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# Self-assembly of quantum dots: effect of neighbor islands on the wetting in coherent Stranski-Krastanov growth

## Abstract

The wetting of the homogeneously strained wetting layer by dislocation-free three-dimensional islands belonging to an array has been studied. The array has been simulated as a chain of islands in 1+1 dimensions. It is found that the wetting depends on the density of the array, the size distribution and the shape of the neighbor islands. Implications for the self-assembly of quantum dots grown in the coherent Stranski-Krastanov mode are discussed.

The instability of planar films against the development of coherently strained three-dimensional (3D) islands in highly mismatched epitaxy is a subject of intense research in recent times due to the optoelectronic applications of the islands as quantum dots.Politi  The term “coherent Stranski-Krastanov (SK) growth” has been coined for this formation of 3D islands that are strained to fit the underlying wetting layer but are nearly strainfree near their top and side walls,Eag ; Vit  in contrast to the “classical” SK growth in which the lattice mismatch is accommodated by misfit dislocations at the interface with the wetting layer.Matt

Experimental studies of arrays of coherent 3D islands of semiconductor materials have shown surprisingly narrow size distributions.Leo ; Moi ; Gru ; Jia  This phenomenon, known as self-assembly,Chris  is highly desirable as it guarantees a specific optical wavelength of the array of quantum dots. The physics of the self-assembly is still not well understood in spite of several studies.ter ; sch ; dobbs ; zang  Priester and Lannoo found that two-dimensional (2D) monolayer-high islands have a minimal energy per atom for a certain size and act as precursors of the 3D pyramidal islands, which become energetically favored at a smaller volume.Pri  Thus at some critical surface coverage the 2D islands spontaneously transform into 3D ones preserving a nearly constant volume. The resulting size distribution reflects that of the 2D islands which is very narrow. This picture has been recently corroborated by Ebiko et al.Ebi  who found that the volume distribution of InAs/GaAs self-assembled quantum dots agrees well with the scaling function characteristic of submonolayer homoepitaxy. Amar  Korutcheva et al.Kor  and Markov and PrietoMarjosem  reached the same conclusion with the exception that the 2D-3D transformation was found to take place through a series of intermediate states with discretely increasing thickness, in monolayer (ML) steps, that are stable in separate consecutive intervals of volume. Khor and Das Sarma arrived to the same conclusion using Montecarlo simulations.Khor

The formation of coherent 3D islands has been discussed within the framework of the traditional concept of wetting.Prieto  The wetting parameter, which accounts for the energetic influence of a crystal B in the heteroepitaxy of a crystal A on top of it, is defined asMar2  $`\mathrm{\Phi }=1E_{\mathrm{AB}}/E_{\mathrm{AA}}`$, where $`E_{\mathrm{AA}}`$ and $`E_{\mathrm{AB}}`$ are the energies per atom required to disjoin a half-crystal A from a like half-crystal A and from an unlike half-crystal B, respectively. The mode of growth of a thin film is determined by the difference $`\mathrm{\Delta }\mu =\mu (n)\mu _{3\mathrm{D}}^0`$, where $`\mu (n)`$ and $`\mu _{3\mathrm{D}}^0`$ are the chemical potentials of the film (as a function of its thickness $`n`$) and of the bulk material A, respectively.Mar2  The chemical potential of the bulk crystal A is given at zero temperature by $`\varphi _{\mathrm{AA}}`$, the negative of the binding energy of an atom to the well known kink or half-crystal position. At this position the atom is bound to a half-atomic row, a half-crystal plane and a half-crystal block.Stran  In the case of a monolayer-thick film of A on the surface of B the chemical potential of A is given by the analogous energy $`\varphi _{\mathrm{AB}}`$ when the the underlying half-crystal block of A is replaced by a half-crystal block of B. Thus $`\mathrm{\Delta }\mu =\varphi _{\mathrm{AA}}\varphi _{\mathrm{AB}}`$. In the simplest case of additivity of bond energies this difference reduces to $`E_{\mathrm{AA}}E_{\mathrm{AB}}`$. Then $`\mathrm{\Delta }\mu `$ is proportional to $`\mathrm{\Phi }`$, i.e. $`\mathrm{\Delta }\mu =E_{\mathrm{AA}}\mathrm{\Phi }`$.Mar2  It follows that the wetting parameter $`\mathrm{\Phi }`$ determines in fact the mechanism of growth of A on B.Rudy

