Coherence represents a phenomenon that involves phase and/or amplitude relationships among distinct entities. Classical coherence is reflected in experiences we are actually all familiar with, e.g., the beat pattern that arises between the turning signals of two cars at a stoplight blinking at slightly different frequencies. When applied to chemical-based systems, coherence is quantum mechanical in that the correlation exists among electronic, nuclear, and/or vibrational degrees freedom of molecules or ensembles. While the experimental observation of coherence is intrinsically interesting - it is literally an observable manifestation of quantum mechanics - coherence is also providing us with information about the molecule, information that could potentially be used to understand and ultimately control chemical behavior at the molecular level. Our focus has been on coherence in excited-state dynamics, specifically in the form of vibronic coherence where electronic and vibrational degrees of freedom are coupled in such a way that coherence between these two degrees of freedom can inform about the nature of this coupling as well as the reaction coordinate that serves to define excited-state evolution. This presentation will describe recent work from our group in two different classes of transition metal-based chromophores where we are using information from vibronic coherence as a roadmap for synthetic design, in effect, allowing coherence to tell us which degrees of freedom to synthetically modify in order to change the excited-state dynamics of the system.

Leveraging vibronic coherence for synthetic control of excited-state dynamics

ACS Fall 2021

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