Proceedings of Asia-Pacific International Conference on Perovskite, Organic Photovoltaics and Optoelectronics (IPEROP27)
Publication date: 22nd October 2026
Dimensional reduction in hybrid organic-inorganic perovskite halides (HOIPs), primarily relies on the A-site cation engineering [1]. Here, introduction of bulky organic spacers (A') between inorganic [BX6]4- layers establishes a robust pathway to discover new layered HOIPs given the extensive choice of available organic spacers [2]. On the other hand, molecular anion substitution, such as incorporating pseudohalides like thiocyanate (SCN⁻) into hybrid perovskites, yet unexplored, offers a compelling pathway to alter framework dimensionality and electronic properties. However, single-metal systems such as lead-based MA2PbI2(SCN)2 suffer from severe environmental instability and limited chemical compositional space [3, 4]. In this work, we demonstrate how transitioning to a mixed Ag–Bi double perovskite architecture, MA4AgBiX4(SCN)4 (X = Br, I), overcomes these structural and stability limitations. Ag+ introduces angular flexibility that relaxes lattice strain, enabling the stabilization of both iodide and bromide phases. This B-site cation engineering allows continuous bandgap tuning from 1.95 to 2.30 eV across a complete solid solution while significantly improving ambient stability. Our approach provides a design strategy for expanding the functional diversity of stable pseudohalide hybrid semiconductors.
The authors acknowledge Prof. Satoshi Horike and Prof. Kitagawa for support with the diffuse-reflectance spectrameasurements. This work was supported by Grant-in-Aid for Transformative Research Areas (A) “Supra-ceramics”. TY was sup-ported by Tokyo Tech Challenging Research Award. Bhawna was supported by the Japan Society for the Promotion of Science (JSPS) for the Postdoctoral Fellowships for Research in Japan. The synchrotron radiation experiments were performed at the BL02B1 and BL13XU of SPring-8 with the approval of the Japan Synchrotron Radiation Research Institute (JASRI).
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