Quantum Plasmonics Research Articles

Plasmonic quantum nonlinear Hall effect in noncentrosymmetric two-dimensional materials

We investigate an interplay between quantum geometrical effects and surface plasmons through surface plasmonic structures, based on an electron hydrodynamic theory. First we demonstrate that the quantum nonlinear Hall effect can be dramatically enhanced over a very broad range of frequency by utilizing plasmonic resonances and near-field effects of grating gates. Under the resonant condition, the enhancement becomes several orders of magnitude larger than the case without the nanostructures, while the peaks of high-harmonic plasmons expand broadly and emerge under the off-resonant condition, leading to a remarkably broad spectrum. Furthermore, we clarify a universal relation between the photocurrent induced by the Berry curvature dipole and the optical absorption, which is essential for computational material design of long-wavelength photodetectors. Next we discuss a novel mechanism of geometrical photocurrent, which originates from an anomalous force induced by oscillating magnetic fields and is described by the dipole moment of orbital magnetic moments of Bloch electrons in the momentum space. Our theory is relevant to 2D quantum materials such as layered WTe${}_2$ and twisted bilayer graphene, thereby providing a promising route toward a novel type of highly sensitive, broadband terahertz photodetectors.

Au Quantum Clusters and Plasmonic Quantum Nanoparticles Synthesized under Femtosecond-Pulse Laser Irradiation in Aqueous Solution and in ZIF-8 for Catalytic Reduction of 4-Nitrophenol

Au Quantum Clusters and Plasmonic Quantum Nanoparticles Synthesized under Femtosecond-Pulse Laser Irradiation in Aqueous Solution and in ZIF-8 for Catalytic Reduction of 4-Nitrophenol

Semiclassical theory for plasmons in spatially inhomogeneous media

Recent progress in experimental techniques has made the quantum regime in plasmonics accessible. Since plasmons correspond to collective electron excitations, the electron–electron interaction plays an essential role in their theoretical description. Within the Random Phase Approximation, this interaction is incorporated through a system of equations of motion, which has to be solved self-consistently. For homogeneous media, an analytical solution can be found using the Fourier transform, giving rise to Lindhard theory. When the medium is spatially inhomogeneous, this is no longer possible and one often uses numerical approaches, which are however limited to smaller systems. In this paper, we present a novel semi-analytical approach for bulk plasmons in inhomogeneous media based on the semiclassical (or WKB) approximation, which is applicable when the charge density varies smoothly. By solving the equations of motion self-consistently, we obtain the expressions of Lindhard theory with a spatially varying Fermi wavevector. The derivation involves passing from the operators to their symbols, which can be thought of as classical observables on phase space. In this way we obtain effective (Hamiltonian) equations of motion for plasmons. We then find the quantized energy levels and the plasmon spectrum using Einstein–Brilllouin–Keller quantization. Our results provide a theoretical basis to describe different setups in quantum plasmonics, such as nanoparticles, quantum dots and waveguides.

Surface plasmaritons: Wave-mechanical and second-quantized theories

In the wake of recently established quantum theories for bulk and surface plasmons, and for bulk plasmaritons [Jung and Keller, Phys. Rev. A 103, 063501 (2021); Phys. Rev. A 104, 053508 (2021)] wave-mechanical and second-quantized (QED) theories for surface plasmaritons are developed. Our photon wave-mechanical theory is based on the covariant four-potential in the Lorenz gauge, where dynamical equations for surface plasmariton quantum particles consisting of scalar ($S$), longitudinal ($L$), and transverse ($T1$, $T2$) photons and driven by a surface current density sheet are obtained. The second quantized QED theory of surface plasmaritons is formulated on the basis of the Heisenberg equations of motion for the contravariant four-potential annihilation operators. The connection of the surface plasmariton quantum theory to the quasiparticle picture of bulk plasmaritons is elucidated by studying the $T$-photon exponential decay lengths appearing in the description. The shortest decay length (equal on both sides of the surface) characterizes the one-dimensional spatial confinement of the $T$-photon source. Starting from a reexamination (and correction) of the dynamic boundary conditions for a flat jellium-vacuum interface carrying a surface current density, the dispersion relation for surface plasmaritons is obtained. The explicit form of the dispersion relation is derived upon a study of the local field in the selvedge region of the boundary. Fundamental aspects of the dispersion relation are pointed out, modeling the electron dynamics by the microscopic electrodynamics of a quantum well. Remarks on (i) our covariant surface plasmariton quantum theory seen in a broader perspective, (ii) suggestions for applications of the theory, and (iii) a comparison of the key ingredients in our trio of papers on plasmon and plasmariton quantum physics are presented.

