Authors: Polina G Lisinetskaya Merle I S Röhr Roland Mitrić
Publish Date: 2016/06/06
Volume: 122, Issue: 6, Pages: 175-
Abstract
We present a theoretical approach for the simulation of the electric field and exciton propagation in ordered arrays constructed of molecularsized noble metal clusters bound to organic polymer templates In order to describe the electronic coupling between individual constituents of the nanostructure we use the ab initio parameterized transition charge method which is more accurate than the usual dipole–dipole coupling The electronic population dynamics in the nanostructure under an external laser pulse excitation is simulated by numerical integration of the timedependent Schrödinger equation employing the fully coupled Hamiltonian The solution of the TDSE gives rise to timedependent partial point charges for each subunit of the nanostructure and the spatiotemporal electric field distribution is evaluated by means of classical electrodynamics methods The timedependent partial charges are determined based on the stationary partial and transition charges obtained in the framework of the TDDFT In order to treat large plasmonic nanostructures constructed of many constituents the approximate selfconsistent iterative approach presented in Lisinetskaya and Mitrić in Phys Rev B 89035433 2014 is modified to include the transitionchargebased interaction The developed methods are used to study the optical response and exciton dynamics of hboxAg 3+ and porphyrinAg4 dimers Subsequently the spatiotemporal electric field distribution in a ring constructed of ten porphyrinAg4 subunits under the action of circularly polarized laser pulse is simulated The presented methodology provides a theoretical basis for the investigation of coupled lightexciton propagation in nanoarchitectures built from molecular size metal nanoclusters in which quantum confinement effects are important
Keywords: