Free Tropospheric Aerosol Research Articles

Influence of columnar versus vertical distribution of aerosol properties on the modulation of shortwave radiative effects

Quantifying the interaction of atmospheric aerosols with incoming solar radiation remains a challenge owing to the limitations associated with measuring aerosol optical properties. This study investigates how the distribution of aerosol properties, whether columnar or vertical, affects the aerosol radiative forcing (ARF) and heating rates (HRs) across different atmospheric layers under cloud-free conditions in the shortwave region. We also assess the atmospheric parameters, namely, pressure, temperature, water vapour density, and ozone density, from in-situ measurements, reanalysis data, and a standard tropical atmosphere to understand their impact on ARF and HR estimates across seasons. Our findings show that aerosol absorption is highest during monsoon, while it is lowest in the winter. Significant atmospheric warming due to aerosols resulted from the substantial cooling at the surface. Columnar properties of aerosols measured at limited or multiple wavelengths yield similar ARF and HR estimates, provided spectral dependency is considered using the Angstrom exponent across seasons. However, the vertical profiles of aerosol extinction, together with a constant single scattering albedo (SSA) along the atmospheric column versus an actual SSA profile, led to notable differences in ARF and HRs, specifically in pre-monsoon and monsoon periods. Free tropospheric aerosol absorption is underestimated when using columnar properties compared to vertical distribution, while boundary layer absorption is overestimated (> 10 Wm-2). The heterogeneity in aerosol types across atmospheric layers significantly influenced aerosol absorption, highlighting the importance of accurate vertical distribution information. HR profiles obtained with vertical distribution reflect the structure of aerosol extinction, whereas those estimated with columnar properties result in smoother profiles that fail to capture altitude gradients. Aerosol-induced HRs are higher within the boundary layer and free troposphere in the monsoon season for all scenarios of defined aerosol properties. These findings underscore the need for actual vertical profile measurements of aerosol properties to quantify aerosol radiation interaction.

Change in precipitation pattern over South Asia in response to the trends in regional warming and free-tropospheric aerosol loading

Spatial and temporal shifts in rainfall patterns over South Asia and the adjoining Seas during the pre-monsoon season have been observed over the past 2 decades from 2000 to 2019. Aerosol particles suspended above the boundary layer are a contributing factor to these changes. These particles not only alter cloud characteristics, but also diminish the lapse rate, thereby suppressing convective activity, leading to precipitation anomalies. Over the past 2 decades, high-rainfall regions have experienced declining rainfall, while low-rainfall regions have received increased rainfall. Coinciding with notable anomalies in precipitation, contrasting trends in aerosol optical depth, particularly due to absorbing aerosols in the elevated regions of the atmosphere, are seen. Apart from aerosols, several factors are considered that are critical in modifying precipitation patterns over the study region, such as water vapor content, convective processes, and lower-level relative humidity. We observed a potential transport of excess water vapor by ambient circulation from the oceanic regions having reduced rain, such as Bay of Bengal and the Arabian Sea, to higher latitudes enabling precipitation anomaly at distant locations.

Above-cloud concentrations of cloud condensation nuclei help to sustain some Arctic low-level clouds

Abstract. Previous studies have found that low-level Arctic clouds often persist for long periods even in the face of very low surface cloud condensation nuclei (CCN) concentrations. Here, we investigate whether these conditions could occur due to continuous entrainment of aerosol particles from the free troposphere (FT). We use an idealized large eddy simulation (LES) modeling framework, where aerosol concentrations are low in the boundary layer (BL) but increased up to 50× in the free troposphere. We find that the tests with higher tropospheric aerosol concentrations simulated clouds, which persisted for longer and maintained higher liquid water paths (LWPs). This is due to direct entrainment of the tropospheric aerosol into the cloud layer, which results in a precipitation suppression from the increase in cloud droplet number and in stronger cloud-top radiative cooling, which causes stronger circulations maintaining the cloud in the absence of surface forcing. Together, these two responses result in a more well-mixed boundary layer with a top that remains in contact with the tropospheric aerosol reservoir and can maintain entrainment of those aerosol particles. The surface aerosol concentrations, however, remained low in all simulations. The free-tropospheric aerosol concentration necessary to maintain the clouds is consistent with concentrations that are frequently seen in observations.

