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Abstract. Soot particles, acting as ice nucleating particles (INPs), can contribute to cirrus cloud formation, which has an important influence on climate. Aviation activities emitting soot particles into the upper troposphere can potentially impact ice nucleation (IN) in cirrus clouds. Pore condensation and freezing (PCF) is an important ice formation pathway for soot particles in the cirrus regime, which requires the soot INP to have specific morphological properties, i.e., mesopore structures. In this study, the morphology and pore size distribution of two kinds of soot samples were modified by a physical agitation method without any chemical modification by which more compacted soot sample aggregates could be produced compared to the unmodified sample. The IN activities of both fresh and compacted soot particles with different sizes, 60, 100, 200 and 400 nm, were systematically tested by the Horizontal Ice Nucleation Chamber (HINC) under mixed-phase and cirrus-cloud-relevant temperatures (T). Our results show that soot particles are unable to form ice crystals at T>235 K (homogeneous nucleation temperature, HNT), but IN is observed for compacted and larger-sized soot aggregates (>200 nm) well below the homogeneous freezing relative humidity (RHhom) for T< HNT, demonstrating PCF as the dominating mechanism for soot IN. We also observed that mechanically compacted soot particles can reach a higher particle activation fraction (AF) value for the same T and RH condition compared to the same aggregate size fresh soot particles. The results also reveal a clear size dependence for the IN activity of soot particles with the same degree of compaction, showing that compacted soot particles with large sizes (200 and 400 nm) are more active INPs and can convey the single importance of soot aggregate morphology for the IN ability. In order to understand the role of soot aggregate morphology for its IN activity, both fresh and compacted soot samples were characterized systematically using particle mass and size measurements, comparisons from TEM (transmission electron microscopy) images, soot porosity characteristics from argon (Ar) and nitrogen (N2) physisorption measurements, as well as soot–water interaction results from DVS (dynamic vapor sorption) measurements. Considering the soot particle physical properties along with its IN activities, the enhanced IN abilities of compacted soot particles are attributed to decreasing mesopore width and increasing mesopore occurrence probability due to the compaction process.

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. Two approaches are commonly used to simulate atmospheric aging processes in the laboratory. The experiments are either performed in large aerosol chambers (several m3) in order to achieve extended observation times or in small chambers (< 1 m3), compensating for the short observation times by elevated reactant concentrations. We present an experimental approach that enables long observation times at atmospherically relevant reactant concentrations in small chamber volumes by operating the aerosol chamber as a continuous-flow stirred tank reactor (CSTR). We developed a mathematical framework that allows the retrieval of data beyond calculating mean values, such as O3 exposure or equivalent atmospheric aging time, using the new metric, activation time (tact). This concept was developed and successfully tested to characterize the change in cloud condensation nuclei (CCN) activity of soot particles due to heterogeneous ozone oxidation. We found very good agreement between the experimental results and the theoretical predictions. This experimental approach and data analysis concept can be applied for the investigation of any transition in aerosol particles properties that can be considered a binary system. Furthermore, we show how tact can be applied to the analysis of data originating from other reactor types such as oxidation flow reactors (OFRs), which are widely used in atmospheric sciences. The new tact concept significantly supports the understanding of data acquired in OFRs, especially those from deviating experimental results in intercomparison campaigns.

&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;