Abstract. The largest contributors to the uncertainty in assessing the anthropogenic contribution in radiative forcing are the direct and indirect effects of aerosol particles on the Earth's radiative budget. Soot particles are of special interest since their properties can change significantly due to aging processes once they are emitted into the atmosphere. Probably the largest obstacle for the investigation of these processes in the laboratory is the long atmospheric lifetime of 1 week, requiring tailored experiments that cover this time span. This work presents results on the ability of two types of soot, obtained using a miniCAST soot generator, to act as cloud condensation nuclei (CCN) after exposure to atmospherically relevant levels of ozone (O3) and humidity. Aging times of up to 12 h were achieved by successful application of the continuous-flow stirred tank reactor (CSTR) concept while allowing for size selection of particles prior to the aging step. Particles of 100 nm diameter and rich in organic carbon (OC) that were initially CCN inactive showed significant CCN activity at supersaturations (SS) down to 0.3 % after 10 h of exposure to 200 ppb of O3. While this process was not affected by different levels of relative humidity in the range of 5 %–75 %, a high sensitivity towards the ambient/reaction temperature was observed. Soot particles with a lower OC content required an approximately 4-fold longer aging duration to show CCN activity at the same SS. Prior to the slow change in the CCN activity, a rapid increase in the particle diameter was detected which occurred within several minutes. This study highlights the applicability of the CSTR approach for the simulation of atmospheric aging processes, as aging durations beyond 12 h can be achieved in comparably small aerosol chamber volumes (<3 m3). Implementation of our measurement results in a global aerosol-climate model, ECHAM6.3-HAM2.3, showed a statistically significant increase in the regional and global CCN burden and cloud droplet number concentration.

Abstract. Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland at the Station for Measuring Ecosystem–Atmosphere Relations (SMEAR II) in the winter–spring of 2018. Measurements with the Portable Ice Nucleation Chamber (PINC) were conducted at 242 K and 105 % relative humidity with respect to water. The median INP number concentration [INP] during a 6-week measurement period was 13 L−1. The [INP] spanned 3 orders of magnitude and showed a general increase from mid-February until early April. No single dominant local or regional sources of INPs in the boreal environment of southern Finland could be identified. Rather, it is hypothesised that the INPs detected at SMEAR II are a result of long-range transport and dilution of INPs sourced far from the measurement site. Despite high variability, the measured [INP] values fall within the range expected for the [INP] measured elsewhere under similar thermodynamic conditions. The [INP] did not correlate with any of the examined parameters during the entire field campaign, indicating that no one single parameter can be used to predict the [INP] at the measurement location during the examined time period. The absence of a correlation across the entire field campaign also suggests that a variety of particles act as INPs at different times, although it was indirectly determined that ambient INPs are most likely within the size range of 0.1–0.5 µm in diameter on average. On shorter timescales, several particle species correlated well with the [INP]. Depending on the meteorological conditions, black carbon (BC), supermicron biological particles and sub-0.1 µm particles, most likely nanoscale biological fragments such as ice-nucleating macromolecules (INMs), correlated with the INP signal. However, an increase in the concentration of any of these particle species may not necessarily lead to the increase in the [INP]; the reasons for this remain unknown. Limitations of the instrumental set-up and the necessity for future field INP studies are addressed.

Abstract. Ice nucleating particle (INP) measurements were performed in the boreal environment of southern Finland at the Station for Measuring Ecosystem-Atmosphere Relations SMEAR II in the winter-spring of 2018. Measurements with the Portable Ice Nucleation Chamber (PINC) were conducted at 242 K and 105 % relative humidity with respect to water. The median INP number concentration [INP] during a six-week measurement period was found to be 13 L−1. [INP] spanned 3 orders of magnitude and showed a general increase from mid-February until early April. No persistent local or regional sources of INPs in the boreal environment of southern Finland could be identified. Rather, it is hypothesised that the INPs at SMEAR II are a result of dilution during long-range transport. Despite high variability, the measured [INP] values fall within the range expected for INP number concentrations measured elsewhere at similar thermodynamic conditions. [INP] did not correlate with any of the examined relevant parameters during the entire field campaign, indicating that no one single parameter can be used to predict the INP number concentration at the measurement location during the examined time period. The absence of correlation across the entire field campaign also suggests that a variety of particles are acting as INPs at different times, although it was indirectly determined that, on average, ambient INPs are most likely in the size range of 0.1–0.5 μm in diameter. On shorter time scales, several particle species correlated well with [INP] implying their potential role as INPs. Depending on the meteorological conditions, signatures of black carbon (BC), supermicron biological particles and sub-0.1 μm particles, most likely nanoscale biological fragments such as ice nucleating macromolecules (INMs), have been found in the INP signal. However, an increase in the concentration of any of these particle species may not necessarily lead to the increase in [INP], reasons for which remain unknown. Limitations of the instrumental setup and the necessity of the future field INP studies are addressed.

&lt;p&gt;&lt;strong&gt;Abstract.&lt;/strong&gt; The largest contributors to the uncertainty in assessing the anthropogenic contribution in radiative forcing are the direct and indirect effects of aerosol particles on the Earth's radiative budget. Soot particles are of special interest since their properties can change significantly due to aging processes once they are emitted to the atmosphere. Probably the largest obstacle for the investigation of these processes in the laboratory is the long atmospheric lifetime of one week, demanding tailored experiments that cover this time span. This work presents results on the ability of two types of soot to act as cloud condensation nuclei (CCN) after exposure to atmospherically relevant levels of ozone and humidity. Aging times of up to 12&amp;#8201;h were achieved by successful application of the continuous-flow stirred tank reactor (CSTR) concept while allowing for size-selection of particles prior to the aging step. 100&amp;#8201;nm particles rich in organic carbon (OC) that were initially CCN-inactive showed significant CCN-activity at supersaturations (SS) down to 0.3&amp;#8201;% after 10&amp;#8201;h of exposure to 200&amp;#8201;ppb of ozone. While this process was not affected by different levels of relative humidity in the range 5&amp;#8211;75&amp;#8201;%, a high sensitivity towards the ambient/reaction temperature was observed. Soot particles with a lower OC-content demanded an approximately four-fold longer aging duration to show CCN-activity for the same SS. Prior to the slow change in the CCN-activity, a rapid increase in the particle diameter was detected which occurred within several minutes. This study highlights the applicability of the CSTR-approach for the simulation of atmospheric aging processes, as aging durations beyond 12&amp;#8201;h can be achieved in comparably small aerosol chamber volumes (&lt;&amp;#8201;3&amp;#8201;m&lt;sup&gt;3&lt;/sup&gt;). Implementation of our measurement results on the CCN-activity of soot particles retrieved from measurements at atmospherically relevant conditions into a global aerosol-climate model showed a statistically significant increase in the regional and global CCN burden and cloud droplet number concentration (CDNC).&lt;/p&gt;

Abstract. 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.