arXiv subjects

Koichiro Tanaka

Publications and source records attributed to Koichiro Tanaka.

At least 19 recordsLinked to original sources

arXiv2026

Prominent Dimensional Effects on High-order Harmonic Generation in Strongly Correlated Electron Systems

Dimensionality strongly affects elementary excitations in correlated quantum materials, yet its impact on extreme nonlinear optical responses remains largely unexplored. Here, we combine high-harmonic generation (HHG) experiments on quasi-one-dimensional SrCuO$_2$ and quasi-two-dimensional Pr$_2$CuO$_4$ with nonequilibrium simulations of Hubbard models. We find a pronounced dimensional contrast: SrCuO$_2$ exhibits a robust plateau-like high-harmonic spectrum with weak temperature dependence, whereas Pr$_2$CuO$_4$ shows a monotonic decrease in harmonic yield and strong thermal suppression, especially at higher harmonics. The simulations qualitatively reproduce these trends and identify dimensionality-dependent doublon--holon dephasing, governed by spin--charge coupling, as their microscopic origin. These results establish dimensionality and spin--charge coupling as key control parameters for extreme nonlinear optical responses in correlated insulators.

cond-mat.str-el↗

arXiv2026

Terahertz Synthetic FM Triplet for Distortion-Free Stabilization and Lamb-Dip Spectroscopy

We demonstrate a distortion-free terahertz frequency stabilization technique using a "synthetic FM triplet" to overcome modulation sideband interference associated with high-density spectral lines in molecular clocks. By applying this method to the rotational transitions of acetonitrile (CH$_3$CN), we successfully generated clean derivative waveforms free from inter-line interference, achieving a fractional frequency instability of $1 \times 10^{-9}$ at an averaging time of $1~\mathrm{s}$. Furthermore, we report the observation of Lamb-dips using this high-fidelity approach. Our results establish acetonitrile as a promising candidate for high-agility molecular clocks and provide a robust solution for precision spectroscopy of molecules with complex hyperfine structures.

physics.optics↗

arXiv2025

Lamb-dip spectroscopy of rotational levels with UTC-PD terahertz emitter

Pump-probe saturation spectroscopy in the sub-terahertz region was performed in the rotational transition (J, K) = (16, 0) <- (15, 0) for gas-phase acetonitrile molecules in the counter-propagating configuration. We observed Lamb-dips at much lower excitation powers than previously reported. The linewidth in the zero-pressure limit was 10 kHz, which was estimated from the intensity and pressure dependence. This corresponds to the transit-time broadening.

physics.optics↗

arXiv2023

Effect of incoherent electron-hole pairs on high harmonic generation in an atomically thin semiconductor

High harmonic generation (HHG) in solids reflects the underlying nonperturbative nonlinear dynamics of electrons in a strong light field and is a powerful tool for ultrafast spectroscopy of electronic structures. Photo-carrier doping allows us to understand the carrier dynamics and the correlations between the carriers in the HHG process. Here, we study the effect of incoherent electron-hole pairs on HHG in an atomically thin semiconductor. The experimentally observed response to photo-carrier doping is successfully reproduced in numerical simulations incorporating the photo-excited carrier distribution, excitonic Coulomb interaction and electron-electron scattering effects. The simulation results reveal that the presence of photo-carriers enhances the intraband current that contributes to high harmonics below the absorption edge. We also clarify that the excitation-induced dephasing process rather than the phase-space filling effect is the dominant mechanism reducing the higher order harmonics above the absorption edge. Our work provides a deeper understanding of high harmonic spectroscopy and the optimum conditions for generating extreme ultraviolet light from solids.

physics.optics↗

arXiv2023

Generation of third-harmonic spin oscillation from strong spin precession induced by terahertz magnetic near fields

