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15 Dec 1974

Volume 61, Issue 12, pp. 4939-5478

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Dynamics of stiff polymer chains. I

M. Fixman and J. Kovac

J. Chem. Phys. 61, 4939 (1974); http://dx.doi.org/10.1063/1.1681833 (11 pages) | Cited 66 times

Online Publication Date: 22 August 2003

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The nonlinear configurational diffusion equation is formulated with bond vector coordinates. Primarily the treatment focuses on low amplitude oscillatory shear flow of the freely jointed chain, but the high frequency limit is formulated also with the constraint of constant bond angles, and is calculable fairly readily for a freely rotating chain or rotational isomeric model. The only numerical result given here concerns the high frequency limit [η]N∞ of freely jointed chains of N bonds. We find by perturbation theory that [η]N∞ ≃ [η]1∞N[1+(N−1)/(6N)+⋯] (for the concentration measured in molecules∕cubic centimeter; in conventional units of grams∕cubic centimeter, [η]N∞ is asymptotically independent of N). In the lowest approximation the relaxing part of the intrinsic viscosity is given by equations quantitatively close to those of Zimm for the Gaussian model.

Dynamics of stiff chains. II. Freely jointed chain

M. Fixman and J. Kovac

J. Chem. Phys. 61, 4950 (1974); http://dx.doi.org/10.1063/1.1681834 (5 pages) | Cited 21 times

Online Publication Date: 22 August 2003

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The equations developed in the preceding paper are applied here to the freely jointed chain. The complex modulus G agrees quite well with Zimm's results for the Gaussian model at low frequencies, even for chains of 5 or 10 bonds, but major differences appear at high frequencies for the imaginary part G″ as a result of the nonvanishing high frequency viscosity of a freely jointed chain.

Energy distributions of field emitted electrons from tungsten in the presence of adsorbed CO

Peter L. Young and Robert Gomer

J. Chem. Phys. 61, 4955 (1974); http://dx.doi.org/10.1063/1.1681835 (18 pages) | Cited 29 times

Online Publication Date: 22 August 2003

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Energy distributions were measured on the (110), (100), (111), and (210) planes under various conditions of CO adsorption. Resonances were seen for the low temperature layer at −7 to 7.5 eV below vacuum on all planes except (100). A comparison of the widths and maximum amplitudes of the resonances shows good agreement with the theory of field emission from adsorbate covered surfaces. On heating, the resonances disappeared at ≤350 K corresponding to conversion of the low temperature states to beta‐precursor states. Readsorption on beta or beta‐precursor layers led to resonances at −7 eV on (210) and (111), but not on (110) or (100). The resonances are interpreted as arising from interaction of CO☒π* orbitals with tungsten d‐t2g orbitals in adsorption via the C atom on single W atoms. Disappearance of the resonances on heating is interpreted as activated rearrangement to new bonding configurations‐for instance, bridge bonding via C‐sp2 orbitals. The intensity of the resonances increases initially with coverage but, on all planes except (210), goes through a maximum and vanishes for θ<1. This is interpreted as interference of neighboring CO molecules, resulting in the squeezing out of charge from the labile‐π orbitals responsible for the resonance. The details of intensity vs θ curves on different planes support this model. On the (100) plane, a resonance at −6.9 eV appeared at 600 K and is attributed to W☒O bonding. A comparison of the temperature behavior of this resonance for O and CO covered emitters leads to the conclusion that CO on the (100) plane is rearranged but not dissociated up to at leat 820 K.

Molecular dynamics study of liquid water under high compression

Frank H. Stillinger and Aneesur Rahman

J. Chem. Phys. 61, 4973 (1974); http://dx.doi.org/10.1063/1.1681836 (8 pages) | Cited 95 times

Online Publication Date: 22 August 2003

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The technique of computer simulation by molecular dynamics has been used to investigate highly compressed water at mass density 1.346 g∕cm3. The calculations involve 216 rigid molecules, subject to an additive interaction (the ``ST2 potential'') whose strong anisotropic character has been shown to describe the hydrogen bond phenomenon. In the light of previous calculations on the same model at ordinary pressures, substantial restructuring of the liquid in response to compression is obvious. No evidence arises to support description of the liquid in terms of crystal structures of ices VI and VII, the solid forms that might be expected to be relevant at the chosen density. The calculations indicate that the initial effect of pressure increase (at 1 atm) leads to increased fluidity, as is known to be the case for real water.

