0000000000054424
AUTHOR
Christian Girard
Generalized bloch equations for optical interactions in confined geometries
By combining the field-susceptibility technique with the optical Bloch equations, a general formalism is developed for the investigation of molecular photophysical phenomena triggered by nanometer scale optical fields in the presence of complex environments. This formalism illustrate the influence of the illumination regime on the fluorescence signal emitted by a single molecule in a complex environment. In the saturated case, this signal is proportional to the optical local density of states, while it is proportional to the near-field intensity in the non-saturated case. (C) 2005 Elsevier B.V. All rights reserved.
Relationship between scanning near-field optical images and local density of photonic states
From numerical calculations based on Green's dyadic formalism, we show that a scanning near-field optical microscope (SNOM) working with a point-like illuminating probe delivers images that contain features directly related to the local density of photonic states (LDOS). More precisely, an unambiguous identification of the partial LDOSs (x, y or z polarized) can be made in the SNOM images when the solid angle of detection reaches 2π sr.
Molecular quenching and relaxation in a plasmonic tunable system
Molecular fluorescence decay is significantly modified when the emitting molecule is located near a plasmonic structure. When the lateral sizes of such structures are reduced to nanometer-scale cross sections, they can be used to accurately control and amplify the emission rate. In this Rapid Communication, we extend Green's dyadic method to quantitatively investigate both radiative and nonradiative decay channels experienced by a single fluorescent molecule confined in an adjustable dielectric-metal nanogap. The technique produces data in excellent agreement with current experimental work.
Electrodynamics in complex systems
This paper discusses recent theoretical efforts to develop a general and flexible method for the calculation of the field distributions around and inside complex optical systems involving both dielectric and metallic materials. Starting from the usual light-matter coupling Hamiltonian, we derive a self-consistent equation for the optical field in arbitrary optical systems composed of N different subdomains. We show that an appropriate solving procedure based on the real-space discretization of each subdomain raises the present approach to the rank of an accurate predictive numerical scheme. In order to illustrate its applicability, we use this formalism to address challenging problems relat…
Scanning optical microscopy modeling in nanoplasmonics
International audience; One of the main purposes of nanoplasmonics is the miniaturization of optical and electro-optical components that could be integrable in coplanar geometry. In this context, we propose a numerical model of a polarized scanning optical microscope able to faithfully reproduce both photon luminescence and temperature distribution images associated with complex plasmonic structures. The images are computed, pixel by pixel, through a complete self-consistent scheme based on the Green dyadic functions (GDF) formalism. The basic principle consists in the numerical implementation of a realistic three-dimensional light beam acting as a virtual light tip able to probe the volume…
Plasmon polaritons of metallic nanowires for controlling submicron propagation of light
Laboratoire de Physique, Optique Submicronique, Universite´de Bourgogne, BP 47870, F-21078 Dijon, France~Received 29 April 1999!We use the Green dyadic technique to study the propagation of a local excitation along metallic nanowiresof a subwavelength cross section. The metallic nanowires are elongated parallelepipeds deposited on a trans-parent substrate. A tightly focused plane wave illuminates one end of the nanowires. The localized surface-plasmon resonances of the nanowires propagate the local excitations over distances larger than the incidentwavelength. The properties of the electromagnetic eigenmodes of the nanowires are analyzed in terms of thelocal density of states. @S0163-1829~9…
Squeezing the Optical Near-Field Zone by Plasmon Coupling of Metallic Nanoparticles
We report on the experimental observation of near-field optical effects close to Au nanoparticles using a photon scanning tunneling microscope (PSTM). Constant height operation of the PSTM allowed an unprecedented direct comparison with theoretical computations of the distribution of the optical near-field intensity. An unexpected squeezing of the optical near field due to plasmon coupling was observed above a chain of Au nanoparticles.
Photon antibunching in the optical near field
International audience; We show that a combination of the field-susceptibility technique with the optical Bloch equations gives access to the temporal evolution of the populations and coherences of any quantum system placed in the optical near field of a nanostructure. In particular, we show that the near-field evanescent states, confined around dielectric or plasmonic particles, can be used to modify and control the photon statistics of the quantum system. This theoretical scheme leads to second-order autocorrelation functions in good agreement with recent experimental measurements performed with nitrogen-vacancy center in diamond nanocrystals placed in interaction with gold nanoparticles.
