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We have applied a many-body Wannier functions method to theoretically calculate an excitonic optical conductivity spectrum and energy structure in a one-dimensional (1D) Mott insulator at absolute zero temperature with large system size. Focusing on full charge fluctuations associated with pairs of a holon and doublon, we employ a charge model, which is interpreted as a good effective model to investigate photoexcitations of a 1D extended Hubbard model at half-filling in the spin-charge separation picture. As a result, the theoretical spectra with appropriate broadenings qualitatively reproduce the recent experimental data of ET-F$_{2}$TCNQ at 294 K with and without a modulated electric field. Regarding the excitonic energy structure, we have found that the excitons, especially for even-parity, are weakly bound by many-body effects. This is also consistent with the fitting parameters reported in the recent experiment. Thus, our theoretical method presented in this paper is practically useful to understand physical roles of charge fluctuations in many-body excited states of a 1D Mott insulator., Comment: 31 pages, 9 figures

We report a newly designed mid-infrared-pump visible-probe measurement system, which can measure phase-sensitive responses to a mid-infrared pulse along the oscillating electromagnetic field. In this system, the pump light is a phase-locked mid-infrared pulse with temporal width of 100 fs, which is produced via difference frequency generation (DFG) from two idler pulses of two optical parametric amplifiers (OPAs) that are excited by the same Ti:sapphire regenerative amplifier. The probe pulse is a visible pulse with temporal width of 9 fs, and it is generated from a custom-built non-collinear OPA. By measuring the electric-field waveforms of mid-infrared pump pulses with electro-optic sampling and evaluating their carrier envelope phase (CEP) and the temporal positions of their envelopes relative to ultrashort visible probe pulses, we are able to perform double feedback corrections that eliminate both the following sources of drift. The CEP drift in mid-infrared pulses originating from fluctuations in the difference of optical-path lengths of the two idler pulses before the DFG is corrected by inserting a wedge plate in one idler path, and the drift in pump-probe delay times due to fluctuations in the difference of the overall optical-path lengths of the pump and probe pulses is corrected with mechanical delay lines. In this double-feedback system, the absolute carrier phase of mid-infrared pulses can be fixed within 200 mrad and errors in the measurement of phase-sensitive responses can be reduced to within 1 fs over a few tens of hours., Comment: 17 pages including 4 figures (Supplementary materials: 4 pages including no figures)

We theoretically revealed that a weak photoexcitation achieves the electric polarization-inversion with approximately $18\%$ of all the charges, which was interpreted as a superimposition of multi-exciton states, from the charge-ordered ferroelectric ground state of (TMTTF)$_{2}$PF$_{6}$ at absolute zero temperature. Regarding a relative change of electric polarization ($\Delta P/P$), the photoexcitation corresponds to $36\%$, which is much larger than $\Delta P/P$ of other typical organic materials. The value of $\Delta P/P\sim 36\%$ can be enlarged by a strong photoexcitation. This fact is useful not only for applications of this material and other analogous materials in optical devices but also for researches toward controlling electric polarizations by light, which is one of the recent attracting issues on photoinduced phase transition phenomena. The photoexcitation of $\Delta P/P\sim 36\%$ corresponds to the single peak of the optical conductivity in the low-energy region, which was also observed at 10 K. Theoretical calculations are based on a quarter-filled one-dimensional effective model with appropriate parameters and 50 unit cells., Comment: 24 pages, 8 figures

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

Using a spatiotemporal terahertz radiation imaging technique, we visualize photogenerated metallic inhomogeneity in the charge-ordered insulating phase of Pr$_{0.7}$Ca$_{0.3}$MnO$_3$ thin film. We reveal that photogenerated metallic regions with micrometer length scales within the charge-ordered insulating matrix are created on subpicoseond time scales. Such an inhomogeneity becomes homogeneous when the laser power and bias voltage are increased. The observed photogenerated metallic regions would act as nucleus of the insulator-metal transition observed in Pr$_{0.7}$Ca$_{0.3}$MnO$_3$., Comment: 10 pages including 3 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

Terahertz magnetic resonance driven by the light electric field, now referred to as electromagnon, has stimulated interest due to its strong candidate for future spin-electronics. One unique characteristic of electromagnons is the terahertz magnetochromism, a color change by external magnetic field, as recently demonstrated in the hexaferrite. By taking perovskite manganites and hexaferrite as model cases, the current understating of the electromagnon activity is discussed in terms of the symmetric exchange mechanism., Comment: 18 pages including 4 figures, Short overview of electromagnon study, Comments are welcome

