A study of long-range transported smoke aerosols in the Upper Troposphere/Lower Stratosphere

Abstract. Long-range transported smoke aerosols in the UTLS (Upper Troposphere/Lower Stratosphere) over Europe were detected in Summer 2017. The measurements of ground-based instruments and satellite sensors indicate that the UTLS aerosol layers were originated from Canadian wildfires and were transported to Europe by UTLS advection. In this study, the observations of two multi-wavelength Raman Lidar systems in northern France (Lille and Palaiseau) are used to derive aerosol properties, such as optical depth of the UTLS layer, Lidar ratios at 355 and 532 nm and particle linear depolarization ratios at 355, 532 and 1064 nm. The optical depth of the UTLS layers at 532 nm varies from 0.05 to above 0.20, with very weak spectral dependence between 355 and 532 nm. Lidar ratios at 355 nm are in 31 ± 15 sr to 45 ± 9 sr range and at 532 nm, the Lidar ratios are in the range of 54 ± 12 sr to 58 ± 9 sr. Such spectral dependence of Lidar ratio is known to be a characteristic feature of aged smoke. The typical particle depolarization ratios in the UTLS smoke layer are 25 ± 4 % at 355 nm, 19 ± 3 % at 532 nm and 4.5 ± 0.8 % at 1064 nm. The relatively high depolarization ratios and such spectral dependence are an indication of a complicated morphology of aged smoke particles. We found an increase of depolarization ratio versus transport time. The depolarization ratio at 532 nm increases from below 2–5 % for fresh smoke to over 20 % for smoke aged more than 20 days. The 3 β + 2 α observations of two cases at Palaiseau and Lille sites were inverted to the aerosol microphysical properties using regularization algorithm. The particles distribute in the 0.1–1.0 μm range with effective radius of 0.33 ± 0.10 μm for both cases. The derived complex refractive indices are 1.52 (± 0.05) + i 0.021 (± 0.010) and 1.55 (± 0.05) + i 0.028 (± 0.014) for Palaiseau and Lille data. The retrieved aerosol properties were used to calculate the direct radiative forcing (DRF) effect specific to the UTLS aerosol layers. The simulations derive daily net DRF efficiency of −79.6 W m −2 τ −1 at the bottom of the atmosphere for Lille observations. At the top of the atmosphere, the net DRF efficiency is −7.9 W m −2 τ −1 . The results indicate that the UTLS aerosols strongly reduce the radiation reaching the terrestrial surface by absorption. The heating rate of the UTLS layers is estimated to be 3.7 K day −1 . The inversion of Palaiseau data leads to similar results. The heating rate predicts a temperature increase within the UTLS aerosol layer, which has been observed by the radiosonde temperature measurements.