text:
# New Outlook on the Possible Existence of Superheavy Elements in Nature1footnote 11footnote 1Paper presented at VII Int. School-Seminar on Heavy Ion Physics, May 27 - June 1, 2002, Dubna Russia.

## I Introduction

The theoretical predictions in the nineteen sixties str64 ; mye66 ; sob66 ; str67 ; won67 ; muz68 ; nil68 ; gru69  of the possible existence of very long-lived superheavy elements around Z=114 and N=184 stirred a lot of excitement among the nuclear scientific community and have initiated the search for the possible existence of superheavy elements in nature. In the present paper we concentrate on two independent well established experimental results which are impossible to understand under the present common knowledge of nuclear physics. These puzzling data are first the observation, in mica minerals, of certain halos which have been attributed to the $`\alpha `$-decay of the short-lived 210Po,214Po and 218Po nuclei hen39 ; gen68 ; gen92 , and secondly the observation in several minerals of a low energy $`\alpha `$-particle group with an energy of about 4.5 MeV cher63 ; che64 ; cher68 ; mei70 .

Halos in mica, which consist of tiny concentric rings, are known for a long time jol07 ; mug07 . For most of them the measured radii of the rings fit with the known ranges of the various $`\alpha `$-particle groups from 238U or 232Th decay chains. Therefore they have been correctly interpreted, back in 1907 jol07 ; mug07 , as due to the existence of very small grains of 238U or 232Th in the centers of the corresponding halos, which have been decaying, through their characteristic decay chains, since the time of crystallization of the crust of the earth. However, other types of halos have been discovered back in 1939 hen39  and have been thoroughly studied by Gentry gen68 . These are the 210Po, 214Po and 218Po halos which consist of respective one, two and three concentric rings, with radii equal to the ranges of the $`\alpha `$-particle groups from the decay chains of the corresponding Po isotopes222Colored pictures of various halos are given in Ref. gen92 .. These Po isotopes belong to the 238U decay chain. However, their half-lives, as well as the half-lives of their $`\beta `$-decay parents, are short, and since rings belonging to their long-lived precursors are absent, their appearance in nature is puzzling fea78 .

Another puzzling phenomenon is the low-energy $`\alpha `$-particle group, around 4.5 MeV, which has been seen in molybdenite cher63 , in thorite che64 , in magnetite cher68  and in OsIr mei70 . The cleanest spectrum, where this group appears without observed residues from U isotopes decays, was obtained by Cherdyntsev et al. cher68 . Based on chemical behavior (having volatile oxides) of the $`\alpha `$-emitter, it has been suggested that it might be due to a decay of an isotope of Eka-Os, the superheavy element with Z=108 (Hs).333Actually Cherdyntsev suggested naming element 108 sergenium, based on part of the great silk path in Kazakhstan (name Serika) where the studied mineral molibdenite was found (private communication from Yu. Lobanov.) Since it was usually found together with 247Cm and 239Pu, it has been suggested mei70  that this low-energy $`\alpha `$-particle group is due to an isotope of element 108 which is a precursor of 247Cm and its descendant 239Pu. The half-life of this activity has been estimated to be around $`(2.5\pm 0.5)\times 10^8`$ y cher63 .

With the current common knowledge of nuclear physics it seemed impossible to understand these data. The predicted energies of ground state to ground state $`\alpha `$ transitions for $`\beta `$ stable Hs nuclei with atomic masses of 274 to 286 are between 9.5 and 6.7 MeV mnk ; kuty ; lmz , and the predicted half-lives for these energies are between $`3\times 10^2`$ s and $`3\times 10^2`$ y vs66 ; roy00 , as compared to half-life of about $`5\times 10^{16}`$ y for 4.5 MeV. The question is why the nucleus decays with such a low energy $`\alpha `$-particle when a much higher energy, with a penetrability factor of at least 14 orders of magnitude higher, is available.

A second question is how the nucleus can decay with about eight orders of magnitude shorter lifetime than what is predicted vs66 ; roy00  from energy versus lifetime relationships for a normal 4.5 MeV $`\alpha `$-transition (experimentally estimated $`2.5\times 10^8`$ as compared to predicted $`5\times 10^{16}`$ y). (A lifetime in the region of $`10^{16}`$ y is certainly impossible, since it implies the existence of about 100 mg of material in the studied samples).

In the following paragraphs similar effects seen in the study of various actinide fractions mar01b  produced via secondary reactions mar71 , and also in the study of the 16O+197Au mar96a ; mar96b  and the 28Si+181Ta mar01a  heavy ion reactions, are summarized. Based on the results of all these experiments, a consistent interpretation for the puzzling phenomena seen in nature is suggested. (See also Ref. mar02 ).

## II Unidentified $`\alpha `$-particle groups in actinides

In a study of actinide fractions from a W target which had been irradiated with 24-GeV protons, long-lived isomeric states were found in the neutron-deficient 236Am and 236Bk nuclei with respective half-lives of 0.6 y and $``$30 d mar87 . Their character however was not clear, being far from closed shell nuclei, where high spin isomers are known, and living much longer than the known fission isomers. In addition, several unidentified $`\alpha `$-particle groups were found in some actinide sources. Thus, 5.14 MeV (t1/2 = 3.8$`\pm `$1 y), 5.27 MeV (t1/2 = 625$`\pm `$84 d) and 5.53 MeV (t1/2 = 26$`\pm `$7 d) groups were respectively found in the Bk, Es and Lr-No sources mar87 ; mar01b  (See Fig. 1 and Table I). Similar to the situation with the 4.5 MeV group seen in nature, also here in the case of the latter unidentified groups, one can not understand their relatively low energies (e.g., 5.53 MeV in Lr-No as compared to typical g.s. to g.s. transitions of around 8 MeV (Column 6 of Table I), which have about 11 orders of magnitude larger penetrability factors (the ratio of Column 4 to Column 7 in Table I)), and their very enhanced character, having 105 \- 107 shorter half-lives than predicted from the systematics of energy versus half-life relationship for normal $`\alpha `$-decays vs66 ; roy00  (See Column 5 in Table I). The deduced evaporation-residue cross sections mar01b , in the mb region, are also several orders of magnitude larger than expected.

