We present a novel approach to fabricate flexible organic solar cells without indium tin oxide (ITO) and poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS). We use junctionfree metal nanonetworks (NNs) as transparent electrodes. The metal NNs are monolithically etched using nanoscale shadow masks, and they exhibit excellent optoelectronic performance. Furthermore, the optoelectrical properties of the NNs can be controlled by both the initial metal layer thickness and NN density. Hence, with an extremely thin silver layer, the appropriate density control of the networks can lead to high transmittance and low sheet resistance. Such NNs can be utilized for thin film devices without planarization by conductive materials such as PEDOT:PSS. As a result, we successfully fabricate a highly efficient flexible organic solar cell with a power conversion efficiency (PCE) of 10.6% and high device yield (93.8%) on PEDOT-free and ITO-free transparent electrodes. Furthermore, the flexible solar cell retains 94.3% of the initial PCE even after 3000 bending stress tests (strain: 3.13%).

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Intrinsically stretchable organic solar cells (IS‐OSCs) have been recently spotlighted for their omnidirectional stretchability, seamless integrability to any surface, and facile fabrication. Due to these attributes, IS‐OSCs are ideal off‐grid power sources, especially for wearable electronics in real‐life. However, under human body elongation as high as ≈40%, cracks in IS‐OSCs are considered inevitable, and the origin of the mechanical failure is rarely identified. Herein, the crack‐initiation and the propagation mechanism are first clarified. Based on this, a crack‐free substrate/transparent electrode platform for stretchable electronics is also suggested. A double‐locking scheme, which reinforces the physical/chemical adsorption within the most mechanically fragile layer, a poly(3,4‐ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) and also with thermoplastic polyurethane substrate, is introduced. As a result, the crack‐onset strain of double‐locked IS‐OSCs surpasses 40%, while that of pristine ones is less than 20%. The IS‐OSCs with the double‐locked system exhibits an efficient power conversion efficiency of 10.2%, and the absence of cracks allows the IS‐OSCs to maintain 79.7% of the initial PCE at 40% strain.

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