Site-selective measurement of coupled spin pairs in an organic semiconductor

S. L. Bayliss; L. R. Weiss; A. Mitioglu; K. Galkowski; Z. Yang; K. Yunusova; A. Surrente; K. J. Thorley; J. Behrends; R. Bittl; J. E. Anthony; A. Rao; R. H. Friend; P. Plochocka; P. C.M. Christianen; N. C. Greenham; A. D. Chepelianskii

doi:10.1073/pnas.1718868115

Site-selective measurement of coupled spin pairs in an organic semiconductor

S. L. Bayliss, L. R. Weiss, A. Mitioglu, K. Galkowski, Z. Yang, K. Yunusova, A. Surrente, K. J. Thorley, J. Behrends, R. Bittl, J. E. Anthony, A. Rao, R. H. Friend, P. Plochocka, P. C.M. Christianen, N. C. Greenham, A. D. Chepelianskii

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29 Scopus citations

Abstract

From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed with combined spin and optical sensitivity. We demonstrate this for bound pairs of spin-triplet excitations formed by singlet fission, with direct applicability across a wide range of synthetic and biological systems. We show that the site sensitivity of exchange coupling allows distinct triplet pairs to be resonantly addressed at different magnetic fields, tuning them between optically bright singlet (S = 0) and dark triplet quintet (S = 1, 2) configurations: This induces narrow holes in a broad optical emission spectrum, uncovering exchange-specific luminescence. Using fields up to 60 T, we identify three distinct triplet-pair sites, with exchange couplings varying over an order of magnitude (0.3–5 meV), each with its own luminescence spectrum, coexisting in a single material. Our results reveal how site selectivity can be achieved for organic spin pairs in a broad range of systems.

Original language	English
Pages (from-to)	5077-5082
Number of pages	6
Journal	Proceedings of the National Academy of Sciences of the United States of America
Volume	115
Issue number	20
DOIs	https://doi.org/10.1073/pnas.1718868115
State	Published - May 15 2018

Bibliographical note

Funding Information:
This work was supported by HFML-RU/FOM and LNCMI-CNRS, members of the European Magnetic Field Laboratory (EMFL), and by EPSRC (United Kingdom) via its membership in the EMFL (Grants EP/N01085X/1 and NS/A000060/1) and through Grant EP/M005143/1. L.R.W. acknowledges support from the Gates-Cambridge and Winton Scholarships. We acknowledge support from Labex ANR-10-LABX-0039-PALM, ANR SPINEX, and DFG SPP-1601 (Bi-464/10-2).

Funding Information:
ACKNOWLEDGMENTS. This work was supported by HFML-RU/FOM and LNCMI-CNRS, members of the European Magnetic Field Laboratory (EMFL), and by EPSRC (United Kingdom) via its membership in the EMFL (Grants EP/N01085X/1 and NS/A000060/1) and through Grant EP/M005143/1. L.R.W. acknowledges support from the Gates-Cambridge and Winton Scholarships. We acknowledge support from Labex ANR-10-LABX-0039-PALM, ANR SPINEX, and DFG SPP-1601 (Bi-464/10-2).

Publisher Copyright:
© 2018 National Academy of Sciences. All Rights Reserved.

Keywords

Exchange coupling
Organic semiconductors
Organic spintronics
Singlet fission
Triplet excitons

ASJC Scopus subject areas

General

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10.1073/pnas.1718868115

Cite this

Bayliss, S. L., Weiss, L. R., Mitioglu, A., Galkowski, K., Yang, Z., Yunusova, K., Surrente, A., Thorley, K. J., Behrends, J., Bittl, R., Anthony, J. E., Rao, A., Friend, R. H., Plochocka, P., Christianen, P. C. M., Greenham, N. C., & Chepelianskii, A. D. (2018). Site-selective measurement of coupled spin pairs in an organic semiconductor. Proceedings of the National Academy of Sciences of the United States of America, 115(20), 5077-5082. https://doi.org/10.1073/pnas.1718868115

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title = "Site-selective measurement of coupled spin pairs in an organic semiconductor",

abstract = "From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed with combined spin and optical sensitivity. We demonstrate this for bound pairs of spin-triplet excitations formed by singlet fission, with direct applicability across a wide range of synthetic and biological systems. We show that the site sensitivity of exchange coupling allows distinct triplet pairs to be resonantly addressed at different magnetic fields, tuning them between optically bright singlet (S = 0) and dark triplet quintet (S = 1, 2) configurations: This induces narrow holes in a broad optical emission spectrum, uncovering exchange-specific luminescence. Using fields up to 60 T, we identify three distinct triplet-pair sites, with exchange couplings varying over an order of magnitude (0.3–5 meV), each with its own luminescence spectrum, coexisting in a single material. Our results reveal how site selectivity can be achieved for organic spin pairs in a broad range of systems.",

keywords = "Exchange coupling, Organic semiconductors, Organic spintronics, Singlet fission, Triplet excitons",

author = "Bayliss, {S. L.} and Weiss, {L. R.} and A. Mitioglu and K. Galkowski and Z. Yang and K. Yunusova and A. Surrente and Thorley, {K. J.} and J. Behrends and R. Bittl and Anthony, {J. E.} and A. Rao and Friend, {R. H.} and P. Plochocka and Christianen, {P. C.M.} and Greenham, {N. C.} and Chepelianskii, {A. D.}",

