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Abstract Surface‐enhanced Raman scattering (SERS) sensors typically employ nanophotonic structures that support high‐field confinement and enhancement in hotspots to increase the Raman scattering from target molecules by orders of magnitude. In general, high field and SERS enhancement can be achieved by reducing the critical dimensions and mode volumes of the hotspots to nanoscale. To this end, a multitude of SERS sensors employing photonic structures with nanometric hotspots have been demonstrated. However, delivering analyte molecules into nanometric hotspots is challenging, and the trade‐off between field confinement/enhancement and analyte delivery efficiency is a critical limiting factor for the performance of many nanophotonic SERS sensors. Here, a new type of SERS sensor employing solid‐metal nanoparticles and bulk liquid metal is demonstrated to form nanophotonic resonators with a nanoparticle‐on‐liquid‐mirror (NPoLM) architecture, which effectively resolves this trade‐off. In particular, this unconventional sensor architecture allows for the convenient formation of nanometric hotspots by introducing liquid metal after analyte molecules are efficiently delivered to the surface of gold nanoparticles. In addition, a cost‐effective and reliable process is developed to produce gold nanoparticles on a substrate suitable for forming NPoLM structures. These NPoLM structures achieve two orders of magnitude higher SERS signals than the gold nanoparticles alone. 

Abstract Gallium‐based liquid metals (LMs) are widely used for stretchable and reconfigurable electronics thanks to their fluidic nature and excellent conductivity. These LMs possess attractive optical properties for photonics applications as well. However, due to the high surface tension of the LMs, it is challenging to form LM nanostructures with arbitrary shapes using conventional nanofabrication techniques. As a result, LM‐based nanophotonics has not been extensively explored. Here, a simple yet effective technique is demonstrated to deterministically fabricate LM nanopatterns with high yield over a large area. This technique demonstrates for the first time the capability to fabricate LM nanophotonic structures of various precisely defined shapes and sizes using two different LMs, that is, liquid gallium and liquid eutectic gallium–indium alloy. High‐density arrays of LM nanopatterns with critical feature sizes down to ≈100 nm and inter‐pattern spacings down to ≈100 nm are achieved, corresponding to the highest resolution of any LM fabrication technique developed to date. Additionally, the LM nanopatterns demonstrate excellent long‐term stability under ambient conditions. This work paves the way toward further development of a wide range of LM nanophotonics technologies and applications.