One-Step Synthesis of NbSe2/Nb-Doped-WSe2 Metal/Doped-Semiconductor van der Waals Heterostructures for Doping Controlled Ohmic Contact.

van der Waals heterostructures (vdWHs) of metallic (m-) and semiconducting (s-) transition-metal dichalcogenides (TMDs) exhibit an ideal metal/semiconductor (M/S) contact in a field-effect transistor. However, in the current two-step chemical vapor deposition process, the synthesis of m-TMD on pregrown s-TMD contaminates the van der Waals (vdW) interface and hinders the doping of s-TMD. Here, NbSe2/Nb-doped-WSe2 metal-doped-semiconductor (M/d-S) vdWHs are created via a one-step synthesis approach using a niobium molar ratio-controlled solution-phase precursor. The one-step growth approach synthesizes Nb-doped WSe2 with a controllable doping concentration and metal/doped-semiconductor vdWHs. The hole carrier concentration can be precisely controlled by controlling the Nb/(W + Nb) molar ratio in the precursor solution from ∼3 × 1011/cm2 at Nb-0% to ∼1.38 × 1012/cm2 at Nb-60%; correspondingly, the contact resistance RC value decreases from 10 888.78 at Nb-0% to 70.60 kΩ.µm at Nb-60%. The Schottky barrier height measurement in the Arrhenius plots of ln(Isat/T2) versus q/KBT demonstrated an ohmic contact in the NbSe2/WxNb1-xSe2 vdWHs. Combining p-doping in WSe2 and M/d-S vdWHs, the mobility (27.24 cm2 V-1 s-1) and on/off ratio (2.2 × 107) are increased 1238 and 4400 times, respectively, compared to that using the Cr/pure-WSe2 contact (0.022 cm2 V-1 s-1 and 5 × 103, respectively). Together, the RC value using the NbSe2 contact shows 2.46 kΩ.µm, which is ∼29 times lower than that of using a metal contact. This method is expected to guide the synthesis of various M/d-S vdWHs and applications in future high-performance integrated circuits.

Selective Pattern Growth of Atomically Thin MoSe2 Films via a Surface-Mediated Liquid-Phase Promoter.

Two-dimensional transition metal dichalcogenides (TMDs) offer numerous advantages over silicon-based application in terms of atomically thin geometry, excellent opto-electrical properties, layer-number dependence, band gap variability, and lack of dangling bonds. The production of high-quality and large-scale TMD films is required with consideration of practical technology. However, the performance of scalable devices is affected by problems such as contamination and patterning arising from device processing; this is followed by an etching step, which normally damages the TMD film. Herein, we report the direct growth of MoSe2 films on selective pattern areas via a surface-mediated liquid-phase promoter using a solution-based approach. Our growth process utilizes the promoter on the selective pattern area by enhancing wettability, resulting in a highly uniform MoSe2 film. Moreover, our approach can produce other TMD films such as WSe2 films as well as control various pattern shapes, sizes, and large-scale areas, thus improving their applicability in various devices in the future. Our patterned MoSe2 field-effect transistor device exhibits a p-type dominant conduction behavior with a high on/off current ratio of ∼106. Thus, our study provides general guidance for direct selective pattern growth via a solution-based approach and the future design of integrated devices for a large-scale application.

Photoinduced Tuning of Schottky Barrier Height in Graphene/MoS2 Heterojunction for Ultrahigh Performance Short Channel Phototransistor.

Two-dimensional (2D) layered materials with properties such as a large surface-to-volume ratio, strong light interaction, and transparency are expected to be used in future optoelectronic applications. Many studies have focused on ways to increase absorption of 2D-layered materials for use in photodetectors. In this work, we demonstrate another strategy for improving photodetector performance using a graphene/MoS2 heterojunction phototransistor with a short channel length and a tunable Schottky barrier. The channel length of sub-30 nm, shorter than the diffusion length, decreases carrier recombination and carrier transit time in the channel and improves phototransistor performance. Furthermore, our graphene/MoS2 heterojunction phototransistor employed a tunable Schottky barrier that is only controlled by light and gate bias. It maintains a low dark current and an increased photocurrent. As a result, our graphene/MoS2 heterojunction phototransistor showed ultrahigh responsivity and detectivity of 2.2 × 105 A/W and 3.5 × 1013 Jones, respectively. This is a considerable improvement compared to previous pristine MoS2 phototransistors. We confirmed an effective method to develop phototransistors based on 2D materials and obtained ultrahigh performance of our phototransistor, which is promising for high-performance optoelectronic applications.

