Xavier Vidal

Amplified stimulated emission in upconversion nanoparticles for super-resolution nanoscopy

Lanthanide-doped glasses and crystals are attractive for laser applications because the metastable energy levels of the trivalent lanthanide ions facilitate the establishment of population inversion and amplified stimulated emission at relatively low pump power. At the nanometre scale, lanthanide-doped upconversion nanoparticles (UCNPs) can now be made with precisely controlled phase, dimension and doping level. When excited in the near-infrared, these UCNPs emit stable, bright visible luminescence at a variety of selectable wavelengths, with single-nanoparticle sensitivity, which makes them suitable for advanced luminescence microscopy applications. Here we show that UCNPs doped with high concentrations of thulium ions (Tm3+), excited at a wavelength of 980 nanometres, can readily establish a population inversion on their intermediate metastable 3H4 level: the reduced inter-emitter distance at high Tm3+ doping concentration leads to intense cross-relaxation, inducing a photon-avalanche-like effect that rapidly populates the metastable 3H4 level, resulting in population inversion relative to the 3H6 ground level within a single nanoparticle. As a result, illumination by a laser at 808 nanometres, matching the upconversion band of the 3H4 → 3H6 transition, can trigger amplified stimulated emission to discharge the 3H4 intermediate level, so that the upconversion pathway to generate blue luminescence can be optically inhibited. We harness these properties to realize low-power super-resolution stimulated emission depletion (STED) microscopy and achieve nanometre-scale optical resolution (nanoscopy), imaging single UCNPs; the resolution is 28 nanometres, that is, 1/36th of the wavelength. These engineered nanocrystals offer saturation intensity two orders of magnitude lower than those of fluorescent probes currently employed in stimulated emission depletion microscopy, suggesting a new way of alleviating the square-root law that typically limits the resolution that can be practically achieved by such techniques.

Subwavelength direct laser patterning of conductive gold nanostructures by simultaneous photopolymerization and photoreduction.

This article presents a new method for fabricating highly conductive gold nanostructures within a polymeric matrix with subwavelength resolution. The nanostructures are directly written in a gold precursor-doped photoresist using a femtosecond pulsed laser. The laser energy is absorbed by a two-photon dye, which induces simultaneous reduction of gold in the precursor and polymerization of the negative photoresist. This results in gold nanoparticle-doped polymeric lines that exhibit both plasmonic effects, due to the constituent gold nanoparticles, and relatively high conductivity (within an order of magnitude of the bulk metal), due to the high density of particles within these lines. Line widths from 150 to 1000 nm have been achieved with this method. Various optically functional structures have been prepared, and their structural and optical properties have been characterized. The influence of laser intensity and scan speed on feature size have been studied and found to be in agreement with predictions of a mathematical model of the process.

Electromagnetic Duality Symmetry and Helicity Conservation for the Macroscopic Maxwell’s Equations

In this Letter, we show that the electromagnetic duality symmetry, broken in the microscopic Maxwells equations by the presence of charges, can be restored for the macroscopic Maxwells equations. The restoration of this symmetry is shown to be independent of the geometry of the problem. These results provide a tool for the study of light-matter interactions within the framework of symmetries and conservation laws. We illustrate its use by determining the helicity content of the natural modes of structures possessing spatial inversion symmetries and by elucidating the root causes for some surprising effects in the scattering off magnetic spheres.

Two‐Photon Lithography of Sub‐Wavelength Metallic Structures in a Polymer Matrix

Interest in femtosecond-pulsed laser-induced two-photon lithography (TPL) has grown dramatically in recent years, especially for applications that require fabrication of three-dimensional microstructures with subwavelenth resolution. [ 1 , 2 ] Conventional lithographic techniques are not well suited for this, as they are inherently limited to two-dimensional processing. [ 1 , 3 , 4 ] However, three-dimensional TPL using photopolymers overcomes these limitations [ 1 , 5 ] and has found broad application in micro/ nanofl uidics, biotechnology and photonics, particularly optical data storage and photonic crystal structures. [ 5–9 ] Most TPL applications involve fabrication of non-metallic structures, and only recently has progress been reported on TPL-based fabrication of metallic microand nanostructures. [ 10–14 ] While research in this fi eld is in an embryonic state, interest is growing rapidly because of its substantial potential impact. Specifi cally, the ability to write three-dimensional metallic structures in a polymeric matrix holds potential for disruptive advances in emerging fi elds such as nanophotonics, fl exible electronics, metamaterials and plasmonics. [ 15–19 ]

