Publications/Patents

Résumé: High refractive index dielectric nanoantennas strongly modify the decay rate via the Purcell effect through the design of radiative channels. Due to their dielectric nature, the field is mainly confined inside the nanostructure and in the gap, which is hard to probe with scanning probe techniques. Here we use single-molecule fluorescence lifetime imaging microscopy (smFLIM) to map the decay rate enhancement in dielectric GaP nanoantenna dimers with a median localization precision of 14 nm. We measure, in the gap of the nanoantenna, decay rates that are almost 30 times larger than on a glass substrate. By comparing experimental results with numerical simulations we show that this large enhancement is essentially radiative, contrary to the case of plasmonic nanoantennas, and therefore has great potential for applications such as quantum optics and biosensing.

Résumé: The strong light−matter coupling, occurring when the light−matter interaction prevails on the damping, has found applications beyond the domain of optics in chemistry or transport. These advances make the development of various structures in strong coupling crucial. In this paper, a new way to hybridize two materials and transfer energy through a surface plasmon over micrometric distances is proposed. For this purpose, two patterned interlocked dye arrays, one donor and one acceptor, are deposited on a silver surface by successive micro-contact printing, leading to a pattern of 5 microns period. The dispersion relation of the structure is measured with reflectometry experiments, showing the hybridization with the plasmon, and the formation of states that mix both excitons and the plasmon with similar weights. The mixing in these polaritonic metasurfaces enables an energy transfer mechanism in the strong coupling, which is observed with luminescence experiments. As the donor and acceptor are spatially separated by a distance larger than the diffraction limit the excitation transfer is directly measured and evaluated by comparison with dye arrays without silver.

Résumé: Probing light-matter interaction at the nanometer scale is one of the most fascinating topics of modern optics. Its importance is underlined by the large span of fields in which such accurate knowledge of light-matter interaction is needed, namely nanophotonics, quantum electrodynamics, atomic physics, biosensing, quantum computing and many more. Increasing innovations in the field of microscopy in the last decade have pushed the ability of observing such phenomena across multiple length scales, from micrometers to nanometers. In bioimaging, the advent of super-resolution single-molecule localization microscopy (SMLM) has opened a completely new perspective for the study and understanding of molecular mechanisms, with unprecedented resolution, which take place inside the cell. Since then, the field of SMLM has been continuously improving, shifting from an initial drive for pushing technological limitations to the acquisition of new knowledge. Interestingly, such developments have become also of great interest for the study of light-matter interaction in nanostructured materials, either dielectric, metallic, or hybrid metallic-dielectric. The purpose of this review is to summarize the recent advances in the field of nanophotonics that have leveraged SMLM, and conversely to show how some concepts commonly used in nanophotonics can benefit the development of new microscopy techniques for biophysics. To this aim, we will first introduce the basic concepts of SMLM and the observables that can be measured. Then, we will link them with their corresponding physical quantities of interest in biophysics and nanophotonics and we will describe state-of-the-art experiments that apply SMLM to nanophotonics. The problem of localization artifacts due to the interaction of the fluorescent emitter with a resonant medium and possible solutions will be also discussed. Then, we will show how the interaction of fluorescent emitters with plasmonic structures can be successfully employed in biology for cell profiling and membrane organization studies. We present an outlook on emerging research directions enabled by the synergy of localization microscopy and nanophotonics.

Résumé: The electromagnetic modes of a sub-wavelength sized antenna can be excited by thermal fluctuations. This thermal radiation is extremely weak, requiring in general the fabrication of a huge number of identical antennas to be detectable. Here, we will first demonstrate experimentally emission spectrum measurement and superresolved mapping of a single nanoantenna, sub-λ in the infrared spectral domain, based on the detection of its thermal radiation despite an overwhelming background thermal radiation [1]. To achieve a background free detection of the thermal radiation from single or a few sub-λ sized resonators, we have developed an infrared spatial modulation spectroscopy (IR-SMS) technique using a lateral modulation of the sample heated at ~150 °C combined with lock-in detection of the infrared signal detected through a Fourier transform infrared spectrometer. We have applied it in combination with thermal radiation scanning tunnelling microscopy [2] to study the thermal radiation from single plasmonic metal-insulator-metal (MIM) antennas both in the near field and in the far field. Our studies performed on single MIMs have revealed the surprising result that when silica is used as insulating material, its strong dispersion in the mid-infrared domain is such that the fundamental spatial mode of the antenna can be thermally excited at various wavelengths. This causes multiple resonances in the thermal radiation spectrum to which correspond the same spatial distribution of near-field thermal radiation [1].

