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The preparations of photochromic dimers of a 2-aryl-4,5-di-phenylimidazyl radical and of a 2,5-diphenyl-3,4-isobenzopyrrole with different substituents in the homocyclic ring are reported. Of the dienes investigated, only 1-4-diphenyl-1,3-butadiene and 2,3-dimethyl-1,3-butadiene gave isolable amounts of the Diels-Adler adducts.
The calculation of the electric dipole polarizability tensor of the He 2 dimer is described, and the results are used in the computation of several dielectric and optical properties of helium gas, at both high (322 K) and low (4 K) temperatures. The properties considered are the second dielectric virial coefficient, the second Kerr virial coefficient, and the depolarization ratio of the integrated intensities for the Raman scattering experiments. The thesis consists of five parts: the polarizability and various properties are defined; the calculation of the polarizability in the long-range region in terms of a quantum mechanical multipole expansion is described; the calculation of the He2 polarizability in the overlap region via coupled Hartree-Fock perturbation theory is described; the calculation of the quantum pair distribution function for both the He-3 and He-4 isotopes at 4 K is discussed; and the calculated values of the properties of helium gas are given.
Results of studies aimed at clarifying the failure of gramicidin A (GA) to sediment in early experiments are analyzed. In the present work, no sedimentation was observed in pure pentanol or ethanol, while normal sedimentation was observed in ethanol-water mixtures. It is concluded that GA exists in two conformations that differ in volume. Since the apparent specific volume in absolute ethanol sinks to its lowest values on increasing concentration, the GA molecule probably unfolds completely in conditions favorable for dimerization.
A simple technique is presented for estimating the energy of formation of monolayer icelike clusters at ice-vapor interfaces. Under the assumptions that the ice surfaces are smooth and sparsely covered with monomers, dimers, etc., in near equilibrium with the vapor, and that the bond energies and configurational entropy dominate the energy of formation, it is found that the basal surfaces prefer triangular embryos with an orientation which reverses from layer to layer, whereas the most stable clusters on the prism surfaces are rectangular in configuration. The preferred prism clusters are determined to have a significantly lower critical energy of formation than the basal clusters due to differences in both corner free energy and configurational entropy. This phenomenon provides a mechanism for strongly anisotropic crystal growth at high saturations.
The parylene coating process developed during this program consists of (1) obtaining a hybrid cover with a hole in it, (2) sealing of the circuit with a hole in the cover, (3) parylene coating through the hole with the external leads protected from parylene by appropriate fixturing, and (4) sealing of the hole by soldering a pretinned kovar tab. Development of the above process required optimization of the parylene coater parameters to obtain a uniform consistent coating which could offer adequate protection to the circuits, fixture design for packages of various types, determination of the size of the deposition hole, and the amount of dimer charge per run, a process to hermetically seal the deposition holes and establishment of quality control techniques or acceptance criteria for the deposited film.
Using a one meter normal incidence grating monochromator, the total absorption of radiation for O2 has been reinvestigated between 2000-2500 A. The absorption cross sections of O2 and O4 are then derived from total absorption measurements and compared with other available data. Additional measurements of O2 absorption have been made in the presence of Ar which does not absorb in this spectral region and is chemically inactive with O2. It is found that the absorption of oxygen increases in the presence of Ar, which is interpreted as due to the formation of O2-Ar dimers.
The extinction coefficient of NO2 has been measured in the spectral range from 185 to 410 nm as a function of temperature between 235 and 298 K. In order to correct for the effect of dimer absorption, the extinction coefficient of N2O4 has also been measured. The effect of a decrease in temperature on NO2 absorption is a reduction in the extinction coefficient of approximately 10% in the range from 320 to 380 nm.
The results of a two-year investigation into the possibility of developing continuous wave excimer lasers are reported. The program included the evaluation and selection of candidate molecular systems and discharge pumping techniques. The K Ar/K2 excimer dimer molecules and the xenon fluoride excimer molecule were selected for study; each used a transverse and capillary discharges pumping technique. Experimental and theoretical studies of each of the two discharge techniques applied to each of the two molecular systems are reported. Discharge stability and fluorine consumption were found to be the principle impediments to extending the XeF excimer laser into the continuous wave regime. Potassium vapor handling problems were the principal difficulty in achieving laser action on the K Ar/K2 system. Of the four molecular systems and pumping techniques explored, the capillary discharge pumped K Ar/K2 system appears to be the most likely candidate for demonstrating continuous wave excimer laser action primarily because of its predicted lower pumping threshold and a demonstrated discharge stability advantage.
Several synthetic routes were studied for the synthesis of the compound 1, 1, 3-trimethyl-1, 3-dicyclohexyl-2 chloropropane. This halogen-labeled fluid would be of use in the study of high traction lubricants under elastohydrodynamic lubrication conditions using infrared emission spectroscopy. The synthetic routes included: dimerization of alpha-methylstyrene, methanol addition to alpha-methylstyrene, a Wittig reaction, and an organometallic approach. Because of steric hindrance and competing reactions, none of these routes were successful.
