Projects

Many properties of solids result from the fact that in a periodic crystal structure, electronic wave functions are delocalized over many lattice sites. Electrons should become increasingly localized when a strong electric field is applied. So far, this Wannier-Stark regime has been reached only in artificial superlattices. Here we show that extremely transient bias over the few-femtosecond period of phase-stable mid-infrared pulses may localize electrons even in a bulk semiconductor like GaAs. The complicated band structure of a three-dimensional crystal leads to a strong blurring of field-dependent steps in the Wannier-Stark ladder. Only the central step emerges strongly in interband electro-absorption because its energetic position is dictated by the electronic structure at an atomic level and therefore insensitive to the external bias. In this way, we demonstrate an extreme state of matter with potential applications due to e.g., its giant optical non-linearity or extremely high chemical reactivity.

We have investigated in detail the continuous-wave (cw) and mode-locked performance of a diode-pumped Cr:Nd:GSGG laser. State-of-the-art single-mode and multimode laser diodes around 665 nm were used as pump sources. In cw operation, we have demonstrated lasing thresholds as low as 14 mW, slope efficiencies as high as 23.4%, and output powers up to 738 mW. The free running emission wavelength was 1061 nm. Lasing could also be obtained at 1051, 1058, 1065, 1068, 1072, 1103, and 1111 nm lines. A saturable Bragg reflector was used to initiate and sustain mode-locking where the Cr:Nd:GSGG laser produced 6-ps-long pulses around 1061 nm with an average power of 160 mW. The repetition rate was 142.65 MHz, resulting in pulse energies of 1.1 nJ and peak powers of 175 W. An off-surface optical axis quartz birefringent filter (BRF) was inserted inside the laser cavity at Brewster’s angle to obtain two-color cw and mode-locked laser operation at the 1051 and 1058 nm and 1058 and 1061 transition pairs, resulting in cw powers up to 60 mW and cw mode-locked average powers up to 45 mW. Unlike many other methods applied for two-color mode-locked laser operation, usage of the BRF enabled regulation of the ratio of the power in each line by fine adjustment of its rotation angle. The method could potentially be used for other gain media as well, which could simplify development of multicolor solid-state laser systems.

Ultrabroadband electro-optic sampling is presented as an extremely sensitive technique to detect electric field amplitudes in free space. The temporal resolution provided by few-femtosecond laser pulses results in a bandwidth exceeding 100 THz, potentially covering the entire infrared spectral range. A pedagogic introduction to the operational principle of the method is given along the lines of a classical coherent input field and a zincblende-type electro-optic sensor. We then show that even the bare vacuum fluctuations of the electric field in the quantum ground state may be detected. This time-domain approach to quantum physics operates directly on sub-cycle scales where no local energy conservation holds. Therefore, signals may be obtained from purely virtual photons without amplification to finite intensity.

Recent demonstrations of passively phase-locked fiber-based combs motivate broadband characterization of the noise associated with the stabilized carrier-envelope offset frequency. In our study, we analyze the phase noise of a 100 MHz Er:fiber system in a wide range spanning from microhertz to the Nyquist frequency. An interferometric detection method enables analysis of the high-frequency output of an f-to-2f interferometer. The dominant contribution of a broadband white noise floor at high frequencies attests quantum-limited performance. An out-of-loop measurement of the carrier-envelope phase reveals its jitter to be as low as 250 mrad when integrated over 12 orders of magnitude of the radio-frequency spectrum.

dc.title:

dc.title:

We study the ac charge and -spin transport through an orbital of a magnetic molecule with spin precessing in a constant magnetic field. We assume that the source and drain contacts have time-dependent chemical potentials. We employ the Keldysh nonequilibrium Green’s functions method to calculate the spin and charge currents to linear order in the time-dependent potentials. The molecular and electronic spins are coupled via exchange interaction. The time-dependent molecular spin drives inelastic transitions between the molecular quasienergy levels, resulting in a rich structure in the transport characteristics. The time-dependent voltages allow us to reveal the internal precession time scale (the Larmor frequency) by a dc conductance measurement if the ac frequency matches the Larmor frequency. In the low-ac-frequency limit the junction resembles a classical electric circuit. Furthermore, we show that the setup can be used to generate dc-spin currents, which are controlled by the molecular magnetization direction and the relative phases between the Larmor precession and the ac voltage.

