Abstract
Abstract. A new methodology for the determination of the changes due to hygroscopic growth with relative humidity of the number size distribution and optical properties of polydispersed aerosols is described. This method uses the simulation chamber CESAM where the hygroscopic properties of polydispersed aerosol particles can be investigated in situ by exposing them to RH ranging from 0 to 100% for approximately 1 h. In situ humidification is used to provide simultaneous information on the RH-dependence of the particle size and the corresponding scattering coefficient (σscat), and that for the entire size distribution. Optical closure studies, based on integrated nephelometer and aethalometer measurements, Mie scattering calculations and measured particle size distributions, can therefore be performed to yield derived parameters such as the complex refractive index (CRI) at λ = 525 nm. The CRI can also be retrieved in the visible spectrum by combining differential mobility analyzer (DMA) and white light aerosol spectrometer (Palas Welas®) measurements. We have applied this methodology to ammonium sulfate particles, which have well known optical and hygroscopic properties. The CRI obtained from the two methods (1.54–1.57) compared favourably to each other and are also in reasonable agreement with the literature values. The particle's growth was compared to values obtained for one selected size of particles (150 nm) with a H-TDMA and the effect of the residence time for particles humidification was investigated. When the humidification was performed in the chamber for a few minutes, a continuous increase of the ammonium sulfate particle's size and σscat was observed from RH values as low as 30% RH. Comparison of the measured and modelled values based on Köhler and Mie theories shows that layers of water are adsorbed on ammonium sulfate particles below the deliquescence point. In contradiction, the particle's growth reported with H-TDMAs showed a prompt deliquescence of ammonium sulfate particles with no continuous growth in size at low RH. These findings highlight the need to allow sufficient time for particle-water vapour equilibrium in investigating the aerosols hygroscopic properties. H-TDMA instruments induce limited residence time for humidification and seem to be insufficient for water adsorption on ammonium sulfate particles.
Highlights
Atmospheric aerosols play an important role in the Earth’s climate by absorbing and scattering incoming solar radiation and outgoing terrestrial radiation (Haywood et al, 1998; Charlson et al, 1992; Forster et al, 2007), and by altering cloud properties by acting as cloud condensation nuclei (CCN) and thereby modifying cloud albedo, lifetime and precipitation (Hansen et al, 1997; Albrecht, 1989; Lohmann and Feichter, 2005).The ability of aerosols to interact with radiation is determined by their optical properties, strong functions both of particle size and chemical composition
We presented in this paper an optimized experimental set up to study, in situ and under controlled conditions close to those in the atmosphere, the hygroscopic behaviour of the size distribution and optical properties for polydispersed aerosols
This set up is based on the use of a high-volume atmospheric simulation chamber, CESAM, where water vapour and aerosols can be injected at various concentrations and kept at equilibrium for several minutes
Summary
Atmospheric aerosols play an important role in the Earth’s climate by absorbing and scattering incoming solar radiation and outgoing terrestrial radiation (direct effect) (Haywood et al, 1998; Charlson et al, 1992; Forster et al, 2007), and by altering cloud properties by acting as cloud condensation nuclei (CCN) and thereby modifying cloud albedo, lifetime and precipitation (indirect effect) (Hansen et al, 1997; Albrecht, 1989; Lohmann and Feichter, 2005). The ability of aerosols to interact with radiation is determined by their optical properties (single scattering albedo, asymmetry factor and efficiency of light extinction), strong functions both of particle size and chemical composition. The chemical composition determines the complex refractive index (CRI) (m = n + ik), which describes the scattering (real part n) and absorbing (imaginary part k) characteristics of a substance. The CRI is a major parameter to make the link between the instrinsic physic-chemical and the optical properties of aerosol particles.
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