Tunable Transport Gap in Phosphorene

In this article, we experimentally demonstrate that the transport gap of phosphorene can be tuned monotonically from ∼0.3 to ∼1.0 eV when the flake thickness is scaled down from bulk to a single layer. As a consequence, the ON current, the OFF current, and the current ON/OFF ratios of phosphorene field effect transistors (FETs) were found to be significantly impacted by the layer thickness. The transport gap was determined from the transfer characteristics of phosphorene FETs using a robust technique that has not been reported before. The detailed mathematical model is also provided. By scaling the thickness of the gate oxide, we were also able to demonstrate enhanced ambipolar conduction in monolayer and few layer phosphorene FETs. The asymmetry of the electron and the hole current was found to be dependent on the layer thickness that can be explained by dynamic changes of the metal Fermi level with the energy band of phosphorene depending on the layer number. We also extracted the Schottky barrier heights for both the electron and the hole injection as a function of the layer thickness. Finally, we discuss the dependence of field effect hole mobility of phosphorene on temperature and carrier concentration

Asymmetric Growth of Bilayer Graphene on Copper Enclosures Using Low-Pressure Chemical Vapor Deposition

In this work, we investigated the growth mechanisms of bilayer graphene on the outside surface of Cu enclosures at low pressures. We observed that the asymmetric growth environment of a Cu enclosure can yield a much higher (up to 100%) bilayer coverage on the outside surface as compared to the bilayer growth on a flat Cu foil, where both sides are exposed to the same growth environment. By simultaneously examining the graphene films grown on both the outside and inside surfaces of the Cu enclosure, we find that carbon can diffuse from the inside surface to the outside <i>via</i> exposed copper regions on the inside surface. The kinetics of this process are examined by coupling the asymmetric growth between the two surfaces through a carbon diffusion model. Finally, using these results, we show that the coverage of bilayer graphene can be tuned simply by changing the thickness of the Cu foil, further confirming our model of carbon delivery through the Cu foil

Black Phosphorus Radio-Frequency Transistors

Few-layer and thin film forms of layered black phosphorus (BP) have recently emerged as a promising material for applications in high performance nanoelectronics and infrared optoelectronics. Layered BP thin films offer a moderate bandgap of around 0.3 eV and high carrier mobility, which lead to transistors with decent on–off ratios and high on-state current densities. Here, we demonstrate the gigahertz frequency operation of BP field-effect transistors for the first time. The BP transistors demonstrated here show respectable current saturation with an on–off ratio that exceeds 2 × 10³. We achieved a current density in excess of 270 mA/mm and DC transconductance above 180 mS/mm for hole conduction. Using standard high frequency characterization techniques, we measured a short-circuit current-gain cutoff frequency <i>f</i>_T of 12 GHz and a maximum oscillation frequency <i>f</i>_max of 20 GHz in 300 nm channel length devices. BP devices may offer advantages over graphene transistors for high frequency electronics in terms of voltage and power gain due to the good current saturation properties arising from their finite bandgap, thus can be considered as a promising candidate for the future high performance thin film electronics technology for operation in the multi-GHz frequency range and beyond

Electrical Transport Properties of Polycrystalline Monolayer Molybdenum Disulfide

Semiconducting MoS₂ monolayers have shown many promising electrical properties, and the inevitable polycrystallinity in synthetic, large-area films renders understanding the effect of structural defects, such as grain boundaries (GBs, or line-defects in two-dimensional materials), essential. In this work, we first examine the role of GBs in the electrical-transport properties of MoS₂ monolayers with varying line-defect densities. We reveal a systematic degradation of electrical characteristics as the line-defect density increases. The two common MoS₂ GB types and their specific roles are further examined, and we find that only tilt GBs have a considerable effect on the MoS₂ electrical properties. By examining the electronic states and sources of disorder using temperature-dependent transport studies, we adopt the Anderson model for disordered systems to explain the observed transport behaviors in different temperature regimes. Our results elucidate the roles played by GBs in different scenarios and give insights into their underlying scattering mechanisms

