Lasing Spaser in Photonic Crystals.

Plasmonic nanolasers (spasers) are of intense interest, attributable to their ability to generate a high-intensity coherent radiation. We infiltrated a three-dimensional silica-based photonic crystal (PhC) film with spasers, composed of spherical gold cores, surrounded by silica shells with dye molecules. In spasers, the gold nanospheres supported the surface plasmons and the dye molecules transferred incoming optical energy to the surface plasmons. Our experiments show that such a structure, consisting of a PhC, which acts as an external distributed feedback resonator, and spasers, can serve as a coherent source of electromagnetic radiation. Spasers were locked in phase by the common radiation causing a phenomenon called the lasing spaser: the emission of spatially and temporarily coherent light normal to the surface of the PhC film. The far-field radiation patterns appeared in the shape of the Star-of-David, which is due to the dispersion along the Brillouin zone boundary. The infiltration of the spasers into the PhC led to drastic narrowing of the emission peak and an 80-fold decrease in the spaser generation threshold with respect to the same spasers in a suspension at room temperature.

Effect of logarithmic perturbations in ohmic like spectral densities in dynamics of electronic excitation using variational polaron transformation approach.

Electronic excitation energy transfer is a ubiquitous process that has generated prime research interest since its discovery. Recently developed variational polaron transformation-based second-order master equation is capable of interpolating between Förster and Redfield limits with exceptional accuracy. Forms of spectral density functions studied so far through the variational approach provide theoretical support for various experiments. Recently introduced ohmic like spectral density function that can account for logarithmic perturbations provides generality and exposition to a unique and practical set of environments. In this paper, we exploit the energy transfer dynamics of a two-level system attached to an ohmic like spectral density function with logarithmic perturbations using a variational polaron transformed master equation. Our results demonstrate that even for a relatively large bath coupling strength, quantum coherence effects can be increased by introducing logarithmic perturbations of the order of one and two in super-ohmic environments. Moreover, for particular values of the ohmicity parameter, the effect of logarithmic perturbations is observed to be insignificant for the overall dynamics. In regard to ohmic environments, as logarithmic perturbations increase, damping characteristics of the coherent transient dynamics also increase in general. It is also shown that, having logarithmic perturbations of the order of one in an ohmic environment can result in a less efficient energy transfer for relatively larger system bath coupling strengths.

Ten years of spasers and plasmonic nanolasers.

Ten years ago, three teams experimentally demonstrated the first spasers, or plasmonic nanolasers, after the spaser concept was first proposed theoretically in 2003. An overview of the significant progress achieved over the last 10 years is presented here, together with the original context of and motivations for this research. After a general introduction, we first summarize the fundamental properties of spasers and discuss the major motivations that led to the first demonstrations of spasers and nanolasers. This is followed by an overview of crucial technological progress, including lasing threshold reduction, dynamic modulation, room-temperature operation, electrical injection, the control and improvement of spasers, the array operation of spasers, and selected applications of single-particle spasers. Research prospects are presented in relation to several directions of development, including further miniaturization, the relationship with Bose-Einstein condensation, novel spaser-based interconnects, and other features of spasers and plasmonic lasers that have yet to be realized or challenges that are still to be overcome.

Topological Spaser.

We theoretically introduce a topological spaser, which consists of a hexagonal array of plasmonic metal nanoshells containing an achiral gain medium in their cores. Such a spaser can generate two mutually time-reversed chiral surface plasmon modes in the K and K^{'} valleys, which carry the opposite topological charges, ±1, and are described by a two-dimensional E^{'} representation of the D_{3h} point symmetry group. Due to the mode competition, this spaser exhibits a bistability: only one of these two modes generates, which is a spontaneous symmetry breaking. Such a spaser can be used for an ultrafast all-optical memory and information processing, and biomedical detection and sensing with chirality resolution.

Ultrafast optical currents in gapped graphene.

