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1.
Nat Commun ; 13(1): 3539, 2022 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-35725723

RESUMO

All-electric switching of perpendicular magnetization is a prerequisite for the integration of fast, high-density, and low-power magnetic memories and magnetic logic devices into electric circuits. To date, the field-free spin-orbit torque (SOT) switching of perpendicular magnetization has been observed in SOT bilayer and trilayer systems through various asymmetric designs, which mainly aim to break the mirror symmetry. Here, we report that the perpendicular magnetization of CoxPt100-x single layers within a special composition range (20 < x < 56) can be deterministically switched by electrical current in the absence of external magnetic field. Specifically, the Co30Pt70 shows the largest out-of-plane effective field efficiency and best switching performance. We demonstrate that this unique property arises from the cooperation of two structural mechanisms: the low crystal symmetry property at the Co platelet/Pt interfaces and the composition gradient along the thickness direction. Compared with that in bilayers or trilayers, the field-free switching in CoxPt100-x single layer greatly simplifies the SOT structure and avoids additional asymmetric designs.

2.
Sci Adv ; 8(13): eabm8550, 2022 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-35363530

RESUMO

The orthorhombic rare-earth manganates and ferrites multiferroics are promising candidates for the next generation multistate spintronic devices. However, their ferroelectric polarization is small, and transition temperature is far below room temperature (RT). The improvement of ferroelectricity remains challenging. Here, through the subtle strain and defect engineering, an RT colossal polarization of 4.14 µC/cm2 is achieved in SmFeO3-δ films, which is two orders of magnitude larger than its bulk and is also the largest one among the orthorhombic rare-earth manganite and ferrite family. Meanwhile, its RT magnetism is uniformly distributed in the film. Combining the integrated differential phase-contrast imaging and density functional theory calculations, we reveal the origin of this superior ferroelectricity in which the purposely introduced oxygen vacancies in the Fe-O layer distorts the FeO6 octahedral cage and drives the Fe ion away from its high-symmetry position. The present approach can be applied to improve ferroelectric properties for multiferroics.

3.
Nat Commun ; 13(1): 1729, 2022 04 01.
Artigo em Inglês | MEDLINE | ID: mdl-35365642

RESUMO

In the quest for emerging in-sensor computing, materials that respond to optical stimuli in conjunction with non-volatile phase transition are highly desired for realizing bioinspired neuromorphic vision components. Here, we report a non-volatile multi-level control of VO2 films by oxygen stoichiometry engineering under ultraviolet irradiation. Based on the reversible regulation of VO2 films using ultraviolet irradiation and electrolyte gating, we demonstrate a proof-of-principle neuromorphic ultraviolet sensor with integrated sensing, memory, and processing functions at room temperature, and also prove its silicon compatible potential through the wafer-scale integration of a neuromorphic sensor array. The device displays linear weight update with optical writing because its metallic phase proportion increases almost linearly with the light dosage. Moreover, the artificial neural network consisting of this neuromorphic sensor can extract ultraviolet information from the surrounding environment, and significantly improve the recognition accuracy from 24% to 93%. This work provides a path to design neuromorphic sensors and will facilitate the potential applications in artificial vision systems.


Assuntos
Redes Neurais de Computação , Visão Ocular , Transição de Fase
4.
Adv Mater ; 34(24): e2109889, 2022 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-35397192

RESUMO

Hafnia-based compounds have considerable potential for use in nanoelectronics due to their compatibility with complementary metal-oxide-semiconductor devices and robust ferroelectricity at nanoscale sizes. However, the unexpected ferroelectricity in this class of compounds often remains elusive due to the polymorphic nature of hafnia, as well as the lack of suitable methods for the characterization of the mixed/complex phases in hafnia thin films. Herein, the preparation of centimeter-scale, crack-free, freestanding Hf0.5 Zr0.5 O2 (HZO) nanomembranes that are well suited for investigating the local crystallographic phases, orientations, and grain boundaries at both the microscopic and mesoscopic scales is reported. Atomic-level imaging of the plan-view crystallographic patterns shows that more than 80% of the grains are the ferroelectric orthorhombic phase, and that the mean equivalent diameter of these grains is about 12.1 nm, with values ranging from 4 to 50 nm. Moreover, the ferroelectric orthorhombic phase is stable in substrate-free HZO membranes, indicating that strain from the substrate is not responsible for maintaining the polar phase. It is also demonstrated that HZO capacitors prepared on flexible substrates are highly uniform, stable, and robust. These freestanding membranes provide a viable platform for the exploration of HZO polymorphic films with complex structures and pave the way to flexible nanoelectronics.

