Multicolour light sources can be used in applications such as lighting and multiplexing signals. In photonic and plasmonic systems, one way to achieve multicolour light is via multi-mode lasing. To achieve this, plasmonic nanoparticle arrays are typically arranged in superlattices that lead to multiple dispersions of the single arrays coupled via the superlattice Bragg modes. Here, we show an alternative way to enable multi-mode lasing in plasmonic nanoparticle arrays. We design a supercell in a square lattice by leaving part of the lattice sites empty. This results in multiple dispersive branches caused by the supercell period and hence creates additional band edges that can support lasing. We experimentally demonstrate multi-mode lasing in such a supercell array. Furthermore, we identify the lasing modes by calculating the dispersion by combining the structure factor of the array design with an empty lattice approximation. We conclude that the lasing modes are the 74th $Γ$- and 106th $X$-point of the supercell. By tuning the square lattice period with respect to the gain emission we can control the modes that lase. Finally, we show that the lasing modes exhibit a combination of transverse electric and transverse magnetic mode characteristics in polarization resolved measurements.
Radiative properties of lasing plasmonic bound state in continuum are analyzed. The topological charge of the lasing signal is analyzed in the far field as well as in the source plane of the finite sized plasmonic lattice. The physical mechanism enabling the coupling of the BIC to radiation continuum is identified. We show that while the BICs have their origin in multipolar resonances, their far-field radiation properties are governed by the position dependent dipole moment distribution induced by the symmetry breaking in a finite plasmonic lattice. Remarkably, this dipole-moment enabled coupl…
Plasmonic nanolasers have ultrahigh lasing thresholds, especially those devices for which all three dimensions are truly subwavelength. Because of a momentum mismatch between the propagating light and localized optical field of the subwavelength nanocavity, poor optical pumping efficiency is another important reason for the ultrahigh threshold but is normally always ignored. Based on a cavity-embedded nanoantenna array design, we demonstrate a room-temperature low-threshold plasmonic nanolaser that is robust, reproducible, and easy-to-fabricate using chemical-template lithography. The mode vol…
We report on lasing at visible wavelengths in arrays of ferromagnetic Ni nanodisks overlaid with an organic gain medium. We demonstrate that by placing an organic gain material within the mode volume of the plasmonic nanoparticles both the radiative and, in particular, the high ohmic losses of Ni nanodisk resonances can be compensated. Under increasing pump fluence, the systems exhibit a transition from lattice-modified spontaneous emission to lasing, the latter being characterized by highly directional and sub-nanometer linewidth emission. By breaking the symmetry of the array, we observe tun…
We demonstrate an electrically controlled coherent random lasing with silver nano-particles dispersed in a dye-doped nematic liquid crystal (NLC), in which external electric field dependent emission intensity and frequency-splitting are recorded. A modified rate equation model is proposed to interpret the observed coherent lasing, which is a manifestation of double enhancements, caused by the plasmon-polariton near-fields of Ag particles, on the population inversion of laser dye molecules and the optical energy density of lasing modes. The noticeable quenching of lasing resonances in a weak ap…
We study lasing at the high-symmetry points of the Brillouin zone in a honeycomb plasmonic lattice. We use symmetry arguments to define singlet and doublet modes at the $\Kp$-points of the reciprocal space. We experimentally demonstrate lasing at the $\Kp$-points \changed{that is based on plasmonic lattice modes and two-dimensional feedback}. By comparing polarization properties to \changed{$T$-matrix} simulations, we identify the lasing mode as one of the singlets with an energy minimum at the $\Kp$-point enabling feedback. Our results offer prospects for studies of topological lasing in radi…
We report room temperature lasing in two-dimensional diffractive lattices of silver and gold plasmon particle arrays embedded in a dye-doped polymer that acts both as waveguide and gain medium. As compared to conventional dielectric distributed feedback lasers, a central question is how the underlying band structure from which lasing emerges is modified by both the much stronger scattering and the disadvantageous loss of metal. We use spectrally resolved back-focal plane imaging to measure the wavelength- and angle dependence of emission below and above threshold, thereby mapping the band stru…
