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Bosonic condensates offer exciting prospects for studies of non-equilibrium quantum dynamics. Understanding the dynamics is particularly challenging in the sub-picosecond timescales typical for room temperature luminous driven-dissipative condensates. Here we combine a lattice of plasmonic nanoparticles with dye molecule solution at the strong coupling regime, and pump the molecules optically. The emitted light reveals three distinct regimes: one-dimensional lasing, incomplete stimulated thermalization, and two-dimensional multimode condensation. The condensate is achieved by matching the thermalization rate with the lattice size and occurs only for pump pulse durations below a critical value. Our results give access to control and monitoring of thermalization processes and condensate formation at sub-picosecond timescale., Comment: Revised version

openaire: EC/H2020/745115/EU//OPLD 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.

openaire: EC/H2020/745115/EU//OPLD 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.

Metal nanoparticle arrays that support surface lattice resonances have emerged as an exciting platform for manipulating light-matter interactions at the nanoscale and enabling a diverse range of applications. Their recent prominence can be attributed to a combination of desirable photonic and plasmonic attributes: high electromagnetic field enhancements extended over large volumes with long-lived lifetimes. This Review will describe the design rules for achieving high-quality optical responses from metal nanoparticle arrays, nanofabrication advances that have enabled their production, and the theory that inspired their experimental realization. Rich fundamental insights will focus on weak and strong coupling with molecular excitons, as well as semiconductor excitons and the lattice resonances. Applications related to nanoscale lasing, solid-state lighting, and optical devices will be discussed. Finally, prospects and future open questions will be described.

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 nanometers 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., Comment: Accepted for publication in Nature Communications

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.

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.