Ultrafast modulation of electronic structure by coherent phonon excitations.

Femtosecond x-ray absorption spectroscopy with a laser-driven high-harmonic source is used to map ultrafast changes of x-ray absorption by femtometer-scale coherent phonon displacements. In LiBH4, displacements along an Ag phonon mode at 10 THz are induced by impulsive Raman excitation and give rise to oscillatory changes of x-ray absorption at the Li K-edge. Electron density maps from femtosecond x-ray diffraction data show that the electric field of the pump pulse induces a charge transfer from the BH4- to neighboring Li+ ions, resulting in a differential Coulomb force that drives lattice vibrations in this virtual transition state.

Impingement-free range of movement, acetabular component cover and early clinical results comparing 'femur-first' navigation and 'conventional' minimally invasive total hip arthroplasty: a randomised controlled trial.

We report the kinematic and early clinical results of a patient- and observer-blinded randomised controlled trial in which CT scans were used to compare potential impingement-free range of movement (ROM) and acetabular component cover between patients treated with either the navigated 'femur-first' total hip arthroplasty (THA) method (n = 66; male/female 29/37, mean age 62.5 years; 50 to 74) or conventional THA (n = 69; male/female 35/34, mean age 62.9 years; 50 to 75). The Hip Osteoarthritis Outcome Score, the Harris hip score, the Euro-Qol-5D and the Mancuso THA patient expectations score were assessed at six weeks, six months and one year after surgery. A total of 48 of the patients (84%) in the navigated 'femur-first' group and 43 (65%) in the conventional group reached all the desirable potential ROM boundaries without prosthetic impingement for activities of daily living (ADL) in flexion, extension, abduction, adduction and rotation (p = 0.016). Acetabular component cover and surface contact with the host bone were > 87% in both groups. There was a significant difference between the navigated and the conventional groups' Harris hip scores six weeks after surgery (p = 0.010). There were no significant differences with respect to any clinical outcome at six months and one year of follow-up. The navigated 'femur-first' technique improves the potential ROM for ADL without prosthetic impingement, although there was no observed clinical difference between the two treatment groups.

High-field terahertz bulk photovoltaic effect in lithium niobate.

The terahertz (THz) response of the ferroelectric prototype material lithium niobate (LiNbO3) is studied in the nonperturbative regime of light-matter interaction. Applying two-dimensional THz spectroscopy with few-cycle pulses of an amplitude E≈100 kV/cm and a center frequency of 2 THz, we dissect the overall nonlinear response into different orders in the electric field. The underlying nonlinear current is of interband character and consists of a strong low-frequency shift current (SC) and higher harmonics of the THz fundamental. The SC component originates from the lack of inversion symmetry and the strong interband decoherence for long electron trajectories in k space as shown by theoretical calculations.

Perspective: structural dynamics in condensed matter mapped by femtosecond x-ray diffraction.

Ultrashort soft and hard x-ray pulses are sensitive probes of structural dynamics on the picometer length and femtosecond time scales of electronic and atomic motions. Recent progress in generating such pulses has initiated new directions of condensed matter research, exploiting a variety of x-ray absorption, scattering, and diffraction methods to probe photoinduced structural dynamics. Atomic motion, changes of local structure and long-range order, as well as correlated electron motion and charge transfer have been resolved in space and time, providing a most direct access to the physical mechanisms and interactions driving reversible and irreversible changes of structure. This perspective combines an overview of recent advances in femtosecond x-ray diffraction with a discussion on ongoing and future developments.

Electron transfer in a virtual quantum state of LiBH4 induced by strong optical fields and mapped by femtosecond x-ray diffraction.

Transient polarizations connected with a spatial redistribution of electronic charge in a mixed quantum state are induced by optical fields of high amplitude. We determine for the first time the related transient electron density maps, applying femtosecond x-ray powder diffraction as a structure probe. The prototype ionic material LiBH4 driven nonresonantly by an intense sub-40 fs optical pulse displays a large-amplitude fully reversible electron transfer from the BH4(-) anion to the Li+ cation during excitation. Our results establish this mechanism as the source of the strong optical polarization which agrees quantitatively with theoretical estimates.

Ultrafast soft-mode driven charge relocation in an ionic crystal.

Transient electron density maps of potassium dihydrogen phosphate (KH(2)PO(4), KDP) are derived from femtosecond X-ray powder diffraction patterns. Upon photoexcitation, the low-frequency TO soft mode is elongated impulsively and modulates the electronic charge distribution on the length scale of interatomic distances, much larger than the vibrational amplitude. The results demonstrate a charge transfer from the volumes around the P-atoms and K(+)-ions to those containing the O-HO units and a quadrupolar distortion of the K(+) charge distribution. This behavior reflects the interplay of nuclear motions and electric polarizations in the ionic crystal lattice.

