Abstract. Aerosol nucleation is an important source of particle number in the atmosphere. However, in order to become cloud condensation nuclei (CCN), freshly nucleated particles must undergo significant condensational growth while avoiding coagulational scavenging. In an effort to quantify the contribution of nucleation to CCN, this work uses the GEOS-Chem-TOMAS global aerosol model to calculate changes in CCN concentrations against a broad range of nucleation rates and mechanisms. We then quantify the factors that control CCN formation from nucleation, including daily nucleation rates, growth rates, coagulation sinks, condensation sinks, survival probabilities, and CCN formation rates, in order to examine feedbacks that may limit growth of nucleated particles to CCN. Nucleation rate parameterizations tested in GEOS-Chem-TOMAS include ternary nucleation (with multiple tuning factors), activation nucleation (with two pre-factors), binary nucleation, and ion-mediated nucleation. We find that nucleation makes a significant contribution to boundary layer CCN(0.2 %), but this contribution is only modestly sensitive to the choice of nucleation scheme, ranging from 49 to 78 % increase in concentrations over a control simulation with no nucleation. Moreover, a two order-of-magnitude increase in the globally averaged nucleation rate (via changes to tuning factors) results in small changes (less than 10 %) to global CCN(0.2 %) concentrations. To explain this, we present a simple theory showing that survival probability has an exponentially decreasing dependence on the square of the condensation sink. This functional form stems from a negative correlation between condensation sink and growth rate and a positive correlation between condensation sink and coagulational scavenging. Conceptually, with a fixed condensable vapor budget (sulfuric acid and organics), any increase in CCN concentrations due to higher nucleation rates necessarily entails an increased aerosol surface area in the accumulation mode, resulting in a higher condensation sink, which lowers vapor concentrations and growth rates. As a result, slowly growing nuclei are exposed to a higher frequency of coagulational scavenging for a longer period of time, thus reducing their survival probabilities and closing a negative feedback loop that dampens the impact of nucleation on CCN. We confirm quantitatively that the decreases in survival probability predicted by GEOS-Chem-TOMAS due to higher nucleation rates are in accordance with this simple theory of survival probability.

Abstract. The flux of cosmic rays to the atmosphere has been reported to correlate with cloud and aerosol properties. One proposed mechanism for these correlations is the "ionaerosol clear-air" mechanism where the cosmic rays modulate atmospheric ion concentrations, ion-induced nucleation of aerosols and cloud condensation nuclei (CCN) concentrations. We use a global chemical transport model with online aerosol microphysics to explore the dependence of CCN concentrations on the cosmic-ray flux. Expanding upon previous work, we test the sensitivity of the cosmic-ray/CCN connection to several uncertain parameters in the model including primary emissions, Secondary Organic Aerosol (SOA) condensation and charge-enhanced condensational growth. The sensitivity of CCN to cosmic rays increases when simulations are run with decreased primary emissions, but show location-dependent behavior from increased amounts of secondary organic aerosol and charge-enhanced growth. For all test cases, the change in the concentration of particles larger than 80 nm between solar minimum (high cosmic ray flux) and solar maximum (low cosmic ray flux) simulations is less than 0.2 %. The change in the total number of particles larger than 10 nm was larger, but always less than 1 %. The simulated change in the column-integratedÅngström exponent was negligible for all test cases. Additionally, we test the predicted aerosol sensitivity to week-long Forbush decreases of cosmic rays and find that the maximum change in aerosol properties for these cases is similar to steady-state aerosol differences between the solar maximum and solar minimum. These results provide evidence that the effect of cosmic rays on CCN and clouds through the ion-aerosol clear-sky mechanism is limited by dampening from aerosol processes.

