Real-time observation of ultrafast Rabi oscillations between excitons and plasmons in metal nanostructures with J-aggregates

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Theoretical Criteria for Scattering Dark States in Nanostructured Particles

Nanostructures with multiple resonances can exhibit a suppressed or even completely eliminated scattering of light, called a scattering dark state. We describe this phenomenon with a general treatment of light scattering from a multiresonant nanostructure that is spherical or nonspherical but subwavelength in size. With multiple resonances in the same channel (i.e., same angular momentum and polarization), coherent interference always leads to scattering dark states in the low-absorption limit, regardless of the system details. The coupling between resonances is inevitable and can be interpreted as arising from far-field or near-field. This is a realization of coupled-resonator-induced transparency in the context of light scattering, which is related to but different from Fano resonances. Explicit examples are given to illustrate these concepts.Massachusetts Institute of Technology. Institute for Soldier Nanotechnologies (Contract W911NF-13-D-0001)National Science Foundation (U.S.). Materials Research Science and Engineering Centers (Program) (Grant DMR-0819762

Universal surface-enhanced Raman tags : individual nanorods for measurements from the visible to the infrared (514 – 1064 nm)

Surface-enhanced Raman scattering (SERS) is a promising imaging modality for use in a variety of multiplexed tracking and sensing applications in biological environments. However, the uniform production of SERS nanoparticle tags with high yield and brightness still remains a significant challenge. Here, we describe an approach based on the controlled co-adsorption of multiple dye species onto gold nanorods to create tags that can be detected across a much wider range of excitation wavelengths (514 – 1064 nm) compared to conventional approaches that typically focus on a single wavelength. This was achieved without the added complexity of nanoparticle aggregation or growing surrounding metallic shells to further enhance the surface-enhanced resonance Raman scattering (SERRS) signal. Correlated Raman and scanning electron microscopy mapping measurements of individual tags were used to clearly demonstrate that strong and reproducible SERRS signals at high particle yields (>92 %) were readily achievable. The polyelectrolyte-wrapped nanorod-dye conjugates were also found to be highly stable as well as non-cytotoxic. To demonstrate the use of these universal tags for the multimodal optical imaging of biological specimens, confocal Raman and fluorescence maps of stained immune cells following nanoparticle uptake were acquired at several excitation wavelengths and compared with dark-field images. The ability to colocalize and track individual optically encoded nanoparticles across a wide range of wavelengths simultaneously will enable the use of SERS alongside other imaging techniques for the real-time monitoring of cell-nanoparticle interactions

Shaping Photoluminescence Spectra with Magnetoelectric Resonances in All-Dielectric Nanoparticles

We measure the near-infrared photoluminescence spectra of colloidal quantum dots coupled to the localized electric and magnetic resonances of subwavelength silicon nanodisks. The spectral position of the resonances with respect to each other is controlled via the nanodisk geometry. We observe a strong influence of the nanodisk resonance positions on the quantum dot photoluminescence spectra. For separate resonances, the spectral density observed in transmittance measurements correlates with the spectral range covered by a broad emission spectrum. For the case of spectral overlap of the electric and magnetic dipolar resonances we enter a new regime for coupling, where the characteristic transparency effect evident in the transmittance spectra is accompanied by a pronounced single emission maximum. Our experimental observations are in good qualitative agreement with numerical calculations

Plasmonic Interactions: From Molecular Plasmonics and Fano Resonances to Ferroplasmons

Plasmon interactions are a subject of great interest from both the technological as well as the fundamental points of view. In this Perspective, we outline the great variety of physical phenomena that are produced by the interactions of localized surface plasmon resonance with molecular excitons; with other plasmonic nanostructures, particularly the Fano effect; and with nonplasmonic nanoparticles, such as the just-reported interaction with ferromagnetic nanoparticles. The theoretical as well as experimental challenges remaining to be elucidated are discussed.Fil: Passarelli, Nicolás. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Pérez, Luis Alberto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Coronado, Eduardo A.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentin

Plasmon-Exciton Interactions in a Core-Shell Geometry: From Enhanced Absorption to Strong Coupling

We present a detailed Mie theory, finite-difference time-domain, and quasi-static study of plasmon-exciton interactions in a spherical core shell geometry. In particular, we report absorption, scattering, and extinction cross sections of a hybrid core-shell system and identify several important interaction regimes that are determined by the electromagnetic field enhancement and the oscillator strength of electronic excitations. We assign these regimes to enhanced-absorption, exciton-induced transparency and strong coupling, depending on the nature of the observed spectra of the coupled plasmon-exciton resonances. We also show the relevance of performing single-particle absorption or extinction measurements in addition to scattering to validate the interaction regime. Furthermore, at relatively high, yet realistic oscillator strengths we observe emergence of a third mode, which is not predicted by a classical coupled harmonic oscillator model and is attributed to the geometrical resonance of the structure as a whole

Tuning the optical coupling between molecular dyes and metal nanoparticles by the templated silica mineralization of J-aggregates

cited By 9International audienceSupramolecular porphyrin aggregates are used as a template for the higher-order assembly of fluorophore–dielectric–metal hybrid nanostructures in which the optical properties of the molecules are modulated by the finely tuned coupling to localized plasmons. First, J-aggregates are encapsulated inside a dielectric silica shell of well-controlled thickness, which reinforces mechanically the template and serves as a precise optical coupling spacer. The silicified J-aggregates are then decorated with gold or silver nanoparticles. UV–visible and fluorescence spectroscopies show that the presence of metal nanoparticles induces a marked enhancement of the J-aggregate fluorescence when the silica thickness is tuned to 7–12 nm, whereas a significant quenching is measured when the dielectric thickness is sub-2 nm. Interestingly, the enhancement is maximized when oxidized silver nanoparticles are placed very close to the J-aggregates