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Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46 °C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L –1 . Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties. Ice nucleating particles impact the global climate by altering cloud formation and properties, but the sources of these emissions are not completely characterized. Here, the authors show that secondary organic aerosols formed from the oxidation of organic gases in the atmosphere can be a source of ice nucleating particles.

One pathway by which the oceans influence climate is via the emission of sea spray that may subsequently influence cloud properties. Sea spray emissions are known to be dependent on atmospheric and oceanic physicochemical parameters, but the potential role of ocean biology on sea spray fluxes remains poorly characterized. Here we show a consistent significant relationship between seawater nanophytoplankton cell abundances and sea-spray derived Cloud Condensation Nuclei (CCN) number fluxes, generated using water from three different oceanic regions. This sensitivity of CCN number fluxes to ocean biology is currently unaccounted for in climate models yet our measurements indicate that it influences fluxes by more than one order of magnitude over the range of phytoplankton investigated.

Internally mixed aerosol particles consisting of one or more hygroscopic compounds can contain both solid and liquid parts, the details depending on the relative humidity (RH). The solid‐to‐liquid transition of such particles as the RH increases influences their light‐scattering properties through changes in particle shape, size, and refractive index. Most techniques used to analyze ambient aerosol particles do not have the ability to view both solid and liquid phases within individual particles. Using a transmission electron microscope fitted with an environmental cell (ETEM), we analyzed laboratory‐prepared and ambient aerosol samples. Our results suggest that solid inclusions inside aqueous droplets at high RH values (e.g., >65%) are likely to be common in atmospheric particles. In order to assess the effects of such inclusions, we calculated their combined light‐scattering efficiencies using a discrete dipole approximation (DDA). The results show differences compared to those from a core‐shell model, with an average increase in light scattering of ∼20%. The results demonstrate that the combination of ETEM measurements of ambient particles with DDA calculations yields new insights into the effects of inclusions on the light‐scattering properties of internally mixed particles.

Hygroscopic aerosol particles change the magnitude of light scattering through condensation and evaporation of water vapor. We collected aerosol particles from two megacities and observed the particle shapes at various values of relative humidity (RH) using an environmental cell within a transmission electron microscope. Many Mexico City samples had sulfate particles that were embedded within weakly hygroscopic organic aerosol, whereas the Los Angeles samples mainly consisted of externally mixed sulfate particles. For the Mexico City samples, when the RH was increased in the microscope, only the sulfate parts deliquesced, but the entire particle did not become spherical, i.e., particles containing deliquescent phases do not necessarily become spherical upon deliquescence. This result conflicts with the assumption used in many models, i.e., that deliquesced particles become spherical. Using a discrete‐dipole approximation to calculate light scattering of simulated particles that resemble the observed ones, we show that, for particles >1.0 μm, the spherical‐shape assumption used in Mie theory underestimates the light scattering by ∼50%, with the exact value depending on the sizes and relative volumes of the constituent phases. Key Points Much pollution sulfate is embedded within weakly hygroscopic organic aerosol Not all internally mixed particles containing deliquesced salts are spherical Assuming sphericity for deliquesced particles can underestimate light scattering

Identifying how aerosol particles interact with atmospheric water is critical to understand climate and precipitation. Ice‐nucleating particles (INP) trigger the formation of atmospheric ice crystals at higher temperatures than pure water. They are difficult to characterize because of their scarce occurrence, and variability, in the atmosphere, especially at temperatures above −20°C. It has been demonstrated that at these temperatures, biological aerosol particles can contribute significantly to INP number concentration. This study incorporates a series of offline, size‐segregated measurements of INPs collected at the Puy de Dôme station (PUY, 1,465 m a.s.l.) over a 6 month period from October to May, covering the transitions from autumn, winter, to spring. These measurements show a general trend of decreasing particle number concentrations during the winter months and higher concentration during autumn and spring. INP concentrations measured in the range of −5 and −18°C, had concentrations of 0.001 INP/Lair at the warmest temperatures, and between 0.01 and 0.1 INP/Lair at the coldest temperatures. The majority of INP measured at temperatures warmer than −15°C were heat labile, suggesting a biological or organic origin. The INP variability was compared with collocated aerosol physical and chemical properties, allowing us to associate highest INP concentrations with local and marine origins. Following these comparisons, we use aerosol total number concentration to develop a new parameterization. In addition, this parameterization is specifically optimized for warmer temperature INP measurements, and demonstrated a good performance when tested on independent data sets. Plain Language Summary Understanding how tiny particles in the air (aerosol particles) interact with water in the atmosphere is crucial for studying climate and precipitation. Ice Nuclei Particles (INP) play a role in forming ice crystals in the atmosphere, especially at higher temperatures. This is important because it's been found that biological aerosol particles can significantly contribute to INP at temperatures above −20°C. The study conducted offline measurements of INPs over 6 months at the Puy de Dôme station, covering the transition from autumn to spring. Results showed a general trend of fewer particles during winter and more during autumn and spring. The INP concentrations were highest at temperatures between −5 and −18°C, with warmer temperatures having 0.001 INP per liter of air and colder temperatures having 0.01 to 0.1 INP per liter of air. Most INPs at temperatures above −15°C were heat‐sensitive, indicating a biological or organic origin. This study linked high INP concentrations to local and marine sources by comparing them with aerosol properties. A new parameterization based on total aerosol number concentration, specifically optimized for warmer temperatures, performed well when tested on independent data sets. Key Points Size‐segregated airborne ice‐nucleating particles (INP) concentrations were measured at an altitude station in Central France over 6 months Seasonal variations are observed with a minimum in winter. The majority of INPs is biological and activated above −18°C We developed a parameterization for predicting INP concentrations at warm temperatures based on total aerosol concentrations