We theoretically study the interaction of ultrashort optical pulses with gapped graphene. Such a strong pulse results in a finite conduction band population and a corresponding electric current, both during and after the pulse. Since gapped graphene has broken inversion symmetry, it has an axial symmetry about the y -axis but not about the x-axis. We show that, in this case, if the linear pulse is polarized along the x-axis, the rectified electric current is generated in the y  direction. At the same time, the conduction band population distribution in the reciprocal space is symmetric about the x-axis. Thus, the rectified current in gapped graphene has an inter-band origin, while the intra-band contribution to the rectified current is zero.

Control of quantum emitter-plasmon strong coupling and energy transport with external electrostatic fields.

We investigate a system comprised of a constellation quantum emitters interacting with a localized surface plasmon mode of a metal nanoparticle subject to an externally applied electrostatic field. Due to the strong interactions among the electric field and the plasmonic setup, we show that system enters collective strong coupling regime generating polariton states when the intensity of the applied electrostatic field is increased. This in turn enhances the exciton energy transport rates between two emitters in the system when a single emitter is incoherently pumped. We further analyze how the placement of quantum emitter dipole moment orientation affects the observed collective strong coupling and how the electrostatic field can be used to put our setup to either weak or strong coupling regimes via the interacting electrostatic field.

Scattering characteristics of an exciton-plasmon nanohybrid made by coupling a monolayer graphene nanoflake to a carbon nanotube.

A hybrid nanostructure where a graphene nanoflake (GNF) is optically coupled to a carbon nanotube (CNT) could potentially possess enhanced sensing capabilities compared to the individual constituents whilst inheriting their high biocompatibility, favourable electrical, mechanical and spectroscopic properties. Therefore, in this paper, we investigate the scattering characteristics of an all-carbon exciton-plasmon nanohybrid which was made by coupling an elliptical GNF resonator to a semiconducting CNT gain element. We analytically model the nanohybrid as an open quantum system using cavity quantum electrodynamics. We derive analytical expressions for the dipole moment operator and the dipole response field of the GNF and characterize the Rayleigh scattering spectrum of the nanohybrid. These analytical expressions are valid for any arbitrary ellipsoidal nanoresonator coupled to a quantum emitter. Furthermore, we perform a detailed numerical analysis, the results of which indicate that the GNF-CNT nanohybrid exhibits enhanced and versatile scattering capabilities compared to the individual constituents. We show that the spectral signatures of the nanohybrid are highly tunable using a multitude of system parameters such as Fermi energy of the GNF, component dimensions, GNF-CNT separation distance and the permittivity of the submerging medium. We finally demonstrate the prospect of using the proposed nanohybrid to reconstruct the permittivity profile of a tumour. The high biocompatibility and high sensitivity to the dielectric properties of the environment make the proposed GNF-CNT nanohybrid an ideal candidate for such biosensing applications.

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.

Spaser as a biological probe.

Understanding cell biology greatly benefits from the development of advanced diagnostic probes. Here we introduce a 22-nm spaser (plasmonic nanolaser) with the ability to serve as a super-bright, water-soluble, biocompatible probe capable of generating stimulated emission directly inside living cells and animal tissues. We have demonstrated a lasing regime associated with the formation of a dynamic vapour nanobubble around the spaser that leads to giant spasing with emission intensity and spectral width >100 times brighter and 30-fold narrower, respectively, than for quantum dots. The absorption losses in the spaser enhance its multifunctionality, allowing for nanobubble-amplified photothermal and photoacoustic imaging and therapy. Furthermore, the silica spaser surface has been covalently functionalized with folic acid for molecular targeting of cancer cells. All these properties make a nanobubble spaser a promising multimodal, super-contrast, ultrafast cellular probe with a single-pulse nanosecond excitation for a variety of in vitro and in vivo biomedical applications.

Direct observation of localized surface plasmon field enhancement by Kelvin probe force microscopy.

