Abstract

Abstract. Most prior field studies of new particle formation (NPF) have been performed at or near ground level, leaving many unanswered questions regarding the vertical extent of NPF. To address this, we measured concentrations of 11–16 nm diameter particles from ground level to 1000 m during the 2013 New Particle Formation Study at the Atmospheric Radiation Measurement Southern Great Plains site in Lamont, Oklahoma. The measurements were performed using a tethered balloon carrying two condensation particle counters that were configured for two different particle cut-off diameters. These observations were compared to data from three scanning mobility particle sizers at the ground level. We observed that 11–16 nm diameter particles were generated at the top region of the boundary layer, and were then rapidly mixed throughout the boundary layer. We also estimate liquid water content of nanoparticles using ground-based measurements of particle hygroscopicity obtained with a Humidified Tandem Differential Mobility Analyzer and vertically resolved relative humidity (RH) and temperature measured with a Raman lidar. Our analyses of these observations lead to the following conclusions regarding nanoparticles formed during NPF events at this site: (1) ground-based observations may not always accurately represent the timing, distribution, and meteorological conditions associated with the onset of NPF; (2) nanoparticles are highly hygroscopic and typically contain up to 50 % water by volume, and during conditions of high RH combined with high particle hygroscopicity, particles can be up to 95 % water by volume; (3) increased liquid water content of nanoparticles at high RH greatly enhances the partitioning of water-soluble species like organic acids into ambient nanoparticles.

Highlights

  • New particle formation (NPF) and growth are frequently observed in the atmosphere worldwide (Finlayson-Pitts and Pitts Jr., 2000; Kulmala et al, 2004; Seinfeld and Pandis, 2006; Zhang et al, 2011)

  • We measured vertical profiles of particle number concentrations in the size range of 11–16 nm with a tethered balloon system at the US Department of Energy Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) field site in Oklahoma. These observations were compared with simultaneous ground-based data obtained from three scanning mobility particle sizers to understand the vertical extent of new particle formation

  • We found that new particle formation was initiated at the top region of the boundary layer, and subsequently mixed downward to ground level in 0.5–1 h due to the strong vertical mixing on the NPF event day of 12 May 2013

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Summary

Introduction

New particle formation (NPF) and growth are frequently observed in the atmosphere worldwide (Finlayson-Pitts and Pitts Jr., 2000; Kulmala et al, 2004; Seinfeld and Pandis, 2006; Zhang et al, 2011). Sulfuric acid is often associated with the formation and growth of new particles (Weber et al, 1996, 1997, 2001; Stolzenburg et al, 2005; Kuang et al, 2008; Sipilä et al, 2010; Kulmala et al, 2013), but other species such as methanesulfonic acid Many observations of NPF have been performed on the ground (Kulmala et al, 2004), but some measurements suggest that nucleation can be altitude-dependent (Weber et al, 1999; Lee et al, 2003). Resolved measurements of NPF are needed to better understand the species involved in NPF and the underlying mechanisms, as well as adequately assess the impacts of NPF on cloud formation and climate

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