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# Percolation on two- and three-dimensional lattices

## I Introduction

Among the several methods for treating disordered systems and geometrical problems, percolation theory is certainly one of the most important. Due to its similarities with transitions that occur in many other systems (not only physical, but biological, social etc.), percolation has been used in studies within a large variety of fields. Forest fires Henley93 , biological evolution Ray94 ; Jovanovic94 , epidemics Moore00 , social influence Solomon00  and dilute magnetism Stinch  are only a few examples of the wide applicability of this theory, as well as percolation (e.g., in porous media) itself Stauffer91 .

Although easily defined, percolation presents theoretical and computational difficulties. For instance, the percolation threshold for the site problem on a simple square lattice is not known exactly. Therefore, approximate solutions are necessary, and much effort has been dedicated in this direction. From the theoretical point of view, one can utilize mean-field Gaveau93 ; Rudnick98  and renormalization group Young75 ; Burkhardt82 ; Sahimi95 ; pla  techniques, among others. In particular, computer simulations constitute a powerful tool in this area, since their application to percolation is simpler than for many other problems in statistical physics landau . Typically, one can obtain a valid configuration by simply populating sites (or bonds) in a given lattice. To measure quantities of interest, such as the percolation threshold or the mean cluster size, it is necessary to identify all clusters in the configuration. For this purpose, many algorithms have been developed, the best known perhaps being that devised by Hoshen and Kopelman Hoshen76 . Other algorithms, like hull-generation Ziff84 ; Grassberger92 , can also be used, but only to answer some specific questions. More recently, Newman and Ziff proposed a new algorithm Newman00 , which is general and quite efficient, both in its computational requirements and in its accuracy. Although the algorithm can be used to obtain any observable of the problem, in their papers they have used it to calculate the so-called wrapping probabilities to investigate a number of aspects of the problem. For example, using exact values of the wrapping probabilities, a high-precision result for the site percolation threshold on the square lattice was obtained Newman00 .

Unfortunately, for most lattices, one does not know the exact wrapping probabilities and, in using them, the problem must be tackled in a different way. One of the wrapping probabilities - $`R_L^{(1)}`$, which is the probability that a cluster wraps around one specified axis, but not around the other ones - is particularly useful. In this case it is not necessary to know its exact value at the critical concentration for the infinite system since it has a maximum from which the critical point can be obtained. The method, however, is indeed capable to properly estimate the other wrapping probabilities which do not exhibit a maximum (in such cases there is just a crossing region close to the critical threshold). On the other hand, as we will see below, there are still some probabilities in dimensions higher than two that present, besides the maximum, a crossing region from where critical behavior is also achieved.

In this work we compute the percolation threshold and the correlation length exponent, as well as the set of the unknown wrapping probabilities using the Newman-Ziff algorithm. These quantities are evaluated by employing the usual finite-size scaling as well as a cell-to-cell schemeziff02 . After summarizing the Newman-Ziff approach in the next section we describe, in section III, the method which enables us to evaluate such geometrical quantities and we apply it to site and bond percolation on the square, simple cubic, HCP (hexagonal close-packed) and simple hexagonal lattices. Concluding remarks are given in the final section.

## II The Newman-Ziff algorithm

To determine the percolation transition, this algorithm uses the wrapping probability $`R_L(p)`$, which, for a given site (or bond) occupation $`p`$, is basically the probability that a cluster wraps around a system with periodic boundary conditions on a lattice of linear dimension $`L`$. This wrapping can, however, be defined in various manners, each with its own probability. For instance, on two-dimensional lattices one has: (i) $`R_L^{(h)}`$ and $`R_L^{(v)}`$, the probabilities that a cluster wraps around the system in the horizontal or vertical direction, respectively (on a square lattice these quantities are equal); (ii) $`R_L^{(e)}`$, the probability that the cluster wraps around the lattice $`either`$ horizontally $`or`$ vertically (or both); (iii) $`R_L^{(b)}`$ for wrapping in $`both`$ horizontal $`and`$ vertical directions; (iv) $`R_L^{(1)}`$ for wrapping around $`one`$ specified direction but $`not`$ the other one. Different lattices can allow for further geometrical choices for $`R_L(p)`$. For example, on a simple cubic lattice, besides $`R_L^{(1)}`$, we can define $`R_L^{(2)}`$ as the probability that there exists a cluster that wraps the system in two directions, but not around the third one. Analogously to $`R_L^{(b)}`$, we have $`R_L^{(3)}`$ for wrapping around the three directions.

In order to evaluate these quantities it is necessary to generate many independent realizations of the algorithm, each of them consisting of the following steps:
(1) Initially, all sites are empty;
(2) Sites are chosen to be occupied at random;
(3) When a new site is added, one must check all its neighbors to verify if the new site forms an isolated cluster (all neighbors empty) or if it joins together two or more clusters. In the first case, we need do nothing. In the latter, we have to update the cluster listing. Clusters are stored in a tree structure, with one site of each cluster considered the $`root`$ site. All sites in a given cluster, other than the root, have a pointer to some other site in the same cluster, such that by following a succession of such pointers one can ultimately reach the root. In order to join two clusters we simply add a pointer from the root of the smaller cluster to the root of the larger one;
(4) Each time step (3) is repeated, we evaluate the quantities of interest $`Q_L^n`$ as a function of the number $`n`$ of occupied sites. $`Q_L^n`$ may be any of the wrapping probabilities $`R_L`$. Let $`n^{}`$ be the number of occupied sites for which percolation first occurs in a given realization. $`Q_L^n`$ represents the fraction of realizations in which $`n^{}`$ is less than or equal to $`n`$. Using all $`Q_L^n`$’s so evaluated, it is possible to calculate the function $`Q_L(p)`$ for all possible values of $`p`$ in the range between $`0`$ and $`1`$ by a convolution with the binomial distribution Newman00 :

$$Q_L(p)=\underset{n}{}\left(\genfrac{}{}{0pt}{}{N}{n}\right)p^n(1p)^{Nn}Q_L^n.$$
(1)
For the bond percolation problem, we just replace sites by bonds in the above steps.

The evaluation of the statistical errors can be done in a conventional fashion. As discussed in reference Newman00  the standard deviation of the binomial distribution (1) is given by

$$\sigma _{Q_L(p)}=\sqrt{\frac{Q_L(p)\left[1Q_L(p)\right]}{MCS}},$$
(2)
where $`Q_L(p)`$ in the above equation has been taken as the mean value of the corresponding wrapping probability and $`MCS`$ is the number of Monte Carlo steps per site.