In the present work we study the behavior of $`\mathrm{\Phi }`$ for islands that belong to an array. For the coherent SK growth, which is in fact the formation of dislocation-free 3D islands of A on the same (strained) material A, it is convenient to define the wetting parameter $`\mathrm{\Phi }`$ as the difference of the interaction energies of misfitting and non-misfitting 3D islands with the wetting layer.Prieto  We study the effect of the array density and of the size and shape distributions of neighbor islands on the wetting parameter $`\mathrm{\Phi }`$ of a given island. We consider an atomistic model in $`1+1`$ dimensions which can be regarded as a cross-section of the real $`2+1`$ case. An implicit assumption is that the islands have a compact rather than a fractal shape and that the lattice misfit is the same in both orthogonal directions. The 3D islands are represented by linear chains of atoms stacked one upon the other.Ratsch  The shape of the islands in our model is given by the slope of the side walls. The array in the 1+1 dimensional space is represented by a row of 3 or 5 islands on a wetting layer consisting of several monolayers (Fig. 1). The distance between two neighbor islands is given by the number $`r`$ of vacant atomic positions between the ends of their base chains.

In order to simplify the computational procedure, the “wetting layer” in our model is in fact composed of several monolayers of the true wetting layer of the overlayer material A plus several monolayers of the unlike substrate material B. This composite wetting layer has the atom spacing of the substrate material B as is the real case, but for the sake of simplicity, it has the atom bonding of the overlayer material A. This underestimates somewhat the value of $`\mathrm{\Phi }`$ because the A-A bonding is weaker than the B-B bonding, but it does not introduce a significant error as the energetic influence of the substrate B is screened by the true wetting layer A.

To find the equilibrium atomic positions, we make use of a simple minimization procedure. Marjosem  The atoms interact through a Morse potential $`V(x)=V_0[e^{12(xa)}2e^{6(xa)}]`$. We calculate the interaction energy of all the atoms as well as its gradient with respect to the atomic coordinates, i.e. the forces. Relaxation of the system is performed by allowing the atoms to displace in the direction of the gradient in an iterative procedure until the forces fall below some negligible cutoff value. Periodic boundary conditions are applied in the lateral direction. We consider only interactions with first neighbors.

As expected, the edge atoms are found to be more weakly bound to the underlying wetting layer than the center atoms (Fig. 2). Compared to an isolated island, the edge atoms of an island in an array adhere weaker to the substrate. This is in fact the essential physical effect exerted by the neighbors on a given island: it loses contact with the substrate and the wetting parameter is increased. We can regard this as the substrate becoming stiffer under the influence of the neighbor islands.

The influence of the density of the array is demonstrated in Fig. 3. As expected, the wetting parameter increases with increasing array density. The figure also allows us to estimate the size of the effect. At a distance $`r`$=10 (about 30 nm), neighbors make $`\mathrm{\Phi }`$ increase by 10%; this represents an effective decrease in adhesion $`\mathrm{\Delta }E_{AB}`$ of 0.10 $`\mathrm{\Phi }`$ $`E_{AA}`$. For Ge/Si(100) (desorption energy of Ge: 4 eV), this gives about 20 meV, a contribution of the same order as the elastic energy per atom (40 meV in this system Mar2 ) that can significantly affect the delicate balance of the energies involved in the growth process: diffusion barriers and surface/interface energies.

Figure 4 shows the wetting parameter of the central island vs. the size of the side islands. Increasing the volume of the side islands leads to an increase of the elastic fields around them and to a further reduction of the bonding between the edge atoms of the central island and the wetting layer.

Figure 5 demonstrates one further important result, the effect of the size distribution on the wetting of the islands. It shows the behavior of the wetting parameter $`\mathrm{\Phi }`$ of the central island as a function of the number of atoms in the base chain of the left island. The sum of the total number of atoms of left and right islands is kept constant and precisely equal to the doubled number of the central island. The facet angle of all three islands is 60. Thus the first (and the last) points give the maximum asymmetry in the size distribution of the array, the left (right) island containing 9 atoms and the right (left) island 105. All three islands are 3 ML thick. The point at the maximal wetting corresponds to the monodisperse distribution: the three islands having one and the same volume of 57 atoms. This means that in the case of perfect self-assembly of the array, the wetting parameter and therefore the tendency to clustering display a maximum value.

The effect of the shape of the side islands, i.e. their facet angles, on the wetting parameter of the central island is demonstrated in Fig. 6. The facet angle of the central island is 60. The effect is greatest when the side islands have the steepest walls. The same result (not shown) is obtained when the central island has a different shape. The explanation follows the same line as the one given above: islands with larger-angle side walls exert a greater elastic effect on the substrate and in turn on the displacements and the bonding of the edge atoms of the central island.

