2010/08/20 by Jan Roden, Walter T. Strunz, Alexander Eisfeld · 4 citations
Chemistry · Engineering · Physics and Astronomy · #Molecular Junctions and Nanostructures #Photochemistry and Electron Transfer Studies #Spectroscopy and Quantum Chemical Studies #cond-mat.soft #physics.chem-ph #quant-ph
paper · pdf · doi:10.1063/1.3512979
published as J. Chem. Phys. 134, 034902 (2011)
arxiv created 2010/08/20 · openalex publication_date 2011/01/20 · arxiv updated 2011/06/14 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
In many molecular systems one encounters the situation where electronic excitations couple to a quasi-continuum of phonon modes. The interaction to that often structured continuum may be highly frequency dependent, e.g. due to some weakly damped high frequency modes. To handle such a situation, an approach combining the non-markovian quantum state diffusion description of open quantum systems with an efficient but abstract approximation was recently applied to calculate energy transfer and absorption spectra of molecular aggregates [J. Roden, A. Eisfeld, W. Wolff, W. T. Strunz, Phys. Rev. Lett. 103, 058301 (2009)]. To explore the validity of the used approximation for such complicated systems, in the present work we compare the calculated (approximative) absorption spectra with exact results. These are obtained from the method of pseudomodes, which we show to be capable of determining the exact spectra for small aggregates and a few pseudomodes. It turns out that in the cases considered, the results of the two approaches mostly agree quite well. The advantages and disadvantages of the two approaches are discussed.