Ultrafast Structural Dynamics in InSb Probed by Time-Resolved X-Ray Diffraction

Chin, A. H.; Schoenlein, R. W.; Glover, T. E.; Balling, P.; Leemans, W.P.; Shank, C. V.

doi:10.1103/physrevlett.83.336

Cited by 172 publications

(75 citation statements)

References 21 publications

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“…Similar delays are found in Refs. [10,12]. Such delays are on the order of the phonon propagation time across the laser penetration depth and are unresolved due to the temporal length of the x-ray probe.…”

Section: (Received 28 November 2000)mentioning

confidence: 99%

“…Recently, time-resolved diffraction patterns of cw ultrasonically excited crystals were obtained with a synchrotron source [7]. Other experiments have employed picosecond time-resolved x-ray diffraction to study transient lattice dynamics in metals [8], organic films [9], and impulsive strain generation and melting in semiconductors [10][11][12][13][14]. In particular Rose-Petruck et al [10] demonstrated transient ultrafast strain propagation in GaAs by laser-pump, x-ray-probe diffraction.…”

Section: (Received 28 November 2000)mentioning

confidence: 99%

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Probing Impulsive Strain Propagation with X-Ray Pulses

et al. 2001

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Pump-probe time-resolved x-ray diffraction of allowed and nearly forbidden reflections in InSb is used to follow the propagation of a coherent acoustic pulse generated by ultrafast laser-excitation. The surface and bulk components of the strain could be simultaneously measured due to the large x-ray penetration depth. Comparison of the experimental data with dynamical diffraction simulations suggests that the conventional model for impulsively generated strain underestimates the partitioning of energy into coherent modes. 78.47.+p 61.10.-i 63.20.-e The absorption of ultrafast laser pulses in opaque materials generates coherent stress when the pulse length is short compared with time for sound to propagate across an optical penetration depth [1]. The resulting strain field consists of both a surface component, static on time scales where thermal diffusion can be ignored, and a bulk component that propagates at the speed of sound (coherent acoustic phonons). This strain is typically probed by optical methods that are sensitive primarily to the phonon component within the penetration depth of the light [1,2]. However, such methods give little information about the surface component of the strain, and, moreover, they are unable to give a quantitative measure of the strain amplitude.Due to their short wavelengths, long penetration depths, and significant interaction with core electrons, x-rays are a sensitive probe of strain. We note that coherent lattice motion adds sidebands to ordinary Bragg reflection peaks due to x-ray Brillouin scattering if the momentum transfer is large compared to the Darwin width, equivalent to phonons of GHz frequency for strong reflections from perfect crystals. This effect was demonstrated many years ago with acoustoelectrically amplified phonons using a conventional x-ray tube [3].With the recent availability of high brightness short-pulse hard x-ray sources, including third generation synchrotron sources and optical laser based sources [4-6], coherent strain generation and propagation can now be probed by x-ray methods in both the frequency and time domains. Recently, time-resolved diffraction patterns of cw ultrasonically excited crystals were obtained with a synchrotron source [7]. Other experiments have employed picosecond time-resolved x-ray diffraction to study transient lattice dynamics in metals [8], organic films [9], and impulsive strain generation and melting in semiconductors [10][11][12][13][14]. In particular Rose-Petruck et al.[10] demonstrated transient ultrafast strain propagation in GaAs by laser-pump x-ray-probe diffraction. In that experiment, x-rays were diffracted far outside the Bragg peak; however, no oscillations in the diffraction efficiency were detected, and the data were consistent with a unipolar strain pulse. In a similar experiment, Lindenberg et al. [13] detected oscillations in the sidebands for an asymmetrically cut InSb crystal using a streak camera. These oscillations were due to lattice compression and were probed for discrete phonon frequencies i...

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Section: (Received 28 November 2000)mentioning

confidence: 99%

Section: (Received 28 November 2000)mentioning

confidence: 99%

Probing Impulsive Strain Propagation with X-Ray Pulses

et al. 2001

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“…The use of short laser pulses to generate high intensity, ultrashort x-ray pulses enables exciting new experimental capabilities, such as femtosecond pump-probe experiments used to temporally resolve the structural dynamics of high-Z materials on atomic (femtosecond) time scales [1,2]. In particular the unique conditions of atomicscale interaction have led to a recent experimental push to develop high-brightness, femtosecond, hard x-ray sources.…”

Section: Introductionmentioning

confidence: 99%

Three-dimensional time and frequency-domain theory of femtosecond x-ray pulse generation through Thomson scattering