When discussing the above results we have to bear in mind that a positive value of the wetting parameter implies in fact a tendency of the deposit to form 3D clusters instead of a planar film. In the case of coherent SK growth the non-zero wetting parameter is due to the weaker adhesion of the atoms close to the island’s edges. The presence of other islands, particularly with large angle facets, in the near vicinity enhances the effect. The transformation of 2D, monolayer-high islands into bilayer islands takes place by detachment of atoms from the edges and their subsequent jumping and nucleating on the top island’s surface.Stmar  This edge effect hints at the influence of the lattice misfit on the rate of second layer nucleation and in turn on the kinetics of the 2D-3D transformation.Fil ; Lin  The presence of neighbor islands favors the formation of 3D clusters and their further growth. For the self-assembled monodisperse population, the highest tendency to clustering is found.

We can regard the flatter islands in our model (11 facet angle) as the “hut” clusters discovered by Mo et al.,Mo  and the clusters with 60 facet angle as the “dome” clusters. It is well known that clusters with steeper side walls relieve the strain more efficiently than flatter clusters Mich  (a planar film, the limiting case of the flat islands, does not relieve strain at all). We see that large-angle facet islands affect more strongly the growth of the neighbor islands, leading to a more narrow size distribution.

From our results, a self-assembled population of quantum dots with highest density is expected at comparatively low temperatures such that the critical wetting layer thickness for 3D islanding approaches an integer number of monolayers. In InAs/GaAs quantum dots the reported values of the critical thickness are found to vary from 1.2 to 2 ML.Pol  The critical wetting layer thickness is given by an integer number $`n`$ of monolayers plus the product of the 2D island density and the critical volume $`N_{12}`$ in the ($`n`$+1)-th ML. The 2D island density increases steeply with decreasing temperature.dobbs  In such a case a dense population of 2D islands will overcome simultaneously the critical size $`N_{12}`$ to produce bilayer islands. The value of $`N_{12}`$ will be slightly reduced when neighbor islands are present due to the increase of $`\mathrm{\Phi }`$.Prieto  Regions of high adatom concentrations will favor the highest degree of self-assembly and, due to the larger elastic forces present, are also likely to promote the spatial ordering of the islands, possibly extending to less dense regions and leading to self-organized arrays. Islands will thus interact with each other from the very beginning of the 2D-3D transformation and will give rise to the maximum possible wetting parameter and, in turn, to islands with large-angle facets and a narrow size distribution. This is in agreement with the observations of self-assembled Ge quantum dots on Si(001).Le  At 700C a population of islands with a concentration ranging from $`10^7`$ to $`10^8`$ cm-2 is obtained. The islands have the shape of truncated square pyramids with their side wall facets formed by (105) planes (inclination angle of about 11). The size distribution of the islands is quite broad. At 550C a population of islands with an areal density of the order of $`10^9`$ to $`10^{10}`$ cm-2 is observed. The islands have larger-angle (113) facets and their size distribution is much more narrow.

In summary, the presence of neighbor islands decreases the wetting of the substrate (in this case the wetting layer) by the 3D islands. The wetting decreases with increasing array density and facet angle of the neighbor islands. The wetting parameter displays a maximum (implying a minimal wetting) when the array shows a monodisperse size distribution. We expect an optimum self-assembled islanding at low temperatures such that the 2D-3D transformation takes place at the highest possible island density.

J. E. P. gratefully acknowledges financial support from the Alexander-von-Humboldt Stiftung and the Spanish MEC (grant No. EX2001 11808094).


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# Spin-Charge Separation in Two-dimensional Frustrated Quantum Magnets

(June 16, 2004)

## Abstract

The dynamics of a mobile hole in two-dimensional frustrated quantum magnets is investigated by exact diagonalization techniques. Our results provide evidence for spin-charge separation upon doping the kagomé lattice, a prototype of a spin liquid. In contrast, in the checkerboard lattice, a symmetry broken Valence Bond Crystal, a small quasi-particle peak is seen for some crystal momenta, a finding interpreted as a restoration of weak holon-spinon confinement.

In the last years, there has been growing interest in the investigation of frustrated magnets, both on experimental and theoretical sides. Spin-1/2 Heisenberg models on two and three dimensional (3D) lattices have been studied extensively providing increasing evidences for new exotic phases like the spin liquid Resonating Valence Bond (RVB) RVB  state or the Valence Bond Crystal (VBC) VBC . In two dimension (2D), the checkerboard lattice pyrochlore2D ; Fouet ; Brenig , i.e. the 2D analog of the 3D pyrochlore lattice, and the kagomé lattice KagomeED ; KagomeED\_2  (see Fig. 1), respectively, seem to provide simple theoretical realizations of VBC and RVB groundstates (GS). In addition, an exotic scenario where magnons break up into ($`S=1/2`$) deconfined spinons spinons  could take place in a RVB state. These theoretical conjectures have triggered a renewal of experimental activity on quantum frustrated magnets like e.g. the ($`S=3/2`$) kagomé compound SrCr9pGa12-9pO19 SCGO  and the pyrochlore titanates RE2Ti2O7 (where RE is a rare-earth magnetic atom such as gadolinium or terbium) titanates . These materials exhibit very rich phase diagrams as a function of chemical composition, temperature, pressure and magnetic field which underline the crucial role of geometric frustration. Furthermore, the recent discovery of superconductivity in a CoO2 based compound with triangular layers cobaltites  has revived interest in exotic RVB mechanisms of superconductivity Baskaran .

