No data available.
Please log in to see this content.
You have no subscription access to this content.
No metrics data to plot.
The attempt to load metrics for this article has failed.
The attempt to plot a graph for these metrics has failed.
The full text of this article is not currently available.
Ultrafast core-loss spectroscopy in four-dimensional electron microscopy
1. P. E. Batson, “ Simultaneous STEM imaging and electron energy-loss spectroscopy with atomic-column sensitivity,” Nature 366, 727–728 (1993).
4. C. Colliex, “ From electron energy-loss spectroscopy to multi-dimensional and multi-signal electron microscopy,” J Electron Microsc. (Tokyo) 60(suppl 1), S161–S171 (2011).
7. E. Najafi, A. P. Hitchcock, D. Rossouw, and G. A. Botton, “ Mapping defects in a carbon nanotube by momentum transfer dependent electron energy loss spectromicroscopy,” Ultramicroscopy 113, 158–164 (2012).
8. D. Rossouw, G. A. Botton, E. Najafi, V. Lee, and A. P. Hitchcock, “ Metallic and semiconducting single-walled carbon nanotubes: Differentiating individual SWCNTs by their carbon 1s spectra,” ACS Nano 6(12), 10965–10972 (2012).
9. D. Rossouw, M. Bugnet, and G. A. Botton, “ Structural and electronic distortions in individual carbon nanotubes under laser irradiation in the electron microscope,” Phys. Rev. B 87, 125403 (2013).
10. N. D. Browning, M. F. Chisholm, and S. J. Pennycook, “ Atomic-resolution chemical analysis using a scanning transmission electron microscope,” Nature 366, 143 (1993).
11. D. A. Muller, Y. Tzou, R. Raj, and J. Silcox, “ Mapping sp2 and sp3 states of carbon at sub-nanometre spatial resolution,” Nature 366, 725–727 (1993).
13. P. Schattschneider, C. Hebert, H. Franco, and B. Jouffrey, “ Anisotropic relativistic cross sections for inelastic electron scattering, and the magic angle,” Phys. Rev. B 72, 045142 (2005).
16. L. X. Chen, X. Zhang, and M. L. Shelby, “ Recent advances on ultrafast X-ray spectroscopy in the chemical sciences,” Chem. Sci. 5, 4136–4152 (2014).
17. H. T. Lemke et al., “ Femtosecond X-ray absorption spectroscopy at a hard X-ray free electron laser: Application to spin crossover dynamics,” J. Phys. Chem. A 117, 735–740 (2013).
20. R. M. van der Veen, O.-H. Kwon, A. Tissot, A. Hauser, and A. H. Zewail, “ Single-nanoparticle phase transitions visualized by four-dimensional electron microscopy,” Nat. Chem. 5, 395–402 (2013).
22. R. F. Egerton, Electron Energy-Loss Spectroscopy in the Electron Microscope ( Springer, 2011).
23. L. Piazza et al., “ Ultrafast structural and electronic dynamics of the metallic phase in a layered manganite,” Struct. Dyn. 1, 014501 (2014).
26. Y. C. Wang, K. Scheerschmidt, and U. Gosele, “ Theoretical investigations of bond properties in graphite and graphitic silicon,” Phys. Rev. B 61, 12864–12870 (2000).
See supplementary material at http://dx.doi.org/10.1063/1.4916897
for a description of the heat diffusion simulations (S1), the core-level spectroscopy simulations (S2), the MD simulations (S3), a comparison between the real and shift-induced transient spectra (Fig. S1), the nanosecond-resolved low-loss EELS data (Fig. S2), the simulated changes in the unit cell dimensions (Fig. S3), and the simulated EELS spectra for simple a
- and c
-axes distortions (Fig. S4).[Supplementary Material]
34. R. W. G. Wyckoff, Cryst. Struct. 1, 7–83 (1963).
35. J. J. Rehr, J. J. Kas, F. D. Vila, M. P. Prange, and K. Jorissen, “ Parameter-free calculations of X-ray spectra with FEFF9,” Phys. Chem. Chem. Phys. 12, 5503–5513 (2010).
36. K. Jorissen and J. J. Rehr, “ Calculations of electron energy loss and x-ray absorption spectra in periodic systems without a supercell,” Phys. Rev. B 81, 245124 (2010).
40. E. Sevillano, H. Meuth, and J. Rehr, “ Extended X-ray absorption fine structure Debye-Waller factors. I. Monatomic crystals,” Phys. Rev. B 20, 4908–4911 (1979).
42. V.-T. Pham et al., “ Probing the transition from hydrophilic to hydrophobic solvation with atomic scale resolution,” J. Am. Chem. Soc. 133, 12740–12748 (2011).
43. P. D'Angelo et al., “ Dynamic investigation of protein metal active sites: Interplay of XANES and molecular dynamics simulations,” J. Am. Chem. Soc. 132, 14901–14909 (2010).
44. F. Vila, J. J. Rehr, J. Kas, R. G. Nuzzo, and A. I. Frenkel, “ Dynamic structure in supported Pt nanoclusters: Real-time density functional theory and X-ray spectroscopy simulations,” Phys. Rev. B 78, 121404(R) (2008).
45. P. Castrucci et al., “ Comparison of the local order in highly oriented pyrolitic graphite and bundles of single-wall carbon nanotubes by nanoscale extended energy loss spectra,” J. Phys. Chem. C 113, 4848–4855 (2009).
47. R. P. Chatelain, V. R. Morrison, B. L. M. Klarenaar, and B. J. Siwick, “ Coherent and incoherent electron-phonon coupling in graphite observed with radio-frequency compressed ultrafast electron diffraction,” Phys. Rev. Lett. 113, 235502 (2014).
52. T. Kampfrath, L. Perfetti, F. Schapper, C. Frischkorn, and M. Wolf, “ Strongly coupled optical phonons in the ultrafast dynamics of the electronic energy and current relaxation in graphite,” Phys. Rev. Lett. 95, 187403 (2005).
60. S. Biernacki, U. Scherz, and B. Meyer, “ Temperature dependence of optical transitions between electronic energy levels in semiconductors,” Phys. Rev. B 49, 4501–4510 (1994).
64. A. H. Zewail and J. M. Thomas, 4D Electron Microscopy: Imaging in Space and Time ( World Scientific Publishing, 2010).
65.Gatan Imaging Filter User Manual, 1996.
66. A. H. Zewail and J. S. Baskin, “ Control imaging methods in advanced ultrafast electron microscopy,” U.S. patent 0,131,574 A1 (2014).
67. S. Schäfer, W. Liang, and A. H. Zewail, “ Structural dynamics and transient electric-field effects in ultrafast electron diffraction from surfaces,” Chem. Phys. Lett. 493, 11–18 (2010).
Article metrics loading...
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.
Full text loading...
Most read this month