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The first microsolvation step for furans : new experiments and benchmarking strategies

Gottschalk, Hannes C.; Poblotzki, Anja; Fatima, Mariyam; Obenchain, Daniel A.; Pérez, Cristóbal; Antony, Jens; Auer, Alexander A.; Baptista, Leonardo; Benoit, David M.; Bistoni, Giovanni; Bohle, Fabian; Dahmani, Rahma; Firaha, Dzmitry; Grimme, Stefan; Hansen, Andreas; Harding, Michael E.; Hochlaf, Majdi; Holzer, Christof; Jansen, Georg; Klopper, Wim; Kopp, Wassja A.; Krasowska, Małgorzata; Kröger, Leif C.; Leonhard, Kai; Mogren Al-Mogren, Muneerah; Mouhib, Halima; Neese, Frank; Pereira, Max N.; Prakash, Muthuramalingam; Ulusoy, Inga S.; Mata, Ricardo A.; Suhm, Martin A.; Schnell, Melanie

Authors

Hannes C. Gottschalk

Anja Poblotzki

Mariyam Fatima

Daniel A. Obenchain

Cristóbal Pérez

Jens Antony

Alexander A. Auer

Leonardo Baptista

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Dr David Benoit D.Benoit@hull.ac.uk
Senior Lecturer in Molecular Physics and Astrochemistry

Giovanni Bistoni

Fabian Bohle

Rahma Dahmani

Dzmitry Firaha

Stefan Grimme

Andreas Hansen

Michael E. Harding

Majdi Hochlaf

Christof Holzer

Georg Jansen

Wim Klopper

Wassja A. Kopp

Małgorzata Krasowska

Leif C. Kröger

Kai Leonhard

Muneerah Mogren Al-Mogren

Halima Mouhib

Frank Neese

Max N. Pereira

Muthuramalingam Prakash

Inga S. Ulusoy

Ricardo A. Mata

Martin A. Suhm

Melanie Schnell



Abstract

The site-specific first microsolvation step of furan and some of its derivatives with methanol is explored to benchmark the ability of quantum-chemical methods to describe the structure, energetics, and vibrational spectrum at low temperature. Infrared and microwave spectra in supersonic jet expansions are used to quantify the docking preference and some relevant quantum states of the model complexes. Microwave spectroscopy strictly rules out in-plane docking of methanol as opposed to the top coordination of the aromatic ring. Contrasting comparison strategies, which emphasize either the experimental or the theoretical input, are explored. Within the harmonic approximation, only a few composite computational approaches are able to achieve a satisfactory performance. Deuteration experiments suggest that the harmonic treatment itself is largely justified for the zero-point energy, likely and by design due to the systematic cancellation of important anharmonic contributions between the docking variants. Therefore, discrepancies between experiment and theory for the isomer abundance are tentatively assigned to electronic structure deficiencies, but uncertainties remain on the nuclear dynamics side. Attempts to include anharmonic contributions indicate that for systems of this size, a uniform treatment of anharmonicity with systematically improved performance is not yet in sight.

Citation

Gottschalk, H. C., Poblotzki, A., Fatima, M., Obenchain, D. A., Pérez, C., Antony, J., …Schnell, M. (2020). The first microsolvation step for furans : new experiments and benchmarking strategies. The Journal of chemical physics, 152(16), 164303. https://doi.org/10.1063/5.0004465

Journal Article Type Article
Acceptance Date Apr 2, 2020
Publication Date Apr 30, 2020
Deposit Date May 13, 2020
Publicly Available Date May 14, 2020
Journal The Journal of Chemical Physics
Print ISSN 0021-9606
Electronic ISSN 1089-7690
Publisher AIP Publishing
Peer Reviewed Peer Reviewed
Volume 152
Issue 16
Pages 164303
DOI https://doi.org/10.1063/5.0004465
Keywords Physical and Theoretical Chemistry; General Physics and Astronomy
Public URL https://hull-repository.worktribe.com/output/3502511
Publisher URL https://aip.scitation.org/doi/10.1063/5.0004465
Additional Information Received: 2020-02-11; Accepted: 2020-04-02; Published: 2020-04-30

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