In this Letter, we investigate the dynamics of a mobile hole injected in various 2D frustrated quantum magnets. This study is indirectly motivated by the long-standing puzzles offered by the “normal phase” of high-$`T_c`$ superconductors whose discovery initiated a search for spin-charge separation mechanisms in 2D and the first proposal of 2D Luttinger liquids 2D-LL . The dynamics of a mobile hole doped into an (Ising) antiferromagnet (AF) was first studied by Brinkman and Rice BrinkmanRice  and a coherent motion was later predicted by Trugman Trugman . However, a close inspection of the hole spectral function showed evidences for a composite nature of the doped hole quasiparticle (QP) showing holon and spinon components Laughlin . Large quantum fluctuations present in frustrated magnets might then induce a complete deconfinement of the hole components. Here we present large scale exact diagonalization results for single hole spectral functions and hole-spin correlations obtained on the checkerboard and the kagomé antiferromagnets. A finite lifetime of the hole (breaking apart into a spin 1/2 spinon and a charge $`Q=e`$ holon) is signaled by the absence of a QP peak in the computed spectral functions. Since the latter could, in principle, be measured by Angular Resolved Photoemission Spectroscopy (ARPES) on high-quality (cleaved) insulating single crystals SrCuOCl , our results can provide motivation and theoretical background to experimentalists. In addition, this investigation might also be relevant to lightly doped samples. Evidences for spin-charge separation in the kagomé spin liquid GS are provided while, in the checkerboard lattice, we find small QP peaks for some momenta.

Before going further, let us first summarize briefly the properties of the undoped insulating systems we are dealing with. The checkerboard lattice is believed to form a VBC with plaquette singlets on a subset of the void plaquettes pyrochlore2D ; Fouet ; AltmanAuerbach ; note\_j1j2 . The groundstate manifold is two fold degenerate \[see Fig. 1 (a)\]. The system has quite a sizable triplet gap $`\mathrm{\Delta }_T0.7J`$ Fouet ; Brenig , and a somewhat smaller singlet gap $`\mathrm{\Delta }_S0.3J`$ Fouet ; AltmanAuerbach  to domain wall like singlet excitations AltmanAuerbach . Based on this picture of a fully gapped system, we expect a coherent QP motion of an injected hole at least in parts of the Brillouin zone (BZ) as observed for example in Heisenberg ladders or dimerized spin chains. On the other hand, the undoped kagomé lattice has a very interesting and puzzling groundstate of a new type: while this system is also magnetically disordered KagomeED , it has quite a small triplet gap ($`\mathrm{\Delta }_T0.05J`$KagomeED\_2 . The singlet sector seems to remain gapless showing an exponentially large number of singlets within the spin gap KagomeED\_2 ; KagomeSinglets . These unconventional low lying excitations open the door to new and surprising phenomena upon hole doping.

Our numerical calculations are based on the standard $`tJ`$ model Hamiltonian:

$$t\underset{i,j,\sigma }{}𝒫\left(c_{i,\sigma }^{}c_{j,\sigma }+\text{h.c.}\right)𝒫+J\underset{i,j}{}\text{S}_i\text{S}_j\frac{1}{4}n_in_j$$
(1)
where on both lattices all bonds have the same couplings $`t`$ and $`J`$. This model is believed to be reliable to describe weakly doped Mott-Hubbard insulators with large optical gaps. Hereafter, a physical value of $`J/|t|=0.4`$ is assumed, unless mentioned otherwise. The spectral functions are defined in the standard way:

$$A^\sigma (𝐤,\omega )=\frac{1}{\pi }\text{Im}[\mathrm{\Psi }_0|c_{𝐤,\sigma }^{}\frac{1}{\omega +E_0+i\eta H}c_{𝐤,\sigma }|\mathrm{\Psi }_0],$$
(2)
and calculated by the Lanczos continued-fraction technique on finite clusters of up to 32 sites with periodic boundary conditions. Here $`|\mathrm{\Psi }_0`$ (of energy $`E_0`$) is the GS of the undoped insulating system, so that the dynamics of a single hole is probed. A simple sum rule is satisfied: $`A^\sigma (𝐤,\omega )\text{d}\omega =N_\sigma /N1/2`$, independent of $`𝐤`$. Therefore the spectral function plots share an arbitrary, but common scale, unless mentioned otherwise. In addition an artificial broadening $`\eta =0.05|t|\text{ or }0.1|t|`$ has been used to plot the data. The weights of the lowest peaks can be obtained exactly, independent of $`\eta `$. We have indicated this weight in the plots when a QP peak is present.

