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Neuromorphic hardware implementation of Boltzmann Machine using a network of stochastic neurons can allow non-deterministic polynomial-time (NP) hard combinatorial optimization problems to be efficiently solved. Efficient implementation of such Boltzmann Machine with simulated annealing desires the statistical parameters of the stochastic neurons to be dynamically tunable, however, there has been limited research on stochastic semiconductor devices with controllable statistical distributions. Here, we demonstrate a reconfigurable tin oxide (SnOx)/molybdenum disulfide (MoS2) heterogeneous memristive device that can realize tunable stochastic dynamics in its output sampling characteristics. The device can sample exponential-class sigmoidal distributions analogous to the Fermi-Dirac distribution of physical systems with quantitatively defined tunable "temperature" effect. A BM composed of these tunable stochastic neuron devices, which can enable simulated annealing with designed "cooling" strategies, is conducted to solve the MAX-SAT, a representative in NP-hard combinatorial optimization problems. Quantitative insights into the effect of different "cooling" strategies on improving the BM optimization process efficiency are also provided.
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Autonomous electronic microsystems smaller than the diameter of a human hair (<100 µm) are promising for sensing in confined spaces such as microfluidic channels or the human body. However, they are difficult to implement due to fabrication challenges and limited power budget. Here we present a 60 × 60 µm electronic microsystem platform, or SynCell, that overcomes these issues by leveraging the integration capabilities of two-dimensional material circuits and the low power consumption of passive germanium timers, memory-like chemical sensors, and magnetic pads. In a proof-of-concept experiment, we magnetically positioned SynCells in a microfluidic channel to detect putrescine. After we extracted them from the channel, we successfully read out the timer and sensor signal, the latter of which can be amplified by an onboard transistor circuit. The concepts developed here will be applicable to microsystems targeting a variety of applications from microfluidic sensing to biomedical research.
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Self-assembly of vertically aligned III-V semiconductor nanowires (NWs) on two-dimensional (2D) van der Waals (vdW) nanomaterials allows for integration of novel mixed-dimensional nanosystems with unique properties for optoelectronic and nanoelectronic device applications. Here, selective-area vdW epitaxy (SA-vdWE) of InAs NWs on isolated 2D molybdenum disulfide (MoS2) domains is reported for the first time. The MOCVD growth parameter space (i.e., V/III ratio, growth temperature, and total molar flow rates of metalorganic and hydride precursors) is explored to achieve pattern-free positioning of single NWs on isolated multi-layer MoS2 micro-plates with one-to-one NW-to-MoS2 domain placement. The introduction of a pre-growth poly-l-lysine surface treatment is highlighted as a necessary step for mitigation of InAs nucleation along the edges of triangular MoS2 domains and for NW growth along the interior region of 2D micro-plates. Analysis of NW crystal structures formed under the optimal SA-vdWE condition revealed a disordered combination of wurtzite and zinc-blend phases. A transformation of the NW sidewall faceting structure is observed, resulting from simultaneous radial overgrowth during axial NW synthesis. A common lattice arrangement between axially-grown InAs NW core segments and MoS2 domains is described as the epitaxial basis for vertical NW growth. A model is proposed for a common InAs/MoS2 sub-lattice structure, consisting of three multiples of the cubic InAs unit cell along the [21Ì1Ì] direction, commensurately aligned with a 14-fold multiple of the Mo-Mo (or S-S) spacing along the [101Ì0] direction of MoS2 hexagonal lattice. The SA-vdWE growth mode described here enables controlled hybrid integration of mixed-dimensional III-V-on-2D heterostructures as novel nanosystems for applications in optoelectronics, nanoelectronics, and quantum enabling technologies.
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Atomic vacancies related to structural disorder and doping variation influence carrier transport in monolayer transition-metal dichalcogenide devices. Here, we investigate the effect of hydrogen plasma exposure (HPE) on monolayer MoS2 field-effect transistors (FETs). We observe that a 1% increase in sulfur vacancy after HPE results in incremental 0.06 eV of the Schottky barrier. Short-range scattering from the sulfur vacancies reduces the carrier mobility of monolayer MoS2 by 2 orders of magnitude. Despite the defects and grain boundaries formed during the chemical vapor deposition and transferring process, the surface desulfurization induced by the proton exposure and thermally accelerated oxidation can be blocked by monolayer graphene cladding with a van der Waals contact distance of 2.5 Å. The material-level study indicates a promising route for a low-cost and robust fabrication of smart sensor circuits on a monolithic MoS2 wafer, where the bare MoS2 FETs can serve as proton sensors, with their electronic readout processed by a logic circuit of graphene-protected pristine FETs with a high on/off ratio.
