skip to main content


This content will become publicly available on August 7, 2024

Title: Hysteresis-free high mobility graphene encapsulated in tungsten disulfide

High mobility is a crucial requirement for a large variety of electronic device applications. The state of the art for high-quality graphene devices is based on heterostructures made with graphene encapsulated in >40 nm-thick flakes of hexagonal boron nitride (hBN). Unfortunately, scaling up multilayer hBN while precisely controlling the number of layers remains an outstanding challenge, resulting in a rough material unable to enhance the mobility of graphene. This leads to the pursuit of alternative, scalable materials, which can be used as substrates and encapsulants for graphene. Tungsten disulfide (WS2) is a transition metal dichalcogenide, which was grown in large (∼mm-size) multi-layers by chemical vapor deposition. However, the resistance vs gate voltage characteristics when gating graphene through WS2 exhibit largely hysteretic shifts of the charge neutrality point on the order of Δn∼ 3 × 1011 cm−2, hindering the use of WS2 as a reliable encapsulant. The hysteresis originates due to the charge traps from sulfur vacancies present in WS2. In this work, we report the use of WS2 as a substrate and overcome the hysteresis issues by chemically treating WS2 with a super-acid, which passivates these vacancies and strips the surface from contaminants. The hysteresis is significantly reduced by about two orders of magnitude, down to values as low as Δn∼ 2 × 109 cm−2, while the room-temperature mobility of WS2-encapsulated graphene is as high as ∼62 × 103 cm2 V−1 s−1 at a carrier density of n ∼ 1 ×1012 cm−2. Our results promote WS2 as a valid alternative to hBN as an encapsulant for high-performance graphene devices.

 
more » « less
Award ID(s):
2052527
NSF-PAR ID:
10496517
Author(s) / Creator(s):
; ; ; ; ; ; ;
Publisher / Repository:
Applied Physics Letters
Date Published:
Journal Name:
Applied Physics Letters
Volume:
123
Issue:
6
ISSN:
0003-6951
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Recently, 2D electron gases have been observed in atomically thin semiconducting crystals, enabling the observation of rich physical phenomena at the quantum level within the ultimate thickness limit. However, the observation of 2D electron gases and subsequent quantum Hall effect require exceptionally high crystalline quality, rendering mechanical exfoliation as the only method to produce high‐quality 2D semiconductors of black phosphorus and indium selenide (InSe), which hinder large‐scale device applications. Here, the controlled one‐step synthesis of high‐quality 2D InSe thin films via chemical vapor transport method is reported. The carrier Hall mobility of hexagonal boron nitride (hBN) encapsulated InSe flakes can be up to 5000 cm2V−1s−1at 1.5 K, enabling to observe the quantum Hall effect in a synthesized van der Waals semiconductor. The existence of the quantum Hall effect in directly synthesized 2D semiconductors indicates a high quality of the chemically synthesized 2D semiconductors, which hold promise in quantum devices and applications with high mobility.

     
    more » « less
  2. Abstract

    The emergence of memristive behavior in amorphous–crystalline 2D oxide heterostructures, which are synthesized by atomic layer deposition (ALD) of a few‐nanometer amorphous Al2O3layers onto atomically thin single‐crystalline ZnO nanosheets, is demonstrated. The conduction mechanism is identified based on classic oxygen vacancy conductive channels. ZnO nanosheets provide a 2D host for oxygen vacancies, while the amorphous Al2O3facilitates the generation and stabilization of the oxygen vacancies. The conduction mechanism in the high‐resistance state follows Poole–Frenkel emission, and in the the low‐resistance state is fitted by the Mott–Gurney law. From the slope of the fitting curve, the mobility in the low‐resistance state is estimated to be ≈2400 cm2V−1s−1, which is the highest value reported in semiconductor oxides. When annealed at high temperature to eliminate oxygen vacancies, Al is doped into the ZnO nanosheet, and the memristive behavior disappears, further confirming the oxygen vacancies as being responsible for the memristive behavior. The 2D heterointerface offers opportunities for new design of high‐performance memristor devices.

