Flexible bioelectrodes with enhanced wrinkle microstructures for reliable electrochemical modification and neuromodulation in vivo.

Limited electrode size with high electrochemical performance and reliability of modified materials are two of the main concerns for flexible neural electrodes in recent years. Here, an effective fabrication method of enhanced micro-scale wrinkles based on oil-pretreated hyperelastic substrates (PDMS and Ecoflex) is proposed for the application of microelectrode biosensors. Compared to pre-stretching or compressing methods, this approach has better advantages including compatibility with MEMS processes on wafer and easy replication. Wrinkled gold microelectrodes exhibit superior electrochemical properties than the flat one, and no crack or delamination occurs after electroplating PEDOT:PSS and platinum black on wrinkled microelectrodes. Cyclic voltammetry (CV) scanning for 2500 times is performed to investigate adhesion and stability of modified materials. For the modified microelectrodes, no significant change is observed in charge storage capacity (CSC) and impedance at 1 kHz, whereas PEDOT:PSS coated flat microelectrodes appears delamination. Ultrasonication and cycling forces are also conducted on modified microelectrodes, which demonstrates little influence on the wrinkled ones. Flexible wrinkled microelectrodes are further verified by in-vivo ECoG recordings combined with optogenetics in mice. These results highlight the importance of micro-structure in neural electrode design and tremendous application potentials in flexible electronics.