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How Exciton Interactions Control Spin-Depolarization in Layered Hybrid Perovskites
Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, United Kingdom.ORCID iD: 0000-0002-7808-0931
Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, United Kingdom.ORCID iD: 0000-0002-0915-6066
IFN-CNR, Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci, 32, 20133, Milano, Italy.
IFN-CNR, Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci, 32, 20133, Milano, Italy.ORCID iD: 0000-0002-3323-1724
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2020 (English)In: Nano Letters, ISSN 1530-6984, E-ISSN 1530-6992, Vol. 20, no 8, p. 5678-5685Article in journal (Refereed) Published
Abstract [en]

Using circularly polarized broadband transient absorption, time-resolved circular photoluminescence, and transient Faraday rotation spectroscopy, we report that spin-dependent interactions have a significant impact on exciton energies and spin depolarization times in layered Ruddlesden–Popper hybrid metal-halide perovskites. In BA2FAPb2I7, we report that room-temperature spin lifetimes are largest (3.2 ps) at a carrier density of ∼1017 cm–3 with increasing depolarization rates at higher exciton densities. This indicates that many-body interactions reduce spin-lifetimes and outcompete the effect of D’yakonov-Perel precessional relaxation that has been previously reported at lower carrier densities. We further observe a dynamic circular dichroism that arises from a photoinduced polarization in the exciton distribution between total angular momentum states. Our findings provide fundamental and application relevant insights into the spin-dependent exciton–exciton interactions in layered hybrid perovskites.

Place, publisher, year, edition, pages
2020. Vol. 20, no 8, p. 5678-5685
National Category
Physical Sciences
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URN: urn:nbn:se:liu:diva-210915DOI: 10.1021/acs.nanolett.0c00867ISI: 000562935200013Scopus ID: 2-s2.0-85089610602OAI: oai:DiVA.org:liu-210915DiVA, id: diva2:1927060
Funder
German Research Foundation (DFG)Available from: 2025-01-14 Created: 2025-01-14 Last updated: 2025-03-14Bibliographically approved

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Gillett, Alexander

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Bourelle, Sean A.Shivanna, RavichandranGhosh, SoumenGillett, AlexanderSenanayak, Satyaprasad P.Feldmann, SaschaCerullo, GiulioFriend, Richard H.Deschler, Felix
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