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Using large-scale, real-time quantum dynamics calculations, we present a detailed analysis of electronic excitation transfer (EET) mechanisms in a multi-particle plasmonic nanoantenna system. Specifically, we utilize real-time, time-dependent, density functional tight binding (RT-TDDFTB) to provide a quantum-mechanical description (at an electronic/atomistic level of detail) for characterizing and analyzing these systems, without recourse to classical approximations. We also demonstrate highly long-range electronic couplings in these complex systems and find that the range of these couplings is more than twice the conventional cutoff limit considered by FRET based approaches. Furthermore, we attribute these unusually long-ranged electronic couplings to the coherent oscillations of conduction electrons in plasmonic nanoparticles. This long-range nature of plasmonic interactions has important ramifications for EET - in particular, we show that the commonly used nearest-neighbor FRET model is inadequate for accurately characterizing EET even in simple plasmonic antenna systems. These findings provide a real-time, quantum-mechanical perspective for understanding EET mechanisms and provide guidance in enhancing plasmonic properties in artificial light-harvesting systems.
Exciton dissociation at heterojunctions in photovoltaic devices is not completely understood despite being fundamentally necessary to generate electrical current. One of the fundamental issues for ab initio calculations is that hybrid interfaces comb
Tunneling in a quantum coherent structure is not restricted to only nearest neighbours. Hopping between distant sites is possible via the virtual occupation of otherwise avoided intermediate states. Here we report the observation of long range transi
The cubic (c) and monoclinic (m) polymorphs of Gd2O3 were studied using the combined analysis of several materials science techniques - X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and photolumi
We report ferromagnetic resonance in the normal configuration of an electrically insulating magnetic bilayer consisting of two yttrium iron garnet (YIG) films epitaxially grown on both sides of a 0.5-mm-thick nonmagnetic gadolinium gallium garnet (GG
Surfaces are at the frontier of every known solid. They provide versatile supports for functional nanostructures and mediate essential physicochemical processes. Being intimately related with 2D materials, interfaces and atomically thin films often f