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1.
Proc Natl Acad Sci U S A ; 116(47): 23404-23409, 2019 Nov 19.
Artigo em Inglês | MEDLINE | ID: mdl-31685626

RESUMO

Phase transitions in halide perovskites triggered by external stimuli generate significantly different material properties, providing a great opportunity for broad applications. Here, we demonstrate an In-based, charge-ordered (In+/In3+) inorganic halide perovskite with the composition of Cs2In(I)In(III)Cl6 in which a pressure-driven semiconductor-to-metal phase transition exists. The single crystals, synthesized via a solid-state reaction method, crystallize in a distorted perovskite structure with space group I4/m with a = 17.2604(12) Å, c = 11.0113(16) Å if both the strong reflections and superstructures are considered. The supercell was further confirmed by rotation electron diffraction measurement. The pressure-induced semiconductor-to-metal phase transition was demonstrated by high-pressure Raman and absorbance spectroscopies and was consistent with theoretical modeling. This type of charge-ordered inorganic halide perovskite with a pressure-induced semiconductor-to-metal phase transition may inspire a range of potential applications.

2.
Adv Mater ; 31(48): e1904991, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31549760

RESUMO

Lithium metal anodes with high energy density are important for further development of next-generation batteries. However, inhomogeneous Li deposition and dendrite growth hinder their practical utilization. 3D current collectors are widely investigated to suppress dendrite growth, but they usually occupy a large volume and increase the weight of the system, hence decreasing the energy density. Additionally, the nonuniform distribution of Li ions results in low utilization of the porous structure. A lightweight, 3D Cu nanowire current collector with a phosphidation gradient is reported to balance the lithiophilicity with conductivity of the electrode. The phosphide gradient with good lithiophilicity and high ionic conductivity enables dense nucleation of Li and its steady deposition in the porous structure, realizing a high pore utilization. Specifically, the homogenous deposition of Li leads to the formation of an oriented texture on the electrode surface at high capacities. A high mass loading (≈44 wt%) of Li with a capacity of 3 mAh cm-2 and a high average Coulombic efficiency of 97.3% are achieved. A lifespan of 300 h in a symmetrical cell is obtained at 2 mA cm-2 , implying great potential to stabilize lithium metal.

3.
Nano Lett ; 19(6): 3830-3837, 2019 06 12.
Artigo em Inglês | MEDLINE | ID: mdl-31059272

RESUMO

Considerable advances in manipulating heat flow in solids have been made through the innovation of artificial thermal structures such as thermal diodes, camouflages, and cloaks. Such thermal devices can be readily constructed only at the macroscale by mechanically assembling different materials with distinct values of thermal conductivity. Here, we extend these concepts to the microscale by demonstrating a monolithic material structure on which nearly arbitrary microscale thermal metamaterial patterns can be written and programmed. It is based on a single, suspended silicon membrane whose thermal conductivity is locally, continuously, and reversibly engineered over a wide range (between 2 and 65 W/m·K) and with fine spatial resolution (10-100 nm) by focused ion irradiation. Our thermal cloak demonstration shows how ion-write microthermotics can be used as a lithography-free platform to create thermal metamaterials that control heat flow at the microscale.

4.
Proc Natl Acad Sci U S A ; 116(19): 9186-9190, 2019 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-31004055

RESUMO

Graphene-based nanodevices have been developed rapidly and are now considered a strong contender for postsilicon electronics. However, one challenge facing graphene-based transistors is opening a sizable bandgap in graphene. The largest bandgap achieved so far is several hundred meV in bilayer graphene, but this value is still far below the threshold for practical applications. Through in situ electrical measurements, we observed a semiconducting character in compressed trilayer graphene by tuning the interlayer interaction with pressure. The optical absorption measurements demonstrate that an intrinsic bandgap of 2.5 ± 0.3 eV could be achieved in such a semiconducting state, and once opened could be preserved to a few GPa. The realization of wide bandgap in compressed trilayer graphene offers opportunities in carbon-based electronic devices.

