Water clusters: Untangling the mysteries of the liquid, one molecule at a time

Extensive terahertz laser vibration-rotation-tunneling spectra and mid-IR laser spectra have been compiled for several isotopomers of small (dimer through hexamer) water clusters. These data, in conjunction with new theoretical advances, quantify the structures, force fields, dipole moments, and hydrogen bond rearrangement dynamics in these clusters. This new information permits us to systematically untangle the intricacies associated with cooperative hydrogen bonding and promises to lead to a more complete molecular description of the liquid and solid phases of water, including an accurate universal force field.

[1]  Geoffrey A. Blake,et al.  Tunable far infrared laser spectrometers , 1991 .

[2]  H. Eugene Stanley,et al.  Liquid-Liquid Phase Transition: Evidence from Simulations , 1997 .

[3]  Geoffrey A. Blake,et al.  Molecular Interactions and Hydrogen Bond Tunneling Dynamics: Some New Perspectives , 1993, Science.

[4]  R. Saykally,et al.  Spectroscopic determination of the water pair potential. , 1999, Science.

[5]  D. D. Lucas,et al.  Pseudorotation in Water Trimer Isotopomers Using Terahertz Laser Spectroscopy , 1997 .

[6]  Z. Huang,et al.  High‐resolution near‐infrared spectroscopy of water dimer , 1989 .

[7]  U. Buck,et al.  The asymmetric cage structure of (H2O)7 from a combined spectroscopic and computational study , 1999 .

[8]  D. Wales,et al.  Theoretical study of the water pentamer , 1996 .

[9]  Sotiris S. Xantheas,et al.  Ab initio studies of cyclic water clusters (H2O)n, n=1–6. I. Optimal structures and vibrational spectra , 1993 .

[10]  K. Seff,et al.  CRYSTAL STRUCTURE OF A SODIUM SORPTION COMPLEX OF ZEOLITE X CONTAINING LINEAR NA32+ CLUSTERS , 1997 .

[11]  David Chandler,et al.  Structure and hydrogen bond dynamics of water-dimethyl sulfoxide mixtures by computer simulations. Interim report, April 1992-October 1993 , 1993 .

[12]  J. B. Paul,et al.  Infrared Cavity Ringdown Spectroscopy of the Water Cluster Bending Vibrations , 1999 .

[13]  L. Coudert,et al.  The submillimeter rotation tunneling spectrum of the water dimer , 1991 .

[14]  G. Blake,et al.  Pseudorotation in the D2O trimer. , 1994, Chemical physics letters.

[15]  R. Saykally,et al.  Vibration-Rotation Tunneling Spectra of the Water Pentamer: Structure and Dynamics , 1996, Science.

[16]  F. Keutsch,et al.  HIGH SYMMETRY EFFECTS ON HYDROGEN BOND REARRANGEMENT : THE 4.1 THZ VIBRATIONAL BAND OF (D2O)4 , 1999 .

[17]  D. Chandler,et al.  Transition pathways in a many-body system: Application to hydrogen-bond breaking in water , 1998 .

[18]  S. H. Chen,et al.  Molecular-dynamics study of incoherent quasielastic neutron-scattering spectra of supercooled water , 1997 .

[19]  Dudley H. Williams,et al.  Far-Infrared Absorption Spectra of Aqueous Solutions of Strong Electrolytes , 1968 .

[20]  R. C. Cohen,et al.  Measurement of the perpendicular rotation‐tunneling spectrum of the water dimer by tunable far infrared laser spectroscopy in a planar supersonic jet , 1989 .

[21]  John S. Muenter,et al.  THE STRUCTURE OF WATER DIMER FROM MOLECULAR BEAM ELECTRIC RESONANCE SPECTROSCOPY: PARTIALLY DEUTERATED DIMERS , 1977 .

[22]  D. Wales,et al.  Rearrangements of the water trimer , 1996 .

[23]  T. Dunning,et al.  The structure of the water trimer from ab initio calculations , 1993 .

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

[25]  E. Becker,et al.  Infrared Studies of Hydrogen Bonding of Water by the Matrix Isolation Technique , 1957 .

[26]  M. Schütz,et al.  Fluxionality and low‐lying transition structures of the water trimer , 1993 .

[27]  H. Lüthi,et al.  An ab initio derived torsional potential energy surface for (H2O)3. II. Benchmark studies and interaction energies , 1995 .

[28]  P. Wormer,et al.  Tunneling dynamics, symmetry, and far-infrared spectrum of the rotating water trimer. II. Calculations and experiments , 1996 .

[29]  J. Tennyson,et al.  The potential energy surface of $H_{2}^{16}O$ , 1996 .

