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Mauricio Terrones

Publications and source records attributed to Mauricio Terrones.

51 records · Page 3Linked to original sources

Nonlinear dark-field imaging of 1D defects in monolayer dichalcogenides

Extended defects with one dimensionality smaller than that of the host, such as 2D grain boundaries in 3D materials or 1D grain boundaries in 2D materials, can be particularly damaging since they directly impede the transport of charge, spin or heat, and can introduce a metallic character into otherwise semiconducting systems. Unfortunately, a technique to rapidly and non-destructively image 1D defects in 2D materials is lacking. Scanning transmission electron microscopy (STEM), Raman, photoluminescence and nonlinear optical spectroscopies, are all extremely valuable, but current implementations suffer from low throughput and a destructive nature (STEM) or limitations in their unambiguous sensitivity at the nanoscale. Here we demonstrate that dark-field second harmonic generation (SHG) microscopy can rapidly, efficiently, and non-destructively probe grain boundaries and edges in monolayer dichalcogenides (i.e. MoSe2, MoS2 and WS2). Dark-field SHG efficiently separates the spatial components of the emitted light and exploits interference effects from crystal domains of different orientations to localize grain boundaries and edges as very bright 1D patterns through a Cerenkov-type SHG emission. The frequency dependence of this emission in MoSe2 monolayers is explained in terms of plasmon-enhanced SHG related to the defects metallic character. This new technique for nanometer-scale imaging of the grain structure, domain orientation and localized 1D plasmons in 2D different semiconductors, thus enables more rapid progress towards both applications and fundamental materials discoveries.

cond-mat.mes-hall↗

Dark-Exciton-Mediated Fano Resonance from a Single Gold Nanostructure Deposited on Monolayer WS2 at Room Temperature

Strong spatial confinement and highly reduced dielectric screening provide monolayer transition metal dichalcogenides (TMDCs) with strong many-body effects, thereby possessing optically forbidden excitonic states (i.e., dark excitons) at room temperature. Herein, we explore the interaction of surface plasmons with dark excitons in hybrid systems consisting of stacked gold nanotriangles (AuNTs) and monolayer WS2. We observe a narrow Fano resonance when the hybrid system is surrounded by water, and we attribute the narrowing of the spectral Fano linewidth to the plasmon-enhanced decay of dark K-K excitons. Our results reveal that dark excitons in monolayer WS2 can strongly modify Fano resonances in hybrid plasmon-exciton systems and can be harnessed for novel optical sensors and active nanophotonic devices.

physics.optics↗

Considerations for utilizing sodium chloride in epitaxial molybdenum disulfide

The utilization of alkali salts, such as NaCl and KI, have enabled the successful growth of large single domain and fully coalesced polycrystalline two-dimensional (2D) transition metal dichalcogenide layers. However, the impact of alkali salts on photonic and electronic properties are not fully established. In this work, we report alkali-free epitaxy of MoS2 on sapphire and benchmark the properties against alkali-assisted growth of MoS2. This study demonstrates that although NaCl can dramatically increase the domain size of monolayer MoS2 by 20 times, it can also induce strong optical and electronic heterogeneities in as-grown large-scale films. This work elucidates that utilization of NaCl can lead to variation in growth rates, loss of epitaxy, and a high density of nanoscale MoS2 particles (4/μm2). Such phenomena suggest that alkali atoms play an important role in Mo and S adatom mobility and strongly influence the 2D/sapphire interface during growth. Compared to alkali-free synthesis under the same growth conditions, MoS2 growth assisted by NaCl results in >1% tensile strain in as-grown domains, which reduces photoluminescence by ~20x and degrades transistor performance.

cond-mat.mtrl-sci↗

Phase Modulators Based on High Mobility Ambipolar ReSe2 Field-Effect Transistors

We fabricated ambipolar field-effect transistors (FETs) from multi-layered triclinic ReSe2, mechanically exfoliated onto a SiO2 layer grown on p-doped Si. In contrast to previous reports on thin layers (~2 to 3 layers), we extract field-effect carrier mobilities in excess of 10^2 cm^2/Vs at room temperature in crystals with nearly ~10 atomic layers. These thicker FETs also show nearly zero threshold gate voltage for conduction and high ON to OFF current ratios when compared to the FETs built from thinner layers. We also demonstrate that it is possible to utilize this ambipolarity to fabricate logical elements or digital synthesizers. For instance, we demonstrate that one can produce simple, gate-voltage tunable phase modulators with the ability to shift the phase of the input signal by either 90^o or nearly 180^o. Given that it is possible to engineer these same elements with improved architectures, for example on h-BN in order to decrease the threshold gate voltage and increase the carrier mobilities, it is possible to improve their characteristics in order to engineer ultra-thin layered logic elements based on ReSe2.

