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  • Articles  (72)
  • American Institute of Physics (AIP)  (34)
  • American Geophysical Union  (14)
  • Institute of Physics (IOP)  (10)
  • Oxford University Press  (9)
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  • Articles  (72)
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  • 11
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 5460-5472 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: An intuitive picture of Λ-doubling in diatomic molecules is presented using a semiclassical theory. A common view of Λ-doubling as arising from electrons "lagging" behind the rotating internuclear axis is shown to be misleading; rather, the eigenfunctions are symmetric about the molecular axes and can be expressed as a superposition of pure nonrotating orbitals and travelling waves. These results are shown to be consistent with a full quantum treatment. We also examine, for the first time, time-dependent states, by monitoring expectation values of electronic- and nuclear-angular momenta. For low rotation frequency, the expectation value of the electronic-angular momentum locks onto the rotating internuclear axis, while for high rotation frequency it locks onto the space-fixed total-angular momentum axis. At intermediate frequencies is a complicated behavior. © 1997 American Institute of Physics.
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  • 12
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 5473-5487 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We investigate collision-induced Λ-doublet transitions in a system similar to NO+Ar, based on a semiclassical model in which nuclear motion is treated classically and electronic motion quantum mechanically. We present a picture of this process by monitoring 〈Λ〉, the expectation value of the projection of electronic orbital-angular momentum onto the molecular NO axis, over the duration of the collision. In a typical collision, the interaction with Ar would cause the electronic orbital-angular momentum to precess about the rotating NO–Ar vector. However, since this angular momentum is locked tightly to the diatomic axis, it is restricted to oscillation along this axis. This oscillation leads to transitions between Λ-doublet states. In addition to providing this physical picture of the collision process, we calculate an alignment effect of 1.2 for a hypothetical three-vector correlation experiment, neglecting spin. © 1997 American Institute of Physics.
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  • 13
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 106 (1997), S. 3504-3511 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Transient absorption and gain spectra of the styryl dye LDS-750 in solution have been studied by the pump/supercontinuum probe (PSCP) technique with excitation at 530 nm. The pump/probe intensity correlation width was 70 fs, providing a time resolution of 40 fs. Spectra were detected in the range 400–800 nm with 1.5 nm resolution. Before 70 fs, prominent spectral structure is observed due to resonant Raman scattering from a 1500 cm−1 active mode of the chromophore. At later time, the gain spectrum undergoes an ultrafast redshift and change of shape, with time constants of ∼200 and ∼600 fs for acetonitrile and chloroform solutions, respectively. At high pumping energy (1.2 μJ), the final emitting state is reached by internal conversion from higher electronic states without a further essential Stokes shift. The emitting state is assigned to an excited isomeric form of the molecule. At low pumping energy (0.3 μJ), the first excited electronic state isomerizes in an ultrafast process followed by a slower process, the dynamics of which is controlled by the solvent. The geometrical and electronic nature of these processes and their coupling to the solvent needs further clarification. © 1997 American Institute of Physics.
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  • 14
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 9463-9468 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We have developed a three-dimensional (3D) extension of the reference interaction site model-self-consistent field (RISM-SCF) method to treat the electronic structure of a solvated molecule. The site–site treatment of the solute–solvent correlations involving the approximation of radial averaging constitutes a bottleneck of the RISM-SCF method, and thus lacks a 3D picture of the solvation structure for complex solutes. To resolve this problem, we devised out a 3D generalization of the RISM integral equations which yields the 3D correlation functions of interaction sites of solvent molecules around a solute of arbitrary shape. In the present article, we propose a SCF combination of the ab initio molecular orbital (MO) methods and 3D-RISM approach. A benchmark result for carbon monoxide in ambient water is also presented. © 2000 American Institute of Physics.
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  • 15
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 109 (1998), S. 5466-5468 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Transient absorption measurements of aminonitrofluorene in acetonitrile reveal for the first time an oscillatory behavior in the dynamic Stokes shift of stimulated emission. The measured relaxation curve for the maximum of the stimulated emission band is in excellent agreement with the solvation correlation function C(t) obtained from the simple continuum theory of dipolar solvation. © 1998 American Institute of Physics.
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  • 16
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Review of Scientific Instruments 67 (1996), S. 1161-1161 
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: The design of the electron-beam ion source (EBIS) "Krion-S'' on the high voltage (HV) platform of the preinjector of the LINAC LU-20 and some results of accelerating argon and krypton ions up to 5 Mev/u are presented. The gas mixing (working gas and Ne) by original technology has been used for the "ion cooling'' procedure. The cryogenic ionizator Krion-S is used as an ion source for multicharged ions with mass charge ratio band 0.35–0.5 at the accelerating facility "NUCLOTRON'' of the Laboratory of High Energies (LNE) JINR in Dubna. © 1996 American Institute of Physics.
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  • 17
    ISSN: 1089-7623
    Source: AIP Digital Archive
    Topics: Physics , Electrical Engineering, Measurement and Control Technology
    Notes: The design of "KRION-C'' with an energy of up to 80 keV and preliminary results on the ionization of sulfur and argon ions are presented. The cryogenic electron beam ionizer "KRION-C'' was used as an ion source for the first run with sulfur relativistic nuclei at the accelerating facility of the Laboratory of High Energies (LHE) in Dubna.
