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Time and Frequency Resolved Hydrogen Dynamics in deuterated LiBH4

Published online by Cambridge University Press:  31 January 2011

Robin Gremaud
Affiliation:
[email protected], Empa, Swiss Federal Laboratories for Materials Testing and Research, Hydrogen & Energy, Dübendorf, Switzerland
Esben R. Andresen
Affiliation:
[email protected], Universität Zürich, Physikalisch-Chemisches Institut, Zürich, Switzerland
Anibal J. Ramirez-Cuesta
Affiliation:
[email protected], Rutherford Appleton Laboratory, ISIS Facility, Chilton, United Kingdom
Keith Refson
Affiliation:
[email protected], Rutherford Appleton Laboratory, ISIS Facility, Chilton, United Kingdom
Zbigniew Łodziana
Affiliation:
[email protected], Empa, Swiss Federal Laboratories for Materials Testing and Research, Hydrogen & Energy, Dübendorf, Switzerland
Andreas Züttel
Affiliation:
[email protected], Empa, Swiss Federal Laboratories for Materials Testing and Research, Hydrogen & Energy, Dübendorf, Switzerland
Peter Hamm
Affiliation:
[email protected], Universität Zürich, Physikalisch-Chemisches Institut, Zürich, Switzerland
Andreas Borgschulte
Affiliation:
[email protected], Empa, Swiss Federal Laboratories for Materials Testing and Research, Hydrogen & Energy, Dübendorf, Switzerland
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Abstract

We study deuterated tetrahydroborate LiBH4 in the low-temperature (LT) phase, focusing on the BH (BD) stretching vibrations, by infrared (IR) and IR-pump-probe spectroscopy. Calculated infrared spectra by density functional theory allow us to disentangle the contributions coming from all the coexisting BH4-nDn (n = 0…4) molecular units. We report on anharmonicity and vibrational lifetime (1.6 ps) of the BD vibrations, as well as on the BH2D2 orientational relaxation by polarization anisotropy IR-pump-probe measurements. We find a constant anisotropy for at least 5 ps confirming the slow reorientational motion and low thermal disorder of the BH4 unit in the LT phase of this potential hydrogen storage material.

Type
Research Article
Copyright
Copyright © Materials Research Society 2010

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