Half-wave plasmonic nanolasers near the localization limit
Harvard Medical School（哈佛医学院）；Massachusetts General Hospital（麻省总医院）；Rice University（莱斯大学）；Harvard-MIT Health Sciences and Technology（哈佛-麻省理工学院健康科学与技术）；Massachusetts Institute of Technology（麻省理工学院）
Linewidth-tunable lasers have great application requirements in the fields of high-resolution spectroscopy, optical communications and other industry and scientific research. Here, the switchable plasmonic scattering of the metal particles with plenty of nanogaps is proposed as an effective method to achieve linewidth-tunable random lasers. By using the nonlinear optical effect of the environment medium, the metal particles demonstrate the transition from local scattering of nanogaps with high spatial frequency to traditional Mie scattering free from detail information with increasing the pump…
Nanophotonic devices take advantage of geometry-dependent optical properties to confine and enhance the interaction of light with matter on small scales. By carefully patterning nanoscale geometries, coupling of responses across distinct physical domains can be achieved, such as photon and phonon modes in optomechanical crystals. Extreme optical confinement of plasmonics can localize strong cross-domain interactions into nanometer-scale volumes, smaller than many nanosystem's thermal and mechanical eigenmodes, opening new regimes for engineering reconfigurable, dynamic nanosystems. Here, we pr…
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 …
Steady-state plasmonic lasing is studied theoretically for a system consisting of many dye molecules arranged regularly around a gold nano-sphere. A three-level model with realistic molecular dissipation is employed to analyze the performance as function of the pump field amplitude and number of molecules. Few molecules and moderate pumping produce a single narrow emission peak because the excited molecules transfer energy to a single dipole plasmon mode by amplified spontaneous emission. Under strong pumping, the single peak splits into broader and weaker emission peaks because two molecular …
Because surface plasmons can be confined below the diffraction limit, metallic lasers that support plasmonic modes can provide miniaturized sources of electromagnetic waves. Such devices often exploit a multilayer design, in which a semiconductor gain layer is placed near a metallic interface with a gap layer in between. However, despite many experimental demonstrations, key considerations for these planar metallic lasers remain understudied, leading to incorrect conclusions about the optimal design. Here, we pursue a detailed experimental and theoretical study of planar metallic lasers to exp…
The nanoscale mode volumes of surface plasmon polaritons have enabled plasmonic lasers and condensates with ultrafast operation. Most plasmonic lasers are based on noble metals, rendering the optical mode structure inert to external fields. Here, we demonstrate active magnetic-field control over lasing in a periodic array of Co/Pt multilayer nanodots immersed in an IR-140 dye solution. We exploit the magnetic nature of the nanoparticles combined with mode tailoring to control the lasing action. Under circularly polarized excitation, angle-resolved photoluminescence measurements reveal a transi…
Surface plasmon polaritons (SPPs) lasing requires population inversion, it is inefficient and possesses poor spectral properties. We develop an inversion-less concept for a quantum plasmonic waveguide that exploits unidirectional superradiant SPP emission of radiation to produce intense coherent surface plasmon beams. Our scheme includes a resonantly driven cold atomic medium in a lossless dielectric situated above an ultra-low loss negative index metamaterial~(NIMM) layer. We propose generating unidirectional superradiant radiation of the plasmonic field within an atomic medium and a NIMM lay…
Recent advances in near-field plasmonic metamaterials, such as nanoresonators or transducers, have demonstrated the ability to generate localized fields of high intensity, and thus maintain relatively large nanoscale heat gradients on the order of $10^1-10^2$~K/nm. A plasmonic near-field transducer (NFT) can achieve such large gradients, making population inversion achievable within phononic media. We herein develop a thermal nanomachine composed of a nanoscale phononic laser using InGaAs quantum dot media where an NFT serves as the plasmonic energy source. We show, on demand, the generation o…
We present a comprehensive study of the polarization and spatial coherence properties of the lasing modes supported by a 4-fold symmetric plasmonic lattice. By modifying only, the scattering properties of the individual particles while keeping the lattice geometry constant, we are able to distinguish the scattering induced effects from the lattice geometry induced effects. Customized interferometric measurements reveal that the lasing emission undergoes a drastic change from 1D to 2D spatial coherence with increasing particle size, accompanied with dramatic changes in the far field polarizatio…
