A Tandem Organic Solar Cell with PCE of 14.52% Employing Subcells with the Same Polymer Donor and Two Absorption Complementary Acceptors

Abstract The tandem structure is an efficient way to simultaneously tackle absorption and thermalization losses of the single junction solar cells. In this work, a high‐performance tandem organic solar cell (OSC) using two subcells with the same donor poly[(2,6‐(4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)‐benzo[1,2‐b:4,5‐b′]dithiophene))‐alt‐(5,5‐(1′,3′‐di‐2‐thienyl‐5′,7′‐bis(2‐ethylhexyl)benzo[1′,2′‐c:4′,5′‐c′]dithiophene‐4,8‐dione))] (PBDB‐T) and two acceptors, F‐M and 2,9‐bis(2‐methylene‐(3(1,1‐dicyanomethylene)benz[f ]indanone))7,12‐dihydro‐(4,4,10,10‐tetrakis(4‐hexylphenyl)‐5,11‐diocthylthieno[3′,2′:4,5]cyclopenta[1,2‐b]thieno[2″,3″:3′,4′]cyclopenta[1′,2′:4,5]thieno[2,3‐f][1]benzothiophene (NNBDT), with complementary absorptions is demonstrated. The two subcells show high V_oc with value of 0.99 V for the front cell and 0.86 V for the rear cell, which is the prerequisite for obtaining high V_oc of their series‐connected tandem device. Although there is much absorption overlap for the subcells, a decent J_sc of the tandem cell is still obtained owing to the complementary absorption of the two acceptors in a wide range. With systematic device optimizations, a best power conversion efficiency of 14.52% is achieved for the tandem device, with a high V_oc of 1.82 V, a notable FF of 74.7%, and a decent J_sc of 10.68 mA cm⁻². This work demonstrates a promising strategy of fabricating high‐efficiency tandem OSCs through elaborate selection of the active layer materials in each subcell and tradeoff of the V_oc and J_sc of the tandem cells.