Nonlinear Optical Properties Of Mixed Oxide Crystals Csnbmoo6 And Cstamoo6: A Periodic Cphf/Ks Study

Abstract

Inorganic crystals are advantageous for use as second harmonic generation (SHG) materials because of their large laser damage threshold and mechanical strength. Here, we focus on the defect pyrochlores based on mixed oxides of MoO3, Ta2O5, Cs2O, and Nb2O5, which were synthesized recently. We predict the linear optical properties (refractive indices and linear polarizabilities) and nonlinear ones [first hyperpolarizabilities and nonlinear optical (NLO) tensors] for the crystals of the defect pyrochlores CsNbMoO6 and CsTaMoO6 using the coupled-perturbed Hartree-Fock/Kohn-Sham method (CPHF/KS) in both full-electron and pseudopotential basis sets. To identify the more accurate computational protocol, the crystals KH2PO4, LiNbO3, (NH2)2CO, and α-SiO2 were used as benchmarks. The best agreement of the predicted NLO parameters with experimental ones is achieved in calculations at the density functional theory/PBE0 level in the POB-TZVP basis. This agreement becomes quantitative when the dimensionless relative value of the NLO activity is used. The calculated relative SHG characteristics of the pyrochlore crystals are (CsNbMoO6/LiNbO3) = 0.016 and (CsTaMoO6/LiNbO3) = 0.022 and (CsNbMoO6/KDP) = 0.39 and CsTaMoO6/KDP) = 0.52. The symmetry of the sublattices of disordered atoms significantly affects the SHG properties of the crystals, and the values of the calculated properties for sublattices of different symmetries can vary by an order of magnitude.

Publication Date

11-1-2018

Publication Title

Journal of Physical Chemistry C

Volume

122

Issue

43

Number of Pages

24907-24916

Document Type

Article

Personal Identifier

scopus

DOI Link

https://doi.org/10.1021/acs.jpcc.8b07117

Socpus ID

85055196547 (Scopus)

Source API URL

https://api.elsevier.com/content/abstract/scopus_id/85055196547

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