A surface plasmon (SP) is a fundamental excitation state that exists in metal nanostructures. Over the past several years, the performance of optoelectronic devices has been improved greatly via the SP enhancement effect. In our previous work, the responsivity of GaN ultraviolet detectors was increased by over 30 times when using Ag nanoparticles. However, the physics of the SP enhancement effect has not been established definitely because of the lack of experimental evidence. To reveal the physical origin of this enhancement, Kelvin probe force microscopy (KPFM) was used to observe the SP-induced surface potential reduction in the vicinity of Ag nanoparticles on a GaN epilayer. Under ultraviolet illumination, the localized field enhancement induced by the SP forces the photogenerated electrons to drift close to the Ag nanoparticles, leading to a reduction of the surface potential around the Ag nanoparticles on the GaN epilayer. For an isolated Ag nanoparticle with a diameter of ~200 nm, the distribution of the SP localized field is located within 60 nm of the boundary of the Ag nanoparticle. For a dimer of Ag nanoparticles, the localized field enhancement between the nanoparticles was the strongest. The results presented here provide direct experimental proof of the localized field enhancement. These results not only explain the high performance of GaN detectors observed with the use of Ag nanoparticles but also reveal the physical mechanism of SP enhancement in optoelectronic devices, which will help us further understand and improve the performance of SP-based optoelectronic devices in the future.

Real and Imaginary Properties of Epsilon-Near-Zero Materials.

From the fundamental principle of causality we show that epsilon-near-zero (ENZ) materials with a very low (asymptotically zero) intrinsic dielectric loss do necessarily possess a very low (asymptotically zero) group velocity of electromagnetic wave propagation. This leads to the loss function being singular and causes high nonradiative damping of the optical resonators and emitters (plasmonic nanoparticles, quantum dots, chromophore molecules) embedded into them or placed at their surfaces. Rough ENZ surfaces do not exhibit hot spots of local fields suggesting that surface modes are overdamped. Reflectors and waveguides also show very large losses both for realistic and idealized ENZ materials.

Nanoscopy of Phase Separation in InxGa1-xN Alloys.

Phase separations in ternary/multinary semiconductor alloys is a major challenge that limits optical and electronic internal device efficiency. We have found ubiquitous local phase separation in In1-xGaxN alloys that persists to nanoscale spatial extent by employing high-resolution nanoimaging technique. We lithographically patterned InN/sapphire substrates with nanolayers of In1-xGaxN down to few atomic layers thick that enabled us to calibrate the near-field infrared response of the semiconductor nanolayers as a function of composition and thickness. We also developed an advanced theoretical approach that considers the full geometry of the probe tip and all the sample and substrate layers. Combining experiment and theory, we identified and quantified phase separation in epitaxially grown individual nanoalloys. We found that the scale of the phase separation varies widely from particle to particle ranging from all Ga- to all In-rich regions and covering everything in between. We have found that between 20 and 25% of particles show some level of Ga-rich phase separation over the entire sample region, which is in qualitative agreement with the known phase diagram of In1-xGaxN system.

Strong-Field Resonant Dynamics in Semiconductors.

We predict that a direct band gap semiconductor (GaAs) resonantly excited by a strong ultrashort laser pulse exhibits a novel regime: kicked anharmonic Rabi oscillations. In this regime, Rabi oscillations are strongly coupled to intraband motion, and interband transitions mainly take place when electrons pass near the Brillouin zone center where electron populations undergo very rapid changes. The asymmetry of the residual population distribution induces an electric current controlled by the carrier-envelope phase of the driving pulse. The predicted effects are experimentally observable using photoemission and terahertz spectroscopies.

Semimetallization of dielectrics in strong optical fields.

At the heart of ever growing demands for faster signal processing is ultrafast charge transport and control by electromagnetic fields in semiconductors. Intense optical fields have opened fascinating avenues for new phenomena and applications in solids. Because the period of optical fields is on the order of a femtosecond, the current switching and its control by an optical field may pave a way to petahertz optoelectronic devices. Lately, a reversible semimetallization in fused silica on a femtosecond time scale by using a few-cycle strong field (~1 V/Å) is manifested. The strong Wannier-Stark localization and Zener-type tunneling were expected to drive this ultrafast semimetallization. Wider spread of this technology demands better understanding of whether the strong field behavior is universally similar for different dielectrics. Here we employ a carrier-envelope-phase stabilized, few-cycle strong optical field to drive the semimetallization in sapphire, calcium fluoride and quartz and to compare this phenomenon and show its remarkable similarity between them. The similarity in response of these materials, despite the distinguishable differences in their physical properties, suggests the universality of the physical picture explained by the localization of Wannier-Stark states. Our results may blaze a trail to PHz-rate optoelectronics.

