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Surface-enhanced Raman scattering (SERS) has garnered substantial attention due to its ability to achieve single-molecule sensitivity by utilizing metallic nanostructures to amplify the exceedingly weak Raman scattering process. However, the introduction of metal nanostructures can induce a background continuum which can reduce the ultimate sensitivity of SERS in ways that are not yet well understood. Here, we investigate the impact of laser irradiation on both Raman scattering and backgrounds from self-assembled monolayers within nanoparticle-on-mirror plasmonic nanocavities with variable geometry. We find that laser irradiation can reduce the height of the monolayer by inducing an irreversible change in molecular conformation. The resulting increased plasmon confinement in the nanocavities not only enhances the SERS signal, but also provides momentum conservation in the inelastic light scattering of electrons, contributing to the enhancement of the background continuum. The plasmon confinement can be modified by changing the size and the geometry of nanoparticles, resulting in a nanoparticle geometry-dependent background continuum in SERS. Our work provides new routes for further modifying the geometry of plasmonic nanostructures to improve SERS sensitivity.

Multiple surface lattice resonances generated with nanoparticle arrays are promising to enhance light-matter interactions at different spectral positions simultaneously, and it is important to tailor these resonances to desired frequencies for practical applications such as multi-modal nanolasing. To this end, this study proposes to generate multiple surface lattice resonances using overlapping nanoparticle arrays with different lattice spacing. Both full-wave numerical simulations and analytical coupled dipole approximation calculations reveal that for the overlapping structures composed with two different gold nanosphere arrays, both surface lattice resonances for the element structures are effectively excited. Considering that the optical responses are governed by the dipole-dipole interactions between the nanoparticles, it is interesting to find that the multiple surface lattice resonances are almost invariant by adjusting the relative shifts between the two arrays, which can be useful to tailor the high-quality factor resonances to desired spectral positions. In addition, due to the same reason, it is also shown that the multiple surface lattice resonances can be further finely tuned by selectively removing specific nanoparticles in the array. We anticipate that the tolerance to generate multiple surface lattice resonances and the flexible tunability make the overlapping nanoparticle arrays useful to design high performance linear and nonlinear nanophotonic devices.

Optical microcavities embedded with transition metal dichalcogenide (TMDC) membranes have been demonstrated as excellent platforms to explore strong light-matter interactions. Most of the previous studies focus on strong coupling between excitons of unpatterned TMDC membranes and optical resonances of various microcavities. It is recently found that TMDC membranes patterned into photonic crystal (PhC) slabs can sustain guided-mode resonances that can be excited and probed by far-fields. Here, we present a comprehensive theoretical and numerical study on optical responses of Fabry-Pérot (F-P) cavity-WS 2 PhC hybrid structures to investigate the multi-mode coupling effects between excitons, guided-mode resonances and F-P modes. We show that both the exciton resonance and the guide-mode resonance of the WS 2 PhC can strongly interact with F-P modes of the cavity to reach strong coupling regime. Moreover, a Rabi splitting as large as 63 meV is observed for the strong coupling between the guided-mode resonance and the F-P mode, which is much larger than their average dissipation rate. We further demonstrate that it is even possible to realize a triple mode strong coupling by tuning the guide-mode resonances spectrally overlapped with the exciton resonance and the F-P modes. The hybrid polariton states generated from the triple mode coupling exhibit a Rabi splitting of 120 meV that greatly exceeds the criterion of a triple mode strong coupling (∼29.3 meV). Our results provide that optical microcavities embedded with TMDC PhCs can serve as promising candidates for polariton devices based on multi-mode strong coupling.

The competition mechanism of exciton decay channels in the multilayer TMDs remains poorly understood. Here, the exciton dynamics in the stacked WS 2 was studied. The exciton decay processes are divided into the fast and slow decay processes, which are dominated by the exciton-exciton annihilation (EEA) and defect-assisted recombination (DAR), respectively. The lifetime of EEA is on the order of hundreds of femtoseconds (400∼1100 fs). It is decreased initially, followed by an increase with adding layer thickness, which can be attributed to the competition between phonon-assisted effect and defect effect. The lifetime of DAR is on the timescale of hundreds of picoseconds (200∼800 ps), which is determined by the defect density especially in a high injected carrier density.

In this manuscript, we explored the performance of a hollow thin film array (HTFA) for the detection of HCl vapor based on fluorescence quenching. The HTFA structure was fabricated by manually stacking layers of an active thin film and a supporting film, alternately, with a hollow structure in each supporting film. The total penetration depth of vapor molecules in the HTFA sample is 2n times increased, where n is the layer number of the active thin film. We tested the sensing performance of the HTFA sample using fluorescence emission and laser emission in a Fabry-Pérot (FP) microcavity. In the fluorescence sensing, the sensing efficiency increases with the vapor concentration, and can be as high as 80% with a vapor concentration of 400 ppm. While in the laser sensing, the efficiency can achieve 100% with an external pump intensity three times of the lasing threshold at a vapor concentration of 85 ppm. The HTFA sample is not only suitable for vapor detection but also suitable for molecule detection in liquid.