As an illustration, we show in Fig. 1(a) and 1(b) the wrapping probabilities $`R_L^{(h)}`$ and $`R_L^{(1)}`$ as a function of the concentration $`p`$ of occupied sites for square lattices of different sizes. The exact values $`R_{\mathrm{}}(p_c)`$ of these quantities for an infinite square system were derived by Pinson Pinson94  and Ziff Ziff99 . In Ref. Newman00  it has been used these exact values to obtain an estimate for the percolation threshold $`p_c`$. For each system size $`L`$, one determines the $`p`$ value yielding a wrapping probability equal to exact critical value. This $`p`$ value provides the estimate of $`p_c^L`$ for that $`L`$. In the critical region, one knows that the estimates $`p_c^L`$ converge to the threshold $`p_c`$ according to

$$p_c^Lp_cL^{\theta 1/\nu }.$$
(3)
For square systems, using the known value $`4/3`$ of the exponent $`\nu `$ and $`\theta =2`$, as obtained in Newman00 , we have $`p_c^Lp_cL^{11/4}`$. By a finite size scaling, Newman and Ziff obtained $`p_c=0.59274621(13)`$ for the infinite system. This procedure is more complicated in higher dimensions. Since neither $`\theta `$ nor $`\nu `$ are known, one has to vary the scaling exponent to obtain a straight line. In Ref. Newman00 , it was found that the estimates of the percolation threshold for a simple cubic lattice scale as $`L^2`$. Thus, it seems to be not so easy to determine $`\nu `$ and $`\theta `$ separately by this method.

One has to note (Fig. 1b) that $`R_L^{(1)}`$ is different from the other probabilities, as it exhibits a maximum. In this case, $`p_c^L`$ can be estimated from the position of this maximum. $`R_L^{(1)}`$ is then of particular utility in systems for which the exact values are not known. We will see, moreover, that all the other wrapping probabilities can also be used to estimate the percolation threshold, as well as the correlation length critical exponent, on any lattice. There are, in addition, some quantities like $`R_L^{(2)}`$ in three dimensions which exhibit both a maximum and a crossing region.

## III approach and results

We have applied the Newman-Ziff algorithm to site percolation on the two-dimensional ($`2d`$) square, the three-dimensional simple hexagonal and simple cubic ($`3d`$) lattices, and to bond percolation on square (2$`d`$), simple cubic and HCP (hexagonal close-packed) lattices. Table 1 gives the system and sample sizes used in our study.

Before discussing the results, we analyze the standard deviation of some particular quantities. Fig. 2 shows the relative error of $`R_L^{(v)}`$ for the square lattice and $`R_L^{(x)}`$ for the hexagonal lattice as a function of the $`L`$, at the critical concentration. Apart from a strong dependence with small $`L`$, we clearly see that for larger lattice sizes the relative error is almost independent of $`L`$, as predicted by Eq. (2) and previously stressed by Newman and Ziff Newman00 , even for the three-dimensional hexagonal lattice. Similar behavior is found for other wrapping probabilities, other three-dimensional lattices, as well as for the bond problem in different lattice structures.

Let us now discuss the evaluation of the critical exponent, the percolation threshold and the wrapping probabilities. In order to get an idea of the performance of the present approach, we will first apply it to the problem in two dimensions where exact (or more accurate) results are available. From Fig. 1(a) one sees that the derivative of $`R_L^{(h)}`$ at the critical concentration increases as the lattice size increases. In fact, one expects that the maximum derivative of any wrapping probability not exhibiting a maximum scales as hu

$$\left(\frac{\mathrm{d}R_L}{\mathrm{d}p}\right)_{max}L^{1/\nu }.$$
(4)
Thus, the critical exponent $`\nu `$ can be estimated without any consideration of the critical concentration $`p_c`$ by taking the scaling behavior of the derivatives of the thermodynamic quantities $`R_L`$. They can be straightforwardly computed from relation (1)

$`{\displaystyle \frac{\mathrm{d}Q_L}{\mathrm{d}p}}={\displaystyle \underset{n}{}}[\left({\displaystyle \genfrac{}{}{0pt}{}{N}{n}}\right)np^{n1}(1p)^{Nn}`$
$`\left({\displaystyle \genfrac{}{}{0pt}{}{N}{n}}\right)(Nn)p^n(1p)^{Nn1}]Q_L^n.`$ (5)
In Fig. 3 we plot, on $`\mathrm{log}_{10}`$ scales, the maximum value of the derivative of $`R_L^{(v)}`$ as a function of system size, for site percolation on the square lattice (the hexagonal lattice will be discussed later); a linear fit yields $`\nu ^{(v)}=1.334(4)`$. Other quantities give independent estimates of the exponent (the corresponding data are too close to those of $`R_L^{(v)}`$ to be distinguished on the scale of Fig. 3). We find $`\nu ^{(h)}=1.331(2)`$; $`\nu ^{(b)}=1.339(4)`$ and $`\nu ^{(e)}=1.327(1)`$. Combining these four estimates we obtain $`\nu =1.333(5)`$, in very good agreement with the exact result $`4/3`$.

Fig. 4 illustrates the approach for evaluating the critical concentration, as well as the wrapping probabilities at $`p_c`$, applied again to the site percolation problem on the square lattice, through a cell-to-cell estimate. For a fixed probability occupation $`p`$, we compute the specified wrapping probability as a function of the lattice size. Fig. 4 shows $`R_L^{(v)}`$ as a function of $`L`$. For $`p<p_c`$, $`R_L^{(v)}`$ decreases with increasing lattice size. For $`p>p_c`$, it increases.

Exactly at $`p_c`$ one expects the wrapping probability to be independent of system size. Thus, by varying $`p`$ in the critical region and searching for a constant $`R_L^{(v)}`$ we obtain an estimate for $`p_c`$. The vertical dashed lines in Fig. 1(a) represent the limits on the $`p`$ values studied. From the data for $`R_L^{(v)}`$ in Fig. 4, we have then $`p_c=0.5928(2)`$ and $`R_L^{(v)}=0.523(4)`$. Combining this estimate with the ones coming from the other quantities we obtain the values listed in Table 2. The results are quite close to the exact or expected ones, despite the small systems (sizes up to $`128\times 128`$) and short runs (see table 1). Table 2 also gives the results obtained from the present procedure to the bond percolation problem (which is easily implemented in the algorithm) with an excellent estimate of the known critical concentration. Moreover, the wrapping probabilities, within the error bars, are the same for site and bond problems, confirming the universal character of these quantities.

Having demonstrated the good performance of the method in cases where exact results are available, we studied some three-dimensional lattices where data are not so ubiquitous in the literature. In particular, we treat the simple cubic, simple hexagonal and the HCP (hexagonal close-packed) lattices. To our knowledge, there are no results available for the wrapping probabilities on such geometries as well as no indication of their universal aspect regarding site and bond dilution.

