Generating a Stable Higher-Symmetry CsPbI₃ Perovskite Phase in Ambient Conditions: Unveiling the Stabilization Mechanism

Rafikul Ali Saha; Athina Papadopoulou; Rocío Ariza; Giedrius Degutis; Irina Skvortsova; Tom Braeckevelt; Francesco De Angelis; Eduardo Solano; João Pedro de Sousa Gouveia dos Anjos; Maria Isabel Pintor Monroy; Ilya Mongilyov; Bart Goderis; Juan Rubio-Zuazo; Jan Genoe; Carlo Meneghini; Julian A. Steele; Sara Bals; Veronique Van Speybroeck; Johan Hofkens; Maarten B. J. Roeffaers

doi:10.1021/acsnano.5c07700

journal article·2025-08-12Open access

Generating a Stable Higher-Symmetry CsPbI₃ Perovskite Phase in Ambient Conditions: Unveiling the Stabilization Mechanism

Rafikul Ali Saha, Athina Papadopoulou, Rocío Ariza, Giedrius Degutis, Irina Skvortsova, Tom Braeckevelt, Francesco De Angelis, Eduardo Solano, João Pedro de Sousa Gouveia dos Anjos, Maria Isabel Pintor Monroy, Ilya Mongilyov, Bart Goderis, Juan Rubio-Zuazo, Jan Genoe, Carlo Meneghini, Julian A. Steele, Sara Bals, Veronique Van Speybroeck, Johan Hofkens, Maarten B. J. Roeffaers

ACS Nano· Volume 19· Issue 31

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Abstract

Black-phase cesium lead iodide (CsPbI 3 ) is a promising candidate for high-efficiency perovskite optoelectronics, but its instability under ambient conditions remains a major challenge. Among several strategies, dimethylammonium iodide (DMAI) has emerged as a potential stabilizer; however, inconsistencies in phase stability (3–7 days) and lower solar power conversion efficiencies (∼20 vs ∼27% for hybrid perovskites) highlight the need for further improvements. This study not only demonstrates enhanced stabilization of the high-symmetry black phase of CsPbI 3 and improved film morphology through optimized composition and annealing conditions but also more importantly provides detailed mechanistic insights obtained from comprehensive experimental and theoretical analyses. Systematic tuning of the DMAI concentration (1.2 M), annealing temperature (200 °C, 1 min), and Cs + substitution (12–15%) significantly extends phase stability to 7 days under ambient conditions (35–52% relative humidity) and maintains stability even after 16 months in a drybox environment by reducing orthorhombic strain and octahedral tilting. Additionally, a minor (∼5%) zero-dimensional (0D) Cs 4 PbI 6 phase fills pinholes, enhancing the film quality. Optimized photodiodes exhibit a low dark current (∼1 μA/cm 2 ), high external quantum efficiency (∼80% at −2 V), and a ≥100 dB linear dynamic range. These findings provide mechanistic insights into the stabilization of the black phase of CsPbI 3, advancing the development of more stable and efficient perovskite-based optoelectronic devices.

Source: openalex_inverted_index · Quality: baseline

Research context

Electronic materials Materials processing

OpenAlex topics: Perovskite Materials and Applications · Solid-state spectroscopy and crystallography · Thermal Expansion and Ionic Conductivity

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

cMACS, Department of Microbial and Molecular Systems, KU Leuven, Celestijnenlaan 200F, 3001 Heverlee, Belgium

imec, Kapeldreef 75, 3001 Leuven, Belgium

Department of Electrical Engineering (ESAT), KU Leuven, Kasteelpark Arenberg 10, 3001 Leuven, Belgium

Electron Microscopy for Materials Science (EMAT) and NANOlab Center of Excellence

University of Antwerp

Center for Molecular Modeling (CMM), Ghent University, Technologiepark 46, 9052 Zwijnaarde, Belgium

Department of Chemistry, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium

Department of Science, Roma Tre University, via Della Vasca Navale 84, 00146 Rome, Italy

NCD-SWEET Beamline, ALBA Synchrotron Light Source

i3N/CENIMAT, Department of Materials Science, Faculty of Science and Technology, Universidade NOVA de Lisboa and CEMOP/UNINOVA, Campus de Caparica, 2829-516 Caparica, Portugal

Polymer Chemistry and Materials, Department of Chemistry, KU Leuven, Celestijnenlaan 200F, 3001 Heverlee, Belgium

BM25-SpLine Beamline at the ESRF, 71 Avenue des Martyrs, Grenoble 38043, France

Instituto de Ciencia de Materiales de Madrid-CSIC, Sor Juana Inés de la Cruz, 3, Cantoblanco, 28049 Madrid, Spain

Australian Institute for Bioengineering and Nanotechnology (AIBN)

The University of Queensland

School of Mathematics and Physics

Department of Molecular Spectroscopy

Max Planck Institute for Polymer Research

Funding

KU Leuven · H2020 Marie Sklodowska-Curie Actions · Universiteit Gent · Fonds Wetenschappelijk Onderzoek

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