5.
ACS Appl Mater Interfaces ; 14(4): 6194-6202, 2022 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-35072446

RESUMO

Interfaces between complex oxides provide a unique opportunity to discover novel interfacial physics and functionalities. Here, we fabricate the multilayers of itinerant ferromagnet SrRuO3 (SRO) and multiferroic BiFeO3 (BFO) with atomically sharp interfaces. Atomically resolved transmission electron microscopy reveals that a large ionic displacement in BFO can penetrate into SRO layers near the BFO/SRO interfaces to a depth of 2-3 unit cells, indicating the ferroelectric proximity effect. A topological Hall effect is indicated by hump-like anomalies in the Hall measurements of the multilayer with a moderate thickness of the SRO layer. With magnetic measurements, it can be further confirmed that each SRO layer in the multilayers can be divided into interfacial and middle regions, which possess different magnetic ground states. Our work highlights the key role of functional heterointerfaces in exotic properties and provides an important guideline to design spintronic devices based on magnetic skyrmions.

6.
Phys Rev Lett ; 128(1): 017202, 2022 Jan 07.
Artigo em Inglês | MEDLINE | ID: mdl-35061447

RESUMO

Heterointerfaces have led to the discovery of novel electronic and magnetic states because of their strongly entangled electronic degrees of freedom. Single-phase chromium compounds always exhibit antiferromagnetism following the prediction of the Goodenough-Kanamori rules. So far, exchange coupling between chromium ions via heteroanions has not been explored and the associated quantum states are unknown. Here, we report the successful epitaxial synthesis and characterization of chromium oxide (Cr_{2}O_{3})-chromium nitride (CrN) superlattices. Room-temperature ferromagnetic spin ordering is achieved at the interfaces between these two antiferromagnets, and the magnitude of the effect decays with increasing layer thickness. First-principles calculations indicate that robust ferromagnetic spin interaction between Cr^{3+} ions via anion-hybridization across the interface yields the lowest total energy. This work opens the door to fundamental understanding of the unexpected and exceptional properties of oxide-nitride interfaces and provides access to hidden phases at low-dimensional quantum heterostructures.

7.
Nano Lett ; 21(24): 10507-10515, 2021 Dec 22.
Artigo em Inglês | MEDLINE | ID: mdl-34870440

RESUMO

Orientation control of the oxygen vacancy channel (OVC) is highly desirable for tailoring oxygen diffusion as it serves as a fast transport channel in ion conductors, which is widely exploited in solid-state fuel cells, catalysts, and ion-batteries. Direct observation of oxygen-ion hopping toward preferential vacant sites is a key to clarifying migration pathways. Here we report anisotropic oxygen-ion migration mediated by strain in ultrathin cobaltites via in situ thermal activation in atomic-resolved transmission electron microscopy. Oxygen migration pathways are constructed on the basis of the atomic structure during the OVC switching, which is manifested as the vertical-to-horizontal OVC switching under tensile strain but the horizontal-to-diagonal switching under compression. We evaluate the topotactic structural changes to the OVC, determine the crucial role of the tolerance factor for OVC stability, and establish the strain-dependent phase diagram. Our work provides a practical guide for engineering OVC orientation that is applicable to ionic-oxide electronics.

8.
J Phys Condens Matter ; 34(6)2021 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-34740209

RESUMO

Oxygen-vacancy-induced topotactic phase transformation between the ABO2.5brownmillerite structure and the ABO3perovskite structure attracts ever-increasing attention due to the perspective applications in catalysis, clean energy field, and memristors. However, a detailed investigation of the electronic-structure evolution during the topotactic phase transformation for understanding the underlying mechanism is highly desired. In this work, multiple analytical methods were used to explore evolution of the electronic structure of SrFeO3-xthin films during the topotactic phase transformation. The results indicate that the increase in oxygen content induces a new unoccupied state of O 2pcharacter near the Fermi energy, inducing the insulator-to-metal transition. More importantly, the hole states are more likely constrained to thedx2-y2orbital than to thed3z2-r2orbital. Our results reveal an unambiguous evolution of the electronic structure of SrFeO3-xfilms during topotactic phase transformation, which is crucial not only for fundamental understanding but also for perspective applications such as solid-state oxide fuel cells, catalysts, and memristor devices.

