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1.
ACS Nano ; 13(12): 14262-14273, 2019 Dec 24.
Artigo em Inglês | MEDLINE | ID: mdl-31790198

RESUMO

Two-dimensional (2D) layered semiconductors have recently emerged as attractive building blocks for next-generation low-power nonvolatile memories. However, challenges remain in the controllable fabrication of bipolar resistive switching circuit components from these materials. Here, the experimental realization of lateral memtransistors from monolayer single-crystal molybdenum disulfide (MoS2) utilizing a focused helium ion beam is reported. Site-specific irradiation with the focused probe of a helium ion microscope creates a nanometer-scale defect-rich region, bisecting the MoS2 lattice. The reversible drift of these defects in the applied electric field modulates the resistance of the channel, enabling versatile memristive functionality. The device can reliably retain its resistance ratios and set/reset biases for 1180 switching cycles. Long-term potentiation and depression with sharp habituation are demonstrated. This work establishes the feasibility of ion irradiation for controllable fabrication of 2D memristive devices with promising key performance parameters, such as low power consumption. The applicability of these devices for synaptic emulation may address the demands of future neuromorphic architectures.

2.
ACS Omega ; 4(17): 17487-17493, 2019 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-31656920

RESUMO

Forming gas annealing is a common process step used to improve the performance of devices based on transition-metal dichalcogenides (TMDs). Here, the impact of forming gas anneal is investigated for PtSe2-based devices. A range of annealing temperatures (150, 250, and 350 °C) were used both in inert (0/100% H2/N2) and forming gas (5/95% H2/N2) environments to separate the contribution of temperature and ambient. The samples are electrically characterized by circular transfer length method structures, from which contact resistance and sheet resistance are analyzed. Ti and Ni are used as metal contacts. Ti does not react with PtSe2 at any given annealing step. In contrast to this, Ni reacts with PtSe2, resulting in a contact alloy formation. The results are supported by a combination of X-ray photoelectron spectroscopy, Raman spectroscopy, energy-dispersive X-ray spectroscopy, and cross-sectional transmission electron microscopy. The work sheds light on the impact of forming gas annealing on TMD-metal interfaces, and on the TMD film itself, which could be of great interest to improve the contact resistance of TMD-based devices.

3.
ACS Nano ; 13(11): 13390-13402, 2019 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-31661247

RESUMO

Cooperite, or platinum sulfide (PtS), is a rare mineral that generally exists as microscale, irregularly shaped crystallites. The presence of impurities, in both naturally occurring and synthesized samples, has hindered the study of its optical properties in the past. In this work, we prepare large-scale, uniform PtS films in bulk to two-dimensional form through the thermally assisted conversion method. An abnormal trend is observed in linear spectral studies whereby the optical bandgap narrows as the film thickness decreases. A model based on the continuous distribution of carriers in real space, which can be regarded as a quantum well normal to the plane, is used to describe the thickness-dependent carrier recombination phenomenon. In the nonlinear optical measurements, PtS exhibits ultrafast saturable absorption and self-defocusing properties in the visible region, which are dominated by the resonant electronic nonlinearities.

4.
Small ; 15(34): e1902728, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-31276302

RESUMO

Carrier interactions in 2D nanostructures are of central importance not only in condensed-matter physics but also for a wide range of optoelectronic and photonic applications. Here, new insights into the behavior of photoinduced carriers in layered platinum diselenide (PtSe2 ) through ultrafast time-resolved pump-probe and nonlinear optical measurements are presented. The measurements reveal the temporal evolution of carrier relaxation, chemical potential and bandgap renormalization in PtSe2 . These results imply that few-layer PtSe2 has a semiconductor-like carrier relaxation instead of a metal-like one. The relaxation follows a triple-exponential decay process and exhibits thickness-dependent relaxation times. This occurs along with a band-filling effect, which can be controlled based on the number of layers and may be applied in saturable absorption for generating ultrafast laser pulses. The findings may provide means to study many-body physics in 2D materials as well as potentially leading to applications in the field of optoelectronics and ultrafast photonics.

