First Principles Study of Adsorption of O2O_{2} on Al Surface with Hybrid Functionals

Adsorption of $O_{2}$ molecule on Al surface has been a long standing puzzle for the first principles calculation. We have studied the adsorption of $O_{2}$ molecule on the Al(111) surface using hybrid functionals. In contrast to the previous LDA/GGA, the present calculations with hybrid functionals successfully predict that $O_{2}$ molecule can be absorbed on the Al(111) surface with a barrier around 0.2$\thicksim$0.4 eV, which is in good agreement with experiments. Our calculations predict that the LUMO of $O_{2}$ molecule is higher than the Fermi level of the Al(111) surface, which is responsible for the barrier of the $O_{2}$ adsorption.Comment: 14 pages, 5 figure

The shortcomings of semi-local and hybrid functionals: what we can learn from surface science studies

A study of the adsorption of CO on late 4d and $5d$ transition metal (111) surfaces (Ru, Rh, Pd, Ag, Os, Ir, and Pt) considering atop and hollow site adsorption is presented. The applied functionals include the gradient corrected PBE and BLYP functional, and the corresponding hybrid Hartree-Fock density functionals HSE and B3LYP. We find that PBE based hybrid functionals (specifically HSE) yield, with the exception of Pt, the correct site order on all considered metals, but they also considerably overestimate the adsorption energies compared to experiment. On the other hand, the semi-local BLYP functional and the corresponding hybrid functional B3LYP yield very satisfactory adsorption energies and the correct adsorption site for all surfaces. We are thus faced with a Procrustean problem: the B3LYP and BLYP functionals seem to be the overall best choice for describing adsorption on metal surfaces, but they simultaneously fail to account well for the properties of the metal, vastly overestimating the equilibrium volume and underestimating the atomization energies. Setting out from these observations, general conclusions are drawn on the relative merits and drawbacks of various semi-local and hybrid functionals. The discussion includes a revised version of the PBE functional specifically optimized for bulk properties and surface energies (PBEsol), a revised version of the PBE functional specifically optimized to predict accurate adsorption energies (rPBE), as well as the aforementioned BLYP functional. We conclude that no semi-local functional is capable to describe all aspects properly, and including non-local exchange also only improves some, but worsens other properties.Comment: 12 pages, 6 figures; to be published in New Journal of Physic

Measurements of Gd 152 (p,γ) Tb 153 and Gd 152 (p,n) Tb 152 reaction cross sections for the astrophysical γ process

The total cross sections for the Gd152(p,γ)Tb153 and Gd152(p,n)152Tb reactions have been measured by the activation method at effective center-of-mass energies 3.47≤Ec.m.eff≤7.94 MeV and 4.96≤Ec.m.eff≤7.94 MeV, respectively. The targets were prepared by evaporation of 30.6% isotopically enriched Gd152 oxide on aluminum backing foils, and bombarded with proton beams provided by a cyclotron accelerator. The cross sections were deduced from the observed γ-ray activity, which was detected off-line by an HPGe detector in a low background environment. The results are presented and compared with predictions of statistical model calculations. This comparison supports a modified optical proton+Gd152 potential suggested earlier.Peer reviewedFinal Accepted Versio

Alpha-induced reactions for the astrophysical p-process: the case of 151Eu

The cross sections of 151Eu(alpha,gamma)155Tb and 151Eu(alpha,n)154Tb reactions have been measured with the activation method. Some aspects of the measurement are presented here to illustrate the requirements of experimental techniques needed to obtain nuclear data for the astrophysical p-process nucleosynthesis. Preliminary cross section results are also presented and compared with the predictions of statistical model calculations.Comment: Accepted for publication in Journal of Physics Conference Series, proceeding of the Nuclear Physics in Astrophysics IV. conferenc

Alpha-induced cross sections of 106Cd for the astrophysical p-process

The 106Cd(alpha,gamma)110Sn reaction cross section has been measured in the energy range of the Gamow window for the astrophysical p-process scenario. The cross sections for 106Cd(alpha,n)109Sn and for 106Cd(alpha,p)109In below the (alpha,n) threshold have also been determined. The results are compared with predictions of the statistical model code NON-SMOKER using different input parameters. The comparison shows that a discrepancy for 106Cd(alpha,gamma)110Sn when using the standard optical potentials can be removed with a different alpha+106Cd potential. Some astrophysical implications are discussed.Comment: 10 pages, 9 figures, accepted for publication in Phys. Rev

Proton induced reaction cross section measurements on Se isotopes for the astrophysical p process

