Radiation-transfer modeling of snow-pack photochemical processes during ALERT 2000

The delta-Eddington radiation transfer model is used to calculate actinic fluxes and photolysis rates within the snow pack during the ALERT 2000 field campaign. Actinic fluxes are enhanced within the snow pack due to the high albedo of snow and conversion of direct light to diffuse light. The conversion of direct to diffuse light is highly dependent on the solar zenith angle, as demonstrated by model calculations. The optical properties of Alert snow are modeled as 100 pm radius ice spheres with impurity added to increase the absorption coefficient over that of pure water ice. Using these optical properties, the model achieves good agreement with observations of irradiance within the snow pack. The model is used to calculate the total actinic flux as a function of solar zenith angle and depth for either clear sky or cloudy conditions. The actinic flux is then used to calculate photochemical production of nitrogen oxides from nitrate photolysis assuming that nitrate in snow has the same absorption cross section and quantum yield in snow as in aqueous solution. Assuming all photo-produced nitrogen oxides are released to the gas phase, we derive a maximal flux of nitrogen oxides (NOx + HONO and possibly other products) from the snow pack. The value of this maximal flux depends critically on the assumed quantum yield for production of NO2, which is unknown in ice. Depending on the assumed quantum yield, the calculated maximal flux varies between values four times smaller than the observed NOx + HONO flux to five times larger than the NOx + HONO flux. Therefore, it appears that the calculated flux is in approximate agreement with the observations with a great need for improved understanding of nitrogen photochemistry in snow. (C) 2002 Elsevier Science Ltd. All rights reserved.