Machine-learning aided first-principles prediction of earth-abundant pnictogen chalcohalide solid solutions for solar-cell devices
Discovering novel families of materials composed of earth-abundant elements and characterized by non-toxicity, high thermodynamic stability, and simple low-temperature synthesis processes, is paramount for the advancement of urgently needed energy storage and conversion technologies. Pnictogen chalc...
| Autores: | , , , , , , , , |
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| Tipo de recurso: | artículo |
| Fecha de publicación: | 2024 |
| País: | España |
| Institución: | Universitat Politècnica de Catalunya (UPC) |
| Repositorio: | UPCommons. Portal del coneixement obert de la UPC |
| Idioma: | inglés |
| OAI Identifier: | oai:upcommons.upc.edu:2117/419915 |
| Acceso en línea: | https://hdl.handle.net/2117/419915 https://dx.doi.org/10.1002/adfm.202406678 |
| Access Level: | acceso abierto |
| Palabra clave: | Àrees temàtiques de la UPC::Física Àrees temàtiques de la UPC::Enginyeria dels materials |
| Sumario: | Discovering novel families of materials composed of earth-abundant elements and characterized by non-toxicity, high thermodynamic stability, and simple low-temperature synthesis processes, is paramount for the advancement of urgently needed energy storage and conversion technologies. Pnictogen chalcohalides, represented by the general formula ABC (A = Bi, Sb; B = S, Se; C = I, Br), emerge as a promising class of energy materials particularly well-suited for photovoltaic applications. However, the compositional landscape of BixSb1 - xSySe1 - yIzBr1 - z is vast and remains largely unexplored, with traditional experimental and theoretical exploration techniques facing limitations in covering the entire solid-solution range due to their labor-intensive and time-consuming nature. Here, an integrated bottom-up approach that combines first-principles calculations, machine learning models, experiments, and device optimizations is introduced to provide a comprehensive fundamental understanding of pnictogen chalcohalides with arbitrary composition and to expedite the design of high-performance multi-junction solar cells. The synergistic investigations unveil a broad and continuous spectrum of bandgaps and optical absorption coefficients ranging from 1.2 to 2.1 eV and from 2.5 · 105 to 6.6 · 105 cm-1, respectively, across a wide variety of thermodynamically stable compounds. Additionally, a tandem BiSBr–BiSeI device is identified as an optimal multi-junction solar cell, exhibiting a maximum short-circuit current density of 18.65 mA cm-2 under intensity-matching conditions. The introduced bottom-up materials design approach may facilitate an unprecedented and rapid translation of basic knowledge into the most demanded solar cell applications. |
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