Field propagator of a dressed junction: Fluorescence lifetime calculations in a confined geometry
The study of the fluorescence phenomenon by near-field optical techniques requires one to describe precisely the spontaneous emission change occurring when the fluorescing particle is placed in a complex optical environment. For this purpose, the field susceptibility (also called the field propagator) of a planar junction formed by a cavity bounded by two semi-infinite bodies with arbitrary optical constant is derived within the framework of linear-response theory. The field propagator associated with the junction is then modified in a self-consistent manner to account for the presence of any arbitrary object inside the junction. As a first illustration the alteration of the fluorescence li…
Atomic diffraction from nanostructured optical potentials
We develop a versatile theoretical approach to the study of cold-atom diffractive scattering from light-field gratings by combining calculations of the optical near-field, generated by evanescent waves close to the surface of periodic nanostructured arrays, together with advanced atom wavepacket propagation on this optical potential.
Detection of the optical magnetic field by circular symmetry plasmons
We report on the influence of coating a sharpened optical fiber tip with Au when observing nanofabricated dielectric structures with a Photon Scanning Tunneling Microscope (PSTM) in constant-height mode. For well-defined incident wavelengths and coating thicknesses, we found that such tips detect the distribution of the magnetic field associated with the optical wave in the near-field zone. A simple tip model indicates that this phenomenon is related to the excitation of circular symmetry plasmons in Au coated tips.
Physical interaction between tip and molecules in scanning force microscopy imaging of adsorbed C 60 and fullerene tubules
International audience
Near-field optics theories
The development of near-field optics theory is reviewed. We first recall that near-field optics is not limited to near-field microscopy. Broadly speaking, it concerns phenomena involving evanescent electromagnetic waves. The importance of such waves was ignored for a long time in optical and surface physics until the emergence of scanning near-field optical microscopes. Taking evanescent waves into account prevents the use of any simple approximation in the set of Maxwell's equations. The various theoretical approaches of near-field optics are discussed from the point of view of their ability to assess evanescent electromagnetic waves. We discuss the main results of the application of the v…
Near-field properties of plasmonic nanostructures with high aspect ratio
International audience; Using the Green's dyad technique based on cuboidal meshing, we compute the electromagnetic field scattered by metal nanorods with high aspect ratio. We investigate the effect of the meshing shape on the numerical simulations. We observe that discretizing the object with cells with aspect ratios similar to the object's aspect ratio improves the computations, without degrading the convergency. We also compare our numerical simulations to finite element method and discuss further possible improvements.
Dielectric versus topographic contrast in near-field microscopy
Using a fully vectorial three-dimensional numerical approach (generalized field propagator, based on Green's tensor technique), we investigate the near-field images produced by subwavelength objects buried in a dielectric surface. We study the influence of the object index, size, and depth on the near field. We emphasize the similarity between the near field spawned by an object buried in the surface (dielectric contrast) and that spawned by a protrusion on the surface (topographic contrast). We show that a buried object with a negative dielectric contrast (i.e., with a smaller index than its surrounding medium) produces a near-field image that is reversed from that of an object with a posi…
Theory of Near‐field Optical Imaging with a Single Molecule as Light Source
Scanning near-field optical microscopes (SNOM) illuminate a sample in the very near-field using a nanometer sized tip. Ideally, the light source should be point-like and many efforts have been made to optimize tip efficiency (see, for example, the article of Heimel et al in this issue). Very recently, Sandoghdar et al have realized a molecular probe tip in which a terrylene molecule inserted in a paraterphenyl microcrystal is attached at the extremity of the probe tip [1]. The excited molecule behaves as a point-like light source which is raster scanned over an aluminium patterned structure. We propose here an analysis of this experiment based on the field-susceptibility formalism (also cal…
Near-field characterization of Bragg mirrors engraved in surface plasmon waveguides
International audience; 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 …
Tailoring the transmittance of integrated optical waveguides with short metallic nanoparticle chains
We study the ability of noble metal nanoparticle chains supporting localized surface plasmons to tailor the transmittance of channel waveguides on which they are deposited. The optical interaction between a microwaveguide ~MWG! and various arrangements of nanoparticles is first analyzed by means numerical calculations based on the Green’s tensor formalism. For specific geometries of the particle chains, the transmission spectra of the composite device ~MWG and nanoparticles! exhibits strong modulations in the optical range with the appearance of a neat band gap. The results of an experiment inspired by this theoretical study are also discussed. The photon scanning tunneling microscope image…
Manipulating and squeezing the photon local density of states with plasmonic nanoparticle networks
International audience; In this Brief Report, we show that when interconnected networks of gold particles are deposited onto a clean planar surface, they strongly modify the photonic local density of states LDOS in the immediate proximity of the self-assembled nanoparticles. They represent unique architectures for the subwavelength patterning of initially flat photonic LDOS. Moreover, we show that their local spectral signatures are well suited for the generation of sites able to enhance molecular fluorescence intensity.
