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1.
Nat Commun ; 11(1): 606, 2020 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-32001696

RESUMO

Manipulating liquids with tunable shape and optical functionalities in real time is important for electroactive flow devices and optoelectronic devices, but remains a great challenge. Here, we demonstrate electrotunable liquid sulfur microdroplets in an electrochemical cell. We observe electrowetting and merging of sulfur droplets under different potentiostatic conditions, and successfully control these processes via selective design of sulfiphilic/sulfiphobic substrates. Moreover, we employ the electrowetting phenomena to create a microlens based on the liquid sulfur microdroplets and tune its characteristics in real time through changing the shape of the liquid microdroplets in a fast, repeatable, and controlled manner. These studies demonstrate a powerful in situ optical battery platform for unraveling the complex reaction mechanism of sulfur chemistries and for exploring the rich material properties of the liquid sulfur, which shed light on the applications of liquid sulfur droplets in devices such as microlenses, and potentially other electrotunable and optoelectronic devices.

2.
Nat Nanotechnol ; 2020 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-31988508

RESUMO

It has recently been shown that sulfur, a solid material in its elementary form S8, can stay in a supercooled state as liquid sulfur in an electrochemical cell. We establish that this newly discovered state could have implications for lithium-sulfur batteries. Here, through in situ studies of electrochemical sulfur generation, we show that liquid (supercooled) and solid elementary sulfur possess very different areal capacities over the same charging period. To control the physical state of sulfur, we studied its growth on two-dimensional layered materials. We found that on the basal plane, only liquid sulfur accumulates; by contrast, at the edge sites, liquid sulfur accumulates if the thickness of the two-dimensional material is small, whereas solid sulfur nucleates if the thickness is large (tens of nanometres). Correlating the sulfur states with their respective areal capacities, as well as controlling the growth of sulfur on two-dimensional materials, could provide insights for the design of future lithium-sulfur batteries.

3.
Nat Commun ; 10(1): 5312, 2019 11 22.
Artigo em Inglês | MEDLINE | ID: mdl-31757949

RESUMO

Two-dimensional heterostructures combined with vertical geometries are candidates to probe and utilize the physical properties of atomically-thin materials. The vertical configuration enables a unique form of hot-carrier spectroscopy as well as atomic-scale devices. Here, we present the room-temperature evolution of heteroepitaxial perovskite hot-electron transistors using a SrRuO3 base down to the monolayer limit (∼4 Å). As a fundamental electronic probe, we observe an abrupt transition in the hot-electron mean free path as a function of base thickness, coinciding with the thickness-dependent resistive transition. As a path towards devices, we demonstrate the integrated synthesis of perovskite one-dimensional electrical edge contacts using water-soluble and growth-compatible Sr3Al2O6 hard masks. Edge-contacted monolayer-base transistors exhibit on/off ratios reaching ∼108, complete electrostatic screening by the base manifesting pure hot-electron injection, and excellent scaling of the output current density with device dimensions. These results open new avenues for incorporating emergent phenomena at oxide interfaces and in heterostructures.

4.
Nano Lett ; 19(11): 8125-8131, 2019 11 13.
Artigo em Inglês | MEDLINE | ID: mdl-31635457

RESUMO

The effects of large external fields on semiconductor nanostructures could reveal much about field-induced shifting of electronic states and their dynamical responses and could enable electro-optic device applications that require large and rapid changes in optical properties. Studies of quasi-dc electric field modulation of quantum dot (QD) properties have been limited by electrostatic breakdown processes observed under high externally applied field levels. To circumvent this, here we apply ultrafast terahertz (THz) electric fields with switching times on the order of 1 ps. We show that a pulsed THz electric field, enhanced by a microslit field enhancement structure (FES), can strongly manipulate the optical absorption properties of a thin film of CdSe and CdSe-CdS core-shell QDs on the subpicosecond time scale with spectral shifts that span the visible to near-IR range. Numerical simulations using a semiempirical tight binding model show that the band gap of the QD film can be shifted by as much a 79 meV during these time scales. The results allow a basic understanding of the field-induced shifting of electronic levels and suggest electro-optic device applications.