Nanoscopy reveals surface-metallic black phosphorus.

Black phosphorus (BP) is an emerging two-dimensional material with intriguing physical properties. It is highly anisotropic and highly tunable by means of both the number of monolayers and surface doping. Here, we experimentally investigate and theoretically interpret the near-field properties of a-few-atomic-monolayer nanoflakes of BP. We discover near-field patterns of bright outside fringes and a high surface polarizability of nanofilm BP consistent with its surface-metallic, plasmonic behavior at mid-infrared frequencies <1176 cm-1. We conclude that these fringes are caused by the formation of a highly polarizable layer at the BP surface. This layer has a thickness of ~1 nm and exhibits plasmonic behavior. We estimate that it contains free carriers in a concentration of n≈1.1 × 1020 cm-3. Surface plasmonic behavior is observed for 10-40 nm BP thicknesses but absent for a 4-nm BP thickness. This discovery opens up a new field of research and potential applications in nanoelectronics, plasmonics and optoelectronics.

Control of plasmonic nanoantennas by reversible metal-insulator transition.

We demonstrate dynamic reversible switching of VO2 insulator-to-metal transition (IMT) locally on the scale of 15 nm or less and control of nanoantennas, observed for the first time in the near-field. Using polarization-selective near-field imaging techniques, we simultaneously monitor the IMT in VO2 and the change of plasmons on gold infrared nanoantennas. Structured nanodomains of the metallic VO2 locally and reversibly transform infrared plasmonic dipole nanoantennas to monopole nanoantennas. Fundamentally, the IMT in VO2 can be triggered on femtosecond timescale to allow ultrafast nanoscale control of optical phenomena. These unique features open up promising novel applications in active nanophotonics.

Atomic-scale diffractive imaging of sub-cycle electron dynamics in condensed matter.

For interaction of light with condensed-matter systems, we show with simulations that ultrafast electron and X-ray diffraction can provide a time-dependent record of charge-density maps with sub-cycle and atomic-scale resolutions. Using graphene as an example material, we predict that diffraction can reveal localised atomic-scale origins of optical and electronic phenomena. In particular, we point out nontrivial relations between microscopic electric current and density in undoped graphene.

Strong-field perspective on high-harmonic radiation from bulk solids.

Mechanisms of high-harmonic generation from crystals are described by treating the electric field of a laser as a quasistatic strong field. Under the quasistatic electric field, electrons in periodic potentials form dressed states, known as Wannier-Stark states. The energy differences between the dressed states determine the frequencies of the radiation. The radiation yield is determined by the magnitudes of the interband and intraband current matrix elements between the dressed states. The generation of attosecond pulses from solids is predicted. Ramifications for strong-field physics are discussed.

All-color plasmonic nanolasers with ultralow thresholds: autotuning mechanism for single-mode lasing.

We report on the first demonstration of broadband tunable, single-mode plasmonic nanolasers (spasers) emitting in the full visible spectrum. These nanolasers are based on a single metal-oxide-semiconductor nanostructure platform comprising of InGaN/GaN semiconductor nanorods supported on an Al2O3-capped epitaxial Ag film. In particular, all-color lasing in subdiffraction plasmonic resonators is achieved via a novel mechanism based on a property of weak size dependence inherent in spasers. Moreover, we have successfully reduced the continuous-wave (CW) lasing thresholds to ultrasmall values for all three primary colors and have clearly demonstrated the possibility of "thresholdless" lasing for the blue plasmonic nanolaser.