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  • 1
    Electronic Resource
    Electronic Resource
    Erratum: "Femtosecond stimulated emission pumping: Characterization of the I2− ground state" [J. Chem. Phys. 112, 8847 (2000)] (2000)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 113 (2000), S. 8854-8854 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.1318753
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  • 2
    Electronic Resource
    Electronic Resource
    Femtosecond photoelectron spectroscopy of I2−(CO2)n clusters (n=4, 6, 9, 12, 14, 16) (2000)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 601-612 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The photodissociation dynamics of I2−(CO2)n(n=4–16) clusters excited at 780 nm have been studied with femtosecond photoelectron spectroscopy (FPES). The range of cluster sizes spans the uncaged and fully-caged product limits for this reaction. We observe time scales for a variety of processes in these clusters, including dissociation of the I2− chromophore, solvation of the I− fragment, the onset of recombination on the ground state of I2−, vibrational relaxation, and solvent evaporation. In addition, substantial trapping in a "solvent-separated" state is seen for clusters with n≥9; this state persists for at least 200 ps, the longest time delay probed here. Simulations of the spectra were performed in order to determine the time dependence of the electronic state populations, the I2− vibrational distribution, and the number of CO2 molecules in the cluster. Results are compared to previous experimental and theoretical studies of I2−(CO2)n photodissociation, and to a recent FPES study of I2−(Ar)n clusters. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.480685
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  • 3
    Electronic Resource
    Electronic Resource
    Femtosecond photoelectron spectroscopy of the I2− anion: Characterization of the A˜′ 2Πg,1/2 excited state (1999)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 110 (1999), S. 3748-3755 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A potential energy curve for the A˜′ 2Πg,1/2 state of I2− is constructed based on femtosecond photoelectron spectroscopy of the I2− A˜′ 2Πg,1/2←X˜ 2Σu+ transition at 780 nm. The experiment is sensitive to the slope of the repulsive potential wall, the well depth, equilibrium bond length, and the long-range attractive portion of the upper state potential. The A˜′ 2Πg,1/2 potential is fit to a piecewise potential which is flexible in each of these regions. Simulations of the spectrum using a previously determined Morse potential for the X˜ 2Σu+ state of I2− [J. Chem. Phys. 107, 7613 (1997)] yields a well depth (De) of 0.017±0.010 eV for the A˜′ 2Πg,1/2 state with an equilibrium bond length (Re) of 6.2±0.6 Å. These values differ significantly from previous semiempirical results. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.478264
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  • 4
    Electronic Resource
    Electronic Resource
    Photodissociation of gas phase I3− using femtosecond photoelectron spectroscopy (1999)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 2991-3003 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The photodissociation dynamics of gas phase I3− following 390 nm excitation are studied using femtosecond photoelectron spectroscopy. Both I− and I2− photofragments are observed; the I2− exhibits coherent oscillations with a period of 550 fs corresponding to ∼0.70 eV of vibrational excitation. The oscillations dephase by 4 ps and rephase at 45 and 90.5 ps on the anharmonic I2− potential. The gas phase frequency of ground state I3− is determined from oscillations in the photoelectron spectrum induced by resonance impulsive stimulated Raman scattering. The dynamics of this reaction are modeled using one- and two-dimensional wave packet simulations from which we attribute the formation of I− to three-body dissociation along the symmetric stretching coordinate of the excited anion potential. The photodissociation dynamics of gas phase I3− differ considerably from those observed previously in solution both in terms of the I2− vibrational distribution and the production of I−. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.479660
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  • 5
    Electronic Resource
    Electronic Resource
    Femtosecond photoelectron spectroscopy of I2−(Ar)n clusters (n=6,9,12,16,20) (1999)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 10566-10577 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The photodissociation of I2− embedded in mass-selected I2−(Ar)n clusters (n=6–20) was studied using femtosecond photoelectron spectroscopy. The A˜′←X˜ transition in the I2− chromophore was excited using a femtosecond pump pulse, and the subsequent dynamics were followed by photodetachment with a femtosecond probe pulse and measurement of the resulting photoelectron spectrum. In all clusters, dissociation of the I2− is complete by 300 fs. From 300 fs to 1 ps, the spectra yield the number of Ar atoms interacting with the I− fragment. At later times, recombination of I2− occurs in I2−(Ar)n≥12 on both the X˜ and A˜ states. Analysis of the spectra yields the time scale for X˜ state vibrational relaxation and solvent evaporation. In I2−(Ar)20, energy transfer from I2− to Ar atoms through vibrational relaxation is slightly faster than energy loss from the cluster through Ar evaporation, indicating the temporary storage of energy within Ar cluster modes. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.480433
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  • 6
    Electronic Resource
    Electronic Resource