Aerosol-related effects on the occurrence of heterogeneous ice formation over Lauder, New Zealand ∕ Aotearoa

Abstract. The presented study investigates the efficiency of heterogeneous ice formation in natural clouds over Lauder, New Zealand / Aotearoa. Aerosol conditions in the middle troposphere above Lauder are subject to huge contrasts. Clean, pristine air masses from Antarctica and the Southern Ocean arrive under southerly flow conditions, while high aerosol loads can occur when air masses are advected from nearby Australia. This study assesses how these contrasts in aerosol load affect the ice formation efficiency in stratiform midlevel clouds in the heterogeneous freezing range (−40 to 0 ∘C). For this purpose, an 11-year dataset was analyzed from a dual-wavelength polarization lidar system operated by National Institute of Water and Atmospheric Research (NIWA), Taihoro Nukurangi, at Lauder in collaboration with the National Institute for Environmental Studies in Japan and the Meteorological Research Institute of the Japan Meteorological Agency. These data were used to investigate the efficiency of heterogeneous ice formation in clouds over the site as a function of cloud-top temperature as in previous studies at other locations. The Lauder cloud dataset was put into context with lidar studies from contrasting regions such as Germany and southern Chile. The ice formation efficiency found at Lauder is lower than in polluted midlatitudes (i.e., Germany) but higher than, for example, in southern Chile. Both Lauder and southern Chile are subject to generally low free-tropospheric aerosol loads, which suggests that the low ice formation efficiency at these two sites is related to low ice-nucleating-particle (INP) concentrations. However, Lauder sees episodes of continental aerosol, more than southern Chile does, which seems to lead to the moderately increased ice formation efficiency. Trajectory-based tools and aerosol model reanalyses are used to relate this cloud dataset to the aerosol load and the air mass sources. Both analyses point clearly to higher ice formation efficiency for clouds which are more strongly influenced by continental aerosol and to lower ice formation efficiency for clouds which are more influenced by Antarctic/marine aerosol and air masses.

Free-tropospheric aerosols contribute to large aerosol optical depth at a remote, inland location with insignificant anthropogenic emissions

In-situ measurements of atmospheric aerosols from remote environments marked with negligible human activities are required to reduce the uncertainties associated with natural aerosols in pre-industrial climate forcings (particularly the aerosol-cloud interactions). In this study, we present long-term continuous aerosol measurements, carried out using ground-based and satellite observations, both close to the surface and in the vertical column, over a remote, rural, inland location in southern peninsular India. The near-surface aerosol concentrations were low, in general conformity to the typical pattern expected for a remote location, with the temporal changes being primarily governed by the background meteorology. However, the columnar aerosol optical depth (AOD) was surprisingly high and resembled that of a typical semi-urban continental location, with an yearly mean AOD of 0.47 ± 0.06. Spaceborne lidar observations in conjunction with ground-based radiometer measurements revealed that around 60% of this AOD was contributed by free-tropospheric aerosol layers during summer and monsoon seasons. Airmass back-trajectory analysis along with particle depolarisation ratio profiles indicate that these aerosol layers are mostly associated with long-range transported dust aerosols. Our findings indicate that benign surface concentration of aerosols at a location need not necessarily be sufficient to consider it as an optimal choice for studying background aerosols.

