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41 result(s) for "Nagarajan, Valanoor"
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Superior polarization retention through engineered domain wall pinning
Ferroelectric materials possess a spontaneous polarization that is switchable by an electric field. Robust retention of switched polarization is critical for non-volatile nanoelectronic devices based on ferroelectrics, however, these materials often suffer from polarization relaxation, typically within days to a few weeks. Here we exploit designer-defect-engineered epitaxial BiFeO 3 films to demonstrate polarization retention with virtually no degradation in switched nanoscale domains for periods longer than 1 year. This represents a more than 2000% improvement over the best values hitherto reported. Scanning probe microscopy-based dynamic switching measurements reveal a significantly increased activation field for domain wall movement. Atomic resolution scanning transmission electron microscopy indicates that nanoscale defect pockets pervade the entire film thickness. These defects act as highly efficient domain wall pinning centres, resulting in anomalous retention. Our findings demonstrate that defects can be exploited in a positive manner to solve reliability issues in ferroelectric films used in functional devices. The use of ferroelectric materials in memory device applications is held back by low retention times. Here, the authors demonstrate that by intentionally introducing defective nanoregions which increase the activation field for domain wall motion, retention times larger than a year can be achieved.
Deterministic optical control of room temperature multiferroicity in BiFeO3 thin films
Controlling ferroic orders (ferroelectricity, ferromagnetism and ferroelasticity) by optical methods is a significant challenge due to the large mismatch in energy scales between the order parameter coupling strengths and the incident photons. Here, we demonstrate an approach to manipulate multiple ferroic orders in an epitaxial mixed-phase BiFeO3 thin film at ambient temperature via laser illumination. Phase-field simulations indicate that a light-driven flexoelectric effect allows the targeted formation of ordered domains. We also achieved precise sequential laser writing and erasure of different domain patterns, which demonstrates a deterministic optical control of multiferroicity at room temperature. As ferroic orders directly influence susceptibility and conductivity in complex materials, our results not only shed light on the optical control of multiple functionalities, but also suggest possible developments for optoelectronics and related applications.The remote, non-volatile and reversible optical control of ferroic orders is challenging. Here, using laser illumination, multiple orders in epitaxial mixed-phase BiFeO3 are manipulated deterministically using a thermally driven flexoelectric effect.
Increase of power conversion efficiency in dye-sensitized solar cells through ferroelectric substrate induced charge transport enhancement
Ferroelectric functionalized dye-sensitized solar cells were fabricated by using a positively-poled LiNbO 3 substrate coated with ITO (ITO-LiNbO 3 ) as a collector electrode and demonstrated enhanced power conversion efficiency. Surface potential properties of TiO 2 nanoparticle film coated on the ITO-LiNbO 3 (TiO 2 /ITO-LiNbO 3 ) examined by Kelvin probe force microscopy (KPFM) confirmed that a large electric field (a few 10 V/µm) generated from LiNbO 3 can penetrate through the ITO layer and is applied to TiO 2 film. This polarization-induced electric field leads to an increased photocurrent density by attracting and promoting electrons to direct transport through the mesoporous TiO 2 network toward the collector electrode and a decreased charge recombination by facilitating electrons to pass through fewer boundaries of nanoparticles, resulting in high power conversion efficiency. The power conversion efficiency was enhanced by more than 40% in comparison with that without polarization-induced electric field. Incorporating functional ferroelectrics into photovoltaic cells would be a good strategy in improving photovoltaic performance and is applicable to other types of photovoltaic devices, such as perovskite solar cells.
Anisotropic epitaxial stabilization of a low-symmetry ferroelectric with enhanced electromechanical response
Piezoelectrics interconvert mechanical energy and electric charge and are widely used in actuators and sensors. The best performing materials are ferroelectrics at a morphotropic phase boundary, where several phases coexist. Switching between these phases by electric field produces a large electromechanical response. In ferroelectric BiFeO 3 , strain can create a morphotropic-phase-boundary-like phase mixture and thus generate large electric-field-dependent strains. However, this enhanced response occurs at localized, randomly positioned regions of the film. Here, we use epitaxial strain and orientation engineering in tandem—anisotropic epitaxy—to craft a low-symmetry phase of BiFeO 3 that acts as a structural bridge between the rhombohedral-like and tetragonal-like polymorphs. Interferometric displacement sensor measurements reveal that this phase has an enhanced piezoelectric coefficient of ×2.4 compared with typical rhombohedral-like BiFeO 3 . Band-excitation frequency response measurements and first-principles calculations provide evidence that this phase undergoes a transition to the tetragonal-like polymorph under electric field, generating an enhanced piezoelectric response throughout the film and associated field-induced reversible strains. These results offer a route to engineer thin-film piezoelectrics with improved functionalities, with broader perspectives for other functional oxides. Strain in thin films can increase piezoelectric properties, but crystallographic constraints may restrict the enhanced response to localized regions. Here, by combining strain and orientation engineering, a low-symmetry bridging phase of BiFeO 3 with enhanced piezoresponse is stabilized uniformly throughout the film.
