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  • 1
    Electronic Resource
    Electronic Resource
    Laser-initiated half-reaction. Vibrational and rotational state distribution of NO produced from the reactant pair O(1D)⋅N2O (1988)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 88 (1988), S. 4739-4747 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The vibrational and rotational state distribution was measured for NO produced from the reaction O(1D)+N2O→2NO via a reactant pair O(1D)⋅N2O, which, in turn, formed by the 193 nm photolysis of the N2O dimer. The dimer was generated by the supersonic expansion through a pulsed nozzle. The distribution was determined by using the laser-induced fluorescence of NO on its A–X transition. The rotational distribution was of the Boltzmann type characterized by a low temperature, 60–100 K, at each vibrational level measured. The vibrational distribution was found to be composed of the two components, one very cold and the other relatively hot. The experiment using an isotopically labeled N2O revealed that the vibrational energy was not equally distributed over two kinds of NO; the NO originally present in N2O was vibrationally cool while that formed from O(1D) and the terminal nitrogen of N2O was vibrationally hot. These results indicate that the reaction occurring is the abstraction of the terminal nitrogen by O(1D). The low rotational temperature, which sharply contrasts with the extremely high rotational excitation observed for the ordinary bimolecular reaction, can be rationalized by considering the geometrical difference in the encounter between the O(1D) atom and N2O. This fact, in turn, indicates that the product energy distribution is significantly affected by the orientation in the reactive encounter.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.454687
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  • 2
    Electronic Resource
    Electronic Resource
    Crossed-beam study of the reaction of van der Waals molecule H+(NO)2 (1990)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 92 (1990), S. 1657-1660 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Chemiluminescent reaction H+(NO)2 →HNO*+NO was studied under single collision condition. The built-in third body much enhanced the formation of HNO*(A 1A‘) in bimolecular relatively large population in bending vibration (ν3 ) as compared with the HNO* produced from the termolecular recombination, H+NO+M. This apparent excitation in bending mode can be attributed to the smaller internal energy of HNO* produced in H+(NO)2 reaction. Higher rotational states of the (001) vibration, if formed in H+NO+M reaction, most probably suffer rapid losses to X 1A' state by internal conversion. The lower energy content of HNO* formed in H+(NO)2 reaction suppresses this internal conversion and hence the relative population of the (001) state becomes large. The reaction probability was also measured as a function of collision energy and the result indicates the absence of the reaction barrier.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.458100
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  • 3
    Electronic Resource
    Electronic Resource
    Microscopic solvation of acetone to 9,9'-bianthryl studied in a free jet: Polar excited state formation (1991)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 94 (1991), S. 3496-3503 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Dynamics of the electronically excited state of 9,9'-bianthryl (BA)–acetone complexes was studied in a free jet. The BA–acetone complexes were produced by supersonic expansion of BA/acetone/He mixtures. The laser induced fluorescence spectrum of the BA–acetone complexes showed several bands which were ascribed to the complexes containing different number of acetone molecules. The number of acetone molecules attaching to BA was determined by mass-selected resonance-enhanced multiphoton ionization (REMPI) spectra for each band. The Stokes shift and lifetime were measured for each band, i.e., for the BA–acetone complex with a specific number of "solvent'' molecules. These measurements revealed that there are two kinds of BA–acetone complexes; one giving the broad laser-induced fluorescence (LIF) spectrum and largely redshifted fluorescence, and the other yielding the structured LIF and the sharp fluorescence spectrum similar to that of bare BA. The Stokes shift and the lifetime of the former complex increased with increasing number of solvated acetone molecules, whereas those of the latter complex are insensitive to the degree of solvation. These findings can be explained in terms of the importance of both the "symmetry breaking'' and the "polar microscopic solvation'' in forming the so-called twisted intramolecular charge–transfer state.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.459770
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  • 4
    Electronic Resource
    Electronic Resource
    Guided-ion beam studies of the reactions of protonated water clusters, H(H2O)+n (n=1–4), with acetonitrile (1993)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 99 (1993), S. 1623-1632 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Reactions of protonated water clusters, H(H2O)n+ (n=1–4), with acetonitrile are studied by using guided-ion beam mass spectrometry. Absolute reaction cross sections are determined as a function of the collision energy from thermal energy to over 10 eV. Proton transfer, charge transfer, and dissociative proton transfer are the reactions seen for n=1. For n=2–4, proton transfer is accompanied by solvent transfer such that the dominant product at low collision energies is H(CH3CN)(H2O)n−1+ in each case. At higher collision energies, additional water ligands are lost and the collision-induced dissociation products, H(H2O)n-m+ where m=1 to n−1, are also observed. The total reaction cross sections are large and decrease slightly with the number of water molecules. The results indicate that energy transfer in these complexes is efficient and thus are consistent with reactions that proceed via hydrogen-bonded intermediate complexes.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.465331
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  • 5
    Electronic Resource
    Electronic Resource
    Reaction of O(1D) with ethylene: Vibrational and rotational state distribution of product OH (1993)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 99 (1993), S. 7677-7686 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Reaction of O(1D) with ethylene was studied under low pressure flow conditions. The O(1D) was formed by photodissociation of N2O by an ArF laser and rotational and vibrational state distributions of product OH were determined by laser induced fluorescence. The rotational distributions of the v=0 and 1 levels showed a bimodal feature. A major part of the OH had a rotational energy higher than the statistical expectation, and about 20% of total available energy appeared as the rotation of OH. About 20% of the total OH was characterized by a rotational distribution that corresponded to a specific temperature, i.e., 546 K and 526 K for v=0 and 1, respectively. The relative populations of the first two vibrational levels were measured to be 1.00 and 0.30, and no inversion was observed. No propensity was observed between formation of the two spin–orbit states, and the Π(A') state was slightly more favored than the Π(A‘) state. These results were explained by a mechanism in which O(1D) inserts into a CH bond of ethylene and OH is eliminated from a bend geometry. The same reaction was studied under cluster conditions where a van der Waals complex of N2O–C2H4 was converted into the reactant pair, O(1D)–C2H4. The rotational distribution of OH formed under these conditions showed little difference from that from the bimolecular reaction.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.465697