[30]  R. Saykally,et al.  Fully coupled six-dimensional calculations of the water dimer vibration-rotation-tunneling states with a split Wigner pseudo spectral approach , 1997 .

[31]  G. Groenenboom,et al.  Water pair potential of near spectroscopic accuracy. II. Vibration-rotation-tunneling levels of the water dimer , 2000 .

[32]  R. Saykally,et al.  Measurement of quantum tunneling between chiral isomers of the cyclic water trimer. , 1992, Science.

[33]  M. Viant,et al.  A long path length pulsed slit valve appropriate for high temperature operation: Infrared spectroscopy of jet-cooled large water clusters and nucleotide bases , 1996 .

[34]  C. J. Keoshian,et al.  QUANTITATIVE CHARACTERIZATION OF THE WATER TRIMER TORSIONAL MANIFOLD BY TERAHERTZ LASER SPECTROSCOPY AND THEORETICAL ANALYSIS. II. (H2O)3 , 1999 .

[35]  Richard J. Saykally,et al.  Terahertz Laser Spectroscopy of the Water Pentamer: Structure and Hydrogen Bond Rearrangement Dynamics , 1997 .

[36]  O. Matsuoka,et al.  CI study of the water dimer potential surface , 1976 .

[37]  Z. Huang,et al.  Sub‐Doppler resolution infrared spectroscopy of water dimer , 1988 .

[38]  P. Wormer,et al.  Tunneling dynamics, symmetry, and far‐infrared spectrum of the rotating water trimer. I. Hamiltonian and qualitative model , 1996 .

[39]  K. Szalewicz,et al.  Effects of monomer geometry and basis set saturation on computed depth of water dimer potential , 1996 .

[40]  S. Leutwyler,et al.  An ab initio study of the torsional-puckering pseudorotation in the cyclic water pentamer , 1999 .

[41]  M. Kaloudis,et al.  Vibrational spectroscopy of small water complexes embedded in large liquid helium clusters , 1996 .

[42]  Y. Shen,et al.  Infrared predissociation spectra of water dimer in a supersonic molecular beam , 1984 .

[43]  J. Tennyson,et al.  The potential energy surface of H2 16O , 1996 .

[44]  U. Buck,et al.  Structure and Spectra of Three-Dimensional ( H 2 O ) n Clusters, n = 8 , 9 , 10 , 1998 .

[45]  Richard J. Saykally,et al.  THE BIFURCATION REARRANGEMENT IN CYCLIC WATER CLUSTERS : BREAKING AND MAKING HYDROGEN BONDS , 1998 .

[46]  D. Coker,et al.  The infrared predissociation spectra of water clusters , 1985 .

[47]  G. Fleming,et al.  Aqueous solvation dynamics studied by photon echo spectroscopy , 1999 .

[48]  R. Saykally,et al.  The far‐infrared vibration–rotation–tunneling spectrum of the water tetramer‐d8 , 1996 .

[49]  R. Saykally,et al.  Water Clusters , 1996, Science.

[50]  Chandler,et al.  Effect of environment on hydrogen bond dynamics in liquid water. , 1996, Physical review letters.

[51]  E. N. Karyakin,et al.  The 583.2 GHz torsional hot-band of (D2O)3 , 2001 .

[52]  R. Saykally,et al.  Vibrational and K’a dependencies of the multidimensional tunneling dynamics in the 82.6 cm−1 intermolecular vibration of the water dimer‐d4 , 1993 .

[53]  Noam Agmon Tetrahedral Displacement: The Molecular Mechanism behind the Debye Relaxation in Water , 1996 .

[54]  Gregory A. Voth,et al.  The computer simulation of proton transport in water , 1999 .

[55]  R. Saykally,et al.  Fully coupled six-dimensional calculations of the water dimer vibration-rotation-tunneling states with split Wigner pseudospectral approach. II. Improvements and tests of additional potentials , 1999 .

[56]  D. Clary,et al.  Characterization of a cage form of the water hexamer , 1996, Nature.

[57]  Richard J. Saykally,et al.  Terahertz Laser Vibration−Rotation Tunneling Spectroscopy and Dipole Moment of a Cage Form of the Water Hexamer , 1997 .

[58]  H. Schaefer,et al.  Detailed study of the water trimer potential energy surface , 1995 .

[59]  J. Ilja Siepmann,et al.  Development of Polarizable Water Force Fields for Phase Equilibrium Calculations , 2000 .

[60]  J. B. Paul,et al.  Characterization of the (D2O)2 Hydrogen-Bond-Acceptor Antisymmetric Stretch by IR Cavity Ringdown Laser Absorption Spectroscopy , 1998 .

[61]  Michele Parrinello,et al.  Structural, electronic, and bonding properties of liquid water from first principles , 1999 .

