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1.
Adv Mater ; 32(7): e1905764, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31850652

RESUMO

Neuromorphic computing consisting of artificial synapses and neural network algorithms provides a promising approach for overcoming the inherent limitations of current computing architecture. Developments in electronic devices that can accurately mimic the synaptic plasticity of biological synapses, have promoted the research boom of neuromorphic computing. It is reported that robust ferroelectric tunnel junctions can be employed to design high-performance electronic synapses. These devices show an excellent memristor function with many reproducible states (≈200) through gradual ferroelectric domain switching. Both short- and long-term plasticity can be emulated by finely tuning the applied pulse parameters in the electronic synapse. The analog conductance switching exhibits high linearity and symmetry with small switching variations. A simulated artificial neural network with supervised learning built from these synaptic devices exhibited high classification accuracy (96.4%) for the Mixed National Institute of Standards and Technology (MNIST) handwritten recognition data set.

2.
ACS Appl Mater Interfaces ; 11(46): 43473-43479, 2019 Nov 20.
Artigo em Inglês | MEDLINE | ID: mdl-31702891

RESUMO

The development of artificial synapses has enabled the establishment of brain-inspired computing systems, which provides a promising approach for overcoming the inherent limitations of current computer systems. The two-terminal memristors that faithfully mimic the function of biological synapses have intensive prospects in the neural network field. Here, we propose a high-performance artificial synapse based on oxide tunnel junctions with oxygen vacancy migration. Both short-term and long-term plasticities are mimicked in one device. The oxygen vacancy migration through oxide ultrathin films is utilized to manipulate long-term plasticity. Essential synaptic functions, such as paired pulse facilitation, post-tetanic potentiation, as well as spike-timing-dependent plasticity, are successfully implemented in one device by finely modifying the shape of the pre- and postsynaptic spikes. Ultralow femtojoule energy consumption comparable to that of the human brain indicates its potential application in efficient neuromorphic computing. Oxide tunnel junctions proposed in this work provide an alternative approach for realizing energy-efficient brain-like chips.

3.
ACS Appl Mater Interfaces ; 11(33): 30089-30097, 2019 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-31342737

RESUMO

Targeted design of organic semiconductors in organic spintronics is relatively limited. Therefore, four conjugated polymers with analogous structures based on isoindigo (IID) units were designed and synthesized to investigate the structure-property relationships in spin and charge carrier transport. Structural design strategies include introduction of pyridinic nitrogen atoms into IID units to change electronic structures and alteration of different branching points of alkyl chains to adjust the aggregation structure. By fabricating polymer field-effect transistors (PFETs) and organic spin valves (OSVs), all of the polymers exhibited good ambipolar field-effect properties (all of the mobilities exceeding 0.3 cm2 V-1 s-1) and relatively high magnetoresistance (MR) values (maximum up to 25%). Most importantly, it is found that the introduction of pyridinic nitrogen into the IID units can improve MR values of OSVs and electron mobilities of PFETs, whereas the extension of alkyl chain branching points can reduce MR values of the conjugated polymers. This work is the first attempt to thoroughly study the structure-property relationship in the OSVs, combined with molecular design of the conjugated polymers, which provides a guideline for molecular engineering, especially for organic spintronics.

4.
iScience ; 16: 368-377, 2019 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-31220760

RESUMO

Oxide-based resistive switching devices, including ferroelectric tunnel junctions and resistance random access memory, are promising candidates for the next-generation non-volatile memory technology. In this work, we propose a ferroionic tunnel junction to realize a giant electroresistance. It functions as a ferroelectric tunnel junction at low resistance state and as a Schottky junction at high resistance state, due to interface engineering through the field-induced migration of oxygen vacancies. An extremely large electroresistance with ON/OFF ratios of 5.1×107 at room temperature and 2.1×109 at 10 K is achieved, using an ultrathin BaTiO3-δ layer as the ferroelectric barrier and a semiconducting Nb-doped SrTiO3 substrate as the bottom electrode. The results point toward an appealing way for the design of high-performance resistive switching devices based on ultrathin oxide heterostructures by ionic controlled interface engineering.

