Cross Section Limits for the 208^{208}Pb(86^{86}Kr,n)293^{293}118 Reaction

In April-May, 2001, the previously reported experiment to synthesize element 118 using the $^{208}$Pb($^{86}$Kr,n)$^{293}$118 reaction was repeated. No events corresponding to the synthesis of element 118 were observed with a total beam dose of 2.6 x 10$^{18}$ ions. The simple upper limit cross sections (1 event) were 0.9 and 0.6 pb for evaporation residue magnetic rigidities of 2.00 $T m$ and 2.12 $T m$, respectively. A more detailed cross section calculation, accounting for an assumed narrow excitation function, the energy loss of the beam in traversing the target and the uncertainty in the magnetic rigidity of the Z=118 recoils is also presented. Re-analysis of the primary data files from the 1999 experiment showed the reported element 118 events are not in the original data. The current results put constraints on the production cross section for synthesis of very heavy nuclei in cold fusion reactions.Comment: 7 pages, 2 figures. Submitted to EPJ

Entrance-channel effects in odd-Z tranactinide compound nucleus reactions

Swiatecki, Siwek-Wilczynska, and Wilczynski's 'Fusion By Diffusion' description [1] of transactinide (TAN) compound nucleus (CN) formation utilizes a three-step model. The first step is the 'sticking', or capture, which can be calculated relatively accurately. The second step is the probability for the formation of a CN by 'diffusion' analogous to that of Brownian motion. Lastly, there exists the probability of the CN 'surviving' deexcitation by neutron emission, which competes with fission and other de-excitation modes. This model predicts and reproduces cross sections typically within a factor of two. Producing the same CN with different projectile-target pairs is a very sensitive way to test entrance channel effects on heavy element production cross sections. If the same CN is produced at or near the same excitation energy the survival portion of the theory is nearly identical for the two reactions. This method can be used as a critical test of the novel 'diffusion' portion of the model. The reactions producing odd-Z TAN CN such as Db, Bh, Mt, and Rg (Z = 105, 107, 109, and 111, respectively) were first studied using even-Z projectiles on {sup 209}Bi targets (as opposed to odd-Z projectiles on {sup 208}Pb targets) because lower effective fissility [2] was expected to lead to larger cross sections. Many odd-Z projectile reactions producing odd-Z CN had not been studied in-depth until very recently. We have completed studies of these reaction pairs with the 88-Inch Cyclotron and the Berkeley Gas-Filled Separator (BGS) at the Lawrence Berkeley National Laboratory (LBNL), see Figure 1. Cross section ratios for several pairs of reactions will be presented and compared with theory

The influence of projectile neutron number in the 208Pb(48Ti, n)255Rf and 208Pb(50Ti, n)257Rf reactions

Four isotopes of rutherfordium,254-257Rf, were produced by the 208Pb(48Ti, xn)256-xRf and 208Pb(50Ti, xn)258-xRf reactions (x = 1, 2) at the Lawrence Berkeley National Laboratory 88-Inch Cyclotron. Excitation functions were measured for the 1n and 2n exit channels. A maximum likelihood technique, which correctly accounts for the changing cross section at all energies subtended by the targets, was used to fit the 1n data to allow a more direct comparison between excitation functions obtained under different experimental conditions. The maximum 1n crosssections of the 208Pb(48Ti, n)255Rf and 208Pb(50Ti, n)257Rf reactions obtained from fits to the experimental data are 0.38 +/- 0.07 nb and 40 +/-5 nb, respectively. Excitation functions for the 2n exit channel were also measured, with maximum cross sections of nb for the 48Ti induced reaction, and 15.7 +/- 0.2 nb for the 50Ti induced reaction. The impact of the two neutron difference in the projectile on the 1n cross section is discussed. The results are compared to the Fusion by Diffusion model developed by Swiatecki, Wilczynska, and Wilczynski

