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1.
Nat Commun ; 11(1): 2836, 2020 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-32504063

RESUMO

Magnetoelectric coupling at room temperature in multiferroic materials, such as BiFeO3, is one of the leading candidates to develop low-power spintronics and emerging memory technologies. Although extensive research activity has been devoted recently to exploring the physical properties, especially focusing on ferroelectricity and antiferromagnetism in chemically modified BiFeO3, a concrete understanding of the magnetoelectric coupling is yet to be fulfilled. We have discovered that La substitutions at the Bi-site lead to a progressive increase in the degeneracy of the potential energy landscape of the BiFeO3 system exemplified by a rotation of the polar axis away from the 〈111〉pc towards the 〈112〉pc discretion. This is accompanied by corresponding rotation of the antiferromagnetic axis as well, thus maintaining the right-handed vectorial relationship between ferroelectric polarization, antiferromagnetic vector and the Dzyaloshinskii-Moriya vector. As a consequence, La-BiFeO3 films exhibit a magnetoelectric coupling that is distinctly different from the undoped BiFeO3 films.

2.
Small ; 16(24): e2000020, 2020 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-32419389

RESUMO

Transparent flexible energy storage devices are considered as important chains in the next-generation, which are able to store and supply energy for electronic devices. Here, aluminum-doped zinc oxide (AZO) nanorods (NRs) and nickel oxide (NiO)-coated AZO NRs on muscovites are fabricated by a radio frequency (RF) magnetron sputtering deposition method. Interestingly, AZO NRs and AZO/NiO NRs are excellent electrodes for energy storage application with high optical transparency, high conductivity, large surface area, stability under compressive and tensile strain down to a bending radius of 5 mm with 1000 bending cycles. The obtained symmetric solid-state supercapacitors based on these electrodes exhibit good performance with a large areal specific capacitance of 3.4 mF cm-2 , long cycle life 1000 times, robust mechanical properties, and high chemical stability. Furthermore, an AZO/NiO//Zn battery based on these electrodes is demonstrated, yielding a discharge capacity of 195 mAh g-1 at a current rate of 8 A g-1 and a discharge capacity of over 1000 cycles with coulombic efficiency to 92%. These results deliver a concept of opening a new opportunity for future applications in transparent flexible energy storage.

3.
Artigo em Inglês | MEDLINE | ID: mdl-32297504

RESUMO

The piezoresistive effect has shown a remarkable potential for mechanical sensor applications and been sought for its excellent performance. A great attention was paid to the giant piezoresistive effect and sensitivity delivered by silicon-based nanostructures. However, low thermal stability and complicated fabrication process hinder their practical applications. To overcome these issues and enhance the functionalities, we envision the substantial piezopotential in a zinc oxide (ZnO)/muscovite (mica) heteroepitaxy system based on theoretical consideration and realize it in practice. High piezoresistive effect with giant change of resistivity (-80 to 240%) and large gauge factor (>1000) are demonstrated through mechanical bending. The detailed features of heteroepitaxy, electrical transport, and strain are probed to understand the mechanism of such a giant resistivity change. In addition, a bending model is established to reveal the distribution of strain. Finally, we demonstrate a flex sensor featuring high sensitivity, optical transparency, and two-segment sensing with a great potential toward practical applications. Such an oxide heteroepitaxy exhibits excellent piezoresistive properties and mechanical flexibility. In the near future, the importance of flex sensors will emerge because of the precise control in the automation industries, and our results lead to a new design in the field of flex sensors.

4.
Nanoscale ; 12(5): 3284-3291, 2020 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-31971196

RESUMO

The employment of flexible muscovite substrates has given us the feasibility of applying strain to heterostructures dynamically by mechanical bending. In this study, this novel approach is utilized to investigate strain effects on the exchange coupling in ferromagnetic Co and anti-ferromagnetic CoO (Co/CoO) bilayers. Two different Co/CoO bilayer heterostructures were grown on muscovite substrates by oxide molecular beam epitaxy, with the CoO layer being purely (111)- and (100)-oriented. The strain-dependent exchange coupling effect can only be observed on Co/CoO(100)/mica but not on Co/CoO(111)/mica. The origin of this phenomenon is attributed to the anisotropic spin re-orientation induced by mechanical bending. The strain-dependent magnetic anisotropy of the bilayers determined by anisotropic magnetoresistance measurements confirms this conjecture. This study elucidates the fundamental understanding of how magnetic exchange coupling can be tuned by externally applied strain via mechanical bending and, hence, provides a novel approach for implementing flexible spintronic devices.