5.
ACS Nano ; 13(3): 3106-3116, 2019 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-30776213

RESUMO

Thin films with large compressive residual stress and low interface adhesion can buckle and delaminate from relatively rigid substrates, which is a common failure mode of film/substrate interfaces. Current studies mainly focused on the geometry of various buckling patterns and related physical origins based on a static point of view. However, fundamental understanding of dynamic propagation of buckles, particularly for the complicated web buckles, remains challenging. We adopt strained two-dimensional MoS2 thin films to study the phenomenon of web buckling because their interface adhesion, namely van der Waals interaction, is naturally low. With a delicately site-controlled initiation, web buckles can be triggered and their dynamic propagation is in situ observed facilely. Finite element modeling shows that the formation of web buckles involves the propagation and multilevel branching of telephone-cord blisters. These buckled semiconducting films can be patterned by spatial confinement and potentially used in diffuse-reflective coatings, microfluidic channels, and hydrogen evolution reaction electrodes. Our work not only reveals the hidden mechanisms and kinematics of propagation of web buckles on rigid substrates but also sheds light on the development of semiconducting devices based on buckling engineering.

6.
Chem Commun (Camb) ; 54(97): 13726-13729, 2018 Dec 04.
Artigo em Inglês | MEDLINE | ID: mdl-30456398

RESUMO

Selective nitrogen-doping of graphene oxide with a high pyridinic N ratio (51%; L-GO) was achieved by laser irradiation of graphene oxide with ammonia. The resulting L-GO exhibited enhanced electrocatalytic properties; specifically, the overpotential of the hydrogen evolution reaction (HER) was improved by over 400 mV at 10 mA cm-2 compared to the pristine graphene oxide.

7.
Adv Mater ; 30(30): e1800754, 2018 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-29893020

RESUMO

2D layered materials have emerged in recent years as a new platform to host novel electronic, optical, or excitonic physics and develop unprecedented nanoelectronic and energy applications. By definition, these materials are strongly anisotropic between the basal plane and cross the plane. The structural and property anisotropies inside their basal plane, however, are much less investigated. Black phosphorus, for example, is a 2D material that has such in-plane anisotropy. Here, a rare chemical form of arsenic, called black-arsenic (b-As), is reported as a cousin of black phosphorus, as an extremely anisotropic layered semiconductor. Systematic characterization of the structural, electronic, thermal, and electrical properties of b-As single crystals is performed, with particular focus on its anisotropies along two in-plane principle axes, armchair (AC) and zigzag (ZZ). The analysis shows that b-As exhibits higher or comparable electronic, thermal, and electric transport anisotropies between the AC and ZZ directions than any other known 2D crystals. Such extreme in-plane anisotropies can potentially implement novel ideas for scientific research and device applications.

8.
Small ; 14(14): e1703621, 2018 04.
Artigo em Inglês | MEDLINE | ID: mdl-29479803

RESUMO

Micro-electromechanical (MEM) switches, with advantages such as quasi-zero leakage current, emerge as attractive candidates for overcoming the physical limits of complementary metal-oxide semiconductor (CMOS) devices. To practically integrate MEM switches into CMOS circuits, two major challenges must be addressed: sub 1 V operating voltage to match the voltage levels in current circuit systems and being able to deliver at least millions of operating cycles. However, existing sub 1 V mechanical switches are mostly subject to significant body bias and/or limited lifetimes, thus failing to meet both limitations simultaneously. Here 0.2 V MEM switching devices with ≳106 safe operating cycles in ambient air are reported, which achieve the lowest operating voltage in mechanical switches without body bias reported to date. The ultralow operating voltage is mainly enabled by the abrupt phase transition of nanolayered vanadium dioxide (VO2 ) slightly above room temperature. The phase-transition MEM switches open possibilities for sub 1 V hybrid integrated devices/circuits/systems, as well as ultralow power consumption sensors for Internet of Things applications.

