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J. Chem. Phys. 135, 214201 (2011); http://dx.doi.org/10.1063/1.3663963 (15 pages)

Structural dynamics of surfaces by ultrafast electron crystallography: Experimental and multiple scattering theory

Sascha Schäfer, Wenxi Liang, and Ahmed H. Zewail

Physical Biology Center for Ultrafast Science and Technology, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology, Pasadena, California 91125, USA

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(Received 1 September 2011; accepted 2 November 2011; published online 2 December 2011)

Recent studies in ultrafast electron crystallography (UEC) using a reflection diffraction geometry have enabled the investigation of a wide range of phenomena on the femtosecond and picosecond time scales. In all these studies, the analysis of the diffraction patterns and their temporal change after excitation was performed within the kinematical scattering theory. In this contribution, we address the question, to what extent dynamical scattering effects have to be included in order to obtain quantitative information about structural dynamics. We discuss different scattering regimes and provide diffraction maps that describe all essential features of scatterings and observables. The effects are quantified by dynamical scattering simulations and examined by direct comparison to the results of ultrafast electron diffraction experiments on an in situ prepared Ni(100) surface, for which structural dynamics can be well described by a two-temperature model. We also report calculations for graphite surfaces. The theoretical framework provided here allows for further UEC studies of surfaces especially at larger penetration depths and for those of heavy-atom materials.

© 2011 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. EXPERIMENTAL METHODS
  3. THEORETICAL METHODS
    1. Dynamical diffraction theory
    2. The two-temperature model and structural dynamics of Ni(100)
  4. RESULTS AND DISCUSSION
    1. Qualitative features in dynamical scattering from static crystal surfaces
    2. Temporal changes of the scattering intensity
    3. Connection between the diffraction map and the diffraction pattern
    4. Dynamical scattering in nickel and graphite
      1. Dynamics of a clean Ni(100) surface
      2. Dynamics of single crystalline graphite
  5. CONCLUSION

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KEYWORDS and PACS

PACS

  • 68.35.B-

    Structure of clean surfaces (and surface reconstruction)

  • 68.35.bp

    Fullerenes

ARTICLE DATA

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

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