Three classes of molecular electronic transition lasers produced by hybrid pumping of high pressure rate gas mixtures are discussed. These are (1) rare gas dimer lasers (such as excited Ar2, Kr2, and Xe2) lasing in the VUV, (2) rare gas halide lasers or excimer lasers (such as KrF, ArF, and XeCl excimers) lasing in the UV, and (3) the charge transfer molecular ion laser (such as N2/+/) lasing in the visible range. Laser excitation methods and kinetic sequences are examined for these lasers.
A microwave afterglow mass spectrometer apparatus is used to determine the dependence on electron temperature T sub e of the recombination coefficients alpha sub n of the dimer and trimer ions of the series CO+.(CO) sub n. It is found that alpha sub 1 = (1.3 + or - 0.3)x 0.000001 (T sub e(K)/300) to the -0.34; and alpha sub 2 = (1.9 + or - 0.4)x 0.000001 (T sub e(K)/300) to the -0.33 cu cm/sec. These dependences on T sub e are quite different from those obtained previously for polar-cluster ions of the hydronium and ammonium series but are similar to that for simple diatomic ions.
An attempt is made to measure the sum of the elastic, rotational and vibrational scattering of electrons by KOH at low impact energies (5 to 20 eV) at angles from 10 to 120 deg. Energy loss spectra taken in the 0 to 18 eV range using an electron impact spectrometer are used to identify the species contributing to electric scattering. At temperatures between 300 and 500 C, only inelastic spectral features belonging to water are detected, while at temperatures from 500 to 800 C strong atomic K lines, indicative of molecular dissociation, and H2 energy loss features become prominent. No features attributable to KOH, the KOH dimer, O2 or potassium oxides were observed, due to the effects of the dissociation products, and it is concluded that another technique will have to be developed in order to measure electron scattering by KOH.
The effect of the exchangeable cation on the condensation of glycine and alanine was investigated using a series of homoionic bentonites. A cycling procedure of drying, warming and wetting was employed. Peptide bond formation was observed, and the effectiveness of metal ions to catalyze the condensation was Cu(2+) greater than Ni(2) approximately equals Zn(2+) greater than Na(+). Glycine showed 6% of the monomer incorporated into oligomers with the largest detected being the pentamer. Alanine showed less peptide bond formation (a maximum of 2%) and only the dimer was observed.
Recent experimental laboratory observations, with high-pressure mass spectroscopy, have revealed the existence of previously unreported species involving water clustered to sodium dimer ions, and alkali metal hydroxides clustered to alkali metal ions. The important implications of these results concerning the existence of such species are here discussed, as well as how from a practical aspect they confirm the stability of certain cluster species proposed by Ferguson (1978) to explain masses recently detected at upper altitudes using mass spectrometric techniques.
The vestibulo oculomotor reflex (nystagmus) was recorded by means of electronystagmography in 33 neurosurgical patients in dynamics prior to and after ventriculography. For contrasting the ventricular system a water soluble medium (Conrey, dimer X or Amipak) was used in 18 patients and contrast mixtures of water soluble agents in combination with Myodil emulsion in 15. It was established that after ventriculography with water soluble media the trunk vestibular reactions in all types of nystagmus grew frequently and sharply and the vestibulovegetative reactions increased markedly.
The binders tested were polyurethanes made from two hydroxy-terminated polybutadienes, R-45 and Butarez HT, one hydroxy-terminated butadiene-acrylonitrile copolymer, Hycar 1300X 17, and a hydroxy-terminated prepolymer, Esterdiol 560, made from the dimerized fatty acid Empol 1010. The isocyanates used most extensively were isophorone diisocyanate (IPDI) and a polymeric diisocyanate, DDI. Stress relaxation was used to examine the chemical changes that took place in the binder when subjected to the sterilization temperatures. The thermal stability of the oxidizer, ammonium perchlorate (AP), was tested by thermogravimetry in the isothermal and nonisothermal modes. The effect of particle size, recrystallization, moisture content, and doping on the heat stability of AP could be evaluated by this method. The volatile degradation products, obtained when AP samples were aged at 135 C for prolonged periods, were analyzed by mass spectroscopy.
An improved physical model of dissociative recombination is presented and applied to experimental data on the temperature dependence of rate coefficients for the rare-gas and atmospheric-gas ions. It is shown that in the charge neutralisation of the rare-gas dimer ions, autoionisation plays an important role (at least in comparison with the atmospheric-gas ions) and contributes to the fast fall-off in the rate coefficient with vibrational excitation observed in shock tube studies. Numerical estimates of the observed fall-off in rate coefficient with increasing vibrational excitation are also presented.
The dependence on electron temperature of the coefficients for electron recombination with molecular cluster ions of the carbon monoxide series, CO(+).(CO)n, is determined. A microwave discharge lasting approximately 0.1 msec was applied in 5-20 Torr neon containing a few tenths percent CO in an afterglow mass spectrometer apparatus, and the time histories of the various afterglow ions were measured. Expressions for the dependence of the recombination coefficients of the dimer and trimer ions CO(+).CO and CO(+).(CO)2 are obtained which are found to be significantly different from those previously obtained for hydronium and ammonium series polar cluster ions, but similar to those of simple diatomic ions.