Measurement report: Spectral and statistical analysis of aerosol hygroscopic growth from multi-wavelength lidar measurements in Barcelona, Spain.

This paper presents the estimation of the hygroscopic growth parameter of atmospheric aerosols retrieved with a multi-wavelength lidar, a micro-pulse lidar (MPL) and daily radiosoundings in the coastal region of Barcelona, Spain. The hygroscopic growth parameter, γ , parameterizes the magnitude of the scattering enhancement in terms of the backscatter coefficient following Hänel parameterization. After searching for time-colocated lidar and radiosounding measurements (performed twice a day, all year round at 00:00 and 12:00 UTC), a strict criterion-based procedure (limiting the variations of magnitudes such as water vapor mixing ratio (WMVR), potential temperature, wind speed and direction) is applied to select only cases of aerosol hygroscopic growth. A spectral analysis (at the wavelengths of 355, 532 and 1064 nm) is performed with the multi-wavelength lidar, and a climatological one, at the wavelength of 532 nm, with the database of both lidars. The spectral analysis shows that below 2 km the regime of local pollution and sea salt γ decreases with increasing wavelengths. Since the 355 nm wavelength is sensitive to smaller aerosols, this behavior could indicate slightly more hygroscopic aerosols present at smaller size ranges. Above 2 km (the regime of regional pollution and residual sea salt) the values of γ at 532 nm are nearly the same as those below 2 km, and its spectral behavior is flat. This analysis and others from the literature are put together in a table presenting, for the first time, a spectral analysis of the hygroscopic growth parameter of a large variety of atmospheric aerosol hygroscopicities ranging from low (pure mineral dust, γ <0.2) to high (pure sea salt, γ > 1.0) hygroscopicity. The climatological analysis shows that, at 532 nm, γ is rather constant all year round and has a large monthly standard deviation, suggesting the presence of aerosols with different hygroscopic properties all year round. The annual γ is 0.55 ± 0.23. The height of the layer where hygroscopic growth was calculated shows an annual cycle with a maximum in summer and a minimum in winter. Former works describing the presence of recirculation layers of pollutants injected at various heights above the planetary boundary layer (PBL) may explain why γ , unlike the height of the layer where hygroscopic growth was calculated, is not season-dependent. The subcategorization of the whole database into No cloud and Below-cloud cases reveals a large difference of γ in autumn between both categories (0.71 and 0.33, respectively), possibly attributed to a depletion of inorganics at the point of activation into cloud condensation nuclei (CCN) in the Below-cloud cases. Our work calls for more in situ measurements to synergetically complete such studies based on remote sensing. [ABSTRACT FROM AUTHOR]

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