As an example, we show in Fig. 1(c) and 1(d) the wrapping probabilities $`R_L^{(x)}`$ and $`R_L^{(1)}`$ as a function of $`p`$ for various lattice sizes, for site percolation on the simple hexagonal lattice. The corresponding scaling behavior of the derivative of $`R_L^{(x)}`$ is depicted in Fig. 3; an estimate for the critical exponent $`\nu `$ may be extracted from these data. In Fig. 5 we show the estimate for $`p_c`$ as well as the value of the wrapping probability $`R_L^{(x)}`$. The combined results are listed in Table 3 together with the values for the simple cubic lattice and those obtained for the bond percolation on the HCP and simple cubic lattices. One can clearly see that the wrapping probabilities are distinct for different geometries, as is the critical concentration. Not only are our $`p_c`$ estimate comparable to the values obtained previously, but the critical exponents found here are close to the expected result for this universality class, namely $`\nu =0.83(5)`$ from series Dunn , $`\nu =0.88(1)`$Stauffer91 , $`\nu =0.8765(16)`$ball  and $`\nu =0.893(40)`$tomita  from Monte Carlo simulations.

The data of Table 3 are, up to our knowledge, quite new for these three dimensional lattices. A by-product of the present results concerns the universality of $`R_L(p_c)`$ at the percolation threshold. One can clearly see that for site or bond percolation the wrapping probabilities of the simple cubic lattice are, within the error bars, the same (as well as for the problem in two dimensions depicted in Table 2). This is in quite good agreement with the expected universal aspect previously obtained for the spanning probability in general dimensions and with both free and periodic boundary conditions hovi .

Another interesting aspect of the three-dimensional lattices is the behavior of the quantity $`R_L^{(2)}(p)`$ giving the probability of wrapping around two directions and not around the third direction. Fig. 6 shows such behavior for the simple cubic site diluted problem. In this case one can obtain an estimate of the critical concentration not only from the position of its maximum but also from the crossings at $`p_c`$. It is noted, however, that a more accurate value is achieved from the analysis of the crossings (as done in Fig. 5) than from the location of its maximum. The same behavior occurs for the other lattice structures.

## IV Concluding remarks

We have seen that the results obtained using the present method are in good agreement with the exact (when available) or expected ones. It is important to note that this procedure has been implemented using relatively small systems and short Monte Carlo runs; better results could be achieved in larger-scale simulations. In addition, from the computed wrapping probabilities at $`p_c`$ for the square and simple cubic lattices one can also confirm their universal aspect regarding site and bond dilution. The same should hold, of course, for the other lattice geometries.

A slightly modified version of the present procedure, not using the cell-to-cell estimate, can also be applied to problems on two-dimensional lattices. Instead of tuning $`p`$, one can tune one of the $`R_L`$ in the critical region. For a given quantity $`R_L`$ (say, for example $`R_L^{(h)}`$) we fix it at a specified value $`R^{}`$ on the vicinity of the critical point, and proceed analogously to Newman and Ziff’s original approach. Observe that $`R^{}`$ is in this case a first estimate for $`R_{\mathrm{}}(p_c)`$. One can then compute, for each $`L`$, the intercept between the function $`R_L(p)`$, previously evaluated, with the fixed $`R^{}`$. Each of these intercepts gives an estimate for $`p_c^L`$, which is expected, for two-dimensional systems, to scale as $`L^\varphi `$ with $`\varphi =11/4`$. Therefore, plotting $`p_c^L\times L^{11/4}`$ for different values of $`R^{}`$, we can estimate the true $`R_{\mathrm{}}`$ as well as the percolation threshold by looking for the value of $`R^{}`$ that yields the best straight line. Table 2 reports the critical values so obtained for the two-dimensional lattice. The results are quite good and comparable to those obtained in the previous section for both the wrapping probabilities and the critical concentration. However, the errors are in general considerably larger. In three dimensions this procedure can be implemented only if we know the exponent $`\varphi `$ beforehand.

###### Acknowledgements.

Fruitful discussions with R. Dickman and D. P. Landau are gratefully acknowledged. We would also like to thank the referee for several comments on this work. This research was supported in part by Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq), Fundação Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES) and Fundação de Amparo à Pesquisa do Estado de Minas Gerais (FAPEMIG) \- Brazilian Agencies.


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# Quantum computing with antiferromagnetic spin clusters

## I Introduction

During the past years, the discovery of several powerful quantum algorithms bennett:00  has triggered substantial research efforts aiming at the implementation of a quantum computer in a physical system. The main difficulty is that qubits must be prepared, manipulated, and read out with high fidelity while decoherence is required to remain small. divincenzo:95  Solid-state implementations of qubits exploit the versatility of nanoscale fabrication, but suffer from decoherence times which are usually shorter than in many quantum optics proposals. cirac:00  Electron loss:98 ; burkard:99 ; levy:01  and nuclear privman:98 ; kane:98  spins have been identified as promising candidates for qubits in a solid state system. The main advantage of electron or nuclear spins is that they are natural two state systems and that decoherence times for the spin degree of freedom kikkawa:97 ; feher:59  are usually larger than for charge degrees of freedom.

Here we show that a wide variety of spin clusters are promising candidate systems for qubits. Qubits formed by several spins have so far mainly been discussed in the context of exchange-only quantum computing, divincenzo:00 ; levy:02 ; lidar:02  coherence-preserving qubits bacon:01 , and quantum computing schemes in which the requirements on the control of exchange interactions between spins are relaxed. benjamin:02  However, all these schemes require control at the single-spin level, either with local magnetic fields benjamin:02  or exchange interactions. divincenzo:00 ; bacon:01  For the spin clusters considered here, control for both magnetic fields and exchange interactions is required only on the length scale of the spin cluster diameter. As we have shown in Ref. meier:02, , spin chains formed by an odd number of antiferromagnetically coupled spins $`s=1/2`$ allow one to define a logical qubit. The logical state of the qubit is encoded in the collective state of the spin cluster. Here we detail that this construction remains valid for a wide range of spin clusters, independent of the details of intracluster exchange interaction and spin placement. Initialization and readout of the spin cluster is achieved with the methods developed for single spins. loss:98 ; burkard:99  The main advantage of spin clusters is that the requirements on spatial control can be traded for gate operation times. The scaling of the decoherence rate with the size of the spin cluster depends on the microscopic decoherence mechanism. While the decoherence rate induced by fluctuating local magnetic fields increases with cluster size, we show that magnetic dipolar interactions for the spin cluster qubit are smaller than for single spins. The optimum size of the spin cluster qubit is determined by a trade-off between the increase in gate operation times and the decoherence rate effected by local fluctuating magnetic fields, the decrease in magnetic dipolar interaction energy, and the relaxed conditions on local control.

