Spaser Research Articles

Is metal a friend or foe?

A thorough study comparing the performance of more than a hundred photonic and plasmonic lasers concludes that the latter are advantageous when their cavity volumes are close to the diffraction limit.

Solid and Hollow Gold Nanostructures for Nanomedicine: Comparison of Photothermal Properties

The photothermal properties of solid and hollow gold nanostructures represented by colloidal solutions of spherical nanoparticles, nanoshells, and nanocages upon irradiation with a 100 mW 808 nm continuous-wave laser for the first time were experimentally compared under identical optical density and nanoparticle concentration conditions. Accompanying computer modeling of light absorption by the studied gold nanostructures revealed the general parameters influencing the photothermal efficiency, which is of significance for nanomedical applications. The spectral position of localized plasmonic excitations of the studied nanostructures ranged from 518 nm for solid gold nanoparticles to 718 nm for gold nanocages, which provided a possibility to observe a direct influence of the wavelength proximity between the localized surface plasmon resonance and laser line on the heat generation capability of the nanostructures. As a result, the best photothermal efficiency was registered for gold nanocages, which proves them as an efficient photothermal treatment agent and a possible candidate to build a nanocarrier platform for drug delivery with a controlled release. Light absorption modeling demonstrated an existence of optimal wall thickness for gold nanoshells that should lead to the maximum photothermal efficiency when irradiated with 808 nm light, which varied from about 0.1 to 0.4 in units of external nanoshell radius with an increase of the wall porosity. Additionally, computer modeling results show that increased wall porosity should lead to enhanced photothermal efficiency of polydisperse colloidal solutions of hollow gold nanostructures.

Unusual scaling laws for plasmonic nanolasers beyond the diffraction limit

Plasmonic nanolasers are a new class of amplifiers that generate coherent light well below the diffraction barrier bringing fundamentally new capabilities to biochemical sensing, super-resolution imaging, and on-chip optical communication. However, a debate about whether metals can enhance the performance of lasers has persisted due to the unavoidable fact that metallic absorption intrinsically scales with field confinement. Here, we report plasmonic nanolasers with extremely low thresholds on the order of 10 kW cm−2 at room temperature, which are comparable to those found in modern laser diodes. More importantly, we find unusual scaling laws allowing plasmonic lasers to be more compact and faster with lower threshold and power consumption than photonic lasers when the cavity size approaches or surpasses the diffraction limit. This clarifies the long-standing debate over the viability of metal confinement and feedback strategies in laser technology and identifies situations where plasmonic lasers can have clear practical advantage.

Plasmonic nanolaser for intracavity spectroscopy and sensorics

We demonstrate intracavity plasmonic laser spectroscopy using a plasmonic laser created from a periodically perforated silver film with a liquid gain medium. An active zone of the laser is formed by a highly elongated spot of pumping. This results in a significantly more efficient diffusive mixing of dye molecules, which suppresses the effect of their bleaching, and in the ability to reduce the volume of the gain medium to as little as 400 nl. We use this design for a stable plasmonic laser in multiple measurements and demonstrate that it is highly effective as a spaser spectroscopy sensor for intracavity detection of an absorptive dye at 0.07 ppm. This work provides an opportunity to develop applications of intracavity plasmonic laser spectroscopy in biological label detection and other fields.

Open Resonator Electric Spaser.

The inception of the plasmonic laser or spaser (surface plasmon amplification by stimulated emission of radiation) concept in 2003 provides a solution for overcoming the diffraction limit of electromagnetic waves in miniaturization of traditional lasers into the nanoscale. From then on, many spaser designs have been proposed. However, all existing designs use closed resonators. In this work, we use cavity quantum electrodynamics analysis to theoretically demonstrate that it is possible to design an electric spaser with an open resonator or a closed resonator with much weak feedback in the extreme quantum limit in an all-carbon platform. A carbon nanotube quantum dot plays the role of a gain element, and Coulomb blockade is observed. Graphene nanoribbons are used as the resonator, and surface plasmon polariton field distribution with quantum electrodynamics features can be observed. From an engineering perspective, our work makes preparations for integrating spasers into nanocircuits and/or photodynamic therapy applications.