5.
Phys Rev Lett ; 122(8): 087401, 2019 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-30932617

RESUMO

Large coupling strengths in exciton-photon interactions are important for the quantum photonic network, while strong cavity-quantum dot interactions have been focused on s-shell excitons with small coupling strengths. Here we demonstrate strong interactions between cavities and p-shell excitons with a great enhancement by the in situ wave-function control. The p-shell excitons are demonstrated with much larger wave-function extents and nonlocal interactions beyond the dipole approximation. Then the interaction is tuned from the nonlocal to the local regime by the wave function shrinking, during which the enhancement is obtained. A large coupling strength of 210 µeV has been achieved, indicating the great potential of p-shell excitons for coherent information exchange. Furthermore, we propose a distributed delay model to quantitatively explain the coupling strength variation, revealing the intertwining of excitons and photons beyond the dipole approximation.

6.
Adv Mater ; 31(19): e1900379, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-30924206

RESUMO

Hardware implementation of artificial synaptic devices that emulate the functions of biological synapses is inspired by the biological neuromorphic system and has drawn considerable interest. Here, a three-terminal ferrite synaptic device based on a topotactic phase transition between crystalline phases is presented. The electrolyte-gating-controlled topotactic phase transformation between brownmillerite SrFeO2.5 and perovskite SrFeO3- δ is confirmed from the examination of the crystal and electronic structure. A synaptic transistor with electrolyte-gated ferrite films by harnessing gate-controllable multilevel conduction states, which originate from many distinct oxygen-deficient perovskite structures of SrFeOx induced by topotactic phase transformation, is successfully constructed. This three-terminal artificial synapse can mimic important synaptic functions, such as synaptic plasticity and spike-timing-dependent plasticity. Simulations of a neural network consisting of ferrite synaptic transistors indicate that the system offers high classification accuracy. These results provide insight into the potential application of advanced topotactic phase transformation materials for designing artificial synapses with high performance.

7.
ACS Appl Mater Interfaces ; 10(50): 43792-43801, 2018 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-30474948

RESUMO

Exploring and manipulating domain configurations in ferroelectric thin films are of critical importance for the design and fabrication of ferroelectric heterostructures with a novel functional performance. In this study, BiFeO3 (BFO) ultrathin films with various Bi/Fe ratios from excess Bi to deficient Bi have been grown on (La0.7Sr0.3)MnO3 (LSMO)-covered SrTiO3 substrates by a laser molecular beam epitaxy system. Atomic force microscopy and piezoresponse force microscopy measurements show that both the surface morphology and ferroelectric polarization of the films are relevant to Bi nonstoichiometry. More significantly, a Bi-excess thin film shows an upward (from substrate to film surface) uniform ferroelectric polarization, whereas a Bi-deficient thin film exhibits a downward uniform polarization, which means the as-grown polarization of BFO thin films can be controlled by changing the Bi contents. Atomic-scale structural and chemical characterizations and second-harmonic generation measurements reveal that two different kinds of structural distortions and interface atomic configurations in the BFO/LSMO heterostructures can be induced by the change of Bi nonstoichiometry, leading to the two opposite as-grown ferroelectric polarizations. It has also been revealed that the band gap of BFO thin films can be modulated via Bi nonstoichiometry. These results demonstrate that Bi nonstoichiometry plays a key role on the ferroelectric domain states and physical properties of BFO thin films and also open a new avenue to manipulate the structure and ferroelectric domain states in BFO thin films.

8.
Adv Mater ; : e1801548, 2018 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-29974526

RESUMO

Considering that the human brain uses ≈1015 synapses to operate, the development of effective artificial synapses is essential to build brain-inspired computing systems. In biological synapses, the voltage-gated ion channels are very important for regulating the action-potential firing. Here, an electrolyte-gated transistor using WO3 with a unique tunnel structure, which can emulate the ionic modulation process of biological synapses, is proposed. The transistor successfully realizes synaptic functions of both short-term and long-term plasticity. Short-term plasticity is mimicked with the help of electrolyte ion dynamics under low electrical bias, whereas the long-term plasticity is realized using proton insertion in WO3 under high electrical bias. This is a new working approach to control the transition from short-term memory to long-term memory using different gate voltage amplitude for artificial synapses. Other essential synaptic behaviors, such as paired pulse facilitation, the depression and potentiation of synaptic weight, as well as spike-timing-dependent plasticity are also implemented in this artificial synapse. These results provide a new recipe for designing synaptic electrolyte-gated transistors through the electrostatic and electrochemical effects.

