Casimir–Polder Size Consistency: A Constraint Violated by Some Dispersion Theories

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Gould, Tim
Toulouse, Julien
Angyan, Janos G
Dobson, John F
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2017
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A key goal in quantum chemistry methods, whether ab initio or otherwise, is to achieve size consistency. In this work we formulate the related idea of “Casimir–Polder size consistency” that manifests in long-range dispersion energetics. We show that local approximations in time-dependent density functional theory dispersion energy calculations violate the consistency condition because of incorrect treatment of highly nonlocal “xc kernel” physics, by up to 10% in our tests on closed-shell atoms.

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Journal of Chemical Theory and Computation

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13

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12

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This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Chemical Theory and Computation, copyright 2017 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see 10.1021/acs.jctc.7b00996.

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Software engineering

Theoretical and computational chemistry

Theoretical and computational chemistry not elsewhere classified

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Physical chemistry

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