9.
Science ; 374(6563): 100-104, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34591628

RESUMO

Electrostatic energy storage technology based on dielectrics is fundamental to advanced electronics and high-power electrical systems. Recently, relaxor ferroelectrics characterized by nanodomains have shown great promise as dielectrics with high energy density and high efficiency. We demonstrate substantial enhancements of energy storage properties in relaxor ferroelectric films with a superparaelectric design. The nanodomains are scaled down to polar clusters of several unit cells so that polarization switching hysteresis is nearly eliminated while relatively high polarization is maintained. We achieve an ultrahigh energy density of 152 joules per cubic centimeter with markedly improved efficiency (>90% at an electric field of 3.5 megavolts per centimeter) in superparaelectric samarium-doped bismuth ferrite­barium titanate films. This superparaelectric strategy is generally applicable to optimize dielectric and other related functionalities of relaxor ferroelectrics.

10.
Nano Lett ; 21(19): 8324-8331, 2021 Oct 13.
Artigo em Inglês | MEDLINE | ID: mdl-34546060

RESUMO

Rare earth nickelates including LaNiO3 are promising catalysts for water electrolysis to produce oxygen gas. Recent studies report that Fe substitution for Ni can significantly enhance the oxygen evolution reaction (OER) activity of LaNiO3. However, the role of Fe in increasing the activity remains ambiguous, with potential origins that are both structural and electronic in nature. On the basis of a series of epitaxial LaNi1-xFexO3 thin films synthesized by molecular beam epitaxy, we report that Fe substitution tunes the Ni oxidation state in LaNi1-xFexO3 and a volcano-like OER trend is observed, with x = 0.375 being the most active. Spectroscopy and ab initio modeling reveal that high-valent Fe3+δ cationic species strongly increase the transition-metal (TM) 3d bandwidth via Ni-O-Fe bridges and enhance TM 3d-O 2p hybridization, boosting the OER activity. These studies deepen our understanding of structural and electronic contributions that give rise to enhanced OER activity in perovskite oxides.

11.
Adv Sci (Weinh) ; 8(13): 2100177, 2021 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-34258162

RESUMO

A variety of emergent phenomena are enabled by interface engineering in the complex oxides heterostructures. While extensive attention is attracted to LaMnO3 (LMO) thin films for observing the control of functionalities at its interface with substrate, the nature of the magnetic phases in the thin film is, however, controversial. Here, it is reported that the ferromagnetism in two and five unit cells thick LMO films epitaxially deposited on (001)-SrTiO3 substrates, a ferromagnetic/ferromagnetic coupling in eight and ten unit cells ones, and a striking ferromagnetic/antiferromagnetic pinning effect with apparent positive exchange bias in 15 and 20 unit cells ones are observed. This novel phenomenon in both 15 and 20 unit cells films indicates a coexistence of three magnetic orderings in a single LMO film. The high-resolution scanning transmission electron microscopy suggests a P21/n to Pbnm symmetry transition from interface to surface, with the spatial stratification of MnO6 octahedral morphology, corresponding to different magnetic orderings. These results can shed some new lights on manipulating the functionality of oxides by interface engineering.

12.
Nano Lett ; 21(7): 3146-3154, 2021 Apr 14.
Artigo em Inglês | MEDLINE | ID: mdl-33750141

RESUMO

Manipulation of octahedral distortion at atomic scale is an effective means to tune the ground states of functional oxides. Previous work demonstrates that strain and film thickness are variable parameters to modify the octahedral parameters. However, selective control of bonding geometry by structural propagation from adjacent layers is rarely studied. Here we propose a new route to tune the ferromagnetism in SrRuO3 (SRO) ultrathin layers by oxygen coordination of adjacent SrCuO2 (SCO) layers. The infinite-layered CuO2 exhibits a structural transformation from "planar-type" to "chain-type" with reduced film thickness. Two orientations dramatically modify the polyhedral connectivity at the interface, thus altering the octahedral distortion of SRO. The local structural variation changes the spin state of Ru and orbital hybridization strength, leading to a significant change in the magnetoresistance and anomalous Hall resistivity. These findings could launch investigations into adaptive control of functionalities in quantum oxide heterostructures using oxygen coordination.

