二次谐波在二维材料结构表征中的应用

doi:10.15541/jim20210074

无机材料学报 ›› 2021, Vol. 36 ›› Issue (10): 1022-1030.DOI: 10.15541/jim20210074 CSTR: 32189.14.10.15541/jim20210074

所属专题：【虚拟专辑】新型材料表征技术(2020~2021)

二次谐波在二维材料结构表征中的应用

夏芳芳¹(), 王发坤¹, 胡海龙², 许翔¹, 李阳¹, 翟天佑¹()

1.华中科技大学材料成形与模具技术国家重点实验室, 材料科学与工程学院, 武汉430074
2.威泰克(北京)科学技术有限公司, 北京100027

收稿日期:2021-02-05 修回日期:2021-03-26 出版日期:2021-10-20 网络出版日期:2021-06-01
通讯作者: 翟天佑, 教授. E-mail: zhaity@hust.edu.cn
作者简介:夏芳芳(1986-), 女, 工程师. E-mail: xiafangfang@hust.edu.cn
基金资助:
国家自然科学基金(21825103)

Application of Second Harmonic Generation in Characterization of 2D Materials

XIA Fangfang¹(), WANG Fakun¹, HU Hailong², XU Xiang¹, LI Yang¹, ZHAI Tianyou¹()

1. State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
2. WITec (Beijing) Scientific Technology Co., Ltd., Beijing 100027, China

Received:2021-02-05 Revised:2021-03-26 Published:2021-10-20 Online:2021-06-01
Contact: ZHAI Tianyou, professor. E-mail: zhaity@hust.edu.cn
About author:XIA Fangfang(1986-), female, engineer. E-mail: xiafangfang@hust.edu.cn
Supported by:
National Natural Science Foundation of China(21825103)

摘要/Abstract

摘要：

二次谐波作为非线性光学的重要分支, 逐渐成为表征晶体结构的重要手段之一。在众多表征方法中, 二次谐波因其无损检测、高稳定性、可调谐性、超快响应、偏振敏感性、通用性、操作简单等特点被广泛应用于二维材料结构表征, 为二维材料的物性研究和功能应用提供了重要信息, 大大推动了二维材料基础研究的快速发展。本文综述了近几年二次谐波在二维材料结构表征中的研究, 简述了二次谐波产生原理, 介绍了飞秒激光器接入共聚焦拉曼光谱仪产生二次谐波测试装置, 分别讨论了二次谐波在二维材料的层间堆垛层数、层间堆垛角度、单层二维材料晶界及晶体取向表征方面的应用。同时, 本文还介绍了采用二次谐波强度直接、灵敏地检测晶体中应变幅度以及通过二次谐波信号变化跟踪材料中的缺陷变化, 接着讨论了二次谐波与拉曼光谱、光致发光的多维度关联分析在材料全面深度表征方面的重要性。最后展望了二次谐波未来在材料结构表征中的潜在研究方向。

关键词: 二次谐波, 二维材料, 非线性光学, 结构表征, 综述

Abstract:

As an important branch of nonlinear optics, second harmonic generation (SHG) is becoming one of the most important means to characterize crystal structure. Among various methods of characterization, because of nondestructive detection, high stability, tunability, ultrafast response, polarization sensitivity, versatility and simplicity, SHG is widely used to characterize the structure of two-dimensional (2D) materials. It provides important information for the physical properties and functional applications of 2D materials, as well as greatly promotes the rapid development of basic research on 2D materials. Here, the current state of the art focuses on the recent research work of SHG in 2D material structure characterization. Firstly, the principle of the second harmonic generation is briefly introduced. Then, the second harmonic generation device with femtosecond laser connected to confocal Raman spectrometer is taken as an example to present the mechanism of SHG. Afterwards, the applications of SHG are demonstrated in the thickness of interlayer stacking of 2D materials, the stacking angle between different layers of 2D materials, the grain boundary and the crystal orientation of monolayer 2D materials. The second harmonic intensity is used as a direct and sensitive means to monitor the strain amplitude, and the SHG signal changes are used to track defects in materials. Meanwhile, the importance of multi-dimensional correlation analysis of second harmonic generation, Raman spectroscopy and photoluminescence in comprehensive and in-depth characterization of materials is also explored. Finally, the potential research directions and prospects based on SHG in material characterization in the future is prospected.