5.
Adv Mater ; : e1905132, 2020 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-31967707

RESUMO

Nanoelectronic devices based on ferroelectric domain walls (DWs), such as memories, transistors, and rectifiers, have been demonstrated in recent years. Practical high-speed electronics, on the other hand, usually demand operation frequencies in the gigahertz (GHz) regime, where the effect of dipolar oscillation is important. Herein, an unexpected giant GHz conductivity on the order of 103 S m-1 is observed in certain BiFeO3 DWs, which is about 100 000 times greater than the carrier-induced direct current (dc) conductivity of the same walls. Surprisingly, the nominal configuration of the DWs precludes the alternating current (ac) conduction under an excitation electric field perpendicular to the surface. Theoretical analysis shows that the inclined DWs are stressed asymmetrically near the film surface, whereas the vertical walls in a control sample are not. The resultant imbalanced polarization profile can then couple to the out-of-plane microwave fields and induce power dissipation, which is confirmed by the phase-field modeling. Since the contributions from mobile-carrier conduction and bound-charge oscillation to the ac conductivity are equivalent in a microwave circuit, the research on local structural dynamics may open a new avenue to implement DW nano-devices for radio-frequency applications.

6.
ACS Nano ; 14(1): 985-992, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31904930

RESUMO

The most pressing barrier for the development of advanced electronics based on two-dimensional (2D) layered semiconductors stems from the lack of site-selective synthesis of complementary n- and p-channels with low contact resistance. Here, we report an in-plane epitaxial route for the growth of interlaced 2D semiconductor monolayers using chemical vapor deposition with a gas-confined scheme, in which patterned graphene (Gr) serves as a guiding template for site-selective growth of Gr-WS2-Gr and Gr-WSe2-Gr heterostructures. The Gr/2D semiconductor interface exhibits a transparent contact with a nearly ideal pinning factor of 0.95 for the n-channel WS2 and 0.92 for the p-channel WSe2. The effective depinning of the Fermi level gives an ultralow contact resistance of 0.75 and 1.20 kΩ·µm for WS2 and WSe2, respectively. Integrated logic circuits including inverter, NAND gate, static random access memory, and five-stage ring oscillator are constructed using the complementary Gr-WS2-Gr-WSe2-Gr heterojunctions as a fundamental building block, featuring the prominent performance metrics of high operation frequency (>0.2 GHz), low-power consumption, large noise margins, and high operational stability. The technology presented here provides a speculative look at the electronic circuitry built on atomic-scale semiconductors in the near future.

7.
ACS Appl Mater Interfaces ; 11(38): 35162-35168, 2019 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-31476857

RESUMO

Materials with high spin-polarization play an important role in the development of spintronics. Co-based Heusler compounds are a promising candidate for practical applications because of their high Curie temperature and tunable half-metallicity. However, it is a challenge to integrate Heusler compounds into thin film heterostructures because of the lack of control on crystallinity and chemical disorder, critical factors of novel behaviors. Here, muscovite is introduced as a growth substrate to fabricate epitaxial Co2MnGa films with mechanical flexibility. The feature of heteroepitaxy is evidenced by the results of X-ray diffraction and transmission electron microscopy. Moreover, high chemical ordering with superior properties is delivered according to the observation of large Hall conductivity (680 Ω-1 cm-1) and highly saturated magnetic moment (∼3.93 µB/f.u.), matching well with bulk crystals. Furthermore, the excellence of magnetic and electrical properties is retained under the various mechanical bending conditions. Such a result suggests that the development of Co2MnGa/muscovite heteroepitaxy provides not only a pathway to the thin film heterostructure based on high-quality Heusler compounds but also a new aspect of spintronic applications on flexible substrates.