9.
Phys Rev Lett ; 120(21): 213901, 2018 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-29883144

RESUMO

Two-photon Rabi splitting in a cavity-dot system provides a basis for multiqubit coherent control in a quantum photonic network. Here we report on two-photon Rabi splitting in a strongly coupled cavity-dot system. The quantum dot was grown intentionally large in size for a large oscillation strength and small biexciton binding energy. Both exciton and biexciton transitions couple to a high-quality-factor photonic crystal cavity with large coupling strengths over 130 µeV. Furthermore, the small binding energy enables the cavity to simultaneously couple with two exciton states. Thereby, two-photon Rabi splitting between the biexciton and cavity is achieved, which can be well reproduced by theoretical calculations with quantum master equations.

10.
Small ; 14(17): e1704429, 2018 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-29611286

RESUMO

Defects are detrimental for optoelectronics devices, such as stacking faults can form carrier-transportation barriers, and foreign impurities (Au) with deep-energy levels can form carrier traps and nonradiative recombination centers. Here, self-catalyzed p-type GaAs nanowires (NWs) with a pure zinc blende (ZB) structure are first developed, and then a photodetector made from these NWs is fabricated. Due to the absence of stacking faults and suppression of large amount of defects with deep energy levels, the photodetector exhibits room-temperature high photoresponsivity of 1.45 × 105 A W-1 and excellent specific detectivity (D*) up to 1.48 × 1014 Jones for a low-intensity light signal of wavelength 632.8 nm, which outperforms previously reported NW-based photodetectors. These results demonstrate these self-catalyzed pure-ZB GaAs NWs to be promising candidates for optoelectronics applications.

11.
ACS Appl Mater Interfaces ; 10(12): 10211-10219, 2018 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-29510620

RESUMO

Structure determines material's functionality, and strain tunes the structure. Tuning the coherent epitaxial strain by varying the thickness of the films is a precise route to manipulate the functional properties in the low-dimensional oxide materials. Here, to explore the effects of the coherent epitaxial strain on the properties of SrCoO2.5 thin films, thickness-dependent evolutions of the structural properties and electronic structures were investigated by X-ray diffraction, Raman spectra, optical absorption spectra, scanning transmission electron microscopy (STEM), and first-principles calculations. By increasing the thickness of the SrCoO2.5 films, the c-axis lattice constant decreases, indicating the relaxation of the coherent epitaxial strain. The energy band gap increases and the Raman spectra undergo a substantial softening with the relaxation of the coherent epitaxial strain. From the STEM results, it can be concluded that the strain causes the variation of the oxygen content in the BM-SCO2.5 films, which results in the variation of band gaps with varying the strain. First-principles calculations show that strain-induced changes in bond lengths and angles of the octahedral CoO6 and tetrahedral CoO4 cannot explain the variation band gap. Our findings offer an alternative strategy to manipulate structural and electronic properties by tuning the coherent epitaxial strain in transition-metal oxide thin films.

12.
Appl Opt ; 56(30): 8348-8352, 2017 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-29091611

RESUMO

Analogous with scanning electron microscopy, we use an oblique-incidence reflectivity difference (OIRD) approach for morphology detection. By scanning the active carbon clusters in a one-dimensional way and the reservoir rocks in a two-dimensional way, the morphology of the samples' surface can be revealed in OIRD signal images. High OIRD signals of active carbon samples refer to the centralized distribution areas of carbon, and the fluctuations are caused by the uneven distribution of carbon pellets. OIRD intensity is proportional to the thickness of materials. In terms of rocks, the trough areas with smaller values refer to the low-lying fields. The areas with relatively large OIRD intensities correspond to the protuberance areas of rocks. Consequently, OIRD is a sensitive yet rapid measure of surface detection in material and petrogeology science.

13.
Adv Mater ; 29(38)2017 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-28833592

RESUMO

Interference-free hyperbolic phonon polaritons (HPPs) excited by natural wrinkles in a hexagonal boron nitride (hBN) microcrystal are reported both experimentally and theoretically. Although their geometries are off-resonant with the excitation wavelength, the wrinkles compensate for the large momentum mismatch between photon and phonon polariton, and launch the HPPs without interference. The spatial feature of wrinkles is about 200 nm, which is an order of magnitude smaller than resonant metal antennas at the same excitation wavelength. Compared with phonon polaritons launched by an atomic force microscopy tip, the phonon polaritons launched by wrinkles are interference-free, independent of the launcher geometry, and exhibit a smaller damping rate (γ ≈ 0.028). On the same hBN microcrystal, in situ nanoinfrared imaging of HPPs launched by different mechanisms is performed. In addition, the dispersion of HPPs is modified by changing the dielectric environments of hBN crystals. The wavelength of HPPs is compressed twofold when the substrate is changed from SiO2 to gold. The findings provide insights into the intrinsic properties of hBN-HPPs and demonstrate a new way to launch and control polaritons in van der Waals materials.