Multiferroics with coexistent ferroelectric and magnetic orders can provide an interesting laboratory to test unprecedented magnetoelectric responses and their possible applications. One such example is the dynamical and/or resonant coupling between magnetic and electric dipoles in a solid. As the examples of such dynamical magnetoelectric effects, (1) the multiferroic domain wall dynamics and (2) the electric-dipole active magnetic responses are discussed with the overview of recent experimental observations., Comment: 15 pages including 6 figures; Accepted for publication in Phil. Trans. A Roy. Soc. (Special issue, Spin on Electronics)

Effects of temperature (6--225 K) and magnetic field (0--7 T) on the low-energy (1.2--5 meV) electrodynamics of the electromagnon, the magnetic resonance driven by the light electric field, have been investigated for a hexaferrite magnet Ba$_2$Mg$_2$Fe$_{12}$O$_{22}$ by using terahertz time-domain spectroscopy. We find the gigantic terahertz magnetochromism via electromagnons; the magnetochromic change, as defined by the difference of the absorption intensity with and without magnetic field, exceeds 500% even at 0.6 T. The results arise from the fact that the spectral intensity of the electromagnon critically depends on the magnetic structure. With changing the conical spin structures in terms of the conical angle $\theta$ from the proper screw ($\theta=0^\circ$) to the ferrimagnetic ($\theta=90^\circ$) through the conical spin-ordered phases ($0^\circ<\theta<90^\circ$) by external magnetic fields, we identify the maximal magnetochromism around $\theta\approx45^\circ$. On the contrary, there is no remarkable signature of the electromagnon in the proper screw and spin-collinear (ferrimagnetic) phases, clearly indicating the important role of the conical spin order to produce the magnetically-controllable electromagnons. The possible origin of this electromagnon is argued in terms of the exchange-striction mechanism., Comment: 19 pages including 7 figures; Accepted for publication in Phys. Rev. B

We propose that concurrently magnetic and ferroelectric, i.e. multiferroic, compounds endowed with electrically-active magnetic excitations (electromagnons) provide a key to produce large directional dichroism for long wavelengths of light. By exploiting the control of ferroelectric polarization and magnetization in a multiferroic oxide Ba$_2$CoGe$_2$O$_7$, we demonstrate the realization of such a directional light-switch function at terahertz frequecies in resonance with the electromagnon absorption. Our results imply that this hidden potential is present in a broad variety of multiferroics.

Terahertz time-domain spectroscopy was performed to directly probe the low-energy (1-5 meV) electrodynamics of triangular lattice antiferromagnets CuFe1-xGaxO2 (x = 0.00, 0.01, and 0.035). We discovered an electromagnon (electric-field-active magnon) excitation at 2.3 meV in the paraelectric up-up-down-down collinear magnetic phase, while this electromagnon vanishes in the ferroelectric helimagnetic phase. Anti-correlation with noncollinear magnetism excludes the exchange-striction mechanism as the origin of dynamical magnetoelectric coupling, and hence evidences the observation of spin-orbit coupling mediated electromagnon in the present compound., Comment: 5 pages, 5 figures. Accepted in Physical Review Letters

Recent spectroscopic studies at terahertz frequencies for a variety of multiferroics endowed with both ferroelectric and magnetic orders have revealed the possible emergence of a new collective excitation, frequently referred to as electromagnon. It is magnetic origin, but becomes active in response to the electric field component of light. Here we give an overview on our recent advance in the terahertz time-domain spectroscopy of electromagnons or electric-dipole active magnetic resonances, focused on perovskite manganites--$R$MnO$_3$ ($R$ denotes rare-earth ions). The respective electric and magnetic contributions to the observed magnetic resonance are firmly identified by the measurements of the light-polarization dependence using a complete set of the crystal orientations. We extract general optical features in a variety of the spin ordered phases, including the $A$-type antiferromagnetic, collinear spin ordered, and ferroelectric $bc$ and $ab$ spiral spin ordered phases, which are realized by tuning the chemical composition of $R$, temperature, and external magnetic field. In addition to the antiferromagnetic resonances of Mn ions driven by the magnetic field component of light, we clarify that the electromagnon appears only for light polarized along the a-axis even in the collinear spin ordered phase and grows in intensity with evolution of the spiral spin order, but independent of the direction of the spiral spin plane ($bc$ or $ab$) or equivalently the direction of the ferroelectric polarization $P_{\rm s}$ ($P_{\rm s}\| c$ or $P_{\rm s}\| a$). A possible origin of the observed magnetic resonances at terahertz frequencies is discussed by comparing the systematic experimental data presented here with theoretical considerations based on Heisenberg model., Comment: 19 pages including 15 figures and 2 tables; Invited Paper in Special Issue on Terahertz Wave Photonics in J. Opt. Soc. Am. B (Accepted for publication)