Wavelength Tunable Plasmonic Lasers Based on Intrinsic Self-Absorption of Gain Material

Multicolor plasmonic nanowire lasers enable below diffraction-limit directional optical waveguiding and amplification vital to the development of next generation compact on-chip optical communications, super-resolution imaging, display technologies, and so on. However, progress in developing these compact lasers for different wavelengths is severely curtailed by the few complex fabrication methods available. In this work, we demonstrate wavelength-tunable plasmonic nanowire lasers by leveraging the intrinsic optical self-absorption of the gain medium. The plasmonic lasing wavelength is tunable from 465 to 491 nm by simply adjusting the nanowire length, that is, by approximately 76% over the interval width of the emission spectrum. The Purcell factor of plasmonic nanowire cavity decreases with increasing nanowire length; while the propagation loss increases from 1020 to 8354 cm–1 with decreasing nanowire diameter, exhibiting a plasmonic-photonic mode transition at diameters around 120–150 nm. Importantly, ...

Plasmon-Induced Accelerated Exciton Recombination Dynamics in ZnO/Ag Hybrid Nanolasers

The recent development of plasmonics has break through the optical diffraction limit and realized ultracompact nanolasers that can directly generate coherent optical fields at the nanometre scale. However, it remains to a profound understanding on the light and matter interactions in so-called Spaser, especially on the coupling mechanism between the surface plasmon and exciton although many reports have claimed surface plasmonic lasers. Here, we demonstrated a ZnO/SiO2/Ag structural hybrid plasmonic nanolaser and compared with a conventional photonic laser systematically. We proposed that these two kinds of lasers originated from the entirely different optical gain mechanisms, and resulted in the generation of lasing mode shift. Time-resolved spectra collected from these two samples at room temperature presented the dynamic process of exciton recombination and revealed the energy-transfer from excitons to SPs. Our research provides an important theoretical and experimental basis for the practical applicat...

Millimeter-Scale Spatial Coherence from a Plasmon Laser.

Coherent light sources have been demonstrated based on a wide range of nanostructures, however, little effort has been devoted to probing their underlying coherence properties. Here, we report long-range spatial coherence of lattice plasmon lasers constructed from a periodic array of gold nanoparticles and a liquid gain medium at room temperature. By combining spatial and temporal interferometry, we demonstrate millimeter-scale (∼1 mm) spatial coherence and picosecond (∼2 ps) temporal coherence. The long-range spatial coherence occurs even without the presence of strong coupling with the lattice plasmon mode extending over macroscopic distances in the lasing regime. This plasmonic lasing system thus provides a platform for understanding the emergence of long-range coherence from collections of nanoscale resonators and points toward novel types of distributed lasing sources.

Tailoring Eigenmodes at Spectral Singularities in Graphene-based PT Systems

The spectral singularity existing in PT-synthetic plasmonic system has been widely investigated. Only lasing-mode can be excited resulting from the passive characteristic of metallic materials. Here, we investigated the spectral singularity in the hybrid structure composed of the photoexcited graphene and one-dimensional PT-diffractive grating. In this system, both lasing- and absorption-modes can be excited with the surface conductivity of photoexcited graphene being loss and gain, respectively. Remarkably, the spectral singularity will disappear with the optically pumped graphene to be lossless. In particular, we find that spectral singularities can exhibit symmetry-modes, when the loss and gain of the grating is unbalanced. Meanwhile, by tuning the loss (gain) of graphene and non-PT diffraction grating, lasing- and absorption-modes can also be excited. We hope that tunable optical modes at spectral singularities can have some applications in designing novel surface-enhanced spectroscopies and plasmon lasers.

Distributed feedback lasing in a metallic cavity

Distributed feedback (DFB) lasing is observed in a metallic cavity, which consists of a gold grating and a polymer membrane. The gold grating is prepared by evaporating a 25 nm thin film of gold on the photoresist grating fabricated by interference lithography. A 150 nm thick polymer membrane is directly attached on the gold grating, forming a suspended membrane supported by the grating ridge. The assembly method decreases the metallic contact area, which makes the mode more photonic and thereby reduces the ohmic loss of the metal. Low threshold DFB lasing can be achieved when the sample is optically pumped. The fabrication technique provides a facile way to realize plasmonic DFB polymer lasers.

All-plasmonic Optical Phased Array Integrated on a Thin-film Platform

Optical phased arrays have been demonstrated to enable a variety of applications ranging from high-speed on-chip communications to vertical surface emitting lasers. Despite the prosperities of the researches on optical phased arrays, presently, the reported designs of optical phased arrays are based on silicon photonics while plasmonic-based optical phased arrays have not been demonstrated yet. In this paper, a passive plasmonic optical phased array is proposed and experimentally demonstrated. The beam of the proposed plasmonic optical phased array is steerable in the far-field area and a high directivity can be achieved. In addition, radio frequency phased array theory is demonstrated to be applicable to the description of the coupling conditions of the delocalized surface plasmons in optical phased arrays and thus the gap between the phased arrays at two distinctly different wavelengths can be bridged. The potential applications of the proposed plasmonic phased arrays include on-chip optical wireless nanolinks, optical interconnections and integrated plasmonic lasers.

