Atomic spectral-product representations of molecular electronic structure: metric matrices and atomic-product composition of molecular eigenfunctions

Recent progress is reported in development of ab initio computational methods for the electronic structures of molecules employing the many-electron eigenstates of constituent atoms in spectral-product forms. The approach provides a universal atomic-product description of the electronic structure of matter as an alternative to more commonly employed valence-bond- or molecular-orbital-based representations. The Hamiltonian matrix in this representation is seen to comprise a sum over atomic energies and a pairwise sum over Coulombic interaction terms that depend only on the separations of the individual atomic pairs. Overall electron antisymmetry can be enforced by unitary transformation when appropriate, rather than as a possibly encumbering or unnecessary global constraint. The matrix representative of the antisymmetrizer in the spectral-product basis, which is equivalent to the metric matrix of the corresponding explicitly antisymmetric basis, provides the required transformation to antisymmetric or linearly independent states after Hamiltonian evaluation. Particular attention is focused in the present report on properties of the metric matrix and on the atomic-product compositions of molecular eigenstates as described in the spectral-product representations. Illustrative calculations are reported for simple but prototypically important diatomic (H_2, CH) and triatomic (H_3, CH_2) molecules employing algorithms and computer codes devised recently for this purpose. This particular implementation of the approach combines Slater-orbital-based one- and two-electron integral evaluations, valence-bond constructions of standard tableau functions and matrices, and transformations to atomic eigenstate-product representations. The calculated metric matrices and corresponding potential energy surfaces obtained in this way elucidate a number of aspects of the spectral-product development, including the nature of closure in the representation, the general redundancy or linear dependence of its explicitly antisymmetrized form, the convergence of the apparently disparate atomic-product and explicitly antisymmetrized atomic-product forms to a common invariant subspace, and the nature of a chemical bonding descriptor provided by the atomic-product compositions of molecular eigenstates. Concluding remarks indicate additional studies in progress and the prognosis for performing atomic spectral-product calculations more generally and efficiently

Quasi-fission reactions as a probe of nuclear viscosity

Fission fragment mass and angular distributions were measured from the ^{64}Ni+^{197}Au reaction at 418 MeV and 383 MeV incident energy. A detailed data analysis was performed, using the one-body dissipation theory implemented in the code HICOL. The effect of the window and the wall friction on the experimental observables was investigated. Friction stronger than one-body was also considered. The mass and angular distributions were consistent with one-body dissipation. An evaporation code DIFHEAT coupled to HICOL was developed in order to predict reaction time scales required to describe available data on pre-scission neutron multiplicities. The multiplicity data were again consistent with one-body dissipation. The cross-sections for touch, capture and quasi-fission were also obtained.Comment: 25 pages REVTeX, 3 tables, 13 figures, submitted to Phys. Rev

Angular anisotropy of the fusion-fission and quasifission fragments

The anisotropy in the angular distribution of the fusion-fission and quasifission fragments for the $^{16}$O+$^{238}$U, $^{19}$F+$^{208}$Pb and $^{32}$S+$^{208}$Pb reactions is studied by analyzing the angular momentum distributions of the dinuclear system and compound nucleus which are formed after capture and complete fusion, respectively. The orientation angles of axial symmetry axes of colliding nuclei to the beam direction are taken into account for the calculation of the variance of the projection of the total spin onto the fission axis. It is shown that the deviation of the experimental angular anisotropy from the statistical model picture is connected with the contribution of the quasifission fragments which is dominant in the $^{32}$S+$^{208}$Pb reaction. Enhancement of anisotropy at low energies in the $^{16}$O+$^{238}$U reaction is connected with quasifission of the dinuclear system having low temperature and effective moment of inertia.Comment: 17 pages 8 figures. Submitted to Euro. Phys. Jour.

Thermal fission rate around super-normal phase transition

Using Langer's $Im F$ method, we discuss the temperature dependence of nuclear fission width in the presence of dissipative environments. We introduce a low cut-off frequency to the spectral density of the environmental oscillators in order to mimic the pairing gap. It is shown that the decay width rapidly decreases at the critical temperature, where the phase transition from super to normal fluids takes place. Relation to the recently observed threshold for the dissipative fission is discussed.Comment: 12 pages, Latex, Submitted to Physical Review C for publication, 3 Postscript figures are available by request from [email protected]

