Polaritonic chemistry is emerging as a powerful approach to modifying the properties and reactivity of molecules and materials. However, probing how the electronics and dynamics of molecular systems change under strong coupling has been challenging due to the narrow range of spectroscopic techniques that can be applied in situ. Here we develop microfluidic optical cavities for vibrational strong coupling (VSC) that are compatible with nuclear magnetic resonance (NMR) spectroscopy using standard liquid NMR tubes. VSC is shown to influence the equilibrium between two conformations of a molecular balance sensitive to London dispersion forces, revealing an apparent change in the equilibrium constant under VSC. In all compounds studied, VSC does not induce detectable changes in chemical shifts, J-couplings, or spin-lattice relaxation times. This unexpected finding indicates that VSC does not substantially affect molecular electron density distributions, and in turn has profound implications for the possible mechanisms at play in polaritonic chemistry under VSC and suggests that the emergence of collective behavior is critical.

Site-selectivity is fundamental for steering chemical reactivity towards a given product and various efficient chemical methods have been developed for this purpose. Here we explore a very different approach by using vibrational strong coupling (VSC) between a reactant and the vacuum field of a microfluidic optical cavity. For this purpose, the reactivity of a compound bearing two possible silyl bond cleavage sites, at Si-C and Si-O, was studied as a function of VSC of its various vibrational modes in the dark. The results show that VSC can indeed tilt the reactivity landscape to favor one product over the other. Thermodynamic parameters reveal the presence of a large activation barrier and significant changes to the activation entropy, confirming the modified chemical landscape under strong coupling. This study shows for the first time that VSC can impart site-selectivity for chemical reactions without the need for chemical intervention.

Much effort over the past decades has been focused on improving carrier mobility in organic thin-film transistors by optimizing the organization of the material or the device architecture. Here we take a different path to solving this problem, by injecting carriers into states that are hybridized to the vacuum electromagnetic field. To test this idea, organic semiconductors were strongly coupled to plasmonic modes to form coherent states that can extend over as many as 10(5) molecules and should thereby favour conductivity. Experiments show that indeed the current does increase by an order of magnitude at resonance in the coupled state, reflecting mostly a change in field-effect mobility. A theoretical quantum model confirms the delocalization of the wavefunctions of the hybridized states and its effect on the conductivity. Our findings illustrate the potential of engineering the vacuum electromagnetic environment to modify and to improve properties of materials.

We exploit plasmonic and thermo-hydrodynamical forces to sort gold nanoparticles in a microfluidic environment. In the appropriate regime, the experimental data extracted from a Brownian statistical analysis of the kinetic motions are in good agreement with Mie-type theoretical evaluations of the optical forces acting on the nanoparticles in the plasmonic near field. This analysis enables us to demonstrate the importance of thermal and hydrodynamical effects in a sorting perspective.

Photonic crystals (PC) have demonstrated unique features that have renewed the fields of classical and quantum optics. Although holding great promises, associated mechanical effects have proven challenging to observe. We demonstrate for the first time that one of the most salient properties of PC, namely negative refraction, can induce specific forces on metal nanoparticles. By integrating a periodically patterned metal film in a fluidic cell, we show that near-field optical forces associated with negatively refracted surface plasmons are capable of controlling particle trajectories. Coupling particle motions to PC band structures draws new approaches and strategies for parallel and high resolution all-optical control of particle flows with applications for micro- and nanofluidic systems.

We investigate both experimentally and theoretically the far-field diffraction patterns of single circular apertures as a function of their diameters d and at a given illumination wavelength λ. We observe the transition between the well-known pseudoscalar regime of large holes (d≫λ) and the less-known vectorial regime of subwavelength ones (d≪λ). Four different diffraction regimes are identified for different d/λ regions, each one with its polarization dependence. A thorough comparison with a theoretical model, which takes into account both finite hole size and the dielectric properties of the metal, allows us to explain and understand the physical processes leading to this behavior. Our results reveal the subtle interplay between two competing factors, one related to polarization symmetries associated with surface-plasmon excitations and the other originating in the coupling of the field to the waveguide mode of the aperture.

We demonstrate that optical trapping can be driven by delocalized surface plasmon modes resonantly excited within a standing wave trap. Dynamical modifications are shown to be determined by the near-field symmetry of the plasmonic modes with negligible thermal effect. With low trapping powers and polarization control, remarkable stiffness enhancements are recorded, the larger the smaller the particle. The results can be simply modeled accounting for a coherent interaction between the plasmon field and the Gaussian standing wave of the trap.