As a first step it is of special interest to consider the static limit i.e. the case $`t=0`$ (equivalent to an infinite hole mass) where a spin 1/2 is replaced by an inert (impurity-like) site. The spectral function, which becomes here independent of momentum $`𝐤`$, gives useful hints on the host magnetic disturbance induced by the static hole. Results in Fig. 2 show very different qualitative behaviors for the checkerboard and the kagomé lattices. A sharp peak which exhausts most of the spectral weight is found in the checkerboard lattice. This is consistent with the picture of breaking a local plaquette singlet, therefore producing a localized moment, which remains confined to the hole. The very large peak weight shows that the bare state $`c_{i,\sigma }|\mathrm{\Psi }_0`$ is a very good approximation of the true one hole groundstate. This however seems to be quite different for the kagomé case: the spectral function shows a rather broad response, with no pronounced low energy peak \[see weight distribution (circles) in Fig. 2 (b)\]. Here the overlap of the bare electron removal state and the true groundstate of the one impurity problem is tiny. This can be nicely understood in the “dimer freezing” picture advocated in Ref. StaticKagomeImpurities , where the screening of the impurity constitutes an important deformation of the RVB spin liquid groundstate. This suggests that a single dopant in the kagomé lattice generates a dimer-screened holon with charge $`Q`$=$`e`$ and spin $`S`$=0 and a deconfined spinon ($`Q`$=0, $`S`$=1/2).

We now move to the case of a dynamic hole ($`t0`$). Because of the absence of particle-hole symmetry in frustrated lattices one has to distinguish between $`t>0`$ and $`t<0`$. Note that for $`t<0`$ frustration can also appear in the hole motion. For example, a tight-binding particle on an isolated triangle gains a kinetic energy $`|t|`$ per particle, a factor of two smaller than for $`t>0`$. Our results for a 32 cluster clustershape  are shown in Fig. 3 along the $`\mathrm{\Gamma }M`$ line of the BZ \[Fig.1 (b)\]. In all cases most of the spectral weight is found to be incoherent, distributed over a range of $`79|t|`$. However, a small QP peak is visible, in particular for momenta close to the $`M`$-point. The region close to the $`\mathrm{\Gamma }`$ point has a tiny or no QP peak and the shape of the spectral function at $`\mathrm{\Gamma }`$ itself is very special, probably because of a higher point group symmetry. It is interesting to notice, in the case $`t<0`$, the presence of a pseudo-gap in the region $`\omega 0`$.

We have estimated the QP bandwidth $`W`$ of the checkerboard lattice from the dispersion of its QP pole. As shown in the left panel of Fig. 4 the single hole bandwidth is much smaller than in a 2-leg spin ladder, which has a gapped spectrum, ($`W2t`$ for strong magnetic rung couplings ladder ) or even in the square lattice, which has a gapless spectrum, where $`W2.2J`$. In the latter case, the strong renormalization of the coherent motion can be explained e.g. by long-wavelength spin-waves scattering Trugman ; Laughlin . In the checkerboard lattice the QP are more massive, almost localized, although the VBC host has no low energy excitations. We believe that this remarkable fact is due to a destructive interference effect between the paths available for the hole to hop from one plaquette to the next. One can define QP weights $`Z_{\text{1h}}(𝐤)`$ as the relative weights contained in the first $`\delta `$-function appearing at the bottom of each spectrum in Fig. 3. Its behavior versus $`J/t`$ is shown in the right panel of Fig. 4 and compared with existing data for the square lattice. We note that, although there are quantitative differences, the qualitative behavior is similar; larger $`J`$ leads to larger holon-spinon confinement and hence to an increase of $`Z_{\text{1h}}`$.

The spectral functions of the kagomé lattice shown in Fig. 5 show exotic behaviors; they are very broad for all momenta (width $`68|t|`$) and, in contrast to the checkerboard lattice, do not show visible QP peaks both for $`t>0`$ (left panel) and $`t<0`$ (right panel). Note that the broad appearance is not due to a large $`\eta `$, but is an intrinsic feature of the spectral function as can be seen from the large number of poles carrying spectral weight (circles in Fig. 5). Note that the GS $`|\mathrm{\Psi }_0`$ of the 27 site undoped kagomé cluster is a spin 1/2 state, e.g. $`S^Z=+1/2`$, $``$. Therefore, the initial state of charge $`Q=e`$ and spin projection $`S^Z=0`$, $`c_{𝐤,}`$, is an equal-weight superposition of a singlet and a triplet state leading to two contributions. We have checked that both components are consistent with the decay of the original hole into a holon and a spinon (with no QP peak). Close similarities of the singlet and triplet channels also suggest that the spinons in the final state (with either parallel or anti-parallel spins) are weakly interacting in agreement with the mechanism of spinon deconfinement.