## III Study of the 16O+197Au reaction and long-lived high spin superdeformed isomeric states

Possible explanation for the above puzzling data comes from the study of the 16O+197Au reaction at ELab=80 MeV which is around the Coulomb barrier mar96a ; mar96b , and of the 28Si+181Ta reaction at ELab=125 MeV mar01a , about 10% below the Coulomb barrier. In the first reaction a 5.2 MeV $`\alpha `$-particle group with a half-life of about 90 m has been found in 210Fr. This group has the same unusual properties as the abnormal $`\alpha `$-particle groups found in the actinides and produced via secondary reactions, and of the 4.5 MeV found in nature. 5.2 MeV is a low energy as compared to 6.5 MeV, the g.s. to g.s. transition from 210Fr, and 90 m half-life is about 4$`\times `$105 enhanced as compared to the prediction vs66 ; roy00  for normal $`\alpha `$-particles of this energy from 210Fr. However, the 5.2 MeV group has been found in coincidence with $`\gamma `$-rays which fit the energies of a superdefermed band transitions. Therefore, the $`\alpha `$-decay is through a barrier of a superdeformed nucleus, and the large enhancement can quantitatively be understood mar96a  if one takes into account typical superdeformed radius parameters in the penetrability calculations. The data were consistently interpreted mar96a  in terms of production of a long-lived high spin isomeric state in the second well of the potential energy surface of 210Fr which decays, by a very enhanced $`\alpha `$-transition, to a high-spin state in the second well of 206At.

The predicted sat91 ; kri92  excitation energies of the second minima in 210Fr and nearby nuclei are above the proton separation energies aud93 . Therefore, the decay of isomeric states from the second minima, by emitting protons, is in principle possible. In a separate study of the same 16O+197Au reaction mar96b , long-lived proton radioactivities with half-lives of about 5.8 h and 67.3 h have been discovered. They were interpreted as due to very retarded decays from superdeformed isomeric states in the parent nuclei to normal deformed or to the ground states of the daughters. In particular, the indicated line with Ep = 2.19 MeV mar96b  may be associated with the predicted sat91  (Ep = 2.15 MeV) second minimum to ground state transition from 198Tl, which can be produced by three consecutive superdeformed to superdeformed $`\alpha `$-transitions from 210Fr.

## IV Study of the 28Si+181Ta reaction and long-lived high spin hyperdeformed isomeric states

The 28Si+181Ta reaction has been studied at ELab = 125 MeV, which is about 10% below the Coulomb barrier, and at ELab = 135 MeV mar01a . A fusion cross section of about 10 mb is predicted at 125 MeV using a coupled-channel deformation code fer85  with deformation parameters $`\beta _2`$ = 0.41 for 28Si and $`\beta _2`$ = 0.26 for 181Ta ram87  and allowing for 2+ and 3- excitations in 28Si. Only 2 $`\mu `$b is predicted when no deformations are included in the calculations. For 135 MeV the corresponding predicted fusion cross sections are 95 mb with deformations and 40 mb without.

Figure 2 (left) shows an $`\alpha `$ \- $`\gamma `$ two-dimensional coincidence plot obtained at ELab = 125 MeV. Quite a few coincidence events are seen between a relatively high energy $`\alpha `$-particle group around 8.6 MeV and various $`\gamma `$-rays. The half-life of this coincidence group has been measured mar01a  to be 40 d $``$ t1/2 $``$ 2.1 y. Figure 2 (right) shows that the $`\gamma `$-rays which are in coincidence with these high-energy $`\alpha `$-particles fit nicely with a J(J + 1) law assuming Ex = 4.42$`\times `$J(J +1) keV and $`\mathrm{\Delta }`$J = 1. Based on the observation of a Pt X-ray in coincidence with the 8.6 MeV $`\alpha `$’s and on kinematic arguments it was suggested mar01a  that the $`\alpha `$-transition is from 195Hg to 191Pt. (195Hg may be produced via 1p1n evaporation reaction and 3 consecutive IIImin$``$IIImin $`\alpha `$-decays. See below). An energy parameter of 4.42 keV is typical to superdeformed band $`\gamma `$-ray transitions in this region of nuclei.

An $`\alpha `$-energy of 8.6 MeV is a very high energy for 195Hg which does not decay by emitting $`\alpha `$-particles and its g.s. to g.s. $`Q_\alpha `$-value is 2.190 MeV aud93 . A half-life of 40 d is about 13 orders of magnitude too long as compared to the systematics of energy versus half-life relationship roy00  which predicts t$`{}_{1/2}{}^{}6\times 10^8`$ s. Since the $`\alpha `$-particles are in coincidence with a superdeformed band $`\gamma `$-ray transitions, the $`\alpha `$-decay is to the superdeformed well of the daughter nucleus. However, it could not be a IImin$``$IImin transition, since such a transition is very enhanced as opposed to the large retardation measured in the experiment. A consistent interpretation, both from the point of view of the high energy of the $`\alpha `$-particles and their very long lifetime, is that the decay is from a long-lived high spin (J$``$39/2) isomeric state in the IIImin, the hyperdeformed minimum how80 ; naz93 ; cwi94 ; kra98  of 195Hg, which decays by strongly retarded transition to the IImin of the potential in 191Pt mar01a . As seen in Fig. 3 the predicted $`Q_\alpha `$-value for such a transition is about 8.7 MeV, taking into account an extrapolated value from Ref. naz93  for the excitation energy of the IIImin in 195Hg and the predictions of Refs. sat91 ; kri92  for the excitation energy of the IImin in 191Pt. This value fits rather nicely with the measured $`Q_\alpha `$-value of about 8.8 MeV. (The excitation energy of the state in the third minimum of 195Hg was assumed to be around the rotational 39/2 state with estimated energy of Ex=2.2$`\times `$J(J +1) keV kra98 ).

