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Title: Direct assignment of molecular vibrations via normal mode analysis of the neutron dynamic pair distribution function technique

For over a century, vibrational spectroscopy has enhanced the study of materials. Yet, assignment of particular molecular motions to vibrational excitations has relied on indirect methods. Here, we demonstrate that applying group theoretical methods to the dynamic pair distribution function analysis of neutron scattering data provides direct access to the individual atomic displacements responsible for these excitations. Applied to the molecule-based frustrated magnet with a potential magnetic valence-bond state, LiZn{sub 2}Mo{sub 3}O{sub 8}, this approach allows direct assignment of the constrained rotational mode of Mo{sub 3}O{sub 13} clusters and internal modes of MoO{sub 6} polyhedra. We anticipate that coupling this well known data analysis technique with dynamic pair distribution function analysis will have broad application in connecting structural dynamics to physical properties in a wide range of molecular and solid state systems.
Authors:
; ;  [1] ;  [2] ;  [2] ; ;  [3] ; ; ;  [4]
  1. Department of Chemistry, The Johns Hopkins University, Baltimore, Maryland 21218 (United States)
  2. (United States)
  3. Department of Applied Physics, Cornell University, Ithaca, New York 14853 (United States)
  4. Institute for Quantum Matter and Department of Physics and Astronomy, The Johns Hopkins University, Baltimore, Maryland 21218 (United States)
Publication Date:
OSTI Identifier:
22489634
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 143; Journal Issue: 12; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ALLOCATIONS; ATOMIC DISPLACEMENTS; DATA ANALYSIS; DISTRIBUTION FUNCTIONS; EXCITATION; NEUTRON DIFFRACTION; NEUTRONS; NORMAL-MODE ANALYSIS; PHYSICAL PROPERTIES; SOLIDS; SPECTROSCOPY