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

Matthew Beard, Xihan Chen, Haipeng Lu, Paul Ndione, Joseph Berry, Kai Zhu, Yaxin Zhai, Zhen Li, Ye Yang

Research output: Contribution to journalArticlepeer-review

124 Scopus Citations

Abstract

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.

Original languageAmerican English
Pages (from-to)2273-2279
Number of pages7
JournalACS Energy Letters
Volume3
Issue number9
DOIs
StatePublished - 2018

Bibliographical note

Publisher Copyright:
© 2018 American Chemical Society.

NREL Publication Number

  • NREL/JA-5900-71748

Keywords

  • 2D perovskite
  • carrier dynamics
  • spin decoherence

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