A typical slow reaction H（2S） ＋ S2（X3∑g） → SH（X2П） ＋S（3P） ona new surface： Quantum dynamics calculations

Quantum dynamics calculations for the title reaction H(2S) + S2(X3-Σg) → SH(X2Π) + S(3P) are performed by using a globally accurate double many-body expansion potential energy surface [J. Phys. Chem. A 115 5274(2011)].The Chebyshev real wave packet propagation method is employed to obtain the dynamical information, such as reaction probability, initial state-specified integral cross section, and thermal rate constant. It is found not only that there is a reaction threshold near 0.7 eV in both reaction probabilities and integral cross section curves, but also that both the probability and cross section increase firstly and then decrease as the collision energy increases. The existence of the resonance structure in both the probability and cross section curves is ascribed to the deep potential well. The calculation of the rate constant reveals that the reaction occurring on the potential energy surface of the ground-state HS2is slow to take place.     

Quantum State-Resolved Nonadiabatic Dynamics of the H+NaF→Na+HF Reaction

<正>The H+NaF reaction is investigated at the quantum state-resolved level using the time-dependent wavepacket method based on a set of accurate diabatic potential energy surfaces. Oscillatory structures in the total reaction probability indicate the presence of the short-lived intermediate complex,     

Study of the H＋HS reaction on a newly built potential energy surface using the quasi-classical trajectory method

<正>The quasi-classical trajectory（QCT） method is used to study the H+HS reaction on a newly built potential energy surface（PES） of the triplet state of H₂S（³A″） in a collision energy range of 0-60 kcal/mol.Both scalar properties, such as the reaction probability and the integral cross section（ICS）,and the vector properties,such as the angular distribution between the relative velocity vector of the reactant and that of the product,etc.,are investigated using the QCT method.It is found that the ICSs obtained by the QCT method and the quantum mechanical（QM） method accord well with each other.In addition,the distribution for the product vibrational states is cold,while that for the product rotational states is hot for both reaction channels in the whole energy range studied here.     

Stereodynamics study of the exchange reaction O(~3P)+CH_4 →H+OCH_3

A new London-Eyring-Polanyi-Sato potential energy surface is employed in this work to study the stereo properties of the O(3P)+CH4 →H+CH3O reaction in its rovibrationally ground state using the quasiclassical trajectory method(QCT).Our calculations are performed at a range of collision energies,Ec=1.5eV～3.5eV,and the excitation function obtained by the QCT method accords well with the experimental data.The product rotational polarization is calculated,and the product shows a strong rotational polarization in the centre-of-mass coordinate system.The orientation of the product rotational angular momenta is sensitive to the increase in collision energy,and the alignment of the product rotational angular momenta shows some of the properties of the heavy heavy-light mass combination reactions.In the isotopic substituted reaction study,when the H atoms in methane are replaced by D atoms,the rotational polarization is obviously reduced.The polarization-dependent differential cross section is also studied by this QCT calculation to provide detailed information about the rotational alignment and orientation of the product.     

Intermolecular Interaction Potentials of CH4-Ne Complex Calculated with Local Density Approximation Methods

The intermolecular interactions potentials for two configurations of CH4-Ne complex are calculated with localdensity approximation methods in the frame of density functional theory. It is found that the calculated potentialshave two minima when the distance between the carbon atom of CH4 and the Ne atom takes R = 5.80a.u.and 6.20a.u. for both the two configurations. For the edge configuration, the corresponding depth of thepotential is 0.0669536eV and 0.0671416eV. For the face configuration, the corresponding depth of the potentialis 0,0737956 eV and 0.0645506 eV. The global minimum occurs at R = 5.80 a.u. for the face configuration with adepth of the potential 0.0737956eV. The depths of our calculation are in better agreement with the experimentaldata than the quantum chemical calculation approach~ while the position of minimum potential for our calculationis underestimated.     

