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Mixed-phase clouds (MPCs) are key players in the Arctic climate system due to their role in modulating solar and terrestrial radiation. Such radiative interactions rely, among other factors, on the ice content of MPCs, which is regulated by the availability of ice-nucleating particles (INPs). While it appears that INPs are associated with the presence of primary biological aerosol particles (PBAPs) in the Arctic, the nuances of the processes and patterns of INPs and their association with clouds and moisture sources have not been resolved. Here, we investigated for a full year the abundance of and variability in fluorescent PBAPs (fPBAPs) within cloud residuals, directly sampled by a multiparameter bioaerosol spectrometer coupled to a ground-based counterflow virtual impactor inlet at the Zeppelin Observatory (475 m a.s.l.) in Ny-Ålesund, Svalbard. fPBAP concentrations (10 -3 –10 -2 L -1) and contributions to coarse-mode cloud residuals (0.1 to 1 in every 10 3 particles) were found to be close to those expected for high-temperature INPs. Transmission electron microscopy confirmed the presence of PBAPs, most likely bacteria, within one cloud residual sample. Seasonally, our results reveal an elevated presence of fPBAPs within cloud residuals in summer. Parallel water vapor isotope measurements point towards a link between summer clouds and regionally sourced air masses. Low-level MPCs were predominantly observed at the beginning and end of summer, and one explanation for their presence is the existence of high-temperature INPs. In this study, we present direct observational evidence that fPBAPs may play an important role in determining the phase of low-level Arctic clouds. These findings have potential implications for the future description of sources of ice nuclei given ongoing changes in the hydrological and biogeochemical cycles that will influence the PBAP flux in and towards the Arctic. [ABSTRACT FROM AUTHOR]

Clouds are crucial for Earth's climate and radiation budget. Great attention has been paid to low, high and vertically thick tropospheric clouds such as stratus, cirrus and deep convective clouds. However, much less is known about tropospheric mid-level clouds as these clouds are challenging to observe in situ and difficult to detect by remote sensing techniques. Here we use Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite observations to show that thin mid-level clouds (TMLCs) are ubiquitous in the tropics. Supported by high-resolution regional model simulations, we find that TMLCs are formed by detrainment from convective clouds near the zero-degree isotherm. Calculations using a radiative transfer model indicate that tropical TMLCs have a cooling effect on climate that could be as large in magnitude as the warming effect of cirrus. We conclude that more effort has to be made to understand TMLCs, as their influence on cloud feedbacks, heat and moisture transport, and climate sensitivity could be substantial.

Black carbon (BC) is a major component of sub-micron particulate matter (PM) with significant health and climate impacts. Many cities in emerging countries lack comprehensive knowledge about BC emissions and exposure levels. This study investigates BC concentration levels, identify its emission sources, and characterize the optical properties of BC at urban background sites of the two largest high-altitude Bolivian cities: La Paz (LP) (3600 m above sea level) and El Alto (EA) (4050 m a.s.l.) where atmospheric oxygen levels and intense radiation may affect BC production. The study relies on concurrent measurements of equivalent black carbon (eBC), elemental carbon (EC), and refractory black carbon (rBC), and their comparison with analogous data collected at the nearby Global Atmosphere Watch-Chacaltaya station (5240 m a.s.l). The performance of two independent source-apportionment techniques was compared: a bilinear model and a least squares multilinear regression (MLR). Maximum eBC concentrations were observed during the local dry season (LP: eBC=1.5±1.6 μg m-3; EA: 1.9±2.0 μg m-3). While eBC concentrations are lower at the mountain station, daily transport from urban areas is evident. Average mass absorption cross sections of 6.6-8.2 m2 g-1 were found in the urban area at 637 nm. Both source apportionment methods exhibited a reasonable level of agreement in the contribution of biomass burning (BB) to absorption. The MLR method allowed the estimation of the contribution and the source-specific optical properties for multiple sources including open waste burning. [ABSTRACT FROM AUTHOR]

