Few-Femtosecond MeV Electron Bunches for Ultrafast Electron Diffraction

Recent development of X-ray free-electron lasers and megaelectronvolt radio-frequency electron guns have made ultrafast Xray and electron diffraction measurements possible, thereby capturing chemical dynamics with atomic-spatial and femtosecond-temporal resolutions. We present a unified formulation of standard homodynedetected and heterodyne-detected signals for both techniques. Noting that X-rays scatter from molecular electrons while electrons scatter from both molecular electrons and nuclei, we show how the two diffraction signals can be combined to reveal novel chemical information that is unavailable by solely using each technique alone. By subtracting the homodyne-detected X-ray and electron diffraction signals, a mixed electronic−nuclear interference in electron diffraction can be identified with a self-heterodyne nature for the direct imaging of attosecond electron dynamics where the scattering off molecular nuclei serves as a local oscillator for the scattering off molecular electrons. By subtracting heterodyne-detected X-ray and electron diffraction, the purely nuclear charge density can be singled out.

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Attosecond Charge Migration in Molecules Imaged by Combined X-ray and Electron Diffraction

Yong

Sun

et al. 2022

J. Am. Chem. Soc.

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We show how ultrafast gas-phase X-ray and electron diffraction signals can be combined to generate real-space movies of charge migration dynamics in molecules. Charge migration denotes short time electronic charge redistribution upon photoexcitation of molecules where the nuclei are frozen. In this regime, we identify a mixed electronic–nuclear interference term that can be cleanly singled out. Using the ground-state nuclear structure as a reference, the phase information in this signal allows its inversion to real space and the capture of electronic charge density movies on the attosecond time scale.

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Few-Femtosecond MeV Electron Bunches for Ultrafast Electron Diffraction

Cited by 6 publications

References 40 publications

State-of-the-art electron beams for compact tools of ultrafast science

State-of-the-art electron beams for compact tools of ultrafast science

Novel Ultrafast Molecular Imaging Based on the Combination of X-ray and Electron Diffraction

Attosecond Charge Migration in Molecules Imaged by Combined X-ray and Electron Diffraction

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