14.
Sci Rep ; 7(1): 9051, 2017 08 22.
Artigo em Inglês | MEDLINE | ID: mdl-28831169

RESUMO

For ferroelectric materials, where the polar state breaks the inversion symmetry, second harmonic generation is a useful tool to prove their ferroelectric properties. However, the correlation between the anisotropy patterns and the polarization orientation of the ferroelectric domains has not been clarified yet. In this work, we systematically investigated this correlation in a typical perovskite oxide ferroelectric, Barium Titanate (BaTiO3) crystal, by second harmonic generation and the piezoresponse force microscopy technique. The evolution of polarization-dependent anisotropy patterns proves that there is a linear relationship between the rotation angle of second harmonic generation anisotropy patterns and the polarization angle of BaTiO3 single crystals. It is a direct evidence illustrating that the polarization of BaTiO3 crystal can be qualitatively identified in 0°-180° by second harmonic generation technology. This work gives a glance at improving a nonintrusive and convenient method to identify the polarization of perovskite ferroelectric materials.

15.
Sci Rep ; 7(1): 7693, 2017 08 09.
Artigo em Inglês | MEDLINE | ID: mdl-28794426

RESUMO

Artificial superlattices constructed with ferromagnetic La0.7Sr0.3MnO3 layer and ferroelectric Ba0.7Sr0.3TiO3 layer were designed and fabricated on SrTiO3 substrates. An epitaxial growth with sharp interfaces between La0.7Sr0.3MnO3 and Ba0.7Sr0.3TiO3 layers was confirmed by scanning transmission electron microscopy and x-ray diffraction. An unambiguous charge transfer involving an electron transferring from the La0.7Sr0.3MnO3 layers to Ba0.7Sr0.3TiO3 layers (Mn3+→Mn4+; Ti4+→Ti3+) across the interface were resolved by electron energy loss spectra analysis. These observations are attributed to the possible modification in the stereochemistry of the Ti and Mn ions in the interfacial region. The out-of-plane lattice parameter, Curie temperature, and magnetoresistance are strongly affected by the thicknesses of the La0.7Sr0.3MnO3 and Ba0.7Sr0.3TiO3 layers. Huge magnetoresistance subsisting to low temperature was also observed in the La0.7Sr0.3MnO3/Ba0.7Sr0.3TiO3 superlattices. All spectral changes identified at a nanometer scale and their potential effect on the degradation of magnetic and transport properties at a macroscopic level. These findings highlight the importance of dependence on sublayer thickness, illustrating the high degree of tenability in these artificially low-dimensional oxide materials.

16.
Nat Commun ; 8(1): 104, 2017 07 24.
Artigo em Inglês | MEDLINE | ID: mdl-28740076

RESUMO

Oxygen ion transport is the key issue in redox processes. Visualizing the process of oxygen ion migration with atomic resolution is highly desirable for designing novel devices such as oxidation catalysts, oxygen permeation membranes, and solid oxide fuel cells. Here we show the process of electrically induced oxygen migration and subsequent reconstructive structural transformation in a SrCoO2.5-σ film by scanning transmission electron microscopy. We find that the extraction of oxygen from every second SrO layer occurs gradually under an electrical bias; beyond a critical voltage, the brownmillerite units collapse abruptly and evolve into a periodic nano-twined phase with a high c/a ratio and distorted tetrahedra. Our results show that oxygen vacancy rows are not only natural oxygen diffusion channels, but also preferred sites for the induced oxygen vacancies. These direct experimental results of oxygen migration may provide a common mechanism for the electrically induced structural evolution of oxides.Information on how oxygen ions transport is crucial to understanding field-induced phase transformations in materials. Here, Zhang et al. directly image atomic-scale oxygen migration and the subsequent structural reconstruction in a SrCoO2.5-σ film in the presence of an electric field.

