Silica-encapsulated Raman-reporter embedded SERS nanoprobes, named nanoaggregate embedded beads (NAEBs), were conjugated to the Salmonella specific tailspike protein (TSP) isolated from the P22 bacteriophage to enable a highly specific and ultrasensitive optical transduction platform. We demonstrate three successful surface conjugation strategies and highlight the detection of a single bacterium using SERS.

Paper‐based surface‐enhanced Raman spectroscopy (SERS) sensors can be fabricated easily by dropcasting or inkjet printing colloidal Au nanoparticles onto cellulose‐based filter papers. They are flexible, economical, and sensitive and provide the crucial advantage of point‐of‐need sampling for application in the field. In this study, paper‐based SERS sensors are fabricated through inkjet printing of a colloidal Au sol onto a filter paper substrate. We have characterized their SERS performances with benzenethiol and pyridine molecules using a handheld Raman analyzer. Due to the heterogeneous loading of the Au nanoclusters on the paper substrate, we introduce the concept of receiver operating characteristic as an alternate measurand to quantify the performance of these sensors. With their inherent filtration sampling capability, we demonstrate the use of paper SERS sensors for the detection of chemical aerosols. Lastly, we present the use of a precision materials printer to deposit quantifiable amounts of analyte (fentanyl) uniformly across the active sensing area of a paper SERS sensor. This will allow for analyte‐loaded certified references to be prepared and used in the field as standards for comparison.

Optical excitation of small Au nanoparticle (NP) clusters of appropriate wavelength is known to generate intense electromagnetic fields localized uniquely at NP junction sites within the nanoclusters. These intense and localized field hot-sites can induce intense surface-enhanced Raman scattering (SERS) of molecules residing at the junction hot-sites. In this paper, we present a series of electromagnetic simulations, experimental SERS and extinction data obtained from small self-assembled Au NP clusters coated to saturation with a Raman reporter molecule. Our experimental data show that the SERS enhancement factor remains relatively constant despite the heterogeneity of the nanocluster and this is supported by the simulation results. Furthermore, our simulation results show significant variations in the localized electric field intensities of the junction hot-sites in different nanocluster geometries. This explains the observation that increasing the number of hot-sites does not necessarily result in a higher SERS enhancement factor.

An inkjet-printed paper-based Surface-enhanced Raman scattering (SERS) sensor is a robust and versatile device that provides trace sensing capabilities for the detection and analysis of narcotics and drugs. Such sensors generally work well for analytes with good binding affinity towards the Au or Ag plasmonic nanoparticles (NPs) resident in the sensors. In this report, we show that iodide functionalization of the printed sensors helps to remove adsorbed contaminants from AuNP surfaces enabling superior performance with improved detection of narcotics such as fentanyl, heroin and cocaine by SERS. SERS signals are easily doubled with the iodide-functionalized sensors which also showed orders of magnitude improvement in detection limit. In this report, we show that a short (90 s) iodide treatment of the sensors significantly improved the detection of heroin. We propose that iodide functionalization be integrated into field detection kits through the solvent that wets paper-based sensor prior to swabbing for narcotics. Alternatively, we have also demonstrated that iodide functionalized sensors can be stored in ambient for up to 1 week and retain the improved performance towards heroin detection. This report will help to significantly improve the performance of paper-based sensors for field detection of narcotic drugs.