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

By Marco Schröter

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

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The environmental part of the spectral densities can be described by so-called Ohmic spectral densities, which are characterised by a linear rise of J(ω) for small frequencies and an exponential or Lorentzian cut-off. 3. Spectral density models 35 where the Heaviside function Θ assures that Jm (ω) = 0 for ω < 0. ηm represents the strength of the system-bath interaction and the cut-off term exp(−ω/˜ γm ) determines the shape of Jm (ω) for values of ω which are similar to or larger than the cut-off frequency γ˜m .

The monomeric correlation function associated with the Debye spectral density can be calculated analytically using Eq. 106) and the residue theorem. One obtains [46] Cm (t) = 2 β˜ γm ηm γ˜m cot − i e−˜γm t 2 2 2 ∞ γ e−γν t 2ηm γ˜m ν + . e. the hyperbolic cotangent in Eq. 106), whereas the first term stems from the pole of the spectral density itself [46]. Note that the Ohmic and Debye spectral densities describe the environmental part of the overall spectral density fairly well, but provide a rather crude approximation for the intra-molecular part as the latter is usually not continuous.

88) −∞ Expanding the integral on the right-hand side of Eq. 89) allows one to express C(t) by the half-sided Fourier integral 1 C(t) = 2π = 1 2π ∞ dω e− iωt (1 + n(ω)) + e iωt n(ω) C (−) (ω) 0 ∞ dω cos(ωt) coth 0 βω 2 − i sin(ωt) C (−) (ω). 3. Spectral density models 31 However, the bath correlation functions C(t) for the system-bath models introduced in Sec. 1 can be evaluated analytically. The bath correlation function for SBM I and IIa can be evaluated introducing creation and annihilation operators for the harmonic oscillator [31].

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