Plasmonic Photocatalysis with Nonthermalized Hot Carriers

Hot carriers generated by plasmonic damping have been suggested to promote photocatalysis, yet it remains unclear how the nonthermalized hot carriers dynamically activate and promote the energy transfer processes. Here, we present an Anderson-Newns model to describe the vibrational excitation and bond dissociation induced by plasmonic hot carriers. The nonthermal distribution of the hot carriers generated by plasmon damping is accounted for on equal footing with thermal carriers at a given temperature in the electron-molecule scattering. We found that the nonthermal electrons in the high energy region can, albeit in much smaller populations, provide an efficient and dominant channel for photodissociation especially in the low-temperature and quantum plasmon regime. Our model captures the wavelength dependence and reproduces the enhancement factors observed by experiments for oxygen dissociation on silver nanoparticles. It also paves a way to harvesting nonthermal plasmonic energy for photocatalysis in the quantum regime.

Cavity-enhanced magnetic dipole resonance induced hot luminescence from hundred-nanometer-sized silicon spheres

Abstract In this paper, we demonstrate the first example of phonon-assisted hot luminescence (PAHL) emission from silicon (Si) spheres (diameter > 100nm) without using the plasmonic effect or quantum confinement effect. Instead, we excite the hot luminescence of Si by a strong thin-film-cavity-enhanced magnetic dipole resonance. The thin-film cavity (80 nm SiO2/Ag) shows a strong co-enhancement with the magnetic dipole resonance of Si sphere (diameter = 120 nm). The concentrated electromagnetic fields induce significant light–matter interaction. Our Si sphere coupled with a thin-film cavity achieves a 10-fold field enhancement relative to the Si sphere without an enhancement substrate. Furthermore, we experimentally use cavity-enhanced magnetic dipole resonance to a 50-fold enhancement in PAHL. The measured internal quantum efficiency for the visible light emitted from the Si spheres was approximately 2.4%. Furthermore, we demonstrate the tunability of emission peaks merely by adjusting the sizes of Si spheres using thermal oxidation and etching processes. For comparison, we calculated the peak wavelength (λ peak) sensitivities (Δλ peak/ΔDiameter) of Si spheres and Si QDs through Mie theory and effective mass approximation, respectively. The predicated peak sensitivities of the Si spheres ranged from 1.3 to 3.2; they were much more controllable than those of the Si QDs (200–400). Thus, the peak wavelengths of the PAHL of the Si spheres could be modulated and controlled much more precisely and readily than that of the Si QDs. With the tunability and strong electromagnetic field confinement, the cavity-enhanced magnetic dipole resonance appears to have great potential in the development of all-optical processing based on Si photonics.

Switching from electromagnetic to chemical mechanism in quantum plasmonic tip-induced graphene oxide enhanced Raman scattering

Surface-enhanced Raman scattering (SERS) is based on the ability of a surface substrate to increase Raman signals for sensing and imaging applications. The most widely used Au and Ag SERS substrates are primarily based on the electromagnetic mechanism (EM) with large enhancement factors (EFs), which are, however, limited by small gaps due to tunneling. Graphene has been explored as an alternative substrate for graphene-enhanced Raman scattering based on the chemical mechanism (CM). However, the limits of CM EFs in graphene-based substrates have not been well understood, especially as a function of tip-sample distance (TSD). Here we performed tip-enhanced Raman scattering of carbon nanotubes on Au and graphene-oxide (GO) hybrid substrates for different TSDs. We show evidence of quantum plasmonics with GO as a tunneling junction in an Au-GO-Au cavity with a 2-nm gap size. We demonstrate Raman signal enhancement by four orders of magnitude beyond the EM tunneling limit by switching to the CM regime for the resonant GO excitation at small TSD. Tip-induced GO-enhanced Raman scattering may be used to improve nanoimaging and biosensing on novel hybrid GO/Au substrates.

