skip to main content


Title: Representational analysis of extended disorder in atomistic ensembles derived from total scattering data

With the increased availability of high-intensity time-of-flight neutron and synchrotron X-ray scattering sources that can access wide ranges of momentum transfer, the pair distribution function method has become a standard analysis technique for studying disorder of local coordination spheres and at intermediate atomic separations. In some cases, rational modeling of the total scattering data (Bragg and diffuse) becomes intractable with least-squares approaches, necessitating reverse Monte Carlo simulations using large atomistic ensembles. However, the extraction of meaningful information from the resulting atomistic ensembles is challenging, especially at intermediate length scales. Representational analysis is used here to describe the displacements of atoms in reverse Monte Carlo ensembles from an ideal crystallographic structure in an approach analogous to tight-binding methods. Rewriting the displacements in terms of a local basis that is descriptive of the ideal crystallographic symmetry provides a robust approach to characterizing medium-range order (and disorder) and symmetry breaking in complex and disordered crystalline materials. Lastly, this method enables the extraction of statistically relevant displacement modes (orientation, amplitude and distribution) of the crystalline disorder and provides directly meaningful information in a locally symmetry-adapted basis set that is most descriptive of the crystal chemistry and physics.
 [1] ;  [2]
  1. Colorado State Univ., Fort Collins, CO (United States). Dept. of Chemistry
  2. Johns Hopkins Univ., Baltimore, MD (United States). Dept. of Chemistry, Materials Science and Engineering, and Physics and Astronomy
Publication Date:
Grant/Contract Number:
FG02-08ER46544; AC52-06NA25396
Accepted Manuscript
Journal Name:
Journal of Applied Crystallography (Online)
Additional Journal Information:
Journal Name: Journal of Applied Crystallography (Online); Journal Volume: 48; Journal Issue: 5; Journal ID: ISSN 1600-5767
International Union of Crystallography
Research Org:
Johns Hopkins Univ., Baltimore, MD (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; extended disorder; atomistic ensembles; modeling; pair distribution function analysis
OSTI Identifier: