Related papers: Resonant Vibrational-Electronic Coupling between P…
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…
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…
We demonstrate that the coupling of excitonic and vibrational motion in biological complexes can provide mechanisms to explain the long-lived oscillations that have been obtained in non linear spectroscopic signals of different…
We recently proposed effective normal modes for excitonically coupled aggregates which exactly transform the energy transfer Hamiltonian into a sum of one-dimensional Hamiltonians along the effective normal modes. Identifying physically…
Understanding how the effectiveness of natural photosynthetic energy harvesting systems arises from the interplay between quantum coherence and environmental noise represents a significant challenge for quantum theory. Recently it has begun…
A vibronic-exciton model is applied to investigate the mechanism of enhancement of coherent oscillations due to mixing of electronic and nuclear degrees of freedom recently proposed as the origin of the long-lived oscillations in 2D spectra…
The concept of \textit{optical} exciton - a photo-excited bound electron-hole pair within a crystal - is routinely used to interpret and model a wealth of excited-state phenomena in semiconductors. Beside originating sub-band gap signatures…
We report two-dimensional electronic spectroscopy (2DES) experiments on the bacterial reaction center (BRC) from purple bacteria, revealing hidden excitonic and vibronic structure. Through analysis of the coherent dynamics of the BRC we…
A general theory of electronic excitations in aggregates of molecules coupled to intramolecular vibrations and the harmonic environment is developed for simulation of the third-order nonlinear spectroscopy signals. The model is applied in…
The biological effects of electromagnetic fields on proteins remain controversial beyond well-established thermal mechanisms, particularly with respect to frequency-dependent responses. Here, we propose that electromagnetic waves can…
The interplay between exctions and vibrations is considered to be a key factor in determining the exciton transfer properties in light-harvesting exciton transfer complexes. Here we study this interplay theoretically in a model for exciton…
In this paper we consider the essential electronic excited states in parallel chains of semiconducting polymers that are currently being explored for photovoltaic and light-emitting diode applications. In particular, we focus upon various…
Recently, nuclear vibrational contribution signatures in 2D electronic spectroscopy have attracted considerable interest, in particular as regards interpretation of the oscillatory transients observed in light-harvesting complexes. These…
Recent time-resolved spectroscopic experiments have indicated that vibronic coupling plays a vital role in facilitating the process of singlet fission. In this work, which forms the first article of a series, we set out to unravel the…
Singlet fission, the molecular process through which photons are effectively converted into pairs of lower energy triplet excitons, holds promise as a means of boosting photovoltaic device efficiencies. In the preceding article of this…
The time-development of photoexcitations in molecular aggregates exhibits specific dynamics of electronic states and vibrational wavefunction. We discuss the dynamical formation of entanglement between electronic and vibrational degrees of…
In 2D electronic spectroscopy studies, long-lived quantum beats have recently been observed in photosynthetic systems, and it has been suggested that the beats are produced by quantum mechanically mixed electronic and vibrational states.…
Vibronic coupling constants in the monoanionic, trianionic, and excited states of picene are evaluated from the total energy gradients using the density functional theory. Employing the calculated vibronic coupling constants in the excited…
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…
The effects of the electron-phonon interaction on optical excitations can be understood in terms of exciton-phonon coupling, and require a careful treatment in low-dimensional materials with strongly bound excitons or strong electron-hole…