Strong correlation of electronic and lattice excitations in GaAs/AlGaAs semiconductor quantum wells revealed by two-dimensional terahertz spectroscopy.

Coulomb-mediated interactions between intersubband excitations of electrons in GaAs/AlGaAs double quantum wells and longitudinal optical phonons are studied by two-dimensional spectroscopy in the terahertz frequency range. The multitude of diagonal and off-diagonal peaks in the 2D spectrum gives evidence of strong polaronic signatures in the nonlinear response. A quantitative theoretical analysis reveals a dipole coupling of electrons to the polar lattice that is much stronger than in bulk GaAs, due to a dynamic localization of the electron wave function by scattering processes.

The rotating-crystal method in femtosecond X-ray diffraction.

We report the first implementation of the rotating-crystal method in femtosecond X-ray diffraction. Applying a pump-probe scheme with 100 fs hard X-ray probe pulses from a laser-driven plasma source, the novel technique is demonstrated by mapping structural dynamics of a photoexcited bismuth crystal via changes of the diffracted intensity on a multitude of Bragg reflections. The method is compared to femtosecond powder diffraction and to Bragg diffraction from a crystal with stationary orientation.

Two-dimensional terahertz correlation spectra of electronic excitations in semiconductor quantum wells.

We discuss a novel approach for nonlinear two-dimensional (2D) spectroscopy in the terahertz (THz) frequency range which is based on a collinear interaction geometry of a sequence of THz pulses with the sample. The nonlinear polarization is determined by a phase-resolved measurement of the electric field transmitted through the sample as a function of the delay τ between two phase-locked pulses and the "real" time t. The information provided by a single 2D scan along the τ and t axes is equivalent to that from a noncollinear photon-echo setup equipped with four local oscillators, each interacting with a different diffracted order. We address basic concepts of collinear 2D THz spectroscopy, in particular data analysis and phasing issues. Different rephasing and nonrephasing contributions to the third-order response are separated and 2D correlation spectra derived. As a prototype application, 2D correlation spectra of intersubband excitations of electrons in semiconductor quantum wells are presented.

High-field transport in an electron-hole plasma: transition from ballistic to drift motion.

The time evolution of high-field carrier transport in bulk GaAs is studied with intense femtosecond THz pulses. While ballistic transport of electrons occurs in an n-type sample, a transition from ballistic to driftlike motion is observed in an electron-hole plasma. This onset of friction is due to the holes, which are heated by THz absorption. Theoretical calculations, which reproduce the data quantitatively, show that both electron-hole scattering and local-field effects in the electron-hole plasma are essential for the time-dependent friction.

Ultrafast spatiotemporal dynamics of terahertz generation by ionizing two-color femtosecond pulses in gases.

We present a combined theoretical and experimental study of spatiotemporal propagation effects in terahertz (THz) generation in gases using two-color ionizing laser pulses. The observed strong broadening of the THz spectra with increasing gas pressure reveals the prominent role of spatiotemporal reshaping and of a plasma-induced blueshift of the pump pulses in the generation process. Results obtained from (3+1)-dimensional simulations are in good agreement with experimental findings and clarify the mechanisms responsible for THz emission.

Coherent ballistic motion of electrons in a periodic potential.

Electrons in bulk n-doped GaAs at a lattice temperature of 300 K are driven by ultrashort high-field transients of up to 300 kV/cm in the terahertz frequency range. In the lowest conduction band the carriers show coherent ballistic motion, which is detected via the THz field emitted by them. This partial Bloch oscillation is reproduced by a quantum-kinetic theory of coherent transport on ultrafast time scales.

Femtosecond powder diffraction with a laser-driven hard X-ray source.

X-ray powder diffraction with a femtosecond time resolution is introduced to map ultrafast structural dynamics of polycrystalline condensed matter. Our pump-probe approach is based on photoexcitation of a powder sample with a femtosecond optical pulse and probing changes of its structure by diffracting a hard X-ray pulse generated in a laser-driven plasma source. We discuss the key aspects of this scheme including an analysis of detection sensitivity and angular resolution. Applying this technique to the prototype molecular material ammonium sulfate, up to 20 powder diffraction rings are recorded simultaneously with a time resolution of 100 fs. We describe how to derive transient charge density maps of the material from the extensive set of diffraction data in a quantitative way.

Phase-resolved two-dimensional spectroscopy based on collinear n-wave mixing in the ultrafast time domain.

