Self-referenced coherent diffraction x-ray movie of Angstrom- and femtosecond-scale atomic motion

Abstract

Time-resolved femtosecond x-ray diffraction patterns from laser-excited molecular iodine are used to create a movie of intramolecular motion with time and space resolution of $30$fs and $0.3$ Å. The high spatial fidelity is due to interference between the moving excitation and the static initial charge distribution. This x-ray interference has not been employed to image internal motion in molecules before. The initial state is used as the local oscillator for heterodyne amplification of the excited charge distribution to retrieve real-space movies of atomic motion on Ångstrom and femtosecond scales. Coherent vibrational motion and dispersion, dissociation, and rotational dephasing are all clearly visible in the data, thereby demonstrating the stunning sensitivity of heterodyne methods.

Accepted by Physical Review Letters

References in corpus (2)

• Imaging electronic quantum motion with light
• Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules

Cited by in corpus (20)

• Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules
• Time-resolved inner-shell photoelectron spectroscopy: from a bound molecule to an isolated atom
• Monitoring Nonadiabatic Avoided Crossing Dynamics in Molecules by Ultrafast X-Ray Diffraction
• Diffractive molecular orbital tomography
• An Assessment of Different Electronic Structure Approaches for Modeling Time-Resolved X-ray Absorption Spectroscopy
• Excited Electronic States in Total Isotropic Scattering From Molecules
• Multiple orbital effects in laser-induced electron diffraction of aligned molecules
• Time-resolved ultrafast x-ray scattering from an incoherent electronic mixture
• Resolving Multiphoton Processes with High-Order Anisotropy Ultrafast X-ray Scattering
• Characterizing and optimizing a laser-desorption molecular beam source
• Real-Space Inversion and Super-Resolution of Ultrafast Scattering
• On the Proper Derivation of the Floquet-based Quantum Classical Liouville Equation and Surface Hopping Describing a Molecule or Material Subject to an External Field
• Ultrafast Molecular Frame Quantum Tomography
• Three Dimensional Orientation of Complex Molecules Excited by Two-Color Femtosecond Pulses
• Probing the Effect of Molecular Structure Saddling on Ultrafast Charge Migration via Time-Resolved X-ray Diffraction
• A Laboratory Frame Density Matrix for Ultrafast Quantum Molecular Dynamics
• Simultaneous imaging of vibrational, rotational, and electronic wave packet dynamics in a triatomic molecule
• Time-resolved Coulomb explosion imaging of vibrational wave packets in alkali dimers on helium nanodroplets
• Non-adiabatic Dynamics in a Laser Field with Floquet Fewest Switches Surface Hopping: The Need for An Accurate Treatment of Coherence and Decoherence Remains
• Ultrafast electron diffractive imaging of the dissociation of pre-excited molecules