Duality symmetry and Kerker conditions

We unveil the relationship between two anomalous scattering processes known as Kerker conditions and the duality symmetry of Maxwell equations. We generalize these conditions and show that they can be applied to any particle with cylindrical symmetry, not only to spherical particles as the original Kerker conditions were derived for. We also explain the role of the optical helicity in these scattering processes. Our results find applications in the field of metamaterials, where new materials with directional scattering are being explored.

Angular momentum-induced circular dichroism in non-chiral nanostructures

Circular dichroism, that is, the differential absorption of a system to left and right circularly polarized light, is one of the only techniques capable of providing morphological information of certain samples. In biology, for instance, circular dichroism spectroscopy is widely used to study the structure of proteins. More recently, it has also been used to characterize metamaterials and plasmonic structures. Typically, circular dichorism can only be observed in chiral objects. Here we present experimental results showing that a non-chiral sample such as a subwavelength circular nanoaperture can produce giant circular dichroism when a vortex beam is used to excite it. These measurements can be understood by studying the symmetries of the sample and the total angular momentum that vortex beams carry. Our results show that circular dichroism can provide a wealth of information about the sample when combined with the control of the total angular momentum of the input field.

Excitation of single multipolar modes with engineered cylindrically symmetric fields

We present a new method to address multipolar resonances and to control the scattered field of a spherical scatterer. This method is based on the engineering of the multipolar content of the incident beam. We propose experimentally feasible techniques to generate light beams which contain only a few multipolar modes. The technique uses incident beams with a well defined component of the angular momentum and appropriate focusing with aplanatic lenses. The control of the multipolar content of light beams allow for the excitation of single Mie resonances and unprecedented control of the scattered field from spherical particles.

Dual and anti-dual modes in dielectric spheres

We present how the angular momentum of light can play an important role to induce a dual or anti-dual behaviour on a dielectric particle. Although the material the particle is made of is not dual, i.e. a dielectric does not interact with an electrical field in the same way as it does with a magnetic one, a spherical particle can behave as a dual system when the correct excitation beam is chosen. We study the conditions under which this dual or anti-dual behaviour can be induced.

Necessary symmetry conditions for the rotation of light

Two conditions on symmetries are identified as necessary for a linear scattering system to be able to rotate the linear polarization of light: Lack of at least one mirror plane of symmetry and electromagnetic duality symmetry. Duality symmetry is equivalent to the conservation of the helicity of light in the same way that rotational symmetry is equivalent to the conservation of angular momentum. When the system is a solution of a single species of particles, the lack of at least one mirror plane of symmetry leads to the familiar requirement of chirality of the individual particle. With respect to helicity preservation, according to the analytical and numerical evidence presented in this paper, the solution preserves helicity if and only if the individual particle itself preserves helicity. However, only in the particular case of forward scattering the helicity preservation condition on the particle is relaxed: We show that the random orientation of the molecules endows the solution with an effective rotational symmetry; at its turn, this leads to helicity preservation in the forward scattering direction independently of any property of the particle. This is not the case for a general scattering direction. These results advance the current understanding of the phenomena of molecular optical activity and provide insight for the design of polarization control devices at the nanoscale.

Optical second-harmonic scattering from a non-diffusive random distribution of nonlinear domains.

We show that the weak second harmonic light generated from a random distribution of nonlinear domains of transparent Strontium Barium Niobate crystals can display a particularly intense generation in the forward direction. By using a theoretical model able to analyze the optical response of arbitrary distributions of three-dimensional nonlinear volumes of any shape, we found that the physical origin of this observation can be explained in terms of the scattering of light by a single nonlinear domain.