Download Dissipative Exciton Dynamics in Light-Harvesting Complexes by Marco Schröter PDF

By Marco Schröter

Marco Schröter investigates the impression of the neighborhood surroundings at the exciton dynamics inside molecular aggregates, which construct, e.g., the light-harvesting complexes of crops, micro organism or algae via the hierarchy equations of movement (HEOM) strategy. He addresses the subsequent questions intimately: How can coherent oscillations inside a approach of coupled molecules be interpreted? What are the adjustments within the quantum dynamics of the procedure for expanding coupling power among digital and nuclear levels of freedom? To what volume does decoherence govern the strength move homes of molecular aggregates?.

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146) and 44 2. Dissipative quantum dynamics due to the conservation of energy and momentum. The integer numbers ji account for the possibility of multiple interactions of the sample with the same pulse. The phase-matching condition, Eq. 145), limits the observable signal in the experiment to certain contributions of the overall nonlinear signal. This gives rise to a variety of different nonlinear spectroscopy techniques focussing on special contributions. Frequently, third order spectroscopy techniques are used to investigate the excitation energy transport in molecular aggregates and other processes.

64), required by the HEOM formalism, cf. 2. This is not the case for arbitrary spectral densities. Meier and Tannor [61] developed a numerical parametrization scheme which is based on the assumption that the actual dynamics of the system only depends on the value of the spectral density at the transition energies of the system and not on the shape of its individual components. They successfully parametrized an Ohmic spectral density, Eq. 109), by an expansion into three Lorentzian terms, using the parametrized spectral density, K ¯ J(ω) = xk k=1 ω [(ω + yk )2 zk2 ][(ω + − yk )2 + zk2 ] .

According to Eq. 1) it can be decomposed into a system, a bath, and a system-bath interaction part. Thus, the time evolution of the full density matrix in path integral representation is given by [52] αt αt Dα ρ(αt , αt , t) = α0 Dα e i(Ss [α]+Sb [α]+Ss−b [α]) ρ(α0 , α0 , t0 ) α0 × e− i(Ss [α ]+Sb [α ]+Ss−b [α ]) = U(αt , αt , t; α0 , α0 , t0 )ρ(α0 , α0 , t0 ). 59) α0 where the system-bath interaction is fully covered by the FeynmanVernon influence functional F[α, α ] [55]. Note that while working in Liouville space it is necessary to keep track of the order of the terms as for instance the time evolution operator does not commute with the density operator.

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