Fluorescence Enhancement in Topologically Optimized Gallium Phosphide All-Dielectric Nanoantennas.

Nanoantennas capable of large fluorescence enhancement with minimal absorption are crucial for future optical technologies from single-photon sources to biosensing. Efficient dielectric nanoantennas have been designed, however, evaluating their performance at the individual emitter level is challenging due to the complexity of combining high-resolution nanofabrication, spectroscopy and nanoscale positioning of the emitter. Here, we study the fluorescence enhancement in infinity-shaped gallium phosphide (GaP) nanoantennas based on a topologically optimized design. Using fluorescence correlation spectroscopy (FCS), we probe the nanoantennas enhancement factor and observe an average of 63-fold fluorescence brightness enhancement with a maximum of 93-fold for dye molecules in nanogaps between 20 and 50 nm. The experimentally determined fluorescence enhancement of the nanoantennas is confirmed by numerical simulations of the local density of optical states (LDOS). Furthermore, we show that beyond design optimization of dielectric nanoantennas, increased performances can be achieved via tailoring of nanoantenna fabrication.

Opto-thermoelectric trapping of fluorescent nanodiamonds on plasmonic nanostructures.

Deterministic optical manipulation of fluorescent nanodiamonds (FNDs) in fluids has emerged as an experimental challenge in multimodal biological imaging. Designing and developing nano-optical trapping strategies to serve this purpose is an important task. In this Letter, we show how chemically prepared gold nanoparticles and silver nanowires can facilitate an opto-thermoelectric force to trap individual entities of FNDs using a long working distance lens, low power-density illumination (532-nm laser, 12 µW/µm2). Our trapping configuration combines the thermoplasmonic fields generated by individual plasmonic nanoparticles and the opto-thermoelectric effect facilitated by the surfactant to realize a nano-optical trap down to a single FND that is 120 nm in diameter. We use the same trapping excitation source to capture the spectral signatures of single FNDs and track their position. By tracking the FND, we observe the differences in the dynamics of the FND around different plasmonic structures. We envisage that our drop-casting platform can be extrapolated to perform targeted, low-power trapping, manipulation, and multimodal imaging of FNDs inside biological systems such as cells.

Ultraviolet Nanophotonics Enables Autofluorescence Correlation Spectroscopy on Label-Free Proteins with a Single Tryptophan.

Using the ultraviolet autofluorescence of tryptophan amino acids offers fascinating perspectives to study single proteins without the drawbacks of fluorescence labeling. However, the low autofluorescence signals have so far limited the UV detection to large proteins containing several tens of tryptophan residues. This limit is not compatible with the vast majority of proteins which contain only a few tryptophans. Here we push the sensitivity of label-free ultraviolet fluorescence correlation spectroscopy (UV-FCS) down to the single tryptophan level. Our results show how the combination of nanophotonic plasmonic antennas, antioxidants, and background reduction techniques can improve the signal-to-background ratio by over an order of magnitude and enable UV-FCS on thermonuclease proteins with a single tryptophan residue. This sensitivity breakthrough unlocks the applicability of UV-FCS technique to a broad library of label-free proteins.

Single Molecule Surface Enhanced Raman Scattering in a Single Gold Nanoparticle-Driven Thermoplasmonic Tweezer.

Surface enhanced Raman scattering (SERS) is optically sensitive and chemically specific to detect single-molecule spectroscopic signatures. Facilitating this capability in optically trapped nanoparticles at low laser power remains a significant challenge. In this letter, we show single molecule SERS signatures in reversible assemblies of trapped plasmonic nanoparticles using a single laser excitation (633 nm). Importantly, this trap is facilitated by the thermoplasmonic field of a single gold nanoparticle dropcasted on a glass surface. We employ the bianalyte SERS technique to ascertain the single molecule statistical signatures and identify the critical parameters of the thermoplasmonic tweezer that provide this sensitivity. Furthermore, we show the utility of this low power (≈ 0.1 mW/µm2) tweezer platform to trap a single gold nanoparticle and transport assembly of nanoparticles. Given that our configuration is based on a dropcasted gold nanoparticle, we envisage its utility to create reconfigurable plasmonic metafluids in physiological and catalytic environments and to be potentially adapted as an in vivo plasmonic tweezer.

Optothermal pulling, trapping, and assembly of colloids using nanowire plasmons.

Optical excitation of colloids can be harnessed to realize soft matter systems that are out of equilibrium. In this paper, we present our experimental studies on the dynamics of silica colloids in the vicinity of a silver nanowire propagating surface plasmon polaritons (SPPs). Due to the optothermal interaction, the colloids are directionally pulled towards the excitation point of the nanowire. Having reached this point, they are spatio-temporally trapped around the excitation location. By increasing the concentration of colloids in the system, we observe multi-particle assembly around the nanowire. This process is thermophoretically driven and assisted by the SPPs. Furthermore, we find such an assembly to be sensitive to the excitation polarization at the input of the nanowire. Numerically-simulated temperature distribution around an illuminated nanowire corroborates sensitivity to the excitation polarization. Our study will find relevance in exploration of SPP-assisted optothermal pulling, trapping and assembly of colloids, and can serve as a test-bed of plasmon-driven active matter.

