Quantum Plasmonics Research Articles

Quantum plasmons with optical-range frequencies in doped few-layer graphene

Although plasmon modes exist in doped graphene, the limited range of doping achieved by gating restricts the plasmon frequencies to a range that does not include the visible and infrared. Here we show, through the use of first-principles calculations, that the high levels of doping achieved by lithium intercalation in bilayer and trilayer graphene shift the plasmon frequencies into the visible range. To obtain physically meaningful results, we introduce a correction of the effect of plasmon interaction across the vacuum separating periodic images of the doped graphene layers, consisting of transparent boundary conditions in the direction perpendicular to the layers; this represents a significant improvement over the exact Coulomb cutoff technique employed in earlier works. The resulting plasmon modes are due to local field effects and the nonlocal response of the material to external electromagnetic fields, requiring a fully quantum mechanical treatment. We describe the features of these quantum plasmons, including the dispersion relation, losses, and field localization. Our findings point to a strategy for fine-tuning the plasmon frequencies in graphene and other two-dimensional materials.

Plasmon confinement in fractal quantum systems

Recent progress in the fabrication of materials has made it possible to create arbitrary non-periodic two-dimensional structures in the quantum plasmon regime. This paves the way for exploring the plasmonic properties of electron gases in complex geometries such as fractals. In this work, we study the plasmonic properties of Sierpinski carpets and gaskets, two prototypical fractals with different ramification, by fully calculating their dielectric functions. We show that the Sierpinski carpet has a dispersion comparable to a square lattice, but the Sierpinski gasket features highly localized plasmon modes with a flat dispersion. This strong plasmon confinement in finitely ramified fractals can provide a novel setting for manipulating light at the quantum scale.

Excitonic terahertz photoconductivity in intrinsic semiconductor nanowires

Excitonic terahertz photoconductivity in intrinsic semiconductor nanowires is studied. Based on the excitonic theory, the numerical method to calculate the photoconductivity spectrum in the nanowires is developed, which can simulate optical pump terahertz-probe spectroscopy measurements on real nanowires and thereby calculate the typical photoconductivity spectrum. With the help of the energetic structure deduced from the calculated linear absorption spectrum, the numerically observed shift of the resonant peak in the photoconductivity spectrum is found to result from the dominant exciton transition between excited or continuum states to the ground state, and the quantitative analysis is in good agreement with the quantum plasmon model. Besides, the dependence of the photoconductivity on the polarization of the terahertz field is also discussed. The numerical method and supporting theoretical analysis provide a new tool for experimentalists to understand the terahertz photoconductivity in intrinsic semiconductor nanowires at low temperatures or for nanowires subjected to below bandgap photoexcitation, where excitonic effects dominate.

Plasmonic interferences of two-particle N00N states

Quantum plasmonics lies at the intersection between nanophotonics and quantum optics. Genuine quantum effects can be observed with non-classical states such as Fock states and with entangled states. A N00N state combines both aspects: it is a quantum superposition state of a Fock state with N excitations in two spatial modes. Here we report the first observation of two-plasmon (N = 2) N00N state interferences using a plasmonic beamsplitter etched on a planar interface between gold and air. We analyze in detail the role of losses at the beamsplitter and during the propagation along the metal/air interface. While the intrinsic losses of the beamsplitter are responsible for the emergence of quantum nonlinear absorption, we note that N00N states decay N times faster than classical states due to propagation losses.

Soluble Supercapacitors: Large and Reversible Charge Storage in Colloidal Iron-Doped ZnO Nanocrystals.

