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  • 1
    Electronic Resource
    Electronic Resource
    Photodissociation and geminate recombination dynamics of iodine (I2-) in mass-selected iodine-carbon dioxide (I2-(CO2)n) cluster ions (1991)
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 95 (1991), S. 8028-8040 
    Details
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/j100174a008
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  • 2
    Electronic Resource
    Electronic Resource
    I2− photofragmentation/recombination dynamics in size-selected I2−(CO2)n cluster ions: Observation of coherent I...I− vibrational motion (1992)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 97 (1992), S. 7002-7005 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We have employed picosecond pump–probe techniques in conjunction with a tandem time-of-flight mass spectrometer to investigate the caging dynamics of photodissociated I2− solvated with a specific number of CO2 molecules. In this paper, we report the observation of a recurrence at ≈2 ps in the I2− absorption recovery, a feature which is attributed to coherent I...I− nuclear motion following I2− photoexcitation.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.463206
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  • 3
    Electronic Resource
    Electronic Resource
    Time-resolved measurements of the photodissociation and recombination dynamics of I−2 in mass selected cluster ions (1989)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 91 (1989), S. 6533-6534 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We present picosecond time-resolved pump-probe measurements of the photodissociation and recombination dynamics of I−2 surrounded by a specific number of CO2 molecules in mass selected I−2 (CO2)n clusters. The transient bleaching data can be fit to an exponential absorption recovery of 30±10 ps in I−2 (CO2)9 clusters and 10±5 ps in I−2 (CO2)16 clusters. The data demonstrate the feasibility of measurements of real-time reaction dynamics in microsolvent environments.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.457370
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  • 4
    Electronic Resource
    Electronic Resource
    I−2 photodissociation and recombination dynamics in size-selected I−2(CO2)n cluster ions (1993)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 99 (1993), S. 8733-8750 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Pump–probe techniques are used in conjunction with a tandem time-of-flight mass spectrometer to investigate the I...I− cage recombination dynamics following I−2 photodissociation in size-selected I−2(CO2)n cluster ions. The absorption recovery, which reflects the recombination and vibrational relaxation of the photodissociated I−2, exhibits a strong cluster size dependence in the range of n=13–15. Over this limited cluster size range, the absorption recovery time decreases from ∼40 ps (n≤12) to ∼10 ps (n≥15). In addition, a recurrence is observed at ≈2 ps in the absorption recovery of the larger clusters (n=14–17). This feature results from coherent I...I− motion following photodissociation. Measurement of the absorption recovery with both parallel and perpendicular pump–probe polarizations demonstrates that the pump and probe transition dipoles lie in the same direction. Analysis of the I−2 transition dipole directions shows that the coherent motion takes place on the first two repulsive excited potential surfaces. The two-photon photofragment distribution reflects the solvent cage structure as a function of pump–probe delay time.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.466211
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  • 5
    Electronic Resource
    Electronic Resource
    Effects of hydrogen bonding on the low-lying electronic states of a model polyene aldehyde (1990)
    s.l. : American Chemical Society
    Journal of the American Chemical Society 112 (1990), S. 1912-1920 
    Details
    ISSN: 1520-5126
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/ja00161a041
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  • 6
    Electronic Resource
    Electronic Resource
    Wave-packet dynamics in the Li2 E(1Σ+g) shelf state: Simultaneous observation of vibrational and rotational recurrences with single rovibronic control of an intermediate state (1995)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 103 (1995), S. 7269-7276 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A three-step excitation sequence is used to study the wave-packet dynamics in the E(1Σ+g) "shelf'' state of lithium dimer. In the first excitation step, a continuous wave (cw) dye laser prepares a single rovibrational level (v=14, J=22) in the intermediate 7Li2 A(1Σ+u) state. Ultrafast excitation of this single level with a 200 fs laser pulse centered at 803 nm creates a rovibrational wave packet (v=13–16; J=21 and 23) in the shelf region of the E(1Σ+g) state. The motion of this three-dimensional wave packet is probed via ionization by a second ultrafast laser pulse of the same color. The initial cw excitation step allows precise control of the states that compose the wave packet. Fourier analysis of the pump–probe transients shows 15 frequency components that correspond to energy differences between the levels that constitute the wave packet. Because of the large rotational energy splitting, the rotational beats occur in the same frequency range as the vibrational beats. Experiments performed with parallel and perpendicular pump-probe polarizations provide a "magic angle'' transient in which only the pure vibrational beats are observed, thus aiding in the spectroscopic assignment. The observed beat frequencies agree well with conventional high resolution frequency-domain spectroscopy. Applications of the intermediate-state control of the initial wave packet are discussed. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.470301
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  • 7
    Electronic Resource
    Electronic Resource
