Nonlinear Optical Properties in an Epitaxial YbFe2O4 Film Probed by Second Harmonic and Terahertz Generation.

An epitaxial film of YbFe2O4, a candidate for oxide electronic ferroelectrics, was fabricated on yttrium-stabilized zirconia (YSZ) substrate by magnetron sputtering technique. For the film, second harmonic generation (SHG), and a terahertz radiation signal were observed at room temperature, confirming a polar structure of the film. The azimuth angle dependence of SHG shows four leaves-like profiles and is almost identical to that in a bulk single crystal. Based on tensor analyses of the SHG profiles, we could reveal the polarization structure and the relationship between the film structure of YbFe2O4 and the crystal axes of the YSZ substrate. The observed terahertz pulse showed anisotropic polarization dependence consistent with the SHG measurement, and the intensity of the emitted terahertz pulse reached about 9.2% of that emitted from ZnTe, a typical nonlinear crystal, implying that YbFe2O4 can be applied as a terahertz wave generator in which the direction of the electric field can be easily switched.

Generation of sub-100 fs electron pulses for time-resolved electron diffraction using a direct synchronization method.

To investigate photoinduced phenomena in various materials and molecules, ultrashort pulsed x-ray and electron sources with high brightness and high repetition rates are required. The x-ray and electron's typical and de Broglie wavelengths are shorter than lattice constants of materials and molecules. Therefore, photoinduced structural dynamics on the femtosecond to picosecond timescales can be directly observed in a diffraction manner by using these pulses. This research created a tabletop ultrashort pulsed electron diffraction setup that used a femtosecond laser and electron pulse compression cavity that was directly synchronized to the microwave master oscillator (∼3 GHz). A compressed electron pulse with a 1 kHz repetition rate contained 228 000 electrons. The electron pulse duration was estimated to be less than 100 fs at the sample position by using photoinduced immediate lattice changes in an ultrathin silicon film (50 nm). The newly developed time-resolved electron diffraction setup has a pulse duration that is comparable to femtosecond laser pulse widths (35-100 fs). The pulse duration, in particular, fits within the timescale of photoinduced phenomena in quantum materials. Our developed ultrafast time-resolved electron diffraction setup with a sub-100 fs temporal resolution would be a powerful tool in material science with a combination of optical pump-probe, time-resolved photoemission spectroscopic, and pulsed x-ray measurements.

Separation between low-energy hole dynamics and spin dynamics in a frustrated magnet.

An angle-resolved photoemission spectroscopy (ARPES) study is reported on a Mott insulator NiGa2S4 in which Ni2+ (S=1) ions form a triangular lattice and the Ni spins do not order even in its ground state. The first ARPES study on the two-dimensional spin-disordered system shows that low-energy hole dynamics at high temperatures is characterized by wave vectors Q(E) which are different from wave vectors Q(M) dominating low-energy spin excitations at low temperatures. The unexpected difference between Q(E) and Q(M) is deeply related to charge fluctuation across the Mott gap in the frustrated lattice and is a key issue to understand the spin-disordered ground states in Mott insulators.