Studies of electronic excitations in functionalized semiconductor materials

该项目继续发展计算方法来研究半导体纳米结构中的电子激发。全原子模拟将研究超快量子动力学现象和分子吸附表面光致电子激发的相干控制，用于太阳能转换。这些项目包括电子-空穴对分离和复合路径的表征，用于激光操纵电子激发的光激发方法，光诱导电子动力学和陷阱机制，以及拟议的研究与针对少数族裔学生的外展教育计划的整合，以及与南美洲研究小组的合作。在功能化半导体全原子化模型中，界面电子转移的控制和校正结合了基于大规模从头算分子动力学和非平衡态格林？S函数的严格计算方法，以及与广泛实验的直接比较。广泛影响：半导体纳米结构中的量子动力学研究将影响到在分子电子学、光电器件、成像和存储单元以及基于半导体材料的光催化、电化学和人工光合作用等领域的广泛应用。将拟议的研究计划与科学、技术和研究学者(STAR)计划相结合，自然会扩大未被充分代表的少数群体在自然科学领域的参与。通过拟议的维基界面传播研究成果将使整个科学界受益，促进在公共领域迅速交流和分发成果、软件开发和教学材料。

This project continues the development of computational methods to study electronic excitations in semiconductor nanostructures. Fully atomistic simulations will investigate ultrafast quantum dynamical phenomena and coherent control of photoinduced electronic excitations in TiO2, SnO2 and ZnO surfaces functionalized with molecular adsorbates for solar energy conversion. The projects include the characterization of electron-hole pair separation and recombination pathways, photoexcitation methods for laser manipulation of electronic excitations, photoinduced electronic dynamics and trapping mechanisms, and the integration of the proposed research with an outreach educational program for minority students and collaborations with research groups in South America.Intellectual Merit: These studies of quantum electronic relaxation, control and rectification of interfacial electron transfer in fully atomistic models of functionalized semiconductors combine rigorous computational approaches based on large-scale ab initio molecular dynamics and nonequilibrium Green?s function (NEGF) methods as well as direct comparisons with a wide range of experiments.Broad Impact: Studies of quantum dynamics in semiconductor nanostructures will impact a wide range of applications in molecular electronics, photooptic devices, imaging and memory units, as well as photocatalysis, electrochemistry and artificial photosynthesis based on semiconductor materials with common photoinduced electronic excitations. The integration of the proposed research program with the Science, Technology and Research Scholars (STARS) program will naturally broaden the participation of underrepresented minorities in the physical sciences. Dissemination of research findings through the proposed Wiki interface will benefit the whole scientific community, facilitating the rapid exchange and distribution of results, software developments and pedagogical materials in the public domain.