TY  - JOUR
AU  - Ji, Sang-Geun
AU  - Noh, Eunseo
AU  - Kim, Jongbeom
AU  - Duan, Weiyuan
AU  - Kang, Bong Joo
AU  - Lee, Yonghui
AU  - Ding, Kaining
AU  - Seok, Sang Il
TI  - Cooperative Dipole Engineering Unlocks 92.8% Shockley–Queisser Voltage Limit in Wide-Bandgap Perovskites for Tandem Photovoltaics
JO  - ACS energy letters
VL  - 11
IS  - 1
SN  - 2380-8195
CY  - Washington, DC
PB  - American Chemical Society
M1  - FZJ-2026-01212
SP  - 442 - 450
PY  - 2026
AB  - 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.
LB  - PUB:(DE-HGF)16
UR  - <Go to ISI:>//WOS:001644774500001
DO  - DOI:10.1021/acsenergylett.5c02738
UR  - https://juser.fz-juelich.de/record/1052856
ER  -