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Infrared spectroscopy of an endohedral water in fullerene

Infrared spectroscopy of an endohedral water in fullerene
Infrared spectroscopy of an endohedral water in fullerene

An infrared absorption spectroscopy study of the endohedral water molecule in a solid mixture of H2O@C60 and C60 was carried out at liquid helium temperature. From the evolution of the spectra during the ortho-para conversion process, the spectral lines were identified as para-H2O and ortho-H2O transitions. Eight vibrational transitions with rotational side peaks were observed in the mid-infrared: ω1, ω2, ω3, 2ω1, 2ω2, ω1 + ω3, ω2 + ω3, and 2ω2 + ω3. The vibrational frequencies ω2 and 2ω2 are lower by 1.6% and the rest by 2.4%, as compared to those of free H2O. A model consisting of a rovibrational Hamiltonian with the dipole and quadrupole moments of H2O interacting with the crystal field was used to fit the infrared absorption spectra. The electric quadrupole interaction with the crystal field lifts the degeneracy of the rotational levels. The finite amplitudes of the pure v1 and v2 vibrational transitions are consistent with the interaction of the water molecule dipole moment with a lattice-induced electric field. The permanent dipole moment of encapsulated H2O is found to be 0.50 ± 0.05 D as determined from the far-infrared rotational line intensities. The translational mode of the quantized center-of-mass motion of H2O in the molecular cage of C60 was observed at 110 cm-1 (13.6 meV).

0021-9606
Shugai, A.
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Nagel, U.
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Murata, Y.
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Li, Yongjun
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Mamone, S.
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Krachmalnicoff, A.
a2f4706c-ac18-41fc-87cc-73f6a5bec1c2
Alom, S.
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Whitby, R. J.
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Levitt, M. H.
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Rõõm, T.
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Shugai, A.
919cb44b-125c-4f62-bd57-b9253615ab2b
Nagel, U.
944a312f-5244-4b83-b3d3-e173b9534b23
Murata, Y.
60965676-5251-4502-bde1-fb34b1bda592
Li, Yongjun
6403177f-2dde-4e65-b28e-e31ff34d8d3a
Mamone, S.
7f4c620f-8bb6-4eea-a95f-1173ce69bf80
Krachmalnicoff, A.
a2f4706c-ac18-41fc-87cc-73f6a5bec1c2
Alom, S.
f6b56fb1-7f94-432a-87cd-887f6e5d9f64
Whitby, R. J.
45632236-ab00-4ad0-a02d-6209043e818b
Levitt, M. H.
bcc5a80a-e5c5-4e0e-9a9a-249d036747c3
Rõõm, T.
5d87213d-c0cb-4a9b-b9c8-96b63bbca59b

Shugai, A., Nagel, U., Murata, Y., Li, Yongjun, Mamone, S., Krachmalnicoff, A., Alom, S., Whitby, R. J., Levitt, M. H. and Rõõm, T. (2021) Infrared spectroscopy of an endohedral water in fullerene. Journal of Chemical Physics, 154 (12), [124311]. (doi:10.1063/5.0047350).

Record type: Article

Abstract

An infrared absorption spectroscopy study of the endohedral water molecule in a solid mixture of H2O@C60 and C60 was carried out at liquid helium temperature. From the evolution of the spectra during the ortho-para conversion process, the spectral lines were identified as para-H2O and ortho-H2O transitions. Eight vibrational transitions with rotational side peaks were observed in the mid-infrared: ω1, ω2, ω3, 2ω1, 2ω2, ω1 + ω3, ω2 + ω3, and 2ω2 + ω3. The vibrational frequencies ω2 and 2ω2 are lower by 1.6% and the rest by 2.4%, as compared to those of free H2O. A model consisting of a rovibrational Hamiltonian with the dipole and quadrupole moments of H2O interacting with the crystal field was used to fit the infrared absorption spectra. The electric quadrupole interaction with the crystal field lifts the degeneracy of the rotational levels. The finite amplitudes of the pure v1 and v2 vibrational transitions are consistent with the interaction of the water molecule dipole moment with a lattice-induced electric field. The permanent dipole moment of encapsulated H2O is found to be 0.50 ± 0.05 D as determined from the far-infrared rotational line intensities. The translational mode of the quantized center-of-mass motion of H2O in the molecular cage of C60 was observed at 110 cm-1 (13.6 meV).

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Accepted/In Press date: 12 March 2021
Published date: 29 March 2021
Additional Information: Funding Information: We thank Professor Zlatko Bacic for useful discussions. This research was supported by the Estonian Ministry of Education and Research through institutional research funding under Grant No. IUT23-3 and personal research funding under Grant No. PRG736 and the European Regional Development Fund under Project No. TK134. We acknowledge the EPSRC (UK) for support under Grant Nos. EP/P009980/1 and EP/T004320/1. Publisher Copyright: © 2021 Author(s). Copyright: Copyright 2021 Elsevier B.V., All rights reserved.

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Local EPrints ID: 448327
URI: http://eprints.soton.ac.uk/id/eprint/448327
ISSN: 0021-9606
PURE UUID: 6bc84356-73d7-42bc-ab61-25842560a348
ORCID for R. J. Whitby: ORCID iD orcid.org/0000-0002-9891-5502
ORCID for M. H. Levitt: ORCID iD orcid.org/0000-0001-9878-1180

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Date deposited: 20 Apr 2021 16:33
Last modified: 21 Apr 2021 01:38

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