Molecular photochemistry and laser control: From small molecules to fluorescent proteins

自从激光发明以来，人们的一个愿景就是用它在分子尺度上操纵物质。在过去的25年里，使用定制的（成形的）激光场来控制原子和分子已经变得非常成熟。这一进展在一定程度上是由波长从中红外到紫外的成形激光源的发展所推动的。这些技术创新使得激光控制的各种各样的过程被证明，例如，振转和/或电子态布居转移、光异构化、光解离。最近，来自激光控制的想法刺激了探测分子动力学和潜在分子结构的新方法的发展-所谓的量子控制光谱学。对这些实验的一个重要补充，往往也是灵感的来源，是发展新的理论来理解导致控制的机制。这些理论必须通过复杂的计算机模拟来验证和测试。拟议的研究将开发新的理论和计算工具，用于预测和理解光化学和光谱过程的控制。特别是，我们感兴趣的新方法来解决控制问题的大分子-一个具有挑战性的任务，由于激光控制的量子力学性质。

Since the invention of the laser, one of the visions has been to use it to manipulate matter on the molecular scale. Over the last 25 years, the use of tailored (shaped) laser fields to control atoms and molecules has become well-established. This progress has been driven, in part, by the development of shaped laser sources with wavelengths from the mid-infrared to the ultraviolet. These technical innovations have allowed laser control of a wide variety of processes to be demonstrated, e.g., rovibrational and/or electronic state population transfer, photoisomerization, photodissociation. More recently, ideas from laser control have spurred the development of new methods for probing molecular dynamics and the underlying molecular structure - so-called quantum control spectroscopy. An important complement, and often a source of inspiration, to these experiments is the development of new theories for understanding the mechanisms leading to control. These theories must be validated and tested through sophisticated computer simulations. The proposed research will develop new theoretical and computational tools for predicting and understanding the control of photochemical and spectroscopic processes. In particular, we are interested in new methods to tackle control problems in large molecules - a challenging task due to the quantum mechanical nature of laser control.