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The mechanical and electronic properties of two-dimensional materials make them promising for use in flexible electronics1-3. Their atomic thickness and large-scale synthesis capability could enable the development of 'smart skin'1,3-5, which could transform ordinary objects into an intelligent distributed sensor network6. However, although many important components of such a distributed electronic system have already been demonstrated (for example, transistors, sensors and memory devices based on two-dimensional materials1,2,4,7), an efficient, flexible and always-on energy-harvesting solution, which is indispensable for self-powered systems, is still missing. Electromagnetic radiation from Wi-Fi systems operating at 2.4 and 5.9 gigahertz8 is becoming increasingly ubiquitous and would be ideal to harvest for powering future distributed electronics. However, the high frequencies used for Wi-Fi communications have remained elusive to radiofrequency harvesters (that is, rectennas) made of flexible semiconductors owing to their limited transport properties9-12. Here we demonstrate an atomically thin and flexible rectenna based on a MoS2 semiconducting-metallic-phase heterojunction with a cutoff frequency of 10 gigahertz, which represents an improvement in speed of roughly one order of magnitude compared with current state-of-the-art flexible rectifiers9-12. This flexible MoS2-based rectifier operates up to the X-band8 (8 to 12 gigahertz) and covers most of the unlicensed industrial, scientific and medical radio band, including the Wi-Fi channels. By integrating the ultrafast MoS2 rectifier with a flexible Wi-Fi-band antenna, we fabricate a fully flexible and integrated rectenna that achieves wireless energy harvesting of electromagnetic radiation in the Wi-Fi band with zero external bias (battery-free). Moreover, our MoS2 rectifier acts as a flexible mixer, realizing frequency conversion beyond 10 gigahertz. This work provides a universal energy-harvesting building block that can be integrated with various flexible electronic systems.
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Integration schemes are implemented with a plane-wave basis in the context of real-time time-dependent density functional theory. Crank-Nicolson methods and three classes of explicit integration schemes are explored and assessed in terms of their accuracy and stability properties. Within the framework of plane-wave density functional theory, a graphene monolayer system is used to investigate the error, stability, and serial computational cost of these methods. The results indicate that Adams-Bashforth and Adams-Bashforth-Moulton methods of orders 4 and 5 outperform commonly used methods, including Crank-Nicolson and Runge-Kutta methods, in simulations where a relatively low error is desired. Parallel runtime scaling of the most competitive serial methods is presented, further demonstrating that the Adams-Bashforth and Adams-Bashforth-Moulton methods are efficient methods for propagating the time-dependent Kohn-Sham equations. Our integration schemes are implemented as an extension to the Quantum ESPRESSO code.
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The chemical vapor deposition (CVD)-grown two-dimensional molybdenum disulfide (MoS2) structures comprise of flakes of few layers with different dimensions. The top layers are relatively smaller in size than the bottom layers, resulting in the formation of edges/steps across adjacent layers. The strain response of such few-layer terraced structures is therefore likely to be different from exfoliated few-layered structures with similar dimensions without any terraces. In this study, the strain response of CVD-grown few-layered MoS2 terraced structures is investigated at the atomic scales using classic molecular dynamics (MD) simulations. MD simulations suggest that the strain relaxation of CVD-grown triangular terraced structures is observed in the vertical displacement of the atoms across the layers that results in the formation of Moiré patterns. The Moiré islands are observed to nucleate at the corners or edges of the few-layered structure and propagate inwards under both tensile and compressive strains. The nucleation of these islands is observed to happen at tensile strains of ~ 2% and at compressive strains of ~2.5%. The vertical displacements of the atoms and the dimensions of the Moiré islands predicted using the MD simulation are in excellent agreement with that observed experimentally.
RESUMEN
Two-dimensional transition-metal dichalcogenides (TMDs) are unique candidates for the development of next-generation electronic devices. However, the large contact resistance between metal and the monolayer TMDs have significantly limited the devices' performance. Also, the integration of ultrathin high- k dielectric layers with TMDs remains difficult due to the lack of dangling bonds on the surface of TMDs. We present monolayer molybdenum disulfide field-effect transistors with bottom local gates consisting of monolayer graphene. The atomic-level thickness and surface roughness of graphene facilitate the growth of high-quality ultrathin HfO2 and suppress gate leakage. Strong displacement fields above 8 V/nm can be applied using a single graphene gate to electrostatically dope the MoS2, which reduces the contact resistances between Ni and monolayer MoS2 to 2.3 kΩ·µm at low gate voltages. The devices exhibit excellent switching characteristics including a near-ideal subthreshold slope of 64 millivolts per decade, low threshold voltage (â¼0.5 V), high channel conductance (>100 µS/µm), and low hysteresis. Scaled devices with 50 and 14 nm channels as well as ultrathin (5 nm) gate dielectrics show effective immunity to short-channel effects. The device fabricated on flexible polymeric substrate also exhibits high performance and has a fully transparent channel region that is desirable in optical-related studies and practical applications.