Any quantum computation can be decomposed into a sequence of one- and two-qubit quantum gates. bareno:95  For a single-spin qubit, the $`\widehat{s}_z`$ eigenstates $`|`$ and $`|`$ are identified as logical basis states $`|0`$ and $`|1`$, respectively. loss:98 ; burkard:99  The phase shift gate can then be realized by a magnetic field $`B_z(t)`$ and the one-qubit rotation gate $`U_{\mathrm{rot}}`$ by a transverse field $`B_x(t)`$ which rotates $`|`$ into $`|`$ and vice versa. More generally, the equations

$$0|\widehat{H}^{}|0=1|\widehat{H}^{}|1\mathrm{and}1|\widehat{H}^{}|00$$
(1)
constitute a sufficient condition that a Hamiltonian $`\widehat{H}^{}`$ induces the unitary time evolution required for $`U_{\mathrm{rot}}`$. For single spins, $`\widehat{H}^{}=g\mu _BB_x(t)\widehat{s}_x`$ fulfills Eq. (1). Similarly, an exchange interaction $`\widehat{H}_{}=J_{}\widehat{𝐬}_1\widehat{𝐬}_2`$ generates the unitary time evolution required for the square-root of SWAP gate loss:98  because, in the two-qubit product basis,

$$10|\widehat{H}_{}|010.$$
(2)
In contrast to a single spin $`s=1/2`$, clusters formed by $`n_c`$ coupled spins are not intrinsically two-state systems. In order to prove that a logical qubit can be defined in terms of the energy eigenstates of a spin cluster we will (a) identify spin clusters with a ground state doublet $`\{|0,|1\}`$ separated from the next excited state by an energy gap $`\mathrm{\Delta }`$; (b) identify Hamiltonians $`\widehat{H}^{}`$ and $`\widehat{H}_{}`$ which satisfy Eqs. (1) and (2) and, hence, allow one to generate a universal set of quantum gates; and (c) quantify leakage and decoherence for the spin cluster qubit. In particular, the evaluation of the matrix elements in Eqs. (1) and (2) and the quantification of excitation out of the computational basis (leakage) requires a detailed characterization of the states $`\{|0,|1\}`$ which is, in general, nontrivial.

This paper is organized as follows. In Sec. II we discuss the computational basis states for spin-$`1/2`$ chains. For this simple geometry, it is possible to derive analytical expressions for the matrix elements in Eqs. (1) and (2) for various anisotropies and spatially varying intracluster exchange interaction. Section III discusses the insensitivity of spin cluster qubits to the details of interactions within the cluster, such as the relative placement of spins and the exchange strengths. In Sec. IV, spins with spin quantum numbers larger than $`1/2`$ are discussed. In Sec. V, we draw our conclusions.

## II Spin chains

For simplicity, we first consider a spin cluster qubit formed by a spin chain,

$$\widehat{H}=\underset{i=1}{\overset{n_c1}{}}f_j[J_{}(\widehat{s}_{j,x}\widehat{s}_{j+1,x}+\widehat{s}_{j,y}\widehat{s}_{j+1,y})+J_z\widehat{s}_{j,z}\widehat{s}_{j+1,z}]$$
(3)
where $`n_c`$ is odd and $`J_{},J_z>0`$. The real numbers $`f_j>0`$ account for a spatial variation of the exchange interaction, and $`J_{}f_j`$ ($`J_zf_j`$) denotes the transverse (longitudinal) exchange interaction between sites $`j`$ and $`j+1`$.

### II.1 Isotropic spin chains

For electron spins in quantum dots, the nearest neighbor exchange is usually of the Heisenberg form, burkard:99  $`J=J_{}=J_z`$. We first consider $`f_j1`$,

$$\widehat{H}=J\underset{j=1}{\overset{n_c1}{}}\widehat{𝐬}_j\widehat{𝐬}_{j+1}$$
(4)
with $`J>0`$. Note that this is an open spin chain; a closed spin chain would have a fourfold degenerate ground state multiplet for odd $`n_c`$ that would make it unsuitable for representing a single qubit. Because the intracluster exchange interaction $`J`$ is time independent and no external control is required, $`J`$ can be adjusted already during sample growth.

Spin chains have been studied in great detail during the past decades. orbach:58 ; walker:59 ; lieb:61  The theoretical description of the antiferromagnetic spin chain Eq. (4) is particularly challenging because the classical Néel ordered state is not an energy eigenstate and quantum fluctuations are pronounced. We define the operator of total spin,

$$\widehat{S}_\alpha =\underset{j=1}{\overset{n_c}{}}\widehat{s}_{j,\alpha }$$
(5)
for $`\alpha =x,y,z`$. Energy eigenstates can be labeled according to their quantum numbers of total spin $`\widehat{𝐒}`$ and the $`z`$-component of total spin, $`\widehat{S}_z`$, because

$$[\widehat{H},\widehat{𝐒}^2]=[\widehat{H},\widehat{S}_z]=0.$$
(6)
Due to the antiferromagnetic exchange coupling, states in which the total spin of the chain is minimized are energetically most favorable. lieb:62  For even $`n_c`$, the minimum possible spin is $`S=0`$, and the system has a nondegenerate ground state. In contrast, for odd $`n_c`$, there is a ground state doublet (Fig. 1). lieb:62  This parity effect is well known for thermodynamic quantities. bonner:64  The energy gap $`\mathrm{\Delta }`$ separating the ground state doublet from the next excited state,

$$\mathrm{\Delta }\frac{J\pi }{2}k_{\mathrm{min}}\frac{J\pi ^2}{2n_c},$$
(7)
can be estimated from the lower bound of the des Cloiseaux-Pearson spectrum and the minimum wave vector $`k_{\mathrm{min}}=\pi /n_c`$ (Ref. nagaosa, ). Henceforth, we will restrict our attention to spin chains with odd $`n_c`$.

The requirements on a candidate system for qubits include initialization of the quantum computer, a universal set of quantum gates, decoherence times long compared to gate operation times, and readout of the qubit. divincenzo:95

#### II.1.1 Definition of the spin cluster qubit

For the chain with an odd number of sites \[Fig. 2(a)\], we define the spin cluster qubit in terms of the $`S=1/2`$ ground state doublet by

$`\widehat{S}_z|0`$ $`=`$ $`{\displaystyle \frac{1}{2}}|0,`$
$`\widehat{S}_z|1`$ $`=`$ $`{\displaystyle \frac{1}{2}}|1.`$ (8)
The states $`\{|0,|1\}`$ do not in general have a simple representation in the single-spin product basis, but rather are complicated superpositions of $`n_c!/[(n_c1)/2]![(n_c+1)/2]!`$ states \[Figs. 2(b) and (c)\] as evidenced by the local magnetization density \[Fig. 2(d)\]. The largest amplitude in this superposition corresponds to the Néel ordered states $`|_1|_2\mathrm{}|_{n_c}`$ ($`|0`$) and $`|_1|_2\mathrm{}|_{n_c}`$ ($`|1`$), respectively. For $`n_c=9`$, the Néel configuration has only a $`20`$% probability; the remaining $`80`$% represent quantum fluctuations \[see Figs. 2(b) and (c)\].