8.
ACS Appl Mater Interfaces ; 11(29): 25882-25890, 2019 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-31257841

RESUMO

With the rise of Internet of Things, the presence of flexible devices has attracted significant attention owing to design flexibility. A ferroelectric field-effect transistor (FeFET), showing the advantages of high speed, nondestructive readout, and low-power consumption, plays a key role in next-generation technology. However, the performance of these devices is restricted since conventional flexible substrates show poor thermal stability to integrate traditional ferroelectric materials, limiting the compatibility of wearable devices. In this study, we adopt flexible muscovite mica as a substrate due to its good thermal properties and epitaxial integration ability. A flexible FeFET composed of oxide heteroepitaxy on muscovite is realized by combining an aluminum-doped zinc oxide film as the semiconductor channel layer and a Pb(Zr0.7Ti0.3)O3 film as the ferroelectric gate dielectric. The excellent characteristics of the transistor together with superior thermal stability and mechanical flexibility are demonstrated through various mechanical bending and temperature measurements. The on/off current ratio of the FeFET is higher than 103, which based on the field effect in the transfer curve. The smallest bending radius that can be achieved is 5 mm with a cyclability of 300 times and a retention of 100 h. This study opens an avenue to use oxide heteroepitaxy to construct a FeFET for next-generation flexible electronic systems.

9.
Nat Mater ; 18(6): 580-587, 2019 06.
Artigo em Inglês | MEDLINE | ID: mdl-31061484

RESUMO

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.

10.
Nano Lett ; 19(3): 1445-1450, 2019 03 13.
Artigo em Inglês | MEDLINE | ID: mdl-30724569

RESUMO

The misfit dislocations formed at heteroepitaxial interfaces create long-ranging strain fields in addition to the epitaxial strain. For systems with strong lattice coupling, such as ferroic oxides, this results in unpredictable and potentially debilitating functionality and device performance. In this work, we use dark-field X-ray microscopy to map the lattice distortions around misfit dislocations in an epitaxial film of bismuth ferrite (BiFeO3), a well-known multiferroic. We demonstrate the ability to precisely quantify weak, long-ranging strain fields and their associated symmetry lowering without modifying the mechanical state of the film. We isolate the screw and edge components of the individual dislocations and show how they result in weak charge heterogeneities via flexoelectric coupling. We show that even systems with small lattice mismatches and additional mechanisms of stress relief (such as mechanical twinning) may still give rise to measurable charge and strain heterogeneities that extend over mesoscopic length scales. This sets more stringent physical limitations on device size, dislocation density, and the achievable degree of lattice mismatch in epitaxial systems.

11.
Adv Mater ; 31(16): e1900458, 2019 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-30811706

RESUMO

Ionic-liquid-gating- (ILG-) induced proton evolution has emerged as a novel strategy to realize electron doping and manipulate the electronic and magnetic ground states in complex oxides. While the study of a wide range of systems (e.g., SrCoO2.5 , VO2 , WO3 , etc.) has demonstrated important opportunities to incorporate protons through ILG, protonation remains a big challenge for many others. Furthermore, the mechanism of proton intercalation from the ionic liquid/solid interface to whole film has not yet been revealed. Here, with a model system of inverse spinel NiCo2 O4 , an increase in system temperature during ILG forms a single but effective method to efficiently achieve protonation. Moreover, the ILG induces a novel phase transformation in NiCo2 O4 from ferrimagnetic metallic into antiferromagnetic insulating with protonation at elevated temperatures. This study shows that environmental temperature is an efficient tuning knob to manipulate ILG-induced ionic evolution.

12.
Adv Mater ; 31(11): e1806335, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30663174

RESUMO

Electric field control of magnetism ultimately opens up the possibility of reducing energy consumption of memory and logic devices. Electric control of magnetization and exchange bias are demonstrated in all-oxide heterostructures of BiFeO3 (BFO) and La0.7 Sr0.3 MnO3 (LSMO). However, the role of the polar heterointerface on magnetoelectric (ME) coupling is not fully explored. Here, the ME coupling in BFO/LSMO heterostructures with two types of interfaces, achieved by exploiting the interface engineering at the atomic scale, is investigated. It is shown that both magnetization and exchange bias are reversibly controlled by switching the ferroelectric polarization of BFO. Intriguingly, distinctly different modulation behaviors that depend on the interfacial atomic sequence are observed. These results provide new insights into the underlying physics of ME coupling in the model system. This study highlights that designing interface at the atomic scale is of general importance for functional spintronic devices.