5.
Nano Lett ; 19(10): 7293-7300, 2019 10 09.
Artigo em Inglês | MEDLINE | ID: mdl-31499003

RESUMO

A variety of methods including tuning chemical compositions, structures, crystallinity, defects and strain, and electrochemical intercalation have been demonstrated to enhance the catalytic activity. However, none of these tuning methods provide direct dynamical control during catalytic reactions. Here we propose a new method to tune the activity of catalysts through solid-state ion gating manipulation and adjustment (SIGMA) using a catalysis transistor. SIGMA can electrostatically dope the surface of catalysts with a high electron concentration over 5 × 1013 cm-2 and thus modulate both the chemical potential of the reaction intermediates and their electrical conductivity. The hydrogen evolution reaction (HER) on both pristine and defective MoS2 were investigated as model reactions. Our theoretical and experimental results show that the overpotential at 10 mA/cm2 and Tafel slope can be in situ, continuously, dynamically, and reversibly tuned over 100 mV and around 100 mV/dec, respectively.

6.
Nat Commun ; 10(1): 4026, 2019 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-31492862

RESUMO

The single-crystal SrTiO3 (001) has two different surface terminations, TiO2 and SrO. One most remarkable observation in previous studies is that only the heterointerfaces with TiO2-terminated SrTiO3, which usually combines with polar oxides such as LaAlO3, host an electron gas. Here we show that a robust electron gas can be generated between a non-polar oxide, CaHfO3, and SrTiO3 (001) with either termination. Unlike the well-known electron gas of LaAlO3/SrTiO3, the present one of CaHfO3/SrTiO3 essentially has no critical thickness of CaHfO3, can survive a long-time oxygen annealing at high temperature, and its transport properties are stable under exposure to water and other polar solvents. By electrostatic gating through CaHfO3, field-effect devices are demonstrated using CaHfO3/SrTiO3 heterointerfaces with both terminations. These results show that the electron gas reported in the present study is unique and promising for applications in oxide electronics.

7.
Nature ; 572(7771): 624-627, 2019 08.
Artigo em Inglês | MEDLINE | ID: mdl-31462797

RESUMO

The discovery of unconventional superconductivity in (La,Ba)2CuO4 (ref. 1) has motivated the study of compounds with similar crystal and electronic structure, with the aim of finding additional superconductors and understanding the origins of copper oxide superconductivity. Isostructural examples include bulk superconducting Sr2RuO4 (ref. 2) and surface-electron-doped Sr2IrO4, which exhibits spectroscopic signatures consistent with a superconducting gap3,4, although a zero-resistance state has not yet been observed. This approach has also led to the theoretical investigation of nickelates5,6, as well as thin-film heterostructures designed to host superconductivity. One such structure is the LaAlO3/LaNiO3 superlattice7-9, which has been recently proposed for the creation of an artificially layered nickelate heterostructure with a singly occupied [Formula: see text] band. The absence of superconductivity observed in previous related experiments has been attributed, at least in part, to incomplete polarization of the eg orbitals10. Here we report the observation of superconductivity in an infinite-layer nickelate that is isostructural to infinite-layer copper oxides11-13. Using soft-chemistry topotactic reduction14-20, NdNiO2 and Nd0.8Sr0.2NiO2 single-crystal thin films are synthesized by reducing the perovskite precursor phase. Whereas NdNiO2 exhibits a resistive upturn at low temperature, measurements of the resistivity, critical current density and magnetic-field response of Nd0.8Sr0.2NiO2 indicate a superconducting transition temperature of about 9 to 15 kelvin. Because this compound is a member of a series of reduced layered nickelate crystal structures21-23, these results suggest the possibility of a family of nickelate superconductors analogous to copper oxides24 and pnictides25.

8.
Nano Lett ; 19(6): 3999-4003, 2019 06 12.
Artigo em Inglês | MEDLINE | ID: mdl-31136184

RESUMO

Crystalline oxide ferroelectric tunnel junctions enable persistent encoding of information in electric polarization, featuring nondestructive readout and scalability that can exceed current commercial high-speed, nonvolatile ferroelectric memories. However, the well-established fabrication of epitaxial devices on oxide substrates is difficult to adapt to silicon substrates for integration into complementary metal-oxide-semiconductor electronics. In this work, we report ferroelectric tunnel junctions based on 2.8 nm-thick BaTiO3 films grown epitaxially on SrTiO3 growth substrates, released, and relaminated onto silicon. The performance of the transferred devices is comparable to devices characterized on the oxide substrate, suggesting a viable route toward next-generation nonvolatile memories broadly integrable with different materials platforms.

