The role of lattice dynamics in ferroelectric switching

Shi, Qiwu; Parsonnet, Eric; Cheng, Xiaoxing; Fedorova, Natalya S.; Peng, Ren‐Ci; Fernández, Abel; Qualls, Alexander; Huang, Xiaoxi; Chang, Xue; Zhang, Hongrui; Pesquera, David; Das, Sujit; Nikonov, Dmitri E.; Young, Ian A.; Chen, Lei; Martin, Lane W.; Huang, Yen-Lin; Íñiguez, Jorgé; Ramesh, R.

doi:10.1038/s41467-022-28622-z

Cited by 37 publications

(25 citation statements)

References 61 publications

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“…In particular, it has been shown that deposition of La 1−x Sr x MnO 3 via pulsed-laser deposition in low partial pressures of oxygen can drive high defect densities which allow coherent deposition of films to commercially available oxide substrates from LaAlO 3 (pseudocubic lattice parameter of 3.78 Å) to NdScO 3 (4.00 Å) [103]. As such, this has enabled the deposition of epitaxial films of large latticeparameter FEs including BaTiO 3 and 0.68PbMg 1/3 Nb 2/3 O 3 -0.32PbTiO 3 [102], in addition to PbZr 0.2 Ti 0.8 O 3 (PZT) [101] and BiFeO 3 [104].…”

Section: Chemical Lift-offmentioning

confidence: 99%

“…The substrate clamping effect has been extensively studied in FE films [194,195], as a limiting factor for their piezoresponse as well as for their poling ability, which plays a significant role in the thickness scalability of these materials and the energy required to activate polarization-switching processes. The role of the mechanical boundary conditions on the energetics and lattice dynamics of these systems was explored in detail in BaTiO 3 [102] and BiFeO 3 [104] capacitors fabricated on silicon after epitaxial lift-off and transfer. These works revealed how the removal of substrate bonding strongly alters the FE switching paths by facilitating structural distortions upon voltage application that were restricted by the substrate-imposed mechanical constraint.…”

Section: Improved Performance In Transferred Devicesmentioning

confidence: 99%

“…The propagation of lattice vibrations in a solid depends on the elastic properties of the medium, as well as its boundary conditions. Measuring phonon dispersion relations would provide relevant insights into the lattice dynamics of freestanding-complex oxides, fundamental to understand their improved FE switching speeds [104] and explore photoinduced effects [203] or the role of microstructure and size scaling on functional properties [56,58]. Time-resolved structural evolution upon application of an external field could be obtained using pump-probe techniques such as ultrafast electron diffraction which, although not suitable for epitaxial films on substrates, would be able to provide a complete picture of the structural dynamics of freestanding membranes in the femtosecond regime [204].…”

Section: Lattice Dynamicsmentioning

confidence: 99%

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Freestanding complex-oxide membranes

Pesquera

Fernández

Khestanova

et al. 2022

J. Phys.: Condens. Matter

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Complex oxides show a vast range of functional responses, unparalleled within the inorganic solids realm, making them promising materials for applications as varied as next-generation field-effect transistors, spintronics, electro-optic modulators, pyroelectric detectors, or oxygen reduction catalysts. Their stability in ambient conditions, chemical versatility, and large susceptibility to minute structural and electronic modifications make them ideal subjects of study to discover emergent phenomena and to generate novel functionalities for next-generation devices. Recent advances in the synthesis of single-crystal, freestanding complex oxide membranes provide an unprecedented opportunity to study these materials in a nearly-ideal system (e.g., free of mechanical/thermal interaction with substrates) as well as expanding the range of tools for tweaking their order parameters (i.e., (anti-)ferromagnetic, (anti-)ferroelectric, ferroelastic), and increasing the possibility of achieving novel heterointegration approaches (including interfacing dissimilar materials) by avoiding the chemical, structural, or thermal constraints in synthesis processes. Here, we review the recent developments in the fabrication and characterization of complex-oxide membranes and discuss their potential for unraveling novel physicochemical phenomena at the nanoscale and for futher exploiting their functionalities in technologically relevant devices.

