Nucleation and condensational growth to CCN sizes during a sustained pristine biogenic SOA event in a forested mountain valley

Abstract

The Whistler Aerosol and Cloud Study (WACS 2010), included intensive measurements of trace gases and particles at two sites on Whistler Mountain. Between 6–11 July 2010 there was a sustained high-pressure system over the region with cloud-free conditions and the highest temperatures of the study. During this period, the organic aerosol concentrations rose from <1 μg m⁻³ to &sim;6 μg m⁻³. Precursor gas and aerosol composition measurements show that these organics were almost entirely of secondary biogenic nature. Throughout 6–11 July, the anthropogenic influence was minimal with sulfate concentrations <0.2 μg m⁻³ and SO₂ mixing ratios &approx; 0.05–0.1 ppbv. Thus, this case provides excellent conditions to probe the role of biogenic secondary organic aerosol in aerosol microphysics. Although SO₂ mixing ratios were relatively low, box-model simulations show that nucleation and growth may be modeled accurately if <i>J</i>_nuc = 3 × 10^&minus;7[H₂SO₄] and the organics are treated as effectively non-volatile. Due to the low condensation sink and the fast condensation rate of organics, the nucleated particles grew rapidly (2–5 nm h^&minus;1) with a 10–25% probability of growing to CCN sizes (100 nm) in the first two days as opposed to being scavenged by coagulation with larger particles. The nucleated particles were observed to grow to &sim;200 nm after three days. Comparisons of size-distribution with CCN data show that particle hygroscopicity (&kappa;) was &sim;0.1 for particles larger 150 nm, but for smaller particles near 100 nm the κ value decreased near midway through the period from 0.17 to less than 0.06. In this environment of little anthropogenic influence and low SO₂, the rapid growth rates of the regionally nucleated particles – due to condensation of biogenic SOA – results in an unusually high efficiency of conversion of the nucleated particles to CCN. Consequently, despite the low SO₂, nucleation/growth appear to be the dominant source of particle number.