Quantifying the sensitivity of aerosol optical properties to the parameterizations of physico-chemical processes during the 2010 Russian wildfires and heatwave

摘要

The impact of aerosol–radiation and aerosol–cloud interactions on the radiative forcing is subject to large uncertainties. This is caused by the limited understanding of aerosol optical properties and the role of aerosols as cloud condensation/ice nuclei (CCN/IN). On the other hand, aerosol optical properties and vertical distribution are highly related, and their uncertainties come from different processes. This work attempts to quantify the sensitivity of aerosol optical properties (i.e. aerosol optical depth; AOD) and their vertical distribution (using the extinction coefficient, backscatter coefficient, and concentrations' species profiles) to key processes. In order to achieve this objective, sensitivity tests have been carried out, using the WRF-Chem regional fully coupled model by modifying the dry deposition, sub-grid convective transport, relative humidity, and wet scavenging. The 2010 Russian heatwave–wildfires episode has been selected as case study. Results indicate that AOD is sensitive to these key processes in the following order of importance: (1)?modification of relative humidity, causing AOD differences of up to 0.6; (2)?modification of vertical convection transport with AOD differences around ?0.4; and (3)?the dry deposition with AOD absolute differences of up to ?0.35 and 0.3. Moreover, these AOD changes exhibit a nonlinear response. Both an increase and a decrease in the RH result in higher AOD values. On the other hand, both the increase and offset of the sub-grid convective transport lead to a reduction in the AOD over the fire area. In addition, a similar nonlinear response is found when reducing the dry deposition velocity; in particular, for the accumulation mode where the concentration of several species increases (while a decrease might be expected). These nonlinear responses are highly dependent on the equilibrium of the thermodynamics system sulfate–nitrate–SOA (secondary organic aerosol). In this sense, small changes in the concentration of one species can strongly affect others, finally affecting aerosol optical properties. Changes in this equilibrium could come from modifications in relative humidity, dry deposition, or vertical convective transport. By itself, dry deposition also presents a high uncertainty influencing the AOD representation.