The anisotropic interaction between nitrogen molecules from solid state data

The development of an angle‐dependent interaction potential for slightly nonspherical molecules is outlined, concentrating on molecular nitrogen. The suggested N2–N2 pair potential combines the radial dependence of the Barker type potential used for the rare gases with a modification of the treatment of anisotropy by the Berne–Pechukas Gaussian overlap model. This potential includes quadrupolar and long range dispersion contributions as determined from experiment or semiempirical studies. The valence potential parameters are determined by a fit of beam scattering and solid state measurements. This potential provides satisfactory agreement with Raman and neutron scattering measurements only when the anharmonic contributions to the lattice potential energy are included. A comparison of the suggested potential with a number of other presently available potentials, determined from a variety of measurements, as well as recommendations as to the limits of possible use are made. Possible steps which would lead t...

[1]  R. L. Mills,et al.  Crystal Structures of the Three Modifications of Nitrogen 14 and Nitrogen 15 at High Pressure , 1970 .

[2]  A. B. Harris,et al.  Effect of Anharmonic Libron Interactions on the Single-Libron Spectrum of Solid H 2 and D 2 , 1971 .

[3]  R. L. Roy,et al.  Anisotropic intermolecular potentials from an analysis of spectra of H2‐ and D2‐inert gas complexes , 1974 .

[4]  R. L. Mills,et al.  alpha-gamma Transition in Solid Nitrogen and Carbon Monoxide at High Pressure , 1971 .

[5]  C. Swenson.  New Modification of Solid Nitrogen , 1955 .

[6]  M. Henkelman,et al.  Librational Motion in the α Phase of Solid N2 and CO , 1971 .

[7]  E. J. Allin,et al.  Low Frequency Raman Spectra of α-16O2, α-18O2, and α-N2 , 1971 .

[8]  J. Pople,et al.  Intermolecular vibrations of solid carbon dioxide , 1964 .

[9]  E. A. Mason,et al.  SCATTERING OF HIGH VELOCITY NEUTRAL PARTICLES. X.HE-N2;A-N2 , 1957 .

[10]  B. Quentrec,et al.  Angular correlations and rotational motion in computer-simulated liquid nitrogen , 1975 .

[11]  O. Schnepp,et al.  Empirical intermolecular potentials for N2 and CO2 from crystal data , 1973 .

[12]  R. L. Mills,et al.  Sound velocity and the equation of state of N2 to 22 kbar , 1975 .

[13]  L. Slutsky,et al.  Model for the lattice vibrations of a crystal of diatomic molecules—I. Frequency distributions, Debye-Waller factors, and infrared spectra* , 1972 .

[14]  M. Klein,et al.  Rare gas solids , 1976 .

[15]  J. Ely,et al.  The statistical mechanics of non-spherical polyatomic molecules , 1975 .

[16]  E. D. Adams,et al.  Thermal expansion and isothermal compressibility of solid nitrogen , 1970 .

[17]  A. Mckellar,et al.  Spectra of (H2)2, (D2)2, and H2–D2 Van der Waals Complexes , 1974 .

[18]  D. Wallace,et al.  Thermodynamics of Crystals , 1972 .

[19]  J. Raich.  k=0 Librational Spectrum for Solid α‐N2 , 1972 .

[20]  Bruce J. Berne,et al.  Intermolecular potential models for anisotropic molecules, with applications to N2, CO2, and benzene , 1976 .

[21]  P. W. Langhoff,et al.  Padé Approximants for Two‐ and Three‐Body Dipole Dispersion Interactions , 1970 .

[22]  M. Mandell.  Computer study of a classical quadrupole solid , 1974 .

[23]  J. G. Powles,et al.  The properties of liquid nitrogen , 1976 .

[24]  G. Maitland,et al.  Critical reassessment of viscosities of 11 common gases , 1972 .

[25]  Michael L. Klein,et al.  Thermodynamic properties for a simple model of solid carbon dioxide: Monte Carlo, cell model, and quasiharmonic calculations , 1974 .

[26]  W. England,et al.  Properties of solid and gaseous hydrogen, based upon anisotropic pair interactions , 1975 .

[27]  T. Kihara.  Virial Coefficients and Models of Molecules in Gases , 1953 .

[28]  J. A. Barker,et al.  Lattice Dynamics with Three-Body Forces: Argon , 1970 .

[29]  A. Bondi,et al.  Physical properties of molecular crystals liquids, and glasses , 1968 .

[30]  A. Zunger,et al.  Calculation of structural properties and vibrational frequencies of α‐ and γ‐N2 crystals , 1975 .