Random lasing occurs as the result of a coherent optical feedback from multiple scattering centers. Here, we demonstrate that plasmonic gold nanostars are efficient light scattering centers, exhibiting strong field enhancement at their nanotips, which assists a very narrow bandwidth and highly amplified coherent random lasing with a low lasing threshold. First, by embedding plasmonic gold nanostars in a rhodamine 6G dye gain medium, we observe a series of very narrow random lasing peaks with full-width at half-maximum ~ 0.8 nm. In contrast, free rhodamine 6G dye molecules exhibit only a single…
Arrays of metallic particles patterned on a substrate have emerged as a promising design for on-chip plasmonic lasers. In past examples of such devices, the periodic particles provided feedback at a single resonance wavelength, and organic dye molecules were used as the gain material. Here, we introduce a flexible template-based fabrication method that allows a broader design space for Ag particle-array lasers. Instead of dye molecules, we integrate colloidal quantum dots (QDs), which offer better photostability and wavelength tunability. Our fabrication approach also allows us to easily adjus…
In 2003 Bergman and Stockman introduced the spaser, a quantum amplifier of surface plasmons by stimulated emission of radiation [1]. They argued that, by exploiting a metal/dielectric composite medium, it should be possible to construct a nano-device, where a strong coherent field is built up in a spatial region much smaller than the wavelength [1,2]. V-shaped metallic inclusion, combined with a collection of semiconductor quantum dots were discussed as a possible realization of the spaser [1]. Here we introduce a further development of the spaser concept. We show that by combining the metamat…
Metallic nanostructures provide a toolkit for the generation of coherent light below the diffraction limit. Plasmonic based lasing relies on the population inversion of emitters (such as organic fluorophores) along with feedback provided by plasmonic resonances. In this regime, known as weak light matter coupling, the radiative characteristics of the system can be described by the Purcell effect. Strong light matter coupling between the molecular excitons and electromagnetic field generated by the plasmonic structures leads to the formation of hybrid quasi-particles known as plasmon exciton po…
Coherent nanoscale photon sources are of paramount importance to achieving all-optical communication. Several nanolasers smaller than the diffraction limit have been theoretically proposed and experimentally demonstrated using plasmonic cavities to confine optical fields. Such compact cavities exhibit large Purcell factors, thereby enhancing spontaneous emission, which feeds into the lasing mode. However, most plasmonic nanolasers reported so far have employed resonant nanostructures and therefore had the lasing restricted to the proximity of the resonance wavelength. Here, we report on an app…
Photoluminescence is a phenomenon of significant interest due to its wide range of technological applications in plasmonics, nanolasers, spasers, lasing spasers, loss compensation and gain in metamaterials, and luminescent media. Nanostructured materials are known to have very different luminescence characteristics to bulk samples or planar films. Here we show that by engineering a nanostructured meta-surface, we can choose the position of photoluminescence absorption and emission lines of thin gold films. The nanostructuring also aids to strong enhancement of the emission from gold, by a fact…
Nanolasers have great potential as both on-chip light sources and optical barcoding particles. We demonstrate ultrasmall InGaP and InGaAsP disk lasers with diameters down to 360 nm (198 nm in height) in the red spectral range. Optically pumped, room-temperature, single-mode lasing was achieved from both disk-on-pillar and isolated particles. When isolated disks were placed on gold, plasmon polariton lasing was obtained with Purcell-enhanced stimulated emission. UV lithography and plasma ashing enabled the fabrication of nanodisks on a wafer-scale, with intended random size variation. Silica-co…
Plasmonic nanolasers have received a substantial interest for their promising applications in integrated photonics, optical sensing, and biomedical imaging. To date, a room-temperature plasmonic nanolaser, submicron in all dimensions, remains elusive in the visible regime due to high metallic losses. Here, we demonstrate single-particle lasing around 2.3 eV with full-submicron, cesium lead bromide perovskite (CsPbBr3) crystals atop polymer-coated gold substrates at room temperature. With a large number (~100) of devices in total, we systematically study the lasing action of plasmonic test and …
