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  Regioselective On-Surface Synthesis of [3]Triangulene Graphene Nanoribbons

Daugherty, M. C., Jacobse, P. H., Jiang, J., Jornet-Somoza, J., Dorit, R., Wang, Z., et al. (2024). Regioselective On-Surface Synthesis of [3]Triangulene Graphene Nanoribbons. Journal of the American Chemical Society, 146(23), 15879-15886. doi:10.1021/jacs.4c02386.

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Supporting Information: Materials and methods, synthetic procedures, STM topographic and BRSTM images, dI/dV maps, STS data, and NMR spectra
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daugherty-et-al-2024-regioselective-on-surface-synthesis-of-3-triangulene-graphene-nanoribbons.pdf (Verlagsversion), 6MB
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© The Authors. Published by American Chemical Society.

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https://arxiv.org/abs/2402.15882 (Preprint)
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https://doi.org/10.1021/jacs.4c02386 (Verlagsversion)
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Urheber

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 Urheber:
Daugherty, M. C.1, Autor
Jacobse, P. H.2, Autor
Jiang, J.2, 3, Autor
Jornet-Somoza, J.4, 5, Autor           
Dorit, R.1, Autor
Wang, Ziyi1, 3, 6, Autor
Lu, J.2, Autor
McCurdy, R.1, Autor
Tang, W.2, 3, Autor
Rubio, A.4, 5, 7, Autor           
Louie, S. G.2, 3, Autor
Crommie, M. F.2, 3, 6, Autor
Fischer, F. R.1, 3, 6, 8, Autor
Affiliations:
1Department of Chemistry, University of California, ou_persistent22              
2Department of Physics, University of California, ou_persistent22              
3Materials Sciences Division, Lawrence Berkeley National Laborator, ou_persistent22              
4Nano-Bio Spectroscopy Group and ETSF, Universidad del País Vasco UPV/EHU, ou_persistent22              
5Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
6Kavli Energy NanoSciences Institute at the University of California Berkeley and the Lawrence Berkeley National Laboratory, ou_persistent22              
7Center for Computational Quantum Physics (CCQ), The Flatiron Institute, ou_persistent22              
8Bakar Institute of Digital Materials for the Planet, Division of Computing, Data Science, and Society, University of California, ou_persistent22              

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 Zusammenfassung: The integration of low-energy states into bottom-up engineered graphene nanoribbons (GNRs) is a robust strategy for realizing materials with tailored electronic band structure for nanoelectronics. Low-energy zero-modes (ZMs) can be introduced into nanographenes (NGs) by creating an imbalance between the two sublattices of graphene. This phenomenon is exemplified by the family of [n]triangulenes (n ∈ ℕ). Here, we demonstrate the synthesis of [3]triangulene-GNRs, a regioregular one-dimensional (1D) chain of [3]triangulenes linked by five-membered rings. Hybridization between ZMs on adjacent [3]triangulenes leads to the emergence of a narrow band gap, Eg,exp ∼ 0.7 eV, and topological end states that are experimentally verified using scanning tunneling spectroscopy. Tight-binding and first-principles density functional theory calculations within the local density approximation corroborate our experimental observations. Our synthetic design takes advantage of a selective on-surface head-to-tail coupling of monomer building blocks enabling the regioselective synthesis of [3]triangulene-GNRs. Detailed ab initio theory provides insights into the mechanism of on-surface radical polymerization, revealing the pivotal role of Au–C bond formation/breakage in driving selectivity.

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Sprache(n): eng - English
 Datum: 2024-05-012024-02-162024-05-212024-05-302024-06-12
 Publikationsstatus: Erschienen
 Seiten: 8
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: arXiv: 2402.15882
DOI: 10.1021/jacs.4c02386
 Art des Abschluß: -

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Projektname : This work was primarily funded by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division under contract DE-AC02-05-CH11231 (Nanomachine program KC1203) (STS analysis and DFT calculations) and contract DE-SC0023105 (molecular synthesis). Research was also supported by the National Science Foundation under award CHE-2203911 (molecular design) and DMR-2325410 (TB and topological analyses). Part of this research program was generously supported by the Heising-Simons Faculty Fellows Program at UC Berkeley. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under contract DE-AC02-05CH11231. Computational resources were also provided by the NSF TACC Frontera and NSF through ACCESS resources at the NICS (stampede2). J.J.S. and A.R. acknowledge support from the cluster of excellence CUI: Advanced Imaging of Matter EXC 2056 project ID 390715994 of the Deutsche Forschungsgemeinschaft (DFG) and UPV/EHU Grupos Consolidados (IT1453-22). We acknowledge support from the Max Planck-New York City Center for Non-Equilibrium Quantum Phenomena. The Flatiron Institute is a division of the Simons Foundation. M.C.D. acknowledges a National Defense Science and Engineering Graduate Fellowship. The authors thank Dr. Hasan Çelik and the College of Chemistry (CoC) for use of resources at their NMR facility. Instruments in the CoC-NMR facility are supported in part by NIH S10-OD024998.
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Titel: Journal of the American Chemical Society
  Andere : JACS
  Kurztitel : J. Am. Chem. Soc.
Genre der Quelle: Zeitschrift
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Affiliations:
Ort, Verlag, Ausgabe: Washington, DC : American Chemical Society
Seiten: - Band / Heft: 146 (23) Artikelnummer: - Start- / Endseite: 15879 - 15886 Identifikator: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870