Mikolaj K. Schmidt

Dielectric antennas--a suitable platform for controlling magnetic dipolar emission.

Plasmonic nanoparticles are commonly used to tune and direct the radiation from electric dipolar emitters. Less progress has been made towards understanding complementary systems of magnetic nature. However, it has been recently shown that high-index dielectric spheres can act as effective magnetic antennas. Here we explore the concept of coupling dielectric magnetic antennas with either an electric or magnetic dipolar emitter in a similar fashion to the purely electric systems reported previously. We investigate the enhancement of radiation from systems comprising admixtures of these electric and magnetic elements and perform a full study of its dependence on the distance and polarization of the emitter with respect to the antenna. A comparison to the plasmon antennas reveals remarkable symmetries between electric and magnetic systems, which might lead to novel paradigms in the design of nanophotonic devices that involve magnetic activity.

Single-molecule optomechanics in “picocavities”

A cool route to nanospectroscopy Confining light to a cavity is often used to enhance the interaction between the light and a particle stored within the cavity. Benz et al. worked with a self-assembled monolayer of biphenyl-4-thiol molecules sandwiched between a gold film and a gold nanoparticle. They used laser irradiation to move atoms in the nanoparticle and produced a “picocavity” that was stable at cryogenic temperatures. The authors were then able to obtain time-dependent Raman spectra from individual molecules. Such subwavelength cavities that can localize light to volumes well below 1 nm3 will enable optical experiments on the atomic scale. Science, this issue p. 726 Strongly subwavelength optical cavities can be used to spectroscopically probe single molecules. Trapping light with noble metal nanostructures overcomes the diffraction limit and can confine light to volumes typically on the order of 30 cubic nanometers. We found that individual atomic features inside the gap of a plasmonic nanoassembly can localize light to volumes well below 1 cubic nanometer (“picocavities”), enabling optical experiments on the atomic scale. These atomic features are dynamically formed and disassembled by laser irradiation. Although unstable at room temperature, picocavities can be stabilized at cryogenic temperatures, allowing single atomic cavities to be probed for many minutes. Unlike traditional optomechanical resonators, such extreme optical confinement yields a factor of 106 enhancement of optomechanical coupling between the picocavity field and vibrations of individual molecular bonds. This work sets the basis for developing nanoscale nonlinear quantum optics on the single-molecule level.

Rabi Splitting in Photoluminescence Spectra of Hybrid Systems of Gold Nanorods and J-Aggregates

We experimentally and theoretically investigate the interactions between localized plasmons in gold nanorods and excitons in J-aggregates under ambient conditions. Thanks to our sample preparation procedure we are able to track a clear anticrossing behavior of the hybridized modes not only in the extinction but also in the photoluminescence (PL) spectra of this hybrid system. Notably, while previous studies often found the PL signal to be dominated by a single mode (emission from so-called lower polariton branch), here we follow the evolution of the two PL peaks as the plasmon energy is detuned from the excitonic resonance. Both the extinction and PL results are in good agreement with the theoretical predictions obtained for a model that assumes two interacting modes with a ratio between the coupling strength and the plasmonic losses close to 0.4, indicative of the strong coupling regime with a significant Rabi splitting estimated to be ∼200 meV. The evolution of the PL line shape as the plasmon is detuned depends on the illumination wavelength, which we attribute to an incoherent excitation given by decay processes in either the metallic rods or the J-aggregates.

Quantum Mechanical Description of Raman Scattering from Molecules in Plasmonic Cavities

Plasmon-enhanced Raman scattering can push single-molecule vibrational spectroscopy beyond a regime addressable by classical electrodynamics. We employ a quantum electrodynamics (QED) description of the coherent interaction of plasmons and molecular vibrations that reveal the emergence of nonlinearities in the inelastic response of the system. For realistic situations, we predict the onset of phonon-stimulated Raman scattering and a counterintuitive dependence of the anti-Stokes emission on the frequency of excitation. We further show that this QED framework opens a venue to analyze the correlations of photons emitted from a plasmonic cavity.

Antenna resonances in low aspect ratio semiconductor nanowires

We present numerical simulations of low aspect ratio gallium phosphide nanowires under plane wave illumination, which reveal the interplay between transverse and longitudinal antenna-like resonances. A comparison to the limiting case of the semiconducting sphere shows a gradual, continuous transition of resonant electric and magnetic spherical Mie modes into Fabry-Pérot cavity modes with mixed electric and magnetic characteristics. As the length of the nanowires further increases, these finite-wire modes converge towards the leaky-mode resonances of an infinite cylindrical wire. Furthermore, we report a large and selective enhancement or suppression of electric and magnetic field in structures comprising two semiconducting nanowires. For an interparticle separation of 20 nm, we observe up to 300-fold enhancement in the electric field intensity and an almost complete quenching of the magnetic field in specific mode configurations. Angle-dependent extinction spectra highlight the importance of symmetry and phase matching in the excitation of cavity modes and show the limited validity of the infinite wire approximation for describing the response of finite length nanowires toward glancing angles.

