Impact of Layer Thickness on the Charge Carrier and Spin Coherence Lifetime in Two-Dimensional Layered Perovskite Single Crystals

We report the charge carrier recombination rate and spin coherence lifetimes in single crystals of two-dimensional (2D) Ruddlesden–Popper perovskites PEA2PbI4·(MAPbI3)n−1 (PEA, phenethylammonium; MA, methylammonium; n = 1, 2, 3, 4). Layer thickness-dependent charge carrier recombination rates are observed, with the fastest rates for n = 1 because of the large exciton binding energy, and the slowest rates are observed for n = 2. Room-temperature spin coherence times also show a nonmonotonic layer thickness dependence with an increasing spin coherence lifetime with increasing layer thickness from n = 1 to n = 4, followed by a decrease in lifetime from n = 4 to ∞. The longest coherence lifetime of ∼7 ps is observed in the n = 4 sample. Our results are consistent with two contributions: Rashba splitting increases the spin coherence lifetime going from the n = ∞ to the layered systems, while phonon scattering, which increases for smaller layers, decreases the spin coherence lifetime. The interplay between these two factors contributes to the layer thickness dependence.