The spectral function data strongly support a spin-charge separation scenario for the kagomé lattice. In order to get further evidence and more insight about the origin of this phenomenon we also investigate the spin density profile in the vicinity of the hole, i.e. the hole-spin correlation function $`n_i^hS_j^Z`$ in the one hole-doped 30 site kagomé cluster (for which $`S_Z=1/2`$). Results are shown in Fig. 6 for $`t=+1`$ (a) and $`t=1`$ (b). In the case $`t=+1`$ we clearly see a repulsion between the net $`S`$=1/2 moment and the mobile hole. The case $`t=1`$ displays a different picture, showing a rather uncorrelated behavior between the spinon and the holon. Nevertheless a spinon-holon confinement does not seem to be present, in agreement with spectral function data. In contrast we have checked that on a checkerboard lattice a clear localization of the spinon close to the holon takes place.

Finally we consider the GS of the one hole-doped 27 site kagomé cluster of total charge $`Q=e`$ and spin $`S=0`$ to mimic the holon wavefunction. Figs. 6 (c,d) show a snapshot of the nearest neighbor spin correlations around the mobile holon. Surprisingly in the case $`t=+1`$ a “dimer freezing” is observed very similar to the static impurities considered in Ref. StaticKagomeImpurities . In contrast, the case $`t=1`$ shows two slightly ferromagnetic bonds on the two triangles containing the holon, while the other bonds remain largely unaffected. This behavior of the magnetic environment is fairly well described by a simple energetic consideration on a 3-site ring $`tJ`$ model; for $`t=+1`$ the propagating holon is accompanied by a singlet, while in the opposite $`t=1`$ case an accompanying ferromagnetic bond appears.

To conclude, based on extensive analysis of the single particle spectral functions and various charge-spin correlations in the single hole GS, we have addressed the issue of spin-charge separation in 2D magnetically disordered magnets. We show strong evidence that it occurs in the kagomé lattice and we expect it to be robust for small but finite doping. This provides the first example of observed spin-charge separation in a two-dimensional microscopic model. The RVB nature of the undoped groundstate (characterized by a gapless low-excitation singlet spectrum) seems to be crucial for this behavior. Indeed, in the checkerboard lattice, which exhibits a VBC structure, a weak hole-spinon confinement manifests itself as QP peaks for some momenta.

###### Acknowledgements.

We thank M. Mambrini for useful discussions. A.L. acknowledges support from the Swiss National Fund and the CNRS. D.P. thanks the Institute for Theoretical Physics, ETH Zürich, for hospitality during the final stage of this work. We thank IDRIS (Orsay) and the LRZ München for allocation of CPU-time.


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# Half-life Limit of {^"19"}"Mg"

## I Introduction

The search for the di-proton decay predicted over 40 years ago Gol60  has recently intensified with the observation of two-proton decay from $`{}_{}{}^{\text{45}}\text{Fe}`$ Gio02 ; Pfu02 . These experiments extracted the total energy of the decay, but they did not measure the individual proton energies and angles. This information is necessary in order to determine the nature of this decay, whether it is a di-proton ($`{}_{}{}^{\text{2}}\text{He}`$) or a three-body decay.

Another promising candidate for di-proton decay is $`{}_{}{}^{\text{19}}\text{Mg}`$ Jan64 ; Gri00 . $`{}_{}{}^{\text{19}}\text{Mg}`$ is predicted to be unbound by 0.9$`\pm `$0.3 MeV with respect to two-proton emission and bound by 0.66$`\pm `$0.5 MeV with respect to one-proton emission Aud93 , which is the ideal situation for the possibility of di-proton decay Gol60 . The predictions of the two-proton decay energy are based on extrapolations of the mass tables Aud93 . Microscopic calculations have predicted that $`{}_{}{}^{\text{19}}\text{Mg}`$ might even be bound depending on the choice of the force used in the calculation Des98 . However, recent theoretical work by Grigorenko et al. suggests a half-life that is significantly smaller than the previously mentioned calculation Gri03 . Although a potentially very interesting nucleus, no dedicated searches for the existence of $`{}_{}{}^{\text{19}}\text{Mg}`$ have been performed so far.