Influence of projectile neutron number on cross section in cold fusion reactions

Elements 107-112 [1,2] have been discovered in reactions between {sup 208}Pb or {sup 209}Bi targets and projectiles ranging from {sup 54}Cr through {sup 70}Zn. In such reactions, the compound nucleus can be formed at excitation energies as low as {approx}12 MeV, thus this type of reaction has been referred to as 'cold fusion'. The study of cold fusion reactions is an indispensable approach to gaining a better understanding of heavy element formation and decay. A theoretical model that successfully predicts not only the magnitudes of cold fusion cross sections, but also the shapes of excitation functions and the cross section ratios between various reaction pairs was recently developed by Swiatecki, Siwek-Wilczynska, and Wilczynski [3,4]. This theoretical model, also referred to as Fusion by Diffusion, has been the guide in all of our cold fusion studies. One particularly interesting aspect of this model is the large predicted difference in cross sections between projectiles differing by two neutrons. The projectile pair where this difference is predicted to be largest is {sup 48}Ti and {sup 50}Ti. To test and extend this model, {sup 208}Pb({sup 48}Ti,n){sup 255}Rf and {sup 208}Pb({sup 50}Ti,n){sup 257}Rf excitation functions were recently measured at the Lawrence Berkeley National Laboratory's (LBNL) 88-Inch Cyclotron utilizing the Berkeley Gas-filled Separator (BGS). The {sup 50}Ti reaction was carried out with thin lead targets ({approx}100 {micro}g/cm{sup 2}), and the {sup 48}Ti reaction with both thin and thick targets ({approx}470 {micro}g/cm{sup 2}). In addition to this reaction pair, reactions with projectile pairs {sup 52}Cr and {sup 54}Cr [5], {sup 56}Fe and {sup 58}Fe [6], and {sup 62}Ni [7] and {sup 64}Ni [8] will be discussed and compared to the Fusion by Diffusion predictions. The model predictions show a very good agreement with the data

Extraction systems for the study of dubnium

The chemistry of transactinide elements (Z {ge} 104) is a topic of great interest in current nuclear chemistry research. The chemical systems that can be used in these studies are limited by the short half-lives of the isotopes and the small production rates of atoms per minute or even atoms per week. In the initial investigations, the chemistry used had to be very selective to the periodic group of interest to separate the transactinide atom from all the other unwanted nuclear reaction products, e.g., transfer products. By using the Berkeley Gas-filled Separator (BGS) as a physical pre-separator, we are able concentrate on systems that are selective between the members of the group of interest, because all other interfering products and the beam are being suppressed by the BGS [1]. We are developing suitable extraction systems for the study of element 105, dubnium. For this purpose we have studied the extraction of niobium and tantalum, the lighter homologs of dubnium, from mineral acids with different organophosphorus compounds. All studies were performed online, using short-lived niobium and tantalum produced in the {sup 124}Sn({sup 51}V,5n){sup 170}Ta and {sup 74}Se({sup 18}O,p3n){sup 88}Nb reactions. This allowed for the study of the lighter homologues at metal concentrations of 10{sup -16} M. At these low metal concentrations, the formation of polymeric species is largely prohibited. As seen in Fig. 1, by varying the extractant and the hydrochloric acid concentration from 1 to 11 M, we are able to see a difference in extraction behavior between niobium and tantalum. While the system is suitable for determining chemical differences between the lighter homologues, the extraction of tantalum from hydrochloric acid shows slow kinetics. Figure 2 shows that after 90 seconds of mixing, the system is not in equilibrium. However, experiments indicate that equilibrium is reached faster at higher acid concentrations. We have studied the influence of hydrogen ion concentration on the extraction kinetics. By varying the chloride concentration while holding the hydrogen ion concentration at a low, fixed value, equilibrium can be reached in less than 10 s. Results for different extractants and various aqueous phase compositions will be presented and discussed

Characterization of Group V Dubnium Homologs on DGA Extraction Chromatography Resin from Nitric and Hydrofluoric Acid Matrices

