(669e) Extending Spin-Dephasing Lifetimes in Metal-Halide Perovskites By Morphology Engineering | AIChE

(669e) Extending Spin-Dephasing Lifetimes in Metal-Halide Perovskites By Morphology Engineering


Crane, M. - Presenter, University of Washington
Jacoby, L., University of Washington
Gamelin, D., University of Washington
Inorganic metal-halide perovskites have emerged as a promising platform for quantum information and spintronic applications, due to their large spin-orbit coupling, high photoluminescence quantum yields, photostability, and optical spin selection rules. Specifically, CsPbBr3 nanocrystals also exhibit long optical coherence times and short photoluminescence lifetimes, marking metal-halide perovskites as enticing single-photon emitters. For quantum information and spintronic devices, metal-halide perovskites materials also require long inhomogeneous spin-dephasing time (T2*), for reliable initialization, transport, manipulation, and read out spins. Recently, we demonstrated that CsPbBr3 nanocrystals exhibit photoluminescence lifetime-limited hole spin dephasing and we predicted that tuning geometry could significantly extend hole dephasing lifetime to potentially enable this exciting class of materials for spin-based applications.

Here, we use time-resolved Faraday rotation to study the inhomogeneous spin dephasing dynamics in CsPbBr3 thin films for this first time and quantify the impact of morphology. Combining temperature and magnetic field dependent time-resolved Faraday rotation and photoluminescence, we describe a cohesive mechanism for spin dephasing in CsPbBr3. Leveraging these results, we engineer photoluminescence lifetime limited T2* in CsPbBr3 thin films. These measurements initiate metal-halide perovskite nanomaterials for spintronic and quantum-information applications and provide design rules for the future development of inorganic and hybrid metal-halide perovskites