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Register a new userThermoelastic study of nanolayered structures using time-resolved x-ray diffraction at high repetition rate
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We investigate the thermoelastic response of a nanolayered sample composed of a metallic SrRuO3 (SRO) electrode sandwiched between a ferroelectric Pb(Zr0.2Ti0.8)O3 (PZT) film with negative thermal expansion and a SrTiO3 substrate. SRO is rapidly heated by fs-laser pulses with 208 kHz repetition rate. Diffraction of x-ray pulses derived from a synchrotron measures the transient out-of-plane lattice constant c of all three materials simultaneously from 120 ps to 5 mus with a relative accuracy up to Delta c/c = 10^-6. The in-plane propagation of sound is essential for understanding the delayed out of plane expansion.
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We present here an overview of Coherent X-ray Diffraction Imaging (CXDI) with its application to nanostructures. This imaging approach has become especially important recently due to advent of X-ray Free-Electron Lasers (XFEL) and its applications to the fast developing technique of serial X-ray crystallography. We start with the basic description of coherent scattering on the finite size crystals. The difference between conventional crystallography applied to large samples and coherent scattering on the finite size samples is outlined. The formalism of coherent scattering from a finite size crystal with a strain field is considered. Partially coherent illumination of a crystalline sample is developed. Recent experimental examples demonstrating applications of CXDI to the study of crystalline structures on the nanoscale, including experiments at FELs, are also presented.
Using a time-resolved detection scheme in scanning transmission X-ray microscopy (STXM) we measured element resolved ferromagnetic resonance (FMR) at microwave frequencies up to 10,GHz and a spatial resolution down to 20,nm at two different synchrotrons. We present different methods to separate the contribution of the background from the dynamic magnetic contrast based on the X-ray magnetic circular dichroism (XMCD) effect. The relative phase between the GHz microwave excitation and the X-ray pulses generated by the synchrotron, as well as the opening angle of the precession at FMR can be quantified. A detailed analysis for homogeneous and inhomogeneous magnetic excitations demonstrates that the dynamic contrast indeed behaves as the usual XMCD effect. The dynamic magnetic contrast in time-resolved STXM has the potential be a powerful tool to study the linear and non-linear magnetic excitations in magnetic micro- and nano-structures with unique spatial-temporal resolution in combination with element selectivity.
Attosecond pulses, produced through high-order harmonic generation in gases, have been successfully used for observing ultrafast, sub-femtosecond electron dynamics in atoms, molecules and solid state systems. Todays typical attosecond sources, however, are often impaired by their low repetition rate and the resulting insufficient statistics, especially when the number of detectable events per shot is limited. This is the case for experiments where several reaction products must be detected in coincidence, and for surface science applications where space-charge effects compromise spectral and spatial resolution. In this work, we present an attosecond light source operating at 200 kHz, which opens up the exploration of phenomena previously inaccessible to attosecond interferometric and spectroscopic techniques. Key to our approach is the combination of a high repetition rate, few-cycle laser source, a specially designed gas target for efficient high harmonic generation, a passively and actively stabilized pump-probe interferometer and an advanced 3D photoelectron/ion momentum detector. While most experiments in the field of attosecond science so far have been performed with either single attosecond pulses or long trains of pulses, we explore the hitherto mostly overlooked intermediate regime with short trains consisting of only a few attosecond pulses.e also present the first coincidence measurement of single-photon double ionization of helium with full angular resolution, using an attosecond source. This opens up for future studies of the dynamic evolution of strongly correlated electrons.
Heterostructures of PbTiO$_3$/SrTiO$_3$ superlattices have shown the formation of polar vortices, in which a continuous rotation of ferroelectric polarization spontaneously forms. Recently, Shafer {it{et al.}} [Proc. Natl. Acad. Sci. (PNAS) {bf{115}}, 915 (2018)] reported strong {it{non-magnetic}} circular dichroism (CD) in resonant soft x-ray diffraction at the Ti $L_3$ edge from such superlattices. The authors ascribe the CD to the chiral rotation of a polar vector. However, a polar vector is invisible to the parity-even electric-dipole transition which governs absorption in the soft x-ray region. A realistic, non-magnetic explanation of the observed effect is found in Templeton-Templeton scattering. Following this route, the origin of the CD in Bragg diffraction is shown by us to be the chiral array of charge quadrupole moments that forms in these heterostructures. While there is no charge quadrupole moment in the spherically symmetric $3d^0$ valence state of Ti$^{4+}$, the excited state $2p_{3/2}3d(t_{2g})$ at the Ti $L_3$ resonance is known to have a quadrupole moment. Our expressions for intensities of satellite Bragg spots in resonance-enhanced diffraction of circularly polarized x-rays, including their harmonic content, account for all observations reported by Shafer {it{et al.}} We predict both intensities of Bragg spots for the second harmonic of a chiral superlattice and circular polarization created from unpolarized x-rays, in order that our successful explanation of existing diffraction data can be further scrutinized through renewed experimental investigations. The increased understanding of chiral dipole arrangements could open the door to switchable optical polarization.
Time- and angle-resolved photoelectron spectroscopy (trARPES) is a powerful method to track the ultrafast dynamics of quasiparticles and electronic bands in energy and momentum space. We present a setup for trARPES with 22.3 eV extreme-ultraviolet (XUV) femtosecond pulses at 50-kHz repetition rate, which enables fast data acquisition and access to dynamics across momentum space with high sensitivity. The design and operation of the XUV beamline, pump-probe setup, and UHV endstation are described in detail. By characterizing the effect of space-charge broadening, we determine an ultimate source-limited energy resolution of 60 meV, with typically 80-100 meV obtained at 1-2e10 photons/s probe flux on the sample. The instrument capabilities are demonstrated via both equilibrium and time-resolved ARPES studies of transition-metal dichalcogenides. The 50-kHz repetition rate enables sensitive measurements of quasiparticles at low excitation fluences in semiconducting MoSe$_2$, with an instrumental time resolution of 65 fs. Moreover, photo-induced phase transitions can be driven with the available pump fluence, as shown by charge density wave melting in 1T-TiSe$_2$. The high repetition-rate setup thus provides a versatile platform for sensitive XUV trARPES, from quenching of electronic phases down to the perturbative limit.
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