Multi-cation perovskites prevent carrier reflection from grain surfaces

Saidaminov, Makhsud I.; Williams, Kristopher; Wei, Mingyang; Johnston, Andrew; Quintero-Bermudez, Rafael; Vafaie, Maral; Pina, Joao M.; Proppe, Andrew H.; Hou, Yi; Walters, Grant; Kelley, Shana O.; Tisdale, William A.; Sargent, Edward H.

doi:10.1038/s41563-019-0602-2

Multi-cation perovskites prevent carrier reflection from grain surfaces

Journal Article · Mon Feb 10 00:00:00 EST 2020 · Nature Materials

DOI:https://doi.org/10.1038/s41563-019-0602-2· OSTI ID:1803715

^[1]; Williams, Kristopher ^[2]; ^[3]; ^[3]; Quintero-Bermudez, Rafael ^[3]; Vafaie, Maral ^[3]; ^[3]; ^[3]; ^[3]; Walters, Grant ^[3]; ^[3]; ^[2]; ^[3]

Univ. of Victoria, BC (Canada); Univ. of Toronto, ON (Canada); OSTI
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Univ. of Toronto, ON (Canada)

The composition of perovskite has been optimized combinatorially such that it often contains six components (A_xB_yC_1-x-yPbX_zY_3-z) in state-of-art perovskite solar cells. Questions remain regarding the precise role of each component, and the lack of a mechanistic explanation limits the practical exploration of the large and growing chemical space. Here, aided by transient photoluminescence microscopy, we find that, in perovskite single crystals, carrier diffusivity is in fact independent of composition. In polycrystalline thin films, the different compositions play a crucial role in carrier diffusion. In this work, we report that methylammonium (MA)-based films show a high carrier diffusivity of 0.047 cm² s^-1, while MA-free mixed caesium-formamidinium (CsFA) films exhibit an order of magnitude lower diffusivity. Elemental composition studies show that CsFA grains display a graded composition. This curtails electron diffusion in these films, as seen in both vertical carrier transport and surface potential studies. Incorporation of MA leads to a uniform grain core-to-edge composition, giving rise to a diffusivity of 0.034 cm² s^-1 in CsMAFA films. A model that invokes competing crystallization processes allows us to account for this finding, and suggests further strategies to achieve homogeneous crystallization for the benefit of perovskite optoelectronics.

View Accepted Manuscript (DOE)

Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019345

OSTI ID:: 1803715

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 4 Vol. 19; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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