Atomic sized plasmonic tunnel junctions are of fundamental interest, with great promise as the smallest on-chip light sources in various optoelectronic applications. Several mechanisms of light emission in electrically driven plasmonic tunnel junctions have been proposed, from single-electron or higher order multi-electron inelastic tunneling to recombination from a steady-state population of hot carriers. By progressively altering the tunneling conductance of an aluminum junction, we tune the dominant light emission mechanism through these possibilities for the first time, finding quantitative agreement with theory in each regime. Improved plasmonic resonances in the energy range of interest increase photon yields by two orders of magnitude. These results demonstrate that the dominant emission mechanism is set by a combination of tunneling rate, hot carrier relaxation timescales, and junction plasmonic properties.
A class of hybrid photonic-plasmonic structures (HPPS) with vertical cylindrical cavities is proposed and its performance in providing a coherent light from spontaneous emission is investigated. It is shown that the proposed easy-to-fabricate and robust anodic aluminum oxide structure dramatically enhances the temporal and spatial coherence compared to the previously examined HPPS. The physical mechanism of achieving the temporal and spatial coherence is explained based on the special optical properties of the proposed HPPS and it is discussed how this structure enables one adjusting hybrid ph…
Plasmonic devices have advanced significantly in the past decade. Being one of the most intriguing devices, plamonic nanolasers plays an important role in biomedicine, chemical sensor, information technology, and optical integrated circuits. However, nanoscale plasmonic devices, particularly in ultraviolet regime, are extremely sensitive to metal and interface quality, which renders the development of ultraviolet plasmonics. Here, by addressing the material issues, we demonstrate a low threshold, high characteristic temperature metal-oxide-semiconductor ZnO nanolaser working at room temperatur…
Plasmonics applications have been extending into the ultraviolet region of the electromagnetic spectrum. Unfortunately the commonly used noble metals have intrinsic optical properties that limit their use above 350 nm. Aluminum is probably the most suitable material for UV plasmonics and in this work we show that nanoporous aluminum can be prepared starting from an alloy of Mg3Al2. The porous metal is obtained by means of a galvanic replacement reaction. Such a nanoporous metal can be exploited to achieve a plasmonic material for enhanced UV Raman spectroscopy and fluorescence. Thanks to the l…
Aluminum, as a metallic material for plasmonics, is of great interest because it extends the applications of surface plasmon resonance into the ultraviolet (UV) region and excels noble metals in the natural abundance, cost and compatibility with modern semiconductor fabrication process. Here, we present UV to near-infrared (NIR) plasmonic resonance of single-crystalline aluminum nanoslits and nanoholes. The high-definition nanostructures are fabricated with focused ion-beam (FIB) milling into an ultrasmooth single-crystalline aluminum film grown on a semiconducting GaAs substrate with molecula…
Plasmonic nanocrystals with hot spots are able to localize optical energy in small spaces. In such physical systems, near-field interactions between molecules and plasmons can become especially strong. This paper considers the case of a nanoparticle dimer and a chiral biomolecule. In our model, a chiral molecule is placed in the gap between two plasmonic nanoparticles, where the electromagnetic hot spot occurs. Since many important biomolecules have optical transitions in the UV, we consider the case of Aluminum nanoparticles, as they offer strong electromagnetic enhancements in the blue and U…
Numerous applications of nanotechnologies rely on the wide availability of high-quality crystalline nanoparticles (NPs). Although the chemical synthesis of noble metal nanoparticles (gold and silver) is well mastered, pushing the optical response of metallic nanoparticles towards the ultraviolet requires other materials, such as aluminum. Although a few demonstrations of chemical synthesis of Al nanoparticles have been reported so far, an elaboration path allowing for a wide range of NP size that is compatible with mass production has yet to be demonstrated. In this article, we report on the p…
Plasmonic nanoparticles provide an ideal environment for the enhancement of fluorescent emission. On the one hand, they locally amplify the electromagnetic fields, increasing the emitter excitation rate, and on the other hand, they provide a high local density of states that accelerates spontaneous emission. However, when the emitter is placed in close proximity to a single metal nanoparticle, the number of nonradiative states increases dramatically, causing the fluorescence to quench. It has been predicted theoretically that, through a judicious placing of the emitter, fluorescence in plasmon…
This letter presents experiments on junctions fabricated by a new technique that enables the use of high quality aluminum oxide tunnel barriers with normal metal electrodes at low temperatures. Inverse proximity effect is applied to diminish the superconductivity of an aluminum dot through a clean lateral connection to a normal metal electrode. To demonstrate the effectiveness of this method, fully normal-state single electron transistors (SET) and normal metal-insulator-superconductor (NIS) junctions applying proximized Al junctions were fabricated. The transport characteristics of the juncti…
We report a complementary metal oxide semiconductor (CMOS) technology compatible ferroelectric tunnel junction memristor grown directly on top of a Silicon substrate using a scandium doped aluminum nitride as the ferroelectric layer.
