The relationship between halogen content and the elastic/vibrational properties of MAPbBr_3−xCl_x mixed crystals (x = 1.5, 2, 2.5, and 3) with MA = CH₃NH₃⁺ has been studied using Brillouin and Raman spectroscopy at room temperature. The longitudinal and transverse sound velocities, the absorption coefficients and the two elastic constants C₁₁ and C₄₄ could be obtained and compared for the four mixed-halide perovskites. In particular, the elastic constants of the mixed crystals have been determined for the first time. A quasi-linear increase in the sound velocity and the elastic constant C₁₁ with increasing chlorine content was observed for the longitudinal acoustic waves. C₄₄ was insensitive to the Cl content and very low, indicating a low elasticity to shear stress in mixed perovskites regardless of the Cl content. The acoustic absorption of the LA mode increased with increasing heterogeneity in the mixed system, especially for the intermediate composition where the Br and Cl ratio was 1:1. In addition, a significant decrease in the Raman-mode frequency of the low-frequency lattice modes and the rotational and torsional modes of the MA cations was observed with decreasing Cl content. It clearly showed that the changes in the elastic properties as the halide composition changes were correlated with the lattice vibrations. The present findings may facilitate a deeper understanding of the complex interplay between halogen substitution, vibrational spectra and elastic properties, and may also pave the way for optimizing the operation of perovskite-based photovoltaic and optoelectronic devices by tailoring their chemical composition. Full article

Uniaxial ferroelectrics with tetragonal tungsten bronze structure are important functional materials with photorefractive, electrooptic, piezoelectric, and pyroelectric properties. Sr_xBa_1−xNb₂O₆ (SBN100x) with x > 50 is known as a typical uniaxial relaxor ferroelectric, while Ca_xBa_1−xNb₂O₆ (CBN100x) undergoes nearly normal ferroelectric phase transitions. Single crystals of CSBN100x = [x(CBN28) + (1 − x) (SBN61)] = xCa_0.28Ba_0.72Nb₂O₆ + (1 − x) Sr_0.61Ba_0.39Nb₂O₆ with nominal x = 0.00, 0.25, 0.50, 0.75, and 1.00 were studied to clarify the dynamical properties at the crossover from relaxor (x = 0) to normal (x = 1) ferroelectric behavior. The longitudinal acoustic (LA) and transverse acoustic (TA) modes and a central peak (CP) related to the relaxation process of polarization fluctuations along the polar c-axis were studied in uniaxial ferroelectric CSBN single crystals as a function of temperature via Brillouin scattering spectroscopy. A CBN28 (x = 1.00) crystal shows the sharp elastic anomaly of the LA mode in the gigahertz range toward Curie temperature, T_c. However, those of CSBN25 (x = 0.25) and SBN61 (x = 0.00) crystals show diffusive anomalies due to stronger random fields. The relaxation time determined from the width of a CP shows a critical slowing down in the vicinity of T_c. The elastic anomaly and slowing down of relaxation time of CSBN100x crystals become diffusive in the vicinity of T_c as the CBN28 content decreases. The origin of the crossover from relaxor to normal ferroelectric phase transitions is discussed in terms of the difference in the A1 and A2 sites’ occupancies. Full article

Brillouin scattering spectroscopy with diamond anvil cells was used by measuring the pressure dependence of the sound-relevant polymer material, glass-forming liquid, and H₂O (water and ice VII) velocities of the material from ambient pressure to 12 GPa at room temperature. Measurements of 20%, 10%, and 4% gelatin solutions were performed. For comparison purposes, we also measured the pressure dependence of the sound velocity of animal tissue up to 10 GPa. We analyzed the Brillouin data using the Tait and Vinet equations of state. We discussed the possible influence of frequency dispersion on bulk modulus at low pressure. We compared the elastic moduli obtained for gelatin to those of several other polymers. Full article

In this paper, the behavior of quasielastic light scattering (QELS) in a PbMg_1/3Nb_2/3O₃ (PMN) crystal under broadband Brillouin light scattering in a temperature range from 750 K to 80 K was studied. It was shown that QELS consists of two components: narrow (0.9 GHz to 11 GHz) and wide (80 GHz to 600 GHz). The dependencies of the intensity, I, of these components on the frequency, ν, are well described by the power law I ~ eν^α, with different α, and are determined by the distribution of the relaxation times. The analysis of the Brillouin spectra showed that the behavior of the relaxation time of both the components of QELS with temperature change is well described by the Arrhenius law. Additionally, in the vicinity of the intermediate temperature T* ≈ 380 K, a critical relaxation time behavior for the narrow component of QELS was detected. In the vicinity of the same temperature, a maximum in the integral intensity of both the components of QELS was observed, which is adjacent to another maximum in the region of the Vogel–Fulcher temperature T_VF ≈ 250 K corresponding to the transformation of the crystal to a nonergodic state. Full article