note = "Funding Information: This work was supported by HFML-RU/FOM and LNCMI-CNRS, members of the European Magnetic Field Laboratory (EMFL), and by EPSRC (United Kingdom) via its membership in the EMFL (Grants EP/N01085X/1 and NS/A000060/1) and through Grant EP/M005143/1. L.R.W. acknowledges support from the Gates-Cambridge and Winton Scholarships. We acknowledge support from Labex ANR-10-LABX-0039-PALM, ANR SPINEX, and DFG SPP-1601 (Bi-464/10-2). Funding Information: ACKNOWLEDGMENTS. This work was supported by HFML-RU/FOM and LNCMI-CNRS, members of the European Magnetic Field Laboratory (EMFL), and by EPSRC (United Kingdom) via its membership in the EMFL (Grants EP/N01085X/1 and NS/A000060/1) and through Grant EP/M005143/1. L.R.W. acknowledges support from the Gates-Cambridge and Winton Scholarships. We acknowledge support from Labex ANR-10-LABX-0039-PALM, ANR SPINEX, and DFG SPP-1601 (Bi-464/10-2). Publisher Copyright: {\textcopyright} 2018 National Academy of Sciences. All Rights Reserved.",

year = "2018",

month = may,

day = "15",

doi = "10.1073/pnas.1718868115",

language = "English",

volume = "115",

pages = "5077--5082",

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Bayliss, SL, Weiss, LR, Mitioglu, A, Galkowski, K, Yang, Z, Yunusova, K, Surrente, A, Thorley, KJ, Behrends, J, Bittl, R, Anthony, JE, Rao, A, Friend, RH, Plochocka, P, Christianen, PCM, Greenham, NC & Chepelianskii, AD 2018, 'Site-selective measurement of coupled spin pairs in an organic semiconductor', Proceedings of the National Academy of Sciences of the United States of America, vol. 115, no. 20, pp. 5077-5082. https://doi.org/10.1073/pnas.1718868115

TY - JOUR

T1 - Site-selective measurement of coupled spin pairs in an organic semiconductor

AU - Bayliss, S. L.

AU - Weiss, L. R.

AU - Mitioglu, A.

AU - Galkowski, K.

AU - Yang, Z.

AU - Yunusova, K.

AU - Surrente, A.

AU - Thorley, K. J.

AU - Behrends, J.

AU - Bittl, R.

AU - Anthony, J. E.

AU - Rao, A.

AU - Friend, R. H.

AU - Plochocka, P.

AU - Christianen, P. C.M.

AU - Greenham, N. C.

AU - Chepelianskii, A. D.

N1 - Funding Information: This work was supported by HFML-RU/FOM and LNCMI-CNRS, members of the European Magnetic Field Laboratory (EMFL), and by EPSRC (United Kingdom) via its membership in the EMFL (Grants EP/N01085X/1 and NS/A000060/1) and through Grant EP/M005143/1. L.R.W. acknowledges support from the Gates-Cambridge and Winton Scholarships. We acknowledge support from Labex ANR-10-LABX-0039-PALM, ANR SPINEX, and DFG SPP-1601 (Bi-464/10-2). Funding Information: ACKNOWLEDGMENTS. This work was supported by HFML-RU/FOM and LNCMI-CNRS, members of the European Magnetic Field Laboratory (EMFL), and by EPSRC (United Kingdom) via its membership in the EMFL (Grants EP/N01085X/1 and NS/A000060/1) and through Grant EP/M005143/1. L.R.W. acknowledges support from the Gates-Cambridge and Winton Scholarships. We acknowledge support from Labex ANR-10-LABX-0039-PALM, ANR SPINEX, and DFG SPP-1601 (Bi-464/10-2). Publisher Copyright: © 2018 National Academy of Sciences. All Rights Reserved.

PY - 2018/5/15

Y1 - 2018/5/15

N2 - From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed with combined spin and optical sensitivity. We demonstrate this for bound pairs of spin-triplet excitations formed by singlet fission, with direct applicability across a wide range of synthetic and biological systems. We show that the site sensitivity of exchange coupling allows distinct triplet pairs to be resonantly addressed at different magnetic fields, tuning them between optically bright singlet (S = 0) and dark triplet quintet (S = 1, 2) configurations: This induces narrow holes in a broad optical emission spectrum, uncovering exchange-specific luminescence. Using fields up to 60 T, we identify three distinct triplet-pair sites, with exchange couplings varying over an order of magnitude (0.3–5 meV), each with its own luminescence spectrum, coexisting in a single material. Our results reveal how site selectivity can be achieved for organic spin pairs in a broad range of systems.

AB - From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed with combined spin and optical sensitivity. We demonstrate this for bound pairs of spin-triplet excitations formed by singlet fission, with direct applicability across a wide range of synthetic and biological systems. We show that the site sensitivity of exchange coupling allows distinct triplet pairs to be resonantly addressed at different magnetic fields, tuning them between optically bright singlet (S = 0) and dark triplet quintet (S = 1, 2) configurations: This induces narrow holes in a broad optical emission spectrum, uncovering exchange-specific luminescence. Using fields up to 60 T, we identify three distinct triplet-pair sites, with exchange couplings varying over an order of magnitude (0.3–5 meV), each with its own luminescence spectrum, coexisting in a single material. Our results reveal how site selectivity can be achieved for organic spin pairs in a broad range of systems.

KW - Exchange coupling

KW - Organic semiconductors

KW - Organic spintronics

KW - Singlet fission

KW - Triplet excitons

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Site-selective measurement of coupled spin pairs in an organic semiconductor

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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