Potential energy surfaces of superheavy nuclei

We investigate the structure of the potential energy surfaces of the superheavy nuclei 158258Fm100, 156264Hs108, 166278112, 184298114, and 172292120 within the framework of self-consistent nuclear models, i.e., the Skyrme-Hartree-Fock approach and the relativistic mean-field model. We compare results obtained with one representative parametrization of each model which is successful in describing superheavy nuclei. We find systematic changes as compared to the potential energy surfaces of heavy nuclei in the uranium region: there is no sufficiently stable fission isomer any more, the importance of triaxial configurations to lower the first barrier fades away, and asymmetric fission paths compete down to rather small deformation. Comparing the two models, it turns out that the relativistic mean-field model gives generally smaller fission barriers

Potential energy surfaces of superheavy nuclei

We investigate the structure of the potential energy surfaces of the superheavy nuclei 258Fm, 264Hs, (Z=112,N=166), (Z=114,N=184), and (Z=120,N=172) within the framework of self-consistent nuclear models, i.e. the Skyrme-Hartree-Fock approach and the relativistic mean-field model. We compare results obtained with one representative parametrisation of each model which is successful in describing superheavy nuclei. We find systematic changes as compared to the potential energy surfaces of heavy nuclei in the uranium region: there is no sufficiently stable fission isomer any more, the importance of triaxial configurations to lower the first barrier fades away, and asymmetric fission paths compete down to rather small deformation. Comparing the two models, it turns out that the relativistic mean-field model gives generally smaller fission barriers.Comment: 8 pages RevTeX, 6 figure

Potential energy surfaces for cluster emitting nuclei

Potential energy surfaces are calculated by using the most advanced asymmetric two-center shell model allowing to obtain shell and pairing corrections which are added to the Yukawa-plus-exponential model deformation energy. Shell effects are of crucial importance for experimental observation of spontaneous disintegration by heavy ion emission. Results for 222Ra, 232U, 236Pu and 242Cm illustrate the main ideas and show for the first time for a cluster emitter a potential barrier obtained by using the macroscopic-microscopic method.Comment: 10 pages, 21 figures, revtex

Potential-energy surfaces, unimolecular processes and spectroscopy

The present symposium brings together research in a number of fields: the quantum-chemical calculation of molecular potential-energy surfaces, rotational–vibrational spectroscopy, methods of calculating rotational–vibrational energy levels, unimolecular reactions and intramolecular dynamics. Several aspects of the work are discussed including some recent developments on rates and products' quantum state distributions for unimolecular dissociations having highly flexible transition states. The usefulness of having improved potential-energy surfaces, particularly the bonding and hindered rotational potentials in the dissociations, is noted. In various other studies in this symposium a better knowledge of the surfaces would be particularly helpful. New results on a semiclassical quantization method are also described

Molecular potential energy surfaces constructed from interpolation of systematic fragment surfaces

A systematic method for approximating the ab initio electronic energy of molecules from the energies of molecular fragments has previously been presented. Here it is shown that this approach provides a feasible, systematic method for constructing a global molecular potential energy surface (PES) for reactions of a moderate-sized molecule from the corresponding surfaces for small molecular fragments. The method is demonstrated by construction of PESs for the reactions of a hydrogen atom with propane and n-pentane

Computed potential energy surfaces for chemical reactions

The minimum energy path for the addition of a hydrogen atom to N2 is characterized in CASSCF/CCI calculations using the (4s3p2d1f/3s2p1d) basis set, with additional single point calculations at the stationary points of the potential energy surface using the (5s4p3d2f/4s3p2d) basis set. These calculations represent the most extensive set of ab initio calculations completed to date, yielding a zero point corrected barrier for HN2 dissociation of approx. 8.5 kcal mol/1. The lifetime of the HN2 species is estimated from the calculated geometries and energetics using both conventional Transition State Theory and a method which utilizes an Eckart barrier to compute one dimensional quantum mechanical tunneling effects. It is concluded that the lifetime of the HN2 species is very short, greatly limiting its role in both termolecular recombination reactions and combustion processes

Computed potential energy surfaces for chemical reactions

The work on the NH + NO system which was described in the last progress report was written up and a draft of the manuscript is included in the appendix. The appendix also contains a draft of a manuscript on an Ar + H + H surface. New work which was completed in the last six months includes the following: (1) calculations on the (1)CH2 + H2O, H2 + HCOH, and H2 + H2CO product channels in the CH3 + OH reaction; (2) calculations for the NH2 + O reaction; (3) calculations for the CH3 + O2 reaction; and (4) calculations for CH3O and the two decomposition channels--CH2OH and H + H2CO. Detailed descriptions of this work will be given in manuscripts; however, brief descriptions of the CH3 + OH and CH3 + O2 projects are given

Computed Potential Energy Surfaces for Chemical Reactions

A manuscript describing the calculations on the (1)CH2 + H2O, H2 + HCOH, and H2 + H2CO product channels in the CH3 + OH reaction, which were described in the last progress report, has been accepted for publication in J. Chem. Phys., and a copy of the manuscript is included in the appendix. The production of (1)CH2 in this reaction is important in hydrocarbon combustion since (1)CH2 is highly reactive and would be expected to insert into N2, possibly leading to a new source for prompt NO(x) (vide infra). During the last six months new calculations have been carried out for the NH2 + NO system, which is important in the thermal de-NO(x) process

Local Approximation of Potential‐Energy Surfaces by Surfaces Permitting Separation of Variables

In the immediate vicinity of a potential‐energy minimum or of a saddle point, it is shown that major topographical features of a "nonseparable" potential‐energy surface can be imitated by those of a surface permitting separation of variables. For each extremal path of descent or ascent to the cited critical point of the surface, there is an exact match of the tangent, the first curvature vector in configuration space, and the force constant along that path provided that the known curvature vector satisfies an equation containing the metric tensor of the selected coordinate system and known force constants. Because of the wide choice of coordinate systems available for selection, it is anticipated that this relation may be fulfilled for each extremal path, partly by choice of the coordinate system and partly by subsequent choice of the curvilinear coordinates of the critical point. There are several possible applications of this local approximation, including those to problems involving anharmonic coupling of normal modes and those involving n‐dimensional tunneling and other calculations in reaction‐rate theory. Use will be made of the formalism to extend the activated complex theory in chemical kinetics. As a preliminary test of the local‐approximation concept, literature data on n‐ and one‐dimensional tunneling rates are compared. They are found to be fairly similar when proper cognizance is taken of zero‐point energies