Bubble-blowing-inspired sub-micron thick freestanding silk films for programmable electronics

Thin film electronics that are capable of deforming and interfacing with nonplanar surfaces have attracted widespread interest in wearable motion detection or physiological signal recording due to their light weight, low stiffness, and high conformality. However, it is still a challenge to fabricate freestanding thin film substrates or matrices with only sub-micron thickness in a simple way, especially for those materials with metastable conformations, like regenerated silk protein. Herein, we developed a dip-coating method for the fabrication of sub-micron thick freestanding silk films inspired by blowing soap bubbles. Using a closed-loop frame to dip-coat in a concentrated silk fibroin aqueous solution, the substrate-free silk films with a thickness as low as hundreds of nanometres (∼150 nm) can be easily obtained after solvent evaporation. The silk films have extremely smooth surfaces (R_q < 3 nm) and can be tailored with different geometric shapes. The naturally dried silk films possess random coil dominated uncrystallized secondary structures, exhibiting high modulation ability and adaptability, which can be conformally attached on wrinkled skin or wrapped on human hair. Considering the methodological advantages and the unique properties of the obtained sub-micron thick silk films, several thin film based programmable electronics including transient/durable circuits, skin electrodes, transferred skin light-emitting devices and injectable electronics are successfully demonstrated after being deposited with gold or conducting polymer layers. This research provides a new avenue for preparing freestanding thin polymer films, showing great promise for developing thin film electronics in wearable and biomedical applications.