Sea‐salt aerosol (SSA) particles affect the Earth's radiative balance and moderate heterogeneous chemistry in the marine boundary layer. Using conventional and environmental transmission electron microscopes (ETEM), we investigated the hygroscopic growth and liquid‐layer compositions of particles generated from three types of aqueous salt solutions: sodium chloride, laboratory‐synthesized seawater (S‐SSA particles), and natural seawater (N‐SSA particles). Three levels of morphological change were observed with the ETEM as the laboratory‐generated particles were exposed to increasing relative humidity (RH). The first level, onset of observable morphological changes, occurred on average at 70, 48, and 35% RH for the NaCl, S‐SSA, and N‐SSA particles, respectively. The second level, rounding, occurred at 74, 66, and 57% RH for NaCl, S‐SSA, and N‐SSA particles, respectively. The third level, complete deliquescence, occurred at 75% RH for all particles. Collected ambient SSA particles were also examined. With the exception of deliquescence, they did not exhibit the same hygroscopic characteristics as the NaCl particles. The ambient particles, however, behaved most similarly to the synthesized and natural SSA particles, although the onset of morphological change was slightly higher for the S‐SSA particles. We used energy‐dispersive X‐ray spectrometry to study the composition of the liquid layer formed on the S‐SSA and N‐SSA particles. The layer was enriched in Mg, S, and O relative to the solid particle core. An important implication of these results is that MgSO4‐enriched solutions on the surface of SSA particles may be the solvents of many heterogeneous reactions.

Background: Exposure to fine particulate air pollution is associated with increased cardiovascular morbidity and mortality. We previously demonstrated that exposure to dilute diesel exhaust causes vascular dysfunction in humans. Objectives: We conducted a study to determine whether exposure to ambient particulate matter causes vascular dysfunction. Methods: Twelve male patients with stable coronary heart disease and 12 age-matched volunteers were exposed to concentrated ambient fine and ultrafine particles (CAPs) or filtered air for 2 hr using a randomized, double-blind cross-over study design. We measured peripheral vascular vasomotor and fibrinolytic function, and inflammatory variables-including circulating leukocytes, serum C-reactive protein, and exhaled breath 8-isoprostane and nitrotyrosine-6-8 hr after both exposures. Results: Particulate concentrations (mean ± SE) in the exposure chamber $(190\\pm 37\\ \\mu {\\rm g}/{\\rm m}^{3})$ were higher than ambient levels $(31\\pm 8\\ \\mu {\\rm g}/{\\rm m}^{3})$ and levels in filtered air $(0.5\\pm 0.4\\ \\mu {\\rm g}/{\\rm m}^{3};p<0.001)$. Chemical analysis of CAPs identified low levels of elemental carbon. Exhaled breath 8-isoprostane concentrations increased after exposure to CAPs (16.9 ± 8.5 vs. 4.9 ± 1.2 pg/mL, p < 0.05), but markers of systemic inflammation were largely unchanged. Although there was a dose-dependent increase in blood flow and plasma tissue plasminogen activator release (p < 0.001 for all), CAPs exposure had no effect on vascular function in either group. Conclusions: Despite achieving marked increases in particulate matter, exposure to CAPs-low in combustion-derived particles-did not affect vasomotor or fibrinolytic function in either middle-aged healthy volunteers or patients with coronary heart disease. These findings contrast with previous exposures to dilute diesel exhaust and highlight the importance of particle composition in determining the vascular effects of particulate matter in humans.

