Relatively high concentrations
of preexisting particles, acting
as a condensation sink (CS) of gaseous precursors, have been thought
to suppress the occurrence of new particle formation (NPF) in urban
environments, yet NPF still occurs frequently. Here, we aim to understand
the factors promoting and inhibiting NPF events in urban Beijing by
combining one-year-long measurements of particle number size distributions
and PM
2.5
chemical composition. Our results show that indeed
the CS is an important factor controlling the occurrence of NPF events,
with its chemical composition affecting the efficiency of the background
particles in removing gaseous H
2
SO
4
(effectiveness
of the CS) driving NPF. During our observation period, the CS was
found to be more effective for ammonium nitrate-rich (NH
4
NO
3
-rich) fine particles. On non-NPF event days, particles
acting as CS contained a larger fraction of NH
4
NO
3
compared to NPF event days under comparable CS levels. In particular,
in the CS range from 0.02 to 0.03 s
–1
, the nitrate
fraction was 17% on NPF event days and 26% on non-NPF event days.
Overall, our results highlight the importance of considering the chemical
composition of preexisting particles when estimating the CS and their
role in inhibiting NPF events, especially in urban environments.
Abstract. Atmospheric new particle formation (NPF) events are regularly observed in urban Beijing, despite high concentrations of background particles which, based on theory, should inhibit NPF due to high values of coagulation sink (CoagS). The survival probability, which depends on both CoagS and particle growth rate (GR) is a key parameter in determining occurrence of NPF events, as it describes the fraction of newly formed particles that survive from a smaller diameter to a larger diameter. In this study, we investigate and compare survival probabilities from 1.5 to 3 nm (J3/J1.5), from 3 to 6 nm (J6/J3) and from 6 to 10 nm (J10/J6) based on analytical formulae, cluster population simulations, and atmospheric observations from Beijing. We find that survival probabilities based on the cluster population simulations and one of the analytical formulae are in a good agreement. However, at low ratios between the background condensation sink (CS) and GR, and at high concentrations of sub-3 nm clusters, cluster-cluster collisions efficiently lower survival probabilities in the cluster population simulations. Due to the large concentrations of clusters and small particles required to considerably affect the survival probabilities, we consider it unlikely that cluster-cluster collisions significantly affect atmospheric survival probabilities. The values of J10/J6 observed in Beijing show high variability, most likely due to influences of primary particle emissions, but are on average in a relatively good agreement with the values based on the simulations and the analytical formula. The observed values of J6/J3 are mostly lower than those predicted based on the simulations and the analytical formula, which could be explained by uncertainties in CS and GR. The observed values of J3/J1.5 at high CS/GR are much higher than predicted based on the simulations and the analytical formula. We argue that uncertainties in GR or CS are unlikely to solely explain the observed values of J3/J1.5 under high CS conditions. Thus, further work is needed to better understand the factors influencing survival probabilities of sub-3 nm atmospheric particles in polluted environments.
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