Attosecond and XUV Physics: Ultrafast Dynamics and Spectroscopy

Vrakking, Marc J. J.

doi:10.1002/9783527677689.ch1

Cited by 8 publications

(9 citation statements)

References 94 publications

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“…The optical process of materials under optical field can be expressed by expanding the macroscopic polarization P , as follows: [ 58,59 ]

P = ε_{0} [χ_{1} + χ_{2} : E + χ_{3} ⋮ EE + \dots] E

where ɛ 0 , χ 1 and χ n ( n ≥ 2) represent the dielectric constant of free space, linear optical susceptibility, and n ‐th‐order nonlinear susceptibility, respectively. The linear optical susceptibility corresponds to conventional linear optical effects such as refraction and absorption.…”

Section: Ultrafast Pump‐probe Spectroscopymentioning

confidence: 99%

Probing Ultrafast Dynamics of Ferroelectrics by Time‐Resolved Pump‐Probe Spectroscopy

et al. 2021

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Ferroelectric materials have been a key research topic owing to their wide variety of modern electronic and photonic applications. For the quick exploration of higher operating speed, smaller size, and superior efficiencies of novel ferroelectric devices, the ultrafast dynamics of ferroelectrics that directly reflect their respond time and lifetimes have drawn considerable attention. Driven by time-resolved pump-probe spectroscopy that allows for probing, controlling, and modulating dynamic processes of ferroelectrics in real-time, much research efforts have been made to understand and exploit the ultrafast dynamics of ferroelectric. Herein, the current state of ultrafast dynamic features of ferroelectrics tracked by time-resolved pump-probe spectroscopy is reviewed, which includes ferroelectrics order parameters of polarization, lattice, spin, electronic excitation, and their coupling. Several potential perspectives and possible further applications combining ultrafast pump-probe spectroscopy and ferroelectrics are also presented. This review offers a clear guidance of ultrafast dynamics of ferroelectric orders, which may promote the rapid development of next-generation devices.

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“…The optical process of materials under optical field can be expressed by expanding the macroscopic polarization P , as follows: [ 58,59 ]

P = ε_{0} [χ_{1} + χ_{2} : E + χ_{3} ⋮ EE + \dots] E

Section: Ultrafast Pump‐probe Spectroscopymentioning

confidence: 99%

Probing Ultrafast Dynamics of Ferroelectrics by Time‐Resolved Pump‐Probe Spectroscopy

et al. 2021

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“…Beyond X-ray pulse characterization, angular streaking (and streaking experiments in general) can be used to probe photoionization dynamics on the attosecond timescale [4,6]. In one of the first experiments of attosecond physics, linear streaking was used to time-resolve the Auger process in krypton atoms [83].…”

Section: (C) Site-specific Window On Photoionization and Electron Correlation Dynamicsmentioning

confidence: 99%

“…This nuclear motion, however, is rather slow compared with far more rapid motion of the electrons, whose charge provides the screening to stabilize molecules, and whose redistribution initiates all chemical changes, including isomerization and dissociation. The natural timescale for electron motion in atoms and molecules is about 100 times faster than the timescale for nuclear motion: electrons move across a molecular bond in 0.1-1 fs [2][3][4]. Dynamics on this timescale is a science frontier both for experiments and for quantum many-body theory [5][6][7].…”

Section: Introductionmentioning

confidence: 99%

Development of ultrafast capabilities for X-ray free-electron lasers at the linac coherent light source

Coffee

Cryan

Duris

et al. 2019

Phil. Trans. R. Soc. A.

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The ability to produce ultrashort, high-brightness X-ray pulses is revolutionizing the field of ultrafast X-ray spectroscopy. Free-electron laser (FEL) facilities are driving this revolution, but unique aspects of the FEL process make the required characterization and use of the pulses challenging. In this paper, we describe a number of developments in the generation of ultrashort X-ray FEL pulses, and the concomitant progress in the experimental capabilities necessary for their characterization and use at the Linac Coherent Light Source. This includes the development of sub-femtosecond hard and soft X-ray pulses, along with ultrafast characterization techniques for these pulses. We also describe improved techniques for optical cross-correlation as needed to address the persistent challenge of external optical laser synchronization with these ultrashort X-ray pulses. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays’.

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“…Extreme ultraviolet (XUV) transient absorption spectroscopy makes this possible using a probe pulse in the XUV regime to measure core-level electronic transitions to characterize the occupancies and structural features of the valence and conduction bands. Promoting electrons from the silicon 2p orbital to unoccupied states creates localized core-hole excitons that impart interpretable structural information on the XUV absorption spectra. , The femtosecond resolution of the technique allows for the observation of short-lived excited carrier and phonon states …”

Section: Introductionmentioning

confidence: 99%

Characterization of Carrier Cooling Bottleneck in Silicon Nanoparticles by Extreme Ultraviolet (XUV) Transient Absorption Spectroscopy

et al. 2021

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Silicon nanoparticles have the promise to surpass the theoretical efficiency limit of single-junction silicon photovoltaics by the creation of a "phonon bottleneck," a theorized slowing of the cooling rate of hot optical phonons that in turn reduces the cooling rate of hot carriers in the material. Verifying the presence of a phonon bottleneck in silicon nanoparticles requires simultaneous resolution of electronic and structural changes at short timescales. Here, extreme ultraviolet transient absorption spectroscopy is used to observe the excited-state electronic and lattice dynamics in polycrystalline silicon nanoparticles following 800 nm photoexcitation, which excites carriers with 0.35 ± 0.03 eV excess energy above the Δ 1 conduction band minimum. The nanoparticles have nominal 100 nm diameters with crystalline grain sizes of about ∼16 nm. The extracted carrier−phonon and phonon−phonon relaxation times of the nanoparticles are compared to those for a silicon (100) single-crystal thin film at similar carrier densities (2 × 10 19 cm −3 for the nanoparticles and 6 × 10 19 cm −3 for the film). The measured carrier− phonon and phonon−phonon scattering lifetimes for the polycrystalline nanoparticles are 870 ± 40 fs and 17.5 ± 0.3 ps, respectively, versus 195 ± 20 fs and 8.1 ± 0.2 ps, respectively, for the silicon thin film. The reduced scattering rates observed in the nanoparticles are consistent with the phonon bottleneck hypothesis.

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Attosecond and XUV Physics: Ultrafast Dynamics and Spectroscopy

Cited by 8 publications

References 94 publications

Probing Ultrafast Dynamics of Ferroelectrics by Time‐Resolved Pump‐Probe Spectroscopy

Probing Ultrafast Dynamics of Ferroelectrics by Time‐Resolved Pump‐Probe Spectroscopy

Development of ultrafast capabilities for X-ray free-electron lasers at the linac coherent light source

Characterization of Carrier Cooling Bottleneck in Silicon Nanoparticles by Extreme Ultraviolet (XUV) Transient Absorption Spectroscopy

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