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.

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.

Universal magnetic proximity effect in ferromagnet-semiconductor quantum well hybrid structures.

Hybrid ferromagnet-semiconductor systems possess new outstanding properties, which emerge when bringing magnetic and semiconductor materials into contact. In such structures, the long-range magnetic proximity effect couples the spin systems of the ferromagnet and semiconductor on distances exceeding the carrier wave function overlap. The effect is due to the effective p-d exchange interaction of acceptor-bound holes in the quantum well with d-electrons of the ferromagnet.

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.

Optical Orientation of Excitons in a Longitudinal Magnetic Field in Indirect-Band-Gap (In,Al)As/AlAs Quantum Dots with Type-I Band Alignment.

Exciton recombination and spin dynamics in (In,Al)As/AlAs quantum dots (QDs) with indirect band gap and type-I band alignment were studied. The negligible (less than 0.2 μeV) value of the anisotropic exchange interaction in these QDs prevents the mixing of the excitonic basis states and makes the formation of spin-polarized bright excitons possible under quasi-resonant, circularly polarized excitation.

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.

The Landé factors of electrons and holes in lead halide perovskites: universal dependence on the band gap.

The Landé or g-factors of charge carriers are decisive for the spin-dependent phenomena in solids and provide also information about the underlying electronic band structure. We present a comprehensive set of experimental data for values and anisotropies of the electron and hole Landé factors in hybrid organic-inorganic (MAPbI, MAPb(BrCl), MAPb(BrCl), FAPbBr, FACsPbIBr, MA=methylammonium and FA=formamidinium) and all-inorganic (CsPbBr) lead halide perovskites, determined by pump-probe Kerr rotation and spin-flip Raman scattering in magnetic fields up to 10 T at cryogenic temperatures. Further, we use first-principles density functional theory (DFT) calculations in combination with tight-binding and k ⋅ p approaches to calculate microscopically the Landé factors.

Lead-Dominated Hyperfine Interaction Impacting the Carrier Spin Dynamics in Halide Perovskites.

The outstanding optical quality of lead halide perovskites inspires studies of their potential for the optical control of carrier spins as pursued in other materials. Entering largely uncharted territory, time-resolved pump-probe Kerr rotation is used to explore the coherent spin dynamics of electrons and holes in bulk formamidinium caesium lead iodine bromide (FA Cs PbI Br ) and to determine key parameters characterizing interactions of their spins, such as the g-factors and relaxation times. The demonstrated long spin dynamics and narrow g-factor distribution prove the perovskites as promising competitors for conventional semiconductors in spintronics.

Magneto-Optics of Excitons Interacting with Magnetic Ions in CdSe/CdMnS Colloidal Nanoplatelets.

Excitons in diluted magnetic semiconductors represent excellent probes for studying the magnetic properties of these materials. Various magneto-optical effects, which depend sensitively on the exchange interaction of the excitons with the localized spins of the magnetic ions can be used for probing. Here, we study core/shell CdSe/(Cd,Mn)S colloidal nanoplatelets hosting diluted magnetic semiconductor layers.

Single and Double Electron Spin-Flip Raman Scattering in CdSe Colloidal Nanoplatelets.

CdSe colloidal nanoplatelets are studied by spin-flip Raman scattering in magnetic fields up to 5 T. We find pronounced Raman lines shifted from the excitation laser energy by an electron Zeeman splitting. Their polarization selection rules correspond to those expected for scattering mediated by excitons interacting with resident electrons.

Low voltage control of exchange coupling in a ferromagnet-semiconductor quantum well hybrid structure.

Voltage control of ferromagnetism on the nanometer scale is highly appealing for the development of novel electronic devices with low power consumption, high operation speed, reliable reversibility and compatibility with semiconductor technology. Hybrid structures based on the assembly of ferromagnetic and semiconducting building blocks are expected to show magnetic order as a ferromagnet and to be electrically tunable as a semiconductor. Here, we demonstrate the electrical control of the exchange coupling in a hybrid consisting of a ferromagnetic Co layer and a semiconductor CdTe quantum well, separated by a thin non-magnetic (Cd,Mg)Te barrier.