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1.
Nanotechnology ; 33(40)2022 Jul 13.
Artigo em Inglês | MEDLINE | ID: mdl-35705009

RESUMO

The electron and heat transports in solids are through the movement of carrier electrons and quantized lattice vibrations (phonons), which are sensitive to the lattice distortion and ionized impurities, and are essential aspects for the development of novel thermoelectric materials. In this study, we systematically investigated the modulations of electrical and thermal conductivities of BaTi1-xNbxO3solid solution (BTNO, 0 ≤ x ≤ 1) epitaxial films. At room temperature, BaTiO3belongs to tetragonal perovskite and exhibits electron conduction through doubly degenerated Ti 3d-t2gorbitals upon doping, while BaNbO3belongs to cubic perovskite and exhibits metallic electron conduction through partially filled triply degenerate Nb 4d-t2gorbitals. By controlling the Ti/Nb ratio, we found a dual modulation effect on both the lattice structures and conduction band, which affects the electrical and thermal conductivities. Similar to the SrTi1-xNbxO3solid solution (STNO, 0 ≤ x ≤ 1) system, a phase transition was detected atx âˆ¼ 0.5, at which both the electron and heat transports exhibit abrupt changes. Unlike the transition in STNO, which was attributed to a polaronic phase transition, the transition in BTNO was due to contributions from both the lattice distortion and polaron effect. By controlling the lattice distortion, conduction band, and polaronic phase transitions, the electrical and thermal conductivity of BTNO epitaxial films are modulated within a much greater range than those of the STNO epitaxial films. Due to the double contribution of electron carriers and phonon to thermal conductivity (κ), the maximumκmodulation ratio of BTNO epitaxial films was ∼6.9. Our research provides an effective route to design electrical/thermal management materials.

2.
Nano Lett ; 21(14): 6282-6288, 2021 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-34279972

RESUMO

Lithium lanthanum titanate (LLTO) is one of the excellent candidates for an electrolyte in the all-solid-state Li-ion battery, owing to the high Li-ion conductivity in the bulk. However, the Li-ion conductivity at the grain boundary (GB) is largely reduced, and it is therefore important to reveal the origin of Li-ion conductivity reduction at the GB. Here, by using atomic-resolution scanning transmission electron microscopy combined with atomic force microscopy, we investigate the charge states, Li-ion conductivities, atomic and electronic structures at the LLTO Σ5 and Σ13 GBs. Although the Σ5 GB has no significant influence on Li-ion conductivity, the Σ13 GB shows the evident reduction of Li-ion conductivity. We further elucidate that the Σ13 GB is positively charged by the formation of oxygen vacancies at the GB. Such a positive charge would form the Li-ion depletion layers adjacent to the GB, which causes the significant reduction of Li-ion conductivity.

3.
Nano Lett ; 21(21): 9217-9223, 2021 Nov 10.
Artigo em Inglês | MEDLINE | ID: mdl-34724619

RESUMO

Polycrystalline anatase titanium dioxide has drawn great interest, because of its potential applications in high-efficiency photovoltaics and photocatalysts. There has been speculation on the electronic properties of grain boundaries but little direct evidence, because grain boundaries in anatase are challenging to probe experimentally and to model. We present a combined experimental and theoretical study of anatase grain boundaries that have been fabricated by epitaxial growth on a bicrystalline substrate, allowing accurate atomic-scale models to be determined. The electronic structure in the vicinity of stoichiometric grain boundaries is relatively benign to device performance but segregation of oxygen vacancies introduces barriers to electron transport, because of the development of a space charge region. An intrinsically oxygen-deficient boundary exhibits charge trapping consistent with electron energy loss spectroscopy measurements. We discuss strategies for the synthesis of polycrystalline anatase in order to minimize the formation of such deleterious grain boundaries.