Magnetization relaxation of uniaxial anisotropic ferromagnetic particles with linear reaction dynamics driven by DC/AC magnetic field

The response of uniaxial anisotropic ferromagnetic particles with linear reaction dynamics subjected to alternating current(AC) or direct current(DC) bias magnetic field is evaluated by the reaction–diffusion equation for the probability distribution function of the molecular concentration in the spherical coordinate system. The magnetization function and the probability distribution function of the magnetic particles in the reaction system are derived by using the Legendre polynomials and Laplace transform. We discuss the characteristics of magnetization and probability distribution of the magnetic particles with different anisotropic parameters driven by a DC and AC magnetic fields, respectively. It is shown that both the magnetization and the probability distribution decrease with time increasing due to the reaction process. The uniformity of the probability distribution and the amplitude of the magnetization are both affected by the anisotropic parameters.Meanwhile, the difference between the case with linear reaction dynamics and the non-reaction case is discussed.     

Cross Section of Heavy Ion Reaction （14.5 MeV/u） ^132Xe ＋ Bi

We investigate the cross section of the heavy ion reaction （14.5 MeV/u） ^132Xe ＋ Bi by using a CR-39 plastic track detector. The target-detector assembly is exposed at UNILAC beam facility of GSI, Germany. After etching under appropriate etching conditions, the detector is scanned for multipronged events produced as a result of interactions of projectile ions with target atoms. The elastic events are separated from binary events and used for the determination of the quarter-point angle. The quarter-point angle obtained is used to determine the total reaction cross section. The total experimental reaction cross section is determined by using statistics of inelastic events of two-pronged and higher multiplicity events. The experimental reaction cross sections determined by using elastic and inelastic data observed in the reaction under study are found to be in good agreement with the theoretically calculated value of reaction cross section using a sharp cutoff model.     

A CLASSICAL TRAJECTORY STUDY BASED ON MBE POTENTIAL ENERGY FUNCTIONS—REACTIVE COLLISIONS OF C＋CH

Classical trajectories have been calculated for the reaction C CH→C2 H using many-body expansion(MBE) potential energy function of C2H.The present work gives the reactive cross sections at relative kinetic energy of 1.0,7.5,13.0,20.0and 30.0 kcal,From which it is found that this is a reaction without energy thres-hold.     

Optical planar waveguides in yb3＋-doped phosphate glasses produced by He＋ ion implantation

Optical planar waveguides in Yb 3+-doped phosphate glasses are fabricated by implanting triple-energy helium ions. The guiding modes and the near-field intensity distribution are measured by using the prism-coupling method and the end-face coupling setup with a He-Ne laser at 633 nm The intensity calculation method (ICM) is used to reconstruct the refractive index profile of the waveguide. The absorption and the fluorescence investigations reveal that the glass bulk features are well preserved in the active volumes of the waveguides, suggesting the fabricated structures for possible applications as waveguide lasers.     

Influence of D-state in 4He on S Factor for the 2H（d, γ）^4He Reaction

We employ a direct capture method to study the influence of D-state in ^4He on S factor for the ^2H（d,γ）^4He reaction, in which the D-state component of the colliding deuterons and D-state component in ^4He ground state are considered. The parameters of Woods-Saxon （WS） potentials are obtained by reproducing the binding energy of d-d （i.e. ^2H-^2H） system, and d-d elastic scattering phase shifts calculated by the resonating group method. The theoretical results are in good agreement with the experimental data at Ec.m〈 3 MeV. The impact of the D state probability in ^4He on the extrapolated value of the astrophysical S factor for ^2H（d, γ）^4He reaction is discussed.     

Energy diffusion controlled reaction rate in dissipative Hamiltonian systems

In this paper the energy diffusion controlled reaction rate in dissipative Hamiltonian systems is investigated by using the stochastic averaging method for quasi Hamiltonian systems. The boundary value problem of mean first-passage time (MFPT) of averaged system is formulated and the energy diffusion controlled reaction rate is obtained as the inverse of MFPT. The energy diffusion controlled reaction rate in the classical Kramers bistable potential and in a two-dimensional bistable potential with a heat bath are obtained by using the proposed approach respectively. The obtained results are then compared with those from Monte Carlo simulation of original systems and from the classical Kramers theory. It is shown that the reaction rate obtained by using the proposed approach agrees well with that from Monte Carlo simulation and is more accurate than the classical Kramers rate.     

