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Updated: Jun 21, 2025

Generation and Coherent Control of Pulsed Quantum Frequency Combs
Published on: June 8, 2018
Coherent control from quantum commitment probabilities
Michelle C Anderson1, Amro Dodin1,2, Thomas P Fay1
1Department of Chemistry, University of California, Berkeley, California 94720, USA.
Abstract:
We introduce a general definition of a quantum committor in order to clarify reaction mechanisms and facilitate control in processes where coherent effects are important. With a quantum committor, we generalize the notion of a transition state to quantum superpositions and quantify the effect of interference on the progress of the reaction. The formalism is applicable to any linear quantum master equation supporting metastability for which absorbing boundary conditions designating the reactant and product states can be applied. We use this formalism to determine the dependence of the quantum transition state on coherences in a polaritonic system and optimize the initialization state of a conical intersection model to control reactive outcomes, achieving yields of the desired state approaching 100%. In addition to providing a practical tool, the quantum committor provides a conceptual framework for understanding reactions in cases when classical intuitions fail.
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