论文标题
通过核心核心水平光谱法解决的非绝热电子和振动开环动力学
Non-Adiabatic Electronic and Vibrational Ring-Opening Dynamics resolved with Attosecond Core-Level Spectroscopy
论文作者
论文摘要
非绝热动力学和圆锥形交集在大多数多原子分子的化学中起着核心作用，从异构化到杂环开环和避免DNA的光损伤。研究电子和核波包的基础相关动力学是实时的主要挑战，很多时候都涉及光学上的深色瞬态状态。我们表明，Attosond核心水平的光谱揭示了中性呋喃的途径动力学，其圆锥形交集和暗状态。我们的方法测量了电子核相关性，以检测由于核运动引起的电子相干性的脱位，并将开环的异构体确定为主要产物。这些结果证明了Attosend Core水平光谱学作为研究复杂分子系统中光化学反应途径的实时动力学的有效方法的功效。
Non-adiabatic dynamics and conical intersections play a central role in the chemistry of most polyatomic molecules, ranging from isomerization to heterocyclic ring opening and avoided photo-damage of DNA. Studying the underpinning correlated dynamics of electronic and nuclear wave packets is a major challenge in real-time and, many times involves optically dark transient states. We show that attosecond core-level spectroscopy reveals the pathway dynamics of neutral furan across its conical intersections and dark states. Our method measures electronic-nuclear correlations to detect the dephasing of electronic coherence due to nuclear motion and identifies the ring-opened isomer as the dominant product. These results demonstrate the efficacy of attosecond core level spectroscopy as a potent method to investigate the real-time dynamics of photochemical reaction pathways in complex molecular systems.
