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• W2807776384 abstract "It has been recently shown that in the presence of an applied voltage, hydrogen and deuterium nuclei can be separated from one another using graphene membranes as a nuclear sieve, resulting in a 10-fold enhancement in the concentration of the lighter isotope. While previous studies, both experimental and theoretical, have attributed this effect mostly to differences in vibrational zero point energy (ZPE) of the various isotopes near the membrane surface, we propose that multi-dimensional quantum mechanical tunneling of nuclei through the graphene membrane influences this proton permeation process in a fundamental way. We perform ring polymer molecular dynamics calculations in which we include both ZPE and tunneling effects of various hydrogen isotopes as they permeate the graphene membrane and compute rate constants across a range of temperatures near 300 K. While capturing the experimentally observed separation factor, our calculations indicate that the transverse motion of the various isotopes across the surface of the graphene membrane is an essential part of this sieving mechanism. An understanding of the multi-dimensional quantum mechanical nature of this process could serve to guide the design of other such isotopic enrichment processes for a variety of atomic and molecular species of interest." @default.
• W2807776384 created "2018-06-21" @default.
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• W2807776384 date "2018-06-11" @default.
• W2807776384 modified "2023-10-15" @default.
• W2807776384 title "Theoretical description of quantum mechanical permeation of graphene membranes by charged hydrogen isotopes" @default.
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• W2807776384 doi "https://doi.org/10.1063/1.5027821" @default.
• W2807776384 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/29907032" @default.
• W2807776384 hasPublicationYear "2018" @default.
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