We have investigated planar metal - insulator - metal tunnel junctions with aluminum oxide as dielectricum. These oxide barriers were grown on an aluminum electrode in pure oxygen at room temperature till saturation. We observed discrete barrier widths separated by Δs \approx 0.38 nm, corresponding to the addition of one layer of oxygen atoms. The minimum thickness of s_0 \approx 0.54 nm is due to a double layer of oxygen. We found a strong and systematic dependence of the barrier height Φ_0 on the thickness s like Φ_0 \approx 2.5 eV / s^2(nm), which nearly coincides with the kinetic electron …
We present two approaches for studying the uniformity of a tunnel barrier. The first approach is based on measuring single-electron and two-electron tunneling in a hybrid single-electron transistor. Our measurements indicate that the effective area of a conduction channel is about one order of magnitude larger than predicted by theoretical calculations. With the second method, transmission electron microscopy, we demonstrate that variations in the barrier thickness are a plausible explanation for the larger effective area and an enhancement of higher order tunneling processes.
Electrically-driven optical antennas can serve as compact sources of electromagnetic radiation operating at optical frequencies. In the most widely explored configurations, the radiation is generated by electrons tunneling between metallic parts of the structure when a bias voltage is applied across the tunneling gap. Rather than relying on an inherently inefficient inelastic light emission in the gap, we suggest to use a ballistic nanoconstriction as the feed element of an optical antenna supporting plasmonic modes. We discuss the underlying mechanisms responsible for the optical emission, an…
Localized surface plasmon resonance (LSPR) excitation of nanostructures and charge transfer in plasmonic nanocavities plays a central role in nanoscale optoelectronics and in applications for plasmonic devices. However, the direct observation of near-filed induced charge transfer has remained as a challenging experiment. Here we present LSPR-assisted resonant electron tunneling from an Ag or Au tip to the image potential states of a Ag(111) surface using scanning tunneling microscopy (STM). The LSPR-assisted tunneling process results in an incident photon-energy dependent red-shift of the fiel…
Aluminum nanostructures have recently been at the focus of numerous studies due to their properties including oxidation stability and surface plasmon resonances covering the ultraviolet and visible spectral windows. In this article, we reveal a new facet of this metal relevant for both plasmonics purpose and photo-thermal conversion. The field distribution of high order plasmonic resonances existing in two-dimensional Al structures is studied by nonlinear photoluminescence (nPL) microscopy in a spectral region where electronic interband transitions occur. The polarization sensitivity of the fi…
We report experimental signatures of plasmonic effects due to electron tunneling between adjacent graphene layers. At sub-nanometer separation, such layers can form either a strongly coupled bilayer graphene with a Bernal stacking or a weakly coupled double-layer graphene with a random stacking order. Effects due to interlayer tunneling dominate in the former case but are negligible in the latter. We found through infrared nano-imaging that bilayer graphene supports plasmons with a higher degree of confinement compared to single- and double-layer graphene, a direct consequence of interlayer tu…
The accurate determination of electronic temperatures in metallic nanostructures is essential for many technological applications, like plasmon-enhanced catalysis or lithographic nanofabrication procedures. In this Letter we demonstrate that the electronic temperature can be accurately measured by the shape of the tunnel electroluminescence emission edge in tunnel plasmonic nanocavities, which follows a universal thermal distribution with the bias voltage as the chemical potential of the photon population. A significant deviation between electronic and lattice temperatures is found below 30 K …
The electroluminescence of a polythiophene wire suspended between two metallic electrodes is probed using a scanning tunneling microscope. Under positive sample voltage, the spectral and voltage dependencies of the emitted light are consistent with the fluorescence of the wire junction mediated by localized plasmons. This emission is strongly attenuated for the opposite polarity. Both emission mechanism and polarity dependence are similar to what occurs in organic light emitting diodes (OLED) but at the level of a single molecular wire.
