Understanding Graphene-Perovskite Interactions: From Flake Chemistry to Crystallisation and Solar Cell Performance
Abstract
Graphene-derivatives are widely employed materials to improve bulk and interface properties of metal-halide perovskite devices. Yet the implications of their flake chemistry and interactions with the perovskite precursors remain unclear. Here, we show that pristine graphene flakes (GF) and more conventional graphene oxide flakes (GOF) are not interchangeable. Density functional theory calculations reveal that GOF interacts more strongly with the perovskite lattice but induces larger structural distortions, stronger interfacial polarisation, and localised gap states. In contrast, GF forms comparatively non-disruptive contacts, a response retained across a wide compositional range. Machine-learning atomistic simulations further show that GF contacts both Pb- and I-containing regions of solvated perovskite nanocrystals, with a strong solvent dependency. Solution spectroscopic characterization indicates that GF additives serve as scaffold for preorganised Pb/I-containing precursors, favouring film crystallisation. In this sense, GF enhances solar cell performance across perovskite compositions, but particularly those facing a more challenging crystallisation. In mixed Sn-Pb perovskite solar cells, GF raises the champion power-conversion efficiency from 21.5\% to 23.7\% with improved storage stability. These results establish pristine GF as a chemically defined additive and connect its atomic-scale interactions with precursor organisation, crystallisation, device performance, and stability.
Related
- Defect chemistry engineering of cobalt-free La–Sr–Fe–Ni–O perovskites for high-performance solid oxide cell air electrodes
- Multilayer perovskite air-electrode architectures for enhanced performance in intermediate-temperature solid oxide cells
- The convergent laboratory: when AI reasoning, autonomous experiments, high performance and quantum computing reshape chemistry
- Perovskite Nanocrystal-Based Scintillators: Synthesis Routes, Matrix Engineering, and Performance Optimization for Radiation Detection
- Bidirectional Refractive-Index Programming via Three-Stage Sequential Thiol-Click Chemistry for High-Performance Holographic Recording
BibTeX
@misc{erriyahi2026understanding,
title = {{Understanding Graphene-Perovskite Interactions: From Flake Chemistry to Crystallisation and Solar Cell Performance}},
author = {Oussama Er-Riyahi and Dorota Biernacka and Yating Guo and Mikel Ballarena Tellechea and Silver-Hamill Turren-Cruz and Dario Bercioux and Meng Li and Agnieszka Lekawa-Raus and Jorge Pascual and Karolina Z. Milowska},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.02744},
eprint = {2609.02744},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.02744},
}
RIS
TY - UNPB
TI - Understanding Graphene-Perovskite Interactions: From Flake Chemistry to Crystallisation and Solar Cell Performance
AU - Oussama Er-Riyahi
AU - Dorota Biernacka
AU - Yating Guo
AU - Mikel Ballarena Tellechea
AU - Silver-Hamill Turren-Cruz
AU - Dario Bercioux
AU - Meng Li
AU - Agnieszka Lekawa-Raus
AU - Jorge Pascual
AU - Karolina Z. Milowska
PY - 2026
DA - 2026/09/02
PB - arXiv
DO - 10.48550/arxiv.2609.02744
UR - https://arxiv.org/abs/2609.02744
AB - Graphene-derivatives are widely employed materials to improve bulk and interface properties of metal-halide perovskite devices. Yet the implications of their flake chemistry and interactions with the perovskite precursors remain unclear. Here, we show that pristine graphene flakes (GF) and more conventional graphene oxide flakes (GOF) are not interchangeable. Density functional theory calculations reveal that GOF interacts more strongly with the perovskite lattice but induces larger structural distortions, stronger interfacial polarisation, and localised gap states. In contrast, GF forms comparatively non-disruptive contacts, a response retained across a wide compositional range. Machine-learning atomistic simulations further show that GF contacts both Pb- and I-containing regions of solvated perovskite nanocrystals, with a strong solvent dependency. Solution spectroscopic characterization indicates that GF additives serve as scaffold for preorganised Pb/I-containing precursors, favouring film crystallisation. In this sense, GF enhances solar cell performance across perovskite compositions, but particularly those facing a more challenging crystallisation. In mixed Sn-Pb perovskite solar cells, GF raises the champion power-conversion efficiency from 21.5\% to 23.7\% with improved storage stability. These results establish pristine GF as a chemically defined additive and connect its atomic-scale interactions with precursor organisation, crystallisation, device performance, and stability.
ER -