An official website of the United States government
Abstract The understanding of domain dynamics in ferroelectric materials is crucial for optimizing their performance in piezoelectric and electro‐optic applications. Although previous studies have focused on static domain structures and macroscopic characteristics, the time‐resolved approach of domains remains largely unexplored. In this study, we compare the dynamic responses of direct current (DC) and alternating current (AC) poled [001]‐oriented rhombohedral Pb(Mg1/3Nb2/3)O3–PbTiO3(PMN–PT) single crystals using X‐ray photon correlation spectroscopy (XPCS) during the application of external electric fields. Our results demonstrate that the AC‐poled sample exhibit enhanced reconfiguration of domain variants in response to driving fields compared to the DC‐poled counterpart, as evidenced by accelerated correlation decay and faster relaxation time. This phenomenon is attributed to enhanced reversible domain wall motion achieved through AC poling, which facilitates field‐induced domain realignment. These findings provide insight into the relationship between dynamics and macroscopic properties in relaxor‐PT single crystals for high‐performance applications.
more »
« less
Connecting the Multiscale Structure with Macroscopic Response of Relaxor Ferroelectrics
Abstract Lead‐based relaxor ferroelectrics are characterized by outstanding piezoelectric and dielectric properties, making them useful in a wide range of applications. Despite the numerous models proposed to describe the relation between their nanoscale polar structure and the large properties, the multiple contributions to these properties are not yet revealed. Here, by combining atomistic and mesoscopic‐scale structural analyses with macroscopic piezoelectric and dielectric measurements across the (100–x)Pb(Mg1/3Nb2/3)O3–xPbTiO3(PMN–xPT) phase diagram, a direct link is established between the multiscale structure and the large nonlinear macroscopic response observed in the monoclinic PMN‐xPT compositions. The approach reveals a previously unrecognized softening effect, which is common to Pb‐based relaxor ferroelectrics and arises from the displacements of low‐angle nanodomain walls, facilitated by the nanoscale polar character and lattice strain disorder. This comprehensive comparative study points to the multiple, distinct mechanisms that are responsible for the large piezoelectric response in relaxor ferroelectrics.
more »
« less
- Award ID(s):
- 1633587
- PAR ID:
- 10452833
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Functional Materials
- Volume:
- 30
- Issue:
- 52
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Acting like thermal resistances, ferroelectric domain walls can be manipulated to realize dynamic modulation of thermal conductivity (k), which is essential for developing novel phononic circuits. Despite the interest, little attention has been paid to achieving room‐temperature thermal modulation in bulk materials due to challenges in obtaining a high thermal conductivity switching ratio (khigh/klow), particularly in commercially viable materials. Here, room‐temperature thermal modulation in 2.5 mm‐thick Pb(Mg1/3Nb2/3)O3–xPbTiO3(PMN–xPT) single crystals is demonstrated. With the use of advanced poling conditions, assisted by the systematic study on composition and orientation dependence of PMN–xPT, a range of thermal conductivity switching ratios with a maximum of ≈1.27 is observed. Simultaneous measurements of piezoelectric coefficient (d33) to characterize the poling state, domain wall density using polarized light microscopy (PLM), and birefringence change using quantitative PLM reveal that compared to the unpoled state, the domain wall density at intermediate poling states (0<d33<d33,max) is lower due to the enlargement in domain size. At optimized poling conditions (d33,max), the domain sizes show increased inhomogeneity that leads to enhancement in the domain wall density. This work highlights the potential of commercially available PMN–xPT single crystals among other relaxor‐ferroelectrics for achieving temperature control in solid‐state devices.more » « less
-
Understanding the microscopic origin of the superior electromechanical response in relaxor ferroelectrics requires knowledge not only of the atomic-scale formation of polar nanodomains (PNDs) but also the rules governing the arrangements and stimulated response of PNDs over longer distances. Using x-ray coherent nanodiffraction, we show the staggered self-assembly of PNDs into unidirectional mesostructures that we refer to as polar laminates in the relaxor ferroelectric 0.68PbMg1/3Nb2/3O3-0.32PbTiO3(PMN-0.32PT). We reveal the highly heterogeneous electric-field–driven responses of intra- and interlaminate PNDs and establish their correlation with the local strain and the nature of the PND walls. Our observations highlight the critical role of hierarchical lattice organizations on macroscopic material properties and provide guiding principles for the understanding and design of relaxors and a wide range of quantum and functional materials.more » « less
-
Polar nanoregions (PNRs) are believed to play a decisive role in the local and macroscopic polarization in relaxor ferroelectrics. The limited microscopic understanding of the structure and dynamics of PNRs hampers the rational design of new lead-free materials. Here, the local structure of A-site disordered Bi 0.5 K 0.5 TiO 3 (BKT) is investigated using synchrotron x-ray and neutron pair distribution function (PDF) analysis and density functional theory (DFT) optimized special quasirandom structures (SQSs). DFT-relaxed SQS with a 4 × 4 × 4 supercell size can reproduce the experimental PDFs of disordered BKT, as well as the partial PDFs and total polarization, with comparable results to those reported from a combined analysis of x-ray and neutron PDF data with large-box reverse Monte Carlo methods. We find that small Bi 3+ -rich polar clusters are likely to be the microscopic origin of relaxor behavior in disordered BKT, and that the existence of large polar nanoregions (PNRs) is not necessary to explain the relaxor properties. Our results also highlight the great potential of the SQS approach to gain a nanoscale-to-microscopic understanding of other relaxor solid solutions.more » « less
-
Abstract The local compositional heterogeneity associated with the short‐range ordering of Mg and Nb in PbMg1/3Nb2/3O3(PMN) is correlated with its characteristic relaxor ferroelectric behavior. Fully ordered PMN is not prepared as a bulk material. This work examines the relaxor behavior in PMN thin films grown at temperatures below 1073 K by artificially reducing the degree of disorder via synthesis of heterostructures with alternate layers of Pb(Mg2/3Nb1/3)O3and PbNbO3, as suggested by the random‐site model. 100 nm thick, phase‐pure films are grown epitaxially on (111) SrTiO3substrates using alternate target timed pulsed‐laser deposition of Pb(Mg2/3Nb1/3)O3and PbNbO3targets with 20% excess Pb. Selected area electron diffraction confirms the emergence of (1/2, 1/2, 1/2) superlattice spots with randomly distributed ordered domains as large as ≈150 nm. These heterostructures exhibit a dielectric constant of 800, loss tangents of ≈0.03 and 2× remanent polarization of ≈11 µC cm−2at room temperature. Polarization–electric field hysteresis loops, Rayleigh data, and optical second‐harmonic generation measurements are consistent with the development of ferroelectric domains below 140 K. Temperature‐dependent permittivity measurements demonstrate reduced frequency dispersion compared to short range ordered PMN films. This work suggests a continuum between normal and relaxor ferroelectric behavior in the engineered PMN thin films.more » « less