Brown

Hartemann

2004

Phys. Rev. ST Accel. Beams

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The generation of high intensity, ultrashort x-ray pulses enables exciting new experimental capabilities, such as femtosecond pump-probe experiments used to temporally resolve material structural dynamics on atomic time scales. Thomson backscattering of a high intensity laser pulse with a bright relativistic electron bunch is a promising method for producing such high-brightness x-ray pulses in the 10 -100 keV range within a compact facility. While a variety of methods for producing subpicosecond x-ray bursts by Thomson scattering exist, including compression of the electron bunch to subpicosecond bunch lengths and/or colliding a subpicosecond laser pulse in a side-on geometry to minimize the interaction time, a promising alternative approach to achieving this goal while maintaining ultrahigh brightness is the production of a time-correlated (or chirped) x-ray pulse in conjunction with pulse slicing or compression. We present the results of a complete analysis of this process using a recently developed 3D time and frequency-domain code for analyzing the spatial, temporal, and spectral properties an x-ray beam produced by relativistic Thomson scattering. Based on the relativistic differential cross section, this code has the capability to calculate time and space dependent spectra of the x-ray photons produced from linear Thomson scattering for both bandwidth-limited and chirped incident laser pulses. Spectral broadening of the scattered x-ray pulse resulting from the incident laser bandwidth, laser focus, and the transverse and longitudinal phase space of the electron beam were examined. Simulations of chirped x-ray pulse production using both a chirped electron beam and a chirped laser pulse are presented. Required electron beam and laser parameters are summarized by investigating the effects of beam emittance, energy spread, and laser bandwidth on the scattered x-ray spectrum. It is shown that sufficient temporal correlation in the scattered x-ray spectrum to produce sub-100 fs temporal slice resolution can be produced from state-of-the-art, high-brightness electron beams without the need to perform longitudinal compression on the electron bunch.

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“…With the combined spatial and temporal resolutions, it is possible to study macromolecular systems (2) and reach the nonstatistical regime of energy localization and rates (3). The sensitivity to surfaces, nanometer crystals, and adsorbates offers a unique feature for comparison with x-ray bulk studies (4)(5)(6)(7)(8)(9).…”

mentioning

confidence: 99%

Ultrafast electron crystallography: Transient structures of molecules, surfaces, and phase transitions

Ruan

Vigliotti

Lobastov

et al. 2004

Proc. Natl. Acad. Sci. U.S.A.

119

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The static structure of macromolecular assemblies can be mapped out with atomic-scale resolution by using electron diffraction and microscopy of crystals. For transient nonequilibrium structures, which are critical to the understanding of dynamics and mechanisms, both spatial and temporal resolutions are required; the shortest scales of length (0.1-1 nm) and time (10 ؊13 to 10 ؊12 s) represent the quantum limit, the nonstatistical regime of rates. Here, we report the development of ultrafast electron crystallography for direct determination of structures with submonolayer sensitivity. In these experiments, we use crystalline silicon as a template for different adsorbates: hydrogen, chlorine, and trifluoroiodomethane. We observe the coherent restructuring of the surface layers with subangstrom displacement of atoms after the ultrafast heat impulse. This nonequilibrium dynamics, which is monitored in steps of 2 ps (total change <10 ps), contrasts that of the nanometer substrate. The effect of adsorbates and the phase transition at higher fluences were also studied through the evolution of streaks of interferences, Bragg spots (and their rocking curves), and rings in the diffraction patterns. We compare these results with kinematical theory and those of x-ray diffraction developed to study bulk behaviors. The sensitivity achieved here, with the 6 orders of magnitude larger cross section than x-ray diffraction, and with the capabilities of combined spatial (Ϸ0.01 Å) and temporal (300 -600 fs) resolutions, promise diverse applications for this ultrafast electron crystallography tabletop methodology.E lectron and x-ray diffraction, if endowed with ultrafast temporal resolution, can provide the ability of atomic-scale determination of structure and dynamics. In this laboratory, the method of choice has been ultrafast electron diffraction (UED) for many reasons; for recent review see ref. 1 and references therein. The extension of UED to the condensed phase and surface dynamics represents a major challenge, and here, we report on this development. With the combined spatial and temporal resolutions, it is possible to study macromolecular systems (2) and reach the nonstatistical regime of energy localization and rates (3). The sensitivity to surfaces, nanometer crystals, and adsorbates offers a unique feature for comparison with x-ray bulk studies (4-9).The conceptual framework of the approach is illustrated in Fig. 1. On the crystal, with or without the adsorbate (surface terminated by a monolayer of atoms or molecules), an ultrashort packet of electrons of 30 keV (de Broglie wavelength Ϸ0.07 Å), impinges with a wave vector k ជ i at a grazing incidence angle i Ͻ 5°. For elastic scattering, s ជ ϭ k ជ Ϫ k ជ i ; k ជ being the momentum of the scattered electron, s ϭ 4 ͞ ⅐sin ͞2, and is the scattering angle between k ជ and k ជ i . Because electrons interact strongly, the diffraction patterns give characteristics of the surface structure defined by the substrate and adsorbate. A change in temperature of the substrate is introd...

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Ultrafast Structural Dynamics in InSb Probed by Time-Resolved X-Ray Diffraction

Cited by 172 publications

References 21 publications

Probing Impulsive Strain Propagation with X-Ray Pulses

Probing Impulsive Strain Propagation with X-Ray Pulses

Three-dimensional time and frequency-domain theory of femtosecond x-ray pulse generation through Thomson scattering

Ultrafast electron crystallography: Transient structures of molecules, surfaces, and phase transitions

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