In spite of their complicated representation in the single-spin product basis, $`|0`$ and $`|1`$ are in many respects very similar to the states $`|`$ and $`|`$ of a single spin and, hence, define the computational basis for universal quantum computing with *spin cluster qubits*. The reason for this is that $`\{|0,|1\}`$ belong to one $`S=1/2`$ doublet such that

$$\widehat{S}^{}|0=|1,\widehat{S}^+|1=|0,$$
(9)
where $`\widehat{S}^\pm =\widehat{S}_x\pm i\widehat{S}_y`$ are the spin ladder operators of the spin chain.

#### II.1.2 Initialization

Initialization of the spin cluster qubit can be achieved by cooling in a magnetic field with $`g\mu _BB_z\mathrm{\Delta }`$ to temperatures $`Tg\mu _BB_z/k_B`$. The spin cluster will relax to $`|0`$ within the spin relaxation time. Because thermalization is typically slow, the preparation of a given initial state could be facilitated by the measurement of the spins within the clusters, possibly followed by local operations. In this way, a state which is energetically close to the ground state could be prepared.

#### II.1.3 Quantum Gate operation

The one-qubit phase shift gate $`U_\varphi `$, one-qubit rotation gate $`U_{\mathrm{rot}}`$, and CNOT gate $`U_{\mathrm{CNOT}}`$ constitute a universal set of quantum gates. According to Eq. (9), a magnetic field that is constant over the spin cluster qubit acts on the states of the spin cluster qubit in the same way as on a single-spin qubit. meier:02  Constant magnetic fields $`B_z`$ ($`B_x`$) effect the one-qubit phase shift (one-qubit rotation) quantum gate without leakage. Because $`|0`$ and $`|1`$ are degenerate and separated from the next excited state by $`\mathrm{\Delta }`$, one-qubit quantum gates can be realized with high fidelity also by any spatially varying magnetic field for which $`|1|_{j=1}^{n_c}g_j\mu _BB_{j,x}\widehat{s}_{j,x}|0|0`$ ($`U_{\mathrm{rot}}`$) and $`0|_{j=1}^{n_c}g_j\mu _BB_{j,z}\widehat{s}_{j,z}|00`$ ($`U_\varphi `$), respectively. Here, $`g_j`$ is the electron spin $`g`$ factor at site $`j`$. Such spatially varying fields can potentially cause leakage. However, if $`|g_j\mu _BB_j|/\mathrm{\Delta }1`$ and if all $`B_j`$ are switched on and off adiabatically, i.e., on time scales long compared to $`h/\mathrm{\Delta }`$, the quantum gate fidelity is close to $`100`$% as we will discuss in detail in Sec. II.3.

For the CNOT gate, one requires an exchange interaction $`\widehat{H}_{}`$ between one or several spins of neighboring spin cluster qubits I and II which can be switched on and off, e.g., by electrical gates. loss:98  The simplest case of an exchange interaction between the outermost spins of neighboring clusters \[Fig. 2(e)\], $`\widehat{H}_{}=J_{}(t)\widehat{𝐬}_{n_c}^\mathrm{I}\widehat{𝐬}_1^{\mathrm{II}}`$ translates into an isotropic exchange interaction also for the two-qubit product basis. This remains true for any $`\widehat{H}_{}`$ of the form

$$\widehat{H}_{}=J_{}(t)\widehat{𝐬}_{n_c}^\mathrm{I}\widehat{𝐬}_1^{\mathrm{II}}+J_{}(t)\underset{j=1}{\overset{n_c1}{}}(v_j^\mathrm{I}\widehat{𝐬}_j^\mathrm{I}\widehat{𝐬}_{j+1}^\mathrm{I}+v_j^{\mathrm{II}}\widehat{𝐬}_j^{\mathrm{II}}\widehat{𝐬}_{j+1}^{\mathrm{II}}).$$
(10)
Here, the factors $`v_j`$ allow for a spatial variation of the intracluster exchange coupling constants during gate operation, where $`|v_j|<1`$ and $`|J_{}|J`$ is the limit relevant for experiments. $`\widehat{H}_{}`$ will in general not only couple states within the two-qubit product basis $`\{|00,|01,|10,|11\}`$, but will also lead to leakage. As long as $`J_{}(t)`$ changes adiabatically and $`|J_{}(t)|\mathrm{\Delta }`$ for all times, leakage remains small. It should be noted that this adiabaticity condition also holds for single electrons in quantum dots where, however, the energy gap $`\mathrm{\Delta }`$ is usually larger than for the spin cluster qubit. The action of $`\widehat{H}_{}`$ can then be described by an effective Hamiltonian in the two-qubit product basis,

$`\widehat{H}_{}`$ $`=`$ $`J_z(t)\widehat{S}_z^\mathrm{I}\widehat{S}_z^{\mathrm{II}}+{\displaystyle \frac{J_{}(t)}{2}}(\widehat{S}^{\mathrm{I}+}\widehat{S}^{\mathrm{II}}+\widehat{S}^\mathrm{I}\widehat{S}^{\mathrm{II}+})`$ (11)
$`+J_o(t)\mathrm{𝟏},`$
where the roman numbers label the spin clusters, and

$`J_z(t)`$ $`=`$ $`4J_{}(t)|_\mathrm{I}0|\widehat{s}_{n_c,z}^\mathrm{I}|0_\mathrm{I}||_{\mathrm{II}}0|\widehat{s}_{1,z}^{\mathrm{II}}|0_{\mathrm{II}}|,`$
$`J_{}(t)`$ $`=`$ $`4J_{}(t)|_\mathrm{I}1|\widehat{s}_{n_c,x}^\mathrm{I}|0_\mathrm{I}||_{\mathrm{II}}1|\widehat{s}_{1,x}^{\mathrm{II}}|0_{\mathrm{II}}|,`$ (12)
$`J_o(t)`$ $`=`$ $`J_{}(t)[_\mathrm{I}0|{\displaystyle \underset{j=1}{\overset{n_c1}{}}}v_j^\mathrm{I}\widehat{𝐬}_j^\mathrm{I}\widehat{𝐬}_{j+1}^\mathrm{I}|0_\mathrm{I}`$
$`+_{\mathrm{II}}0|{\displaystyle \underset{j=1}{\overset{n_c1}{}}}v_j^{\mathrm{II}}\widehat{𝐬}_j^{\mathrm{II}}\widehat{𝐬}_{j+1}^{\mathrm{II}}|0_{\mathrm{II}}].`$
For the derivation of Eq. (11), see Appendix A.