Nuclear magnetic resonance in antiferromagnetic α‐RbMnCl3⋅2H2O

W. J. M. de Jonge and C. H. W. Swüste

J. Chem. Phys. 61, 4981 (1974); http://dx.doi.org/10.1063/1.1681837 (4 pages) | Cited 1 time

Online Publication Date: 22 August 2003

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α‐RbMnCl3⋅2H2O is found to order antiferromagnetically at TN = 4.560±0.005 K. The magnetic array can be described by P2bc′ca′. The chains are antiferromagnetic. Values for the electric quadrupole coupling and the magnetic interaction parameters are reported for the Rb as well as for the Cl nucleus. The interpretation of the proton spectra gives rise to the assumption of a rather large spin reduction which agrees with the presumed one‐dimensional character of these compounds.

Cluster expansions for hydrogen bonded fluids. II. Dense liquids

Hans C. Andersen

J. Chem. Phys. 61, 4985 (1974); http://dx.doi.org/10.1063/1.1681838 (8 pages) | Cited 34 times

Online Publication Date: 22 August 2003

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The cluster expansion theory of Mayer is formulated in a way that makes it useful for application to dense hydrogen bonded fluids, or, in general, to fluids with very strong attractive intermolecular potentials that are very dependent upon the relative orientations of the molecules. In the resulting diagrammatic series, the hydrogen bond appears only in a renormalized form that is much weaker than the Mayer f function for the original unrenormalized hydrogen bond potential. The diagram series for the pair correlation function is divided into various parts according to the topological structure and physical interpretation of the diagrams, and exact relationships among these parts are derived. These exact relationships can become the starting point for approximate calculations of the pair correlation function for hydrogen bonded liquids such as water.

Absorption spectra of NpCl3 and NpBr3

W. T. Carnall, H. M. Crosswhite, R. G. Pappalardo, D. Cohen, S. Fried, P. Lucas, and F. Wagner

J. Chem. Phys. 61, 4993 (1974); http://dx.doi.org/10.1063/1.1681839 (16 pages) | Cited 9 times

Online Publication Date: 22 August 2003

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Low temperature absorption spectra are reported for NpCl3 and NpBr3 in the range 3300–40 000 cm−1. Term assignments are made to a number of excited levels not previously identified, and the data are interpreted in terms of a refined free‐ion model. Some of the parameters associated with this model are found to have similar values for both 3+ actinide and lanthanide chlorides. The values determined for other of the parameters are in good agreement with those calculated independently using Hartree‐Fock methods. The similar crystal‐field quantum number ordering of levels in the ground states of actinide trichlorides and analogous lanthanides doped into LaCl3 is noted and discussed.

Potential model of dye molecule from measurements of the photocurrent in monolayer assemblies

U. Schoeler, K. H. Tews, and H. Kuhn

J. Chem. Phys. 61, 5009 (1974); http://dx.doi.org/10.1063/1.1681840 (8 pages) | Cited 32 times

Online Publication Date: 22 August 2003

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A semitransparent Al layer is coated with several arachidate layers, one monolayer of quinquethienyl (mixed with arachidate), and some layers of arachidate; the arrangement is contacted with mercury. A bias voltage is applied and the photocurrent is measured as a function of the applied voltage and the temperature for different positions of the dye within the layer assembly. The photocurrent depends on the detailed assemblage, demonstrating the possibility of constructing photoelectric devices based on a planned molecular architecture. The results are in agreement with a simple theoretical model. A reasonably detailed description is obtained for the shape of the potential profile of the excited π electron of the dye responsible for the photocurrent.

