Dynamics in Molecular Solid State Systems

分子固态系统中动力学和分子间相互作用的研究。利用皮秒和亚皮秒非线性实验，结合超高分辨率光谱学、常规光谱学和理论，研究了晶体和玻璃中的分离分子、杂质带体系中的弱相互作用分子和纯晶体激子体系中的强相互作用分子。在玻璃中，通过将光子回波和其他光学相干实验与光学烧孔实验、声学测量和热容相结合，出现了这些非平衡系统中动力学和分子间相互作用的新的详细图像。在杂质带问题中，光子回波实验可以直接观察到混合晶体系统中电子激发的浓度依赖离域。用一种产生具有明确相位关系的皮秒脉冲的新方法，描述了相位相关脉冲序列，特别是光偶极回波，在杂质带问题中的应用。讨论了皮秒瞬态光栅技术在纯分子晶体中激子输运和极化子效应研究中的应用。利用光子回波实验和偏振光栅技术相结合的方法，研究了光减相观察到的分子力学运动与电子态耦合之间的关系。

An investigation of dynamics and intermolecular interactions in molecular solid state systems. Picosecond and subpicosecond nonlinear experiments combined with ultrahigh resolution spectroscopy, conventional optical spectroscopy and theory are used to study isolated molecules in crystals and glasses, weakly interacting molecules in impurity band systems, and strongly interacting molecules in pure crystal exciton systems. In glasses by combining photon echo and other optical coherence experiments with optical holeburning experiments, acoustic measurements and heat capacities, a new and detailed picture of dynamics and intermolecular interactions in these nonequilibrium systems is emerging. In the impurity band problem, photon echo experiments are shown to be a direct observable for the concentration dependent delocalization of electronic excitations in mixed crystal systems. The application of phase related pulse sequences, particularly the optical dipolar echo, to the impurity band problem is described using a new approach for generating picosecond pulses with well defined phase relationships. The applications of picosecond transient grating techniques to the investigation of exciton transport and polariton effects in pure molecular crystals are discussed. A combination of photon echo experiments and polarization grating techniques are used to examine the relationship between the mechanical motions of molecules and coupling to electronic states as observed by optical dephasing.