Electronic Structure of Isolated Graphene Nanoribbons in Solution Revealed by Two-Dimensional Electronic Spectroscopy
Structurally well-defined graphene nanoribbons (GNRs) are nanostructures with unique optoelectronic properties. In the liquid phase, strong aggregation typically hampers the assessment of their intrinsic properties. Recently we reported a novel type of GNRs, decorated with aliphatic side chains, yie...
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| Published in | Nano Letters Vol. 24; no. 3; pp. 797 - 804 |
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| Main Authors | , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
24.01.2024
American Chemical Society (ACS) |
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| Online Access | Get full text |
| ISSN | 1530-6984 1530-6992 1530-6992 |
| DOI | 10.1021/acs.nanolett.3c02665 |
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| Abstract | Structurally well-defined graphene nanoribbons (GNRs) are nanostructures with unique optoelectronic properties. In the liquid phase, strong aggregation typically hampers the assessment of their intrinsic properties. Recently we reported a novel type of GNRs, decorated with aliphatic side chains, yielding dispersions consisting mostly of isolated GNRs. Here we employ two-dimensional electronic spectroscopy to unravel the optical properties of isolated GNRs and disentangle the transitions underlying their broad and rather featureless absorption band. We observe that vibronic coupling, typically neglected in modeling, plays a dominant role in the optical properties of GNRs. Moreover, a strong environmental effect is revealed by a large inhomogeneous broadening of the electronic transitions. Finally, we also show that the photoexcited bright state decays, on the 150 fs time scale, to a dark state which is in thermal equilibrium with the bright state, that remains responsible for the emission on nanosecond time scales. |
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| AbstractList | Structurally well-defined graphene nanoribbons (GNRs) are nanostructures with unique optoelectronic properties. In the liquid phase, strong aggregation typically hampers the assessment of their intrinsic properties. Recently we reported a novel type of GNRs, decorated with aliphatic side chains, yielding dispersions consisting mostly of isolated GNRs. Here we employ two-dimensional electronic spectroscopy to unravel the optical properties of isolated GNRs and disentangle the transitions underlying their broad and rather featureless absorption band. We observe that vibronic coupling, typically neglected in modeling, plays a dominant role in the optical properties of GNRs. Moreover, a strong environmental effect is revealed by a large inhomogeneous broadening of the electronic transitions. Finally, we also show that the photoexcited bright state decays, on the 150 fs time scale, to a dark state which is in thermal equilibrium with the bright state, that remains responsible for the emission on nanosecond time scales. Structurally well-defined graphene nanoribbons (GNRs) are nanostructures with unique optoelectronic properties. In the liquid phase, strong aggregation typically hampers the assessment of their intrinsic properties. Recently we reported a novel type of GNRs, decorated with aliphatic side chains, yielding dispersions consisting mostly of isolated GNRs. Here we employ two-dimensional electronic spectroscopy to unravel the optical properties of isolated GNRs and disentangle the transitions underlying their broad and rather featureless absorption band. We observe that vibronic coupling, typically neglected in modeling, plays a dominant role in the optical properties of GNRs. Moreover, a strong environmental effect is revealed by a large inhomogeneous broadening of the electronic transitions. Finally, we also show that the photoexcited bright state decays, on the 150 fs time scale, to a dark state which is in thermal equilibrium with the bright state, that remains responsible for the emission on nanosecond time scales.Structurally well-defined graphene nanoribbons (GNRs) are nanostructures with unique optoelectronic properties. In the liquid phase, strong aggregation