9.
Nanoscale ; 10(7): 3540-3546, 2018 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-29410997

RESUMO

Two-dimensional semiconducting transition metal dichalcogenides have been employed as key components in various electronic devices. The thermal stability of these ultrathin materials must be carefully considered in device applications because the heating caused by current flow, light absorption, or other harsh environmental conditions is usually unavoidable. In this work, we found that the substrate plays a role in modifying the thermal stability of mono- and few-layer MoS2. Triangular etching holes, which are considered to initiate from defect sites, form on MoS2 when the temperature exceeds a threshold. On Al2O3 and SiO2, monolayer MoS2 is found to be more stable in thermal annealing than few-layer MoS2 either in atmospheric-pressure air or under vacuum; while on mica, the absolute opposite behavior exists. However, this difference due to substrates appears to vanish when using defective, chemical-vapor-deposited MoS2 samples. The substrate modification of the thermal stability of MoS2 with various thicknesses is attributed to the competition between MoS2-substrate interface interaction and MoS2-MoS2 interlayer interaction. Our findings provide important design rules for MoS2-based devices, and also potentially point to a route of controlled patterning of MoS2 with substrate engineering.

10.
Nano Lett ; 18(3): 1637-1643, 2018 03 14.
Artigo em Inglês | MEDLINE | ID: mdl-29400972

RESUMO

Along with the rapid development of hybrid electronic-photonic systems, multifunctional devices with dynamic responses have been widely investigated for improving many optoelectronic applications. For years, microelectro-opto-mechanical systems (MEOMS), one of the major approaches to realizing multifunctionality, have demonstrated profound reconfigurability and great reliability. However, modern MEOMS still suffer from limitations in modulation depth, actuation voltage, or miniaturization. Here, we demonstrate a new MEOMS multifunctional platform with greater than 50% optical modulation depth over a broad wavelength range. This platform is realized by a specially designed cantilever array, with each cantilever consisting of vanadium dioxide, chromium, and gold nanolayers. The abrupt structural phase transition of the embedded vanadium dioxide enables the reconfigurability of the platform. Diverse stimuli, such as temperature variation or electric current, can be utilized to control the platform, promising CMOS-compatible operating voltage. Multiple functionalities, including an active enhanced absorber and a reprogrammable electro-optic logic gate, are experimentally demonstrated to address the versatile applications of the MEOMS platform in fields such as communication, energy harvesting, and optical computing.

11.
Nat Commun ; 9(1): 199, 2018 01 15.
Artigo em Inglês | MEDLINE | ID: mdl-29335411

RESUMO

Doping of traditional semiconductors has enabled technological applications in modern electronics by tailoring their chemical, optical and electronic properties. However, substitutional doping in two-dimensional semiconductors is at a comparatively early stage, and the resultant effects are less explored. In this work, we report unusual effects of degenerate doping with Nb on structural, electronic and optical characteristics of MoS2 crystals. The doping readily induces a structural transformation from naturally occurring 2H stacking to 3R stacking. Electronically, a strong interaction of the Nb impurity states with the host valence bands drastically and nonlinearly modifies the electronic band structure with the valence band maximum of multilayer MoS2 at the Γ point pushed upward by hybridization with the Nb states. When thinned down to monolayers, in stark contrast, such significant nonlinear effect vanishes, instead resulting in strong and broadband photoluminescence via the formation of exciton complexes tightly bound to neutral acceptors.

12.
Adv Mater ; 30(5)2018 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-29226459

RESUMO

The unique correspondence between mathematical operators and photonic elements in wave optics enables quantitative analysis of light manipulation with individual optical devices. Phase-transition materials are able to provide real-time reconfigurability of these devices, which would create new optical functionalities via (re)compilation of photonic operators, as those achieved in other fields such as field-programmable gate arrays (FPGA). Here, by exploiting the hysteretic phase transition of vanadium dioxide, an all-solid, rewritable metacanvas on which nearly arbitrary photonic devices can be rapidly and repeatedly written and erased is presented. The writing is performed with a low-power laser and the entire process stays below 90 °C. Using the metacanvas, dynamic manipulation of optical waves is demonstrated for light propagation, polarization, and reconstruction. The metacanvas supports physical (re)compilation of photonic operators akin to that of FPGA, opening up possibilities where photonic elements can be field programmed to deliver complex, system-level functionalities.

