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  • 1
    Electronic Resource
    Electronic Resource
    Structure of tetraphenylarsonium bis(N-cyanodithiocarbimato)nickelate(II) (1968)
    s.l. : American Chemical Society
    Inorganic chemistry 7 (1968), S. 2140-2144 
    Details
    ISSN: 1520-510X
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/ic50068a038
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    Paper (German National Licenses)
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  • 2
    Electronic Resource
    Electronic Resource
    Torsional dynamics of molecules on barrierless potentials in liquids. I. Temperature and wavelength dependent picosecond studies of triphenyl-methane dyes (1987)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 86 (1987), S. 4856-4870 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The nonradiative decay dynamics of crystal violet, and other triphenyl-methane dyes, dissolved in a variety of solvents, are studied as a function of temperature. A linear viscosity dependence of the excited state absorption decay time in n-alcohol solvents is found at several constant temperatures. The temperature dependence at constant viscosity is anomalously negative over the entire viscosity range (0.6 to 8.0 cP) of these experiments. Various possible mechanisms for the observed behavior are critically discussed. Two color excite-and-probe studies reveal ground state bleach recovery times which are independent of excitation wavelength but strongly dependent on probe wavelength. The faster decay on the red side of the ground state absorption is shown to be the result of stimulated emission rather than the influence of a second state.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.452656
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  • 3
    Electronic Resource
    Electronic Resource
    Torsional dynamics of molecules on barrierless potentials in liquids. III. Pressure dependent picosecond studies of triphenyl-methane dye solutions in a diamond anvil cell (1987)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 86 (1987), S. 6119-6127 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Pressure dependent measurements of the nonradiative torsional dynamics of triphenyl-methane dyes are reported. The viscosity dependence of the excited state absorption and fluorescence decays of crystal violet, dissolved in methanol, ethanol, and n-propanol, are studied over a viscosity range of between 0.5 and 500 cP (pressures up to 1.5 GPa ∼15 000 atm). The overall viscosity dependence of the excited state decay time is linear. The nonlinear viscosity dependencies observed in earlier studies may have resulted from the complex nature of the solvents used and, in the case of fluorescence quantum yield measurements, from a pressure dependence of the radiative rate. Differences between the viscosity dependence observed when varying pressure, temperature, or solvent type at low viscosities are tentatively ascribed to pressure and temperature induced conformational changes.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.452451
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  • 4
    Electronic Resource
    Electronic Resource
    Torsional dynamics of molecules on barrierless potentials in liquids. II. Test of theoretical models (1987)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 86 (1987), S. 5433-5440 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The theoretical predictions of three theories for large amplitude dynamics on a barrierless excited state potential are tested. The predicted forms for the time dependent integrated excited state population are compared with experimentally measured excited state absorption decays of crystal violet in various solvents. We have generalized the early theory of Oster–Nishijima [J. Am. Chem. Soc. 78, 1581 (1956)] to allow for arbitrary placement of the initial excited state population relative of the nonradiative sinks which couple the flat excited state potential to the ground state. An analytic form for decay of the integrated excited state population is derived for this generalized flat potential model. In addition we have found that the predictions of Forster–Hoffmann [Z. Phys. Chem. NF 75, 63 (1971)] cannot be made to fit the experimentally measured excited state decays of crystal violet. Finally we show that the theory of Bagchi–Fleming–Oxtoby [J. Chem. Phys. 78, 7375 (1983)] can fit the decays observed in various solvents fairly well. The best fits, however, are obtained using the generalized flat potential model.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.452567
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  • 5
    Electronic Resource
    Electronic Resource
    Electronic energy transfer at semiconductor interfaces. I. Energy transfer from two-dimensional molecular films to Si(111) (1987)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 86 (1987), S. 6540-6549 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The fluorescence decays from submonolayers of pyrene separated from Si(111) by Xe spacer layers are measured as a function of spacer thickness (17–200 A(ring)), pyrene coverage, and emission wavelength. The results are explained in terms of two decay channels: energy transfer and trapping among the molecules in the two-dimensional pyrene overlayer, and excitation of electrons from the valence to the conduction band in the Si(111) by the dipole near field of the electronically excited pyrene molecule. The intralayer energy transfer is modeled using the Kohlrausch equation N(t)=N0 exp(−t/τ)α, in which α is related to the distribution of pyrene molecules in energy. Energy transfer from the molecule to the semiconductor is modeled using the classical image dipole theory. The classical model is used to calculate the energy transfer rates from a dipole to Si and GaAs as a function of dipole–semiconductor separation, and as a function of dipole emission wavelength.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.452396
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  • 6
    Electronic Resource
    Electronic Resource
    Studies of chemical reactivity in the condensed phase. II. Vibrational relaxation of iodine in liquid xenon following geminate recombination (1986)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 85 (1986), S. 3699-3700 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The geminate recombination of iodine atoms in xenon solutions, has been studied by monitoring the transient absorptions at wavelengths between 350 and 1000 nm.(AIP) ;m
