Improving our understanding of electron dynamics is essential for advancing energy transfer, optoelectronics, light harvesting systems and quantum computing. Recent developments in attosecond x-ray sources provide the fundamental possibility of observing these dynamics with atomic-scale resolution. However, connecting a time-resolved signal to dynamics is challenging due to the broad bandwidth of an attosecond probe pulse. This makes exploring the capabilities of different attosecond imaging techniques crucial. Here, we propose attosecond momentum-resolved resonant inelastic x-ray scattering as a prominent technique for tracking ultrafast dynamics. We demonstrate that the scattering signal contains an information about the instantaneous distribution of charge density across the scattering atoms. To illustrate this, we consider scattering from an $α$-sexithiophene molecule, in which coupled electron-hole dynamics are excited.
Improving our understanding of electron dynamics is essential for advancing energy transfer, optoelectronics, light harvesting systems and quantum computing. Recent developments in attosecond x-ray sources provide the fundamental possibility of observing these dynamics with atomic-scale resolution. However, connecting a time-resolved signal to dynamics is challenging due to the broad bandwidth of an attosecond probe pulse. This makes exploring the capabilities of different attosecond imaging techniques crucial. Here, we propose attosecond momentum-resolved resonant inelastic x-ray scattering as a prominent technique for tracking ultrafast dynamics. We demonstrate that the scattering signal contains an information about the instantaneous distribution of charge density across the scattering atoms. To illustrate this, we consider scattering from an α-sexithiophene molecule, in which coupled electron-hole dynamics are excited.
The past thirty years witnessed rapid developing of strong field physics that leads to the first generation of attosecond (10−18 s) pulses. The duration of available pulses has recently been reduced to less than 100 as, approaching the Kepler period of a classical electron revolving around the nucleus. For the first time, electron motions inside atoms, molecules and solids can be traced, probed and even steered in real time. It pushed the study on ultrafast dynamic processes into a new frontier, giving birth to attosecond physics. The development of attosecond pulses provides unprecedented coherent ultrashort XUV (extreme ultra-violet) of soft X-ray sources that enable imaging the atomic structure and resolving the related quantum dynamics for matter science. In particular, it allows the probing and monitoring of electron dynamics in the natural time scale of attoseconds with atomic spatial resolution. The generation and applications of attosecond pulses are directly related to the control and manipulation of the sub-cycle electron dynamics. Recent studies on the correlated multielectron dynamics have provided insight into the optical and dynamical properties of matter in the perspectives of time, phase and entanglement. It deepens our understanding on some of the fundamental questions, e.g., how the single or multiple photons are absorbed and how short are the quantum processes such as photoionization, tunneling ionization and charge migration. Although currently attosecond pulses are limited by the flux and pulse duration, the combination of attosecond pulses with intense infrared laser pulses paves new ways of controlling and probing electron dynamics in the domains of energy, time and space that lays the foundation for petahertz optoelectronics and attosecond pulse based transient spectroscopy. In this review, we will first briefly summarize the advancement of strong field and ultrafast physics including the relevant experimental findings, the theoretical explorations, the related technologies and the possible applications. Then we focus on the sub-cycle electron or multielectron dynamics and their manifestation on the ionization and coherent radiation properties. We start with the time behavior of Fano resonance and how it can be probed in time domain. In section 2, the correlated electron dynamics is discussed in term of anti-screening effect and Pauli effect that influence strong field ionization and high harmonic generation processes. In section 3, the coherent emission with frequency from terahertz to soft XUV and their joint measurement are discussed by emphasizing the generation mechanism of terahertz wave in two-color laser pulses. The developed high-harmonic and terahertz wave spectroscopy (HATS) is shown capable of imaging the molecular structure and dynamics. In section 4, the time-resolving of electron and hole dynamics and their coherence is proposed based on attosecond transient absorption technique. The coherence of ionization and the correlated electron dynamics is hinted crucial for electron-hole interaction. The topics are very limited and mainly selected from the perspectives of our group.
