Abstract
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 (∣FractionalBias ∣ < 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.
Published Version
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Disclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.