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Sum Frequency Generation Spectra from Velocity-Velocity Correlation Functions: New Developments and Applications

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High Performance Computing in Science and Engineering ' 17

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Abstract

At the interface, the properties of water can be rather different from those observed in the bulk. In this chapter we present an overview of our computational approach to understand water structure and dynamics at the interface including atomistic and electronic structure details. In particular we show how Density Functional Theory-based molecular dynamics simulations (DFT-MD) of water interfaces can provide a microscopic interpretation of recent experimental results from surface sensitive vibrational Sum Frequency Generation spectroscopy (SFG). In our recent work we developed an expression for the calculation of the SFG spectra of water interfaces which is based on the projection of the atomic velocities on the local normal modes. Our approach permits to obtain the SFG signal from suitable velocity-velocity correlation functions, reducing the computational cost to that of the accumulation of a molecular dynamics trajectory, and therefore cutting the overhead costs associated to the explicit calculation of the dipole moment and polarizability tensor. Our method permits to interpret the peaks in the spectrum in terms of local modes, also including the bending region. The results for the water-air interface, obtained using extensive ab initio molecular dynamics simulations over 400 ns, are discussed in connection to recent phase resolved experimental data.

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Acknowledgements

This work was supported by the DFG Research Grant SU 752/2-1 and the DFG TRR146. All the dynamics were simulated on the supercomputers of the High Performance Computing Center (HLRS) of Stuttgart (Grant 2DSFG).

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Authors and Affiliations

  1. Johannes Gutenberg University Mainz, Staudinger Weg 7, 55099, Mainz, Germany

    Khatib Rémi & Sulpizi Marialore

Authors
  1. Khatib RĂ©mi
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  2. Sulpizi Marialore
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Correspondence to Sulpizi Marialore .

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Editors and Affiliations

  1. Zentrum fĂ¼r Informationsdienste und Hochleistungsrechnen (ZIH), Technische Universität Dresden, Dresden, Germany

    Wolfgang E. Nagel

  2. Abteilung fĂ¼r Angewandte Mathematik, Universität Freiburg, Freiburg, Germany

    Dietmar H. Kröner

  3. Höchstleistungsrechenzentrum Stuttgart (HLRS), Universität Stuttgart, Stuttgart, Germany

    Michael M. Resch

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Rémi, K., Marialore, S. (2018). Sum Frequency Generation Spectra from Velocity-Velocity Correlation Functions: New Developments and Applications. In: Nagel, W., Kröner, D., Resch, M. (eds) High Performance Computing in Science and Engineering ' 17 . Springer, Cham. https://doi.org/10.1007/978-3-319-68394-2_8

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