Optical Properties of Boundary Layer Aerosols From High Spectral Resolution Lidar Measurements in a Polluted Urban Environment (Seoul, Korea)

AbstractContinuous measurements of aerosol extinction coefficient (σext) from the High Spectral Resolution Lidar (HSRL) in Seoul from 2016 to 2018 were used to investigate the diurnal variation of the aerosol optical depth (AOD). Nighttime AOD displayed a larger mean and standard deviation (0.45 ± 0.47) than daytime (0.40 ± 0.29). Hygroscopic growth of aerosols under humid conditions was a key factor in the relative enhancement of nighttime AOD. Taking advantage of the HSRL's vertically resolved measurements, the contribution of aerosols within the boundary layer (BL) and free troposphere (FT) to AOD and its temporal variation were investigated. Unlike the diurnal AOD variation, AOD within the BL (AODBL) showed similar diurnal variations with the mixing layer height (MLH), displaying lower nighttime values with a peak around 14–15 local standard time. However, the low correlation between MLH and AODBL (R2 = 0.06) implied that MLH was not the sole deterministic factor of AODBL. A larger AOD of FT aerosols (AODFT) was observed during spring due to frequent elevated dust layers. Using mean σext within the BL and surface PM10 concentrations, the mass extinction efficiency (MEE) of aerosols in Seoul was estimated. The PM10 MEE showed a mean of 5.40 g m−2 and displayed significant variability by PM2.5 to PM10 ratio, season, and ambient relative humidity. The uncertainty of estimated surface PM10 concentrations was minimized when the seasonality and humidity factor in MEE were taken into account (the normalized mean bias decreased from 10.6%, using a single MEE value, to 6.2%).

Cloud adjustments from large-scale smoke–circulation interactions strongly modulate the southeastern Atlantic stratocumulus-to-cumulus transition

Abstract. Smoke from southern Africa blankets the southeastern Atlantic Ocean from June to October, producing strong and competing aerosol radiative effects. Smoke effects on the transition between overcast stratocumulus and scattered cumulus clouds are investigated along a Lagrangian (air-mass-following) trajectory in regional climate and large eddy simulation models. Results are compared with observations from three recent field campaigns that took place in August 2017: ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES), CLouds and Aerosol Radiative Impacts and Forcing: Year 2017 (CLARIFY), and Layered Atlantic Smoke Interactions with Clouds (LASIC). The case study is set up around the joint ORACLES–CLARIFY flight that took place near Ascension Island on 18 August 2017. Smoke sampled upstream on an ORACLES flight on 15 August 2017 likely entrained into the marine boundary layer later sampled during the joint flight. The case is first simulated with the WRF-CAM5 regional climate model in three distinct setups: (1) FireOn, in which smoke emissions and any resulting smoke–cloud–radiation interactions are included; (2) FireOff, in which no smoke emissions are included; (3) RadOff, in which smoke emissions and their microphysical effects are included but aerosol does not interact directly with radiation. Over the course of the Lagrangian trajectory, differences in free tropospheric thermodynamic properties between FireOn and FireOff are nearly identical to those between FireOn and RadOff, showing that aerosol–radiation interactions are primarily responsible for the free tropospheric effects. These effects are non-intuitive: in addition to the expected heating within the core of the smoke plume, there is also a “banding” effect of cooler temperature (∼1–2 K) and greatly enhanced moisture (>2 g kg−1) at the plume top. This banding effect is caused by a vertical displacement of the former continental boundary layer in the free troposphere in the FireOn simulation resulting from anomalous diabatic heating due to smoke absorption of sunlight that manifests primarily as a few hundred meters per day reduction in large-scale subsidence over the ocean. A large eddy simulation (LES) is then forced with free tropospheric fields taken from the outputs for the WRF-CAM5 FireOn and FireOff runs. Cases are run by selectively perturbing one variable (e.g., aerosol number concentration, temperature, moisture, vertical velocity) at a time to better understand the contributions from different indirect (microphysical), “large-scale” semi-direct (above-cloud thermodynamic and subsidence changes), and “local” semi-direct (below-cloud smoke absorption) effects. Despite a more than 5-fold increase in cloud droplet number concentration when including smoke aerosol concentrations, minimal differences in cloud fraction evolution are simulated by the LES when comparing the base case with a perturbed aerosol case with identical thermodynamic and dynamic forcings. A factor of 2 decrease in background free tropospheric aerosol concentrations from the FireOff simulation shifts the cloud evolution from a classical entrainment-driven “deepening–warming” transition to trade cumulus to a precipitation-driven “drizzle-depletion” transition to open cells, however. The thermodynamic and dynamic changes caused by the WRF-simulated large-scale adjustments to smoke diabatic heating strongly influence cloud evolution in terms of both the rate of deepening (especially for changes in the inversion temperature jump and in subsidence) and in cloud fraction on the final day of the simulation (especially for the moisture “banding” effect). Such large-scale semi-direct effects would not have been possible to simulate using a small-domain LES model alone.