Enhanced Quantum Reflection of Ultracold Atoms with Strong Interatomic Interaction

We calculate the reflection probability for ultracold alkali atoms incident on a solid surface. By considering the interatomic interaction and using the WKB method, it is shown that the repulsive interaction between atoms has the effect of increasing the reflection probability. The increasing amplitude is related with the interatomic interaction and the depth of atom-surface potential. In addition, we also perform a numerical calculation to testify the effect of the interatomic interaction, and the analytic result is proven by the numerical result.     

Bidirectional reflectance distribution function modeling of one-dimensional rough surface in the microwave band

In this study, the bidirectional reflectance distribution function(BRDF) of a one-dimensional conducting rough surface and a dielectric rough surface are calculated with different frequencies and roughness values in the microwave band by using the method of moments, and the relationship between the bistatic scattering coefficient and the BRDF of a rough surface is expressed. From the theory of the parameters of the rough surface BRDF, the parameters of the BRDF are obtained using a genetic algorithm. The BRDF of a rough surface is calculated using the obtained parameter values. Further, the fitting values and theoretical calculations of the BRDF are compared, and the optimization results are in agreement with the theoretical calculation results. Finally, a reference for BRDF modeling of a Gaussian rough surface in the microwave band is provided by the proposed method.     

Bidirectional reflectance one-dimensional rough distribution function modeling of surface in the microwave band

In this study, the bidirectional reflectance distribution function （BRDF） of a one-dimensional conducting rough surface and a dielectric rough surface are calculated with different frequencies and roughness values in the microwave band by using the method of moments, and the relationship between the bistatic scattering coefficient and the BRDF of a rough surface is expressed. From the theory of the parameters of the rough surface BRDF, the parameters of the BRDF are obtained using a genetic algorithm. The BRDF of a rough surface is calculated using the obtained parameter values. Further, the fitting values and theoretical calculations of the BRDF are compared, and the optimization results are in agreement with the theoretical calculation results. Finally, a reference for BRDF modeling of a Gaussian rough surface in the microwave band is provided by the proposed method.     

Time-dependent quantum dynamics study for reaction of D+CH4→CH3+HD

The semirigid vibrating rotor target (SVRT) model has been applied to the study of the reaction of D+CH_4→CH_3+HD using a time-dependent wave packet method. The energy dependence of the calculated reaction probability shows oscillatory structures similar to those observed in the abstraction reaction of H+H_2, H+CH_4 etc. We have also studied the influence of rotational and vibrational excitation of the reacting molecule (CH_4) on reaction probability. The excitation of the H－CH_3 stretching vibration gives significant enhancement of reaction probability, which rises significantly with the enhancement of rotational quantum number j. Finally, we have compared the cross section and the rate constant of the D+CH_4 system with that of the H+CH_4 system.     

Stereodynamics in reaction O（1D） ＋ CH4 〉OH ＋ CH3

A theoretical study of the stereodynamics for reaction O(1D) + CH4→OH + CH3 has been carried out using the quasiclassical trajectory method(QCT) on a potential energy surface structured by Gonzalez et al. The integral cross sections(ICSs), differential cross sections(DCSs) and product rotational angular momentum polarization have been calculated. With the collision energy increasing, the ICS decreases. There is no threshold energy, because no barrier is found on the minimum energy path. The DCS results show that the backward and forward scatterings exist at the same time. With the collision energy increasing, the dominant rotation of the product changes from the right-handed direction to the left-handed direction in planes parallel to the scattering plane. In the isotopic effect study, the decrease of the mass factor weakens the polarization degree of the rotational angular momentum vectors of the products.     