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  • 6
    Electronic Resource
    Electronic Resource
    Ion desorption from H2O chemisorbed on Si(100) by O 1s electron excitation at room temperature (1995)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 102 (1995), S. 1422-1431 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The photon stimulated ion desorption (PSID) of H+ and O+ from monolayer H2O adsorbed on the Si(100) has been studied using pulsed synchrotron radiation in the 510–620 eV range. Ions were detected and mass analyzed by means of time-of-flight spectroscopy. Relative yield spectra of these ions indicated characteristic behavior near the O K edge. The predominant H+ fragment ion shows a sharp rise at about 530 eV and two broad peaks (535 eV, 558 eV), while O+ shows a delayed threshold at about 570 eV and gradual increase up to 700 eV. Above the O K edge, these ion yields were found to deviate significantly from the O(KVV) Auger electron yield. This was interpreted by the fact that ion desorption was enhanced by multiple ionization and is strongly affected by the decay process with the surface. In order to elucidate the mechanism of the PSID, the technique of photoion–photoion coincidence between H+ and O+ ions was also applied. The results suggested the formation of multiply charged intermediates, i.e., OH4+ ions, which were incompletely reneutralized despite of strong interaction with substrate and desorbed as singly charged H+ and O+ ions. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.468929
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  • 7
    Electronic Resource
    Electronic Resource
    Radiative dissociation of C2H2, C2HD, and C2D2 superexcited at 50–90 nm region (1995)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 102 (1995), S. 5301-5308 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Radiative dissociation of superexcited acetylene was studied at hν=13.8–24.8 eV (90–50 nm) by using C2H2, C2HD, and C2D2. The observed emission bands were d 3Πg→a 3Πu, e 3Πg→a 3Πu, C 1Πg→A 1Πu, and D 1∑+u→X 1∑−g of C2 radical, and A 2Δ→X 2Πr, B 2Σ−→X 2Πr, and C 2Σ+→X 2Πr of CH and CD radicals. The fluorescence cross sections of the electronically excited C*2 radicals showed a hydrogen isotope effect, i.e., the cross sections were in order of σf[C2(C2H2)](approximately-greater-than)σf[C2(C2HD)](approximately-greater-than)σf[C2(C2D2)]. Reverse is true for the fluorescence cross sections of CH* and CD*, i.e., σf(C2H2)〈σf(C2HD)〈σf(C2D2). These isotope effects were interpreted by the competition of some decay processes from the superexcited states. Hydrogen isotope effect in simple C–H and C–D bond dissociation is important for the C*2 formation. As a result of the competition with this C*2 formation, the "reverse'' isotope effect emerges in the CH* and CD* formations. Another important competing process is the isomerization followed by formation of nonradiative fragments. Since H atom migrates more easily than D atom through a cyclic cavitated complex and the nonradiative fragmentation competes with the CH* and CD* formation, the radiative intensities of the CH* and CD* radicals inevitably show the apparent inverse hydrogen isotope effect. The isomerization seems to be specially important in the wavelength region, λ(approximately-greater-than)80 nm, where a trans-bent superexcited state is formed. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.469256
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  • 8
    Electronic Resource
    Electronic Resource
    Laser initiated half reaction study of H+O2→OH+O (1995)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 102 (1995), S. 7856-7863 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The H+O2 reaction system was studied under geometry limited half reaction conditions. The weakly bonded complex O2–H2S was formed by supersonic expansion, and reaction was initiated by 193 nm photoirradiation of the complex. Rotational, spin-orbit, and lambda doublet state distributions of product OH were determined by a laser-induced fluorescence (LIF) technique. The populations of the two spin-orbit states were observed to be statistical. The population of the Π(A') level was almost twice that of the Π(A‘) level, and the planar geometry was suggested for reaction path. These populations of the fine structures of OH were similar to those of OH formed under bimolecular reaction conditions. On the other hand, the rotational state distribution of OH from the half reaction has two components and the dominant one shows a very cold rotational distribution, in sharp contrast with that of the bimolecular reaction where rotation is highly excited. This cold rotational distribution could be partially explained by the absorption of a part of available energy by the internal motion of SH. However, the distribution with a peak at the lowest rotational level could not be explained by this effect, but ascribed to the exit interaction between SH and OH and/or the entrance channel specificity, i.e., the reaction occurs in limited impact parameters. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.468986
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  • 9
    Electronic Resource
    Electronic Resource
    Symmetry demand in polar excited state formation of 9,9'-bianthryl in clusters with some ketones (1994)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 101 (1994), S. 1752-1754 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Laser-induced fluorescence (LIF) and dispersed fluorescence (DF) spectra have been studied for clusters of 9,9'-bianthryl (BA) with acetone, diethyl ketone, and methyl–ethyl ketone. Two different kinds of clusters have been observed in clusters containing the symmetric ketones. One shows broad LIF and DF spectra which are characteristic to the polar excited state of BA. The other shows sharp LIF bands and short lifetime which indicate the absence of the electron transfer.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.467734
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  • 10
    Electronic Resource
    Electronic Resource
    Vector correlations in the 193 nm photodissociation of the NO dimer (1995)
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 99 (1995), S. 13652-13658 
    Details
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/j100037a012
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