## V Super- and Hyper-deformed Isomeric States in the Actinide Region

Based on the discovery of the long-lived super- and hyper-deformed isomeric states (Secs. III and IV), a consistent interpretation has been given mar01b  to the unidentified $`\alpha `$-particle groups seen in the actinide sources and described in Sec. II above. IImin$``$IImin and IIImin$``$IIImin $`\alpha `$-particle transition energies have been deduced from the predicted how80  excitation energies. Table II shows that the low energy 5.14, 5.27 and 5.53 MeV groups seen in the Bk, Es and No-Lr sources, can consistently be interpreted as due to the low-energy IImin$``$IImin transition from 238Am and IIImin$``$IIImin transitions from 247Es and 252No, respectively. Their energies are considerably lower than the corresponding g.s. to g.s. transitions (Column 6 in Table II).

Table III shows that the very enhanced measured half-lives of the low-energy $`\alpha `$-particle groups seen in the various actinide sources are consistent with calculated values mar01b , taking into account in the penetrability calculations the deformation parameters of the superdeformed and hyperdeformed isomeric states.

The potential energies as function of quadrupole deformations, taking from Ref. how80 , are shown in Fig. 4 for the 238Am, 238Cm, 247Es, and 248Fm nuclei. It is seen that in 238Am the inner and the outer barriers of the second minimum are quite large, while in 247Es and 248Fm the outer barriers of the second minima are small, and the inner barriers of the third minima are large. In fact, the third minima in 247Es and 248Fm are predicted to be the ground states of these nuclei, being 0.61 and 1.76 MeV below the normal, slightly deformed, ground states. Unfortunately there are no predictions in these cases for the potential at even larger deformations, beyond the third minimum. (In the case of 232Th cwi94  the outer barrier in the third minimum is quite high).

In Ref. mar01b  detailed estimates for the various production cross sections of the actinide nuclei, as well as of the superheavy element with Z = 112 and N $``$ 160, are given. It is argued that the relatively large fusion cross sections, in the mb region, are due to two effects. First, the compound nucleus is produced in an isomeric state in the second or third minimum of the potential, rather than in the normal ground state. As shown in Fig. 5 much less overlapping and penetration are needed under these conditions, and therefore the compound nucleus formation probability increases drastically. Secondly, in the secondary reaction experiment the projectile is a fragment which has been produced within 2$`\times `$10-14 s before interacting with another W nucleus in the target. During this short time it is at high excitation energy and quite deformed. Figure 6 gives the results of couple-channel calculations fer85  for the fusion cross section as function of bombarding energy for the 70Zn+186W reaction, taking into account the known deformation of 186W and various deformations of the projectile. Figure 6d shows the results when the projectile has a deformation which is typical for the second minimum of the potential. It is seen that, due to the reduced Coulomb repulsion between the two nuclei for the tip to tip configuration, the cross section reduces very slowly with decreasing bombarding energy.

An idea about the relative importance of the above two effects can be deduced from the following arguments: The difference from a typical cross section of about 1 pb hof96  obtained in the 70Zn + 208Pb reaction producing the nucleus 277112 in its ground state, to a cross section of about 20 nb producing 271(2)112 in an isomeric state via the 88Sr + 184W reaction mar93 , is due to the first effect. The additional difference from 20 nb to about 3.8 mb mar01b  of producing element 112 in an isomeric state via secondary reactions, is due to the second effect.

## VI Summary of the properties of the super- and hyper-deformed isomeric states

Figure 7 summarizes the results obtained about the super- and hyper-deformed isomeric states. The nucleus may have a long lifetime in its ground state, but also in long-lived isomeric states in the second and third minima of the potential-energy surfaces. Long-lived superdeformed isomeric states may decay by very enhanced $`\alpha `$-particles to superdeformed states in the daughter nuclei, or by strongly retarded $`\alpha `$-particles to the normal deformed states in the corresponding nuclei. It also may decay by very retarded proton radioactivity. Similarly, hyperdeformed isomeric states may decay by strongly enhanced $`\alpha `$-particle decay to the hyperdeformed potential well in the daughter, or by very retarded $`\alpha `$-decay to the superdeformed minimum in the same nucleus. All these extremely unusual decay properties have been discovered experimentally as summarized in Fig. 7.

It should be mentioned that the half-lives of the newly discovered isomeric states are longer than those of their corresponding ground states. Such a comparison for the isomeric states in the actinide region is presented in Table IV.

It should be mentioned that back in 1969 nil69  a new type of fission isomeric state has been predicted for nuclei with N $``$ 144-150, A specialization energy in excess of 4 MeV for the second barrier was predicted for a $`\frac{11}{2}^{}`$ state, which is associated with a factor of about 1015 increase in the half-life of a normal fission shape isomer.

## VII Super- and hyper-deformed isomeric states and the puzzling phenomena seen in nature

The discovered super- and hyper-deformed long-lived isomeric states enable one to understand the previously puzzling phenomena seen in nature (See the Introduction).

The source for the Po halos hen39 ; gen68  may be such isomeric states in isotopes with Z $``$ 84 which decayed, by $`\beta `$\- or $`\gamma `$-decays, to the ground states of 210Po, 214Po and 218Po.

The low energy $`\alpha `$-particles around 4.5 MeV cher63 ; che64 ; cher68 ; mei70  can consistently be interpreted as due to a very enhanced IIImin $``$ IIImin transition in Z$``$108 and A$``$271. The predicted mar96a ; mar01b  half-life in this case is around 109 y, as seen in Table V. This resolves the first difficulty in understanding these data, namely the about eight orders of magnitude shorter lifetime than what is predicted vs66 ; roy00  from energy versus lifetime relationship for a normal $`\alpha `$-transition. (About $`2.5\times 10^8`$ y estimated experimentally as compared to $`5\times 10^{16}`$ y. See the Introduction).

In addition, an extrapolation of the deduced $`\alpha `$-energies for IIImin$``$IIImin transitions from the predictions of Ref. how80  shows that for Z=108, Eα of about 4.5 MeV corresponds to N$``$162 (see Fig. 8). This is consistent with the suggestion mei70  that 247Cm may be a descendent of the superheavy element with Z=108 which decays by the 4.5 MeV $`\alpha `$-particles, since 247Cm can be obtained from $`{}_{108}{}^{}{}_{}{}^{271}`$Hs163 by successive six $`\alpha `$-decays. Another possibility is that the long-lived isotope is 267Hs which decays by two $`\beta ^+`$ or electron capture decays to 267Sg which then follows by five successive $`\alpha `$-decays to 247Cm. It should however be mentioned that in principle the above 4.5 MeV $`\alpha `$-particles may also be due to a strongly retarded IImin$``$Imin or IIImin$``$IImin transition in the region of Os itself. (For normal 4.5 MeV $`\alpha `$-particles in Os the expected vs66 ; roy00  half-life is about 1 y. Such short-lived nuclide can not exist in nature).

