%0 Journal Article %1 Lisinetskaya2016 %A Lisinetskaya, Polina G. %A Röhr, Merle I. S. %A Mitrić, Roland %D 2016 %J Applied Physics B %K ag_pub1 %N 6 %P 175 %R 10.1007/s00340-016-6436-6 %T First-principles simulation of light propagation and exciton dynamics in metal cluster nanostructures %U https://doi.org/10.1007/s00340-016-6436-6 %V 122 %X We present a theoretical approach for the simulation of the electric field and exciton propagation in ordered arrays constructed of molecular-sized 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 time-dependent Schrödinger equation employing the fully coupled Hamiltonian. The solution of the TDSE gives rise to time-dependent partial point charges for each subunit of the nanostructure, and the spatio-temporal electric field distribution is evaluated by means of classical electrodynamics methods. The time-dependent 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 self-consistent iterative approach presented in (Lisinetskaya and Mitrić in Phys Rev B 89:035433, 2014) is modified to include the transition-charge-based interaction. The developed methods are used to study the optical response and exciton dynamics of \$\$\backslashhbox\Ag\\_\3\^\+\\$\$Ag3+and porphyrin-Ag4 dimers. Subsequently, the spatio-temporal electric field distribution in a ring constructed of ten porphyrin-Ag4 subunits under the action of circularly polarized laser pulse is simulated. The presented methodology provides a theoretical basis for the investigation of coupled light-exciton propagation in nanoarchitectures built from molecular size metal nanoclusters in which quantum confinement effects are important.

@article{Lisinetskaya2016, abstract = {We present a theoretical approach for the simulation of the electric field and exciton propagation in ordered arrays constructed of molecular-sized 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 time-dependent Schr{\"o}dinger equation employing the fully coupled Hamiltonian. The solution of the TDSE gives rise to time-dependent partial point charges for each subunit of the nanostructure, and the spatio-temporal electric field distribution is evaluated by means of classical electrodynamics methods. The time-dependent 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 self-consistent iterative approach presented in (Lisinetskaya and Mitri{\'{c}} in Phys Rev B 89:035433, 2014) is modified to include the transition-charge-based interaction. The developed methods are used to study the optical response and exciton dynamics of {\$}{\$}{\backslash}hbox{\{}Ag{\}}{\_}{\{}3{\}}^{\{}+{\}}{\$}{\$}Ag3+and porphyrin-Ag4 dimers. Subsequently, the spatio-temporal electric field distribution in a ring constructed of ten porphyrin-Ag4 subunits under the action of circularly polarized laser pulse is simulated. The presented methodology provides a theoretical basis for the investigation of coupled light-exciton propagation in nanoarchitectures built from molecular size metal nanoclusters in which quantum confinement effects are important.}, added-at = {2019-10-24T14:09:15.000+0200}, author = {Lisinetskaya, Polina G. and R{\"o}hr, Merle I. S. and Mitri{\'{c}}, Roland}, biburl = {https://www.bibsonomy.org/bibtex/25d6449352dd9861a4134d75d2403d2f5/sagasucy}, day = 06, doi = {10.1007/s00340-016-6436-6}, interhash = {4f51ff75cc87841a23d138611cae4159}, intrahash = {5d6449352dd9861a4134d75d2403d2f5}, issn = {1432-0649}, journal = {Applied Physics B}, keywords = {ag_pub1}, month = jun, number = 6, pages = 175, timestamp = {2019-10-24T14:09:15.000+0200}, title = {First-principles simulation of light propagation and exciton dynamics in metal cluster nanostructures}, url = {https://doi.org/10.1007/s00340-016-6436-6}, volume = 122, year = 2016 }