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Charge Transport in Polycrystalline Graphene: Challenges and Opportunities

Published 22 Jul 2015 in cond-mat.mtrl-sci | (1507.06272v1)

Abstract: Graphene has attracted significant interest both for exploring fundamental science and for a wide range of technological applications. Chemical vapor deposition (CVD) is currently the only working approach to grow graphene at wafer scale, which is required for industrial applications. Unfortunately, CVD graphene is intrinsically polycrystalline, with pristine graphene grains stitched together by disordered grain boundaries, which can be either a blessing or a curse. On the one hand, grain boundaries are expected to degrade the electrical and mechanical properties of polycrystalline graphene, rendering the material undesirable for many applications. On the other hand, they exhibit an increased chemical reactivity, suggesting their potential application to sensing or as templates for synthesis of one-dimensional materials. Therefore, it is important to gain a deeper understanding of the structure and properties of graphene grain boundaries. Here, we review experimental progress on identification and electrical and chemical characterization of graphene grain boundaries. We use numerical simulations and transport measurements to demonstrate that electrical properties and chemical modification of graphene grain boundaries are strongly correlated. This not only provides guidelines for the improvement of graphene devices, but also opens a new research area of engineering graphene grain boundaries for highly sensitive electrobiochemical devices.

Citations (170)

Summary

Charge Transport in Polycrystalline Graphene: Challenges and Opportunities

Polycrystalline graphene synthesized via chemical vapor deposition (CVD) emerges as a critical subject of research due to its widespread applications in both fundamental science and industrial technology. This paper by Cummings et al. explores the complex interplay between grain boundaries (GGBs) within polycrystalline graphene and the material's charge transport properties. The investigation underscores both the challenges and opportunities presented by these unique and intricate structures.

Graphene’s exceptional mechanical and electronic properties make it a highly sought-after material for various applications, including flexible electronics and optoelectronic devices. The ability to grow graphene at wafer-scale using CVD is particularly beneficial for large-area applications, yet it inherently produces polycrystalline sheets. GGBs, with their intrinsic disorder, pose significant challenges for achieving high carrier mobility—a crucial factor for electronic applications. However, their enhanced chemical reactivity presents opportunities for novel sensor applications and templating for one-dimensional material synthesis.

Structural Characterization of Grain Boundaries

The structure of GGBs significantly influences their mechanical, electrical, and chemical properties. These boundaries feature chains of pentagonal, hexagonal, and heptagonal rings that emerge between graphene domains with differing orientations. Characterized by techniques such as TEM and STM, GGBs can drastically alter the mechanical properties of graphene, reducing its intrinsic strength due to stress concentrations that lead to buckling or fracture. Furthermore, advancements in TEM have facilitated mapping of graphene grain orientations, aiding in the visualization and understanding of GGBs.

Charge Transport Characteristics

Electrical transport through GGBs remains a focal point due to their role in scattering carriers, thus limiting carrier mobility. Various experimental techniques including two-probe STM measurements, four-probe resistivity assessments, and global scaling laws, elucidate the contributions of GGBs to electron transport. Notably, these boundaries introduce energy barriers and localized states on account of defects within the lattice, which correlate to increased resistance across them. Charge transport mapping reveals that while GGBs diminish mobility, they can also exhibit p-n junction-like characteristics that may be harnessed for electronic devices.

Functionalization and Reactivity

The unique chemical reactivity of GGBs provides opportunities for selective functionalization, which is pivotal for sensing applications. Experimental studies demonstrate that GGBs can be selectively functionalized with ozone in an oxygen-rich environment, as confirmed through changes in resistivity measurements post-functionalization. This selective reactivity is attributed to the non-hexagonal atomic arrangements prevalent in GGBs, which are more chemically active compared to the basal plane of graphene.

Future Directions and Implications

The paper posits potential future directions for the engineering of GGBs, advocating for controlled synthesis methodologies to enhance the material's electronic properties. Additionally, the ability to selectively functionalize GGBs opens avenues for their use as templates in synthesis and for high-sensitivity biochemical sensors. Understanding and ultimately controlling the atomic structure of these grain boundaries presents a substantial opportunity for advancements in spintronic and optoelectronic applications based on graphene.

Overall, this paper offers a comprehensive analysis of the challenges inherent in polycrystalline graphene due to GGBs, while highlighting viable strategies for exploiting these features for advanced applications. Continuous research aimed at tailoring GGBs will undoubtedly foster the development of new technologies leveraging the attributes of this promising material.

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