14-CO in glacial ice from Law Dome, Antarctica as a tracer of changes in atmospheric OH abundance from 1870 AD to present

Abstract
Hydroxyl, OH, is the main tropospheric oxidant and determines the lifetime of methane and most other trace gases in the atmosphere, thereby controlling the amount of greenhouse warming produced by these gases. Changes in OH concentration ([OH]) in response to large changes in reactive trace gas emissions (which may occur in the future) are uncertain. Measurements of 14C containing carbon monoxide (14CO) and other tracers such as methyl chloroform over the last ≈25 years have been successfully used to monitor changes in average [OH], but there are no observational constraints on [OH] further back in time. Reconstructions of 14CO from ice cores could in principle provide such constraints but are complicated by in-situ production of 14CO by cosmic rays directly in the ice. Recent work in Antarctica and Greenland shows that this in-situ component would be relatively small and can be accurately corrected for at sites with very high snow accumulation rates. A joint US and Australian team sampled and measured firn air and ice at Law Dome, Antarctica (2018-19 season, site DE08-OH, 1.2 m a-1 ice-equivalent snow accumulation), to a maximum depth of 240 m. Trapped air was extracted from the ice using an onsite large-volume ice melting system. Preliminary comparisons of methane measured in the samples to existing ice core records and atmospheric measurements suggest ice core air sample ages spanning from the 1870s to the early 2000s. Firn-air samples from the snow surface to 81 m depth capture air from the early 2000s to present. Analyses of [CO] and halocarbons in the samples show a relatively low and stable procedural CO blank and demonstrate that the samples are unaffected by ambient air inclusion. 14CO analyses in these firn and ice core air samples have been successfully completed. Corrections for in-situ 14CO production, validated against direct atmospheric measurements for the more recent samples, have allowed us to develop a preliminary 14CO history. This history will be interpreted with the aid of the GEOS-Chem chemistry-transport model to place the first observational constraints on the variability of Southern Hemisphere [OH] since ≈1870 AD. © The Authors
Description
Keywords
Carbon 14, Glaciers, Antarctica, Gases, Controlled atmospheres, Greenhouse effect, Greenhouse gases, Carbon monoxide, Ice, Drill cores, Snow, Southern Hemisphere
Citation
Smith, A., Neff, P., Petrenko, V., Etheridge, D., Crosier, E., Hmiel, B., Thornton, D., Jong, L., Beaudette, R., Harth, C., Langenfelds, R., Mitrevski, B., Buizert, C. Murray, L., Trudinger, C., Dyonisius, M., Ng, J., Severinghaus, J. & Weiss, R. (2021). 14-CO in glacial ice from Law Dome, Antarctica as a tracer of changes in atmospheric OH abundance from 1870 AD to present. Paper presented to the 15th International Conference on Accelerator Mass Spectrometry, ANSTO, Sydney, Australia, November 15th – 19th. (pp. 23). Retrieved from: https://ams15sydney.com/wp-content/uploads/2021/11/AMS-15-Full-Program-and-Abstract-Book-R-1.pdf