Résumé: The study of hybrid modes in a single dimer of neighboring antennas is an essential step to optimize the far-field electromagnetic (EM) response of large-scale metasurfaces or any complex antenna structure made up of subwavelength building blocks. Here we present far-field infrared spatial modulation spectroscopy (IR-SMS) measurements of a single thermally excited asymmetric dimer of square metal-insulator-metal (MIM) antennas separated by a nanometric gap. Through thermal fluctuations, all the EM modes of the antennas are excited, and hybrid bonding and anti-bonding modes can be observed simultaneously. We study the latter within a plasmon hybridization model, and analyze their effect on the far-field response.

Résumé: Copyright © 2020 American Chemical Society. Single-molecule localization microscopy is a powerful technique with vast potential to study light-matter interactions at the nanoscale. Nanostructured environments can modify the fluorescence emission of single molecules, and the induced decay-rate modification can be retrieved to map the local density of optical states (LDOS). However, the modification of the emitter's point spread function (PSF) can lead to its mislocalization, setting a major limitation to the reliability of this approach. In this paper, we address this by simultaneously mapping the position and decay rate of single molecules and by sorting events by their decay rate and PSF size. With the help of numerical simulations, we are able to infer the dipole orientation and to retrieve the real position of mislocalized emitters. We have applied our approach of single-molecule fluorescence lifetime imaging microscopy (smFLIM) to study the LDOS modification of a silver nanowire over a field of view of ∼ 10 μm2 with a single-molecule localization precision of ∼ 15 nm. This is possible thanks to the combined use of an EMCCD camera and an array of single-photon avalanche diodes, enabling multiplexed and super-resolved fluorescence lifetime imaging.

Résumé: © 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement Measuring the lifetime of fluorescent emitters by time-correlated single photon counting (TCSPC) is a routine procedure in many research areas spanning from nanophotonics to biology. The precision of such measurement depends on the number of detected photons but also on the various sources of noise arising from the measurement process. Using Fisher information theory, we calculate the lower bound on the precision of lifetime estimations for mono-exponential and bi-exponential distributions. We analyse the dependence of the lifetime estimation precision on experimentally relevant parameters, including the contribution of a non-uniform background noise and the instrument response function (IRF) of the setup. We also provide an open-source code to determine the lower bound on the estimation precision for any experimental conditions. Two practical examples illustrate how this tool can be used to reach optimal precision in time-resolved fluorescence microscopy.

Résumé: © 2019 Optical Society of America. Nanophotonics offers a promising range of applications spanning from the development of efficient solar cells to quantum communications and biosensing. However, the ability to efficiently couple fluorescent emitters with nanostructured materials requires one to probe light-matter interactions at a subwavelength resolution, which remains experimentally challenging. Here, we introduce an approach to performsuperresolved fluorescence lifetime measurements on samples that are densely labeled with photo-activatable fluorescent molecules. The simultaneous measurement of the position and the decay rate of the molecules provides direct access to the local density of states (LDOS) at the nanoscale.We experimentally demonstrate the performance of the technique by studying the LDOS variations induced in the near field of a silver nanowire, and we show via a Cramér-Rao analysis that the proposed experimental setup enables a single-molecule localization precision of 6 nm.