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Section: Chemical Lift-offmentioning

confidence: 99%

Section: Improved Performance In Transferred Devicesmentioning

confidence: 99%

Section: Lattice Dynamicsmentioning

confidence: 99%

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Freestanding complex-oxide membranes

Pesquera

Fernández

Khestanova

et al. 2022

J. Phys.: Condens. Matter

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“…Aside from providing further methods of strain control, it was found that the freestanding membranes had markedly increased switching speeds and reduced coercive fields, pointing to the significant role that elastic constraints can play in ferroelectric switching processes and warranting further study. [ 246 ] Utilizing freestanding membranes of oxide ferroelectrics is still in its infancy, and researchers are envisioning new experiments in hybrid epitaxy to combine perovskite and nonperovskite layers to achieve new ferroic coupling, for example, magnetoelectric coupling, [ 247 ] as well as novel Moire pattern physics in oxide systems. [ 248 ]…”

Section: Advanced Epitaxy and Beyondmentioning

confidence: 99%

Thin‐Film Ferroelectrics

et al. 2022

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non-centrosymmetric structures which can possess a spontaneous electric polarization which can be controlled using applied electric fields (Figure 1). Ferroelectrics themselves are inherently hierarchical materials-wherein picometer ionic displacements give rise to polarization which can collectively extend over millimeters or self-organize into complex mesoscopic structures or collectively reorient under applied stimuli (e.g., electric fields, temperature, or stress). Understanding these complex behaviors necessitates a multilevel approach, wherein atomistic, microscopic, mesoscopic, and macroscopic properties are studied in concert. Parallel advances in synthesis, characterization, and simulation have enabled such multimodal studies and provided a methodology through which a multitude of ferroelectric functionalities can now be achieved and studied.The promise of utilizing these functionalities in a number of applications kick-started the modern era of ferroelectric research in the mid-20th century. [1] Looking further back, in the 1920s, the ability to switch the polarization of sodium potassium tartrate tetrahydrate (commonly known as Rochelle salt) was first observed, along with dielectric and piezoelectric anomalies near the ferroelectric transition-now called the Curie point. In the 1940s, as part of the accelerated research push associated with World War II, ferroelectric BaTiO 3 was discovered by accident. When modifying TiO 2 with BaO to enhance its dielectric properties, a record-high dielectric permittivity was discovered and subsequent studies demonstrated a hysteretic switchable polarization. This discovery ushered in a new understanding of ferroelectricity as more than a rare phenomenon associated with salts that contained hydrogen bonding, but rather as a phenomenon that could exist in simple oxides like perovskites. Over the subsequent decades, the number of ferroelectric compositions exploded, particularly within the perovskite oxides, introducing new chemistries including LiNbO 3 and the PbZr x Ti 1−x O 3 system. Meanwhile, theoretical descriptions of ferroelectricity were advanced through lattice-dynamical models invoking a soft-mode optical phonon. Studies of the piezoelectric, thermodynamic, and optical properties in ferroelectric ceramics allowed for their deployment in a number of applications including piezoelectric sensors and pyroelectric infrared detectors. By the 1960s, increased interest in using ferroelectric polarization for nonvolatile memory was driving research into Over the last 30 years, the study of ferroelectric oxides has been revolutionized by the implementation of epitaxial-thin-film-based studies, which have driven many advances in the understanding of ferroelectric physics and the realization of novel polar structures and functionalities. New questions have motivated the development of advanced synthesis, characterization, and simulations of epitaxial thin films and, in turn, have provided new insights and applications across the micro-, meso-, and macroscopic length sc...

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“…For three-dimensional compounds there has been a vivid search for new ferroelectrics with optimal properties. For example with respect to lead-free energy storage materials [33] or low switching barriers for memory applications [34]. To this end, high throughput DFT calculations has proven a powerful strategy that can be used to rapidly screen thousands of materials for desired properties.…”

Section: Introductionmentioning

confidence: 99%