We generate self-collimating surface plasmon beams in a doubly periodic plasmonic grating. The self-collimation effect is understood from the local anisotropy of the isofrequency surface of the grating in the vicinity of the bandgap. The properties of the beams are analyzed by leakage radiation microscopy and show to an unprecedented level significantly reduced diffraction as compared with plasmon beams propagating on a flat metal film.

The authors report that gold nanoapertures surrounded by periodic corrugations transform standard molecules into bright unidirectional fluorescence sources. The authors obtain enhancement factors of the fluorescence rate per molecule up to 75 fold simultaneously with a directional emission of the fluorescence into a narrow angular cone into a cone of ±15° in the direction normal to the sample plane. The bright emission and narrow directionality enable the detection of single molecules with a low numerical aperture objective, and improve the effectiveness of fluorescence-based applications.

We present numerical and experimental analyses showing the formation of (2+1)D spatial photorefractive solitons at visible wavelengths in electrically biased lithium niobate crystals for ordinary and extraordinary light polarizations. Similarly sized self-trapped beams are observed for both polarizations, despite the polarization-dependent electro-optic coefficients. The tensorial character of the photovoltaic effect is shown to play a key role. The soliton-induced waveguides are able to properly guide telecommunication wavelengths. Finally, a higher degree of anisotropy is observed for ordinary polarized solitons for specific electro-optic configurations, which reveals the presence of the photorefractive field component perpendicular to the applied field. Experimental results are confirmed by a time-dependent numerical model.

Surface plasmon-polaritons have recently attracted renewed interest in the scientific community for their potential in sub-wavelength optics, light generation and non-destructive sensing. Given that they cannot be directly excited by freely propagating light due to their intrinsical binding to the metal surface, the light-plasmon coupling efficiency becomes of crucial importance for the success of any plasmonic device. Here we present a comprehensive study on the modulation (enhancement or suppression) of such coupling efficiency by means of one-dimensional surface corrugation. Our approach is based on simple wave interference and enables us to make quantitative predictions which have been experimentally confirmed at both the near infra-red and telecom ranges.

We discuss the implications of a frequency-dependent complex dielectric function ε ( ω ) of a metal for the interpretation of scanning near-field optical microscopy (SNOM) measurements in the vicinity of metallic nanoapertures. For subwavelength slits in gold films we observe distinct spatial intensity oscillations in the near-field signal for specific wavelengths in the visible spectrum. These oscillations of the SNOM signal far away from the nanoslit are ascribed to a constructive interference between the propagating surface plasmon (SP) with light scattered parallel to the gold–air interface. In these spatial SNOM-signal oscillations information about the surface plasmon dielectric function is encoded which can be extracted, for example, in surface plasmon interferometry for applications as sensors or waveguides.

Channel plasmon polaritons (CPPs) propagating along the bottom of subwavelength grooves cut into a metal surface were recently shown to exhibit strong confinement combined with low propagation loss, a feature that makes this guiding configuration very promising for the realisation of ultracompact photonic components. Here, the results of our investigations of CPP guiding by V-grooves cut into gold are presented, demonstrating efficient large-angle bending and splitting of radiation as well as waveguide-ring resonators and Bragg grating filters. Additionally, we present a simple model based on the effective-index method that accounts for the main features of CPP guiding, thus, providing a clear physical picture of this phenomenon.

The launching of surface plasmons by micro-gratings of subwavelength apertures milled in a thick metal film is important for the development of surface plasmon based circuits. By comparing the near-field optical images of such surface plasmon sources with the results of a Huygens-Fresnel principle based scattering model, we show that the properties of the locally launched SP beams such as divergence or uniformity can be tuned by adjusting the shape of the micro-gratings. This allows us to propose an optimized source array well adapted for providing a narrow, collimated and uniform beam.

The emerging field of plasmonics is based on exploiting the coupling between light and collective electronic excitations within conducting materials known as surface plasmons. Because the so-called surface plasmon polariton (SPP) modes that arise from this coupling are not constrained by the optical diffraction limit, it is hoped that they could enable the construction of ultracompact optical components1,2. But in order that such potential can be realized, it is vital that the relatively poor light–SPP coupling be improved. This is made worse by the fact that the incident light that is conventionally used to launch SPPs in a metal film 3,4,5,6 is a significant source of noise, unless directed away from a region of interest, which then decreases the signal and increases the system's size. Back-side illumination of subwavelength apertures in optically thick metal films7,8,9,10,11,12,13 eliminates this problem but does not ensure a unique propagation direction for the SPP. We propose a novel back-side slit-illumination method that incorporates a periodic array of grooves carved into the front side of a thick metal film. Bragg reflection enhances the propagation of SPPs away from the array, enabling them to be unidirectionally launched from, and focused to, a localized point.

