The white-light humidified optical particle spectrometer (WHOPS) - a novel airborne system to characterize aerosol hygroscopicity

Abstract

Aerosol particles experience hygroscopic growth at enhanced relative humidity (RH), which leads to changes in their optical properties. We developed the white-light humidified optical particle spectrometer (WHOPS), a new instrument to investigate the particles' hygroscopic growth. Here we present a detailed technical description and characterization of the WHOPS in laboratory and field experiments. The WHOPS consists of a differential mobility analyzer, a humidifier/bypass and a white-light aerosol spectrometer (WELAS) connected in series to provide fast measurements of particle hygroscopicity at subsaturated RH and optical properties on airborne platforms. The WELAS employs a white-light source to minimize ambiguities in the optical particle sizing. In contrast to other hygroscopicity instruments, the WHOPS retrieves information of relatively large particles (i.e., diameter D > 280 nm), therefore investigating the more optically relevant size ranges. The effective index of refraction of the dry particles is retrieved from the optical diameter measured for size-selected aerosol samples with a well-defined dry mobility diameter. The data analysis approach for the optical sizing and retrieval of the index of refraction was extensively tested in laboratory experiments with polystyrene latex size standards and ammonium sulfate particles of different diameters. The hygroscopic growth factor (GF) distribution and aerosol mixing state is inferred from the optical size distribution measured for the size-selected and humidified aerosol sample. Laboratory experiments with pure ammonium sulfate particles revealed good agreement with Köhler theory (mean bias of ~3% and maximal deviation of 8% for GFs at RH = 95%). During first airborne measurements in the Netherlands, GFs (mean value of the GF distribution) at RH = 95% between 1.79 and 2.43 with a median of 2.02 were observed for particles with a dry diameter of 500 nm. This corresponds to hygroscopicity parameters (κ) between 0.25 and 0.75 with a median of 0.38. The GF distributions indicate externally mixed particles covering the whole range of GFs between ~1.0 and 3.0. On average, ~74% of the 500 nm particles had GFs > 1.5, ~15% had GF < 1.1 and the remaining ~1% showed values of 1.1 < GF < 1.5. The more hygroscopic mode sometimes peaked at GF > 2, indicating influence of sea-salt particles, consistent with previous ground-based particle hygroscopicity measurements in this area. The mean dry effective index of refraction for 500 nm particles was found to be rather constant with a value of 1.42 ± 0.04 (mean ± 1SD).