Unveiling the Hot Carrier Distribution in Vertical Graphene/h-BN/Au van der Waals Heterostructures for High-Performance Photodetector.

Graphene is one of the most promising materials for photodetectors due to its ability to convert photons into hot carriers within approximately 50 fs and generate long-lived thermalized states with lifetimes longer than 1 ps. In this study, we demonstrate a wide range of vertical photodetectors having a graphene/h-BN/Au heterostructure in which an hexagonal boron nitride (h-BN) insulating layer is inserted between an Au electrode and graphene photoabsorber. The photocarriers effectively tunnel through the small hole barrier (1.93 eV) at the Au/h-BN junction while the dark carriers are highly suppressed by a large electron barrier (2.27 eV) at the graphene/h-BN junction. Thus, an extremely low dark current of ∼10-13 A is achieved, which is 8 orders of magnitude lower than that of graphene lateral photodetector devices (∼10-5 A). Also, our device displays an asymmetric photoresponse behavior due to photothermionic emission at the graphene/h-BN and Au/h-BN junctions. The asymmetric behavior generates additional thermal carriers (hot carriers) to enable our device to generate photocurrents that can overcome the Schottky barrier. Furthermore, our device shows the highest value of the Iph/Idark ratio of ∼225 at 7 nm thick h-BN insulating layer, which is 3 orders of magnitude larger than that of the previously reported graphene lateral photodetectors without any active materials. In addition, we achieve a fast response speed of 12 µs of rise time and 5 µs of fall time, which are about 100 times faster than those of other graphene integrated photodetectors.

Schottky Barrier Variable Graphene/Multilayer-MoS2 Heterojunction Transistor Used to Overcome Short Channel Effects.

A single-layer MoS2 achieves excellent gate controllability within the nanoscale channel length of a field-effect transistor (FET) owing to an ultra-short screening length. However, multilayer MoS2 (ML-MoS2) is more vulnerable to short channel effects (SCEs) owing to its thickness and long screening length. We eliminated the SCEs in an ML-MoS2 FET (thickness of 4-13 nm) at a channel length of sub-30 nm using a Schottky barrier (SB) variable graphene/ML-MoS2 heterojunction. Although the band modulation in the ML-MoS2 channel worsens with a decrease in the channel length, which is similar to the SCEs occurring in conventional FETs, the variable Fermi level (EF) of a graphene electrode along the gate voltage allows control of the SB at the graphene/MoS2 junction and backs up the current modulation through a variable SB. Electrical measurements and a theoretical band simulation demonstrate the efficient SB modulation of our graphene nanogap (GrNG) ML-MoS2 FET with three distinct carrier transports along Vgs: a thermionic emission at a low SB, Fowler-Nordheim tunneling at a moderate SB, and direct tunneling at a high SB. Our GrNG FET shows an extremely high on-off current ratio of ∼108, which is approximately three-orders of magnitude better than a previously reported metal nanogap (MeNG) FET and a self-aligned metal/graphene nanogap FET with a similar MoS2 thickness. Our GrNG FET also exhibits a 100,000-times higher on-off ratio, 100-times lower subthreshold swing, and 10-times lower drain induced barrier.

Ultrahigh Gauge Factor in Graphene/MoS2 Heterojunction Field Effect Transistor with Variable Schottky Barrier.

