Hyperfine interaction of electrons confined in CsPbI$_3$ nanocrystals with nuclear spin fluctuations

TL;DR

This study investigates the hyperfine interactions affecting electron spin dynamics in CsPbI$_3$ nanocrystals, revealing nuclear spin fluctuation effects and quantifying hyperfine constants through experimental and theoretical analysis.

Contribution

It provides the first detailed analysis of hyperfine interactions in CsPbI$_3$ nanocrystals, identifying the contributions of lead and iodine orbitals to electron spin splitting.

Findings

Electron Landé g-factor of 2.07 in nanocrystals.

Finite zero-field Larmor precession frequency of 0.8 μeV.

Hyperfine interaction mainly from iodine atoms.

Abstract

The coherent spin dynamics of electrons are investigated for CsPbI$_3$ perovskite nanocrystals in a glass matrix using time-resolved Faraday ellipticity. In nanocrystals with a diameter of about 11 nm, the Larmor precession frequency has a linear dependence on magnetic field corresponding to the electron Land\'e $g$-factor of 2.07. We find a finite Larmor precession frequency at zero magnetic field, corresponding to the electron spin splitting of $0.8$ $\mu$eV. This splitting is explained by the hyperfine interaction with nuclear spin fluctuations. Our model analysis shows that the hyperfine interaction for the conduction band electrons is contributed both by the $p$-orbitals of the lead atoms and by the $s$-orbitals of the iodine atoms, with the leading contribution to the hyperfine field fluctuations coming from iodine. This fact agrees well with the 9% iodine contribution to the Bloch amplitude of the conduction band, obtained by DFT calculations. From these findings, the atomic hyperfine constant for the $5s$-orbital of iodine is evaluated as 190 $\mu$eV.