Aaro I. Väkeväinen

Plasmonic Surface Lattice Resonances at the Strong Coupling Regime

We show strong coupling involving three different types of resonances in plasmonic nanoarrays: surface lattice resonances (SLRs), localized surface plasmon resonances on single nanoparticles, and excitations of organic dye molecules. The measured transmission spectra show splittings that depend on the molecule concentration. The results are analyzed using finite-difference time-domain simulations, a coupled-dipole approximation, coupled-modes models, and Fano theory. The delocalized nature of the collective SLR modes suggests that in the strong coupling regime molecules near distant nanoparticles are coherently coupled.

Lasing in dark and bright modes of a finite-sized plasmonic lattice

Lasing at the nanometre scale promises strong light-matter interactions and ultrafast operation. Plasmonic resonances supported by metallic nanoparticles have extremely small mode volumes and high field enhancements, making them an ideal platform for studying nanoscale lasing. At visible frequencies, however, the applicability of plasmon resonances is limited due to strong ohmic and radiative losses. Intriguingly, plasmonic nanoparticle arrays support non-radiative dark modes that offer longer life-times but are inaccessible to far-field radiation. Here, we show lasing both in dark and bright modes of an array of silver nanoparticles combined with optically pumped dye molecules. Linewidths of 0.2 nm at visible wavelengths and room temperature are observed. Access to the dark modes is provided by a coherent out-coupling mechanism based on the finite size of the array. The results open a route to utilize all modes of plasmonic lattices, also the high-Q ones, for studies of strong light-matter interactions, condensation and photon fluids.

Controlling quantum dot emission by plasmonic nanoarrays.

Metallic nanoparticle arrays support localized surface plasmon resonances (LSPRs) and propagating surface lattice resonances (SLRs). We study the control of quantum dot (QD) emission coupled to the optical modes of silver nanoparticle arrays, both experimentally and numerically. With a hybrid lithography-functionalization method, the QDs are deposited in the vicinity of the nanoparticles. Directionality and enhancement of the emission are observed in photoluminescence spectra and fluorescence lifetime measurements, respectively. Similar features are also demonstrated in the numerical simulations. The tunable emission of this type of hybrid structures could lead to potential applications in light sources.

Surface plasmon polariton-controlled tunable quantum-dot emission

The unique properties of surface plasmon polaritons, such as strong field confinement and local field enhancement effects, make them ideal candidates to enhance and shape the emission of luminescent nanoparticles. Of these nanoparticles, quantum dots are highly versatile, suitable for vastly different applications due to their size and material tunability. In many cases however, the emission wavelength of the quantum dots is fixed after manufacturing, allowing no control over the in situ emission properties. Here, we show fully optical, in situ tunability of the emission wavelength of quantum dots, with shifts of over 30 nm, employing surface plasmon polaritons to control the emission wavelength.

Bose–Einstein condensation in a plasmonic lattice

Bose–Einstein condensation is a remarkable manifestation of quantum statistics and macroscopic quantum coherence. Superconductivity and superfluidity have their origin in Bose–Einstein condensation. Ultracold quantum gases have provided condensates close to the original ideas of Bose and Einstein, while condensation of polaritons and magnons has introduced novel concepts of non-equilibrium condensation. Here, we demonstrate a Bose–Einstein condensate of surface plasmon polaritons in lattice modes of a metal nanoparticle array. Interaction of the nanoscale-confined surface plasmons with a room-temperature bath of dye molecules enables thermalization and condensation in picoseconds. The ultrafast thermalization and condensation dynamics are revealed by an experiment that exploits thermalization under propagation and the open-cavity character of the system. A crossover from a Bose–Einstein condensate to usual lasing is realized by tailoring the band structure. This new condensate of surface plasmon lattice excitations has promise for future technologies due to its ultrafast, room-temperature and on-chip nature.Surface plasmon polaritons in an array of metallic nanoparticles evolve quickly into the band minimum by interacting with a molecule bath, forming a Bose–Einstein condensate at room temperature within picoseconds.

Ultrafast Pulse Generation in an Organic Nanoparticle-Array Laser

Nanoscale coherent light sources offer potentially ultrafast modulation speeds, which could be utilized for novel sensors and optical switches. Plasmonic periodic structures combined with organic gain materials have emerged as promising candidates for such nanolasers. Their plasmonic component provides high intensity and ultrafast nanoscale-confined electric fields, while organic gain materials offer fabrication flexibility and a low acquisition cost. Despite reports on lasing in plasmonic arrays, lasing dynamics in these structures have not been experimentally studied yet. Here we demonstrate, for the first time, an organic dye nanoparticle-array laser with more than a 100 GHz modulation bandwidth. We show that the lasing modulation speed can be tuned by the array parameters. Accelerated dynamics is observed for plasmonic lasing modes at the blue side of the dye emission.

Strong Coupling Between Organic Molecules and Plasmonic Nanostructures

This chapter introduces the theory behind strong coupling of plasmonic modes, such as surface plasmon polaritons, with electronic transitions that are typical for quantum emitters, such as dye molecules and quantum dots. A brief historical overview of the experimental endeavor of measuring such strong coupling is provided, after which we look more carefully at the dynamics in such systems. We proceed with a more in-depth discussion of strong coupling between emitters and delocalized plasmonic modes, called surface lattice resonances, but not before devoting some space to the ideas and theory behind surface lattice resonances for the readers who might not be familiar with the topic. We end the chapter with an outlook on the potential strong coupling has for new and exciting fundamental phenomena and applications of light on the nanoscale.

Vacuum Rabi splitting for surface plasmon polaritons and Rhodamine 6G molecules

We report on strong coupling between surface-plasmon polaritons and Rhodamine 6G molecules at room temperature. As a reference to compare with, we first determine the dispersion curve of (uncoupled) surface plasmon polaritons on a 50 nm thick film of silver. Consequently, we determine the dispersion curve of surface plasmon polaritons strongly coupled to Rhodamine 6G molecules, which exhibits vacuum Rabi splitting. Depending on the Rhodamine 6G concentration, we find splitting energies between 0.05 eV and 0.13 eV.

From vacuum Rabi splitting towards stimulated emission with surface plasmon polaritons

We report on strong coupling between surface plasmon polaritons and Rhodamine 6G molecules at room temperature. As a reference to compare with, we first determine the dispersion curve of (uncoupled) surface plasmon polaritons on a 50 nm thick film of silver. Consequently, we determine the dispersion curve of surface plasmon polaritons strongly coupled to Rhodamine 6G molecules, which exhibits vacuum Rabi splitting. Furthermore, we present spontaneous emission spectra of Rhodamine 6G on silver, which are shown to change with detector angle due to surface plasmon polariton generation by Rhodamine 6G molecules.

Strong light-matter interactions in plasmonic lattices

We show strong coupling involving three different types of resonances in plasmonic nanoarrays: surface lattice resonances, localized surface plasmon resonances on single nanoparticles, and excitations of organic dye molecules. We study spatial coherence properties of a plasmonic nanoarray covered with a dye molecule film by a double slit experiment. A continuous evolution of coherence from the weak to the strong coupling regime is observed. Finally, we show with magnetic nanoparticles how the intrinsic spin-orbit coupling of the material interplays with the symmetries of the nanoparticle array, and mention our latest results on light-matter interactions in plasmonic lattices.