    Femtosecond stimulated emission pumping: Characterization of the I2− ground state (2000)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 8847-8854 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Femtosecond stimulated emission pumping in combination with femtosecond photoelectron spectroscopy is used to characterize the potential energy function of the I2−(X˜ 2Σu+) ground state up to vibrational energies within 2% of the dissociation limit. The frequency and anharmonicity of this state are measured at a series of vibrational energies up to 0.993 eV by coherently populating a superposition of ground state vibrational levels using femtosecond stimulated emission pumping, and monitoring the resulting wave packet oscillations with femtosecond photoelectron spectroscopy. The dissociative I2−(A˜′ 2Πg,1/2) state is used for intermediate population transfer, allowing efficient population transfer to all ground state levels. Using the measured frequencies and anharmonicities, the X˜ 2Σu+ state has been fit to a modified Morse potential with the β-parameter expanded in a Taylor series, and the bond length, well depth, and υ=0–1 fundamental frequency set equal to our previously determined Morse potential [J. Chem. Phys. 107, 7613 (1997)]. At high vibrational energies, the modified potential deviates significantly from the previously determined potential. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.481499
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  • 7
    Electronic Resource
    Electronic Resource
    Femtosecond photoelectron spectroscopy of the I2− anion: A semiclassical molecular dynamics simulation method (1999)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 110 (1999), S. 3736-3747 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: In this paper we describe a new semiclassical method for simulating femtosecond pump–probe photoelectron spectroscopy, and its implementation to study the excited state photodissociation dynamics of the I2− anion. Our algorithm involves a forward–backward (FB) semiclassical (SC) initial value representation (IVR) method for calculating the time dependent photodetachment spectrum P(ε,Δt) as a function of the kinetic energy ε of the photodetached electron and the delay time Δt between the pump and probe pulses. We describe the radiation-chromophore interaction perturbatively to first order in both pulse fields, assuming the Condon approximation for the electronic transition dipole moments. Our computed spectra are in excellent agreement with full quantum mechanical simulations. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.478263
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  • 8
    Electronic Resource
    Electronic Resource
    Characterization of the I3 radical by anion photoelectron spectroscopy (1999)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 110 (1999), S. 7607-7609 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The ground and first excited states of the I3 radical are characterized by photoelectron spectroscopy of I3− and Ar⋅I3− at 266 nm. The electron affinity of I3 is 4.226±0.013 eV. Based on the recently determined bond dissociation energy of I3−, the I3 ground state is bound by 0.143±0.06 eV. The first excited state of I3 lies 0.27 eV above the ground state. A vibrational progression is seen in the ground state band of the I3− photoelectron spectrum. The addition of an argon atom to I3− reduces the contribution of hot bands to the photoelectron spectrum, facilitating the interpretation of the vibrational structure. Simulations indicate that the I3 ground state is linear with a symmetric stretch frequency of 115±5 cm−1 and is likely to be centrosymmetric. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.478672
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  • 9
    Electronic Resource
    Electronic Resource
    Characterization of the I2− anion ground state using conventional and femtosecond photoelectron spectroscopy (1997)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 7613-7619 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The X˜ 2Σu+ state of the I2− anion has been fit to a Morse potential using data from two techniques: conventional and femtosecond photoelectron spectroscopy (FPES). Conventional photoelectron spectroscopy is used to determine the adiabatic electron affinity of I2 as well as the well depth and equilibrium nuclear geometry of I2−. In the FPES experiment, the pump pulse induces coherent nuclear motion on the ground state of I2− by resonant impulsive stimulated Raman scattering (RISRS), and the vibrational frequency of the anion is determined from the resulting oscillatory structure in the time-dependent photoelectron spectra. We find the electron affinity (EA) of I2 to be 2.524±0.005 eV, the well depth (De) for I2− to be 1.014±0.005 eV, the equilibrium internuclear separation (Re) to be 3.205±0.005 Å, and the vibrational frequency to be 110±2 cm−1. These values for the I2− potential parameters differ significantly from previous results. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.475110
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  • 10
    Electronic Resource
    Electronic Resource
    Solvent effects on the vibrational frequency of I2〈sup ARRANGE="STAGGER"〉− in size-selected I2〈sup ARRANGE="STAGGER"〉−(Ar)n and I2〈sup ARRANGE="STAGGER"〉−(CO2)n clusters (1998)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 109 (1998), S. 9648-9651 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The vibrational frequency of the I2〈sup ARRANGE="STAGGER"〉− chromophore in size-selected I2〈sup ARRANGE="STAGGER"〉−(Ar)n and I2〈sup ARRANGE="STAGGER"〉−(CO2)n clusters has been measured to wave-number accuracy. The frequencies are determined by creating a coherent superposition of vibrational levels with a femtosecond laser pulse via a resonance impulsive stimulated Raman scattering process. The resulting wave-packet oscillations are detected with femtosecond photoelectron spectroscopy. Blueshifting of the frequency occurs upon solvation, with larger shifts observed for solvation with CO2. The nature of the shifting is discussed and related to specific cluster geometries. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.477631
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