Five-Membered Rings Create Off-Zero Modes in Nanographene

Jacobse, Peter H.; Daugherty, Michael C.; Čerņevičs, Kristia̅ns; Wang, Ziyi; McCurdy, Ryan D.; Yazyev, Oleg V.; Fischer, Felix R.; Crommie, Michael F.

doi:10.1021/acsnano.3c06006

Title: Five-Membered Rings Create Off-Zero Modes in Nanographene

Journal Article · 05 December 2023 · ACS Nano

DOI: https://doi.org/10.1021/acsnano.3c06006 · OSTI ID:2228544

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^[2]; Čerņevičs, Kristia̅ns ^[3];

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University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
University of California, Berkeley, CA (United States)
Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne (Switzerland)

The low-energy electronic structure of nanographenes can be tuned through zero-energy π-electron states, typically referred to as zero-modes. Customizable electronic and magnetic structures have been engineered by coupling zero-modes through exchange and hybridization interactions. Manipulation of the energy of such states, however, has not yet received significant attention. We find that attaching a five-membered ring to a zigzag edge hosting a zero-mode perturbs the energy of that mode and turns it into an off-zero mode: a localized state with a distinctive electron-accepting character. Whereas the end states of typical 7- atom-wide armchair graphene nanoribbons (7-AGNRs) lose their electrons when physisorbed on Au(111) (due to its high work function), converting them into off-zero modes by introducing cyclopentadienyl five-membered rings allows them to retain their single-electron occupation. This approach enables the magnetic properties of 7-AGNR end states to be explored using scanning tunneling microscopy (STM) on a gold substrate. We find a gradual decrease of the magnetic coupling between offzero mode end states as a function of GNR length, and evolution from a more closed-shell to a more open-shell ground state.

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Research Organization:: University of California, Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); US Department of the Navy, Office of Naval Research (ONR); National Science Foundation (NSF); Swiss National Science Foundation (SNSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0023105; AC02-05-CH11231; N00014-19-1-2503; N00014-19-1-2596; CHE-2204252; 172543

OSTI ID:: 2228544

Alternate ID(s):: OSTI ID: 2263358

Journal Information:: ACS Nano, Vol. 17, Issue 24; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
nanographenes
five-membered rings
electronic structure
magnetic ground state
open shell
zero-modes
scanning tunneling microscopy
aromatic compounds
energy
hydrocarbons
quantum mechanics

Title: Five-Membered Rings Create Off-Zero Modes in Nanographene

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