We present a novel approach for femtosecond two-dimensional (2D) spectroscopy in the midinfrared combining a collinear beam geometry and phase-resolved detection. Two phase-locked pulses of variable time delay tau interact with the sample. The transmitted electric fields are measured in real time t by electro-optic sampling. 2D spectra are generated by Fourier transforming the signal along the two time axes tau and t. In the 2D spectra, nonlinear signals originating from different orders n in the electric field are separated. Such decomposition of the overall response is demonstrated by mapping the nonlinear response of intersubband transitions in GaAs/AlGaAs multiple quantum wells.

Internal motions of a quasiparticle governing its ultrafast nonlinear response.

A charged particle modifies the structure of the surrounding medium: examples include a proton in ice, an ion in a DNA molecule, an electron at an interface, or an electron in an organic or inorganic crystal. In turn, the medium acts back on the particle. In a polar or ionic solid, a free electron distorts the crystal lattice, displacing the atoms from their equilibrium positions. The electron, when considered together with its surrounding lattice distortion, is a single quasiparticle, known as the Fröhlich polaron. The basic properties of polarons and their drift motion in a weak electric field are well known. However, their nonlinear high-field properties--relevant for transport on nanometre length and ultrashort timescales--are not understood. Here we show that a high electric field in the terahertz range drives the polaron in a GaAs crystal into a highly nonlinear regime where, in addition to the drift motion, the electron is impulsively moved away from the centre of the surrounding lattice distortion. In this way, coherent lattice vibrations (phonons) and concomitant drift velocity oscillations are induced that persist for several hundred femtoseconds. They modulate the optical response at infrared frequencies between absorption and stimulated emission. Such quantum coherent processes directly affect high-frequency transport in nanostructures and may be exploited in novel terahertz-driven optical modulators and switches.

Ultrafast changes of molecular crystal structure induced by dipole solvation.

Femtosecond photoexcitation of organic chromophores in a molecular crystal induces strong changes of the electronic dipole moment via intramolecular charge transfer as is evident from transient vibrational spectra. The structural response of the crystal to the dipole change is mapped directly for the first time by ultrafast x-ray diffraction or diffuse scattering. Changes of diffracted and transmitted x-ray intensity demonstrate an angular rearrangement of molecules around excited dipoles following the 10 ps kinetics of charge transfer and leaving lattice plane spacings unchanged. Transient x-ray scattering is governed by solvation, masking changes of the chromophore molecular structure.

Coupled ultrafast lattice and polarization dynamics in ferroelectric nanolayers.

We report the first analysis of the polarization and lattice dynamics in a metal/ferroelectric/metal nanolayer system by femtosecond x-ray diffraction. Two Bragg reflections provide information on the coupled dynamics of the two relevant phonon modes for ferroelectricity in perovskites, the tetragonal distortion and the soft mode. Optical excitation of the SrRuO(3) metal layers generates giant stress (>1 GPa) compressing the PbZr(0.2)Ti(0.8)O(3) layers by up to 2%. The resulting change of tetragonality reaches a maximum after 1.3 ps. As a result, the ferroelectric polarization P is reduced by up to 100% with a slight delay that is due to the anharmonic coupling of the two modes.

Nonlinear terahertz response of -type GaAs.

Excitation of an n-type GaAs layer by intense ultrashort terahertz pulses causes coherent emission at 2 THz. Phase-resolved nonlinear propagation experiments show a picosecond decay of the emitted field, despite the ultrafast carrier-carrier scattering at a sample temperature of 300 K. While the linear THz response is in agreement with the Drude response of free electrons, the nonlinear response is dominated by the super-radiant decay of optically inverted impurity transitions. A quantum mechanical discrete state model using the potential of the disordered impurities accounts for all experimental observations.

Recent progress in ultrafast X-ray diffraction.

X-ray diffraction with femtosecond time-resolution represents a direct probe of ultrafast structural changes in condensed matter. The generation of ultrashort X-ray pulses in laser-driven plasma and/or accelerator-based sources has made substantial progress, and has allowed for studies of transient structures with an unprecedented accuracy. Herein, recent work on transient crystalline structures is reviewed, with the focus on laser-based experiments.

Generation of single-cycle THz transients with high electric-field amplitudes.

Single-cycle terahertz (THz) transients in the frequency range 0.3-7 THz with electric-field amplitudes of more than 400 kV/cm are generated by four-wave mixing of the fundamental and the second harmonic of 25 fs pulses from a Ti:sapphire amplifier in ionized air. These transients are fully characterized by electro-optic sampling with ZnTe and GaP crystals. One can tune the center frequency of the THz transients by varying the length of the incident pulse. The electric-field amplitude increases linearly with the incident pulse energy.