13.
Sci Rep ; 7(1): 7131, 2017 08 02.
Artigo em Inglês | MEDLINE | ID: mdl-28769057

RESUMO

Efficient thermal management at the nanoscale is important for reducing energy consumption and dissipation in electronic devices, lab-on-a-chip platforms and energy harvest/conversion systems. For many of these applications, it is much desired to have a solid-state structure that reversibly switches thermal conduction with high ON/OFF ratios and at high speed. Here we describe design and implementation of a novel, all-solid-state thermal switching device by nanostructured phase transformation, i.e., modulation of contact pressure and area between two poly-silicon surfaces activated by microstructural change of a vanadium dioxide (VO2) thin film. Our solid-state devices demonstrate large and reversible alteration of cross-plane thermal conductance as a function of temperature, achieving a conductance ratio of at least 2.5. Our new approach using nanostructured phase transformation provides new opportunities for applications that require advanced temperature and heat regulations.

14.
Nano Lett ; 17(8): 4982-4988, 2017 08 09.
Artigo em Inglês | MEDLINE | ID: mdl-28657751

RESUMO

van der Waals (vdW) forces, despite being relatively weak, hold the layers together in transition metal dichalcogenides (TMDs) and play a key role in their band structure evolution, hence profoundly affecting their physical properties. In this work, we experimentally probe the vdW interactions in MoS2 and other TMDs by measuring the valence band maximum (VBM) splitting (Δ) at K point as a function of pressure in a diamond anvil cell. As high pressure increases interlayer wave function coupling, the VBM splitting is enhanced in 2H-stacked MoS2 multilayers but, due to its specific geometry, not in 3R-stacked multilayers, hence allowing the interlayer contribution to be separated out of the total VBM splitting, as well as predicting a negative pressure (2.4 GPa) where the interlayer contribution vanishes. This negative pressure represents the threshold vdW interaction beyond which neighboring layers are electronically decoupled. This approach is compared to first-principles calculations and found to be widely applicable to other group-VI TMDs.

15.
Nano Lett ; 17(4): 2512-2516, 2017 04 12.
Artigo em Inglês | MEDLINE | ID: mdl-28266861

RESUMO

The complexity of strongly correlated electron physics in vanadium dioxide is exemplified as its rich phase diagrams of all kinds, which in turn shed light on the mechanisms behind its various phase transitions. In this work, we map out the hydrostatic pressure-temperature phase diagram of vanadium dioxide nanobeams by independently varying pressure and temperature with a diamond anvil cell. In addition to the well-known insulating M1 (monoclinic) and metallic R (tetragonal) phases, the diagram identifies the existence at high pressures of the insulating M1' (monoclinic, more conductive than M1) phase and two metallic phases of X (monoclinic) and O (orthorhombic, at high temperature only). Systematic optical and electrical measurements combined with density functional calculations allow us to delineate their phase boundaries as well as reveal some basic features of the transitions.

16.
ACS Nano ; 11(2): 2115-2123, 2017 02 28.
Artigo em Inglês | MEDLINE | ID: mdl-28117983

RESUMO

Broadband optoelectronics such as artificial light harvesting technologies necessitate efficient and, ideally, tunable coupling of excited states over a wide range of energies. In monolayer MoS2, a prototypical two-dimensional layered semiconductor, the excited state manifold spans the visible electromagnetic spectrum and is comprised of an interconnected network of excitonic and free-carrier excitations. Here, photoluminescence excitation spectroscopy is used to reveal the energetic and spatial dependence of broadband excited state coupling to the ground-state luminescent excitons of monolayer MoS2. Photoexcitation of the direct band gap excitons is found to strengthen with increasing energy, demonstrating that interexcitonic coupling across the Brillouin zone is more efficient than previously reported, and thus bolstering the import and appeal of these materials for broadband optoelectronic applications. Narrow excitation resonances that are superimposed on the broadband photoexcitation spectrum are identified and coincide with the energetic positions of the higher-energy excitons and the electronic band gap as predicted by first-principles calculations. Identification of such features outlines a facile route to measure the optical and electronic band gaps and thus the exciton binding energy in the more sophisticated device architectures that are necessary for untangling the rich many-body phenomena and complex photophysics of these layered semiconductors. In as-grown materials, the excited states exhibit microscopic spatial variations that are characteristic of local carrier density fluctuations, similar to charge puddling phenomena in graphene. Such variations likely arise from substrate inhomogeneity and demonstrate the possibility to use substrate patterning to tune local carrier density and dynamically control excited states for designer optoelectronics.

