Ultrafast Spin Dynamics in Chiral Metal-Halide Perovskites

Materials that combine optoelectronic function with control over the spin degree of freedom are central for emerging quantum technologies, opto-spintronics, and provide exciting avenues for generating polarized light-emission. Hybrid metal-halide perovskites exhibit spin-split Rashba bands and strong spin-orbit coupling, which offer directions for extended spin life-times of excited states and efficient optical spin manipulation. To achieve optimal performance in applications, an understanding how material chirality links to spin state properties and dynamics needs to be established.
In the first part of this talk, we will present our efforts on gaining control over spin properties and dynamics in solution-processable chiral hybrid perovskites through compositional and structural tuning. For this, we tailor the chiral crystal symmetry in novel chiral lead-free bismuth-based materials, highly-emissive low-dimensional chiral lead-halide systems, as well as chiral-achiral heterostructures.
In the second part, we will discuss time- and space-resolved investigations of excited state and spin dynamics in our novel chiral perovskites. We will present results on spin dynamics from ultrafast Faraday Rotation, polarized recombination dynamics, as well as spatio-temporal imaging of excitations using ultrafast transient microscopies.