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001052856 1001_ $$0P:(DE-HGF)0$$aJi, Sang-Geun$$b0
001052856 245__ $$aCooperative Dipole Engineering Unlocks 92.8% Shockley–Queisser Voltage Limit in Wide-Bandgap Perovskites for Tandem Photovoltaics
001052856 260__ $$aWashington, DC$$bAmerican Chemical Society$$c2026
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001052856 520__ $$aWide-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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001052856 7001_ $$0P:(DE-HGF)0$$aNoh, Eunseo$$b1
001052856 7001_ $$0P:(DE-HGF)0$$aKim, Jongbeom$$b2
001052856 7001_ $$0P:(DE-Juel1)169946$$aDuan, Weiyuan$$b3
001052856 7001_ $$0P:(DE-HGF)0$$aKang, Bong Joo$$b4
001052856 7001_ $$0P:(DE-HGF)0$$aLee, Yonghui$$b5
001052856 7001_ $$0P:(DE-Juel1)130233$$aDing, Kaining$$b6$$ufzj
001052856 7001_ $$0P:(DE-HGF)0$$aSeok, Sang Il$$b7$$eCorresponding author
001052856 773__ $$0PERI:(DE-600)2864177-2$$a10.1021/acsenergylett.5c02738$$gVol. 11, no. 1, p. 442 - 450$$n1$$p442 - 450$$tACS energy letters$$v11$$x2380-8195$$y2026
001052856 8564_ $$uhttps://juser.fz-juelich.de/record/1052856/files/Post-Print.docx$$yPublished on 2025-12-22. Available in OpenAccess from 2026-12-22.
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