Gap plasmonics deals with the properties of surface plasmons in the narrow region between two metallic nanoparticles forming the gap. For sub-nanometer gap distances electrons can tunnel between the nanoparticles leading to the emergence of novel charge transfer plasmons. These are conveniently described within the quantum corrected model by introducing an artificial material with a tunnel conductivity inside the gap region. Here we develop a methodology for computing such tunnel conductivities within the first-principles framework of density functional theory, and apply our approach to a jell…
Understanding and controlling the interaction between the excitonic states of a quantum emitter and the plasmonic modes of a nanocavity is one of the most relevant current scientific challenges, key for the development of many applications, from quantum information processing devices to polaritonic catalysts. In this paper we demonstrate that the tunnel electroluminescence of C60 nanocrystals enclosed in the plasmonic nanocavity between a metallic surface and the tip of a Scanning Tunnelling Microscope, and isolated from the metal surface by a thin NaCl film, can be switched from a broad emiss…
We theoretically investigate gap plasmons for two silver nanocubes coupled through a molecular tunnel junction. In absence of tunneling, the red-shift of the bonding mode saturates with decreasing gap distance. Tunneling at small gap distances leads to a damping and slight blue-shift of the bonding mode, but no low-energy charge transfer plasmon mode appears in the spectra. This finding is in stark contrast to recent work of Tan et al. [Science 343, 1496 (2014)].
We investigate the statistics of photons emitted by tunneling electrons in a single electronic level plasmonic nanojunction. We compute the waiting-time distribution of successive emitted photons $w(τ)$. When the cavity damping rate $κ$ is larger than the electronic tunneling rate $Γ$, we show that in the photon-antibunching regime, $w(τ)$ indicates that the average delay-time between two successive photon emission events is given by $1/Γ$. This is in contrast with the usually considered second-order correlation function of emitted photons, $g^{(2)}(τ)$, which displays the single time scale $1…
Above-threshold light emission from plasmonic tunnel junctions, when emitted photons have energies significantly higher than the energy scale of the incident electrons, has attracted much recent interest in nano-optics, while the underlying physical mechanism remains elusive. We examine above-threshold light emission in electromigrated tunnel junctions. Our measurements over a large ensemble of devices demonstrate a giant material dependence of photon yield (emitted photons per incident electrons), as large as four orders of magnitude. This dramatic effect cannot be explained only by the radia…
We present a variant of the recently developed quantum corrected model (QCM) for plasmonic nanoparticles [Nature Commun. 3, 825 (2012)] using non-local boundary conditions. The QCM accounts for electron tunneling in narrow gap regions of coupled metallic nanoparticles, leading to the appearance of new charge transfer plasmons. Our approach has the advantages that it emphasizes the non-local nature of tunneling and introduces only contact resistance, but not ohmic losses through tunneling. Additionally, it can be implemented much easier in boundary element method (BEM) approaches. We develop th…
We propose and analyze the terahertz (THz) detectors based on a gated graphene p-i-n (GPIN) field-effect transistor (FET) structure. The reverse-biased i-region between the gates plays the role of the electrons and holes injectors exhibiting nonlinear $I-V$ characteristics due to the Zener-Klein tunneling. This region enables the THz signal rectification, which provides their detection. The gated regions serve as the electron and hole reservoirs and the THz resonant plasma cavities. The resonant excitation of the electron and hole plasmonic oscillations results in a substantial increase in the…
Recent scanning tunnelling microscopy (STM) experiments reported single-molecule fluorescence induced by tunneling currents in the nanoplasmonic cavity formed by the STM tip and the substrate.The electric field of the cavity mode couples with the current-induced charge fluctuations of the molecule, allowing the excitation of the mode. We investigate theoretically this system for the experimentally relevant limit of large damping rate $κ$ for the cavity mode and arbitrary coupling strength to a single-electronic level. We find that for bias voltages close to the first inelastic threshold of pho…