Giant Mechano-Optoelectronic Effect in an Atomically Thin Semiconductor

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 E_2g, A_1g, and A²_1g 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

Integrated Circuits Based on Bilayer MoS₂ Transistors

Two-dimensional (2D) materials, such as molybdenum disulfide (MoS₂), have been shown to exhibit excellent electrical and optical properties. The semiconducting nature of MoS₂ allows it to overcome the shortcomings of zero-bandgap graphene, while still sharing many of graphene’s advantages for electronic and optoelectronic applications. Discrete electronic and optoelectronic components, such as field-effect transistors, sensors, and photodetectors made from few-layer MoS₂ show promising performance as potential substitute of Si in conventional electronics and of organic and amorphous Si semiconductors in ubiquitous systems and display applications. An important next step is the fabrication of fully integrated multistage circuits and logic building blocks on MoS₂ to demonstrate its capability for complex digital logic and high-frequency ac applications. This paper demonstrates an inverter, a NAND gate, a static random access memory, and a five-stage ring oscillator based on a direct-coupled transistor logic technology. The circuits comprise between 2 to 12 transistors seamlessly integrated side-by-side on a single sheet of bilayer MoS₂. Both enhancement-mode and depletion-mode transistors were fabricated thanks to the use of gate metals with different work functions

A Dynamically Reconfigurable Ambipolar Black Phosphorus Memory Device

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

Intricate Resonant Raman Response in Anisotropic ReS₂

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 <i>differently</i> 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

Graphene/MoS₂ Hybrid Technology for Large-Scale Two-Dimensional Electronics

Two-dimensional (2D) materials have generated great interest in the past few years as a new toolbox for electronics. This family of materials includes, among others, metallic graphene, semiconducting transition metal dichalcogenides (such as MoS₂), and insulating boron nitride. These materials and their heterostructures offer excellent mechanical flexibility, optical transparency, and favorable transport properties for realizing electronic, sensing, and optical systems on arbitrary surfaces. In this paper, we demonstrate a novel technology for constructing large-scale electronic systems based on graphene/molybdenum disulfide (MoS₂) heterostructures grown by chemical vapor deposition. We have fabricated high-performance devices and circuits based on this heterostructure, where MoS₂ is used as the transistor channel and graphene as contact electrodes and circuit interconnects. We provide a systematic comparison of the graphene/MoS₂ heterojunction contact to more traditional MoS₂-metal junctions, as well as a theoretical investigation, using density functional theory, of the origin of the Schottky barrier height. The tunability of the graphene work function with electrostatic doping significantly improves the ohmic contact to MoS₂. These high-performance large-scale devices and circuits based on this 2D heterostructure pave the way for practical flexible transparent electronics

Rapid Identification of Stacking Orientation in Isotopically Labeled Chemical-Vapor Grown Bilayer Graphene by Raman Spectroscopy

The growth of large-area bilayer graphene has been of technological importance for graphene electronics. The successful application of graphene bilayers critically relies on the precise control of the stacking orientation, which determines both electronic and vibrational properties of the bilayer system. Toward this goal, an effective characterization method is critically needed to allow researchers to easily distinguish the bilayer stacking orientation (i.e., AB stacked or turbostratic). In this work, we developed such a method to provide facile identification of the stacking orientation by isotope labeling. Raman spectroscopy of these isotopically labeled bilayer samples shows a clear signature associated with AB stacking between layers, enabling rapid differentiation between turbostratic and AB-stacked bilayer regions. Using this method, we were able to characterize the stacking orientation in bilayer graphene grown through Low Pressure Chemical Vapor Deposition (LPCVD) with enclosed Cu foils, achieving almost 70% AB-stacked bilayer graphene. Furthermore, by combining surface sensitive fluorination with such hybrid ¹²C/¹³C bilayer samples, we are able to identify that the second layer grows underneath the first-grown layer, which is similar to a recently reported observation