Properties of binary tin chalcogenides determined by Mossbauer spectroscopy

Vincenzo Fano and Ida Ortalli

J. Chem. Phys. 61, 5017 (1974); http://dx.doi.org/10.1063/1.1681841 (5 pages) | Cited 20 times

Online Publication Date: 22 August 2003

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The parameters of the resonance absorption of the 23.8 keV γ quanta emitted by 119+Sn were measured in the temperature range of 78 to 300°K for the chalcogenides of tin: SnS, SnSe, and SnTe. Measurements of the width at half‐height, quadrupole interactions, and chemical isomer shifts are used to analyze the properties of the chemical bonds and the structures of the investigated compounds. The temperature dependence of the probability of resonance absorption fa is correlated with the phonon spectrum of these semiconductors. The behavior of the fa and Γexp values and the appearance of an electric field gradient in SnTe at low temperature suggest the existence of a phase transition at about 160°K.

Photodissociation quantum yields of CO2 between 1200 and 1500 Å

Tom G. Slanger, Robert L. Sharpless, Graham Black, and Stephen V. Filseth

J. Chem. Phys. 61, 5022 (1974); http://dx.doi.org/10.1063/1.1681842 (6 pages) | Cited 12 times

Online Publication Date: 22 August 2003

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Measurements of the photodissociation quantum yields of CO2 have been carried out using various atomic line sources between 1200 and 1500 Å. The production of CO was monitored by resonance fluorescence, and the results indicate that where the CO2 absorption spectrum is continuous, the CO quantum yield is high, but where there is structure, the yield is low. At the commonly employed 1236 Å resonance line, the CO quantum yield is 0.85±0.17, relative to the absolute value at 1470 Å of 0.75 obtained by Inn. On the same scale, the other values are (a) 1216 Å, 0.57 ±0.11, (b) 1302–1306 Å, 0.21±0.07, (c) ∼1390 Å, 0.46±0.05, (d) 1492–1495 Å, 0.58±0.06. The CO2 pressures employed were in the range 0.4–4.0 Torr. If these same quantum yields are valid at the pressures of the Mars and Venus atmospheres, the CO and O atom production rates are less than presently assumed.

Infrared spectra and anharmonic force field of NCO− in CsCl, CsBr, and Csl

D. Foss Smith and Robert J. York

J. Chem. Phys. 61, 5028 (1974); http://dx.doi.org/10.1063/1.1681843 (4 pages) | Cited 5 times

Online Publication Date: 22 August 2003

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The infrared spectra of NCO− isolated in CsCl, CsBr, and CsI have been obtained using the alkali halide pressed disk technique. Samples enriched with both 13C and 15N were prepared. The anharmonic force field of NCO− has been determined in each lattice using a simplified quartic force field. The anharmonicity constants, Xij, the anharmonic force constants, and the quadratic stretch‐stretch interaction force constant have been determined to be essentially independent of the matrix.

Nuclear quadrupole coupling in the hydrogen molecule: A molecular orbital description

Lawrence C. Snyder

J. Chem. Phys. 61, 5032 (1974); http://dx.doi.org/10.1063/1.1681844 (3 pages) | Cited 7 times

Online Publication Date: 22 August 2003

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The electric field gradient at a nucleus of H2 has been computed from an SCF determinantal wavefunction in a Gaussian orbital basis set centered at the nuclei. It is found that both p and d polarization functions must be added if the true electric field gradient is to be represented within a few percent.

Abstraction fraction in the reaction of deuterium atoms with HBr and HI

Avigdor Persky and Aron Kuppermann

J. Chem. Phys. 61, 5035 (1974); http://dx.doi.org/10.1063/1.1681845 (5 pages) | Cited 11 times

Online Publication Date: 22 August 2003

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The reaction between D atoms and HX molecules (X=Br or I) may result in either abstraction of H atoms to yield HD+X or exchange of H atoms to yield DX+H. This reaction was studied at 300°K by photolyzing HX+DX+He mixtures with monochromatic light at two wavelengths. It was found that the abstraction fraction is 0.76±0.10 for X=Br and 0.88±0.08 for X=I. These results are discussed in terms of the dynamics of these reactions.

