Cove-edged Chiral Graphene Nanoribbons with Chirality-Dependent Bandgap and Carrier Mobility

TL;DR

This study introduces a new class of cove-edged chiral graphene nanoribbons with tunable electronic properties, achieved through innovative synthesis and detailed characterization, enabling precise control over bandgap and carrier mobility for nanoelectronic applications.

Contribution

The paper presents the first synthesis and characterization of cove-edged chiral GNRs with adjustable chirality and optoelectronic properties, expanding the design space for graphene-based nanoelectronics.

Findings

(6,2)-CcGNR has a 1.37 eV bandgap and 8 cm²/Vs mobility.

(4,2)-CcGNR has a 1.26 eV bandgap and 14 cm²/Vs mobility.

Chirality-dependent tuning of GNR properties demonstrated.

Abstract

Graphene nanoribbons (GNRs) have garnered significant interest due to their highly customizable physicochemical properties and potential utility in nanoelectronics. Besides controlling widths and edge structures, the inclusion of chirality in GNRs brings another dimension for fine-tuning their optoelectronic properties, but related studies remain elusive owing to the absence of feasible synthetic strategies. Here, we demonstrate a novel class of cove-edged chiral GNRs (CcGNRs) with a tunable chiral vector (n,m). Notably, the bandgap and effective mass of (n,2)- CcGNR show a distinct positive correlation with the increasing value of n, as indicated by theory. Within this GNR family, two representative members, namely, (4,2)- CcGNR and (6,2)-CcGNR, are successfully synthesized. Both CcGNRs exhibit prominently curved geometries arising from the incorporated [4]helicene motifs along their peripheries, as also evidenced by the single-crystal structures of the two respective model compounds (1 and 2). The chemical identities and optoelectronic properties of (4,2)- and (6,2)-CcGNRs are comprehensively investigated via a combination of IR, Raman, solid-state NMR, UV-vis, and THz spectroscopies as well as theoretical calculations. In line with theoretical expectation, the obtained (6,2)-CcGNR possesses a low optical bandgap of 1.37 eV along with charge carrier mobility of 8 cm2/Vs, whereas (4,2)-CcGNR exhibits a narrower bandgap of 1.26 eV with increased mobility of 14 cm2/Vs. This work opens up a new avenue to precisely engineer the bandgap and carrier mobility of GNRs by manipulating their chiral vector.