Using ab initio calculations we predict the existence of one-dimensional (1D), atomically confined plasmons at the edges of a zigzag MoS2 nanoribbon. The strongest plasmon originates from a metallic edge state localized on the sulfur dimers decorating the Mo edge of the ribbon. A detailed analysis of the dielectric function reveals that the observed deviations from the ideal 1D plasmon behavior result from single-particle transitions between the metallic edge state and the valence and conduction bands of the MoS2 sheet. The Mo and S edges of the ribbon are clearly distinguishable in calculated spatially resolved electron energy loss spectrum owing to the different plasmonic properties of the two edges. The edge plasmons could potentially be utilized for tuning the photocatalytic activity of MoS2 nanoparticles.
Plasmonics takes advantage of the collective response of electrons to electromagnetic waves, enabling dramatic scaling of optical devices beyond the diffraction limit. Here, we demonstrate the mid-infrared (4 to 15 microns) plasmons in deeply scaled graphene nanostructures down to 50 nm, more than 100 times smaller than the on-resonance light wavelength in free space. We reveal, for the first time, the crucial damping channels of graphene plasmons via its intrinsic optical phonons and scattering from the edges. A plasmon lifetime of 20 femto-seconds and smaller is observed, when damping throug…
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure o…
An ab initio theory for Fano resonances in plasmonic nanostructures and metamaterials is developed using Feshbach formalism. It reveals the role played by the electromagnetic modes and material losses in the system, and enables the engineering of Fano resonances in arbitrary geometries. A general formula for the asymmetric resonance in a non-conservative system is derived. The influence of the electromagnetic interactions on the resonance line shape is discussed and it is shown that intrinsic losses drive the resonance contrast, while its width is mostly determined by the coupling strength bet…
A promising trend in plasmonics involves shrinking the size of plasmon-supporting structures down to a few nanometers, thus enabling control over light-matter interaction at extreme-subwavelength scales. In this limit, quantum mechanical effects, such as nonlocal screening and size quantization, strongly affect the plasmonic response, rendering it substantially different from classical predictions. For very small clusters and molecules, collective plasmonic modes are hard to distinguish from other excitations such as single-electron transitions. Using rigorous quantum mechanical computational …
We investigate the excitation of electrostatic wakefields in metallic nanostructures (nanowires) due to the propagation of a short electron pulse. For that purpose, a dispersive (nonlocal) dielectric response of the system is considered, accounting for both the finiteness of the system and the quantum (Bohm) difraction of the conduction electron band, generalizing the results obtained previously in the literature [Phys. Rev. Lett. \textbf{103}, 097403 (2009)]. We discuss on the stability conditions of wakefields and show that the underling mechanism can be useful to investigate new sources of …
Localized plasmons in metallic nanostructures have been widely used to enhance nonlinear optical effects due to their ability to concentrate and enhance light down to extreme-subwavelength scales. As alternatives to noble metal nanoparticles, graphene nanostructures can host long-lived plasmons that efficiently couple to light and are actively tunable via electrical doping. Here we show that doped graphene nanoislands present unique opportunities for enhancing nonlinear optical wave-mixing processes between two externally applied optical fields at the nanoscale. These small islands can support…
In this paper we discuss the field enhancement due to surface plasmons resonances of metallic nanostructures, in particular nano spheres on top of a metal, and find maximum field enhancement of the order of 10^2, intensities enhancement of the order of 10^4. Naturally these fields can produce temporal fields of the order of 0.5V/Å that yield field emission of electrons. Although the fields enhancements we calculated are factor of 10 smaller than those reported in recent experiments, our results explain very well the experimental data. Very large atomic fields destabilize the system completely …
We develop a quantum-mechanical theory for Landau damping of surface plasmons in metal nanostructures larger that the characteristic length for nonlocal effects. We show that the electron surface scattering, which facilitates plasmon decay in small nanostructures, can be incorporated into the metal dielectric function on par with phonon and impurity scattering. The derived surface scattering rate is determined by the plasmon local field polarization relative to the metal-dielectric interface and is highly sensitive to the system geometry. We illustrate our model by providing analytical results…
Hybrid plasmonic devices involve a nanostructured metal supporting localized surface plasmons to amplify light-matter interaction, and a non-plasmonic material to functionalize charge excitations. Application-relevant epitaxial heterostructures, however, give rise to ballistic ultrafast dynamics that challenge the conventional semiclassical understanding of unidirectional nanometal-to-substrate energy transfer. We study epitaxial Au nanoislands on WSe$_2$ with time- and angle-resolved photoemission spectroscopy and femtosecond electron diffraction: this combination of techniques resolves mater…
We develop a unified theory of plasmon-assisted resonance energy transfer (RET) between molecules near a metal nanostructure that maintains energy balance between transfer, dissipation, and radiation. We show that in a wide range of parameters, including in the near field, RET is dominated by plasmon-enhanced radiative transfer (PERT) rather than by a nonradiative transfer mechanism. Our numerical calculations performed for molecules near the Ag nanoparticle indicate that RET magnitude is highly sensitive to molecules' positions.
