An emissive charge-transfer excited-state at the well-defined hetero-nanostructure interface of an organic conjugated molecule and two-dimensional inorganic nanosheet.

Autor: Umeyama T; Department of Applied Chemistry, Graduate School of Engineering, University of Hyogo Himeji Hyogo 671-2280 Japan umeyama@eng.u-hyogo.ac.jp., Mizutani D; Department of Molecular Engineering, Graduate School of Engineering, Kyoto University Kyoto 615-8510 Japan higashi@moleng.kyoto-u.ac.jp imahori@scl.kyoto-u.ac.jp., Ikeda Y; Department of Molecular Engineering, Graduate School of Engineering, Kyoto University Kyoto 615-8510 Japan higashi@moleng.kyoto-u.ac.jp imahori@scl.kyoto-u.ac.jp., Osterloh WR; Department of Molecular Engineering, Graduate School of Engineering, Kyoto University Kyoto 615-8510 Japan higashi@moleng.kyoto-u.ac.jp imahori@scl.kyoto-u.ac.jp., Yamamoto F; Department of Applied Chemistry, Graduate School of Engineering, University of Hyogo Himeji Hyogo 671-2280 Japan umeyama@eng.u-hyogo.ac.jp., Kato K; Graduate School of Natural Science and Technology, Okayama University Okayama 700-8530 Japan yamakata@okayama-u.ac.jp., Yamakata A; Graduate School of Natural Science and Technology, Okayama University Okayama 700-8530 Japan yamakata@okayama-u.ac.jp., Higashi M; Department of Molecular Engineering, Graduate School of Engineering, Kyoto University Kyoto 615-8510 Japan higashi@moleng.kyoto-u.ac.jp imahori@scl.kyoto-u.ac.jp., Urakami T; Department of Molecular Engineering, Graduate School of Engineering, Kyoto University Kyoto 615-8510 Japan higashi@moleng.kyoto-u.ac.jp imahori@scl.kyoto-u.ac.jp., Sato H; Department of Molecular Engineering, Graduate School of Engineering, Kyoto University Kyoto 615-8510 Japan higashi@moleng.kyoto-u.ac.jp imahori@scl.kyoto-u.ac.jp., Imahori H; Department of Molecular Engineering, Graduate School of Engineering, Kyoto University Kyoto 615-8510 Japan higashi@moleng.kyoto-u.ac.jp imahori@scl.kyoto-u.ac.jp.; Institute for Integrated Cell-Material Sciences (WPI-iCeMS), Kyoto University Kyoto 606-8501 Japan.; Institute for Liberal Arts and Sciences (ILAS), Kyoto University Kyoto 606-8501 Japan.
Jazyk: angličtina
Zdroj: Chemical science [Chem Sci] 2023 Oct 17; Vol. 14 (42), pp. 11914-11923. Date of Electronic Publication: 2023 Oct 17 (Print Publication: 2023).
DOI: 10.1039/d3sc03604a
Abstrakt: Precise engineering of excited-state interactions between an organic conjugated molecule and a two-dimensional semiconducting inorganic nanosheet, specifically the manipulation of charge-transfer excited (CTE) states, still remains a challenge for state-of-the-art photochemistry. Herein, we report a long-lived, highly emissive CTE state at structurally well-defined hetero-nanostructure interfaces of photoactive pyrene and two-dimensional MoS 2 nanosheets via an N -benzylsuccinimide bridge (Py-Bn-MoS 2 ). Spectroscopic measurements reveal that no charge-transfer state is formed in the ground state, but the locally-excited (LE) state of pyrene in Py-Bn-MoS 2 efficiently generates an unusual emissive CTE state. Theoretical studies elucidate the interaction of MoS 2 vacant orbitals with the pyrene LE state to form a CTE state that shows a distinct solvent dependence of the emission energy. This is the first example of organic-inorganic 2D hetero-nanostructures displaying mixed luminescence properties by an accurate design of the bridge structure, and therefore represents an important step in their applications for energy conversion and optoelectronic devices and sensors.
Competing Interests: There are no conflicts to declare.
(This journal is © The Royal Society of Chemistry.)
Databáze: MEDLINE
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