A broad continuum-like spin excitation (1--10 meV) with a peak structure around 2.4 meV has been observed in the ferroelectric $ab$ spiral spin phase of Gd$_{0.7}$Tb$_{0.3}$MnO$_3$ by using terahertz (THz) time-domain spectroscopy. Based on a complete set of light-polarization measurements, we identify the spin excitation active for the light $E$ vector only along the a-axis, which grows in intensity with lowering temperature even from above the magnetic ordering temperature but disappears upon the transition to the $A$-type antiferromagnetic phase. Such an electric-dipole active spin excitation as observed at THz frequencies can be ascribed to the two-magnon excitation in terms of the unique polarization selection rule in a variety of the magnetically ordered phases., Comment: 11 pages including 3 figures

Temperature (5--250 K) and magnetic field (0--70 kOe) variations of the low-energy (1--10 meV) electrodynamics of spin excitations have been investigated for a complete set of light-polarization configurations for a ferroelectric magnet DyMnO$_3$ by using terahertz time-domain spectroscopy. We identify the pronounced absorption continuum (1--8 meV) with a peak feature around 2 meV, which is electric-dipole active only for the light $E$-vector along the a-axis. This absorption band grows in intensity with lowering temperature from the spin-collinear paraelectric phase above the ferroelectric transition, but is independent of the orientation of spiral spin plane ($bc$ or $ab$), as shown on the original $P_{\rm s}$ (ferroelectric polarization) $\parallel c$ phase as well as the magnetic field induced $P_{\rm s}\parallel a$ phase. The possible origin of this electric-dipole active band is argued in terms of the large fluctuations of spins and spin-current., Comment: New version, 11 pages including colored 8 figures

Cross-correlation between magnetic and dielectric properties has been attracting renewed interest because of the fundamental as well as technological importance of controlling the electric (magnetic) polarization by an external magnetic (electric) field. Here, we report the novel phenomenon that an external magnetic field induces and/or modifies ferroelectric states in a magnetic material, DyMn2O5. Measurements of temperature dependence of hysteretic polarization curves, pyroelectric current, specific heat, optical second harmonic generation, and x-ray superlattice peaks have revealed successive phase transitions between 43 K and 4 K, accompanying three ferroelectric phases. The zero-field lowest-temperature phase (<8 K) induced by the Dy-moment ordering is a reentrant paraelectric state, but is turned to a ferroelectric state with increasing the magnetic field. The phenomenon is closely related to the metamagnetic transitions of the Dy f-moment, indicating that all the ferroelectric phases of this material are strongly tied to the antiferromagnetic Mn spin structure affected by the f-d exchange interaction. The electric phase diagram for DyMn2O5 is presented in the plane of temperature and magnetic field., Comment: 19 pages, 6 figures

A combined study with use of time-domain pump-probe spectroscopy and time-domain terahertz transmission spectroscopy have been carried out on an underdoped Bi$_2$Sr$_2$CaCu$_2$O$_{8+{\delta}}$ thin film. It was observed that the low energy multi-excitation states were decomposed into superconducting gap and pseudogap. The pseudogap locally opens below $T^*{\simeq}210$ K simultaneously with the appearance of the high-frequency partial pairs around 1.3 THz. With decreasing temperature, the number of the local domains with the partial phase coherence increased and saturated near 100 K, and the macroscopic superconductivity appeared below 76 K through the superconductivity fluctuation state below 100 K. These experimental results indicate that the pseudogap makes an important role for realization of the superconductivity as a precursor to switch from the partial to the macroscopic phase coherence., Comment: Revtex4, 4 pages, 4 figures

Terahertz (THz) radiation with its spectrum extending up to 1 THz has been observed by an illumination of femtosecond optical pulses to optical switching devices fabricated on magnetoresistive manganite thin films; Pr$_{0.7}$Ca$_{0.3}$MnO$_3$. The THz radiation strongly depends on temperature $T$ and its $T$ trend reverses sign across charge-orbital and spin ordering $T$'s., Comment: Revtex4, 4 pages including 3 figures

Direct experimental estimations of the low-energy ($1.5\sim10$ meV) complex dielectric constants spectrum and its temperature variation have been investigated for La$_{0.7}$Ca$_{0.3}$MnO$_3$ thin films using terahertz time-domain spectroscopy. At low temperatures, a clear Drude-term emerges. With increasing temperature, the scattering rate increases, while the plasma frequency decreases, derived both from a simple Drude model. Finally, a Drude-term submerges well below the insulator-metal transition temperature. On the basis of the present results, low-energy charge dynamics are discussed., Comment: REVTeX 13 pages, 3 figures