We demonstrate synthesis of ultrabroadband and phase-locked two-color transients in the multi-terahertz frequency range with amplitudes exceeding 13 MV cm⁻¹. Subcycle polar asymmetry of the electric field is adjusted by changing the relative phase between superposed fundamental and second harmonic components. The resultant broken symmetry of the field profile is directly resolved via electro-optic sampling. Access to such waveforms provides a direct route for control of low-energy degrees of freedom in condensed matter as well as non-perturbative light–matter interactions under highest non-resonant electric bias.

A combination of Er/Yb:fiber and Yb:thin-disk technology produces 615 fs pulses at 1030 nm with an average output power of 72 W. The regenerative amplifier allows variation of the repetition rate between 3 and 5 kHz with pulse energies from 13 to 17 mJ. A broadband and intense seed provided by the compact and versatile fiber front-end minimizes gain narrowing. The resulting sub-ps performance is ideal for nonlinear frequency conversion and pulse compression. Operating in the upper branch of a bifurcated pulse train, the system exhibits exceptional noise performance and stability.

The ground state of quantum systems is characterized by zero-point motion. Those vacuum fluctuations are generally deemed an elusive phenomenon that manifests itself only indirectly. Here, we report direct detection of the vacuum fluctuations of electromagnetic radiation in free space. The ground-state electric field variance is found to be inversely proportional to the four-dimensional space-time volume sampled electro-optically with tightly focused few-femtosecond laser pulses. Sub-cycle temporal readout and nonlinear coupling far from resonance provide signals from purely virtual photons without amplification. Our findings enable an extreme time-domain approach to quantum physics with nondestructive access to the quantum state of light. Operating at multi-terahertz frequencies, such techniques might also allow time-resolved studies of intrinsic fluctuations of elementary excitations in condensed matter.

Noncollinear parametric amplification based on type-II phase matching for the generation of ultrabroadband and tunable spectra in the near infrared is investigated. In a noncollinear geometry the group velocity matching condition between signal and idler can be obtained in frequently used crystals such as β-barium borate (BBO) even for wavelengths fully located in the anomalous dispersion region. The extremely broadband operation, peculiar tuning possibilities and straightforward experimental implementation with the standard BBO crystal pave the way for a versatile NIR source in ultrafast spectroscopy.

We directly trace the near- and midinfrared transmission change of a VO₂ thin film during an ultrafast insulator-to-metal transition triggered by high-field multiterahertz transients. Nonthermal switching into a metastable metallic state is governed solely by the amplitude of the applied terahertz field. In contrast to resonant excitation below the threshold fluence, no signatures of excitonic self-trapping are observed. Our findings are consistent with the generation of spatially separated charge pairs and a cooperative transition into a delocalized metallic state by THz field-induced tunneling. The tunneling process is a condensed-matter analog of the Schwinger effect in nonlinear quantum electrodynamics. We find good agreement with the pair production formula by replacing the Compton wavelength with an electronic correlation length of 2.1 Å.

A high-power femtosecond Yb:fiber amplifier operating with exceptional noise performance and long-term stability is demonstrated. It generates a 10-MHz train of 145-fs pulses at 1.03 μm with peak powers above 36 MW. The system features a relative amplitude noise of 1.5⋅10⁻⁶  Hz^−1/2 at 1 MHz and drifts of the 60-W average power below 0.3% over 72 hours of continuous operation. The passively phase-stable Er:fiber seed system provides ultrabroadband pulses that are synchronized at a repetition rate of 40 MHz. This combination aims at new schemes for sensitive experiments in ultrafast scientific applications.

Direct detection of vacuum fluctuations and analysis of subcycle quantum properties of the electric field are explored by a paraxial quantum theory of ultrafast electro-optic sampling. The feasibility of such experiments is demonstrated by realistic calculations adopting a thin ZnTe electro-optic crystal and stable few-femtosecond laser pulses. We show that nonlinear mixing of a short near-infrared probe pulse with the multiterahertz vacuum field leads to an increase of the signal variance with respect to the shot noise level. The vacuum contribution increases significantly for appropriate length of the nonlinear crystal, short pulse duration, tight focusing, and a sufficiently large number of photons per probe pulse. If the vacuum input is squeezed, the signal variance depends on the probe delay. Temporal positions with a noise level below the pure vacuum may be traced with subcycle resolution.

