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.

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.

We study spatial coherence properties of a system composed of periodic silver nanoparticle arrays covered with a fluorescent organic molecule (DiD) film. The evolution of spatial coherence of this composite structure from the weak to the strong coupling regime is investigated by systematically varying the coupling strength between the localized DiD excitons and the collective, delocalized modes of the nanoparticle array known as surface lattice resonances. A gradual evolution of coherence from the weak to the strong coupling regime is observed, with the strong coupling features clearly visible in interference fringes. A high degree of spatial coherence is demonstrated in the strong coupling regime, even when the mode is very excitonlike (80 %), in contrast to the purely localized nature of molecular excitons. We show that coherence appears in proportion to the weight of the plasmonic component of the mode throughout the weak-to-strong coupling crossover, providing evidence for the hybrid nature of the normal modes.

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 have introduced novel concepts of non-equilibrium condensation. Here, we demonstrate a Bose-Einstein condensate (BEC) 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 BEC 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.Bosonic quantum statistics imply that below a certain critical temperature or above a critical density the occupation of excited states is strictly limited, and consequently, a macroscopic population of bosons accumulates on the ground state 1 . This phenomenon is known as Bose-Einstein condensation (BEC). Superconductivity of metals and high-temperature superconducting materials are understood as BEC of Cooper pairs 2, 3 . The BEC phenomenon is central in superfluidity of helium although the condensate constitutes a small fraction of the particles 4 . Textbook Bose-Einstein condensates with large condensate fractions and weak interactions were created with ultracold alkali atoms 5-7 , and the fundamental connection between the superfluidity of Cooper pairs and the Bose-Einstein condensation was confirmed by experiments with ultracold Fermi gases 3 . While all these condensates allow essentially equilibrium description, as was the original one by Bose and Einstein, the phenomenology has expanded to non-equilibrium systems [8][9][10][11][12] . Hybrid particles of semiconductor excitons and cavity photons, called exciton-polaritons, have shown condensation and interaction effects [13][14][15][16][17][18][19] , creating coherent light output that deviates from usual laser light. Magnons, that is, spin-wave excitations in magnetic materials 20, 21 , and photons in microcavities 22, 23 form condensates as well. The most technologically groundbreaking manifestation of macroscopic population due to bosonic statistics has so far been laser light, which is a highly non-equilibrium state not thermalized to a temperature of any reservoir. As the BEC phenomenon has been observed only in a limited number of systems, new ones are needed for pushing the time, temperature and spatial scales where a BEC can exist, as well as for opening viable routes to technological applications of BEC.Here we report the observation of BEC for bosonic quasip...

Nanocelluloses with native crystalline internal structures have attracted considerable interest due to their plant-based origin, high mechanical properties, modifiability, and chiral liquid crystallinity, which suggest novel functional sustainable materials. [1−27] In particular, cellulose nanocrystals (CNCs) are colloidal rods, having a typical lateral dimension of 5−10 nm and length of 50−300 nm. Above a critical aqueous concentration, they exhibit lefthanded chiral nematic (cholesteric) liquid crystallinity (LC) and optical iridescence, [4][5][6] which is preserved in dried films [4,28] . It allows templating for photonic materials using inorganics, nanoparticles, polymers, and pyrolyzed carbonized matter. [10,12,16,25,26] On the other hand, the CNCs have been suggested to possess a right-handed twist along their nanorod axis to explain the left-handed twist in their chiral LC. [6] Recently, the right-handed twist of individual CNCs and nanocelluloses of three different origins was observed by cryo-electron tomography (cryo-ET), and electron and atomic force microscopy [27,29] supported by molecular dynamics simulations [30−32] .Exploiting the twisting shape along the individual CNC nanorods could allow new optical functions in the nano/colloidal scale in dilute aqueous dispersions, i.e. not limited to the chiral LC based on the inter-rod assembly involving a larger length scale. Surprisingly, such optical findings have not been reported so far.Surface plasmons, i.e. collective oscillations of the conduction electrons on metal surfaces, allow physics and applications ranging from photonic devices, sensing, and solar cells to pharmacology. [33−37] In nanoparticles (NPs) the oscillations become coupled to allow a chiral plasmonic response, provided that they are sufficiently closely positioned and assembled in a chiral manner. This manifests in circular dichroism (CD) spectroscopy, which describes the difference in absorption between left-and right-handed circularly polarized light. The chiral coupling of surface plasmons induces a bisignated CD signal with a zerocrossing at the characteristic localized surface plasmon resonance wavelength of the isolated NPs. Such a Cotton effect is either dip−peak or peak−dip, depending on the handedness of chirality. [38−42] In chiral biological molecules, such as DNA, proteins and polypeptides, the CD signal is at ultraviolet wavelengths, whereas the CD signal of helical metal nanoparticle assemblies is at the visible wavelengths. This extends the applications to e.g. in biosensing. [37] Chiral nanoparticle assemblies have been shown using helical polymers, supramolecular fibers, and DNA-based constructs as templates. [40−42] In particular, a chiral plasmonic signal is obtained using DNA-origami to organize the nanoparticles in well-defined helices with tunable pitch, separation, and handedness. [40,41] Even if the above approaches are promising allowing in-depth tunable chiral plasmonic response, introducing rapid, scalable, and economic ways for producing chiral plas...