Synergic Effects of Randomly Aligned SWCNT Mesh and Self‐Assembled Molecule Layer for High‐Performance, Low‐Bandgap, Polymer Solar Cells with Fast Charge Extraction

Abstract

Currently, most of the promising organic solar cells (OSCs) are based on low bandgap polymer donors with deep‐lying highest occupied molecular orbit (HOMO) levels, which impose the challenges for device architecture design. In terms of fast charge extraction and suppression of bimolecular recombination, elaborate interface design in low bandgap OSCs is of significance to further boost their ultimate efficiency. In this work, a facile solution‐processed functionalized single wall carbon nanotube (f‐SWCNT) mesh/self‐assembled molecule (SAM) hybrid structure is reported as hole transport layer (HTL) in low bandgap OSCs. The effectiveness of such hybrid HTL originates from two aspects: (i) SAM layer can effectively realize Ohmic contact between f‐SWCNT and low bandgap polymer donors with deep‐lying HOMO levels due to the reduction of interface energy barrier; (ii) f‐SWCNT mesh can provide fast hole extraction pathways to quickly sweep out photogenerated charges. As a consequence of synergic effects of such hybrid HTL, both photocurrent and fill factor are greatly enhanced due to the reduced bimolecular recombination. Together with careful light management by using ZnO optical spacer, a high efficiency of 10.5% has been achieved. This work offers an excellent choice for large‐scale processable and effective HTL toward the application in low bandgap OSCs with deep‐lying energy levels.