Cargando…
Modeling Excited-State Proton Transfer Using the Lindblad Equation: Quantification of Time-Resolved Spectroscopy with Mechanistic Insights
[Image: see text] 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]qu...
Autores principales: | , , , , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2022
|
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9881171/ https://www.ncbi.nlm.nih.gov/pubmed/36718263 http://dx.doi.org/10.1021/acsphyschemau.2c00038 |
_version_ | 1784879057301667840 |
---|---|
author | Zhang, Luhao Fassioli, Francesca Fu, Bo She, Zhen-Su Scholes, Gregory D. |
author_facet | Zhang, Luhao Fassioli, Francesca Fu, Bo She, Zhen-Su Scholes, Gregory D. |
author_sort | Zhang, Luhao |
collection | PubMed |
description | [Image: see text] 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. |
format | Online Article Text |
id | pubmed-9881171 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-98811712023-01-28 Modeling Excited-State Proton Transfer Using the Lindblad Equation: Quantification of Time-Resolved Spectroscopy with Mechanistic Insights Zhang, Luhao Fassioli, Francesca Fu, Bo She, Zhen-Su Scholes, Gregory D. ACS Phys Chem Au [Image: see text] 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. American Chemical Society 2022-12-21 /pmc/articles/PMC9881171/ /pubmed/36718263 http://dx.doi.org/10.1021/acsphyschemau.2c00038 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/). |
spellingShingle | Zhang, Luhao Fassioli, Francesca Fu, Bo She, Zhen-Su Scholes, Gregory D. Modeling Excited-State Proton Transfer Using the Lindblad Equation: Quantification of Time-Resolved Spectroscopy with Mechanistic Insights |
title | Modeling Excited-State
Proton Transfer Using the Lindblad
Equation: Quantification of Time-Resolved Spectroscopy with Mechanistic
Insights |
title_full | Modeling Excited-State
Proton Transfer Using the Lindblad
Equation: Quantification of Time-Resolved Spectroscopy with Mechanistic
Insights |
title_fullStr | Modeling Excited-State
Proton Transfer Using the Lindblad
Equation: Quantification of Time-Resolved Spectroscopy with Mechanistic
Insights |
title_full_unstemmed | Modeling Excited-State
Proton Transfer Using the Lindblad
Equation: Quantification of Time-Resolved Spectroscopy with Mechanistic
Insights |
title_short | Modeling Excited-State
Proton Transfer Using the Lindblad
Equation: Quantification of Time-Resolved Spectroscopy with Mechanistic
Insights |
title_sort | modeling excited-state
proton transfer using the lindblad
equation: quantification of time-resolved spectroscopy with mechanistic
insights |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9881171/ https://www.ncbi.nlm.nih.gov/pubmed/36718263 http://dx.doi.org/10.1021/acsphyschemau.2c00038 |
work_keys_str_mv | AT zhangluhao modelingexcitedstateprotontransferusingthelindbladequationquantificationoftimeresolvedspectroscopywithmechanisticinsights AT fassiolifrancesca modelingexcitedstateprotontransferusingthelindbladequationquantificationoftimeresolvedspectroscopywithmechanisticinsights AT fubo modelingexcitedstateprotontransferusingthelindbladequationquantificationoftimeresolvedspectroscopywithmechanisticinsights AT shezhensu modelingexcitedstateprotontransferusingthelindbladequationquantificationoftimeresolvedspectroscopywithmechanisticinsights AT scholesgregoryd modelingexcitedstateprotontransferusingthelindbladequationquantificationoftimeresolvedspectroscopywithmechanisticinsights |