The importance of ammonia for springtime atmospheric new particle formation and aerosol number abundance over the United States

New particle formation (NPF) and subsequent growth can contribute upwards of 50 % of the global cloud condensation nuclei (CCN) budget. It is also a significant source of ultrafine aerosols (PM0.1) with health implications. Ammonia (NH3) can play a significant role in enhancing NPF and contributing to the growth of nucleated particles. Understanding these processes are vital for air quality and climate. Here, we examine the role of NH3 in NPF and consequent effects on aerosol number concentrations (including CCN) and size distributions during springtime over the United States (US). We use the GEOS-Chem chemistry transport model coupled with the size-resolved Advanced Particle Microphysics (APM) Model. We also employ measurements of particle number size distributions, CN10 (condensation nuclei > 10 nm), CCN0.4 (CCN at 0.4 % supersaturation), and aerosol composition (SO4, NO3, NH4, Organics) at the Southern Great Plains site (SGP). The impact of NH3 in ion-mediated nucleation is the improved capturing of the occurrence of almost all springtime (March-April) NPF events observed at SGP during 2015-2020. Furthermore, this brings the magnitude and temporal variations of particle number concentrations in stronger agreement with observations; mean fractional bias for modeled CN10(CCN0.4) reducing from -1.26 to -0.27 (-0.75 to -0.54) and overall good-agreement ( divide FractionalBias divide < 0.6) improving from 8.5 to 54 % (31 to 42 %). The contribution of NH3 in new particle formation is important for springtime abundance of ultrafine aerosols (explaining 63 +/- 15 % of CN10) and CCN (16 +/- 10 % of CCN0.4) over the US. Our analysis shows that the deviation of CCN0.4 is strongly correlated with PM1-NH4+ deviations, suggesting the importance of improved model representation of ammonium for more accurate quantification of potential cloud forming particles.

Automated summary

This article examines the role of ammonia (NH3) in new particle formation (NPF) and its effects on aerosol number concentrations and size distributions during springtime in the United States. The study shows that NH3 contributes significantly to ion-mediated nucleation and improves the agreement between modeled and observed particle number concentrations. NH3 plays an important role in the abundance of ultrafine aerosols and cloud condensation nuclei (CCN) during springtime, explaining a considerable percentage of both.