A Congruent-Melting Mid-Infrared Nonlinear Optical Vanadate Exhibiting Strong Second-Harmonic Generation

Chao Wu; Xingxing Jiang; Lin Lin; Yilei Hu; Tianhui Wu; Zheshuai Lin; Zhipeng Huang; Mark G. Humphrey; Chi Zhang

doi:10.1002/anie.202108886

A Congruent-Melting Mid-Infrared Nonlinear Optical Vanadate Exhibiting Strong Second-Harmonic Generation

Chao Wu, Xingxing Jiang, Lin Lin, Yilei Hu, Tianhui Wu, Zheshuai Lin, Zhipeng Huang, Mark G. Humphrey, Chi Zhang^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

36 Citations (Scopus)

Abstract

Study of mid-infrared (mid-IR) nonlinear optical (NLO) materials is hindered by the competing requirements of optimized second-harmonic generation (SHG) coefficient d_ij and laser-induced damage threshold (LIDT) as well as the harsh synthetic conditions. Herein, we report facile hydrothermal synthesis of a polar NLO vanadate Cs₄V₈O₂₂ (CVO) featuring a quasi-rigid honeycomb-layered structure with [VO₄] and [VO₅] polyhedra aligned parallel. CVO possesses a wide IR-transparent window, high LIDT, and congruent-melting behavior. It has very strong phase-matchable SHG intensities in metal vanadate family (12.0 × KDP @ 1064 nm and 2.2 × AGS @ 2100 nm). First-principles calculations suggest that the exceptional SHG responses of CVO largely originate from virtual electronic transitions within [V₄O₁₁]_∞ layer; the excellent optical transmittance of CVO arises from the special characteristics of vibrational phonons resulting from the layered structure.

Original language	English
Pages (from-to)	22447-22453
Number of pages	7
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	41
DOIs	https://doi.org/10.1002/anie.202108886
Publication status	Published - 4 Oct 2021

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title = "A Congruent-Melting Mid-Infrared Nonlinear Optical Vanadate Exhibiting Strong Second-Harmonic Generation",

abstract = "Study of mid-infrared (mid-IR) nonlinear optical (NLO) materials is hindered by the competing requirements of optimized second-harmonic generation (SHG) coefficient dij and laser-induced damage threshold (LIDT) as well as the harsh synthetic conditions. Herein, we report facile hydrothermal synthesis of a polar NLO vanadate Cs4V8O22 (CVO) featuring a quasi-rigid honeycomb-layered structure with [VO4] and [VO5] polyhedra aligned parallel. CVO possesses a wide IR-transparent window, high LIDT, and congruent-melting behavior. It has very strong phase-matchable SHG intensities in metal vanadate family (12.0 × KDP @ 1064 nm and 2.2 × AGS @ 2100 nm). First-principles calculations suggest that the exceptional SHG responses of CVO largely originate from virtual electronic transitions within [V4O11]∞ layer; the excellent optical transmittance of CVO arises from the special characteristics of vibrational phonons resulting from the layered structure.",

keywords = "density functional calculations, mid-infrared, nonlinear optics, second-harmonic generation, vanadates",

author = "Chao Wu and Xingxing Jiang and Lin Lin and Yilei Hu and Tianhui Wu and Zheshuai Lin and Zhipeng Huang and Humphrey, {Mark G.} and Chi Zhang",

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AU - Wu, Chao

AU - Jiang, Xingxing

AU - Lin, Lin

AU - Hu, Yilei

AU - Wu, Tianhui

AU - Lin, Zheshuai

AU - Huang, Zhipeng

AU - Humphrey, Mark G.

AU - Zhang, Chi

PY - 2021/10/4

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N2 - Study of mid-infrared (mid-IR) nonlinear optical (NLO) materials is hindered by the competing requirements of optimized second-harmonic generation (SHG) coefficient dij and laser-induced damage threshold (LIDT) as well as the harsh synthetic conditions. Herein, we report facile hydrothermal synthesis of a polar NLO vanadate Cs4V8O22 (CVO) featuring a quasi-rigid honeycomb-layered structure with [VO4] and [VO5] polyhedra aligned parallel. CVO possesses a wide IR-transparent window, high LIDT, and congruent-melting behavior. It has very strong phase-matchable SHG intensities in metal vanadate family (12.0 × KDP @ 1064 nm and 2.2 × AGS @ 2100 nm). First-principles calculations suggest that the exceptional SHG responses of CVO largely originate from virtual electronic transitions within [V4O11]∞ layer; the excellent optical transmittance of CVO arises from the special characteristics of vibrational phonons resulting from the layered structure.

AB - Study of mid-infrared (mid-IR) nonlinear optical (NLO) materials is hindered by the competing requirements of optimized second-harmonic generation (SHG) coefficient dij and laser-induced damage threshold (LIDT) as well as the harsh synthetic conditions. Herein, we report facile hydrothermal synthesis of a polar NLO vanadate Cs4V8O22 (CVO) featuring a quasi-rigid honeycomb-layered structure with [VO4] and [VO5] polyhedra aligned parallel. CVO possesses a wide IR-transparent window, high LIDT, and congruent-melting behavior. It has very strong phase-matchable SHG intensities in metal vanadate family (12.0 × KDP @ 1064 nm and 2.2 × AGS @ 2100 nm). First-principles calculations suggest that the exceptional SHG responses of CVO largely originate from virtual electronic transitions within [V4O11]∞ layer; the excellent optical transmittance of CVO arises from the special characteristics of vibrational phonons resulting from the layered structure.

KW - density functional calculations

KW - mid-infrared

KW - nonlinear optics

KW - second-harmonic generation

KW - vanadates

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DO - 10.1002/anie.202108886

M3 - Article

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JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

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ER -

A Congruent-Melting Mid-Infrared Nonlinear Optical Vanadate Exhibiting Strong Second-Harmonic Generation

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