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Henrik T. Lemke

Publications and source records attributed to Henrik T. Lemke.

11 recordsLinked to original sources

THz-induced phonon mode mixing and collective dynamics in a polar nanolattice

Manipulating phonons through symmetry is a fundamental approach to alter the dynamic responses of materials. Most often new phases are sought through control of the unit-cell (e.g. via strain, doping, light, etc.). By comparison, there is vast potential to look beyond the unit-cell into higher-order architectures to control wave scattering and interference effects that remains less explored. We describe the THz-induced dynamics of an SrTiO$_{3}$ thin film with a nanoscale ordered interfacial dislocation network probed with 2- and 3-dimensional time-resolved x-ray diffraction and classical molecular dynamics simulations. We find that symmetry breaking at all scales is an effective approach to create a dynamical electric polarization and to control phonon mixing that generates previously unreported collective modes in the THz regime with circular vortex-like displacements. This work opens a new pathway to explore dynamical functional properties that can be extended to magnetic, electric, and ferroelectric systems by controlling the real-space topology via epitaxy.

cond-mat.str-el↗

Ultrafast Decoherence of Charge Density Waves in K$_{0.3}$MoO$_{3}$

Recent works have suggested that transient suppression of a charge density wave (CDW) by an ultra-short excitation can lead to an inversion of the CDW phase. We experimentally investigate the dynamics of the CDW in K$_{0.3}$MoO$_{3}$ by time resolved x-ray diffraction after excitation with optical pulses. Our results indicate a transient inversion of the CDW phase close to the surface that evolves into a highly disordered state in less than one picosecond. Numerical simulations solving the Ginzburg-Landau equation including disorder from strong pinning defects reproduce our main observations. Our findings highlight the critical role of disorder in schemes for coherent control in condensed matter systems.

cond-mat.str-el↗

Ultrafast surface melting of orbital order in La0.5Sr1.5MnO4

Understanding how light modifies long-range order in quantum materials is key to improving our ability to control functionality. However, this is challenging if the response is heterogeneous. Here we address the most common form of light-induced heterogeneity, surface melting, and measure the dynamics of orbital order in the layered manganite, La0.5Sr1.5MnO4. We isolate the surface dynamics from the bulk by measuring the orbital truncation rod as well as orbital Bragg peak. After photoexcitation, the orbital Bragg peak shows an unusual narrowing, which suggests an increase in the correlation length in the probed volume. In contrast, the correlation length at the surface decreases. These differences can be reconciled if the material is heterogeneous, and light melts a less ordered surface. By isolating the surface response, we determine that the loss of long-range order is an incoherent process, which is likely accompanied by the formation of local polarons.

cond-mat.str-el↗

A set-up for Hard X-ray Time-resolved Resonant Inelastic X-ray Scattering at SwissFEL

We present a new set up for resonant inelastic hard X-ray scattering at the Bernina beamline of SwissFEL with energy, momentum, and temporal resolution. The compact R=0.5 m Johann-type spectrometer can be equipped with up to 3 crystal analysers and allows efficient collection of RIXS spectra. Optical pumping for time-resolved studies can be realized with a broad span of optical wavelengths. We demonstrate the performance of the set-up at overall ~180 meV resolution in a study of ground-state and photoexcited (at 400 nm) honeycomb 5d iridate $α$-$\mathrm{Li_2IrO_3}$. Steady-state RIXS spectra at the Iridium ${L_3}$-edge (11.214 keV) have been collected and are in very good agreement with data collected at synchrotrons. The time-resolved RIXS transients (pumped minus unpumped spectra) exhibit changes in the energy-loss region <2 eV, whose features mostly result from the hopping nature of 5d electrons in the honeycomb lattice. These changes are ascribed to modulations of the Ir-to-Ir intersite transition scattering efficiency, which we associate to a transient screening of the on-site Coulomb interaction.

cond-mat.str-el↗

Effect of intense x-ray free-electron laser transient gratings on the magnetic domain structure of Tm:YIG

Magnetic patterns can be controlled globally using fields or spin polarized currents. In contrast, the local control of the magnetization on the nanometer length scale remains challenging. Here, we demonstrate how magnetic domain patterns in a Tm-doped yttrium iron garnet (Tm:YIG) thin film with perpendicular magnetic anisotropy can be permanently and locally imprinted by high intensity photon pulses of a hard x-ray transient grating (XTG). Micromagnetic simulations provide a qualitative understanding of the observed changes in the orientation of magnetic domains in Tm:YIG and XTG-induced changes. The presented results offer a route for the local manipulation of the magnetic state using hard XTG.

cond-mat.mtrl-sci↗

Hard X-ray Transient Grating Spectroscopy on Bismuth Germanate

Optical-domain Transient Grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique used to probe vibrational, magnetic and electronic degrees of freedom in the time domain. The newly developed coherent X-ray Free Electron Laser sources allow its extension to the X-ray regime. Xrays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element-specificity can address core-excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. We demonstrate for the first time TG excitation in the hard X-ray range at 7.1 keV. In Bismuth Germanate (BGO), the nonresonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods.

