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14 March 2016Theory of coupled hybrid inorganic/organic systems: Excitation transfer at semiconductor/molecule interfaces
We derive a theoretical framework for describing hybrid organic-inorganic systems consisting of an ordered organic molecular layer coupled to a semiconductor quantum well (e.g., ZnO). A Heisenberg equation of motion technique based on a density matrix formalism is applied to derive dynamical equations for the composite system on a mesoscopic scale. Our theoretical approach focuses on the inuence of nonradiative Förster excitation transfer across the hybrid interface on linear optical absorption spectra. Therefore, the dielectric screening is discussed at the interface of two materials with different dielectric constants. Moreover, the Förster transfer matrix element is calculated in the point-dipole approximation. For a consistent theoretical description of both constituents (i.e., the molecular layer and the semiconductor substrate), the problem is treated in momentum space. Solving the equations of motion for the microscopic polarizations in frequency space directly leads to an equation for the frequency-dependent linear absorption coefficient. Our theoretical approach forms the basis for studying parameter regimes and geometries with optimized excitation transfer efficiency across the semiconductor/ molecule interface.
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Judith Specht, Eike Verdenhalven, Sverre Theuerholz, Andreas Knorr, Marten Richter, "Theory of coupled hybrid inorganic/organic systems: Excitation transfer at semiconductor/molecule interfaces," Proc. SPIE 9746, Ultrafast Phenomena and Nanophotonics XX, 97460F (14 March 2016); https://doi.org/10.1117/12.2207638