13.
ACS Appl Mater Interfaces ; 11(2): 2205-2210, 2019 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-30408951

RESUMO

Self-assembled heteroepitaxial nanostructures have played an important role for miniaturization of electronic devices, e.g., the ultrahigh density ferroelectric memories, and cause for great concern. Our first principle calculations predict that the materials with low formation energy of the interface ( Ef) tend to form matrix structure in self-assembled heteroepitaxial nanostructures, whereas those with high Ef form nanopillars. Under the guidance of the theoretical modeling, perovskite BiFeO3 (BFO) nanopillars are swimmingly grown into CeO2 matrix on single-crystal (001)-SrTiO3 (STO) substrates by pulsed laser deposition, where CeO2 has a lower formation energy of the interface ( Ef) than BFO. This work provides a good paradigm for controlling self-assembled nanostructures as well as the application of self-assembled ferroelectric nanoscale memory.

14.
ACS Appl Mater Interfaces ; 11(1): 1655-1664, 2019 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-30561192

RESUMO

The ability of band offsets at multiferroic/metal and multiferroic/electrolyte interfaces in controlling charge transfer and thus altering the photoactivity performance has sparked significant attention in solar energy conversion applications. Here, we demonstrate that the band offsets of the two interfaces play the key role in determining charge transport direction in a downward self-polarized BFO film. Electrons tend to move to BFO/electrolyte interface for water reduction. Our experimental and first-principle calculations reveal that the presence of neodymium (Nd) dopants in BFO enhances the photoelectrochemical performance by reduction of the local electron-hole pair recombination sites and modulation of the band gap to improve the visible light absorption. This opens a promising route to the heterostructure design by modulating the band gap to promote efficient charge transfer.

15.
Nano Lett ; 18(12): 7742-7748, 2018 12 12.
Artigo em Inglês | MEDLINE | ID: mdl-30407834

RESUMO

Photostriction, optical stimulus driven mechanical deformation in materials, provides a solution toward next-generation technology. Here, the giant photostriction (∼2% change of lattice) of epitaxial strontium iridate (SrIrO3) films under illumination at room temperature is revealed via power-dependent Raman scattering, which is significantly larger as compared to conventional inorganic materials. The time scale and mechanism of this giant photostriction in SrIrO3 are further studied through time-resolved transient reflectivity measurements. The main mechanism is determined to be the electron-phonon coupling. In addition, we find that such an exotic behavior happens within few picoseconds and remains up to 107 cyclic on/off operations. The observation of giant photostriction in SrIrO3 films with superior endurance promises the advance of shape responsive solids that are sensitive to environmental stimuli, which could be widely utilized for multifunctional optoelectronics and optomechanical devices.

16.
J Synchrotron Radiat ; 25(Pt 6): 1711-1718, 2018 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-30407181

RESUMO

The properties of many materials can be strongly affected by the atomic valence of the contained individual elements, which may vary at surfaces and other interfaces. These variations can have a critical impact on material performance in applications. A non-destructive method for the determination of layer-by-layer atomic valence as a function of material thickness is presented for La0.7Sr0.3MnO3 (LSMO) thin films. The method utilizes a combination of bulk- and surface-sensitive X-ray absorption spectroscopy (XAS) detection modes; here, the modes are fluorescence yield and surface-sensitive total electron yield. The weighted-average Mn atomic valence as measured from the two modes are simultaneously fitted using a model for the layer-by-layer variation of valence based on theoretical model Hamiltonian calculations. Using this model, the Mn valence profile in LSMO thin film is extracted and the valence within each layer is determined to within an uncertainty of a few percent. The approach presented here could be used to study the layer-dependent valence in other systems or extended to different properties of materials such as magnetism.

