Pseudo-atomic orbital behavior in graphene nanoribbons with four-membered rings

Jacobse, Peter H.; Jin, Zexin; Jiang, Jingwei; Peurifoy, Samuel; Yue, Ziqin; Wang, Ziyi; Rizzo, Daniel J.; Louie, Steven G.; Nuckolls, Colin; Crommie, Michael F.

doi:10.1126/sciadv.abl5892

Title: Pseudo-atomic orbital behavior in graphene nanoribbons with four-membered rings

Journal Article · 23 December 2021 · Science Advances

DOI: https://doi.org/10.1126/sciadv.abl5892 · OSTI ID:1854847

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Univ. of California, Berkeley, CA (United States)
Columbia Univ., New York, NY (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoSciences Institute, Berkeley, CA (United States)

The incorporation of nonhexagonal rings into graphene nanoribbons (GNRs) is an effective strategy for engineering localized electronic states, bandgaps, and magnetic properties. Here, we demonstrate the successful synthesis of nanoribbons having four-membered ring (cyclobutadienoid) linkages by using an on-surface synthesis approach involving direct contact transfer of coronene-type precursors followed by thermally assisted [2 + 2] cycloaddition. The resulting coronene-cyclobutadienoid nanoribbons feature a narrow 600-meV bandgap and novel electronic frontier states that can be interpreted as linear chains of effective p_x and p_y pseudo-atomic orbitals. We show that these states give rise to exceptional physical properties, such as a rigid indirect energy gap. This provides a previously unexplored strategy for constructing narrow gap GNRs via modification of precursor molecules whose function is to modulate the coupling between adjacent four-membered ring states.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); Office of Naval Research; USDOE Office of Science (SC), High Energy Physics (HEP) (SC-25)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1854847

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 52 Vol. 7; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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