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Journal article
Microscopic Origins of Optical Second Harmonic Generation in Noncentrosymmetric-Nonpolar Materials
Chemistry of materials, v 26(19), pp 5773-5781
14 Oct 2014
Abstract
We use a symmetry-based structural analysis combined with an electronic descriptor for bond covalency to explain the origin of the second-order nonlinear optical response (second harmonic generation, SHG) in noncentrosymmetric nonpolar ATeMoO(6) compounds (where A = Mg, Zn, or Cd). We show that the SHG response has a complex dependence on the asymmetric geometry of the AO(6) and AO(4) functional units and the orbital character at the valence band edge, which we are able to distinguish using an A-O bond covalency descriptor. The degree of covalency between the divalent A-site cation and the oxygen ligands dominates over the geometric contributions to the SHG arising from the acentric polyhedra, and this can be understood from considerations of the local static charge density distribution. The use of a local dipole model for the polyhedral moieties (AO(4)/AO(6), MoO4, and TeO4) can account for a nonzero SHG response, even though the materials exhibit nonpolar structures; however, it is insufficient to explain the change in the magnitude of the SHG response upon A-cation substitution. The atomic scale and electronic structure understanding of the macroscopic SHG behavior is then used to identify hypothetical HgTeMoO6 as a candidate telluromolybdate with an enhanced nonlinear optical response.
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Details
- Title
- Microscopic Origins of Optical Second Harmonic Generation in Noncentrosymmetric-Nonpolar Materials
- Creators
- Antonio Cammarata - Czech Technical University in PragueWeiguo Zhang - University of HoustonP. Shiv Halasyamani - University of HoustonJames M. Rondinelli - Drexel University
- Publication Details
- Chemistry of materials, v 26(19), pp 5773-5781
- Publisher
- American Chemical Society; Washington, DC
- Number of pages
- 9
- Grant note
- N00014-11-1-0664 / ONR; Office of Naval Research E-1457 / Welch Foundation; The Welch Foundation 52138-DNI10 / American Chemical Society Petroleum Research Fund; American Chemical Society DE-AC02-06CH11357 / U.S. DOE, Office of Science, Office of Basic Energy Sciences; United States Department of Energy (DOE)
- Resource Type
- Journal article
- Language
- English
- Web of Science ID
- WOS:000343195600046
- Scopus ID
- 2-s2.0-84925328859
- Other Identifier
- 991019330616704721
InCites Highlights
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- Collaboration types
- Domestic collaboration
- International collaboration
- Web of Science research areas
- Chemistry, Physical
- Materials Science, Multidisciplinary