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Nevertheless, for the deposition of SAMs with a monolayer thickness and a high packing density on metal oxide substrates, critical challenges persist. To overcome these, the study focuses on the impact of annealing temperature \u2013 an intrinsic yet so far unexplored process parameter \u2013 during the formation of SAMs. By performing in situ angle\u2010resolved X\u2010ray photoelectron spectroscopy combined with advanced data analysis routines, it is revealed that increasing the annealing temperature reduces the formed SAM layer thickness from a multilayer stack of \u22485\u00a0nm at 100\u00a0\u00b0C (conventional temperature employed in literature) to a monolayer at 150\u00a0\u00b0C. Furthermore, denser adsorption of the SAM to the metal oxide surface is promoted at high temperatures, which enhances the interfacial SAM\/perovskite passivation quality. With this strategy, a 1.3%\n                    <jats:sub>abs<\/jats:sub>\n                    power conversion efficiency (\n                    <jats:italic>PCE<\/jats:italic>\n                    ) increment is obtained in fully\u2010textured perovskite\/silicon tandem solar cells, with improved reproducibility, and a champion device approaching 30%\n                    <jats:italic>PCE<\/jats:italic>\n                    . This study advances the understanding of SAMs formation and presents a promising strategy for further progress in high\u2010efficiency perovskite\u2010based solar cells.\n                  <\/jats:p>","DOI":"10.1002\/smtd.202401758","type":"journal-article","created":{"date-parts":[[2025,2,26]],"date-time":"2025-02-26T04:17:47Z","timestamp":1740543467000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":32,"title":["Tuning Self\u2010Assembly of Hole\u2010Selective Monolayers for Reproducible Perovskite\/Silicon Tandem Solar Cells"],"prefix":"10.1002","volume":"9","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-2128-9467","authenticated-orcid":false,"given":"Oussama","family":"Er\u2010Raji","sequence":"first","affiliation":[{"name":"Fraunhofer Institute for Solar Energy Systems ISE  Heidenhofstr. 2 79110 Freiburg Germany"},{"name":"Chair of Photovoltaic Energy Conversion Department of Sustainable Systems Engineering (INATECH) University of Freiburg  Emmy\u2010Noether\u2010Str.2 79110 Freiburg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Stefan","family":"Lange","sequence":"additional","affiliation":[{"name":"Fraunhofer Center for Silicon Photovoltaics CSP  Otto\u2010Eissfeldt\u2010Str. 12 06120 Halle Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Carl Eric","family":"Hartwig","sequence":"additional","affiliation":[{"name":"Fraunhofer Center for Silicon Photovoltaics CSP  Otto\u2010Eissfeldt\u2010Str. 12 06120 Halle Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Adi","family":"Prasetio","sequence":"additional","affiliation":[{"name":"KAUST Solar Center (KSC) Physical Sciences and Engineering Division (PSE) King Abdullah University of Science and Technology (KAUST)  Thuwal 23955 Saudi Arabia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Martin","family":"Bivour","sequence":"additional","affiliation":[{"name":"Fraunhofer Institute for Solar Energy Systems ISE  Heidenhofstr. 2 79110 Freiburg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Martin","family":"Hermle","sequence":"additional","affiliation":[{"name":"Fraunhofer Institute for Solar Energy Systems ISE  Heidenhofstr. 2 79110 Freiburg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Marko","family":"Turek","sequence":"additional","affiliation":[{"name":"Fraunhofer Center for Silicon Photovoltaics CSP  Otto\u2010Eissfeldt\u2010Str. 12 06120 Halle Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Stefaan","family":"De Wolf","sequence":"additional","affiliation":[{"name":"KAUST Solar Center (KSC) Physical Sciences and Engineering Division (PSE) King Abdullah University of Science and Technology (KAUST)  Thuwal 23955 Saudi Arabia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Stefan W.","family":"Glunz","sequence":"additional","affiliation":[{"name":"Fraunhofer Institute for Solar Energy Systems ISE  Heidenhofstr. 2 79110 Freiburg Germany"},{"name":"Chair of Photovoltaic Energy Conversion Department of Sustainable Systems Engineering (INATECH) University of Freiburg  Emmy\u2010Noether\u2010Str.2 79110 Freiburg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juliane","family":"Borchert","sequence":"additional","affiliation":[{"name":"Fraunhofer Institute for Solar Energy Systems ISE  Heidenhofstr. 2 79110 Freiburg Germany"},{"name":"Chair of Photovoltaic Energy Conversion Department of Sustainable Systems Engineering (INATECH) University of Freiburg  Emmy\u2010Noether\u2010Str.2 79110 Freiburg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Patricia S. 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