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Until recently it was believed that photosynthesis, a fundamental process for life on earth, could be fully understood with semi-classical models. However, puzzling quantum phenomena have been observed in several photosynthetic…
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…
Light-harvesting and excitation energy transfer in photosynthesis generally involve chlorophyll-molecules, maintained by their host proteins at short distances from each other, this resulting in excitonic coupling. The transfer of…
Determining how energy flows within and between molecules is crucial for understanding chemical reactions, material properties, and even vital processes such as photosynthesis. While the general principles of energy transfer are well…
The functioning and efficiency of natural photosynthetic complexes is strongly influenced by their embedding in a noisy protein environment, which can even serve to enhance the transport efficiency. Interactions with the environment induce…
Inter- or intramolecular coupling processes between chromophores such as excimer formation or H- and J-aggregation are crucial to describing the photophysics of closely packed films of conjugated polymers. Such coupling is highly distance…
In the present paper we address the problem of the energy downconversion of the light absorbed by a protein into its internal vibrational modes. We consider the case in which the light receptors are fluorophores either naturally…
The exciton relaxation dynamics of photoexcited electronic states in poly($p$-phenylenevinylene) (PPV) are theoretically investigated within a coarse-grained model, in which both the exciton and nuclear degrees of freedom are treated…
Giant strides in ultrashort laser pulse technology have enabled real-time observation of dynamical processes in complex molecular systems. Specifically, the discovery of oscillatory transients in the two-dimensional electronic spectra of…
We theoretically investigate exciton relaxation dynamics in molecular aggregates based on model photosynthetic complexes under various conditions of incoherent excitation. We show that noise-induced quantum coherence is generated between…
Representation of molecular vibrational degrees of freedom by independent harmonic oscillators, when describing electronic spectra or electronic excitation energy transport, raises unfavourable effects as vibrational energy relaxation…
We consider the dependence of the electron transfer in photosynthetic complexes on correlation properties of random fluctuations of the protein environment. The electron subsystem is modeled by a finite network of connected electron…
Energy relaxation in light-harvesting complexes has been extensively studied by various ultrafast spectroscopic techniques, the fastest processes being in the sub-100 fs range. At the same time much slower dynamics have been observed in…
Energy transfer between chromophores in photosynthesis proceeds with near unity quantum efficiency. Understanding the precise mechanisms of these processes is made difficult by the complexity of the electronic structure and interactions…
Photosynthetic organisms use networks of chromophores to absorb sunlight and deliver the energy to reaction centres, where charge separation triggers a cascade of chemical steps to store the energy. We present a detailed model of the…
Conjugated polymers offer potential for many diverse applications but we still lack a fundamental microscopic understanding of their electronic structure. Elementary photoexcitations - excitons - span only a few nanometres of a molecule,…
Photosystem I is a protein-pigment complex that performs photosynthesis in plants, green algae, and cyanobacteria. It contains an aggregate of chlorophylls that absorbs light and delivers the resulting electronic excitation to the special…
Excitation of a model photosynthetic molecular aggregate by incoherent sunlight is systematically examined. For a closed system, the excited state coherence induced by the sunlight oscillates with an average amplitude that is inversely…
A vibrational wavepacket in SF$_6$, created by impulsive stimulated Raman scattering with a few-cycle infrared pulse, is mapped onto five sulfur core-excited states using table-top soft X-ray transient absorption spectroscopy between…
Phycobilisomes are antenna protein complexes in cyanobacteria and red algae. In phycobilisomes, energy transfer is unidirectional with an extremely high quantum efficiency close to unity. We investigate intraprotein energy relaxation and…