Because, for the isotropic chain,

$${}_{\mathrm{I}}{}^{}0|\widehat{s}_{n_c,z}^\mathrm{I}|0_{\mathrm{I}}^{}=|_\mathrm{I}1|\widehat{s}_{n_c,x}^\mathrm{I}|0_\mathrm{I}|,$$
(13)
the coupling $`\widehat{H}_{}`$ is isotropic also in the two-qubit product basis and acts on the states $`|0`$ and $`|1`$ of neighboring spin chains in the same way as an isotropic exchange interaction between two single spins.

An explicit switching sequence for the CNOT gate based on single-qubit rotations and the unitary time evolution governed by the exchange interaction in Eq. (11) is meier:02

$`U_{\mathrm{CNOT}}e^{i\pi S_y^{\mathrm{II}}/2}e^{i2\pi 𝐧_1𝐒^\mathrm{I}/3}e^{i2\pi 𝐧_2𝐒^{\mathrm{II}}/3}U_{}(\pi /2)`$
$`\times e^{i\pi S_y^\mathrm{I}}U_{}(\pi /2)e^{i\pi S_x^\mathrm{I}/2}e^{i\pi S_x^{\mathrm{II}}/2}e^{i\pi S_y^{\mathrm{II}}/2}`$ (14)
for the general case where $`J_zJ_{}`$. Here, $`𝐧_1=(1,1,1)/\sqrt{3}`$ and $`𝐧_2=(1,1,1)/\sqrt{3}`$, and we have defined the unitary time evolution operator $`U_{}(\pi /2)=\widehat{\mathrm{T}}_t\mathrm{exp}\left(i𝑑t\widehat{H}_{}/\mathrm{}\right)`$, with $`𝑑tJ_{}(t)/\mathrm{}=\pi /2`$.

The gate operation time for $`U_{}(\pi /2)`$ is limited from below by $`h/16J_{}|_\mathrm{I}1|\widehat{s}_{n_c,x}^\mathrm{I}|0_\mathrm{I}||_{\mathrm{II}}1|\widehat{s}_{1,x}^{\mathrm{II}}|0_{\mathrm{II}}|`$, where $`J_{}`$ is the maximum value of the exchange coupling. Matrix elements such as $`|_\mathrm{I}1|\widehat{s}_{n_c,x}^\mathrm{I}|0_\mathrm{I}|`$ decrease with increasing $`n_c`$, which leads to an increase in gate operation time. For realistic parameters and small $`n_c`$ (see Sec. II.6 below), $`J_{}`$ is limited by experimental constraints rather than the condition $`J_{}\mathrm{\Delta }`$. Then, the increase in gate operation time compared to single-spin qubits is $`1/(4|_\mathrm{I}1|\widehat{s}_{n_c,x}^\mathrm{I}|0_\mathrm{I}||_{\mathrm{II}}1|\widehat{s}_{1,x}^{\mathrm{II}}|0_{\mathrm{II}}|)`$ and depends only on the matrix elements of the spin operators. Similarly, for a given magnetic field, the increase of the time required for a one-qubit rotation depends only on the matrix elements $`|1|\widehat{s}_{j,x}|0|`$.

#### II.1.4 Decoherence

For spin clusters, decoherence usually is faster than for single spins. The scaling of the decoherence time $`\tau _\varphi `$ with system size depends on the microscopic decoherence mechanism. For electron spins in quantum dots, fluctuating fields and nuclear spins have been identified as dominant sources. loss:98 ; burkard:99 ; khaetskii:02 ; merkulov:02 ; schliemann:02 ; khaetskii:03 ; sousa:03  In the following, we discuss two scenarios for decoherence in which (i) a fluctuating field couples to the total magnetic moment of the spin cluster qubit, and (ii) independent fluctuating fields act on each spin of the spin cluster qubit individually.

In order to obtain analytical estimates for the scaling of $`\tau _\varphi `$ with $`n_c`$, we restrict our analysis to a phenomenological model in which decoherence is effected by a fluctuating classical field $`\mathrm{}b(t)`$. In case (i),

$$\widehat{H}^B=\mathrm{}b(t)\widehat{S}_z.$$
(15)
The decoherence rate is obtained from blum:96

$`{\displaystyle \frac{1}{\tau _\varphi }}`$ $`=`$ $`\pi {\displaystyle \underset{|k|0}{}}|k|\widehat{S}_z|0|^2C(E_kE_0)`$
$`+\pi {\displaystyle \underset{|k|1}{}}|k|\widehat{S}_z|1|^2C(E_kE_1)`$
$`+\pi (0|\widehat{S}_z|01|\widehat{S}_z|1)^2C(0),`$
where

$$C(E)=\frac{1}{2\pi }_{\mathrm{}}^{\mathrm{}}𝑑te^{iEt/\mathrm{}}b(t)b(0)$$
(17)
is the spectral density of the random field in Eq. (15). Because of Eq. (8), we find that the decoherence rate $`1/\tau _\varphi =\pi C(0)`$ is independent of $`n_c`$. This result, which is in stark contrast to the standard result that the decoherence rate increases with system size, can be traced back to the fact that in Eq. (15) only the total magnetic moment couples to the fluctuating field and the magnetic moment $`\pm g\mu _B/2`$ of the spin cluster qubit is identical to the one of a single spin. Similarly, for a non-diagonal coupling $`\widehat{H}^B=\mathrm{}b(t)\widehat{S}_x`$, from Eq. (II.1.4) we find $`1/\tau _\varphi =\pi C(0)/2`$.

Decoherence due to the coupling to nuclear spins is a complicated theoretical problem in its own right. khaetskii:02 ; merkulov:02 ; schliemann:02 ; khaetskii:03 ; sousa:03  In order to obtain a heuristic estimate for the scaling of the decoherence time with $`n_c`$ for this decoherence scenario, we consider fluctuating classical fields which act independently on each site of the spin cluster,

$$\widehat{H}^B=\underset{j=1}{\overset{n_c}{}}\mathrm{}b_j(t)\widehat{s}_{j,z},$$
(18)
where $`b_i(t)b_j(0)\delta _{ij}`$. For Gaussian white noise with

$$b_i(t)b_j(0)=2\pi \gamma ^B\delta _{ij}\delta (t),$$
(19)
$`1/\tau _\varphi n_c\pi \gamma ^B`$ scales linearly with $`n_c`$, i.e., if fluctuating fields act independently on the individual spins of the cluster, the decoherence rate increases with $`n_c`$. This result for the scaling of $`1/\tau _\varphi `$ with system size agrees with the standard result for $`n_c`$ qubits which are subject to independently fluctuating fields. unruh:95  Note that an increase in the decoherence rate by a factor $`n_c`$ implies that the probability for the state of the spin cluster qubit to remain unaffected by the fluctuating fields for a certain time $`t`$ decreases exponentially with $`n_c`$ (Ref. unruh:95, ).