Recent research has shown that secondary organic aerosols (SOA) are major contributors to ultrafine particle growth to climatically relevant sizes, increasing global cloud condensation nuclei (CCN) concentrations within the continental boundary layer. However, there are three recent developments regarding the condensation of SOA that lead to uncertainties in the contribution of SOA to particle growth and CCN concentrations: (1) while many global models contain only biogenic sources of SOA (with annual production rates generally 10–30 Tg yr^-1), recent studies have shown that an additional source of SOA around 100 ^-1 correlated with anthropogenic carbon monoxide (CO) emissions may be required to match measurements. (2) Many models treat SOA solely as semivolatile, which leads to condensation of SOA proportional to the aerosol mass distribution; however, recent closure studies with field measurements show nucleation mode growth can be captured only if it is assumed that a significant fraction of SOA condenses proportional to the Fuchs aerosol surface area. This suggests a very low volatility of the condensing vapors. (3) Other recent studies of particle growth show that SOA condensation deviates from Fuchs surface-area condensation at sizes smaller than 10 nm and that size-dependent growth rate parameterizations (GRP) are needed to match measurements. We explore the significance of these three findings using GEOS-Chem-TOMAS global aerosol microphysics model and observations of aerosol size distributions around the globe. The change in the concentration of particles of size D_p > 40 nm (N40) within the BL assuming surface-area condensation compared to mass-distribution net condensation yielded a global increase of 11% but exceeded 100% in biogenically active regions. The percent change in N40 within the BL with the inclusion of the additional 100 Tg SOA yr^-1 compared to the base simulation solely with biogenic SOA emissions (19 Tg yr^-1) both using surface area condensation yielded a global increase of 13.7%, but exceeded 50% in regions with large CO emissions. The inclusion of two different GRPs in the additional-SOA case both yielded a global increase in N40 of <1%, however exceeded 5% in some locations in the most extreme case. All of the model simulations were compared to measured data obtained from diverse locations around the globe and the results confirmed a decrease in the model-measurement bias and improved slope for comparing modeled to measured CCN when non-volatile SOA was assumed and the extra SOA was included

Abstract. Aerosol nucleation is an important source of particle number in the atmosphere. However, in order to become cloud condensation nuclei (CCN), freshly nucleated particles must undergo significant condensational growth while avoiding coagulational scavenging. In an effort to quantify the contribution of nucleation to CCN, this work uses the GEOS-Chem-TOMAS global aerosol model to calculate changes in CCN concentrations against a broad range of nucleation rates and mechanisms. We then quantify the factors that control CCN formation from nucleation, including daily nucleation rates, growth rates, coagulation sinks, condensation sinks, survival probabilities, and CCN formation rates, in order to examine feedbacks that may limit growth of nucleated particles to CCN. Nucleation rate parameterizations tested in GEOS-Chem-TOMAS include ternary nucleation (with multiple tuning factors), activation nucleation (with two pre-factors), binary nucleation, and ion-mediated nucleation. We find that nucleation makes a significant contribution to boundary layer CCN0.2, but this contribution is only modestly sensitive to choice of nucleation scheme, ranging from 49–78% increase in concentrations over a control simulation with no nucleation. Moreover, a two order-of-magnitude increase in the globally averaged nucleation rate (via changes to tuning factors) results in small changes (less than 10%) to global CCN0.2 concentrations. To explain this, we present a simple theory showing that survival probability has an exponentially-decreasing dependence on the square of the condensation sink. This functional form stems from a negative correlation between condensation sink and growth rate and a positive correlation between condensation sink and coagulational scavenging. Conceptually, with a fixed condensable vapor budget (sulfuric acid and organics), any increase in CCN concentrations due to higher nucleation rates necessarily entails an increased aerosol surface area in the accumulation mode resulting in a higher condensation sink, which lowers vapor concentrations and growth rates. As a result, slowly growing nuclei are exposed to a higher frequency of coagulational scavenging for a longer period of time, thus reducing their survival probabilities, and closing a negative feedback loop that dampens the impact of nucleation on CCN. We confirm quantitatively that the decreases in survival probability predicted by GEOS-Chem-TOMAS due to higher nucleation rates are in accordance with this simple theory of survival probability.

The flux of cosmic rays to the atmosphere has been observed to correlate with cloud and aerosol properties. One proposed mechanism for these correlations is the "ion-aerosol clear-air" mechanism where the cosmic rays modulate atmospheric ion concentrations, ion-induced nucleation of aerosols and cloud condensation nuclei (CCN) concentrations. We use a global chemical transport model with online aerosol microphysics to explore the dependence of CCN concentrations on the cosmic-ray flux. Expanding upon previous work, we test the sensitivity of the cosmic-ray/CCN connection to several uncertain parameters in the model including primary emissions, Secondary Organic Aerosol (SOA) condensation and charge-enhanced condensational growth. The sensitivity of CCN to cosmic rays increases when simulations are run with decreased primary emissions, but show location-dependent behavior from increased amounts of secondary organic aerosol and charge-enhanced growth. For all test cases, the change in the concentration of particles larger than 80 nm between solar minimum (high cosmic ray flux) and solar maximum (low cosmic ray flux) simulations is less than 0.2%. The change in the total number of particles larger than 10 nm was larger, but always less than 1%. The simulated change in the column-integrated Ångström exponent was negligible for all test cases. Additionally, we test the predicted aerosol sensitivity to week-long Forbush decreases of cosmic rays and find that the maximum change in aerosol properties for these cases is similar to steady-state aerosol differences between the solar maximum and solar minimum. These results provide evidence that the effect of cosmic rays on CCN and clouds through the ion-aerosol clear-sky mechanism is limited by dampening from aerosol processes