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  • 1
    Electronic Resource
    Electronic Resource
    Molecular beam study of the 6Π–X 6Δ electronic transition in FeCl (2000)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 10221-10227 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The 6Π–X 6Δ band system of Fe35Cl near 357 nm has been recorded at 0.3 and 0.08 cm−1 resolution by laser fluorescence excitation in a free-jet supersonic expansion of photolyzed Fe(CO)5 diluted in seed gases containing CCl4. The 6ΠΩ′=Ω″−1–X 6ΔΩ″ subbands for Ω′=7/2, 5/2, and 3/2 and v′≤4 of the Δv=1, 0, −1, and −2 sequences were assigned, and excitation energies and rotational constants were derived for the relevant upper and lower vibronic levels. With the exception of the (0,0) band, for which one subband could be rotationally analyzed, it was not possible to assign any of the subbands with Ω′=1/2, −1/2, or −3/2; these fine-structure components are expected to be strongly affected by homogeneous spin–orbit interactions with nearby sextet electronic states, leading to large Λ doubling in the Ω′=1/2 and −1/2 components. A subband with a large upper-state Λ doubling was rotationally analyzed and assigned as the 6Π1/2–X 6Δ3/2 (0,0) subband. The effect of the off-diagonal spin–orbit interactions is discussed in light of the present results and previous theoretical work. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.481664
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  • 2
    Electronic Resource
    Electronic Resource
    Photodissociation of CH stretch overtone excited CH3Cl and CHD2Cl(vCH=5): Cl spin–orbit branching and atomic fragment yields (1998)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 109 (1998), S. 7810-7820 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The photodissociation dynamics of CH3Cl and CHD2Cl excited through their respective fourth C–H stretch overtone transitions have been investigated by detection of ground state Cl(2P3/2), spin–orbit excited Cl(2P1/2), H, and D atomic fragments by 2+1 resonance enhanced multiphoton ionization in a time-of-flight mass spectrometer. The yield of atomic Cl fragments from the vibrationally mediated photodissociation of CHD2Cl is significantly less than for CH3Cl, more than can be accounted for from differences in the cross sections for overtone excitation. This suggests that state mixing leads to a greater amplitude of the wave function of the vibrationally excited level along the dissociation coordinate in CH3Cl than in CHD2Cl. The observed differences in the Cl spin–orbit branching in the photolysis of ground state versus vibrationally excited molecules are ascribed to differences in the nuclear dissociation dynamics, rather than access to other excited electronic states. The relative yields of H and D atoms from the photodissociation of ground and vibrationally excited CHD2Cl are also reported and discussed. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.477427
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  • 3
    Electronic Resource
    Electronic Resource
    Rotational analysis of the B˜2A′′−X˜2A′′ origin band of the CH2CFO radical (1997)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 9755-9758 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The laser fluorescence excitation spectrum of the origin band of an electronic transition in the CH2CFO radical was recorded with partial rotational resolution using a supersonic, rotationally cold beam. The radical was prepared in a pulsed free jet by 193 nm photolysis of acetyl fluoride diluted in helium or argon. The rotational structure of the band is consistent with an in-plane electronic transition of this near oblate rotor. In analogy with the vinoxy radical, this transition is designated as B˜2A′′−X˜2A′′. Spectroscopic constants were derived from a fit to the assigned rotational transitions. The lower state rotational constants agree with those calculated from an ab initio CH2CFO equilibrium structure [M. Furubayashi, I. Bridier, S. Inomata, N. Washida, and K. Yamashita, J. Chem. Phys. 106, 6302 (1997)]. The present study thus provides confirmation of the assignment of the molecular carrier as CH2CFO and eliminates the alternative assignment to FCO [B. A. Williams and J. W. Fleming, J. Chem. Phys. 106, 4376 (1997)]. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.475272
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  • 4
    Electronic Resource
    Electronic Resource
    Fluorescence excitation and depletion spectroscopy of the BAr complex: Electronic states correlating with the excited valence B(2s2p2 2D) asymptote (1997)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 106 (1997), S. 6596-6606 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Laser fluorescence excitation and depletion spectra of the BAr van der Waals complex, in the spectral region around the B atomic 2s2p2 2D←2s22p 2P transition at 208.9 nm, are reported. The fluorescence excitation spectrum displays a series of structured bands, whose excited levels are weakly bound (≤60 cm−1), and an unstructured continuum to the blue. The onset of the latter allows determination of the ground state dissociation energy D0″=102.4±0.3 cm−1. The fluorescence depletion spectrum reveals, in addition, bands at lower wave numbers to a strongly bound, predissociating state, assigned as C2Δ. The bands observed by fluorescence excitation are assigned to the D2Π, E2Σ+–X2Π transitions. The derived spectroscopic data are used to construct potential energy curves for the C2Δ and D2Π states. The predissociation of the C2Δ state is due to spin–orbit coupling to a repulsive 4Π state correlating with the B(2s2p2 4P)+Ar asymptote, as shown in the accompanying paper [K. Sohlberg and D. R. Yarkony, J. Chem. Phys. 106, 6607 (1997)]. A weak nonradiative decay process is also observed for the D2Π state. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.473649
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  • 5
    Electronic Resource
    Electronic Resource
    Electronic Spectroscopy and Excited State Dynamics of the KrAlH(X1Σ+,A1ΠI.) van der Waals Complex (1995)
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 99 (1995), S. 3430-3437 
    Details
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/j100011a005
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  • 6
    Electronic Resource
    Electronic Resource
    Product State Distributions and Angular Differential Cross Sections from Photoinitiated Reactions of Chlorine Atoms with Small Hydrocarbons (1995)
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 99 (1995), S. 9843-9853 