[31]  J. Kjems,et al.  Crystal dynamics of nitrogen: the cubic. cap alpha. -phase , 1975 .

[32]  Edward A. Mason,et al.  Interactions between Ground‐State Nitrogen Atoms and Molecules. The N–N, N–N2, and N2–N2 Interactions , 1959 .

[33]  M. Mandell.  On the intermolecular potential in solid N2. II. Libronic frequencies , 1975 .

[34]  Bruce J. Berne,et al.  Gaussian Model Potentials for Molecular Interactions , 1972 .

[35]  T. Kihara,et al.  Intermolecular forces for D2, N2, O2, F2 and CO2 , 1974 .

[36]  J. Barker,et al.  Atomic interactions in argon , 1968 .

[37]  M. Thiéry,et al.  Raman spectra of solid α‐N2 and γ‐N2 under high pressure at 4.2 K , 1973 .

[38]  G. Ewing,et al.  The infrared spectrum of the (N2)2 van der waals molecule , 1973 .

[39]  V. B. Leonas,et al.  The short-range interaction of molecules: the experimental investigation of potential energy surfaces , 1971 .

[40]  J. Barojas,et al.  Simulation of Diatomic Homonuclear Liquids , 1973 .

[41]  M. Krauss,et al.  Quadrupole moment of CO, N2, and NO+ , 1974 .

[42]  W. Giauque,et al.  The Heat Capacity and Entropy of Nitrogen. Heat of Vaporization. Vapor Pressures of Solid and Liquid. The Reaction 1/2 N2 + 1/2 O2 = NO from Spectroscopic Data , 1933 .

[43]  O. Schnepp,et al.  Quantum Lattice Dynamics of Molecular Solids. II. Application to the Librations of Solid CO2, α‐N2, and o‐H2 , 1972 .

[44]  C. F. Curtiss,et al.  Molecular Theory Of Gases And Liquids , 1954 .

[45]  Saburo Koba.  Convex-Core Model of Molecules in Crystalline State. II , 1959 .

[46]  G. Pawley,et al.  On the lattice dynamics of solid nitrogen , 1974 .

[47]  M. Donkersloot,et al.  An empirical intermolecular potential function for solid carbon dioxide , 1971 .

[48]  W. B. Daniels,et al.  Raman spectrum of solid nitrogen at high pressures and low temperatures , 1976 .

[49]  J. G. Powles,et al.  The intermolecular potential for nitrogen , 1976 .

[50]  A. C. Wahl,et al.  Electronic Structure of Diatomic Molecules. III. A. Hartree—Fock Wavefunctions and Energy Quantities for N2(X1Σg+) and N2+(X2Σg+, A2Πu, B2Σu+) Molecular Ions , 1966 .

[51]  R. K. Crawford,et al.  Isochoric measurement of the equation of state of solid argon at high pressure , 1974 .

[52]  V. Popov,et al.  Thermal Capacity of Solid Nitrogen , 1968, April 1.

[53]  B. C. Kohin.  Molecular Rotation in Crystals of N2 and CO , 1960 .

[54]  N. S. Gillis,et al.  Self‐consistent calculation of the phonon‐libron spectrum in α‐N2 , 1974 .

[55]  V. H. Smith,et al.  Molecular interactions in nitrogen and oxygen , 1975 .

[56]  A. B. Harris,et al.  Librational anharmonicity in solid α-N2 , 1972 .

[57]  J. Raich,et al.  The anisotropic interaction between hydrogen molecules , 1976 .

[58]  A. Warshel,et al.  Intermolecular Potentials for N2 Molecules and the Lattice Vibrations of Solid α‐N2 , 1970 .

[59]  Linear Spin‐Wave Theory of Librational Motion in the α Phase of N2 and CO , 1972 .

[60]  A. Anderson,et al.  Raman spectra and lattice dynamics of the α phases of nitrogen and carbon monoxide crystals , 1970 .

[61]  R. D. Murphy,et al.  Elastic Constants of Solid Ar, Kr, and Xe: A Monte Carlo Study , 1972 .

[62]  B. Quentrec.  Simulation of solid a-nitrogen , 1975 .

[63]  R. Kiehn,et al.  Neutron Inelastic Scattering , 1954 .

[64]  A. Buckingham,et al.  Quadrupole moments of some simple molecules , 1968 .

[65]  W. B. Daniels,et al.  Raman spectrum of γ‐N2 , 1973 .

[66]  M. Thiéry,et al.  Intermolecular potential energy functions and Gruneisen Parameters of simple molecular crystals , 1974 .