There has been an intense search in recent years for long-lived spin-polarized carriers for spintronic and quantum-computing devices. Here we report that spin polarized quasi-particles in superconducting aluminum layers have surprisingly long spin-lifetimes, nearly a million times longer than in their normal state. The lifetime is determined from the suppression of the aluminum's superconductivity resulting from the accumulation of spin polarized carriers in the aluminum layer using tunnel spin injectors. A Hanle effect, observed in the presence of small in-plane orthogonal fields, is shown to…
We report on spatial measurements of the superconducting proximity effect in epitaxial graphene induced by a graphene-superconductor interface. Superconducting aluminum films were grown on epitaxial multilayer graphene on SiC. The aluminum films were discontinuous with networks of trenches in the film morphology reaching down to exposed graphene terraces. Scanning tunneling spectra measured on the graphene terraces show a clear decay of the superconducting energy gap with increasing separation from the graphene-aluminum edges. The spectra were well described by Bardeen-Cooper-Schrieffer (BCS) …
Surface plasmon enhanced processes and hot-carrier dynamics in plasmonic nanostructures are of great fundamental interest to reveal light-matter interactions at the nanoscale. Using plasmonic tunnel junctions as a platform supporting both electrically- and optically excited localized surface plasmons, we report a much greater (over 1000x) plasmonic light emission at upconverted photon energies under combined electro-optical excitation, compared with electrical or optical excitation separately. Two mechanisms compatible with the form of the observed spectra are interactions of plasmon-induced h…
We report on the nanoparticle-size-dependent onset of quantum tunneling of electrons across the sub-nanometer gaps in three different sizes (30, 50, and 80 nm) of highly uniform gold nanosphere dimers. For precision plasmonics, the gap distance is systematically controlled at the level of single C-C bonds via a series of alkanedithiol linkers (C2-C16). The corresponding single-particle scattering spectra reveal that for the larger dimers the onset of quantum effects occurs at larger gap distances: C6 for 80 nm, C5 for 50 nm, and C4 for 30 nm dimers. 2D non-local and quantum-corrected model (QC…
The tunnel junction between tip and sample in a scanning tunneling microscope is an ideal platform to access the local density of states in the sample through the differential conductance. We show that the energy resolution that can be obtained is principally limited by the electromagnetic interaction of the tunneling electrons with the surrounding environmental impedance as well as the capacitative noise of the junction. The parameter tuning the sensitivity to the environmental impedance is the capacitance of the tunnel junction. The higher the junction capacitance, the less sensitive the tun…
We demonstrate that surface plasmon resonances excited by photon tunneling through an adjacent dielectric medium enhance photocurrent detected by a graphene photodetector. The device is created by overlaying a graphene sheet over an etched gap in a gold film deposited on glass. The detected photocurrents are compared for five different excitation wavelengths, ranging from nm to nm. The photocurrent excited with incident p-polarized light (the case for resonant surface plasmon excitation) is significantly amplified in comparison with that for s-polarized light (without surface plasmon resonance…
The presence of spin-orbit scattering within an aluminum nanoparticle affects measurements of the discrete energy levels within the particle by (1) reducing the effective g-factor below the free-electron value of 2, (2) causing avoided crossings as a function of magnetic field between predominantly-spin-up and predominantly-spin-down levels, and (3) introducing magnetic-field-dependent changes in the amount of current transported by the tunneling resonances. All three effects can be understood in a unified fashion by considering a simple Hamiltonian. Spin-orbit scattering from 4% gold impuriti…
We present a theoretical study of the local optical conductivity, plasmon spectra, and thermoelectric properties of twisted bilayer graphene (TBG) at different filling factors and twist angles $θ$. Our calculations are based on the electronic band structures obtained from a continuum model that has two tunable parameters, $u_0$ and $u_1$, which parametrize the intra-sublattice inter-layer and inter-sublattice inter-layer tunneling rate, respectively. In this Article we focus on two key aspects: i) we study the dependence of our results on the value of $u_0$, exploring the whole range $0\leq u_…
A hallmark of quantum control is the ability to manipulate quantum emission at the nanoscale. Through scanning tunneling microscopy induced luminescence (STML) we are able to generate plasmonic light originating from inelastic tunneling processes that occur in a few-nanometer thick molecular film of C$_{60}$ deposited on Ag(111). Single photon emission, not of excitonic origin, occurs with a 1/$e$ lifetime of a tenth of a nanosecond or less, as shown through Hanbury Brown and Twiss photon intensity interferometry. We have performed tight-binding calculations of the electronic structure for the…