Source attribution of cloud condensation nuclei and their impact on stratocumulus clouds and radiation in the south-eastern Atlantic

Abstract. The semi-permanent stratocumulus clouds over the south-eastern Atlantic Ocean (SEA) can act as an “air conditioner” to the regional and global climate system. The interaction of aerosols and clouds becomes important in this region and can lead to negative radiative effects, partially offsetting the positive radiative forcing of greenhouse gases. A key pathway by which aerosols affect cloud properties is by acting as cloud condensation nuclei (CCN). In this paper, we use the United Kingdom Earth System Model (UKESM1) to investigate the sources of CCN (from emissions and atmospheric processes) in the SEA as well as the response of the cloud droplet number concentration (CDNC), the cloud liquid water path (LWP), and radiative forcing to these sources during 2016 and 2017. Overall, free and upper troposphere nucleated aerosols are the dominant source of the boundary layer CCN concentration at 0.2 % supersaturation (CCN0.2 %), contributing an annual average of ∼ 41 % as they subside and entrain into the marine boundary layer, which is consistent with observations highlighting the important role of nucleation in the boundary layer CCN concentration. In terms of emission sources, anthropogenic emissions (from energy, industry, agriculture, etc.) contribute the most to the annual average CCN0.2 % in the marine boundary layer (∼ 26 %), followed by biomass burning (BB, ∼ 17 %). In the cloud layer, BB contributes about 34 % of the annual CCN0.2 %, midway between the contributions from aerosol nucleation (36 %) and anthropogenic sources (31 %). The contribution of aerosols from different sources to the CDNC is consistent with their contribution to CCN0.2 % within the marine boundary layer, with free and upper troposphere aerosol nucleation being the most important source of the CDNC overall. In terms of emission sources, anthropogenic sources are also the largest contributors to the annual average CDNC, closely followed by BB. However, during the BB season, BB and free and upper troposphere aerosol nucleation are equally the most important sources of the CDNC. The contribution of BB to the CDNC is more significant than its increase to CCN0.2 %, mainly because BB aerosols are mostly located directly above the inversion layer in the model; thus, they can increase the in-cloud CDNC by enhancing the supersaturation through the dynamical feedback due to short-wave absorption. An aerosol source that shows an increase in the CDNC also shows an increase in the LWP resulting from a reduction in autoconversion. Due to the absorption effect, BB aerosol can enhance existing temperature inversions and reduce the entrainment of sub-saturated air, leading to a further increase in the LWP. As a result, the contribution of BB to the LWP is second only to aerosol nucleation on annual averages. These findings demonstrate that BB is not the dominant source of CCN within the marine boundary layer from an emission source perspective. However, as most BB aerosols are located directly above the inversion layer, their effect on clouds increases due to their absorption effect (about the same as anthropogenic sources for the CDNC and more than anthropogenic sources for the LWP), highlighting the crucial role of their radiative effect on clouds. The results on the radiative effects of aerosols show that BB aerosol exhibits an overall positive RFari (radiative forcing associated with aerosol–radiation interactions), but its net effective radiative forcing remains negative due to its effect on clouds (mainly due to its absorbing effect). By quantifying aerosol and cloud properties affected by different sources, this paper provides a framework for understanding the effects of aerosol sources on marine stratocumulus clouds and radiation in the SEA.

Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources

Abstract. Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigate the chemical composition and provide an overview of the phase states of individual particles that have undergone long-range transport over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP) in the Azores. The OMP is an ideal site for studying long-range-transported free tropospheric particles because local emissions have a negligible influence and contributions from the boundary layer are rare. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origins and transport trajectories of sampled air masses and found that most of them originated from North America and recirculated over the North Atlantic Ocean. The FLEXPART analysis showed that the sampled air masses were highly aged (average plume age >10 d). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results showed that the most abundant particle types were carbonaceous (∼ 29.9 % to 82.0 %), sea salt (∼ 0.3 % to 31.6 %), and sea salt with sulfate (∼ 2.4 % to 31.5 %). We used a tilted stage interfaced within an environmental scanning electron microscope (ESEM) to determine the phase states of individual submicron particles. We found that most particles (∼ 47 % to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed substantial fractions of solid and semisolid particles (∼ 0 % to 30 % and ∼ 1 % to 42 %, respectively) during different transport patterns and events, reflecting the particles' phase-state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART-simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would lead to an overestimation of the viscosity of free tropospheric particles. Our findings warrant future investigation aiming at the quantitative assessment of the influence of internal mixing on the phase states of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can help models to reduce uncertainties about the effects of ambient aerosol particles on climate.

Coalescence Scavenging Drives Droplet Number Concentration in Southern Ocean Low Clouds

AbstractCloud droplet number concentration (Nd) is a key microphysical property that is largely controlled by the balance between sources and sinks of aerosols that serve as cloud condensation nuclei (CCN). Despite being a key sink of CCN, the impact of coalescence scavenging on Southern Ocean (SO) cloud is poorly known. We apply a simple source‐and‐sink budget model based on parameterizations to austral summer aircraft observations to test model behavior and examine the relative influence of processes that determine Nd in SO stratocumulus clouds. The model predicts Nd with little bias and a correlation coefficient of ∼0.7 compared with observations. Coalescence scavenging is found to be an important sink of CCN in both liquid and mixed‐phase precipitating stratocumulus and reduces the predicted Nd by as much as 90% depending on the precipitation rate. The free tropospheric aerosol source controls Nd more strongly than the surface aerosol source during austral summer.

Enhancement in free-tropospheric aerosol loading over India

Free-tropospheric aerosol loading and its changes assume importance as the diabatic heating due to radiation absorption by aerosols is more intense at higher altitudes. The present study quantifies trends in free-tropospheric aerosol loading over Indian landmass and examines the role of local production and long range transport, using multi-satellite observations and reanalysis data. Increasing trends in free-tropospheric aerosol abundance are seen over most of the regions in almost all the seasons. Strongest positive trend over the Indian landmass is seen in post-monsoon, with mean rate of increase in free-tropospheric aerosol optical depth (AODFree Troposphere) 0.063dec−1. While dust aerosol loading in the free-troposphere decreases, smoke aerosol concentration increases over the Indian landmass. While increase in columnar and free-tropospheric aerosol loading is seen over larger regions of the Indian landmass, including regions of northwest India, Indo Gangetic Plain (IGP), central India and southern peninsula, enhancement in aerosol production is observed mainly over the regions of northwest India in post-monsoon. Due to the prevailing westerly winds, aerosols over northwest India are transported through IGP to its central and eastern regions. Increase in aerosol production over northwest India and strengthening of updrafts over the central and eastern IGP lead to vertical uplift of more aerosols into the free-tropospheric altitudes. These free-tropospheric aerosols are subsequently transported, by the prevailing anti-cyclonic system, to the regions of central India and southern peninsula and cause the enhancement in free-tropospheric aerosol loading over these regions in post-monsoon. Though strengthening of updraft is observed over the regions of central India and southern Peninsula, net aerosol production is not seen to be increasing over these regions. The observed enhancement in free-tropospheric aerosols over Indian landmass is important as they can affect the thermal structure and stability of the atmosphere and modify the properties and distribution of clouds.