4.
Nano Lett ; 21(13): 5586-5592, 2021 Jul 14.
Artigo em Inglês | MEDLINE | ID: mdl-34138575

RESUMO

Dislocations often exhibit unique physical properties distinct from those of the bulk material. However, functional applications of dislocations are challenging due to difficulties in the construction of high-performance devices of dislocations. Here we demonstrate unidirectional single-dislocation Schottky diode arrays in a Fe2O3 thin film on Nb-doped SrTiO3 substrates. Conductivity measurements using conductive atomic force microscopy indicate that a net current will flow through individual dislocation Schottky diodes under forward bias and disappear under reverse bias. Under cyclic bias voltages, the single-dislocation Schottky diodes exhibit a distinct resistive switching behavior containing low-resistance and high-resistance states with a high resistance ratio of ∼103. A combined study of transmission electron microscopy and first-principles calculations reveals that the Fe2O3 dislocations comprise mixed Fe2+ and Fe3+ ions due to O deficiency and exhibit a one-dimensional electrical conductivity. The single-dislocation Schottky diodes may find applications for developing ultrahigh-density electronic and memory devices.

5.
Nano Lett ; 20(2): 1047-1053, 2020 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-31877055

RESUMO

Ferroelectricity and electrical conductivity are two fundamentally incompatible properties that are difficult to simultaneously achieve in a material. Here, we combine these two contradictory properties by embedding conducting SrNbO3 micro/nanopillars into a ferroelectric SrNbO3.5 (i.e., Sr2Nb2O7) thin film. The high-Tc ferroelectric SrNbO3.5 thin film is epitaxially grown on a LaAlO3 substrate by pulsed laser deposition. The conducting SrNbO3 micro/nanopillars are introduced into the film via an electron-irradiation-induced SrNbO3.5-to-SrNbO3 phase transformation triggered by a focused electron beam. The sizes and distribution of the SrNbO3 micro/nanopillars can be accurately controlled through artificial manipulation of the electron-irradiation-induced SrNbO3.5-to-SrNbO3 phase transformation. The ferroelectric SrNbO3/SrNbO3.5 thin film with an in-plane polarization exhibits an electrical conductivity in the out-of-plane direction. Such conducting ferroelectric thin films may lead to the discovery of plentiful physical phenomena and have great potential for pyroelectric, photoelectric, and multiferroic applications.

6.
Phys Rev Lett ; 124(2): 026401, 2020 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-32004053

RESUMO

Artificial crystals synthesized by atomic-scale epitaxy provide the ability to control the dimensions of the quantum phases and associated phase transitions via precise thickness modulation. In particular, the reduction in dimensionality via quantized control of atomic layers is a powerful approach to revealing hidden electronic and magnetic phases. Here, we demonstrate a dimensionality-controlled and induced metal-insulator transition (MIT) in atomically designed superlattices by synthesizing a genuine two-dimensional (2D) SrRuO_{3} crystal with highly suppressed charge transfer. The tendency to ferromagnetically align the spins in an SrRuO_{3} layer diminishes in 2D as the interlayer exchange interaction vanishes, accompanying the 2D localization of electrons. Furthermore, electronic and magnetic instabilities in the two SrRuO_{3} unit cell layers induce a thermally driven MIT along with a metamagnetic transition.

7.
J Chem Phys ; 152(3): 034705, 2020 Jan 21.
Artigo em Inglês | MEDLINE | ID: mdl-31968952

RESUMO

Localized surface plasmon resonances (LSPRs) are gaining considerable attention due to the unique far-field and near-field optical properties and applications. Additionally, the Fermi energy, which is the chemical potential, of plasmonic nanoparticles is one of the key properties to control hot-electron and -hole transfer at the interface between plasmonic nanoparticles and a semiconductor. In this article, we tried to control the diffusion potential of the plasmonic system by manipulating the interface dipole. We fabricated solid-state photoelectric conversion devices in which gold nanoparticles (Au-NPs) are located between strontium titanate (SrTiO3) as an electron transfer material and nickel oxide (NiO) as a hole transport material. Lanthanum aluminate as an interface dipole layer was deposited on the atomic layer scale at the three-phase interface of Au-NPs, SrTiO3, and NiO, and the effect was investigated by photoelectric measurements. Importantly, the diffusion potential between the plasmonic metal and a semiconductor can be arbitrarily controlled by the averaged thickness and direction of the interface dipole layer. The insertion of an only one unit cell (uc) interface dipole layer, whose thickness was less than 0.5 nm, dramatically controlled the diffusion potential formed between the plasmonic nanoparticles and surrounding media. This is a new methodology to control the plasmonic potential without applying external stimuli, such as an applied potential or photoirradiation, and without changing the base materials. In particular, it is very beneficial for plasmonic devices in that the interface dipole has the ability not only to decrease but also to increase the open-circuit voltage on the order of several hundreds of millivolts.

