Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy

Abstract

Coherence can drive wave-like motion of electrons and nuclei in photoexcited systems, which can yield fast and efficient ways to exert materials’ functionalities beyond the thermodynamic limit. The search for coherent phenomena has been a central topic in chemical physics although their direct characterization is often elusive. Here, we highlight recent advances in time-resolved x-ray absorption spectroscopy (tr-XAS) to investigate coherent phenomena, especially those that utilize the eminent light source of isolated attosecond pulses. The unparalleled time and state sensitivities of tr-XAS in tandem with the unique element specificity render the method suitable to study valence electronic dynamics in a wide variety of materials. The latest studies have demonstrated the capabilities of tr-XAS to characterize coupled electronic–structural coherence in small molecules and coherent light–matter interactions of core-excited excitons in solids. We address current opportunities and challenges in the exploration of coherent phenomena, with potential applications for energy- and bio-related systems, potential crossings, strongly driven solids, and quantum materials. With the ongoing developments in both theory and light sources, tr-XAS holds great promise for revealing the role of coherences in chemical dynamics.