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The mechanisms of carrier transport in the cross-plane crystal orientation of transition metal dichalcogenides are examined. The study of in-plane electronic properties of these van der Waals compounds has been the main research focus in recent years. However, the distinctive physical anisotropies, short-channel physics, and tunability of cross layer interactions can make the study of their electronic properties along the out-of-plane crystal orientation valuable. Here, the out-of-plane carrier transport mechanisms in niobium diselenide and hafnium disulfide are explored as two broadly different representative materials. Temperature-dependent current-voltage measurements are preformed to examine the mechanisms involved. First principles simulations and a tunneling model are used to understand these results and quantify the barrier height and hopping distance properties. Using Raman spectroscopy, the thermal response of the chemical bonds is directly explored and the insight into the van der Waals gap properties is acquired. These results indicate that the distinct cross-plane carrier transport characteristics of the two materials are a result of material thermal properties and thermally mediated transport of carriers through the van der Waals gaps. Exploring the cross-plane electron transport, the exciting physics involved is unraveled and potential new avenues for the electronic applications of van der Waals layers are inspired.
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Transition metal dichalcogenides (TMDs) are particularly sensitive to mechanical strain because they are capable of experiencing high atomic displacements without nucleating defects to release excess energy. Being promising for photonic applications, it has been shown that as certain phases of layered TMDs MX2 (M = Mo or W; X = S, Se, or Te) are scaled to a thickness of one monolayer, the photoluminescence response is dramatically enhanced due to the emergence of a direct electronic band gap compared with their multilayer or bulk counterparts, which typically exhibit indirect band gaps. Recently, mechanical strain has also been predicted to enable direct excitonic recombination in these materials, in which large changes in the photoluminescence response will occur during an indirect-to-direct band gap transition brought on by elastic tensile strain. Here, we demonstrate an enhancement of 2 orders of magnitude in the photoluminescence emission intensity in uniaxially strained single crystalline WSe2 bilayers. Through a theoretical model that includes experimentally relevant system conditions, we determine this amplification to arise from a significant increase in direct excitonic recombination. Adding confidence to the high levels of elastic strain achieved in this report, we observe strain-independent, mode-dependent Grüneisen parameters over the entire range of tensile strain (1-3.59%), which were obtained as 1.149 ± 0.027, 0.307 ± 0.061, and 0.357 ± 0.103 for the E2g, A1g, and A21g optical phonon modes, respectively. These results can inform the predictive strain-engineered design of other atomically thin indirect semiconductors, in which a decrease in out-of-plane bonding strength may lead to an increase in the strength of strain-coupled optoelectronic effects.
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The application of strain to semiconductors allows for controlled modification of their band structure. This principle is employed for the manufacturing of devices ranging from high-performance transistors to solid-state lasers. Traditionally, strain is typically achieved via growth on lattice-mismatched substrates. For two-dimensional (2D) semiconductors, this is not feasible as they typically do not interact epitaxially with the substrate. Here, we demonstrate controlled strain engineering of 2D semiconductors during synthesis by utilizing the thermal coefficient of expansion mismatch between the substrate and semiconductor. Using WSe2 as a model system, we demonstrate stable built-in strains ranging from 1% tensile to 0.2% compressive on substrates with different thermal coefficient of expansion. Consequently, we observe a dramatic modulation of the band structure, manifested by a strain-driven indirect-to-direct bandgap transition and brightening of the dark exciton in bilayer and monolayer WSe2, respectively. The growth method developed here should enable flexibility in design of more sophisticated devices based on 2D materials.Strain engineering is an essential tool for modifying local electronic properties in silicon-based electronics. Here, Ahn et al. demonstrate control of biaxial strain in two-dimensional materials based on the growth substrate, enabling more complex low-dimensional electronics.