Three-dimensional direct laser writing technology enables one to print polymer microstructures whose size varies from a few hundred nanometers to a few millimeters. It has been shown that, by tuning the laser power during writing, one can adjust continuously the optical and elastic properties with the same base material. This process is referred to as gray-tone lithography. In this paper, we characterize by Brillouin light scattering the complex elastic constant $C_{11}$ of different reticulated isotropic polymers, at longitudinal phonon frequencies of the order of 16 GHz. We estimate the real part of the $C_{11}$ constant to vary from 7 to 11 GPa as a function of laser power, whereas its imaginary part varies between 0.25 and 0.6 GPa. The linear elastic properties are further measured at a fixed laser power as a function of temperature, from $20{}^{\circ }$C to $80{}^{\circ }$C. Overall, we show that our 3D printed samples have a good elastic quality with high Q factors only ten times smaller than fused silica at hypersonic frequencies. Full article

Inelastic light scattering spectra of organic–inorganic halide perovskite MAPbCl₃ single crystals were investigated by using Brillouin spectroscopy. Sound velocities and acoustic absorption coefficients of longitudinal and transverse acoustic modes propagating along the cubic [100] direction were determined in a wide temperature range. The sound velocities exhibited softening upon cooling in the cubic phase, which was accompanied by the increasing acoustic damping. The obtained relaxation time showed a critical slowing-down behavior, revealing the order–disorder nature of the phase transition, which is consistent with the growth of strong central peaks upon cooling toward the phase transition point. The temperature dependences of the two elastic constants C₁₁ and C₄₄ were obtained in the cubic phase for the first time. The comparison of C₁₁ and C₄₄ with those of other halide perovskites showed that C₁₁ of MAPbCl₃ is larger and C₄₄ is slightly smaller compared to the values of MAPbBr₃ and MAPbI₃. It suggests that MAPbCl₃ has a more compact structure (smaller lattice constant) along with stronger binding forces, causing larger C₁₁ and bulk modulus in this compound, and that the shear rigidity is exceedingly small similar to other halide perovskites. The reported elastic constants in this study may serve as a testbed for theoretical and calculational approaches for MAPbCl₃. Full article

Brillouin light scattering (BLS) has been established as a standard technique to study thermally excited sound waves with frequencies up to ~100 GHz in transparent materials. In BLS experiments, one usually uses a Fabry–Pérot interferometer (FPI) as a spectrometer. The drastic improvement of the FPI contrast factor over 10¹⁰ by the development of the multipass type and the tandem multipass type FPIs opened a gateway to investigate low energy excitations (ħω ≤ 1 meV) in various research fields of condensed matter physics, including surface acoustic waves and spin waves from opaque surfaces. Over the last four decades, the BLS technique has been successfully applied to study collective spin waves (SWs) in various types of magnetic structures including thin films, ultrathin films, multilayers, superlattices, and artificially arranged dots and wires using high-contrast FPIs. Now, the BLS technique has been fully established as a unique and powerful technique not only for determination of the basic magnetic constants, including the gyromagnetic ratio, the magnetic anisotropy constants, the magnetization, the SW stiffness constant, and other features of various magnetic materials and structures, but also for investigations into coupling phenomena and surface and interface phenomena in artificial magnetic structures. BLS investigations on the Fe/Cr multilayers, which exhibit ferromagnetic-antiferromagnetic arrangements of the adjacent Fe layer’s magnetizations depending on the Cr layer’s thickness, played an important role to open the new field known as “spintronics” through the discovery of the giant magnetoresistance (GMR) effect. In this review, I briefly surveyed the historical development of SW studies using the BLS technique and theoretical background, and I concentrated our BLS SW studies performed at Tohoku University and Ishinomaki Senshu University over the last thirty five years. In addition to the ferromagnetic SW studies, the BLS technique can be also applied to investigations of high-frequency magnetization dynamics in superparamagnetic (SPM) nanogranular films in the frequency domain above 10 GHz. One can excite dipole-coupled SPM excitations under external magnetic fields and observe them via the BLS technique. The external field strength determines the SPM excitations’ frequencies. By performing a numerical analysis of the BLS spectrum as a function of the external magnetic field and temperature, one can investigate the high-frequency magnetization dynamics in the SPM state and determine the magnetization relaxation parameters. Full article