## VIII Summary

It was shown that the newly discovered long-lived super- and hyper-deformed isomeric states can provide consistent interpretations to two previously unexplained phenomena seen in nature. Thus, the Po halos can be understood as due to the existence of such isomeric states in nuclei with Z values around 84 and atomic masses in the region of 210 - 218. The observed 4.5 MeV $`\alpha `$-particle group can be understood as due to a low energy and strongly enhanced hyperdeformed to hyperdeformed transition in a nucleus with Z = 108 and A $``$ 271.

It seems to us that the existence of superheavy elements in nature is not impossible.

## IX Acknowledgements

We appreciate very much the valuable discussions with J. L. Weil and N. Zeldes.


format: text

text:
# Ab-initio density functional studies of stepped TaC surfaces

## Abstract

We report on density functional total energy calculations of the step formation and interaction energies for vicinal TaC(001) surfaces. Our calculations show that double and triple-height steps are favored over single-height steps for a given vicinal orientation, which is in agreement with recent experimental observations. We provide a description of steps in terms of atomic displacements and charge localization and predict an experimentally observable rumpled structure of the step-edges, where the Ta atoms undergo larger displacements compared to the C atoms.

The stepped surfaces of transition metal carbides (TiC, TaC, etc.) are technologically important due to their applications as surface catalysts with high corrosion resistance. From a fundamental point of view, these surfaces have received attention as they provide a rich ground for studying faceting transitions that involve single and multiple-height steps. In a series of experiments, Zuo and coworkers Zuo310 Zuo910  have investigated the structure of several surfaces vicinal to TaC(001) and found that multiple-height steps are favored over single-height steps in all the cases. Motivated by these experiments, we perform ab-initio density functional calculations to obtain the first quantitative results for the step formation and interaction energies for steps of different heights on these surfaces.

The preference for single or multiple-height steps for a certain vicinal orientation is determined by the energy required to create an isolated step of a certain height and the repulsive interactions between these steps. In general, it costs more energy to create multiple-height steps, as the number of bonds that are broken in the process of creating a step increases with its height. On the other hand, the energetic contribution from the repulsive step-step interactions can be the lower in the case of a vicinal surface with multiple-height steps due to a lowering of the number of step pairs per unit length. As we will see, both of these effects are borne out by our calculations. Furthermore, we will show that the increase in the formation energies of double and triple-height steps over the single-height steps is not large enough to offset the effect of step-step interactions. Consequently, the former types of steps are favored for the vicinal orientations that we consider. In what follows, we also will report on the structures of different types of steps in terms of charge density and atomic displacements, and develop a phenomenological model for the electrostatic step interactions.

The density functional calculations were carried out with the VASP package Vasp , using the projector augmented-wave pseudopotentials paw  and the Perdew-Wang functional form pw91  for exchange correlation energy. Bulk calculations with an 8-atom cell and a 35 k-point Brillouin zone sampling gave an optimum Ta-C separation of $`a=2.2415`$Å. For surface calculations, the Brillouin zone was sampled using a $`\mathrm{\Gamma }`$-centered $`8\times 8\times 1`$ grid. This sampling yielded 15 k-points for TaC(001) and 21 to 25 k-points for the vicinal surfaces. The ions were relaxed using a conjugate-gradient algorithm until the total energy converged to $`0.01`$eV. The energy cut-off for the plane waves was set to 400eV (29.40 Ry) in all the calculations.

Before we proceed with the discussion of vicinal surfaces, we compare the predictions of the surface structure of TaC(001) obtained using the present model with experimental observations and previous theoretical studies. It is well-known Gruzalski Kobayashi  that this surface exhibits a rumpling reconstruction, where the C atoms are displaced out of the surface while the Ta atoms are pulled inwards. It can be seen from Table 1 that our results for the relative displacements of the atoms in the first and second surface layers are in close agreement with available experimental Gruzalski  and theoretical Kobayashi  data.

For vicinal surfaces, we used supercells as illustrated in Fig. 1, where $`L_x`$ and $`L_z`$ denote the terrace-width of the stepped surface and height of the supercell, respectively. The dimension of the supercell in the $`y`$-direction ($`L_y`$) is determined by the period in the direction parallel to the step, which in the present case is the lattice constant of TaC, $`2a`$. To create the steps, we employ shifted (i.e. non-orthogonal) boundary conditions Poon , in which the amount of shift in the $`z`$\- direction determines the height of the steps. The structures of the single (Sh), double (Dh) and triple (Th) -height steps that we consider in the present work are shown in Fig. 1. All calculations on vicinal surfaces were carried out using a slab of TaC with 8 atomic rows (17.932 Å) and a vacuum thickness of 10Å. In order to ensure that these results are not influenced by finite-size effects, we repeated the calculations for certain selected step structures and terrace widths by increasing the cell thickness to 10 atomic rows and the dimension of the vacuum to 15Å; the results were found to change by less than 5% in all the cases that were considered.

The energetics of stepped surfaces can be understood by considering the ledge energy, defined as $`\lambda _n=(EN_pe_b\gamma _0A)/2L_y`$ Poon , where $`E`$ is the total energy of the $`N_p`$ Ta-C pairs in the slab, $`e_b=22.1536`$eV is the bulk energy per pair, $`\gamma _0=95.53`$meV/Å2 is the surface energy of the TaC(001) surface and the subscript $`n`$ denotes the step-height. The ledge energy is the energy per unit length of the vicinal surface in excess of the surface energy of the terraces that separate the steps, and includes both the step formation and interaction energies. Using the fact that both the elastic and electrostatic effects give rise to dipolar interactions marchenko ; Jay , the ledge energy can be expressed as

$$\lambda _n=\lambda _n^f+\frac{\lambda _n^d}{L_x^2},$$
(1)
where $`\lambda _n^f`$ and $`\lambda _n^d`$ denote the formation energy and the dipolar interaction strength of a step with height $`na`$, respectively. The computed ledge energies for the three types of steps are plotted in Fig. 2, along with linear fits to the functional form assumed in Eq. (1) later . The fitting parameters $`\lambda _n^f`$ and $`\lambda _n^d`$ are given in Table 2.

