journal article·2025-07Open access

The Role of Fluorine‐Functionalized Organic Spacers for Defect Passivation and Low‐Dimensional Phase Formation in 3D MAPI Perovskite Solar Cells

Ali Semerci, Javier Urieta‐Mora, Sander Driessen, Ali Buyruk, Rik Hooijer, Agustín Molina‐Ontoria, Bülent Alkan, Seckin Akin, Mattia Fanetti, Harishankar Balakrishnan, Achim Hartschuh, Shuxia Tao, Nazario Martín, Peter Müller‐Buschbaum, Saim Emin, Tayebeh Ameri

Advanced Functional Materials· Volume 35· Issue 27

Abstract

Abstract Widespread application of organic‐inorganic halide perovskites (OIHP) still faces a major obstacle in mitigating moisture‐induced degradation. Integrating organic spacers, as defect passivation facilitators along with low‐dimensional phase (LDP) formation is an effective approach to enhance the efficiency and robustness of 3D methyl ammonium lead iodide (MAPI) in photovoltaics (PV). Here, the formamidinium cation (FA+) employing 3,5‐difluorobenzene‐1‐carboximidamidium iodide (2F), 4‐(trifluoromethyl)benzene‐1‐carboximidamidium iodide (3F), and 2,3,4,5,6‐pentafluorobenzene‐1‐carboximidamidium iodide (5F) organic spacers as passivation layer in 3D/LDP OIHP solar cells is utilized. Fluorine atom position and quantity in organic spacers change the optoelectronic characteristics of the perovskites, enhancing hydrophobicity, facilitating LDP formation, and augmenting dipole moments, thereby facilitating charge separation processes. PV performance analysis reveals that 3F‐treated 3D/LDP devices achieve the highest efficiency of 19.22%. Experimental results and density functional theory (DFT) studies attribute the higher performance of 3F‐modified devices to effective LDP formation, enhanced passivation of defect states at perovskite surfaces and grain boundaries, the highest dipole moment and lowest band gap among the evaluated spacers. The stability tests show that, after 1000 h, 3F‐ and 5F‐modified 3D/LDP OIHP devices retain over 85% of their initial efficiency. This research opens novel avenues for designing appropriate organic spacers to attenuate defects in 3D/LDP PV devices.
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Research context

OpenAlex topics: Perovskite Materials and Applications · Conducting polymers and applications · Chalcogenide Semiconductor Thin Films

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

Affiliations

Department of Chemistry and Center for NanoScience (CeNS) Ludwig‐Maximilians‐Universität München Butenandtstrasse 5–13 (E) 81377 Munich Germany

Faculty of Science, Department of Energy Science and Technologies Türk‐Alman University 2nd Floor Şahinkaya Street No:94, Beykoz İstanbul 34820 Turkey

IMDEA‐Nanociencia, C/ Faraday, 9 Campus de Cantoblanco Madrid 28049 Spain

Department of Organic Chemistry, Faculty of Chemistry Complutense University of Madrid Avenida Complutense s/n Madrid 28040 Spain

Materials Simulation and Modelling, Department of Applied Physics Eindhoven University of Technology Eindhoven 5600 MB The Netherlands

Department of Metallurgical and Materials Engineering Hitit University Corum 19030 Turkey

Department of Metallurgical and Materials Engineering Necmettin Erbakan University Konya 42090 Turkey

Materials Research Laboratory University of Nova Gorica Vipavska 13c Ajdovščina 5270 Slovenia

TUM School of Natural Sciences, Department of Physics Chair for Functional Materials Technical University of Munich James‐Franck‐Str. 1 85748 Garching Germany

Chair for Composite Materials, Department of Materials Science Faculty of Engineering Christian‐Albrechts‐Universität zu Kiel Kaiserstrasse 2 24143 Kiel Germany

Kiel Nano, Surface and Interface Science KiNSIS Kiel University Christian‐Albrechts‐Platz 4 D‐24118 Kiel Germany

Funding

Deutsche Forschungsgemeinschaft · Javna Agencija za Raziskovalno Dejavnost RS · Comunidad de Madrid

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