We develop a theory for spontaneous decay of a quantum emitter (QE) situated near metal-dielectric structure supporting localized surface plasmons. If plasmon resonance is tuned close to the QE emission frequency, the emission is enhanced due to energy transfer from the QE to a localized plasmon mode followed by photon emission by plasmonic antenna. The emission rate is determined by intimate interplay between the plasmon coupling to radiation field and the Ohmic losses in metal. Here we develop plasmon Green's function approach that includes plasmon's interaction with radiation to obtain expl…
A significant interest in combining plasmonics and magnetism at the nanoscale gains momentum in both photonics and magnetism sectors that are concerned with the resonant enhancement of light-magnetic-matter interaction in nanostructures. These efforts result in a considerable amount of literature, which is difficult to collect and digest in limited time. Furthermore, there is insufficient exchange of results between the two research sectors. Consequently, the goal of this review paper is to bridge this gap by presenting an overview of recent progress in the field of magneto-plasmonics from two…
Plasmonic resonance of a metallic nanostructure results from coherent motion of its conduction electrons driven by incident light. At the resonance, the induced dipole in the nanostructure is proportional to the number of the conduction electrons, hence $10^{7}$ times larger than that in an atom. The interaction energy between the induced dipole and fluctuating virtual field of the incident light can reach a few tenths of an eV. Therefore, the classical electromagnetism dominating the field becomes inadequate. We argue that quantum electrodynamics (QED) should be used instead as the fundamenta…
Usually, the liner waveguides with single quantum emitters are utilized as routers to construct the quantum network in quantum information processings. Here, we investigate the influence of the nonlinear dispersion on quantum routing of single surface plasmons, between two metal nanowires with a pair of quantum dots. By using a full quantum theory in real space, we obtain the routing probabilities of a single surface plasmon into the four outports of two plasmonic waveguides scattered by a pair of quantum dots. It is shown that, by properly designing the inter-dot distance and the dot-plasmon …
We demonstrate propagation of plasmons in single crystalline silver nanostructures fabricated using a combination of a bottom-up and a top-down approach. Silver nanoplates of thickness around 65 nm and a surface area of about 100 μm^2 are made using a wet chemical method. Silver nanotips and nanowires are then sculptured by focused ion beam milling. The plasmons are excited by using the fluorescence from the redeposited silver clusters during the milling process. Propagation of plasmons in the nanowires is observed in the visible spectral region. We also observe a cavity effect by measuring th…
The discovery of many fascinating new phenomena associated with the surface plasmon polariton (SPP) has triggered the rapid development of nanophotonics and nanoelectronics. We report here the experimental observation of a fundamentally new physical process, nonlinear electron scattering, stimulated by the SPP excitation of Ag nanostructures on graphite surface in scanning probe electron energy loss spectroscopy. The observed intensity of SPP energy loss peak normalized to the elastic scattering intensity shows clearly a quadratic dependence on the external electric field strength generated by…
Tomonaga-Luttinger (T-L) theory predicts collective plasmon resonances in 1-D nanostructure conductors of finite length, that vary roughly in inverse proportion to the length of the structure. In-depth quantitative understanding of such resonances which have not been clearly identified in experiments so far, would be invaluable for future generations of nano-photonic and nano-electronic devices that employ 1-D conductors. Here we provide evidence of the plasmon resonances in a number of representative 1-D finite carbon-based nanostructures using first-principle computational electronic spectro…
