Single Plasmon Research Articles

Probing Decoherence in Plasmonic Waveguides in the Quantum Regime

We experimentally investigate the decoherence of single surface plasmon polaritons in metal stripe waveguides. In our study we use a Mach-Zehnder configuration previously considered for measuring decoherence in atomic, electronic and photonic systems. By placing waveguides of different length in one arm we are able to measure the amplitude damping time T_1 = 1.90 +/- 0.01 x 10^-14 s, pure phase damping time T_2^* = 11.19 +/- 4.89 x 10^-14 s and total phase damping time T_2 = 2.83 +/- 0.32 x 10^-14 s. We find that decoherence is mainly due to amplitude damping and thus loss arising from inelastic electron and photon scattering plays the most important role in the decoherence of plasmonic waveguides in the quantum regime. However, pure phase damping is not completely negligible. The results will be useful in the design of plasmonic waveguide systems for carrying out phase-sensitive quantum applications, such as quantum sensing. The probing techniques developed may also be applied to other plasmonic nanostructures, such as those used as nanoantennas, as unit cells in metamaterials and as nanotraps for cold atoms.

Amplified emission and lasing in a plasmonic nanolaser with many three-level molecules

Steady-state plasmonic lasing is studied theoretically for a system consisting of many dye molecules arranged regularly around a gold nano-sphere. A three-level model with realistic molecular dissipation is employed to analyze the performance as function of the pump field amplitude and number of molecules. Few molecules and moderate pumping produce a single narrow emission peak because the excited molecules transfer energy to a single dipole plasmon mode by amplified spontaneous emission. Under strong pumping, the single peak splits into broader and weaker emission peaks because two molecular excited levels interfere with each other through coherent coupling with the pump field and with the dipole plasmon field. A large number of molecules gives rise to a Poisson-like distribution of plasmon number states with a large mean number characteristic of lasing action. These characteristics of lasing, however, deteriorate under strong pumping because of the molecular interference effect.

Homogeneous spectral broadening of pulsed terahertz quantum cascade lasers by radio frequency modulation.

The authors present an experimental investigation of radio frequency modulation on pulsed terahertz quantum cascade lasers (QCLs) emitting around 4.3 THz. The QCL chip used in this work is based on a resonant phonon design which is able to generate a 1.2 W peak power at 10 K from a 400-µm-wide and 4-mm-long laser with a single plasmon waveguide. To enhance the radio frequency modulation efficiency and significantly broaden the terahertz spectra, the QCLs are also processed into a double-metal waveguide geometry with a Silicon lens out-coupler to improve the far-field beam quality. The measured beam patterns of the double-metal QCL show a record low divergence of 2.6° in vertical direction and 2.4° in horizontal direction. Finally we perform the inter-mode beat note and terahertz spectra measurements for both single plasmon and double-metal QCLs working in pulsed mode. Since the double-metal waveguide is more suitable for microwave signal transmission, the radio frequency modulation shows stronger effects on the spectral broadening for the double-metal QCL. Although we are not able to achieve comb operation in this work for the pulsed lasers due to the large phase noise, the homogeneous spectral broadening resulted from the radio frequency modulation can be potentially used for spectroscopic applications.

Nanoplasmonic Alloy of Au/Ag Nanocomposites on Paper Substrate for Biosensing Applications.

Plasmonic alloy has attracted much interest in tailoring localized surface plasmon resonance (LSPR) for recent biosensing techniques. In particular, paper-based plasmonic substrates allow capillary-driven lateral flow as well as three-dimensional metal nanostructures, and therefore they become actively transferred to LSPR-based biosensing such as surface-enhanced Raman spectroscopy (SERS) or metal-enhanced fluorescence (MEF). However, employing plasmonic alloy nanoislands on heat-sensitive substrate is still challenging, which significantly inhibits broad-range tailoring of the plasmon resonance wavelength (PRW) for superior sensitivity. Here we report paper-based plasmonic substrate with plasmonic alloy of Au/Ag nanocomposites for highly sensitive MEF and SERS biosensing applications. The nanofabrication procedures include concurrent deposition of Au and Ag below 100 °C without any damage on cellulose fibers. The Au/Ag nanocomposites feature nanoplasmonic alloy with single plasmon peak as well as broad-range tunability of PRW by composition control. This paper-based plasmonic alloy substrate enables about twofold enhancement of fluorescence signals and selective MEF after paper chromatography. The experimental results clearly demonstrate extraordinary enhancement in SERS signals for picomolar detection of folic acid as a cancer biomarker. This new method provides huge opportunities for fabricating plasmonic alloy on heat-sensitive substrate and biosensing applications.

