Rapid Spin Depolarization in the Layered 2D Ruddlesden-Popper Perovskite (BA)(MA)PbI.
Michael Andreas KempfPhilipp MoserMaximilian TomoscheitJulian SchröerJean-Christophe BlanconRico SchwartzSwarup DebAditya MohiteAndreas V StierJonathan J FinleyTobias KornPublished in: ACS nano (2023)
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 degree of polarization. Time-resolved PL shows a photocarrier lifetime on the order of nanoseconds. From simultaneously recorded time-resolved differential reflectivity (TRΔR) and time-resolved Kerr ellipticity (TRKE), a photocarrier lifetime of a few nanoseconds and a spin relaxation time on the order of picoseconds was found. This stark contrast in lifetimes clearly explains the lack of spin polarization in steady-state PL. While we observe clear temperature-dependent effects on the PL dynamics that can be related to structural dynamics, spin relaxation is nearly T -independent. Our results highlight that spin relaxation in 2D (BA)(MA)PbI occurs at time scales faster than the exciton recombination time, which poses a bottleneck for applications aiming to utilize this degree of freedom.
Keyphrases
- single molecule
- room temperature
- transition metal
- density functional theory
- ionic liquid
- perovskite solar cells
- magnetic resonance
- high resolution
- high efficiency
- dna damage
- highly efficient
- molecular dynamics
- reduced graphene oxide
- computed tomography
- oxidative stress
- magnetic resonance imaging
- solar cells
- mass spectrometry