Controlling the Orientation-Dependent Second Harmonic Generation in Hybrid Germanium Perovskites

Guo, Zhu1; Han, Dingchong2; Liu, Huan3; Hu, Yaoqiao4; Zhang, Weixiong2; Chen, Rui3; Mao, Lingling1

2024-06-01

10.1002/anie.202407675

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   影响因子和分区

1433-7851

1521-3773

Manipulating the crystal orientation plays a crucial role in the conversion efficiency during second harmonic generation (SHG). Here, we provide a new strategy in controlling the surface-dependent anisotropic SHG with the precise design of (101) and (210) MAGeI(3) facets. Based on the SHG measurement, the (101) MAGeI(3) single crystal exhibits larger SHG (1.3x(210) MAGeI(3)). Kelvin probe force microscopy imaging shows a smaller work function for the (101) MAGeI(3) compared with the (210), which indirectly demonstrates the stronger intrinsic polarization on the (101) surface. X-ray photoelectron spectroscopy confirms the band bending within the (101) facet. Temperature-dependent steady-state and time-resolved photoluminescence spectroscopy show shorter lifetime and wider emission band in the (101) MAGeI(3) single crystal, revealing the higher defect states. Additionally, powder X-ray diffraction patterns show the (101) MAGeI(3) possesses larger in-plane polar units [GeI3](-) density, which could directly enhance the spontaneous polarization in the (101) facet. Density functional theory (DFT) calculation further demonstrates the higher intrinsic polarization in the (101) facet compared with the (210) facet, and the larger built-in electric field in the (101) facet facilitates surface vacancy defect accumulation. Our work provides a new angle in tuning and optimizing hybrid perovskite-based nonlinear optical materials.

perovskite phases single crystal second harmonic generation polarization built-in electric field

SCI ; EI

英语

第一 ; 通讯

National Natural Science Foundation of China (NSFC)[22275077] ; Stable Support Plan Program of ShenZhen Natural Science Fund[20220814233319001]

Chemistry

Chemistry, Multidisciplinary

WOS:001254367600001

WILEY-V C H VERLAG GMBH

20242616440527

Conversion efficiency ; Crystal orientation ; Density functional theory ; Design for testability ; Electric fields ; Germanium ; Harmonic generation ; Hybrid materials ; Nonlinear optics ; Optical materials ; Perovskite ; Photoluminescence spectroscopy ; Polarization ; X ray photoelectron spectroscopy

Minerals:482.2 ; Energy Conversion Issues:525.5 ; Nonferrous Metals and Alloys excluding Alkali and Alkaline Earth Metals:549.3 ; Electricity: Basic Concepts and Phenomena:701.1 ; Nonlinear Optics:741.1.1 ; Optical Devices and Systems:741.3 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4 ; Crystalline Solids:933.1 ; Crystal Lattice:933.1.1 ; Optical Variables Measurements:941.4

CHEMISTRY

Web of Science

1.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
2.Sun Yat Sen Univ, Sch Chem, MOE Key Lab Bioinorgan & Synthet Chem, Guangzhou 510275, Guangdong, Peoples R China
3.Southern Univ Sci & Technol, Dept Elect & Elect Engn, Shenzhen 518055, Guangdong, Peoples R China
4.Univ Texas Dallas, Dept Mat Sci & Engn, Richardson, TX 75080 USA

Guo, Zhu,Han, Dingchong,Liu, Huan,et al. Controlling the Orientation-Dependent Second Harmonic Generation in Hybrid Germanium Perovskites[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2024,63.

Guo, Zhu.,Han, Dingchong.,Liu, Huan.,Hu, Yaoqiao.,Zhang, Weixiong.,...&Mao, Lingling.(2024).Controlling the Orientation-Dependent Second Harmonic Generation in Hybrid Germanium Perovskites.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,63.

Guo, Zhu,et al."Controlling the Orientation-Dependent Second Harmonic Generation in Hybrid Germanium Perovskites".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63(2024).