9.
J Phys Chem Lett ; 10(7): 1516-1522, 2019 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-30883127

RESUMO

Understanding how structural properties affect the oxygen evolution reaction (OER) of a catalyst can reveal important information not only on the catalytic mechanism but also on the general design strategy of OER catalysts. We report a variation of ∼0.15 V in the overpotential of the recently discovered IrO x/SrIrO3 OER catalysts, which directly correlates with the structural parameters of the as-synthesized SrIrO3 epitaxial films. This variation is caused by both extrinsic area enhancement and intrinsic electronic structure modification driven by defect formation. These correlations not only indicate that microscopic film defects play an important role in the activity of the IrO x/SrIrO3 catalyst but also provide readily accessible parameters predictive of the activity post-transformation to IrO x/SrIrO3. Establishing strong associations between the catalytic activity and key structural and electronic parameters, rather than synthetic variables, provides important guidance to control and study these complex catalysts independent of the synthetic technique.

10.
Rev Sci Instrum ; 89(10): 103901, 2018 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-30399873

RESUMO

Elastoresistivity, the relation between resistivity and strain, can elucidate the subtle properties of the electronic structure of a material and is an increasingly important tool for the study of strongly correlated materials. To date, elastoresistivity measurements have predominantly been performed with quasi-static (DC) strain. In this work, we demonstrate a method using AC strain in elastoresistivity measurements. A sample experiencing AC strain has a time-dependent resistivity, which modulates the voltage produced by an AC current; this effect produces time-dependent variations in resistivity that are directly proportional to the elastoresistivity, and which can be measured more quickly, with less strain on the sample, and with less stringent requirements for temperature stability than the previous DC technique. Example measurements between 10 Hz and 3 kHz are performed on a material with a large, well-characterized and temperature dependent elastoresistivity: the representative iron-based superconductor Ba(Fe0.975Co0.025)2As2. These measurements yield a frequency independent elastoresistivity and reproduce results from previous DC elastoresistivity methods to within experimental accuracy. We emphasize that the dynamic (AC) elastoresistivity is a distinct material-specific property that has not previously been considered.

11.
Phys Rev Lett ; 121(16): 167003, 2018 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-30387624

RESUMO

We have examined the intrinsic spin-orbit coupling and orbital depairing in thin films of Nb-doped SrTiO_{3} by superconducting tunneling spectroscopy. The orbital depairing is geometrically suppressed in the two-dimensional limit, enabling a quantitative evaluation of the Fermi level spin-orbit scattering using Maki's theory. The response of the superconducting gap under in-plane magnetic fields demonstrates short spin-orbit scattering times τ_{so}≤1.1 ps. Analysis of the orbital depairing indicates that the heavy electron band contributes significantly to pairing. These results suggest that the intrinsic spin-orbit scattering time in SrTiO_{3} is comparable to those associated with Rashba effects in SrTiO_{3} interfacial conducting layers and can be considered significant in all forms of superconductivity in SrTiO_{3}.

12.
Nat Commun ; 9(1): 4570, 2018 10 29.
Artigo em Inglês | MEDLINE | ID: mdl-30374115

RESUMO

The original HTML version of this Article omitted to list Harold Y. Hwang as a corresponding author and incorrectly listed Adrian G. Swartz as a corresponding author. This has been corrected in the HTML version of the Article. The PDF version was correct from the time of publication.

13.
Nat Commun ; 9(1): 4008, 2018 10 01.
Artigo em Inglês | MEDLINE | ID: mdl-30275443

RESUMO

Quantum ground states that arise at atomically controlled oxide interfaces provide an opportunity to address key questions in condensed matter physics, including the nature of two-dimensional metallic behaviour often observed adjacent to superconductivity. At the superconducting LaAlO3/SrTiO3 interface, a metallic ground state emerges upon the collapse of superconductivity with field-effect gating and is accompanied with a pseudogap. Here we utilize independent control of carrier density and disorder of the interfacial superconductor using dual electrostatic gates, which enables the comprehensive examination of the electronic phase diagram approaching zero temperature. We find that the pseudogap corresponds to precursor pairing, and the onset of long-range phase coherence forms a two-dimensional superconducting dome as a function of the dual-gate voltages. The gate-tuned superconductor-metal transitions are driven by macroscopic phase fluctuations of Josephson coupled superconducting puddles.

