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Relaxor ferrolectrics are important in technological applications due to a strong electromechanical response, energy storage capacity, electrocaloric effect, and pyroelectric energy conversion properties. Current efforts to discover and design new materials in this class generally rely on substitutional doping of known ferroelectrics, as slight changes to local compositional order can significantly affect the Curie temperature, morphotropic phase boundary, and electromechanical responses. In this work, we demonstrate that moving to the strong limit of compositional complexity in an ABO3 perovskite allows stabilization of novel relaxor responses that do not rely on a single narrow phase transition region. Entropy-assisted synthesis approaches are used to create single crystal Ba(Ti0.2Sn0.2Zr0.2Hf0.2Nb0.2)O3 [Ba(5B)O] films. The high levels of configurational disorder present in this system is found to influence dielectric relaxation, phase transitions, nano-polar domain formation, and Curie temperature. Temperature-dependent dielectric, Raman spectroscopy and second-harmonic generation measurements reveal multiple phase transitions, a high Curie temperature of 570 K, and the relaxor ferroelectric nature of Ba(5B)O films. The first principles theory calculations are used to predict possible combinations of cations to quantify the relative feasibility of formation of highly disordered single-phase perovskite systems. The ability to stabilize single-phase perovskites with such a large number of different cations on the B-sites offers new possibilities for designing high-performance materials for piezoelectric, pyroelectric and tunable dielectric applications.
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Relaxor ferroelectrics are difficult to study and understand. The experiment shows that at low energy scattering there is an acoustic mode, an optic mode, dynamic quasi-elastic scattering and strictly elastic scattering as well as Bragg peaks at the zone centre. We have studied the scattering using the TASP spectrometer at PSI and have analysed the data using a model with interactions between the different components particularly to determine the properties of the elastic scattering. The quasi-elastic scattering begins to become significant at the Burns temperature of 620 K. It steadily increases in intensity on cooling reaching a maximum at ~400 K. Below this temperature the strictly elastic scattering begins to increase and shows a broadened line shape characteristic of crystals in a random applied field. We show that all the results obtained from PMN for the elastic scattering are consistent with the crystal having a random field transition at ~400 K. We have obtained similar results for PMN-PT and PZN-PT suggesting that random fields of the nano-regions also play an important role in these materials.
Relaxor ferroelectrics, which can exhibit exceptional electromechanical coupling are some of the most important functional materials with applications ranging from ultrasound imaging to actuators and sensors in microelectromechanical devices. Since their discovery nearly 60 years ago, the complexity of nanoscale chemical and structural heterogeneity in these systems has made understanding the origins of their unique electromechanical properties a seemingly intractable problem. A full accounting of the mechanisms that connect local structure and chemistry with nanoscale fluctuations in polarization has, however, remained a need and a challenge. Here, we employ aberration-corrected scanning transmission electron microscopy (STEM) to quantify various types of nanoscale heterogeneity and their connection to local polarization in the prototypical relaxor ferroelectric system Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$-PbTiO3 (PMN-PT). We identify three main contributions that each depend on Ti content: chemical order, oxygen octahedral tilt, and oxygen octahedral distortion. These heterogeneities are found to be spatially correlated with low angle polar domain walls, indicating their role in disrupting long-range polarization. Specifically, these heterogeneities lead to nanoscale domain formation and the relaxor response. We further locate nanoscale regions of monoclinic distortion that correlate directly with Ti content and the electromechanical performance. Through this approach, the elusive connection between chemical heterogeneity, structural heterogeneity and local polarization is revealed, and the results validate models needed to develop the next generation of relaxor ferroelectric materials.
Neutron and x-ray scattering studies on relaxor ferroelectric systems Pb(Zn$_{1/3}$Nb$_{2/3}$)O$_3$ (PZN), Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_3$ (PMN), and their solid solutions with PbTiO$_3$ (PT) have shown that inhomogeneities and disorder play important roles in the materials properties. Although a long-range polar order can be established at low temperature - sometimes with the help of an external electric field; short-range local structures called the ``polar nano-regions (PNR) still persist. Both the bulk structure and the PNR have been studied in details. The coexistence and competition of long- and short-range polar orders and how they affect the structural and dynamical properties of relaxor materials are discussed.
The conductive domain wall (CDW) is extensively investigated in ferroelectrics, which can be considered as a quasi-two-dimensional reconfigurable conducting channel embedded into an insulating material. Therefore, it is highly important for the application of ferroelectric nanoelectronics. Hitherto, most CDW investigations are restricted in oxides, and limited work has been reported in non-oxides to the contrary. Here, by successfully synthesizing the non-oxide ferroelectric Sn2P2S6 single crystal, we observed and confirmed the domain wall conductivity by using different scanning probe techniques which origins from the nature of inclined domain walls. Moreover, the domains separated by CDW also exhibit distinguishable electrical conductivity due to the interfacial polarization charge with opposite signs. The result provides a novel platform for understanding electrical conductivity behavior of the domains and domain walls in non-oxide ferroelectrics.
We report for the first time the magnetic structure of the high entropy oxide $(Mg_{0.2}Co_{0.2}Ni_{0.2}Cu_{0.2}Zn_{0.2})O$ using neutron powder diffraction. This material exhibits a sluggish magnetic transition but possesses a long-range ordered antiferromagnetic ground state, as revealed by DC and AC magnetic susceptibility, elastic and inelastic neutron scattering measurements. The magnetic propagation wavevector is k=(1/2, 1/2, 1/2) based on the cubic structure Fm-3m, and the magnetic structure consists of ferromagnetic sheets in the (111) planes with spins antiparallel between two neighboring planes. Inelastic neutron scattering reveals strong magnetic excitations at 100 K that survive up to room temperature. This work demonstrates that entropy-stabilized oxides represent a unique platform to study long range magnetic order with extreme chemical disorder.
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