    Details
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/j100024a028
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  • 7
    Electronic Resource
    Electronic Resource
    Experimental and theoretical study of rotationally inelastic collisions of highly rotationally excited CN(A 2Π) with Ar (2000)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 4474-4484 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A collaborative experimental and theoretical study of rotationally inelastic collisions of CN(A 2Π,v=3,N=60) fine-structure Λ-doublet levels with argon is presented. Experimental state-to-state rate constants were determined with an optical–optical double resonance technique. The CN radical was prepared by 193 nm photolysis of BrCN diluted in slowly flowing argon at a total pressure of ∼0.9 Torr. Specific levels of CN(A 2Π,v=3,N=60) were prepared by excitation with a pulsed dye laser on various rotational lines in the A 2Π–X 2Σ+(3,0) band, and collisionally populated levels were probed after a short delay by laser fluorescence excitation in the B 2Σ+–A 2Π(3,3) band. Final state distributions (relative state-to-state rate constants) are reported. To calibrate their magnitude, absolute total removal rate constants and the large state-to-state rate constants for ΔN=−1 fine-structure conserving, Λ-doublet symmetry-conserving transitions were determined. The measured rate constants were compared with theoretical rate constants computed in a quantum scattering treatment of the dynamics with ab initio CN(A 2Π)–Ar potential energy surfaces. The agreement of measured and computed rate constants is very good. The rate constants display dramatic Λ-doublet propensities which depend upon the reflection symmetry of the initial level. From examination of coupled-state partial cross sections as a function of the projection quantum number specifying the angle of approach of the Ar atom to the CN plane of rotation, these propensities are shown to arise from a "helicopter" approach orientation which facilitates curve crossings between effective potential energy curves correlating with different rotational asymptotes. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.481010
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  • 8
    Electronic Resource
    Electronic Resource
    Spin–orbit branching in the photofragmentation of HCl at long wavelength (1998)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 108 (1998), S. 4460-4466 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We report a new experimental determination of the branching ratio for formation of ground state Cl(2P3/2) and spin–orbit excited Cl(2P1/2) fragments subsequent to excitation of the HCl molecule to the repulsive A 1Π electronic state. Our work extends previous experimental measurements well into the long-wavelength tail of the A 1Π←X 1Σ+ absorption profile. The branching into the spin–orbit excited Cl(2P1/2) fragment is found to reach a maximum near 220 nm, before falling to zero at threshold. Our new measured branching fractions are reproduced nearly quantitatively by new calculations which supplement those reported previously [M. H. Alexander, B. Pouilly, and T. Duhoo, J. Chem. Phys. 99, 1752 (1993)]. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.475857
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  • 9
    Electronic Resource
    Electronic Resource
    Fluorescence excitation spectroscopy of the Ar–HCO(X˜ 2A′,B˜ 2A′) van der Waals complex (1997)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 680-690 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The fluorescence excitation spectrum of the Ar–HCO van der Waals complex in the vicinity of the B˜ 2A′–X˜ 2A′ 000 band of free HCO is reported. At least eight bands associated with the complex have been detected. From the spectral shift of the lowest energy Ar–HCO band from the origin of the free HCO transition, we estimate the Ar–HCO binding energy in the excited electronic state to be at least 13 cm−1 greater than that in the ground state. Rotational analysis of some of the bands has been carried out, and average Ar–HCO separations (∼3.7 Å) in both electronic states determined. Several of the bands were assigned as hot bands from the first excited bend–stretch level (K″=1) in the ground electronic state. From the derived A rotational constants, we conclude that the ArCO framework has an approximately T-shaped geometry in both electronic states. The decay lifetime of the upper state of the strongest Ar–HCO band was measured and was found to be somewhat smaller than those previously measured for low rotational levels of free HCO. With the high signal-to-noise ratio in this study, it was also possible to observe transitions in the free H13CO isotopomer. A rotational analysis of the B˜ 2A′–X˜ 2A′ 000 band of the H13CO isotopomer was carried out. The isotopic shifts of the origins of the 301 and 201 bands were also measured, and a normal mode analysis of HCO(B˜) was carried out. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.474469
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  • 10
    Electronic Resource
    Electronic Resource
    Experimental study of rotationally inelastic collisions of AlH(A 1Π) with Ar: State-to-state rate constants and Λ-doublet propensities (2000)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 113 (2000), S. 4124-4131 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A study of rotationally inelastic collisions of AlH(A 1Π) with Ar is reported. AlH was prepared by 193 nm photolysis of trimethylaluminum diluted in slowly flowing Ar at ∼0.5 Torr total pressure. Specific rotational, Λ-doublet levels of AlH(A 1Π,v=0) were prepared by pulsed dye laser excitation on rotational lines in the AlH A 1Π–X 1Σ+ (0,0) band, and final levels were detected by spectrally resolving the fluorescence emission. Bimolecular state-to-state and total removal rate constants were determined. The state-to-state rate constants display dramatic Λ-doublet propensities. In particular, for high initial rotational levels the ΔJ=−1 f→e Λ-doublet symmetry changing transitions had significantly larger rate constants than for ΔJ=−1 f→f Λ-doublet symmetry conserving transitions. These Λ-doublet changing transitions are facilitated by curve crossing between the effective potential energy curves correlating with different rotational asymptotes. The total removal rate constants decrease with increasing initial J, reflecting the increasing rotational spacings. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.1288174
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