The aerosol particles that provide cloud condensation and ice nuclei contribute to key cloud processes associated with cold-air outbreak (CAO) events but are poorly constrained in climate models due to sparse observations. Here we retrieve aerosol size distribution modes from measurements at Andenes, Norway during the Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) and at Zeppelin Observatory, approximately 1000 km upwind in Svalbard. During CAO events at Andenes, the sea spray mode number concentration is correlated to strong over-ocean winds with a mean of 8±4 cm-3 that is 71 % higher than during non-CAO conditions. Additionally during CAO events at Andenes, the mean Hoppel minimum diameter is 6 nm smaller than during non-CAO conditions though the estimated supersaturation is lower and the number concentration of particles that likely activated in-cloud is 109±61 cm-3 (similar to non-CAO conditions). For CAO trajectories between Zeppelin Observatory and Andenes, the upwind-to-downwind change in number concentration is largest for the accumulation mode with a mean decrease of 93±95 cm-3, likely attributable primarily to precipitation scavenging. These characteristic properties of aerosol size distributions during CAO events provide guidance for evaluating CAO aerosol-cloud interaction processes in models. [ABSTRACT FROM AUTHOR]

The chemical composition of PM 10 and non-overlapping PM 2.5 was studied at the summit of Mt. Chacaltaya (5380 m a.s.l., lat. - 16.346950°, long. - 68.128250°) providing a unique long-term record spanning from December 2011 to March 2020. The chemical composition of aerosol at the Chacaltaya Global Atmosphere Watch (GAW) site is representative of the regional background, seasonally affected by biomass burning practices and by nearby anthropogenic emissions from the metropolitan area of La Paz–El Alto. Concentration levels are clearly influenced by seasons with minima occurring during the wet season (December to March) and maxima occurring during the dry and transition seasons (April to November). Ions, total carbon (EC + OC), and saccharide interquartile ranges for concentrations are 558–1785, 384–1120, and 4.3–25.5 ng m -3 for bulk PM 10 and 917–2308, 519–1175, and 3.9–24.1 ng m -3 for PM 2.5 , respectively, with most of the aerosol seemingly present in the PM 2.5 fraction. Such concentrations are overall lower compared to other high-altitude stations around the globe but higher than Amazonian remote sites (except for OC). For PM 10 , there is dominance of insoluble mineral matter (33 %–56 % of the mass), organic matter (7 %–34 %), and secondary inorganic aerosol (15 %–26 %). Chemical composition profiles were identified for different origins: EC, NO 3- , NH 4+ , glucose, and C 2 O 42- for the nearby urban and rural areas; OC, EC, NO 3- , K + , acetate, formate, levoglucosan, and some F - and Br - for biomass burning; MeSO 3- , Na + , Mg 2+ , K + , and Ca 2+ for aged marine emissions from the Pacific Ocean; arabitol, mannitol, and glucose for biogenic emissions; Na + , Ca 2+ , Mg 2+ , and K + for soil dust; and SO 42- , F - , and some Cl - for volcanism. Regional biomass burning practices influence the soluble fraction of the aerosol between June and November. The organic fraction is present all year round and has both anthropogenic (biomass burning and other combustion sources) and natural (primary and secondary biogenic emissions) origins, with the OC/EC mass ratio being practically constant all year round (10.5 ± 5.7, IQR 8.1–13.3). Peruvian volcanism has dominated the SO 42- concentration since 2014, though it presents strong temporal variability due to the intermittence of the sources and seasonal changes in the transport patterns. These measurements represent some of the first long-term observations of aerosol chemical composition at a continental high-altitude site in the tropical Southern Hemisphere. [ABSTRACT FROM AUTHOR]

We investigated long-term changes using a harmonised 22-year data set of aerosol light absorption measurements, in conjunction with air mass history and aerosol source analysis. The measurements were performed at Zeppelin Observatory, Svalbard, from 2002 to 2023. We report a statistically significant decreasing long-term trend for the light absorption coefficient. However, the last 8 years of 2016–2023 showed a slight increase in the magnitude of the light absorption coefficient for the Arctic haze season. In addition, we observed an increasing trend in the single-scattering albedo from 2002 to 2023. Five distinct source regions, representing different transport pathways, were identified. The trends involving air masses from the five regions showed decreasing absorption coefficients, except for the air masses from Eurasia. We show that the changes in the occurrences of each transport pathway cannot explain the reductions in the absorption coefficient observed at the Zeppelin station. An increase in contributions of air masses from more marine regions, with lower absorption coefficients, is compensated for by an influence from high-emission regions. The proportion of air masses en route to Zeppelin, which have been influenced by active fires, has undergone a noticeable increase starting in 2015. However, this increase has not impacted the long-term trends in the concentration of light-absorbing aerosol. Along with aerosol optical properties, we also show an increasing trend in accumulated surface precipitation experienced by air masses en route to the Zeppelin Observatory. We argue that the increase in precipitation, as experienced by air masses arriving at the station, can explain a quarter of the long-term reduction in the light absorption coefficient. We emphasise that meteorological conditions en route to the Zeppelin Observatory are critical for understanding the observed trends. [ABSTRACT FROM AUTHOR]

