Observation of interplay between phonon chirality and electronic band topology.

The recently demonstrated chiral modes of lattice motion carry angular momentum and therefore directly couple to magnetic fields. Notably, their magnetic moments are predicted to be strongly influenced by electronic contributions. Here, we have studied the magnetic response of transverse optical phonons in a set of PbSnTe films, which is a topological crystalline insulator for > 0.

Ultrafast pump-probe spectroscopy via chirped-pulse up-conversion with dispersion compensation.

In this study, ultrafast transient signals were detected on a single-shot basis using chirped-pulse up-conversion spectroscopy with dispersion compensation. Unlike in the conventional time-encoding technique using chirped pulses, distortion of the ultrafast waveform was reduced by applying dispersion compensation to the chirped probe pulses and using sum-frequency generation with the chirped readout pulses. The method was applied to terahertz time-domain spectroscopy and near-infrared pump-probe spectroscopy, providing ultrafast observations with an improved temporal resolution comparable to the transform-limited pulse durations.

Pulse-to-pulse detection of terahertz radiation emitted from the femtosecond laser ablation process.

Determining the dynamics of electrons and ions emitted from a target material during laser ablation is crucial for desirable control of laser processing. However, these dynamics are still challenging to understand because of a lack of ubiquitous spectroscopic tools to observe tangled-up dynamics appearing at ultrafast timescales. Here by harnessing highly sensitive single-shot terahertz time-domain spectroscopy using an echelon mirror, we investigate pulse-to-pulse temporal profile of terahertz radiation generated from the material surface.

K-point longitudinal acoustic phonons are responsible for ultrafast intervalley scattering in monolayer MoSe.

In transition metal dichalcogenides, valley depolarization through intervalley carrier scattering by zone-edge phonons is often unavoidable. Although valley depolarization processes related to various acoustic phonons have been suggested, their optical verification is still vague due to nearly degenerate phonon frequencies on acoustic phonon branches at zone-edge momentums. Here we report an unambiguous phonon momentum determination of the longitudinal acoustic (LA) phonons at the K point, which are responsible for the ultrafast valley depolarization in monolayer MoSe.

Magnetic Control of Soft Chiral Phonons in PbTe.

PbTe crystals have a soft transverse optical phonon mode in the terahertz frequency range, which is known to efficiently decay into heat-carrying acoustic phonons, resulting in anomalously low thermal conductivity. Here, we studied this phonon via polarization-dependent terahertz spectroscopy. We observed softening of this mode with decreasing temperature, indicative of incipient ferroelectricity, which we explain through a model including strong anharmonicity with a quartic displacement term.

Ultrastrong magnon-magnon coupling dominated by antiresonant interactions.

Exotic quantum vacuum phenomena are predicted in cavity quantum electrodynamics systems with ultrastrong light-matter interactions. Their ground states are predicted to be vacuum squeezed states with suppressed quantum fluctuations owing to antiresonant terms in the Hamiltonian. However, such predictions have not been realized because antiresonant interactions are typically negligible compared to resonant interactions in light-matter systems.

High-throughput terahertz spectral line imaging using an echelon mirror.

This work demonstrates terahertz (THz) line imaging that acquires broadband spectral information by combining echelon-based single-shot THz spectroscopy with high-sensitivity phase-offset electrooptic detection. An approximately 40 dB signal-to-noise ratio is obtained for a THz spectrum from a single line of the camera, with a detection bandwidth up to 2 THz at the peak electric-field strength of 1.2 kV/cm.

Observation of Photoinduced Terahertz Gain in GaAs Quantum Wells: Evidence for Radiative Two-Exciton-to-Biexciton Scattering.

We have observed photoinduced negative optical conductivity, or gain, in the terahertz frequency range in a GaAs multiple-quantum-well structure in a strong perpendicular magnetic field at low temperatures. The gain is narrow band: it appears as a sharp peak (linewidth <0.45  meV) whose frequency shifts with applied magnetic field.

Spatially resolved spectral phase interferometry with an isolated attosecond pulse.

We demonstrate spatially resolved supercontinuum spectral phase interferometry with an isolated attosecond pulse (IAP). The measured spatial-spectral interferogram over the broadband region indicates a high degree of IAP coherence in both spatial and spectral domains. In addition, the spectral-delay interferogram shows periodic temporal oscillations over the full IAP continuous spectrum, which indicates high temporal coherence.

Macroscopic Ionic Flow in a Superionic Conductor Na^{+} β-Alumina Driven by Single-Cycle Terahertz Pulses.

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^{+} β-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.

Subcycle mid-infrared coherent transients at 4 MHz repetition rate applicable to light-wave-driven scanning tunneling microscopy.

We produce subcycle mid-infrared (MIR) pulses at a 4 MHz repetition rate via the optical rectification (OR) of sub-10 fs near-infrared pulses delivered by an optical parametric chirped pulse amplifier. The coherent MIR pulses generated in a GaSe crystal under an ultrabroadband phase-matching condition contain only 0.58-0.

Selective Reduction Mechanism of Graphene Oxide Driven by the Photon Mode the Thermal Mode.

A two-dimensional nanocarbon, graphene, has attracted substantial interest due to its excellent properties. The reduction of graphene oxide (GO) has been investigated for the mass production of graphene used in practical applications. Different reduction processes produce different properties in graphene, affecting the performance of the final materials or devices.