As a continuation of a systematic study of reactions relevant to the astrophysical p process, the cross sections of the 74,76Se(p,gamma)75,77Br and 82Se(p,n)82Br reactions have been measured at energies from 1.3 to 3.6 MeV using an activation technique. The results are compared to the predictions of Hauser-Feshbach statistical model calculations using the NON-SMOKER and MOST codes. The sensitivity of the calculations to variations in the optical proton potential and the nuclear level density was studied. Good agreement between theoretical and experimental reaction rates was found for the reactions 74Se(p,gamma)75Br and 82Se(p,n)82Br.Comment: 9 pages, 6 figures (in 12 eps files), accepted for publication in Phys. Rev C, RevTeX styl

Measurements of proton induced reaction cross sections on 120Te for the astrophysical p-process

The total cross sections for the 120Te(p,gamma)121I and 120Te(p,n)120I reactions have been measured by the activation method in the effective center-of-mass energies between 2.47 MeV and 7.93 MeV. The targets were prepared by evaporation of 99.4 % isotopically enriched 120Te on Aluminum and Carbon backing foils, and bombarded with proton beams provided by the FN tandem accelerator at the University of Notre Dame. The cross sections and $S$ factors were deduced from the observed gamma ray activity, which was detected off-line by two Clover HPGe detectors mounted in close geometry. The results are presented and compared with the predictions of statistical model calculations using the codes NON-SMOKER and TALYS.Comment: 17 pages, 5 figures, 5 tables, regular articl

Electron screening in molecular fusion reactions

Recent laboratory experiments have measured fusion cross sections at center-of-mass energies low enough for the effects of atomic and molecular electrons to be important. To extract the cross section for bare nuclei from these data (as required for astrophysical applications), it is necessary to understand these screening effects. We study electron screening effects in the low-energy collisions of Z=1 nuclei with hydrogen molecules. Our model is based on a dynamical evolution of the electron wavefunctions within the TDHF scheme, while the motion of the nuclei is treated classically. We find that at the currently accessible energies the screening effects depend strongly on the molecular orientation. The screening is found to be larger for molecular targets than for atomic targets, due to the reflection symmetry in the latter. The results agree fairly well with data measured for deuteron collisions on molecular deuterium and tritium targets.Comment: 15 Page RevTeX document, twelve postscript figures, now in a uufile packag

Hydrogen Production From Photolysis of Steam Adsorbed Onto Platinized SrTiO{Sub 3}

Photodissociation of high presssure (1-8 atm) water vapor adsorbed onto the partially platinized surface of single crystal SrTiO{sub 3} has been observed. The reaction is catalytic; several thousands of monolayers of hydrogen have been produced. The reaction requires light of greater than bandgap (3.1 eV) energy, and proceeds vigorously only if elevated temperatures (375- 450 K) and high pressures are used. Recombination of products and poisoning of the metal appears to diminish the reaction rate after several hours. This reaction differs from the photolysis of water in the analogous short-circuit electrochemical cell in that we use no electrolyte and we are able to use non-conducting, stoichiometric SrTiO{sub 3} because bulk electrical conductivity has little influence on localized surface reactions. We have observed evidence for the following steps during photolysis of water on platinized SrTiO{sub 3} : (1) generation of electron-hole pairs by light of greater than bandgap energy, (2) dissociative chemisorption of water vapor on the hydroxylated semiconductor surface, (3) diffusion of a surface hydrogen species to platinum islands and desorption of hydrogen from the islands, and (4) recombination of hydrogen and oxygen which limits the amount of hydrogen that can be generated in a batch reactor

Experimental cross sections of Ho 165 (α,n) Tm 168 and Er 166 (α,n) Yb 169 for optical potential studies relevant for the astrophysical γ process

Background: Optical potentials are crucial ingredients for the prediction of nuclear reaction rates needed in simulations of the astrophysical γ process. Associated uncertainties are particularly large for reactions involving α particles. This includes (γ,α) reactions which are of special importance in the γ process. Purpose: The measurement of (α,n) reactions allows for an optimization of currently used α-nucleus potentials. The reactions Ho165(α,n) and Er166(α,n) probe the optical model in a mass region where γ process calculations exhibit an underproduction of p nuclei which is not yet understood. Method: To investigate the energy-dependent cross sections of the reactions Ho165(α,n) and Er166(α,n) close to the reaction threshold, self-supporting metallic foils were irradiated with α particles using the FN tandem Van de Graaff accelerator at the University of Notre Dame. The induced activity was determined afterwards by monitoring the specific β-decay channels. Results: Hauser-Feshbach predictions with a widely used global α potential describe the data well at energies where the cross sections are almost exclusively sensitive to the α widths. Increasing discrepancies appear towards the reaction threshold at lower energy. Conclusions: The tested global α potential is suitable at energies above 14 MeV, while a modification seems necessary close to the reaction threshold. Since the γ and neutron widths show non-negligible impact on the predictions, complementary data are required to judge whether or not the discrepancies found can be solely assigned to the α width. © 2014 American Physical Society.Peer reviewedFinal Accepted Versio