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X-Ray Studies of Water

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Synchrotron Light Sources and Free-Electron Lasers

Abstract

In this chapter we discuss a number of x-ray techniques that have been used at synchrotron radiation and x-ray free-electron laser facilities to study the water structure and dynamics as well as its thermodynamic response functions. The focus of these investigations is on temperature-dependent properties ranging from hot water at 363 K down to deep supercooled conditions at 227 K. We review the experimental information content obtained from x-ray absorption spectroscopy (XAS), x-ray emission spectroscopy (XES), or often denoted resonant x-ray inelastic scattering (RIXS), wide- (WAXS) and small-angle x-ray scattering (SAXS), x-ray photon correlation spectroscopy (XPCS), and lastly x-ray speckle visibility spectroscopy (XSVS). We propose a number of hypotheses related to water that can be tested against the information obtained from the various x-ray techniques. The picture emerging which is mostly consistent with all the information content is the following:

At ambient temperatures, most molecules favor a closer packing arrangement than tetrahedral coordination, with strongly distorted hydrogen bonds, which allows the quantized low-energy vibrational modes to be excited and contribute to the entropy. On the other hand, the enthalpically favored tetrahedrally bonded water patches appear as local fluctuations, leading to a competition between entropy and enthalpy. Upon cooling, the number of molecules participating in tetrahedral structures and the size of the tetrahedral patches increase. The two local structures are connected to the liquid-liquid critical point hypothesis in supercooled water and correspond to macroscopic high-density liquid (HDL) and low-density liquid (LDL) phases. We demonstrate that the HDL-like local structure deviates from a tetrahedral coordination not only through a collapse of the second shell but also through severe distortions around the first coordination shell. Furthermore, from dynamic measurements on amorphous ice, we show evidence of an HDL glass transition and that ultraviscous supercooled liquid also undergoes a liquid-liquid transition (LLT). Lastly, we report that the appearance of a temperature-dependent cage effects in the ultrafast dynamics is strongly correlated to the formation and breaking up of tetrahedral LDL-like structures.

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Abbreviations

HDA:

high-density amorphous ice

HDL:

high-density liquid

HWHM:

half width at half maximum

IXS:

inelastic x-ray scattering

LDA:

low-density amorphous ice

LDL:

low-density liquid

LLCP:

liquid-liquid critical point

LLT:

liquid-liquid transition

PDF:

pair distribution function

RIXS:

resonant x-ray inelastic scattering

SAXS:

small-angle x-ray scattering

VHDA:

very high-density amorphous ice

WAXS:

wide-angle x-ray scattering

XAS:

x-ray absorption spectroscopy

XES:

x-ray emission spectroscopy

XPCS:

x-ray photon correlation spectroscopy

XRS:

x-ray Raman scattering

XSVS:

x-ray speckle visibility spectroscopy

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Acknowledgments

In particular we like to thank for the close collaboration over two decades with Lars G.M. Pettersson at Stockholm University. The experimental results discussed in the present chapter have naturally been obtained together with a large number of extraordinary scientists who have worked very dedicatedly on these, many times very difficult, experiments. All have been essential to this effort, but K. Amann-Winkel, C. Benmore, U. Bergmann, C. Chen, G. Grübel, Y. Harada, C. Huang, N. Huang, K. H, Kim, T. J. Lane, F. Lehmkühler, D. Mariedahl, T. McQueen, D. Nordlund, L. Å. Näslund, H. Ogasawara, H. Pathak, J. Sellberg, L. B. Skinner, A. Späh, T. Tokushima, I. Waluyo, and Ph. Wernet deserve special credit. We acknowledge support from the European Research Council (ERC) Advanced Grant under Project No. 667205 and the Swedish National Research Council (VR) under Grant No. 2013-8823.

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  1. Physics Department, Stockholm University, Stockholm, Sweden

    Anders Nilsson & Fivos Perakis

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  1. Anders Nilsson
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  2. Fivos Perakis
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Correspondence to Anders Nilsson .

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Editors and Affiliations

  1. Helmholtz-Zentrum Berlin, BESSY II, Berlin, Germany

    Eberhard J. Jaeschke

  2. Zentrum für Synchrotronstrahlung (DELTA), Technische Universität Dortmund, Dortmund, Germany

    Shaukat Khan

  3. Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron DESY, Hamburg, Germany

    Jochen R. Schneider

  4. Linac Coherent Light Source, SLAC National Accelerator Laboratory Linac Coherent Light Source, Menlo Park, CA, USA

    Jerome B. Hastings

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Nilsson, A., Perakis, F. (2020). X-Ray Studies of Water. In: Jaeschke, E., Khan, S., Schneider, J., Hastings, J. (eds) Synchrotron Light Sources and Free-Electron Lasers. Springer, Cham. https://doi.org/10.1007/978-3-030-23201-6_69

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