It can be seen from Table 2 that the formation energies of the steps increase with their heights, in agreement with bond counting arguments presented earlier. The dipolar interactions, on the other hand, do not show a monotonic trend; the interaction strength of the Dh step is smaller than the corresponding values for the Sh and Th steps. The relative importance of these two contributions can be understood by considering the surface energy of a vicinal surface made of steps with height $`na`$, given by

$$\gamma _n(\theta )=\gamma _0\mathrm{cos}\theta +\beta _n^f|\mathrm{sin}\theta |+\beta _n^d\frac{|\mathrm{sin}^3\theta |}{\mathrm{cos}^2\theta },$$
(2)
where $`\theta `$ is the vicinal angle and the parameters $`\beta _n^f=\lambda _n^f/(na)`$ and $`\beta _n^d=\lambda _n^d/(na)^3`$ denote scaled step formation and interaction contributions, respectively. Using the values of these parameters tabulated in Table 2, we find that both the scaled formation and interaction parts show a monotonic decrease with increasing step height, indicating that multiple-step heights are favored over the single height steps for any vicinal orientation. In the following paragraph we consider experimental work of Zuo and coworkers Zuo310 Zuo910  and show that the predictions of our calculations are in agreement with their observations.

Using a statistical analysis einstein  of the step separation distributions on TaC(103) and (102) surfaces, Zuo and coworkers have determined that the former surface consists of a large number of triple-height steps and a smaller number of double-height steps while the latter surface consists of almost equal amounts of areas that contain either triple or quadruple-height steps. In order to understand these results, in Table 3, we have used Eq. (2) and the data in Table 2 to calculate the surface energies of these vicinal surfaces made up of Sh, Dh and Th steps. For both the surfaces considered in the experimental work, we find that the single-step vicinal is much larger (by $``$ 10-20 meV/Å2) in energy than the vicinals with multiple-height steps. Furthermore, the triple-height steps are favored over the double-height steps (by $``$ 4 meV/Å2) in both the cases, explaining their stability and their presence on (103) and (102) surfaces. The presence of a few Dh steps and the complete absence of Sh steps on (103) surfaces is consistent with the fact that the former is closer in energy to the Th steps than the latter by about 8 meV/Å2 (refer to Table 3). At the present time, we are unable to consider the energetics of quadruple-height steps due to the size of this model limit .

We now turn our attention to the description of the steps in terms of the atomic displacements at the step-edges, which are shown in Fig. 3 for the (105)-Sh and the (102)-Dh surfaces. The figure shows that the atoms at the step-edges undergo both horizontal ($`x`$) and vertical ($`z`$) displacements. On moving a few atomic spacings away from the step-edge, the atoms on the terraces are predominantly displaced in the vertical direction, as in the case of the (001) surface. Overall, the displacement field of the step resembles the field produced by a force-dipole marchenko  located at the step-edge, though there are new features that emerge. In particular, the step-edge is rumpled, such that the horizontal displacements of the Ta atoms at the step-edges are significantly larger than the corresponding displacements of the C atoms. Since both the components of the rumpling vector $`𝐬`$ given in Fig. 3 are comparable to the rumpling amplitudes for Ta(001) given in Table 1, we believe that this effect could be observed in experiments. The step rumpling also leads to formation of electric dipoles, which will be considered next.

The magnitudes of the electric dipoles at the step-edges due to rumpling can be estimated as $`Q|𝐬|`$, where $`Q`$ is the amount of charge transferred from C to Ta due to the partially ionic character of the TaC-bond. Since $`Q|e|`$ and $`|𝐬|0.1a`$ (refer to Fig. 3), where $`e`$ is the electronic charge, the linear dipole density due to step rumpling is $`P0.1|e|`$. In addition to the dipoles that arise as a result of step-rumpling, we also find that there are additional dipoles that are created due to charge distortions at the step-edge. We observe that the valence shell around the C atoms expands out of the surface leading to formation of electric dipoles, denoted by $`𝐩`$ and $`𝐩^{}`$ in Fig. 4. Such electronic distortions also exist for the Ta surface atoms, but to a much smaller extent. The magnitude of these dipoles can be obtained from the electron localization functions, which are shown in Fig. 4 for the (105)-Sh and the (102)-Dh surfaces. Our calculations show that the typical magnitude the linear dipole density due to charge spill-out at the step-edge is $`P0.30.7|e|`$.

The interaction energy between steps characterized by the effective electrostatic dipole density $`𝐏`$ and the force moment $`𝐃=(D_x,D_z)`$ is given by marchenko ; Jay  :

$$\frac{\lambda _n^d}{L_x^2}=\frac{\pi ^2(P_{}^2P_{||}^2)}{3L_x^2}+\frac{\pi (1\nu ^2)(\tau ^2n^2a^2+D_x^2)}{3EL_x^2},$$
(3)
where $`P_{||}(P_{}`$) is the component of $`𝐏`$ parallel (perpendicular) to the unit-vector $`𝐧`$ in Fig. 4, $`\tau `$ is the surface stress which generates the $`z`$-component of the elastic dipole moment ($`D_z=\tau na`$), $`E`$ is the Young’s modulus, and $`\nu `$ is the Poisson’s ratio toth . While separating the elastic and electrostatic contributions to step interactions is a difficult task, we can use the information from Fig. 4 to obtain estimates for these two effects.

