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.