Fast polarization mechanisms in the uniaxial tungsten-bronze relaxor strontium barium niobate SBN-81.

The high-frequency dielectric response of the uniaxial strontium barium niobate crystals with 81% of Sr has been studied from 1 kHz to 30 THz along the polar c axis by means of several techniques (far infrared, time domain terahertz, high-frequency and low-frequency dielectric spectroscopies) in a wide temperature interval 20-600 K. Relaxor properties were observed in the complex dielectric response and four main excitations were ascertained below the phonon frequencies. These fast polarization mechanisms take place at THz, GHz and MHz ranges and show different temperature evolution. The central mode excitation in the THz range, related to anharmonic dynamics of cations, slightly softens from high temperatures and then hardens below T ~ 400 K. Below the phase transition (at T ~ 330 K) an additional microwave excitation appears near 10 GHz related to micro domain wall oscillations. The strongest relaxation appears in the GHz range and slows down on cooling according to the Arrhenius law. Finally, another relaxation, present in the MHz range at high temperatures, also slows down on cooling at least to the kHz range. These two relaxations are due to polar fluctuations and nanodomains dynamics. Altogether, the four excitations explain the dielectric permittivity maximum in the kHz range.

Incipient ferroelectricity of water molecules confined to nano-channels of beryl.

Water is characterized by large molecular electric dipole moments and strong interactions between molecules; however, hydrogen bonds screen the dipole-dipole coupling and suppress the ferroelectric order. The situation changes drastically when water is confined: in this case ordering of the molecular dipoles has been predicted, but never unambiguously detected experimentally. In the present study we place separate H2O molecules in the structural channels of a beryl single crystal so that they are located far enough to prevent hydrogen bonding, but close enough to keep the dipole-dipole interaction, resulting in incipient ferroelectricity in the water molecular subsystem. We observe a ferroelectric soft mode that causes Curie-Weiss behaviour of the static permittivity, which saturates below 10 K due to quantum fluctuations. The ferroelectricity of water molecules may play a key role in the functioning of biological systems and find applications in fuel and memory cells, light emitters and other nanoscale electronic devices.

Bulk magnetic terahertz metamaterials based on dielectric microspheres.

Rigid metamaterials were prepared by embedding TiO2 microspheres into polyethylene. These structures exhibit a series of Mie resonances where the lowest-frequency one is associated with a strong dispersion in the effective magnetic permeability. Using time-domain terahertz spectroscopy, we experimentally demonstrated the magnetic nature of the observed resonance. The presented approach shows a way for low-cost massive fabrication of mechanically stable terahertz metamaterials based on dielectric microresonators.

Spectroscopic studies of the ferroelectric and magnetic phase transitions in multiferroic Sr1-xBaxMnO3.

Dielectric response of perovskite Sr1-xBaxMnO3 (x = 0.43 and 0.45) ceramics was investigated using microwave, THz and infrared spectroscopic techniques in order to study the ferroelectric and antiferromagnetic phase transitions with critical temperatures TC ≈ 350 K and TN ≈ 200 K, respectively. The two lowest-frequency polar phonons are overdamped above TN and they exhibit pronounced softening on heating towards TC. Nevertheless, permittivity ε' in the THz range shows only a small anomaly at TC because the phonon contribution to ε' is rather small. The phonons are coupled with a central mode which provides the main contribution to the dielectric anomaly at TC. Thus, the ferroelectric phase transition has characteristics of a crossover from displacive to order-disorder type. At the same time, the intrinsic THz central peak is partially screened by conductivity and related Maxwell-Wagner relaxation, which dominates the microwave and lower-frequency spectra. Below TN, the ferroelectric distortion markedly decreases, which has an influence on the frequencies of both the central and soft modes. Therefore, ε' in the THz range increases at TN on cooling. In spite of the strong spin-phonon coupling near TN, surprisingly no magnetodielectric effect was observed in the THz spectra upon applying magnetic field of up to 7 T, which is in contradiction with the theoretically expected huge magnetoelectric coupling. We explain this fact as due to the insensitivity of TN to magnetic field.

Multiple soft-mode vibrations of lead zirconate.

Polarized Raman, IR, and time-domain THz spectroscopy of orthorhombic lead zirconate single crystals have yielded a comprehensive picture of temperature-dependent quasiharmonic frequencies of its low-frequency phonon modes. It is argued that these modes primarily involve vibrations of Pb ions and librations of oxygen octahedra. Their relation to phonon modes of the parent cubic phase is proposed. Counts of the observed IR and Raman active modes belonging to distinct irreducible representations agree quite well with group-theory predictions. Analysis of the results yields insight into the phase transition mechanism, involving a soft ferroelectric branch coupled by a trilinear term to another two oxygen octahedra tilt modes.