Anharmonic force field of ethylene

Katsunosuke Machida and Yumiko Tanaka

J. Chem. Phys. 61, 5040 (1974); http://dx.doi.org/10.1063/1.1681846 (10 pages) | Cited 14 times

Online Publication Date: 22 August 2003

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A simple anharmonic force field of ethylene is proposed. It includes the principal cubic and quartic stretching constants derived from appropriate Morse functions for individual bonds and two other higher‐order constants. The quadratic part consists of general valence type constants that show the characteristics of the Pulay‐Meyer Set II force field. The perturbation method including a general treatment of the first‐ and the second‐order resonances has been used, and about 190 vibrational frequencies of ethylene and six deuterated ethylenes have been calculated to agree fairly well with the experimental values. The proposed potential gives also reasonable values of the Coriolis coupling constants, the centrifugal distortion constants, and the 13C‐isotope shifts. The signs of the compliance constants are consistent with the assumption of monotone changes of internal coordinates on the dehydrogenation into acetylene and on the dissociation into two methylene radicals.

Formulation of molecular forces and their analytical calculation

Shalom Srebrenik, Harel Weinstein, and Ruben Pauncz

J. Chem. Phys. 61, 5050 (1974); http://dx.doi.org/10.1063/1.1681847 (4 pages) | Cited 5 times

Online Publication Date: 22 August 2003

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A general definition of forces in a molecular system is considered, with the Hellmann‐Feynmann relation representing the special case for the Born‐Oppenheimer approximation. Analytic formulas are given for the calculation of forces within the fixed nuclei approximation. Derived from the analytic formulation of electrostatic potential, this calculation procedure remains valid for other average values of the form 〈r−∣n∣〉.

Magnetic parameters of p2,4, dt22,4, and d2 configurations in axial symmetric crystal fields

Ad Lagendijk

J. Chem. Phys. 61, 5054 (1974); http://dx.doi.org/10.1063/1.1681848 (6 pages)

Online Publication Date: 22 August 2003

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The energies and wavefunctions of a p2,4 configuration under the influence of a crystal field possessing axial symmetry are calculated. If the crystal field parameter Δ is smaller than, or of the order of, the Slater‐Condon parameter F2, the 3P wavefunctions have the lowest energies. In that case one finds, depending on the sign of Δ, that either an orbital doublet or an orbital singlet has the lowest energy. For the latter, the fine structure parameters, the g values, and the hyperfine parameters are calculated. Using an irreducible tensor formalism, it is shown that the results for p2,4 can be used to find the interactions within dt22,4. Tetragonal as well as trigonal symmetry are treated and it is found that the hyperfine interactions differ substantially for both cases. Finally, the interactions within 3F(d2) under the influence of a crystal field possessing tetragonal symmetry are treated.

Model for H+2(v = 0)☒He collisions above 2 eV

G. R. North, H. H. Harris, J. J. Leventhal, and P. B. James

J. Chem. Phys. 61, 5060 (1974); http://dx.doi.org/10.1063/1.1681849 (6 pages) | Cited 5 times

Online Publication Date: 22 August 2003

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A classical model with no adjustable parameters employing Lennard‐Jones type potentials is used to describe collision processes between H2+(ν = 0) ions and He atoms at relative energies above 2 eV. The assumptions that justify such an approach are discussed as well as the possibility of additional simplifications. Model predictions for collision‐induced dissociation and reactive scattering cross sections compare favorably with data from four laboratories. Predicted angular distributions of product HeH+ and H2+ as well as vibrational and rotational energy partitioning for these products are also reported.

Uncoupled Hartree‐Fock perturbation theory and the Pople‐Schofield approximation

A. T. Amos and R. J. Crispin

J. Chem. Phys. 61, 5066 (1974); http://dx.doi.org/10.1063/1.1681850 (6 pages) | Cited 4 times

Online Publication Date: 22 August 2003

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The first‐order perturbation equation in UCPT is derived in a form which reflects the essential lack of uniqueness of the perturbed orbital. The functionals leading to this equation and the other forms of the first‐order equation are compared and this functional found to be best, although equivalent to the others if additional conditions are applied to their variation. The Pople‐Schofield approximation, which is frequently applied to simplify the computation of the variational functional, is examined and found to be exact in the sense that H0 can be constructed to make it so. A simpler way of regarding the Pople‐Schofield approximation is presented using a method due to Hirschfelder and originally designed to deal with exchange forces.

