Time-, Frequency-, and Wavevector-Resolved X-Ray Diffraction from Single Molecules

Abstract

Using a quantum electrodynamic framework, we calculate the off-resonant scattering of a broad-band X-ray pulse from a sample initially prepared in an arbitrary superposition of electronic states. The signal consists of single-particle (incoherent) and two-particle (coherent) contributions that carry different particle form factors that involve different material transitions. Single-molecule experiments involving incoherent scattering are more influenced by inelastic processes compared to bulk measurements. The conditions under which the technique directly measures charge densities (and can be considered as diffraction) as opposed to correlation functions of the charge-density are specified. The results are illustrated with time- and wavevector-resolved signals from a single amino acid molecule (cysteine) following an impulsive excitation by a stimulated X-ray Raman process resonant with the sulfur K-edge. Our theory and simulations can guide future experimental studies on the structures of nano-particles and proteins.

References in corpus (7)

• Resonant Inelastic X-ray Scattering Studies of Elementary Excitations
• Femtosecond Diffractive Imaging with a Soft-X-ray Free-Electron Laser
• Imaging electronic quantum motion with light
• Radiation Generated by Charge Migration Following Ionization
• Time-, Frequency-, and Wavevector-Resolved X-Ray Diffraction from Single Molecules
• Multidimensional X-Ray Spectroscopy of Valence and Core Excitations in Cysteine
• Nonlinear light scattering in molecules triggered by an impulsive X-ray Raman process

Cited by in corpus (12)

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• Time-, Frequency-, and Wavevector-Resolved X-Ray Diffraction from Single Molecules
• Time-resolved ultrafast x-ray scattering from an incoherent electronic mixture
• Detecting Electronic Coherence by Multidimensional Broadband Stimulated X-Ray Raman Signals
• Comment on "Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion"
• Imaging Electron Dynamics with Ultrashort Light Pulses: A Theory Perspective
• Theory of high-energy correlated multiphoton x-ray diffraction for synchrotron radiation sources
• Simulations for x-ray imaging of wave-packet dynamics
• Unified image formation theory for microscopy and optical coherence tomography in 4-D space-time