Molecular Radiative and Relaxation Processes

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Shaul Mukamel of the University of California, Irvine is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to study how light and matter interact. Lasers and other light sources are tools with which one can probe, measure, and even control the behavior of molecules. In this project, new ways to interact light with molecules are designed by incorporating the wave properties of light such as phase and polarization. Although the interaction of a single small package (photon) of light with a molecule is quite well understood, multiple photons can be combined into pulses that influence molecules in new ways. These interactions of photons and molecules are best described by quantum mechanics, a the mathematical description of the motion and interaction of subatomic particles, incorporating the concepts of quantization of energy, wave-particle duality, the uncertainty principle, etc. The methods developed in this project will provide new information within this framework. Success in this area could lead to new technologies such as quantum computers. To benchmark the predictions, the project includes extensive collaborations and student exchanges with leading experimental groups all over the world.Professor Mukamel is developing methods to study the response of complex molecules to sequences of ultrafast optical laser pulses that provide a multidimensional view of electronic and vibrational dynamics and correlations. Experimental techniques involving novel pulse sequences are designed. Theoretical and computational tools for their analysis are developed and broadly applied to molecules in the condensed phase. Models and practical computational tools are developed for the interpretation and analysis of these signals. Novel spectroscopic techniques, which make use of the quantum nature of light, photon entanglement and photon coincidence detection are explored. These provide additional tools for probing molecules and chromophore aggregates by providing information that is not accessible by classical light. Detection schemes that combine coincidence measurements of individual entangled photons and interferometry are applied to study the elementary charge and energy migration processes in molecular complexes. Manipulating molecular properties in microcavities (polariton chemistry) and coherent control schemes are employed to optimize and refine nonlinear optical signals.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.