Non-reversible aging can increase solar absorption in African biomass burning aerosol plumes of intermediate age

Recent studies highlight that biomass-burning aerosol over the remote southeast Atlantic is some of the most sunlight-absorbing aerosol on the planet. In-situ measurements of single-scattering albedo at the 530 nm wavelength (SSA530nm) range from 0.83 to 0.89 within six flights (five in September, 2016 and one in late August, 2017) of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) aircraft campaign, increasing with the organic aerosol to black carbon (OA : BC) mass ratio. OA : BC mass ratios of 10 to 14 are lower than some model values and consistent with BC-enriched source emissions, based on indirect inferences of fuel type (savannah grasslands) and dry, flame-efficient combustion conditions. These primarily explain the low single-scattering albedos. We investigate whether continued chemical aging of aerosol plumes of intermediate age (4–7 days after emission, as determined from model tracers) within the free troposphere can further lower the SSA530nm. A mean OA to organic carbon mass ratio of 2.2 indicates highly oxygenated aerosol with the chemical marker f44 indicating the free-tropospheric aerosol continues to oxidize after advecting offshore of continental Africa. Two flights, for which BC to carbon monoxide (CO) ratios remain constant with increasing chemical age, are analyzed further. In both flights, the OA : BC mass ratio decreases over the same time span, indicating continuing net aerosol loss. One flight sampled younger (∼ 4 days) aerosol within the strong zonal outflow of the 4–6 km altitude African Easterly Jet-South. This possessed the highest OA : BC mass ratio of the 2016 campaign and overlaid slightly older aerosol with proportionately less OA, although the age difference of one day is not enough to attribute to a large-scale recirculation and subsidence pattern. The other flight sampled aerosol constrained closer to the coast by a mid-latitude disturbance and found older aerosol aloft overlying younger aerosol. Its vertical increase in OA : BC and nitrate to BC was less pronounced than when younger aerosol overlaid older aerosol, consistent with compensation between a net aerosol loss through aging and a thermodynamical partitioning. Organic nitrate provided 68 % on average of the total nitrate for the 6 flights, in contrast to measurements made at Ascension Island that only found inorganic nitrate. Some evidence for the thermodynamical partitioning to the particle phase at higher altitudes with higher relative humidities for nitrate is still found. The 470–660 nm absorption Angstrom exponent is slightly higher near the African coast than further offshore (approximately 1.2 versus 1.0–1.1), indicating some brown carbon may be present near the coast. The data support the following parameterization: SSA530nm = 0.80+0056*(OA : BC). This indicates a 20 % decrease in SSA can be attributed to chemical aging, or the net 25 % reduction in OA : BC documented for constant BC : CO ratios.

Aerosol-light interactions reduce the carbon budget imbalance

Current estimates of the global land carbon sink contain substantial uncertainties on interannual timescales which contribute to a non-closure in the global carbon budget in any given year. This budget imbalance (BIM) partly arises due to the use of imperfect models which are missing or misrepresenting processes. One such omission is the separate treatment of downward direct and diffuse solar radiation on photosynthesis. Here we evaluate and use an improved high-resolution (6-hourly), gridded dataset of surface solar diffuse and direct fluxes, over 1901-2017, constrained by satellite and ground-level observations, to drive two global land models. Results show that tropospheric aerosol-light interactions have the potential for substantial land carbon impacts (up to 0.4 PgCyr-1 enhanced sink) at decadal timescales, however large uncertainties remain, with models disagreeing on the direction of change in carbon uptake. On interannual timescales, results also show an enhancement of the land sink (up to 0.9 PgCyr-1) and subsequent reduction in BIM by 55% in years following volcanic eruptions. We therefore suggest global carbon budget assessments include this dataset in order to improve land sink estimates.

Controls on surface aerosol particle number concentrations and aerosol-limited cloud regimes over the central Greenland Ice Sheet

This study presents the first full annual cycle (2019–2020) of ambient surface aerosol particle number concentration measurements (condensation nuclei > 20 nm, N20) collected at Summit Station (Summit), in the centre of the Greenland Ice Sheet (72.58∘ N, −38.45∘ E; 3250 ma.s.l.). The mean surface concentration in 2019 was 129 cm−3, with the 6 h mean ranging between 1 and 1441 cm−3. The highest monthly mean concentrations occurred during the late spring and summer, with the minimum concentrations occurring in February (mean: 18 cm−3). High-N20 events are linked to anomalous anticyclonic circulation over Greenland and the descent of free-tropospheric aerosol down to the surface, whereas low-N20 events are linked to anomalous cyclonic circulation over south-east Greenland that drives upslope flow and enhances precipitation en route to Summit. Fog strongly affects particle number concentrations, on average reducing N20 by 20 % during the first 3 h of fog formation. Extremely-low-N20 events (< 10 cm−3) occur in all seasons, and we suggest that fog, and potentially cloud formation, can be limited by low aerosol particle concentrations over central Greenland.

