Highly-Polarized Emission Provided by Giant Optical Orientation of Exciton Spins in Lead Halide Perovskite Crystals.

Quantum technologic and spintronic applications require reliable material platforms that enable significant and long-living spin polarization of excitations, the ability to manipulate it optically in external fields, and the possibility to implement quantum correlations between spins, i.e., entanglement.

Coherent Carrier Spin Dynamics in FAPbBr Perovskite Crystals.

Coherent spin dynamics of electrons and holes are studied in hybrid organic-inorganic lead halide perovskite FAPbBr bulk single crystals using the time-resolved Kerr ellipticity technique at cryogenic temperatures. The Larmor spin precession of the carrier spins in a magnetic field is monitored to measure the Landé -factors of electrons (+2.44) and holes (+0.

Weak Dispersion of Exciton Landé Factor with Band Gap Energy in Lead Halide Perovskites: Approximate Compensation of the Electron and Hole Dependences.

The optical properties of lead halide perovskite semiconductors in vicinity of the bandgap are controlled by excitons, so that investigation of their fundamental properties is of critical importance. The exciton Landé or g-factor g is the key parameter, determining the exciton Zeeman spin splitting in magnetic fields. The exciton, electron, and hole carrier g-factors provide information on the band structure, including its anisotropy, and the parameters contributing to the electron and hole effective masses.

Long-Lived Exciton Coherence in Mixed-Halide Perovskite Crystals.

Compositional engineering of the optical properties of hybrid organic-inorganic lead halide perovskites is crucial for the realization of efficient solar cells and light-emitting devices. We study the effect of band gap fluctuations on coherent exciton dynamics in a mixed FACsPbIBr perovskite crystal by using photon echo spectroscopy. We reveal a narrow homogeneous exciton line width of 16 μeV at a temperature of 1.

Spin-Flip Raman Scattering on Electrons and Holes in Two-Dimensional (PEA) PbI Perovskites.

The class of Ruddlesden-Popper type (PEA) PbI perovskites comprises 2D structures whose optical properties are determined by excitons with a large binding energy of about 260 meV. It complements the family of other 2D semiconductor materials by having the band structure typical for lead halide perovskites, that can be considered as inverted compared to conventional III-V and II-VI semiconductors. Accordingly, novel spin phenomena can be expected for them.

Coherent Spin Dynamics of Electrons in Two-Dimensional (PEA)PbI Perovskites.

The versatile potential of lead halide perovskites and two-dimensional materials is merged in the Ruddlesden-Popper perovskites having outstanding optical properties. Here, the coherent spin dynamics in Ruddlesden-Popper (PEA)PbI perovskites is investigated by picosecond pump-probe Kerr rotation in an external magnetic field. The Larmor spin precession of resident electrons with a spin dephasing time of 190 ps is identified.

Compositional Variation in FAPbSnI and Its Impact on the Electronic Structure: A Combined Density Functional Theory and Experimental Study.

Given their comparatively narrow band gap, mixed Pb-Sn iodide perovskites are interesting candidates for bottom cells in all-perovskite tandems or single junction solar cells, and their luminescence around 900 nm offers great potential for near-infrared optoelectronics. Here, we investigate mixed FAPbSnI offering the first accurate determination of the crystal structure over a temperature range from 293 to 100 K. We demonstrate that all compositions exhibit a cubic structure at room temperature and undergo at least two transitions to lower symmetry tetragonal phases upon cooling.