Zhang Luhao, Fassioli Francesca, Fu Bo, She Zhen-Su, Scholes Gregory D
Department of Chemistry, Princeton University, Princeton, New Jersey08544, United States.
SISSA - Scuola Internazionale Superiore di Studi Avanzati, 34136Trieste, TS, Italy.
ACS Phys Chem Au. 2022 Dec 21;3(1):107-118. doi: 10.1021/acsphyschemau.2c00038. eCollection 2023 Jan 25.
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[]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.
利用多级振子哈密顿量和林德布拉德主方程研究了激发态分子内质子转移（ESIPT）的量子动力学。我们模拟了2-（2'-羟基苯基）苯并噻唑（HBT）和10-羟基苯并喹啉（HBQ）的时间分辨荧光光谱，这表明光谱中初始超快上升和衰减背后的潜在机制是与质子波包动力学同时演化的电子态布居。结果预测，不同波长处的初始上升和衰减信号在形状、时间和最大值强度方面随系统性质有显著变化。这些发现为数据解释、机制验证和动力学控制提供了线索，该模型旨在通过与时间分辨光谱直接比较来阐明ESIPT。
