Publication date: 17th February 2025
Flexible perovskite solar cells (f-PSCs) are particularly well-suited for a range of applications, including outdoor consumer products (e.g., portable chargers, wearables, tents, backpacks, deployable roll-ups, vehicles, drones, sails, etc.),([1]-[3]) indoor internet-of-things (IoT) devices,[4] and space technology.[5] Additionally, lightweight and manufacturability (e.g. roll-to-roll) are attractive features of f-PSCs for residential rooftop [6] and utility-scale PV applications.([7], [8])
Typically, f-PSCs are subjected to much higher applied mechanical stresses (stretching, bending, twisting) during manufacturing and operation, compared to their rigid counterparts on glass substrates.([9], [10]) Thus, the mechanical reliability of f-PSCs plays an outsized role in determining their durability.([9], [10]) Although numerous studies have documented cracking in the brittle, thin layers of multilayer f-PSCs, such as transparent-conducting oxide (TCO) electrode and perovskite, during bending tests, ([11], [12]) effects on polymer substrates in f-PSCs, and other flexible electronic devices, remain underexplored. This oversight likely stems from the assumption that polymer substrates, given their high toughness and substantial thickness relative to the other layers, are unlikely to crack. Contrary to this assumption, here we reveal pervasive, severe, and extensive cracking of polymer substrates in f-PSCs subjected to bending. Importantly, we show that such cracking of polymer substrates in the simple TCO/polymer bilayer, which is widely used in flexible electronic devices, is a general phenomenon. Substrate cracking undermines the mechanical integrity and reliability of the entire device, making it susceptible to cyclic fatigue and other time-dependent failure mechanisms, such as creep and environment-assisted cracking or degradation.
Based on in-situ experiments and modeling studies, we identify the substrate-cracking mechanisms specific to f-PSCs, which are related to the film/substrate elastic mismatch. Based on this understanding, we design and demonstrate a substrate-cracking mitigation strategy that relies on interlayer engineering. This approach is generic and holds promise for application to not only f-PSCs and OPVs but also myriad other flexible devices.
Experimental assistance from H.F. Garces and M. Poma is gratefully acknowledged. Funding: The work at Brown University was supported by the U.S. Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy (EERE) under the Solar Energy Technology Office (SETO) (Award No. DE-EE0009511). The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. S.K. and H.K. gratefully acknowledge the support of the U.S. Office of Naval Research (ONR) (Award Nos. Panther 4 N00014-21-1-2851, Panther 6 N00014-24-1-2200, and Tiger N00014-21-1-2054; managed by Dr. T. Bentley). Additional support from U.S. ONR (Award Nos. N00014-21-1-2815 and N00014-23-1-2688) is gratefully acknowledged. S.K. is also grateful for the support she received through the James R. Rice Graduate Fellowship in Solid Mechanics and the Miss Abbott’s School Alumnae Fellowship. S.S. acknowledges the support from Brown University as part of his Professor-at-Large appointment. The work at Yale University was supported by the National Science Foundation (Grant No. CBET-2315077 and NSF-GRFP (Grant No. DGE-2139841).
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