Femtosecond X-ray Studies of Photo-induced Structural Phase Transitions

Cavalleri, A.; Blome, C.; Forget, Philippe; Kieffer, Jérôme; Magnan, S.; Siders, C. W.; Sokolowski‐Tinten, K.; Squier, Jeffrey A.; Tóth, Cs.; Linde, D. Vonder

doi:10.1080/0141159021000008936

Cited by 8 publications

(4 citation statements)

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“…The birth and development of synchrotron facilities provided X-ray photon fluxes that were several orders of magnitude higher than X-rays generated by a rotating anode. During the past decade, three new types of pulsed X-ray sources have been developed, 1) the third generation synchrotron sources [42] (Figure 3), 2) ultrafast laser-generated-plasma X-ray sources, [43][44][45][46][47][48][49][50] and 3) ultrafast laser-generated high-harmonic soft X-rays. Early studies by using older generation synchrotron sources were carried out mainly by one of three approaches: 1) gating detectors or chopping an X-ray pulse to gain the time resolution, [22][23][24][25][26][27][28][29][30] 2) cryogenic trapping of excited-state species for a long period of time so that they can be examined by the steady-state methods, [31][32][33][34][35] and 3) by using energy dispersive X-ray absorption, which captures the excited-state structure within the detector readout time.…”

Section: Why Is Direct Molecular Structural Information On Excitedmentioning

confidence: 99%

Taking Snapshots of Photoexcited Molecules in Disordered Media by Using Pulsed Synchrotron X‐rays

Chen

2004

Angew Chem Int Ed

112

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Photoexcited molecules are quintessential reactants in photochemistry. Structures of these photoexcited molecules in disordered media in which a majority of photochemical reactions take place remained elusive for decades owing to a lack of suitable X-ray sources, despite their importance in understanding fundamental aspects in photochemistry. As new pulsed X-ray sources become available, short-lived excited-state molecular structures in disordered media can now be captured by using laser-pulse pump, X-ray pulse-probe techniques of third-generation synchrotron sources with time resolutions of 30-100 ps, as demonstrated by examples in this review. These studies provide unprecedented information on structural origins of molecular properties in the excited states. By using other ultrafast X-ray facilities that will be completed in the near future, time-resolution for the excited-state structure measurements should reach the femtosecond time scales, which will make "molecular movies" of bond breaking or formation, and vibrational relaxation, a reality.

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Section: Why Is Direct Molecular Structural Information On Excitedmentioning

confidence: 99%

Taking Snapshots of Photoexcited Molecules in Disordered Media by Using Pulsed Synchrotron X‐rays

Chen

2004

Angew Chem Int Ed

112

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“…The duration of this x-ray burst is similar to the duration of the laser pulse, and therefore can be as short as tens of femtoseconds. These pulses have allowed for numerous useful experiments [21][22][23][24][25][26][27][28][29][30] . The significant downside is the fixed energy of the x-ray pulse.…”

Section: Figurementioning

confidence: 99%

A High-Energy, Ultrashort-Pulse X-Ray System for the Dynamic Study of Heavy, Dense Materials

Gibson

2004

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Thomson-scattering based x-ray radiation sources, in which a laser beam is scattered off a relativistic electron beam resulting in a high-energy x-ray beam, are currently being developed by several groups around the world to enable studies of dynamic material properties which require temporal resolution on the order of tens of femtoseconds to tens of picoseconds. These sources offer pulses that are shorter than available from synchrotrons, more tunable than available from so-called K a sources, and more penetrating and more directly probing than ultrafast lasers. Furthermore, Thomson-scattering sources can scale directly up to x-ray energies in the few MeV range, providing peak brightnesses far exceeding any other sources in this regime. This dissertation presents the development effort of one such source at Lawrence Livermore National Laboratory, the Picosecond Laser-Electron InterAction for the Dynamic Evaluation of Structures (PLEIADES) project, designed to target energies from 30 keV to 200 keV, with a peak brightness on the order of 10 18 photons•s-1 •mm-2 •mrad-2 •0.01% bandwidth-1. A 10 TW Ti:Sapphire based laser system provides the photons for the interaction, and a 100 MeV accelerator with a 1.6 cell S-Band photoinjector at the front end provides the electron beam. The details of both these systems are presented, as is the initial x-ray production and characterization, validating the theory of Thomson scattering. In addition to the systems used to enable PLEIADES, two alternative systems are discussed. An 8.5 GHz X-Band photoinjector, capable of sustaining higher accelerating gradients and producing lower emittance electron beams in a smaller space than the S-Band gun, is presented, and the initial operation and commissioning of this gun is presented. Also, a hybrid chirped-pulse amplification system is presented as an alternative to the standard regenerative amplifier technology in high-power ultrafast laser systems. This system combines an optical-parametric chirped-pulse amplification (OPCPA) system with a titanium:sapphire-based four-pass amplifier to provide the high pre-pulse contrast and ease of assembly of an OPCPA using a commercial pump laser while avoiding the loss of efficiency such a system would normally entail. v 3.3.4.5 Bunch duration measurements..

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“…The relatively low flux and availability of these sources have limited their utility. Nonetheless these sources were critical in developing the nascent field of ultrafast x-ray science [45,46,47,48] including the experiments described here.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast x-ray probes of dynamics in solids

Trigo¹,

Dean²,

Reis³

2021

Preprint

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Advances in our ability to understand and utilize the world around us have always relied on the development of advanced tools for probing and manipulating materials properties. X-ray matter interactions played a critical role in the development of the modern theory of solid-state materials that has continued over more than a century. The development of ever-brighter x-ray sources has facilitated ever more sensitive x-ray scattering and spectroscopy measurements that are able to probe not just the lattice structure, but also the spectrum of elementary excitations in complex materials. The interactions underlying the electronic, magnetic and thermal properties of solids tend to be associated with lengthscales comparable to the atomic separation and timescales ranging from femtosecond to picoseconds. The short wavelength, femtosecond pulses from x-ray free-electron laser (XFEL)s therefore offer unprecedented opportunities to probe and understand material properties on their natural lengthscales and timescales of these processes. This chapter reviews a number of exemplary XFEL-based experiments on lattice and electronic dynamics, and their microscopic interactions both near and out of equilibrium. We conclude with a brief discussion of new forms of spectroscopy enabled by the combination of high flux and short pulse duration and give an outlook for how the field will develop in the future.

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Femtosecond X-ray Studies of Photo-induced Structural Phase Transitions

Cited by 8 publications

References 0 publications

Taking Snapshots of Photoexcited Molecules in Disordered Media by Using Pulsed Synchrotron X‐rays

Taking Snapshots of Photoexcited Molecules in Disordered Media by Using Pulsed Synchrotron X‐rays

A High-Energy, Ultrashort-Pulse X-Ray System for the Dynamic Study of Heavy, Dense Materials

Ultrafast x-ray probes of dynamics in solids

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