全椅式边含薁缺陷石墨烯纳米片的二阶非线性光学性质  

The Second Order Nonlinear Optical Properties of Azulene-defect Graphene Nanosheets with Full Armchair Edge

作　　者：郑雪莲[1,2] 杨翠翠 田维全 ZHENG Xuelian;YANG Cuicui;TIAN Weiquan(College of Chemistry and Chemical Engineering,Mianyang Normal University,Mianyang 621000,China;Chongqing Key Laboratory of Theoretical and Computational Chemistry,College of Chemistry and Chemical Engineering,Chongqing University,Chongqing 401331,China)

机构地区：[1]绵阳师范学院化学与化学工程学院,绵阳621000 [2]重庆大学化学化工学院,理论与计算化学重庆市重点实验室,重庆401331

出　　处：《高等学校化学学报》2022年第3期104-111,共8页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号:21673025);超分子结构与材料国家重点实验室开放课题(批准号:SKLSSM2021020);多酸与网格材料化学教育部重点实验室开放课题资助。

摘　　要：基于全椅式边石墨烯纳米片(GNSs),在保证GNSs化学稳定性的前提下并考虑了纳米片形状(六边形、三角形和平行四边形),在全椅式边GNSs中分别引入2,3和4个薁构成的常见本征缺陷来调节这些GNSs的二阶非线性光学性质.研究结果表明,薁缺陷数量对于这些GNSs的二阶非线性光学响应起主导作用.含有4个薁缺陷的GNSs具有较大的二阶非线性光学响应,其中AP-4a纳米片具有最大的静态第一超极化率(<β;>,230387.70 a.u.,平均每个重原子的<β;>为2260.42 a.u.).纳米片形状对体系的二阶非线性光学响应也有一定的影响.薁单元片段在GNSs中不仅诱导GNSs发生电荷分布极化,而且还在对非线性光学响应起重要贡献的主要电子跃迁中起主要作用.薁单元作为碳基纳米材料的功能单元极大改善了其光电性质.Based on the graphene nanosheets(GNSs)with full armchair edge,the second order nonlinear optical properties of these GNSs in different shapes with good chemical stability were modulated by introducing two,three and four azulenes.The result shows that the number of azulene defects plays a dominant role in the second order nonlinear optical responses of these GNSs.The GNSs with four azulenes have large second order nonlinear optical responses,among which AP-4a has the largest static first hyperpolarizability(<β;>,230387.70 a.u.,2260.42 a.u.per heavy atom).In addition,the nanosheet shape also has a certain effect.The azulene moieties not only induce charge distribution polarization of GNSs,but also dominate in the major electron transitions with important contribution to the nonlinear optical responses.Azulene as a functional unit of carbon-based nanomaterials significantly improves the photoelectric properties of carbon-based nanomaterials,and this finding provides practical strategies and useful information for future carbon-based nonlinear optical materials design.

关 键 词：全椅式边石墨烯纳米片 薁缺陷 纳米片形状 二阶非线性光学性质 功能单元 

分 类 号：O641[理学—物理化学]