Complex anisotropy ratio of third harmonic generation in a semiconductor using a terahertz free electron laser.

The nonlinear susceptibility in the terahertz region is expected to have a non-negligible imaginary part originating from the momentum-dependent scattering time of free carriers, but it has been scarcely reported. By utilizing an intense 4 THz beam from a terahertz free electron laser, we investigated the azimuth angle dependence of the third harmonic generation (THG) from semiconductors. The observed angular anisotropy of THG revealed the contribution of the imaginary part of the nonlinear susceptibility originating from the momentum-scattering time relation in addition to its real part originating from the band nonparabolicity. The results provide a deeper understanding of nonlinear optics in the terahertz region.

Third harmonic generation due to free carrier in InSb using a terahertz free electron laser.

We report on the third harmonic generation (THG) in InSb semiconductor irradiated by a terahertz (THz) free electron laser (FEL). The conversion of 4 THz (wavelength 70 µm) FEL outputs into its third harmonic 12 THz was observed. We found that by tuning the sample temperature to 360 K, high conversion efficiency up to 1% can be obtained and is the highest in the THz and FIR regions below 10 THz. We also discuss the observed intensity dependence of the THG with the nonlinear order lower than 3 when the pumping intensity was high.

Plane photoacoustic wave generation in liquid water using irradiation of terahertz pulses.

We demonstrate photoacoustic wave propagation with a plane wavefront in liquid water using a terahertz (THz) laser pulse. The THz light can effectively generate the photoacoustic wave in water because of strong absorption via a stretching vibration mode of the hydrogen bonding network. The excitation of a large-area water surface irradiated by loosely focused THz light produces a plane photoacoustic wave. This is in contrast with conventional methods using absorbers or plasma generation using near-infrared laser light. The photoacoustic wave generation and plane wave propagation are observed using a system with a THz free-electron laser and shadowgraph imaging. The plane photoacoustic wave is generated by incident THz light with a small radiant exposure of < 1 mJ/cm2 and delivered 600 times deeper than the penetration depth of THz light for water. The THz-light-induced plane photoacoustic wave offers great advantages to non-invasive operations for industrial and biological applications as demonstrated in our previous report (Yamazaki et al. in Sci Rep 10:9008, 2020).

Propagation of THz irradiation energy through aqueous layers: Demolition of actin filaments in living cells.

The effect of terahertz (THz) radiation on deep tissues of human body has been considered negligible due to strong absorption by water molecules. However, we observed that the energy of THz pulses transmits a millimeter thick in the aqueous solution, possibly as a shockwave, and demolishes actin filaments. Collapse of actin filament induced by THz irradiation was also observed in the living cells under an aqueous medium. We also confirmed that the viability of the cell was not affected under the exposure of THz pulses. The potential of THz waves as an invasive method to alter protein structure in the living cells is demonstrated.

Reconfiguration of magnetic domain structures of ErFeO3 by intense terahertz free electron laser pulses.

Understanding the interaction between intense terahertz (THz) electromagnetic fields and spin systems has been gaining importance in modern spintronics research as a unique pathway to realize ultrafast macroscopic magnetization control. In this work, we used intense THz pulses with pulse energies in the order of 10 mJ/pulse generated from the terahertz free electron laser (THz-FEL) to irradiate the ferromagnetic domains of ErFeO3 single crystal. It was found that the domain shape can be locally reconfigured by irradiating the THz - FEL pulses near the domain boundary. Observed domain reconfiguration mechanism can be phenomenologically understood by the combination of depinning effect and the entropic force due to local thermal gradient exerted by terahertz irradiation. Our finding opens up a new possibility of realizing thermal-spin effects at THz frequency ranges by using THz-FEL pulses.

Significant Volume Expansion as a Precursor to Ablation and Micropattern Formation in Phase Change Material Induced by Intense Terahertz Pulses.

With rapid advances occurring in terahertz (THz) radiation generation techniques, the interaction between matter and intense THz fields has become an important research topic. Among different types of THz radiation sources, the free electron laser (FEL) is a promising experimental tool that is expected to pave the way for new forms of material processing, control of phase transitions, and serve as a test bench for extreme operating conditions in high-speed small-size electrical and magnetic devices through the exploitation of strong THz electrical and magnetic fields without the presence of interband electronic excitation. In the current work, we irradiated Ge2Sb2Te5 phase change memory material with intense THz pulse trains from an FEL and observed THz-induced surface changes due to damage as a precursor to ablation and the formation of fine surface undulations whose spatial period is comparable to or slightly smaller than the wavelength of the excitation THz pulses in the material. The formation of undulations as well as the fact that no significant thermal effect was observed below the volume expansion threshold suggests that THz-induced effects mainly contributed to the observed changes. To the best of our knowledge, this is the first experimental observation of THz-induced undulations (so-called "LIPSS"), which are of potential importance for laser material processing.

Polymer Morphological Change Induced by Terahertz Irradiation.

As terahertz (THz) frequencies correspond to those of the intermolecular vibrational modes in a polymer, intense THz wave irradiation affects the macromolecular polymorph, which determines the polymer properties and functions. THz photon energy is quite low compared to the covalent bond energy; therefore, conformational changes can be induced "softly," without damaging the chemical structures. Here, we irradiate a poly(3-hydroxybutylate) (PHB) / chloroform solution during solvent casting crystallization using a THz wave generated by a free electron laser (FEL). Morphological observation shows the formation of micrometer-sized crystals in response to the THz wave irradiation. Further, a 10-20% increase in crystallinity is observed through analysis of the infrared (IR) absorption spectra. The peak power density of the irradiating THz wave is 40 MW/cm(2), which is significantly lower than the typical laser intensities used for material manipulation. We demonstrate for the first time that the THz wave effectively induces the intermolecular rearrangement of polymer macromolecules.