Publication date: 3rd June 2020
Using circularly-polarised 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. We observe a dynamic circular dichroism that arises from a photoinduced polarization in the exciton distribution between total angular momentum states. Our findings provide fundamental, insights into the spin-dependent exciton-exciton interactions in layered hybrid perovskites. In this poster, we demonstrate how a J-polarisation within two-dimensional perovskites gives rise to contrasting optical transitions. We relate these transitions to opposing shifts in the absorption spectra and show that they scale with the exciton to free carrier ratio, as set by the binding energy of the material. Further, we use ultrafast circularly polarised time-resolved photoluminescence measurements to demonstrate early time circularly polarised photoluminescence. Finally, we propose that the presented data originates from J-dependent exciton-exciton interactions.
S.A.B acknowledges the support from the EPSRC Centre for Doctoral Training in Graphene Technology (EP/L016087/1). R.S. and R.H.F. acknowledge support from EPSRC project ‘Strategic University Network to Revolutionise Indian Solar Energy-SUNRISE (EP/P032591/1)’. R.S. acknowledges the Royal Society Newton-Bhabha International Fellowship. TWJ acknowledges support from the EPSRC Cambridge NanoDTC, EP/L015978/1. S.G. and G.C. acknowledge the Marie Curie actions (project H2020‐ MSCA‐IF‐ 2018841356). F.D acknowledges a Winton Advanced Research Fellowship and funding from the DFG Emmy Noether Program.
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