Plasmonic amplification of terahertz radiation in a periodic graphene structure with the carrier injection

Injection pumping of the pristine graphene is a promising alternative to optical pumping, but it is not obvious how to properly combine electronic and plasmonic features in one and the same device in order to obtain the terahertz plasmon amplification in graphene with injection pumping. This paper shows that an amplified plasmon mode can be effectively excited at the plasmon resonance frequencies in an active ungated region graphene with injecting (absorbing) gated parts of the periodic graphene structure. Necessary conditions for the plasmon lasing in the structure are found.

Role of Absorbing Nanocrystal Cores in Soft Photonic Crystals: A Spectroscopy and SANS Study.

Periodic superstructures of plasmonic nanoparticles have attracted significant interest because they can support coupled plasmonic modes, making them interesting for plasmonic lasing, metamaterials, and as light-management structures in thin-film optoelectronic devices. We have recently shown that noble metal hydrogel core-shell colloids allow for the fabrication of highly ordered 2-dimensional plasmonic lattices that show surface lattice resonances as the result of plasmonic/diffractive coupling (Volk, K.; Fitzgerald, J. P. S.; Ruckdeschel, P.; Retsch, M.; König, T. A. F.; Karg, M. Reversible Tuning of Visible Wavelength Surface Lattice Resonances in Self-Assembled Hybrid Monolayers. Adv. Optical Mater. 2017, 5, 1600971, DOI: 10.1002/adom.201600971). In the present work, we study the photonic properties and structure of 3-dimensional crystalline superstructures of gold hydrogel core-shell colloids and their pitted counterparts without gold cores. We use far-field extinction spectroscopy to investigate the optical response of these superstructures. Narrow Bragg peaks are measured, independently of the presence or absence of the gold cores. All crystals show a significant reduction in low-wavelength scattering. This leads to a significant enhancement of the plasmonic properties of the samples prepared from gold-nanoparticle-containing core-shell colloids. Plasmonic/diffractive coupling is not evident, which we mostly attribute to the relatively small size of the gold cores limiting the effective coupling strength. Small-angle neutron scattering is applied to study the crystal structure. Bragg peaks of several orders clearly assignable to an fcc arrangement of the particles are observed for all crystalline samples in a broad range of volume fractions. Our results indicate that the nanocrystal cores do not influence the overall crystallization behavior or the crystal structure. These are important prerequisites for future studies on photonic materials built from core-shell particles, in particular, the development of new photonic materials from plasmonic nanocrystals.

Broadband Surface Plasmon Lasing in One-dimensional Metallic Gratings on Semiconductor

We report surface plasmon (SP) lasing in metal/semiconductor nanostructures, where one-dimensional periodic silver slit gratings are placed on top of an InGaAsP layer. The SP nature of the lasing is confirmed from the emission wavelength governed by the grating period, polarization analysis, spatial coherence, and comparison with the linear transmission. The excellent performance of the device as an SP source is demonstrated by its tunable emission in the 400-nm-wide telecom wavelength band at room temperature. We show that the stimulated emission enhanced by the Purcell effect enables successful SP lasing at high energies above the gap energy of the gain. We also discuss the dependence of the lasing efficiency on temperature, grating dimension, and type of metal.

Manipulable and Hybridized, Ultralow‐Threshold Lasing in a Plasmonic Laser Using Elliptical InGaN/GaN Nanorods

Manipulating stimulated‐emission light in nanophotonic devices on scales smaller than their emission wavelengths to meet the requirements for optoelectronic integrations is a challenging but important step. Surface plasmon polaritons (SPPs) are one of the most promising candidates for sub‐wavelength optical confinement. In this study, based on the principle of surface plasmon amplification by the stimulated emission of radiation (SPASER), III‐Nitride‐based plasmonic nanolaser with hybrid metal–oxide–semiconductor (MOS) structures is designed. Using geometrically elliptical nanostructures fabricated by nanoimprint lithography, elliptical nanolasers able to demonstrate single‐mode and multimode lasing with an optical pumping power density as low as 0.3 kW cm−2 at room temperature and a quality Q factor of up to 123 at a wavelength of ≈490 nm are achieved. The ultralow lasing threshold is attributed to the SPP‐coupling‐induced strong electric‐field‐confinement in the elliptical MOS structures. In accordance with the theoretical and experimental results, the size and shape of the nanorod are the keys for manipulating hybridization of the plasmonic and photonic lasing modes in the SPASER. This finding provides innovative insight that will contribute to realizing a new generation of optoelectronic and information devices.

