We show that attosecond core-level spectroscopy is a powerful tool for investigating molecular dynamics due to its combined attosecond temporal resolution and the broad coherent spectrum that allows deciphering the signatures of nuclear and electronic motion through their different energetic signatures. The method reveals that the correlated real-time electronic and nuclear wavepacket dynamics and non-adiabatic transitions across conical intersections identify electronic and nuclear coherences and directly register symmetry changes in the X-ray absorption spectrum. We demonstrate the method’s efficacy to unveil the entire time history of the ring-opening dynamics of furan. The investigation establishes attosecond core-level spectroscopy as a potent method to investigate the real-time dynamics of photochemical reaction pathways in molecular systems.

我们证明，阿秒核心级光谱学是研究分子动力学的强大工具，因为它结合了阿秒时间分辨率和广泛的相干光谱，可以通过不同的能量特征来破译核和电子运动的特征。该方法揭示了相关的实时电子和核波包动力学以及锥形交叉点的非绝热跃迁识别电子和核相干性并直接记录 X 射线吸收光谱中的对称性变化。我们证明了该方法能够揭示呋喃开环动力学的整个时间历史。该研究将阿秒核心级光谱学确立为研究分子系统中光化学反应路径实时动态的有效方法。