The solvation of molecules in water is pivotal for a myriad of molecular phenomena and is of crucial importance to understand diverse issues such as chemical reactivity and biomolecular function. It has been shown that laser techniques in the infrared (IR) and Terahertz (THz) frequency ranges offer fundamental insights into hydration from small solutes to proteins. In bulk liquid, motions of water molecules lead to ultrafast fluctuations at femto- to pico-second time scales. Underlying molecular processes range from diffusional motions spanning nanoseconds, rattling modes of anions and cations within their solvation shells on a ps time scale, the breaking and reformation of hydrogen bonds, and includes sub-100 fs librational motions. Here we report unprecedented non-linear THz experiments on water molecules in the liquid phase. This novel finding indicate that inducing anisotropy in bulk liquids is feasible.
*Funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy – EXC-2033 – Projektnummer 390677874, ERC Advanced Grant 695437. This work is part of the research programme of the Netherlands Organisation for Scientific Research (NWO) and supported by CALIPSOplus (grant agreement no. 730872, EU-H2020). T. H.-G. and L. R. P. thank the U.S. DOE under the Basic Energy Sciences program CPIMS, Contract No. DE-AC02-05CH11231. K. C. B. thanks the California Alliance Postdoctoral Fellowship. T. H.-G. appreciates the support received as a RESOLV Fellow while on sabbatical in Bochum Germany. This research used computational resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, under an ASCR Leadership Computing Challenge (ALCC) award.
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Presenters
Fabio Novelli
Department of Physical Chemistry II, Ruhr University Bochum, 44780 Bochum, Germany
Authors
Fabio Novelli
Department of Physical Chemistry II, Ruhr University Bochum, 44780 Bochum, Germany
Luis Ruiz Pestana
Pitzer Center for Theoretical Chemistry, Departments of Chemistry, Chemical and Biomolecular
Kochise Bennett
Pitzer Center for Theoretical Chemistry, Departments of Chemistry, Chemical and Biomolecular
Nils Dessmann
Radboud University, FELIX Laboratory, Toernooiveld 7, Nijmegen, Netherlands
Federico Sebastiani
Department of Physical Chemistry II, Ruhr University Bochum, 44780 Bochum, Germany
Ellen Adams
Department of Physical Chemistry II, Ruhr University Bochum, 44780 Bochum, Germany
Kamyar Saeedi Ilkhchy
Radboud University, FELIX Laboratory, Toernooiveld 7, Nijmegen, Netherlands
Nikolas Stavrias
Radboud University, FELIX Laboratory, Toernooiveld 7, Nijmegen, Netherlands
Viktoria Eless
Radboud University, FELIX Laboratory, Toernooiveld 7, Nijmegen, Netherlands
Thorsten Ockelmann
Department of Physical Chemistry II, Ruhr University Bochum, 44780 Bochum, Germany
Alejandro Colchero
Department of Physical Chemistry II, Ruhr University Bochum, 44780 Bochum, Germany
Claudius Hoberg
Department of Physical Chemistry II, Ruhr University Bochum, 44780 Bochum, Germany
Gerhard Schwaab
Department of Physical Chemistry II, Ruhr University Bochum, 44780 Bochum, Germany
Teresa Head-Gordon
Pitzer Center for Theoretical Chemistry, Departments of Chemistry, Chemical and Biomolecular
University of California, Berkeley
Chemistry, University of California, Berkeley
Martina Havenith
Department of Physical Chemistry II, Ruhr University Bochum, 44780 Bochum, Germany