typically hampers the assessment of their intrinsic properties. Recently we reported a novel type of GNRs, decorated with aliphatic side chains, yielding dispersions consisting mostly of isolated GNRs. Here we employ two-dimensional electronic spectroscopy to unravel the optical properties of isolated GNRs and disentangle the transitions underlying their broad and rather featureless absorption band. We observe that vibronic coupling, typically neglected in modeling, plays a dominant role in the optical properties of GNRs. Moreover, a strong environmental effect is revealed by a large inhomogeneous broadening of the electronic transitions. Finally, we also show that the photoexcited bright state decays, on the 150 fs time scale, to a dark state which is in thermal equilibrium with the bright state, that remains responsible for the emission on nanosecond time scales. |
| Author | Polli, Dario Mai, Yiyong Feng, Xinliang Cerullo, Giulio Heisler, Ismael A. Ganzer, Lucia Camargo, Franco V. A. Müllen, Klaus Russo, Mattia de la Cruz Valbuena, Gabriel D’Andrea, Cosimo Xu, Fugui Perri, Antonio Zhang, Pengfei Nagahara, Tetsuhiko |
| AuthorAffiliation | IFN-CNR School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules Max Planck Institute for Polymer Research Department of Chemistry and Materials Technology Dipartimento di Fisica Departamento de Física Department of Chemistry and Food Chemistry Universidade Federal do Paraná |
| AuthorAffiliation_xml | – name: Universidade Federal do Paraná – name: Dipartimento di Fisica – name: Department of Chemistry and Food Chemistry – name: Department of Chemistry and Materials Technology – name: Max Planck Institute for Polymer Research – name: IFN-CNR – name: Departamento de Física – name: School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules |
| Author_xml | – sequence: 1 givenname: Tetsuhiko orcidid: 0000-0003-1405-5515 surname: Nagahara fullname: Nagahara, Tetsuhiko organization: Department of Chemistry and Materials Technology – sequence: 2 givenname: Franco V. A. surname: Camargo fullname: Camargo, Franco V. A. organization: IFN-CNR – sequence: 3 givenname: Fugui orcidid: 0000-0003-2652-0656 surname: Xu fullname: Xu, Fugui email: xufg1227@sjtu.edu.cn organization: School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules – sequence: 4 givenname: Lucia surname: Ganzer fullname: Ganzer, Lucia organization: Dipartimento di Fisica – sequence: 5 givenname: Mattia surname: Russo fullname: Russo, Mattia organization: Dipartimento di Fisica – sequence: 6 givenname: Pengfei orcidid: 0000-0001-7559-7348 surname: Zhang fullname: Zhang, Pengfei organization: School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules – sequence: 7 givenname: Antonio surname: Perri fullname: Perri, Antonio organization: Dipartimento di Fisica – sequence: 8 givenname: Gabriel surname: de la Cruz Valbuena fullname: de la Cruz Valbuena, Gabriel organization: Dipartimento di Fisica – sequence: 9 givenname: Ismael A. orcidid: 0000-0002-8581-4745 surname: Heisler fullname: Heisler, Ismael A. organization: Universidade Federal do Paraná – sequence: 10 givenname: Cosimo surname: D’Andrea fullname: D’Andrea, Cosimo organization: Dipartimento di Fisica – sequence: 11 givenname: Dario orcidid: 0000-0002-6960-5708 surname: Polli fullname: Polli, Dario organization: Dipartimento di Fisica – sequence: 12 givenname: Klaus orcidid: 0000-0001-6630-8786 surname: Müllen fullname: Müllen, Klaus organization: Max Planck Institute for Polymer Research – sequence: 13 givenname: Xinliang orcidid: 0000-0003-3885-2703 surname: Feng fullname: Feng, Xinliang organization: Department of Chemistry and Food Chemistry – sequence: 14 givenname: Yiyong orcidid: 0000-0002-6373-2597 surname: Mai fullname: Mai, Yiyong organization: School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules – sequence: 15 givenname: Giulio orcidid: 0000-0002-9534-2702 surname: Cerullo fullname: Cerullo, Giulio email: giulio.cerullo@polimi.it organization: IFN-CNR |
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| Title | Electronic Structure of Isolated Graphene Nanoribbons in Solution Revealed by Two-Dimensional Electronic Spectroscopy |
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