Global dispersal and potential sources of antibiotic resistance genes in atmospheric remote depositions.

Antibiotic resistance has become a major Global Health concern and a better understanding on the global spread mechanisms of antibiotic resistant bacteria (ARB) and intercontinental ARB exchange is needed. We measured atmospheric depositions of antibiotic resistance genes (ARGs) by quantitative (q)PCR in rain/snow collected fortnightly along 4 y. at a remote high mountain LTER (Long-Term Ecological Research) site located above the atmospheric boundary layer (free troposphere). Bacterial composition was characterized by 16S rRNA gene sequencing, and air mass provenances were determined by modelled back trajectories and rain/snow chemical composition. We hypothesize that the free troposphere may act as permanent reservoir and vector for ARB and ARGs global dispersal. We aimed to i) determine whether ARGs are long-range intercontinental and persistently dispersed through aerosols, ii) assess ARGs long-term atmospheric deposition dynamics in a remote high mountain area, and iii) unveil potential diffuse ARGs pollution sources. We showed that the ARGs sul1 (resistance to sulfonamides), tetO (resistance to tetracyclines), and intI1 (a proxy for horizontal gene transfer and anthropogenic pollution) were long-range and persistently dispersed in free troposphere aerosols. Major depositions of tetracyclines resistance matched with intensification of African dust outbreaks. Potential ARB mostly traced their origin back into agricultural soils. Our study unveils that air masses pathways are shaping ARGs intercontinental dispersal and global spread of antibiotic resistances, with potential predictability for interannual variability and remote deposition rates. Because climate regulates aerosolization and long-range air masses movement patterns, we call for a more careful evaluation of the connections between land use, climate change and ARB long-range intercontinental dispersal.

Undersizing of aged African biomass burning aerosol by an ultra-high-sensitivity aerosol spectrometer

Abstract. The ultra-high-sensitivity aerosol spectrometer (UHSAS) differs from most other optical particle spectrometers by using a high-power infrared (IR) laser to detect small particles and reduce the sizing ambiguity due to the non-monotonicity of scattering with particle size. During the NASA ORACLES project (ObseRvations of Aerosols above CLouds and their intEractionS) over the southeast Atlantic Ocean, the UHSAS clearly undersized particles in the biomass burning plume extending from southern Africa. Since the horizontal and vertical extent of the plume was vast, the NASA P-3B research aircraft often flew through a fairly uniform biomass burning plume for periods exceeding 30 min, sufficient time to explore the details of the UHSAS response by selecting single particle sizes with a differential mobility analyzer (DMA) and passing them to the UHSAS. This was essentially an in-flight calibration of the UHSAS using the particles of interest. Two modes of responses appeared. Most particles were undersized by moderate amounts, ranging from not at all for 70 nm aerosols to 15 % for 280 nm particles. Mie scattering calculations show that composition-dependent refractive index of the particles cannot explain the pattern. Heating of brown carbon or tarballs in the beam causing evaporation and shrinking of the particles is the most plausible explanation, though mis-sizing due to non-sphericity cannot be ruled out. A small fraction (10 %–30 %) of the particles were undersized by 25 % to 35 %. Those were apparently the particles containing refractory black carbon. Laboratory calibrations confirm that black carbon is drastically undersized by the UHSAS, because particles heat to their vaporization point and shrink. A simple empirical correction equation was implemented that dramatically improves agreement with DMA distributions between 100 and 500 nm. It raised the median particle diameter by 18 nm, from 163 to 181 nm, during the August 2017 deployment and by smaller amounts during deployments with less intense pollution. Calculated scattering from UHSAS size distributions increased by about 130 %, dramatically improving agreement with scattering measured by nephelometers. The correction is only valid in polluted instances; clean marine boundary layer and free troposphere aerosols behaved more like the calibration spheres. We were unable to directly test the correction between 500 and 1000 nm, though aerodynamic particle sizer (APS) data appear to show that the correction is poor at the largest diameters, which is no surprise as the composition of those particles is likely to be quite different than that of the accumulation mode. This adds to the evidence that UHSAS data must be treated cautiously whenever the aerosol may absorb infrared light. Similar corrections may be required whenever brown carbon aerosol is present.

