Enhancement of the local asymmetry in the hydrogen bond network of liquid water by an ultrafast electric field pulse

Condensed phase electron decomposition analysis based on density functional theory has recently revealed an asymmetry in the hydrogen-bond network in liquid water, in the sense that a significant population of water molecules are simultaneously donating and accepting one strong hydrogen-bond and another substantially weaker one. Here we investigate this asymmetry, as well as broader structural and energetic features of water’s hydrogen-bond network, following the application of an intense electric field square pulse that invokes the ultrafast reorientation of water molecules. We find that the necessary field-strength required to invoke an ultrafast alignment in a picosecond time window is on the order of 108 Vm−1. The resulting orientational anisotropy imposes an experimentally measurable signature on the structure and dynamics of the hydrogen-bond network, including its asymmetry, which is strongly enhanced. The dependence of the molecular reorientation dynamics on the field-strength can be understood by relating the magnitude of the water dipole–field interaction to the rotational kinetic energy, as well as the hydrogen-bond energy.

[1]  A. M. Saitta,et al.  Ab initio molecular dynamics study of dissociation of water under an electric field. , 2012, Physical review letters.

[2]  Rustam Z. Khaliullin,et al.  Analysis of charge transfer effects in molecular complexes based on absolutely localized molecular orbitals. , 2008, The Journal of chemical physics.

[3]  A. Kalinichev,et al.  Hydrogen Bonding in Supercritical Water. 1. Experimental Results , 1995 .

[4]  C. Vega,et al.  Phase diagram of water under an applied electric field. , 2011, Physical review letters.

[5]  Matthias Krack,et al.  Static and Dynamical Properties of Liquid Water from First Principles by a Novel Car-Parrinello-like Approach. , 2009, Journal of chemical theory and computation.

[6]  Field-exposed water in a nanopore: liquid or vapour? , 2008, Physical chemistry chemical physics : PCCP.

[7]  Joost VandeVondele,et al.  Isobaric-isothermal molecular dynamics simulations utilizing density functional theory: an assessment of the structure and density of water at near-ambient conditions. , 2009, The journal of physical chemistry. B.

[8]  M. Gavish,et al.  The Role of Crystal Polarity in α-Amino Acid Crystals for Induced Nucleation of Ice , 1992, Science.

[9]  S. Suresh.  Disruption of hydrogen bond structure of water near charged electrode surfaces. , 2007, The Journal of chemical physics.

[10]  Michael F. Toney,et al.  Voltage-dependent ordering of water molecules at an electrode–electrolyte interface , 1994, Nature.

[11]  H. M. Jones,et al.  The influence of pressure and conductivity on the pulsed breakdown of water , 1994 .

[12]  J. Finney,et al.  Water? What's so special about it? , 2004, Philosophical transactions of the Royal Society of London. Series B, Biological sciences.

[13]  David Vanderbilt,et al.  First-principles approach to insulators in finite electric fields. , 2002, Physical review letters.

[14]  Rustam Z. Khaliullin,et al.  Covalency of hydrogen bonds in liquid water can be probed by proton nuclear magnetic resonance experiments , 2015, Nature Communications.

[15]  M. Eisenstein,et al.  The role of crystal polarity in alpha-amino acid crystals for induced nucleation of ice. , 1992, Science.

[16]  W. M. Haynes.  CRC Handbook of Chemistry and Physics , 1990 .

[17]  Matthias Krack,et al.  Efficient and accurate Car-Parrinello-like approach to Born-Oppenheimer molecular dynamics. , 2007, Physical review letters.

[18]  G. D'Inzeo,et al.  Water response to intense electric fields: A molecular dynamics study , 2015, Bioelectromagnetics.

[19]  Julia M. Goodfellow,et al.  Molecular dynamics study , 1997 .

[20]  M. Liberti,et al.  Human aquaporin 4 gating dynamics under and after nanosecond-scale static and alternating electric-field impulses: a molecular dynamics study of field effects and relaxation. , 2013, The Journal of chemical physics.

[21]  Rustam Z. Khaliullin,et al.  Microscopic properties of liquid water from combined ab initio molecular dynamics and energy decomposition studies. , 2013, Physical chemistry chemical physics : PCCP.

[22]  J. Bass,et al.  Hydrogen bonding in supercritical water. 2. Computer simulations , 1997 .

[23]  Rustam Z. Khaliullin,et al.  Nature of the asymmetry in the hydrogen-bond networks of hexagonal ice and liquid water. , 2014, Journal of the American Chemical Society.

[24]  Mischa Bonn,et al.  Vibrational Spectroscopy and Dynamics of Water. , 2016, Chemical reviews.

[25]  R. Levy,et al.  Field strength dependence of dielectric saturation in liquid water , 1990 .

[26]  B. Bagchi.  Molecular Relaxation in Liquids , 2012 .

[27]  Niall J. English,et al.  Dipolar response and hydrogen-bond kinetics in liquid water in square-wave time-varying electric fields , 2014 .

[28]  D. Chandler,et al.  Hydrogen-bond kinetics in liquid water , 1996, Nature.

