TY  - JOUR
A1  - Lisinetskaya, Polina
A1  - Braun, Christian
A1  - Proch, Sebastian
A1  - Kim, Young Dok
A1  - Ganteför, Gerd
A1  - Mitrić, Roland
T1  - Excited state nonadiabatic dynamics of bare and hydrated anionic gold clusters Au\(^−_3\)[H\(_2\)O]\(_n\) (n=0-2)
JF  - Physical Chemistry Chemical Physics
N2  - We present a joint theoretical and experimental study of excited state dynamics in pure and hydrated anionic gold clusters Au\(^-_3\)[H\(_2\)O]\(_n\) (n = 0-2). We employ mixed quantum-classical dynamics combined with femtosecond time-resolved photoelectron spectroscopy in order to investigate the influence of hydration on excited state lifetimes and photo-dissociation dynamics. A gradual decrease of the excited state lifetime with the number of adsorbed water molecules as well as gold cluster fragmentation quenching by two or more water molecules are observed both in experiment and in simulations. Non-radiative relaxation and dissociation in excited states are found to be responsible for the excited state population depletion. Time constants of these two processes strongly depend on the number of water molecules leading to the possibility to modulate excited state dynamics and fragmentation of the anionic cluster by adsorption of water molecules.
KW  - nonadiabatic dynamics
KW  - metal cluster
KW  - time-resolved photoelectron spectroscopy
Y1  - 2016
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-159176
UR  - https://doi.org/10.1039/C5CP04297F
SN  - 1463-9076
N1  - Accepted version
VL  - 18
IS  - 9
ER  - 
TY  - JOUR
A1  - Lisinetskaya, Polina
A1  - Röhr, Merle I. S.
A1  - Mitrić, Roland
T1  - First-principles simulation of light propagation and exciton dynamics in metal cluster nanostructures
JF  - Applied Physics B
N2  - 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.
KW  - metal-cluster hybrid systems
KW  - exciton transfer
KW  - optical response
KW  - transition density
KW  - total electric field
KW  - electric field distribution
KW  - transition dipole moment
KW  - transition charge
Y1  - 2016
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-159193
UR  - https://doi.org/10.1007/s00340-016-6436-6
SN  - 0946-2171
N1  - This is a post-peer-review, pre-copyedit version of an article published in Apllied Physcis B. The final authenticated version is available online at: http://dx.doi.org/10.1007/s00340-016-6436-6
VL  - 122
IS  - 6
ER  -