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Cloud properties are strongly influenced by ice formation; hence, we need to understand the sources of ice-nucleating particles (INPs) around the globe. Boreal forests are known as sources of bioaerosol, and recent work indicates that these dominate the INP spectra above −24 °C. To quantify the INP population at temperatures below −24 °C, we deployed a portable cloud expansion chamber (PINE) in a Finnish boreal forest from 13 March 2018 to 11 May 2018. Using the 6 min time resolution PINE data, we present several lines of evidence that INPs below −24 °C in this location are also from biological sources: (i) an INP parameterization developed for a pine forest site in Colorado, where many INPs were shown to be biological, produced a good fit to our measurements; a moderate correlation of INPs with aerosol concentration larger than 0.5 µm and the fluorescent bioaerosol concentration; (ii) a negative correlation with relative humidity that may relate to enhanced release of bioaerosol at low humidity from local sources such as the prolific lichen population in boreal forests; and (iii) the absence of correlation with ultra-fine particles (3.5 to 50 nm), indicating that new particle formation events are not sources of INPs. This study should motivate further work to establish whether the commonality in bioaerosol ice-nucleating properties between spring in Finland and summer in Colorado is more generally applicable to different coniferous forest locations and times and also to determine to what extent these bioaerosols are transported to locations where they may affect clouds.

Ice crystal formation in mixed-phase clouds is initiated by specific aerosol particles, termed ice-nucleating particles (INPs). Only a tiny fraction of all aerosol particles are INPs, providing a challenge for contemporary INP measurement techniques. Models have shown that the presence of INPs in clouds can impact their radiative properties and induce precipitation formation. However, for a qualified implementation of INPs in models, measurement techniques able to accurately detect the temperature-dependent INP concentration are needed. Here we present measurements of INP concentrations in ambient air under conditions relevant to mixed-phase clouds from a total of 10 INP methods over 2 weeks in October 2018 at the Puy de Dôme observatory in central France. A special focus in this intercomparison campaign was placed on having overlapping sampling periods. Although a variety of different measurement principles were used, the majority of the data show INP concentrations within a factor of 5 of one another, demonstrating the suitability of the instruments to derive model-relevant INP data. Lower values of comparability are likely due to instrument-specific features such as aerosol lamina spreading in continuous-flow diffusion chambers, demonstrating the need to account for such phenomena when interpreting INP concentration data from online instruments. Moreover, consistently higher INP concentrations were observed from aerosol filters collected on the rooftop at the Puy de Dôme station without the use of an aerosol inlet.

Polar nephelometers provide in situ measurements of aerosol angular light scattering and play an essential role in validating numerically calculated phase functions or inversion algorithms used in space-borne and land-based aerosol remote sensing. In this study, we present a prototype of a new polar nephelometer called uNeph. The instrument is designed to measure the phase function, F11, and polarized phase function, -F12/F11, over the scattering range of around 5 to 175∘, with an angular resolution of 1∘ at a wavelength of 532 nm. In this work, we present details of the data processing procedures and instrument calibration approaches. uNeph was validated in a laboratory setting using monodisperse polystyrene latex (PSL) and di-ethyl-hexyl-sebacate (DEHS) aerosol particles over a variety of sizes ranging from 200 to 800 nm. An error model was developed, and the level of agreement between the uNeph measurements and Mie theory was found to be consistent within the uncertainties in the measurements and the uncertainties in the input parameters for the theoretical calculations. The estimated measurement errors were between 5 % and 10 % (relative) for F11 and smaller than ∼ 0.1 (absolute) for -F12/F11. Additionally, by applying the Generalized Retrieval of Aerosol and Surface Properties (GRASP) inversion algorithm to the measurements conducted with broad unimodal DEHS aerosol particles, the volume concentration, size distribution, and refractive index of the ensemble of aerosol particles were accurately retrieved. This paper demonstrates that the uNeph prototype can be used to conduct accurate measurements of aerosol phase function and polarized phase function and to retrieve aerosol properties through inversion algorithms.

