Wolfgang Schweinberger

Controlling dielectrics with the electric field of light

The control of the electric and optical properties of semiconductors with microwave fields forms the basis of modern electronics, information processing and optical communications. The extension of such control to optical frequencies calls for wideband materials such as dielectrics, which require strong electric fields to alter their physical properties. Few-cycle laser pulses permit damage-free exposure of dielectrics to electric fields of several volts per ångström and significant modifications in their electronic system. Fields of such strength and temporal confinement can turn a dielectric from an insulating state to a conducting state within the optical period. However, to extend electric signal control and processing to light frequencies depends on the feasibility of reversing these effects approximately as fast as they can be induced. Here we study the underlying electron processes with sub-femtosecond solid-state spectroscopy, which reveals the feasibility of manipulating the electronic structure and electric polarizability of a dielectric reversibly with the electric field of light. We irradiate a dielectric (fused silica) with a waveform-controlled near-infrared few-cycle light field of several volts per angström and probe changes in extreme-ultraviolet absorptivity and near-infrared reflectivity on a timescale of approximately a hundred attoseconds to a few femtoseconds. The field-induced changes follow, in a highly nonlinear fashion, the turn-on and turn-off behaviour of the driving field, in agreement with the predictions of a quantum mechanical model. The ultrafast reversibility of the effects implies that the physical properties of a dielectric can be controlled with the electric field of light, offering the potential for petahertz-bandwidth signal manipulation.

Femtosecond x-ray pulse length characterization at the Linac Coherent Light Source free-electron laser

Two-color, single-shot time-of-flight electron spectroscopy of atomic neon was employed at the Linac Coherent Light Source (LCLS) to measure laser-assisted Auger decay in the x-ray regime. This x-ray-optical cross-correlation technique provides a straightforward, non-invasive and on-line means of determining the duration of femtosecond (>40?fs) x-ray pulses. In combination with a theoretical model of the process based on the soft-photon approximation, we were able to obtain the LCLS pulse duration and to extract a mean value of the temporal jitter between the optical pulses from a synchronized Ti-sapphire laser and x-ray pulses from the LCLS. We find that the experimentally determined values are systematically smaller than the length of the electron bunches. Nominal electron pulse durations of 175 and 75?fs, as provided by the LCLS control system, yield x-ray pulse shapes of 120?20?fs full-width at half-maximum (FWHM) and an upper limit of 40?20?fs FWHM, respectively. Simulations of the free-electron laser agree well with the experimental results.

Attosecond nonlinear polarization and light-matter energy transfer in solids

Electric-field-induced charge separation (polarization) is the most fundamental manifestation of the interaction of light with matter and a phenomenon of great technological relevance. Nonlinear optical polarization produces coherent radiation in spectral ranges inaccessible by lasers and constitutes the key to ultimate-speed signal manipulation. Terahertz techniques have provided experimental access to this important observable up to frequencies of several terahertz. Here we demonstrate that attosecond metrology extends the resolution to petahertz frequencies of visible light. Attosecond polarization spectroscopy allows measurement of the response of the electronic system of silica to strong (more than one volt per ångström) few-cycle optical (about 750 nanometres) fields. Our proof-of-concept study provides time-resolved insight into the attosecond nonlinear polarization and the light-matter energy transfer dynamics behind the optical Kerr effect and multi-photon absorption. Timing the nonlinear polarization relative to the driving laser electric field with sub-30-attosecond accuracy yields direct quantitative access to both the reversible and irreversible energy exchange between visible-infrared light and electrons. Quantitative determination of dissipation within a signal manipulation cycle of only a few femtoseconds duration (by measurement and ab initio calculation) reveals the feasibility of dielectric optical switching at clock rates above 100 terahertz. The observed sub-femtosecond rise of energy transfer from the field to the material (for a peak electric field strength exceeding 2.5 volts per ångström) in turn indicates the viability of petahertz-bandwidth metrology with a solid-state device.

Generation of sub-3 fs pulses in the deep ultraviolet

We demonstrate generation and measurement of intense deep-ultraviolet light pulses with a duration of approximately 2.8 fs (FWHM of the intensity envelope) and a wavelength distribution between 230 and 290 nm. They emerge via direct frequency upconversion of sub-4 fs laser pulses of a carrier wavelength of approximately 750 nm focused into an Ne-filled, quasi-static gas cell. Dispersion-free, third-order autocorrelation measurements provide access to their temporal intensity profile.

Waveform-controlled near-single-cycle milli-joule laser pulses generate sub-10 nm extreme ultraviolet continua.

We demonstrate the generation of waveform-controlled laser pulses with 1 mJ pulse energy and a full-width-half-maximum duration of ∼4  fs, therefore lasting less than two cycles of the electric field oscillating at their carrier frequency. The laser source is carrier-envelope-phase stabilized and used as the backbone of a kHz repetition rate source of high-harmonic continua with unprecedented flux at photon energies between 100 and 200 eV (corresponding to a wavelength range between 12-6 nm respectively). In combination we use these tools for the complete temporal characterization of the laser pulses via attosecond streaking spectroscopy.

Femtosecond profiling of shaped x-ray pulses

Arbitrary manipulation of the temporal and spectral properties of x-ray pulses at free-electron lasers would revolutionize many experimental applications. At the Linac Coherent Light Source at Stanford National Accelerator Laboratory, the momentum phase-space of the free-electron laser driving electron bunch can be tuned to emit a pair of x-ray pulses with independently variable photon energy and femtosecond delay. However, while accelerator parameters can easily be adjusted to tune the electron bunch phase-space, the final impact of these actuators on the x-ray pulse cannot be predicted with sufficient precision. Furthermore, shot-to-shot instabilities that distort the pulse shape unpredictably cannot be fully suppressed. Therefore, the ability to directly characterize the x-rays is essential to ensure precise and consistent control. In this work, we have generated x-ray pulse pairs via electron bunch shaping and characterized them on a single-shot basis with femtosecond resolution through time-resolved photoelectron streaking spectroscopy. This achievement completes an important step toward future x-ray pulse shaping techniques.

Attosecond nonlinear polarization and energy transfer in solids

Attosecond polarization spectroscopy is a new experimental technique resolving the nonlinear polarization and energy-transfer induced by visible few-cycle strong fields in solids. It reveals the intensity dependent response time of the system with attosecond resolution.