LaserLaB Amsterdam and Department of Chemistry, Vrije Universiteit, de Boelelaan 1083, 1081 HV Amsterdam, The Netherlands.
Chemphyschem. 2011 Jun 6;12(8):1459-73. doi: 10.1002/cphc.201100107. Epub 2011 Apr 19.
Herein, we review the current capabilities and potential of advanced single-particle imaging techniques to study photodynamics in isolated molecules. These reaction microscopes are able to measure the full three-dimensional energy and angular distribution of (correlated) particles such as electrons and molecular fragments ejected after photoexcitation of molecules. In particular, we discuss the performance and capabilities of a novel photoelectron-photoion coincidence imaging spectrometer constructed at LaserLaB Amsterdam. This microscope was developed for the study of nonadiabatic effects in ultrafast time-resolved experiments. It is specifically targeted at optimal control studies of photodynamics to foster and advance our understanding of mechanisms in optimal control with shaped ultrafast laser pulses. We review a few recent experimental results illustrating the wealth of detailed information that can be obtained in such imaging experiments about the interplay between (shaped) laser fields, molecular dynamics, ionization processes and competing multichannel pathways. Furthermore, the recently developed photoelectron-circular-dichroism imaging technique to detect enantiomers and to study chirality effects will be discussed, as a further illustration of the potential of modern reaction microscopes in stereochemistry.
在这里，我们回顾了先进的单粒子成像技术在研究孤立分子光动力学方面的现有能力和潜力。这些反应显微镜能够测量分子光激发后发射的（相关）电子和分子碎片等粒子的全三维能量和角分布。特别是，我们讨论了在阿姆斯特丹激光实验室构建的新型光电离-光电离符合成像光谱仪的性能和能力。该显微镜是为超快时间分辨实验中的非绝热效应研究而开发的。它特别针对光动力学的最优控制研究，以促进和推进我们对具有成形超快激光脉冲的最优控制中的机制的理解。我们回顾了一些最近的实验结果，这些结果说明了在这种成像实验中可以获得关于（成形）激光场、分子动力学、电离过程和竞争多通道途径之间相互作用的丰富详细信息。此外，还将讨论最近开发的光电离圆二色成像技术，以检测对映体和研究手性效应，进一步说明了现代反应显微镜在立体化学中的潜力。