14.
Nano Lett ; 18(7): 4273-4278, 2018 07 11.
Artigo em Inglês | MEDLINE | ID: mdl-29792812

RESUMO

Pure spin currents, unaccompanied by dissipative charge flow, are essential for realizing energy-efficient nanomagnetic information and communications devices. Thin-film magnetic insulators have been identified as promising materials for spin-current technology because they are thought to exhibit lower damping compared with their metallic counterparts. However, insulating behavior is not a sufficient requirement for low damping, as evidenced by the very limited options for low-damping insulators. Here, we demonstrate a new class of nanometer-thick ultralow-damping insulating thin films based on design criteria that minimize orbital angular momentum and structural disorder. Specifically, we show ultralow damping in <20 nm thick spinel-structure magnesium aluminum ferrite (MAFO), in which magnetization arises from Fe3+ ions with zero orbital angular momentum. These epitaxial MAFO thin films exhibit a Gilbert damping parameter of ∼0.0015 and negligible inhomogeneous linewidth broadening, resulting in narrow half width at half-maximum linewidths of ∼0.6 mT around 10 GHz. Our findings offer an attractive thin-film platform for enabling integrated insulating spintronics.

15.
Nano Lett ; 18(4): 2387-2392, 2018 04 11.
Artigo em Inglês | MEDLINE | ID: mdl-29580055

RESUMO

Electric-double-layer (EDL) gating with liquid electrolyte has been a powerful tool widely used to explore emerging interfacial electronic phenomena. Due to the large EDL capacitance, a high carrier density up to 1014 cm-2 can be induced, directly leading to the realization of field-induced insulator to metal (or superconductor) transition. However, the liquid nature of the electrolyte has created technical issues including possible side electrochemical reactions or intercalation, and the potential for huge strain at the interface during cooling. In addition, the liquid coverage of active devices also makes many surface characterizations and in situ measurements challenging. Here, we demonstrate an all solid-state EDL device based on a solid superionic conductor LaF3, which can be used as both a substrate and a fluorine ionic gate dielectric to achieve a wide tunability of carrier density without the issues of strain or electrochemical reactions and can expose the active device surface for external access. Based on LaF3 EDL transistors (EDLTs), we observe the metal-insulator transition in MoS2. Interestingly, the well-defined crystal lattice provides a more uniform potential distribution in the substrate, resulting in less interface electron scattering and therefore a higher mobility in MoS2 transistors. This result shows the powerful gating capability of LaF3 solid electrolyte for new possibilities of novel interfacial electronic phenomena.

16.
Proc Natl Acad Sci U S A ; 115(7): 1475-1480, 2018 02 13.
Artigo em Inglês | MEDLINE | ID: mdl-29382769

RESUMO

The nature of superconductivity in the dilute semiconductor SrTiO3 has remained an open question for more than 50 y. The extremely low carrier densities ([Formula: see text]-[Formula: see text] cm-3) at which superconductivity occurs suggest an unconventional origin of superconductivity outside of the adiabatic limit on which the Bardeen-Cooper-Schrieffer (BCS) and Migdal-Eliashberg (ME) theories are based. We take advantage of a newly developed method for engineering band alignments at oxide interfaces and access the electronic structure of Nb-doped SrTiO3, using high-resolution tunneling spectroscopy. We observe strong coupling to the highest-energy longitudinal optic (LO) phonon branch and estimate the doping evolution of the dimensionless electron-phonon interaction strength ([Formula: see text]). Upon cooling below the superconducting transition temperature ([Formula: see text]), we observe a single superconducting gap corresponding to the weak-coupling limit of BCS theory, indicating an order of magnitude smaller coupling ([Formula: see text]). These results suggest that despite the strong normal state interaction with electrons, the highest LO phonon does not provide a dominant contribution to pairing. They further demonstrate that SrTiO3 is an ideal system to probe superconductivity over a wide range of carrier density, adiabatic parameter, and electron-phonon coupling strength.

