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A Computational Study on Closed-Shell Molecular Hexafluorides MF6 (M=S, Se, Te, Po, Xe, Rn, Cr, Mo, W, U) – Molecular Structure, Anharmonic Frequency Calculations, and Prediction of the NdF6 Molecule

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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä

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ChemPhysChem, Volume 24, issue 9

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Quantum chemical methods were used to study the molecular structure and anharmonic IR spectra of the experimentally known closed-shell molecular hexafluorides MF6 (M=S, Se, Te, Xe, Mo, W, U). First, the molecular structures and harmonic frequencies were investigated using Density Functional Theory (DFT) with all-electron basis sets and explicitly considering the influence of spin-orbit coupling. Second, anharmonic frequencies and IR intensities were calculated with the CCSD(T) coupled cluster method and compared, where available, with IR spectra recorded by us. These comparisons showed satisfactory results. The anharmonic IR spectra provide means for identifying experimentally too little studied or unknown MF6 molecules with M=Cr, Po, Rn. To the best of our knowledge, we predict the NdF6 molecule for the first time and show it to be a true local minimum on the potential energy surface. We used intrinsic bond orbital (IBO) analyses to characterize the bonding situation in comparison with the UF6 molecule.

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Funding Information: T. G. thanks the HPC‐EUROPA3 (INFRAIA‐2016‐1‐730897) for a travel grant and CSC, the Finnish IT Center for Science, for the computing resources. We would like to thank Björn Koch and Dr. Tobias Chemnitz for the recording of all infrared spectra of the currently experimentally accessible molecular hexafluorides presented in this paper. We thank Solvay for the kind donations of F. Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2023 The Authors. ChemPhysChem published by Wiley-VCH GmbH.

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Graubner, T, Karttunen, A J & Kraus, F 2023, 'A Computational Study on Closed-Shell Molecular Hexafluorides MF 6 (M=S, Se, Te, Po, Xe, Rn, Cr, Mo, W, U) – Molecular Structure, Anharmonic Frequency Calculations, and Prediction of the NdF 6 Molecule', ChemPhysChem, vol. 24, no. 9, e202200903. https://doi.org/10.1002/cphc.202200903

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