Colloidal ZnO semiconductor nanocrystals have previously been shown to accumulate multiple delocalized conduction-band electrons under chemical, electrochemical, or photochemical reducing conditions, leading to emergent semimetallic characteristics such as quantum plasmon resonances and raising prospects for application in multielectron redox transformations. Here, we demonstrate a dramatic enhancement in the capacitance of colloidal ZnO nanocrystals through aliovalent Fe3+-doping. Very high areal and volumetric capacitances (33 μF cm-2, 233 F cm-3) are achieved in Zn0.99Fe0.01O nanocrystals that rival those of the best supercapacitors used in commercial energy-storage devices. The redox properties of these nanocrystals are probed by potentiometric titration and optical spectroscopy. These data indicate an equilibrium between electron localization by Fe3+ dopants and electron delocalization within the ZnO conduction band, allowing facile reversible charge storage and removal. As "soluble supercapacitors", colloidal iron-doped ZnO nanocrystals constitute a promising class of solution-processable electronic materials with large charge-storage capacity attractive for future energy-storage applications.

Intersubband plasmons in the quantum limit in gated and aligned carbon nanotubes

Confined electrons collectively oscillate in response to light, resulting in a plasmon resonance whose frequency is determined by the electron density and the size and shape of the confinement structure. Plasmons in metallic particles typically occur in the classical regime where the characteristic quantum level spacing is negligibly small compared to the plasma frequency. In doped semiconductor quantum wells, quantum plasmon excitations can be observed, where the quantization energy exceeds the plasma frequency. Such intersubband plasmons occur in the mid- and far-infrared ranges and exhibit a variety of dynamic many-body effects. Here, we report the observation of intersubband plasmons in carbon nanotubes, where both the quantization and plasma frequencies are larger than those of typical quantum wells by three orders of magnitude. As a result, we observed a pronounced absorption peak in the near-infrared. Specifically, we observed the near-infrared plasmon peak in gated films of aligned single-wall carbon nanotubes only for probe light polarized perpendicular to the nanotube axis and only when carriers are present either in the conduction or valence band. Both the intensity and frequency of the peak were found to increase with the carrier density, consistent with the plasmonic nature of the resonance. Our observation of gate-controlled quantum plasmons in aligned carbon nanotubes will not only pave the way for the development of carbon-based near-infrared optoelectronic devices but also allow us to study the collective dynamic response of interacting electrons in one dimension.

Terahertz wave interaction with metallic nanostructures

AbstractUnderstanding light interaction with metallic structures provides opportunities of manipulation of light, and is at the core of various research areas including terahertz (THz) optics from which diverse applications are now emerging. For instance, THz waves take full advantage of the interaction to have strong field enhancement that compensates their relatively low photon energy. As the THz field enhancement have boosted THz nonlinear studies and relevant applications, further understanding of light interaction with metallic structures is essential for advanced manipulation of light that will bring about subsequent development of THz optics. In this review, we discuss THz wave interaction with deep sub-wavelength nano structures. With focusing on the THz field enhancement by nano structures, we review fundamentals of giant field enhancement that emerges from non-resonant and resonant interactions of THz waves with nano structures in both sub- and super- skin-depth thicknesses. From that, we introduce surprisingly simple description of the field enhancement valid over many orders of magnitudes of conductivity of metal as well as many orders of magnitudes of the metal thickness. We also discuss THz interaction with structures in angstrom scale, by reviewing plasmonic quantum effect and electron tunneling with consequent nonlinear behaviors. Finally, as applications of THz interaction with nano structures, we introduce new types of THz molecule sensors, exhibiting ultrasensitive and highly selective functionalities.

Array of nanoparticles coupling with quantum-dot: Lattice plasmon quantum features

In this study, we analyze the interaction of lattice plasmon with quantum-dot in order to mainly examine the quantum features of the lattice plasmon containing the photonic/plasmonic properties. Despite optical properties of the localized plasmon, the lattice plasmon severely depends on the array geometry, which may influence its quantum features such as uncertainty and the second-order correlation function. To investigate this interaction, we consider a closed system containing an array of the plasmonic nanoparticles and quantum-dot. We analyze this system with full quantum theory by which the array electric far field is quantized and the strength coupling of the quantum-dot array is analytically calculated. Moreover, the system's dynamics are evaluated and studied via the Heisenberg-Langevin equations to attain the system optical modes. We also analytically examine the Purcell factor, which shows the effect of the lattice plasmon on the quantum-dot spontaneous emission. Finally, the lattice plasmon uncertainty and its time evolution of the second-order correlation function at different spatial points are examined. These parameters are dramatically affected by the retarded field effect of the array nanoparticles. We found a severe quantum fluctuation at points where the lattice plasmon occurs, suggesting that the lattice plasmon photons are correlated.

