Macroscopic Ionic Flow in a Superionic Conductor Na

Ionic motion significantly contributes to conductivity in devices such as memory, switches, and rechargeable batteries. In our work, we experimentally demonstrate that intense terahertz electric-field transients can be used to manipulate ions in a superionic conductor, namely Na^{+} ß-alumina. The cations trapped in the local potential minima are accelerated using single-cycle terahertz pulses, thereby inducing a macroscopic current flow on a subpicosecond timescale. Our results clearly show that single-cycle terahertz pulses can be used to significantly modulate the nature of superionic conductors and could possibly serve as a basic tool for application in future electronic devices.

High-Acquisition-Rate Single-Shot Pump-Probe Measurements Using Time-Stretching Method.

Recent advances of ultrafast spectroscopy allow the capture of an entire ultrafast signal waveform in a single probe shot, which greatly reduces the measurement time and opens the door for the spectroscopy of unrepeatable phenomena. However, most single-shot detection schemes rely on two-dimensional detectors, which limit the repetition rate of the measurement and can hinder real-time visualization and manipulation of signal waveforms. Here, we demonstrate a new method to circumvent these difficulties and to greatly simplify the detection setup by using a long, single-mode optical fiber and a fast photodiode. Initially, a probe pulse is linearly chirped (the optical frequency varies linearly across the pulse in time), and the temporal profile of an ultrafast signal is then encoded in the probe spectrum. The probe pulse and encoded temporal dynamics are further chirped to nanosecond time scales using the dispersion in the optical fiber, thus, slowing down the ultrafast signal to time scales easily recorded with fast detectors and high-bandwidth electronics. We apply this method to three distinct ultrafast experiments: investigating the power dependence of the Kerr signal in LiNbO3, observing an irreversible transmission change of a phase change material, and capturing terahertz waveforms.

Terahertz-induced acceleration of massive Dirac electrons in semimetal bismuth.

Dirac-like electrons in solid state have been of great interest since they exhibit many peculiar physical behaviors analogous to relativistic mechanics. Among them, carriers in graphene and surface states of topological insulators are known to behave as massless Dirac fermions with a conical band structure in the two-dimensional momentum space, whereas electrons in semimetal bismuth (Bi) are expected to behave as massive Dirac-like fermions in the three-dimensional momentum space, whose dynamics is of particular interest in comparison with that of the massless Dirac fermions. Here, we demonstrate that an intense terahertz electric field transient accelerates the massive Dirac-like fermions in Bi from classical Newtonian to the relativistic regime; the electrons are accelerated approaching the effective "speed of light" with the "relativistic" beta ß = 0.89 along the asymptotic linear band structure. As a result, the effective electron mass is enhanced by a factor of 2.4.

Terahertz-field-induced nonlinear electron delocalization in Au nanostructures.

Improved control over the electromagnetic properties of metal nanostructures is indispensable for the development of next-generation integrated nanocircuits and plasmonic devices. The use of terahertz (THz)-field-induced nonlinearity is a promising approach to controlling local electromagnetic properties. Here, we demonstrate how intense THz electric fields can be used to modulate electron delocalization in percolated gold (Au) nanostructures on a picosecond time scale. We prepared both isolated and percolated Au nanostructures deposited on high resistivity Si(100) substrates. With increasing the applied THz electric fields, large opacity in the THz transmission spectra takes place in the percolated nanostructures; the maximum THz-field-induced transmittance difference, 50% more, is reached just above the percolation threshold thickness. Fitting the experimental data to a Drude-Smith model, we found furthermore that the localization parameter and the damping constant strongly depend on the applied THz-field strength. These results show that ultrafast nonlinear electron delocalization proceeds via strong electric field of THz pulses; the intense THz electric field modulates the backscattering rate of localized electrons and induces electron tunneling between Au nanostructures across the narrow insulating bridges without any material breakdown.

Terahertz time-domain observation of spin reorientation in orthoferrite ErFeO3 through magnetic free induction decay.

Terahertz time domain spectroscopy was performed on orthoferrite ErFeO3. Through the emission from the two magnetic resonance modes, we succeeded in observing the spin reorientation transition. Depending on the orientation of the single crystal, the reorientation can be detected as either mode switching between the two modes or polarization change of the emission. This method enables picosecond resolved observation of the reorientation without disturbances such as electronic excitation and heating, and it is expected to open the doorway to observe ultrafast reorientation with the terahertz pulse.

Experimental verification of femtosecond laser ablation schemes by time-resolved soft x-ray reflective imaging.

Pump and probe reflective imaging using a soft x-ray laser probe was applied to the observation of the early stage of femtosecond laser ablation process on platinum. In strongly excited area, drastic and fast reflectivity drop was observed. In moderately excited area, the decay of the reflectivity is slower than that in the strongly excited area, and the reflectivity reaches its minimum at t = 160 ps. In weakly excited area, laser-induced reflectivity change was not observed. In addition, the point where the reflectivity dip was observed at t = 10 ps and t = 40 ps, coincides with the position of the edge of reflectivity drop at t = 160 ps. These results give the critical information about the femtosecond laser ablation.

Single-shot picosecond interferometry with one-nanometer resolution for dynamical surface morphology using a soft X-ray laser.

Using highly coherent radiation at a wavelength of 13.9 nm from a Ag-plasma soft X-ray laser, we constructed a pump-and-probe interferometer based on a double Lloyd's mirror system. The spatial resolutions are evaluated with a test pattern, showing 1.8-mum lateral resolution, and 1-nm depth sensitivity. This instrument enables a single-shot observation of the surface morphology with a 7-ps time-resolution. We succeeded in observing a nanometer scale surface dilation of Pt films at the early stage of the ablation process initiated by a 70 fs near infrared pump pulse.

Ripplon on high viscosity liquid.

A ripplon is a thermally excited capillary wave propagating on liquid surface. Propagation of the ripplon reflects surface mechanical properties such as surface tension and viscoelasticity of the liquid. An optical beating ripplon spectroscopy technique developed by us was applied mainly to the observation of various surface phenomena on a lowly viscous liquid surface in the frequency range from 1 kHz to several 10 MHz. In this study, we carried out a light scattering observation of the highly damped ripplon on the surface of the viscous liquid. The spectral peak width of the damped ripplon was smaller for the higher viscosity and the optical beating technique could resolve such a structure. A strict description of the dynamic structure factor of the ripplon was employed to fit the experimental power spectrum of overdamped ripplon to viscosity up to 1000 cS.