Related papers: Exact description of excitonic dynamics in molecul…
In this paper we consider dynamics of a molecular system subjected to external pumping by a light source. Within a completely quantum mechanical treatment, we derive a general formula, which enables to asses effects of different light…
Organic molecules store the energy of absorbed light in the form of charge-neutral molecular excitations -- Frenkel excitons. Usually, in amorphous organic materials, excitons are viewed as quasiparticles, localized on single molecules,…
The exciton dynamics in a molecular heterodimer is studied as a function of differences in excitation and reorganization energies, asymmetry in transition dipole moments and excited state lifetimes. The heterodimer is composed of two…
Excitonic models of light-harvesting complexes, where the vibrational degrees of freedom are treated as a bath, are commonly used to describe the motion of the electronic excitation through a molecule. Recent experiments point toward the…
We analyze the exciton dynamics in PhotosystemI from Thermosynechococcus elongatus using the distributed memory implementation of the hierarchical equation of motion (DM-HEOM) for the 96 Chlorophylls in the monomeric unit. The…
The recently suggested possibility that weak vibronic transitions can be excitonically enhanced in light-harvesting complexes is studied in detail. A vibronic exciton dimer model which includes ground state vibrations is investigated using…
Recent ultrafast optical experiments show that excitons in large biological light-harvesting complexes are coupled to molecular vibration modes. These high-frequency vibrations will not only affect the optical response, but also drive the…
Photosynthesis, the process by which energy from sunlight drives cellular metabolism, relies on a unique organization of light-harvesting and reaction center complexes. Recently, the organization of light-harvesting LH2 complexes and…
Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of cavity quantum electrodynamics. They are highly tunable, scalable, easy to synthesize and offer sub-wavelength confinement, all while…
We derive a Hierarchical Equations of Motion (HEOM) description of nonadiabatic Herzberg-Teller type coupling effects and of non-Condon effects in a system of electronic transitions interacting with intra- and inter-molecular vibrational…
In the context of Frenkel exciton dynamics in aggregated molecules the polaron transformation technique facilitates a treatment where diagonal elements attributed to electronic excited-state populations are decoupled from fluctuations…
Frenkel exciton population dynamics of an excitonic dimer is studied by comparing results from a quantum master equation (QME) involving rates from second-order perturbative treatment with respect to the excitonic coupling with…
Time-resolved spectroscopy provides the main tool for analyzing the dynamics of excitonic energy transfer in light-harvesting complexes. To infer time-scales and effective coupling parameters from experimental data requires to develop…
We have developed a model accounting for the photo-excitation dynamics and the photoluminescence of strongly coupled J-aggregate microcavities. Our model is based on a description of the J-aggregate film as a disordered Frenkel exciton…
The present review is devoted to our recent studies on the excitonic motion in photosynthetic systems. In photosynthesis, the light photon is absorbed to create an exciton in the antenna complex of the photosynthetic pigments. This exciton…
We present a theory that efficiently describes the quantum dynamics of an electronic excitation that is coupled to a continuous, highly structured phonon environment. Based on a stochastic approach to non-Markovian open quantum systems, we…
The theoretical description and the properties of Frenkel excitons in non-covalently bonded molecular aggregates are reviewed from a multi-exciton perspective of dissipative quantum dynamics. First, the photophysical and quantum chemical…
Intense light with frequencies above typical atomic or molecular ionization potentials as provided by free-electron lasers couples many photons into extended targets such as clusters and biomolecules. This implies, in contrast to…
The prospect of coherent dynamics and excitonic delocalization across several light-harvesting structures in photosynthetic membranes is of considerable interest, but challenging to explore experimentally. Here we demonstrate theoretically…
When the interaction between a molecular system and confined light modes in an optical or plasmonic cavity is strong enough to overcome the dissipative process, hybrid light-matter states (polaritons) emerge as the fundamental excitations…