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  • 18
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 115 (2001), S. 8620-8633 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We develop a replica generalization of the reference interaction site model (replica RISM) integral equation theory to describe the structure and thermodynamics of quenched-annealed systems comprising polar molecular species. It provides a successful approach to realistic models of molecular liquids, and properly allows for the effect of a quenched disordered matrix on the sorbed liquid. The description can be extended to an electrolyte solution in a disordered material containing charged chemical functionalities that determine its adsorption character. The replica reference interaction site model (RISM) equations are complemented with the hypernetted chain (HNC) closure and its partial linearization (PLHNC), adequate to ionic and polar molecular liquids. In these approximations, the excess chemical potentials are derived in a closed analytical form. We extend the description to a quenched-annealed system with soft-core interaction potentials between all species, in which the liquid and matrix equilibrium distributions are characterized in general by two different temperatures. The replica RISM/PLHNC-HNC theory is applied to water sorbed in a quenched disordered microporous network of atoms associated into interconnected branched chains, with activating polar groups grafted to matrix chains. The results are in qualitative agreement with experiment for water confined in disordered materials. © 2001 American Institute of Physics.
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  • 19
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 115 (2001), S. 3256-3273 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The cooling of p-nitroaniline (PNA), dimethylamino-p-nitroaniline (DPNA) and trans-stilbene (t-stilbene) in solution is studied experimentally and theoretically. Using the pump–supercontinuum probe (PSCP) technique we observed the complete spectral evolution of hot absorption induced by femtosecond optical pumping. In t-stilbene the hot S1 state results from Sn→S1 internal conversion with 50 fs characteristic time. The time constant of intramolecular thermalization or intramolecular vibrational redistribution (IVR) in S1 is estimated as τIVR(very-much-less-than)100 fs. In PNA and DPNA the hot ground state is prepared by S1→S0 relaxation with characteristic time 0.3–1.0 ps. The initial molecular temperature is 1300 K for PNA and 860 K for t-stilbene. The subsequent cooling dynamics (vibrational cooling) is deduced from the transient spectra by assuming: (i) a Gaussian shape for the hot absorption band, (ii) a linear dependence of its peak frequency νm and width square Γ2 on molecular temperature T. Within this framework we derive analytic expressions for the differential absorption signal ΔOD(T(t),ν). After calibration with stationary absorption spectra in a low temperature range, the solute temperature T(t) may be evaluated from a transient absorption experiment. For highly polar PNA and DPNA, T(t) is well described by a biexponential decay which reflects local heating effects, while for nonpolar t-stilbene the local heating is negligible and the cooling proceeds monoexponentially. To rationalize this behavior, an analytic model is developed, which considers energy flow from the hot solute to a first solvent shell and then to the bulk solvent. Fastest cooling is found for PNA in water: a time constant of 0.64 ps (68%) corresponds to solute–solvent energy transfer while 2.0 ps (32%) characterizes the cooling of the first shell. In aprotic solvents cooling is slower than in alcohols and slows down further with decreasing solvent polarity. This contrasts with nonpolar t-stilbene which cools down with 8.5 ps both in acetonitrile and cyclohexane. Comparison of the cooling kinetics for PNA in water with those for DPNA in water-acetonitrile mixtures suggests that the solute–solvent energy transfer proceeds mainly through hydrogen bonds. © 2001 American Institute of Physics.
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  • 20
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Physics of Plasmas 6 (1999), S. 335-342 
    ISSN: 1089-7674
    Source: AIP Digital Archive
    Topics: Physics
    Notes: Nonlinear evolution of one-dimensional planar perturbations in an optically thin, radiatively cooling medium in the long-wavelength limit is studied numerically. The accepted cooling function generates, in thermal equilibrium, a bistable equation of state P(ρ). The unperturbed state is taken close to the upper (low-density) unstable state with infinite compressibility (dP/dρ=0). The evolution is shown to proceed in three different stages. At the first stage, pressure and density set in the equilibrium equation of state, and velocity profile steepens gradually, as in the case of pressure-free flows. At the second stage, those regions of the flow where anomalous pressure (i.e., with negative compressibility) holds create a velocity profile sharper than in the pressure-free case, which in turn results in formation of a very narrow (short-wavelength) region where gas separates the equilibrium equation of state and pressure equilibrium sets in rapidly. At this stage, the variation in pressure between the narrow dense region and the extended environment does not exceed more than 0.01 of the unperturbed value. At the third stage, gas in the short-wavelength region reaches the second (high-density) stable state, and pressure balance establishes through the flow, with pressure equal to the one in the unperturbed state. In external (long-wavelength) regions, gas forms slow isobaric inflow toward the short-wavelength layer. The duration of these stages decreases when the ratio of the acoustic time to the radiative cooling time increases. The limits in which nonlinear evolution of thermally unstable long-wavelength perturbations develops in isobaric regime are obtained. © 1999 American Institute of Physics.
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