We conduct DNA high-resolution melting (HRM) analysis using optofluidic lasers based on a Fabry-Pérot microcavity. Compared to the fluorescence-based HRM, the laser-based HRM has advantages of higher emission intensity for better signal-to-noise ratio and sharper transition for better temperature resolution. In addition, the melting temperature can be lowered by optimizing the laser conditions such as external pump and cavity Q-factor. In this work, we first theoretically analyze the laser-based HRM. Then experiments are performed on three long DNA sequences as model systems, one being 99 bases and the other two being 130 bases long but with different GC contents. We show that the laser-based HRM is able to distinguish the target and the single-base mismatched DNA as long as 130 bases and with nearly 50% GC content. The dependence of laser threshold on the temperature for each DNA sample is first experimentally investigated and by optimizing the external pump, the melting temperature is reduced by more than 10 °C, compared to the fluorescence-based HRM for long DNA sequences up to 130 bases. Finally, we demonstrate an alternative method of using the laser-based HRM for rapid DNA screening that does not exist for the fluorescence-based HRM, in which laser excitation is scanned at a fixed temperature to distinguish the target and the base-mismatched DNA sequences. It is shown that the 130-bases-long DNA with nearly 50% GC content can have as much as 20% difference in the laser threshold and 40% difference in the laser output slope between the target and the single-base mismatched sequences, despite only 0.5 °C difference in their melting temperature, indicating that the laser-excitation-scanning method can also be suitable for long DNA sequences with higher GC content.

The enhancement of biosensing sensitivity based on a quantum dot (QD) is limited by the long distance between the QD and the substrate in in vitro detection, which prevents the development of biosensors. Here an individual sharp convex gold groove is proposed to enhance remote fluorescence by exciting and collecting fluorescence efficiently. The structure shows a higher emission power than other wider gold groove structures when the QD is individually placed at five random positions inside the groove. Compared with bare glass, the total power enhancement factor of our structure is up to 17.0 times, 6.6 times and 6.4 times when the QD is 3.5 μm, 7.6 μm and 9.0 μm away from the bottom of the groove, respectively, due to the scattered emission of the QD and guided resonance modes inside the groove. In addition, the structure is easy to fabricate. The individual sharp convex gold groove is expected to be used as one unit of multi-channels in micro/nano fluidic biosensing. The sample volume could be very small or large according to real applications due to the particular geometric features of our structure.

We report the development of an optofluidic laser array fabricated on a chip using stable plano-concave Fabry-Pérot (FP) microcavities, which are far less susceptible to optical misalignment during device assembly than the commonly used plano-plano FP microcavities. The concave mirrors in our FP microcavities were created by first generating an array of microwells of a few micrometers in depth and a few tens of micrometers in diameter on a fused silica chip using a CO2 laser, followed by coating of distributed Bragg reflection (DBR) layers. The plano-concave FP microcavity had a Q-factor of 5.6 × 10(5) and finesse of 4 × 10(3), over 100 times higher than those for the FP microcavities in existing optofluidic lasers. 1 mM R6G dye in ethanol was used to test the plano-concave FP microcavities, showing an ultralow lasing threshold of only 90 nJ mm(-2), over 10 times lower than that in the corresponding unstable plano-plano FP microcavities formed by the same DBR coatings on the same chip. Simultaneous laser emission from the optofluidic laser array on the chip and single-mode lasing operation were also demonstrated. Our work will lead to the development of optofluidic laser-based biochemical sensors and novel on-chip photonic devices with extremely low lasing thresholds (nJ mm(-2)) and mode volumes (fL).

We show a hybrid structure consisting of Si film with photonic crystal surface and random triangular gold grooves reflector at the bottom, which is capable of realizing efficient, broad-band, wide-angle optical absorption. It is numerically demonstrated that the enhanced absorption in a broad wavelength range (0.3-9.9 μm) due to the scattering effect of both sides of the structure and the created resonance modes. Larger thickness and period are favored to enhance the absorption in broader wavelength range. Substantial electric field concentrates in the grooves of surface photonic crystal and in the Si film. Our structure is versatile for solar cells, broadband photodetection and stealth coating.

We theoretically and numerically investigate the quadratic cascading effect of third-harmonic (TH) generation in a locally quasi-periodic nonlinear photonic structure. We study the effect of structure parameters on the acceptance bandwidth and conversion efficiency of the cascading process. We demonstrate that the conversion efficiency of the cascading process can be enhanced by using a longer locally quasi-periodic nonlinear photonic crystal, without adversely affecting the acceptance bandwidth of the emitted radiation.

Using density functional theory and the non-equilibrium Green's function technique, we performed theoretical investigations on the magnetic and quantum transport properties of benzene-vanadium-borazine mixed organic/inorganic ligand sandwich clusters. The calculated results show that these finite sandwich clusters coupled to Ni electrodes exhibit novel quantum transport properties such as half-metallicity, negative differential resistance and spin-reversal effect, and can be viewed as a new kind of spin filter. However, for the infinite molecular wire, the ground state was identified as a ferromagnetic semiconductor with high stability. These findings suggest that the mixed organic/inorganic ligand sandwich clusters and molecular wires are promising materials for application in molecular electronics and spintronics.