Piezoelectricity of transition metal dichalcogenides (TMDs) under mechanical strain has been theoretically and experimentally studied. Powerful strain sensors using Schottky barrier variation in TMD/metal junctions as a result of the strain-induced lattice distortion and associated ion-charge polarization were demonstrated. However, the nearly fixed work function of metal electrodes limits the variation range of a Schottky barrier. We demonstrate a highly sensitive strain sensor using a variable Schottky barrier in a MoS2/graphene heterostructure field effect transistor (FET). The low density of states near the Dirac point in graphene allows large modulation of the graphene Fermi level and corresponding Schottky barrier in a MoS2/graphene junction by strain-induced polarized charges of MoS2. Our theoretical simulations and temperature-dependent electrical measurements show that the Schottky barrier change is maximized by placing the Fermi level of the graphene at the charge neutral (Dirac) point by applying gate voltage. As a result, the maximum Schottky barrier change (ΔΦSB) and corresponding current change ratio under 0.17% strain reach 118 meV and 978, respectively, resulting in an ultrahigh gauge factor of 575 294, which is approximately 500 times higher than that of metal/TMD junction strain sensors (1160) and 140 times higher than the conventional strain sensors (4036). The ultrahigh sensitivity of graphene/MoS2 heterostructure FETs can be developed for next-generation electronic and mechanical-electronic devices.

Direct growth of doping controlled monolayer WSe2 by selenium-phosphorus substitution.

Although many studies have been carried out on the doping of transition metal dichalcogenides (TMDCs), introducing controllable amounts of dopants into a TMD lattice is still insufficient. Here we demonstrate doping controlled TMDC growth by the replacement of selenium with phosphorus during the synthesis of the monolayer WSe2. The phosphorus doping density was precisely controlled by fine adjustment of the amount of P2O5 dopant powder along the pre-annealing time. Raman spectroscopy, photoluminescence (PL), X-ray photoelectron spectroscopy (XPS), and high-angle annular bright field scanning tunneling electron microscopy (HAADF STEM) provide evidence that P doping occurs within the WSe2 crystal with P occupying the substitutional Se sites. With regard to its electrical characteristics, the hole majority current of P-doped WSe2 is 100-times higher than that of the intrinsic WSe2. The measured doping concentration ranged from ∼8.16 × 1010 to ∼1.20 × 1012 depending on the amount of P2O5 dopant powder by pre-annealing.

Mobility Engineering in Vertical Field Effect Transistors Based on Van der Waals Heterostructures.

Vertical integration of 2D layered materials to form van der Waals heterostructures (vdWHs) offers new functional electronic and optoelectronic devices. However, the mobility in vertical carrier transport in vdWHs of vertical field-effect transistor (VFET) is not yet investigated in spite of the importance of mobility for the successful application of VFETs in integrated circuits. Here, the mobility in VFET of vdWHs under different drain biases, gate biases, and metal work functions is first investigated and engineered. The traps in WSe2 are the main source of scattering, which influences the vertical mobility and three distinct transport mechanisms: Ohmic transport, trap-limited transport, and space-charge-limited transport. The vertical mobility in VFET can be improved by suppressing the trap states by raising the Fermi level of WSe2 . This is achieved by increasing the injected carrier density by applying a high drain voltage, or decreasing the Schottky barrier at the graphene/WSe2 and metal/WSe2 junctions by applying a gate bias and reducing the metal work function, respectively. Consequently, the mobility in Mn vdWH at +50 V gate voltage is about 76 times higher than the initial mobility of Au vdWH. This work enables further improvements in the VFET for successful application in integrated circuits.

Two-terminal floating-gate memory with van der Waals heterostructures for ultrahigh on/off ratio.

Concepts of non-volatile memory to replace conventional flash memory have suffered from low material reliability and high off-state current, and the use of a thick, rigid blocking oxide layer in flash memory further restricts vertical scale-up. Here, we report a two-terminal floating gate memory, tunnelling random access memory fabricated by a monolayer MoS2/h-BN/monolayer graphene vertical stack. Our device uses a two-terminal electrode for current flow in the MoS2 channel and simultaneously for charging and discharging the graphene floating gate through the h-BN tunnelling barrier. By effective charge tunnelling through crystalline h-BN layer and storing charges in graphene layer, our memory device demonstrates an ultimately low off-state current of 10(-14) A, leading to ultrahigh on/off ratio over 10(9), about ∼10(3) times higher than other two-terminal memories. Furthermore, the absence of thick, rigid blocking oxides enables high stretchability (>19%) which is useful for soft electronics.