Phase-stabilized 2D/3D hetero-bilayers via lattice matching for efficient and stable inverted solar cells

Ramakrishnan, Shripathi; Chen, Baitao; Zhang, Xiaoyu; Xie, Yi; Tong, Xiao; Xu, Yuanze; Alphenaar, Anna Niamh; Ruthen, Amar; Babatunde, Adewale Joseph; Zhang, Yugang; Cotlet, Mircea; Mitzi, David B.; Yu, Qiuming

doi:10.1016/j.joule.2025.101954

Phase-stabilized 2D/3D hetero-bilayers via lattice matching for efficient and stable inverted solar cells

Journal Article · Fri May 09 00:00:00 EDT 2025 · Joule

DOI:https://doi.org/10.1016/j.joule.2025.101954· OSTI ID:2575407

Ramakrishnan, Shripathi ^[1]; Chen, Baitao ^[1]; Zhang, Xiaoyu ^[1]; Xie, Yi ^[2]; Tong, Xiao ^[3]; Xu, Yuanze ^[1]; Alphenaar, Anna Niamh ^[1]; Ruthen, Amar ^[2]; Babatunde, Adewale Joseph ^[1]; Zhang, Yugang ^[3]; ^[3]; Mitzi, David B. ^[2]; ^[1]

Cornell Univ., Ithaca, NY (United States)
Duke Univ., Durham, NC (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

2D-on-3D (2D/3D) perovskite heterostructures with engineered energy landscapes offer the potential to realize efficient and stable inverted solar cells. However, managing the energy landscape using 2D perovskites with thicker inorganic layers n > 1 necessitates the usage of the chemically unstable methylammonium MA⁺. Here, we synthesized formamidinium (FA)-rich and pure-FA n = 3 Ruddlesden-Popper (RPP) and Dion-Jacobson perovskite (DJP) single crystals by identifying ligands with suitably lattice-matched organic and inorganic components of the 2D lattice. These crystals were translated onto 3D perovskites as capping layers, forming 2D/3D hetero-bilayers (HBs). Degradation studies revealed that HBs with butylammonium-based RPPs as capping layers rapidly phase segregate into non-perovskites under combined extrinsic stressors, compromising the underlying 3D layer, whereas FA-rich DJPs based on 3-aminomethylpiperidine retain their phase stability. The DJP HBs also possess a favorable energy landscape and electron transport at the 2D/3D interface, enabling inverted solar cells with a champion PCE of 25.33% and remarkable stability.

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:: 2575407

Report Number(s):: BNL--228503-2025-JAAM

Journal Information:: Joule, Journal Name: Joule Journal Issue: 6 Vol. 9; ISSN 2542-4351

Publisher:: Elsevier - Cell PressCopyright Statement

Country of Publication:: United States

Language:: English

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