Peter Gaal

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.

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.

Localized excited charge carriers generate ultrafast inhomogeneous strain in the multiferroic BiFeO3.

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.

Normalization schemes for ultrafast x-ray diffraction using a table-top laser-driven plasma source

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.

Ultrafast phase-resolved pump-probe measurements on a quantum cascade laser

The dynamics of optical gain in an InGaAs/AlInAs quantum cascade laser is studied in midinfrared pump-probe measurements. Pump and probe pulses of identical wavelength, polarization, and propagation direction through the laser waveguide are detected separately by electro-optic sampling. For injection currents below the lasing threshold, we observe an absorption decrease in the laser transition with a ≈3 ps recovery time. Above threshold, the gain strongly saturates and shows a fast recovery time decreasing with current. Such kinetics is superimposed by oscillations with a frequency of 0.8 THz originating from coherent electron tunneling through the injection barrier.

Synchrotron-based ultrafast x-ray diffraction at high repetition rates

We present a setup for ultrafast x-ray diffraction (UXRD) based at the storage ring BESSY II, in particular, a pump laser that excites the sample using 250 fs laser-pulses at repetition rates ranging from 208 kHz to 1.25 MHz. We discuss issues connected to the high heat-load and spatio-temporal alignment strategies in the context of a UXRD experiment at high repetition rates. The spatial overlap between laser pump and x-ray probe pulse is obtained with 10 μm precision and transient lattice changes can be recorded with an accuracy of δa/a(0) = 10(-6). We also compare time-resolved x-ray diffraction signals from a laser excited LSMO/STO superlattice with phonon dynamics simulations. From the analysis we determine the x-ray pulse duration to 120 ps in standard operation mode and below 10 ps in low-α mode.

Nanoscale heat transport studied by high-resolution time-resolved x-ray diffraction

We report on synchrotron-based high-repetition rate ultrafast x-ray diffraction (UXRD) experiments monitoring the transport of heat from an epitaxial La0.7Sr0.3MnO3/SrTiO3 superlattice (SL) into the substrate on timescales from 100ps to 4µs. Transient thermal lattice expansion was determined with an accuracy of 10 7 , corresponding to a sensitivity to temperature changes down to 0.01K. We follow the heat flow within the SL and into the substrate after the impulsive laser heating leads to a small temperature rise of 1T = 6K. 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 SrRuO3 for more than 200ps. The disagreement could be resolved by assuming that the heat conductivity changes in the first hundred picoseconds.

Following strain-induced mosaicity changes of ferroelectric thin films by ultrafast reciprocal space mapping.

We investigate coherent phonon propagation in a thin film of ferroelectric PbZr(0.2)Ti(0.8)O(3) (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.

Detecting optically synthesized quasi-monochromatic sub-terahertz phonon wavepackets by ultrafast x-ray diffraction

We excite an epitaxial SrRuO3 thin film transducer by a pulse train of ultrashort laser pulses, launching coherent sound waves into the underlying SrTiO3 substrate. Synchrotron-based x-ray diffraction (XRD) data exhibiting separated sidebands to the substrate peak evidence the excitation of a quasi-monochromatic phonon wavepacket with sub-THz central frequency. The frequency and bandwidth of this sound pulse can be controlled by the optical pulse train. We compare the experimental data to combined lattice dynamics and dynamical XRD simulations to verify the coherent phonon dynamics. In addition, we observe a lifetime of 130 ps of such sub-THz phonons in accordance with the theory.

Direct time-domain sampling of subterahertz coherent acoustic phonon spectra in SrTiO3 using ultrafast x-ray diffraction

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 Akhiezers 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.