2014, Tao, J.C., Zhao, C.S., Ma, N., Liu, P.F.

Hygroscopic growth of aerosol particles can significantly affect their single-scattering albedo (ω), and consequently alters the aerosol effect on tropospheric photochemistry. In this study, the impact of aerosol hygroscopic growth on ω and its application to the NO2 photolysis rate coefficient (JNO2) are investigated for a typical aerosol particle population in the North China Plain (NCP). The variations of aerosol optical properties with relative humidity (RH) are calculated using a Mie theory aerosol optical model, on the basis of field measurements of number–size distribution and hygroscopic growth factor (at RH values above 90%) from the 2009 HaChi (Haze in China) project. Results demonstrate that ambient ω has pronouncedly different diurnal patterns from ω measured at dry state, and is highly sensitive to the ambient RHs. Ambient ω in the NCP can be described by a dry state ω value of 0.863, increasing with the RH following a characteristic RH dependence curve. A Monte Carlo simulation shows that the uncertainty of ω from the propagation of uncertainties in the input parameters decreases from 0.03 (at dry state) to 0.015 (RHs > 90%). The impact of hygroscopic growth on ω is further applied in the calculation of the radiative transfer process. Hygroscopic growth of the studied aerosol particle population generally inhibits the photolysis of NO2 at the ground level, whereas accelerates it above the moist planetary boundary layer. Compared with dry state, the calculated JNO2 at RH of 98% at the height of 1 km increases by 30.4%, because of the enhancement of ultraviolet radiation by the humidified scattering-dominant aerosol particles. The increase of JNO2 due to the aerosol hygroscopic growth above the upper boundary layer may affect the tropospheric photochemical processes and this needs to be taken into account in the atmospheric chemical models.

2011, Stock, M., Cheng, Y.F., Birmili, W., Massling, A., Wehner, B., Müller, T., Leinert, S., Kalivitis, N., Mihalopoulos, N., Wiedensohler, A.

This work examines the effect of direct radiative forcing of aerosols in the eastern Mediterranean troposphere as a function of air mass composition, particle size distribution and hygroscopicity, and relative humidity (RH). During intensive field measurements on the island of Crete, Greece, the hygroscopic properties of atmospheric particles were determined using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Hygroscopicity Differential Mobility Analyzer-Aerodynamic Particle Sizer (H-DMA-APS). Similar to former studies, the H-TDMA identified three hygroscopic sub-fractions of particles in the sub-μm range: a more hygroscopic group, a less hygroscopic group and a nearly hydrophobic particle group. The average hygroscopic particle growth factors at 90 % RH were a significant function of particle mobility diameter (Dp): 1.42 (± 0.05) at 30 nm compared to 1.63 (± 0.07) at 250 nm. The H-DMA-APS identified up to three hygroscopic sub-fractions at mobility diameters of 1.0 and 1.2 μm. The data recorded between 12 August and 20 October 2005 were classified into four distinct synoptic-scale air mass types distinguishing between different regions of origin (western Mediterranean vs. the Aegean Sea) as well as the degree of continental pollution (marine vs. continentally influenced). The hygroscopic properties of particles with diameter Dp≥150 nm showed the most pronounced dependency on air mass origin, with growth factors in marine air masses exceeding those in continentally influenced air masses. Particle size distributions and hygroscopic growth factors were used to calculate aerosol light scattering coefficients at ambient RH using a Mie model. A main result was the pronounced enhancement of particle scattering over the eastern Mediterranean due to hygroscopic growth, both in the marine and continentally influenced air masses. When RH reached its summer daytime values around 70–80 %, up to 50–70 % of the calculated visibility reduction was due to the hygroscopic growth of the particles by water compared to the effect of the dry particles alone. The estimated aerosol direct radiative forcings for both, marine and continentally influenced air masses were negative indicating a net cooling of the atmosphere due to the aerosol. The radiative forcing ΔFr was nevertheless governed by the total aerosol concentration most of the time: ΔFr was typically more negative for continentally influenced aerosols (ca. −4 W m−2) compared to rather clean marine aerosols (ca. −1.5 W m−2). When RH occasionally reached 90 % in marine air masses, ΔFr even reached values down to −7 W m−2. Our results emphasize, on the basis of explicit particle hygroscopicity measurements, the relevance of ambient RH for the radiative forcing of regional atmospheres.

2015, Denjean, C., Formenti, P., Picquet-Varrault, B., Pangui, E., Zapf, P., Katrib, Y., Giorio, C., Tapparo, A., Monod, A., Temime-Roussel, B., Decorse, P., Mangeney, C., Doussin, J.F.

Secondary organic aerosol (SOA) were generated from the ozonolysis of α-pinene in the CESAM (French acronym for Experimental Multiphasic Atmospheric Simulation Chamber) simulation chamber. The SOA formation and aging were studied by following their optical, hygroscopic and chemical properties. The optical properties were investigated by determining the particle complex refractive index (CRI). The hygroscopicity was quantified by measuring the effect of relative humidity (RH) on the particle size (size growth factor, GF) and on the scattering coefficient (scattering growth factor, f(RH)). The oxygen to carbon atomic ratios (O : C) of the particle surface and bulk were used as a sensitive parameter to correlate the changes in hygroscopic and optical properties of the SOA composition during their formation and aging in CESAM. The real CRI at 525 nm wavelength decreased from 1.43–1.60 (±0.02) to 1.32–1.38 (±0.02) during the SOA formation. The decrease in the real CRI correlated to the O : C decrease from 0.68 (±0.20) to 0.55 (±0.16). In contrast, the GF remained roughly constant over the reaction time, with values of 1.02–1.07 (±0.02) at 90% (±4.2%) RH. Simultaneous measurements of O : C of the particle surface revealed that the SOA was not composed of a homogeneous mixture, but contained less oxidised species at the surface which may limit water absorption. In addition, an apparent change in both mobility diameter and scattering coefficient with increasing RH from 0 to 30% was observed for SOA after 14 h of reaction. We postulate that this change could be due to a change in the viscosity of the SOA from a predominantly glassy state to a predominantly liquid state.