Microwave spectrum, quadrupole coupling, and barrier to internal rotation of 1‐chloro‐1‐fluoroethane

Clarence H. Thomas, Kenneth D. Nisbet, and Georges Graner

J. Chem. Phys. 61, 5072 (1974); http://dx.doi.org/10.1063/1.1681851 (4 pages) | Cited 4 times

Online Publication Date: 22 August 2003

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The microwave spectra of the ground state of the 35Cl and 37Cl isotopic species of 1‐chloro‐1‐fluoroethane have been investigated in the K‐band region. An analysis of the 35Cl quadrupole splittings shows that the χ tensor is asymmetric, presumably owing to the partial double bond character of the C☒C1 bond. A satellite spectrum of the 35Cl isotope has been assigned to the first excited state of the torsion. The relative intensity of the satellite spectrum leads to a value of the barrier hindering internal torsion of 4300±300 cal∕mole.

Vibration‐rotation inelasticity in He☒H2

Herschel Rabitz and George Zarur

J. Chem. Phys. 61, 5076 (1974); http://dx.doi.org/10.1063/1.1681852 (9 pages) | Cited 70 times

Online Publication Date: 22 August 2003

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Vibration‐rotation inelasticity in He☒H2 is studied up to total energy 1.5 eV. This extends the previous lower energy pure rotational studies with the effective potential method. Comparison is made with breathing sphere calculations, and the corresponding vibration‐rotation differential and total cross sections are similar. However, it is shown that there are many other nonbreathing sphere type vibration‐rotation cross sections of comparable magnitude. The competitive roles of coupling and energetic resonance effects are quite apparent in the cross sections. The differential and total cross sections are examined for general characteristic behavior. An analysis is presented of the energy dependence of the cross sections. Finally, comments on general effective Hamiltonian methods are included.

Inelastic scattering in atom‐diatomic molecule collisions. I Rotational transitions in the sudden approximation

James R. Stallcop

J. Chem. Phys. 61, 5085 (1974); http://dx.doi.org/10.1063/1.1681853 (13 pages) | Cited 13 times

Online Publication Date: 22 August 2003

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The impact parameter method and the sudden approximation are applied to determine the total probability of inelastic rotational transitions arising from a collision of an atom and a homonuclear diatomic molecule at large impact parameters. An analytical approximation to this probability is found for conditions where the electron exchange or overlap forces dominate the scattering. An approximate upper bound to the range of impact parameters for which rotational scattering can be important is determined. In addition, an estimate of the total inelastic cross section is found at conditions for which a statistical model describes the scattering well. The results of this analysis are applied to Ar☒O2 collisions and may be readily applied to other combinations of atoms and molecules.

Effect of pressure on 14N nuclear quadrupole relaxation in hexamethylenetetramine

Avigdor Zussman and Eliezer Rapoport

J. Chem. Phys. 61, 5098 (1974); http://dx.doi.org/10.1063/1.1681854 (4 pages) | Cited 7 times

Online Publication Date: 22 August 2003

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14N nuclear quadrupole resonance frequencies and spin‐lattice relaxation time, T1, in hexamethylenetetramine (HMT) were measured as a function of hydrostatic pressure up to 6 katm at 257, 273, 294.5, 309, and 317°K. For the three higher isotherms T1 depends exponentially on pressure up to 3 katm. In this region T1 is determined mainly by molecular reorientation of the tetrahedral HMT molecule around its four threefold axes. This mechanism is discussed in terms of a simple activation process. The activation volume, ΔV*=23.6±1 cm3∕mole, and activation enthalpy, ΔH*=17±1 kcal∕mole were determined. From thermal expansion and compressibility data, the thermal pressure, Pt = T(∂p∕∂T)v, of 6.2 katm and activation energy ΔE* = 12–15 kcal∕mole were deduced. These values of ΔH*, ΔE*, and ΔV* are higher than the corresponding values reported by Anderson and Slichter for three other organic solids and might indicate the effect of the large number of hydrogen bonds in HMT.

