Relaxation, Coherence, and Optical Control of Time-Dependent Molecular Condensed-Phase Dynamics

Jeffrey Cina得到了理论和计算化学计划的资助，继续他在含时凝聚相分子系统的相干性和光学控制领域的理论研究。CINA致力于发展一种全面的超短脉冲传播子理论，这将有助于模拟各种时间分辨的非线性光学实验，并为进一步发展分子和固体的光学控制提供有用的工具。影响分子内和分子间电子和能量转移速率的各种弛豫过程也将被研究。要研究的具体弛豫包括那些显示出电子基态的相干变化的松弛；那些具有电子基态大小或形状变化的松弛；以及那些涉及经典可区分的分子内或主体-介质组态之间的长程叠加的松弛。这项拟议的工作将使用形式分析理论和计算模拟相结合的方法，并将与几个实验小组直接合作。超短激光脉冲提供了一种强大的手段，可以将物质置于远离热平衡的异常状态。这些状态可能具有不寻常的化学或材料性质，与凝聚态物质在更正常状态下的性质大不相同。这项赠款下的工作涉及探索这些不寻常状态的性质以及如何准备它们和如何检测它们的理论研究。这项工作是在与进行相关实验研究的人密切和直接接触的情况下进行的。通过这种方式，从理论工作中得到的理解将在短期内应用于实验数据的分析和解释。

Jeffrey Cina is supported by a grant from the Theoretical and Computational Chemistry Program to continue his theoretical research in the area of coherence and optical control of time-dependent condensed-phase molecular systems. Cina seeks to develop a comprehensive theory of ultrashort-pulse propagators that will facilitate the simulation of a wide variety of time-resolved nonlinear optical experiments and provide a useful tool for the further development of optical control of molecules and solids. Various types of relaxation processes that influence the rate of electron- and energy-transfer within and between molecules will also be investigated. Specific relaxations to be investigated include those exhibiting coherent changes in the electronic ground state; those featuring large-amplitude size or shape changes in the electronic ground state; and those involving long-range superpositions between classically distinguishable intra-molecular or host-medium configurations. The proposed work will use a combination of formal analytical theory and computational simulation, and will involve a direct collaboration with the several experimental groups.Ultra-short pulses of laser light provide a powerful means to place matter into unusual states, far from thermal equilibrium. These states may have unusual chemical or material properties quite different from those of condensed matter in its more normal states. The work under this grant involves theoretical studies which explore the properties of these unusual states as well as how they may be prepared and how they may be detected. The work is being carried out in close and direct contact with people who are making related experimental studies. In this way, the understanding coming from the theoretical work is being applied, in the near term, to the analysis and interpretation of experimental data.