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Here, we utilize pressure as an effective thermodynamic probe to decouple these interactions in BDA(EA)\n                    <jats:sub>2<\/jats:sub>\n                    Pb\n                    <jats:sub>3<\/jats:sub>\n                    Br\n                    <jats:sub>10<\/jats:sub>\n                    (BDA is 1,4\u2010butanediammonium, EA is ethylammonium), achieving the first pressure\u2010engineered synergistic enhancement of short\u2010circuit current (\n                    <jats:italic>I<\/jats:italic>\n                    <jats:sub>SC<\/jats:sub>\n                    ) and open\u2010circuit voltage (\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>OC<\/jats:sub>\n                    ). Comprehensive in situ characterizations reveal that pressure\u2010strengthened N\u2500H\u00b7\u00b7\u00b7Br hydrogen bonding induces cooperative organic cation ordering and inorganic octahedral distortion. This structural synergy amplifies spontaneous polarization, resulting in a 530\u2010fold increase in BPVE efficiency to 0.18% at 1.5\u00a0GPa, a value surpassing all previously reported OIHPs. Moreover, the enhanced organic\u2010inorganic interaction stabilizes the ferroelectric state, elevating the Curie temperature to 433 K. These results elucidate the microscopic mechanism underlying BPVE enhancement in 2D OIHP ferroelectrics and establish pressure modulation as an effective strategy for mechanistic studies and photovoltaic optimization.\n                  <\/jats:p>","DOI":"10.1002\/adma.75197","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T06:43:34Z","timestamp":1790750614000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Enhanced Bulk Photovoltaics in Polar 2D Hybrid Perovskite via Pressure\u2010Strengthened Organic\u2010Inorganic Interactions"],"prefix":"10.1002","author":[{"given":"Shiyu","family":"Fang","sequence":"first","affiliation":[{"name":"Center for High Pressure Science and Technology Advanced Research (HPSTAR)  Shanghai 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