cond-mat.mes-hall↗

Dynamics of liquid crystal on hexagonal lattice

Nematic liquid crystal (LC) molecules adsorbed on two dimensional materials are aligned along the crystal directions of the hexagonal lattice. It was demonstrated that short electric pulses can reorient the aligned LC molecules in the preferred armchair direction of hexagonal boron nitride (h-BN). Several states with a variety of colors were obtained by changing the direction and strength of the electric pulses. The ab initio calculations based on density functional theory was carried out to determine the favorable adsorption configurations of the LC molecules on the h-BN surface. A non-volatile display, in which pixel resolution can be determined by grains of hexagonal surface, is proposed, which can offer a pathway towards dynamic high-quality pixels with low power consumption, and could define a new paradigm for all non-volatile display applications.

cond-mat.soft↗

Unique excitonic effects in tungsten disulphide monolayers on two-layer graphene

Light emission in atomically thin heterostructures is known to depend on the type of materials, number and stacking sequence of the constituent layers. Here we show that the thickness of a two-dimensional substrate can be crucial in modulating the light emission. We study the layer-dependent charge transfer in vertical heterostructures built from monolayer tungsten disulphide (WS2) on one- and two-layer epitaxial graphene, unravelling the effect that the interlayer electronic coupling has on the excitonic properties of such heterostructures. We bring evidence that the excitonic properties of WS2 can be effectively tuned by the number of supporting graphene layers. Integrating WS2 monolayers with two-layer graphene leads to a significant enhancement of the photoluminescence response, up to one order of magnitude higher compared to WS2 supported on one-layer graphene. Our findings highlight the importance of substrate engineering when constructing atomically thin layered heterostructures.

cond-mat.mtrl-sci↗

Tunable Resonance Coupling in Single Si Nanoparticle-Monolayer WS2 Structures

Two-dimensional semiconducting transition metal dichalcogenides (TMDCs) are extremely attractive materials for optoelectronic applications in the visible and near-IR range. Here, we address for the first time to the best of our knowledge the issue of resonance coupling in hybrid exciton-polariton structures based on single Si nanoparticles coupled to monolayer WS2. We predict a transition from weak to strong coupling regime , with a Rabi splitting energy exceeding 200 meV for a Si nanoparticle covered by monolayer WS 2 at the magnetic optical Mie resonance. This large transition is achieved due to the symmetry of magnetic dipole Mie mode and by changing the surrounding dielectric material from air to water. The prediction is based on the experimental estimation of TMDC dipole moment variation obtained from measured photoluminescence (PL) spectra of WS2 monolayers in different solvents. An ability of such a system to tune the resonance coupling is realized experimentally for optically resonant spherical Si nanoparticles placed on a WS2 monolayer. The Rabi splitting energy obtained for this scenario increases from 49.6 meV to 86.6 meV after replacing air by water. Our findings pave the way to develop high-efficiency optoelectronic, nanophotonic and quantum optical devices.

physics.optics↗

Low temperature synthesis of heterostructures of transition metal dichalcogenide alloys (WxMo1-xS2) and graphene with superior catalytic performance for hydrogen evolution

Large-area ($\sim$cm$^2$) films of vertical heterostructures formed by alternating graphene and transition-metal dichalcogenide(TMD) alloys are obtained by wet chemical routes followed by a thermal treatment at low temperature (300 $^\circ$C). In particular, we synthesized stacked graphene and W$_x$Mo$_{1-x}$S$_2$ alloy phases that were used as hydrogen evolution catalysts. We observed a Tafel slope of 38.7 mV dec$^{-1}$ and 96 mV onset potential (at current density of 10 mA cm$^{-2}$) when the heterostructure alloy is annealed at 300 $^o$C. These results indicate that heterostructure formed by graphene and W$_{0.4}$Mo$_{0.6}$S$_2$ alloys are far more efficient than WS$_2$ and MoS$_2$ by at least a factor of two, and it is superior than any other reported TMD system. This strategy offers a cheap and low temperature synthesis alternative able to replace Pt in the hydrogen evolution reaction (HER). Furthermore, the catalytic activity of the alloy is stable over time, i.e. the catalytic activity does not experience a significant change even after 1000 cycles. Using density functional theory calculations, we found that this enhanced hydrogen evolution in the W$_x$Mo$_{1-x}$S$_2$ alloys is mainly due to the lower energy barrier created by a favorable overlap of the d-orbitals from the transition metals and the s-orbitals of H$_2$, with the lowest energy barrier occurring for W$_{0.4}$Mo$_{0.6}$S$_2$ alloy. Thus, it is now possible to further improve the performance of the "inert" TMD basal plane via metal alloying, in addition to the previously reported strategies of creation of point defects, vacancies and edges. The synthesis of graphene/W$_{0.4}$Mo$_{0.6}$S$_2$ produced at relatively low temperatures is scalable and could be used as an effective low cost Pt-free catalyst.