Description and evaluation of the tropospheric aerosol scheme in the Integrated Forecasting System (IFS-AER, cycle 47R1) of ECMWF

This article describes the IFS-AER aerosol scheme used operationally in the Integrated Forecasting System (IFS) cycle 47R1, operated by the European Centre for Medium Range Weather Forecasts (ECMWF) in the framework of the Copernicus Atmosphere Monitoring Services (CAMS). It represents an update of the Rémy et al. (2019) article which focused on cycle 45R1 of IFS-AER. The parameterizations of sources and sinks that have been updated since cycle 45R1 are described, as well as changes in the configuration used operationally within CAMS. As compared to cycle 45R1, a greater integration of aerosol and chemistry has been achieved. Primary aerosol sources have been updated, with the implementation of new dust and seasalt aerosol emission schemes. New dry and wet deposition parameterizations have also been implemented. Sulfate production rates are now provided by the global chemistry component of the IFS. This paper aims to describe most of the updates that have been implemented since cycle 45R1 and not only the ones that are used operationally in cycle 47R1; components that are not used operationally will be clearly flagged. Cycle 47R1 of IFS-AER has been evaluated against a wide range surface and total column observations. The final simulated products such as Particulate Matter (PM) and Aerosol Optical Depth (AOD) generally show a significant increase in skill as compared to results obtained with cycle 45R1. Similarly, the simulated surface concentration of sulphate, organic matter and sea-salt aerosol is improved by cycle 47R1 as compared to cycle 45R1. Some imbalances persist, such as a too high surface concentration of nitrate and organic matter. The new wet and dry deposition schemes that have been implemented into cycle 47R1 have a mostly positive impact on simulated AOD, PM and speciated aerosol surface concentration.

Retrieval of tropospheric aerosol, NO₂ and HCHO vertical profiles from MAX-DOAS observations over Thessaloniki, Greece

In this study we focus on the retrieval of aerosol and trace gas vertical profiles from Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations for the first time over Thessaloniki, Greece. We use two independent inversion algorithms for the profile retrievals: The Mexican MAX-DOAS Fit (MMF) and the Mainz Profile Algorithm (MAPA). The former is based on the Optimal Estimation Method (OEM), while the latter follows a parameterization approach. We evaluate the performance of MMF and MAPA and we validate their retrieved products with ancillary data measured by other co-located reference instruments. We find an excellent agreement between the tropospheric column densities of NO2 retrieved by MMF and MAPA (Slope = 1.009, Pearson's correlation coefficient R = 0.982) and a good correlation for the case of HCHO (R = 0.927). For aerosols, we find better agreement for the aerosol optical depths (AODs) in the visible (i.e., at 477 nm), compared to the UV (360 nm) and we show that the agreement strongly depends on the O4 scaling factor that is used in the analysis. The trace gas differential slant column densities (dSCDs), simulated by the forward models, are also in good agreement, except for HCHO, where larger scatter is observed due to the increased spectral noise of the measurements in the UV. The agreement for NO2 and HCHO surface concentrations is similar to the comparison of the integrated columns with slightly decreased correlation coefficients. The AODs retrieved by the MAX-DOAS are validated by comparing them with AOD values measured by a CIMEL sun-photometer and a Brewer spectrophotometer. Four different flagging schemes were applied to the data in order to evaluate their performance. Qualitatively, a generally good agreement is observed for both wavelengths, but we find a systematic bias from the CIMEL and Brewer measurements, due to the limited sensitivity of the MAX-DOAS in retrieving information at higher altitudes, especially in the UV. An in-depth validation of the aerosol vertical profiles retrieved by the MAX-DOAS is not possible since only in very few cases the true aerosol profile is known during the period of study. However, we examine four cases, where the MAX-DOAS provided a generally good estimation of the shape of the profiles retrieved by a co-located multi-wavelength lidar system. The NO2 surface concentrations are validated against in situ observations and the comparison of both MMF and MAPA revealed good agreement with correlation coefficients of R = 0.78 and R = 0.73, respectively. Finally, the effect of the O4 scaling factor is investigated by intercomparing the integrated columns retrieved by the two algorithms and also by comparing the AODs derived by MAPA for different values of the scaling factor with AODs measured by the CIMEL and the Brewer.