Résumé: © 2018 American Physical Society. The far-field spectral and near-field spatial responses of an individual metal-insulator-metal nanoantenna are reported, using thermal fluctuations as an internal source of the electromagnetic field. The far-field spectra, obtained by combining Fourier transform infrared spectroscopy with spatial modulation based on a light falloff effect in a confocal geometry, have revealed two distinct emission peaks attributed to the excitation of the fundamental mode of the nanoantenna at two distinct wavelengths. Superresolved near-field images of the thermally excited mode have been obtained by thermal radiation scanning tunneling microscopy. Experimental results are supported by numerical simulations showing that it is possible to excite the same mode at different wavelengths near a resonance of the insulating dielectric material forming the antenna.

Résumé: © 2018 American Chemical Society. Near-field scanning optical microscopy (NSOM) achieves subwavelength resolution by bringing a nanosized probe close to the surface of the sample. This extends the spectrum of spatial frequencies that can be detected with respect to a diffraction limited microscope. The interaction of the probe with the sample is expected to affect its radiation to the far field in a way that is often hard to predict. Here we address this question by proposing a general method based on full-field off-axis digital holography microscopy which enables to study in detail the far-field radiation from a NSOM probe as a function of its environment. A first application is demonstrated by performing a three-dimensional (3D) tomographic reconstruction of light scattered from the subwavelength aperture tip of a NSOM, in free space or coupled to transparent and plasmonic media. A single holographic image recorded in one shot in the far field contains information on both the amplitude and the phase of the scattered light. This is sufficient to reverse numerically the propagation of the electromagnetic field all the way to the aperture tip. Finite Difference Time Domain (FDTD) simulations are performed to compare the experimental results with a superposition of magnetic and electric dipole radiation.

Résumé: © 2017 American Physical Society.We observe time-correlated emission between a single CdSe/CdS/ZnS quantum dot exhibiting single-photon statistics and a fluorescent nanobead located micrometers apart. This is accomplished by coupling both emitters to a silver nanowire. Single plasmons are created on the latter from the quantum dot, and transfer energy to excite in turn the fluorescent nanobead. We demonstrate that the molecules inside the bead show the same blinking behavior as the quantum dot.

Résumé: © 2015 American Chemical Society. We present a novel method to extract the various contributions to the photonic local density of states from near-field fluorescence maps. The approach is based on the simultaneous mapping of the fluorescence intensity and decay rate and on the rigorous application of the reciprocity theorem. It allows us to separate the contributions of the radiative and the apparent nonradiative local density of states to the change in the decay rate. The apparent nonradiative contribution accounts for losses due to radiation out of the detection solid angle and to absorption in the environment. Data analysis relies on a new analytical calculation, and does not require the use of numerical simulations. One of the most relevant applications of the method is the characterization of nanostructures aimed at maximizing the number of photons emitted in the detection solid angle, which is a crucial issue in modern nanophotonics.

Résumé: We report on the experimental and theoretical study of the spatial fluctuations of the local density of states (EM-LDOS) and of the fluorescence intensity in the near-field of a gold nanoantenna. EM-LDOS, fluorescence intensity and topography maps are acquired simultaneously by scanning a fluorescent nanosource grafted on the tip of an atomic force microscope at the surface of the sample. The results are in good quantitative agreement with numerical simulations. This work paves the way for a full near-field characterization of an optical nanoantenna. © 2013 Optical Society of America.

Résumé: Disordered semi-continuous metallic films are a particularly striking example of complex photonic systems. They exhibit peculiar optical properties that cannot be explained from the behavior of bulk metals or ensembles of isolated nanoparticles [1]. The interplay between surface-plasmon excitations and scattering by multiscale (fractal) metallic clusters leads to spatial localization of the electromagnetic field in subwavelength areas (hot spots). A feature of these hot-spots modes is the expected coexistence of both localized and delocalized modes at the same frequency [2,3], a situation referred to as inhomogeneous localization. © 2011 IEEE.

Résumé: We measure the statistical distribution of the local density of optical states (LDOS) on disordered semicontinuous metal films. We show that LDOS fluctuations exhibit a maximum in a regime where fractal clusters dominate the film surface. These large fluctuations are a signature of surface-plasmon localization on the nanometer scale. © 2010 The American Physical Society.