Design of Infrared Nonlinear Optical Compounds with Diamond-like Structures and Balanced Optical Performance

Dongdong Chu; Congwei Xie; Zhihua Yang

doi:10.1021/acs.inorgchem.2c01838

Design of Infrared Nonlinear Optical Compounds with Diamond-like Structures and Balanced Optical Performance

Inorg Chem. 2022 Jul 25;61(29):11454-11462. doi: 10.1021/acs.inorgchem.2c01838. Epub 2022 Jul 11.

Authors

Dongdong Chu^{1

2}, Congwei Xie¹, Zhihua Yang^{1

2}

Affiliations

¹ Research Center for Crystal Materials; CAS Key Laboratory of Functional Materials and Devices for Special Environments, Xinjiang Technical Institute of Physics & Chemistry, CAS, 40-1 South Beijing Road, Urumqi 830011, China.
² Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China.

PMID: 35817760
DOI: 10.1021/acs.inorgchem.2c01838

Abstract

Infrared (IR) nonlinear optical (NLO) crystals are the major materials to widen the output range of solid-state lasers to mid-infrared regions, but they are still inadequate for application due to the difficulties in balancing the large band gaps and strong NLO response. The diamond-like structure is a potential structural template to explore IR NLO materials. Herein, a computational workflow is proposed for exploring compounds with diamond-like structures, a series of LiMgGaSe₃ structures were predicted successfully through this workflow, and LiMgGaSe₃-I-III exhibited good optical performances in a large band gap (2.75-2.92 eV), strong SHG response (1.2-1.3 × AGS), and suitable birefringence (0.0470-0.0783 at 1064 nm). The in-depth mechanism explorations strongly demonstrate that the synergistic effect of alkaline earth metal tetrahedral [MgSe₄] and [GaSe₄] units is the main origin of large SHG response. The foregoing results suggest that our workflow can accelerate the discovery of new mid-IR NLO materials with diamond-like structures.