First, observe that the dipole density due to step-rumpling is about 20-30% of the dipole density arising from charge spill-out; it is therefore reasonable to calculate the electrostatic interactions by focusing on the latter effect. Next, we see from Fig. 4 that compared to the Sh-step, the Dh-step has a larger value of $`P_{||}`$ due to the presence of an additional C atom with dipole $`𝐩^{}`$ that is aligned closely with the vector $`𝐧`$. With increasing step-height, the number of such atoms increases, leading to even larger values of $`P_{||}`$ and a monotonic decrease in the electrostatic contribution (refer to Eq. (3)). However, we see from Table. 2 that the step interaction parameters show a non-monotonic trend, which we attribute to an increase in the strength of elastic interactions with the height of steps in the following paragraph.

Using Eq.(3), we calculate the electrostatic contribution to the interactions of Sh steps to be $``$ 1eVÅ, which is close to the value of $`\lambda _1^d`$ given in Table 2, indicating that the step interactions are dominated by the electrostatic effects. This observation is also in agreement with the fact that a typical value of surface stress $`\tau `$ 100meV/Å2 yields a small repulsive elastic contribution which is $``$ 0.01meVÅ. In the case of Dh-steps, a decrease in step interaction parameter ($`\lambda _2^d`$) is consistent with a decrease in the electrostatic contribution with increasing step-height. However, a subsequent increase in the interaction parameter ($`\lambda _3^d`$) for the Th-step can only be explained if the magnitude of the elastic dipole, $`|D|=\sqrt{D_x^2+D_z^2}`$ increases with the height of the step. In this case, we expect both the electrostatic and elastic contributions to be comparable in magnitude.

In summary, by calculating step formation and interaction energies we have shown that Dh and Th steps lead to more stable vicinal surfaces, a result consistent with experimental observations Zuo310 Zuo910 . We have described the atomic displacements of the surfaces and proposed a simple model for the electrostatic interaction of the steps in terms of electric dipoles of carbon atoms and step rumpling.

We gratefully acknowledge research support from the National Science Foundation through grants CMS-0093714 and CMS-0210095 and the Brown University MRSEC program. Computational support for this work was provided by the National Center for Supercomputing Applications through grant DMR-020032N and the Graduate School at Brown University through the Salomon Research Award.


text:
# High-redshift objects and the generalized Chaplygin gas

## I Introduction

The question about the nature of the energy content of the Universe was always a central topic in Cosmology. In the last few years, however, such a discussion has become even more critical due to a convergence of observational results that strongly support the idea of an accelerated universe dominated by cold dark matter (CDM) and an exotic fluid with a large negative pressure. Dark matter is inferred from galactic rotation curves which show a general behavior that is significantly different from that one predicted by Newtonian mechanics. The most direct evidence for the dark energy component or “quintessence” cames from distance measurements of type Ia supernovae (SNe Ia) which indicate that the expansion of te Universe is speeding up, not slowing down perlmutter . Another important evidence arises from a discrepancy between the measurements of the cosmic microwave background (CMB) anysotropies which indicate $`\mathrm{\Omega }_{\mathrm{Total}}=1.1\pm 0.07`$ bern  and clustering estimates providing $`\mathrm{\Omega }_m=0.3\pm 01`$ calb . While the combination of these two latter results implies the existence of a smooth component of energy that contibutes with $`2/3`$ of the critical density, the SNe Ia results requires this component to have a negative pressure which leads to a repulsive gravity.

The main distinction between these two dominant forms of energy (or matter) existent in the Universe is manisfested through their gravitational effects. Cold dark matter agglomerates at small scales whereas the dark energy seems to be a smooth component, a fact that is directly linked to the equation of state of both components. Recently, the idea of a unified description for the CDM and dark energy scenarios has received much attention uni ; wat ; kasu ; pad . For example, Wetterich wat  suggested that dark matter migth consist of quintessence lumps while Kasuya kasu  showed that spintessence-like scenarios are generally unstable to formation of $`Q`$ balls which behave as pressureless matter. More recently, Padmanabhan and Choudhury pad  investigated such a possibility via a string theory motivated tachyonic field.

Another interesting attempt of unification was suggested by Kamenshchik et al. kame  and developed by Bilić et al. bilic . It refers to an exotic fluid, the so-called Chaplygin gas, whose equation of state is given by bento

$$p=A/\rho ^\alpha ,$$
(1)
with $`\alpha =1`$ and $`A`$ a positive constant. In actual fact, the above equation for $`\alpha 1`$ constitutes a generalization of the original Chaplygin gas equation of state recently proposed in Ref. bento . By inserting the Eq. (1) into the energy conservation law we find the following expression for the density of this generalized Chaplygin gas

$$\rho _{Cg}=\left[A+B\left(\frac{R_o}{R}\right)^{3(1+\alpha )}\right]^{\frac{1}{1+\alpha }},$$
(2)
or, equivalently,

$$\rho _{Cg}=\rho _{Cg_o}\left[A_s+(1A_s)\left(\frac{R_o}{R}\right)^{3(1+\alpha )}\right]^{\frac{1}{1+\alpha }},$$
(3)
where the subscript $`o`$ denotes present day quantities, $`R(t)`$ is the cosmological scale factor, $`B=\rho _{Cg_o}^{1+\alpha }A`$ is a constant and $`A_s=A/\rho _{Cg_o}^{1+\alpha }`$ is a quantity related with the sound speed for the Chaplygin gas today. As can be seen from the above equations, the Chaplygin gas interpolates between non-relativistic matter ($`\rho _{Cg}(R0)\sqrt{B}/R^3`$) and negative-pressure dark component regimes ($`\rho _{Cg}(R\mathrm{})\sqrt{A}`$).

From the theoretical viewpoint, an interesting connection between the Chaplygin gas equation of state and String theory has been identified hoppe ; hoppe1  (see also jac  for a detailed review). As explained in these references, a Chaplygin gas-type equation of state is associated with the parametrization invariant Nambu-Goto $`d`$-brane action in a $`d+2`$ spacetime. In the light-cone parametrization, such an action reduces itself to the action of a Newtonian fluid which obeys Eq. (1) with $`\alpha =1`$ so that the Chaplygin gas corresponds effectively to a gas of $`d`$-branes in a $`d+2`$ spacetime. Moreover, the Chaplygin gas is the only gas known to admit supersymmetric generalization jac . From the observational viewpoint, these cosmological scenarios have interesting features gorini  which make them in agreement with the most recent observations of SNe Ia fabris1 ; avelino ; ioav , the location of the CMB peaks b11 , age estimates of globular clusters, as well as with the current gravitational lensing data aba .