8.
Small ; 15(8): e1805394, 2019 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-30698912

RESUMO

The transparent oxide semiconductor (TOS) with large bandgap (Eg ≈ 4 eV) based thin-film transistors (TFTs) showing both high carrier mobility and UV-visible transparency has attracted increasing attention as a promising component for next generation optoelectronics. Among TOSs, BaSnO3 -SrSnO3 solid-solutions (Eg = 3.5-4.2 eV) are good candidates because the single crystal shows very high mobility. However, the TFT performance has not been optimized due to the lack of fundamental knowledge especially the effective thickness (teff ) and the carrier effective mass (m*). Here, it is demonstrated that the electric field thermopower (S) modulation method addresses this problem by combining with the standard volume carrier concentration (n3D ) dependence of S measurements. By comparing the electric field accumulated sheet carrier concentration (n2D ) and n3D at same S, it is clarified that the teff (n2D /n3D ) of the conducting channel becomes thicker with increasing Sr concentration, whereas the m* becomes lighter. The former would be due to the increase of Eg and latter would be due to the enhancement of overlap population of neighboring Sn 5s orbitals. The present analyses technique is useful to experimentally clarify the teff and m*, and essentially important to realize advanced TOS-based TFTs showing both high optical transparency and high mobility.

9.
Nano Lett ; 17(10): 6140-6145, 2017 10 11.
Artigo em Inglês | MEDLINE | ID: mdl-28902517

RESUMO

Demands on high-quality layer structured two-dimensional (2D) thin films such as pnictogen chalcogenides and transition metal dichalcogenides are growing due to the findings of exotic physical properties and potentials for device applications. However, the difficulties in controlling epitaxial growth and the unclear understanding of van der Waals epitaxy (vdWE) for a 2D chalcogenide film on a three-dimensional (3D) substrate have been major obstacles for the further advances of 2D materials. Here, we exploit the spontaneous vdWE of a high-quality 2D chalcogenide (Bi0.5Sb1.5Te3) film by the chalcogen-driven surface reconstruction of a conventional 3D sapphire substrate. It is verified that the in situ formation of a pseudomorphic Te atomic monolayer on the surface of sapphire, which results in a dangling bond-free surface, allows the spontaneous vdWE of 2D chalcogenide film. Since this route uses the natural surface reconstruction of sapphire with chalcogen under vacuum condition, it can be scalable and easily utilized for the developments of various 2D chalcogenide vdWE films through conventional thin-film fabrication technologies.

10.
J Clin Biochem Nutr ; 56(2): 123-31, 2015 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-25759518

RESUMO

Lysine-specific demethylase 1 (LSD1/KDM1A), a histone-modifying enzyme, is upregulated in many cancers, especially in neuroblastoma, breast cancer and hepatoma. We have established a simple method to measure LSD1 activity using a synthetic N-terminal 21-mer peptide of histone H3, which is dimethylated at Lys-4 (H3K4me2). After the enzyme reaction, a substrate of H3K4me2 and two demethylated products, H3K4me1 and H3K4me0, were quantitatively determined by flow injection time-of-flight mass spectrometry (FI-TOF/MS). By using recombinant human LSD1, a nonlinear fitting simulation of the data obtained by FI-TOF/MS produced typical consecutive-reaction kinetics. Apparent K m and k cat values of hLSD1 for the first and second demethylation reactions were found to be in the range of reported values. Tranylcypromine was shown to inhibit LSD1 activity with an IC50 of 6.9 µM for the first demethylation reaction and 5.8 µM for the second demethylation reaction. The FI-TOF/MS assay revealed that the endogenous LSD1 activity was higher in the nuclear extracts of SH-SY5Y cells than in HeLa or PC-3 cells, and this is in accordance with the immunoblotting data using an anti-LSD1 antibody. A simple, straightforward FI-TOF/MS assay is described to efficiently measure LSD1 activity in the nuclear extracts of cultured cells.

