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Silicon nitride fabricated by low-pressure chemical vapor deposition (LPCVD) to be silicon-rich (SiNx), is a ubiquitous insulating thin film in the microelectronics industry, and an exceptional structural material for nanofabrication. Free-standing <100 nm-thick SiNx membranes are especially compelling, particularly when used to deliver forefront molecular sensing capabilities in nanofluidic devices. We developed an accessible, gentle, and solution-based photo-directed surface metallization approach well-suited to forming patterned metal films as integral structural and functional features in thin-membrane-based SiNx devices—for use as electrodes or surface chemical functionalization platforms, for example—augmenting existing device capabilities and properties for a wide range of applications.