Modeling Excited-State Proton Transfer Using the Lindblad Equation: Quantification of Time-Resolved Spectroscopy with Mechanistic Insights

Luhao Zhang, Francesca Fassioli, Bo Fu, Zhen Su She, Gregory D. Scholes

Research output: Contribution to journalArticlepeer-review

Abstract

The quantum dynamics of excited-state intramolecular proton transfer (ESIPT) is studied using a multilevel vibronic Hamiltonian and the Lindblad master equation. We simulate time-resolved fluorescence spectroscopy of 2-(2′-hydroxyphenyl) benzothiazole (HBT) and 10-hydroxybenzo[h]quinoline (HBQ), which suggests that the underlying mechanism behind the initial ultrafast rise and decay in the spectra is electronic state population that evolves simultaneously with proton wave packet dynamics. The results predict that the initial rise and decay signals at different wavelengths vary significantly with system properties in terms of their shape, the time, and the intensity of the maximum. These findings provide clues for data interpretation, mechanism validation, and control of the dynamics, and the model serves as an attempt toward clarifying ESIPT by direct comparison to time-resolved spectroscopy.

Original languageEnglish (US)
Pages (from-to)107-118
Number of pages12
JournalACS Physical Chemistry Au
Volume3
Issue number1
DOIs
StatePublished - Jan 25 2023

All Science Journal Classification (ASJC) codes

  • Chemistry (miscellaneous)
  • Computer Science Applications
  • Physical and Theoretical Chemistry
  • Computational Theory and Mathematics

Keywords

  • Lindblad equation
  • electron−proton interplay
  • excited-state proton transfer
  • quantum dynamics
  • ultrafast spectroscopy

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