Influence of the flip–flop interaction on a single plasmon transport in 1D waveguide

Transport of a single plasmon in the 1D waveguide coupled to two emitters with the flip–flop interaction is discussed theoretically via the real-space approach. We showed that the transmission and reflection of a single plasmon could be changeable by adjusting the flip–flop coupling strength of the QDs, the interaction of QDs with the metallic nanowaveguide, interparticle distance of the QDs and detuning. Setting the interparticle distances properly results in the switching between the complete transmission and the complete reflection. Especially, our results show that the QDs with the flip–flop interaction play important role in the transport of the propagating single plasmon, which is relevant to the Forster resonance energy transfer from donor QD to acceptor QD.

Splitting of the ultraviolet plasmon resonance from controlling FePt nanoparticles morphology

We show a designed FePt nanoparticles for embedding in a single crystal MgO matrix and demonstrate plasmon resonance absorption can appear in the ultraviolet region. The state of the FePt alloy is confirmed by X-ray photoelectron spectroscopy and selected area electron diffraction. By increasing the laser energy density from 4 to 6 J/cm2, the shape of the FePt nanoparticles is changed from quasi-spherical to quasi-elliptical. Compared with pure MgO, a single plasmon resonance peak at 234 nm was found in the ultraviolet region for the embedded FePt. Increasing the laser energy density induces peak splitting into two peaks, located at 225 and 262 nm, respectively. With a high laser energy density, a red-shift and a blue-shift are observed for the two peaks, respectively. These results are accordance with the theoretical calculations. The ultraviolet plasmon resonance absorption for FePt NPs can be tuned by changing the shape of the nanoparticles.

Dynamically controllable plasmon induced transparency based on hybrid metal-graphene metamaterials

Novel hybrid metal-graphene metamaterials featuring dynamically controllable single, double and multiple plasmon induced transparency (PIT) windows are numerically explored in the terahertz (THz) regime. The designed plasmonic metamaterials composed of a strip and a ring with graphene integration generate a novel PIT window. Once the ring is divided into pairs of asymmetrical arcs, double PIT windows both with the spectral contrast ratio 100% are obtained, where one originates from the destructive interference between bright-dark modes, and the other is based on the interaction of bright-bright modes. Just because the double PIT windows are induced by two different mechanisms, the continuously controllable conductivity and damping of graphene are employed to appropriately interpret the high tunability in double transparency peaks at the resonant frequency, respectively. Moreover, multiple PIT windows can be achieved by introducing an additional bright mode to form the other bright-bright modes coupling. At the PIT transparent windows, the dispersions undergo tremendous modifications and the group delays reach up to 43 ps, 22 ps, and 25 ps, correspondingly. Our results suggest the existence of strong interaction between the monolayer graphene layer and metal-based resonant plasmonic metamaterials, which may hold widely applications in filters, modulators, switching, sensors and optical buffers.

Panchromatic thin perovskite solar cells with broadband plasmonic absorption enhancement and efficient light scattering management by Au@Ag core-shell nanocuboids

Enhancing the low-energy sunlight harvesting is of great importance for improving the efficiency of organic-inorganic halide perovskite solar cells (PSCs) but still remains a big challenge. Herein, we propose an improved light harvesting and management strategy by using rationally-designed Au@Ag core-shell nanocuboids as plasmonic inclusions, aiming at achieving panchromatic thin PSCs. Compared to conventional metal nanostructures with a single narrow plasmon resonance band, the Au@Ag nanocuboids exhibit multiple broader and stronger plasmon resonances that can be tuned by adjusting structural dimensions to spectrally match the absorption band of the perovskite, particularly in its weak absorption region. By carefully tailoring the location of the Au@Ag nanocuboids in the electrodes, both plasmonic near-field enhancement and increased light-scattering effects can be fully exploited to boost up the performance of the PSCs. As a result, the hybrid devices demonstrate high photon-to-electron conversion efficiency (IPCE) over the entire visible range, with a remarkable IPCE enhancement (ΔIPCE/IPCE) of 20–60% in the range of 550–750nm, compared with pristine devices. This also leads to an average power conversion efficiency (PCE) of 17.83% for the optimized Au@Ag incorporated cells, with a champion PCE of 18.31% recorded for the best plasmonic PSC, corresponding to a PCE enhancement of 20.8%.

