Browsing by Author "Young, Edward D."
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Item Atmospheric species concentrations and reaction rates relevant to N2 chemistry derived from WACCM-X model used in Yeung et al., Extreme enrichment in atmospheric 15N15N. Sci. Adv. 3, eaao6741 (2017)(Rice University, 2017) Yeung, Laurence Y.; Young, Edward D.; Earth, Environmental, and Planetary SciencesItem Experimental and modeling data used in Yeung et al., Extreme enrichment in atmospheric 15N15N. Sci. Adv. 3, eaao6741 (2017)(Rice University, 2017) Yeung, Laurence Y.; Young, Edward D.; National Science Foundation; Deep Carbon Observatory, Department of Energy; Earth, Environmental, and Planetary SciencesItem Extreme enrichment in atmospheric 15N15N(AAAS, 2017) Yeung, Laurence Y.; Li, Shuning; Kohl, Issaku E.; Haslun, Joshua A.; Ostrom, Nathaniel E.; Hu, Huanting; Fischer, Tobias P.; Schauble, Edwin A.; Young, Edward D.Molecular nitrogen (N2) comprises three-quarters of Earth’s atmosphere and significant portions of other planetary atmospheres. We report a 19 per mil (‰) excess of 15N15N in air relative to a random distribution of nitrogen isotopes, an enrichment that is 10 times larger than what isotopic equilibration in the atmosphere allows. Biological experiments show that the main sources and sinks of N2 yield much smaller proportions of 15N15N in N2. Electrical discharge experiments, however, establish 15N15N excesses of up to +23‰. We argue that 15N15N accumulates in the atmosphere because of gas-phase chemistry in the thermosphere (>100 km altitude) on time scales comparable to those of biological cycling. The atmospheric 15N15N excess therefore reflects a planetary-scale balance of biogeochemical and atmospheric nitrogen chemistry, one that may also exist on other planets.Item In Situ Quantification of Biological N2 Production Using Naturally Occurring 15N15N(American Chemical Society, 2019) Yeung, Laurence Y.; Haslun, Joshua A.; Ostrom, Nathaniel E.; Sun, Tao; Young, Edward D.; van Kessel, Maartje A.H.J.; Lücker, Sebastian; Jetten, Mike S.M.We describe an approach for determining biological N2 production in soils based on the proportions of naturally occurring 15N15N in N2. Laboratory incubation experiments reveal that biological N2 production, whether by denitrification or anaerobic ammonia oxidation, yields proportions of 15N15N in N2 that are within 1‰ of that predicted for a random distribution of 15N and 14N atoms. This relatively invariant isotopic signature contrasts with that of the atmosphere, which has 15N15N proportions in excess of the random distribution by 19.1 ± 0.1‰. Depth profiles of gases in agricultural soils from the Kellogg Biological Station Long-Term Ecological Research site show biological N2 accumulation that accounts for up to 1.6% of the soil N2. One-dimensional reaction-diffusion modeling of these soil profiles suggests that subsurface N2 pulses leading to surface emission rates as low as 0.3 mmol N2 m–2 d–1 can be detected with current analytical precision, decoupled from N2O production.Item 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.