We present a detailed investigation of Kerr-lens mode-locking in diode-pumped Cr:LiSAF lasers employing gain-matched output couplers (GMOCs). Single-mode diodes (660 nm, 130 mW) and tapered diodes (685 nm, 1 W) were investigated as diode pump sources. We have shown that, by reducing the gain-filtering effect, GMOC enhances the effective self-amplitude modulation depth and provides a significant improvement in both efficiency and robustness of KLM operation. From the single-mode diode pumped system, 13 fs pulses with an average power of 25 mW and a peak power 25 kW have been generated at an incident pump power of only 120 mW (21% optical-to-optical conversion efficiency). The tapered diode pumped Cr:LiSAF oscillator provided pulses as short as 14.5 fs with 106-mW average power and 60-kW peak power at an incident pump power of 940 mW (11% optical-to-optical conversion efficiency). A femtosecond tuning range extending from 807 to 919 nm was also realized with sub-50-fs long pulses. To our knowledge, demonstrated optical-to-optical conversion efficiencies, peak powers and fs tuning ranges are record results for Cr:LiSAF laser oscillators. The obtainable pulsewidth and fs tuning range are currently limited by the dispersion/reflectivity bandwidth of the available optics.

We investigate the optoelectronic properties of the semiconducting (6,5) species of single-walled carbon nanotubes by measuring ultrafast transient transmission changes with 20 fs time resolution. We demonstrate that photons with energy below the lowest exciton resonance efficiently lead to linear excitation of electronic states. This finding challenges the established picture of a vanishing optical absorption below the fundamental excitonic resonance. Our result points towards below-gap electronic states as an intrinsic property of semiconducting nanotubes.

Optical frequency combs based on erbium-doped fiber lasers are attractive tools in precision metrology due to their inherent compactness and stability. Here we study a femtosecond Er:fiber comb that passively eliminates the carrier–envelope phase slip by difference frequency generation. Quantum statistics inside the all-fiber soliton oscillator governs its free-running performance. Active stabilization of the repetition rate supports a subhertz optical linewidth and does not necessitate additional intracavity elements. Direct locking to an optical atomic frequency standard enables generation of a 100 MHz microwave signal with a stability of 3.4 mHz maintained over 15 min.

The recent discovery of the Higgs boson has created a lot of excitement among scientists. Celebrated as one of the most fundamental results in experimental physics (1), the observation of this particle confirms the existence of the associated Higgs field that plays a pivotal role in the Standard Model of particle physics. Because of the Higgs boson's large mass (about 125 GeV), it could be detected only in the world's largest and most powerful accelerator—the Large Hadron Collider at CERN, Geneva. Although it sounds strange, the theoretical proposal of the Higgs mechanism was actually inspired by ideas from condensed matter physics, which typically works at much lower energies (a few electron volts or less). In 1958, Anderson discussed the appearance of a coherent excited state in superconducting condensates with spontaneously broken symmetry (2). Later, this approach was advanced by Nambu (3). The existence of superconducting condensates has been firmly established. In contrast, unambiguous experimental evidence for the coherent excited state (called the Higgs mode) had been missing. On page 1145 of this issue, Matsunaga et al. (4) report direct observation of the Higgs mode in the conventional superconductor niobium nitride (NbN) excited by intense electric field transients.

We demonstrate sub-cycle manipulation of mid-infrared optical waveforms in the time domain. This goal is accomplished via efficient reflection at a semiconductor surface induced by femtosecond interband excitation. The ultrafast response of this process allows slicing of high-field multi-terahertz transients down to the single optical cycle. Ultrabroadband and phase-stable transients with peak amplitudes beyond 10 MVcm-1 are obtained, paving the way for efficient coherent control of light–matter interaction in the non-perturbative regime. The microscopic analysis of electron–hole plasma generation in germanium reveals a decisive role of two-photon absorption allowing efficient slicing up to midinfrared frequencies.

