石墨炔的非线性光学特异性研究

Two-dimensional (2D) material is a class of important materials that have attracted broad attention. Graphdiyne is a novel 2D carbon material with both sp- and sp2- hybridized carbon atoms. Because of its special chemical and electronic structures, graphdiyne features rich carbon bonds, extended π-conjugation, chemical stability, and have been widely applied in the fields ranging from photocatalysis, photovoltaic devices, gas/ion seperation, to energy storagy. Graphdiyne has a tunable intrinsic semiconductive band gap, which promises its advanced applications in the field of optoelectronic information and communication technologies. To explore the applications of graphdiyne in these important aspects, it is very important to study the nonlinear optical properties of this novel material. In this proposal, we will systematically study the nonlinear optical properties of grphdiyne 2D materials with distinctive topological structures, by combining the theoretical simulations with controlled material synthesis and ultrafast spectroscopic studies. The second- and third- order optical nonlinearity of graphdiyne and their dependences on the size, edge, and orientation will be studied. We intend to explore the relationship between the nonlinear optical properties and the structures of graphdiyne that is highly related to the band gap of the 2D material. We will attempt to clarify the mechanisms of the assembly of graphdiyne 2D material and their nonlinear optical emission. The research prosed in this project will establish the theoretical basis for the further optimization and functionalization of graphdiyne 2D materials, and will provide technical supports for their wide applications in information and communication technologies.

二维材料是一类被广泛关注的重要材料。石墨炔作为一种新型的二维材料，是第一个以sp和sp2两种杂化态形成的碳同素异形体，因其特殊的化学和电子结构而具有丰富的碳化学键、大共轭体系、优良的化学稳定性，在光催化、光伏器件、气体及离子分离、能源存储等领域得到了广泛应用。石墨炔可调控的半导体特性的本征带隙使其在光电信息等领域具有广阔的应用前景。为开发石墨炔在这些重要领域的应用，其非线性光学基本问题的研究迫在眉睫。本项目从石墨炔二维材料的可控制备入手，结合理论模拟，通过基于飞秒激光的超快速光谱研究，系统考察不同形貌特征的石墨炔二维材料的非线性光学响应，探讨其二阶及三阶非线性光学的尺寸效应、边界效应、取向效应等基本问题，建立其与能带对应的非线性光学构效关系，阐明石墨炔二维材料的组装机理及二阶和三阶非线性发光机制，为石墨炔材料的进一步修饰优化奠定理论基础，并为其在光电子信息等领域的广泛应用提供技术支持。

二维材料因其独特的化学结构和电子特性成为一类被广泛关注的重要材料。石墨炔作为一种新型的二维材料，是第一个以sp和sp2两种杂化态形成的碳同素异形体，因其特殊的化学和电子结构而具有丰富的碳化学键、大共轭体系、优良的化学稳定性，在光催化、光伏器件、气体及离子分离、能源存储等领域得到了广泛应用，尤其是石墨炔可调控的半导体特性的本征带隙使其在光电信息等领域具有广阔的应用前景。为开发石墨炔在这些重要领域的应用，本项目对石墨炔二维材料的线性及非线性光学基本问题进行了系统深入的研究。. 本项目从石墨炔二维材料的可控制备入手，制备合成了不同拓扑结构和形貌特征的石墨炔二维材料及相关碳基及富碳晶态材料。结合理论模拟，通过基于飞秒激光的超快速光谱研究，系统考察了这些新型材料的非线性光学响应，探究了其二阶及三阶非线性光学的与结构之间的构效关系，阐明石墨炔二维材料的组装机理及二阶和三阶非线性发光机制，在此基础上探索了它们在光子二极管器件、超快光子器件、光探测器件、人工突触器件等领域的应用。同时，基于以上研究方法，发展了手性钙钛矿、有机分子晶体等一系列新型非线性光学晶体材料，研究了它们的相变过程及与其依赖的光电和机械性能。本项目研究为石墨炔二维材料及相关碳基及富碳晶态材料的进一步修饰优化奠定理论基础，并为其在光电子信息等领域的广泛应用提供技术支持。