The functionality enhancement of ferroelectrics by local polar clusters called polar nanoregions (PNRs) is one of the current interests in materials science. KTa_1−xNb_xO₃ (KTN) with perovskite structure is a well-known electro-optic crystal with a large Kerr effect. The existence of PNRs in relaxor-like ferroelectric Nb-rich KTN with homovalent B-site cations is controversial. This paper reviews recent progress in understanding precursor dynamics in Nb-rich KTN crystals studied using Brillouin scattering. The intense central peak (CP) and significant softening of sound velocity are observed above the Curie temperature (T_C) due to the polarization fluctuations in PNRs. The effects of Li-doping, defects, and electric fields on the growth and/or creation of PNRs are found using changes in acoustic properties. The electric-field-induced T_C, which is shifted to higher values with increases in applied voltage, including critical endpoint (CEP) and field gradient by trapped electrons, are discussed as well. This new knowledge may give new insight into advanced functionality in perovskite ferroelectrics. Full article

Compositionally disordered perovskite compounds have been one of the exotic topics of research during the past several years. Colossal piezoelectric and electrostrictive effects have been observed in disordered perovskite ferroelectric materials. The key ingredient in the physical behavior of disordered perovskites is the nucleation and growth of the local dipolar regions called polar nanoregions (PNRs). PNRs begin to nucleate far above the temperature of the dielectric maximum T_m and exhibit varied relaxation behavior with temperature. The evidence for the existence of various stages in the relaxation dynamics of PNRs was revealed through the study of the temperature evolution of optical phonons by Raman scattering. The quasi-static regime of PNRs is characterized by the strong coupling between the local polarization and strain with the local structural phase transition and the critical slowing of the relaxation time. Strong anomalies in the frequency and the width of the acoustic phonons, and emergence of the central peak in the quasi-static region of the relaxation dynamics of PNRs have been observed through Brillouin scattering studies. In this review, we discuss the anomalies observed in Brillouin scattering in selected disordered perovskite ferroelectrics crystals such as Pb(Mg_1/3Ta_2/3)O_3, Pb(Sc_1/2Ta_1/2)O₃, 0.65PIN-0.35PT and Sr_0.97Ca_0.03TiO₃ to understand dynamical behavior of PNRs. Full article

Perovskite oxides with the general formula ABO₃ comprise a large number of families among the structures of oxide-based materials, and currently, several perovskite structures have been identified. From a variety of compositions and structures, various functions are observed in perovskite compounds, and therefore, they became very useful for various applications in the electronic and medical industries. One of the most puzzling issues for perovskite compounds is the understanding of the vibration and relaxation dynamics in the gigahertz range. In that sense, the micro-Brillouin scattering system is a very effective tool to probe the gigahertz dynamics, and also, first-principles calculations can be used to describe the phonon structure with different atomic contributions. The micro-Brillouin scattering system and first-principles calculations provide the fundamental information on a variety of vibration and relaxation processes related to structural phase transitions under different external conditions such as temperature, electric field, and pressure. This review article summarizes the Brillouin scattering and first-principles studies on BaMO₃ (M = Ti, Zr, and Cu). Through a detailed analysis of the existing results, we summarize the existing limitations and future perspectives in these research areas, which may propel the development of different perovskite ferroelectrics and extend their practical application areas. Full article

L. Brillouin predicted inelastic light scattering by thermally excited sound waves in 1922. Brillouin scattering is a non-contact and non-destructive method to measure sound velocity and attenuation. It is possible to investigate the elastic properties of gases, liquids, glasses, and crystals. Various kinds of phase transitions, i.e., liquid–glass transitions, crystallization, polymorphism, and denaturation have been studied by changing the temperature, pressure, time, and external fields such as the electric, magnetic, and stress fields. Nowadays, Brillouin scattering is extensively used to measure various elementary excitations and quasi-elastic scattering in the gigahertz range between 0.1 and 1000 GHz. A brief history, spectroscopic methods, and Brillouin scattering studies in materials science on ferroelectric materials, glasses, and proteins are reviewed. Full article