Here, we introduce and experimentally demonstrate optical amplification and stimulated emission from a single optically pumped molecular tunneling junction of a scanning tunneling microscope. The gap between a sharp gold tip and a flat gold substrate covered with a self-assembled monolayer of 5-chloro-2-mercaptobenzothiazole molecules forms an extremely small optical gain medium. When electrons tunnel from the molecules highest occupied molecular orbital to the tip, holes are left behind. These can be repopulated by hot electrons induced by the laser-driven plasmon oscillation on the metal sur…
We study fluctuations in plasmonic electroluminescence at the single-atom limit profiting from the precision of a low-temperature scanning tunneling microscope. First, we investigate the influence of a controlled single-atom transfer on the plasmonic properties of the junction. Next, we form a well-defined atomic contact of several quanta of conductance. In contact, we observe changes of the electroluminescence intensity that can be assigned to spontaneous modifications of electronic conductance, plasmonic excitation and optical antenna properties all originating from minute atomic rearrangeme…
Quantum aspects, such as electron tunneling between closely separated metallic nanoparticles, are crucial for understanding the plasmonic response of nanoscale systems. We explore quantum effects on the response of the conductively coupled metallic nanoparticle dimer. This is realized by stretching a nanorod, which leads to the formation of a narrowing atomic contact between the two nanorod ends. Based on first-principles time-dependent density-functional-theory calculations, we find a discontinuous evolution of the plasmonic response as the nanorod is stretched. This is especially pronounced …
Giant near-field nonlinear electrophotonic effects in an angstrom-scale plasmonic junction
Institute for Molecular Science, National Institutes of Natural Sciences（国立自然科学研究所分子科学研究所）；Graduate Institute for Advanced Studies, SOKENDAI（综合研究大学院大学）
Inelastic electron tunneling and surface-enhanced optical spectroscopies at the molecular scale require cryogenic local temperatures even under illumination - conditions that are challenging to achieve with plasmonically resonant metallic nanostructures. We report a detailed study of the laser heating of plasmonically active nanowires at substrate temperatures from 5 to 60 K. The increase of the local temperature of the nanowire is quantified by a bolometric approach and could be as large as 100 K for a substrate temperature of 5 K and typical values of laser intensity. We also demonstrate tha…
We present ab initio calculations of transport properties of atomic-sized aluminum contacts in the presence of oxygen. The experimental situation is modeled by considering a single oxygen atom (O) or one of the molecules O2 and O3 bridging the gap between electrodes forming ideal, atomically sharp pyramids. The transport characteristics are computed for these geometries with increasing distances between the leads, simulating the opening of a break junction. To facilitate comparison with experiments further, the vibrational modes of the oxygen connected to the electrodes are studied. It is foun…
Electrically driven plasmon-polaritonic bistability in Dirac electron tunneling transistors
Columbia University（哥伦比亚大学）；ETH Zürich（苏黎世联邦理工学院）；National Institute for Materials Science（国立材料研究所）；Air Force Research Laboratory（空军研究实验室）；ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（巴塞罗那光子科学研究所，巴塞罗那科学技术研究院）；ICREA-Institució Catalana de Recerca i Estudis Avançats（加泰罗尼亚高级研究学院）
We demonstrate a technique for creating high quality, large area tunnel junction barriers for normal-insulating- superconducting or superconducting-insulating-superconducting tunnel junctions. We use atomic layer depo- sition and an aluminum wetting layer to form a nanometer scale insulating barrier on gold films. Electronic transport measurements confirm that single-particle electron tunneling is the dominant transport mechanism, and the measured current-voltage curves demonstrate the viability of using these devices as self-calibrated, low temperature thermometers with a wide range of tunabl…
We demonstrate tunnel magnetoresistance (TMR) junctions based on a tri layer system consisting of an epitaxial NiMnSb, aluminum oxide and CoFe tri layer. The junctions show a tunnelling magnetoresistance of Delta R/R of 8.7% at room temperature which increases to 14.7% at 4.2K. The layers show clear separate switching and a small ferromagnetic coupling. A uniaxial in plane anisotropy in the NiMnSb layer leads to different switching characteristics depending on the direction in which the magnetic field is applied, an effect which can be used for sensor applications.