cond-mat.mtrl-sci↗

Programmable Molecular Composites of Tandem Proteins with Graphene-Oxide for Efficient Bimoprh Actuators

The rapid expansion in the spectrum of two-dimensional (2D) materials has driven the efforts of research on the fabrication of 2D composites and heterostructures. Highly ordered structure of 2D materials provides an excellent platform for controlling the ultimate structure and properties of the composite material with precision. However, limited control over the structure of the adherent material and its interactions with highly ordered 2D materials results in defective composites with inferior performance. Here, we demonstrate the successful synthesis, integration, and characterization of hybrid 2D material systems consisting of tandem repeat (TR) proteins inspired by squid ring teeth and graphene oxide (GO). The TR protein layer acts as a unique programmable molecular spacer between GO layers. As an application, we further demonstrate thermal actuation using bimorph molecular composite films. Bimorph actuators made of molecular composite films (GO/TR) can lead to energy efficiencies 18 times higher than regular bimorph actuators consisting of a GO layer and a TR protein layer (i.e., conventional bulk composite of GO and TR). Additionally, molecular composite bimorph actuators can reach curvature values as high as 1.2 cm-1 by using TR proteins with higher molecular weight, which is 3 times higher than conventional GO and TR composites.

cond-mat.soft↗

Photoconductivity of few-layered p-WSe2 phototransistors via multi-terminal measurements

Recently, two-dimensional materials and in particular transition metal dichalcogenides (TMDs) were extensively studied because of their strong light-matter interaction and the remarkable optoelectronic response of their field-effect transistors (FETs). Here, we report a photoconductivity study from FETs built from few-layers of p-WSe2 measured in a multi-terminal configuration under illumination by a 532 nm laser source. The photogenerated current was measured as a function of the incident optical power, of the drain-to-source bias and of the gate voltage. We observe a considerably larger photoconductivity when the phototransistors were measured via a four-terminal configuration when compared to a two-terminal one. For an incident laser power of 248 nW, we extract 18 A/W and ~4000% for the two-terminal responsivity (R) and the concomitant external quantum efficiency (EQE) respectively, when a bias voltage Vds = 1 V and a gate voltage Vbg = 10 V are applied to the sample. R and EQE are observed to increase by 370% to ~85 A/W and ~20000% respectively, when using a four-terminal configuration. Thus, we conclude that previous reports have severely underestimated the optoelectronic response of transition metal dichalcogenides, which in fact reveals a remarkable potential for photosensing applications.

cond-mat.mes-hall↗

Zone-center phonons of bulk, few-layer, and monolayer 1T-TaS$_2$: Detection of the commensurate charge density wave phase through Raman scattering

We present first-principles calculations of the vibrational properties of the transition metal dichalcogenide 1T-TaS$_2$ for various thicknesses in the high-temperature (undistorted) phase and the low-temperature commensurate charge density wave (CDW) phase. We also present measurements of the Raman spectra for bulk, few-layer, and monolayer samples at temperatures well below that of the bulk transition to the commensurate phase. Through our calculations, we identify the low-frequency folded-back acoustic modes as a convenient signature of the commensurate CDW wave structure in vibrational spectra. In our measured Raman spectra, this signature is clearly evident in all of the samples, indicating that the commensurate phase remains the ground state as the material is thinned, even down to a single layer. This is in contrast to some previous studies which suggest a suppression of the commensurate CDW transition in thin flakes. We also use polarized Raman spectroscopy to probe c-axis orbital texture in the low-T phase, which has recently been suggested as playing a role in the metal-insulator transition that accompanies the structural transition to the commensurate CDW phase.