    Recombination and relaxation of molecular ions in size-selected clusters: Monte Carlo and molecular dynamics simulations of I−2 (CO2)n (1995)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 102 (1995), S. 2452-2470 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The equilibrium structures and the recombination dynamics of I−2 molecular ions embedded in clusters of 3–17 CO2 molecules are studied by Monte Carlo and molecular dynamics simulations. The potential model incorporates, in a self-consistent manner, a description of the I−2 electronic structure that depends on both the I−2 bond length and the solvent degrees of freedom. The influence of the solvent upon the I−2 electronic structure is treated by means of a single effective solvent coordinate, in a manner reminiscent of the theory of electron transfer reactions. This causes the electronic charge to localize on a single I atom when the I–I bond is long or when the solvent cage has become highly asymmetric. The primary focus is the I−2 vibrational relaxation that follows recombination. Simulations of I−2(CO2)16 and I−2(CO2)9 yield vibrational relaxation times of less than 3 ps, even faster than the experimentally observed absorption recovery time of 10–40 ps. It is suggested that the latter time scale is determined by electronic as well as vibrational relaxation mechanisms. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.468675
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  • 8
    Electronic Resource
    Electronic Resource
    Manipulation of rovibrational wave packet composition in the Li2 E(1Σg+) shelf state using intermediate state selection and shaped femtosecond laser pulses (1997)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 4172-4178 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The composition of a rovibrational wave packet in the E(1Σg+) state of Li2 is controlled using a combination of intermediate state selection and femtosecond optical pulse shaping techniques. Intermediate state selection is accomplished using a cw laser to prepare a steady state population of a single rovibrational level in the A(1Σu+) state of Li2, which acts as the initial state for subsequent ultrafast pump/probe studies in the "shelf" region of the E(1Σg+) state. An initial set of relative amplitudes of the wave packet eigenstates is defined by the intermediate level. Femtosecond optical pulse shaping, performed using a grating pair and a mechanical amplitude mask, is then used to further alter the wave packet composition. Quantitative changes in the Fourier transform of the pump/probe transient demonstrate that combining these two techniques can be a facile approach to manipulating wave packet composition, with the ultimate goal of controlling wave packet evolution into a desired final form. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.474141
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  • 9
    Electronic Resource
    Electronic Resource
    Compositional control of rovibrational wave packets in the E(1Σg+) "shelf" state of Li2 via quantum-state-resolved intermediate state selection (1997)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 106 (1997), S. 8310-8323 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Compositional control in the preparation of rovibrational wave packets is demonstrated in the E(1Σg+) state of gas-phase Li2 molecules using ultrafast pump–probe laser spectroscopy combined with quantum-state-resolved intermediate state selection. The intermediate state, from which subsequent ultrafast excitation occurs, is a stationary rovibrational level in the A(1Σu+) state of Li2, produced by cw laser excitation from the ground X(1Σg+) state. The effect that the intermediate state has on the final composition of the wave packet is investigated by comparing the transients resulting from ultrafast pump–probe excitation of two different intermediate states (vA=14, JA=18 versus vA=13, JA=18). In these experiments the pump wavelength is compensated so that in each case the same E-state eigenstates (vE=13–18, JE=JA±1) make up the wave packet, but with different amplitudes. Theory predicts, and experiments confirm, that the relative amplitudes of the rovibrational eigenstates are strongly dependent upon the intermediate state and determine the spatial and temporal evolution of the wave packet. Evidence for this includes differences in the observed pump–probe transients and dramatically different amplitudes of the beat frequencies in the Fourier analysis of the time-domain transients. Theoretical three-dimensional wave packet simulations highlight how the composition of the wave packet is used to vary its spatial and temporal evolution. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.473894
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  • 10
    Electronic Resource
    Electronic Resource
    Phase and amplitude control in the formation and detection of rotational wave packets in the E 1Σg+ state of Li2 (1998)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 108 (1998), S. 9259-9274 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Femtosecond laser pulse amplitude/phase masking techniques are employed to control the formation and detection of rotational wave packets in the electronic E 1Σg+ state of lithium dimer. The wave packets are prepared by coherent excitation of rovibronic E 1Σg+(νE,JE) states of Li2 from a single intermediate state, A 1Σu+(νA=11, JA=28), and probed by time-resolved photoionization. In the detection step, the wave packet is projected onto the X 2Σg+ state of Li2+. New resonance structure in the X 2Σu+ ionic state continuum is obtained by measuring the wave packet signal modulation amplitude as a function of the frequencies removed from the spectrally dispersed probe pulse by insertion of a wire mask in a single-grating pulse shaper. A split glass phase mask inserted into the pulse shaper is used to produce step function changes in the spectral phase of the pulse. The phase relation among the wave packet states is varied by changing the relative phases of spectral components in the pump pulse and is monitored by measuring the changes in the phase of the rotational wave packet recurrences using an unmodified probe pulse. By altering the relative phases among the wave packet components, the spatial distribution of the initial wave packet probability density is varied, resulting in phase-dependent "alignment" of the probability density in angular space. Phase changes in the signal recurrences are also observed when a phase modified pulse is used in the wave packet detection step after wave packet preparation with an unmodified pulse. The formation and detection of the wave packets is discussed in terms of quantum interference between different excitation routes. The relative phase factors encoded in a single optical pulse (pump or probe) are transferred into the interference term of the measured signal through the molecule–photon interaction. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.476381
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