Aerosol Composition, Mixing State, and Phase State of Free Tropospheric Particles and Their Role in Ice Cloud Formation

The prediction of ice cloud formation in the atmosphere remains challenging. Free tropospheric aerosols can act as ice nucleating particles, affecting cloud properties and precipitation. The physicochemical properties of free tropospheric particles are modified upon long-range transport by different atmospheric processes. These modifications affect the ice formation potential of individual particles. We investigated the physicochemical properties of free tropospheric particles collected at the remote Pico Mountain Observatory at 2225 m a.s.l. in the North Atlantic Ocean using multimodal micro-spectroscopy and chemical imaging techniques. We probed their ice nucleation (IN) activity using an IN stage interfaced with an environmental scanning electron microscope. Retroplume analysis, chemical imaging, and micro-spectroscopy analysis indicated that the size-resolved chemical composition, mixing state, and phase state of the particles with similar aging times but different transport patterns were substantially different. Relative humidity-dependent glass-transition temperatures estimated from meteorological conditions were consistent with the observed organic component of the particles’ phase. More viscous (solid and semi-solid-like) particles are more ice active in the deposition mode at temperatures ranging from 205 to 220 K than less viscous particles. This study provides a better understanding of the phase and mixing state of long-range transported free tropospheric aerosols and their role in ice cloud formation.

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

Abstract. 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.

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

Abstract. 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.

Cloud drop number concentrations over the western North Atlantic Ocean: seasonal cycle, aerosol interrelationships, and other influential factors.

Cloud drop number concentrations (Nd) over the western North Atlantic Ocean (WNAO) are generally highest during the winter (DJF) and lowest in summer (JJA), in contrast to aerosol proxy variables (aerosol optical depth, aerosol index, surface aerosol mass concentrations, surface cloud condensation nuclei (CCN) concentrations) that generally peak in spring (MAM) and JJA with minima in DJF. Using aircraft, satellite remote sensing, ground-based in situ measurement data, and reanalysis data, we characterize factors explaining the divergent seasonal cycles and furthermore probe into factors influencing Nd on seasonal timescales. The results can be summarized well by features most pronounced in DJF, including features associated with cold-air outbreak (CAO) conditions such as enhanced values of CAO index, planetary boundary layer height (PBLH), low-level liquid cloud fraction, and cloud-top height, in addition to winds aligned with continental outflow. Data sorted into high- and low-Nd days in each season, especially in DJF, revealed that all of these conditions were enhanced on the high-Nd days, including reduced sea level pressure and stronger wind speeds. Although aerosols may be more abundant in MAM and JJA, the conditions needed to activate those particles into cloud droplets are weaker than in colder months, which is demonstrated by calculations of the strongest (weakest) aerosol indirect effects in DJF (JJA) based on comparing Nd to perturbations in four different aerosol proxy variables (total and sulfate aerosol optical depth, aerosol index, surface mass concentration of sulfate). We used three machine learning models and up to 14 input variables to infer about most influential factors related to Nd for DJF and JJA, with the best performance obtained with gradient-boosted regression tree (GBRT) analysis. The model results indicated that cloud fraction was the most important input variable, followed by some combination (depending on season) of CAO index and surface mass concentrations of sulfate and organic carbon. Future work is recommended to further understand aspects uncovered here such as impacts of free tropospheric aerosol entrainment on clouds, degree of boundary layer coupling, wet scavenging, and giant CCN effects on aerosol–Nd relationships, updraft velocity, and vertical structure of cloud properties such as adiabaticity that impact the satellite estimation of Nd.

