Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells.

Solution-processed perovskite quantum wells have been used to fabricate increasingly efficient and stable optoelectronic devices. Little is known about the dynamics of photogenerated excitons in perovskite quantum wells within the first few hundred femtoseconds - a crucial timescale on which energy and charge transfer processes may compete. Here we use ultrafast transient absorption and two-dimensional electronic spectroscopy to clarify the movement of excitons and charges in reduced-dimensional perovskite solids. We report excitonic funneling from strongly to weakly confined perovskite quantum wells within 150 fs, facilitated by strong spectral overlap and orientational alignment among neighboring wells. This energy transfer happens on timescales orders of magnitude faster than charge transfer, which we find to occur instead over 10 - 100s of picoseconds. Simulations of both Förster-type interwell exciton transfer and free carrier charge transfer are in agreement with these experimental findings, with theoretical exciton transfer calculated to occur in 100s of fs.