Vibrationally averaged dipole moments of methane and benzene isotopologues

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Universidade Federal de Minas Gerais

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DFT-B3LYP post-Born-Oppenheimer (finite-nuclear-mass-correction (FNMC)) calculations of vibrationally averaged isotopic dipole moments of methane and benzene, which compare well with experimental values, are reported. For methane, in addition to the principal vibrational contribution to the molecular asymmetry, FNMC accounts for the surprisingly large Born-Oppenheimer error of about 34% to the dipole moments. This unexpected result is explained in terms of concurrent electronic and vibrational contributions. The calculated dipole moment of C6H3D3 is about twice as large as the measured dipole moment of C6H5D. Computational progress is advanced concerning applications to larger systems and the choice of appropriate basis sets. The simpler procedure of performing vibrational averaging on the Born-Oppenheimer level and then adding the FNMC contribution evaluated at the equilibrium distance is shown to be appropriate. Also, the basis set choice is made by heuristic analysis of the physical behavior of the systems, instead of by comparison with experiments.

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Mecânica Hamiltoniana, Astrofísica, Compostos orgânicos, Compostos heterocíclicos

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Correlation-consistent basis sets, Hamiltonian mechanics, Astrophysics, Perturbation theory, Molecular properties, Organic compounds, Heterocyclic compounds

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https://pubs.aip.org/aip/jcp/article/144/14/144301/194920/Vibrationally-averaged-dipole-moments-of-methane

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