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Balancing the efficiency and mechanical endurance of flexible Cu 2 ZnSn(S,Se) 4 (CZTSSe) thin film solar cells is challenging its potential applications of the day. Here, a straightforward strategy is developed to prepare flexible solar cells with the coexistence of photovoltaic performance and flexibility by introducing a novel SbCl 3 in precursor solution. Sb-doped CZTSSe thin film with progressive grain growth from nanoscale to microscale and strengthened toughness with porosity from 8.13 % to 2.44 % is obtained. By exploiting the benefits of upgrading the band matching and tailoring the residual stress, SbCl 3 solution with a concentration of 0.30 mol/L achieves the optimum heterojunction characteristic and mechanical performance. The final structured device with improved efficiency from 3.27 % to 4.98 % and indomitable mechanical endurance is attained, which can reserve 93 % of its original efficiency after bending 200 times. The present work indubitably paves a convenient way toward efficient and flexible photovoltaic devices. • Sb doping is applied to the tailor residual stress of flexible CZTSSe thin film. • Alleviated residual stress contributes to a superior microstructure of CZTSSe. • 0.30 mol/L SbCl 3 exhibits the best PCE with satisfying bending durability. [ABSTRACT FROM AUTHOR]

Antisite defects induced undesirable open-circuit voltage (Voc) and fill factor (FF) have always been considerable factors that plagued the efficiency enhancement of Cu 2 ZnSn(S,Se) 4 (CZTSSe)-based photovoltaic devices. Accordingly, sputtered Cu–Zn–Sn–S precursor with e-beam evaporated CdS layer on its top and bottom followed by selenization process was firstly proposed to obtain Cd-alloyed flexible CZTSSe thin film solar cells. The introduced CdS significantly improved crystalline quality and promoted grain growth of CZTSSe absorber. Besides, captured conduction band offset (CBO) exhibited a "cliff-like" structure with the maximum value of −0.15 eV when CdS layer was evaporated on top of Cu–Zn–Sn–S precursor, which largely relieved the band alignment issue in CZTSSe/CdS heterojunction. Interestingly, for CZTSSe prepared with CdS on top, Cd element shows a better uniform distribution in absorber than that with CdS on bottom. Finally, thanks to the evaporated CdS layer on precursor top, the efficiency of flexible CZTSSe thin film solar cell was improved from 2.31% to 4.52%, featuring a Voc of 343.53 mV, Jsc of 27.94 mA/cm2 and FF of 47.70%. • Cd-alloyed CZTSSe was obtained by evaporating CdS layer on CZTS precursor. • The evaporated CdS layer largely relieved band mismatching of CZTSSe/CdS. • CBO exhibited a maximum value of −0.15 eV when CdS was on precursor top. • Evaporated CdS on top of precursor can better guarantee the device performance. [ABSTRACT FROM AUTHOR]