The development of surface plasmon polariton (SPP) optical elements is mandatory in order to achieve surface plasmon based photonics. A current approach to reach this goal is to take advantage of the interaction of SPP with defects and design elements obtained by the micro- or nano-structuration of the metal film. In this work, we have performed a detailed study of the performance and behavior of SPP-Bragg mirrors, designed for 45 degrees incidence, based on this approach. Mirrors consisting of gratings of both metal ridges on the metal surface and grooves engraved in the metal, fabricated by means of electron beam lithography and focused ion beam, have been considered. The performance of the mirrors has been characterized via near-field optical microscopy. An original procedure to obtain quantitative values of the mirrors' reflectivity and transmission coefficient from the near-field images is exposed. The mirrors composed of metal ridges are shown to act very efficiently, and a rather low number of elements (15 for the specific geometry studied) is able to deflect almost 100% of the incoming power. Conversely, the arrays of grooves produce a much lower reflectivity, which we attribute mostly to radiative scattering in the forward direction induced by the grooves. Besides, the considered systems have also been simulated by using the differential method. The results obtained from the numerical calculations present an excellent agreement with the experimental data, proving the reliability of this method to predict the behavior of this kind of systems while interacting with SPP. Based on the numerical modeling of the SPP-Bragg mirrors, the evolution of the mirrors' behavior with the ridges height is analyzed.

We report on realization of channel plasmon-polariton (CPP) propagation along a subwavelength metal groove. Using imaging with a near-field microscope and end-fire coupling with a tapered fiber connected to a tunable laser at telecommunication wavelengths (1425-1620 nm), we demonstrate low-loss (propagation length approximately 100 microm) and well-confined (mode width approximately 1.1 microm) CPP guiding along a triangular 0.6 microm-wide and 1 microm-deep groove in gold. We develop a simple model based on the effective-index method that accounts for the main features of CPP guiding and provides a clear physical picture of this phenomenon.

We present results of the transmitted, reflected, and absorbed power associated with the enhanced transmittance of light through a silver film pierced by a periodic array of subwavelength holes. Comparing experimentally acquired dispersion curves under different polarization conditions shows that the transmission features of the array are consistent with p-polarized resonant modes of the structure. By exploring the regime in which no propagating diffracted orders are allowed, we further show that the transmittance maxima are associated with both reflectance minima and absorption maxima. These new results provide strong experimental evidence for transmission based on diffraction, assisted by the enhanced fields associated with surface plasmon polaritons.

Surface plasmon waveguides (SPW's) are metal ridges featuring widths in the micrometer range and thicknesses of a few tens of nanometers. A focused ion beam has been used to carve microscatterers into gold SPW's and the near-field distributions around these microstructures are observed by means of photon scanning tunneling microscopy (PSTM). On the basis of near-field images, we show that a finite length periodic arrangement of narrow slits can reflect a surface plasmon mode propagating along a SPW. The reflection efficiency of the micrograting is found to depend upon the number of slits, the period of the grating, and the incident wavelength. The optimum reflection efficiency is obtained for a period of the micrograting equal to half the incident wavelength in vacuum. The PSTM images of the plasmon mirrors taken at different wavelengths allow us to measure the experimental dispersion curve of the SPW in the near-infrared. From this dispersion curve, we found that, in analogy with a surface plasmon (SP) excited on extended thin films, the group velocity of a SPW mode is close to the speed of light. For a given frequency in the near-infrared, the effective index of the SP mode supported by a 2.5-mum-wide SPW is also found to be significantly larger than the effective index of an extended thin film SP. Finally, we show that the optical properties of microgratings engraved into a SPW can be qualitatively approached by a standard Bragg mirror model.

In case of metallic hole arrays we need to establish how structures transmit, reflect and absorb light. We fabricated hole arrays using a focused ion beam etching system (FBI DB235). The period of the array was 430/spl plusmn/5 nm, the hole diameter 250/spl plusmn/5 nm and the thickness of the silver 180/spl plusmn/5 nm. We made arrays with relatively large dimensions, 1 mm/sup 2/ so as to make the measurement of the reflectivity possible with existing facilities. We next performed optical measurements to find the transmittance and the reflectivity as a function of incident angle and incident frequency. In this way we are able to build up a map of the dispersion of the surface plasmon (SP) modes associated with the enhanced transmission.