Investigating nanoplasmonics in an explicit time-dependent perspective is a natural choice when light pulses are used and may also reveal aspects that are hidden in a frequency-based picture. In the past, we proposed a method time domain-boundary element method (TD-BEM) to simulate the time dependent polarization of nanoparticles based on a boundary element method that is particularly suitable to interface with a quantum atomistic description of nearby molecules. So far, however, metal dielectric functions in TD-BEM have been modeled through analytic expressions, such as those of Debye and Drude–Lorentz, which cannot account for multiple electronic resonances. Our approach allows us to include in the TD-BEM framework also the description of metals with complicate dielectric function profiles in the frequency domain. Particularly, among all metals, gold is a challenging case due to the presence of many transition frequencies. We applied our methods to different metals (gold, silver, and the less commonly investigated rhodium) and different shaped nanoparticles (spheres, ellipsoids, and cubes), the approach has been tested comparing TD-BEM and frequency domain BEM absorption spectra, and it has been used to investigate the time-dependent field acting locally close to nanoparticle vertices.
Tip-enhanced photoluminescence (TEPL) experiments have recently reached the ability to investigate single molecules exploiting resolution at submolecular level. Localised surface plasmon resonances of metallic nanostructures have the capability of enhancing an impinging electromagnetic radiation in proximity of their surface, with evident consequences both on absorption and emission of molecules placed in the same region. We propose a theoretical analysis of these
A computational approach to optimize molecules near metal nanoparticles and incident electric field for desired photophysical properties based on the time-dependent QM/PCM–NP method is proposed.
We consider the notion of equilibration for an isolated quantum system exhibiting Anderson localization. The system is assumed to be in a pure state, i.e., described by a wave-function undergoing unitary dynamics. We focus on the simplest model of a 1D disordered chain and we analyse both the dynamics of an initially localized state and the dynamics of quantum states drawn at random from the ensemble corresponding to the minimum knowledge about the initial state. While in the former case the site distribution remains confined in a limited portion of the chain, the site distribution of random pure state fluctuates around an equilibrium average that is delocalized over the entire chain. A clear connection between the equilibration observed when the system is initialized in a fully localized state and the amplitude of dynamical fluctuations of a typical random pure state is established.
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