Material chemical composition impacts on the band alignments: preliminary results on the 3D/2D perovskite interfaces
Abstract
While hybrid organic-inorganic halide perovskite solar cells have achieved remarkable certified efficiencies, their widespread industrial and societal adoption is hindered by instabilities against light, heat, and moisture. A strategy to mitigate issues, such as moisture sensitivity, involves depositing 2D perovskites on 3D thin films for passivation, but their precise impact on cell performance requires detailed understanding. This work employs atomistic first-principles simulation, based on hybrid functionals, to investigate the structural and electronic properties of 2D/3D interfaces. Specifically, it focuses on interfaces formed by (PEA)2PbI4 (PEA = C6H5CH2CH2NH3, as 2D perovskite) and complex 3D perovskites (Cs0.125MA0.14FA0.735Pb(I0.87Br0.13)3, with MA = CH3NH3 and FA = CH(NH2)2) which are ones of the most used perovskites. The approach is based on optimized hybrid functional methods to consistently determine work function (WF), electron affinity, and band offset (EBO) across different layers. Preliminary results demonstrate that WF are strongly dependent on the cleavage and chemical nature of the surfaces. Furthermore, the creation of interfaces significantly impacts macroscopic potential, with a noticeable slope linked to the polarization of the 3D materials due to ionic substitutions. The band alignment is also highly sensitive to the termination and chemical nature of the perovskites, with valence and conduction EBOs varying from 0.2 to 0.7 eV and of approximately 0.25 eV, respectively. This ongoing work aims to provide a systematic description of these effects, with further investigation into the impact of dimensionality loss on perovskite stability.
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BibTeX
@misc{baranek2026material,
title = {{Material chemical composition impacts on the band alignments: preliminary results on the 3D/2D perovskite interfaces}},
author = {Philippe Baranek},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.21654},
eprint = {2609.21654},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.21654},
}
RIS
TY - UNPB
TI - Material chemical composition impacts on the band alignments: preliminary results on the 3D/2D perovskite interfaces
AU - Philippe Baranek
PY - 2026
DA - 2026/09/21
PB - arXiv
DO - 10.48550/arxiv.2609.21654
UR - https://arxiv.org/abs/2609.21654
AB - While hybrid organic-inorganic halide perovskite solar cells have achieved remarkable certified efficiencies, their widespread industrial and societal adoption is hindered by instabilities against light, heat, and moisture. A strategy to mitigate issues, such as moisture sensitivity, involves depositing 2D perovskites on 3D thin films for passivation, but their precise impact on cell performance requires detailed understanding. This work employs atomistic first-principles simulation, based on hybrid functionals, to investigate the structural and electronic properties of 2D/3D interfaces. Specifically, it focuses on interfaces formed by (PEA)2PbI4 (PEA = C6H5CH2CH2NH3, as 2D perovskite) and complex 3D perovskites (Cs0.125MA0.14FA0.735Pb(I0.87Br0.13)3, with MA = CH3NH3 and FA = CH(NH2)2) which are ones of the most used perovskites. The approach is based on optimized hybrid functional methods to consistently determine work function (WF), electron affinity, and band offset (EBO) across different layers. Preliminary results demonstrate that WF are strongly dependent on the cleavage and chemical nature of the surfaces. Furthermore, the creation of interfaces significantly impacts macroscopic potential, with a noticeable slope linked to the polarization of the 3D materials due to ionic substitutions. The band alignment is also highly sensitive to the termination and chemical nature of the perovskites, with valence and conduction EBOs varying from 0.2 to 0.7 eV and of approximately 0.25 eV, respectively. This ongoing work aims to provide a systematic description of these effects, with further investigation into the impact of dimensionality loss on perovskite stability.
ER -