Time-, Frequency-, and Wavevector-resolved X-ray Diffraction from Single Molecules

Overview

Journal J Chem Phys

Publisher American Institute of Physics

Specialties Biophysics
Chemistry

Date 2014 Jun 2

PMID 24880284

Citations 9

Authors

Kochise Bennett

Jason D Biggs

Yu Zhang

Konstantin E Dorfman

Shaul Mukamel

Affiliations

Soon will be listed here.

Abstract

Using a quantum electrodynamic framework, we calculate the off-resonant scattering of a broadband 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.

Citing Articles

Monitoring vibronic coherences and molecular aromaticity in photoexcited cyclooctatetraene with an X-ray probe: a simulation study.

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Unveiling the spatial distribution of molecular coherences at conical intersections by covariance X-ray diffraction signals.

Cavaletto S, Keefer D, Rouxel J, Aleotti F, Segatta F, Garavelli M Proc Natl Acad Sci U S A. 2021; 118(22).

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A general theory of far-field optical microscopy image formation and resolution limit using double-sided Feynman diagrams.

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Ultrafast Spectroscopy of Photoactive Molecular Systems from First Principles: Where We Stand Today and Where We Are Going.

Conti I, Cerullo G, Nenov A, Garavelli M J Am Chem Soc. 2020; 142(38):16117-16139.

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Imaging of transition charge densities involving carbon core excitations by all X-ray sum-frequency generation.

Cho D, Rouxel J, Kowalewski M, Lee J, Mukamel S Philos Trans A Math Phys Eng Sci. 2019; 377(2145):20170470.

PMID: 30929629 PMC: 6452053. DOI: 10.1098/rsta.2017.0470.

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