Beaming Elastic and SERS Emission from Bent-Plasmonic Nanowire on a Mirror Cavity.

We report on the experimental observation of beaming elastic and surface enhanced Raman scattering (SERS) emission from a bent-nanowire on a mirror (B-NWoM) cavity. The system was probed with polarization resolved Fourier plane and energy-momentum imaging to study the spectral and angular signature of the emission wavevectors. The out-coupled elastically scattered light from the kink occupies a narrow angular spread. We used a self-assembled monolayer of molecules with a well-defined molecular orientation to utilize the out-of-plane electric field in the cavity for enhancing Raman emission from the molecules and in achieving beaming SERS emission. Calculated directionality for elastic scattering and SERS emission was found to be 16.2 and 12.5 dB, respectively. The experimental data were corroborated with three-dimensional numerical finite element and finite difference time domain based numerical simulations. The results presented here may find relevance in understanding coupling of emitters with elongated plasmonic cavities and in designing on-chip optical antennas.

Large-scale optothermal assembly of colloids mediated by a gold microplate.

Light-activated colloidal assembly and swarming can act as model systems to explore non-equilibrium state of matter. In this context, creating new experimental platforms to facilitate and control two-dimensional assembly of colloidal crystals are of contemporary interest. In this paper, we present an experimental study of assembly of colloidal silica microparticles in the vicinity of a single-crystalline gold microplate evanescently excited by a 532 nm laser beam. The gold microplate acts as a source of heat and establishes a thermal gradient in the system. The created optothermal potential assembles colloids to form a two-dimensional poly-crystal, and we quantify the coordination number and hexagonal packing order of the assembly in such a driven system. Our experimental investigation shows that for a given particle size, the variation in assembly can be tuned as a function of excitation-polarization and surface to volume ratio of the gold microplates. Furthermore, we observe that the assembly is dependent on size of the particle and its material composition. Specifically, silica colloids assemble but polystyrene colloids do not, indicating an intricate behaviour of the forces under play. Our work highlights a promising direction in utilizing metallic microstructures that can be harnessed for optothermal colloidal crystal assembly and swarming studies. Our experimental system can be utilized to explore optically driven matter and photophoretic interactions in soft-matter including biological systems such as cells and micro organisms.

Doughnut-shaped emission from vertical organic nanowire coupled to thin plasmonic film.

Vertical nanowires facilitate an innovative mechanism to channel the optical field in the orthogonal direction and act as a nanoscale light source. Subwavelength, vertically oriented nanowire platforms, both of plasmonic and semiconducting variety, can facilitate interesting far-field emission profiles and potentially carry orbital angular momentum states. Motivated by these prospects, in this Letter, we show how a hybrid plasmonic-organic platform can be harnessed to engineer far-field radiation. The system that we have employed is an organic nanowire made of diaminoanthroquinone grown on a plasmonic gold film. We experimentally and numerically studied angular distribution of surface plasmon polariton mediated emission from a single, vertical organic nanowire by utilizing evanescent excitation and Fourier plane microscopy. Photoluminescence and elastic scattering from a single nanowire was analyzed individually in terms of inplane momentum states of the outcoupled photons. We found that the emission is doughnut-shaped in both photoluminescence and elastic scattering regimes. We anticipate that the discussed results can be relevant in designing efficient, polariton-mediated nanoscale photon sources that can carry orbital angular momentum states.

Differential Wavevector Distribution of Surface-Enhanced Raman Scattering and Fluorescence in a Film-Coupled Plasmonic Nanowire Cavity.

We report on the experimental observation of differential wavevector distribution of surface-enhanced Raman scattering (SERS) and fluorescence from dye molecules confined to a gap between plasmonic silver nanowire and a thin, gold mirror. The fluorescence was mainly confined to higher values of in-plane wavevectors, whereas SERS signal was uniformly distributed along all the wavevectors. The optical energy-momentum spectra from the distal end of the nanowire revealed strong polarization dependence of this differentiation. All these observations were corroborated by full-wave three-dimensional numerical simulations, which further revealed an interesting connection between out-coupled wavevectors and parameters such as hybridized modes in the gap-plasmon cavity, and orientation and location of molecular dipoles in the geometry. Our results reveal a new prospect of discriminating electronic and vibrational transitions in resonant dye molecules using a subwavelength gap plasmonic cavity in the continuous-wave excitation limit, and can be further harnessed to engineer molecular radiative relaxation processes in momentum space.