Evidence for hydrogen transport in deuterated LiBH4 from low-temperature Raman-scattering measurements and first-principles calculations

R. Gremaud; Z. Łodziana; P. Hug; B. Willenberg; A. M. Racu; J. Schoenes; A. J. Ramirez-Cuesta; S. J. Clark; K. Refson; A. Züttel; A. Borgschulte

doi:10.1103/PhysRevB.80.100301

Evidence for hydrogen transport in deuterated LiBH4 from low-temperature Raman-scattering measurements and first-principles calculations

R. Gremaud
, Z. Łodziana
, P. Hug
, B. Willenberg
, A. M. Racu
, J. Schoenes
, A. J. Ramirez-Cuesta
, S. J. Clark
, K. Refson
, A. Züttel
, A. Borgschulte

Research output: Contribution to journal › Article › peer-review

36 Scopus citations

Abstract

We provide direct evidence for successive exchange of D atoms in the isotopically pure BH 4- units of the crystalline solid lithium borohydride. We prove the coexistence of all BH4-n Dn- (0≤n≤4) units in the bulk by deconvolution of the D-stretching vibrations band of Raman spectra at 83 and 5 K in partially D-exchanged LiBH4 and comparison with first-principles Raman intensity calculations. The measured distribution of BH4-n Dn- units is in good agreement with a binomial distribution biased by H-D zero-point motions. This implies breaking the strong D2 covalent bond and transport of hydrogen in LiBH4 below the melting temperature.

Original language	English
Article number	100301
Journal	Physical Review B - Condensed Matter and Materials Physics
Volume	80
Issue number	10
DOIs	https://doi.org/10.1103/PhysRevB.80.100301
State	Published - Sep 10 2009
Externally published	Yes

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Gremaud, R., Łodziana, Z., Hug, P., Willenberg, B., Racu, A. M., Schoenes, J., Ramirez-Cuesta, A. J., Clark, S. J., Refson, K., Züttel, A., & Borgschulte, A. (2009). Evidence for hydrogen transport in deuterated LiBH4 from low-temperature Raman-scattering measurements and first-principles calculations. Physical Review B - Condensed Matter and Materials Physics, 80(10), Article 100301. https://doi.org/10.1103/PhysRevB.80.100301

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title = "Evidence for hydrogen transport in deuterated LiBH4 from low-temperature Raman-scattering measurements and first-principles calculations",

abstract = "We provide direct evidence for successive exchange of D atoms in the isotopically pure BH 4- units of the crystalline solid lithium borohydride. We prove the coexistence of all BH4-n Dn- (0≤n≤4) units in the bulk by deconvolution of the D-stretching vibrations band of Raman spectra at 83 and 5 K in partially D-exchanged LiBH4 and comparison with first-principles Raman intensity calculations. The measured distribution of BH4-n Dn- units is in good agreement with a binomial distribution biased by H-D zero-point motions. This implies breaking the strong D2 covalent bond and transport of hydrogen in LiBH4 below the melting temperature.",

author = "R. Gremaud and Z. {\L}odziana and P. Hug and B. Willenberg and Racu, \{A. M.\} and J. Schoenes and Ramirez-Cuesta, \{A. J.\} and Clark, \{S. J.\} and K. Refson and A. Z{\"u}ttel and A. Borgschulte",

year = "2009",

month = sep,

day = "10",

doi = "10.1103/PhysRevB.80.100301",

language = "English",

volume = "80",

journal = "Physical Review B - Condensed Matter and Materials Physics",

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Gremaud, R, Łodziana, Z, Hug, P, Willenberg, B, Racu, AM, Schoenes, J, Ramirez-Cuesta, AJ, Clark, SJ, Refson, K, Züttel, A & Borgschulte, A 2009, 'Evidence for hydrogen transport in deuterated LiBH4 from low-temperature Raman-scattering measurements and first-principles calculations', Physical Review B - Condensed Matter and Materials Physics, vol. 80, no. 10, 100301. https://doi.org/10.1103/PhysRevB.80.100301

TY - JOUR

T1 - Evidence for hydrogen transport in deuterated LiBH4 from low-temperature Raman-scattering measurements and first-principles calculations

AU - Gremaud, R.

AU - Łodziana, Z.

AU - Hug, P.

AU - Willenberg, B.

AU - Racu, A. M.

AU - Schoenes, J.

AU - Ramirez-Cuesta, A. J.

AU - Clark, S. J.

AU - Refson, K.

AU - Züttel, A.

AU - Borgschulte, A.

PY - 2009/9/10

Y1 - 2009/9/10

N2 - We provide direct evidence for successive exchange of D atoms in the isotopically pure BH 4- units of the crystalline solid lithium borohydride. We prove the coexistence of all BH4-n Dn- (0≤n≤4) units in the bulk by deconvolution of the D-stretching vibrations band of Raman spectra at 83 and 5 K in partially D-exchanged LiBH4 and comparison with first-principles Raman intensity calculations. The measured distribution of BH4-n Dn- units is in good agreement with a binomial distribution biased by H-D zero-point motions. This implies breaking the strong D2 covalent bond and transport of hydrogen in LiBH4 below the melting temperature.

AB - We provide direct evidence for successive exchange of D atoms in the isotopically pure BH 4- units of the crystalline solid lithium borohydride. We prove the coexistence of all BH4-n Dn- (0≤n≤4) units in the bulk by deconvolution of the D-stretching vibrations band of Raman spectra at 83 and 5 K in partially D-exchanged LiBH4 and comparison with first-principles Raman intensity calculations. The measured distribution of BH4-n Dn- units is in good agreement with a binomial distribution biased by H-D zero-point motions. This implies breaking the strong D2 covalent bond and transport of hydrogen in LiBH4 below the melting temperature.

UR - https://www.scopus.com/pages/publications/70349897836

U2 - 10.1103/PhysRevB.80.100301

DO - 10.1103/PhysRevB.80.100301

M3 - Article

AN - SCOPUS:70349897836

SN - 1098-0121

VL - 80

JO - Physical Review B - Condensed Matter and Materials Physics

JF - Physical Review B - Condensed Matter and Materials Physics

IS - 10

M1 - 100301

ER -

Evidence for hydrogen transport in deuterated LiBH4 from low-temperature Raman-scattering measurements and first-principles calculations

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