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Molecular beam kinetics

Description: The design of a crossed molecular beam ''supermachine'' for neutral-- neutral collisions is discussed. The universal electron bombardment ionizer, mass filter, and ion detection system of the detector, the supersonic nozzle sources, the differential pumping arrangement for the sources and detector, the time-of-flight detection of scattered products, and the overall configuration of the apparatus are described. The elastic scattering of two systems, CH$sub 4$ + Ar and NH$sub 3$ + Ar, has been measured using the supermachine with two supersonic nozzle sources. The rainbow structure and the interference oscillations are seen in each system. The best fit to the data was found using a Morse--Spline--Van der Waals (MSV) potential. The three potential parameters epsilon, r/sub m/, and $beta$ were found to be 2.20(+-0.04) x 10$sup -14$ ergs, 3.82(+-0.04)A, and 7.05 +- 0.20 for CH$sub 4$ + Ar, and 2.21(+-0.04) x 10$sup - 14$ ergs 3.93 (+-0.05)A, and 8.45 +- 0.30 for NH$sub 3$ + Ar. A new phenomenon in crossed molecular beams of condensation of a molecule on a cluster to form a complex was observed. A bromine molecule condensed on clusters of chlorine (Cl$sub 2$)/sub chi/ and ammonia (NH$sub 3$)/sub chi/. The value of chi for measurements in these experiments ranges from 7 to 40 for chlorine clusters and from 10 to 70 ammonia clusters. (auth)
Date: November 1, 1975
Creator: Behrens, R. Jr.
Partner: UNT Libraries Government Documents Department

Thermal decomposition of energetic materials by STMBMS measurements: Application of Simultaneous Thermogravimetric Modulated Beam Mass Spectrometry (STMBMS) to the study of energetic materials

Description: Simultaneous thermogravimetric modulated beam mass spectrometry (STMBMS) and time-of-flight velocity (TOF) spectra have been developed to study reactions that occur during the thermal decomposition of liquids and solids. The data obtained with these techniques are the identity of the reaction products and their rates of gas formation as a function of time. Over the past several years, these techniques have been applied to the study of energetic materials that are used in propellants and explosives. In this presentation, the details of the STMBMS and TOF velocity spectra techniques will be reviewed, the advantages of the techniques over more conventional thermal analysis and mass spectrometry measurements will be discussed, and the use of the techniques will be illustrated with results on the thermal decomposition of hexahydro-1,3,5-trinitro-s-triazine (RDX).
Date: August 1, 1995
Creator: Behrens, R. Jr.
Partner: UNT Libraries Government Documents Department

Thermal decomposition studies of 1,3,3-trinitroazetidine (TNAZ) and 1-nitroso-3,3-dinitroazetidine (NDNAZ) by simultaneous thermogravimetric modulated beam mass spectroscopy

Description: The initial results from a study of the thermal decomposition of TNAZ, TNAZ-1-{sup 15}NO{sub 2} and NDNAZ using the simultaneous thermogravimetric modulated beam mass spectrometer (STMBMS) are presented. The major products formed in the decomposition of TNAZ are NO{sub 2} and NO with slightly lesser amounts of H{sub 2}O, HCN, CO/N{sub 2}, CO{sub 2}/N{sub 2}O and NDNAZ. The major product formed in the decomposition of NDNAZ is NO with lesser amounts of H{sub 2}O, HCN, CO/N{sub 2}O. The lower molecular weight products are similar to those observed in RSFTIR and IRMPD studies conducted previously by others. However, this study has shown that the mononitroso analogue of TNAZ, NDNAZ, is an important intermediate formed during the decomposition of TNAZ. It plays an important role in determining the identity of the products formed in the decomposition of TNAZ. The temporal behaviors Of the ion signals associated with the various thermal decomposition products from TNAZ, TNAZ-1-{sup 15}NO{sub 2} and NDNAZ are also presented. The illustrate the evolution sequence of the various products that are associated with the different reaction pathways that control the decomposition of these materials. In particular, the study of the {sup 15}N-labeled sample revealed that NO{sub 2} originates from both the likely sites in the TNAZ molecule and that the cleavage of the nitramine-NO{sub 2} group precedes that of the C-NO{sub 2} cleavage, resulting in similar sequences in the formation of NO and NDNAZ also.
Date: December 1, 1995
Creator: Behrens, R., Jr. & Bulusu, S.
Partner: UNT Libraries Government Documents Department

Solid-phase thermal decomposition of 2,4-dinitroimidazole (2,4-DNI)

Description: The solid-phase thermal decomposition of the insensitive energetic nitroaromatic heterocycle 2,4-dinitroimidazole (2,4-DNI: mp 265--274C) is studied utilizing simultaneous thermogravimetric modulated beam mass spectrometry (STMBMS) between 200 and 247C. The pyrolysis products have been identified using perdeuterated and {sup 15}N-labeled isotopomers. The products consist of low molecular-weight gases and a thermally stable solid residue. The major gaseous products are NO, CO{sub 2}, CO, N{sub 2}, HNCO and H{sub 2}O. Minor gaseous products are HCN, C{sub 2}N{sub 2}, NO{sub 2}, C{sub 3}H{sub 4}N{sub 2}, C{sub 3}H{sub 3}N{sub 3}O and NH{sub 3}. The elemental formula of the residue is C{sub 2}HN{sub 2}O and FTIR analysis suggests that it is polyurea- and polycarbamate-like in nature. Rates of formation of the gaseous products and their respective quantities have been determined for a typical isothermal decomposition experiment at 235C. The temporal behaviors of the gas formation rates indicate that the overall decomposition is characterized by a sequence of four events; (1) an early decomposition period induced by impurities and water, (2) an induction period where C0{sub 2} and NO are the primary products formed at relatively constant rates, (3) an autoacceleratory period that peaks when the sample is depleted and (4) a final period in which the residue decomposes. Arrhenius parameters for the induction period are E{sub a} = 46.9 {plus_minus} 0.7 kcal/mol and Log(A) = 16.3 {plus_minus} 0.3. Decomposition pathways that are consistent with the data are presented.
Date: December 31, 1996
Creator: Minier, L.; Behrens, R. Jr. & Bulusu, S.
Partner: UNT Libraries Government Documents Department

Thermal decomposition reactions of HMX and RDX and their importance in predicting cookoff hazards

Description: To develop robust models for predicting the response of munitions under abnormal conditions associated with cookoff, it is necessary to be able to accurately characterize the following: the time to ignition, the location of the ignition point within the munition, and the combustive behavior of the damaged energetic material after ignition. For, the response of the munition, as controlled by these parameters, will determine whether its response will be characterized by a relatively mild deflagration or whether it will be characterized by a more damaging detonation. Several of the underlying properties of the energetic materials used in munitions that must be understood in order to accurately characterize these parameters are the chemical and physical changes that occur in these energetic materials as they are heated. The chemical changes involve overcoming the forces that tend to stabilize these materials, such as binding within the crystal lattice or intermolecular hydrogen bonding, and their transformation to less stable forms, such as mixtures of gases with high energy content. The physical changes typically involve phase changes of the material. One significant phase change is the slow transformation of the energetic materials from the solid reactant to gas phase products. This transformation can lead initially to the formation of high pressure gas bubbles within the solid particles and ultimately to changes in the porosity and gas permeability of the energetic material formulation. The presence of these reactive gases within high pressure bubbles can lead to increased hot spot formation of the material if it is compressed. The increased porosity can lead to significant increases in the burn rates of these materials at high pressures.
Date: May 1, 1994
Creator: Behrens, R. Jr. & Bulusu, S.
Partner: UNT Libraries Government Documents Department