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Convergent-beam attosecond x-ray crystallography.
Struct Dyn
January 2025
Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, Germany.
Sub-ångström spatial resolution of electron density coupled with sub-femtosecond to few-femtosecond temporal resolution is required to directly observe the dynamics of the electronic structure of a molecule after photoinitiation or some other ultrafast perturbation, such as by soft X-rays. Meeting this challenge, pushing the field of quantum crystallography to attosecond timescales, would bring insights into how the electronic and nuclear degrees of freedom couple, enable the study of quantum coherences involved in molecular dynamics, and ultimately enable these dynamics to be controlled. Here, we propose to reach this realm by employing convergent-beam x-ray crystallography with high-power attosecond pulses from a hard-x-ray free-electron laser.
View Article and Find Full Text PDFSimulations of Attosecond Metallization in Quartz and Diamond Probed with Inner-Shell Transient Absorption Spectroscopy.
J Phys Chem A
January 2025
Department of Chemistry, Louisiana State University, Baton Rouge, Louisiana 70803, United States.
When dielectrics are hit with intense infrared (IR) laser pulses, transient metalization can occur. The initial attosecond dynamics behind this metallization are not entirely understood. Therefore, simulations are needed to understand this process and to help interpret experimental observations of it, such as with attosecond transient absorption (ATA).
View Article and Find Full Text PDFObservation of Laser-Assisted Dynamic Interference by Attosecond Controlled Photoelectron Spectroscopy.
Phys Rev Lett
December 2024
Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012, China.
Article Synopsis
- The study reveals that laser-assisted dynamic interference in electron spectra can be experimentally observed using attosecond pulse trains, demonstrating fine interference patterns smaller than the energy of individual laser photons.
- Theoretical simulations align with experimental findings, utilizing methods like the time-dependent Schrödinger equation and strong-field approximation to support the results.
- Further analysis emphasizes the significance of phase variations in electron wave packets, showing that the manipulation of electron behavior in the continuum is achievable through advanced multicolor laser techniques controlled at attosecond timescales.
Non-Resonant Magnetic X-ray Scattering as a Probe of Ultrafast Molecular Spin-State Dynamics: An Ab Initio Theory.
J Chem Theory Comput
January 2025
State Key Laboratory for Mesoscopic Physics and Collaborative Innovation Center of Quantum Matter, School of Physics, Peking University, Beijing 100871, China.
Article Synopsis
- Advanced techniques like high harmonic generation and X-ray free-electron lasers have enabled the study of ultrafast electron and spin dynamics on extremely short timescales.
- The authors propose using magnetic X-ray scattering (MXS) to measure molecular spin-state dynamics and outline a protocol for simulating MXS patterns using multiconfigurational quantum chemistry.
- The method is validated through simulations of spin-flip dynamics in the TiCl molecule, showcasing MXS's ability to detect real-time spin-state changes and infer spatial characteristics of spin density from diffraction patterns.
Strong-Field Theory of Attosecond Tunneling Microscopy.
Phys Rev Lett
December 2024
Department of Physics, Technion-Israel Institute of Technology, Haifa 32000, Israel; Solid State Institute, Technion-Israel Institute of Technology, Haifa 32000, Israel; and The Helen Diller Quantum Center, Technion-Israel Institute of Technology, Haifa 32000, Israel.
Attosecond observations of coherent electron dynamics in molecules and nanostructures can be achieved by combining conventional scanning tunneling microscopy (STM) with ultrashort femtosecond laser pulses. While experimental studies in the subcycle regime are under way, a robust strong-field theory description has remained elusive. Here we devise a model based on the strong-field approximation.
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