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The (X)over-tilde B-2(1), B-2(2), (2)A(1), and (2)A(2) states of oxygen difluoride cation (F2O+): High-level ab initio calculations and simulation of the ultraviolet photoelectron spectrum of F2O

The (X)over-tilde B-2(1), B-2(2), (2)A(1), and (2)A(2) states of oxygen difluoride cation (F2O+): High-level ab initio calculations and simulation of the ultraviolet photoelectron spectrum of F2O
The (X)over-tilde B-2(1), B-2(2), (2)A(1), and (2)A(2) states of oxygen difluoride cation (F2O+): High-level ab initio calculations and simulation of the ultraviolet photoelectron spectrum of F2O
The ultraviolet photoelectron spectrum of F2O was recorded with a higher resolution than previously published. New vibrational structure was observed in the second and third bands. Near state-of-the-art molecular orbital calculations were performed on the (X) over tilde (1)A(1) state of F2O and the (X) over tilde B-2(1), B-2(2), (2)A(1), and (2)A(2) state of F2O+, and their potential energy functions were computed. Spectral simulations based on Franck-Condon factor calculations including the Duchinsky effect were carried out within the harmonic oscillator model and also with the inclusion of anharmonicity, in order to assist spectral assignment. Based on the computed ionization energies obtained with the coupled cluster and multireference configuration interaction methods with basis sets of up to quintuple zeta quality, the order of the low-lying cationic states of F2O+ has been firmly established. However, the detailed assignment of the overlapping second and third photoelectron bands was only achieved with the aid of spectral simulation. The iterative Franck-Condon analysis (IFCA) procedure was carried out for the first band {F2O+ ((X) over tilde B-2(1))<--F2O ((X) over tilde (1)A(1))} in the photoelectron spectrum. With the geometrical parameters of F2O ((X) over tilde (1)A(1)) being fixed at the available experimental values, geometrical parameters of the (X) over tilde B-2(1) state of F2O+ were derived. Based on anharmonic Franck-Condon factor calculations, the recommended IFCA geometrical parameters for the ground state of F2O+ are R(FO) = 1.323 +/-0.002 Angstrom and angle FOF=107.3 +/-0.2 degrees.
anharmonic-force fields, vertical ionization-potentials, diode-laserspectroscopy, least-squares algorithm, basis-set extrapolation, franck-condon analysis, perturbation corrections, emission-spectra, koopmans theorem, molecules
0021-9606
10682-10694
Wang, De-Chao
bf0a990c-f20e-411e-b63d-318334910ab6
Chau, Foo-Tim
e15ec394-d11b-4cbe-91f3-cdac037d9d0e
Mok, Daniel Kam-Wah
49a4e516-0e71-4f59-a3ec-bd607b47ef33
Lee, Edmond P. F.
f47c6d5d-2d1f-4f03-a3ff-03658812d80b
Beeching, Levi
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Ogden, J. Steven
5a99fd42-75e7-4f7b-a347-ac2b1717b8b3
Dyke, John M.
46393b45-6694-46f3-af20-d7369d26199f
Wang, De-Chao
bf0a990c-f20e-411e-b63d-318334910ab6
Chau, Foo-Tim
e15ec394-d11b-4cbe-91f3-cdac037d9d0e
Mok, Daniel Kam-Wah
49a4e516-0e71-4f59-a3ec-bd607b47ef33
Lee, Edmond P. F.
f47c6d5d-2d1f-4f03-a3ff-03658812d80b
Beeching, Levi
8ba45cb9-4761-4940-bd8d-3e7e52e93ce5
Ogden, J. Steven
5a99fd42-75e7-4f7b-a347-ac2b1717b8b3
Dyke, John M.
46393b45-6694-46f3-af20-d7369d26199f

Wang, De-Chao, Chau, Foo-Tim, Mok, Daniel Kam-Wah, Lee, Edmond P. F., Beeching, Levi, Ogden, J. Steven and Dyke, John M. (2001) The (X)over-tilde B-2(1), B-2(2), (2)A(1), and (2)A(2) states of oxygen difluoride cation (F2O+): High-level ab initio calculations and simulation of the ultraviolet photoelectron spectrum of F2O. The Journal of Chemical Physics, 114 (24), 10682-10694. (doi:10.1063/1.1373690).

Record type: Article

Abstract

The ultraviolet photoelectron spectrum of F2O was recorded with a higher resolution than previously published. New vibrational structure was observed in the second and third bands. Near state-of-the-art molecular orbital calculations were performed on the (X) over tilde (1)A(1) state of F2O and the (X) over tilde B-2(1), B-2(2), (2)A(1), and (2)A(2) state of F2O+, and their potential energy functions were computed. Spectral simulations based on Franck-Condon factor calculations including the Duchinsky effect were carried out within the harmonic oscillator model and also with the inclusion of anharmonicity, in order to assist spectral assignment. Based on the computed ionization energies obtained with the coupled cluster and multireference configuration interaction methods with basis sets of up to quintuple zeta quality, the order of the low-lying cationic states of F2O+ has been firmly established. However, the detailed assignment of the overlapping second and third photoelectron bands was only achieved with the aid of spectral simulation. The iterative Franck-Condon analysis (IFCA) procedure was carried out for the first band {F2O+ ((X) over tilde B-2(1))<--F2O ((X) over tilde (1)A(1))} in the photoelectron spectrum. With the geometrical parameters of F2O ((X) over tilde (1)A(1)) being fixed at the available experimental values, geometrical parameters of the (X) over tilde B-2(1) state of F2O+ were derived. Based on anharmonic Franck-Condon factor calculations, the recommended IFCA geometrical parameters for the ground state of F2O+ are R(FO) = 1.323 +/-0.002 Angstrom and angle FOF=107.3 +/-0.2 degrees.

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Published date: 22 June 2001
Keywords: anharmonic-force fields, vertical ionization-potentials, diode-laserspectroscopy, least-squares algorithm, basis-set extrapolation, franck-condon analysis, perturbation corrections, emission-spectra, koopmans theorem, molecules

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Local EPrints ID: 19631
URI: http://eprints.soton.ac.uk/id/eprint/19631
ISSN: 0021-9606
PURE UUID: 15216cf3-7690-4f67-ac32-cbd6e1b721d4
ORCID for John M. Dyke: ORCID iD orcid.org/0000-0002-9808-303X

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Date deposited: 13 Feb 2006
Last modified: 16 Mar 2024 02:36

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Contributors

Author: De-Chao Wang
Author: Foo-Tim Chau
Author: Daniel Kam-Wah Mok
Author: Edmond P. F. Lee
Author: Levi Beeching
Author: J. Steven Ogden
Author: John M. Dyke ORCID iD

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