Early growth of atmospheric particles is essential for their survival and ability to participate in cloud formation. Many different atmospheric vapors contribute to the growth, but even the main contributors still remain poorly identified in many environments, such as high-altitude sites. Based on measured organic vapor and sulfuric acid concentrations under ambient conditions, particle growth during new particle formation events was simulated and compared with the measured particle size distribution at the Chacaltaya Global Atmosphere Watch station in Bolivia (5240 m a.s.l.) during April and May 2018, as a part of the SALTENA (Southern Hemisphere high-ALTitude Experiment on particle Nucleation and growth) campaign. Despite the challenging topography and ambient conditions around the station, the simple particle growth model used in the study was able to show that the detected vapors were sufficient to explain the observed particle growth, although some discrepancies were found between modeled and measured particle growth rates. This study, one of the first of such studies conducted on high altitude, gives insight on the key factors affecting the particle growth on the site and helps to improve the understanding of important factors on high-altitude sites and the atmosphere in general. Low-volatility organic compounds originating from multiple surrounding sources such as the Amazonia and La Paz metropolitan area were found to be the main contributor to the particle growth, covering on average 65 % of the simulated particle mass in particles with a diameter of 30 nm. In addition, sulfuric acid made a major contribution to the particle growth, covering at maximum 37 % of the simulated particle mass in 30 nm particles during periods when volcanic activity was detected on the area, compared to around 1 % contribution on days without volcanic activity. This suggests that volcanic emissions can greatly enhance the particle growth. [ABSTRACT FROM AUTHOR]

New particle formation (NPF) in the tropical free troposphere (FT) is a globally important source of cloud condensation nuclei, affecting cloud properties and climate. Oxidized organic molecules (OOMs) produced from biogenic volatile organic compounds are believed to contribute to aerosol formation in the tropical FT, but without direct chemical observations. We performed in situ molecular-level OOMs measurements at the Bolivian station Chacaltaya at 5240 m above sea level, on the western edge of Amazonia. For the first time, we demonstrate the presence of OOMs, mainly with 4–5 carbon atoms, in both gas-phase and particle-phase (in terms of mass contribution) measurements in tropical FT air from Amazonia. These observations, combined with air mass history analyses, indicate that the observed OOMs are linked to isoprene emitted from the rainforests hundreds of kilometers away. Based on particle-phase measurements, we find that these compounds can contribute to NPF, at least the growth of newly formed nanoparticles, in the tropical FT on a continental scale. Thus, our study is a fundamental and significant step in understanding the aerosol formation process in the tropical FT. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is a short-lived climate forcer affecting the Arctic climate through multiple mechanisms, which vary substantially from winter to summer. Several models still fail in reproducing BC seasonal variability, limiting the ability to fully describe BC climate implications. This study aims at gaining insights into the mechanisms controlling BC transport from lower latitudes to the Arctic lower troposphere. Here we investigate the drivers controlling black carbon daily and seasonal variability in the Arctic using generalized additive models (GAMs). We analysed equivalent black carbon (eBC) concentrations measured at the Gruvebadet Atmospheric Laboratory (GAL – Svalbard archipelago) from March 2018 to December 2021. The eBC showed a marked seasonality with higher values in winter and early spring. The eBC concentration averaged 22 ± 20 ngm-3 in the cold season (November–April) and 11 ± 11 ngm-3 in the warm season (May–October). The seasonal and interannual variability was mainly modulated by the efficiency of wet scavenging removal during transport towards higher latitudes. Conversely, the short-term variability was controlled by boundary layer dynamics as well as local-scale and synoptic-scale circulation patterns. During both the cold and warm seasons, the transport of air masses from Europe and northern Russia was an effective pathway for the transport of pollution to the European Arctic. Finally, in the warm season we observed a link between the intrusion of warm air from lower latitudes and the increase in eBC concentration. Changes in the synoptic-scale circulation system and precipitation rate in the Northern Hemisphere, linked to climate change, are expected to modify the BC burden in the Arctic. [ABSTRACT FROM AUTHOR]

