Résumé: In a recent article generalization of the binomial distribution associated with a sequence of positive numbers was examined. The analysis of the nonnegativeness of the formal probability distributions was a key point to allow to give them a statistical interpretation in terms of probabilities. In this article we present an approach based on generating functions that solves the previous difficulties. Our main theorem makes explicit the conditions under which those formal probability distributions are always non-negative. Therefore, the constraints of non-negativeness are automatically fulfilled giving a complete characterization in terms of generating functions. A large number of analytical examples becomes available. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4757601]

Résumé: The application of atto-second streaking spectroscopy (ASS) to direct time-domain studies of the plasmonic excitations in metallic nano-objects is addressed theoretically. The streaking spectrograms for a rectangular gold nano-antenna and spherical gold clusters are obtained within strong field approximation using classical electron trajectory calculations. The results reported here for spherical clusters are also representative of spherical nano-shells. This study demonstrates that ASS allows for detailed characterization of plasmonic modes, including near-field enhancement, frequency and decay rate. The role of the inhomogeneity of the induced electric fields is also demonstrated.

Résumé: Electromagnetic coupling between plasmonic resonances in metallic nanoparticles allows for engineering of the optical response and generation of strong localized near-fields. Classical electrodynamics fails to describe this coupling across sub-nanometer gaps, where quantum effects become important owing to non-local screening and the spill-out of electrons. However, full quantum simulations are not presently feasible for realistically sized systems. Here we present a novel approach, the quantum-corrected model (QCM), that incorporates quantum-mechanical effects within a classical electrodynamic framework. The QCM approach models the junction between adjacent nanoparticles by means of a local dielectric response that includes electron tunnelling and tunnelling resistivity at the gap and can be integrated within a classical electrodynamical description of large and complex structures. The QCM predicts optical properties in excellent agreement with fully quantum mechanical calculations for small interacting systems, opening a new venue for addressing quantum effects in realistic plasmonic systems.

Résumé: The advent of milli-kelvin scanning tunneling microscopes (STM) with inbuilt magnetic fields has opened access to the study of magnetic phenomena with atomic resolution at surfaces. In the case of single atoms adsorbed on a surface, the existence of different magnetic energy levels localized on the adsorbate is due to the breaking of the rotational invariance of the adsorbate spin by the interaction with its environment, leading to energy terms in the meV range. These structures were revealed by STM experiments in IBM Almaden in the early 2000s for atomic adsorbates on CuN surfaces. The experiments consisted in the study of the changes in conductance caused by inelastic tunneling of electrons (IETS, inelastic electron tunneling spectroscopy). Manganese and Iron adatoms were shown to have different magnetic anisotropies induced by the substrate. More experiments by other groups followed up, showing that magnetic excitations could be detected in a variety of systems: e.g. complex organic molecules showed that their magnetic anisotropy was dependent on the molecular environment, piles of magnetic molecules showed that they interact via intermolecular exchange interaction, spin waves were excited on ferromagnetic surfaces and in Mn chains, and magnetic impurities have been analyzed on semiconductors. These experiments brought up some intriguing questions: the efficiency of magnetic excitations was very high, the excitations could or could not involve spin flip of the exciting electron and singular-like behavior was sometimes found at the excitation thresholds. These facts called for extended theoretical analysis: perturbation theories, sudden-approximation approaches and a strong coupling scheme successfully explained most of the magnetic inelastic processes. In addition, many-body approaches were also used to decipher the interplay between inelastic processes and the Kondo effect. Spin torque transfer has been shown to be effective in changing spin orientations of an adsorbate in theoretical works, and soon after it was shown experimentally. More recently, the previously mentioned strong coupling approach was extended to treat the excitation of spin waves in atomic chains and the ubiquitous role of electron-hole pair creation in de-exciting spins on surfaces has been analyzed. This review article expounds these works, presenting the theoretical approach by the authors while trying to thoroughly review parallel theoretical and experimental works. (C) 2012 Elsevier Ltd. All rights reserved.