Quantum random number generation using an on-chip plasmonic beamsplitter

We report an experimental realisation of a quantum random number generator using a plasmonic beamsplitter. Free-space single photons are converted into propagating single surface plasmon polaritons on a gold stripe waveguide via a grating. The surface plasmons are then guided to a region where they are scattered into one of two possible outputs. The presence of a plasmonic excitation in a given output determines the value of a random bit generated from the quantum scattering process. Using a stream of single surface plasmons injected into the beamsplitter we achieve a quantum random number generation rate of 2.37 Mbits s−1 even in the presence of loss. We characterise the quality of the random number sequence generated, finding it to be comparable to sequences from other quantum photonic-based devices. The compact nature of our nanophotonic device makes it suitable for tight integration in on-chip applications, such as in quantum computing and communication schemes.

Remote preparation of single-plasmon states

Quantum entanglement is a stunning consequence of the superposition principle. This universal property of quantum systems has been intensively explored with photons, atoms, ions and electrons. Collective excitations such as surface plasmons exhibit quantum behaviors. For the first time, we report an experimental evidence of non-local control of single plasmon interferences through entanglement of a single plasmon with a single photon. We achieved photon-plasmon entanglement by converting one photon of an entangled photon pair into a surface plasmon. The plasmon is tested onto a plasmonic platform in a Mach-Zehnder interferometer. A projective measurement on the polarization of the photon allows the non-local control of the interference state of the plasmon. Entanglement between particles of various natures paves the way to the design of hybrid systems in quantum information networks.

Interparticle Coupling Effects of Two Quantum Dots System on the Transport Properties of a Single Plasmon

Transport properties of a single plasmon interacting with two quantum dots (QDs) system coupled to one-dimensional surface plasmonic waveguide are investigated theoretically via the real-space approach. We mainly focus on the coupling effects of the two QDs on the transmission properties of a single incident plasmon. We demonstrated that switching of a single plasmon can be achieved by controlling the interparticle distance, the interparticle coupling strength, and the QD-waveguide coupling strength, as well as spectral detuning. We also showed that the coupling between the continuum excitations and the discrete excitations results in the Fano-type transmission spectrum. The transport properties of a single plasmon interacting with such a two direct coupled QDs system could find the applications in the design of plasmonic nanodevices, such as single photon switching and nanomirrors, and in quantum information processing.

Terahertz and mid-infrared plasmons in three-dimensional nanoporous graphene

Two-dimensional (2D) graphene emerged as an outstanding material for plasmonic and photonic applications due to its charge-density tunability, high electron mobility, optical transparency and mechanical flexibility. Recently, novel fabrication processes have realised a three-dimensional (3D) nanoporous configuration of high-quality monolayer graphene which provides a third dimension to this material. In this work, we investigate the optical behaviour of nanoporous graphene by means of terahertz and infrared spectroscopy. We reveal the presence of intrinsic 2D Dirac plasmons in 3D nanoporous graphene disclosing strong plasmonic absorptions tunable from terahertz to mid-infrared via controllable doping level and porosity. In the far-field the spectral width of these absorptions is large enough to cover most of the mid-Infrared fingerprint region with a single plasmon excitation. The enhanced surface area of nanoporous structures combined with their broad band plasmon absorption could pave the way for novel and competitive nanoporous-graphene based plasmonic-sensors.

Homogeneous spectral spanning of terahertz semiconductor lasers with radio frequency modulation

Homogeneous broadband and electrically pumped semiconductor radiation sources emitting in the terahertz regime are highly desirable for various applications, including spectroscopy, chemical sensing, and gas identification. In the frequency range between 1 and 5 THz, unipolar quantum cascade lasers employing electron inter-subband transitions in multiple-quantum-well structures are the most powerful semiconductor light sources. However, these devices are normally characterized by either a narrow emission spectrum due to the narrow gain bandwidth of the inter-subband optical transitions or an inhomogeneous broad terahertz spectrum from lasers with heterogeneous stacks of active regions. Here, we report the demonstration of homogeneous spectral spanning of long-cavity terahertz semiconductor quantum cascade lasers based on a bound-to-continuum and resonant phonon design under radio frequency modulation. At a single drive current, the terahertz spectrum under radio frequency modulation continuously spans 330 GHz (~8% of the central frequency), which is the record for single plasmon waveguide terahertz lasers with a bound-to-continuum design. The homogeneous broadband terahertz sources can be used for spectroscopic applications, i.e., GaAs etalon transmission measurement and ammonia gas identification.