The ability to drive a spin system to state far from the equilibrium is indispensable for investigating spin structures of antiferromagnets and their functional nonlinearities for spintronics. While optical methods have been considered for spin excitation, terahertz (THz) pulses appear to be a more convenient means of direct spin excitation without requiring coupling between spins and orbitals or phonons. However, room-temperature responses are usually limited to small deviations from the equilibrium state because of the relatively weak THz magnetic fields in common approaches. Here, we studied the magnetization dynamics in a HoFeO3 crystal at room temperature. A custom-made spiral-shaped microstructure was used to locally generate a strong multicycle THz magnetic near field perpendicular to the crystal surface; the maximum magnetic field amplitude of about 2 T was achieved. The observed time-resolved change in the Faraday ellipticity clearly showed second- and third-order harmonics of the magnetization oscillation and an asymmetric oscillation behaviour. Not only the ferromagnetic vector M but also the antiferromagnetic vector L plays an important role in the nonlinear dynamics of spin systems far from equilibrium.

physics.optics↗

arXiv2022

Spacetime-emergent ring toward tabletop quantum gravity experiments

We propose a way to discover, in tabletop experiments, spacetime-emergent materials, that is, materials holographically dual to higher-dimensional quantum gravity systems under the AdS/CFT correspondence. The emergence of the holographic spacetime is verified by a mathematical imaging transform of the response function on the material. We consider theories on a 1-dimensional ring-shaped material, and compute the response to a scalar source locally put at a point on the ring. When the theory on the material has a gravity dual, the imaging in the low temperature phase exhibits a distinct difference from the ordinary materials: the spacetime-emergent material can look into the holographically emergent higher-dimensional curved spacetime and provides an image as if a wave had propagated there. Therefore the image is an experimental signature of the spacetime emergence. We also estimate temperature, ring size and source frequency usable in experiments, with an example of a quantum critical material, TlCuCl$_3$.

hep-th↗

arXiv2022

Anomalous temperature dependence of high-harmonic generation in Mott insulators

We reveal the crucial effect of strong spin-charge coupling on high-harmonic generation (HHG) in Mott insulators. In a system with antiferromagnetic correlations, the HHG signal is drastically enhanced with decreasing temperature, even though the gap increases and the production of charge carriers is suppressed. This anomalous behavior, which has also been observed in recent HHG experiments on Ca$_2$RuO$_4$, originates from a cooperative effect between the spin-charge coupling and the thermal ensemble, and the strongly temperature-dependent coherence between charge carriers. We argue that the peculiar temperature dependence of HHG is a generic feature of Mott insulators, which can be controlled via the Coulomb interaction and dimensionality of the system. Our results demonstrate that correlations between different degrees of freedom, which are a characteristic feature of strongly correlated solids, have significant and nontrivial effects on nonlinear optical responses.

cond-mat.str-el↗

arXiv2022

Phase-resolved measurement and control of ultrafast dynamics in terahertz electronic oscillators

As a key component for next-generation wireless communications (6G and beyond), terahertz (THz) electronic oscillators are being actively developed. Precise and dynamic phase control of ultrafast THz waveforms is essential for high-speed beam steering and high-capacity data transmission. However, measurement of such ultrafast dynamic process is beyond the scope of electronics due to the limited bandwidth of the electrical measuring instruments. Here we surpass this limit by applying photonic technology. Using a femtosecond laser, we generate offset-free THz pulses to phase-lock the electronic oscillators based on a resonant tunneling diode. This enables us to perform phase-resolved measurement of the emitted THz electric field waveform in time-domain with sub-cycle time resolution. Ultrafast dynamic response such as anti-phase locking behaviour is observed, which is distinct from in-phase stimulated emission observed in laser oscillators. We also show that the dynamics follows the universal synchronization theory for limit cycle oscillators. This provides a basic guideline for dynamic phase control of THz electronic oscillators, enabling many key performance indicators to be achieved in the new era of 6G and beyond.

physics.optics↗

arXiv2022

Exciton-coherence generation through diabatic and adiabatic dynamics of Floquet state

Floquet engineering of electronic systems is a promising way of controlling quantum material properties on an ultrafast time scale. So far, the energy structure of Floquet states in solids has been observed through time and angle-resolved photoelectron spectroscopy or pump-probe measurement techniques. However, the dynamical aspects of the photon-dressed states under ultrashort pulse driving have not been explored yet. Their dynamics become highly sensitive to the envelope of the driving field when the light-matter interaction enters non-perturbative regime, and thus, understanding of them is crucial for ultrafast manipulation of quantum state. Here, we observed coherent exciton emissions under intense and non-resonant mid-infrared fields in monolayer WSe2 at room temperature, which is unexpected in perturbative nonlinear optics. Together with numerical calculations, our measurements revealed that the coherent exciton emission reflects the diabatic and adiabatic dynamics of Floquet states. Our results provide a new approach to probing the dynamics of the Floquet state and lead to control of quantum materials through pulse shaping of the driving field.

