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By Marco Schröter

ISBN-10: 3658092815

ISBN-13: 9783658092818

ISBN-10: 3658092823

ISBN-13: 9783658092825

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

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This facilitates a strong mixing of the electronic and vibrational DOFs, which has been discussed as one possible origin of long-living oscillations in the 2Dspectra of FMO [21]. , S1,1 = S1,2 = S, and therefore the monomer index m and the mode index ξ will be skipped. The temperature of the bath is chosen to be T = 300 K. e. the Huang-Rhys factor S, on the system dynamics, four different dimer scenarios are considered. They are characterised by means of their linear absorption spectra, population dynamics and 2D-spectra.

E. the interaction of the system and the field is described by Eq. 24), P [E(t), t] of a homogeneous sample is given by [31] P [E(t), t] = nmol tr {ρ(t)d} . 129) Here, d denotes the microscopic dipole operator, Eq. 26), and nmol stands for the volume density of the molecules in the sample volume. Note that E(t), d and P [E(t), t] are in general vectors, but for simplicity the vector character will be neglected in the following. , by the Schrödinger equation or the equations of motion introduced 40 2.

E(t − tn − . . − t1 ). 141) The nth order response function is defined as R(n) (tn , . . , t1 ) = in nmol Θ(t1 ) . . 142) with K(n) = . . d(I) (tn + . . + t1 ), d(I) (tn−1 + . . + t1 ) . . , × d(I) (t1 ) , d(I) (0) . 143) In analogy to the linear response function R(1) the nth order one, R(n) , contains all necessary information to evaluate the corresponding signals. The electric field, E(t), is in general defined by Eq. 132). e. n E(t) = ˜ ∗ (t) e− ikj r+ iωj t . 144) j=1 Note that the wave-vector and the carrier frequency of the signal field, resulting from the nonlinear polarization, need to obey the conditions ks = ±j1 k1 ± j2 k2 ± .

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Dissipative Exciton Dynamics in Light-Harvesting Complexes by Marco Schröter

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