cond-mat.mtrl-sci↗

Metal to insulator quantum-phase transition in few-layered ReS$_2$

In ReS$_2$ a layer-independent direct band-gap of 1.5 eV implies a potential for its use in optoelectronic applications. ReS$_2$ crystallizes in the 1T$^{\prime}$-structure which leads to anisotropic physical properties and whose concomitant electronic structure might host a non-trivial topology. Here, we report an overall evaluation of the anisotropic Raman response and the transport properties of few-layered ReS$_2$ field-effect transistors. We find that ReS$_2$ exfoliated on SiO$_2$ behaves as an $n$-type semiconductor with an intrinsic carrier mobility surpassing $μ_i$ ~30 cm$^2$/Vs at $T = 300$ K which increases up to ~350 cm$^2$/Vs at 2 K. Semiconducting behavior is observed at low electron densities $n$, but at high values of n the resistivity decreases by a factor > 7 upon cooling to 2 K and displays a metallic $T^2$-dependence. This indicates that the band structure of 1T$^{\prime}$-ReS$_2$ is quite susceptible to an electric field applied perpendicularly to the layers. The electric-field induced metallic state observed in transition metal dichalcogenides was recently claimed to result from a percolation type of transition. Instead, through a scaling analysis of the conductivity as a function of $T$ and $n$, we find that the metallic state of ReS$_2$ results from a second-order metal to insulator transition driven by electronic correlations. This gate-induced metallic state offers an alternative to phase engineering for producing ohmic contacts and metallic interconnects in devices based on transition metal dichalcogenides.

cond-mat.mes-hall↗

Gate-modulated conductance of few-layer WSe_2 field-effect transistors in the subgap regime: Schottky barrier transistor and subgap impurity states

Two key subjects stand out in the pursuit of semiconductor research: material quality and contact technology. The fledging field of atomically thin transition metal dichalcogenides (TMDCs) faces a number of challenges in both efforts. This work attempts to establish a connection between the two by examining the gate-dependent conductance of few-layer (1-5L) WSe2 field effect devices. Measurements and modeling of the subgap regime reveal Schottky barrier transistor behavior. We show that transmission through the contact barrier is dominated by thermionic field emission (TFE) at room temperature, despite the lack of intentional doping. The TFE process arises due to a large number of subgap impurity states, the presence of which also leads to high mobility edge carrier densities. The density of states of such impurity states is self-consistently determined to be approximately 1-2x10^13 /cm^2/eV in our devices. We demonstrate that substrate is unlikely to be a major source of the impurity states and suspect that lattice defects within the material itself are primarily responsible. Our experiments provide key information to advance the quality and understanding of TMDC materials and electrical devices.

cond-mat.mes-hall↗

Field-Effect Transistors Based on Few-Layered alpha-MoTe_2

Here we report the properties of field-effect transistors based on few layers of chemical vapor transport grown alpha- MoTe_2 crystals mechanically exfoliated onto SiO_2. We performed field-effect and Hall mobility measurements, as well as Raman scattering and transmission electron microscopy. In contrast to both MoS_2 and MoSe_2, our MoTe_2 field-effect transistors (FETs) are observed to be hole-doped, displaying on/off ratios surpassing 106 and typical sub-threshold swings of ~ 140 mV per decade. Both field-effect and Hall mobilities indicate maximum values approaching or surpassing 10 cm^2/Vs which are comparable to figures previously reported for single or bi-layered MoS_2 and/or for MoSe_2 exfoliated onto SiO_2 at room temperature and without the use of dielectric engineering. Raman scattering reveals sharp modes in agreement with previous reports, whose frequencies are found to display little or no dependence on the number of layers. Given that both MoS_2 is electron doped, the stacking of MoTe_2 onto MoS_2 could produce ambipolar field-effect transistors and a gap modulation. Although the overall electronic performance of MoTe_2 is comparable to those of MoS_2 and MoSe_2, the heavier element Te should lead to a stronger spin orbit-coupling and possibly to concomitantly longer decoherence times for exciton valley and spin indexes.

cond-mat.mes-hall↗

Extraordinary room-temperature photoluminescence in WS2 monolayers

Individual monolayers of metal dichalcogenides are atomically thin two-dimensional crystals with attractive physical properties different from their bulk layered counterpart. Here we describe the direct synthesis of WS2 monolayers with triangular morphologies and strong room-temperature photoluminescence (PL). Bulk WS2 does not present PL due to its indirect band gap nature. The edges of these monolayers exhibit PL signals with extraordinary intensity, around 25 times stronger than the platelets center. The structure and composition of the platelet edges appear to be critical for the PL enhancement effect. Electron diffraction revealed that platelets present zigzag edges, while first-principles calculations indicate that sulfur-rich zigzag WS2 edges possess metallic edge states, which might tailor the optical response reported here. These novel 2D nanoscale light sources could find diverse applications including the fabrication of flexible/transparent/low-energy optoelectronic devices.

cond-mat.mes-hall↗