NER: Modeling Quantum-coherent Electronic Excitations in Functionalized Semiconductor Nanostructures

这项研究的目的是继续发展描述扩展半导体纳米结构中量子动力学的方法，并应用这些方法来探索与纳米结构中电子激发行为相关的各种量子动力学现象。这些目标包括探索在固定在二氧化钛纳米结构上的有机分子的无序排列中产生和操作相干电子激发的可行性，重点是量子纠缠、退相干和条件量子动力学方案的研究。这种方法结合了大规模从头计算分子动力学模拟和基于紧束缚方法得到的模型哈密顿量的电子弛豫量子动力学模拟。半导体纳米结构中的量子动力学研究对于各种各样的系统来说是重要的，并且仍然是一个开放的问题。该研究计划的重点是模拟有机分子中电子激发的量子动力学，使二氧化钛纳米结构功能化。然而，由此产生的理论进展将具有更广泛的适用性，包括许多其他具有常见电子激发的功能化纳米结构。拟议研究的影响可能超越对所调查的模型系统的理解，涉及从高效太阳能转换电池的设计到光催化分解含有大量二氧化钛的土壤中的污染物(例如有机物质)的问题。此外，该项目还将通过为各个学术部门的学生创造一个多学科的前沿研究机会，自然会扩大少数族裔在科学领域的参与度，并使耶鲁大学的教育基础设施受益。

The objective of this research is the continued development of methods to describe quantum dynamics in extended semiconductor nanostructures, and the application of these methods to explore a variety of quantum dynamical phenomena associated with the behavior of electronic excitations in nanoscale structures. These objective includes exploring the feasibility of creating and manipulating coherent electronic excitations in disordered arrangements of organic molecules anchored to TiO2 nanostructures, with emphasis on studies of quantum entanglement, decoherence and schemes for conditional quantum dynamics. The approach is a combination of large-scale ab-initio molecular dynamics simulations with quantum dynamics simulations of electronic relaxation based on model Hamiltonians gained from a tight binding approach.The study of quantum dynamics in semiconductor nanostructures is important for a huge variety of systems and remains an open problem. The emphasis of the research program is on modeling quantum dynamics of electronic excitations in organic molecules functionalizing TiO2 nanostructures. However, the resulting theoretical advances will have a much wider applicability, including many other functionalized nanostructures with common electronic excitations. The implications of the proposed studies will likely extend beyond an understanding of the model systems investigated to problems that range from the design of efficient solar energy conversion cells to the problem of photocatalytic decomposition of pollutants (e.g., organic material) in soil with significant TiO2 content. In addition, the program will naturally broaden the participation of underrepresented minorities in the sciences and benefit the educational infrastructure at Yale by creating a multi-disciplinary frontier research opportunity for students from various academic departments.