Dissipative quantum dynamics and response of adsorbates on solid surfaces

这个项目的目标是发展新的理论和计算方法来描述固体表面局域分子现象的耗散动力学和光谱，其中电子激发和原子重排是由碰撞或光吸收引起的。感兴趣的现象是激发电子在纳米结构半导体表面的光致飞秒动力学(瞬变光谱、电子转移、电荷分离和电流)，以及被吸附的团簇的光致异构化和光解离。具体的应用包括吸附在硅表面的银团簇，以及掺有III族和V族元素的系统。这项工作的影响包括光伏和光电电极新材料设计的基本特征。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生物分子的动力学和光生物学(如视觉、光合作用和组织的辐射损伤)。此外，这些方法与表面物种的拉曼增强光谱有关。将组织国际会议，以整合研究生的研究和教育，并传播跨学科研究。研究成果与佛罗里达大学的其他教职员工合作被纳入研究生课程。对本科生的指导包括代表人数不足的群体，并积极开展有关该理论的数学方面的博士后助理培训。该奖项由化学部的理论模型和计算方法项目资助。

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.