Molecular Radiative and Relaxation Processes

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With support from the Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry, Shaul Mukamel of the University of California, Irvine is developing new methods for studying molecular processes which make use of the quantum nature of light pulses. In particular, Mukamel will explore how the quantum correlation of photons, known as entanglement, which has been extensively studied in quantum computing applications, can be used to control the interaction between molecules and light. The quantum nature of light offers numerous new opportunities for monitoring elementary molecular events through windows that are unavailable by classical light. Models and practical computational tools will be developed for the interpretation and analysis of the proposed measurements. Interpreting the proposed quantum signals will be made by the combination of electronic structure and quantum dynamics simulations with state-of-the-art quantum optics technology. In addition, optical microcavities can manipulate electron and nuclear dynamics by strong light-matter coupling to localized cavity modes, which create hybrid light-matter particles known as polaritons. The collective response of many molecules interacting with the same cavity mode will be investigated. Coherent control schemes will be employed to optimize the proposed nonlinear optical signals. Coincidence measurements of individual entangled photons and quantum interferometry techniques will be employed to probe molecular chirality. Students working on this project will be immersed in frontier research relevant to quantum information science. Also contributing to the broader impacts, Dr. Mukamel will continue to serve an advisory role on the boards of several worldwide research centers in the field of nonlinear ultrafast spectroscopy and quantum light technology.Novel spectroscopic techniques that involve optical cavities and quantum light will be developed and applied to study elementary photophysical and photochemical processes in molecules. Computational techniques that combine nonadiabatic molecular dynamics, wavepacket simulations of quantum nuclear degrees of freedom, and quantum photon statistics will be employed. Pulse shaping, phase control, and chiral polarization configurations will be utilized. Stimulated Raman techniques that can directly probe the passage of molecules through conical intersections in microcavities will be predicted. Engineered states of quantum light developed in quantum optics will be adopted to molecular spectroscopy applications with unprecedented temporal, spectral, and spatial resolutions. The back and forth transfer of entanglement between photons and matter will be used to create new classes of correlated excited states in molecular aggregates. The elementary charge and energy migration processes in molecular aggregates and in photosynthesis will be investigated using the new techniques. These have the potential for broad long-term scientific impact for the design of artificial light harvesting systems that convert sunlight to chemical energy with high efficiency.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.