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This research has received funding from the European Union H2020 Framework Program under through the SENSATE project: low dimensional semiconductors for optically tunable solar harvesters (grant agreement number 866018). Other funding from the Ministry of science and innovation of the Government of Spain under the MATER-ONE (PID2020-116719RB-C41) and MIRACLE projects. I. C. acknowledges UPC and Banco Santander for his FPI-UPC PhD scholarship. M. P. acknowledges the financial support from Ministry of science and innovation within the Ramon y Cajal program (RYC-2017-23758). C. C. acknowledges support from the Spanish Ministry of Science, Innovation and Universities under the fellowship RYC2018-024947-I and grant TED2021-130265B-C22. P. B., C. L. and C. C. thankfully acknowledge the computer resources at MareNostrum and the technical support provided by Barcelona Supercomputing Center (RES-FI-1-0006, RES-FI-2022-2-0003, RES-FI-2023-1-0002 and RES-FI-2023-2-0004). E. S. acknowledges the ICREA Academia program. J. W. T. and R. A. are appreciative of the funding support from the National Science Foundation through grants 1735282-NRT (SFEWS) and 10001536 (INFEWS).

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Novel synthesis of semiconductor chalcohalide anti-perovskites by low-temperature molecular precursor ink deposition methodologies

Publicated to:Journal of Materials Chemistry C. 12 (9): 3154-3163 - 2024-02-01 12(9), DOI: 10.1039/d3tc04410f

Authors: Cano, Ivan; Turnley, Jonathan W; Benitez, Pol; Lopez-Alvarez, Cibran; Asensi, Jose-Miguel; Payno, David; Puigdollers, Joaquim; Placidi, Marcel; Cazorla, Claudio; Agrawal, Rakesh; Saucedo, Edgardo

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Abstract

In recent years, a growing interest in the development of new energy harvesting technologies based on earth-abundant, environmentally-friendly semiconductors, has led to the re-discovery of hitherto overlooked materials. Among them, Ag-based chalcohalides stand out for their abundancy and low-toxicity, as well as the crystal structure analogous to perovskite, albeit with cations in place of anions and vice-versa (i.e. anti-perovskite). Until now, inorganic anti-perovskites have generally been studied as solid-state electrolytes. Indeed, Ag3SI was identified in the 1960s as a superionic conductor. On the other hand, theorical calculations have demonstrated bandgaps in the visible range, suggesting that they could be suitable for PV applications. However, there is little published information on their potential as energy harvesting materials and so far, thin films have been prepared by solid-state reactions or physical vapor deposition techniques at high temperature and/or vacuum conditions, which limits their commercial viability owing to costly, non-scalable processes. In this work, we present a new procedure to synthesize Ag-based chalcohalides by a low-temperature solution-based methodology, using an thiol-amine reactive solvent system to dissolve Ag2S and AgX (X = Br, I) precursors, followed by spin coating deposition to obtain polycrystalline films. Through this process, it has been possible to synthesize Ag3S(IxBr1-x) (x = 0-1) films for the first time, which have been characterized, demonstrating the formation of the anti-perovskite phase and a linear correlation between structural parameters and composition. Optical characterization shows bandgap ranging from 0.9 eV (Ag3SI) to 1.0 eV (Ag3SBr), with a bowing effect for the intermediate solid solutions. First solar cells prototypes demonstrate photo-response and promising electrical characteristics. Ag3SX (X = I, Br) possess a unique anti-perovskite structure (similar to perovskites but switching anions by cations and vice-versa). Here, we propose a new low-cost low-temperature synthesis methodology based on thiol-amine molecular ink deposition.

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