The Combination of Structure Prediction and Experiment for the Exploration of Alkali-Earth Metal-Contained Chalcopyrite-Like IR Nonlinear Optical Material

Peng Wang; Yu Chu; Abudukadi Tudi; Congwei Xie; Zhihua Yang; Shilie Pan; Junjie Li

doi:10.1002/advs.202106120

The Combination of Structure Prediction and Experiment for the Exploration of Alkali-Earth Metal-Contained Chalcopyrite-Like IR Nonlinear Optical Material

Adv Sci (Weinh). 2022 May;9(15):e2106120. doi: 10.1002/advs.202106120. Epub 2022 Apr 11.

Authors

Peng Wang¹, Yu Chu^{1

2}, Abudukadi Tudi^{1

2}, Congwei Xie^{1

3}, Zhihua Yang^{1

2}, Shilie Pan^{1

2}, Junjie Li^{1

2}

Affiliations

¹ CAS Key Laboratory of Functional Materials and Devices for Special Environments, Xinjiang Technical Institute of Physics & Chemistry CAS, Xinjiang Key Laboratory of Electronic Information Materials and Devices, Urumqi, 830011, P. R. China.
² Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
³ Skolkovo Institute of Science and Technology, Skolkovo Innovation Center, 3 Nobel Street, Moscow, 143026, Russian Federation.

Abstract

Design and fabrication of new infrared (IR) nonlinear optical (NLO) materials with balanced properties are urgently needed since commercial chalcopyrite-like (CL) NLO crystals are suffering from their intrinsic drawbacks. Herein, the first defect-CL (DCL) alkali-earth metal (AEM) selenide IR NLO material, DCL-MgGa₂ Se₄ , has been rationally designed and fabricated by a structure prediction and experiment combined strategy. The introduction of AEM tetrahedral unit MgSe₄ effectively widens the band gap of DCL compounds. The title compound exhibits a wide band gap of 2.96 eV, resulting in a high laser induced damage threshold (LIDT) of ≈3.0 × AgGaS₂ (AGS). Furthermore, the compound shows a suitable second harmonic generation (SHG) response (≈0.9 × AGS) with a type-I phase-matching (PM) behavior and a wide IR transparent range. The results indicate that DCL-MgGa₂ Se₄ is a promising mid-to-far IR NLO material and give some insights into the design of new CL compound with outstanding IR NLO properties based on the AEM tetrahedra and the structure predication and experiment combined strategy.

Keywords: alkaline earth metals; chalcogenide; chalcopyrite-like structures; nonlinear optical materials; tetrahedral units.

Abstract

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