Mode locking of hole spin coherences in CsPb(Cl, Br)<sub>3</sub> perovskite nanocrystals.

Kirstein, E; Kopteva, N E; Yakovlev, D R; Zhukov, E A; Kolobkova, E V; Kuznetsova, M S; Belykh, V V; Yugova, I A et al. · Nat Commun · 2023

basic_science · Level V

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Abstract

The spin physics of perovskite nanocrystals with confined electrons or holes is attracting increasing attention, both for fundamental studies and spintronic applications. Here, stable [Formula: see text] lead halide perovskite nanocrystals embedded in a fluorophosphate glass matrix are studied by time-resolved optical spectroscopy to unravel the coherent spin dynamics of holes and their interaction with nuclear spins of the <sup>207</sup>Pb isotope. We demonstrate the spin mode locking effect provided by the synchronization of the Larmor precession of single hole spins in each nanocrystal in the ensemble that are excited periodically by a laser in an external magnetic field. The mode locking is enhanced by nuclei-induced frequency focusing. An ensemble spin dephasing time [Formula: see text] of a nanosecond and a single hole spin coherence time of T<sub>2</sub> = 13 ns are measured. The developed theoretical model accounting for the mode locking and nuclear focusing for randomly oriented nanocrystals with perovskite band structure describes the experimental data very well.