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ABSTRACT: Competition between dissociation and ionization of H(2)(+) in intense laser field has been investigated by using an accurate three-dimensional time-dependent wavepacket approach. The disagreement between the experiment and the former one-dimensional theory has been resolved. In a comparison of the calculated results with the available experimental data, a good agreement is reached, not only for the relative probabilities between dissociation and ionization but also for the two-peak structures and the peak energy locations for these two processes.
The Journal of chemical physics 01/2012; 136(2):024311. · 3.09 Impact Factor
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ABSTRACT: The seams of conical intersection exist between the ground (1 (2)A(')) and the first-excited (2 (2)A(')) electronic potential energy surfaces (PESs) of OH(A (2)Σ(+),X (2)Π) + H(2) system. This intersection induces the nonadiabatic quenching of OH(A (2)Σ(+)) by D(2). We present nonadiabatic quantum dynamics study for OH(A (2)Σ(+)) + D(2) on new five-dimensional coplanar PESs. The ab initio calculations of PESs are based on multireference configuration interaction (MRCI)/aug-cc-pVQZ level. A back-propagation neural network is utilized to fit the PESs and nonadiabatic coupling. High degrees of rotational excitation of quenched OH(X (2)Π) products are found in nonreactive quenching channel, and the quenched D(2) products are vibrationally excited up to quantum number v(2) (')=8. The theoretical results of nonadiabatic time-dependent wave-packet calculation are in good agreement with the existing experimental data.
The Journal of chemical physics 11/2010; 133(17):174316. · 3.09 Impact Factor
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ABSTRACT: Nonadiabatic quantum scattering calculations have been carried out for the reactive and nonreactive quenching of OH(A(2)Sigma(+)) in collisions with molecular H(2) on two new potential energy surfaces of the 1A' and 2A' states. Integral cross sections of the reactive and nonreactive quenching channels and the quantum state distributions of the nonreactive channel have been obtained. The theory reveals a high degree of rotational excitation of the quenched OH(X(2)II) products and vibrational excitation of the H(2) products. The calculated results are in good agreement with the existing experimental data. The topography of the potential energy surfaces in the conical intersection regions is provided in order to discuss the origin of the internal excitations of nonreactive products and the branching of the reactive and nonreactive channels.
The Journal of Physical Chemistry A 06/2010; 114(24):6565-8. · 2.95 Impact Factor
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Angewandte Chemie International Edition 03/2010; 49(19):3330-3. · 13.45 Impact Factor
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ABSTRACT: We present a method of producing single attosecond pulses by using a few-cycle (5 fs) driving pulse with two additional weak control pulses. We discuss how single attosecond pulses produced from high-order harmonic generation processes in a synthesized three-colour laser field are similar to those processes in a much shorter single-colour laser field. Based on the high-order harmonic spectrum, classical ionizing and returning energy maps, time–frequency maps and time profiles of the attosecond pulses, the actions of the synthesized three-colour laser field are analogous to a 3 fs field although some differences still exist, and our method is proved to be a potential way to reduce the attosecond pulse duration from high-order harmonic generation with a currently available ultrafast laser source instead of a shorter pulse.
Journal of Physics B Atomic Molecular and Optical Physics 11/2009; 42(22):225601. · 1.88 Impact Factor
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ABSTRACT: We propose a method of generating an ultrabroad extreme ultraviolet continuum spectrum with a two-color scheme. By combining a phase-stabilized few-cycle laser pulse and its subharmonic laser, the electron quantum paths in the laser field are significantly modulated, a broadened continuum spectrum of 190 eV can be obtained, and an isolated 85 attosecond (as) pulse is generated. By increasing the intensity of the subharmonic controlling pulse, the continuum spectrum is extended effectively and a single 53 as pulse is predicted. © 2009 Wiley Periodicals, Inc. Int J Quantum Chem, 2009
International Journal of Quantum Chemistry 05/2009; 109(14):3410 - 3415. · 1.36 Impact Factor
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ABSTRACT: By the incorporation of N atoms into naphthalene, we present a theoretical investigation to seek for improved organic hydrogen carriers with an explicit guideline, the release of H2 is found to be greatly favored thermodynamically and the corresponding cycloalkanes possess high hydrogen storage capacity, this offers extensive candidates for practical applications of the promising hydrogen energy.
Chemical Communications 05/2009; · 6.17 Impact Factor
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ABSTRACT: A parallel quantum electron and nuclei wave packet computer code, LZH-DICP, has been developed to study laser-atom-molecule interaction in the nonperturbative regime with attosecond resolution. The nonlinear phenomena occurring in that regime can be studied with the code in a rigorous way by numerically solving the time-dependent Schrödinger equation of electrons and nuclei. Time propagation of the wave functions is performed using a split-operator approach, and based on a sine discrete variable representation. Photoelectron spectra for hydrogen and kinetic-energy spectra for molecular hydrogen ion in linearly polarized laser fields are calculated using a flux operator scheme, which testifies to the validity and the high efficiency of LZH-DICP.
