Northern Hemisphere atmospheric history of carbon monoxide since preindustrial times reconstructed from multiple Greenland ice cores

• Published in: Climate of the Past
• Main Authors: Fain, Xavier, Rhodes, Rachael H., Place, Philip, Petrenko, Vasilii V., Fourteau, Kevin, Chellman, Nathan, Crosier, Edward, McConnell, Joseph R., Brook, Edward J., Blunier, Thomas, Legrand, Michel, Chappellaz, Jerome
• Format: Article in Journal/Newspaper
• Language: English
• Published: 2022
• Subjects: RECORD; EMISSIONS; CHEMISTRY; 20TH-CENTURY; AEROSOLS; MODELS; RATIOS; Greenland; Greenland ice cores; ice core; Ice Sheet
• Online Access: https://curis.ku.dk/portal/da/publications/northern-hemisphere-atmospheric-history-of-carbon-monoxide-since-preindustrial-times-reconstructed-from-multiple-greenland-ice-cores(ecd96736-7870-40c1-a444-a81bd3c3323c).html; https://doi.org/10.5194/cp-18-631-2022; https://curis.ku.dk/ws/files/303443765/cp_18_631_2022.pdf

Carbon monoxide (CO) is a regulated pollutant and one of the key components determining the oxidizing capacity of the atmosphere. Obtaining a reliable record of atmospheric CO mixing ratios ([CO]) since preindustrial times is necessary to evaluate climate-chemistry models under conditions different from today and to constrain past CO sources. We present high-resolution measurements of CO mixing ratios from ice cores drilled at five different sites on the Greenland ice sheet that experience a range of snow accumulation rates, mean surface temperatures, and different chemical compositions. An optical-feedback cavity-enhanced absorption spectrometer (OF-CEAS) was coupled with continuous melter systems and operated during four analytical campaigns conducted between 2013 and 2019. Overall, continuous flow analysis (CFA) of CO was carried out on over 700 m of ice. The CFA-based CO measurements exhibit excellent external precision (ranging from 3.3 to 6.6 ppbv, 1 sigma) and achieve consistently low blanks (ranging from 4.1 +/- 1.2 to 12.6 +/- 4.4 ppbv), enabling paleoatmospheric interpretations. However, the five CO records all exhibit variability that is too large and rapid to reflect past atmospheric mixing ratio changes. Complementary tests conducted on discrete ice samples demonstrate that these variations are not artifacts of the analytical method (i.e., production of CO from organics in the ice during melting) but are very likely related to in situ CO production within the ice before analysis. Evaluation of the signal resolution and co-investigation of high-resolution records of CO and total organic carbon (TOC) suggest that past atmospheric CO variations can be extracted from the records' baselines with accumulation rates higher than 20 cm w.e. yr(-1) (water equivalent per year). Consistent baseline CO records from four Greenland sites are combined to produce a multisite average ice core reconstruction of past atmospheric CO for the Northern Hemisphere high latitudes, covering the period from 1700 to 1957 CE. ...