Alejandro Varas

Real-space grids and the Octopus code as tools for the development of new simulation approaches for electronic systems

Real-space grids are a powerful alternative for the simulation of electronic systems. One of the main advantages of the approach is the flexibility and simplicity of working directly in real space where the different fields are discretized on a grid, combined with competitive numerical performance and great potential for parallelization. These properties constitute a great advantage at the time of implementing and testing new physical models. Based on our experience with the Octopus code, in this article we discuss how the real-space approach has allowed for the recent development of new ideas for the simulation of electronic systems. Among these applications are approaches to calculate response properties, modeling of photoemission, optimal control of quantum systems, simulation of plasmonic systems, and the exact solution of the Schrödinger equation for low-dimensionality systems.

Quantum plasmonics: from jellium models to ab initio calculations

Abstract Light-matter interaction in plasmonic nanostructures is often treated within the realm of classical optics. However, recent experimental findings show the need to go beyond the classical models to explain and predict the plasmonic response at the nanoscale. A prototypical system is a nanoparticle dimer, extensively studied using both classical and quantum prescriptions. However, only very recently, fully ab initio time-dependent density functional theory (TDDFT) calculations of the optical response of these dimers have been carried out. Here, we review the recent work on the impact of the atomic structure on the optical properties of such systems. We show that TDDFT can be an invaluable tool to simulate the time evolution of plasmonic modes, providing fundamental understanding into the underlying microscopical mechanisms.

Anisotropy Effects on the Plasmonic Response of Nanoparticle Dimers

We present an ab initio study of the anisotropy and atomic relaxation effects on the optical properties of nanoparticle dimers. Special emphasis is placed on the hybridization process of localized surface plasmons, plasmon-mediated photoinduced currents, and electric-field enhancement in the dimer junction. We show that there is a critical range of separations between the clusters (0.1-0.5 nm) in which the detailed atomic structure in the junction and the relative orientation of the nanoparticles have to be considered to obtain quantitative predictions for realistic nanoplasmonic devices. It is worth noting that this regime is characterized by the emergence of electron tunneling as a response to the driven electromagnetic field. The orientation of the particles not only modifies the attainable electric field enhancement but can lead to qualitative changes in the optical absorption spectrum of the system.

Au13-nAgn clusters: a remarkably simple trend.

The planar to three dimensional transition of Au13-nAgn clusters is investigated. To do so the low lying energy configurations for all possible concentrations (n values) are evaluated. Many thousands of possible conformations are examined. They are generated using the procedure developed by Rogan et al. in combination with the semi-empirical Gupta potential. A large fraction of these (the low lying energy ones) are minimized by means of Density Functional Theory (DFT) calculations. We employ the Tao, Perdew, Staroverov, and Scuseria (TPSS) meta-GGA functional and the Perdew, Burke and Ernzerhof (PBE) GGA functional, and compare their results. The effect of spin-orbit coupling is studied as well as the s-d hybridization. As usual in this context the results are functional-dependent. However, both functionals lead to agreement as far as trends are concerned, yielding just two relevant motifs, but their results differ quantitatively.

A strategy to find minimal energy nanocluster structures

An unbiased strategy to search for the global and local minimal energy structures of free standing nanoclusters is presented. Our objectives are twofold: to find a diverse set of low lying local minima, as well as the global minimum. To do so, we use massively the fast inertial relaxation engine algorithm as an efficient local minimizer. This procedure turns out to be quite efficient to reach the global minimum, and also most of the local minima. We test the method with the Lennard–Jones (LJ) potential, for which an abundant literature does exist, and obtain novel results, which include a new local minimum for LJ13, 10 new local minima for LJ14, and thousands of new local minima for 15≤N≤65 . Insights on how to choose the initial configurations, analyzing the effectiveness of the method in reaching low‐energy structures, including the global minimum, are developed as a function of the number of atoms of the cluster. Also, a novel characterization of the potential energy surface, analyzing properties of the local minima basins, is provided. The procedure constitutes a promising tool to generate a diverse set of cluster conformations, both two‐ and three‐dimensional, that can be used as an input for refinement by means of ab initio methods.

Structural, electronic, and magnetic properties of FexCoyPdz (x + y + z ≤ 7) clusters: a density functional theory study

Transition metal alloy nanoparticles are of interest both theoretically and experimentally, particularly due to their potential technological applications, and to their novel structural and magnetic properties in the subnanometer region. Here we compute structural parameters, chemical and magnetic properties, and the fragmentation channels of Fe

Structural, electronic, and magnetic properties of FexCoyNiz (x+y+z=13) clusters: A density-functional-theory study

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Binary cluster collision dynamics and minimum energy conformations

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