17.
Nano Lett ; 18(2): 1410-1415, 2018 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-29385803

RESUMO

Layered metal chalcogenide materials provide a versatile platform to investigate emergent phenomena and two-dimensional (2D) superconductivity at/near the atomically thin limit. In particular, gate-induced interfacial superconductivity realized by the use of an electric-double-layer transistor (EDLT) has greatly extended the capability to electrically induce superconductivity in oxides, nitrides, and transition metal chalcogenides and enable one to explore new physics, such as the Ising pairing mechanism. Exploiting gate-induced superconductivity in various materials can provide us with additional platforms to understand emergent interfacial superconductivity. Here, we report the discovery of gate-induced 2D superconductivity in layered 1T-SnSe2, a typical member of the main-group metal dichalcogenide (MDC) family, using an EDLT gating geometry. A superconducting transition temperature Tc ≈ 3.9 K was demonstrated at the EDL interface. The 2D nature of the superconductivity therein was further confirmed based on (1) a 2D Tinkham description of the angle-dependent upper critical field Bc2, (2) the existence of a quantum creep state as well as a large ratio of the coherence length to the thickness of superconductivity. Interestingly, the in-plane Bc2 approaching zero temperature was found to be 2-3 times higher than the Pauli limit, which might be related to an electric field-modulated spin-orbit interaction. Such results provide a new perspective to expand the material matrix available for gate-induced 2D superconductivity and the fundamental understanding of interfacial superconductivity.

18.
Top Curr Chem (Cham) ; 376(1): 6, 2018 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-29362935

RESUMO

Multidimensional spectroscopy in the visible and infrared spectral ranges has become a powerful technique to retrieve dynamic correlations and couplings in wide-ranging systems by utilizing multiple correlated light-matter interactions. Its extension to the terahertz (THz) regime of the electromagnetic spectrum, where rich material degrees of freedom reside, however, has been progressing slowly. This chapter reviews some of the THz-frequency two-dimensional (2D) spectroscopy techniques and experimental results realized in recent years. Examples include gas molecule rotations, spin precessions in magnetic systems, and liquid molecular dynamics studied by 2D THz or hybrid 2D THz-Raman spectroscopy techniques. The methodology shows promising applications to different THz-frequency degrees of freedom in various chemical systems and processes.


Assuntos
Espectroscopia Terahertz , Simulação de Dinâmica Molecular
19.
Sci Adv ; 3(11): eaao5173, 2017 11.
Artigo em Inglês | MEDLINE | ID: mdl-29167822

RESUMO

Long-range order and phase transitions in two-dimensional (2D) systems-such as magnetism, superconductivity, and crystallinity-have been important research topics for decades. The issue of 2D crystalline order has reemerged recently, with the development of exfoliated atomic crystals. Understanding the dimensional limit of crystalline phases, with different types of bonding and synthetic techniques, is at the foundation of low-dimensional materials design. We study ultrathin membranes of SrTiO3, an archetypal perovskite oxide with isotropic (3D) bonding. Atomically controlled membranes are released after synthesis by dissolving an underlying epitaxial layer. Although all unreleased films are initially single-crystalline, the SrTiO3 membrane lattice collapses below a critical thickness (5 unit cells). This crossover from algebraic to exponential decay of the crystalline coherence length is analogous to the 2D topological Berezinskii-Kosterlitz-Thouless (BKT) transition. The transition is likely driven by chemical bond breaking at the 2D layer-3D bulk interface, defining an effective dimensional phase boundary for coherent crystalline lattices.

20.
Nat Mater ; 16(12): 1203-1208, 2017 12.
Artigo em Inglês | MEDLINE | ID: mdl-28920939

RESUMO

Electrostatic fields tune the ground state of interfaces between complex oxide materials. Electronic properties, such as conductivity and superconductivity, can be tuned and then used to create and control circuit elements and gate-defined devices. Here we show that naturally occurring twin boundaries, with properties that are different from their surrounding bulk, can tune the LaAlO3/SrTiO3 interface 2DEG at the nanoscale. In particular, SrTiO3 domain boundaries have the unusual distinction of remaining highly mobile down to low temperatures, and were recently suggested to be polar. Here we apply localized pressure to an individual SrTiO3 twin boundary and detect a change in LaAlO3/SrTiO3 interface current distribution. Our data directly confirm the existence of polarity at the twin boundaries, and demonstrate that they can serve as effective tunable gates. As the location of SrTiO3 domain walls can be controlled using external field stimuli, our findings suggest a novel approach to manipulate SrTiO3-based devices on the nanoscale.

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