We report on the observation of terahertz radiation in a non-centrosymmetric insulating oxide, paratellurite (α-TeO2) 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 ∼ 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 ∼ 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.
We report on the emission of terahertz radiation by irradiation of femtosecond laser pulses in non-centrosymmetric paraelectric and ferroelectric phases of Co3B7O13I 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 (500 × 500 m 2 ), the observed polarization vector of the radiated terahertz wave was tilted from directions of spontaneous polarization, i.e.,
100, 010 , and 001 in cubic setting, which can be explained by the presence of a ferroelectric 90 domain wall of the 101 plane.
1. Second-order nonlinear optical susceptibility in paraelectric phase
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 ∼ 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 ∼ 800 µm 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.
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