11.
Nat Mater ; 12(11): 1057-63, 2013 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-23975056

RESUMO

Fast, reversible redox reactions in solids at low temperatures without thermomechanical degradation are a promising strategy for enhancing the overall performance and lifetime of many energy materials and devices. However, the robust nature of the cation's oxidation state and the high thermodynamic barrier have hindered the realization of fast catalysis and bulk diffusion at low temperatures. Here, we report a significant lowering of the redox temperature by epitaxial stabilization of strontium cobaltites (SrCoO(x)) grown directly as one of two distinct crystalline phases, either the perovskite SrCoO(3-δ) or the brownmillerite SrCoO(2.5). Importantly, these two phases can be reversibly switched at a remarkably reduced temperature (200-300 °C) in a considerably short time (< 1 min) without destroying the parent framework. The fast, low-temperature redox activity in SrCoO(3-δ) is attributed to a small Gibbs free-energy difference between two topotatic phases. Our findings thus provide useful information for developing highly sensitive electrochemical sensors and low-temperature cathode materials.

12.
ACS Appl Mater Interfaces ; 16(14): 17832-17837, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38557007

RESUMO

Hexagonal rare-earth iron oxides (h-RFeO3) exhibit spontaneous magnetization and room-temperature ferroelectricity simultaneously. However, achieving a large magnetoelectric coupling necessitates further exploration. Herein, we report the impact of the magnetic phase transition on the ferroelectric properties of epitaxial h-RFeO3 (R = Tb and Ho) films prepared by pulsed laser deposition. The metastable h-RFeO3 phase is successfully stabilized with high crystallinity and low leakage current due to the ITO buffer layer, making it possible to investigate the ferroelectric properties. The h-TbFeO3 film exhibits a magnetic-field-induced transition from antiferromagnetic (AFM) to weak ferromagnetic (wFM) phases below 30 K, while also exhibiting ferroelectricity at 300 K. The dielectric constants change with the magnetic phase transition, demonstrating hysteresis in the magnetocapacitance. In contrast, the h-HoFeO3 film exhibits antiferroelectric-like behavior and an AFM-wFM phase transition. Notably, the h-HoFeO3 film shows a rapid increase in the remnant polarization during the AFM-wFM phase transition accompanied by an increase in the ferroelectric component. Considering the strong connection between the antiferroelectric behavior in the h-RFeO3 system and the ferroelectric domain wall motion, this considerable modification of ferroelectric properties during the magnetic phase transition is probably due to the faster movement of the ferroelectric domain walls in the wFM phase induced by the clamping effect. Our findings indicate the effectiveness of magnetic phase transitions in enhancing the magnetoelectric coupling, particularly when utilizing domain wall clamping properties.

13.
Adv Sci (Weinh) ; : e2401331, 2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38923788

RESUMO

Thermal switches that switch the thermal conductivity (κ) of the active layers are attracting increasing attention as thermal management devices. For electrochemical thermal switches, several transition metal oxides (TMOs) are proposed as active layers. After electrochemical redox treatment, the crystal structure of the TMO is modulated, which results in the κ switching. However, the κ switching width is still small (<4 W m-1 K-1). In this study, it demonstrates that LaNiOx-based solid-state electrochemical thermal switches have a κ switching width of 4.3 W m-1 K-1. Fully oxidized LaNiO3 (on state) has a κ of 6.0 W m-1 K-1 due to the large contribution of electron thermal conductivity (κele, 3.1 W m-1 K-1). In contrast, reduced LaNiO2.72 (off state) has a κ of 1.7 W m-1 K-1 because the phonons are scattered by the oxygen vacancies. The LaNiOx-based electrochemical thermal switch is cyclable of κ and the crystalline lattice of LaNiOx. This electrochemical thermal switch may be a promising platform for next-generation devices such as thermal displays.