Altitude Aerosol Measurements in Central France: Seasonality, Sources and Free‐Troposphere/Boundary Layer Segregation

AbstractThe chemical composition of nonrefractory submicron aerosol particles was measured at the Puy‐de‐Dôme (PUY) station (1,465 m a.s.l) during 2015 using a Time‐of‐Flight Aerosol Chemical Speciation Monitor (ToF‐ACSM). These aerosol chemistry measurements are combined with online black carbon (BC) measurements to provide an overview of the submicron aerosol composition. Averaged over the entire year, and normalized to standard temperature and pressure, organic aerosol (OA) dominates the PM1 concentration during all seasons and within all air mass types (2.12 ± 1.73 µgm−3), and is responsible for summertime increases in aerosol concentration. Highest mass concentrations were measured during the summer, when air masses were arriving over mainland Europe and lowest in the winter months (when most air masses were of Atlantic origin). OA source apportionment was performed separately during each season, using the Source Finder (SoFi) interface for the multilinear engine. The PUY site, situated at 1,465 m a.s.l, although mainly sampling in the atmospheric boundary layer, it is sometimes sampling in the lower free troposphere (FT), providing the opportunity to identify the characteristics of FT aerosol. In order to accurately identify these sampling periods, the methodology described in Farah et al. (2018), during the same time period (2015/2016), was applied to the data. During this period, FT air masses are sampled approximately 20% of the time. This work provides, on one hand, a description of long‐term aerosol chemical properties at a remote regional site in central Europe and, on the other hand a characteristic chemical signature of FT aerosols over this region. This data can be used to improve our understanding of the transport and aging properties of aerosols at regional observation sites.

Changing patterns in aerosol vertical distribution over South and East Asia

Changing patterns in aerosol concentrations over the Asian region is well documented with a concurrent increase over India and a marked reduction over China. However, aerosol vertical distribution in the changing climate is not fully understood. By combining long-term satellite observations from MODIS and CALIOP, here we show rapid changes in the aerosol vertical distribution over the South and East Asia covering India and China. A statistically significant decreasing (increasing) trend in the boundary layer (free troposphere) aerosol concentrations is noticed over India. ERA-Interim reanalysis model suggests that this increase in free tropospheric aerosol concentrations are due to the lifting of boundary layer pollutants through an increase in convection (and vertical velocity) in a changing climate. In contrast, a consistent decreasing trend is observed over China irrespective of the altitude. Interestingly, a decreasing trend in Aerosol Optical Depth is observed over the northwest India and we relate this to an observed increase in precipitation leading to increase in the vegetation. It is also found that long-term oscillations like QBO, ENSO and solar cycle significantly affect the aerosol concentrations. Thus, it is prudent to conclude that background meteorology and dynamics play an important role in changing patterns of aerosol vertical distribution.

Biogenic particles formed in the Himalaya as an important source of free tropospheric aerosols

Aerosols of biogenic and anthropogenic origin affect the total radiative forcing of global climate. Poor knowledge of the pre-industrial aerosol concentration and composition, in particular of particles formed directly in the atmosphere from gaseous precursors, constitutes a large uncertainty in the anthropogenic radiative forcing. Investigations of new particle formation at pre-industrial-like conditions can contribute to the reduction of this uncertainty. Here we present observations taken at the remote Nepal Climate Observatory Pyramid station at 5,079 m above sea level, a few kilometres from the summit of Everest. We show that up-valley winds funnel gaseous aerosol precursors to higher altitudes. During this transport, these are oxidized into compounds of very low volatility, which rapidly form a large number of aerosol particles. These are then transported into the free troposphere, which suggests that the whole Himalayan region may act as an ‘aerosol factory’ and contribute substantially to the free tropospheric aerosol population. Aerosol production in this region occurs mainly via organic precursors of biogenic origin with little evidence of the involvement of anthropogenic pollutants. This process is therefore likely to be essentially unchanged since the pre-industrial period, and may have been one of the major sources that contributes to the upper tropospheric aerosol population during that time. Newly formed biogenic particles in the Himalaya increase free-tropospheric background aerosol concentration by a factor of up to two.