International Collaboration in Chemistry: A Theoretical Investigation Of The Role Of The Chemical Bond In The Raman And Fluorescence Response Of Molecule-Nanoparticle Hybrids

国际化学合作：化学键在分子-纳米颗粒杂化物拉曼和荧光响应中作用的理论研究

• 批准号: 1124895
• 负责人: Vladimiro Mujica
• 金额: $ 40万
• 依托单位: Arizona State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2011
• 资助国家: 美国
• 起止时间: 2011-09-01 至 2015-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1124895&HistoricalAwards=false
• 关键词: International; Collaboration; Chemistry; Theoretical; Investigation

Vladimiro Mujica at Arizona State University is funded by the Chemical Theory, Models and Computational Methods program in an International Collaboration in Chemistry, with partners Arne Keller at the University of Paris in Orsay as well as Osman Atabek and Monica Calatayd all funded by France's Agence Nationale de la Recherche. This is co-funded by the NSF Office of International Science and Engineering (OISE). This project aims at a theoretical investigation of the influence of the chemical bond between a molecule and a semiconducting nanoparticle on the Raman and fluorescence responses of these hybrid systems. These processes must be jointly considered, as the excitation and decay pathways become interdependent due to the appearance of midgap states, induced by the formation of the chemical bond and interfacial charge transfer that play a fundamental role in both photoexcitation and electron injection into the nanoparticle. This involves the calculation of the cross section for both Raman scattering and fluorescence, based on the properties of the time-correlation function of the effective dipole moment of the system. The emphasis is on processes that are resonant in the hybrid but not in the separate components, due to the reduction of the energy gap for electron excitation. Laser photoexcitation simultaneously provokes the creation of an electron-hole exciton and probes the Raman and fluorescence responses.By developing reliable procedures to predict the light that emerges when laser light shines on these molecule-nanoparticle hybrid systems, greater understanding will be obtained of the fundamental physical and chemical processes in bio-sensors and also in solar cells and photocatalysis. These three areas are crucial for energy and health-related research and for the technological implementation of new photovoltaic devices and sensors. The project involves a strong international scientific cooperation between teams of researchers in France and the U.S and it also contemplates active collaboration with experimental groups and human resources formation.

亚利桑那州立大学的Vladimiro Mujica由国际化学合作中的化学理论，模型和计算方法项目资助，合作伙伴阿恩凯勒在奥赛的巴黎大学，以及奥斯曼阿塔贝克和莫妮卡卡拉塔德都由法国国家研究机构资助。 该项目由NSF国际科学与工程办公室（OISE）共同资助。 本计画旨在从理论上探讨分子与半导体奈米粒子之间的化学键对这些混合系统的拉曼与萤光反应的影响。这些过程必须共同考虑，因为激发和衰变途径变得相互依赖，由于midgap状态的出现，诱导的化学键和界面电荷转移，在光激发和电子注入到纳米粒子中发挥了重要作用的形成。这涉及到拉曼散射和荧光的截面的计算，基于系统的有效偶极矩的时间相关函数的属性。重点是在混合动力中共振的过程，但不是在单独的组件，由于电子激发的能隙的减少。激光光激发同时激发电子-空穴激子的产生并探测拉曼和荧光响应。通过开发可靠的方法来预测激光照射这些分子-纳米颗粒混合系统时出现的光，将更好地理解生物传感器以及太阳能电池和微电子器件中的基本物理和化学过程。这三个领域对于能源和健康相关研究以及新光伏器件和传感器的技术实施至关重要。该项目涉及法国和美国研究人员团队之间强有力的国际科学合作，还考虑与实验小组和人力资源形成积极合作。