We have designed multifunctional silver alginate hydrogel microcontainers referred to as loaded microcapsules with different sizes by assembling them via a template assisted approach using natural, highly porous calcium carbonate cores. Sodium alginate was immobilized into the pores of calcium carbonate particles of different sizes followed by cross-linking via addition of silver ions, which had a dual purpose: on one hand, the were used as a cross-linking agent, albeit in the monovalent form, while on the other hand they have led to formation of silver nanoparticles. Monovalent silver ions, an unusual cross-linking agent, improve the sensitivity to ultrasound, lead to homogeneous distribution of silver nanoparticles. Silver nanoparticles appeared on the shell of the alginate microcapsules in the twin-structure as determined by transmission electron microscopy. Remote release of a payload from alginate containers by ultrasound was found to strongly depend on the particle size. The possibility to use such particles as a platform for label-free molecule detection based on the surface enhanced Raman scattering was demonstrated. Cytotoxicity and cell uptake studies conducted in this work have revealed that microcontainers exhibit nonessential level of toxicity with an efficient uptake of cells. The above-described functionalities constitute building blocks of a theranostic system, where detection and remote release can be achieved with the same carrier.

Nanophotonic waveguide enhanced Raman spectroscopy (NWERS) is a sensing technique that uses a highly confined waveguide mode to excite and collect the Raman scattered signal from molecules in close vicinity of the waveguide. The most important parameters defining the figure of merit of an NWERS sensor include its ability to collect the Raman signal from an analyte, i.e. "the Raman conversion efficiency" and the amount of "Raman background" generated from the guiding material. Here, we compare different photonic integrated circuit (PIC) platforms capable of on-chip Raman sensing in terms of the aforementioned parameters. Among the four photonic platforms under study, tantalum oxide and silicon nitride waveguides exhibit high signal collection efficiency and low Raman background. In contrast, the performance of titania and alumina waveguides suffers from a strong Raman background and a weak signal collection efficiency, respectively.

A hybrid integration of nanoplasmonic antennas with silicon nitride waveguides enables miniaturized chips for surface-enhanced Raman spectroscopy at visible and near-infrared wavelengths. This integration can result in high-throughput SERS assays on low sampling volumes. However, current fabrication methods are complex and rely on electron-beam lithography, thereby obstructing the full use of an integrated photonics platform. Here, we demonstrate the electron-beam-free fabrication of gold nanotriangles on deep-UV patterned silicon nitride waveguides using nanosphere lithography. The localized surface-plasmon resonance of these nanotriangles is optimized for Raman excitation at 785 nm, resulting in a SERS substrate enhancement factor of 2.5 × 10⁵. Furthermore, the SERS signal excited and collected through the waveguide is as strong as the free-space excited and collected signal through a high NA objective.

Recent studies have shown that evanescent Raman spectroscopy using a silicon nitride (SiN) nanophotonic waveguide platform has higher signal enhancement when compared to free-space systems. However, signal-to-noise ratio from the waveguide at a low analyte concentration is constrained by the shot-noise from the background light originating from the waveguide itself. Hence, understanding the origin and properties of this waveguide background luminescence (WGBL) is essential to developing mitigation strategies. Here, we identify the dominating component of the WGBL spectrum composed of a broad Raman scattering due to momentum selection-rule breaking in amorphous materials, and several peaks specific to molecules embedded in the core. We determine the maximum of the Raman scattering efficiency of the WGBL at room temperature for 785 nm excitation to be 4.5 ± 1 × 10⁻⁹ cm⁻¹·sr⁻¹, at a Stokes shift of 200 cm⁻¹. This efficiency decreases monotonically for higher Stokes shifts. Additionally, we also demonstrate the use of slotted waveguides and quasi-transverse magnetic polarization as some mitigation strategies.

The integration of plasmonic antennas on single‐mode silicon nitride waveguides offers great perspective for integrated surface‐enhanced Raman spectroscopy (SERS). However, the few reported experimental demonstrations still require multiple plasmonic antennas to obtain a detectable SERS spectrum. Here, we show, for the first time, SERS signal detection by a single nanoplasmonic antenna integrated on a single‐mode SiN waveguide. For this purpose, we investigated a backscattering detection scheme in combination with background noise reduction, which allowed an optimization of the signal‐to‐noise ratio (SNR) of this platform. Furthermore, a comparison with the free‐space SERS spectrum of the same antenna shows that the conversion efficiency from pump power to total radiated Stokes power is twice as efficient in the case of waveguide excitation. As such, we explored several important aspects in the optimization of on‐chip SERS sensors and experimentally demonstrated the power of exciting nanoplasmonic antennas using the evanescent field of a waveguide. This observation not only is useful for Raman sensing but also could be beneficial for any process involving plasmonic enhancement.

Surface-Enhanced Raman Spectroscopy (SERS) allows for the highly specific detection of molecules by enhancing the inherently weak Raman signals near the surface of plasmonic nanostructures. A variety of plasmonic nanostructures have been developed for SERS signal excitation and collection in a conventional free-space microscope, among which the gold nanodomes offer one of the highest SERS enhancements. Nanophotonic waveguides have recently emerged as an alternative to the conventional Raman microscope as they can be used to efficiently excite and collect Raman signals. Integration of plasmonic structures on nanophotonic waveguides enables reproducible waveguide-based excitation and collection of SERS spectra, such as in nanoplasmonic slot waveguides. In this paper, we compare the SERS performance of gold nanodomes, in which the signal is excited and collected in free space, and waveguide-based nanoplasmonic slot waveguide. We evaluate the SERS signal enhancement and the SERS background of the different SERS platforms using a monolayer of nitrothiophenol. We show that the nanoplasmonic slot waveguide approaches the gold nanodomes in terms of the signal-to-background ratio. We additionally demonstrate the first-time detection of a peptide monolayer on a waveguide-based SERS platform, paving the way towards the SERS monitoring of biologically relevant molecules on an integrated lab-on-a-chip platform.