In this study, we quantified aerosol hygroscopicity parameter using aerosol microphysical observation data (κphy), analyzing monthly and seasonal trends in κphy by correlating it with aerosol chemical composition over 6 years from April 2007 to March 2013 at the Zeppelin Observatory in Svalbard, Arctic region. The monthly mean κphy value exhibited distinct seasonal variations, remaining high from winter to spring, reaching its minimum in summer, followed by an increase in fall, and maintaining elevated levels in winter. To verify the reliability of κphy, we employed the hygroscopicity parameter calculated from chemical composition data (κchem). The chemical composition and PM2.5 mass concentration required to calculate κchem was obtained through Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) reanalysis data and the calculation of κchem assumed that Arctic aerosols comprise only five species: black carbon (BC), organic matter (OM), ammonium sulfate (AS), sea salt aerosol less than a diameter of 2.5 μm (SSA2.5), and dust aerosol less than a diameter of 2.5 μm (Dust2.5). The κchem had no distinct correlation but had a similar seasonal trend compared to κphy. The κchem value followed a trend of SSA2.5 and was much higher by a factor of 1.6 ± 0.3 than κphy on average, due to a large proportion of SSA2.5 mass concentration in MERRA-2 reanalysis data. This may be due to the overestimation of sea salt aerosols in MERRA-2 reanalysis. The relationship between monthly mean κphy and the chemical composition used to calculate κchem was also analyzed. The elevated κphy from October to February resulted from the dominant influence of SSA2.5, while the maximum κphy in March was concurrently influenced by increasing AS and Dust2.5 associated with long-range transport from mid-latitude regions during Arctic haze periods and by SSA mass concentration obtained from in-situ sampling, which remained high from the preceding winter. The relatively low κphy from April to September can be attributed to low SSA2.5 and the dominance of organic compounds in the Arctic summer. Either natural sources such as those of marine and terrestrial biogenic origin or long-range-transported aerosols may contribute to the increase in organic aerosols in summer, potentially influencing the reduction in κphy of atmospheric aerosols. To our knowledge, this is the first study to analyze the monthly and seasonal variation of aerosol hygroscopicity calculated using long-term microphysical data, and this result provides evidence that changes in monthly and seasonal hygroscopicity variation occur depending on chemical composition.

The Italian Po Valley is one of the most polluted regions in Europe. During winter, meteorological conditions favor long and dense fogs, which strongly affect visibility and human health. In spring, the frequency of nighttime fogs reduces while daytime new particle formation events become more common. This transition is likely caused by a reduction in particulate matter (PM_2.5), leading to a decrease in the relevant condensation sink. The physics and chemistry of fog and aerosol have been studied at the San Pietro Capofiume site since the 1980s, but the detailed processes driving the observed trends are not fully understood. Hence, during winter and spring 2021/22, the Fog and Aerosol Interaction Research Italy (FAIRARI) campaign was carried out, using a wide spectrum of approaches, including in situ measurements, outdoor chamber experiments, and remote sensing. Atmospheric constituents and their properties were measured ranging from gas molecules and molecular clusters to fog droplets. One unique aspect of this study is the direct measurement of the aerosol composition inside and outside of fog, showing a slightly greater dominance of organic compounds in the interstitial compared to the droplet phase. Satellite observations of fog provided a spatial context and agreed well with in situ measurements of droplet size. They were complemented with in situ chamber experiments, providing insights into oxidative processes and revealing a large secondary organic aerosol-forming potential of ambient air upon chemical aging. The oxidative potential of aerosol and fog water inferred the impact of aerosol–fog interactions on particle toxicity.

The susceptibility of cloud droplet number to cloud condensation nuclei number is one of the major factors controlling the highly uncertain change in the amount of solar radiation reflected by clouds when aerosol emissions are perturbed (the radiative forcing due to aerosol–cloud interactions). We investigate this susceptibility in low-level stratiform clouds using long-term (3–10-yr) in situ observations of aerosols and clouds at three high-latitude locations. The in situ observations show higher susceptibility for low-level stratiform clouds than values reported for satellite data. We estimate −1.16 W m−2 for the aerosol indirect radiative forcing on the basis of our observations, which is at the higher end of satellite-derived forcing estimates and the uncertainty range of the most recent Intergovernmental Panel on Climate Change report. We evaluate four Earth system models against the observations and find large inter-model variability in the susceptibility. Our results demonstrate that, even if the susceptibility in some of the models is relatively close to observations, the underlying physics in the models is unrealistic when compared with observations. We show that the inter-model variability is driven by differences in sub-grid-scale updraught velocities and aerosol size distributions, raising a need to improve these aspects in models.

