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100 1 _ |a Ji, Sang-Geun
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245 _ _ |a Cooperative Dipole Engineering Unlocks 92.8% Shockley–Queisser Voltage Limit in Wide-Bandgap Perovskites for Tandem Photovoltaics
260 _ _ |a Washington, DC
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|b American Chemical Society
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520 _ _ |a Wide-bandgap (WBG) perovskite solar cells (PSCs, Eg ≃ 1.67 eV) still suffer from pronounced open-circuit-voltage (VOC) deficits. Here, we report a synergistic surface-passivation strategy that coassembles a dipolar quaternary-ammonium salt, acetylcholine chloride (ACCl), with an electron-rich long-chain alkylammonium halide, n-octylammonium iodide (OAI). A mixed ACCl:OAI treatment reconstructs the perovskite surface, lowers surface-trap density, and aligns the valence band with the hole-transport layer. Consequently, the champion WBG PSC delivers VOC = 1.29 V, JSC = 20.0 mA cm–2, FF = 82.8%, and PCE = 21.27%, corresponding to 92.8% of the Shockley–Queisser voltage limit. When integrated as the top absorber in a monolithic n-i-p perovskite/p-type Si tandem, the passivated WBG cell contributed to a PCE of 26.8% with a VOC of 1.91 V. These results reveal that cooperative defect passivation and energy-level engineering are both essential to unlock the full voltage potential of WBG perovskites.
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700 1 _ |a Noh, Eunseo
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700 1 _ |a Kim, Jongbeom
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700 1 _ |a Duan, Weiyuan
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700 1 _ |a Kang, Bong Joo
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700 1 _ |a Lee, Yonghui
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700 1 _ |a Ding, Kaining
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700 1 _ |a Seok, Sang Il
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773 _ _ |a 10.1021/acsenergylett.5c02738
|g Vol. 11, no. 1, p. 442 - 450
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|t ACS energy letters
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|y 2026
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856 4 _ |y Published on 2025-12-22. Available in OpenAccess from 2026-12-22.
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