Substantially positive contributions of new particle formation to Cloud Condensation Nuclei under low supersaturation in China based on numerical model improvements

Abstract. New particle formation (NPF) and subsequent particle growth are important sources of condensation nuclei (CN) and cloud condensation nuclei (CCN). While a number of observations have shown positive contributions of NPF to CCN at low supersaturation, negative NPF contributions were often simulated. Using the observations in a typical coastal city of Qingdao, we thoroughly evaluate the simulated number concentrations of CN and CCN using a NPF-explicit parameterization embedded in WRF-Chem model. In terms of CN, the initial simulation shows large biases of particle number concentrations at 10–40 nm (CN_10–40) and 40–100 nm (CN_40–100). By adjusting the process of gas-particle partitioning, including mass accommodation coefficient of sulfuric acid, the phase changes of primary organic aerosol emissions and the condensational amount of nitric acid, the concomitant improvement of the particle growth process yields a substantial reduction of overestimates of CN_10–40 and CN_40–100. Regarding CCN, SOA formed from the oxidation of semi-volatile and intermediate volatility organic vapors (SI-SOA) yield is an important contributor. In the original WRF-Chem model with 20 size bins setting, the yield of SI-SOA is too high without considering the differences in oxidation rates of the precursors. Lowering the SI-SOA yield results in much improved simulations of the observed CCN concentrations. On the basis of the bias-corrected model, we find substantial positive contributions of NPF to CCN at low supersaturation (~0.2 %) in Qingdao and over the broad areas of China, primarily due to the competing effects of increasing particle hygroscopicity surpassing that of particle size decrease. This study highlights the potentially much larger NPF contributions to CCN on a regional and even global basis.