近日，西班牙巴塞罗那科技学院的J.Biegert及其研究团队取得一项新进展。经过不懈努力，他们通过阿秒核级吸收光谱揭示分子开环的电子动力学和核动力学。相关研究成果已于2024年4月29日在国际知名学术期刊《自然—光子学》上发表。

该研究团队表明，阿秒核级光谱学是研究分子动力学的有力工具，因为它结合了阿秒时间分辨率和宽相干光谱，能够依据不同的能量特征来解析核与电子的运动特性。通过这一方法，相关的实时电子和核波包动力学以及锥形交叉上的非绝热跃迁，都被用于识别电子与核的相干性，并且直接记录了X射线吸收光谱的对称性变化。

研究人员已经验证了该方法的有效性，成功揭示了呋喃开环动力学的完整时间历程。这一研究确立了阿秒核级光谱学在研究分子系统中光化学反应途径实时动力学方面的有效性。

附：英文原文

Title: Attosecond core-level absorption spectroscopy reveals the electronic and nuclear dynamics of molecular ring opening

Author: Severino, S., Ziems, K. M., Reduzzi, M., Summers, A., Sun, H.-W., Chien, Y.-H., Grfe, S., Biegert, J.

Issue&Volume: 2024-04-29

Abstract: 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.

DOI: 10.1038/s41566-024-01436-9

Source: https://www.nature.com/articles/s41566-024-01436-9