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Reciprocal space slicing
(2021)
An experimental technique that allows faster assessment of out-of-plane strain dynamics of thin film heterostructures via x-ray diffraction is presented. In contrast to conventional high-speed reciprocal space-mapping setups, our approach reduces the measurement time drastically due to a fixed measurement geometry with a position-sensitive detector. This means that neither the incident (ω) nor the exit (2θ) diffraction angle is scanned during the strain assessment via x-ray diffraction. Shifts of diffraction peaks on the fixed x-ray area detector originate from an out-of-plane strain within the sample. Quantitative strain assessment requires the determination of a factor relating the observed shift to the change in the reciprocal lattice vector. The factor depends only on the widths of the peak along certain directions in reciprocal space, the diffraction angle of the studied reflection, and the resolution of the instrumental setup. We provide a full theoretical explanation and exemplify the concept with picosecond strain dynamics of a thin layer of NbO2.
Reciprocal space slicing
(2021)
An experimental technique that allows faster assessment of out-of-plane strain dynamics of thin film heterostructures via x-ray diffraction is presented. In contrast to conventional high-speed reciprocal space-mapping setups, our approach reduces the measurement time drastically due to a fixed measurement geometry with a position-sensitive detector. This means that neither the incident (ω) nor the exit (2θ) diffraction angle is scanned during the strain assessment via x-ray diffraction. Shifts of diffraction peaks on the fixed x-ray area detector originate from an out-of-plane strain within the sample. Quantitative strain assessment requires the determination of a factor relating the observed shift to the change in the reciprocal lattice vector. The factor depends only on the widths of the peak along certain directions in reciprocal space, the diffraction angle of the studied reflection, and the resolution of the instrumental setup. We provide a full theoretical explanation and exemplify the concept with picosecond strain dynamics of a thin layer of NbO2.
We employ ultrafast X-ray diffraction to compare the lattice dynamics of laser-excited continuous and granular FePt films on MgO (100) substrates. Contrary to recent results on free-standing granular films, we observe in both cases a pronounced and long-lasting out-of-plane expansion. We attribute this discrepancy to the in-plane expansion, which is suppressed by symmetry in continuous films. Granular films on substrates are less constrained and already show a reduced out-of-plane contraction. Via the Poisson effect, out-of-plane contractions drive in-plane expansion and vice versa. Consistently, the granular film exhibits a short-lived out-of-plane contraction driven by ultrafast demagnetization which is followed by a reduced and delayed expansion. From the acoustic reflections of the observed strain waves at the film-substrate interface, we extract a 13% reduction of the elastic constants in thin 10 nm FePt films compared to bulk-like samples. (C) 2018 Author(s).
We report on synchrotron-based high-repetition rate ultrafast x-ray diffraction (UXRD) experiments monitoring the transport of heat from an epitaxial La(0.7)Sr(0.3)MnO(3)/SrTiO(3) superlattice (SL) into the substrate on timescales from 100 ps to 4 mu s. Transient thermal lattice expansion was determined with an accuracy of 10(-7), corresponding to a sensitivity to temperature changes down to 0.01 K. We follow the heat flow within the SL and into the substrate after the impulsive laser heating leads to a small temperature rise of Delta T = 6 K. The transient lattice temperature can be simulated very well using the bulk heat conductivities. This contradicts the interpretation of previous UXRD measurements, which predicted a long-lasting expansion of SrRuO(3) for more than 200 ps. The disagreement could be resolved by assuming that the heat conductivity changes in the first hundred picoseconds.
We synthesize sub-THz longitudinal quasimonochromatic acoustic phonons in a SrTiO3 single crystal using a SrRuO3/SrTiO3 superlattice as an optical-acoustic transducer. The generated acoustic phonon spectrum is determined using ultrafast x-ray diffraction. The analysis of the generated phonon spectrum in the time domain reveals a k-vector dependent phonon lifetime. It is observed that even at sub-THz frequencies the phonon lifetime agrees with the 1/omega(2) power law known from Akhiezer's model for hyper sound attenuation. The observed shift of the synthesized spectrum to the higher q is discussed in the framework of nonlinear effects appearing due to the high amplitude of the synthesized phonons.
We report generation of ultra-broadband longitudinal acoustic coherent phonon wavepackets in SrTiO3 (STO) with frequency components extending throughout the first Brillouin zone. The wavepackets are efficiently generated in STO using femtosecond infrared laser excitation of an atomically flat 1.6 nm-thick epitaxial SrRuO3 film. We use femtosecond x-ray diffraction at the European X-Ray Free Electron Laser Facility to study the dispersion and damping of phonon wavepackets. The experimentally determined damping constants for multi-THz frequency phonons compare favorably to the extrapolation of a simple ultrasound damping model over several orders of magnitude.
Localized excited charge carriers generate ultrafast inhomogeneous strain in the multiferroic BiFeO3
(2014)
We apply ultrafast x-ray diffraction with femtosecond temporal resolution to monitor the lattice dynamics in a thin film of multiferroic BiFeO3 after above-band-gap photoexcitation. The sound-velocity limited evolution of the observed lattice strains indicates a quasi-instantaneous photoinduced stress which decays on a nanosecond time scale. This stress exhibits an inhomogeneous spatial profile evidenced by the broadening of the Bragg peak. These new data require substantial modification of existing models of photogenerated stresses in BiFeO3: the relevant excited charge carriers must remain localized to be consistent with the data.
Using ultrafast X-ray diffraction, we study the coherent picosecond lattice dynamics of photoexcited thin films in the two limiting cases, where the photoinduced stress profile decays on a length scale larger and smaller than the film thickness. We solve a unifying analytical model of the strain propagation for acoustic impedance-matched opaque films on a semi-infinite transparent substrate, showing that the lattice dynamics essentially depend on two parameters: One for the spatial profile and one for the amplitude of the strain. We illustrate the results by comparison with high-quality ultrafast X-ray diffraction data of SrRuO3 films on SrTiO3 substrates. (C) 2014 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.
Normalization schemes for ultrafast x-ray diffraction using a table-top laser-driven plasma source
(2012)
We present an experimental setup of a laser-driven x-ray plasma source for femtosecond x-ray diffraction. Different normalization schemes accounting for x-ray source intensity fluctuations are discussed in detail. We apply these schemes to measure the temporal evolution of Bragg peak intensities of perovskite superlattices after ultrafast laser excitation.
We investigate coherent phonon propagation in a thin film of ferroelectric PbZr0.2Ti0.8O3 (PZT) by ultrafast x-ray diffraction experiments, which are analyzed as time-resolved reciprocal space mapping in order to observe the in-and out-of-plane structural dynamics, simultaneously. The mosaic structure of the PZT leads to a coupling of the excited out-of-plane expansion to in-plane lattice dynamics on a picosecond time scale, which is not observed for out-of-plane compression.