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The strong in-plane anisotropy of rhenium disulfide (ReS2) offers an additional physical parameter that can be tuned for advanced applications such as logic circuits, thin-film polarizers, and polarization-sensitive photodetectors. ReS2 also presents advantages for optoelectronics, as it is both a direct-gap semiconductor for few-layer thicknesses (unlike MoS2 or WS2) and stable in air (unlike black phosphorus). Raman spectroscopy is one of the most powerful characterization techniques to nondestructively and sensitively probe the fundamental photophysics of a 2D material. Here, we perform a thorough study of the resonant Raman response of the 18 first-order phonons in ReS2 at various layer thicknesses and crystal orientations. Remarkably, we discover that, as opposed to a general increase in intensity of all of the Raman modes at excitonic transitions, each of the 18 modes behave differently relative to each other as a function of laser excitation, layer thickness, and orientation in a manner that highlights the importance of electron-phonon coupling in ReS2. In addition, we correct an unrecognized error in the calculation of the optical interference enhancement of the Raman signal of transition metal dichalcogenides on SiO2/Si substrates that has propagated through various reports. For ReS2, this correction is critical to properly assessing the resonant Raman behavior. We also implemented a perturbation approach to calculate frequency-dependent Raman intensities based on first-principles and demonstrate that, despite the neglect of excitonic effects, useful trends in the Raman intensities of monolayer and bulk ReS2 at different laser energies can be accurately captured. Finally, the phonon dispersion calculated from first-principles is used to address the possible origins of unexplained peaks observed in the Raman spectra, such as infrared-active modes, defects, and second-order processes.
RESUMEN
The potential of the applicability of two-dimensional molybdenum disulfide (MoS2) structures, in various electronics, optoelectronics, and flexible devices requires a fundamental understanding of the effects of strain on the electronic, magnetic and optical properties. Particularly important is the recent capability to grow large flakes of few-layered structures using chemical vapor deposition (CVD) wherein the top layers are relatively smaller in size than the bottom layers, resulting in the presence of edges/steps across adjacent layers. This paper investigates the strain response of such suspended few-layered structures at the atomic scales using classic molecular dynamics (MD) simulations. MD simulations suggest that the suspended CVD-grown structures are able to relax the applied in-plane strain through the nucleation of ripples under both tensile and compressive loading conditions. The presence of terraced edges in these structures is the cause for the nucleation of ripples at the edges that grow towards the center of the structure under applied in-plane strains. The peak amplitudes of ripples observed are in excellent agreement with the experimental observations. The study provides critical insights into the mechanisms of strain relaxation of suspended few-layered MoS2 structures that determine the interplay between the mechanical response and the electronic properties of CVD-grown structures.
RESUMEN
The interfaces in devices made of two-dimensional materials such as MoS2 can effectively control their optoelectronic performance. However, the extent and nature of these deterministic interactions are not fully understood. Here, we investigate the role of substrate interfaces on the photodetector properties of MoS2 devices by studying its photocurrent properties on both SiO2 and self-assembled monolayer-modified substrates. Results indicate that while the photoresponsivity of the devices can be enhanced through control of device interfaces, response times are moderately compromised. We attribute this trade-off to the changes in the electrical contact resistance at the device metal-semiconductor interface. We demonstrate that the formation of charge carrier traps at the interface can dominate the device photoresponse properties. The capture and emission rates of deeply trapped charge carriers in the substrate-semiconductor-metal regions are strongly influenced by exposure to light and can dynamically dope the contact regions and thus perturb the photodetector properties. As a result, interface-modified photodetectors have significantly lower dark-currents and higher on-currents. Through appropriate interfacial design, a record high device responsivity of 4.5 × 103 A/W at 7 V is achieved, indicative of the large signal gain in the devices and exemplifying an important design strategy that enables highly responsive two-dimensional photodetectors.
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Nonvolatile charge-trap memory plays an important role in many modern electronics technologies, from portable electronic systems to large-scale data centers. Conventional charge-trap memory devices typically work with fixed channel carrier polarity and device characteristics. However, many emerging applications in reconfigurable electronics and neuromorphic computing require dynamically tunable properties in their electronic device components that can lead to enhanced circuit versatility and system functionalities. Here, we demonstrate an ambipolar black phosphorus (BP) charge-trap memory device with dynamically reconfigurable and polarity-reversible memory behavior. This BP memory device shows versatile memory properties subject to electrostatic bias. Not only the programmed/erased state current ratio can be continuously tuned by the back-gate bias, but also the polarity of the carriers in the BP channel can be reversibly switched between electron- and hole-dominated conductions, resulting in the erased and programmed states exhibiting interchangeable high and low current levels. The BP memory also shows four different memory states and, hence, 2-bit per cell data storage for both n-type and p-type channel conductions, demonstrating the multilevel cell storage capability in a layered material based memory device. The BP memory device with a high mobility and tunable programmed/erased state current ratio and highly reconfigurable device characteristics can offer adaptable memory device properties for many emerging applications in electronics technology, such as neuromorphic computing, data-adaptive energy efficient memory, and dynamically reconfigurable digital circuits.