Controlling plasmon modes and damping in buckled two-dimensional material open systems

Full ranges of both hybrid plasmon-mode dispersions and their damping are studied systematically by our recently developed mean-field theory in open systems involving a conducting substrate and a two-dimensional (2D) material with a buckled honeycomb lattice, such as silicene, germanene, and a group IV dichalcogenide as well. In this hybrid system, the single plasmon mode for a free-standing 2D layer is split into one acoustic-like and one optical-like mode, leading to a dramatic change in the damping of plasmon modes. In comparison with gapped graphene, critical features associated with plasmon modes and damping in silicene and molybdenum disulfide are found with various spin-orbit and lattice asymmetry energy bandgaps, doping types and levels, and coupling strengths between 2D materials and the conducting substrate. The obtained damping dependence on both spin and valley degrees of freedom is expected to facilitate measuring the open-system dielectric property and the spin-orbit coupling strength of individual 2D materials. The unique linear dispersion of the acoustic-like plasmon mode introduces additional damping from the intraband particle-hole modes, which is absent for a free-standing 2D material layer, and the use of molybdenum disulfide with a large bandgap simultaneously suppresses the strong damping from the interband particle-hole modes.

Formation of bimetallic dumbbell shaped particles with a hollow junction during galvanic replacement reaction.

The galvanic replacement reaction (GRR) has been shown to be an effective method to fine tune the structure of monometallic nanoparticles by controlling the precursor concentration and surface ligands. However, the structural evolution of nanoparticles is not well understood in multimetallic systems, where along with oxidation, dealloying and diffusion occur simultaneously. Here, we demonstrate that by controlling the rate of GRR in AuCu alloy nanorods, they can be transformed into either AuCu hollow rods or AuCu@Au core-shell spheroids. Interestingly, the transformation of rods into spheroids involved a critical intermediate state with a hollow junction and dumbbell shape. The formation of a hollow junction region was attributed to preferential diffusion of Cu atoms to the tips caused by the polycrystallinity and high curvature of the tips of the initial template. This structural transformation was also monitored in situ by single particle scattering spectroscopy. The coupling between the two ends of the dumbbell-shaped intermediate connected with a hollow metallic junction gives rise to additional plasmonic features compared with regular rods. Electrodynamic simulations showed that varying the dimensions of the hollow part by even one nanometer altered the plasmon resonance wavelength and lineshape drastically. This study shows that single particle plasmon resonance can be used as an exquisite tool to probe the internal structure of the nanoscale junctions.

Far-field analysis of third-order distributed feedback terahertz quantum cascade lasers

The single lobe far-field patterns produced from terahertz quantum cascade lasers (QCLs) are greatly demanded for various applications, such as imaging, data transmission, etc. However, for a ridge waveguide terahertz QCL, the far-field beam divergence is large due to the fact that the waveguide aperture is far smaller than the terahertz wavelength. This is the case typically for double-metal waveguide terahertz QCL which emits terahertz photons in almost every direction in the space. Even for a single plasmon waveguide terahertz QCL, the divergence angle is as large as 30 in both horizontal and vertical direction. Here, in this work we design and fabricate a double metal third-order distributed feedback terahertz QCL emitting around 4.3 THz, and investigate the characteristics of the longitudinal and transverse modes. This work aims to achieve high beam quality for terahertz QCL by exploiting the third-order distributed feedback geometry, and in the meantime to achieve single longitudinal mode operation. The electromagnetic field distribution in the waveguide is modelled by employing a finite element method. The mode selection mechanism is studied by using the eigen frequency analysis, and the far-field beam is simulated by applying the near-field to far-field Fourier transform technique. The QCL active region used in this work is based on the resonant-phonon design, which is grown by a molecular beam epitaxy (MBE) system on a semi-insulating GaAs (100) substrate. The wafer bonding and traditional semiconductor device fabrication technology, i.e., optical lithography, electron beam evaporation, lift-off, wet and dry etching, are used to process the MBE-growth wafer into the third-order distributed feedback geometry with double-metal waveguides. By carefully designing the grating structures and optimizing the fabrication process, we achieve third-order distributed feedback terahertz QCL with quasi-single-longitudinal mode operation and single lobe far-field beam pattern with low beam divergence in both vertical and horizontal directions. The effect of grating duty cycle on the far-field beam divergence is systematically studied theoretically and experimentally. By the simulation, we finally achieve the divergence angle of 1213 for a third-order distributed feedback laser with a grating duty cycle of 12% that results in an effective refractive index close to 3. The experimental results show good agreement with the simulation. There is still room to further reduce the beam divergence of third-order distributed feedback terahertz QCL by improve the accuracy of the simulation and the fabrication.