Mixed-phase clouds (MPC) are key players in the Arctic climate system due to their role in modulating solar and terrestrial radiation. Such radiative interactions critically rely on the ice content of MPC which, in turn, also depend on the availability of ice nucleating particles (INP). INP sources and concentrations are poorly understood in the Arctic. Recently, INP active at high temperatures were associated with the presence of primary biological aerosol particles (PBAP). Here, we investigated for a full year the abundance and variability of fluorescent PBAP (fPBAP) within cloud residuals, directly sampled by a multiparameter bioaerosol spectrometer coupled to a ground-based counterflow virtual impactor inlet at the Zeppelin Observatory (475 m asl), Ny-Ålesund, Svalbard. fPBAP concentrations (10-3–10-2 L-1) and contributions to coarse-mode aerosol (0.1 to 1 in every 103 particles) within cloud residuals were found to be close to those expected for concentrations of high-temperature INP. Transmission electron microscopy also confirmed the presence of fPBAP, most likely bacteria, within the cloud residual samples. Seasonally, our results reveal an elevated presence of fPBAP within cloud residuals in summer. Parallel water vapor isotope measurements point towards a link between summer clouds and regionally sourced air masses. Low-level MPC were predominantly observed at the beginning and end of summer, and one explanation for their presence is the existence of high-temperature INP. In this study, we present observational evidence that fPBAP may play an important role in determining the phase of low-level Arctic clouds. These findings have potential implications for the future description of sources of cloud condensation nuclei given ongoing changes in the hydrological and biogeochemical cycles that will influence the PBAP flux in and towards the Arctic. [ABSTRACT FROM AUTHOR]

The Arctic is one of the most rapidly warming regions of the globe. Low-level clouds and fog modify the energy transfer from and to space and play a key role in the observed strong Arctic surface warming, a phenomenon commonly termed "Arctic amplification". The response of low-level clouds to changing aerosol characteristics throughout the year is therefore an important driver of Arctic change that currently lacks sufficient constraints. As such, during the NASCENT campaign (Ny-Ålesund AeroSol Cloud ExperimeNT) extending over a full year from October 2019 to October 2020, microphysical properties of aerosols and clouds were studied at the Zeppelin station (475 m a.s.l.), Ny-Ålesund, Svalbard, Norway. Particle number size distributions obtained from differential mobility particle sizers as well as chemical composition derived from filter samples and an aerosol chemical speciation monitor were analyzed together with meteorological data, in particular vertical wind velocity. The results were used as input to a state-of-the-art cloud droplet formation parameterization to investigate the particle sizes that can activate to cloud droplets, the levels of supersaturation that can develop, the droplet susceptibility to aerosol and the role of vertical velocity. We evaluate the parameterization and the droplet numbers calculated through a droplet closure with in-cloud in situ measurements taken during nine flights over 4 d. A remarkable finding is that, for the clouds sampled in situ, closure is successful in mixed-phase cloud conditions regardless of the cloud glaciation fraction. This suggests that ice production through ice–ice collisions or droplet shattering may have explained the high ice fraction, as opposed to rime splintering that would have significantly reduced the cloud droplet number below levels predicted by warm-cloud activation theory. We also show that pristine-like conditions during fall led to clouds that formed over an aerosol-limited regime, with high levels of supersaturation (generally around 1 %, although highly variable) that activate particles smaller than 20 nm in diameter. Clouds formed in the same regime in late spring and summer, but aerosol activation diameters were much larger due to lower cloud supersaturations (ca. 0.5 %) that develop because of higher aerosol concentrations and lower vertical velocities. The contribution of new particle formation to cloud formation was therefore strongly limited, at least until these newly formed particles started growing. However, clouds forming during the Arctic haze period (winter and early spring) can be limited by updraft velocity, although rarely, with supersaturation levels dropping below 0.1 % and generally activating larger particles (20 to 200 nm), including pollution transported over a long range. The relationship between updraft velocity and the limiting cloud droplet number agrees with previous observations of various types of clouds worldwide, which supports the universality of this relationship. [ABSTRACT FROM AUTHOR]