Ultrafast Long-Distance Electron-Hole Plasma Expansion in GaAs Mediated by Stimulated Emission and Reabsorption of Photons.

Electron-hole plasma expansion with velocities exceeding c/50 and lasting over 10 ps at 300 K was evidenced by time-resolved terahertz spectroscopy. This regime, in which the carriers are driven over >30 µm is governed by stimulated emission due to low-energy electron-hole pair recombination and reabsorption of the emitted photons outside the plasma volume. At low temperatures a speed of c/10 was observed in the regime where the excitation pulse spectrally overlaps with emitted photons, leading to strong coherent light-matter interaction and optical soliton propagation effects.

Orientation and dynamics of water molecules in beryl.

Behavior of individual molecules of normal and heavy water in beryl single crystals was studied by 1H and 2H nuclear magnetic resonance spectroscopy. From temperature dependences of the spectra, we deduce that type-I water molecules embedded in the beryl voids are oriented quite differently from the view established in the literature: Different from the earlier assumptions, their H-H lines deviate by about 18° from the hexagonal axis. We suggest that this is due to the molecules attaching to the oxygen atoms forming the beryl structural voids by a hydrogen bond. Our analysis shows that the molecules perform two types of movement: (i) rapid librations around the axis of the hydrogen bond and (ii) less frequent orientational jumps among the 12 possible binding sites in the beryl voids. The frequencies of the librational motions are evaluated from a simple thermodynamic model, providing good quantitative agreement with the frequencies of librations from optical experiments reported earlier.

Unusual features of lattice dynamics in lawsonite near its phase transitions.

Lattice dynamics of a single crystal of lawsonite were studied over a broad range of frequencies (1 Hz to 20 THz) using impedance, THz time-domain and infrared spectroscopies. Based on polarized spectra of complex permittivity [Formula: see text] measured as a function of temperature between 10 K and 500 K, we analyzed the properties of the two known phase transitions-an antiferrodistortive one near [Formula: see text] and a ferroelectric one, occurring at [Formula: see text]. The former one is accompanied by a flat maximum in the THz-range permittivity [Formula: see text] near [Formula: see text], which is due to an overdamped polar excitation in the [Formula: see text] spectra reflecting the dynamics of water and hydroxyl groups. The strength of this mode decreases on cooling below [Formula: see text], and the mode vanishes below [Formula: see text] due to hydrogen ordering. At the pseudoproper ferroelectric phase transition, two independent anomalies in permittivity were observed. First, [Formula: see text] exhibits a peak at [Formula: see text] due to critical slowing down of a relaxation in the GHz range. Second, infrared and THz spectra revealed an optical phonon softening towards [Formula: see text] which causes a smaller but pronounced maximum in [Formula: see text]. Such anomaly, consisting in a soft mode polarized perpendicularly to the ferroelectric axis, is unusual in ferroelectrics.

Fingerprints of Critical Phenomena in a Quantum Paraelectric Ensemble of Nanoconfined Water Molecules.

We have studied the radio frequency dielectric response of a system consisting of separate polar water molecules periodically arranged in nanocages formed by the crystal lattice of the gemstone beryl. Below T = 20-30 K, quantum effects start to dominate the properties of the electric dipolar system as manifested by a crossover between the Curie-Weiss and the Barrett regimes in the temperature-dependent real dielectric permittivity ε'(T). When analyzing in detail the temperature evolution of the reciprocal permittivity (ε')-1 down to T ≈ 0.3 K and comparing it with the data obtained for conventional quantum paraelectrics, like SrTiO3, KTaO3, we discovered clear signatures of a quantum-critical behavior of the interacting water molecular dipoles: Between T = 6 and 14 K, the reciprocal permittivity follows a quadratic temperature dependence and displays a shallow minimum below 3 K. This is the first observation of "dielectric fingerprints" of quantum-critical phenomena in a paraelectric system of coupled point electric dipoles.

Assessing skin hydration status in haemodialysis patients using terahertz spectroscopy: a pilot/feasibility study.

Terahertz (THz) time-domain spectroscopy was used in vivo to measure the body reflectance with the aim of determining experimentally the influence of haemodialysis on the content of water in the human skin. For this purpose, an original methodology of determining the skin properties at THz frequencies from the reflectance was developed. A series of measurements were performed before and after dialysis with ten subjects. The results strongly indicate that the surface body hydration is not the main parameter determining the skin conductivity in the THz range.

Materials with on-demand refractive indices in the terahertz range.

We demonstrate the possibility to create materials with chosen refractive indices and a strong birefringence in the terahertz range by etching of patterns with appropriate filling factors in a dielectric substrate. We show that by using deep inductive plasma etching of silicon wafers, it is possible to achieve a birefringence as high as 1.2 in an 80 microm thick layer. The resulting stacks were used as building blocks for a photonic crystal displaying sharp defect mode peaks in transmittance.

Nonresonant ionization of oxygen molecules by femtosecond pulses: plasma dynamics studied by time-resolved terahertz spectroscopy.

We show that optical pump-terahertz probe spectroscopy is a direct experimental tool for exploring laser-induced ionization and plasma formation in gases. Plasma was produced in gaseous oxygen by focused amplified femtosecond pulses. The ionization mechanisms at 400- and 800-nm excitation wavelengths differ significantly being primarily of a multiphoton character in the former case and a strong-field process in the latter case. The generation of the plasma in the focal volume of the laser and its expansion on subnanosecond time scale is directly monitored through its density-dependent susceptibility. A Drude model used to evaluate the plasma densities and electron-scattering rates successfully captures the observations for a wide range of pump intensities. In addition, rotational fingerprints of molecular and ionic species were also observed in the spectra.

Study of terahertz radiation generated by optical rectification on thin gold films.

Emission of terahertz (THz) radiation as a result of optical rectification of intense femtosecond laser pulses on thin gold films has been studied by time-domain THz spectroscopy. The THz amplitude was measured as a function of film thickness and incidence angle. The experiments reveal that the emitted THz field is suppressed for a thickness below 100 nm, which gives evidence of the nonlocal character of the response. The variation of incidence angle allows us to estimate the components of susceptibility tensor chi2ijk. For thicker films and near grazing incidence, the emitted THz field attains a peak value of 4 kV/cm.

Optical rectification at metal surfaces.

The emission of freely propagating terahertz (THz) radiation coming from optical rectification at metallic surfaces has been detected and characterized for the first time to the authors' knowledge. The observed THz transients are induced through nonlinear electronic processes at gold and silver surfaces on intense pulsed optical photoexcitation and exhibit a peak electric field of as much as 200 V/cm. This finding opens a qualitatively new way to investigate nonlinear phenomena at metal surfaces and also can be exploited for the development of new THz emitters.

Optical pump-terahertz probe spectroscopy of dyes in solutions: probing the dynamics of liquid solvent or solid precipitate?

The optical pump-terahertz probe spectroscopy was used together with ab initio calculations and molecular dynamics simulations to investigate ultrafast dynamics following electronic excitation of Coumarin 153 and TBNC (2,11,20,29-tetra-tert-butyl-2,3-naphtalocyanine) dyes in polar solvents. By scanning the terahertz waveform for different pump-probe delays this experimental technique allows us to obtain two dimensional spectra directly reflecting the temporal response of the system. A distinct signal was obtained for TBNC in chloroform, 2-propanol, and n-butanol, while no signal was recorded for Coumarin 153 in either of these solvents. We explain the nonequilibrium signal detected in TBNC solutions by the presence of a solid, polycrystalline phase of the dye resulting from irradiating the solution by intense optical pulses.