14.
Dalton Trans ; 52(19): 6317-6323, 2023 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-37079005

RESUMO

La-doped BaSnO3 (LBSO), which exhibits both high electron mobility and visible-light transparency, is a promising transparent electrode/transistor material that does not require expensive elements such as indium. However, because a high crystal orientation is necessary for high mobility, the development of a synthetic technique is crucial for next-generation optoelectronic applications. One promising method for achieving this is the lift-off and transfer method. Epitaxial films are first deposited on single-crystal substrates, peeled off from the substrates, and subsequently transferred onto other substrates. However, such transferred sheets typically contain a high density of cracks. Therefore, LBSO sheets with flexibility, high mobility, and transparency have not yet been reported. In this study, we successfully synthesized crack-free LBSO epitaxial sheets via a lift-off and transfer method using a water-soluble Sr3Al2O6 sacrificial layer and amorphous (a-)Al2O3 protection layer. The LBSO sheet simultaneously exhibited a high electron mobility of 80 cm2 V-1 s-1 and a wide optical bandgap of 3.5 eV owing to the epitaxial crystallinity of the sheet. Moreover, two types of LBSO sheets were prepared, flat and rolled sheets, by tuning the lift-off process. The flat sheet had a lateral size of 5 mm × 5 mm, whereas the rolled sheet had a tube shape with a height of 5 mm and a diameter of 1 mm. Such large crack-free area and flexibility were achieved in LBSO sheets owing to the use of the a-Al2O3 protection layer.

15.
ACS Appl Mater Interfaces ; 15(13): 16842-16852, 2023 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-36952672

RESUMO

Amorphous metal oxides with analog resistive switching functions (i.e., continuous controllability of the electrical resistance) are gaining emerging interest due to their neuromorphic functionalities promising for energy efficient electronics. The mechanisms are currently attributed to field-driven migration of the constituent ions, but the applications are being hindered by the limited understanding of the physical mechanisms due to the difficulty in analyzing the causal ion migration, which occurs on a nanometer or even atomic scale. Here, the direct electrical transport measurement of analog resistive switching and ångström scale imaging of the causal ion migration is demonstrated in amorphous TaOx (a-TaOx) by conductive atomic force microscopy. Atomically flat thin films of a-TaOx, which is a practical material for commercial resistive random access memory, are fabricated in this study, and the mechanisms of the three known types of analog resistive switching phenomena (current-dependent set, voltage-dependent reset, and time-dependent switching) are directly visualized on the surfaces. The observations indicate that highly analog type of resistive switching can be induced in a-TaOx by inducing the continuous redox reactions for 2.0 < x < 2.5, which are characteristic of a-TaOx. The measurements also demonstrate drastic control of the switching stochasticity, which is attributable to controlled segregation of a metastable a-TaO2 phase. The findings provide direct clues for tuning the analog resistive switching characteristics of amorphous metal oxides and developing new functions for future neuromorphic computing.

16.
ACS Appl Mater Interfaces ; 15(19): 23512-23517, 2023 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-37134115

RESUMO

Thermal transistors have potential as thermal management devices because they can electrically control the thermal conductivity (κ) of the active layer. Recently, we realized solid-state electrochemical thermal transistors by utilizing the electrochemical redox reaction of SrCoOy (2 ≤ y ≤ 3). However, the guiding principle to improve the on/off κ ratio has yet to be clarified because the κ modulation mechanism is unclear. This study systematically modulates κ of SrCo1-xFexOy (0 ≤ x ≤ 1, 2 ≤ y ≤ 3) solid solutions used as the active layers in solid-state electrochemical thermal transistors. When y = 3, the lattice κ of SrCo1-xFexOy is ∼2.8 W m-1 K-1 and insensitive to x. When x = 0 and y = 3, κ increases to ∼3.8 W m-1 K-1 due to the contribution of the electron κ. When y = 2, κ slightly depends on the ordered atomic arrangement. Materials that are high electrical conductors with highly ordered lattices when the transistor is on but are electrical insulators with disordered lattices when the transistor is off should be well-suited for the active layers of solid-state electrochemical thermal transistors.