Influence of the Saharan Air Layer on Hurricane Nadine (2012). Part I: Observations from the Hurricane and Severe Storm Sentinel (HS3) Investigation and Modeling Results

This study uses a model with aerosol-cloud-radiation coupling to examine the impact of Saharan dust and other aerosols on Hurricane Nadine (2012). In order to study aerosol direct (radiation) and indirect (cloud microphysics) effects from individual, as well as all aerosol species, eight different NU-WRF simulations were conducted. In several simulations, aerosols led to storm strengthening, followed by weakening relative to the Ctrl simulation. This variability of the aerosol impact may be related to whether aerosols are ingested into clouds within the outer rainbands or the eyewall. Upper tropospheric aerosol concentrations indicate vertical transport of all aerosol types in the outer bands but only vertical transport of sea salt in the inner core. The results suggest that aerosols, particularly sea salt, may have contributed to a stronger initial intensification, but that aerosols ingestion into the outer bands at later times may have weakened the storm in the longer term. In most aerosol experiments, aerosols led to a reduction in cloud and precipitation hydrometeors, the exception being the dust-only case that produced periods of enhanced hydrometeor growth. The Saharan Air Layer (SAL) also impacted Nadine by causing a region of strong easterlies impinging on the eastern side of the storm. At the leading edge of these easterlies, cool and dry air near the top of the SAL was being ingested into the outer-band convection. This midlevel low equivalent-potential-temperature air gradually lowered toward the surface and eventually contributed to significant cold pool activity in the eastern rain band and in the northeast quadrant of the storm. Such enhanced downdraft activity could have led to weakening of the storm, but it is not presently possible to quantify this impact.

Sunlight-absorbing aerosol amplifies the seasonal cycle in low-cloud fraction over the southeast Atlantic

The mean altitude of the smoke loading over the southeast Atlantic moves from the boundary layer in July to the free troposphere by October. This study details the month-by-month changes in cloud properties and the large-scale environment as a function of the biomass burning aerosol loading at Ascension Island (8∘ S, 14.5∘ W) from July to October, based on island measurements, satellite retrievals, and reanalysis. In July and August, the smoke loading predominantly varies within the boundary layer. During both months, the low-cloud fraction is less and is increasingly cumuliform when more smoke is present, with the exception of a late morning boundary layer deepening that encourages a short-lived cloud development. The meteorology varies little, suggesting aerosol–cloud interactions explain the cloudiness changes. September marks a transition month during which midlatitude disturbances can intrude into the Atlantic subtropics, constraining the free tropospheric aerosol closer to the African coast. Stronger boundary layer winds on cleaner days help deepen, dry, and cool much of the marine boundary layer compared to that on days with high smoke loadings, with stratocumulus reducing everywhere but at the northern deck edge. The September free troposphere is better mixed on smoky days compared to October. Longwave cooling rates, generated by a sharp water vapor gradient at the aerosol layer top, encourage a small-scale vertical mixing that could help maintain the well-mixed smoky September free troposphere. The October meteorology primarily varies as a function of the strength of the free tropospheric winds advecting aerosol offshore. The free tropospheric aerosol loading is less than in September, and the moisture variability is greater. Low-level clouds increase and are more stratiform in October when the smoke loadings are higher. The increased free tropospheric moisture can help sustain the clouds through a reduction in evaporative drying during cloud-top entrainment. Enhanced subsidence above the coastal upwelling region, increasing cloud droplet number concentrations, may further prolong cloud lifetime through microphysical interactions. Reduced subsidence underneath stronger free tropospheric winds at Ascension Island supports slightly higher cloud tops during smokier conditions. Overall, the monthly changes in the large-scale aerosol and moisture vertical structure act to amplify the seasonal cycle in low-cloud amount and morphology. This is climatically important, as cloudiness changes dominate changes in the top-of-atmosphere radiation budget.

Australian Fires 2019–2020: Tropospheric and Stratospheric Pollution Throughout the Whole Fire Season

The historically large and severe wildfires in Australia from September 2019 to March 2020 are known to have injected a smoke plume into the stratosphere around New Year, due to pyro-cumulonimbus (pyro-Cb) activity, that was subsequently distributed throughout the Southern Hemisphere (SH). We show with satellite, ground based remote sensing, and in situ observations that the fires before New Year, had already a substantial impact on the SH atmosphere, starting as early as September 2019, with subsequent long-range transport of trace gas plumes in the upper-troposphere. Airborne in situ measurements above Southern Argentina in November 2019 show elevated CO mixing ratios at an altitude of 11 km and can be traced back using FLEXPART trajectories to the Australian fires in mid-November 2019. Ground based solar-FTS (Fourier Transform Spectroscopy) observations of biomass burning tracers CO, HCN and C2H6 at Lauder, South Island, New Zealand show enhanced tropospheric columns already starting in September 2019. In MLS observations averaged over 30°–60°S, enhanced CO mixing ratios compared to previous years become visible in late October 2019 only at and below the 147 hPa pressure level. Peak differences are found with satellite and ground-based observations for all altitude levels in the Southern Hemisphere in January. With still increased aerosol values following the Ulawun eruption in 2019, averaged satellite observations show no clear stratospheric and upper-tropospheric aerosol enhancements from the Australian fires, before the pyro-Cb events at the end of December 2019. However, with the clear enhancement of fire tracers, we suggest the period September to December 2019 (prior to the major pyro-Cb events) should be taken into account in terms of fire pollutant emissions when studying the impact of the Australian fires on the SH atmosphere.