4.8 Article

Long carrier diffusion length in two-dimensional lead halide perovskite single crystals

Journal

CHEM
Volume 8, Issue 4, Pages 1107-1120

Publisher

CELL PRESS
DOI: 10.1016/j.chempr.2022.01.008

Keywords

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Funding

  1. Laboratory Directed Research Directions program office (LDRD) at Los Alamos National Laboratory (LANL)
  2. J. Robert Oppenheimer (JRO) Distinguished Postdoc Fellowship at LANL
  3. National Science Foundation DMR Program [DMR-1905990, 89233218CNA000001]
  4. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DEAC02-06CH11357]
  5. Ministry of Science and Technology, Taiwan [MOST 108-2113-M-002-015-MY3, 108-2911-I-002-561]
  6. Academia Sinica, Taiwan [AS-iMATE-109-31]
  7. Center of Atomic Initiative for New Materials, National Taiwan University

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In this work, the authors investigated the carrier diffusion length in two-dimensional Ruddlesden-Popper perovskite single crystals using scanning photocurrent microscopy. They observed a long in-plane carrier diffusion length and attributed it to the dominating dissociated free carrier transport. The results suggest that semiconducting devices fabricated from RP perovskite single crystals can be as efficient as their 3D counterparts.
Ruddlesden-Popper (RP) perovskites are two-dimensional semiconductors for high-performance optoelectronic devices. In this work, we report a long in-plane carrier diffusion length in 2D RP perovskite single crystals probed by scanning photocurrent microscopy. Carrier diffusion lengths of 7-14 mm are observed when the number of PbI6-2 octahedra between organic spacers increases from 1 to 3. Using detailed light intensity and electric-field-dependent photo current measurements, we attribute the observed long diffusion length to the dominating dissociated free carrier transport. This is further validated by time-resolved photoluminescence measurements, where the decay lifetime increases in the presence of an electric field. From our experiments, we conclude that the in-plane transport in RP perovskites is efficient because of the partial free carrier generation, which overcomes strong excitonic effects. Our results suggest that semiconducting devices fabricated from RP perovskite single crystals can be as efficient as their 3D counterparts.

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