An echelon-based single shot optical and terahertz Kerr effect spectrometer.

We report on the design and performance of an echelon-based single shot visible/near-infrared spectrometer with adequate sensitivity to measure the nonlinear optical and terahertz Kerr effects in neat molecular liquids at room temperature. Useful molecular information spanning tens of picoseconds can be measured in just a few milliseconds, and the signal-to-noise performance scales favorably with respect to the standard stage scan technique. These results demonstrate the viability of stage-free nonlinear Kerr effect measurements and provide a route for improvements to the speed of future multidimensional Kerr effect studies.

High precision frequency measurement of terahertz waves using optical combs from a Mach-Zehnder-modulator-based flat comb generator.

Using a frequency-tunable optical comb generated from a Mach-Zehnder-modulator-based flat comb generator (MZ-FCG) and a nonlinear optical fiber, we demonstrated a frequency measurement of continuous terahertz wave sources with the frequency of 0.1 and 0.6 THz by an electro-optic sampling method.

Fast-frame single-shot pump-probe spectroscopy with chirped-fiber Bragg gratings.

To acquire single-shot pump-probe waveforms for each laser pulse at a high repetition rate and high signal-to-noise ratio, we combined the photonic time-stretch technique and time-encoding method using a chirped-fiber Bragg grating (CFBG) and a grating-pair pulse compressor. By changing the pre-chirping of the probe pulse, a variable time window of the pump-probe traces from 1.4 to 17 ps was demonstrated.

Simultaneous acquisition of complex transmittance and birefringence with two counter-rotating, circularly polarized THz pulses.

Here we demonstrate simultaneous measurements of the complex transmittance and birefringence using left- and right-handed circularly polarized terahertz (THz) pulses. We change the polarization of the THz pulses periodically by modulating the polarization of the pump pulses directed onto a ZnTe (111) crystal, and we convert linear to circular polarization using a broadband THz quarter-wave retarder. By integrating the alternating-emission system with the polarization-sensitive terahertz time-domain spectrometer, we are able to obtain the electric-field vector of the transmitted terahertz pulses for both the left- and right-handed circular polarizations.

Tailoring Single-Cycle Near Field in a Tunnel Junction with Carrier-Envelope Phase-Controlled Terahertz Electric Fields.

Light-field-driven processes occurring under conditions far beyond the diffraction limit of the light can be manipulated by harnessing spatiotemporally tunable near fields. A tailor-made carrier envelope phase in a tunnel junction formed between nanogap electrodes allows precisely controlled manipulation of these processes. In particular, the characterization and active control of near fields in a tunnel junction are essential for advancing elaborate manipulation of light-field-driven processes at the atomic-scale.

Multi-petahertz electron interference in Cr:AlO solid-state material.

Lightwave-field-induced ultrafast electric dipole oscillation is promising for realizing petahertz (10 Hz: PHz) signal processing in the future. In building the ultrahigh-clock-rate logic operation system, one of the major challenges will be petahertz electron manipulation accompanied with multiple frequencies. Here we study multi-petahertz interference with electronic dipole oscillations in alumina with chromium dopant (Cr:AlO).

Single-shot terahertz time-domain spectroscopy in pulsed high magnetic fields.

We have developed a single-shot terahertz time-domain spectrometer to perform optical-pump/terahertz-probe experiments in pulsed, high magnetic fields up to 30 T. The single-shot detection scheme for measuring a terahertz waveform incorporates a reflective echelon to create time-delayed beamlets across the intensity profile of the optical gate beam before it spatially and temporally overlaps with the terahertz radiation in a ZnTe detection crystal. After imaging the gate beam onto a camera, we can retrieve the terahertz time-domain waveform by analyzing the resulting image.

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.

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 β = 0.

Ultrafast time-resolved electron diffraction revealing the nonthermal dynamics of near-UV photoexcitation-induced amorphization in Ge2Sb2Te5.

Because of their robust switching capability, chalcogenide glass materials have been used for a wide range of applications, including optical storages devices. These phase transitions are achieved by laser irradiation via thermal processes. Recent studies have suggested the potential of nonthermal phase transitions in the chalcogenide glass material Ge2Sb2Te5 triggered by ultrashort optical pulses; however, a detailed understanding of the amorphization and damage mechanisms governed by nonthermal processes is still lacking.

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.

Single-shot time-frequency imaging spectroscopy using an echelon mirror.

We demonstrate single-shot time-frequency imaging spectroscopy with an echelon mirror for measuring ultrashort laser pulses as well as ultrafast responses of materials using the same optical setup. The echelon mirror produces a spatially encoded time delay for the probe pulse whereby both the probe and pump pulses are focused on samples with small spot size. Using the optical Kerr gate apparatus, we successfully mapped the time-frequency images of ultrashort laser pulses and subsequently evaluated the chirp characteristics with the phase-retrieval procedure on a single-shot basis.

Ultrafast dynamics of surface-enhanced Raman scattering due to Au nanostructures.

Ultrafast dynamics of surface-enhanced Raman scattering (SERS) was investigated at cleaved graphite surfaces bearing deposited gold (Au) nanostructures (∼10 nm in diameter) by using sensitive pump-probe reflectivity spectroscopy with ultrashort (7.5 fs) laser pulses. We observed enhancement of phonon amplitudes (C═C stretching modes) in the femtosecond time domain, considered to be due to the enhanced electromagnetic (EM) field around the Au nanostructures.