Single-molecule electroluminescence and photoluminescence of polyfluorene unveils the photophysics behind the green emission band

Yoshihiro Honmou; Shuzo Hirata; Hideaki Komiyama; Junya Hiyoshi; Susumu Kawauchi; Tomokazu Iyoda; Martin Vacha

doi:10.1038/ncomms5666

Single-molecule electroluminescence and photoluminescence of polyfluorene unveils the photophysics behind the green emission band

Yoshihiro Honmou, Shuzo Hirata, Hideaki Komiyama, Junya Hiyoshi, Susumu Kawauchi, Tomokazu Iyoda, Martin Vacha

Research output: Contribution to journal › Article › peer-review

64 Scopus citations

Abstract

Optoelectronic properties of polyfluorene, a blue light-emitting organic semiconductor, are often degraded by the presence of green emission that originates mainly from oxidation of the polymer. Here, we use single-molecule electroluminescence (EL) and photoluminescence (PL) spectroscopy on polyfluorene chains confined in vertical cylinders of a phase-separated block copolymer to spectrally resolve the green band and investigate in detail the photophysical processes responsible for its appearance. In both EL and PL, a substantial fraction of polyfluorene chains shows spectrally stable green emission which is ascribed to a keto defect. In addition, in EL, we observe a new type of vibrationally resolved spectra distributed over a wide range of frequencies and showing strong spectral dynamics. Based on quantum chemical calculations, this type is proposed to originate from charge-assisted formation and stabilization of ground-state aggregates. The results are expected to have broad implications in the fields of photophysics and material design of polyfluorene materials. © 2014 Macmillan Publishers Limited. All rights reserved.

Original language	English (US)
Journal	NATURE COMMUNICATIONS
Volume	5
Issue number	1
DOIs	https://doi.org/10.1038/ncomms5666
State	Published - 2014
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2021-10-07
Acknowledgements: Ban Xuan Dong and Dr Satoshi Habuchi (currently at KAUST, Saudi Arabia) were present during the early stages of the research and their contributions as well as discussions are gratefully acknowledged. Dr Shingo Hadano is acknowledged for invaluable assistance in the synthesis of the BC and polyfluorene. Tatsuya Ishii and Shoki Matsuda helped with the analysis of the single-molecule PL spectra. The work was supported by Grants-in-Aid for Scientific Research No. 23651107 and 26287097 of the Japan Society for the Promotion of Science. The numerical calculations were carried out on the TSUBAME 2.0 supercomputer in the Tokyo Institute of Technology, Tokyo, Japan and on the supercomputer in the Research Center for Computational Science, Okazaki, Japan.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

ASJC Scopus subject areas

General Biochemistry, Genetics and Molecular Biology
General Chemistry
General Physics and Astronomy

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10.1038/ncomms5666

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title = "Single-molecule electroluminescence and photoluminescence of polyfluorene unveils the photophysics behind the green emission band",

abstract = "Optoelectronic properties of polyfluorene, a blue light-emitting organic semiconductor, are often degraded by the presence of green emission that originates mainly from oxidation of the polymer. Here, we use single-molecule electroluminescence (EL) and photoluminescence (PL) spectroscopy on polyfluorene chains confined in vertical cylinders of a phase-separated block copolymer to spectrally resolve the green band and investigate in detail the photophysical processes responsible for its appearance. In both EL and PL, a substantial fraction of polyfluorene chains shows spectrally stable green emission which is ascribed to a keto defect. In addition, in EL, we observe a new type of vibrationally resolved spectra distributed over a wide range of frequencies and showing strong spectral dynamics. Based on quantum chemical calculations, this type is proposed to originate from charge-assisted formation and stabilization of ground-state aggregates. The results are expected to have broad implications in the fields of photophysics and material design of polyfluorene materials. {\textcopyright} 2014 Macmillan Publishers Limited. All rights reserved.",

author = "Yoshihiro Honmou and Shuzo Hirata and Hideaki Komiyama and Junya Hiyoshi and Susumu Kawauchi and Tomokazu Iyoda and Martin Vacha",

