In this section we return to the topic of the description of nuclei on the prolate side of deformation. Molecular structures were predicted in the early stages of the understanding of the structure of light nuclei [24] and have been studied extensively [25,26,27,28,29].
It has been shown above that the prolate nuclei have well-developed cluster structures when the shells are closed and that these clusters are those associated with spherical nuclei such as \(^4\)He, \(^{16}\)O and \(^{40}\)Ca as the clusters. The subset of nuclei that are \(\alpha \)-conjugate and have the property that each harmonic oscillator level is fully occupied, is relatively small. The question as to what happens when valence neutrons are added to such cluster systems needs therefore to be also understood.
In instances when the cluster structure is well-developed and a valence neutron (or proton) is added, it is found that the underlying clustering has a profound impact on the structure of the states. The orbitals of the valence particle are described in terms of molecular orbitals formed from the linear combination of the individual orbitals at each cluster centre [1, 2].
There are some simple examples of such cluster states which include the case of \(^9\)Be. Here the valence neutron lies in a p-orbital outside the \(\alpha \)-particle core. The linear combination of the p-orbitals gives rise to molecular \(\pi \) and \(\sigma \)-bonds. These two molecular orbitals correspond to linear combinations of p-type (\(L=1\)) orbitals at the two centres. The \(\sigma \) molecular orbital has the densities of the dumbbell shape of the p-orbital aligned with the separation axis, with a projection of the angular momentum of the molecular orbital onto that axis of zero. The \(\pi \)-orbital has the dumbbell densities perpendicular to the separation and with an orbital angular momentum projection of 1\(\hbar \). These delocalised orbitals result in the binding of the two \(\alpha \)-particles, which are unbound in \(^8\)Be. In this instance, the molecular orbitals can be traced to collection of orbitals with a degeneracy of 6 in Fig. 1 which lie immediately above the two levels labelled with degeneracy 2 at a deformation of 2:1 (\(\delta _{OSC}=0.6\)). These latter two levels would be those occupied by an \(^8\)Be nucleus in the ground state. In other words, the molecular orbitals associated with \(^9\)Be are the next available orbitals once the two \(\alpha \) cluster system has been formed and hence would be associated with low-lying states in \(^9\)Be, as observed experimentally [2].
A recent study has examined the nature of all of the orbitals above the closure of a shell related to a cluster structure [8].
Figures 11 and 12 show two cases. These correspond to building the molecular orbitals around the cluster structures \(^{16}\)O+\(^{16}\)O and \(^{40}\)Ca+\(^{40}\)Ca, i.e. \(^{33}\)S and \(^{81}\)Zr.
\(^{33}\)S can be considered as a 2:1 deformed nucleus with two \(^{16}\)O clusters with a delocalised neutron. In the DHO model, where the oscillation frequency in the z-direction is half that in the x or y directions, the orbitals occupied linked to \(^{32}\)S are \([n_x,n_y,n_z]=\) [0,0,0], [0,0,1], [0,0,2], [0,1,0], [1,0,0], [0,0,3], [0,1,1] and [1,0,1]. The orbitals available, associated with the next shell closure, for the valence neutron are [0,0,4], [0,1,2], [1,0,2], [0,2,0], [2,0,0] and [1,1,0], these are all degenerate. In the two-centre description, each \(^{16}\)O cluster occupies the orbitals [0,0,0], [1,0,0], [0,1,0] and [0,0,1], which leaves the following orbitals available for the valence neutron centred on each cluster \([n_x,n_y,n_z]=\) [0,0,2], [0,2,0], [2,0,0], [0,1,1], [1,0,1] and [1,1,0]. Linear combinations of these latter orbitals give rise to those in the DHO in a 1 to 1 match.
