Optical Rectification and Electro-Optic Sampling in Quartz

We report electro-optic sampling (EOS) response and terahertz (THz) optical rectification (OR) in z-cut alpha-quartz. Due to its small effective second-order nonlinearity, echo-free waveform of intense THz pulses with a few MV/cm electric-field strength can be measured faithfully with no saturation effect. Both its OR and EOS responses are broad with extension up to ~8 THz. Strikingly, the latter responses are independent of the crystal thickness, a plausible indication of strong surface contribution to the total second-order nonlinear susceptibility of quartz. Our study introduces thin quartz plates as the reliable THz electro-optic medium for echo-free, high field THz detection

Energy transfer within the hydrogen bonding network of water following resonant terahertz excitation

Energy dissipation in water is very fast and more efficient than in many other liquids. This behavior is commonly attributed to the intermolecular interactions associated with hydrogen bonding. Here, we investigate the dynamic energy flow in the hydrogen bond network of liquid water by a pump-probe experiment. We resonantly excite intermolecular degrees of freedom with ultrashort single-cycle terahertz pulses and monitor its Raman response. By using ultrathin sample cell windows, a background-free bipolar signal whose tail relaxes monoexponentially is obtained. The relaxation is attributed to the molecular translational motions, using complementary experiments, force field, and ab initio molecular dynamics simulations. They reveal an initial coupling of the terahertz electric field to the molecular rotational degrees of freedom whose energy is rapidly transferred, within the excitation pulse duration, to the restricted translational motion of neighboring molecules. This rapid energy transfer may be rationalized by the strong anharmonicity of the intermolecular interactions

Optically Gated Terahertz-Field-Driven Switching of Antiferromagnetic CuMnAs

We show scalable and complete suppression of the recently reported terahertz-pulse-induced switching between different resistance states of antiferromagnetic CuMnAs thin films by ultrafast gating. The gating functionality is achieved by an optically generated transiently conductive parallel channel in the semiconducting substrate underneath the metallic layer. The photocarrier lifetime determines the timescale of the suppression. As we do not observe a direct impact of the optical pulse on the state of CuMnAs, all observed effects are primarily mediated by the substrate. The sample region of suppressed resistance switching is given by the optical spot size, thereby making our scheme potentially applicable for transient low-power masking of structured areas with feature sizes of about 200 nm and even smaller

Macroscopic conductivity of aqueous electrolyte solutions scales with ultrafast microscopic ion motions

Despite the widespread use of aqueous electrolytes as conductors, the molecular mechanism of ionic conductivity at moderate to high electrolyte concentrations remains largely unresolved. Using a combination of dielectric spectroscopy and molecular dynamics simulations, we show that the absorption of electrolytes at similar to 0.3 THz sensitively reports on the local environment of ions. The magnitude of these high-frequency ionic motions scales linearly with conductivity for a wide range of ions and concentrations. This scaling is rationalized within a harmonic oscillator model based on the potential of mean force extracted from simulations. Our results thus suggest that long-ranged ionic transport is intimately related to the local energy landscape and to the friction for short-ranged ion dynamics: a high macroscopic electrolyte conductivity is thereby shown to be related to large-amplitude motions at a molecular scale

Rotational coherence of encapsulated ortho and para water in fullerene-C60 revealed by time-domain terahertz spectroscopy

We resolve the real-time coherent rotational motion of isolated water molecules encapsulated in fullerene-C60 cages by time-domain terahertz (THz) spectroscopy. We employ single-cycle THz pulses to excite the low-frequency rotational motion of water and measure the subsequent coherent emission of electromagnetic waves by water molecules. At temperatures below ~100 K, C60 lattice vibrational damping is mitigated and the quantum dynamics of confined water are resolved with a markedly long rotational coherence, extended beyond 10 ps. The observed rotational transitions agree well with low-frequency rotational dynamics of single water molecules in the gas phase. However, some additional spectral features with their major contribution at ~2.26 THz are also observed which may indicate interaction between water rotation and the C60 lattice phonons. We also resolve the real-time change of the emission pattern of water after a sudden cooling to 4 K, signifying the conversion of ortho-water to para-water over the course of 10s hours. The observed long coherent rotational dynamics of isolated water molecules confined in C60 makes this system an attractive candidate for future quantum technology