Collective excitations contain rich information about photoinduced transient states in correlated systems. In a Mott insulator, charge degrees of freedom are frozen, but can be activated by photodoping. The energy-momentum distribution of the charge excitation spectrum reflects the propagation of charge degrees of freedom and provides information about the interplay among various intertwined instabilities on the timescale set by the pump. To reveal charge excitations out of equilibrium, we simulate time-resolved x-ray absorption and resonant inelastic x-ray scattering using a Hubbard model. After pumping, the former resolves photodoping, while the latter characterizes the formation, dispersion, weight, and nonlinear effects of collective excitations. Intermediate-state information from time-resolved resonant inelastic x-ray scattering (trRIXS) can be used to decipher the origin of these excitations, including bimagnons, Mott-gap excitations, doublon and single-electron in-gap states, and anti-Stokes relaxation during an ultrafast pump. This paper provides a theoretical foundation for existing and future trRIXS experiments.
We propose an approach to probe coherent spin-state dynamics of molecules using circularly polarized hard X-ray pulses. For the dynamically aligned nitric oxide molecules in a coherent superposition spin-orbit coupled electronic state that can be prepared through stimulated Raman scattering, we demonstrate the capability of ultrafast X-ray diffraction to not only reveal the quantum beating of the coherent spin-state wave packet but also image the spatial spin density of the molecule. With a circularly polarized ultrafast X-ray diffraction signal, we show that the electronic density matrix can be retrieved. The spatiotemporal resolving power of ultrafast X-ray diffraction paves the way for tracking transient spatial wave function in molecular dynamics involving the spin degree of freedom.
Photoionization is one of the most fundamental processes in light-matter interaction. Advanced attosecond photoelectron spectroscopy provides the possibility to characterize the ultrafast photoemission process in an extremely short attosecond time scale. Following scattering symmetry rules, residual ions encode ultrafast photoionization prints at the instant of electron removal forming an alternative electron emission chronoscope. Here, we experimentally illustrate the attosecond ion reconstruction of attosecond beating by interference of two-photon transition (RABBIT)-like interferometry through the development of high-resolution ion momentum detection in atomic photoionization processes. Our ion interferometry presents identical momentum- and time-dependent scattering phase shift, as we observed in photoelectron spectroscopy, and thus demonstrates that ion interferometry can be a possible alternative attosecond approach to resolve the photoionization process, without the electron homogeneity limitation.
Characterizing and controlling entanglement in quantum materials is crucial for the development of next-generation quantum technologies. However, defining a quantifiable figure of merit for entanglement in macroscopic solids is theoretically and experimentally challenging. At equilibrium the presence of entanglement can be diagnosed by extracting entanglement witnesses from spectroscopic observables and a nonequilibrium extension of this method could lead to the discovery of novel dynamical phenomena. Here, we propose a systematic approach to quantify the time-dependent quantum Fisher information and entanglement depth of transient states of quantum materials with time-resolved resonant inelastic x-ray scattering. Using a quarter-filled extended Hubbard model as an example, we benchmark the efficiency of this approach and predict a light-enhanced many-body entanglement due to the proximity to a phase boundary. Our work sets the stage for experimentally witnessing and controlling entanglement in light-driven quantum materials via ultrafast spectroscopic measurements.
Excited-state dynamics in condensed matter systems plays a crucial role in determining their properties. Understanding and controlling ultrafast dynamics across multiple dimensions—such as time, space, energy, momentum, and spin—has become a key emerging direction in modern condensed matter physics. In recent decades, time-resolved ultrafast laser technology based on pump-probe techniques has advanced significantly. This technology has been integrated with various experimental methods, leading to developments in ultrafast spectroscopy, time- and angle-resolved photoemission spectroscopy (TR-ARPES), ultrafast scanning tunneling microscopy (STM), ultrafast electron diffraction (UED), and ultrafast X-ray techniques, enabling the study of lattice, electron, and spin dynamics. Meanwhile, to provide a clearer physical picture of ultrafast dynamics, real-time first-principles methods have been developed by combining electronic structure methods with dynamic approaches, allowing the study of multidimensional lattice, electron, and spin behaviors. This article reviews recent progress in the field and discusses its future challenges and opportunities.