Self-referenced coherent diffraction x-ray movie of Angstrom- and femtosecond-scale atomic motion
arXiv:1608.03039 · doi:10.1103/PhysRevLett.117.153003
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 fs and 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.
arXiv commentAccepted by Physical Review Letters
References in corpus (4)
- X-ray diffraction from isolated and strongly aligned gas-phase molecules with a free-electron laser
- Imaging electronic quantum motion with light
- Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules
- Diffractive imaging of a molecular rotational wavepacket with femtosecond Megaelectronvolt electron pulses
Cited by in corpus (33)
- Real-time observation of dissipative optical soliton molecular motions
- Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules
- Field-free Three-Dimensional Orientation of Asymmetric-Top 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
- Probing Electronic Fluxes via Time-Resolved X-ray Scattering
- Mixed Quantum-Classical Electrodynamics: Understanding Spontaneous Decay and Zero Point Energy
- Anisotropy enhanced X-ray scattering from solvated transition metal complexes
- X-Ray sum frequency generation; direct imaging of ultrafast electron dynamics
- 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
- Local Terahertz Field Enhancement for Time-Resolved X-ray Diffraction
- Atomic-resolution imaging of carbonyl sulfide by laser-induced electron diffraction
- Characterizing dissociative motion in time-resolved x-ray scattering from gas-phase diatomic molecules
- Characterizing multiphoton excitation using time-resolved X-ray scattering
- Time-resolved ultrafast x-ray scattering from an incoherent electronic mixture
- Multiple orbital effects in laser-induced electron diffraction of aligned molecules
- Comment on "Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion"
- 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
- Ultrafast Molecular Frame Quantum Tomography
- 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
- Three Dimensional Orientation of Complex Molecules Excited by Two-Color Femtosecond Pulses
- Ultrafast Structural Dynamics of Photo-Reactions Revealed by Model-Independent X-ray Cross-Correlation Analysis
- Characterizing gas flow from aerosol particle injectors
- A Laboratory Frame Density Matrix for Ultrafast Quantum Molecular Dynamics
- Probing the Effect of Molecular Structure Saddling on Ultrafast Charge Migration via Time-Resolved X-ray Diffraction
- 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
- Ultrafast electron diffractive imaging of the dissociation of pre-excited molecules
- Non-adiabatic Dynamics in a Laser Field with Floquet Fewest Switches Surface Hopping: The Need for An Accurate Treatment of Coherence and Decoherence Remains