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

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. Brandt, Clément Faugeras, Andreas V. Stier and Felix Deschler ()
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Timo Neumann: University of Cambridge
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
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
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

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-23602-1

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