[29]  D. Elton,et al.  Polar nanoregions in water: a study of the dielectric properties of TIP4P/2005, TIP4P/2005f and TTM3F. , 2014, The Journal of chemical physics.

[30]  P. Cummings,et al.  Hydrogen bonding in supercritical water , 1994 .

[31]  A. Pasquarello,et al.  Dynamical monopoles and dipoles in a condensed molecular system: The case of liquid water , 2003 .

[32]  Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation , 2018, Nature Communications.

[33]  Oriol Vendrell,et al.  Ultrafast energy transfer to liquid water by sub-picosecond high-intensity terahertz pulses: an ab initio molecular dynamics study. , 2013, Angewandte Chemie.

[34]  J. B. Baxter,et al.  Terahertz spectroscopy. , 2011, Analytical chemistry.

[35]  S J Suresh,et al.  Influence of electric field on the hydrogen bond network of water. , 2006, The Journal of chemical physics.

[36]  Rustam Z Khaliullin,et al.  Electronic signature of the instantaneous asymmetry in the first coordination shell of liquid water , 2013, Nature Communications.

[37]  Alfredo Pasquarello,et al.  Ab initio molecular dynamics in a finite homogeneous electric field. , 2002, Physical review letters.

[38]  L. Skinner,et al.  Structure of the floating water bridge and water in an electric field , 2012, Proceedings of the National Academy of Sciences.

[39]  Mark S. Conradi,et al.  ARE THERE HYDROGEN BONDS IN SUPERCRITICAL WATER , 1997 .

[40]  Daniel Molter,et al.  Terahertz time-domain spectroscopy of gases, liquids, and solids. , 2011, Chemphyschem : a European journal of chemical physics and physical chemistry.

[41]  P. Kusalik,et al.  Electrofreezing of Liquid Water: A Microscopic Perspective , 1996 .

[42]  Rustam Z. Khaliullin,et al.  Recent achievements in ab initio modelling of liquid water , 2013, 1303.2067.

[43]  A. Zasetsky.  Dielectric relaxation in liquid water: two fractions or two dynamics? , 2011, Physical review letters.

[44]  W. Luck,et al.  Spectroscopic investigations of the structure of liquid water and aqueous solutions , 1979 .

[45]  Mischa Bonn,et al.  Ultrafast vibrational energy transfer at the water/air interface revealed by two-dimensional surface vibrational spectroscopy. , 2011, Nature chemistry.

[46]  Michele Parrinello,et al.  Water Molecule Dipole in the Gas and in the Liquid Phase , 1999 .

[47]  Gerhard Hummer,et al.  Water in nonpolar confinement: from nanotubes to proteins and beyond. , 2008, Annual review of physical chemistry.

[48]  A. Mark,et al.  Electrofreezing of confined water. , 2004, The Journal of chemical physics.

[49]  Raffaele Resta,et al.  MACROSCOPIC POLARIZATION IN CRYSTALLINE DIELECTRICS : THE GEOMETRIC PHASE APPROACH , 1994 .

[50]  M. Jhon,et al.  The effect of an external electric field on the structure of liquid water using molecular dynamics simulations , 1999 .

[51]  Michele Parrinello,et al.  A hybrid Gaussian and plane wave density functional scheme , 1997 .

[52]  A. Vegiri.  Dynamic response of liquid water to an external static electric field at T=250 K ☆ , 2004 .

[53]  Y. Zhang,et al.  Amyloid Properties of Asparagine and Glutamine in Prion-like Proteins. , 2016, ACS chemical neuroscience.

[54]  Joost VandeVondele,et al.  Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases. , 2007, The Journal of chemical physics.

[55]  W. Luck.  The importance of cooperativity for the properties of liquid water , 1998 .

[56]  Michele Parrinello,et al.  Quickstep: Fast and accurate density functional calculations using a mixed Gaussian and plane waves approach , 2005, Comput. Phys. Commun..

[57]  Howard Goldstein,et al.  What's So Special? , 1999 .

[58]  Niall J. English,et al.  Hydrogen bonding and molecular mobility in liquid water in external electromagnetic fields , 2003 .

[59]  S. Grimme,et al.  A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. , 2010, The Journal of chemical physics.

[60]  G. Sutmann.  Structure formation and dynamics of water in strong external electric fields , 1998 .

[61]  Daniel C. Elton,et al.  Understanding the dielectric properties of water , 2016 .

[62]  T. Kampfrath,et al.  Transient birefringence of liquids induced by terahertz electric-field torque on permanent molecular dipoles , 2016, Nature Communications.

[63]  Efthimios Kaxiras,et al.  New Insights into the Structure of the Vapor/Water Interface from Large-Scale First-Principles Simulations. , 2011, The journal of physical chemistry letters.

[64]  N. English,et al.  Perspectives on external electric fields in molecular simulation: progress, prospects and challenges. , 2015, Physical chemistry chemical physics : PCCP.

[65]  T. Kühne,et al.  Second generation Car–Parrinello molecular dynamics , 2012, 1201.5945.

[66]  N. Kondo,et al.  Hydration and hydrogen bond network of water around hydrophobic surface investigated by terahertz spectroscopy. , 2014, The Journal of chemical physics.