13.
Nat Commun ; 12(1): 1853, 2021 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-33767171

RESUMO

Dedicated control of oxygen vacancies is an important route to functionalizing complex oxide films. It is well-known that tensile strain significantly lowers the oxygen vacancy formation energy, whereas compressive strain plays a minor role. Thus, atomic reconstruction by extracting oxygen from a compressive-strained film is challenging. Here we report an unexpected LaCoO2.5 phase with a zigzag-like oxygen vacancy ordering through annealing a compressive-strained LaCoO3 in vacuum. The synergetic tilt and distortion of CoO5 square pyramids with large La and Co shifts are quantified using scanning transmission electron microscopy. The large in-plane expansion of CoO5 square pyramids weaken the crystal field splitting and facilitated the ordered high-spin state of Co2+, which produces an insulating ferromagnetic state with a Curie temperature of ~284 K and a saturation magnetization of ~0.25 µB/Co. These results demonstrate that extracting targeted oxygen from a compressive-strained oxide provides an opportunity for creating unexpected crystal structures and novel functionalities.

14.
Sci Rep ; 11(1): 2744, 2021 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-33531569

RESUMO

The emergence of ferromagnetism in two-dimensional van der Waals materials has aroused broad interest. However, the ferromagnetic instability has been a problem remained. In this work, by using the first-principles calculations, we identified the critical ranges of strain and doping for the bilayer Cr2Ge2Te6 within which the ferromagnetic stability can be enhanced. Beyond the critical range, the tensile strain can induce the phase transition from the ferromagnetic to the antiferromagnetic, and the direction of magnetic easy axis can be converted from out-of-plane to in-plane due to the increase of compressive strain, or electrostatic doping. We also predicted an electron doping range, within which the ferromagnetism can be enhanced, while the ferromagnetic stability was maintained. Moreover, we found that the compressive strain can reverse the spin polarization of electrons at the conduction band minimum, so that two categories of half-metal can be induced by controlling electrostatic doping in the bilayer Cr2Ge2Te6. These results should shed a light on achieving ferromagnetic stability for low-dimensional materials.

15.
Adv Mater ; 33(2): e2005920, 2021 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-33289203

RESUMO

Strain engineering provides the ability to control the ground states and associated phase transition in epitaxial films. However, the systematic study of the intrinsic character and strain dependency in transition-metal nitrides remains challenging due to the difficulty in fabricating stoichiometric and high-quality films. Here the observation of an electronic state transition in highly crystalline antiferromagnetic CrN films with strain and reduced dimensionality is reported. By shrinking the film thickness to a critical value of ≈30 unit cells, a profound conductivity reduction accompanied by unexpected volume expansion is observed in CrN films. The electrical conductivity is observed surprisingly when the CrN layer is as thin as a single unit cell thick, which is far below the critical thickness of most metallic films. It is found that the metallicity of an ultrathin CrN film recovers from insulating behavior upon the removal of the as-grown strain by the fabrication of freestanding nitride films. Both first-principles calculations and linear dichroism measurements reveal that the strain-mediated orbital splitting effectively customizes the relatively small bandgap at the Fermi level, leading to an exotic phase transition in CrN. The ability to achieve highly conductive nitride ultrathin films by harnessing strain-control over competing phases can be used for utilizing their exceptional characteristics.

16.
Adv Mater ; 33(4): e2001324, 2021 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-33314400

RESUMO

Low-dimensional quantum materials that remain strongly ferromagnetic down to monolayer thickness are highly desired for spintronic applications. Although oxide materials are important candidates for the next generation of spintronics, ferromagnetism decays severely when the thickness is scaled to the nanometer regime, leading to deterioration of device performance. Here, a methodology is reported for maintaining strong ferromagnetism in insulating LaCoO3 (LCO) layers down to the thickness of a single unit cell. It is found that the magnetic and electronic states of LCO are linked intimately to the structural parameters of adjacent "breathing lattice" SrCuO2 (SCO). As the dimensionality of SCO is reduced, the lattice constant elongates over 10% along the growth direction, leading to a significant distortion of the CoO6 octahedra, and promoting a higher spin state and long-range spin ordering. For atomically thin LCO layers, surprisingly large magnetic moment (0.5 µB /Co) and Curie temperature (75 K), values larger than previously reported for any monolayer oxides are observed. The results demonstrate a strategy for creating ultrathin ferromagnetic oxides by exploiting atomic heterointerface engineering, confinement-driven structural transformation, and spin-lattice entanglement in strongly correlated materials.