Magnetic dipolar interactions are another source of decoherence. Consider two single-spin qubits $`\widehat{𝐬}_1`$ and $`\widehat{𝐬}_2`$ with coordinate vectors $`𝐫_1`$ and $`𝐫_2`$, respectively, that are coupled by the magnetic dipolar interaction,

$$\widehat{H}_{\mathrm{dip}}=\frac{\mu _0(g\mu _B)^2}{4\pi }\frac{\widehat{𝐬}_1\widehat{𝐬}_23(\widehat{𝐬}_1𝐞_r)(\widehat{𝐬}_2𝐞_r)}{d^3},$$
(20)
where $`𝐫=𝐫_1𝐫_2`$, $`d=|𝐫|`$ is the distance between the single-spin qubits, and $`𝐞_r=𝐫/|𝐫|`$. In first order perturbation theory, the dipolar interaction leads to an energy shift $`\pm E_{\mathrm{dip}}`$ for the product states with parallel and antiparallel spin configurations, respectively. For lateral quantum dots with spin quantization axis perpendicular to $`𝐞_r`$,

$`E_{\mathrm{dip}}`$ $`=`$ $`,|\widehat{H}_{\mathrm{dip}}|,`$ (21)
$`=`$ $`{\displaystyle \frac{\mu _0(g\mu _B)^2}{4\pi }}{\displaystyle \frac{,|\widehat{𝐬}_1\widehat{𝐬}_2|,}{d^3}}={\displaystyle \frac{\mu _0(g\mu _B)^2}{16\pi d^3}},`$
because the expectation value of $`(\widehat{𝐬}_1𝐞_r)(\widehat{𝐬}_2𝐞_r)`$ vanishes identically. Similarly, we find

$`,|\widehat{H}_{\mathrm{dip}}|,`$ $`=`$ $`+E_{\mathrm{dip}},`$
$`,|\widehat{H}_{\mathrm{dip}}|,`$ $`=`$ $`E_{\mathrm{dip}},`$ (22)
$`,|\widehat{H}_{\mathrm{dip}}|,`$ $`=`$ $`E_{\mathrm{dip}}.`$
The deterministic phase shift due to the different dipolar energies for parallel and antiparallel spin configurations could be accounted for at the end of a quantum algorithm if no other error sources were present. However, it leads to correlated errors when spins are coupled to an environment that induces, e.g., spin flip errors. While $`E_{\mathrm{dip}}`$ is too small to induce errors of order $`10^4`$ for electron spins in quantum dots, dipolar interactions are large for, e.g., P dopants in a Si matrix (see Sec. II.6). We show next that dipolar interactions for spin cluster qubits are smaller than for single-spin qubits. For definiteness, we consider two clusters with spins at sites $`𝐫_j^\mathrm{I}=jd𝐞_y`$ and $`𝐫_j^{\mathrm{II}}=(j+n_c)d𝐞_y`$ for clusters I and II, respectively, with $`j=1,2,\mathrm{},n_c`$ \[Fig. 2(c)\]. The intracluster dipolar interactions lead to an unimportant energy shift that is identical for both $`|0`$ and $`|1`$,

$`{\displaystyle \underset{i>j}{}}{\displaystyle \frac{\mu _0(g\mu _B)^2}{4\pi d^3}}0|{\displaystyle \frac{\widehat{𝐬}_i\widehat{𝐬}_j3\widehat{s}_{i,y}\widehat{s}_{j,y}}{(ij)^3}}|0`$
$`={\displaystyle \underset{i>j}{}}{\displaystyle \frac{\mu _0(g\mu _B)^2}{4\pi d^3}}1|{\displaystyle \frac{\widehat{𝐬}_i\widehat{𝐬}_j3\widehat{s}_{i,y}\widehat{s}_{j,y}}{(ij)^3}}|1`$ (23)
because of symmetry. The interqubit dipolar interaction,

$$\widehat{H}_{\mathrm{dip}}^{\mathrm{sc}}=\frac{\mu _0(g\mu _B)^2}{4\pi d^3}\underset{i,j}{}\frac{\widehat{𝐬}_i^\mathrm{I}\widehat{𝐬}_j^{\mathrm{II}}3\widehat{s}_{i,y}^\mathrm{I}\widehat{s}_{j,y}^{\mathrm{II}}}{(ij+n_c)^3},$$
(24)
gives rise to an energy shift of the states $`|00`$ and $`|11`$ relative to $`|01`$ and $`|10`$, where $`|0`$ and $`|1`$ denote the logical basis of the spin cluster qubit,

$`00|\widehat{H}_{\mathrm{dip}}^{\mathrm{sc}}|00=11|\widehat{H}_{\mathrm{dip}}^{\mathrm{sc}}|11`$ $`=`$ $`E_{\mathrm{dip}}^{\mathrm{sc}},`$
$`01|\widehat{H}_{\mathrm{dip}}^{\mathrm{sc}}|01=10|\widehat{H}_{\mathrm{dip}}^{\mathrm{sc}}|10`$ $`=`$ $`E_{\mathrm{dip}}^{\mathrm{sc}},`$ (25)
similarly to single-spin qubits. Evaluating the matrix elements numerically, we find that the characteristic dipolar energy $`E_{\mathrm{dip}}^{\mathrm{sc}}`$ decreases with increasing $`n_c`$ We find $`E_{\mathrm{dip}}^{\mathrm{sc}}/E_{\mathrm{dip}}=0.42,0.25,0.16`$, and $`0.12`$ for $`n_c=3,5,7`$, and $`9`$, respectively, where $`E_{\mathrm{dip}}`$ is the dipolar energy for single-spin qubits. This shows that decoherence effected by magnetic dipolar interactions is indeed smaller for spin cluster qubits than for single spins.

#### II.1.5 Readout

Readout of the spin cluster qubit is achieved by measuring the individual spins within the cluster ($`\widehat{s}_{i,z}`$) or the state of the total spin of the cluster ($`\widehat{S}_z`$). The measurement of individual spins still is a considerable experimental challenge. However, as has been shown theoretically, loss:98 ; recher:00  measurement of single spins is feasible via charge degrees of freedom. More specifically, the state of a single spin on a quantum dot can be detected by a current flowing between spin polarized leads that are tunnel coupled to the quantum dot. recher:00

If an experimental technique is established that allows one to measure the state of a single spin, it will also be possible to measure the state of a spin cluster qubit by measurement of all spins of the cluster. Because $`0|_{i=1}^{n_c}\widehat{s}_{i,z}|0=1/2`$ and $`1|_{i=1}^{n_c}\widehat{s}_{i,z}|1=1/2`$, this will allow one to unambiguously determine the state of the cluster qubit. However, the state of the cluster determines the local spin density at each site \[Fig. 2(d)\], and a probabilistic readout is possible also by measurement of single spins only. For example, for $`n_c=9`$, if the measurement of the central spin of the chain yields $`+1/2`$, the spin cluster qubit has been in state $`|0`$ with a probability of $`70`$%. A selective readout of several spins of the spin cluster qubit would also reduce the requirements on the readout sensitivity. For example, the sublattice spin $`0|\widehat{s}_{1,z}+\widehat{s}_{3,z}+\widehat{s}_{5,z}+\widehat{s}_{7,z}+\widehat{s}_{9,z}|01`$ for $`n_c=9`$ is twice as large as the total magnetic moment $`0|\widehat{S}_z|0`$ and could be measured after separating the electron spins at even and odd sites of the cluster. This illustrates that readout of single spins is sufficient but not necessary to measure the state of the spin cluster qubit.