[62]  R. Saykally,et al.  Quantifying Hydrogen Bond Cooperativity in Water: VRT Spectroscopy of the Water Tetramer , 1996, Science.

[63]  K. Jordan,et al.  Resonant ion-dip infrared spectroscopy of the S4 and D2d water octamers in benzene-(water)8 and benzene2-(water)8 , 1998 .

[64]  Kai Liu,et al.  Terahertz laser spectroscopy of the water dimer intermolecular vibrations. II. (H2O)2 , 2000 .

[65]  G. Groenenboom,et al.  Water pair potential of near spectroscopic accuracy. I. Analysis of potential surface and virial coefficients , 2000 .

[66]  I. Uchida,et al.  ION- AND ELECTRON-TRANSPORT PROPERTIES OF A SINGLE PARTICLE OF DISORDERED CARBON DURING THE LITHIUM INSERTION REACTION , 1999 .

[67]  Claude Leforestier,et al.  Grid method for the Wigner functions. Application to the van der Waals system Ar–H2O , 1994 .

[68]  D. Wales Theoretical Study of Water Trimer , 1993 .

[69]  Faraday Discuss , 1985 .

[70]  K. Jordan,et al.  Resonant ion-dip infrared spectroscopy of benzene–(water)9: Expanding the cube , 2000 .

[71]  Nauta,et al.  Formation of cyclic water hexamer in liquid helium: the smallest piece of Ice , 2000, Science.

[72]  Sotiris S. Xantheas,et al.  Ab initio studies of cyclic water clusters (H2O)n, n=1–6. II. Analysis of many‐body interactions , 1994 .

[73]  M. Viant,et al.  Quantitative characterization of the (D2O)(3) torsional manifold by terahertz laser spectroscopy and theoretical analysis , 1999 .

[74]  S. Leutwyler,et al.  Rotational constants of all H/D substituted water trimers: Coupling of intermolecular torsional and symmetric stretching modes , 1999 .

[75]  Geoffrey A. Blake,et al.  The Berkeley tunable far infrared laser spectrometers , 1991 .

[76]  K. Jordan,et al.  Infrared Spectrum of a Molecular Ice Cube: The S4 and D2d Water Octamers in Benzene-(Water)8 , 1997 .

[77]  G. T. Fraser (H2O)2: spectroscopy, structure and dynamics , 1991 .

[78]  J. B. Paul,et al.  Infrared cavity ringdown spectroscopy of water clusters: O–D stretching bands , 1998 .

[79]  J. R.,et al.  Chemistry , 1929, Nature.

[80]  Y. Shen,et al.  Vibrational predissociation spectra and dynamics of small molecular clusters of H2O and HF , 1982 .

[81]  Water pair and three-body potential of spectroscopic quality from Ab initio calculations , 2000, Physical review letters.

[82]  F. Keutsch,et al.  Hydrogen bond breaking dynamics of the water trimer in the translational and librational band region of liquid water. , 2001, Journal of the American Chemical Society.

[83]  R. Leighton,et al.  Feynman Lectures on Physics , 1971 .

[84]  Lasse Makkonen,et al.  SURFACE MELTING OF ICE , 1997 .

[85]  Huib J. Bakker,et al.  Femtosecond Mid-IR Pump-Probe Spectroscopy of Liquid Water: Evidence , 1997 .

[86]  J. B. Paul,et al.  Direct Measurement of Water Cluster Concentrations by Infrared Cavity Ringdown Laser Absorption Spectroscopy , 1997 .

[87]  D. Clary,et al.  Tunneling dynamics in water tetramer and pentamer , 1996 .

[88]  J. Rzepiela,et al.  Dynamics of Structural Rearrangements in the Water Trimer , 1994 .

[89]  D. Wales,et al.  Theoretical study of the water tetramer , 1997 .

[90]  Wayne B. Bosma,et al.  Simulation of the intermolecular vibrational spectra of liquid water and water clusters , 1993 .

[91]  S. Woutersen,et al.  Reorientational motion and hydrogen-bond stretching dynamics in liquid water , 2000 .

[92]  Richard Buchner,et al.  Dielectric spectra of some common solvents in the microwave region. Water and lower alcohols , 1990 .

[93]  H. Stanley,et al.  Low frequency depolarized Raman spectra in water: results from normal mode analysis , 1994 .

[94]  D. D. Lucas,et al.  TERAHERTZ LASER VIBRATION-ROTATION-TUNNELING SPECTRUM OF THE WATER PENTAMER-D 10. CONSTRAINTS ON THE BIFURCATION TUNNELING DYNAMICS , 1998 .

[95]  J. Barthel,et al.  The dielectric relaxation of water between 0°C and 35°C , 1999 .

[96]  A. Stone,et al.  Towards an accurate intermolecular potential for water , 1992 .