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Inverse chirality-induced spin selectivity effect in chiral assemblies of π-conjugated polymers

Nature Materials (2024)Cite this article

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Abstract

Coupling of spin and charge currents to structural chirality in non-magnetic materials, known as chirality-induced spin selectivity, is promising for application in spintronic devices at room temperature. Although the chirality-induced spin selectivity effect has been identified in various chiral materials, its Onsager reciprocal process, the inverse chirality-induced spin selectivity effect, remains unexplored. Here we report the observation of the inverse chirality-induced spin selectivity effect in chiral assemblies of π-conjugated polymers. Using spin-pumping techniques, the inverse chirality-induced spin selectivity effect enables quantification of the magnitude of the longitudinal spin-to-charge conversion driven by chirality-induced spin selectivity in different chiral polymers. By widely tuning conductivities and supramolecular chiral structures via a printing method, we found a very long spin relaxation time of up to several nanoseconds parallel to the chiral axis. Our demonstration of the inverse chirality-induced spin selectivity effect suggests possibilities for elucidating the puzzling interplay between spin and chirality, and opens a route for spintronic applications using printable chiral assemblies.

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Fig. 1: Schematic illustrations of CISS, ICISS and chirality formation in π-conjugated PII2T polymers.
Fig. 2: ISHE and ICISS effects in chiral polymers.
Fig. 3: Hanle effect under oblique magnetic field.
Fig. 4: Interplays of StC conversion coefficient, carrier mobility and spin relaxation time in chiral PII2T polymers.

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All data in the main text or the Supplementary Information is available upon reasonable request. Source data are provided with this paper.

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Acknowledgements

D.S., Y.D., A.H., W.Y., D.B. and P.Z. acknowledge financial support from the Air Force Office of Scientific Research, Multidisciplinary University Research Initiatives (MURI) programme under award number FA9550-23-1-0311. Device fabrication at NC State University was partially supported by the Department of Energy under award number DE-SC0020992 and the National Science Foundation under award DMR-2143642. Y.D. acknowledges financial support from the National Science Foundation under award DMR-1847828 and partial support by the Office of Naval Research under award number N00014-2220-1-2202. W.Y. acknowledges financial support from the Office of Naval Research under award number N00014-20-1-2181. Z.-G.Y. acknowledges financial support by the US Air Force (FA9550-22-P-0014). A.H. acknowledges financial support from the Illinois Materials Research Science and Engineering Center, supported by the National Science Foundation Materials Research Science and Engineering Centers (MRSEC) programme under National Science Foundation award no. DMR-1720633.

Author information

Author notes

  1. These authors contributed equally: R. Sun, K. S. Park.

Authors and Affiliations

  1. Department of Physics and Organic and Carbon Electronics Lab (ORaCEL), North Carolina State University, Raleigh, NC, USA

    Rui Sun, Andrew H. Comstock, Aeron McConnell & Dali Sun

  2. Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana-Champaign, Urbana, IL, USA

    Kyung Sun Park, Yen-Chi Chen & Ying Diao

  3. Department of Chemistry, Duke University, Durham, NC, USA

    Peng Zhang & David Beratan

  4. Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC, USA

    Wei You

  5. Department of Materials Science & Engineering and Materials Research Laboratory, University of Illinois at Urbana-Champaign, Urbana, IL, USA

    Axel Hoffmann

  6. Sivananthan Laboratories, Bolingbrook, Illinois, USA

    Zhi-Gang Yu

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Contributions

D.S., Y.D. and R.S. conceived the experiment and supervised this research. R.S. and K.S.P. were responsible for the spin and electron transport measurements. K.S.P., R.S., A.H.C., A.M. and Y.-C.C. fabricated the samples. Z.-G.Y. provided the theoretical models. R.S., P.Z., D.B., W.Y. and A.H. conducted the spin transport analysis. R.S. and D.S. wrote the paper. All authors contributed to editing the paper.

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Correspondence to Ying Diao or Dali Sun.

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Supplementary Sections I–VII, Figs. 1–25 and Tables I–III.

Source data

Source Data Fig. 1

CD spectra data plotted in Fig. 1d.

Source Data Fig. 2

Spin-pumping response data plotted in Fig. 2b–d.

Source Data Fig. 3

Hanle effect data plotted in Fig. 3a,b.

Source Data Fig. 4

Summary data of StC conversion efficiency plotted in Fig. 4a, and spin relaxation time summary data plotted in Fig. 4b.

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Sun, R., Park, K.S., Comstock, A.H. et al. Inverse chirality-induced spin selectivity effect in chiral assemblies of π-conjugated polymers. Nat. Mater. (2024). https://doi.org/10.1038/s41563-024-01838-8

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