Local detection of the optical magnetic field in the near zone of dielectric samples
International audience; We present a study of the influence of the probe composition on the formation of constant-height photon scanning tunneling microscope images when observing a dielectric sample. Dramatic effects due to the metallization of the tip are presented and discussed in detail. We show how the recorded images can look quite different when the probe is dielectric or coated with gold. Comparison with numerical calculations indicate that the experimental signals are of electric or magnetic nature depending on the composition of the tip. For well-defined conditions, gold-coated tips provide images of the distribution of the magnetic field intensity associated with the optical near…
Resonant optical tunnel effect through dielectric structures of subwavelength cross sections.
We show that optical tunnel effects through elongated structures of subwavelength cross sections can be enhanced by the appropriate structuration of the local dielectric function. Even under total internal reflection, transfer channels can be excited to perform spatially confined photonic transfer between transparent media linked by such subwavelength structures. The optical properties of such systems are analyzed using field susceptibilities, also known as electromagnetic Green's dyadics, which determine both the local density of photon states and the optical transmittance of the system. Green's dyadics obtained by solving numerically a set of dyadic Dyson equations are applied to study th…
Physical interaction between tip and molecules in scanning force microscopy imaging of adsorbed C60 and fullerene tubules
After the discovery of C60, a large family of fullerene molecules was also identified. Among them, elongated fullerenes are formed by the tubular assembly of carbon atoms. The van der Waals bonds between fullerene molecules are due to the correlations between fluctuating charge densities inside the molecules. The interaction is then dominated by collective excitations which are sensitive to the shape of the molecules. Therefore, van der Waals attraction is expected to be modified when considering successively spherical C60, C70 and more elongated fullerenes (tubules). This paper presents self‐consistent computations of the van der Waals interaction between a (111) diamond probe tip and vari…
Strongly directional scattering from dielectric nanowires
It has been experimentally demonstrated only recently that a simultaneous excitation of interfering electric and magnetic resonances can lead to uni-directional scattering of visible light in zero-dimensional dielectric nanoparticles. We show both theoretically and experimentally, that strongly anisotropic scattering also occurs in individual dielectric nanowires. The effect occurs even under either pure transverse electric or pure transverse magnetic polarized normal illumination. This allows for instance to toggle the scattering direction by a simple rotation of the incident polarization. Finally, we demonstrate that directional scattering is not limited to cylindrical cross-sections, but…
Direct interpretation of near-field optical images.
The interpretation of the detection process in near-field optical microscopy is reviewed on the basis of a discussion about the possibility of establishing direct comparisons between experimental images and the solutions of Maxwell equations or the electromagnetic local density of states. On the basis of simple physical arguments, it is expected that the solutions of Maxwell equations should agree with images obtained by collecting mode near-field microscopes, while the electromagnetic local density of states should be considered to provide a practical interpretation of illumination mode near-field microscopes. We review collecting mode near-field microscope images where the conditions to o…
Observation of Light Confinement Effects with a Near-Field Optical Microscope.
