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Low\u2010dimensional perovskite structures are widely explored for surface passivation due to their effective suppression of interfacial defects and enhanced environmental stability. While terminal molecules for constructing low\u2010dimensional structures provide excellent passivation, they can introduce potential barriers for charge transport if the energy levels are not well\u2010aligned. Herein, a tryptamine molecule is explored as the terminal molecule for the construction of a low\u2010dimensional structure for passivating the buried interface of perovskite solar cells. Based on the inclusion of nitrogen atoms in the aromatic heterocyclic structure, the terminal molecule shows an uplifted HOMO level that aligns well with the perovskite skeleton, giving rise to enhanced orbit coupling. Therefore, this low\u2010dimensional structure enables excellent surface passivation and interfacial carrier transport simultaneously, generating an outstanding open\u2010circuit voltage (\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>OC<\/jats:sub>\n                    ) up to 1.266 V and an efficiency of 23.53% for single\u2010junction wide\u2010bandgap (1.68 eV) perovskite solar cells. This improvement enables the fabrication of the perovskite\/silicon tandem solar cell with an efficiency of 33.22% (32.88% assessed by a third party) and a\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>OC<\/jats:sub>\n                    of 1.987 V. Moreover, the fast carrier transport at the interface suppressed the halide phase segregation, bringing much enhanced operation stability.\n                  <\/jats:p>","DOI":"10.1002\/adma.202523069","type":"journal-article","created":{"date-parts":[[2026,5,6]],"date-time":"2026-05-06T08:38:58Z","timestamp":1778056738000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Tryptamine Terminated Low\u2010Dimensional Interfaces Enabled High Performance Perovskite\/Silicon Tandem Solar Cells"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4662-4292","authenticated-orcid":false,"given":"Hao","family":"Liang","sequence":"first","affiliation":[{"name":"School of Physical Science and Technology Shanghai Tech University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-4208-7165","authenticated-orcid":false,"given":"Wenjing","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Physical Science and Technology Shanghai Tech University  Shanghai China"},{"name":"Mathematics and Science College Shanghai Normal University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5966-0175","authenticated-orcid":false,"given":"Xianyuan","family":"Jiang","sequence":"additional","affiliation":[{"name":"School of Physical Science and Technology Shanghai Tech University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin","family":"Wen","sequence":"additional","affiliation":[{"name":"School of Physical Science and Technology Shanghai Tech University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hang","family":"Yu","sequence":"additional","affiliation":[{"name":"School of Physical Science and Technology Shanghai Tech University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ye","family":"Ding","sequence":"additional","affiliation":[{"name":"Ideal Energy Sunflower (Shanghai) Equipment Inc.  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