Highly-Polarized Emission Provided by Giant Optical Orientation of Exciton Spins in Lead Halide Perovskite Crystals.

Autor: Kopteva NE; Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany., Yakovlev DR; Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany., Yalcin E; Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany., Akimov IA; Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany., Nestoklon MO; Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany., Glazov MM; Ioffe Institute, Russian Academy of Sciences, St. Petersburg, 194021, Russia., Kotur M; Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany., Kudlacik D; Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany., Zhukov EA; Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany., Kirstein E; Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany., Hordiichuk O; Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Zürich, CH-8093, Switzerland.; Laboratory for Thin Films and Photovoltaics, Empa-Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, CH-8600, Switzerland., Dirin DN; Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Zürich, CH-8093, Switzerland.; Laboratory for Thin Films and Photovoltaics, Empa-Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, CH-8600, Switzerland., Kovalenko MV; Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Zürich, CH-8093, Switzerland.; Laboratory for Thin Films and Photovoltaics, Empa-Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, CH-8600, Switzerland., Bayer M; Experimentelle Physik 2, Technische Universität Dortmund, 44227, Dortmund, Germany.
Jazyk: angličtina
Zdroj: Advanced science (Weinheim, Baden-Wurttemberg, Germany) [Adv Sci (Weinh)] 2024 Aug; Vol. 11 (31), pp. e2403691. Date of Electronic Publication: 2024 Jun 17.
DOI: 10.1002/advs.202403691
Abstrakt: Quantum technologic and spintronic applications require reliable material platforms that enable significant and long-living spin polarization of excitations, the ability to manipulate it optically in external fields, and the possibility to implement quantum correlations between spins, i.e., entanglement. Here it is demonstrated that these conditions are met in bulk crystals of lead halide perovskites. A giant optical orientation of 85% of excitons, approaching the ultimate limit of unity, in FA 0.9 Cs 0.1 PbI 2.8 Br 0.2 crystals is reported. The exciton spin orientation is maintained during the exciton lifetime of 55 ps resulting in high circular polarization of the exciton emission. The optical orientation is robust to detuning of the excitation energy up to 0.3 eV above the exciton resonance and remains larger than 20% up to detunings of 0.9 eV. It evidences pure chiral selection rules and suppressed spin relaxation of electrons and holes, even with large kinetic energies. The exciton and electron-hole recombinations are distinguished by means of the spin dynamics detected via coherent spin quantum beats in magnetic field. Further, electron-hole spin correlations are demonstrated through linear polarization beats after circularly polarized excitation. These findings are supported by atomistic calculations. All-in-all, the results establish lead halide perovskite semiconductors as suitable platform for quantum technologies.
(© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)
Databáze: MEDLINE
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