Four-dimensional ultrafast electron microscopy of phase transitions

Reported here is direct imaging (and diffraction) by using 4D ultrafast electron microscopy (UEM) with combined spatial and temporal resolutions. In the first phase of UEM, it was possible to obtain snapshot images by using timed, single-electron packets; each packet is free of space–charge effects. Here, we demonstrate the ability to obtain sequences of snapshots (“movies”) with atomic-scale spatial resolution and ultrashort temporal resolution. Specifically, it is shown that ultrafast metal–insulator phase transitions can be studied with these achieved spatial and temporal resolutions. The diffraction (atomic scale) and images (nanometer scale) we obtained manifest the structural phase transition with its characteristic hysteresis, and the time scale involved (100 fs) is now studied by directly monitoring coordinates of the atoms themselves.

[1]  T. Kawakubo Crystal Distortion and Electric and Magnetic Transition in VO2 , 1965 .

[2]  K. Harris,et al.  Prospects for Exploiting 4D Ultrafast Electron Microscopy in Solid-State Organic and Biological Chemistry† , 2005 .

[3]  Nevill Mott,et al.  Metal-Insulator Transition , 1968 .

[4]  Masatoshi Imada,et al.  Metal-insulator transitions , 1998 .

[5]  V. Lobastov,et al.  Four-dimensional ultrafast electron microscopy. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[6]  Allen,et al.  VO2: Peierls or Mott-Hubbard? A view from band theory. , 1994, Physical review letters.

[7]  Antonio Marcus Nogueira Lima,et al.  Modeling of the hysteretic metal-insulator transition in a vanadium dioxide infrared detector , 2002 .

[8]  F Venturini,et al.  Transfer of spectral weight and symmetry across the metal-insulator transition in VO(2). , 2006, Physical review letters.

[9]  Pouget,et al.  Comment on "VO2: Peierls or Mott-Hubbard? A view from band theory" , 1994, Physical Review Letters.

[10]  Deborah P. Partlow,et al.  Switchable vanadium oxide films by a sol‐gel process , 1991 .

[11]  X. Li JECP/PCED--a computer program for simulation of polycrystalline electron diffraction pattern and phase identification. , 2004, Ultramicroscopy.

[12]  A. Cavalleri,et al.  Femtosecond Structural Dynamics in VO2 during an Ultrafast Solid-Solid Phase Transition. , 2001, Physical review letters.

[13]  J. Thomas A revolution in electron microscopy. , 2005, Angewandte Chemie.

[14]  Nevill Francis Mott,et al.  Metal-insulator transition in vanadium dioxide , 1975 .

[15]  Shao-Wei Wang,et al.  Properties of VO2 thin film prepared with precursor VO(acac)2 , 2004 .

[16]  A. Zewail 4D ultrafast electron diffraction, crystallography, and microscopy. , 2006, Annual review of physical chemistry.

[17]  Volker Eyert,et al.  The metal‐insulator transitions of VO2: A band theoretical approach , 2002, Annalen der Physik.

[18]  Howard A. Padmore,et al.  Picosecond soft X-ray absorption measurement of the photo-inducedinsulator-to-metal transition in VO2. , 2004 .

[19]  J. Gavarri,et al.  The thermochromic vanadium dioxide. I. Role of stresses and substitution on switching properties , 1993 .

[20]  John B. Goodenough,et al.  The two components of the crystallographic transition in VO2 , 1971 .

[21]  Charra,et al.  Interband electronic excitation-assisted atomic-scale restructuring of metal surfaces by nanosecond pulsed laser light , 1998, Science.

[22]  Keith Rogers,et al.  An X-ray diffraction study of semiconductor and metallic vanadium dioxide , 1993, Powder Diffraction.