Structure of ZnCl2 melt. Part I: Raman spectroscopy analysis driven by Ab initio methods

Abduljabar Q. Alsayoud, Manga Venkateswara Rao, Angharad N. Edwards, Pierre A Deymier, Krishna Muralidharan, Barrett G Potter, Keith A Runge, Pierre Lucas

Research output: Contribution to journalArticle

10 Citations (Scopus)

Abstract

The structure of molten ZnCl2 is investigated using a combination of computer simulation and experimental methods. Ab initio molecular dynamics (AIMD) is used to model the structure of ZnCl2 at 600 K. The structure factors and pair distribution functions derived from AIMD show a good match with those previously measured by neutron diffraction (ND). In addition, Raman spectroscopy is used to investigate the structure of liquid ZnCl2 and identify the relative fractions of constituent structural units. To ascertain the assignment of each Raman mode, a series of ZnCl2 crystalline prototypes are modeled and the corresponding Raman modes are derived by first-principles calculations. Curve fitting of experimental Raman spectra using these mode assignments shows excellent agreement with both AIMD and ND. These results confirm the presence of significant fractions of edge-sharing tetrahedra in liquid ZnCl2. The presence of these structural motifs has significant impact on the fragility of this tetrahedral glass-forming liquid. The assignment of Raman bands present in molten ZnCl2 is revised and discussed in view of these results.

Original languageEnglish (US)
Pages (from-to)4174-4181
Number of pages8
JournalJournal of Physical Chemistry B
Volume120
Issue number17
DOIs
StatePublished - May 5 2016

Fingerprint

Raman spectroscopy
Molecular dynamics
Neutron diffraction
molecular dynamics
neutron diffraction
Molten materials
Liquids
liquids
curve fitting
Curve fitting
tetrahedrons
Distribution functions
Raman scattering
computerized simulation
distribution functions
prototypes
Raman spectra
Crystalline materials
Glass
glass

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Materials Chemistry
  • Surfaces, Coatings and Films

Cite this

Structure of ZnCl2 melt. Part I : Raman spectroscopy analysis driven by Ab initio methods. / Alsayoud, Abduljabar Q.; Venkateswara Rao, Manga; Edwards, Angharad N.; Deymier, Pierre A; Muralidharan, Krishna; Potter, Barrett G; Runge, Keith A; Lucas, Pierre.

In: Journal of Physical Chemistry B, Vol. 120, No. 17, 05.05.2016, p. 4174-4181.

Research output: Contribution to journalArticle

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