The spin physics of perovskite nanocrystals with confined electrons or holes is attracting increasing attention, both for fundamental studies and spintronic applications. Here, stable $${{{{{{{\rm{CsPb}}}}}}}}{({{{{{{{{\rm{Cl}}}}}}}}}_{0.56}{{{{{{{{\rm{Br}}}}}}}}}_{0.44})}_{3}$$ 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 207Pb 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 $${T}_{2}^{ * }$$ of a nanosecond and a single hole spin coherence time of T2 = 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.
1 September 2016 in Superlattices and Microstructures
Lead halide perovskite nanocrystals (NCs) in a glass matrix combine excellent optical properties and stability against environment. The spectral and temporal characteristics of photoluminescence from and CsPb(Cl,Br) nanocrystals in a fluorophosphate glass matrix are measured in a temperature range from 6 to 270 K in order to reveal factors that determine their quantum yield and recombination dynamics. At low temperatures, the recombination dynamics is characterized by three decay components with timescales on the order of 1 ns, 10 ns, and 1 . The relative contributions of the corresponding processes and their characteristic times are strongly temperature dependent. The emission intensity decreases with growing temperature. This effect is stronger in smaller NCs, which highlights the role of surface states. These experimental results are discussed on the basis of a model taking into account the NC energy structure and the presence of electron and hole surface trap states. The photoluminescence dynamics at low temperatures is dominated by charge-carrier radiative recombination and relaxation to shallow traps. At temperatures exceeding 100 K, the dynamics is affected by carrier activation to the excited states.
The photoluminescence polarizations of (In,Ga)As/GaAs quantum dots annealed at different temperatures are studied as a function of external magnetic field (Hanle curves). In these dependencies, remarkable resonant features appear due to all-optical nuclear magnetic resonances (NMR) for optical excitation with modulated circular polarization. Application of an additional radio-frequency field synchronously with the polarization modulation strongly modifies the NMR features. The resonances can be related to transitions between different nuclear spin states split by the strain-induced gradient of the crystal field and by the externally applied magnetic field. A theoretical model is developed to simulate quadrupole and Zeeman splittings of the nuclear spins in a strained quantum dot. Comparison with the experiment allows us to uniquely identify the observed resonances. The large broadening of the NMR resonances is attributed to variations of the quadrupole splitting within the quantum dot volume, which is well described by the model.