Browsing by Author "Murray, Lee T."

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    Clumped-Isotope Constraint on Upper-Tropospheric Cooling During the Last Glacial Maximum
    (Wiley, 2022) Banerjee, Asmita; Yeung, Laurence Y.; Murray, Lee T.; Tie, Xin; Tierney, Jessica E.; Legrande, Allegra N.
    Ice cores and other paleotemperature proxies, together with general circulation models, have provided information on past surface temperatures and the atmosphere's composition in different climates. Little is known, however, about past temperatures at high altitudes, which play a crucial role in Earth's radiative energy budget. Paleoclimate records at high-altitude sites are sparse, and the few that are available show poor agreement with climate model predictions. These disagreements could be due to insufficient spatial coverage, spatiotemporal biases, or model physics; new records that can mitigate or avoid these uncertainties are needed. Here, we constrain the change in upper-tropospheric temperature at the global scale during the Last Glacial Maximum (LGM) using the clumped-isotope composition of molecular oxygen trapped in polar ice cores. Aided by global three-dimensional chemical transport modeling, we exploit the intrinsic temperature sensitivity of the clumped-isotope composition of atmospheric oxygen to infer that the upper troposphere (effective mean altitude 10–11 km) was 6–9°C cooler during the LGM than during the late preindustrial Holocene. A complementary energy balance approach supports a minor or negligible steepening of atmospheric lapse rates during the LGM, which is consistent with a range of climate model simulations. Proxy-model disagreements with other high-altitude records may stem from inaccuracies in regional hydroclimate simulation, possibly related to land-atmosphere feedbacks.
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    Isotopic ordering in atmospheric O2 as a tracer of ozone photochemistry and the tropical atmosphere
    (Wiley, 2016) Yeung, Laurence Y.; Murray, Lee T.; Ash, Jeanine L.; Young, Edward D.; Boering, Kristie A.; Atlas, Elliot L.; Schauffler, Sue M.; Lueb, Richard A.; Langenfelds, Ray L.; Krummel, Paul. B.; Steele, L. Paul; Eastham, Sebastian D.
    The distribution of isotopes within O2 molecules can be rapidly altered when they react with atomic oxygen. This mechanism is globally important: while other contributions to the global budget of O2 impart isotopic signatures, the O(3P) + O2 reaction resets all such signatures in the atmosphere on subdecadal timescales. Consequently, the isotopic distribution within O2 is determined by O3 photochemistry and the circulation patterns that control where that photochemistry occurs. The variability of isotopic ordering in O2 has not been established, however. We present new measurements of 18O18O in air (reported as Δ36 values) from the surface to 33 km altitude. They confirm the basic features of the clumped-isotope budget of O2: Stratospheric air has higher Δ36 values than tropospheric air (i.e., more 18O18O), reflecting colder temperatures and fast photochemical cycling of O3. Lower Δ36 values in the troposphere arise from photochemistry at warmer temperatures balanced by the influx of high-Δ36 air from the stratosphere. These observations agree with predictions derived from the GEOS-Chem chemical transport model, which provides additional insight. We find a link between tropical circulation patterns and regions where Δ36 values are reset in the troposphere. The dynamics of these regions influences lapse rates, vertical and horizontal patterns of O2 reordering, and thus the isotopic distribution toward which O2 is driven in the troposphere. Temporal variations in Δ36 values at the surface should therefore reflect changes in tropospheric temperatures, photochemistry, and circulation. Our results suggest that the tropospheric O3 burden has remained within a ±10% range since 1978.
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    Tropospheric Ozone During the Last Interglacial
    (Wiley, 2022) Yan, Yuzhen; Banerjee, Asmita; Murray, Lee T.; Tie, Xin; Yeung, Laurence Y.
    The history of tropospheric O3, an important atmospheric oxidant, is poorly constrained because of uncertainties in its historical budget and a dearth of independent records. Here, we estimate the mean tropospheric O3 burden during the Last Interglacial period (LIG; 115 to 130 thousand years ago) using a record of the clumped isotopic composition of O2 (i.e., Δ36 values) preserved in Antarctic ice. The measured LIG Δ36 value is 0.03 ± 0.02‰ (95% CI) higher than the late pre-industrial Holocene (PI; 1,590–1,850 CE) value and corresponds to a modeled 9% reduction in LIG tropospheric O3 burden (95% CI: 3%–15%), caused in part by a substantial reduction in biomass burning emissions during the LIG relative to the PI. These results are consistent with the hypothesis that late-Pleistocene megafaunal extinctions caused woody and grassy fuels to accumulate on land, leading to enhanced biomass burning in the preindustrial Holocene.