing aerosol properties from different types of fires and their downwind evolution should be considered when modelling regional radiative forcing. These observational results will be very important for predicting climate effects of BB aerosol in regions controlled by flaming burning of agricultural waste and savannah-like biomass fuels.