Sub-barrier capture with quantum diffusion approach: actinide-based reactions

With the quantum diffusion approach the behavior of capture cross sections and mean-square angular momenta of captured systems are revealed in the reactions with deformed nuclei at subbarrier energies. The calculated results are in a good agreement with existing experimental data. With decreasing bombarding energy under the barrier the external turning point of the nucleusnucleus potential leaves the region of short-range nuclear interaction and action of friction. Because of this change of the regime of interaction, an unexpected enhancement of the capture cross section is expected at bombarding energies far below the Coulomb barrier. This effect is shown its worth in the dependence of mean-square angular momentum of captured system on the bombarding energy. From the comparison of calculated and experimental capture cross sections, the importance of quasifission near the entrance channel is shown for the actinide-based reactions leading to superheavy nuclei.Comment: 11 pages, 16 figures, Regular Articl

Food sharing among captive gibbons ( Hylobates lar )

A captive family group of gibbons engages in food sharing during consistently patterned sequences of behaviors in which begging gestures are employed. The predominant occurrence of the behavior involves the juvenile female begging from her older, adult sister who acted as her “surrogate mother”. An examination of the variables potentially affecting the behavior, such as hunger, the availability and accessibility of preferred foods, the inability to forage individually, and the social relationships between members of the family, indicates that food sharing may assist the young in acquiring appropriate food habits, supplement their foraging capabilities, and may serve to reinforce the social bonds between adult and immature members of the family group.Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/41598/1/10329_2006_Article_BF02383142.pd

EquiFACS: the Equine Facial Action Coding System

Although previous studies of horses have investigated their facial expressions in specific contexts, e.g. pain, until now there has been no methodology available that documents all the possible facial movements of the horse and provides a way to record all potential facial configurations. This is essential for an objective description of horse facial expressions across a range of contexts that reflect different emotional states. Facial Action Coding Systems (FACS) provide a systematic methodology of identifying and coding facial expressions on the basis of underlying facial musculature and muscle movement. FACS are anatomically based and document all possible facial movements rather than a configuration of movements associated with a particular situation. Consequently, FACS can be applied as a tool for a wide range of research questions. We developed FACS for the domestic horse (Equus caballus) through anatomical investigation of the underlying musculature and subsequent analysis of naturally occurring behaviour captured on high quality video. Discrete facial movements were identified and described in terms of the underlying muscle contractions, in correspondence with previous FACS systems. The reliability of others to be able to learn this system (EquiFACS) and consistently code behavioural sequences was high—and this included people with no previous experience of horses. A wide range of facial movements were identified, including many that are also seen in primates and other domestic animals (dogs and cats). EquiFACS provides a method that can now be used to document the facial movements associated with different social contexts and thus to address questions relevant to understanding social cognition and comparative psychology, as well as informing current veterinary and animal welfare practices

The impact of relationship quality on life satisfaction and well-being in dementia caregiving dyads: findings from the IDEAL study

Objectives: The quality of the relationship between people with dementia and their informal caregiver maybe an important determinant of life satisfaction and well-being for both members of the dyad. Taking a dyadic perspective, the aim of this study was to examine whether self- and partner-rated relationship quality influences life satisfaction and well-being for both people with dementia and their caregivers. Design and methods: Using data from 1283 dyads in the Improving the Experience of Dementia and Enhancing Active Life (IDEAL) cohort, we examined the impact of current relationship quality on life satisfaction and well-being in dementia caregiving dyads. Data were analysed using the Actor–Partner Interdependence Model (APIM) framework. Results: Self-rated relationship quality was associated with own life satisfaction and well-being for both people with dementia and caregivers. Partner-rated relationship quality did not influence own life satisfaction or well-being for either member of the dyad. Conclusion: This study is the first to use the APIM framework to explore the dyadic associations between relationship quality and life satisfaction and well-being in a large cohort of dementia caregiving dyads. The obtained findings suggest that the individual perception of the quality of the caregiving relationship held by each member of the caregiving dyad is an important factor for that member’s life satisfaction and well-being, while the partner’s perception of relationship quality is not. The findings highlight the importance of considering the individual perspective of both the person with dementia and the caregiver and enabling each to maintain positive perceptions of relationship quality

Molecular excitation in the Interstellar Medium: recent advances in collisional, radiative and chemical processes

We review the different excitation processes in the interstellar mediumComment: Accepted in Chem. Re

Adoptive gay father families: parent-child relationships and children's psychological adjustment

Findings are presented on a U.K. study of 41 gay father families, 40 lesbian mother families, and 49 heterosexual parent families with an adopted child aged 3–9 years. Standardized interview and observational and questionnaire measures of parental well-being, quality of parent–child relationships, child adjustment, and child sex-typed behavior were administered to parents, children, and teachers. The findings indicated more positive parental well-being and parenting in gay father families compared to heterosexual parent families. Child externalizing problems were greater among children in heterosexual families. Family process variables, particularly parenting stress, rather than family type were found to be predictive of child externalizing problems. The findings contribute to theoretical understanding of the role of parental gender and parental sexual orientation in child development