Ice nucleating particles (INPs) initiate ice formation, affecting the liquid versus ice distribution and radiative properties of clouds. INPs have been measured around the Arctic, but few INP concentration measurements have been reported for air during movement south out of central Arctic pack ice regions during cold air outbreaks (CAOs). We analyzed cases of transports connecting the Central Arctic location of the Multidisciplinary Drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition to the near sea ice edge in Svalbard and across ice-free ocean to the Cold-air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) site at Andenes, Norway, during the 2019–2020 Arctic winter. Aerosol surface area concentration measurements during CAOs indicate a switch from primarily accumulation mode at MOSAiC toward marine coarse mode (from sea spray emissions) at COMBLE. INP concentrations were independent of aerosol surface area or volume over the pack ice in MOSAiC in winter. At Svalbard, INPs related best to supermicron aerosol surface area and supermicron volume. At the COMBLE site, INPs related best with total aerosol surface area and total aerosol volume. In 5 of 6 case studies analyzed, INP concentrations increased in association with the transition to a dominance of sea spray aerosols. The INPs at COMBLE had a unique INP concentration mode near −18°C and higher ice nucleation active site densities (e.g., INPs per surface area) compared to those previously reported for other open ocean regions dominated by marine aerosols. While the INP sources in this case appear to be from oceanic emissions from shallower oceans under turbid water conditions, attribution solely to sea spray aerosols versus mixing down of free tropospheric aerosols by CAO clouds remains as a future topic. These studies provide a basis for parameterization of INPs for numerical modeling studies of CAO cloud systems.

The aerosol particles serving as 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 number 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 from Andenes at Svalbard. During CAO events at Andenes, the sea-spray-mode number concentration is correlated with 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 mean number concentration of particles that likely activated in-cloud is 109±61 cm-3 with no statistically significant difference from the non-CAO mean of 99±66 cm-3. For CAO trajectories between Zeppelin Observatory and Andenes, the upwind-to-downwind change in number concentration is the 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 number size distributions during CAO events provide guidance for evaluating CAO aerosol-cloud interaction processes in models.

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.

Black carbon (BC) is a major component of submicron 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, identifies its emission sources, and characterizes 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 Chacaltaya Global Atmosphere Watch 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.

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 (475ma.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 103 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.

Active vegetation fires in south-eastern (SE) Europe resulted in a notable increase in the number concentration of aerosols and cloud condensation nuclei (CCN) particles at two high latitude locations—the SMEAR IV station in Kuopio, Finland, and the Zeppelin Observatory in Svalbard, high Arctic. During the fire episode aerosol hygroscopicity κ slightly increased at SMEAR IV and at the Zeppelin Observatory κ decreased. Despite increased κ in high CCN conditions at SMEAR IV, the aerosol activation diameter increased due to the decreased supersaturation with an increase in aerosol loading. In addition, at SMEAR IV during the fire episode, in situ measured cloud droplet number concentration (CDNC) increased by a factor of ∼7 as compared to non-fire periods which was in good agreement with the satellite observations (MODIS, Terra). Results from this study show the importance of SE European fires for cloud properties and radiative forcing in high latitudes.

Atmospheric aerosol particles are essential for forming clouds and precipitation, thereby influencing Earth’s energy budget, water cycle and climate on regional and global scales. However, the origin of aerosol particles over the Amazon rainforest during the wet season is poorly understood. Earlier studies showed new particle formation in the outflow of deep convective clouds and suggested a downward flux of aerosol particles during precipitation events. Here we use comprehensive aerosol, trace gas and meteorological data from the Amazon Tall Tower Observatory to show that rainfall regularly induces bursts of nanoparticles in the nucleation size range. This can be attributed to rain-related scavenging of larger particles and a corresponding reduction of the condensation sink, along with an ozone injection into the forest canopy, which could increase the oxidation of biogenic volatile organic compounds, especially terpenes, and enhance new particle formation. During and after rainfall, the nucleation particle concentrations directly above the canopy are greater than those higher up. This gradient persists throughout the wet season for the nucleation size range, indicating continuous particle formation within the canopy, a net upward flux of newly formed particles and a paradigm shift in understanding aerosol–cloud–precipitation interactions in the Amazon. Particle bursts provide a plausible explanation for the formation of cloud condensation nuclei, leading to the local formation of green-ocean clouds and precipitation. Our findings suggest that an interplay of a rain-related reduction in the condensation sink, primary emissions of gases, mainly terpenes, and particles from the forest canopy, and convective cloud processing determines the population of cloud condensation nuclei in pristine rainforest air.