Single-molecule surface-enhanced Raman scattering (SM-SERS) is one of the vital applications of plasmonic nanoparticles. The SM-SERS sensitivity critically depends on plasmonic hot-spots created at the vicinity of such nanoparticles. In conventional fluid-phase SM-SERS experiments, plasmonic hot-spots are facilitated by chemical aggregation of nanoparticles. Such aggregation is usually irreversible, and hence, nanoparticles cannot be re-dispersed in the fluid for further use. Here, we show how to combine SM-SERS with plasmon polariton-assisted, reversible assembly of plasmonic nanoparticles at an unstructured metal–fluid interface. One of the unique features of our method is that we use a single evanescent-wave optical excitation for nanoparticle assembly, manipulation and SM-SERS measurements. Furthermore, by utilizing dual excitation of plasmons at metal–fluid interface, we create interacting assemblies of metal nanoparticles, which may be further harnessed in dynamic lithography of dispersed nanostructures. Our work will have implications in realizing optically addressable, plasmofluidic, single-molecule detection platforms. Plasmonic hot-spot generation in solution is not reversible for single-molecule surface-enhanced Raman scattering, which limits its applications. Patra et al.tackle this problem by integrating this technique with thermo-plasmon-assisted reconfiguration of nanoparticles at a metal–fluid interface.

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Plasmofluidic single-molecule surface-enhanced Raman scattering from dynamic assembly of plasmonic nanoparticles

In the last two decades, plasmon resonance in gold nanoparticles (Au NPs) has been the subject of intense research efforts. Plasmon physics is intriguing and its precise modelling proved to be challenging. In fact, plasmons are highly responsive to a multitude of factors, either intrinsic to the Au NPs or from the environment, and recently the need emerged for the correction of standard electromagnetic approaches with quantum effects. Applications related to plasmon absorption and scattering in Au NPs are impressively numerous, ranging from sensing to photothermal effects to cell imaging. Also, plasmon-enhanced phenomena are highly interesting for multiple purposes, including, for instance, Raman spectroscopy of nearby analytes, catalysis, or sunlight energy conversion. In addition, plasmon excitation is involved in a series of advanced physical processes such as non-linear optics, optical trapping, magneto-plasmonics, and optical activity. Here, we provide the general overview of the field and the background for appropriate modelling of the physical phenomena. Then, we report on the current state of the art and most recent applications of plasmon resonance in Au NPs.

Surface plasmon resonance in gold nanoparticles: a review.

Optical Waveguide Theory

Optical trapping and manipulation of micrometre-sized particles was first reported in 1970. Since then, it has been successfully implemented in two size ranges: the subnanometre scale, where light-matter mechanical coupling enables cooling of atoms, ions and molecules, and the micrometre scale, where the momentum transfer resulting from light scattering allows manipulation of microscopic objects such as cells. But it has been difficult to apply these techniques to the intermediate - nanoscale - range that includes structures such as quantum dots, nanowires, nanotubes, graphene and two-dimensional crystals, all of crucial importance for nanomaterials-based applications. Recently, however, several new approaches have been developed and demonstrated for trapping plasmonic nanoparticles, semiconductor nanowires and carbon nanostructures. Here we review the state-of-the-art in optical trapping at the nanoscale, with an emphasis on some of the most promising advances, such as controlled manipulation and assembly of individual and multiple nanostructures, force measurement with femtonewton resolution, and biosensors.

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Optical trapping and manipulation of nanostructures

Wave front shaping, the ability to manipulate light fields both spatially and temporally, in complex media is an emerging field with many applications. This review summarizes how insights from mesoscopic scattering theory have direct relevance for optical wave control experiments and vice versa. The results are expected to have an impact on a number of fields ranging from biomedical imaging to nanophotonics, quantum information, and communication technology.

Light fields in complex media: Mesoscopic scattering meets wave control

The prediction of light propagation up to hundreds of millimetres within straight or even deformed segments of multimode fibres is demonstrated. The concept is applied in an endoscope and exceptional resolution and footprint are obtained.

Seeing through chaos in multimode fibres

We present a generic technique allowing size-based all-optical sorting of gold nanoparticles. Optical forces acting on metallic nanoparticles are substantially enhanced when they are illuminated at a wavelength near the plasmon resonance, as determined by the particle’s geometry. Exploiting these resonances, we realize sorting in a system of two counter-propagating evanescent waves, each at different wavelengths that selectively guide nanoparticles of different sizes in opposite directions. We validate this concept by demonstrating bidirectional sorting of gold nanoparticles of either 150 or 130 nm in diameter from those of 100 nm in diameter within a mixture.

Bidirectional Optical Sorting of Gold Nanoparticles

Achieving intravital optical imaging with diffraction-limited spatial resolution of deep-brain structures represents an important step toward the goal of understanding the mammalian central nervous system1-4. Advances in wavefront-shaping methods and computational power have recently allowed for a novel approach to high-resolution imaging, utilizing deterministic light propagation through optically complex media and, of particular importance for this work, multimode optical fibers (MMFs)5-7. We report a compact and highly optimized approach for minimally invasive in vivo brain imaging applications. The volume of tissue lesion was reduced by more than 100-fold, while preserving diffraction-limited imaging performance utilizing wavefront control of light propagation through a single 50-μm-core MMF. Here, we demonstrated high-resolution fluorescence imaging of subcellular neuronal structures, dendrites and synaptic specializations, in deep-brain regions of living mice, as well as monitored stimulus-driven functional Ca2+ responses. These results represent a major breakthrough in the compromise between high-resolution imaging and tissue damage, heralding new possibilities for deep-brain imaging in vivo.

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Subcellular spatial resolution achieved for deep-brain imaging in vivo using a minimally invasive multimode fiber.

The Maxwell stress tensor method is used to calculate the optical forces acting upon a glass nanosphere in the proximity of optically excited gold nanoantenna structures The dependence of optical forces over a full range of excitation angles is explored: the total internal reflection excitation does not bring any particular advantage to trapping efficiency when compared to the normal incidence excitation Our calculations show multiple trapping sites with similar trapping properties for the normal and the total internal reflection cases, respectively; furthermore, the convective heating probably dominates over any optical forces in such systems

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Optical forces near a nanoantenna

We present a GPU accelerated toolbox for shaping the light propagation through multimode fibre using a spatial light modulator (SLM). The light is modulated before being coupled to the proximal end of the fibre in order to achieve arbitrary light patterns at the distal end of the fibre. First, the toolbox optimises the acquisition time of the transformation matrix of the fibre by synchronous operation of CCD and SLM. Second, it uses the acquired transformation matrix retained within the GPU memory to design, in real-time, the desired holographic mask for on-the-fly modulation of the output light field. We demonstrate the functionality of the toolbox by acquiring the transformation matrix at the maximum refresh rate of the SLM - 204Hz, and using it to display an on-demand oriented cube, at the distal end of the fibre. The user-controlled orientation of the cube and the corresponding holographic mask are obtained in 20ms intervals. Deleterious interference effects between the neighbouring points are eliminated by incorporating an acousto-optic deflector (AOD) into the system. We remark that the usage of the toolbox is not limited to multimode fibres and can be readily used to acquire transformation matrix and implement beam-shaping in any other linear optical system.

Martin Ploschner

Papers

Seeing through chaos in multimode fibres

Bidirectional Optical Sorting of Gold Nanoparticles

Subcellular spatial resolution achieved for deep-brain imaging in vivo using a minimally invasive multimode fiber.

Optical forces near a nanoantenna

GPU accelerated toolbox for real-time beam-shaping in multimode fibres