A search for the $`T_z=\frac{5}{2}`$ nuclei $`{}_{}{}^{\text{23}}\text{Si}`$, $`{}_{}{}^{\text{27}}\text{S}`$, $`{}_{}{}^{\text{31}}\text{Ar}`$, and $`{}_{}{}^{\text{35}}\text{Ca}`$, discussed in Ref. Lan86 , should have observed $`{}_{}{}^{\text{19}}\text{Mg}`$ if it was indeed bound, however, it was not observed and the implications of this are not mentioned. If $`{}_{}{}^{\text{19}}\text{Mg}`$ is unbound, the experimental requirements to study its decay mode depend critically on the expected lifetime. The lifetime is a strong function of the decay energy and the predicted range covers many orders of magnitude.

We started a dedicated search for $`{}_{}{}^{\text{19}}\text{Mg}`$ using projectile fragmentation and extracted a first limit on its lifetime from the time-of-flight through the fragment separator.

## II Experimental Procedure

The experiment was performed at the Coupled Cyclotron Facility (CCF) at the National Superconducting Cyclotron Laboratory (NSCL) at Michigan State University. $`{}_{}{}^{\text{36}}\text{Ar}`$ nuclei were accelerated by the K500$`\times `$K1200 combination to 150 MeV/nucleon with a charge state of 18+ and bombarded a 689 mg/cm2 thick beryllium production target. The average beam intensity was 4.3 pnA. The fragments of interest were selected with the A1900 fragment separator Mor03  shown in Figure 1. A 300-mg/cm2-thick aluminum wedge was placed at the intermediate image and the momentum acceptance was limited to 0.5%. The detectors at the focal plane of the separator consisted of a 470-$`\mu `$m-thick $`\mathrm{\Delta }E`$ silicon detector and a 10 cm thick plastic scintillator. The horizontal position acceptance at the focal plane was limited to 15 mm in order to reduce the background from lighter ions. The fragments were identified by their energy loss in the silicon detector and the time-of-flight measured between the plastic scintillator and a thin scintillator located at the intermediate image. The total length of the A1900 from the production target to the focal plane is 35.5 m.

## III Data Analysis and Results

Figure 2 shows the energy loss versus time-of-flight as measured at the focal plane. The $`N=7`$ isotones $`{}_{}{}^{\text{13}}\text{C}`$, $`{}_{}{}^{\text{14}}\text{N}`$, $`{}_{}{}^{\text{15}}\text{O}`$, and $`{}_{}{}^{\text{17}}\text{Ne}`$ were clearly identified while no events for $`{}_{}{}^{\text{19}}\text{Mg}`$ were detected. Although contributions from pile-up, incomplete charge collection, and other processes produced counts in the spectrum, the region where $`{}_{}{}^{\text{19}}\text{Mg}`$ is expected is background free. This non-observation confirms that $`{}_{}{}^{\text{19}}\text{Mg}`$ is indeed unbound with respect to proton emission. It could be unbound with respect to one- or two-proton emission, or both.

An upper limit of the half-life can be extracted from the predicted number of produced $`{}_{}{}^{\text{19}}\text{Mg}`$ and the transmission efficiency, and the time of flight through the A1900 separator.

The fragment production of nuclei along the proton dripline has to be extrapolated from the production of nuclei closer to the line of stability and depends strongly on the reaction model. The most commonly used approaches are the EPAX parameterizations Sum90 ; Sum00  and calculations based on the abrasion-ablation model Fri00 . In order to select the best reaction model for the production of $`{}_{}{}^{\text{19}}\text{Mg}`$, we tuned the A1900 to maximize the production of $`{}_{}{}^{\text{20}}\text{Mg}`$, which is particle stable. With the 689-mg/cm2-thick Be target, we measured a rate of 4 pps/pnA of $`{}_{}{}^{\text{20}}\text{Mg}`$. The simulation program LISE++ Baz02 ; Tar02  predicted rates of 5 pps/pnA, 10 pps/pnA, and 25 pps/pnA employing the EPAX1 Sum90 , EPAX2 Sum00 , and the abrasion-ablation model, respectively. The fragment velocities and momentum distributions were calculated following the parameterization of Morrissey Mor89 . The EPAX1 calculation is within 20% of the measured $`{}_{}{}^{\text{20}}\text{Mg}`$ rates and is the smallest prediction for the production of very proton rich nuclei in this mass region for the given projectile and target combination. Since the prediction by EPAX1 is the smallest of the three approaches, they represent the most conservative approach for extracting the upper limit of the half-life of $`{}_{}{}^{\text{19}}\text{Mg}`$.

It should be mentioned that 36Ar is not the optimum choice as a primary beam. A more intense and pure beam of secondary beam of 20Mg can be produced from a primary beam of 24Mg Pie95 . However, this beam was not available for the present experiment.