17.
ACS Nano ; 16(12): 21013-21019, 2022 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-36411060

RESUMO

Flexible and functional perovskite oxide sheets with high orientation and crystallization are the next step in the development of next-generation devices. One promising synthesis method is the lift-off and transfer method using a water-soluble sacrificial layer. However, the suppression of cracks during lift-off is a crucial problem that remains unsolved. In this study, we demonstrated that this problem can be solved by depositing amorphous Al2O3 capping layers on oxide sheets. Using this simple method, over 20 mm2 of crack-free, deep-ultraviolet transparent electrode La:SrSnO3 and ferroelectric Ba0.75Sr0.25TiO3 flexible sheets were obtained. By contrast, the sheets without any capping layers broke. The obtained sheets showed considerable flexibility and high functionality. The La:SrSnO3 sheet simultaneously exhibited a wide bandgap (4.4 eV) and high electrical conductivity (>103 S/cm). The Ba0.75Sr0.25TiO3 sheet exhibited clear room-temperature ferroelectricity with a remnant polarization of 17 µC/cm2. Our findings provide a simple transfer method for obtaining large, crack-free, high-quality, single-crystalline sheets.

18.
Sci Adv ; 8(15): eabl6192, 2022 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-35427155

RESUMO

In a ferromagnetic Weyl metal SrRuO3, a large effective magnetic field Heff exerted on a magnetic domain wall (DW) by current has been reported. We show that the ratio of Heff to current density exhibits nonmonotonic temperature dependence and surpasses those of conventional spin-transfer torques and spin-orbit torques. This enhancement is described well by topological Hall torque (THT), which is exerted on a DW by Weyl electrons emerging around Weyl points when an electric field is applied across the DW. The ratio of the Heff arising from the THT to current density is over one order of magnitude higher than that originating from spin-transfer torques and spin-orbit torques reported in metallic systems, showing that the THT may provide a better way for energy-efficient manipulation of magnetization in spintronics devices.

19.
Artigo em Inglês | MEDLINE | ID: mdl-35819907

RESUMO

Thermoelectric energy conversion technology has attracted attention as an energy harvesting technology that converts waste heat into electricity by means of the Seebeck effect. Oxide-based thermoelectric materials that show a high figure of merit are promising because of their good chemical and thermal stability as well as their harmless nature compared to chalcogenide-based state-of-the-art thermoelectric materials. Although several high-ZT thermoelectric oxides (ZT > 1) have been reported thus far, the reliability is low due to a lack of careful observation of their stability at elevated temperatures. Here, we show a reliable high-ZT thermoelectric oxide, Ba1/3CoO2. We fabricated Ba1/3CoO2 epitaxial films by the reactive solid-phase epitaxy method (Na3/4CoO2) followed by ion exchange (Na+ → Ba2+) treatment and performed thermal annealing of the film at high temperatures and structural and electrical measurements. The crystal structure and electrical resistivity of the Ba1/3CoO2 epitaxial films were found to be maintained up to 600 °C. The power factor gradually increased to ∼1.2 mW m-1 K-2 and the thermal conductivity gradually decreased to ∼1.9 W m-1 K-1 with increasing temperature up to 600 °C. Consequently, the ZT reached ∼0.55 at 600 °C in air.

20.
Nano Lett ; 10(11): 4668-72, 2010 Nov 10.
Artigo em Inglês | MEDLINE | ID: mdl-20977250

RESUMO

Determining both cation and oxygen sublattices of grain boundaries is essential to understand the properties of oxides. Here, with scanning transmission electron microscopy, electron energy-loss spectroscopy, and first-principles calculations, both the Ce and oxygen sublattices of a (210)Σ5 CeO(2) grain boundary were determined. Oxygen vacancies are shown to play a crucial role in the stable grain boundary structure. This finding paves the way for a comprehensive understanding of grain boundaries through the atomic scale determination of atom and defect locations.


Assuntos
Cério/química , Modelos Químicos , Modelos Moleculares , Oxigênio/química , Simulação por Computador , Teste de Materiais , Conformação Molecular , Transição de Fase
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