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Register a new userProbing plasmon-NV$^0$ coupling at the nanometer scale with photons and fast electrons
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Added by
Luiz Henrique Galvao Tizei
Publication date
2019
fields
Physics
and research's language is
English
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The local density of optical states governs an emitters lifetime and quantum yield through the Purcell effect. It can be modified by a surface plasmon electromagnetic field, but such a field has a spatial extension limited to a few hundreds of nanometers, which complicates the use of optical methods to spatially probe the emitter-plasmon coupling. Here we show that a combination of electron-based imaging, spectroscopies and photon-based correlation spectroscopy enables measurement of the Purcell effect with nanometer and nanosecond spatio-temporal resolutions. Due to the large variability of radiative lifetimes of emitters embedded in nanoparticles with inhomogeneous sizes we relied on a statistical approach to unambiguously probe the coupling between nitrogen-vacancy centers (NV^0) in nanodiamonds and surface plasmons in silver nanocubes. We quantified the Purcell effect by measuring the NV^0 excited state lifetimes in a large number of either isolated nanodiamonds or nanodiamond-nanocube dimers and demonstrated a statistically significant lifetime reduction for dimers.
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The Rashba effect as an electrically tunable spin-orbit interaction is the base for a multitude of possible applications such as spin filters, spin transistors, and quantum computing using Majorana states in nanowires. Moreover, this interaction can determine the spin dephasing and antilocalization phenomena in two dimensions. However, the real space pattern of the Rashba parameter has never been probed, albeit it critically influences, e.g., the more robust spin transistors using the spin helix state and the otherwise forbidden electron backscattering in topologically protected channels. Here, we map this pattern down to nanometer length scales by measuring the spin splitting of the lowest Landau level using scanning tunnelling spectroscopy. We reveal strong fluctuations correlated with the local electrostatic potential for an InSb inversion layer with a large Rashba coefficient (~1 eV{AA}). The novel type of Rashba field mapping enables a more comprehensive understanding of the critical fluctuations, which might be decisive towards robust semiconductor-based spintronic devices.
Friction is a complicated phenomenon involving nonlinear dynamics at different length and time scales[1, 2]. The microscopic origin of friction is poorly understood, due in part to a lack of methods for measuring the force on a nanometer-scale asperity sliding at velocity of the order of cm/s.[3, 4] Despite enormous advance in experimental techniques[5], this combination of small length scale and high velocity remained illusive. Here we present a technique for rapidly measuring the frictional forces on a single asperity (an AFM tip) over a velocity range from zero to several cm/s. At each image pixel we obtain the velocity dependence of both conservative and dissipative forces, revealing the transition from stick-slip to a smooth sliding friction[1, 6]. We explain measurements on graphite using a modified Prandtl-Tomlinson model that takes into account the damped elastic deformation of the asperity. With its greatly improved force sensitivity and very small sliding amplitude, our method enables rapid and detailed surface mapping of the full velocity-dependence of frictional forces with less than 10~nm spatial resolution.
Plasmon-emitter interactions are of paramount importance in modern nanoplasmonics and are generally maximal at short emitter-surface separations. However, when the separation falls below 10-20 nm, the classical theory progressively deteriorates due to its neglect of quantum mechanical effects such as nonlocality, electronic spill-out, and Landau damping. Here, we show how this neglect can be remedied by presenting a unified theoretical treatment of mesoscopic electrodynamics grounded on the framework of Feibelman $d$-parameters. Crucially, our technique naturally incorporates nonclassical resonance shifts and surface-enabled Landau damping - a nonlocal damping effect - which have a dramatic impact on the amplitude and spectral distribution of plasmon-emitter interactions. We consider a broad array of plasmon-emitter interactions ranging from dipolar and multipolar spontaneous emission enhancement, to plasmon-assisted energy transfer and enhancement of two-photon transitions. The formalism presented here gives a complete account of both plasmons and plasmon-emitter interactions at the nanoscale, constituting a simple yet rigorous and general platform to incorporate nonclassical effects in plasmon-empowered nanophotonic phenomena.
We present a model for exciton-plasmon coupling based on an energy exchange mechanism between quantum emitters (QE) and localized surface plasmons in metal-dielectric structures. Plasmonic correlations between QEs give rise to a collective state exchanging its energy cooperatively with a resonant plasmon mode. By defining carefully the plasmon mode volume for a QE ensemble, we obtain a relation between QE-plasmon coupling and a cooperative energy transfer rate that is expressed in terms of local fields. For a single QE near a sharp metal tip, we find analytically the enhancement factor for QE-plasmon coupling relative to QE coupling to a cavity mode. For QEs distributed in an extended region enclosing a plasmonic structure, we find that the ensemble QE-plasmon coupling saturates to a universal value independent of system size and shape, consistent with the experiment.
We employ tip-enhanced infrared near-field microscopy to study the plasmonic properties of epitaxial quasi-free-standing monolayer graphene on silicon carbide. The near-field images reveal propagating graphene plasmons, as well as a strong plasmon reflection at gaps in the graphene layer, which appear at the steps between the SiC terraces. When the step height is around 1.5 nm, which is two orders of magnitude smaller than the plasmon wavelength, the reflection signal reaches 20% of its value at graphene edges, and it approaches 50% for step heights as small as 5 nm. This intriguing observation is corroborated by numerical simulations, and explained by the accumulation of a line charge at the graphene termination. The associated electromagnetic fields at the graphene termination decay within a few nanometers, thus preventing efficient plasmon transmission across nanoscale gaps. Our work suggests that plasmon propagation in graphene-based circuits can be tailored using extremely compact nanostructures, such as ultra-narrow gaps. It also demonstrates that tip-enhanced near-field microscopy is a powerful contactless tool to examine nanoscale defects in graphene.
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