Tuning and Switching a Plasmonic Quantum Dot "Sandwich" in a Nematic Line Defect.

We study the quantum-mechanical effects arising in a single semiconductor core/shell quantum dot (QD) controllably sandwiched between two plasmonic nanorods. Control over the position and the "sandwich" confinement structure is achieved by the use of a linear-trap liquid crystal (LC) line defect and laser tweezers that "push" the sandwich together. This arrangement allows for the study of exciton-plasmon interactions in a single structure, unaltered by ensemble effects or the complexity of dielectric interfaces. We demonstrate the effect of plasmonic confinement on the photon antibunching behavior of the QD and its luminescence lifetime. The QD behaves as a single emitter when nanorods are far away from the QD but shows possible multiexciton emission and a significantly decreased lifetime when tightly confined in a plasmonic "sandwich". These findings demonstrate that LC defects, combined with laser tweezers, enable a versatile platform to study plasmonic coupling phenomena in a nanoscale laboratory, where all elements can be arranged almost at will.

Quantum plasmon and Rashba-like spin splitting in self-assembled CoxC60 composites with enhanced Co content (x > 15)

Driving by interplay between plasmonic and magnetic effects in organic composite semiconductors is a challenging task with a huge potential for practical applications. Here, we present evidence of a quantum plasmon excited in the self-assembled CoxC60 nanocomposite films with x > 15 (interval of the Co cluster coalescence) and analyse it using the optical absorption (OA) spectra. In the case of CoxC60 film with x = 16 (LF sample), the quantum plasmon generated by the Co/CoO clusters is found as the 1.5 eV-centred OA peak. This finding is supported by the establishment of four specific C60-related OA lines detected at the photon energies Ep > 2.5 eV. Increase of the Co content up to x = 29 (HF sample) leads to pronounced enhancement of OA intensity in the energy range of Ep > 2.5 eV and to plasmonic peak downshift of 0.2 eV with respect to the peak position in the LF spectrum. Four pairs of the OA peaks evaluated in the HF spectrum at Ep > 2.5 eV reflect splitting of the C60-related lines, suggesting great change in the microscopic conditions with increasing x. Analysis of the film nanostructure and the plasmon-induced conditions allows us to propose a Rashba-like spin splitting effect that suggests valuable sources for spin polarization.

An eigenvalue approach to quantum plasmonics based on a self-consistent hydrodynamics method

Plasmonics has attracted much attention not only because it has useful properties such as strong field enhancement, but also because it reveals the quantum nature of matter. To handle quantum plasmonics effects, ab initio packages or empirical Feibelman d-parameters have been used to explore the quantum correction of plasmonic resonances. However, most of these methods are formulated within the quasi-static framework. The self-consistent hydrodynamics model offers a reliable approach to study quantum plasmonics because it can incorporate the quantum effect of the electron gas into classical electrodynamics in a consistent manner. Instead of the standard scattering method, we formulate the self-consistent hydrodynamics method as an eigenvalue problem to study quantum plasmonics with electrons and photons treated on the same footing. We find that the eigenvalue approach must involve a global operator, which originates from the energy functional of the electron gas. This manifests the intrinsic nonlocality of the response of quantum plasmonic resonances. Our model gives the analytical forms of quantum corrections to plasmonic modes, incorporating quantum electron spill-out effects and electrodynamical retardation. We apply our method to study the quantum surface plasmon polariton for a single flat interface.

