Theoretical Investigations on Surface Enhanced Raman Spectroscopy and Interfacial Electrochemistry

固体-溶液或固体-气体界面是多相化学反应的主要场所，故界面化学是长期受到重视的一个重要的科学技术领域。因为吸附在界面的分子能显著地改变界面的性质，其分子吸附行为一直是该领域的重点研究内容，各种新的实验技术和理论方法被不断地引进和运用到这一领域，以期在分子和原子水平对复杂的分子吸附行为进行深入的探讨。表面增强拉曼光谱(SERS)和电化学技术是二类重要的原位实验手段，但是从实验结果直接推测界面分子的结构细节仍然存在难度，往往需要结合理论模拟来确定界面的结构。在前人所建立的模型的基础上，本论文对有关SERS和界面电化学二类不同体系分别提出了新的理论模型，使之能够更好地模拟实验的真实情况，从而在分子层...Since many heterogeneous chemical reactions take place at solid-liquid or solid-gas interfaces, there is no doubt that interfacial chemistry is an important branch of science and technology that has attracted intensive attention for a long time. Adsorbed molecules can change the properties of interfaces significantly. Hence, the study of adsorptions is a key issue in interfacial chemistry. Various...学位：理学博士院系专业：化学化工学院化学系_物理化学(含化学物理)学号：B20042503

DFT理论探讨银电极表面吸附吡啶和水分子的表面增强拉曼光谱

本文利用密度泛函方法计算了吡啶和水分子分别吸附于粗糙银电极表面的拉曼光谱强度。结果表明,在不发生共振拉曼散射情况下,拉曼强度随电极表面负电荷量的增加而显著增大。理论预测与实验结果一致

Epitaxial growth of heterogeneous metal nanocrystals: From gold nano-octahedra to palladium and silver nanocubes

通讯作者地址: Xie, ZX (通讯作者), Xiamen Univ, State Key Lab Phys Chem Solid Surfaces, Xiamen, Peoples R China 地址: 1. Xiamen Univ, State Key Lab Phys Chem Solid Surfaces, Xiamen, Peoples R China 2. Xiamen Univ, Dept Chem, Coll Chem & Chem Engn, Xiamen, Peoples R China 电子邮件地址: [email protected], [email protected] octahedral Au nanocrystals as seeds, highly monodisperse Au@Pd and Au@Ag core-shell nanocubes were synthesized by a two-step seed-mediated method in aqueous solution. Accordingly, we have preliminarily proposed a general rule that the atomic radius, bond dissociation energy, and electronegativity of the core and shell metals play key roles in determining the conformal epitaxial layered growth mode

Observation of inhomogeneous plasmonic field distribution in a nanocavity

等离激元材料和器件中电场的强度分布是等离激元技术及其应用的重要基础。虽然针尖增强光谱成像技术的发展已经实现了亚纳米的横向空间分辨率，并发现了亚纳米级电场的不均匀性，但是迄今人们对电场的纵向场强分布仍然知之甚少。李剑锋教授课题组设计了一种具有~2Å空间分辨率的分子尺，利用金单晶基底和壳层隔绝金纳米粒子来构筑等离激元纳米腔，并通过分子尺的拉曼信号强度，精准地直接表征纳米腔中的纵轴方向上高度不均匀的场强分布。中国科学技术大学罗毅教授课题组利用基于量子场论的局域场光谱理论，精确地模拟得到了与实验相符的等离激元纳腔中的场分布，并发现了因分子自聚焦作用而引起的“等离激元梳”。该工作提供了一种通用有效的定量表征纳腔中场强分布的方法，完善了对等离激元学基础的理解，为超高空间分辨的拉曼光谱成像、光学力调控分子组装、单分子反应操控提供指导。 该工作是在李剑锋教授和中国科学技术大学罗毅教授共同指导下完成的。实验部分主要由李超禹（论文第一作者，已毕业博士）、温宝英（在读博士）、李松波（已毕业硕士）完成，复旦大学段赛研究员（论文共同第一作者）和陈舒（已毕业博士）进行了局域场光谱理论计算。谢立强（已毕业博士）和毛秉伟教授帮助完成了扫描探针显微镜实验。浙江师范大学周小顺教授和王亚浩老师提供了自组装膜表征方面的重要帮助。印度的Kathiresan、叶龙武教授课题组和浙江大学陆展教授课题组在分子合成方面提供了重要帮助。瑞士伯尔尼大学Wandlowski教授和田中群教授为该工作提供了指导。【Abstract】The progress of plasmon-based technologies relies on an understanding of the properties of the enhanced electromagnetic fields generated by the coupling nanostrucutres.Plasmon-enhanced applications include advanced spectroscopies, optomechanics, optomagnetics and biosensing. However, precise determination of plasmon field intensity distribution within a nanogap remains challenging. Here, we demonstrate a molecular ruler made from a set of viologen-based, self-assembly monolayers with which we precisely measures field distribution within a plasmon nanocavity with ~2-Å spatial resolution. We observed an unusually large plasmon field intensity inhomogeneity that we attribute to the formation of a plasmonic comb in the nanocavity. As a consequence, we posit that the generally adopted continuous media approximation for molecular monolayers should be used carefully.The progress of plasmon-based technologies relies on an understanding of the properties of the enhanced electromagnetic fields generated by the coupling nanostrucutres1,2,3,4,5,6. Plasmon-enhanced applications include advanced spectroscopies7,8,9,10, optomechanics11, optomagnetics12 and biosensing13,14,15,16,17. However, precise determination of plasmon field intensity distribution within a nanogap remains challenging. Here, we demonstrate a molecular ruler made from a set of viologen-based, self-assembly monolayers with which we precisely measures field distribution within a plasmon nanocavity with ~2-Å spatial resolution. We observed an unusually large plasmon field intensity inhomogeneity that we attribute to the formation of a plasmonic comb in the nanocavity. As a consequence, we posit that the generally adopted continuous media approximation for molecular monolayers should be used carefully.The Swedish National Infrastructure for Computing is acknowledged for computer time. S.D. is sponsored by Shanghai Pujiang Programme (grant no. 19PJ1400600). 该研究工作得到国家自然科学基金、国家重点研发计划、安徽省量子信息技术引导专项等的资助和支持

光学元件表面灰尘位置测试装置

本实用新型涉及一种光学元件表面灰尘位置测试装置，该测试装置包括激光器、取样单元以及测试单元；激光器、取样单元以及测试单元设置在同一光路上。本实用新型提供了一种具有定位准确，工作效率高，自动化程度高，使用方便的光学元件表面灰尘位置测试装置

大口径取样光栅取样率的测试装置

本实用新型涉及一种大口径取样光栅取样率的测试装置，该大口径取样光栅取样率的测试装置包括激光器、分束镜、第一积分球功率计、第二积分球功率计、用于对大口径取样光栅进行扫描的二维扫描镜组以及控制与采集处理系统；分束镜设置于激光器的出射光路上；第一积分球功率计置于经分束镜的透射光路上；二维扫描镜组置于经分束镜的反射光路上；第二积分球功率计置于经二维扫描镜组后透过被测取样光栅的-1级衍射光路上；第一积分球功率计以及第二积分球功率计分别与控制与采集处理系统相连。本实用新型提供了一种可解决大口径取样光栅取样率的测试问题，并很好的保证了测试精度的大口径取样光栅取样率的测试装置