Physical Review E 06/2008; 77(6 Pt 2):066701. · 2.26 Impact Factor
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ABSTRACT: Six new potential energy surfaces of four singlet states and two triplet states for the title oxygen molecule reaction along with the spin-orbit coupling among them have been constructed from the complete active space second-order perturbation theory with a 6-311+G(d) basis. Accurate integral cross sections are calculated with a full six-dimensional nonadiabatic time-dependent quantum wave packet method. The thermal rate constant based on the integral cross sections agrees well with the result of the experimental measurements, and the intersystem crossing effects are also discussed in this electronic energy-transfer process.
The Journal of Chemical Physics 04/2008; 128(9):091103. · 3.33 Impact Factor
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ABSTRACT: Five-dimensional nonadiabatic quantum dynamics studies have been carried out on two new potential energy surfaces of S(2)((1)A(')) and T(7)((3)A(")) states for the title oxygen molecules collision with coplanar configurations, along with the spin-orbit coupling between them. The ab initio calculations are based on complete active state second-order perturbation theory with the 6-31+G(d) basis set. The calculated spin-orbit induced transition probability as a function of collision energy is found to be very small for this energy pooling reaction. The rate constant obtained from a uniform J-shifting approach is compared with the existing theoretical and experimental data, and the spin-orbit effect is also discussed in this electronic energy-transfer process.
The Journal of Chemical Physics 04/2007; 126(12):124304. · 3.33 Impact Factor
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ABSTRACT: Five-dimensional nonadiabatic quantum dynamics studies have been carried out on two new potential energy surfaces of S2(1A′) and T7(3A″) states for the title oxygen molecules collision with coplanar configurations, along with the spin-orbit coupling between them. The ab initio calculations are based on complete active state second-order perturbation theory with the 6‐31+G(d) basis set. The calculated spin-orbit induced transition probability as a function of collision energy is found to be very small for this energy pooling reaction. The rate constant obtained from a uniform J-shifting approach is compared with the existing theoretical and experimental data, and the spin-orbit effect is also discussed in this electronic energy-transfer process.
The Journal of Chemical Physics 03/2007; 126(12):124304-124304-5. · 3.33 Impact Factor
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ABSTRACT: The state-to-state dynamics of the H+D2 reaction is studied by the reactant-product decoupling method using the double many-body expansion potential energy surface. Two approaches are compared: one uses only the lowest adiabatic sheet while the other employs both coupled diabatic sheets. Rotational distributions for the reaction H+D2 (upsilon = 0, j = 0)-->HD(upsilon' = 3, j')+D are obtained at eight different collision energies between 1.49 and 1.85 eV; no significant difference are found between the two approaches. Initial state-selected total reaction probabilities and integral cross sections are also given for energies ranging from 0.25 up to 2.0 eV with extremely small differences being observed between the two sets of results, thus showing that the nonadiabatic effects in the title reaction are negligible at least for small energies below 2.0 eV.
The Journal of Chemical Physics 10/2006; 125(13):133108. · 3.33 Impact Factor
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ABSTRACT: The exact three-dimensional nonadiabatic quantum dynamics calculations were carried out for the title reaction by a time-dependent wave packet approach based on a newly constructed diabatic potential energy surface (Kamisaka et al. J. Chem. Phys. 2002, 116, 654). Three processes including those of reactive charge transfer, nonreactive charge transfer, and reactive noncharge transfer were investigated to determine the initial state-resolved probabilities and reactive cross sections. The results show that a large number of resonances can be observed in the calculated probabilities due to the deep well on adiabatic ground surface and the dominant process is the reactive noncharge-transfer process. Some interesting dynamical features such as v-dependent and j-dependent behaviors of the probabilities are also revealed. In addition, a good agreement has been achieved in the comparison between the calculated quantum cross sections from the ground rovibrational initial state and the experimental measurement data.
The Journal of Physical Chemistry A 09/2005; 109(30):6683-8. · 2.95 Impact Factor
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ABSTRACT: The quantum scattering dynamics calculation was carried out for the titled reaction in the collision energy range of 0.0-2.4 eV with reactant H(2) (+) in the rotational state j = 1 and vibrational states v = 0-2, 4, and 6. The present time-dependent wave-packet calculation takes into account the Coriolis coupling (CC) and uses the accurate ab initio potential-energy surface of Palmieri et al. [Mol. Phys. 98, 1835 (2000)]. The importance of including the CC quantum scattering calculation has been revealed by the comparison between the CC calculation and the previous coupled state (CS) calculation. The CC total cross sections for the v = 2, 4, and 6 states show collision energy-dependent behaviors different from those based on the CS calculation. Furthermore, the collision energy dependence of the total cross sections obtained in the present CC calculation only exhibits minor oscillations, indicating that the chance is slim for reactive resonances in total cross sections to survive through the partial-wave averaging. The magnitude and profile of the CC total cross sections for v = 0-2 in the collision energy range of 0.0-2.5 eV are found to be consistent with experimental cross sections obtained recently by Tang et al. [J. Chem. Phys. 122, 164301 (2005)] after taking into account the experimental uncertainties.
The Journal of Chemical Physics 07/2005; 122(24):244322. · 3.33 Impact Factor