Plasmonic Enhanced EIT and Velocity Selective Optical Pumping Measurements with Atomic Vapor

In this work, we experimentally observe for the first time nanoscale plasmonic enhanced Electromagnetically Induced Transparency (EIT) and Velocity Selective Optical Pumping (VSOP) effects in miniaturized Integrated Quantum Plasmonic Device (IQPD) for D2 transitions in rubidium (Rb). Our device consists of a vapor cell integrated on top of a prism coated with a thin layer of metal. This configuration is known to allow efficient excitation of Surface Plasmon Resonance (SPR). The evanescent field of the surface plasmon mode interacts with the atomic media in close vicinity to the metal. In spite of the limited interaction length between SPR and Rb atoms, the signature of EIT along with VSOP signals could be clearly observed in our miniaturized IQPD under proper conditions of pump and probe intensities. A gradual decrease in the contrast of the plasmonic enhanced EIT and VSOP signals was observed as the excitation was detuned from the SPR critical angle, due to reduction in electromagnetic field enhancement,...

Quantum Control of Graphene Plasmon Excitation and Propagation at Heaviside Potential Steps.

Quantum mechanical effects of single particles can affect the collective plasmon behaviors substantially. In this work, the quantum control of plasmon excitation and propagation in graphene is demonstrated by adopting the variable quantum transmission of carriers at Heaviside potential steps as a tuning knob. First, the plasmon reflection is revealed to be tunable within a broad range by varying the ratio γ between the carrier energy and potential height, which originates from the quantum mechanical effect of carrier propagation at potential steps. Moreover, the plasmon excitation by free-space photos can be regulated from fully suppressed to fully launched in graphene potential wells also through adjusting γ, which defines the degrees of the carrier confinement in the potential wells. These discovered quantum plasmon effects offer a unified quantum-mechanical solution toward ultimate control of both plasmon launching and propagating, which are indispensable processes in building plasmon circuitry.

Nonlinear optical response of embedded-semiconductor quantum dots covered by plasmonic metasurfaces

We report the first experimental finding of nonlinear responses of photoluminescence (PL) intensity in coupling systems of plasmonic metasurface and InAs quantum dots (QDs) embedded in a GaAs substrate. We numerically designed the coupling systems and experimentally studied the PL at room temperature (RT). We found that even weak excitation induces superlinear response of the PL intensities. For comparison, we fabricated and tested a series of metallic grating couplers on the QD-embedded GaAs substrate. Although the excitation light efficiently couples to grating structures, we found that the degree of nonlinearity of the PL assisted by the plasmonic metasurfaces is higher than the case of the grating structures. These results indicate that the coupled systems of QD emitters and the plasmonic metasurfaces are essentially nonlinear systems.

Plasmon mass scale and quantum fluctuations of classical fields on a real time lattice

Classical real-time lattice simulations play an important role in understanding non-equilibrium phenomena in gauge theories and are used in particular to model the prethermal evolution of heavy-ion collisions. Above the Debye scale the classical Yang-Mills (CYM) theory can be matched smoothly to kinetic theory. First we study the limits of the quasiparticle picture of the CYM fields by determining the plasmon mass of the system using 3 different methods. Then we argue that one needs a numerical calculation of a system of classical gauge fields and small linearized fluctuations, which correspond to quantum fluctuations, in a way that keeps the separation between the two manifest. We demonstrate and test an implementation of an algorithm with the linearized fluctuation showing that the linearization indeed works and that the Gauss’s law is conserved.

Plasmonic molybdenum trioxide quantum dots with noble metal-comparable surface enhanced Raman scattering

We propose a one-pot solution strategy to prepare sub-stoichiometric MoO3 quantum dots (MoO3−χ-QDs) with single-layered, vacancy-containing and few-crystalline features, which display surface plasmon resonance (SPR) in both visible and near-infrared regions without illumination.