In this paper we discuss new observational constraints on Chaplygin gas cosmologies from age considerations due to the existence of three recently reported old high-redshift objects, namely, the LBDS 53W091, a 3.5-Gyr-old radio galaxy at $`z=1.55`$ dunlop , the LBDS 53W069, a 4.0-Gyr-old radio galaxy at $`z=1.43`$ dunlop1  and a quasar, the APM 08279+5255 at $`z=3.91`$ whose age is estimated between 2 - 3 Gyr karm . Two different cases will be studied: a flat scenario in which the generalized Chaplygin gas together with the observed baryonic content are responsible by the dynamics of the present-day Universe \[unifying dark matter-energy\] (UDME) and a flat scenario driven by non-relativistic matter plus the generalized Chaplygin gas (GCgCDM). For UDME scenarios we adopt in our computations $`\mathrm{\Omega }_b=0.04`$, in accordance with the latest measurements of the Hubble parameter friedman  and of the baryon density at nucleosynthesis burles . For GCgCDM models we assume $`\mathrm{\Omega }_m=0.3`$, as sugested by dynamical estimates on scales up to about $`2h^1`$ calb . For the sake of completeness an additional analysis for the conventional case ($`\alpha =1`$) is also included. The plan of this paper is as follows. In Sec. II we present the most relevant formulas to our analysis, as well as the main assumptions for the age-redshift test. We then proceed to discuss the constraints provided by this test on the cosmological scenarios decribed above in Sec. III. We end this paper by summarizing the main results in the conclusion section.

## II Age-redshift Test

The general Friedmann’s equation for the kind of models we are considering is

$`({\displaystyle \frac{\dot{R}}{R}})^2`$ $`=`$ $`H_o^2\{\mathrm{\Omega }_j({\displaystyle \frac{R_o}{R}})^3+`$
$`+(1\mathrm{\Omega }_j)[A_s+(1A_s)({\displaystyle \frac{R_o}{R}})^{3(\alpha +1)}]^{\frac{1}{\alpha +1}}\},`$
where $`H_o`$ is the present value of the Hubble parameter and $`\mathrm{\Omega }_j`$ stands for the baryonic matter density parameter ($`j=b`$) in UDME scenarios and the baryonic + dark matter density parameter ($`j=m`$) in GCgCDM models.

The age-redshift relation as a function of the observable parameters is written as

$`t_z={\displaystyle \frac{1}{H_o}}`$ $`{\displaystyle _0^{(1+z)^1}}{\displaystyle \frac{dx}{xf(\mathrm{\Omega }_j,A_s,\alpha ,x)}}`$
$`={\displaystyle \frac{1}{H_o}}g(\mathrm{\Omega }_j,A_s,\alpha ,z),`$
where $`x`$ is a convenient integration variable and the dimensionless function $`f(\mathrm{\Omega }_j,A_s,\alpha ,x)`$ is given by

$`f(\mathrm{\Omega }_j,A_s,\alpha ,x)=\sqrt{{\displaystyle \frac{\mathrm{\Omega }_j}{x^3}}+(1\mathrm{\Omega }_j)\left[A_s+{\displaystyle \frac{(1A_s)}{x^{3(\alpha +1)}}}\right]^{\frac{1}{\alpha +1}}}`$ (6)
The total expanding age of the Universe is obtained by taking $`z=0`$ in Eq. (II). As one may check, for $`\alpha =1`$ and $`A_s=1`$ Eq. (II) reduces to the $`\mathrm{\Lambda }`$CDM case while for $`\alpha =1`$ and $`A_s=0`$ the standard relation \[$`t_z=\frac{2}{3}H_o^1(1+z)^{\frac{3}{2}}`$\] is recovered. A recent discussion about the globular clusters constraints on the total expanding age in the context of Chaplygin gas cosmologies can be found in aba .

In order to constrain the cosmological parameters from the age estimates of the above mentioned high-$`z`$ objects we take for granted that the age of the Universe at a given redshift is bigger than or at least equal to the age of its oldest objects. In this case, the comparison of these two quantities implies a lower (upper) bound for $`A_s`$ ($`\alpha `$), since the predicted age of the Universe increases (decreases) for larger values of this quantity (see Fig. 1). Note also that the age parameter $`H_ot_o`$ is an almost insensitive function to the parameter $`\alpha `$ but that it depends strongly on variations of $`A_s`$. This means that age considerations will be much more efficient to constrain the sound speed $`A_s`$ than the values of the parameter $`\alpha `$.

To quantify the above considerations we follow jailson  and introduce the expression

$$\frac{t_z}{t_g}=\frac{g(\mathrm{\Omega }_j,A_s,\alpha ,z)}{H_ot_g}1,$$
(7)
where $`t_g`$ is the age of an arbitrary object, say, a galaxy or a quasar at a given redshift $`z`$ and $`g(\mathrm{\Omega }_j,A_s,\alpha ,z)`$ is the dimensionless factor defined in Eq. (5). For each extragalatic object, the denominator of the above equation defines a dimensionless age parameter $`T_g=H_ot_g`$. In particular, the 3.5-Gyr-old galaxy (53W091) at $`z=1.55`$ yields $`T_g=3.5H_o`$Gyr which, for the most recent determinations of the Hubble parameter, $`H_o=72\pm 8`$ $`\mathrm{kms}^1\mathrm{Mpc}^1`$ friedman , takes values on the interval $`0.229T_g0.286`$. It thus follows that $`T_g0.229`$. Therefore, for a given value of $`H_o`$, only models having an expanding age bigger than this value at $`z=1.55`$ will be compatible with the existence of this object. Naturally, similar considerations may also be applied to the 4.0-Gyr-old galaxy (53W069) at $`z=1.43`$ and to the 2-Gyr-old quasar (APM 08279+5255) at $`z=3.91`$ . In this case, we obtain, respectively, $`T_g0.261`$ and $`T_g0.131`$. To assure the robustness of the limits, we have systematically adopted in our computations the minimal value of the Hubble parameter, i.e., $`H_o=64`$ $`\mathrm{kms}^1\mathrm{Mpc}^1`$, as well as the underestimated age of the objects. In other words, it means that conservative bounds are always favored in the estimates presented here (see jailson  for details).

