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Using a combined theoretical and experimental approach, we investigate the non-adiabatic dynamics of the prototypical ethylene (C2H4) molecule upon {\pi} \to {\pi}* excitation. In this first part of a two part series, we focus on the…

Recent seminal experiments have utilized time-resolved X-ray absorption spectroscopy (XAS) to investigate the ultrafast photo-induced renormalization of the electron interaction (''Hubbard $U$'') in Mott and charge transfer insulators. In…

Strongly Correlated Electrons · Physics 2025-08-19 Denis Golez , Eva Paprotzki , Philipp Werner , Martin Eckstein

The development of X-ray free-electron lasers (XFELs) has enabled ultrafast X-ray diffraction (XRD) experiments, which are capable of resolving electronic/vibrational transitions and structural changes in molecules, or capturing molecular…

Chemical Physics · Physics 2024-08-29 Sebastian V. Pios , Jiaji Zhang , Maxim F. Gelin , Hong-Guang Duan , Lipeng Chen

We show that time-resolved x-ray scattering from molecules prepared in a superposition of electronic states moving through an avoided crossing has new features not found in diffraction from the corresponding classical mixed state.…

Ultrafast two-dimensional spectroscopy utilizes correlated multiple light-matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum. Its extension to the terahertz regime of the…

We applied angular X-ray Cross-Correlation analysis (XCCA) to scattering images from a femtosecond resolution LCLS X-ray free-electron laser (XFEL) pump-probe experiment with solvated PtPOP ([Pt$_2$(P$_2$O$_5$H$_2$)$_4$]$^{4-}$) metal…

Time-resolved x-ray scattering (TRXS) measures internuclear separations in a molecule following laser-induced photoexcitation. The molecular dynamics induced by the excitation laser may lie on one or several bound or dissociative electronic…

Atomic Physics · Physics 2019-09-25 MR Ware , JM Glownia , N Al-Sayyad , JT O'Neal , PH Bucksbaum

Topological soliton is a nonperturbative excitation in commensurate density wave states and connects degenerate ground states. In incommensurate density wave states, ground states are continuously degenerate and topological soliton is…

Mesoscale and Nanoscale Physics · Physics 2021-09-22 Xiao-Xiao Zhang , Dirk Manske , Naoto Nagaosa

How molecules convert light energy to perform a specific transformation is a fundamental question in photophysics. Ultrafast spectroscopy reveals the kinetics associated with electronic energy flow, but little is known about how absorbed…

A wide range of ultrafast phenomena in various atomic, molecular and condense matter systems is governed by electron dynamics. Therefore, the ability to image electronic motion in real space and real time would provide a deeper…

Atomic Physics · Physics 2018-02-27 Daria Popova-Gorelova

The requirement of high space-time resolution and brightness is a great challenge for imaging atomic motion and making molecular movies. Important breakthroughs in ultrabright tabletop laser, x-ray and electron sources have enabled the…

Atomic Physics · Physics 2022-02-10 Ming Zhang , Zhenning Guo , Xiaoyu Mi , Zheng Li , Yunquan Liu

Approaching energy coupling in laser-irradiated metals, we point out the role of electron-electron collision as an efficient control factor for ultrafast optical absorption. The high degree of laser-induced electron-ion nonequilibrium…

Quantum material systems upon applying ultrashort laser pulses provide a rich platform to access excited material phases and their transformations that are not entirely like their equilibrium counterparts. The addressability and potential…

Strongly Correlated Electrons · Physics 2021-08-19 Xiaoyi Sun , Shuaishuai Sun , Chong-Yu Ruan

Conical intersections serve as critical gateways in photochemical reactions, enabling rapid nonradiative transitions between potential energy surfaces that underpin fundamental processes such as photosynthesis or vision. Their calculation…

Chemical Physics · Physics 2025-02-19 Rhyan Barrett , Christoph Ortner , Julia Westermayr

We investigate ultrafast dynamics of the lowest singlet excited electronic state in liquid nitrobenzene using Ultrafast Transient Polarization Spectroscopy (UTPS), extending the well-known technique of Optical-Kerr Effect (OKE) spectroscopy…

New experimental techniques based on non-linear ultrafast spectroscopies have been developed over the last few years, and have been demonstrated to provide powerful probes of quantum dynamics in different types of molecular aggregates,…

Frontier orbitals, i.e., the highest occupied and lowest unoccupied orbitals of a molecule, generally determine molecular properties, such as chemical bonding and reactivities. Consequently, there has been a lot of interest in measuring…

In this manuscript we present a theoretical framework and its numerical implementation to simulate the out-of-equilibrium electron dynamics induced by the interaction of ultrashort laser pulses in condensed-matter systems. Our approach is…

Unveiling the key mechanisms that determine optically driven spin dynamics is essential both to probe the fundamental nature of ultrafast light-matter interactions, but also to drive future technologies of smaller, faster, and more energy…