Large-area, photo-programmable 2D semiconductors with chromic molecular functionalization

Reconfigurable electronics expands device functionality and promises previously unknown computing paradigms, as the channel layer characteristics can be dynamically controlled. Two-dimensional semiconductors coupled with photo-responsive chromic molecules offer a compelling route as atomically thin channels are highly sensitive to molecular conformation changes. However, most demonstrations have been limited to microscale single-flake devices, limiting scalability and technological relevance. Here, we report an optically reconfigurable platform integrating centimeter-scale monolayer WS₂ and WSe₂ with an azobenzene (Azo) overlayer. Wavelength-selective trans-cis Azo photoisomerization generates a reversible interfacial dipole that serves as an optical gate, enabling precise and uniform modulation of both electron and hole densities (~2.5 × 10¹² cm^-2) over large areas. This optical actuation further supports spatially programmable patterning of optoelectronic properties and delivers repeatable modulation across large transistor arrays. Together, these results establish a scalable smart materials platform for reconfigurable optoelectronics that is light-programmable.