Nanomaterial-based single-molecule optical immunosensors for supersensitive detection

Unlike bulk materials, nanomaterials have unique properties that make them suitable for biosensor applications. Nanomaterial-based biosensors have a series of advantages that can help realize high throughput and ultrasensitive detection. In recent years, considerable research has been performed on integrating nanomaterials and single-molecule immunosensors. This review provides an overview on the various types of nanomaterials used for signal amplification in single-molecule immunosensors, with a focus on the development of optics-based immunosensors using precious plasmonic noble metals (e.g., gold, silver), magnetic beads, quantum dots, upconversion nanoparticles, and nanocomposites. In particular, an approach is presented of using single-molecule immunosensors to detect and quantify biomolecular interactions (e.g., antibody–antigen). Integrating supersensitive bio-devices and nanomaterials is expected to offer significant advantages for trace element diagnosis and early diagnosis.

Smooth Sidewalls on Crystalline Gold through Facet-Selective Anisotropic Reactive Ion Etching: Toward Low-Loss Plasmonic Devices.

Quantum plasmonics aims to harness the deeply subwavelength confinement provided by plasmonic devices to engineer more efficient interfaces to quantum systems in particular single emitters. Realizing this vision is hampered by the roughness-induced scattering and loss inherent in most nanofabricated devices. In this work, we show evidence of a reactive ion etching process to selectively etch gold along select crystalline facets. Since the etch is facet selective, the sidewalls of fabricated devices are smoother than the lithography induced line-edge roughness with the prospect of achieving atomic smoothness by further optimization of the etch chemistry. This opens up a route toward fabricating integrated plasmonic circuits that can achieve loss metrics close to fundamental bounds.

Plasmonic Waveguides: Enhancing quantum electrodynamic phenomena at nanoscale

The emerging field of plasmonics can lead to enhanced light matter interactions at extremely nanoscale regions. Plasmonic (metallic) devices promise to efficiently control both classical and quantum properties of light. Plasmonic waveguides are usually used to excite confined electromagnetic modes at the nanoscale that can strongly interact with matter. The analysis of these nanowaveguides exhibits similarities with their low frequency microwave counterparts. In this article, we review ways to study plasmonic nanostructures coupled to quantum optical emitters from a classical electromagnetic perspective. These quantum emitters are mainly used to generate single photon quantum light that can be employed as a quantum bit or qubit in the envisioned quantum information technologies. We demonstrate different ways to enhance a diverse range of quantum electrodynamic phenomena based on plasmonic configurations by using the classical dyadic tensor Green function formalism. More specifically, spontaneous emission and superradiance are analyzed by using the Green function based field quantization. The exciting new field of quantum plasmonics will lead to a plethora of novel optical devices for communications and computing applications operating in the quantum realm, such as efficient single-photon sources, quantum sensors, and compact on-chip nanophotonic circuits.

Quantum surface effects in the electromagnetic coupling between a quantum emitter and a plasmonic nanoantenna: time-dependent density functional theory vs. semiclassical Feibelman approach.

We use time-dependent density functional theory (TDDFT) within the jellium model to study the impact of quantum-mechanical effects on the self-interaction Green's function that governs the electromagnetic interaction between quantum emitters and plasmonic metallic nanoantennas. A semiclassical model based on the Feibelman parameters, which incorporates quantum surface-response corrections into an otherwise classical description, confirms surface-enabled Landau damping and the spill out of the induced charges as the dominant quantum mechanisms strongly affecting the nanoantenna-emitter interaction. These quantum effects produce a redshift and broadening of plasmonic resonances not present in classical theories that consider a local dielectric response of the metals. We show that the Feibelman approach correctly reproduces the nonlocal surface response obtained by full quantum TDDFT calculations for most nanoantenna-emitter configurations. However, when the emitter is located in very close proximity to the nanoantenna surface, we show that the standard Feibelman approach fails, requiring an implementation that explicitly accounts for the nonlocality of the surface response in the direction parallel to the surface. Our study thus provides a fundamental description of the electromagnetic coupling between plasmonic nanoantennas and quantum emitters at the nanoscale.

