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N=8 armchair graphene nanoribbons: solution synthesis and high charge carrier mobility

N=8 armchair graphene nanoribbons: solution synthesis and high charge carrier mobility
N=8 armchair graphene nanoribbons: solution synthesis and high charge carrier mobility

Structurally defined graphene nanoribbons (GNRs) have emerged as promising candidates for nanoelectronic devices. Low band gap (<1 eV) GNRs are particularly important when considering the Schottky barrier in device performance. Here, we demonstrate the first solution synthesis of 8-AGNRs through a carefully designed arylated polynaphthalene precursor. The efficiency of the oxidative cyclodehydrogenation of the tailor-made polymer precursor into 8-AGNRs was validated by FT-IR, Raman, and UV/Vis-near-infrared (NIR) absorption spectroscopy, and further supported by the synthesis of naphtho[1,2,3,4-ghi]perylene derivatives (1 and 2) as subunits of 8-AGNR, with a width of 0.86 nm as suggested by the X-ray single crystal analysis. Low-temperature scanning tunneling microscopy (STM) and solid-state NMR analyses provided further structural support for 8-AGNR. The resulting 8-AGNR exhibited a remarkable NIR absorption extending up to ∼2400 nm, corresponding to an optical band gap as low as ∼0.52 eV. Moreover, optical-pump TeraHertz-probe spectroscopy revealed charge-carrier mobility in the dc limit of ∼270 cm2 V−1 s−1 for the 8-AGNR.

Carbon Materials, Graphene Nanoribbons, High Charge Carrier Mobility, Low Bandgap, Time-Resolved Spectroscopy
1433-7851
Yao, Xuelin
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Zhang, Heng
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Kong, Fanmiao
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Hinaut, Antoine
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Pawlak, Rémy
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Okuno, Masanari
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Graf, Robert
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Horton, Peter N.
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Coles, Simon J.
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Meyer, Ernst
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Bogani, Lapo
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Bonn, Mischa
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Wang, Hai I.
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Müllen, Klaus
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Narita, Akimitsu
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Yao, Xuelin
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Zhang, Heng
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Kong, Fanmiao
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Hinaut, Antoine
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Pawlak, Rémy
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Okuno, Masanari
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Graf, Robert
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Horton, Peter N.
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Coles, Simon J.
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Meyer, Ernst
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Bogani, Lapo
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Bonn, Mischa
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Wang, Hai I.
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Müllen, Klaus
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Narita, Akimitsu
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Yao, Xuelin, Zhang, Heng, Kong, Fanmiao, Hinaut, Antoine, Pawlak, Rémy, Okuno, Masanari, Graf, Robert, Horton, Peter N., Coles, Simon J., Meyer, Ernst, Bogani, Lapo, Bonn, Mischa, Wang, Hai I., Müllen, Klaus and Narita, Akimitsu (2023) N=8 armchair graphene nanoribbons: solution synthesis and high charge carrier mobility. Angewandte Chemie - International Edition, 62 (46), [e202312610]. (doi:10.1002/anie.202312610).

Record type: Article

Abstract

Structurally defined graphene nanoribbons (GNRs) have emerged as promising candidates for nanoelectronic devices. Low band gap (<1 eV) GNRs are particularly important when considering the Schottky barrier in device performance. Here, we demonstrate the first solution synthesis of 8-AGNRs through a carefully designed arylated polynaphthalene precursor. The efficiency of the oxidative cyclodehydrogenation of the tailor-made polymer precursor into 8-AGNRs was validated by FT-IR, Raman, and UV/Vis-near-infrared (NIR) absorption spectroscopy, and further supported by the synthesis of naphtho[1,2,3,4-ghi]perylene derivatives (1 and 2) as subunits of 8-AGNR, with a width of 0.86 nm as suggested by the X-ray single crystal analysis. Low-temperature scanning tunneling microscopy (STM) and solid-state NMR analyses provided further structural support for 8-AGNR. The resulting 8-AGNR exhibited a remarkable NIR absorption extending up to ∼2400 nm, corresponding to an optical band gap as low as ∼0.52 eV. Moreover, optical-pump TeraHertz-probe spectroscopy revealed charge-carrier mobility in the dc limit of ∼270 cm2 V−1 s−1 for the 8-AGNR.

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Angew Chem Int Ed - 2023 - Yao - N 8 Armchair Graphene Nanoribbons Solution Synthesis and High Charge Carrier Mobility - Version of Record
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e-pub ahead of print date: 26 September 2023
Published date: 13 November 2023
Additional Information: Funding Information: This work was financially supported by the Max Planck Society, the FLAG-ERA Grant OPERA by DFG 437130745, and JSPS KAKENHI (Grant Number 21KK0091). X. Yao is grateful for Marie Skłodowska-Curie Research Fellowship (894761-MolecularMAGNET). The authors would like to acknowledge the use of the University of Oxford Advanced Research Computing (ARC) facility. Open Access funding enabled and organized by Projekt DEAL. Funding Information: This work was financially supported by the Max Planck Society, the FLAG‐ERA Grant OPERA by DFG 437130745, and JSPS KAKENHI (Grant Number 21KK0091). X. Yao is grateful for Marie Skłodowska‐Curie Research Fellowship (894761‐MolecularMAGNET). The authors would like to acknowledge the use of the University of Oxford Advanced Research Computing (ARC) facility. Open Access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
Keywords: Carbon Materials, Graphene Nanoribbons, High Charge Carrier Mobility, Low Bandgap, Time-Resolved Spectroscopy

Identifiers

Local EPrints ID: 483741
URI: http://eprints.soton.ac.uk/id/eprint/483741
ISSN: 1433-7851
PURE UUID: 7374492f-b5bb-4c81-9e7d-37cff8919f9b
ORCID for Peter N. Horton: ORCID iD orcid.org/0000-0001-8886-2016
ORCID for Simon J. Coles: ORCID iD orcid.org/0000-0001-8414-9272

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Date deposited: 03 Nov 2023 18:06
Last modified: 06 Jun 2024 01:38

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Contributors

Author: Xuelin Yao
Author: Heng Zhang
Author: Fanmiao Kong
Author: Antoine Hinaut
Author: Rémy Pawlak
Author: Masanari Okuno
Author: Robert Graf
Author: Peter N. Horton ORCID iD
Author: Simon J. Coles ORCID iD
Author: Ernst Meyer
Author: Lapo Bogani
Author: Mischa Bonn
Author: Hai I. Wang
Author: Klaus Müllen
Author: Akimitsu Narita

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