Transition between metamaterial and photonic-crystal behavior in arrays of dielectric rods.

Using finite-difference time-domain simulations, we study the interactions of electromagnetic radiation with a square array of dielectric rods parallel to the electric vector. We observe the electric and magnetic Mie resonances which induce intervals of negative effective permittivity and permeability and which contribute to the formation of the photonic band gaps. Owing to the interplay of these phenomena, a narrow spectral range with a negative refractive index can occur. However, this requires the filling fraction of the dielectric to fall into a well defined interval of values and its permittivity to exceed a minimum of about 50. We discuss these phenomena from the perspective of both photonic crystal and metamaterial concepts.

Gouy shift correction for highly accurate refractive index retrieval in time-domain terahertz spectroscopy.

Terahertz spectroscopic measurements are usually performed in focused beam geometry while the standard routine for the retrieval of the sample refractive index assumes plane-wave approximation. In this paper we propose a model for the transmission function which accounts for spatially limited Gaussian terahertz beams. We demonstrate experimentally its validity and applicability for an accurate extraction of the refractive index from experimental data.

Systematic study of Mn-doping trends in optical properties of (Ga,Mn)As.

We report on a systematic study of optical properties of (Ga,Mn)As epilayers spanning the wide range of accessible Mn(Ga) dopings. The material synthesis was optimized for each nominal Mn doping in order to obtain films which are as close as possible to uniform uncompensated (Ga,Mn)As mixed crystals. We observe a broad maximum in the mid-infrared absorption spectra whose position exhibits a prevailing blueshift for increasing Mn doping. In the visible range, a peak in the magnetic circular dichroism also shifts with increasing Mn doping. The results are consistent with the description of ferromagnetic (Ga,Mn)As based on the microscopic valence band theory. They also imply that opposite trends seen previously in the optical data on a limited number of samples are not generic and cannot serve as an experimental basis for postulating the impurity band model of ferromagnetic (Ga,Mn)As.

Broadband dielectric terahertz metamaterials with negative permeability.

We present a design of dielectric metamaterials exhibiting a broad range of negative effective permeability in the terahertz spectral region. The investigated structures consist of an array of high-permittivity rods that exhibit a series of Mie resonances giving rise to the effective magnetic response. The spectral positions of resonances depend on the geometrical parameters of the rods and on their permittivity, which define the resonant confinement of the electromagnetic field within the rods. The electromagnetic coupling between the adjacent rods is negligible. With a suitable aspect ratio of the rods, a broadband magnetic response can be obtained.

High tunability of the soft mode in strained SrTiO(3)/DyScO(3) multilayers.

SrTiO(3)/DyScO(3) epitaxial multilayers with variable number and thickness (10-100 nm) of bilayers deposited on DyScO(3) substrates were investigated by means of time-domain terahertz spectroscopy at room temperature. A tensile strain develops in the SrTiO(3) films and shifts the eigenfrequency of the ferroelectric soft mode down by ∼25-45 cm(-1) with respect to the value found for single crystals. In all films the soft mode strongly hardens upon the electrical bias and a linear coupling to a silent excitation of relaxation type at 10 cm(-1) is observed. We show that the change in the THz and sub-THz response of the layers with an increasing field is determined solely by the soft mode eigenfrequency and we propose a phenomenological model describing the origin of the tunability and the peculiar properties of the ferroelectric soft mode in the terahertz spectral range.

Coexistence of the phonon and relaxation soft modes in the terahertz dielectric response of tetragonal BaTiO3.

The dielectric response to infrared waves polarized along the tetragonal axis of a ferroelectric single-domain crystal of BaTiO3 was determined by time-domain THz spectroscopy and Fourier-transform infrared reflectivity techniques. In addition to the three well-known polar lattice modes, the experiment shows an additional mode of the relaxation type in the THz spectral region, which accounts for the Curie-Weiss behavior of the c-axis dielectric constant. A comparison of experimental results with ab initio based effective-Hamiltonian simulations allows us to elucidate its relation to the order-disorder model of Comes, Lambert, and Guinier [Solid State Commun. 6, 715 (1968)10.1016/0038-1098(68)90571-1].

Ultrafast far-infrared dynamics probed by terahertz pulses: a frequency-domain approach. II. Applications.

We present data obtained by time-resolved terahertz spectroscopy in selected semiconducting and molecular systems exhibiting subpicosecond far-infrared dynamics. We use a frequency-domain method which eliminates the influence of instrumental functions and artifacts due to frequency mixing and yields a two-dimensional transient conductivity of the photoexcited sample. This technique enables improving the attainable experimental time resolution and allows a simple qualitative interpretation of the results without a priori modeling. The quantitative interpretation is based on the time-dependent Drude and damped harmonic oscillator models.