High performance 4.7 THz GaAs quantum cascade lasers based on four quantum wells

GaAs/AlGaAs quantum cascade lasers based on four quantum well structures operating at 4.7 THz are reported. A large current density dynamic range is observed, leading to a maximum operation temperature of 150 K for the double metal waveguide device and a high peak output power more than 200 mW for the single surface plasmon waveguide device. A continuous wave, single mode, third order distributed feedback laser with a low electrical power dissipation and a narrow far-field beam pattern, which is required for a local oscillator in astronomy heterodyne spectrometers, is also demonstrated.

Síntese de biofilmes de Quitosana reticulados com Tripolifosfato atuando como agente quelante na fixação de nanopartículas de Prata

Silver nanoparticles have been incorporated in the various materials, using different complexation agents. The work aims at the incorporation of silver nanoparticles in biofilms of chitosan using as agent crosslinker and complexing sodium tripolyphosphate. We used the method of reduction of silver salts in aqueous medium for synthesis of nanoparticles, determining the through the analysis of their plasmonic band by UV-Vis spectrophotometry. In order to compare the efficiency of tripolyphosphate was used biofilms non-crosslinked and filter paper as material control. The analyses in UV-Vis showed the presence of a single plasmon band centered around 400 nm, which is indicative of nanoparticles with spherical shape. Studies of incorporation of the silver nanoparticles showed the efficiency of tripolyphosphate in fixing, complexing all the silver colloidal solution tested in comparison to others materials, thus proving the efficiency of tripolyphosphate as a chelating agent in the fixation of silver nanoparticles. Keywords: Silver nanoparticles, chitosan, tripolyphosphate, polymer, adsorption.

Chitosan stabilized Ag-Au nanoalloy for colorimetric sensing and 5-Fluorouracil delivery

Fluorescent CS/Ag-Au (chitosan/silver-gold) nanocomposite containing different weight percentage of Ag and Au was synthesized using the chemical reduction method. 5-Fluorouracil (5-FU) encapsulated nanocomposite was also synthesized and its cytotoxicity towards breast cancer cell lines (MCF-7) studied. The XRD pattern of the nanocomposite shows peaks of chitosan, silver and gold. The peaks corresponding to gold and silver indicate the face centered cubic structure of silver and gold nanoparticles. The polymer matrix nanocomposite structure with chitosan as the matrix and silver-gold as the filler phase is evident from the high resolution transmission electron microscopy (HRTEM) images and an increase in particle size from∼5nm to about 12nm is noticeable on encapsulation of 5-Fluorouracil (5-FU). The presence of fluorine in the case of 5-FU encapsulated nanocomposite and the presence of reflections corresponding to 5-FU in the SAED pattern confirms the encapsulation of 5-FU into the nanocomposite, which is also confirmed by elemental mapping. The presence of a single surface plasmon resonance (SPR) peak in the case of the nanocomposite in a position in between the SPR bands of pure silver and gold nanoparticles confirms the formation of Ag-Au alloy and the elemental mapping results obtained for the nanocomposite also supports the UV–vis results. The photoluminescence (PL) spectrum clearly shows an emission peak in the near infrared region (700–900nm), which makes the nanocomposite suitable for use in cellular imaging. The application of the nanocomposite as a colorimetric sensor was also studied and it was found to be useful for the specific detection of mercury (Hg) without much interference and the detection limit was found to be 5.0×10−8M.

Visible quantum plasmonics from metallic nanodimers

We report theoretical evidence that bulk nonlinear materials weakly interacting with highly localized plasmonic modes in ultra-sub-wavelength metallic nanostructures can lead to nonlinear effects at the single plasmon level in the visible range. In particular, the two-plasmon interaction energy in such systems is numerically estimated to be comparable with the typical plasmon linewidths. Localized surface plasmons are thus predicted to exhibit a purely nonclassical behavior, which can be clearly identified by a sub-Poissonian second-order correlation in the signal scattered from the quantized plasmonic field under coherent electromagnetic excitation. We explicitly show that systems sensitive to single-plasmon scattering can be experimentally realized by combining electromagnetic confinement in the interstitial region of gold nanodimers with local infiltration or deposition of ordinary nonlinear materials. We also propose configurations that could allow to realistically detect such an effect with state-of-the-art technology, overcoming the limitations imposed by the short plasmonic lifetime.