Dyadic Helmholtz Green’s Function for Electromagnetic Wave Transmission/Diffraction through a Subwavelength Nano-Hole in a 2D Quantum Plasmonic Layer: An Exact Solution Using “Contact Potential”-like Dirac Delta Functions

The dyadic Helmholtz Green’s function for electromagnetic (EM) wave transmission/ diffraction through a subwavelength nano-hole in a two-dimensional (2D) plasmonic layer is discussed here analytically and numerically, employing “contact potential”-like Dirac delta functions in 1 and 2 dimensions (δ(z) and δ(x)δ(y)≡δ(2)(r→)). This analysis is carried out employing a succession of two coupled integral equations. The first integral equation determines the dyadic electromagnetic Green’s function G^fs for the full non-perforated 2D quantum plasma layer in terms of the bulk 3D infinite-space dyadic electromagnetic Green’s function G^3D, with δ(z) representing the confinement of finite quantum plasma conductivity to the plane of the plasma layer at z=0. The second integral equation determines the dyadic electromagnetic “hole” Green’s function G^hole for the perforated 2D quantum plasma layer (containing the nano-hole) in terms of the dyadic electromagnetic Green’s function G^fs for the full non-perforated 2D plasma layer, with δ(2)(r→) describing the exclusion of the quantum plasma layer conductivity properties from the nano-hole region in the vicinity of r→=0 on the plane. Taking the radius of the subwavelength nano-hole to be the smallest length scale of the system in conjunction with the 2D Dirac delta function representation of the excluded nano-hole plasma conductivity, both of the successive coupled integral equations are solved exactly, and we present a thorough numerical analysis (based on the exact analytic solution) for the resulting dyadic “hole” Green’s function G^hole in full detail in both 3D and density plots. This result has been successfully applied to the determination of electromagnetic wave transmission/diffraction through the nano-hole of the perforated quantum plasmonic layer, jointly with the EM wave transmission through the rest of the plasma layer. This success necessarily involves spatial translational asymmetry induced by the use of spatial Dirac delta functions confining finite conductivity to the 2D quantum plasma sheet and the excision at a bit of it about the origin to represent the nano-hole perforation, thus breaking spatial translational invariance symmetry.

Efficient exciton generation in a semiconductor quantum-dot–metal-nanoparticle composite structure using conventional chirped pulses

We consider a nanostructure consisting of a semiconductor quantum dot coupled to a metal nanoparticle, and show with numerical simulations that the exciton state of the quantum dot can be robustly generated from the ground state even for small interparticle distances, using conventional chirped pulses with Gaussian and hyperbolic secant envelopes. The asymmetry observed in the final exciton population with respect to the chirp sign of the applied pulses is explained using the nonlinear density matrix equations describing the system, and is attributed to the real part of the parameter emerging from the interaction between excitons in the quantum dot and plasmons in the metal nanoparticle. The simplicity of the conventional chirped pulses, which can also be easily implemented in the laboratory, make the proposed robust quantum control scheme potentially useful for the implementation of ultrafast nanoswitches and quantum information processing tasks with semiconductor quantum dots.

Direct Electro Plasmonic and Optic Modulation via a Nanoscopic Electron Reservoir.

Direct electrical tuning of localized plasmons at optical frequencies boasts the fascinating prospects of being ultrafast and energy efficient and having an ultrasmall footprint. However, the prospects are obscured by the grand challenge of effectively modulating the very large number of conduction electrons in three-dimensional metallic structures. Here we propose the concept of nanoscopic electron reservoir (NER) for direct electro plasmonic and electro-optic modulation. A NER is a few-to-ten-nanometer size metal feature on a metal host and supports a localized plasmon mode. We provide a general guideline to construct highly electrically susceptible NERs and theoretically demonstrate pronounced direct electrical tuning of the plasmon mode by exploiting the nonclassical effects of conduction electrons. Moreover, we show the electro-plasmonic tuning can be efficiently translated into modulation of optical scattering by utilizing the antenna effect of the metal host for the NER. Our work extends the landscape of electro plasmonic modulation and opens appealing new opportunities for quantum plasmonics.