17.
ACS Appl Mater Interfaces ; 9(6): 5600-5606, 2017 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-28097864

RESUMO

In this work, the surface structure of a single-domain epitaxial BiFeO3 film with (111) orientation was investigated by in situ grazing incidence X-ray diffraction and X-ray reflectivity. We found that a large strain gradient exists in the surface region (2-3 nm) of the BiFeO3 film. The strain gradient is approximately 107 m-1, which is 2 or 3 orders of magnitude larger than the value inside the film. Moreover, we found that a surface layer with a lower electron density compared with the underlying BiFeO3 layer exists on the surface of BiFeO3 film, and this layer exhibits an irreversible surface structure transition occurs at 500 K, which should be associated with the surface flexoelectric field. We considered that this large strain gradient is originated from the surface depolarization field of ferroelectrics. Our results suggest a coupling between the surface structure and the flexoelectricity and imply that the surface layer and properties would be controlled by the strain gradient in ferroelectric films.

18.
Sci Rep ; 6: 38268, 2016 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-27905565

RESUMO

BiFeO3 thin films have drawn much attention due to its potential applications for novel magnetoelectric devices and fundamental physics in magnetoelectric coupling. However, the structural evolution of BiFeO3 films with thickness remains controversial. Here we use an optical second-harmonic generation technique to explore the phase-related symmetry evolution of BiFeO3 thin films with the variation of thickness. The crystalline structures for 60 and 180-nm-thick BiFeO3 thin films were characterized by high-resolution X-ray diffractometry reciprocal space mapping and the local piezoelectric response for 60-nm-thick BiFeO3 thin films was characterized by piezoresponse force microscopy. The present results show that the symmetry of BiFeO3 thin films with a thickness below 60 nm belongs to the point group 4 mm. We conclude that the disappearance of fourfold rotational symmetry in SHG s-out pattern implies for the appearance of R-phase. The fact that the thinner the film is, the closer to 1 the tensor element ratio χ31/χ15 tends, indicates an increase of symmetry with the decrease of thickness for BiFeO3 thin films.

19.
Sci Rep ; 6: 39306, 2016 12 15.
Artigo em Inglês | MEDLINE | ID: mdl-27976746

RESUMO

Current geological extraction theory and techniques are very limited to adequately characterize the unconventional oil-gas reservoirs because of the considerable complexity of the geological structures. Optical measurement has the advantages of non-interference with the earth magnetic fields, and is often useful in detecting various physical properties. One key parameter that can be detected using optical methods is the dielectric permittivity, which reflects the mineral and organic properties. Here we reported an oblique-incidence reflectivity difference (OIRD) technique that is sensitive to the dielectric and surface properties and can be applied to characterization of reservoir rocks, such as shale and sandstone core samples extracted from subsurface. The layered distribution of the dielectric properties in shales and the uniform distribution in sandstones are clearly identified using the OIRD signals. In shales, the micro-cracks and particle orientation result in directional changes of the dielectric and surface properties, and thus, the isotropy and anisotropy of the rock can be characterized by OIRD. As the dielectric and surface properties are closely related to the hydrocarbon-bearing features in oil-gas reservoirs, we believe that the precise measurement carried with OIRD can help in improving the recovery efficiency in well-drilling process.

20.
ACS Appl Mater Interfaces ; 8(50): 34590-34597, 2016 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-27936535

RESUMO

The defect chemistry of perovskite oxides involves the cause to most of their abundant functional properties, including interface magnetism, charge transport, ionic exchange, and catalytic activity. The possibility to achieve dynamic control over oxygen anion vacancies offers a unique opportunity for the development of appealing switchable devices, which at present are commonly based on ferroelectric materials. Herein, we report the discovery of a switchable photovoltaic effect, that the sign of the open voltage and the short circuit current can be reversed by inverting the polarity of the applied field, upon electrically tailoring the distribution of oxygen vacancies in perovskite oxide films. This phenomenon is demonstrated in lateral photovoltaic devices based on both ferroelectric BiFeO3 and paraelectric SrTiO3 films, under a reversed applied field whose magnitude is much smaller than the coercivity value of BiFeO3. The migration of oxygen vacancies was directly observed by employing an advanced annular bright-field scanning transmission electron microscopy technique with in situ biasing equipment. We conclude that the band bending induced by the motion of oxygen vacancies is the driving force for the reversible switching between two photovoltaic states. The present work can provide an active path for the design of novel switchable photovoltaic devices with a wide range of transition metal oxides in terms of the ionic degrees of freedom.

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