Phonon-Induced Relocation of Valence Charge in Boron Nitride Observed by Ultrafast X-Ray Diffraction.

The impact of coherent phonon excitations on the valence charge distribution in cubic boron nitride is mapped by femtosecond x-ray powder diffraction. Zone-edge transverse acoustic (TA) two-phonon excitations generated by an impulsive Raman process induce a steplike increase of diffracted x-ray intensity. Charge density maps derived from transient diffraction patterns reveal a spatial transfer of valence charge from the interstitial region onto boron and nitrogen atoms. This transfer is modulated with a frequency of 250 GHz due to a coherent superposition of TA phonons related to the ^{10}B and ^{11}B isotopes. Nuclear and electronic degrees of freedom couple through many-body Coulomb interactions.

Sub-picosecond temporal resolution of anomalous Hall currents in GaAs.

The anomalous Hall (AH) and spin Hall effects are important tools for the generation, control, and detection of spin and spin-polarized currents in solids and, thus, hold promises for future spintronic applications. Despite tremendous work on these effects, their ultrafast dynamic response is still not well explored. Here, we induce ultrafast AH currents in a magnetically-biased semiconductor by optical femtosecond excitation at room temperature. The currents' dynamics are studied by detecting the simultaneously emitted THz radiation. We show that the temporal shape of the AH currents can be extracted by comparing its THz radiation to the THz radiation emitted from optically induced currents whose temporal shape is well known. We observe a complex temporal shape of the AH currents suggesting that different microscopic origins contribute to the current dynamics. This is further confirmed by photon energy dependent measurements revealing a current inversion at low optical excitation intensities. Our work is a first step towards full time resolution of AH and spin Hall currents and helps to better understand the underlying microscopic origins, being a prerequisite for ultrafast spintronic applications using such currents.

Detection of the Anomalous Velocity with Subpicosecond Time Resolution in Semiconductor Nanostructures.

We report on the time-resolved detection of the anomalous velocity, constituting charge carriers moving perpendicular to an electric driving field, in undoped GaAs quantum wells. For this we optically excite the quantum wells with circularly polarized femtosecond laser pulses, thereby creating a state which breaks time-inversion symmetry. We then employ a quasi-single-cycle terahertz pulse as an electric driving field to induce the anomalous velocity. The electromagnetic radiation emitted from the anomalous velocity is studied with a subpicosecond time resolution and reveals intriguing results. We are able to distinguish between intrinsic (linked to the Berry curvature) and extrinsic (linked to scattering) contributions to the anomalous velocity both originating from the valence band and observe local energy space dependence of the anomalous velocity. Our results thus constitute a significant step towards noninvasive probing of the anomalous velocity locally in the full energy-momentum space and enable the investigation of many popular physical effects such as the anomalous Hall effect and spin Hall effect on ultrafast time scales.

All-optically induced ultrafast photocurrents: beyond the instantaneous coherent response.

It is demonstrated that the noninstantaneous response of the optically induced coherent polarization tremendously influences the real-space shift of electronic charges in semiconductors. The possibility of coherently controlling this real-space shift with temporally nonoverlapping excitation pulses allows for the observation of a new type of shift current, which only exists for certain polarization-shaped excitation pulses and vanishes in the continuous-wave limit. In contrast to previously studied shift currents, the new current requires a phase mismatch between two orthogonal transition dipole moments and leads, within a nonlinear second-order description, to a tensor which is antisymmetric with respect to the order of the two exciting electric field amplitudes. These observations, which can even be made at room temperature and are expected to occur in a variety of semiconductor crystal classes, contribute to a better understanding of light-matter interaction involving degenerate bands. Thus, they are expected to prove important for future studies of coherent and nonlinear optical effects in semiconductors.

Coherent control of ultrafast shift currents in GaAs with chirped optical pulses.

We demonstrate the coherent control of ultrafast shift currents in GaAs with two orthogonally polarized linearly chirped laser pulses. By varying the chirp and phase delay between the pulses, we achieve the control of the shape of the shift current transients in a wide range from a monopolar shape to different bipolar shapes (alternating currents). Moreover, the terahertz emission patterns resulting from the ultrafast shift currents allow one to determine the sign of the chirp of the laser pulses.

Molecular structure-property correlations from optical nonlinearity and thermal-relaxation dynamics.

We apply ultrafast single beam Z-scan technique to measure saturation absorption coefficients and nonlinear-refraction coefficients of primary alcohols at 1560 nm. The nonlinear effects result from vibronic transitions and cubic nonlinear-refraction. To measure the pure total third-order nonlinear susceptibility, we removed thermal effects with a frequency optimized optical-chopper. Our measurements of thermal-relaxation dynamics of alcohols, from 1560 nm thermal lens pump and 780 nm probe experiments revealed faster and slower thermal-relaxation timescales, respectively, from conduction and convection. The faster timescale accurately predicts thermal-diffusivity, which decreases linearly with alcohol chain-lengths since thermal-relaxation is slower in heavier molecules. The relation between thermal-diffusivity and alcohol chain-length confirms structure-property relationship.