Résumé: Wave-particle complementarity is one of the most intriguing features of quantum physics. To emphasize this measurement apparatus–dependent nature, experiments have been performed in which the output beam splitter of a Mach-Zehnder interferometer is inserted or removed after a photon has already entered the device. A recent extension suggested using a quantum beam splitter at the interferometer’s output; we achieve this using pairs of polarization-entangled photons. One photon is tested in the interferometer and is detected, whereas the other allows us to determine whether wave, particle, or intermediate behaviors have been observed. Furthermore, this experiment allows us to continuously morph the tested photon’s behavior from wavelike to particle-like, which illustrates the inadequacy of a naive wave or particle description of light.

Résumé: Recent advances in attosecond spectroscopy techniques have fueled the interest in the theoretical description of electronic processes taking place in the subfemtosecond time scale. Here we study the coupled dynamic screening of a localized hole and a photoelectron emitted from a metal cluster using a semi-classical model. Electron density dynamics in the cluster is calculated with time-dependent density functional theory, and the motion of the photoemitted electron is described classically. We show that the dynamic screening of the hole by the cluster electrons affects the motion of the photoemitted electron. At the very beginning of its trajectory, the photoemitted electron interacts with the cluster electrons that pile up to screen the hole. Within our model, this gives rise to a significant reduction of the energy lost by the photoelectron. Thus, this is a velocity-dependent effect that should be accounted for when calculating the average losses suffered by photoemitted electrons in metals.

Résumé: When two metal nanostructures are placed nanometres apart, their optically driven free electrons couple electrically across the gap. The resulting plasmons have enhanced optical fields of a specific colour tightly confined inside the gap. Many emerging nanophotonic technologies depend on the careful control of this plasmonic coupling, including optical nanoantennas for high-sensitivity chemical and biological sensors(1), nanoscale control of active devices(2-4), and improved photovoltaic devices(5). But for subnanometre gaps, coherent quantum tunnelling becomes possible and the system enters a regime of extreme non-locality in which previous classical treatments(6-14) fail. Electron correlations across the gap that are driven by quantum tunnelling require a new description of non-local transport, which is crucial in nanoscale optoelectronics and single-molecule electronics. Here, by simultaneously measuring both the electrical and optical properties of two gold nanostructures with controllable subnanometre separation, we reveal the quantum regime of tunnelling plasmonics in unprecedented detail. All observed phenomena are in good agreement with recent quantum-based models of plasmonic systems(15), which eliminate the singularities predicted by classical theories. These findings imply that tunnelling establishes a quantum limit for plasmonic field confinement of about 10(-8) lambda(3) for visible light (of wavelength lambda). Our work thus prompts new theoretical and experimental investigations into quantum-domain plasmonic systems, and will affect the future of nanoplasmonic device engineering and nanoscale photochemistry.

Résumé: For energetic atomic beams grazingly incident at a surface along low-index directions, the fast motion of the projectile in the surface plane and the slow motion in the direction perpendicular to the surface appear nearly decoupled. Fast-atom diffraction (FAD) experiments reveal two-dimensional (2D) diffraction patterns associated with exchange of the reciprocal vector perpendicular to the low-index direction of fast motion. These results are usually interpreted within the axial-channeling approximation, where the effective 2D potential experienced by the projectile is set as an average of the 3D surface potential along the atomic strings forming the channel. In this work, using the example of grazing scattering of He atoms at a LiF(001) surface, we address theoretically the range of validity of the axial-channeling approximation. Full quantum wave-packet-propagation calculations are used to study the transition from the 2D (fast atom) to the 3D diffraction pattern characteristic for low-energy atomic and molecular projectiles scattered from surfaces. Along with exact calculations, a semianalytical perturbative treatment based on the Lippmann-Schwinger equation allows an explanation of why the diffraction processes involving the exchange of reciprocal-lattice vectors along the fast-motion direction are exponentially small in typical FAD conditions.