We study decoherence in superconducting qubits due to quasiparticle tunneling which is enhanced by two known deviations from the equilibrium BCS theory. The first process corresponds to tunneling of an already existing quasiparticle across the junction. The quasiparticle density is increased, e.g., because of an effective quasiparticle doping of the system. The second process is quasiparticle tunneling by breaking of a Cooper pair. This can happen at typical energies of superconducting qubits if there is an extended quasiparticle density inside the gap. We calculate the induced energy decay an…
We have fabricated superconductor-quantum dot-superconductor (SC-QD-SC) junctions by using SC aluminum electrodes with narrow gaps laterally contacting a single self-assembled InAs QD. The fabricated junctions exhibited clear Coulomb staircases and Coulomb oscillations at 40 mK. Furthermore, clear suppression in conductance was observed for the source-drain voltage $|V_{\rm SD}| < 2Δ/e$, where $Δ$ is the SC energy gap of Al. The absence of Josephson current that flows through QDs is due to the strong Coulomb interaction and non-negligible thermal fluctuation in our measurement system.
Plasmons in van der Waals heterostructures comprised of graphene and related layered materials demonstrate deep subwavelength confinement and large propagation length. In this letter, we show that graphene-insulator-graphene tunnel structures can serve as plasmonic gain media. The gain stems from the stimulated electron tunneling accompanied by the emission of coherent plasmons under interlayer population inversion. The probability of tunneling with plasmon emission appears to be resonantly large at certain values of frequency and interlayer voltage corresponding to the transitions between ele…
Probing up-conversion electroluminescence of decoupled porphyrin molecules in a plasmonic nanocavity
Max-Planck-Institut für Festkörperforschung（马克斯·普朗克固体研究所）；Institut de Physique, École Polytechnique Fédéral Lausanne（洛桑联邦理工学院物理研究所）；Gleb Wataghin Institute of Physics - University of Campinas - UNICAMP（坎皮纳斯大学格莱布·瓦塔金物理研究所）；Nanjing University（南京大学）
The short wavelength of graphene plasmons relative to the light wavelength makes them attractive for applications in optoelectronics and sensing. However, this property limits their coupling to external light and our ability to create and detect them. More efficient ways of generating plasmons are therefore desirable. Here we demonstrate through realistic theoretical simulations that graphene plasmons can be efficiently excited via electron tunneling in a sandwich structure formed by two graphene monolayers separated by a few atomic layers of hBN. We obtain plasmon generation rates of $\sim10^…
Study of In-plane and Interlayer Interactions During Aluminum Fluoride Intercalation in Graphite: Implications for the Development of Rechargeable Batteries
We evaluate the proposed resonant terahertz (THz) detectors on the base of field-effect transistors (FETs) with split gates, electrically induced lateral p-n junctions, uniform graphene layer (GL) or perforated (in the p-n junction depletion region) graphene layer (PGL) channel. The perforated depletion region forms an array of the nanoconstions or nanoribbons creating the barriers for the holes and electrons. The operation of the GL-FET- and PGL-FET detectors is associated with the rectification of the ac current across the lateral p-n junction enhanced by the excitation of bound plasmonic os…
In this work, we investigate the use of nanoscale polarization engineering to achieve efficient hole injection from metals to ultra-wide band gap AlGaN, and we show that UV-reflective aluminum (Al) layers can be used for hole injection into p-AlGaN. The dependence of tunneling on the work function of the metal was investigated, and it was found that highly reflective Al metal layers can enable efficient hole injection into p-AlGaN, despite the relatively low work function of Al. Efficient tunneling hole injection was confirmed by light emission at 326 nm with on-wafer peak external quantum eff…