## III discussion

Figures 2a and 2b show the parameter space $`A_s\alpha `$ for a fixed value of the dimensionless age parameter $`H_ot_z`$ for UDME and GCgCDM scenarios, respectively. For a given object, each contour represents the minimal value of its age parameter at the respective redshift with the arrows indicating the available parameter space allowed by each object. As discussed earlier, the main constraints from this kind of cosmological test are on the value of the parameter $`A_s`$ (see Fig. 1). Note also that the allowed range for this parameter is reasonably narrow. For example, for UDME scenarios the age-redshift relation for the LBDS 53W091 and LBDS 53W069 requires, respectively, $`A_s0.52`$ and $`A_s0.58`$ while the same analysis for GCgCDM models provides $`A_s0.72`$ and $`A_s0.80`$. As physically expected, the limits from age considerations are much more restrictive for GCgCDM models than for UDME scenarios. It happens because the larger the contribution of non-relativistic matter ($`\mathrm{\Omega }_j`$) the smaller the predicted age of the Universe at a given redshift and, as a consequence, the larger the value of the parameter $`A_s`$ that is required in order to fit the observational data. The most restrictive bounds on $`A_s`$ are provided by the quasar APM 08279+5255 at $`z=3.91`$ whose age is estimated to be $`2.0`$ Gyr karm . In this case, we find $`A_s0.81`$ for UDME models. Our analysis also reveals that GCgCDM scenarios with $`\mathrm{\Omega }_m=0.3`$ are not compatible with the existence of this quasar once the predicted age of the Universe at $`z=3.91`$ is smaller than the underestimated age for this object. The maximum age predicted by this model at this redshift is 1.7 Gyr ($`H_o=64`$ $`\mathrm{kms}^1\mathrm{Mpc}^1`$) for values of $`\alpha =0`$ and $`A_s=1`$ (the point of maximum age; see Fig. 1). By inverting the analysis, i.e., by fixing the values of $`\alpha `$ and $`A_s`$, it is also possible to infer the maximum allowed value of the matter density parameter in order to make GCgCDM models compatible with the existence of this particular object. For $`\alpha =0`$ and $`A_s=1`$, we find $`\mathrm{\Omega }_m0.21`$. In other words, it means that if the age estimates for the quasar APM 08279+5255 are correct there is an ”age crisis” in the context of GCgCDM models for values of the matter density parameter $`\mathrm{\Omega }_m0.21`$. We still recall, in line with the arguments presented in karm , that recent x-ray observations show an Fe/O ratio for this object that is compatible with an age of 3 Gyr. In this case, GCgCDM models are compatible with the existence of such a object only for values of $`\mathrm{\Omega }_m<0.1`$. The restrictive bounds imposed by the age estimates of the quasar APM 08279+5255 on $`\mathrm{\Lambda }`$CDM models, quintessence scenarios with a equation of state $`p=\omega \rho `$ ($`1\omega <0`$), as well as on the first epoch of quasar formation can be found in jnew .

In Fig. 3 we show the $`A_s\mathrm{\Omega }_m`$ diagram allowed by the age estimates of the above mentioned objects for the specific case in which $`\alpha =1`$ (Chaplygin gas cosmologies). As in Fig. 2, the arrows indicate the available parameter space allowed by each object. The shadowed horizontal region corresponds to the observed interval $`\mathrm{\Omega }_m=0.20.4`$ calb  which now is used to fix the lower bounds to $`A_s`$. By considering this interval, the LBDS 53W091 and LBDS 53W069 provides, respectively, $`A_s0.85`$, $`A_s0.96`$ and $`A_s0.90`$ and $`A_s0.99`$. These values are even more restrictive than those obtained in the previous analyses because the predicted age of the Universe is smaller for larger values of $`\alpha `$. Such limits also provide a minimal total age of the Universe of the order of 13 Gyr. Finally, as expected from previous analyses, the quasar APM 08279+5255 provides the most restrictive bounds on these cosmologies. In reality, its existence is not compatible with Chaplygin gas cosmologies ($`\alpha =1`$) unless the matter density parameter is $`0.17`$. Such a result may be used to reinforce the idea of dark matter-energy unification once UDME models are not only compatible with the existence of these high-$`z`$ objects (and, as a consequence, with general age considerations) but also provide the best fit for the SNe data fabris1 . The main results of the present paper are summarized in Table I.

## IV conclusion

We have investigated new observational constraints from age estimates of high-$`z`$ objects on generalized Chaplygin gas cosmologies. Two diferent cases have been analysed, namely, UDME scenarios in which the dynamics of the present day Universe is completely determined by the generalized Chaplygin gas and the observed baryonic content ($`\mathrm{\Omega }_b=0.04`$) and GCgCDM models in which the generalized Chaplygin gas plays the role of dark energy only and is responsable by the dynamics of the Universe together with the dark matter ($`\mathrm{\Omega }_m=0.3`$). The former kind of cosmological scenarios is inspired by the ideas of dark matter-energy unification while the latter follows the conventional “quintessence” program. By considering the age estimates of the radio galaxies LBDS 53W091, LBDS 53W069 and of the quasar APM 08279+5255, we have derived very restrictive constraints on the free parameters of these models (see Table I). In particular, we have found that, similarly to models with a relic cosmological constant, there is no “age of the Universe problem” in the context of UDME scenarios while GCgCDM models are imcompatible with the age estimates of the quasar APM 08279+5255 for values of $`\mathrm{\Omega }0.21`$. Such result may be understood as a backup to the idea of dark matter-energy unification once UDME models also provide the best fit for SNe Ia data fabris1 . However, we emphasize that only with new and more precise set of observations will be possible to show whether or not this class of models constitutes a viable possibility of unification for the dark matter and dark energy scenarios.

###### Acknowledgements.

JSA is supported by the Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq - Brasil) and CNPq (62.0053/01-1-PADCT III/Milenio).