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Rotationally Commensurate Growth of MoS2 on Epitaxial Graphene

Published 3 Apr 2016 in cond-mat.mtrl-sci | (1604.00677v1)

Abstract: Atomically thin MoS2/graphene heterostructures are promising candidates for nanoelectronic and optoelectronic technologies. Among different graphene substrates, epitaxial graphene (EG) on SiC provides several potential advantages for such heterostructures including high electronic quality, tunable substrate coupling, wafer-scale processability, and crystalline ordering that can template commensurate growth. Exploiting these attributes, we demonstrate here the thickness-controlled van der Waals epitaxial growth of MoS2 on EG via chemical vapor deposition, giving rise to transfer-free synthesis of a two-dimensional heterostructure with registry between its constituent materials. The rotational commensurability observed between the MoS2 and EG is driven by the energetically favorable alignment of their respective lattices and results in nearly strain-free MoS2, as evidenced by synchrotron X-ray scattering and atomic-resolution scanning tunneling microscopy (STM). The electronic nature of the MoS2/EG heterostructure is elucidated with STM and scanning tunneling spectroscopy, which reveals bias-dependent apparent thickness, band bending, and a reduced bandgap of ~0.4 eV at the monolayer MoS2 edges.

Citations (169)

Summary

Rotationally Commensurate Growth of MoS₂ on Epitaxial Graphene

The study on rotationally commensurate growth of MoS₂ on epitaxial graphene (EG) offers significant insights into the advancements of van der Waals heterostructures, particularly in the context of nanoelectronic and optoelectronic applications. This paper demonstrates the transfer-free van der Waals epitaxial growth of MoS₂ on EG, leveraging the chemical vapor deposition (CVD) method to achieve thickness-controlled assembly and rotational commensurability. Key markers of this work include synchrotron X-ray scattering and scanning tunneling microscopy, which provide evidence of nearly strain-free MoS₂, hence indicating high quality crystal growth.

The qualitative advantages of epitaxial graphene on SiC substrates, such as wafer-scale processability, tunable substrate coupling, and high electronic quality, are harnessed to induce rotational commensurability in the MoS₂/EG heterostructure. The paper infers that due to the energetically favorable alignment of respective lattices, rotational commensurability results in reduced defect densities and sharper interfaces. X-ray scattering further underscores the lack of significant in-plane strain, asserting the ideal nature of this heterostructure for foundational studies and device applications.

Key Findings

The research achieves noteworthy progress in understanding the electronic properties of the MoS₂/EG heterostructure. Scanning tunneling spectroscopy (STS) analysis divulges distinct characteristics such as bias-dependent apparent thickness, band bending, and a reduced bandgap (~0.4 eV) at monolayer MoS₂ edges. The ability to control MoS₂ domain thickness by managing growth pressure is established, extending practical avenues for modulating electronic and structural behaviors. Additionally, significant electronic features, such as semiconducting MoS₂ density of states inversions at variable biases, are meticulously documented.

Through Raman spectroscopy and synchrotron X-ray scattering, researchers provided substantive validation of the nearly strain-free nature of the synthesized MoS₂ domains. By utilizing graphene as a substrate, significant enhancements in the electronic properties—particularly evident through bandgap modulation and doping levels—are demonstrated, reflecting the impact of substrate interactions on the growth dynamics of MoS₂.

Implications and Future Directions

This study paves the way for enhanced device functionalities using MoS₂/graphene heterostructures. The epitaxial method employed here holds expansive potential for extending van der Waals epitaxy to other two-dimensional materials. Exploring the formation of mirror twin grain boundaries, as proposed in the paper, presents a fertile area for future research, promising refined control over anisotropic properties like thermal conductance. It may also inspire inquiries into the role of grain boundaries in influencing optoelectronic properties and device efficiency.

The findings have concrete implications for energy applications, such as Li-ion battery anodes and hydrogen evolution catalysts, where MoS₂ has shown tremendous promise. As rotational commensurability is achieved, the fundamental exploration of interfacial interactions may yield insights into novel electronic functionalities, reinforcing the relevance of these heterostructures in next-generation electronic and optical devices.

This study provides a well-defined framework to further explore the properties and applications of van der Waals heterostructures, pushing the boundaries of material science and engineering in the field of two-dimensional materials. Its methodical approach in examining the MoS₂/EG interaction dynamics presents a compelling case for leveraging epitaxial graphene substrates in future material synthesis endeavors.

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