Motional Narrowing Effects in the Excited State Spin Populations of Mn-Doped Hybrid Perovskites

Spin–orbit coupling in the electronic states of solution-processed hybrid metal halide perovskites forms complex spin-textures in the band structures and allows for optical manipulation of the excited state spin-polarizations. Here, we report that motional narrowing acts on the photoexcited spin-polarization in CH3NH3PbBr3 thin films, which are doped at percentage-level with Mn2+ ions. Using ultrafast circularly polarized broadband transient absorption spectroscopy at cryogenic temperatures, we investigate the spin population dynamics in these doped hybrid perovskites and find that spin relaxation lifetimes are increased by a factor of 3 compared to those of undoped materials. Using quantitative analysis of the photoexcitation cooling processes, we reveal increased carrier scattering rates in the doped perovskites as the fundamental mechanism driving spin-polarization-maintaining motional narrowing. Our work reports transition-metal doping as a concept to extend spin lifetimes of hybrid perovskites

Optically Triggered Néel Vector Manipulation of a Metallic Antiferromagnet Mn₂Au under Strain

The absence of stray fields, their insensitivity to external magnetic fields, and ultrafast dynamics make antiferromagnets promising candidates for active elements in spintronic devices. Here, we demonstrate manipulation of the Néel vector in the metallic collinear antiferromagnet Mn2Au by combining strain and femtosecond laser excitation. Applying tensile strain along either of the two in-plane easy axes and locally exciting the sample by a train of femtosecond pulses, we align the Néel vector along the direction controlled by the applied strain. The dependence on the laser fluence and strain suggests the alignment is a result of optically triggered depinning of 90° domain walls and their motion in the direction of the free energy gradient, governed by the magneto-elastic coupling. The resulting, switchable state is stable at room temperature and insensitive to magnetic fields. Such an approach may provide ways to realize robust high-density memory device with switching time scales in the picosecond range