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Author: Publisher: ISBN: Category : Languages : en Pages : 6
Book Description
The objectives of this effort were as follows: (1) extend the technical development of pulsed infrared (IR) cavity ringdown spectroscopy to longer wavelengths and higher spectral resolution; (2) develop its capacity as a general tool for trace gas analysis; and (3) study spectra, structures, hydrogen tunneling dynamics of hydrocarbon ions and complexes of relevance to ion-enhanced combustion processes. High-resolution, pulsed infrared cavity ringdown laser spectroscopy was developed and implemented for the study of carbon clusters and hydrocarbon ions. Several supersonic molecular beam sources of ions and hydrocarbons were constructed and tested by infrared cavity ringdown spectroscopy. The Stokes downconversion of pulsed visible laser radiation into the mid-infrared was explored in solid and liquid hydrogen media in an effort to explore more powerful and convenient infrared sources. Cavity ringdown studies of several different carbon/hydrocarbon systems were carried out. Nine related publications and three conference presentations are listed.
Author: Publisher: ISBN: Category : Languages : en Pages : 6
Book Description
The objectives of this effort were as follows: (1) extend the technical development of pulsed infrared (IR) cavity ringdown spectroscopy to longer wavelengths and higher spectral resolution; (2) develop its capacity as a general tool for trace gas analysis; and (3) study spectra, structures, hydrogen tunneling dynamics of hydrocarbon ions and complexes of relevance to ion-enhanced combustion processes. High-resolution, pulsed infrared cavity ringdown laser spectroscopy was developed and implemented for the study of carbon clusters and hydrocarbon ions. Several supersonic molecular beam sources of ions and hydrocarbons were constructed and tested by infrared cavity ringdown spectroscopy. The Stokes downconversion of pulsed visible laser radiation into the mid-infrared was explored in solid and liquid hydrogen media in an effort to explore more powerful and convenient infrared sources. Cavity ringdown studies of several different carbon/hydrocarbon systems were carried out. Nine related publications and three conference presentations are listed.
Author: Oscar Rodriguez (Jr) Publisher: ISBN: Category : Languages : en Pages :
Book Description
Many biological and environmental systems contain ion, water, and hydrophobic components; and it is the balance between these competing interactions which governs their chemistry. This Thesis aims at exploring ion0́Ø0́Ø0́Øhydrocarbon interactions, then ion0́Ø0́Ø0́Øwater0́Ø0́Ø0́Øalkane interactions. To accomplish this, a combination of gas phase infrared predissociation spectroscopy (IRPD) and tandem mass spectrometry is utilized. The solvation of alkali metal ions by methane is discussed first, beginning with the effects of multiple argon atoms on Li+0́Ø0́Ø0́ØCH4 dimer clusters followed by a study of M+(CH4)n clusters where it is revealed that ions have a weak electrostatic effect beyond the first solvent shell. Next, the argon tagging and monitoring unique fragmentation channels are used to selectively probe for high energy Li+(H2O)3-4Ar1 conformers which contain extensive water hydrogen bonding. Finally, ion0́Ø0́Ø0́Øwater0́Ø0́Ø0́Øalkane interactions are probed in Li+(H2O)n clusters containing CH4 or C6H12 molecules. Some spectra contain hydrogen bonded peaks correlating to weak water0́Ø0́Ø0́Øalkane interactions. Furthermore, there is strong evidence that high energy conformers containing water hydrogen bonding are present in the cluster ion beam. This analysis is expanded to anionic Cl-(Water)m(CH4)n clusters to compare with cations. Density functional theory or MP2 level calculations were used to support and help characterize experimental data.
Author: Richard Saykally Publisher: ISBN: Category : Languages : en Pages : 5
Book Description
A high resolution infrared cavity ringdown laser absorption spectrometer has been developed to study proposed HEDM molecules and metal containing clusters. Using a novel tunable pulsed Alexandrite ring laser, we are able to generate tunable visible radiation with ca, 40 MHz bandwidth. This tunable visible light is downconverted to the infrared using stimulated Raman scattering in H2 and D2. With this system, tunable radiation from the UV to the far infrared can be generated with ca, 100 MHz bandwidth. We will test this system using our pulsed supersonic laser vaporization source to study both metal and carbon containing species. Infrared Cavity Ringdown Spectroscopy has also been used to study water clusters in both pulsed supersonic beams and pulsed discharged nozzles.
