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Here, we report how NO\n                    <jats:sub>2<\/jats:sub>\n                    physisorption precisely modulates band alignment and built\u2010in potentials in self\u2010powered InSe\/SnS\n                    <jats:sub>2<\/jats:sub>\n                    heterojunction photodetectors. Using electrostatic gating, we identify three distinct regimes: (I) a robust p\u2013n configuration (\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>g<\/jats:sub>\n                    \u2264 \u201350\u2009V), where adsorption induces a collective electron\u2010withdrawing effect, enabling efficient p\u2010i\u2010n\u2010like behavior with near\u2010ideal charge separation; (II) an intermediate p\u2013n regime (\u201350\u2009V\u2009&lt;\u2009\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>g<\/jats:sub>\n                    &lt; \u201330\u2009V), where competing electron withdrawal and recombination effects allow dynamic tuning the electronic structure and optoelectronic properties, and (III) an illumination\u2010sensitive n\u2013n\n                    <jats:sup>+<\/jats:sup>\n                    mode (\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>g<\/jats:sub>\n                    \u2265 \u201330\u2009V), where NO\n                    <jats:sub>2<\/jats:sub>\n                    molecules act as recombination centers, suppressing the built\u2010in potential. This dual control via gating and molecular adsorption provides unprecedented manipulation of charge separation and transport, opening avenues for next\u2010generation multifunctional optoelectronic devices.\n                  <\/jats:p>","DOI":"10.1002\/smsc.202500616","type":"journal-article","created":{"date-parts":[[2026,3,8]],"date-time":"2026-03-08T21:10:51Z","timestamp":1773004251000},"source":"Crossref","is-referenced-by-count":2,"title":["Dynamic Control of Band Alignment and Built\u2010In Potential in High Performance Self\u2010Powered InSe\/SnS\n                    <sub>2<\/sub>\n                    Van der Waals Photodetectors via Gas Molecular Physisorption"],"prefix":"10.1002","volume":"6","author":[{"given":"Ze","family":"Cao","sequence":"first","affiliation":[{"name":"School of Physics Beijing Institute of Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mohamed","family":"Abid","sequence":"additional","affiliation":[{"name":"EduAI dynamics  Astana Kazakhstan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cormac","family":"\u00d3 Coile\u00e1in","sequence":"additional","affiliation":[{"name":"Department of Electrical Power Systems and Information Technology Institute of Physics University of the Bundeswehr Munich  Neubiberg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5731-2257","authenticated-orcid":false,"given":"Fengjiang","family":"An","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Explosion Science and Safety Beijing Institute of Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ching\u2010Ray","family":"Chang","sequence":"additional","affiliation":[{"name":"Department of Physics National Taiwan University  Taipei Taiwan, ROC"},{"name":"Quantum Information Center Chung Yuan Christian University  Taoyuan Taiwan, ROC"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuh\u2010Renn","family":"Wu","sequence":"additional","affiliation":[{"name":"Graduate Institute of Photonics and Optoelectronics and Department of Electrical Engineering National Taiwan University  Taipei Taiwan, ROC"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0293-9022","authenticated-orcid":false,"given":"Han\u2010Chun","family":"Wu","sequence":"additional","affiliation":[{"name":"School of Physics Beijing Institute of Technology  Beijing P. R. 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