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Theoretical perspectives on the structure, electronic, and optical properties of titanosilicates Li2M4[(TiO)Si4O12] (M = K+, Rb+)

Abstract

It is still a challenge to design and synthesize the high performance broader ultraviolet nonlinear optical (NLO) materials nowadays. Two new transition-metal silicates have recently attracted much attention due to their strong phase-matched second harmonic generation (SHG) responses (about 4.5 times higher than KDP). However, the electronic and optical properties underlying the high performance of this material and consequently, the possibilities for designing more efficient silicates for NLO applications are not at present clear. In the present work, the geometric structure and bonding character, electronic structure and optical properties of Li2M4[(TiO)Si4O12] (M = K+, Rb+) crystals have been systematically determined based on the density functional theory. Satisfactory agreement between experimental and theoretical results indicates that the used method and conditions are suitable. A detailed analysis of the precise electronic structure and dipole moments of the two compounds suggests that it is the strong covalent character between Ti (Si) and O, and the same orientation alignment of dipole moment vector of the constituent asymmetry [TiO5]6- square pyramid anion units that gives the large SHG responses for the two compounds. Additionally, the experimental unavailable linear and nonlinear optical parameters including dielectric function, optical absorption, birefringence, and all components of SHG coefficients are reported for the first time. This investigation unravels the structure-property relationship of titanosilicates, and may be significant in terms of providing an efficient strategy to design more potential and competitive NLO materials.

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Publication details

The article was received on 27 Mar 2017, accepted on 16 May 2017 and first published on 17 May 2017


Article type: Paper
DOI: 10.1039/C7CP01946G
Citation: Phys. Chem. Chem. Phys., 2017, Accepted Manuscript
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    Theoretical perspectives on the structure, electronic, and optical properties of titanosilicates Li2M4[(TiO)Si4O12] (M = K+, Rb+)

    J. Hu, Z. Ma, R. Sa, Y. Zhang and W. Kechen, Phys. Chem. Chem. Phys., 2017, Accepted Manuscript , DOI: 10.1039/C7CP01946G

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