Given that the neutron could exist at either cluster centre with equal probability, the resulting two-centre molecular wave-functions can be matched to the DHO orbitals with a one-to-one correspondence:
$$\begin{aligned} \left[ 0,0,4\right]\equiv & {} \frac{1}{\sqrt{2}} \Big [ [0,0,2] + [0,0,2] \Big ], \nonumber \\ \left[ 0,1,2\right]\equiv & {} \frac{1}{\sqrt{2}} \Big [ [0,1,1] + [0,1,1] \Big ], \nonumber \\ \left[ 1,0,2\right]\equiv & {} \frac{1}{\sqrt{2}} \Big [ [1,0,1] + [1,0,1] \Big ], \nonumber \\ \left[ 0,2,0\right]\equiv & {} \frac{1}{\sqrt{2}} \Big [ [0,2,0] + [0,2,0] \Big ], \nonumber \\ \left[ 2,0,0\right]\equiv & {} \frac{1}{\sqrt{2}} \Big [ [2,0,0] + [2,0,0] \Big ], \nonumber \\ \left[ 1,1,0\right]\equiv & {} \frac{1}{\sqrt{2}} \Big [ [1,1,0] + [1,1,0] \Big ]. \end{aligned}$$
(10)
Here the \(n_z\) quantum number in the DHO is the sum of the two-centre \(n_z\) quantum numbers and the \(n_x\) and \(n_y\) values remain unchanged as predicted by the two-centre shell model. In this instance the orbitals in the DHO immediately above those responsible for the \(^{32}\)S cluster structure all have a molecular structure.
Similarly, \(^{81}\)Zr, can be thought of as two \(^{40}\)Ca clusters with a single delocalised neutron. In the 2:1 DHO model, the orbitals filled with nucleons from the \(^{80}\)Zr core are \([n_x,n_y,n_z]=\) [0,0,0], [0,0,1], [0,0,2], [0,1,0], [1,0,0], [0,0,3], [0,1,1], [1,0,1], [0,0,4], [0,1,2], [1,0,2], [0,2,0], [2,0,0], [1,1,0], [0,0,5], [0,1,3], [1,0,3], [0,2,1], [2,0,1] and [1,1,1]. The next highest energy orbitals available for the delocalised neutron are then [0,0,6], [0,1,4], [1,0,4], [1,1,2], [0,2,2], [2,0,2], [0,3,0], [3,0,0], [1,2,0] and [2,1,0]. These are all degenerate at the 2:1 deformation. In the two-centre approach, each \(^{40}\)Ca cluster occupies the orbitals: [0,0,0], [1,0,0], [0,1,0], [0,0,1], [2,0,0], [0,2,0], [0,0,2], [1,1,0], [1,0,1] and [0,1,1]. The valence neutron then occupies the orbitals [0,0,3], [0,3,0], [3,0,0], [1,1,2], [1,0,2], [1,1,1], [0,2,1], [2,0,1], [1,2,0] and [2,1,0] around each centre. Again the combination of the single-centre orbitals give the complete set of valence DHO orbitals. Once more this is a demonstration that the DHO orbitals have a molecular character.
As the delocalised neutron in \(^{81}\)Zr exists at a much higher energy than \(^{33}\)S, the degeneracy is much larger. This means that there are a greater number of molecular orbitals which must be constructed using linear combinations, but there is still only one possible combination of wave-functions from each cluster centre which give the correct orbital shape, Fig. 12. Once again, it can be seen there is a good match between the properties of the 2:1 deformed orbitals and the explicit two-centre molecular counterparts. These two examples demonstrate that at a deformation of 2:1 the deformed harmonic oscillator orbitals above the deformed shell closure all have a molecular structure and thus the deformed harmonic oscillator explicitly includes the 2-centre molecular behaviour.
This feature evident at a deformation of 2:1 has been explored at other deformations and asymmetric choices of cluster and the same conclusions are reached [8].
The conclusions of this analysis are pretty clear. Above every shell-closure for the prolate nuclei lies a series of energy levels which correspond to the molecular orbitals which would have been formed from the linear combination of the valence orbitals around each spherical cluster component. In other words, irrespective of the cluster structure, symmetric or asymmetric, there exist valence orbitals which would allow the covalent exchange of protons or neutrons between the clusters. This makes the molecular symmetries a ubiquitous feature of prolate deformed nuclei.
Of course, it is one thing for such symmetries to exist and it is another for them to survive the complexity which arises from the mixing of the sea of other possible structures and states, as illustrated in Fig. 4.