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We report temperature-dependent spectroscopy on the layered (n=4)two-dimensional (2D) Ruddlesden-Popper perovskite (BA)(MA)PbI.Helicity-resolved steady-state photoluminescence (PL) reveals no optical degreeof polarization. Time-resolved PL shows a photocarrier lifetime on the order ofnanoseconds. From simultaneaously recorded time-resolved differentialreflectivity (TR$\Delta$R) and time-resolved Kerr ellipticity (TRKE), aphotocarrier lifetime of a few nanoseconds and a spin dephasing time on theorder of picoseconds was found. This stark contrast in lifetimes clearlyexplains the lack of spin polarization in steady-state PL. While we observeclear temperature-dependent effects on the PL dynamics that can be related tostructural dynamics, the spin dephasing is nearly T-independent. Our resultshighlight that spin dephasing in 2D (BA)(MA)PbI occurs at time scales fasterthan the exciton recombination time, which poses a bottleneck for applicationsaimingto utilize this degree of freedom.

Rapid spin depolarization in the layered 2D Ruddlesden Popper perovskite (BA)(MA)PbI