Aerosol particles are important due to their direct and indirect impacts on climate. Within the planetary boundary layer (BL), these particles have a relatively short lifetime due to their frequent removal process by wet deposition. When aerosols are transported into the free troposphere (FT), their atmospheric lifetime increases significantly, making them representative of large spatial areas. In this work, we use a combination of in situ measurements performed at the high altitude PUY (Puy de Dôme, 45°46′ N, 2°57′ E, 1465 m a.s.l) station, together with LIDAR profiles at Clermont-Ferrand for characterizing FT conditions, and further characterize the physical properties of aerosol in this poorly documented area of the atmosphere. First, a combination of four criteria was used to identify whether the PUY station lies within the FT or within the BL. Results show that the PUY station is located in BL with frequencies ranging from 50% during the winter, up to 97% during the summer. Then, the classification is applied to a year-long dataset (2015) of particle size distribution data to study the differences in particle physical characteristics (size distribution) and black carbon (BC) concentrations between the FT and the BL. Although BC, Aitken, and the accumulation mode particles concentrations were higher in the BL than in the FT in winter and autumn, they were measured to be higher in the FT compared to BL in spring. No significant difference between the BL and the FT concentrations was observed for the nucleation mode particles for all seasons, suggesting a continuous additional source of nucleation mode particles in the FT during winter and autumn. Coarse mode particle concentrations were found higher in the FT than in the BL for all seasons and especially during summer. This indicates an efficient long-range transport of large particles in the FT from distant sources (marine and desert) due to higher wind speeds in the FT compared to BL. For FT air masses, we used 204-h air mass back-trajectories combined with boundary layer height estimations from ECMWF ERA-Interim to assess the time they spent in the FT since their last contact with the BL and to evaluate the impact of this parameter on the aerosol properties. We observed that even after 75 h without any contact with the BL, FT aerosols preserve specific properties of their air mass type.

This study presents in situ aircraft measurements of Saharan mineral dust transported over the western Mediterranean basin in June–July 2013 during the ChArMEx/ADRIMED (the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) airborne campaign. Dust events differing in terms of source region (Algeria, Tunisia and Morocco), time of transport (1–5 days) and height of transport were sampled. Mineral dust were transported above the marine boundary layer, which conversely was dominated by pollution and marine aerosols. The dust vertical structure was extremely variable and characterized by either a single layer or a more complex and stratified structure with layers originating from different source regions. Mixing of mineral dust with pollution particles was observed depending on the height of transport of the dust layers. Dust layers carried a higher concentration of pollution particles below 3 km above sea level (a.s.l.) than above 3 km a.s.l., resulting in a scattering Ångström exponent up to 2.2 below 3 km a.s.l. However, the optical properties of the dust plumes remained practically unchanged with respect to values previously measured over source regions, regardless of the altitude. Moderate absorption of light by the dust plumes was observed with values of aerosol single scattering albedo at 530 nm ranging from 0.90 to 1.00. Concurrent calculations from the aerosol chemical composition revealed a negligible contribution of pollution particles to the absorption properties of the dust plumes that was due to a low contribution of refractory black carbon in regards to the fraction of dust and sulfate particles. This suggests that, even in the presence of moderate pollution, likely a persistent feature in the Mediterranean, the optical properties of the dust plumes could be assumed similar to those of native dust in radiative transfer simulations, modelling studies and satellite retrievals over the Mediterranean. Measurements also showed that the coarse mode of mineral dust was conserved even after 5 days of transport in the Mediterranean, which contrasts with the gravitational depletion of large particles observed during the transport of dust plumes over the Atlantic. Simulations with the WRF mesoscale meteorological model highlighted a strong vertical turbulence within the dust layers that could prevent deposition of large particles during their atmospheric transport. This has important implications for the dust radiative effects due to surface dimming, atmospheric heating and cloud formation. The results presented here add to the observational data set necessary for evaluating the role of mineral dust on the regional climate and rainfall patterns in the western Mediterranean basin and understanding their atmospheric transport at global scale.

Future change in sea surface temperature may influence climate via various air–sea feedbacks and pathways. In this study, we investigate the influence of surface seawater biogeochemical composition on the temperature dependence of number-based sea spray emission fluxes. The dependence of sea spray fluxes was investigated in different water masses (i.e., subantarctic, subtropical and frontal bloom) with contrasting biogeochemical properties across a temperature range from ambient (13–18 ∘C) to 2 ∘C using seawater circulating in a plunging jet sea spray generator. We observed a significant increase in the sea spray total concentration at temperatures below 8 ∘C. Specifically, at 2 ∘C, there was an average 4-fold increase compared to the initial concentration at ambient temperatures. This temperature dependence was more pronounced for smaller-sized sea spray particles (i.e., nucleation and Aitken modes). Moreover, the temperature dependence varied based on the seawater type and its biogeochemical properties. While the sea spray flux at moderate temperatures (8–11 ∘C) was highest in frontal-bloom waters, the effect of low temperature on the sea spray flux was highest in subtropical seawaters. The temperature dependence of the sea spray flux was found to be inversely proportional to the abundance of the cyanobacterium Synechococcus in seawater. This relationship allows for parameterizing the temperature dependence of sea spray emission fluxes based on Synechococcus, which may be utilized in future modeling exercises.