Plasmon resonance coupling phenomena in self-assembled colloidal monolayers

Colloidal self-assembly merges the flexibility provided by (wet-chemical) colloid synthesis and the structural diversity offered by self-assembly. Using plasmonic nanocrystals as colloidal building blocks, this enables the fabrication of plasmonic superstructures that show optical response superior to the individual colloid properties. In this review, we highlight recent examples of colloidal monolayers featuring coupled plasmonic resonances. Depending on the average inter-particle distance and the structure of such monolayers, the discussed examples show either near-field or radiative coupling signatures depending on the critical interference length scale of the localized resonances. In addition, templated assembly is highlighted as a pathway for the preparation of monolayers that show anisotropic optical coupling. The collected works not only reflect the recent state of the art in plasmonic resonance engineering in self-assembled monolayers, but also point to future directions relevant for their use in nanophotonic applications such as plasmonic lasing.

Limitations of Particle-Based Spasers.

We present a semiclassical analytic model for spherical core-shell surface plasmon lasers. Within this model, we drop the widely used one-mode approximations in favor of fully electromagnetic Mie theory. This allows for incorporation of realistic gain relaxation rates that so far are massively underestimated. Especially, higher order modes can undermine and even reverse the beneficial effects of the strong Purcell effect in such systems. Our model gives a clear view on gain and resonator requirements, as well as on the output characteristics that will help experimenters to design more efficient particle-based spasers.

Low-Threshold Plasmonic Lasers on a Single-Crystalline Epitaxial Silver Platform at Telecom Wavelength

We report on the first demonstration of metal–insulator–semiconductor-type plasmonic lasers at the telecom wavelength (∼1.3 μm) using top-down fabricated semiconductor waveguides on single-crystalline metallic platforms formed using epitaxially grown Ag films. The critical role of the Ag film thickness in sustaining plasmonic lasing at the telecom wavelength is investigated systematically. Low-threshold (0.2 MW/cm2) and continuous-wave operation of plasmonic lasing at cryogenic temperatures can be achieved on a 150 nm Ag platform with minimum radiation leakage into the substrate. Plasmonic lasing occurs preferentially through higher-order surface-plasmon-polariton modes, which exhibit a higher mode confinement factor, lower propagation loss, and better field–gain coupling. We observed plasmonic lasing up to ∼200 K under pulsed excitations. The plasmonic lasers on large-area epitaxial Ag films open up a scalable platform for on-chip integrations of plasmonics and optoelectronics at the telecom wavelength.

Random lasing assisted by CuSO_4 and Au nanoparticles in random gain systems

Random laser actions from a dye pyrromethene-597(PM597)-doped CuSO4 mixture infiltrated in glass capillaries are demonstrated. Discrete lasing modes are observed at the complete solid angle. Low threshold and variable emission wavelength of the random lasers are realized by adjusting the concentration of CuSO4 in the mixtures. With the exception of the multiple scattering of light caused by micro-crystals dispersed in the mixtures, another underlying physical mechanism for tuning random laser is closely related to energy transfer between the molecules of PM597 and CuSO4. Meanwhile, we also demonstrate the realization of a plasmonic random laser by doping Au nanoparticles (NPS) in the PM597-doped CuSO4 mixture. We find that the localized surface plasmon resonance of Au NPS lowers the threshold, increases the emission intensity and reduces the number of the lasing modes of the random lasers. Our results indicate that CuSO4 paves a new avenue towards designing low-cost photonic devices based on the random lasers.

Quantum-coherence-enhanced transient surface plasmon lasing

Quantum coherence and interference offer novel pathways to control light–matter interaction at the atomic scale, with enticing prospects in both fundamental and applied science. Here, we demonstrate coherent control over transient excitation of localized surface plasmon modes of a silver nanosphere adjacent to a quantum coherence medium composed of three-level quantum emitters, using a theoretical approach. We show that quantum interference enables more than two orders of magnitude enhancement in the surface plasmon field generated when the quantum emitters are driven coherently, in comparison to incoherent pumping. Furthermore, under optimal conditions, intense surface plasmon lasing can be induced without population inversion on the spasing transition. Our results open up the possibility of overcoming dissipative losses in plasmonic modes in the transient regime when steady-state population inversion is difficult to achieve due to fast relaxation rates and impractical pumping requirements.