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We demonstrate ultrafast core-electron energy-loss spectroscopy in four-dimensional electron microscopy as an element-specific probe of nanoscale dynamics. We apply it to the study of photoexcited graphite with femtosecond and nanosecond resolutions. The transient core-loss spectra, in combination with ab initio molecular dynamics simulations, reveal the elongation of the carbon-carbon bonds, even though the overall behavior is a contraction of the crystal lattice. A prompt energy-gap shrinkage is observed on the picosecond time scale, which is caused by local bond length elongation and the direct renormalization of band energies due to temperature-dependent electron–phonon interactions.
Author(s): van der Veen RM, Penfold TJ, Zewail AH
Publication type: Article
Publication status: Published
Journal: Structural Dynamics
Online publication date: 28/04/2015
Acceptance date: 23/03/2015
ISSN (electronic): 2329-7778
Publisher: AIP Publishing LLC
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