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Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites

Author

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  • Timo Neumann

    (University of Cambridge
    Walter Schottky Institut and Physik Department, Technische Universität München)

  • Sascha Feldmann

    (University of Cambridge)

  • Philipp Moser

    (Walter Schottky Institut and Physik Department, Technische Universität München)

  • Alex Delhomme

    (Université Grenoble Alpes, INSA Toulouse, Univ. Toulouse Paul Sabatier, EMFL, CNRS, LNCMI)

  • Jonathan Zerhoch

    (Walter Schottky Institut and Physik Department, Technische Universität München)

  • Tim van de Goor

    (University of Cambridge)

  • Shuli Wang

    (Laboratoire National des Champs Magnétiques Intenses, UPR 3228, CNRS-UGA-UPS-INSA)

  • Mateusz Dyksik

    (Laboratoire National des Champs Magnétiques Intenses, UPR 3228, CNRS-UGA-UPS-INSA
    Wroclaw University of Science and Technology)

  • Thomas Winkler

    (University of Cambridge)

  • Jonathan J. Finley

    (Walter Schottky Institut and Physik Department, Technische Universität München)

  • Paulina Plochocka

    (Laboratoire National des Champs Magnétiques Intenses, UPR 3228, CNRS-UGA-UPS-INSA
    Wroclaw University of Science and Technology)

  • Martin S. Brandt

    (Walter Schottky Institut and Physik Department, Technische Universität München)

  • Clément Faugeras

    (Université Grenoble Alpes, INSA Toulouse, Univ. Toulouse Paul Sabatier, EMFL, CNRS, LNCMI)

  • Andreas V. Stier

    (Walter Schottky Institut and Physik Department, Technische Universität München)

  • Felix Deschler

    (Walter Schottky Institut and Physik Department, Technische Universität München)

Abstract

Materials combining semiconductor functionalities with spin control are desired for the advancement of quantum technologies. Here, we study the magneto-optical properties of novel paramagnetic Ruddlesden-Popper hybrid perovskites Mn:(PEA)2PbI4 (PEA = phenethylammonium) and report magnetically brightened excitonic luminescence with strong circular polarization from the interaction with isolated Mn2+ ions. Using a combination of superconducting quantum interference device (SQUID) magnetometry, magneto-absorption and transient optical spectroscopy, we find that a dark exciton population is brightened by state mixing with the bright excitons in the presence of a magnetic field. Unexpectedly, the circular polarization of the dark exciton luminescence follows the Brillouin-shaped magnetization with a saturation polarization of 13% at 4 K and 6 T. From high-field transient magneto-luminescence we attribute our observations to spin-dependent exciton dynamics at early times after excitation, with first indications for a Mn-mediated spin-flip process. Our findings demonstrate manganese doping as a powerful approach to control excitonic spin physics in Ruddlesden-Popper perovskites, which will stimulate research on this highly tuneable material platform with promise for tailored interactions between magnetic moments and excitonic states.

Suggested Citation

  • Timo Neumann & Sascha Feldmann & Philipp Moser & Alex Delhomme & Jonathan Zerhoch & Tim van de Goor & Shuli Wang & Mateusz Dyksik & Thomas Winkler & Jonathan J. Finley & Paulina Plochocka & Martin S. , 2021. "Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-23602-1
    DOI: 10.1038/s41467-021-23602-1
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    Cited by:

    1. Madeleine Laitz & Alexander E. K. Kaplan & Jude Deschamps & Ulugbek Barotov & Andrew H. Proppe & Inés García-Benito & Anna Osherov & Giulia Grancini & Dane W. deQuilettes & Keith A. Nelson & Moungi G., 2023. "Uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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