The formation of ice particles in Earth's atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice-nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the low and mid latitudes. Although less is known about the sources of ice nucleation at high latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high-latitude boreal forests in the mixed-phase cloud regime. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiälä, Finland, between February and June 2018. The campaign utilized the infrastructure of the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, with additional INP instruments, including the Portable Ice Nucleation Chamber I and II (PINC and PINCii), the SPectrometer for Ice Nuclei (SPIN), the Portable Ice Nucleation Experiment (PINE), the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT) and the Microlitre Nucleation by Immersed Particle Instrument (µL-NIPI), used to quantify the INP concentrations and sources in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018, and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare measured INP concentrations to INP parameterizations, and we observe good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA.

Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C8−10 monomers and C18−20 dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5−7) and C15 compounds (C15H24O5−10) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J1.7 nm) and compared with previous studies, we found lower J1.7 nm values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.

The abundance of aerosol particles and their ability to catalyze ice nucleation are key parameters to correctly understand and describe the aerosol indirect effect on the climate. Cirrus clouds strongly influence the Earth's radiative budget, but their effect is highly sensitive to their formation mechanism, which is still poorly understood. Sulfate and organics are among the most abundant aerosol components in the troposphere and have also been found in cirrus ice crystal residuals. Most of the studies on ice nucleation at cirrus cloud conditions looked at either purely inorganic or purely organic particles. However, particles in the atmosphere are mostly found as internal mixtures, the ice nucleation ability of which is not yet fully characterized. In this study, we investigated the ice nucleation ability of internally mixed particles composed of crystalline ammonium sulfate (AS) and secondary organic material (SOM) at temperatures between −50 and −65 ∘C. The SOM was generated from the ozonolysis of α-pinene. The experiments were conducted in a large cloud chamber, which also allowed us to simulate various aging processes that the particles may experience during their transport in the atmosphere, like cloud cycling and redistribution of the organic matter. We found that the ice nucleation ability of the mixed AS / SOM particles is strongly dependent on the particle morphology. Small organic mass fractions of 5 wt %–8 wt % condensed on the surface of AS crystals are sufficient to completely suppress the ice nucleation ability of the inorganic component, suggesting that the organic coating is evenly distributed on the surface of the seed particles. In this case, the ice nucleation onset increased from a saturation ratio with respect to ice Sice∼1.30 for the pure AS crystals to ≥1.45 for the SOM-coated AS crystals. However, if such SOM-coated AS crystals are subjected to the mentioned aging processes, they show an improved ice nucleation ability with the ice nucleation onset at Sice∼1.35. We suggest that the aging processes change the particle morphology. The organic matter might redistribute on the surface to form a partially engulfed structure, where the ice-nucleation-active sites of the AS crystals are no longer completely masked by the organic coating, or the morphology of the organic coating layer might transform from a compact to a porous structure. Our results underline the complexity in representing the ice nucleation ability of internally mixed particles in cloud models. They also demonstrate the need to further investigate the impact of atmospheric aging and cloud processing on the morphology and related ice nucleation ability of internally mixed particles.

Ice-nucleating particles (INPs) trigger the formation of cloud ice crystals in the atmosphere. Therefore, they strongly influence cloud microphysical and optical properties and precipitation and the life cycle of clouds. Improving weather forecasting and climate projection requires an appropriate formulation of atmospheric INP concentrations. This remains challenging as the global INP distribution and variability depend on a variety of aerosol types and sources, and neither their short-term variability nor their long-term seasonal cycles are well covered by continuous measurements. Here, we provide the first year-long set of observations with a pronounced INP seasonal cycle in a boreal forest environment. Besides the observed seasonal cycle in INP concentrations with a minimum in wintertime and maxima in early and late summer, we also provide indications for a seasonal variation in the prevalent INP type. We show that the seasonal dependency of INP concentrations and prevalent INP types is most likely driven by the abundance of biogenic aerosol. As current parameterizations do not reproduce this variability, we suggest a new mechanistic description for boreal forest environments which considers the seasonal variation in INP concentrations. For this, we use the ambient air temperature measured close to the ground at 4.2 m height as a proxy for the season, which appears to affect the source strength of biogenic emissions and, thus, the INP abundance over the boreal forest. Furthermore, we provide new INP parameterizations based on the Ice Nucleation Active Surface Site (INAS) approach, which specifically describes the ice nucleation activity of boreal aerosols particles prevalent in different seasons. Our results characterize the boreal forest as an important but variable INP source and provide new perspectives to describe these new findings in atmospheric models.