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• W4283323739 endingPage "87" @default.
• W4283323739 startingPage "78" @default.
• W4283323739 abstract "Air-water gas transfer largely influences the geochemical and biogeochemical cycles of essential atmospheric components (e.g. O 2 and CO 2 ), in which gas molecular diffusion in water is recognized as the rate limiting step. Isotope compositions in these gas molecules are useful tools to quantify this mass transfer process, in which diffusional isotope fractionation factors (i.e. α diff ) are the key intrinsic parameters. These α diff s are often determined by gas transfer experiments with large uncertainties because the roughness of water surface can affect the interpretation of experimental data. In this study, molecular dynamic simulations were employed to investigate directly the diffusional isotope fractionation for singly and doubly substituted isotopologues of H 2 , N 2 , and O 2 . The results show that diffusional isotope fractionation factors are dependent on both the molecular mass and moment of inertia, which is consistent with previous findings for polyatomic molecules rather than for monoatomic ones. When comparing with the kinetic isotope fractionation (i.e. α k ) determined by gas transfer experiments, I found that α k is likely close to (α diff ) 1/2 within errors (i.e. α k = (α diff ) 1/2 ), rather than to (α diff ) 2/3 that has often been employed to calculate α diff using α k in literature (i.e. α k = (α diff ) 2/3 ). If this is the case, the results further indicate that the nuclear quantum effect is not significant when α diff is of interest. With these findings, I determined the isotope fractionation relationship θ for different O 2 isotopologues to be 0.5100 ± 0.0002 and 1.9535 ± 0.0013 respectively for 17 θ diff (≡ln 17 α diff /ln 18 α diff ) and 36 θ diff (≡ln 36 α diff /ln 18 α diff ) as an example." @default.
• W4283323739 created "2022-06-24" @default.
• W4283323739 creator A5070947356 @default.
• W4283323739 date "2022-09-01" @default.
• W4283323739 modified "2023-09-25" @default.
• W4283323739 title "Diffusional isotope fractionation of singly and doubly substituted isotopologues of H2, N2 and O2 during air-water gas transfer" @default.
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• W4283323739 doi "https://doi.org/10.1016/j.gca.2022.06.022" @default.
• W4283323739 hasPublicationYear "2022" @default.
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