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X-ray Photon Correlation Spectroscopy (XPCS) enables direct access to atomic-scale dynamics in disordered materials, revealing both spontaneous and X-ray-induced relaxation processes. Here, we study two compositionally similar alloy glasses…

The capability of generating two intense, femtosecond x-ray pulses with controlled time delay opens the possibility of performing time-resolved experiments for x-ray induced phenomena. We have applied this capability to study the…

The squeezed photons, as a quantum-correlated light with reduced noise, have emerged as a great resource for sensing the structures of matter. Here we study the transient absorption (TA) scheme using the squeezed photons whose spectral…

Quantum Physics · Physics 2026-05-29 Jiahao Joel Fan , Feihong Liu , Dangyuan Lei , Zhedong Zhang

Conical intersections are ubiquitous in chemistry and physics, often governing processes such as light harvesting, vision, photocatalysis, and chemical reactivity. They act as funnels between electronic states of molecules, allowing rapid…

We report a novel experimental technique to investigate ultrafast dynamics in photoexcited molecules by probing the third-order nonlinear optical susceptibility. A non-colinear 3-pulse scheme is developed to probe the ultrafast dynamics of…

Atomic-scale disorder shapes the potential energy landscape traversed by photoexcited charge carriers, while the carriers themselves also dynamically reshape this landscape. However, resolving ultrafast photocarrier motion at atomic length…

Mesoscale and Nanoscale Physics · Physics 2026-04-29 Vedran Jelic , Kaedon Cleland-Host , Stefanie Adams , Mohamed Hassan , Austin Hayes , Tyler L. Cocker

Time-resolved X-ray Emission/Absorption Spectroscopy (Tr-XES/XAS) is an informative experimental tool sensitive to electronic dynamics in materials, widely exploited in diverse research fields. Typically, Tr-XES/XAS requires X-ray pulses…

Time- and angle-resolved photoemission spectroscopy (trARPES) is a powerful spectroscopic method to measure the ultrafast electron dynamics directly in momentum-space. However, band gap materials with exceptional strong Coulomb interaction…

Mesoscale and Nanoscale Physics · Physics 2019-12-09 Dominik Christiansen , Malte Selig , Ermin Malic , Ralph Ernstorfer , Andreas Knorr

A central paradigm of non-equilibrium physics concerns the dynamics of heterogeneity and disorder, impacting processes ranging from the behavior of glasses to the emergent functionality of active matter. Understanding these complex…

Processes involving ultrafast laser driven electron-phonon dynamics play a fundamental role in the response of quantum systems in a growing number of situations of interest, as evidenced by phenomena such as strongly driven phase…

Materials Science · Physics 2024-03-01 Kevin Lively , Shunsuke A. Sato , Guillermo Albareda , Angel Rubio , Aaron Kelly

The high flexibility of organic molecules offers great potential for designing the optical properties of light-active materials for the next generation of optoelectronic and photonic applications. However, despite successful implementations…

The direct observation of non-adiabatic dynamics at conical intersections is a long-standing goal of molecular physics. Novel time-resolved spectroscopies have been proposed which are sensitive to electronic coherences induced by the…

Chemical Physics · Physics 2020-11-16 Simon P. Neville , Albert Stolow , Michael S. Schuurman

X-ray photon correlation spectroscopy (XPCS) allows for the resolution of dynamic processes within a material across a wide range of length and time scales. X-ray speckle visibility spectroscopy (XSVS) is a related method that uses a single…

Numerical Analysis · Mathematics 2023-01-09 Shaswat Mohanty , Christopher B. Cooper , Hui Wang , Mengning Liang , Wei Cai

The advent of ultrashort soft x-ray pulse sources permits the use of established gas phase spectroscopy methods to investigate ultrafast photochemistry in isolated molecules with element and site specificity. In the present study, we…

Chemical Physics · Physics 2019-11-26 Ludger Inhester , Zheng Li , Xiaolei Zhu , Nikita Medvedev , Thomas J. A. Wolf

Quantum coherence between electronic states of a photoionized molecule and the resulting process of ultrafast electron-hole migration have been put forward as a possible quantum mechanism of charge-directed reactivity governing the…

We develop an ultrafast frequency-resolved Raman spectroscopy with entangled photons for polyatomic molecules in condensed phases, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal…

Quantum Physics · Physics 2021-06-23 Zhedong Zhang , Tao Peng , Xiaoyu Nie , Girish S. Agarwal , Marlan O. Scully

Time- and angle-resolved photoemission spectroscopy (TrARPES) is a powerful technique for capturing the ultrafast dynamics of charge carriers and revealing photo-induced phase transitions in quantum materials. However, the lack of widely…

Mesoscale and Nanoscale Physics · Physics 2022-01-05 Changhua Bao , Haoyuan Zhong , Shaohua Zhou , Runfa Feng , Yuan Wang , Shuyun Zhou

Photon-based spectroscopies have had a significant impact on both fundamental science and applications by providing an efficient approach to investigate the microscopic physics of materials. Together with the development of synchrotron…

Strongly Correlated Electrons · Physics 2018-09-06 Yao Wang , Martin Claassen , Chaitanya Das Pemmaraju , Chunjing Jia , Brian Moritz , Thomas P. Devereaux

Using time dependent density functional theory (TDDFT) we examine the energy, angular and time-resolved photoelectron spectra (TRPES) of ethylene in a pump-probe setup. To simulate TRPES we expose ethylene to an ultraviolet (UV) femtosecond…

Atomic and Molecular Clusters · Physics 2014-08-28 Alison Crawford-Uranga , Umberto De Giovannini , Duncan John Mowbray , Stefan Kurth , Angel Rubio

We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a…

Optics · Physics 2018-12-11 Daria Popova-Gorelova , Jochen Küpper , Robin Santra