Author: Publisher: ISBN: Category : Languages : en Pages : 14
Book Description
Efforts focused on four activities related to the central objective of studying metal-containing clusters, HEDM molecules, and clusters of ceramic materials. Nineteen AFOSR supported papers were published on the following topics (including five journal cover articles) : 1) Development of high resolution (100 MHz), high sensitivity pulsed infrared cavity ringdown spectroscopy as a general tool for trace species characterization. 2) Infrared cavity ringdown system with medium (900 MHz) resolution constructed and operational. 3) IR studies of hydrogen bonding in water, methanol, ethanol, and butanol clusters carried out. 4) More difficult IR experiments on laser vaporized carbon and silicon carbide initiated.
Author: Jordan P. Beck Publisher: ISBN: Category : Languages : en Pages :
Book Description
Infrared predissociation (IRPD) spectra of several cluster ions are presented, resulting in the emergence of two major themes. Trapped, high energy conformers are observed in argon tagged clusters. In non-argon tagged hydrated alkali metal ion clusters, multiple photon absorption processes can occur. The cluster ions discussed in this dissertation are generated by impacting neutral clusters with ions. If there is an energetic barrier between the neutral cluster configuration and the global minimum cluster ion configuration that is larger than the binding energy of the most labile ligand, then high energy conformers can be trapped. Thus, the trapped conformers retain some of the bonds of their neutral precursors. For example, neutral methanol dimer contains a hydrogen bond and a trapped, high energy Cl (CH3OH)2Ar conformer was observed which also contains a methanol0́Ø0́Ø0́Ømethanol hydrogen bond. Similar results are reported for M+(C6H6)2-4(H2O)2Ar and M+(benzyl alcohol)1(H2O)1-2Ar where IRPD spectra reveal hydrogen bonds resulting from the configurations of the neutral precursors. For most of the clusters studied, spectral features from high energy conformers and global minimum energy conformers were observed in the same spectra. However, a special case is reported in chapter 5 in which spectral features from high energy conformers and global minimum energy conformers of Li+(C6H6)2-4(H2O)2Ar were observed in different spectra corresponding to the fragmentation channel monitored. This conformer specific fragmentation greatly simplified the interpretation of the spectra and provided useful information on the cluster energetics. Conformer specific fragmentation was also observed for M+(H2O)5-7, but for a different reason. In the hydrogen bonded O-H stretching region, IRPD spectra obtained by monitoring the loss of two waters only contained features from linear hydrogen bonds. This mode dependent fragmentation is believed to be the result of multiple photon absorption. This conclusion is supported by laser-fluence dependence studies and by evaporative ensemble calculations.
Author: Publisher: ISBN: Category : Languages : en Pages : 249
Book Description
This thesis describes new experiments wherein the infrared vibrational predissociation spectra of a number of mass-selected ionic cluster systems have been obtained and analyzed in the 2600 to 4000 cm−1 region. The species studied include: the hydrated hydronium ions, H3O (H2O){sub 3 -10}, ammoniated ammonium ions, NH4(NH3){sub 1 -10} and cluster ions involving both water and ammonia around an ammonium ion core, (mixed clusters) NH4(NH3){sub n}(H2O){sub m} (n+m=4). In each case, the spectra reveal well resolved structures that can be assigned to transitions arising from the vibrational motions of both the ion core of the clusters and the surrounding neutral solvent molecules. 154 refs., 19 figs., 8 tabs.
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Author: Oscar Rodriguez (Jr)
Author: Joshua Barron Paul
Author: Jong-Ho Choi
Author: John Michael Price
Author: Richard Saykally
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Author: Jordan P. Beck
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