Spectroscopic studies of semiconductor quantum dots (SQDs) addressing the problem of non-radiative carrier losses is vital for the improvement in the efficiency of various light-emitting devices. Various designs of SQDs emitter like doping, forming core-shell and alloying has been attempted to suppress non-radiative recombination. In this article, we show that forming a hybrid with metal nanoparticles (MNP) having localized surface plasmon resonance overlapped with the emission spectrum of SQD, the non-radiative carrier loss via Auger recombination can be mitigated. Using steady-state and time…
Nonreciprocal plasmons in one-dimensional carbon nanostructures
Max-Born-Institut（马克斯·玻恩研究所）；Center for Nanophotonics, NWO Institute AMOLF（纳米光子学中心，NWO AMOLF研究所）；ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（ICFO-光子科学研究所，巴塞罗那科学技术研究所）；ICREA-Institució Catalana de Recerca i Estudis Avançats（ICREA-加泰罗尼亚研究高级学院）；POLIMA—Center for Polariton-driven Light–Matter Interactions, University of Southern Denmark（POLIMA-极化激元驱动光物质相互作用中心，南丹麦大学）；Danish Institute for Advanced Study, University of Southern Denmark（丹麦高等研究院，南丹麦大学）
Metal photoluminescence (MPL) originates from radiative recombination of photoexcited core holes and conduction band electrons. In metal nanostructures, MPL is enhanced due to the surface plasmon local field effect. We identify another essential process in plasmon-assisted MPL - excitation of Auger plasmons by core holes - that hinders MPL from small nanostructures. We develop a microscopic theory of plasmon-enhanced MPL that incorporates both plasmon-assisted enhancement and suppression mechanisms and derive the enhancement factor for MPL quantum efficiency. Our numerical calculations of MPL …
We image the field enhancement at Ag nanostructures using femtosecond laser pulses with a center wavelength of 1.55 micrometer. Imaging is based on non-linear photoemission observed in a photoemission electron microscope (PEEM). The images are directly compared to ultra violet PEEM and scanning electron microscopy (SEM) imaging of the same structures. Further, we have carried out atomic scale scanning tunneling microscopy (STM) on the same type of Ag nanostructures and on the Au substrate. Measuring the photoelectron spectrum from individual Ag particles shows a larger contribution from higher…
Spin and angular momenta of light are important degrees of freedom in nanophotonics which control light propagation, optical forces and information encoding. Typically, optical angular momentum is generated using q-plates or spatial light modulators. Here, we show that graphene-supported plasmonic nanostructures with broken rotational symmetry provide a surprising spin to orbital angular momentum conversion, which can be continuously controlled by changing the electrochemical potential of graphene. Upon resonant illumination by a circularly polarized plane wave, a polygonal array of indium-tin…
Plasmonic excitations such as surface-plasmon-polaritons (SPPs) and graphene-plasmons (GPs), carry large momenta and are thus able to confine electromagnetic fields to small dimensions. This property makes them ideal platforms for subwavelength optical control and manipulation at the nanoscale. The momenta of these plasmons are even further increased if a scheme of metal-insulator-metal and graphene-insulator-metal are used for SPPs and GPs, respectively. However, with such large momenta, their far-field excitation becomes challenging. In this work, we consider hybrids of graphene and metallic…
The plasma wave instabilities in ballistic Field Effect Transistors (FETs) have a promise of developing sensitive THz detectors and efficient THz sources. One of the difficulties in achieving efficient resonant plasmonic detection and generation is assuring proper boundary conditions at the contacts and at the heterointerfaces and tuning the plasma velocity. We propose using the tunable narrow channel regions of an increased width, which we call "stubs" for optimizing the boundary conditions and for controlling the plasma velocity. We developed a compact model for THz plasmonic devices using t…