Control of single emitter radiation by polarization- and position-dependent activation of dark antenna modes.

We study the modification of the decay rates of a single dipolar emitter positioned in the vicinity of metallic linear nanoantennas when higher-order plasmonic excitations are induced. We show that it is possible to effectively tune the enhancement or suppression of both the radiative and nonradiative decay processes by controlling the position and orientation of the dipole with respect to the antenna. Transverse polarization of a single emitter, with respect to the antenna axis, located at the center of the antenna activates dark antenna modes that modify dramatically both the intensity and the spectral features of the decay rates.

Anisotropic Nanoantenna-Based Magnetoplasmonic Crystals for Highly Enhanced and Tunable Magneto-Optical Activity

We present a novel concept of a magnetically tunable plasmonic crystal based on the excitation of Fano lattice surface modes in periodic arrays of magnetic and optically anisotropic nanoantennas. We show how coherent diffractive far-field coupling between elliptical nickel nanoantennas is governed by the two in-plane, orthogonal and spectrally detuned plasmonic responses of the individual building block, one directly induced by the incident radiation and the other induced by the application of an external magnetic field. The consequent excitation of magnetic field-induced Fano lattice surface modes leads to highly tunable and amplified magneto-optical effects as compared to a continuous film or metasurfaces made of disordered noninteracting magnetoplasmonic anisotropic nanoantennas. The concepts presented here can be exploited to design novel magnetoplasmonic sensors based on coupled localized plasmonic resonances, and nanoscale metamaterials for precise control and magnetically driven tunability of light polarization states.

Polarization control of metal-enhanced fluorescence in hybrid assemblies of photosynthetic complexes and gold nanorods

Fluorescence imaging of hybrid nanostructures composed of a bacterial light-harvesting complex LH2 and Au nanorods with controlled coupling strength is employed to study the spectral dependence of the plasmon-induced fluorescence enhancement. Perfect matching of the plasmon resonances in the nanorods with the absorption bands of the LH2 complexes facilitates a direct comparison of the enhancement factors for longitudinal and transverse plasmon frequencies of the nanorods. We find that the fluorescence enhancement due to excitation of longitudinal resonance can be up to five-fold stronger than for the transverse one. We attribute this result, which is important for designing plasmonic functional systems, to a very different distribution of the enhancement of the electric field due to the excitation of the two characteristic plasmon modes in nanorods.

Theoretical studies of excitation dynamics in a peridinin-chlorophyll-protein coupled to a metallic nanoparticle

In this work we study the influence of plasmon excitations on the excitation dynamics within a protein complex embedding two chlorophyll molecules coupled to a gold nanosphere. Small separation between the chlorophylls and metallic nanoparticle allows us to simplify the calculations of the Förster energy transfer rate and non-radiative processes by replacing a spherical nanoparticle with a metallic surface. Our results show modifications of all relevant processes and the energy transfer pathways within the system as well as the radiative processes. Plasmon induced changes result in strong qualitative effects of the fluorescence of the studied light-harvesting complex.

Spectral Selectivity of Plasmonic Interactions between Individual Up-Converting Nanocrystals and Spherical Gold Nanoparticles

We experimentally demonstrate strong spectral selectivity of plasmonic interaction that occurs between α-NaYF4:Er3+/Yb3+ nanocrystals, which feature two emission bands, and spherical gold nanoparticles, with plasmon frequency resonant with one of the emission bands. Spatially–resolved luminescence intensity maps acquired for individual nanocrystals, together with microsecond luminescence lifetime images, show two qualitatively different effects that result from the coupling between plasmon excitations in metallic nanoparticles and emitting states of the nanocrystals. On the one hand, we observe nanocrystals, whose emission intensity is strongly enhanced for both resonant and non-resonant bands with respect to the plasmon resonance. Importantly, this increase is accompanied with shortening of luminescence decays times. In contrast, a significant number of nanocrystals exhibits almost complete quenching of the emission resonant with the plasmon resonance of gold nanoparticles. Theoretical analysis indicates that such an effect can occur for emitters placed at distances of about 5 nm from gold nanoparticles. While under these conditions, both transitions experience significant increases of the radiative emission rates due to the Purcell effect, the non-radiative energy transfer between resonant bands results in strong quenching, which in that situation nullifies the enhancement.