Self-Passivation of 2D Ruddlesden–Popper Perovskite by Polytypic Surface PbI 2 Encapsulation

Jung, Hee Joon; Stompus, Constantinos C.; Kanatzidis, Mercouri G.; Dravid, Vinayak P.

doi:10.1021/acs.nanolett.9b02069

Title: Self-Passivation of 2D Ruddlesden–Popper Perovskite by Polytypic Surface PbI ₂ Encapsulation

Journal Article · Mon Aug 19 00:00:00 EDT 2019 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.9b02069· OSTI ID:1577089

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Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Div.

Two-dimensional Ruddlesden–Popper (2D RP) halide perovskites, C₂MA_n–1Pb_nI_3n+1 (C = bulky ammonium cation; MA = methylammonium) with low n-members (n < 5), have been garnering sensational attention for photovoltaic and optoelectronic applications because of the long carrier diffusion lengths, long-term stability, and tunable bandgap. Yet, the surface modification of 2D RP under kinetic particle irradiation, such as light or electron irradiation, is ambiguous, even though it is imperative to elucidate long-stabilized conversion efficiency. Herein, we present molecular-scale observations of dynamic surface reconstruction of BA₂MA₂Pb₃I₁₀ (n = 3) 2D RP induced by the electron beam. The surface dynamics reveal lateral growth of polytypic PbI₂ with 3R, 4H, and 2H structures at the edge and surface of the 2D perovskite, accompanied by simultaneous annihilation at the other edges. Local radiolysis occurs dominantly by the internal energy increase of electron momentum transfer, which triggers a sequential layer-by-layer degradation into PbI₂. Here, in situ observation of the polytypic PbI₂ growth at the whole surface and edges of 2D RP under electron irradiation elucidates how the outer PbI₂ self-passivation can protect inner 2D RP, causing longer operando stability.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); Northwestern University, International Institute for Nanotechnology (IIN); W.M. Keck Foundation; State of Illinois; US Department of the Navy, Office of Naval Research (ONR); Air Force Research Laboratory (AFRL); USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1577089

Journal Information:: Nano Letters, Vol. 19, Issue 9; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Self-Passivation of 2D Ruddlesden–Popper Perovskite by Polytypic Surface PbI 2 Encapsulation

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Title: Self-Passivation of 2D Ruddlesden–Popper Perovskite by Polytypic Surface PbI ₂ Encapsulation