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Coherent X-rays reveal the influence of cage effects on ultrafast water dynamics.
Perakis, Fivos; Camisasca, Gaia; Lane, Thomas J; Späh, Alexander; Wikfeldt, Kjartan Thor; Sellberg, Jonas A; Lehmkühler, Felix; Pathak, Harshad; Kim, Kyung Hwan; Amann-Winkel, Katrin; Schreck, Simon; Song, Sanghoon; Sato, Takahiro; Sikorski, Marcin; Eilert, Andre; McQueen, Trevor; Ogasawara, Hirohito; Nordlund, Dennis; Roseker, Wojciech; Koralek, Jake; Nelson, Silke; Hart, Philip; Alonso-Mori, Roberto; Feng, Yiping; Zhu, Diling; Robert, Aymeric; Grübel, Gerhard; Pettersson, Lars G M; Nilsson, Anders.
Afiliación
  • Perakis F; Department of Physics, AlbaNova University Center, Stockholm University, S-106 91, Stockholm, Sweden. f.perakis@fysik.su.se.
  • Camisasca G; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA. f.perakis@fysik.su.se.
  • Lane TJ; Department of Physics, AlbaNova University Center, Stockholm University, S-106 91, Stockholm, Sweden.
  • Späh A; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Wikfeldt KT; Department of Physics, AlbaNova University Center, Stockholm University, S-106 91, Stockholm, Sweden.
  • Sellberg JA; Department of Physics, AlbaNova University Center, Stockholm University, S-106 91, Stockholm, Sweden.
  • Lehmkühler F; Biomedical and X-ray Physics, Department of Applied Physics, AlbaNova University Center, KTH Royal Institute of Technology, S-10691, Stockholm, Sweden.
  • Pathak H; Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607, Hamburg, Germany.
  • Kim KH; Hamburg Centre for Ultrafast Imaging, Luruper Chaussee 149, 22761, Hamburg, Germany.
  • Amann-Winkel K; Department of Physics, AlbaNova University Center, Stockholm University, S-106 91, Stockholm, Sweden.
  • Schreck S; Department of Physics, AlbaNova University Center, Stockholm University, S-106 91, Stockholm, Sweden.
  • Song S; Department of Physics, AlbaNova University Center, Stockholm University, S-106 91, Stockholm, Sweden.
  • Sato T; Department of Physics, AlbaNova University Center, Stockholm University, S-106 91, Stockholm, Sweden.
  • Sikorski M; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Eilert A; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • McQueen T; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Ogasawara H; European XFEL, Holzkoppel 4, 22869, Schenefeld, Germany.
  • Nordlund D; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Roseker W; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Koralek J; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Nelson S; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Hart P; Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607, Hamburg, Germany.
  • Alonso-Mori R; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Feng Y; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Zhu D; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Robert A; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Grübel G; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Pettersson LGM; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
  • Nilsson A; SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California, CA, 94025, USA.
Nat Commun ; 9(1): 1917, 2018 05 15.
Article en En | MEDLINE | ID: mdl-29765052
The dynamics of liquid water feature a variety of time scales, ranging from extremely fast ballistic-like thermal motion, to slower molecular diffusion and hydrogen-bond rearrangements. Here, we utilize coherent X-ray pulses to investigate the sub-100 fs equilibrium dynamics of water from ambient conditions down to supercooled temperatures. This novel approach utilizes the inherent capability of X-ray speckle visibility spectroscopy to measure equilibrium intermolecular dynamics with lengthscale selectivity, by measuring oxygen motion in momentum space. The observed decay of the speckle contrast at the first diffraction peak, which reflects tetrahedral coordination, is attributed to motion on a molecular scale within the first 120 fs. Through comparison with molecular dynamics simulations, we conclude that the slowing down upon cooling from 328 K down to 253 K is not due to simple thermal ballistic-like motion, but that cage effects play an important role even on timescales over 25 fs due to hydrogen-bonding.
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Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2018 Tipo del documento: Article País de afiliación: Suecia
Texto completo
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Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2018 Tipo del documento: Article País de afiliación: Suecia