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We observe a terahertz radiation from a hydrogen-bonded organic molecular ferroelectric 5,6-dichloro-2-methylbenzimidazole excited by a femtosecond laser pulse at room temperature. The emitted terahertz wave consists of three oscillatory components, the frequencies of which agree with those of Raman- and infrared-active phonon modes. This suggests that the terahertz radiation is attributed to polarization modulations by infrared-active phonons excited via the impulsive stimulated Raman scattering processes. By taking into account the Raman polarizability tensor and dipole-moment for each phonon, we succeeded in reproducing not only the spectrum of the terahertz radiation, but also its time characteristic. The analysis method is discussed in detail. Our result provides a new way for the light-induced terahertz radiation in organic ferroelectrics., Comment: 39 pages including Supplemental Material

Photoexcitation in solids brings about transitions of electrons/holes between different electronic bands. If the solid lacks an inversion symmetry, these electronic transitions support spontaneous photocurrent due to the topological character of the constituting electronic bands; the Berry connection. This photocurrent, termed shift current, is expected to emerge on the time-scale of primary photoexcitation process. We observed ultrafast time evolution of the shift current in a prototypical ferroelectric semiconductor by detecting emitted terahertz electromagnetic waves. By sweeping the excitation photon energy across the band gap, ultrafast electron dynamics as a source of terahertz emission abruptly changes its nature, reflecting a contribution of Berry connection upon interband optical transition. The shift excitation carries a net charge flow, and is followed by a swing-over of the electron cloud on the sub-picosecond time-scale of electron-phonon interaction. Understanding these substantive characters of the shift current will pave the way for its application to ultrafast sensors and solar cells., Comment: 19 pages, 5 figures

We demonstrate a new method to detect ferroelectric domains in inside and surface regions of organic ferroelectrics by mapping out two orthogonally polarized terahertz waves radiated from the crystal upon the irradiation of near-infrared femtosecond laser pulses. We used polarization dependence of the effective depths radiating the terahertz waves, which originate from the optical anisotropy in the terahertz frequency region. This allows us to distinguish ferroelectric domains in the inside and surface regions of the crystals. We applied this method to a room-temperature organic supramolecular ferroelectric crystal, 1:1 salt of 5,5'-dimethyl-2,2'-bipyridine and deuterated iodanilic acid. A single domain covering almost all the area of an as-grown crystal ($\sim$600 $\mu$m $\times$ 800 $\mu$m) is discerned in the inside region, while complicated multi-domain in size of $\sim$ 200 $\mu$m is observed in the surface region. By applying external electric field along the 2c-b axis (ferroelectric polarization direction), the polarization switching proceeds with successive propagations of uncharged (neutral) and quasi-one-dimensional 180$^\circ$ domain walls (DWs) along the b-axis ($\perp$ 2c-b axis). This results in the formation of another uncharged and two-dimensional 180$\circ$ DW parallel to the (100) plane, which covers all the area of the crystal. We discuss the usefulness of the present terahertz radiation imaging technique and ferroelectric DW dynamics in terms of anisotropic stacking of hydrogen-bonded chains., Comment: 37 pages including 7 figures

Polarization control of terahertz wave is a challenging subject in terahertz science and technology. Here, we report a simple method to control polarization state of the terahertz wave in terahertz generation process. At room temperature, terahertz radiation from a noncentrosymmetric and chiral oxide, sillenite Bi$_{12}$GeO$_{20}$, is observed by the irradiation of linearly polarized femtosecond laser pulses at 800 nm. The polarization state of the emitted terahertz wave is found to be elliptic with an ellipticity of $\sim$0.37$\pm$0.10. Furthermore, the ellipticity was altered to a nearly zero ($\sim$0.01$\pm$0.01) by changing the polarization of the incident linearly polarized femtosecond laser pulses. Such a terahertz radiation characteristic is attributable to variation of the polarization state of the emitted terahertz waves, which is induced by retardation due to the velocity mismatch between the incident femtosecond laser pulse and generated terahertz wave and by the polarization tilting due to the optical activity at 800 nm., Comment: 23 pages including 4 figures and table

Terahertz radiation by optical rectification has been observed at room temperature in a hydrogen-bonded organic molecular ferroelectric crystal, 2-phenyl malondialdehyde (PhMDA). The radiated electromagnetic wave consisted of a single-cycle terahertz pulse with a temporal width of $\sim$ 0.5 ps. The terahertz radiation amplitude divided by the sample thickness in PhMDA was nearly equivalent to that in a typical terahertz wave emitter ZnTe. This is attributable to a long coherence length in the range of 130 $\sim$ 800 $\mu$m for the terahertz radiation from PhMDA. We also discussed the possibility of PhMDA as a terahertz wave emitter in terms of the phase-matching condition., Comment: 8 pages including 4 figures

We report on the emission of terahertz radiation by irradiation of femtosecond laser pulses in non-centrosymmetric paraelectric and ferroelectric phases of Co$_3$B$_7$O$_{13}$I boracite. The Generation of the terahertz waves in both phases is caused by optical rectification via a second-order nonlinear optical effect. In the ferroelectric phase, we successfully visualized ferroelectric domains by analyzing the polarization state of the terahertz wave radiated from the crystal. In a large area of the crystal ($\sim$ 500 $\times$ 500 $\mu$m$^2$), the observed polarization vector of the radiated terahertz wave was tilted from directions of spontaneous polarization, i.e., [100]$_{\rm cub}$, [010]$_{\rm cub}$, and [001]$_{\rm cub}$ in cubic setting, which can be explained by the presence of a ferroelectric 90$^\circ$ domain wall of the (101)$_{\rm cub}$ plane., Comment: 19 pages including 4 figures

We report on the observation of terahertz radiation in a non-centrosymmetric insulating oxide, paratellurite ($\alpha$-TeO$_2$) by irradiation of a femtosecond laser pulse at room temperature. In the power spectrum of the terahertz radiation, an intensity fringe pattern with a period of $\sim$ 0.25 THz shows up below 3 THz. It can be reproduced by taking into account the effective generation length for the terahertz radiation with a poor phase-matching condition. In addition, a temporal oscillation component appears in the radiated terahertz wave with a frequency of $\sim$ 3.71 THz, which is in good agreement with the center frequency of the Raman active longitudinal optical (LO) $E$ mode. On the basis of comprehensive polarized optical and Raman spectroscopic studies, we explain the generation mechanism of the temporal oscillation component in terms of the coherent phonon generation via impulsive stimulated Raman scattering., Comment: 28 pages including 13 figures and 3 tables: Comments are welcome