Quantum plasmonics of few electrons in strongly confined doped semiconducting oxide: A DFT + U study of ZnGaO

It has been reported in photodoping experiments that localized surface plasmonic resonances can be sustained with electrons as few as 3. We performed first principles calculations of density functional theory, with the Hubbard U correction, to see if localized surface plasmonic resonances can also be sustained by doping a wide bandgap ZnO with few shallow donors of Ga. We distributed 3–6 dopants approximately uniformly, due to quasi-spherical geometry of the quantum dot, in the dilute doping limit. The uniform distribution of dopants in quantum dots has been reported experimentally. Although the dopant configurations are limited due to computational cost, our findings shed light on absorption trends. Results for quantum dots of 1.4 nm, passivated with pseudo-hydrogens, show that localized surface plasmonic resonances can be generated in the near infrared range. The absorption linewidths for such small-sized quantum dots are broad. We find that the resonance linewidth depends on the orientation of surfaces and the number of secondary peaks on the concentration of dopants. The absorption coefficients, as functions of the principal values of the dielectric tensor, indicate that an electric field with orientation parallel to that of the most symmetric surface will produce localized surface plasmonic resonances with high quality factors.

Regular quantum plasmons in segments of graphene nanoribbons

Graphene plasmons have advantages over noble metal plasmons such as high tunability and low loss. However, for graphene nanostructures smaller than 10 nm, little is known about their plasmons or whether regular plasmonic behavior exists, despite their potential applications. Here, we present first-principles calculations of plasmon excitations in zigzag graphene nanoribbon segments. Very regular plasmonic behavior is found: Only one plasmon mode exists in the low-energy regime ([Formula: see text] eV). The classical electrostatic scaling law still approximately holds when the width ([Formula: see text]) is larger than [Formula: see text] nm but totally fails when [Formula: see text] nm due to quantum effects. The scaling with different doping densities shows that the plasmon is nearly free-electron plasmon instead of Dirac plasmon.

Transient Out‐of‐Equilibrium Nucleic Acid‐Based Dissipative Networks and Their Applications

AbstractDynamic, dissipative reactions play important roles in biological processes, and emulating such biological processes by artificial circuits and networks is a challenging topic in the area of Systems Chemistry. The present article summarizes efforts to apply the information encoded in the base sequence of nucleic acids to assemble transient, dissipative DNA‐based networks mimicking natural processes. The design principles of the transient nucleic acid‐based systems are introduced. Triggered reaction moduli lead to a transient intermediary constituent recovered to the parent moduli by enzymes, DNAzyme, or light as control units are described. Transient DNA‐based circuitries of enhanced complexities revealing temporal gated or cascaded transformations are demonstrated. Different applications of dynamically triggered transient circuits are introduced, including the temporal aggregation and deaggregation of plasmonic nanoparticles or semiconductor quantum dots and the control over their optical properties, the transient release and uptake of loads by aptamer scaffolds, and the transient reconfiguration of constitutional dynamic networks and the control over emergent catalytic functions. The future perspectives of dissipative nucleic acid‐based networks and their potential future applications are discussed.

Behavior Comparison of Plasmons in a Multiple Quantum well in Quantum Dots-type Superlattice

Behavior Comparison of Plasmons in a Multiple Quantum well in Quantum Dots-type Superlattice

Detecting nonlocality by second-harmonic generation from a graphene-wrapped nanoparticle.

With the rapid development of nanofabrication technology and nonlinear optics, the nonlinear detection by nanostructures is highly appreciated. In this paper, we study the second-harmonic generation by a spherical nonlocal plasmonic nanoparticle wrapped with graphene. We develop a simple method for calculating the electric field at second-harmonic frequency and analyze the influence of the nonlocal response of the metal on the second-harmonic. We find that this nanostructure can probe the material's properties by detecting the radiation intensity of the second-harmonic generation. In addition, the nonlocal response of the plasmonic core can promote the absorption efficiency of second-harmonic generation. Our study may offer a new way for studying the plasmonic quantum effects and nonlinear probing technology and improving the nonlinear conversion efficiency of photonic devices.

Plasmonic InAs quantum dot MSM nanolaser with low threshold gain

Plasmonic InAs quantum dot MSM nanolaser with low threshold gain