Femtosecond electron diffraction studies of strongly driven structural phase transitions

被引:94
作者
Siwick, BJ
Dwyer, JR
Jordan, RE
Miller, RJD
机构
[1] Univ Toronto, Dept Chem, Toronto, ON M5S 3H6, Canada
[2] Univ Toronto, Dept Phys, Toronto, ON M5S 3H6, Canada
基金
加拿大自然科学与工程研究理事会; 加拿大创新基金会;
关键词
D O I
10.1016/j.chemphys.2003.11.040
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The new technique of femtosecond electron diffraction is applied to the study of a strongly driven, laser induced solid-to-liquid phase transition in polycrystalline aluminum. This method provides an unprecedented view into the microscopic details of this process by providing a direct measurement of the atomic configuration of the system. We employ 600 fs electron pulses to see, in real time, the loss of the long-range order present in the crystalline phase and the emergence of the liquid structure in which only short-range atomic correlations are present;, this transition occurs in 3.5 ps for thin-film aluminum with an excitation fluence of 70 mJ/cm(2). The sensitivity and temporal resolution were sufficient to capture the time-dependent radial distribution function as the material evolved from the solid to the liquid state. These observations provide an atomic level description of the melting process in which the dynamics are best understood as a thermal phase transition under strongly driven conditions. In this paper, we also give a detailed description of the technical challenges associated with the production of femtosecond electron pulses and their application to the study of ultrafast structural dynamics in solid state samples and how these difficulties can be overcome. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码:285 / 305
页数:21
相关论文
共 65 条
[41]   DIRECT OBSERVATION OF THE TRANSITION-STATE [J].
POLANYI, JC ;
ZEWAIL, AH .
ACCOUNTS OF CHEMICAL RESEARCH, 1995, 28 (03) :119-132
[42]  
POLANYI JC, 1993, NOBEL LECT CHEM 1981, P359
[43]   PHOTOEMISSION ENERGY-DISTRIBUTION STUDIES OF GOLD THIN-FILMS UNDER UV EXCITATION BY A PHOTOELECTRON SPECTROSCOPIC METHOD [J].
RANGARAJAN, LM ;
BHIDE, GK .
VACUUM, 1980, 30 (11-1) :515-522
[44]  
REHTFELD B, 2002, PHYS REV B, V65
[45]   A molecular movie at 1.8 Å resolution displays the photocycle of photoactive yellow protein, a eubacterial blue-light receptor, from nanoseconds to seconds [J].
Ren, Z ;
Perman, B ;
Srajer, V ;
Teng, TY ;
Pradervand, C ;
Bourgeois, D ;
Schotte, F ;
Ursby, T ;
Kort, R ;
Wulff, M ;
Moffat, K .
BIOCHEMISTRY, 2001, 40 (46) :13788-13801
[46]   Ultrafast thermal melting of laser-excited solids by homogeneous nucleation [J].
Rethfeld, B ;
Sokolowski-Tinten, K ;
von der Linde, D .
PHYSICAL REVIEW B, 2002, 65 (09) :1-4
[47]   Femtosecond mid-infrared spectroscopy of condensed phase hydrogen-bonded systems as a probe of structural dynamics [J].
Rini, M ;
Kummrow, A ;
Dreyer, J ;
Nibbering, ETJ ;
Elsaesser, T .
FARADAY DISCUSSIONS, 2003, 122 :27-40
[48]   DISORDER EFFECTS AT THE AL(110) SURFACE [J].
SCHOMMERS, W ;
MAYER, C ;
GOBEL, H ;
VONBLANCKENHAGEN, P .
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A-VACUUM SURFACES AND FILMS, 1995, 13 (03) :1413-1415
[49]   Watching a protein as it functions with 150-ps time-resolved X-ray crystallography [J].
Schotte, F ;
Lim, MH ;
Jackson, TA ;
Smirnov, AV ;
Soman, J ;
Olson, JS ;
Phillips, GN ;
Wulff, M ;
Anfinrud, PA .
SCIENCE, 2003, 300 (5627) :1944-1947
[50]   Enzymatic transition state poise and transition state analogues [J].
Schramm, VL .
ACCOUNTS OF CHEMICAL RESEARCH, 2003, 36 (08) :588-596