Nanoscale mapping of optically inaccessible bound-states-in-the-continuum

Bound-states-in-the-continuum (BIC) is an emerging concept in nanophotonics with potential impact in applications, such as hyperspectral imaging, mirror-less lasing, and nonlinear harmonic generation. As true BIC modes are non-radiative, they cannot be excited by using propagating light to investigate their optical characteristics. In this paper, for the 1st time, we map out the strong near-field localization of the true BIC resonance on arrays of silicon nanoantennas, via electron energy loss spectroscopy with a sub-1-nm electron beam. By systematically breaking the designed antenna symmetry, emissive quasi-BIC resonances become visible. This gives a unique experimental tool to determine the coherent interaction length, which we show to require at least six neighboring antenna elements. More importantly, we demonstrate that quasi-BIC resonances are able to enhance localized light emission via the Purcell effect by at least 60 times, as compared to unpatterned silicon. This work is expected to enable practical applications of designed, ultra-compact BIC antennas such as for the controlled, localized excitation of quantum emitter

Spectroscopies nanometriques de structures plasmoniques et de nanocristaux semi-conducteurs

For this thesis, I have realised some experimental works using electron microscopy and electron spectroscopies for the study of plasmonic nanostructures and semiconductor nanocrystals . The aim being to study their optical properties with spatial resolutions of the order of a few nm. At this level it is possible to observe the electric near-field associated to the localised surface plasmon resonances supported by metallic nanostructures . So I was able to study the effect due to the presence of roughness on single gold nanorods and I have found that their presence locally alterate the structure of the electric near-field . Combined measurement of electron energy loss spectroscopy (EELS ) and cathodoluminescence spectroscopy were used to compare the near-field and far-field responses respectively. A study by EELS on the coupling between two metal nanorods positioned end to end and separated by a disance of tens of nanometers was used to map the localisation of hybridised modes separately on each branch of the dimers. Finally, comparative studies of cathodoluminescence and photoluminescence on single quantum dots have shown the equivalence of the information collected by these two techniques for such light emittersJ'ai réalisé pour cette thèse des travaux expérimentaux à l'aide de la microscopie et de la spectroscopie électronique portant sur l'étude de nanostructures plasmoniques et de nanocristaux semi-conducteurs. Le but étant d'etudier leurs propriétés optiques sur des dimensions spatiales de l'ordre du nm. A cette échelle il est possible d'observer le champs proche électrique associé aux modes de résonances plasmons de surface supportées par des nanostructures métalliques. Ainsi j'ai pu étudier l'effet de la présence de rugosités sur des nano-bâtonnets d'or et constater que leur présence modifiait localement la structure du champs proche électrique. Des mesures combinées par spectroscopie de perte d'énergie des électrons (EELS) et de cathodoluminescence ont permis de comparer les réponses mesurées en champs proches à celle effectuées en champs lointain. Une étude faite par EELS portant sur le couplage entre deux nano-bâtonnets métalliques positionnés bout à bout et séparés par une distance de quelques dizaines de nanomètres a permis de cartographier la localisation de modes hybridés séparément sur chaque branche. Enfin des études comparatives de cathodoluminescence et de photoluminescence sur des points quantiques isolés ont permis de constater l'équivalence de l'information collectées par ces deux techniques sur ce type d'émetteurs de lumièr

Couplage métal-émetteur dans des plasmophores : effet de la distance

International audienc

Distance-dependent fluorescence in metal-dye core-shell systems

International audienc

Etudes EELS de nanoantennes métalliques lithographiées

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High-Resolution Imaging and Spectroscopy of Multipolar Plasmonic Resonances in Aluminum Nanoantennas

International audienceWe report on the high resolution imaging of multipolar plasmonic resonances in aluminum nanoantennas using electron energy loss spectroscopy (EELS). Plasmonic resonances ranging from near-infrared to ultraviolet (UV) are measured. The spatial distributions of the multipolar resonant modes are mapped and their energy dispersion is retrieved. The losses in the aluminum antennas are studied through the full width at half-maximum of the resonances, unveiling the weight of both interband and radiative damping mechanisms of the different multipolar resonances. In the blue-UV spectral range, high order resonant modes present a quality factor up to 8, two times higher than low order resonant modes at the same energy. This study demonstrates that near-infrared to ultraviolet tunable multipolar plasmonic resonances in aluminum nanoantennas with relatively high quality factors can be engineered. Aluminum nanoantennas are thus an appealing alternative to gold or silver ones in the visible and can be efficiently used for UV plasmonics

Nanooptical study of lithographied plasmonic nanoantennas

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Nanooptical study of structural imperfections of lithographed plasmonic antennas

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Cathodoluminescence in a Scanning Transmission Electron Microscope: A Nanometer-Scale Counterpart of Photoluminescence for the Study of II–VI Quantum Dots

International audienceWe report on nanometer-scale cathodoluminescence (nanoCL) experiments in a scanning transmission electron microscope on individual core–shell CdSe/CdS quantum dots (QDs). By performing combined photoluminescence (PL) and nanoCL experiments of the same individual QDs, we first show that both spectroscopies can be used equally well to probe the spectral properties of QDs. We then demonstrate that the spatial resolution of the nanoCL is only limited by the size of the QDs themselves by performing nanoCL experiments on QDs lying side by side. Finally, we show how nanoCL can be advantageous with respect to PL as it can rapidly and efficiently characterize the optical properties of a large set of individual QDs. These results contrast with pioneering CL works on II–VI QDs and pave the way to the characterization of any II–VI quantum-confined structure at the relevant scale