17.
Sci Rep ; 8(1): 14313, 2018 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-30254275

RESUMO

The Mn valence in thin film La0.7Sr0.3MnO3 was studied as a function of film thickness in the range of 1-16 unit cells with a combination of non-destructive bulk and surface sensitive X-ray absorption spectroscopy techniques. Using a layer-by-layer valence model, it was found that while the bulk averaged valence hovers around its expected value of 3.3, a significant deviation occurs within several unit cells of the surface and interface. These results were supported by first principles calculations. The surface valence increases to up to Mn3.7+, whereas the interface valence reduces down to Mn2.5+. The change in valence from the expected bulk value is consistent with charge redistribution due to the polar discontinuity at the film-substrate interface. The comparison with theory employed here illustrates how this layer-by-layer valence evolves with film thickness and allows for a deeper understanding of the microscopic mechanisms at play in this effect. These results offer insight on how the two-dimensional electron gas is created in thin film oxide alloys and how the magnetic ordering is reduced with dimensionality.

18.
Nat Commun ; 9(1): 3764, 2018 09 21.
Artigo em Inglês | MEDLINE | ID: mdl-30242162

RESUMO

Electric-field control of magnetism requires deterministic control of the magnetic order and understanding of the magnetoelectric coupling in multiferroics like BiFeO3 and EuTiO3. Despite this critical need, there are few studies on the strain evolution of magnetic order in BiFeO3 films. Here, in (110)-oriented BiFeO3 films, we reveal that while the polarization structure remains relatively unaffected, strain can continuously tune the orientation of the antiferromagnetic-spin axis across a wide angular space, resulting in an unexpected deviation of the classical perpendicular relationship between the antiferromagnetic axis and the polarization. Calculations suggest that this evolution arises from a competition between the Dzyaloshinskii-Moriya interaction and single-ion anisotropy wherein the former dominates at small strains and the two are comparable at large strains. Finally, strong coupling between the BiFeO3 and the ferromagnet Co0.9Fe0.1 exists such that the magnetic anisotropy of the ferromagnet can be effectively controlled by engineering the orientation of the antiferromagnetic-spin axis.

19.
ACS Appl Mater Interfaces ; 10(36): 30574-30580, 2018 Sep 12.
Artigo em Inglês | MEDLINE | ID: mdl-30118205

RESUMO

In the era of Internet of Things, the demand for flexible and transparent electronic devices has shifted to the forefront of materials science research. However, the radiation damage to key performance of transparent devices under radiative environment remains as a critical issue. Here, we present a promising technology for nonvolatile transparent electronic devices based on flexible oxide heteroepitaxy. A direct fabrication of epitaxial lead lanthanum zirconate titanate on transparent flexible mica substrate with indium tin oxide electrodes is presented. The transparent flexible ferroelectric heterostructures not only retain their superior performance, thermal stability, reliability, and mechanical durability, but also exhibit remarkably robust properties against to a strong radiation exposure. Our study demonstrates an extraordinary concept to realize transparent flexible nonvolatile electronic devices for the design and development of next-generation smart devices with potential application in electronics, automotive, aerospace, and nuclear systems.

20.
Nat Commun ; 9(1): 3143, 2018 08 07.
Artigo em Inglês | MEDLINE | ID: mdl-30087328

RESUMO

Interest in bringing p- and n-type monolayer semiconducting transition metal dichalcogenides (TMD) into contact to form rectifying pn diode has thrived since it is crucial to control the electrical properties in two-dimensional (2D) electronic and optoelectronic devices. Usually this involves vertically stacking different TMDs with pn heterojunction or, laterally manipulating carrier density by gate biasing. Here, by utilizing a locally reversed ferroelectric polarization, we laterally manipulate the carrier density and created a WSe2 pn homojunction on the supporting ferroelectric BiFeO3 substrate. This non-volatile WSe2 pn homojunction is demonstrated with optical and scanning probe methods and scanning photoelectron micro-spectroscopy. A homo-interface is a direct manifestation of our WSe2 pn diode, which can be quantitatively understood as a clear rectifying behavior. The non-volatile confinement of carriers and associated gate-free pn homojunction can be an addition to the 2D electron-photon toolbox and pave the way to develop laterally 2D electronics and photonics.

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