Mechanism analysis of reaction S~+(~2D)+H_2(X~1Σ_g~+) → SH~+(X~3Σ~-) + H(~2S) based on the quantum state-to-state dynamics

We present a state-to-state dynamical calculation on the reaction S~++ H_2→ SH~+ +H based on an accurate ~X2 A~″ potential surface. Some reaction properties, such as reaction probability, integral cross sections, product distribution, etc.,are found to be those with characteristics of an indirect reaction. The oscillating structures appearing in reaction probability versus collision energy are considered to be the consequence of the deep potential well in the reaction. The comparison of the present total integral cross sections with the previous quasi-classical trajectory results shows that the quantum effect is more important at low collision energies. In addition, the quantum number inversion in the rotational distribution of the product is regarded as the result of the heavy–light–light mass combination, which is not effective for the vibrational excitation. For the collision energies considered, the product differential cross sections of the title reaction are mainly concentrated in the forward and backward regions, which suggests that there is a long-life intermediate complex in the reaction process.     

丙烷与O(3P)反应机理和动力学的理论研究

The reaction of C₃H₈+O(³P)→C₃H₇+OH is investigated using ab initio calculation and dynamical methods. Electronic structure calculations for all stationary points are obtained using a dual-level strategy. The geometry optimization is performed using the unrestricted second-order Møller-Plesset perturbation method and the single-point energy is computed using the coupled-cluster singles and doubles augmented by a perturbative treatment of triple excitations method. Results indicate that the main reaction channel is C₃H₈+O(³P)→i-C₃H₇+OH. Based upon the ab initio data, thermal rate constants are calculated using the variational transition state theory method with the temperature ranging from 298 K to 1000 K. These calculated rate constants are in better agreement with experiments than those reported in previous theoretical studies, and the branching ratios of the reaction are also calculated in the present work. Furthermore, the isotope effects of the title reaction are calculated and discussed. The present work reveals the reaction mechanism of hydrogen-abstraction from propane involving reaction channel competitions is helpful for the under-standing of propane combustion.     

A full-dimensional analytical potential energy surface for the F+CH_4→HF+CH_3 reaction

A full-dimensional analytical potential energy surface(APES) for the F + CH4 →HF + CH3 reaction is developed based on 7127 ab initio energy points at the unrestricted coupled-cluster with single,double,and perturbative triple excitations.The correlation-consistent polarized triple-split valence basis set is used.The APES is represented with a many-body expansion containing 239 parameters determined by the least square fitting method.The two-body terms of the APES are fitted by potential energy curves with multi-reference configuration interaction,which can describe the diatomic molecules(CH,H2,HF,and CF) accurately.It is found that the APES can reproduce the geometry and vibrational frequencies of the saddle point better than those available in the literature.The rate constants based on the present APES support the experimental results of Moore et al.[Int.J.Chem.Kin.26,813(1994)].The analytical first-order derivation of energy is also provided,making the present APES convenient and efficient for investigating the title reaction with quasiclassical trajectory calculations.     

The g-factors and magnetic rotation in 82Rb

The g-factors of the intra-band states 12,13,14,15 in a magnetic-rotational band built on the 11 state in 82 Rb are measured for the first time by using a transient magnetic field-ion implantation perturbed angular distribution (TMF-IMPAD) method.The magnetic-rotational band in 82 Rb is populated by the 60 Ni(27 Al,4pn) 82 Rb reaction,and the time-integral Larmor precessions are measured after recoil implantation into a polarized Fe foil.The calculation of g-factors is also carried out in terms of a semi-classical model of independent particle angular momentum coupling on the basis of the four-quasiparticle configuration π(g 9/2) 2  π(p 3/2,f 5/2)  ν (g 9/2).The measured and calculated g-factors are in good agreement with each other.The g-factors and deduced shear angles decrease with the increase of spin along the band.This clearly illustrates the shear effect of a step-by-step alignment of the valence protons and neutrons in magnetic rotation.The semi-classical calculation also shows that the alignment of the valence neutron angular momentum is faster than that of the valence protons,which results in a decrease of g-factors with increasing spin.The present results provide solid evidence of the shear mechanism of magnetic rotation.