a Schematic illustration of the impact of molecular ordering on thin film mechanical properties. Desirable molecular organization is required to allow an intrinsically stretchable PSC film to be stretched under not only uniaxial but also multi-directional strains. b Illustration of polymer chain dynamics under strain in a polymer film that possesses high or low stretchability. c A polymer film under multi-directional strain. The PSC film (i.e., P4) is prepared and stretched biaxially on a PDMS substrate. The stretching forces are applied uniformly from 4 directions, and a maximum strain of 100% is introduced biaxially. d Calculated relative stretchability (rS) values of reported neat stretchable PSCs are depicted and compared with P1–P4 in this work. rS values of P1–P4 were averaged from at least 2 DR and 2 rDoC samples over 2 batches under 0, 50, and 100% strain. Results from literature were extracted from corresponding papers. e
rS and corresponding crack onset strain of PSCs. The rS is defined to quantify the stretchability of PSCs. Additional reported PSCs were analyzed, including PDPPTVT (Mn: 20.4 kg mol-1)16, PDPPTVT-PDCA (Mn: 16.2 kg mol-1)16, PDPPTVT-alkyl (Mn: 24.0 kg mol-1)16, P2TDPP2TFT4 (Mn: 29.5 kg mol-1)15, IDTBT (Mn: 109 kg mol-1)17, and PII2T-C8 (Mn: 434 kg mol-1)18. f, g Correlations between charge carrier mobility and rS values. Normalized FET mobility under f 50 and g 100% uniaxial strain (i.e., mobility under 50 or 100% strain divided by the mobility at 0% strain) of the studied and reported PSCs are depicted. Normalized mobility for P1–P4 were averaged from at least 5 devices over 2 batches. Results from literature were extracted from corresponding papers based on reported data. A clear trend shows that the electrical performance can be sustained under strain if the PSC possesses a higher rS value. h Comparison of rS values between neat PSC (i.e., P4), terpolymer (DPP-8TVT in ref. 19), and polymer/additive blends (DPP/DOP-r in ref. 25). rS values for P4 were averaged from at least 2 DR and 2 rDoC samples over 2 batches under 0, 50, and 100% strain. Results of DPP-8TVT and DPP/DOP-r were extracted from corresponding papers.