13 October 2014 to 7 November 2014
Nordita, Stockholm
Europe/Stockholm timezone

Microscopic Properties of Liquid Water from Combined Ab Initio Molecular Dynamics and Energy Decomposition Studies

21 Oct 2014, 17:00
1h
FD5 (Nordita, Stockholm)

FD5

Nordita, Stockholm

Speaker

Prof. Thomas Kuhne (University of Paderborn)

Description

A new energy decomposition analysis for periodic systems based on absolutely localized molecular orbitals is presented [1, 2]. In combination with the recently developed ”Car-Parrinello-like approach to Born-Oppenheimer MD” [3] this not only allows for ab initio molecular dynamics simulations on previously inaccessible time and length scales, but also provide unprecedented insights into the nature of hydrogen bonding between water molecules. The effectiveness of this new combined approach is demonstrated on liquid water and the water/air interface [4, 5]. Our simulations reveal that although a water molecule forms, on average, two strong donor and two strong acceptor bonds, there is a significant asymmetry in the energy of these contacts. We demonstrate that this asymmetry is a result of small instantaneous distortions of hydrogen bonds and show that the distinct features of the X-ray absorption spectra originate from molecules with high instantaneous asymmetry [1, 2, 6, 7]. [1] T. D. Kuhne and R. Z. Khaliullin, Nature Comm. 4, 1450 (2013). [2] R. Z. Khaliullin and T. D. Kuhne, Phys. Chem. Chem. Phys. 15, 15746 (2013). [3] T. D. Kuhne, M. Krack, F. Mohamed and M. Parrinello, Phys. Rev. Lett. 98, 066401 (2007). [4] T. D. Kuhne, M. Krack and M. Parrinello, J. Chem. Theory Comput. 5, 235 (2009). [5] T. D. Kuhne, T. A. Pascal, E. Kaxiras and Y. Jung, J. Phys. Chem. Lett. 2, 105 (2011). [6] C. Zhang, R. Z. Khaliullin, D. Bovi, L. Guidoni and T. D. Kuhne, J. Chem. Phys. Lett. 4, 3245 (2013) [7] R. Z. Khaliullin and T. D. Kuhne, J. Am. Chem. Soc. 136, 3395 (2014).

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