A reassessment of HO x South Pole chemistry based on observations recorded during ISCAT 2000

Reported here are modeling results based on ISCAT (Investigation of Sulfur Chemistry of Antarctic Troposphere) 2000 observations recorded at the South Pole (SP) during the Austral Summer of 2000. The observations included a comprehensive set of photochemical parameters, e.g., NO, O 3, and CO. It is worthy to note that not only were OH and HO 2 observed, but also HO x precursor species CH 2O, H 2O 2, and HONO were measured. Previous studies have suggested that HONO is the major source of OH/HO x in the Arctic; however, observed HONO levels at SP induced dramatic model overprediction of both HO x and NO x when used to constrain the model calculations. In contrast, model predictions constrained by observed values of CH 2O and H 2O 2 are consistent with the observations of OH and HO 2 (i.e., within 20%) for more than half of the data. Significant model overpredictions of OH, however, were seen at the NO levels lower than 50pptv or higher than 150pptv. An analysis of HO x budget at the median NO level suggests that snow emissions of H 2O 2 and CH 2O are the single most important primary source of SP HO x, contributing 46% to the total source. Major sinks for HO x are found to be dry deposition of HO 2NO 2 and HNO 3 as well as their reactions with OH. Although ISCAT 2000 led to a major progress in our understanding of SP HO x chemistry, critical aspects of this chemistry are still in need of further investigation. © 2004 Elsevier Ltd. All rights reserved