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.450938
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  • 7
    Electronic Resource
    Electronic Resource
    Studies of chemical reactivity in the condensed phase. I. The dynamics of iodine photodissociation and recombination on a picosecond time scale and comparison to theories for chemical reactions in solution (1986)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 84 (1986), S. 788-806 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Picosecond transient absorption measurements from 1000–295 nm are used to monitor the recombination dynamics of iodine after photodissociation in a variety of inert solvents. The high time resolution and signal-to-noise ratio of these measurements permits the development of a detailed model of this reaction, which should resolve disagreements over the time scales of geminate recombination and vibrational relaxation and over the role of excited electronic state trapping. Most of the atoms which undergo geminate recombination do so in ≤15 ps, in agreement with the predictions of existing molecular dynamics simulations. The subsequent vibrational and electronic energy relaxation of the recombined molecule is relatively slow and accounts for most of the transient absorption dynamics. The relaxing X-state vibrational population distribution is extracted with an approximate method using calculated spectra of the excited vibrational levels and is compared to recent models. Vibrational relaxation times vary from ∼15 ps near the middle of the ground state well to ∼150 ps for complete relaxation to v=0. The vibrational relaxation rates do not provide support for the predicted role of resonant vibration-to-vibration energy transfer to chlorinated methane solvents, but some evidence for this mechanism is found in alkane solvents. B-state predissociation times of 10–15 ps and A'-state lifetimes of 65–2700 ps are found depending on the solvent. Current theory is not able to satisfactorily explain the large variation of the A'-state lifetime in various solvents.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.450578
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  • 8
    Electronic Resource
    Electronic Resource
    Photodissociation dynamics of Mn2(CO)10 in solution on ultrafast time scales (1991)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 95 (1991), S. 4024-4032 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A study of the photodissociation dynamics of Mn2(CO)10 and the vibrational relaxation of its subsequent photoproducts in solutions has been carried out using picosecond time-resolved laser techniques. The molecule predissociates in less than 2–3 ps after excitation with a 295 nm photon. Two dissociation channels are open for this excitation wavelength, namely, the Mn–Mn bond breaking and the Mn–CO bond breaking, generating internally hot ⋅Mn(CO)5 and Mn2(CO)9, respectively. These two species have a different absorption spectrum in the visible region and are probed independently by varying the probe laser wavelength. The vibrational relaxation of these nascent photoproducts is observed for the first time. In cyclohexane the vibrationally hot Mn2(CO)9 reaches thermal equilibrium with the solvent through two distinct decay channels with time constants of 15 and 170 ps, respectively. The vibrationally cold Mn2(CO)9 then persists for many nanoseconds. The vibrational relaxation is found to be faster in the 2-propanol solution with time constants of 10 and 145 ps. On the other hand, the ⋅Mn(CO)5 species cools down in less than 10 ps and then exists in the solution for many nanoseconds as well. This result indicates that energy transfer from the internally hot ⋅Mn(CO)5 species to the solvent is much faster than from Mn2(CO)9. Comparison is made with Cr(CO)5 in similar solvents.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.460757
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  • 9
    Electronic Resource
    Electronic Resource
    Generalized Brownian dynamics. I. Numerical integration of the generalized Langevin equation through autoregressive modeling of the memory function (1990)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 92 (1990), S. 1304-1311 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A method is presented for numerical integration of the generalized Langevin equation (GLE) based on modeling of the "random force'' as a discrete autoregressive process. This modeling procedure, drawn from digital signal processing and spectral estimation methods which have been used extensively in electrical engineering applications, provides for efficient evaluation of the friction integral in the GLE as well as for generation of a random force process with the desired spectrum. The method is shown, through comparison with molecular dynamics results, to be effective in simulating the force autocorrelation function of an iodine atom dissolved in Lennard-Jones (LJ) xenon. In a companion paper this method is applied in a simulation of the vibrational relaxation of I2 in LJ xenon at two very different densities and found to perform well.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.458140
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  • 10
    Electronic Resource
    Electronic Resource
    Generalized Brownian dynamics. II. Vibrational relaxation of diatomic molecules in solution (1990)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 92 (1990), S. 1312-1319 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A simple classical stochastic model for diatomic vibrational relaxation, based on the generalized Langevin equation, is presented. The memory function in the generalized Langevin equation is determined directly from equilibrium force autocorrelation functions for the individual atoms of the diatomic dissolved in the solvent of interest. A simple autoregressive (AR) procedure, developed in a preceding paper [D. E. Smith and C. B. Harris, J. Chem. Phys. 92, xxx (1990)], is used for modeling the memory functions to arbitrary order. This model is tested on the system of iodine in Lennard–Jones xenon using fourth order AR approximations for the memory functions, and is found to be very effective in reproducing data from molecular dynamics simulations at two very different densities. Results are discussed in terms of the simplifying assumption that the solvent interaction with the diatomic can be characterized by equilibrium dynamics of single atoms in solution.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.458141
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