Publication date: 11th March 2026
Self-assembled monolayers (SAMs) have gained significant attention in the photovoltaic device research due to their outstanding performance as hole-transporting layers, particularly in p–i–n device architectures. In this work, we report the design, synthesis and implementation of a new family of SAMs featuring an extended π-conjugated system based on a characteristic [2,3-α]carbazole core. The molecular design strategy focuses on enhancing charge transport and interfacial energetics through controlled conjugation and anchoring geometry.
A systematic investigation of structural symmetry is presented, comparing SAMs incorporating either one or two anchoring groups, in order to elucidate their influence on the layer formation, interfacial properties, and overall device performance. The SAMs employ phosphonic acid anchoring groups, ensuring robust attachment to indium tin oxide (ITO) electrodes and excellent interfacial stability.
As a key outcome of this study, devices incorporating these newly developed SAMs exhibit high power conversion efficiencies above >23% with fill factors reaching up to 85%, positioning them among the most efficient SAM-based hole transport layers reported to date. Comprehensive interfacial characterisation of ITO/SAM and ITO/SAM/perovskite (PVK) layer reveals favourable energy level alignment, efficient hole extraction, and reduced interfacial recombination losses.
Overall, this work demonstrates that rational molecular engineering of indolocarbazole-based SAMs, combined with symmetry and anchoring group optimisation, provides an effective pathway towards high-performance, dopant-free hole transport layers. These findings highlight the strong potential of tailored SAMs for next-generation high-efficiency photovoltaic devices.
Authors are grateful to the financial support received from the European Union (101122283-PEARL), the spanish Ministerio de Ciencia e innovación PID2022-139866NB-I00 and the Severo Ochoa Grant MCIU/AEI/10.13039/501100011033 (CEX2024-001469-S.
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