Experimental and computational studies on collective hydrogen dynamics in ammonia borane

Incoherent inelastic neutron scattering

Shawn M. Kathmann, Vencislav Parvanov, Gregory K. Schenter, Ashley C. Stowe, Luc L. Daemen, Monika Hartl, John Linehan, Nancy J. Hess, Abhi Karkamkar, Tom Autrey

Research output: Contribution to journalArticle

22 Citations (Scopus)

Abstract

Incoherent inelastic neutron scattering is used to probe the effects of dihydrogen bonding on the vibrational dynamics in the molecular crystal of ammonia borane. The thermal neutron energy loss spectra of B 11 enriched ammonia borane isotopomers (B 11 H3 NH3, B 11 D3NH3, and B 11 H3 ND 3) are presented and compared to the vibrational power spectrum calculated using ab initio molecular dynamics. A harmonic vibrational analysis on NH3 BH3 clusters was also explored to check for consistency with experiment and the power spectrum. The measured neutron spectra and computed ab initio power spectrum compare extremely well (50-500 cm-1). Some assignment of modes to simple harmonic motion, e.g., NH3 and BH3 torsion in the molecular crystal is possible, and it is confirmed that the lowest modes are dominated by collective motion. We show that the vibrational dynamics as modeled with ab initio molecular dynamics provides a more complete description of anharmonic and collective dynamics in the low frequency region of the inelastic incoherent neutron scattering spectra when compared to the conventional harmonic approach.

Original languageEnglish
Article number024507
JournalJournal of Chemical Physics
Volume130
Issue number2
DOIs
Publication statusPublished - 2009

Fingerprint

Boranes
Inelastic neutron scattering
boranes
Power spectrum
Ammonia
Molecular crystals
power spectra
ammonia
Hydrogen
inelastic scattering
neutron scattering
Molecular dynamics
Neutrons
simple harmonic motion
hydrogen
Incoherent scattering
molecular dynamics
harmonics
incoherent scattering
neutron spectra

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Kathmann, S. M., Parvanov, V., Schenter, G. K., Stowe, A. C., Daemen, L. L., Hartl, M., ... Autrey, T. (2009). Experimental and computational studies on collective hydrogen dynamics in ammonia borane: Incoherent inelastic neutron scattering. Journal of Chemical Physics, 130(2), [024507]. https://doi.org/10.1063/1.3042270

Experimental and computational studies on collective hydrogen dynamics in ammonia borane : Incoherent inelastic neutron scattering. / Kathmann, Shawn M.; Parvanov, Vencislav; Schenter, Gregory K.; Stowe, Ashley C.; Daemen, Luc L.; Hartl, Monika; Linehan, John; Hess, Nancy J.; Karkamkar, Abhi; Autrey, Tom.

In: Journal of Chemical Physics, Vol. 130, No. 2, 024507, 2009.

Research output: Contribution to journalArticle

Kathmann, SM, Parvanov, V, Schenter, GK, Stowe, AC, Daemen, LL, Hartl, M, Linehan, J, Hess, NJ, Karkamkar, A & Autrey, T 2009, 'Experimental and computational studies on collective hydrogen dynamics in ammonia borane: Incoherent inelastic neutron scattering', Journal of Chemical Physics, vol. 130, no. 2, 024507. https://doi.org/10.1063/1.3042270
Kathmann, Shawn M. ; Parvanov, Vencislav ; Schenter, Gregory K. ; Stowe, Ashley C. ; Daemen, Luc L. ; Hartl, Monika ; Linehan, John ; Hess, Nancy J. ; Karkamkar, Abhi ; Autrey, Tom. / Experimental and computational studies on collective hydrogen dynamics in ammonia borane : Incoherent inelastic neutron scattering. In: Journal of Chemical Physics. 2009 ; Vol. 130, No. 2.
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