The plasmon-mediated manipulation of light-matter interaction in two-dimensional atomically transition-metal dichalcogenides (TMDs) critically depends on the design of plasmonic nanostructures to achieve the maximum optical field in TMDs. Here, a metal-isolator-metal Salisbury-type perfect absorber was fabricated to serve as a generator of the localized surface plasmons. The significant photoluminescence (PL) enhancement up to 60-fold was observed experimentally in the monolayer (ML) MoS2 on the top of this gold plasmonic hybrid nanostructures. Furthermore, the PL linear polarization can appro…
Optical properties of metallic nanoparticles are most often considered in terms of plasmons, the coupled states of light and quasi-free electrons. Here we predict that confinement of electrons inside the nanostructure leads to another, very different, type of resonance, which determines the optical properties in the frequency range significantly below the plasmonic resonance. We demonstrate that closely placed confinement-induces resonances typically join into a single composite "super-resonance" which produces giant nonlinearity at low frequencies. Our simulations show how such nonlinearities…
Plasmon-Enhanced Second-Harmonic Generation in Atomically Thin Crystalline Silver Nanostructures
ICFO–Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（ICFO-光子科学研究所，巴塞罗那科学技术研究院）；University of Vienna, Faculty of Physics, Vienna Center for Quantum Science and Technology (VCQ)（维也纳大学物理学院，维也纳量子科学与技术中心）；Center for Nanophotonics, NWO Institute AMOLF（纳米光子学中心，NWO AMOLF研究所）；Department of Physics, Dokuz Eylül University（德古兹埃勒大学物理系）；Centro de Física de Materiales CSIC-UPV/EHU and Materials Physics Center（CSIC-巴斯克国立大学物质物理学中心和材料物理中心）
Optimisation and Precision Tuning of Localised Surface Plasmon Resonance in AuFON Systems
Universidad de Pamplona-Colombia（潘普洛纳大学）；Centro Atómico Bariloche e Instituto Balseiro, Comisión Nacional de Energía Atómica (CNEA) - Universidad Nacional de Cuyo (UNCUYO)（巴里洛切原子中心与巴尔塞罗研究所，国家原子能委员会（CNEA）- 昆卡约国立大学 (UNCUYO)）；Instituto de Nanociencia y Nanotecnología (INN-Bariloche), Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET)（纳米科学与技术研究所（INN-巴里洛切），国家科学研究委员会（CONICET)）
Surface plasmon resonances generated in metallic nanostructures can be utilized to tailor electromagnetic fields. The precise spatial arrangement of such structures can result in surprising optical properties that are not found in any naturally occurring material. Here, the designed activity emerges from collective effects of singular components equipped with limited individual functionality. Top-down fabrication of plasmonic materials with a predesigned optical response in the visible range by conventional lithographic methods has remained challenging due to their limited resolution, the comp…
Intense efforts have been made in recent years to realize nonlinear optical interactions at the single-photon level. Much of this work has focused on achieving strong third-order nonlinearities, such as by using single atoms or other quantum emitters while the possibility of achieving strong second-order nonlinearities remains unexplored. Here, we describe a novel technique to realize such nonlinearities using graphene, exploiting the strong per-photon fields associated with tightly confined graphene plasmons in combination with spatially nonlocal nonlinear optical interactions. We show that i…
We show that free electrons can efficiently excite plasmons in doped graphene with probabilities of order one per electron. More precisely, we predict multiple excitations of a single confined plasmon mode in graphene nanostructures. These unprecedentedly large electron-plasmon couplings are explained using a simple scaling law and further investigated through a general quantum description of the electron-plasmon interaction. From a fundamental viewpoint, multiple plasmon excitations by a single electron provides a unique tool for exploring the bosonic quantum nature of these collective modes.…