The state of the art of ultrafast Er:fiber technology is reviewed. Such lasers are increasingly used for generation of ultrabroadband and widely tunable pulse trains. Er:fiber sources prove to be flexible, compact and robust with important applications in fundamental and interdisciplinary sciences. After a short overview of different oscillator and amplifier designs the discussion focuses on coherent and tailored supercontinuum generation in highly nonlinear germanosilicate fibers. This approach enables a tuning range spanning from the visible to the mid infrared, synthesis of single-cycle light pulses and passive locking of the carrier-envelope phase.

Resulting from the availability of improved sources, research in the terahertz (THz) spectral range has increased dramatically over the last decade, leading essentially to the disappearance of the so-called 'THz gap'. While most work to date has been carried out with THz radiation of low field amplitude, a growing number of experiments are using THz radiation with large electric and magnetic fields that induce nonlinearities in the system under study. This 'focus on' collection contains a number of articles, both experimental and theoretical, in the new subfield of THz nonlinear optics and spectroscopy on various systems, among them molecular gases, superconductors, semiconductors, antiferromagnets and graphene.

We study time-dependent electronic and spin transport through an electronic level connected to two leads and coupled with a single-molecule magnet via exchange interaction. The molecular spin is treated as a classical variable and precesses around an external magnetic field. We derive expressions for charge and spin currents by means of the Keldysh nonequilibrium Green’s functions technique in linear order with respect to the time-dependent magnetic field created by this precession. The coupling between the electronic spins and the magnetization dynamics of the molecule creates inelastic tunneling processes which contribute to the spin currents. The inelastic spin currents, in turn, generate a spin-transfer torque acting on the molecular spin. This back-action includes a contribution to the Gilbert damping and a modification of the precession frequency. The Gilbert damping coefficient can be controlled by the bias and gate voltages or via the external magnetic field and has a nonmonotonic dependence on the tunneling rates.

We present recent advances in the generation of highly intense multiterahertz transients and their application to nonlinear spectroscopy of bulk semiconductors. An optimized scheme of parametric amplification results in broadband single- or few-cycle terahertz transients with peak electric fields up to 10 or 25 MV/cm, respectively. Time-resolved four-wave mixing terahertz spectroscopy of InSb far away from the interband resonance demonstrates clear signatures of a nonperturbative regime of Rabi flopping. We qualitatively explain the observed behavior within a model of a quantum two-level system. In addition, we demonstrate the dynamical Franz-Keldysh effect in InP resolved on a subcycle timescale. The field-induced modulation of the interband optical absorption at the second harmonic of the driving terahertz field is observed in full agreement with theoretical predictions.

We demonstrate the generation of 22.6 μJ of combined energy at 3 μm for sub-300fs pulses at a repetition rate of 1 kHz using a LGSe optical parametric amplifier (OPA). The LGSe OPA is pumped by the 140-fs 1.6 μm pulses from a 300-mW KTA optical parametric chirped pulse amplifier (OPCPA) based on an all-optical synchronization scheme. By using a highly-nonlinear fiber, the output of an erbium-doped fiber laser operating at 1560 nm is shifted to 1050 nm in order to coherently seed a Nd:YLF regenerative amplifier. The LGSe OPA is seeded using the MIR coming from the amplification of the 1.6 μm in the OPCPA.

The interplay among charge, spin and lattice degrees of freedom in solids gives rise to intriguing macroscopic quantum phenomena such as colossal magnetoresistance, multiferroicity and high-temperature superconductivity. Strong coupling or competition between various orders in these systems presents the key to manipulate their functional properties by means of external perturbations such as electric and magnetic fields or pressure. Ultrashort and intense optical pulses have emerged as an interesting tool to investigate elementary dynamics and control material properties by melting an existing order. Here, we employ few-cycle multi-terahertz pulses to resonantly probe the evolution of the spin-density-wave (SDW) gap of the pnictide compound BaFe(2)As(2) following excitation with a femtosecond optical pulse. When starting in the low-temperature ground state, optical excitation results in a melting of the SDW order, followed by ultrafast recovery. In contrast, the SDW gap is induced when we excite the normal state above the transition temperature. Very surprisingly, the transient ordering quasi-adiabatically follows a coherent lattice oscillation at a frequency as high as 5.5 THz. Our results attest to a pronounced spin-phonon coupling in pnictides that supports rapid development of a macroscopic order on small vibrational displacement even without breaking the symmetry of the crystal.

dc.title:

dc.title:

dc.contributor.author: Schubert, Olaf