Project B1: Optical Spectroscopy of Condensed-Phase (Hetero-) Diamondoid Systems

本项目研究功能化金刚石团簇宽带发射的光子特性，这一方面与确定其基本微观起源有关，另一方面与在器件应用中的实现有关。后者是光束参数，如光谱光度，包括其角度分布，时间相干性和空间相干性，以及发射的亮度。这些数据将用于通式[(RT)4M6] （R =有机配体；T =例如Sn或C； M =例如S或C）的模型功能化金刚烷型团簇体系，该体系最易于处理和处理。目前，主要的候选材料是溴功能化金刚烷。在这里，光化学非晶化被证明是特别成功的Br2Ph2Ad；但是，该项目将对FOR 2824的其他项目的持续发展作出反应。理想情况下，这些数据可以用于确定介观结构-性质关系，即在光学长度尺度上。由于这些化合物可以采用不同程度的结晶度，因此将建立结构材料性质与光子量的相关性。研究配体中（例如）电子系统与分子主链的耦合进一步阐明了发射过程的性质。特别是，在这些系统中，电子温度和晶格温度的任何潜在的平衡行为和玻恩-奥本海默近似的有效性将被探索，以澄清，在多大程度上-如果有的话-连续体发射的起源是热的。这将有助于通过光谱手段对观测到的光学非线性的起源和性质的微观理解，即监测振动激发，包括它们的时间演变，并澄清单个分子的电子激发之间的过渡在多大程度上起作用。

This project studies the photonic properties of the broadband emission in functionalized diamondoid clusters which are relevant for the identification of its fundamental microscopic origin on the one hand and for the implementation into device applications on the other. The latter, in particular, are the optical beam parameters like the spectral luminosity including its angular distribution, the temporal coherence as well as the spatial coherence, and the brilliance of the emission. These data will be acquired for a model functionalized adamantane-type cluster system of the general formula [(RT)4M6] (R = organic ligand; T = e.g., Sn or C; M = e.g., S or C), which can be handled and processed most easily. Currently, the prime candidates are bromine functionalized adamantanes. Here, photochemical amorphization has proved particularly successful for Br2Ph2Ad; however, the project will react to the ongoing developments in the other projects of FOR 2824. Ideally, these data lead to the identification of the mesoscopic structure-property relationship, i.e., on optical length scales. As these compounds can adopt varying degrees of crystallinity, the correlation of the structural materials properties with the photonic quantities will be established. Studying the coupling of the (e.g., ) electron systems in the ligands to the backbone of the molecules further clarifies the nature of the emission process. In particular, any potential equilibration behaviour of the electronic temperature and the lattice temperature and validity of the Born-Oppenheimer approximation in these systems will be explored to clarify, to what extent – if any – the origin of the continuum emission is thermal. This will contribute to the microscopic understanding of the origin and nature of the observed optical nonlinearities by spectroscopic means, i.e., monitoring vibrational excitations including their time evolution and clarify, to what extent transitions between electronic excitations of the individual molecules contribute.