Assessing the sensitivity of the hydroxyl radical to model biases in composition and temperature using a single-column photochemical model for Lauder, New Zealand

作者：Lopez Comi Laura; Morgenstern Olaf; Zeng Guang; Masters Sarah L; Querel Richard R; Nedoluha Gerald E

来源：Atmospheric Chemistry and Physics, 2016, 16(22): 14599-14619.

DOI：10.5194/acp-16-14599-2016

We assess the major factors contributing to local biases in the hydroxyl radical (OH) as simulated by a global chemistry-climate model, using a single-column photochemical model (SCM) analysis. The SCM has been constructed to represent atmospheric chemistry at Lauder, New Zealand, which is representative of the background atmosphere of the Southern Hemisphere (SH) mid-latitudes. We use long-term observations of variables essential to tropospheric OH chemistry, i.e. ozone (O-3), water vapour (H2O), methane (CH4), carbon monoxide (CO), and temperature, and assess how using these measurements affect OH calculated in the SCM, relative to a reference simulation only using modelled fields. The analysis spans 1994 to 2010. Results show that OH responds approximately linearly to correcting biases in O-3; H2O; CO; CH4, and temperature. The biggest impact on OH is due to correcting an overestimation by approximately 20 to 60% of H2O, using radiosonde observations. Correcting this moist bias leads to a reduction of OH by around 5 to 35 %. This is followed by correcting predominantly overestimated O-3. In the troposphere, the model biases are mostly in the range of -10 to 30%. The impact of changing O-3 on OH is due to two pathways; the OH responses to both are of similar magnitude but different seasonality: correcting in situ tropospheric ozone leads to changes in OH in the range -14 to 4%, whereas correcting the photolysis rate of O-3 in accordance with overhead column ozone changes leads to increases of OH of 8 to 16%. The OH sensitivities to correcting CH4, CO, and temperature biases are all minor effects. The work demonstrates the feasibility of quantitatively assessing OH sensitivity to biases in longer-lived species, which can help explain differences in simulated OH between global chemistry models and relative to observations. In addition to clear-sky simulations, we have performed idealized sensitivity simulations to assess the impact of clouds (ice and liquid) on OH. The results indicate that the impacts on the ozone photolysis rate and OH are substantial, with a general decrease of OH below the clouds of up to 30% relative to the clear-skies situation, and an increase of up to 15% above. Using the SCM simulation we calculate recent OH trends at Lauder. For the period of 1994 to 2010, all trends are insignificant, in agreement with previous studies. For example, the trend in total-column OH is 0.5 +/- 1.3% over this period.

• 出版日期2016-11-23