Solvent-Mediated Formation of Quasi-2D Dion-Jacobson Phases on 3D Perovskites for Inverted Solar Cells Over 23% Efficiency

Ramakrishnan, Shripathi; Song, Donghoon; Xu, Yuanze; Zhang, Xiaoyu; Aksoy, Gavin; Cotlet, Mircea; Li, Mingxing; Zhang, Yugang; Yu, Qiuming

doi:10.1002/aenm.202302240

Solvent-Mediated Formation of Quasi-2D Dion-Jacobson Phases on 3D Perovskites for Inverted Solar Cells Over 23% Efficiency

Journal Article · Wed Sep 27 00:00:00 EDT 2023 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202302240· OSTI ID:2372687

Ramakrishnan, Shripathi ^[1]; Song, Donghoon ^[1]; Xu, Yuanze ^[1]; Zhang, Xiaoyu ^[1]; Aksoy, Gavin ^[1]; Cotlet, Mircea ^[2]; Li, Mingxing ^[2]; Zhang, Yugang ^[2]; ^[1]

Cornell Univ., Ithaca, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)

2D-on-3D (2D/3D) perovskite heterostructures present a promising strategy to realize efficient and stable photovoltaics. However, their applicability in inverted solar cells is limited due to the quantum confinement of the 2D-layer and solvent incompatibilities that disrupt the underlying 3D layer, hampering electron transport at the 2D/3D interface. Herein, solvent-dependent formation dynamics and structural evolution of 2D/3D heterostructures are investigated via in situ X-ray scattering. In this study, it is revealed that solvent interaction with the 3D surface determines the formation sequence and spatial distribution of quasi-2D phases with n = 2–4. Isopropanol (IPA) reconstructs the perovskite into a PbI₂-rich surface, forming a strata with smaller n first, followed by a thinner substratum of larger n. In contrast, 2,2,2-Trifluoroethanol (TFE) preserves the 3D surface, promoting the formation of uniformly distributed larger n domains first, and smaller n last. Leveraging these insights, Dion–Jacobson perovskites are used with superior charge transport properties and structural robustness to fabricate 2D/3D heterostructures dominated by n ≥ 3 and engineer a favorable energy landscape for electron tunneling. Inverted solar cells based on 3-Aminomethylpyridine and TFE achieve a champion efficiency of 23.60%, with V_oc and FF of 1.19 V and 84.5%, respectively, and superior stabilities with t₉₄ of 960 h under thermal stress.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2372687

Report Number(s):: BNL--225692-2024-JAAM

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 45 Vol. 13; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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