Periodic arrays of air nanoholes in thin metal films that support surface plasmon resonances can provide an alternative approach for boosting the light-matter interactions at the nanoscale. Indeed, nanohole arrays have garnered great interest in recent years for their use in biosensing, light emission enhancement and spectroscopy. However, the large-scale use of nanohole arrays in emerging technology requires new low-cost fabrication techniques. Here, we demonstrate a simple technique to fabricate nanohole arrays and examine their photonic applications. In contrast to the complicated and most …
Plasmonic metamaterials support the localized surface plasmon resonance (LSPR), which is sensitive to the change in the dielectric environment and highly desirable for ultrasensitive biochemical sensing. In this work, a novel design of supercell metamaterials of four mutually rotating split ring resonators (SRRs) is proposed, where simultaneous excitations of odd (N=1 and N = 3) and even (N=2) resonance modes are realized due to additional asymmetry from the rotation and show insensitivity to two orthogonal polarizations. The full utilization of these three resonance dips show bright prospects…
By using a self-consistent Maxwell-Bloch method, we demonstrate the simultaneously lasing and spasing behavior in a simple metal grating-film nanostructure, which can be attributed to spatial hole burning and the gain competition of different modes at the band edge and in the plasmonic band gap. We show three modes: one spaser mode in gap with quality factor as high as 248.54, one plasmon lasing mode at band edge which emit vertically from the grating surface, and the other plasmon lasing mode at band edge which is suppressed by the spaser mode. This method may find significant applications in…
Lasers are ubiquitous for information storage, processing, communications, sensing, biological research, and medical applications [1]. To decrease their energy and materials usage, a key quest is to miniaturize lasers down to nanocavities [2]. Obtaining the smallest mode volumes demands plasmonic nanocavities, but for these, gain comes from only single or few emitters. Until now, lasing in such devices was unobtainable due to low gain and high cavity losses [3]. Here, we demonstrate a plasmonic nanolaser approaching the single-molecule emitter regime. The lasing transition significantly broade…
In this work, we study the lasing conditions of the transverse electric (TE) modes of micro- and nanotubes coated internally with a thin metallic layer. This geometry may tackle some of the problems of nanolasers and spasers as it allows the recycling of the active medium while providing a tunable plasmonic cavity. The system presents two types of TE modes: cavity modes (CMs) and whispering-gallery modes (WGMs). On the one hand, we show that the lasing of WGM is only possible in nanoscale tubes. On the other hand, for tubes of some micrometers of diameter, we found that the system presents a l…
We calculate the quantum state of the plasmon field excited by an ensemble of molecular emitters, which are driven by exchange of electrons with metallic nano-particle electrodes. Assuming identical emitters that are coupled collectively to the plasmon mode but are otherwise subject to independent relaxation channels, we show that symmetry constraints on the total system density matrix imply a drastic reduction in the numerical complexity. For $N_{\text{m}}$ three-level molecules we may thus represent the density matrix by a number of terms scaling as $(N_{\rm m}+8)!/(8!N_{\rm m}!)$ instead of…
We demonstrate theoretically that a subwavelength spherical dielectric nanoparticle coated with a gain shell forms a nanolaser. Lasing modes of such a nanolaser are associated with the Mie resonances of the nanoparticle. We establish a general condition for the lasing threshold and show that the use of high refractive index dielectric media allows for lasing with a threshold significantly lower than that for nanolasers incorporating lossy plasmonic metals.
We experimentally observe lasing in a hexamer plasmonic lattice and find that when tuning the scale of the unit cell, the polarization winding of the emission changes. By a theoretical analysis we identify the lasing modes as quasi bound states in continuum (quasi-BICs) of topological charges of zero, one or two. A T-matrix simulation of the structure reveals that the mode quality(Q)-factors depend on the scale of the unit cell, with highest-Q modes favored by lasing. The system thus shows a loss-driven transition between lasing in modes of trivial and high-order topological charge.