     
    more » « less
  3. Abstract

    Heat dissipation is a major limitation of high‐performance electronics. This is especially important in emerging nanoelectronic devices consisting of ultra‐thin layers, heterostructures, and interfaces, where enhancement in thermal transport is highly desired. Here, ultra‐high interfacial thermal conductance in encapsulated van der Waals (vdW) heterostructures with single‐layer transition metal dichalcogenides MX2(MoS2, WSe2, WS2) sandwiched between two hexagonal boron nitride (hBN) layers is reported. Through Raman spectroscopic measurements of suspended and substrate‐supported hBN/MX2/hBN heterostructures with varying laser power and temperature, the out‐of‐plane interfacial thermal conductance in the vertical stack is calibrated. The measured interfacial thermal conductance between MX2and hBN reaches 74 ± 25 MW m−2K−1, which is at least ten times higher than the interfacial thermal conductance of MX2in non‐encapsulation structures. Molecular dynamics (MD) calculations verify and explain the experimental results, suggesting a full encapsulation by hBN layers is accounting for the high interfacial conductance. This ultra‐high interfacial thermal conductance is attributed to the double heat transfer pathways and the clean and tight vdW interface between two crystalline 2D materials. The findings in this study reveal new thermal transport mechanisms in hBN/MX2/hBN structures and shed light on building novel hBN‐encapsulated nanoelectronic devices with enhanced thermal management.

     
    more » « less
  4. Efficient charge collection is critical in large area (quasi-) planar configuration perovskite solar cells (PSCs) as the cell operation relies on the diffusion of photo-generated charge carriers to charge collector layers. Many defects/traps in the polycrystalline perovskite absorber layer strongly affect the charge collection efficiency because the 2D-like top charge collection layer barely penetrates into the 3D grain boundaries in the perovskite layer to efficiently collect the charge carrier. Inspired by blood capillaries for efficient mass exchange, a charge-collection nano-network for efficient charge collection was incorporated into the perovskite absorber using low-cost, stable amino-functionalized graphene (G-NH 2 ). The integration of such an unprecedented structure enables very efficient charge collection, leading to the significant enhancement of the power conversion efficiency of 1 × 1 cm 2 MAPbI 3 PSCs from 14.4 to 18.7% with higher reproducibility, smaller hysteresis and enhanced stability. The physicochemical mechanisms underlying the role of this nano charge-collection nano-network in boosting the charge collection in PSCs are elucidated comprehensively, using a combined experimental and theoretical approach, pointing to a new direction towards up-scaling of high-efficiency PSCs. 
    more » « less
  5. Abstract

    Resonant tunneling diodes with negative differential resistance (NDR) have attracted significant attention due to their unique quantum resonant tunneling phenomena and potential applications in terahertz emission/detection and high‐density logic/memory. In this paper, resonant tunneling devices, where the carriers tunnel through a hexagonal boron nitride (hBN) barrier sandwiched by two black phosphorus (BP) layers, are explored. The resonance occurs when the energy bands of the two black phosphorus layers are aligned. The conductive atomic force microscopy (CAFM) measurements reveal prominent NDR peaks with large peak‐to‐valley ratios at room temperature. It is found that the positions of the NDR peaks are very sensitive to the amplitude and the shape of the voltage waveform used in CAFM, which can be explained by the charge trapping effect. Furthermore, resonant tunneling transistors are demonstrated based on BP/hBN/BP stacks in which the locations of the NDR peaks are tunable by the electrostatic gating. As compared to the traditional tunneling diodes based on bulk materials, the tunneling devices based on thin boron nitride tunneling barrier and high mobility black phosphorus offer ultra‐high‐speed response. This feature, together with the NDR characteristics, provides the potential for applications in THz oscillators and multi‐value logic devices.

     
    more » « less