Ferroelectric solitons crafted in epitaxial bismuth ferrite superlattices
In ferroelectrics, complex interactions among various degrees of freedom enable the condensation of topologically protected polarization textures. Known as ferroelectric solitons, these particle-like structures represent a new class of materials with promise for beyond-CMOS technologies due to their ultrafine size and sensitivity to external stimuli. Such polarization textures have scarcely been demonstrated in multiferroics. Here, we present evidence for ferroelectric solitons in (BiFeO 3 )/(SrTiO 3 ) superlattices. High-resolution piezoresponse force microscopy and Cs-corrected high-angle annular dark-field scanning transmission electron microscopy reveal a zoo of topologies, and polarization displacement mapping of planar specimens reveals center-convergent/divergent topological defects as small as 3 nm. Phase-field simulations verify that some of these structures can be classed as bimerons with a topological charge of ±1, and first-principles-based effective Hamiltonian computations show that the coexistence of such structures can lead to non-integer topological charges, a first observation in a BiFeO 3 -based system. Our results open new opportunities in multiferroic topotronics. Topological structures could spark promising functionalities in next generation nanoelectronics. Here, the authors report the realization of complex topological polar textures in epitaxial multiferroic BiFeO 3 –SrTiO 3 superlattices induced by competing electrical and mechanical boundary conditions.
Top-down patterning of topological surface and edge states using a focused ion beam
The conducting boundary states of topological insulators appear at an interface where the characteristic invariant ℤ 2 switches from 1 to 0. These states offer prospects for quantum electronics; however, a method is needed to spatially-control ℤ 2 to pattern conducting channels. It is shown that modifying Sb 2 Te 3 single-crystal surfaces with an ion beam switches the topological insulator into an amorphous state exhibiting negligible bulk and surface conductivity. This is attributed to a transition from ℤ 2  = 1 → ℤ 2  = 0 at a threshold disorder strength. This observation is supported by density functional theory and model Hamiltonian calculations. Here we show that this ion-beam treatment allows for inverse lithography to pattern arrays of topological surfaces, edges and corners which are the building blocks of topological electronics. Topological edge states offer the prospect of dissipationless transport for nanoelectronics, but a precise method to spatially engineer such nanoscale conducting channels is still lacking. Here, the authors demonstrate patterning of topological boundary states in Sb 2 Te 3 using a focused ion beam to create amorphous, topologically trivial regions.
Unit-cell scale mapping of ferroelectricity and tetragonality in epitaxial ultrathin ferroelectric films
Typically, polarization and strain in ferroelectric materials are coupled, leading to the generally accepted direct relation between polarization and unit-cell tetragonality. Here, by means of high-resolution transmission electron microscopy we map, on the unit-cell scale, the degree of tetragonality and the displacements of cations away from the centrosymmetry positions in an ultrathin epitaxial PbZr 0.2 Ti 0.8 O 3 film on a SrRuO 3 electrode layer deposited on a SrTiO 3 substrate. The lattice is highly tetragonal at the centre of the film, whereas it shows reduced tetragonality close to the interfaces. Most strikingly, we find that the maximum off-centre displacements for the central area of the film do not scale with the tetragonality. This challenges the fundamental belief in a strong polarization–tetragonality coupling in PbTiO 3 -based ferroelectrics, at such thicknesses. Furthermore, a systematic reduction of the atomic displacements is measured at the interfaces, suggesting that interface-induced suppression of the ferroelectric polarization plays a critical role in the size effect of nanoscale ferroelectrics.
Ambient effect on the Curie temperatures and magnetic domains in metallic two-dimensional magnets
The emergent magnetic two-dimensional (2D) materials provide ideal solid-state platforms for a broad range of applications including miniaturized spintronics, nonreciprocal optics, and magnetoelectric sensors. Owing to the general environmental sensitivity of 2D magnets, the understanding of ambient effects on 2D magnetism is critical. Apparently, the nature of itinerant ferromagnetism potentially makes metallic 2D magnets insensitive to environmental disturbance. Nevertheless, our systematic study showed that the Curie temperature of metallic 2D Fe 3 GeTe 2 decreases dramatically in the air but thick Fe 3 GeTe 2 exhibits self-protection. Remarkably, we found the air exposure effectively promotes the formation of multiple magnetic domains in 2D Fe 3 GeTe 2 , but not in bulk Fe 3 GeTe 2 . Our first-principles calculations support the scenario that substrate-induced roughness and tellurium vacancies boost the interaction of 2D Fe 3 GeTe 2 with the air. Our elucidation of the thickness-dependent air-catalyzed evolution of Curie temperatures and magnetic domains in 2D magnets provides critical insights for chemically decorating and manipulating 2D magnets.
Direct evidence for the spin cycloid in strained nanoscale bismuth ferrite thin films
Magnonic devices that utilize electric control of spin waves mediated by complex spin textures are an emerging direction in spintronics research. Room-temperature multiferroic materials, such as bismuth ferrite (BiFeO 3 ), would be ideal candidates for this purpose. To realize magnonic devices, a robust long-range spin cycloid with well-known direction is desired, since it is a prerequisite for the magnetoelectric coupling. Despite extensive investigation, the stabilization of a large-scale uniform spin cycloid in nanoscale (100 nm) thin BiFeO 3 films has not been accomplished. Here, we demonstrate cycloidal spin order in 100 nm BiFeO 3 thin films through the careful choice of crystallographic orientation, and control of the electrostatic and strain boundary conditions. Neutron diffraction, in conjunction with X-ray diffraction, reveals an incommensurate spin cycloid with a unique [11 ] propagation direction. While this direction is different from bulk BiFeO 3 , the cycloid length and Néel temperature remain equivalent to bulk at room temperature. Whilst possessing potential for electrically-controlled magnonic applications, the spin cycloid of bulk BiFeO 3 is lost in technologically-relevant thin films. Here, the authors demonstrate the stabilization of a long-range spin cycloid in BiFeO 3 thin films through careful choice of electrostatic and strain conditions during thin film growth.