AI 中文总结
本研究通过激发态分子动力学探究两种单苯荧光团的超快激发态分子内质子转移，发现特定分子振动可触发单或双质子转移，其动力学激活能调控产率与产物，为ESIPT调控提供原子级指导。
AI 中文摘要
单苯荧光团（SBFs）是极轻质的量子发射体，近期研究表明其具有激发态分子内质子转移（ESIPT）特性及高度可调的双荧光，可应用于多种场景。本研究采用激发态分子动力学，探究两种不同SBFs中ESIPT的超快动力学，其中一种为本文提出的新结构。研究发现，特定分子振动激发可触发单质子或双质子的超快转移；通过原子级对称性分析选定的这类振动的动力学激活，可显著提高质子转移产率，并引导反应生成单转移或双转移产物。深入分析阐明了这种振动态控制的起源，为利用超快红外-可见光谱调控ESIPT的速率和结果提供了原子级层面的指导原则。
英文摘要
Single-benzene fluorophores (SBFs) are exceptionally light-weight quantum emitters which have recently been shown to display Excited State Intramolecular Proton Transfer (ESIPT) and highly tunable dual-fluorescence that could be exploited for multiple applications. Here, we employ excited-state molecular dynamics to investigate the ultrafast dynamics of ESIPT in two different SBFs, one of which with a new structure proposed in this work. We find that both single and double ultrafast proton transfers can be triggered by exciting specific molecular vibrations. Strikingly, the kinetic activation of these vibrations - selected by atomistic, symmetry-based analysis - can considerably enhance the yield of proton transfer(s), as well as direct the reaction towards either single or double-transfer products. In-depth analysis elucidates the origins of this vibronic control, providing atomistic guidelines through which both the rate and fate of ESIPT could be steered using ultrafast IR-Vis spectroscopies.
Comments19 pages, 3 figures, 2 tables + 17 pages