Studies of the chemical properties of superheavy elements (SHE) pose interesting challenges due to their short half-lives and low production rates. Chemical systems must have extremely fast kinetics, fast enough kinetics to be able to examine the chemical properties of interest before the SHE decays to another nuclide. To achieve chemistry on such time scales, the chemical system must also be easily automated. Most importantly however, a chemical system must be developed which provides suitable separation and kinetics before an on-line study of a SHE can be performed. Relativistic effects make studying the chemical properties of SHEs interesting due to the impact these effects could have on the SHEs chemical properties. Relativistic effects arise when the velocity of the s orbital electrons approach the speed of light. As this velocity increases, the Bohr radius of the inner electron orbitals decreases and there is an increase in the particles mass. This contraction results in a destabilization of the energy of the outer d and f electron orbitals (5f and 6d in the case of SHE), which can cause these to expand due to their increased shielding from the nuclear charge. Another relativistic effect is the spin-orbit splitting for p, d, and f orbitals into j = 1 {+-} 1/2 states. This can lead most interestingly to a possible increased stability of element 114, which due to large spin-orbit splitting of the 7p orbital and the relativistically stabilized 7p{sub 1/2} and 7s orbital gives rise to a closed shell ground state of 7s{sup 2}7p{sub 1/2}{sup 2}. The homologs of element 105, dubnium (Db), Ta and Nb and the pseudo-homolog Pa, are well known to hydrolyze and form both neutral and non-neutral monoatomic and polyatomic species that may cause issues with extraction from a given chemical system. Early ion-exchange and solvent-extraction studies show mixed results for the behavior of Db. Some studies show Db behaving most similar to Ta, while others show it behaving somewhere between Nb and Pa. Much more recent studies have examined the properties of Db from HNO{sub 3}/HF matrices, and suggest Db forms complexes similar to those of Pa. Very little experimental work into the behavior of element 114 has been performed. Thermochromatography experiments of three atoms of element 114 indicate that the element 114 is at least as volatile as Hg, At, and element 112. Lead was shown to deposit on gold at temperatures about 1000 C higher than the atoms of element 114. Results indicate a substantially increased stability of element 114. No liquid phase studies of element 114 or its homologs (Pb, Sn, Ge) or pseudo-homologs (Hg, Cd) have been performed. Theoretical predictions indicate that element 114 is should have a much more stable +2 oxidation state and neutral state than Pb, which would result in element 114 being less reactive and less metallic than Pb. The relativistic effects on the 7p{sub 1/2} electrons are predicted to cause a diagonal relationship to be introduced into the periodic table. Therefore, 114{sup 2+} is expected to behave as if it were somewhere between Hg{sup 2+}, Cd{sup 2+}, and Pb{sup 2+}. In this work two commercially available extraction chromatography resins are evaluated, one for the separation of Db homologs and pseudo?homologs from each other as well as from potential interfering elements such as Group IV Rf homologs and actinides, and the other for separation of element 114 homologs. One resin, Eichrom's DGA resin, contains a N,N,N',N'-tetra-n-octyldiglycolamide extractant, which separates analytes based on both size and charge characteristics of the solvated metal species, coated on an inert support. The DGA resin was examined for Db chemical systems, and shows a high degree of selectivity for tri-, tetra-, and hexavalent metal ions in multiple acid matrices with fast kinetics. The other resin, Eichrom's Pb resin, contains a di-t-butylcyclohexano 18-crown-6 extractant with isodecanol solvent, which separates analytes based on steric interactions between the cavity of the crown ether and electrostatic interactions between the oxygen's of the ether and cations in the mobile phase. This particular resin has been shown to have an extremely high uptake affinity for Pb, a direct homolog of element 114, and is thus a good initial extractant to examine for a potential element 114 chemical system. Figure 1.1 shows the respective extractant molecules from the DGA and Pb resins. Batch uptake experiments were conducted to examine the uptake behavior of Ta on the DGA resin. Batch uptake experiments were also conducted to examine the uptake behavior of Ge on the Pb resin. Column experiments were designed based on batch uptake experiments of Ta, Am, Pa, Np, Zr, and Nb to establish a sequential extraction of Group IV/V homologs as well as Am for potential use as a Db chemical system

Gas separation in nanoporous membranes formed by etching ion irradiated polymer foils

Polymer membranes with pores with radii in the range of several 10-100 nm were formed by irradiating polyimide foil with highly energetic heavy ions and etching the latent ion tracks with hypochlorite. The aerial density of the pores could be chosen up to an upper limit of 108 pores cm-2, at which too many pores start to overlap. The straight cylindrical pores were tested for their gas permeation and gas separation performance. With a gas mixture of CO and CO2 as model system, gas chromatographic measurements showed that CO penetrates faster through the membrane than CO2, leading to gas separation. This is possible because the mean free path of the molecules is in the order of the pore radius, which is in the transition flow region close to molecular flow conditions

Filters with <100 nm radius pores for gas separation formed by high-energy ion irradiation of polymers

In the industry, often gases have to be separated from each other for cleaning and other purposes. In principle, this can be achieved by passing a gas mixture through a filter system when the filter pore diameter is very small being comparable to the size of the mean free path of the gases. Such well-defined pores can be fabricated by high-energy ion irradiation of polymers, combined with chemical etching of the resulting damage in the polymer. Polyimide foil was irradiated with high-energy lead ions. The pores were evolved from the ion tracks by exposing the polymer to a chemical etching agent. The pore radius was determined by scanning electron microscopy (SEM). The shape of the pores through the foil was determined by filling them electrochemically with metal, cutting them into small pieces and investigating the edges again by SEM. The results showed that uniform cylindrical pores with radii below 100 nm could be formed. Using the gas mixture CO/CO2 as a model system for the gas separation the filters were tested for their efficiency. The gas mixture was pumped through the filter and analysed by gas chromatography. The results show that a separation of the gas mixture is possible. Filters fabricated by ion irradiation may act as efficient gas separators