5.
Adv Sci (Weinh) ; 5(9): 1800502, 2018 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-30250792

RESUMO

Sulfur (S) is an attractive cathode material with advantages including high theoretical capacity and low cost. However, issues such as the lithium polysulfide shuttle effect and its insulating properties greatly limit the future applications of lithium-sulfur (Li-S) batteries. Here, a viscous aqueous ink with nanoscale S uniformly decorated on the polar, metallically conductive titanium carbide MXene nanosheets (S@Ti3C2T x ) is reported to address these issues. Importantly, it is observed that the conductive Ti3C2T x mediator efficiently chemisorbs the soluble polysulfides and converts them into thiosulfate/sulfate. The in situ formed sulfate complex layer acts as a thick protective barrier, which significantly retards the shuttling of polysulfides upon cycling and improves the sulfur utilization. Consequently, the binder-free, robust, highly electrically conductive composite film exhibits outstanding electrochemical performance, including high capacities (1244-1350 mAh g-1), excellent rate handling, and impressive cycling stability (0.035-0.048% capacity loss per cycle), surpassing the best MXene-S batteries known. The fabrication of a pouch cell based on the freestanding S@Ti3C2T x film is also reported. The prototype device showcases high capacities and excellent mechanical flexibility. Considering the broad family of MXenes and their unique roles in immobilizing the polysulfides, various S@MXene composites can be similarly fabricated with promising Li+ storage capability and long lifetime performance.

6.
Sci Adv ; 4(3): eaao5031, 2018 03.
Artigo em Inglês | MEDLINE | ID: mdl-29511736

RESUMO

Precise tunability of electronic properties of two-dimensional (2D) nanomaterials is a key goal of current research in this field of materials science. Chemical modification of layered transition metal dichalcogenides leads to the creation of heterostructures of low-dimensional variants of these materials. In particular, the effect of oxygen-containing plasma treatment on molybdenum disulfide (MoS2) has long been thought to be detrimental to the electrical performance of the material. We show that the mobility and conductivity of MoS2 can be precisely controlled and improved by systematic exposure to oxygen/argon plasma and characterize the material using advanced spectroscopy and microscopy. Through complementary theoretical modeling, which confirms conductivity enhancement, we infer the role of a transient 2D substoichiometric phase of molybdenum trioxide (2D-MoO x ) in modulating the electronic behavior of the material. Deduction of the beneficial role of MoO x will serve to open the field to new approaches with regard to the tunability of 2D semiconductors by their low-dimensional oxides in nano-modified heterostructures.

7.
ACS Nano ; 12(2): 954-964, 2018 02 27.
Artigo em Inglês | MEDLINE | ID: mdl-29338193

RESUMO

Two-dimensional (2D) nanomaterials have been intensively investigated due to their interesting properties and range of potential applications. Although most research has focused on graphene, atomic layered transition metal dichalcogenides (TMDs) and particularly MoS2 have gathered much deserved attention recently. Here, we report the induction of chirality into 2D chiral nanomaterials by carrying out liquid exfoliation of MoS2 in the presence of chiral ligands (cysteine and penicillamine) in water. This processing resulted in exfoliated chiral 2D MoS2 nanosheets showing strong circular dichroism signals, which were far past the onset of the original chiral ligand signals. Using theoretical modeling, we demonstrated that the chiral nature of MoS2 nanosheets is related to the presence of chiral ligands causing preferential folding of the MoS2 sheets. There was an excellent match between the theoretically calculated and experimental spectra. We believe that, due to their high aspect ratio planar morphology, chiral 2D nanomaterials could offer great opportunities for the development of chiroptical sensors, materials, and devices for valleytronics and other potential applications. In addition, chirality plays a key role in many chemical and biological systems, with chiral molecules and materials critical for the further development of biopharmaceuticals and fine chemicals, and this research therefore should have a strong impact on relevant areas of science and technology such as nanobiotechnology, nanomedicine, and nanotoxicology.

8.
ACS Nano ; 10(10): 9550-9558, 2016 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-27661979

RESUMO

Layered two-dimensional (2D) materials display great potential for a range of applications, particularly in electronics. We report the large-scale synthesis of thin films of platinum diselenide (PtSe2), a thus far scarcely investigated transition metal dichalcogenide. Importantly, the synthesis by thermally assisted conversion is performed at 400 °C, representing a breakthrough for the direct integration of this material with silicon (Si) technology. Besides the thorough characterization of this 2D material, we demonstrate its promise for applications in high-performance gas sensing with extremely short response and recovery times observed due to the 2D nature of the films. Furthermore, we realized vertically stacked heterostructures of PtSe2 on Si which act as both photodiodes and photovoltaic cells. Thus, this study establishes PtSe2 as a potential candidate for next-generation sensors and (opto-)electronic devices, using fabrication protocols compatible with established Si technologies.

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