Coherent Spin Precession and Lifetime-Limited Spin Dephasing in CsPbBr3 Perovskite Nanocrystals

Carrier spins in semiconductor nanocrystals are promising candidates for quantum information processing. Using a combination of timeresolved Faraday rotation and photoluminescence spectroscopies, we demonstrate optical spin polarization and coherent spin precession in colloidal CsPbBr3 nanocrystals that persists up to room temperature. By suppressing the influence of inhomogeneous hyperfine fields with a small applied magnetic field, we demonstrate inhomogeneous hole transverse spin-dephasing times (T-2*) that approach the nanocrystal photoluminescence lifetime, such that nearly all emitted photons derive from coherent hole spins. Thermally activated LO phonons drive additional spin dephasing at elevated temperatures, but coherent spin precession is still observed at room temperature. These data reveal several major distinctions between spins in nanocrystalline and bulk CsPbBr 3 and open the door for using metal-halide perovskite nanocrystals in spin-based quantum technologies.