cond-mat.other↗

arXiv2021

Injection Locking and Noise Reduction of Resonant Tunneling Diode Terahertz Oscillator

We studied the injection-locking properties of a resonant-tunneling-diode terahertz oscillator in the small-signal injection regime with a frequency-stabilized continuous THz wave. The linewidth of the emission spectrum dramatically decreased to less than 120 mHz (HWHM) from 4.4 MHz in the free running state as a result of the injection locking. We experimentally determined the amplitude of injection voltage at the antenna caused by the injected THz wave. The locking range was proportional to the injection amplitude and consistent with Adler's model. As increasing the injection amplitude, we observed decrease of the noise component in the power spectrum, which manifests the free-running state, and alternative increase of the injection-locked component. The noise component and the injection-locked component had the same power at the threshold injection amplitude as small as $5\times10^{-4}$ of the oscillation amplitude. This threshold behavior can be qualitatively explained by Maffezzoni's model of noise reduction in general limit-cycle oscillators.

physics.app-ph↗

arXiv2020

Control of high-harmonic generation by tuning the electronic structure and carrier injection

High-harmonic generation (HHG), which is generation of multiple optical harmonic light, is an unconventional nonlinear optical phenomenon beyond perturbation regime. HHG, which was initially observed in gaseous media, has recently been demonstrated in solid state materials. How to control the extreme nonlinear optical phenomena is a challenging subject. Compared to atomic gases, solid state materials have advantages in controlling electronic structures and carrier injection. Here, we demonstrate control of HHG by tuning electronic structure and carrier injection using single-walled carbon nanotubes (SWCNTs). We reveal systematic changes in the high-harmonic spectra of SWCNTs with a series of electronic structures from a metal to a semiconductor. We demonstrate enhancement or reduction of harmonic generation by more than one order of magnitude by tuning electron and hole injection into the semiconductor SWCNTs through electrolyte gating. These results open a way to control HHG within the concept of field effect transistor devices.

physics.optics↗

arXiv2020

Dynamical symmetry of strongly light-driven electronic system in crystalline solids

The Floquet state, which is a periodically and intensely light driven quantum state in solids, has been attracting attention as a novel state that is coherently controllable on an ultrafast time scale. An important issue has been to demonstrate experimentally novel electronic properties in the Floquet state. One technique to demonstrate them is the light scattering spectroscopy, which offers an important clue to clarifying the symmetries and energy structures of the states through symmetry analysis of the polarization selection rules. Here, we determine circular and linear polarization selection rules of light scattering in a mid-infrared-driven Floquet system in monolayer MoS2 and provide a comprehensive understanding in terms of the "dynamical symmetry" of the Floquet state.

physics.optics↗

arXiv2020

Observation of exotic water in hydrophilic nanospace of porous coordination polymers

The fundamental understanding of water confined in porous coordination polymers (PCPs) is significantly important not only for their applications such as gas storage and separation, but also for exploring the confinement effects in the nanoscale spaces. Here, we report the observation of an exotic water in the well-designed hydrophilic nanopores of PCPs. Single-crystal X-ray diffraction found that nanoconfined water has an ordered structure that is characteristic in ices, but infrared spectroscopy revealed a significant number of broken hydrogen bonds that is characteristic in liquids. We found that their structural properties are quite similar to those of solid-liquid supercritical water predicted in hydrophobic nanospace at extremely high pressure. Our results will open up not only new potential applications of exotic water in PCPs to control chemical reactions but also experimental systems to clarify the existence of solid-liquid critical points.

physics.chem-ph↗

arXiv2019

Inherent Limit to Coherent Phonon Generation under Non-Resonant Light Field Driving