This Letter reports the experimental observation of light confinement effects by near-field optical microscopy. Depolarization effects giving rise to light confinement close to nanoscopic objects have been unambiguously observed in near-field optical images of subwavelength dielectric pads etched on a flat glass substrate. According to the incident polarization, this phenomenon leads to reverse contrasts in the near-field optical image of the same subwavelength objects.
Optical analogy to electronic quantum corrals.
We describe full multiple-scattering calculations of localized surface photonic states set up by lithographically designed nanostructures made of a finite number of dielectric pads deposited on a planar surface. The method is based on a numerical solution of the dyadic Dyson's equation. When the pads are arranged to form a closed circle, we find field patterns that look like the electronic charge density recently observed above quantum corrals. We propose two experimental techniques that could be used to observe these electromagnetic modes in direct space.
Near-field coupling of a point-like dipolar source with a thin metallic film: Implication for STM plasmon excitations
International audience; Recent experiments have shown that it is possible to excite surface plasmons on metallic films by injecting tunnel electrons from a sharp metal tip located in the immediate proximity of the sample. When working close to a bare metal film, the excitation of surface plasmons gives rise to typical circular patterns that can be recorded in both image and Fourier planes. Important physical parameters of surface plasmon propagation such as their propagation length can be extracted from these images. In this Letter, we discuss theoretically the physics of the plasmonic excitations induced by a STM tip.
Theoretical principles of near-field optical microscopies and spectroscopies
International audience; This paper deals with the principles of detection of optical signals near a surface in a manner permitting the mapping of the distribution of the fields close to various kinds of illuminated samples. We begin with a discussion of the main physical properties of the optical fields near a surface in the absence of any probe tip. This mainly concerns phenomena involving evanescent waves for which the local decay lengths are governed not only by the sizes but also by the intrinsic properties of the surface structures. The interpretation of the detection process is reviewed on the basis of a discussion about the possibility of establishing direct comparisons between exper…
Near-field optical contrasts in the Fresnel evanescent wave
The surface waves generated by total internal reflection at the surface of a transparent material may be viewed as quasi-two-dimensional, because they decay exponentially in the direction normal to the sample surface. These waves are appropriate to analyze polarization effects associated with light confinement phenomena in near-field optics. In this paper we derive four useful analytical relations governing the near-field contrast around dielectric nanometer-sized particles versus a limited number of external parameters. In the $p$-polarized mode, unlike to what happens with the electric near field, we show that the magnitude of the magnetic near-field contrast can be adjusted by increasing…
Modelling resonant coupling between microring resonators addressed by optical evanescent waves
In this paper we study the properties of microring resonator structures fabricated with high-index-of-refraction dielectric material. These structures concentrate light and can produce very strong optical potential gradients. They are of great interest for the trapping, manipulation and transport of cold atoms near surfaces. The study consists of two parts: in the first part we investigate the symmetry properties of the resonator response for simple models of the microring structures. In the second part we present detailed numerical calculations of the actual spectra for realistic microfabricated structures. We employ the direct space integral equation method (DSIEM). This method, based on …
Imaging the Local Density of States of Optical Corrals
International audience; This paper reports the experimental observation, at optical frequencies, of the electromagnetic local density of states established by nanostructures corresponding to the recently introduced concept of optical corral [G. Colas des Francs et al., Phys. Rev. Lett. 86, 4950 (2001)]. The images obtained by a scanning near-field optical microscope under specific operational conditions are found in agreement with the theoretical maps of the optical local density of states. A clear functionality of detection by the scanning near-field optical microscope is thereby identified since the theoretical maps are computed without including any specific tip model.
Metal enhanced fluorescence in rare earth doped plasmonic core–shell nanoparticles
International audience; We theoretically and numerically investigate metal enhanced fluorescence of plasmonic core–shell nanoparticles doped with rare earth (RE) ions. Particle shape and size are engineered to maximize the average enhancement factor (AEF) of the overall doped shell. We show that the highest enhancement (11 in the visible and 7 in the near-infrared) is achieved by tuning either the dipolar or the quadrupolar particle resonance to the rare earth ion's excitation wavelength. Additionally, the calculated AEFs are compared to experimental data reported in the literature, obtained in similar conditions (plasmon mediated enhancement) or when a metal–RE energy transfer mechanism is…