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The modeling of the absorption lineshape for embedded molecules through a polarizable QM/MM approach

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Abstract

We present a computational strategy to simulate the absorption lineshape of a molecule embedded in a complex environment by using a polarizable QM/MM approach. This strategy is presented in two alternative formulations, one based on a molecular dynamics simulation of the structural fluctuations of the system and the other using normal modes and harmonic frequencies calculated on optimized geometries. The comparison for the case of a chromophore within a strongly inhomogeneous and structured environment, namely the intercalation pocket of DNA, shows that the MD-based approach is able to reproduce the experimental spectral bandshape. In contrast, the static approach overestimates the vibronic coupling, resulting in a much broader band.

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Acknowledgements

MM gratefully acknowledges financial support from the EU Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement No. 642294 (ITN-EJD: Theoretical Chemistry and Computational Modelling).

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Author notes

  1. Maximilian F. S. J. Menger

    Present address: Present address: Institute of Theoretical Chemistry, University of Vienna, Währinger Str. 17, A-1090, Vienna, Austria

Authors and Affiliations

  1. Department of Chemistry, University of Pisa, via G. Moruzzi 13, 56124, Pisa, Italy

    Daniele Loco, Sandro Jurinovich, Lorenzo Cupellini, Maximilian F. S. J. Menger & Benedetta Mennucci

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  1. Daniele Loco
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Correspondence to Daniele Loco or Benedetta Mennucci.

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Loco, D., Jurinovich, S., Cupellini, L. et al. The modeling of the absorption lineshape for embedded molecules through a polarizable QM/MM approach. Photochem Photobiol Sci 17, 552–560 (2018). https://doi.org/10.1039/c8pp00033f

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  • DOI: https://doi.org/10.1039/c8pp00033f

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