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However, their widespread application remains hindered by challenges such as anisotropic crystal growth, composition control and lack of knowledge on optoelectronic properties. A deeper understanding of the intrinsic limitations of these materials, as well as viable defect mitigation strategies like the engineering of solid solutions, is critical. This work presents a low\u2010temperature synthesis route based on molecular ink deposition enabling direct crystallization of tunable Bi(S\n                    <jats:sub>z<\/jats:sub>\n                    Se\n                    <jats:sub>1\u2010z<\/jats:sub>\n                    )(I\n                    <jats:sub>x<\/jats:sub>\n                    Br\n                    <jats:sub>1\u2010x<\/jats:sub>\n                    ) solid solutions without need for binary chalcogenide precursors. This approach yields phase\u2010pure films with precise control over morphology, composition, and crystallographic orientation. XRD analysis and DFT calculations confirm the formation of homogeneous solid solutions, while optoelectronic measurements reveal the distinct roles of halogen and chalcogen anions in tuning bandgap energy and carrier type, with Se shifting downwards the conduction band. The versatility of this synthesis technique enables morphology control ranging from compact films to rod\u2010shaped microcrystals, expanding the functional adaptability of these materials. These findings offer a foundational framework for defect engineering and the scalable integration of chalcohalides in next\u2010generation energy technologies, including photovoltaics, photocatalysis, thermoelectrics, and chemical sensing.\n                  <\/jats:p>","DOI":"10.1002\/smtd.202501723","type":"journal-article","created":{"date-parts":[[2025,11,10]],"date-time":"2025-11-10T08:31:33Z","timestamp":1762763493000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Molecular Ink\u2010Based Synthesis of Bi(S\n                    <sub>z<\/sub>\n                    Se\n                    <sub>1\u2010z<\/sub>\n                    )(I\n                    <sub>x<\/sub>\n                    Br\n                    <sub>1\u2010x<\/sub>\n                    ) Solid Solutions as Tuneable Materials for Sustainable Energy Applications"],"prefix":"10.1002","volume":"9","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3867-8987","authenticated-orcid":false,"given":"D.","family":"Rovira","sequence":"first","affiliation":[{"name":"Photovoltaic Lab \u2013 Micro and Nano Technologies Group (MNT) Electronic Engineering Department Universitat Polit\u00e8cnica de Catalunya (UPC)  EEBE, Av Eduard Maristany 10\u201314 Barcelona 08019 Spain"},{"name":"Barcelona Centre for Multiscale Science &amp; Engineering Universitat Polit\u00e8cnica de Catalunya (UPC)  Av Eduard Maristany 10\u201314 Barcelona 08019 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4226-1527","authenticated-orcid":false,"given":"I.","family":"Ca\u00f1o","sequence":"additional","affiliation":[{"name":"Photovoltaic Lab \u2013 Micro and Nano Technologies Group (MNT) Electronic Engineering Department Universitat Polit\u00e8cnica de Catalunya (UPC)  EEBE, Av Eduard Maristany 10\u201314 Barcelona 08019 Spain"},{"name":"Barcelona Centre for Multiscale Science &amp; Engineering Universitat Polit\u00e8cnica de Catalunya (UPC)  Av Eduard Maristany 10\u201314 Barcelona 08019 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3949-5058","authenticated-orcid":false,"given":"C.","family":"L\u00f3pez","sequence":"additional","affiliation":[{"name":"Barcelona Centre for Multiscale Science &amp; Engineering Universitat Polit\u00e8cnica de Catalunya (UPC)  Av Eduard Maristany 10\u201314 Barcelona 08019 Spain"},{"name":"Group of Characterization of Materials (GCM) Physics Department Universitat Polit\u00e8cnica de Catalunya (UPC)  EEBE, Av Eduard Maristany 10\u201314 Barcelona 08019 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7037-1443","authenticated-orcid":false,"given":"A.","family":"Navarro\u2010G\u00fcell","sequence":"additional","affiliation":[{"name":"Photovoltaic Lab \u2013 Micro and Nano Technologies Group (MNT) Electronic Engineering Department Universitat Polit\u00e8cnica de Catalunya (UPC)  EEBE, Av Eduard Maristany 10\u201314 Barcelona 08019 Spain"},{"name":"Barcelona Centre for Multiscale Science &amp; Engineering Universitat Polit\u00e8cnica de Catalunya (UPC)  Av Eduard Maristany 10\u201314 Barcelona 08019 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5901-017X","authenticated-orcid":false,"given":"J. 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