Five-Membered Rings Create Off-Zero Modes in Nanographene
Abstract
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.
- Authors:
-
[1];
[2];
[4];
[2];
[3];
[5];
[6]
- Department of Physics, University of California, Berkeley, California 94720, United States, Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
- Department of Chemistry, University of California, Berkeley, California 94720, United States
- Institute of Physics, Ecole Polytechnique Fédérale de Lausanne (EPFL), 1015 Lausanne, Switzerland
- Department of Physics, University of California, Berkeley, California 94720, United States, Department of Chemistry, University of California, Berkeley, California 94720, United States, Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States, Kavli Energy NanoSciences Institute at the University of California, Berkeley and the Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
- Department of Chemistry, University of California, Berkeley, California 94720, United States, Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States, Kavli Energy NanoSciences Institute at the University of California, Berkeley and the Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States, Bakar Institute of Digital Materials for the Planet, Division of Computing, Data Science, and Society, University of California, Berkeley, California 94720, United States
- Department of Physics, University of California, Berkeley, California 94720, United States, Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States, Kavli Energy NanoSciences Institute at the University of California, Berkeley and the Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
- Publication Date:
- Research Org.:
- Univ. of California, Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); 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)
- OSTI Identifier:
- 2228544
- Alternate Identifier(s):
- OSTI ID: 2263358
- Grant/Contract Number:
- SC0023105; AC02-05-CH11231; N00014-19-1-2503; N00014-19-1-2596; CHE-2204252; 172543
- Resource Type:
- Published Article
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Name: ACS Nano Journal Volume: 17 Journal Issue: 24; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 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
Citation Formats
Jacobse, Peter H., Daugherty, Michael C., Čerņevičs, Kristia̅ns, Wang, Ziyi, McCurdy, Ryan D., Yazyev, Oleg V., Fischer, Felix R., and Crommie, Michael F. Five-Membered Rings Create Off-Zero Modes in Nanographene. United States: N. p., 2023.
Web. doi:10.1021/acsnano.3c06006.
Jacobse, Peter H., Daugherty, Michael C., Čerņevičs, Kristia̅ns, Wang, Ziyi, McCurdy, Ryan D., Yazyev, Oleg V., Fischer, Felix R., & Crommie, Michael F. Five-Membered Rings Create Off-Zero Modes in Nanographene. United States. https://doi.org/10.1021/acsnano.3c06006
Jacobse, Peter H., Daugherty, Michael C., Čerņevičs, Kristia̅ns, Wang, Ziyi, McCurdy, Ryan D., Yazyev, Oleg V., Fischer, Felix R., and Crommie, Michael F. Tue .
"Five-Membered Rings Create Off-Zero Modes in Nanographene". United States. https://doi.org/10.1021/acsnano.3c06006.
@article{osti_2228544,
title = {Five-Membered Rings Create Off-Zero Modes in Nanographene},
author = {Jacobse, Peter H. and Daugherty, Michael C. and Čerņevičs, Kristia̅ns and Wang, Ziyi and McCurdy, Ryan D. and Yazyev, Oleg V. and Fischer, Felix R. and Crommie, Michael F.},
abstractNote = {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.},
doi = {10.1021/acsnano.3c06006},
journal = {ACS Nano},
number = 24,
volume = 17,
place = {United States},
year = {Tue Dec 05 00:00:00 EST 2023},
month = {Tue Dec 05 00:00:00 EST 2023}
}
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