17.
Nat Commun ; 11(1): 1371, 2020 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-32170073

RESUMO

Oxygen vacancies in complex oxides are indispensable for information and energy technologies. There are several means to create oxygen vacancies in bulk materials. However, the use of ionic interfaces to create oxygen vacancies has not been fully explored. Herein, we report an oxide nanobrush architecture designed to create high-density interfacial oxygen vacancies. An atomically well-defined (111) heterointerface between the fluorite CeO2 and the bixbyite Y2O3 is found to induce a charge modulation between Y3+ and Ce4+ ions enabled by the chemical valence mismatch between the two elements. Local structure and chemical analyses, along with theoretical calculations, suggest that more than 10% of oxygen atoms are spontaneously removed without deteriorating the lattice structure. Our fluorite-bixbyite nanobrush provides an excellent platform for the rational design of interfacial oxide architectures to precisely create, control, and transport oxygen vacancies critical for developing ionotronic and memristive devices for advanced energy and neuromorphic computing technologies.

18.
Nanomaterials (Basel) ; 10(3)2020 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-32150990

RESUMO

Micrometer-tall vertically aligned single-crystalline CoFe2O4 nanobrush architectures with extraordinarily large aspect ratio have been achieved by the precise control of a kinetic and thermodynamic non-equilibrium pulsed laser epitaxy process. Direct observations by scanning transmission electron microscopy reveal that the nanobrush crystal is mostly defect-free by nature, and epitaxially connected to the substrate through a continuous 2D interface layer. In contrast, periodic dislocations and lattice defects such as anti-phase boundaries and twin boundaries are frequently observed in the 2D interface layer, suggesting that interface misfit strain relaxation under a non-equilibrium growth condition plays a critical role in the self-assembly of such artificial architectures. Magnetic property measurements have found that the nanobrushes exhibit a saturation magnetization value of 6.16 B/f.u., which is much higher than the bulk value. The discovery not only enables insights into an effective route for fabricating unconventional high-quality nanostructures, but also demonstrates a novel magnetic architecture with potential applications in nanomagnetic devices.

19.
Nano Lett ; 20(2): 1131-1140, 2020 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-31978309

RESUMO

Strongly correlated perovskite oxides exhibit a plethera of intriguing phenomena and stimulate a great potential for multifunctional device applications. Utilizing tunable uniaxial strain, rather than biaxial or anisotropic strain, delivered from the crystallography of a single crystal substrate to modify the ground state of strongly correlated perovskite oxides has rarely been addressed for phase-space control. Here, we show that the physical properties of La2/3Ca1/3MnO3 (LCMO) films are remarkably different depending on the crystallographic orientations of the orthorhombic NdGaO3 (NGO) substrates. More importantly, the antiferromagnetic charge-ordered insulating (COI) phase induced in the (100) or (001)-oriented LCMO films can be dramatically promoted (or suppressed) by a uniaxial tensile (or compressive) bending stress along the in-plane [010] direction. By contrast, the COI phase is nearly unaffected along the other transverse in-plane directions. Results from scanning transmission electron microscopy reveal that the (100)- or (001)-oriented LCMO films are uniaxially tensile strained along the [010] direction, while the LCMO/NGO(010) and LCMO/NGO(110) films remaining as a bulklike ferromagnetic metallic state exhibit a different strain state. Density functional theory calculations further reveal that the cooperatively increased Jahn-Teller distortion and charge ordering may be indispensible for the inducing and promoting of the COI phase. These findings provide a path to understand the correlation between local and extended structural distortions imparted by coherent epitaxy and the electronic states for quantum phase engineering.

20.
ACS Appl Mater Interfaces ; 11(49): 45922-45929, 2019 Dec 11.
Artigo em Inglês | MEDLINE | ID: mdl-31718160

RESUMO

The pursuit of high-performance photodetectors functioning in the solar-blind spectrum is motivated by both scientific and practical applications ranging from secure communication, monitoring, sensing, etc. In particular, the fabrication of heterojunctions based on the wide band gap semiconductors has emerged as an attractive strategy to promote the high-efficient photogenerated electron/hole pair separation. However, the precisely controlled growth of heterojunctions remains a huge challenge. The lattice mismatch leads to the formation of defects and/or dislocations at the interface, deteriorating the performance of devices and limiting their envisioned applications. Here, we demonstrate a simple one-step growth of amorphous/crystalline Ga2O3 phase junctions by using sputtering technique, yielding a large responsivity of 0.81 A/W, a superior photo-to-dark current ratio over 107, and an ultrahigh response speed of ∼12 ns. Compared to the previous reported solar-blind photodetectors, the obtained detectivity ≈ 5.67 × 1014 Jones is increased by 2 orders of magnitude. Such excellent photoresponse characteristics can be understood by the interfacial built-in field-promoted electron/hole pair separation for the amorphous/crystalline Ga2O3 phase junctions. Our results provide a novel path toward realizing high-performance optoelectronics functioning in the solar-blind spectrum.

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