title: Electronic, Crystal Chemistry, and Nonlinear Optical Property Relationships in the Dugganite A3B3CD2O14 Family.
abstract: A family of six nonlinear optical (NLO) materials, A3B3CD2O14 (A = Sr, Ba, or Pb; B = Mg or Zn; C = Te or W; and D = P or V), has been synthesized and characterized. In addition to the synthesis and crystal structures, comprehensive characterization of these compounds includes second harmonic generation (SHG) measurements, theoretical calculations, infrared and diffuse reflectance spectroscopies, and thermogravimetric measurements. We find that all of the reported materials are SHG-active at 1064 nm, with responses ranging from 2.8 to 13.5 × KDP, and exhibit absorption edges in the mid- to deep-ultraviolet regime. By systematically replacing the A, B, C, and D cations, we are able to tune these properties and investigate the role of different NLO-active structural units in producing the SHG responses. Specifically, our electronic structure calculations reveal that the presence of Pb(2+) on the A-site and Te(6+) on the C-site is critical for generating a large SHG response. The synthesis and structure-property relationships described in this family of materials will enable the design and discovery of new NLO materials.
authors.affiliation: Department of Chemistry, University of Houston , 112 Fleming Building, Houston, Texas 77204-5003, United States.
authors.forename: Hongwei
authors.initials: H
authors.lastname: Yu
authors.affiliation: Department of Materials Science and Engineering, Northwestern University , 2220 Campus Drive, Evanston, Illinois 60208-3108, United States.
authors.forename: Joshua
authors.initials: J
authors.lastname: Young
authors.affiliation: Department of Chemistry, University of Houston , 112 Fleming Building, Houston, Texas 77204-5003, United States.
authors.forename: Hongping
authors.initials: H
authors.lastname: Wu
authors.affiliation: Department of Chemistry, University of Houston , 112 Fleming Building, Houston, Texas 77204-5003, United States.
authors.forename: Weiguo
authors.initials: W
authors.lastname: Zhang
authors.affiliation: Department of Materials Science and Engineering, Northwestern University , 2220 Campus Drive, Evanston, Illinois 60208-3108, United States.
authors.forename: James M
authors.initials: JM
authors.lastname: Rondinelli
authors.affiliation: Department of Chemistry, University of Houston , 112 Fleming Building, Houston, Texas 77204-5003, United States.
authors.forename: P Shiv
authors.initials: PS
authors.lastname: Halasyamani