Electronic-morphological decoupling in mixed-dimensional halide perovskite heterostructures
Abstract
Surface morphology is widely considered an indicator of thin-film quality, with smoother films generally expected to exhibit more uniform optoelectronic properties. Here, we demonstrate that substantial surface evolution does not necessarily lead to increased electronic heterogeneity in mixed-dimensional perovskite heterostructures. We investigate how low-dimensional Ruddlesden-Popper capping layers derived from the sterically hindered 5-tert-butyl-phenanthridinium cation affect the spatial distributions of photoluminescence (PL) characteristics and quasi-Fermi level splitting (QFLS) in 3D perovskites. By combining statistical atomic force microscopy (AFM) analysis with confocal, spatially resolved PL spectroscopy, we correlate surface topography with microscale optoelectronic properties. Although capping increases surface roughness and height asymmetry, it does not increase electronic inhomogeneity. Instead, the heterostructures exhibit enhanced PL, reduced non-radiative recombination, and improved spatial uniformity of radiative QFLS compared with pristine 3D films. Under accelerated aging, this contrast becomes more pronounced: pristine films develop substantial spatial fluctuations in emission and QFLS, whereas capped heterostructures largely preserve their optoelectronic homogeneity. These findings indicate that the low-dimensional capping layer suppresses aging-induced optoelectronic disorder, demonstrating that electronic uniformity can be maintained despite morphological irregularity. This decoupling provides a design principle for developing durable, high-performance perovskite photovoltaics.
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BibTeX
@misc{samadpour2026electronicmorphological,
title = {{Electronic-morphological decoupling in mixed-dimensional halide perovskite heterostructures}},
author = {Mahmoud Samadpour and Alireza Fathi Beiraghvandi and Kazem Meraji and Tristan Sachsenweger Ballantyne and Fuxiang Ji and Mahdi Mohammadi and Nasim Kabir and Wolfgang Tress},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.37964},
eprint = {2610.37964},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.37964},
}
RIS
TY - UNPB
TI - Electronic-morphological decoupling in mixed-dimensional halide perovskite heterostructures
AU - Mahmoud Samadpour
AU - Alireza Fathi Beiraghvandi
AU - Kazem Meraji
AU - Tristan Sachsenweger Ballantyne
AU - Fuxiang Ji
AU - Mahdi Mohammadi
AU - Nasim Kabir
AU - Wolfgang Tress
PY - 2026
DA - 2026/10/27
PB - arXiv
DO - 10.48550/arxiv.2610.37964
UR - https://arxiv.org/abs/2610.37964
AB - Surface morphology is widely considered an indicator of thin-film quality, with smoother films generally expected to exhibit more uniform optoelectronic properties. Here, we demonstrate that substantial surface evolution does not necessarily lead to increased electronic heterogeneity in mixed-dimensional perovskite heterostructures. We investigate how low-dimensional Ruddlesden-Popper capping layers derived from the sterically hindered 5-tert-butyl-phenanthridinium cation affect the spatial distributions of photoluminescence (PL) characteristics and quasi-Fermi level splitting (QFLS) in 3D perovskites. By combining statistical atomic force microscopy (AFM) analysis with confocal, spatially resolved PL spectroscopy, we correlate surface topography with microscale optoelectronic properties. Although capping increases surface roughness and height asymmetry, it does not increase electronic inhomogeneity. Instead, the heterostructures exhibit enhanced PL, reduced non-radiative recombination, and improved spatial uniformity of radiative QFLS compared with pristine 3D films. Under accelerated aging, this contrast becomes more pronounced: pristine films develop substantial spatial fluctuations in emission and QFLS, whereas capped heterostructures largely preserve their optoelectronic homogeneity. These findings indicate that the low-dimensional capping layer suppresses aging-induced optoelectronic disorder, demonstrating that electronic uniformity can be maintained despite morphological irregularity. This decoupling provides a design principle for developing durable, high-performance perovskite photovoltaics.
ER -