Ultrasensitive optoelectronic biosensor arrays based on twisted bilayer graphene superlattice.

Recent advances in twistronics have revealed tunable optoelectronic properties in twisted bilayer graphene (tBLG), including angle-dependent dielectric responses and enhanced light absorption due to van Hove singularity (VHS). However, achieving high photoresponsivity in tBLG-based sensors typically requires intense illumination. We present an ultrasensitive optoelectronic biosensor integrating tBLG superlattices with Au nanodisks and clustered regularly interspaced short palindromic repeat (CRISPR)-Cas12a via DNA origami. By aligning the 9.4° tBLG's VHS absorption spectrum with Au nanodisks' plasmonic resonance at 60 μW, we achieve a 7-fold photocurrent enhancement over pristine tBLG. CRISPR-Cas12a-mediated trans-cleavage dynamically modulates the local dielectric environment, enabling sub-femtomolar (44.63 attomolar, aM) nucleic acid detection without external amplification. Clinical validation using lung cancer samples shows high concordance with quantitative polymerase chain reaction (qPCR), demonstrating real-time, label-free detection of microRNA (miRNA). This hybrid platform combines moiré-engineered optoelectronics with programmable bio-nanoarrays, offering a scalable solution for precision diagnostics with ultralow detection limits and rapid response times.