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

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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.