RESUMEN
One of the major challenges facing the rapidly growing field of two-dimensional (2D) transition metal dichalcogenides (TMDCs) is the development of growth techniques to enable large-area synthesis of high-quality materials. Chemical vapor deposition (CVD) is one of the leading techniques for the synthesis of TMDCs; however, the quality of the material produced is limited by defects formed during the growth process. A very useful nondestructive technique that can be utilized to probe defects in semiconductors is the room-temperature photoluminescence (PL) quantum yield (QY). It was recently demonstrated that a PL QY near 100% can be obtained in MoS2 and WS2 monolayers prepared by micromechanical exfoliation by treating samples with an organic superacid: bis(trifluoromethane)sulfonimide (TFSI). Here we have performed a thorough exploration of this chemical treatment on CVD-grown MoS2 samples. We find that the as-grown monolayers must be transferred to a secondary substrate, which releases strain, to obtain high QY by TFSI treatment. Furthermore, we find that the sulfur precursor temperature during synthesis of the MoS2 plays a critical role in the effectiveness of the treatment. By satisfying the aforementioned conditions we show that the PL QY of CVD-grown monolayers can be improved from â¼0.1% in the as-grown case to â¼30% after treatment, with enhancement factors ranging from 100 to 1500× depending on the initial monolayer quality. We also found that after TFSI treatment the PL emission from MoS2 films was visible by eye despite the low absorption (5-10%). The discovery of an effective passivation strategy will speed the development of scalable high-performance optoelectronic and electronic devices based on MoS2.
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Gold-mediated exfoliation of ultralarge optoelectronically perfect monolayers with lateral dimensions up to ≈500 µm is reported. Electrical, optical, and X-ray photo-electron spectroscopy characterization show that the quality of the gold-exfoliated flakes is similar to that of tape-exfoliated flakes. Large-area flakes allow manufacturing of large-area mono-layer transition metal dichalcogenide electronics.
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One of the most fascinating properties of molybdenum disulfide (MoS2) is its ability to be subjected to large amounts of strain without experiencing degradation. The potential of MoS2 mono- and few-layers in electronics, optoelectronics, and flexible devices requires the fundamental understanding of their properties as a function of strain. While previous reports have studied mechanically exfoliated flakes, tensile strain experiments on chemical vapor deposition (CVD)-grown few-layered MoS2 have not been examined hitherto, although CVD is a state of the art synthesis technique with clear potential for scale-up processes. In this report, we used CVD-grown terrace MoS2 layers to study how the number and size of the layers affected the physical properties under uniaxial and biaxial tensile strain. Interestingly, we observed significant shifts in both the Raman in-plane mode (as high as -5.2 cm(-1)) and photoluminescence (PL) energy (as high as -88 meV) for the few-layered MoS2 under â¼1.5% applied uniaxial tensile strain when compared to monolayers and few-layers of MoS2 studied previously. We also observed slippage between the layers which resulted in a hysteresis of the Raman and PL spectra during further applications of strain. Through DFT calculations, we contended that this random layer slippage was due to defects present in CVD-grown materials. This work demonstrates that CVD-grown few-layered MoS2 is a realistic, exciting material for tuning its properties under tensile strain.
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In recent times, atomically thin alloys of boron, nitrogen, and carbon have generated significant excitement as a composition-tunable two-dimensional (2D) material that demonstrates rich physics as well as application potentials. The possibility of tunably incorporating oxygen, a group VI element, into the honeycomb sp(2)-type 2D-BNC lattice is an intriguing idea from both fundamental and applied perspectives. We present the first report on an atomically thin quaternary alloy of boron, nitrogen, carbon, and oxygen (2D-BNCO). Our experiments suggest, and density functional theory (DFT) calculations corroborate, stable configurations of a honeycomb 2D-BNCO lattice. We observe micrometer-scale 2D-BNCO domains within a graphene-rich 2D-BNC matrix, and are able to control the area coverage and relative composition of these domains by varying the oxygen content in the growth setup. Macroscopic samples comprising 2D-BNCO domains in a graphene-rich 2D-BNC matrix show graphene-like gate-modulated electronic transport with mobility exceeding 500 cm(2) V(-1) s(-1), and Arrhenius-like activated temperature dependence. Spin-polarized DFT calculations for nanoscale 2D-BNCO patches predict magnetic ground states originating from the B atoms closest to the O atoms and sizable (0.6 eV < E g < 0.8 eV) band gaps in their density of states. These results suggest that 2D-BNCO with novel electronic and magnetic properties have great potential for nanoelectronics and spintronic applications in an atomically thin platform.