Coherent manipulation of quasi-particles is a crucial method to realize ultrafast switching of the relating macroscopic order. In this letter, we studied coherent phonon generation under strong light field which allows to induce non-perturbative nonlinear optical phenomena in solids. The efficiency of coherent phonon generation starts to saturate and deviate from the pronounced linear power dependence when the light intensity goes into the non-perturbative regime. We propose a novel theoretical model based on Floquet picture and show that the saturation is due to a limitation of the driving force inherent in non-resonant driving of the electronic system in the non-perturbative regime.

physics.optics↗

arXiv2019

Interband resonant high-harmonic generation by valley polarized electron-hole pairs

We demonstrated nonperturbative high harmonics induced by intense mid-infrared light up to 18th order that well exceed the material bandgap in monolayer transition metal dichalcogenides. The intensities of the even-order high-harmonic radiation did not monotonically decrease as the harmonic order increased. By comparing the high harmonic spectra with the optical absorption spectra, we found that the enhancement in the even-order high harmonics could be attributed to the resonance to the band nesting energy. The symmetry analysis shows that the valley polarization and anisotropic band structure lead to polarization of the high-harmonic radiation under excitation with the polarization along the zigzag direction. We also examined the possible recombination pathways of electrons and holes by calculating their dynamics in real and momentum spaces based on three-step model in solids. It revealed that, by considering the electrons and holes generated at neighboring lattice sites, the electron-hole polarization driven to the band nesting region should contribute to the high harmonic radiation. Our findings open the way for attosecond science with monolayer materials having widely tunable electronic structures.

cond-mat.mes-hall↗

arXiv2019

Selective excitation of multipolar spoof plasmons using orbital angular momentum of light

The nature of light-matter interaction is governed by the spatial-temporal structures of a light field and material wavefunctions. The emergence of the light beam with transverse phase vortex, or equivalently orbital angular momentum (OAM) has been providing intriguing possibilities to induce unconventional optical transitions beyond the framework of the electric dipole interaction. The uniqueness stems from the OAM transfer from light to material, as demonstrated using the bound electron of a single trapped ion. However, many aspects of the vortex light-matter interaction are still unexplored especially in solids with extended electronic states. Here, we unambiguously visualized dipole-forbidden multipolar excitations in a solid-state electron system; spoof localized surface plasmon, selectively induced by the terahertz vortex beam. The results obey the selection rules governed by the conservation of the total angular momentum, which is numerically confirmed by the electromagnetic field analysis. Our results show light's OAM can be efficiently transferred to an elementary excitation in solids.

physics.optics↗

arXiv2018

Lattice phonon modes of the spin crossover crystal [Fe(phen)2(NCS)2] studied by THz, IR, Raman spectroscopies and DFT calculations

[Fe(phen)2(NCS)2] is a prototype transition metal complex material, which undergoes a phase transition between low-spin (LS) and high-spin (HS) phases, induced by temperature, pressure or light. Vibrational modes play a key role for spin-state switching both in thermal and photo-induced cases, by contributing to vibrational entropy for thermal equilibrium transitions or driving the fast structural trapping of the photoinduced high spin state. Here we study the crystal phonon modes of [Fe(phen)2(NCS)2], by combining THz, IR, and Raman spectroscopies sensitive to modes in different frequency ranges and different symmetries. We compare the experimental results to DFT calculations performed in a periodic 3D crystal for understanding the phonon modes in the crystal, compared to molecular vibrations. Indeed, each vibrational mode of the isolated molecule combines into several modes of different symmetry and frequency in the crystal, as the unit cell contains four molecules. We focus our attention on the HS symmetric and anti-symmetric breathing modes in the crystal as well as on the N-CS stretching modes.

cond-mat.mtrl-sci↗

arXiv2018

Zener Tunneling Breakdown in Phase-Change Materials Revealed by Intense Terahertz Pulses

We have systematically investigated the spatial and temporal dynamics of crystallization that occurs in the phase-change material Ge2Sb2Te5 upon irradiation with an intense THz pulse. THz pump and optical probe spectroscopy revealed that Zener tunneling induces a nonlinear increase in the conductivity of the crystalline phase. This result indicates that the large electric field associated with the THz pulses causes a nonlinear increase only at the edge of the crystallized area. The electric field concentrating in this area causes a temperature increase via Joule heating, which in turn leads to nanometer scale crystal growth parallel to the field and the formation of filamentary conductive domains across the sample.

cond-mat.mtrl-sci↗