17.
Science ; 355(6323): 371-374, 2017 01 27.
Artigo em Inglês | MEDLINE | ID: mdl-28126811

RESUMO

In electrically conductive solids, the Wiedemann-Franz law requires the electronic contribution to thermal conductivity to be proportional to electrical conductivity. Violations of the Wiedemann-Franz law are typically an indication of unconventional quasiparticle dynamics, such as inelastic scattering, or hydrodynamic collective motion of charge carriers, typically pronounced only at cryogenic temperatures. We report an order-of-magnitude breakdown of the Wiedemann-Franz law at high temperatures ranging from 240 to 340 kelvin in metallic vanadium dioxide in the vicinity of its metal-insulator transition. Different from previously established mechanisms, the unusually low electronic thermal conductivity is a signature of the absence of quasiparticles in a strongly correlated electron fluid where heat and charge diffuse independently.

18.
Nano Lett ; 17(1): 194-199, 2017 01 11.
Artigo em Inglês | MEDLINE | ID: mdl-27935309

RESUMO

Hydrostatic pressure applied using diamond anvil cells (DAC) has been widely explored to modulate physical properties of materials by tuning their lattice degree of freedom. Independently, electrical field is able to tune the electronic degree of freedom of functional materials via, for example, the field-effect transistor (FET) configuration. Combining these two orthogonal approaches would allow discovery of new physical properties and phases going beyond the known phase space. Such experiments are, however, technically challenging and have not been demonstrated. Herein, we report a feasible strategy to prepare and measure FETs in a DAC by lithographically patterning the nanodevices onto the diamond culet. Multiple-terminal FETs were fabricated in the DAC using few-layer MoS2 and BN as the channel semiconductor and dielectric layer, respectively. It is found that the mobility, conductance, carrier concentration, and contact conductance of MoS2 can all be significantly enhanced with pressure. We expect that the approach could enable unprecedented ways to explore new phases and properties of materials under coupled mechano-electrostatic modulation.

19.
Sci Rep ; 6: 34428, 2016 10 04.
Artigo em Inglês | MEDLINE | ID: mdl-27698372

RESUMO

Thermal energy transport across the interfaces of physically and chemically modified graphene with two metals, Al and Cu, was investigated by measuring thermal conductance using the time-domain thermoreflectance method. Graphene was processed using a He2+ ion-beam with a Gaussian distribution or by exposure to ultraviolet/O3, which generates structural or chemical disorder, respectively. Hereby, we could monitor changes in the thermal conductance in response to varying degrees of disorder. We find that the measured conductance increases as the density of the physical disorder increases, but undergoes an abrupt modulation with increasing degrees of chemical modification, which decreases at first and then increases considerably. Moreover, we find that the conductance varies inverse proportionally to the average distance between the structural defects in the graphene, implying a strong in-plane influence of phonon kinetics on interfacial heat flow. We attribute the bimodal results to an interplay between the distinct effects on graphene's vibrational modes exerted by graphene modification and by the scattering of modes.

20.
Small ; 12(29): 3976-84, 2016 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-27335137

RESUMO

The atomic thickness and flatness allow properties of 2D semiconductors to be modulated with influence from the substrate. Reversible modulation of these properties requires an "active," reconfigurable substrate, i.e., a substrate with switchable functionalities that interacts strongly with the 2D overlayer. In this work, the photoluminescence (PL) of monolayer molybdenum disulfide (MoS2 ) is modulated by interfacing it with a phase transition material, vanadium dioxide (VO2 ). The MoS2 PL intensity is enhanced by a factor of up to three when the underlying VO2 undergoes the thermally driven phase transition from the insulating to metallic phase. A nonvolatile, reversible way to rewrite the PL pattern is also demonstrated. The enhancement effect is attributed to constructive optical interference when the VO2 turns metallic. This modulation method requires no chemical or mechanical processes, potentially finding applications in new switches and sensors.

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