Attosecond transient absorption instrumentation for thin film materials: Phase transitions, heat dissipation, signal stabilization, timing correction, and rapid sample rotation

Jager, Marieke F.; Ott, Christian; Kaplan, Christopher J.; Kraus, Peter M.; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1063/1.4994041

Cited by 15 publications

(8 citation statements)

References 40 publications

(36 reference statements)

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“…If the pump beam has a waist of 30 μm (≈100 μm FWHM), the time taken for the temperature to fall by 90% of the initial jump is 4 ms. This amount is significantly longer than the approximately 10-ns timescales required for bulk samples or thin films on a substrate, and it has been confirmed by heat-flow simulations in real experimental geometries [18]. The repetition rate of pump-probe experiments should then be much less than 250 Hz in order to avoid heat accumulation.…”

Section: Heating As a Source For Systematic Errorsmentioning

confidence: 77%

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Does Vo2 Host a Transient Monoclinic Metallic Phase?

et al. 2020

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Ultrafast phase transitions induced by femtosecond light pulses present a new opportunity for manipulating the properties of materials. Understanding how these transient states are different from, or similar to, their thermal counterparts is key to determining how materials can exhibit properties that are not found in equilibrium. In this paper, we reexamine the case of the light-induced insulator-metal phase transition in the prototypical, strongly correlated material VO 2 , for which a nonthermal Mott-Hubbard transition has been claimed. Here, we show that heat, even on the ultrafast timescale, plays a key role in the phase transition. When heating is properly accounted for, we find a single phase-transition threshold corresponding to the thermodynamic structural insulator-metal phase transition, and we find no evidence of a hidden transient Mott-Hubbard nonthermal phase. The interplay between the initial thermal state and the ultrafast transition may have implications for other transient states of matter.

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Section: Heating As a Source For Systematic Errorsmentioning

confidence: 77%

“…where α is the thermal diffusivity of the material, which is 2 × 10 −6 m 2 s −1 for VO 2 [18]. If the pump beam has a waist of 30 μm (≈100 μm FWHM), the time taken for the temperature to fall by 90% of the initial jump is 4 ms.…”

Section: Heating As a Source For Systematic Errorsmentioning

confidence: 99%

Does Vo2 Host a Transient Monoclinic Metallic Phase?

et al. 2020

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“…, is computed and averaged over 100 full time-delay scans. The slow drift of the pump-probe delay is stabilized over several hours using periodic reference measurements [14]. The XUV and NIR pulses are s-and p-polarized with respect to the sample surface, respectively [15].…”

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confidence: 99%

Attosecond Time-Domain Measurement of Core-Level-Exciton Decay in Magnesium Oxide

et al. 2020

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Excitation of ionic solids with extreme ultraviolet pulses creates localized core-excitons, which in some cases couple strongly to the lattice. Here, core-excitonic states of magnesium oxide are studied in the time domain at the Mg L2,3 edge with attosecond transient reflectivity spectroscopy. Attosecond pulses trigger the excitation of these short-lived quasiparticles, whose decay is perturbed by time-delayed near infrared optical pulses. Combined with a few-state theoretical model, this reveals that the optical pulse shifts the energy of bright core-exciton states as well as induces features arising from dark core-excitons. We report coherence lifetimes for the first two core-excitons of 2.3±0.2 and 1.6±0.5 femtoseconds and show that these short lifetimes are primarily a consequence of strong exciton-phonon coupling, disclosing the drastic influence of structural effects in this ultrafast relaxation process.

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“…There are, however, a number of effective and proven strategies to enhancing the rate of in-plane thermal transport. For truly "free-standing" thin samples in the quasi-2D limit, a useful model to understand the tradeoffs is provided by the equation (Jager et al, 2018):…”

Section: Heat Dissipation and Limitations In Multi-shot Experimentsmentioning

confidence: 99%

Ultrafast Electron Diffraction: Visualizing Dynamic States of Matter

Filippetto,

Musumeci,

et al. 2022

Preprint

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Since the discovery of electron-wave duality, electron scattering instrumentation has developed into a powerful array of techniques for revealing the atomic structure of matter. Beyond detecting local lattice variations in equilibrium structures with the highest possible spatial resolution, recent research efforts have been directed towards the long sought-after dream of visualizing the dynamic evolution of matter in real-time. The atomic behavior at ultrafast timescales carries critical information on phase transition and chemical reaction dynamics, the coupling of electronic and nuclear degrees of freedom in materials and molecules, the correlation between structure, function and previously hidden metastable or nonequilibrium states of matter. Ultrafast electron pulses play an essential role in this scientific endeavor, and their generation has been facilitated by rapid technical advances in both ultrafast laser and particle accelerator technologies. This review presents a summary of the remarkable developments in this field over the last few decades. The physics and technology of ultrafast electron beams is presented with an emphasis on the figures of merit most relevant for ultrafast electron diffraction (UED) experiments. We discuss recent developments in the generation, manipulation and characterization of ultrashort electron beams aimed at improving the combined spatio-temporal resolution of these measurements. The fundamentals of electron scattering from atomic matter and the theoretical frameworks for retrieving dynamic structural information from solid-state and gas-phase samples is described. Essential experimental techniques and several landmark works that have applied these approaches are also highlighted to demonstrate the widening applicability of these methods. Ultrafast electron probes with ever improving capabilities, combined with other complementary photonbased or spectroscopic approaches, hold tremendous potential for revolutionizing our ability to observe and understand energy and matter at atomic scales.

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Attosecond transient absorption instrumentation for thin film materials: Phase transitions, heat dissipation, signal stabilization, timing correction, and rapid sample rotation

Cited by 15 publications

References 40 publications

Does Vo2 Host a Transient Monoclinic Metallic Phase?

Does Vo2 Host a Transient Monoclinic Metallic Phase?

Attosecond Time-Domain Measurement of Core-Level-Exciton Decay in Magnesium Oxide

Ultrafast Electron Diffraction: Visualizing Dynamic States of Matter

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