Long-Lived Excited State in a Solubilized Graphene Nanoribbon

Drummer, Matthew C.; Weerasooriya, Ravindra B.; Gupta, Nikita; Phelan, Brian T.; Valentine, Andrew J. S.; Cordones, Amy A.; Li, Xiaosong; Chen, Lin X.; Glusac, Ksenija D.

doi:10.1021/acs.jpcc.1c10024

Title: Long-Lived Excited State in a Solubilized Graphene Nanoribbon

Journal Article · 23 January 2022 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.1c10024 · OSTI ID:1877685

Drummer, Matthew C. ^[1]; Weerasooriya, Ravindra B. ^[1]; Gupta, Nikita ^[1]; Phelan, Brian T. ^[2]; Valentine, Andrew J. S. ^[3];

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Univ. of Illinois, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
Univ. of Washington, Seattle, WA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)

Graphene nanoribbons have excellent light-absorbing properties, but often exhibit short excited-state lifetimes that prevent their applications in photocatalysis. Here, we report a long-lived charge-transfer triplet excited state in a well solubilized, chlorinated graphene nanoribbon (Cl-GNR) with edges modified by bipyrimidine (bpm) moieties. The photophysical behavior of Cl-GNR was observed and characterized by steady-state UV-vis absorption and emission spectroscopy, transient absorption spectroscopy on the ps-ms timescale, and density functional theory (DFT) calculations. In this work, both the Cl-GNR and its monomeric subunit, chlorinated graphene quantum dot (Cl-GQD), were synthesized using bottom-up techniques to produce the H- analogs of the compounds followed by edge-chlorination to achieve soluble products. The absorption spectra of Cl-GQD and Cl-GNR appear in the UV-vis range with lowest-energy peaks at 375 and 600 nm, respectively. The excitons in Cl-GNR were found to exhibit charge-transfer character with the bpm edges serving as electron acceptors. DFT calculations indicate that the excitons are relatively localized, spreading over at most two monomeric units of the GNR. Transient absorption spectroscopy shows that singlet excited states of Cl-GQD and Cl-GNR undergo intersystem crossing with ~300 ps lifetime to form triplet states that last for 15.7 μs (Cl-GQD) and 106 μs (Cl-GNR). These properties, combined with the ability of the bpm sites to coordinate transition metals, make Cl-GNRs promising light-harvesting motifs for photocatalytic applications.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1877685

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 4 Vol. 126; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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