Nonequilibrium force fluctuations in an isotopically impure linear harmonic crystal

William L. Greer

J. Chem. Phys. 61, 5102 (1974); http://dx.doi.org/10.1063/1.1681855 (12 pages)

Online Publication Date: 22 August 2003

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A linear, harmonic, isotopically impure crystal is placed into contact with two harmonic oscillator heat baths, each at a different temperature. Force fluctuations on the ends of the crystal are studied in the nonequilibrium steady state that results from the ultimate evolution of the coupled crystal‐heat baths. The exact behavior of steady state force fluctuations is obtained in general and examined in detail for periodic or randomly disordered isotopic lattices. Numerical results for the periodic crystal reveal unexpected complexity in the temporal decay of the force autocorrelation function. From exact expressions for the entire force distribution functions we show that, in general, the distribution is Gaussian and non‐Markovian. However, on a coarse grained, semimicroscopic time scale (∼10−12 sec), the Gaussian force distribution is purely random and in accord with the usual assumptions about heat baths. One case of a macroscopic decay time occurs when one bath is initially at T =0°K in contact with a randomly disordered lattice.

Atomization energies and heats of formation of gaseous Au2, Tb2, TbAu, HoAu, TbAu2, and HoAu2

J. Kordis, K. A. Gingerich, and R. J. Seyse

J. Chem. Phys. 61, 5114 (1974); http://dx.doi.org/10.1063/1.1681856 (8 pages) | Cited 46 times

Online Publication Date: 22 August 2003

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By means of Knudsen effusion mass spectrometric studies the atomization energies, D°0(kcal mol−1), and standard heats of formation, ΔH°f,298(kcal mol−1), respectively, were obtained for the following: Au2(52.9±0.5, 122.0±1.0), Tb2(30.5±6.0, 155.2±7.0), TbAu(69.2±8.0, 110.5±10), HoAu(63.0±8.0, 96.0±8.7), TbAu2(139.1±10, 128.0±11) and HoAu2(127.3±10, 100.6±10). These data were deduced from a critical assessment of the enthalpy changes of the reactions M2(g)=2M(g) and M(s,1)+M(g)=M2(g) for gold and terbium, and of the reactions LnAu(g)=Ln(g) + Au(g), LnAu(g)+Au(g)=Ln(g)+Au2(g), LnAu2(g)=Ln(g)+2Au(g) and LnAu2(g)+2Au(g)=Ln(g)+2Au2(g) for terbium and holmium. The cited standard heats of formation incorporate appropriate literature data as well as the measured reaction enthalpies. The Pauling model of a polar bond has been used for the interpretation of the measured atomization energies of the Ln☒Au molecules and for predicting the dissociation energies of selected intermetallic compounds of terbium.

The collinear Cl + XY system (X,Y=H,D,T). A comparison between quantum mechanical, classical, and transition state theory results

Michael Baer, Uriel Halavee, and Avigdor Persky

J. Chem. Phys. 61, 5122 (1974); http://dx.doi.org/10.1063/1.1681857 (10 pages) | Cited 29 times

Online Publication Date: 22 August 2003

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In this work, exact quantum mechanical (QM) and classical (CL) transition probabilities for the Cl+XY (X,Y=H,D,T) collinear system are compared. The calculations were performed using a semiempirical LEPS surface. The main features discussed are tunneling and threshold behavior for both the ground state and the first excited state of the hydrogen molecule. In the second part, kinetic isotope effects are presented and discussed. Those were calculated in three different ways, using (i) QM transition probabilities, (ii) CL transition probabilities, and (iii) transition state theory (TST‐1D). Tunneling coefficients kQM∕kCL and kQM∕kTST were calculated and discussed. Finally, a brief comparison with experimental data was performed.
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