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A remarkable amount of theoretical research has been carried out to elucidate the physical origins of the recently observed long-lived quantum coherence in the electronic energy transfer process in biological photosynthetic systems.…
The idea that excitonic state (electronic) coherences are of fundamental importance to natural photosynthesis gained popularity when, a decade ago, slowly dephasing quantum beats were observed in the two-dimensional electronic spectra of…
Photosynthetic antenna complexes capture and concentrate solar radiation by transferring the excitation to the reaction center which stores energy from the photon in chemical bonds. This process occurs with near-perfect quantum efficiency.…
During the first steps of photosynthesis, the energy of impinging solar photons is transformed into electronic excitation energy of the light-harvesting biomolecular complexes. The subsequent energy transfer to the reaction center is…
Quantum effects in photosynthetic energy transport in nature, especially for the typical Fenna-Matthews-Olson (FMO) complexes, are extensively studied in quantum biology. Such energy transport processes can be investigated as open quantum…
This thesis looks at the electronic energy transfer in the Fenna-Matthews-Olson complex, in which evidence of long-lived coherence has been observed in 2-dimensional infrared experiments. I use three techniques: the numerically exact…
Energy transfer within photosynthetic systems can display quantum effects such as delocalized excitonic transport. Recently, direct evidence of long-lived coherence has been experimentally demonstrated for the dynamics of the…
Long-lived electronic coherences in various photosynthetic complexes at cryogenic and room temperature have generated vigorous efforts both in theory and experiment to understand their origins and explore their potential role to biological…
We show that the efficient excitation energy transfer in the Fenna-Matthews-Olson molecular aggregate under realistic physiological conditions is fueled by underdamped vibrations of the embedding proteins. For this, we present numerically…
Open quantum system approaches are widely used in the description of physical, chemical and biological systems. A famous example is electronic excitation transfer in the initial stage of photosynthesis, where harvested energy is transferred…
Photosynthesis is an important and complex physical process in nature, whose comprehensive understanding would have many relevant industrial applications, for instance in the field of energy production. In this paper we propose a quantum…
The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond…
We investigate the role of long-lasting quantum coherence in the efficiency of energy transport at room temperature in Fenna-Matthews-Olson photosynthetic complexes. The excitation energy transfer due to the coupling of the light harvesting…
Near-unity energy transfer efficiency has been widely observed in natural photosynthetic complexes. This phenomenon has attracted broad interest from different fields, such as physics, biology, chemistry and material science, as it may…
We present a detailed theoretical study of the transfer of electronic excitation energy through the Fenna-Matthews-Olson (FMO) pigment-protein complex, using the new developed modified scaled hierarchical approach [Shi Q. et al, J Chem Phys…
Enhancing optical nonlinearities so that they become appreciable on the single photon level and lead to nonclassical light fields has been a central objective in quantum optics for many years. After this has been achieved in individual…
Two-dimensional optical spectroscopy experiments have shown that exciton transfer pathways in the Fenna-Matthews-Olson (FMO) photosynthetic complex differ drastically under reduced and oxidised conditions, suggesting a functional role for…
We present numerically exact results for the quantum coherent energy transfer in the Fenna-Matthews-Olson molecular aggregate under realistic physiological conditions, including vibrational fluctuations of the protein and the pigments for…
In the primary step of light-harvesting, the energy of a photon is captured in antenna chlorophyll as an exciton. Its efficient conversion to stored chemical potential occurs in the special pair reaction center, which has to be reached by…
The first exact quantum simulation of a real molecular system (HD$^+$) under strong ro-vibrational coupling to a quantized optical cavity mode in thermal equilibrium is presented. Theoretical challenges in describing strongly coupled…