physics.optics↗

Origin of vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering

Disentangling the dynamics of electrons and nuclei during nonadiabatic molecular transformations remains a considerable experimental challenge. Here we have investigated photoinduced electron transfer dynamics following a metal-to-ligand charge-transfer (MLCT) excitation of the [Fe(bmip)2]2+ photosensitizer, where bmip = 2,6-bis(3-methyl-imidazole-1- ylidine)-pyridine, with simultaneous femtosecond-resolution Fe Kα and K\b{eta} X-ray Emission Spectroscopy (XES) and Wide Angle X-ray Scattering (WAXS). This measurement clearly shows temporal oscillations in the XES and WAXS difference signals with the same 278 fs period oscillation. The oscillatory signal originates from an Fe-ligand stretching mode vibrational wavepacket on a triplet metal-centered (3MC) excited state surface. The vibrational wavepacket is created by 40% of the excited population that undergoes electron transfer from the non-equilibrium MLCT excited state to the 3MC excited state with a 110 fs time constant, while the other 60% relaxes to a 3MLCT excited state in parallel. The sensitivity of the Kα XES spectrum to molecular structure results from core-level vibronic coupling, due to a 0.7% average Fe-ligand bond length difference in the lowest energy geometry of the 1s and 2p core-ionized states. These results highlight the importance of vibronic effects in time-resolved XES experiments and demonstrate the role of metal-centered excited states in the electronic excited state relaxation dynamics of an Fe carbene photosensitizer.

physics.chem-ph↗

Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [Co(terpy)2]2+

We study the structural dynamics of photoexcited [Co(terpy)2]2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of the high spin state is established on a single-picosecond time scale and that this state has a lifetime of ~ 7 ps.

physics.chem-ph↗

Watching coherent molecular structural dynamics during photoreaction: beyond kinetic description

A deep understanding of molecular photo-transformations is challenging because of the complex interaction between the configurations of electrons and nuclei. An initial optical excitation dissipates energy into electronic and structural degrees of freedom, often in less than one trillionth (10^-12) of a second. Molecular dynamics induced by photoexcitation have been very successfully studied with femtosecond optical spectroscopies, but electronic and nuclear dynamics are often very difficult to disentangle. X-ray based spectroscopies can reduce the ambiguity between theoretical models and experimental data, but it is only with the recent development of bright ultrafast X-ray sources, that key information during transient molecular processes can be obtained on their intrinsic timescale. In this letter, Free Electron Laser (FEL) radiation is used to measure ultrafast changes in the X-ray Absorption Near Edge Structure (XANES) during the prototypical photoreaction of a spin crossover compound. We reveal its transformation from the ligand-located electronic photoexcitation to the structural trapping of the high spin state. The results require a description beyond a kinetic model and provide a direct observation of a dynamic breathing of the main structural change. The coherent structural oscillations (period of ~265 fs) in the photoproduct potential lose synchrony within ~330 fs, whereas incoherent motions reveal the energy redistribution and vibrational cooling within ~1.6 ps. We foresee that ultrafast X-ray spectroscopies will provide invaluable insight to understand the complex physics of fundamental light induced phenomena, which are of prime interest in a multitude of chemical, physical and biological processes.

physics.chem-ph↗

Phonon Spectroscopy with Sub-meV Resolution by Femtosecond X-ray Diffuse Scattering

We present a reconstruction of the transverse acoustic phonon dispersion of germanium from femtosecond time-resolved x-ray diffuse scattering measurements at the Linac Coherent Light Source. We demonstrate an energy resolution of 0.3 meV with momentum resolution of 0.01 nm^-1 using 10 keV x-rays with a bandwidth of ~ 1 eV. This high resolution was achieved simultaneously for a large section of reciprocal space including regions closely following three of the principle symmetry directions. The phonon dispersion was reconstructed with less than three hours of measurement time, during which neither the x-ray energy, the sample orientation, nor the detector position were scanned. These results demonstrate how time-domain measurements can complement conventional frequency domain inelastic scattering techniques.

cond-mat.mtrl-sci↗

Performance of an LPD prototype detector at MHz frame rates under Synchrotron and FEL radiation

A MHz frame rate X-ray area detector (LPD - Large Pixel Detector) is under development by the Rutherford Appleton Laboratory for the European XFEL. The detector will have 1 million pixels and allows analogue storage of 512 images taken at 4.5 MHz in the detector front end. The LPD detector has 500 mm thick silicon sensor tiles that are bump bonded to a readout ASIC. The ASICs preamplifier provides relatively low noise at high speed which results in a high dynamic range of 10^5 photons over an energy range of 5-20 keV. Small scale prototypes of 32x256 pixels (LPD 2-Tile detector) and 256x256 pixels (LPD supermodule detector) are now available for X-ray tests. The performance of prototypes of the detector is reported for first tests under synchrotron radiation (PETRA III at DESY) and Free-Electron-Laser radiation (LCLS at SLAC). The initial performance of the detector in terms of signal range and noise, radiation hardness and spatial and temporal response are reported. The main result is that the 4.5 MHz sampling detection chain is reliably working, including the analogue on-chip memory concept. The detector is at least radiation hard up to 5 MGy at 12 keV. In addition the multiple gain concept has been demonstrated over a dynamic range to 10^4 at 12 keV with a readout noise equivalent to <1 photon rms in its most sensitive mode.

physics.ins-det↗