note = "KAUST Repository Item: Exported on 2021-10-07 Acknowledgements: Ban Xuan Dong and Dr Satoshi Habuchi (currently at KAUST, Saudi Arabia) were present during the early stages of the research and their contributions as well as discussions are gratefully acknowledged. Dr Shingo Hadano is acknowledged for invaluable assistance in the synthesis of the BC and polyfluorene. Tatsuya Ishii and Shoki Matsuda helped with the analysis of the single-molecule PL spectra. The work was supported by Grants-in-Aid for Scientific Research No. 23651107 and 26287097 of the Japan Society for the Promotion of Science. The numerical calculations were carried out on the TSUBAME 2.0 supercomputer in the Tokyo Institute of Technology, Tokyo, Japan and on the supercomputer in the Research Center for Computational Science, Okazaki, Japan. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

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AU - Honmou, Yoshihiro

AU - Hirata, Shuzo

AU - Komiyama, Hideaki

AU - Hiyoshi, Junya

AU - Kawauchi, Susumu

AU - Iyoda, Tomokazu

AU - Vacha, Martin

N1 - KAUST Repository Item: Exported on 2021-10-07 Acknowledgements: Ban Xuan Dong and Dr Satoshi Habuchi (currently at KAUST, Saudi Arabia) were present during the early stages of the research and their contributions as well as discussions are gratefully acknowledged. Dr Shingo Hadano is acknowledged for invaluable assistance in the synthesis of the BC and polyfluorene. Tatsuya Ishii and Shoki Matsuda helped with the analysis of the single-molecule PL spectra. The work was supported by Grants-in-Aid for Scientific Research No. 23651107 and 26287097 of the Japan Society for the Promotion of Science. The numerical calculations were carried out on the TSUBAME 2.0 supercomputer in the Tokyo Institute of Technology, Tokyo, Japan and on the supercomputer in the Research Center for Computational Science, Okazaki, Japan. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2014

Y1 - 2014

N2 - Optoelectronic properties of polyfluorene, a blue light-emitting organic semiconductor, are often degraded by the presence of green emission that originates mainly from oxidation of the polymer. Here, we use single-molecule electroluminescence (EL) and photoluminescence (PL) spectroscopy on polyfluorene chains confined in vertical cylinders of a phase-separated block copolymer to spectrally resolve the green band and investigate in detail the photophysical processes responsible for its appearance. In both EL and PL, a substantial fraction of polyfluorene chains shows spectrally stable green emission which is ascribed to a keto defect. In addition, in EL, we observe a new type of vibrationally resolved spectra distributed over a wide range of frequencies and showing strong spectral dynamics. Based on quantum chemical calculations, this type is proposed to originate from charge-assisted formation and stabilization of ground-state aggregates. The results are expected to have broad implications in the fields of photophysics and material design of polyfluorene materials. © 2014 Macmillan Publishers Limited. All rights reserved.

AB - Optoelectronic properties of polyfluorene, a blue light-emitting organic semiconductor, are often degraded by the presence of green emission that originates mainly from oxidation of the polymer. Here, we use single-molecule electroluminescence (EL) and photoluminescence (PL) spectroscopy on polyfluorene chains confined in vertical cylinders of a phase-separated block copolymer to spectrally resolve the green band and investigate in detail the photophysical processes responsible for its appearance. In both EL and PL, a substantial fraction of polyfluorene chains shows spectrally stable green emission which is ascribed to a keto defect. In addition, in EL, we observe a new type of vibrationally resolved spectra distributed over a wide range of frequencies and showing strong spectral dynamics. Based on quantum chemical calculations, this type is proposed to originate from charge-assisted formation and stabilization of ground-state aggregates. The results are expected to have broad implications in the fields of photophysics and material design of polyfluorene materials. © 2014 Macmillan Publishers Limited. All rights reserved.

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Single-molecule electroluminescence and photoluminescence of polyfluorene unveils the photophysics behind the green emission band

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