This paper demonstrates an arbitrary tunable spaser based on double-Fano resonance of a plasmonic nanostructure consisting of two sets of disk-ring (TSDR) nanostructure. TSDR nanostructure supports two Fano resonances, which can be served as the lasing mode and the pumping mode of a spaser. These two mode can be tuned in a very wide wavelength range because of the good tunability of the two nanorings. The tuning range of the lasing mode and the pumping mode can be reached to 710 nm and 620 nm. These results represent a significant step in the pursuit of ultimate spasers and propose a approach …
Plasmonic distributed-feedback lasers based on a two-dimensional periodic array of metallic nanostructures are the main candidate for nanoscale sources of coherent electromagnetic field. Strong localization of the electromagnetic field and the large radiation surface are good opportunities for achieving an ultrashort response time to the external actions and creating beam directionality. At the same time, the investigation of such a system is a challenging problem. In this paper, we present an exhaustive study of the operation of a two-dimensional plasmonic distributed-feedback laser. We show …
On-chip light sources are critical for the realization of fully integrated photonic circuitry. So far, semiconductor miniaturized lasers have been mainly limited to sizes on the order of a few microns. Further reduction of sizes is challenging fundamentally due to the associated radiative losses. While using plasmonic metals helps to reduce radiative losses and sizes, they also introduce Ohmic losses hindering real improvements. In this work, we show that, making use of quasi-bound states in the continuum, or supercavity modes, we circumvent these fundamental issues and realize the smallest pu…
Laser science has tackled physical limitations to achieve higher power, faster and smaller light sources. The quest for ultra-compact laser that can directly generate coherent optical fields at the nano-scale, far beyond the diffraction limit of light, remains a key fundamental challenge. Microscopic lasers based on photonic crystals, micro-disks, metal clad cavities and nanowires can now reach the diffraction limit, which restricts both the optical mode size and physical device dimension to be larger than half a wavelength. While surface plasmons are capable of tightly localizing light, ohmic…
There is increasing interest in filling the gap of miniaturized terahertz/mid-infrared radiation sources and, particularly, in incorporating these sources into micro/nanophotonic circuits. By using rigorous electromagnetic methods, we investigate the lasing conditions and the electric-tunability of radiative and non radiative propagating surface-plasmon modes in cylinders made of active materials coated with a graphene layer. A detailed analysis of the lasing condition of different surface-plasmon modes shows that there is an abrupt change in the gain required when modes become nonradiative. A…
Localized surface plasmon resonances have recently attracted considerable attention due to their ability to dramatically enhance near-field optical intensities and boost nanoscale light-matter interactions. Here we demonstrate unambiguously that polyhedral silver nanoparticles can be tailored to promote enhanced coherent emission from organic dye dispersions in a cavity. In particular, we observe that nanoparticles supporting resonances close to the absorption peak of the dye yield to more efficient lasing, up to one order of magnitude, which is also evidenced by the narrowing of the emission …
We extend Lamb's reduced density matrix laser theory to analyze the inhomogeneous molecular couplings and the mode-correlation in a plasmonic nano-laser consisting of a gold sphere and many dye molecules interacting with a driving optical field and with the quantized plasmon modes. The molecular inhomogeneity is accounted for by simulating their random distribution around the sphere. Our analysis shows that in order to obtain lasing we must employ a large number of strongly driven molecules to compensate strong damping of the plasmon modes. The compact molecular arrangement, however, can lead …
Plasmonic metasurfaces exhibiting collective responses known as surface lattice resonances (SLRs) show potential for realizing tunable and flat photonic components for wavelength-selective processes, including lasing and optical nonlinearities. However, post-fabrication tuning of SLRs remains challenging, limiting the applicability of SLR-based components. Here, we demonstrate how the properties of high quality factor SLRs are easily modified by breaking the symmetry of the nanoparticle surroundings. We break the symmetry by changing the refractive index of the overlying immersion oil simply b…
Tailoring the emission of plasmonic nanowire-based lasers represents one of the major challenges in the field of nanoplasmonics, given the envisaged integration of such devices into on-chip all-optical circuits. In this study, we proposed a mode selection scheme based on distributed feedback, achieved via the external coupling of single zinc oxide nanowires to an aluminum grating, which enabled a quasi-single mode lasing action. The nano-manipulation of a single nanowire allowed for a reliable comparison of the lasing emission characteristics in both planar (i.e. nanowire on the metallic subst…
The interaction between molecules and surface plasmons in defined geometries can lead to new light mater hybrid states where light propagation is strongly influenced by molecular photon absorption. Their application range from lasing LEDs to controlling chemical reactions and are relevant in light harvesting. The coupling between the electromagnetic field and molecular excitations may also lead to macroscopic extended coherent states characterized by an increase in temporal and spatial coherency. In this respect, it is intriguing to explore the coherency of the hybrid system for molecules that…
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 …
Influence of metal nanoparticles on whispering gallery modes of a microcavity
Indian Institute of Technology Madras（印度马德拉斯理工学院）；Indian Institute of Technology Patna（印度巴特那理工学院）；Applied Materials Inc.（应用材料公司）；Optoelectronics Research Centre, University of Southampton（南安普顿大学光电研究中心）；New York University Tandon School of Engineering（纽约大学坦登工程学院）
