Visualization of dielectric constant-electric field-temperature phase maps for imprinted relaxor ferroelectric thin films

Frederick, J.; Kim, T. H.; Maeng, W. J.; Brewer, A.; Podkaminer, Jacob; Saenrang, Wittawat; Vaithyanathan, V.; Li, F.; Chen, Lei; Schlom, Darrell G.; Trolier-McKinstry, Susan; Rzchowski, M. S.; Eom, C. B.

doi:10.1063/1.4944774

Cited by 8 publications

(4 citation statements)

References 30 publications

(29 reference statements)

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“…A small DC bias, corresponding to the average of the field at which the capacitance is maximum during sweep-up and sweepdown in C-V measurements ( Figure S7, Supporting Information) was applied to compensate for the imprint during the temperaturedependent dielectric constant measurement. [44] Room-temperature polarization-electric field hysteresis loops were measured at a frequency of 10 kHz using a Precision Multiferroic tester (Radiant Technologies). Room-temperature displacement-voltage bipolar hysteresis loops were measure at a frequency of 0.2 Hz via piezoresponse force microscopy using a MFP-3D (Asylum Research).…”

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confidence: 99%

Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution

Kim

Takenaka

et al. 2019

Advanced Materials

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Alternatively, molecular-dynamics (MD) simulations have shown that relaxors can be interpreted as exhibiting a multidomain state without a nonpolar matrix (i.e., polar nanodomains or PNDs). [4] The exact nature of order in relaxors, however, remains an ongoing debate [5] and, in turn, new approaches to study these complex materials are required to further illuminate the structure and how it can be controlled and can impact material properties. [5-9] In any case, it is essential to understand the evolution of the polar structure in relaxors (be they PNRs or PNDs) under applied stimuli as these are key to understanding relaxor behavior and large electromechanical effects in relaxors. Over the years, X-ray and neutron diffuse-scattering measurements have emerged as an essential tool to study the structural signatures of relaxor behavior [10-19] and studies on single-crystal relaxors have investigated the evolution of polar regions/domains (e.g., size, morphology) and suggested that they alter their size [14-17] and orientation [18] under different external stimuli. For example, under applied electric fields, which were expected to enhance polar order, the local order was found to align perpendicular to the field [18] and induce an asymmetry in the lattice dynamics [19] that could ultimately be responsible for the large electromechanical effects. [20] Other studies used pressure to push the material in the opposite directionto destabilize polar order [17]-and even induce a crossover from Understanding and ultimately controlling the large electromechanical effects in relaxor ferroelectrics requires intimate knowledge of how the local-polar order evolves under applied stimuli. Here, the biaxial-strain-induced evolution of and correlations between polar structures and properties in epitaxial films of the prototypical relaxor ferroelectric 0.68PbMg 1/3 Nb 2/3 O 3-0.32PbTiO 3 are investigated. X-ray diffuse-scattering studies reveal an evolution from a butterfly-to disc-shaped pattern and an increase in the correlation-length from ≈8 to ≈25 nm with increasing compressive strain. Molecular-dynamics simulations reveal the origin of the changes in the diffuse-scattering patterns and that strain induces polarization rotation and the merging of the polar order. As the magnitude of the strain is increased, relaxor behavior is gradually suppressed but is not fully quenched. Analysis of the dynamic evolution of dipole alignment in the simulations reveals that, while, for most unit-cell chemistries and configurations, strain drives a tendency toward more ferroelectric-like order, there are certain unit cells that become more disordered under strain, resulting in stronger competition between ordered and disordered regions and enhanced overall susceptibilities. Ultimately, this implies that deterministic creation of specific local chemical configurations could be an effective way to enhance relaxor performance.

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confidence: 99%

Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution

Kim

Takenaka

et al. 2019

Advanced Materials

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“…To study the impact of the induced defects on the relaxor behavior, we probed the evolution of the dielectric response as a function of ion dose (see Supplemental Material for details [21], which includes Ref. [25]). Dielectric permittivity studies as a function of frequency [ Fig.…”

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confidence: 99%

Defect-Induced (Dis)Order in Relaxor Ferroelectric Thin Films

et al. 2019

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The effect of intrinsic point defects on relaxor properties of 0.68 PbMg 1=3 Nb 2=3 O 3-0.32 PbTiO 3 thin films is studied across nearly 2 orders of magnitude of defect concentration via ex post facto ion bombardment. A weakening of the relaxor character is observed with increasing concentration of bombardment-induced point defects, which is hypothesized to be related to strong interactions between defect dipoles and the polarization. Although more defects and structural disorder are introduced in the system as a result of ion bombardment, the special type of defects that are likely to form in these polar materials (i.e., defect dipoles) can stabilize the direction of polarization against thermal fluctuations, and in turn, weaken relaxor behavior.

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“…[77,78] In the presence of an internal field, ferroelectric hysteresis loops were biased (asymmetric), that is, imprint (the lateral shift of a polarization-electric field hysteresis loop) was observed. [80,81] A large variety of device performances of ferroelectric capacitors have been directly associated with the imprint failure such as polarization fatigue, [82,83] retention loss, [83][84][85][86] polarization back-switching, [87][88][89][90] dielectric relaxation behaviors, [91][92][93] and increased leakage currents. [59,84] In particular, for imprinted ferroelectric capacitors, the ferroelectric polarization was spontaneously self-poled even in the pristine state.…”

Section: Interfacial Schottky Barrier and Asymmetric Electrodesmentioning

confidence: 99%

Polar Perturbations in Functional Oxide Heterostructures

Wang

Lee

et al. 2023

Adv Funct Materials

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Growth and characterization of metal‐oxide thin films foster successful development of oxide‐material‐integrated thin‐film devices represented by metal‐oxide‐semiconductor field‐effect transistors (MOSFET), drawing enormous technological and scientific interest for several decades. In recent years, functional oxide heterostructures have demonstrated remarkable achievements in modern technologies and provided deeper insights into condensed‐matter physics and materials science owing to their versatile tunability and selective amplification of the functionalities. One of the most critical aspects of their physical properties is the polar perturbation stemming from the ionic framework of an oxide. By engineering and exploiting the structural, electrical, magnetic, and optical characteristics through various routes, numerous perceptive studies have clearly shown how polar perturbations advance functionalities or drive exotic physical phenomena in complex oxide heterostructures. In this review, both intrinsic (engraved by thin‐film heteroepitaxy) and extrinsic (reversibly controllable defect‐mediated disorder and polar adsorbates) elements of polar perturbations, highlighting their abilities for the development of highly tunable functional properties are summarized. Scientifically, the recent approaches of polar perturbations render one to consolidate a prospect of atomic‐level manipulation of polar order in epitaxial oxide thin films. Technologically, this review also offers useful guidelines for rational design to heterogeneously integrated oxide‐based multi‐functional devices with high performances.

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Visualization of dielectric constant-electric field-temperature phase maps for imprinted relaxor ferroelectric thin films

Cited by 8 publications

References 30 publications

Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution

Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution

Defect-Induced (Dis)Order in Relaxor Ferroelectric Thin Films

Polar Perturbations in Functional Oxide Heterostructures

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