Dual-Modal Nanoplasmonic Light Upconversion through Anti-Stokes Photoluminescence and Second-Harmonic Generation from Broadband Multiresonant Metal Nanocavities.

Metal nanocavities can generate plasmon-enhanced light upconversion signals under ultrashort pulse excitations through anti-Stokes photoluminescence (ASPL) or nonlinear harmonic generation processes, offering various applications in bioimaging, sensing, interfacial science, nanothermometry, and integrated photonics. However, achieving broadband multiresonant enhancement of both ASPL and harmonic generation processes within the same metal nanocavities remains challenging, impeding applications based on dual-modal or wavelength-multiplexed operations. Here, we report a combined experimental and theoretical study on dual-modal plasmon-enhanced light upconversion through both ASPL and second-harmonic generation (SHG) from broadband multiresonant metal nanocavities in two-tier Ag/SiO/Ag nanolaminate plasmonic crystals (NLPCs) that can support multiple hybridized plasmons with high spatial mode overlaps.

Plasmonic Electronic Raman Scattering as Internal Standard for Spatial and Temporal Calibration in Quantitative Surface-Enhanced Raman Spectroscopy.

Ultrasensitive surface-enhanced Raman spectroscopy (SERS) still faces difficulties in quantitative analysis because of its susceptibility to local optical field variations at plasmonic hotspots in metallo-dielectric nanostructures. Current SERS calibration approaches using Raman tags have inherent limitations due to spatial occupation competition with analyte molecules, spectral interference with analyte Raman peaks, and photodegradation. Herein, we report that plasmon-enhanced electronic Raman scattering (ERS) signals from metal can serve as an internal standard for spatial and temporal calibration of molecular Raman scattering (MRS) signals from analyte molecules at the same hotspots, enabling rigorous quantitative SERS analysis.

Sub-10 nm Nanolaminated AlO/HfO Coatings for Long-Term Stability of Cu Plasmonic Nanodisks in Physiological Environments.

By supporting localized plasmon modes, metal-based plasmonic nanostructures can confine optical fields at deep-subwavelength scale in various applications, such as biological and chemical sensing, nanoscale light emission, and solar energy harvesting. While Cu is a low-cost complementary metal oxide semiconductor (CMOS) compatible material, its poor chemical stability limits the use of Cu plasmonic nanodevices in corrosive biochemical aqueous environments. In this paper, we demonstrate that sub-10 nm AlO/HfO nanolaminated coatings can significantly extend the lifetime of Cu nanodisk arrays from ∼5 h to ∼180 days in the physiological environment of 1× phosphate-buffered saline (PBS) at 37 °C.

Refractive-Index-Insensitive Nanolaminated SERS Substrates for Label-Free Raman Profiling and Classification of Living Cancer Cells.

Surface-enhanced Raman spectroscopy (SERS) has emerged as an ultrasensitive molecular-fingerprint-based technique for label-free biochemical analysis of biological systems. However, for conventional SERS substrates, SERS enhancement factors (EFs) strongly depend on background refractive index (RI), which prevents reliable spatiotemporal SERS analysis of living cells consisting of different extra-/intracellular organelles with a heterogeneous distribution of local RI values between 1.30 and 1.