Quantum mechanical analysis of nonlinear optical response of interacting graphene nanoflakes

We propose a distant-neighbor quantum-mechanical (DNQM) approach to study the linear and nonlinear optical properties of graphene nanoflakes (GNFs). In contrast to the widely used tight-binding description of the electronic states that considers only the nearest-neighbor coupling between the atoms, our approach is more accurate and general, as it captures the electron-core interactions between all atoms in the structure. Therefore, as we demonstrate, the DNQM approach enables the investigation of the optical coupling between two closely separated but chemically unbound GNFs. We also find that the optical response of GNFs depends crucially on their shape, size, and symmetry properties. Specifically, increasing the size of nanoflakes is found to shift their accommodated quantum plasmon oscillations to lower frequency. Importantly, we show that by embedding a cavity into GNFs, one can change their symmetry properties, tune their optical properties, or enable otherwise forbidden second-harmonic generation processes.

Extraordinary Effects in Quasi-Periodic Gold Nanocavities: Enhanced Transmission and Polarization Control of Cavity Modes.

Plasmonic quasi-periodic structures are well-known to exhibit several surprising phenomena with respect to their periodic counterparts, due to their long-range order and higher rotational symmetry. Thanks to their specific geometrical arrangement, plasmonic quasi-crystals offer unique possibilities in tailoring the coupling and propagation of surface plasmons through their lattice, a scenario in which a plethora of fascinating phenomena can take place. In this paper we investigate the extraordinary transmission phenomenon occurring in specifically patterned Thue-Morse nanocavities, demonstrating noticeable enhanced transmission, directly revealed by near-field optical experiments, performed by means of a scanning near-field optical microscope (SNOM). SNOM further provides an intuitive picture of confined plasmon modes inside the nanocavities and confirms that localization of plasmon modes is based on size and depth of nanocavities, while cross talk between close cavities via propagating plasmons holds the polarization response of patterned quasi-crystals. Our performed numerical simulations are in good agreement with the experimental results. Thus, the control on cavity size and incident polarization can be used to alter the intensity and spatial properties of confined cavity modes in such structures, which can be exploited in order to design a plasmonic device with customized optical properties and desired functionalities, to be used for several applications in quantum plasmonics.

Quantum Plasmon Engineering with Interacting Graphene Nanoflakes

We investigate the potential merits of using nanometer-sized graphene flakes as building blocks for two-dimensional (2D) quantum metamaterials. The choice of the building blocks of metamaterials is crucial to our ability to design quantum metamaterials with desired properties. In this context, graphene nanostructures are promising candidates to fulfill this role as they can be easily grown either by bottom-up chemical synthesis or top-down electron beam patterning in various shapes, topologies, and sizes, down to the molecular scale. This provides a broad range of parameters to tune the optical properties of graphene-based 2D quantum metamaterials. By using time-dependent density functional theory and quantum chemistry computations, we demonstrate that the graphene-based nanostructures accommodate collective charge oscillations, called quantum plasmons, which are qualitatively different in key aspects from their classical counterparts. In particular, our analysis reveals that the exponents characterizing ...

Enhancing Coherent Light-Matter Interactions through Microcavity-Engineered Plasmonic Resonances.

Quantum manipulation is challenging in localized-surface plasmon resonances (LSPRs) due to strong dissipations. To enhance quantum coherence, here we propose to engineer the electromagnetic environment of LSPRs by placing metallic nanoparticles (MNPs) in optical microcavities. An analytical quantum model is first built to describe the LSPR-microcavity interaction, revealing the significantly enhanced coherent radiation and the reduced incoherent dissipation. Furthermore, when a quantum emitter interacts with the LSPRs in the cavity-engineered environment, its quantum yield is enhanced over 40 times and the radiative power over one order of magnitude, compared to those in the vacuum environment. Importantly, the cavity-engineered MNP-emitter system can enter the strong coupling regime of cavity quantum electrodynamics, providing a promising platform for the study of quantum plasmonics, quantum information processing, precise sensing, and spectroscopy.