EPAX1 yields a rate of 0.018 pps/pnA of $`{}_{}{}^{\text{19}}\text{Mg}`$ to be transmitted to the focal plane. We collected a total of 15.5 hours of beam on target with an average beam intensity of 4.3 pnA. This would result in 4320 $`{}_{}{}^{\text{19}}\text{Mg}`$ transmitted to the focal plane detectors if it was particle stable.

The total flight path through the separator consists of two parts. In the first half after the production target the average velocity of $`{}_{}{}^{\text{19}}\text{Mg}`$ is calculated to be $`v=0.46c`$. The velocity in the second half is reduced to $`v=0.44c`$ following the 300 mg/cm2 aluminum wedge. The resulting time of flight is $`T_{\text{A1900}}=263`$ ns.

The upper limit of the half-life assuming that one $`{}_{}{}^{\text{19}}\text{Mg}`$ has not decayed before reaching the focal plane was calculated using the number of transmitted $`{}_{}{}^{\text{19}}\text{Mg}`$ ($`N`$) and the total time-of-flight ($`T_{\text{A1900}}`$):

$$T_{1/2}<T_{\text{A1900}}\frac{\mathrm{ln}2}{\mathrm{ln}N}.$$

This results in an upper limit of 22 ns for the half-life of $`{}_{}{}^{\text{19}}\text{Mg}`$. The number of $`{}_{}{}^{\text{19}}\text{Mg}`$ produced as predicted by LISE++ is the largest uncertainty in the preceeding equation. However, Figure 3 shows the relationship between the extracted limit on the half-life and the predicted production. The half-life is not strongly influenced by over- or under-predicting the rate of $`{}_{}{}^{\text{19}}\text{Mg}`$. For instance, an over-prediction of the rate by a factor of 2 results in an upper half-life limit of 20 ns which is a difference of 10%.

The upper half-life limit can be compared to recent three-body calculations Gri00 ; Gri03 . In contrast to single proton emitters, where the half-life can be directly related to the decay energy through barrier penetration calculations Hof94 , the situation for two proton emitters is more complicated.

Grigorenko et al. derived the half-life of $`{}_{}{}^{\text{19}}\text{Mg}`$ as a function of decay energy for three-body, di-proton and uncorrelated two-proton decay Gri00 . Figure 4 shows the extracted half-life for the possible decay energies of Descouvement ($`<`$0.5 MeV) Des98 , Brown (1.1$`\pm `$0.3 MeV) Bro02 , and Audi-Wapstra (0.9$`\pm `$0.3 MeV) Aud93 . The light shaded areas correspond to the limits based on the decay energy uncertainties and the three-body model of Ref. Gri00 , while the dark shaded areas include the limits for the di-proton and uncorrelated two proton decay. The fourth column of Figure 4 shows the half-life predictions from a refined three-body calculation by Grigorenko et al. Gri03  and the last column is the experimental limit extracted from the present work. The experimental limit is consistent with the predictions. It rules out that $`{}_{}{}^{\text{19}}\text{Mg}`$ is particle-stable but does not put constraints on the calculations.

A different experimental approach is necessary to search for the di-proton emission of $`{}_{}{}^{\text{19}}\text{Mg}`$. Simply increasing the production of $`{}_{}{}^{\text{19}}\text{Mg}`$ nuclei by extending the beam time or increasing the beam intensity will not lead to a significant improvement as can be seen in Figure 3. Fragment separators are particularly useful in this type of experiment because the fragmentation products are cleanly separated and identified. In case no events are observed, it is essential that the region where $`{}_{}{}^{\text{19}}\text{Mg}`$ is expected to occur is background free. However, the limit on the half-life is directly proportional to the flight time. Therefore if one assumes that $`{}_{}{}^{\text{19}}\text{Mg}`$ exists before decay on the order of a few ns, an experiment apparatus with a smaller flight time is necessary.

One possibility to reduce the time-of-flight that is currently pursued is the use of single-neutron stripping reactions from a secondary beam of $`{}_{}{}^{\text{20}}\text{Mg}`$ to direcly observe the decay Muk01 ; Fra02 .

## IV Summary and Conclusions

The non-observation of $`{}_{}{}^{\text{19}}\text{Mg}`$ from the fragmentation of $`{}_{}{}^{\text{36}}\text{Ar}`$ confirms the expected particle instability of this potential di-proton emitter. An upper limit of the lifetime of 22 ns was established for the first time. However, this limit is not yet sufficient to constrain the experimental search for the di-proton decay of $`{}_{}{}^{\text{19}}\text{Mg}`$.

## Acknowledgements

This work has been supported by the National Science Foundation grant number PHY01-10253.