Reply to the ‘Comment on “Enhancement in the production of nucleating clusters due to dimethylamine and large uncertainties in the thermochemistry of amine-enhanced nucleation”’ by Kupiainen-Maatta et al.

Abstract

We analyze the arguments of Kupiainen-Maatta et al. and show clearly that our study is free of ‘misrepresentations of earlier studies’ and that our conclusions are particularly well-justified. We demonstrate why and how the B3RICC2 (B3LYP/CBSB7//RI-CC2/aug-cc-pv(d+T)z) method criticized in our work overestimates the stability of sulfuric acid and sulfuric acid–base clusters compared to conventional DFT and ab initio methods and experimental data and fails to reproduce base dependencies of nucleation and cluster formation rates. We also show that the thermochemistry predicted by the conventional PW91PW91 method is consistent with experiments and can be used for simulations of atmospheric nucleation rates. We discuss uncertainties in simulations and experimental data and their impacts on conclusions about the nature of amine-enhanced nucleation and conclude that further high-resolution laboratory experiments, computational studies and measurements of atmospheric amine concentrations are needed in order to determine the extent, at which amines impact atmospheric nucleation.