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Dependence of Exciton Spin Dynamics on Quantum Confinement Dimensionality in CsPbBr3 Nanocrystals
Evan H Oriel1,2, Kseniia Shcherbak3,4, Ihor Cherniukh3,4
1Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.
Abstract:
Semiconductor nanomaterials offer a promising platform to produce optically addressable spins for use in quantum technologies. Here, we examine CsPbBr3 nanospheres, cubes, and rods spanning the zero-dimensional (0D) to three-dimensional (3D) transition to investigate the influence of dimensionality and shape on exciton spin decoherence. Using circularly polarized transient absorption spectroscopy, we find that the spin relaxation rate is independent of the surface to volume ratio and instead follows a dependence on the length of the shortest dimension. Additionally, differences in surface quality and termination appear to have no effect on the spin relaxation rate for measured materials, and instead the spin relaxation rate is most clearly correlated with the exciton binding energy. Finally, decreasing the dimensionality of the nanomaterials decreases the influence of multiexciton interactions on the spin relaxation rate.
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