Dissipative quantum dynamics and response of adsorbates on solid surfaces

该项目的目标是发展新的理论和计算方法，以描述固体表面局部分子现象的耗散动力学和光谱，其中电子激发和原子重排由碰撞或光吸收引起。感兴趣的现象是光致飞秒动力学（瞬态光谱，电子转移，电荷分离，和电流）的激发电子在纳米结构的半导体表面，和光异构化和光解的吸附集群。具体应用包括吸附在Si表面上的Ag簇，以及掺杂有III族和V族元素的系统。这项工作的影响包括为光电化学和光电极设计新材料的基本特征。研究结果对利用太阳能发电和生产燃料具有重要意义。所开发的计算方法适用于电子激发的生物分子动力学和光生物学（例如视觉，光合作用和组织的辐射损伤）。另外，这些方法与表面处物质的拉曼增强光谱有关。将组织国际会议，以整合研究和研究生教育，并传播跨学科研究。研究成果与佛罗里达大学的其他教员合作纳入研究生课程。本科生的辅导包括代表性不足的群体和博士后助理的理论数学方面的培训正在积极进行。该奖项由化学部的理论模型和计算方法计划资助。

The objective of this project is development of new theoretical and computational methods to describe the dissipative dynamics and spectra of localized molecular phenomena at solid surfaces, where electronic excitation and atomic rearrangement are induced by collisions or by light absorption. Phenomena of interest are the photoinduced femtosecond dynamics (transient spectra, electron transfer, charge separation, and currents) of excited electrons at a nanostructured semiconductor surface, and the photoisomerization and photodissociation of an adsorbed cluster. Specific applications include Ag clusters adsorbed on Si surfaces, and systems doped with group III and V elements. The impact of the work includes features fundamental for the design of new materials for photovoltaics and photoelectrodes. Findings are of importance in the utilization of solar energy for electricity and fuels production. The computational methods developed are applicable to the dynamics of electronically excited biomolecules and photobiology (e.g vision, photosynthesis, and radiation damage of tissue). Additionally, these methods are relevant to Raman enhanced spectroscopy of species at surfaces. International conferences are to be organized to integrate research and education of graduate students and to disseminate interdisciplinary research. Research results are incorporated in graduate courses in collaboration with other faculty members at the University of Florida. Mentoring of undergraduate students includes underrepresented groups and training of postdoctoral associates on mathematical aspects of the theory is actively pursued. This award is funded by the Theory Models and Computational Methods program of the Chemistry Division.