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However, maintaining long\u2010term operational stability and ensuring consistent performance under realistic fabrication and deployment conditions remain critical challenges. To overcome these issues, we propose a dual optimization strategy that integrates electrical interface engineering with tailored optical design. First, we introduce a novel self\u2010assembled monolayer containing a propoxyphenyl\u2010based linker, which enhances molecular packing density and significantly increases the shunt resistance of the device. This interface modification improves hole selectivity and broadens fabrication tolerance by increasing the allowable range of current mismatch between sub\u2010cells while maintaining high efficiency. Second, we design a light\u2010scattering film by embedding shape\u2010controlled phosphor particles into a textured poly(dimethylsiloxane) (PDMS) matrix, which improves light harvesting through UV down\u2010conversion and diffuse transmission. As a result, we achieve a PCE of 31.66% for a 1 cm\n                    <jats:sup>2<\/jats:sup>\n                    device. These findings demonstrate a synergistic design approach and offer a practical route toward robust, high\u2010efficiency PST devices with improved fabrication tolerance.\n                  <\/jats:p>","DOI":"10.1002\/smll.74792","type":"journal-article","created":{"date-parts":[[2026,7,21]],"date-time":"2026-07-21T10:53:26Z","timestamp":1784631206000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Integrated Molecular and Optical Materials Design for High\u2010Efficiency Perovskite\/Si Tandem Cells"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-3305-2843","authenticated-orcid":false,"given":"Young Im","family":"Noh","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST)  Ulsan Republic of 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