@article{LisinetskayaRoehrMitrić2016,
  author    = {Lisinetskaya, Polina and R{\"o}hr, Merle I. S. and Mitrić, Roland},
  title     = {First-principles simulation of light propagation and exciton dynamics in metal cluster nanostructures},
  series = {Applied Physics B},
  volume    = {122},
  journal   = {Applied Physics B},
  number    = {6},
  issn      = {0946-2171},
  doi       = {10.1007/s00340-016-6436-6},
  url       = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-159193},
  pages     = {175},
  year      = {2016},
  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 Schrodinger 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 Mitric 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 Ag-3(+) and porphyrin-Ag-4 dimers. Subsequently, the spatio-temporal electric field distribution in a ring constructed of ten porphyrin-Ag-4 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.},
  language  = {en}
}
@article{RoehrLisinetskayaMitric2016,
  author    = {R{\"o}hr, Merle I. S. and Lisinetskaya, Polina G. and Mitric, Roland},
  title     = {Excitonic Properties of Ordered Metal Nanocluster Arrays: 2D Silver Clusters at Multiporphyrin Templates},
  series = {Journal of Physical Chemistry A},
  volume    = {120},
  journal   = {Journal of Physical Chemistry A},
  number    = {26},
  doi       = {10.1021/acs.jpca.6b04243},
  url       = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-159464},
  pages     = {4465-4472},
  year      = {2016},
  abstract  = {The design of ordered arrays of metal nanoclusters such as for example 2D cluster organic frameworks might open a new route towards the development of materials with tailored optical properties. Such systems could serve as plasmonically enhanced light-harvesting materials, sensors or catalysts. We present here a theoretical approach for the simulation of the optical properties of ordered arrays of metal clusters that is based on the ab initio parametrized Frenkel exciton model. We demonstrate that small atomically precise silver clusters can be assembled in one- and two-dimensional arrays on suitably designed porphyrin templates exhibiting remarkable optical properties. By employing explicit TDDFT calculations on smaller homologs, we show that the intrinsic optical properties of metal clusters are largely preserved but undergo J- and H-type excitonic coupling that results in controllable splitting of their excited states. Furthermore, ab initio parameterized Frenkel exciton model calculations allow us to predict an energetic splitting of up to 0.77 eV in extended two-dimensional square arrays and 0.79 eV in tilted square aggregates containing up to 25 cluster-porphyrin subunits.},
  language  = {en}
}