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We demonstrate vapor-phase, layer-by-layer heteroepitaxial growth exemplified by CsPbBr\n                    <jats:sub>3<\/jats:sub>\n                    deposition on single crystals of PEA\n                    <jats:sub>2<\/jats:sub>\n                    PbBr\n                    <jats:sub>4<\/jats:sub>\n                    (PEA: 2-phenylethylammonium). Angstrom-level thickness control and subangstrom smooth layers enable quantum-confined photoluminescence of CsPbBr\n                    <jats:sub>3<\/jats:sub>\n                    from monolayer, bilayer, and through to bulk. The interfacial structure controls the electronic structure from a Cs\u2012PEA-terminated interface (type II heterojunction) to a PEA\u2012PEA-terminated interface (type I heterojunction), with a layer-tunable band offset shift exceeding 0.5 electron volts. Electron transfer from CsPbBr\n                    <jats:sub>3<\/jats:sub>\n                    to PEA\n                    <jats:sub>2<\/jats:sub>\n                    PbBr\n                    <jats:sub>4<\/jats:sub>\n                    for a type II Cs\u2012PEA heterojunction results in delayed electron-hole recombination beyond 10 microseconds. Precise quantum confinement control and large band offset tunability unlock perovskite heterojunctions as platforms for scalable, superlattice-based optoelectronic applications.\n                  <\/jats:p>","DOI":"10.1126\/science.adx5685","type":"journal-article","created":{"date-parts":[[2025,11,13]],"date-time":"2025-11-13T19:02:59Z","timestamp":1763060579000},"page":"716-721","update-policy":"https:\/\/doi.org\/10.34133\/aaas_crossmark","source":"Crossref","is-referenced-by-count":20,"title":["Layer-by-layer epitaxial growth of perovskite heterostructures with tunable band offsets"],"prefix":"10.1126","volume":"390","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2793-2065","authenticated-orcid":true,"given":"Yang","family":"Lu","sequence":"first","affiliation":[{"name":"Department of Chemical Engineering and Biotechnology, University of Cambridge, Cambridge, UK."},{"name":"Cavendish Laboratory, University of Cambridge, Cambridge, 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