Key words: second harmonic generation, two dimensional materials, nonlinear optics, structural characterization, review

中图分类号:

TQ174

夏芳芳, 王发坤, 胡海龙, 许翔, 李阳, 翟天佑. 二次谐波在二维材料结构表征中的应用[J]. 无机材料学报, 2021, 36(10): 1022-1030.

XIA Fangfang, WANG Fakun, HU Hailong, XU Xiang, LI Yang, ZHAI Tianyou. Application of Second Harmonic Generation in Characterization of 2D Materials[J]. Journal of Inorganic Materials, 2021, 36(10): 1022-1030.

图/表 9

图1 二次谐波产生原理示意图[24]

Fig. 1 Schematic diagram illustrating of the principle of SHG[24]

图2 二次谐波产生装置示意图和实物图

Fig. 2 Schematic diagram and picture of the experimental setup of SHG

图3 二次谐波表征不同堆垛层数的二维层状晶体

Fig. 3 Characterization of 2D layered crystals with different stacking layers by SHG (a) Side view and top view of atomic structure illustration of typical layered WS2 with 2H and 3R stacking; (b-c) Optical images of 2H and 3R phase WS2; (d-e) SHG intensity of 2H and 3R phase WS2 as a function of layer numbers[40]; (f) SHG intensity of 2H and 3R phase MoS2 as a function of layer numbers[41]

图4 二次谐波表征层间堆垛角度

Fig. 4 Characterization of stacking angle between layers by SHG (a) Schematic of SHG process in second harmonic generation of bilayer thin film; (b) Atomic structure of artificially stacked bilayer; (c-d) Optical images for stacked bilayers with different stacking angles and their corresponding SH intensities[42]

图5 二次谐波表征二维材料晶界及晶体取向

Fig. 5 Characterization of the grain boundary and crystal orientation of two-dimensional materials by SHG (a-b) Optical image and SHG image of a polycrystalline monolayer of MoS2 of the same area; (c) Polarized-SHG image showing the crystal orientations[43]; (d) Dark-field SHG imaging of a monolayer MoSe2[44]

图6 二次谐波表征晶界及晶粒的形成机理

Fig. 6 Characterization of the grain boundary by SHG and analysis of grain formation mechanism (a) Optical image and SHG mapping of the flake with boundary; Inset: illustration of the two edges growth at the boundary; (c) Illustration of the armchair directions of the two grains[24]

图7 二次谐波表征二维材料应变

Fig. 7 Characterization of the strain of 2D materials by SHG (a) Schematic of strain apparatus and SHG process in monolayer MoSe2 under uniaxial tensile strain; (b) SHG spectra under different strain; (c) Evolution of normalized SHG intensity with strain[46]; (d, e) Schematic illustration of two-point bending method and SHG patterns for applied tensile strains of 0.1%, 0.5%, and 0.95%[47]

图8 二次谐波表征二维材料的缺陷

Fig. 8 Characterization of the defects of 2D materials by SHG (a-c) Optical image, fluorescence image and second harmonic mapping image of monolayer WS2[51]

图9 二次谐波与光致发光、拉曼光谱联合表征二维材料(MoS2/WS2异质结)

Fig. 9 Characterization of 2D materials (MoS2/WS2 heterojunction) by SHG combined with photoluminescence and Raman spectroscopy (a) Atomic structure diagram; (b-c) Optical image and TEM image; (d, g) SHG intensity and mapping; (e, h) photoluminescence spectra at different positions; (f, i) Corresponding Raman spectra[52]

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二次谐波在二维材料结构表征中的应用

Application of Second Harmonic Generation in Characterization of 2D Materials

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