Interference of nuclear wavepackets in a pair of proton transfer reactions

Xinzi Zhang, Kyra N. Schwarz, Luhao Zhang, Francesca Fassioli, Bo Fu, Lucas Q. Nguyen, Robert R. Knowles, Gregory D. Scholes

Research output: Contribution to journalArticlepeer-review

Abstract

Quantum mechanics revolutionized chemists’ understanding of molecular structure. In contrast, the kinetics of molecular reactions in solution are well described by classical, statistical theories. To reveal how the dynamics of chemical systems transition from quantum to classical, we study femtosecond proton transfer in a symmetric molecule with two identical reactant sites that are spatially apart. With the reaction launched from a superposition of two local basis states, we hypothesize that the ensuing motions of the electrons and nuclei will proceed, conceptually, in lockstep as a superposition of probability amplitudes until decoherence collapses the system to a product. Using ultrafast spectroscopy, we observe that the initial superposition state affects the reaction kinetics by an interference mechanism. With the aid of a quantum dynamics model, we propose how the evolution of nuclear wavepackets manifests the unusual intersite quantum correlations during the reaction.

Original languageEnglish (US)
Article numbere2212114119
JournalProceedings of the National Academy of Sciences of the United States of America
Volume119
Issue number43
DOIs
StatePublished - Oct 25 2022

All Science Journal Classification (ASJC) codes

  • General

Keywords

  • interference
  • kinetic isotope effect
  • proton transfer
  • quantum mechanics

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