Spin readout can also be effected by optical means. A scheme for gate operation based on Pauli blocking has been suggested recently. pazy:03  In a similar way, the creation of a spin polarized exciton by a circularly polarized laser beam and the subsequent obervation of the reemitted photon would allow one to determine the spin state of a single electron. The underlying principle is that, for a quantum dot with an electron spin pointing up, Pauli’s exclusion principle prohibits the creation of an exciton in which the electron with spin up occupies the same orbital state. The creation of an exciton, which can be observed by the photon emitted on recombination, is possible only if the electron spin in the quantum dot points opposite to the one of the exciton created by the laser beam. However, for qubits based on spins in a single quantum dot, the minimum laser focus on the order of the wavelength puts severe constraints on an optical readout scheme. These constraints are relaxed for spin cluster qubits where it is sufficient to have a laser spot size with a diamater smaller than the size of the spin cluster qubit.

### II.2 Varying exchange constants

The formation of a spin cluster qubit from an odd number of antiferromagnetically coupled spins requires little control over intracluster exchange constants. Although both the energy gap $`\mathrm{\Delta }`$ and matrix elements such as $`1|\widehat{s}_{j,x}|0`$ depend on the spatial variation of exchange constants, the general principle of assembling several spins into a cluster qubit remains valid.

In order to demonstrate the robustness of our spin cluster qubit against a variation of exchange constants, we return to the isotropic spin chain but now allow for varying $`f_j`$ in Eq. (3). Because the isotropic spin chain still exhibits a $`S=1/2`$ ground state doublet, lieb:62  quantum computing is possible as discussed for $`f_j1`$ in Sec. II.1. From an experimental point of view, a priori knowledge of the factors $`f_j`$ is not necessary for quantum computing. Rather, the relevant matrix elements such as $`|1|\widehat{s}_{j,x}|0|`$ can be determined experimentally. Similarly, a quantum computer could even be assembled from spin cluster qubits which are not identical.

If the exchange constants can be controlled during sample growth, the properties of the spin cluster qubit can be engineered to a certain extent. For clusters with centrosymmetric exchange constants, the time required to perform the square-root of swap gate $`U_{}(\pi /2)`$ for given $`J_{}`$ increases with $`1/|0|\widehat{s}_{1,z}|0|^2`$. For $`n_c=9`$ and $`f_j1`$, $`|0|\widehat{s}_{1,z}|0|0.18`$ corresponding to an increase in the gate operation time for $`U_{}(\pi /2)`$ by a factor $`(0.5/0.18)^27.7`$ compared to the single-spin qubit for given $`J_{}`$. However, by tuning the outermost couplings to small values $`f_1=f_{n_c1}\mathrm{min}_{j=2,\mathrm{},n_c2}f_j`$, the spin density at the outermost sites increases and approaches $`1/3`$ \[see dashed lines in Fig. 2(d) and Appendix B for a proof of this statement\]. Although the energy gap $`\mathrm{\Delta }`$ also decreases and is approximated by $`Jf_1`$ in this limit, a trade-off between the increasing matrix elements and the decreasing energy gap would allow one to decrease gate operation times compared to the chain with spatially constant exchange coupling.

### II.3 Leakage

We next discuss in more detail the one qubit rotation gate induced by a transverse magnetic field in order to quantify leakage. A related analysis for the CNOT gate has been reported in Ref. meier:02, .

Because $`\widehat{S}_x|0=(\mathrm{}/2)|1`$ and $`\widehat{S}_x|1=(\mathrm{}/2)|0`$, a magnetic field that is uniform over the spin cluster acts on the spin cluster qubit in the same way as on a single spin $`s=1/2`$. In particular, the Hamiltonian

$$\widehat{H}^{}=g\mu _BB_x(t)\widehat{S}_x$$
(26)
induces a coherent rotation from $`|0`$ to $`|1`$ without leakage, as implied by quantum mechanical selection rules. The gate operation time for a rotation by $`\varphi `$ is determined by $`_0^t𝑑t^{}g\mu _BB_x(t^{})/\mathrm{}=\varphi `$ and is identical to the one for single spins. In contrast, the one-qubit rotation effected by a spatially varying magnetic field

$$\widehat{H}^{}=\underset{j=1}{\overset{n_c}{}}g_j\mu _BB_{j,x}(t)\widehat{s}_{j,x}$$
(27)
will in general lead to leakage because of finite matrix elements $`i|\widehat{H}^{}|00`$ and $`i|\widehat{H}^{}|10`$ coupling the computational basis to higher excited states $`|i|0,|1`$. The adiabatic theorem guarantees that leakage remains small if the Fourier transform of $`B_{j,x}`$ vanishes for frequencies larger than $`\mathrm{\Delta }/\mathrm{}`$. Even if this adiabaticity requirement is not met, admixing of higher excited states to $`\{|0,|1\}`$ is controlled by the parameters $`g_j\mu _BB_{j,x}/\mathrm{\Delta }`$ and remains small if $`|g_j\mu _BB_{j,x}|\mathrm{\Delta }`$ for all $`j`$.

In the following, we concentrate on $`n_c=5`$ spins. As shown in Fig. 3(a) and Fig. 4, a magnetic field constant over the cluster coherently rotates $`|0`$ into $`|1`$. This is also evidenced by the in-phase rotation of all spins. In order to illustrate that also a spatially inhomogeneous field can induce the one-qubit rotation with high gate fidelity, we now consider a magnetic field $`B_{3,x}`$ acting only on the central spin ($`j=3`$) of the cluster. The field is switched on instantaneously at $`t=0`$. For $`t>0`$, the time evolution is then governed by the sum of the time-independent Hamiltonian of the spin cluster, $`\widehat{H}`$, and the Zeeman Hamiltonian $`\widehat{H}^{}=g\mu _BB_{3,x}\widehat{s}_{3,x}`$. In Fig. 4(a), for an initial state $`|\psi (t=0)=|0`$, we plot the projection of the state $`|\psi (t)`$ onto the qubit basis states for $`g\mu _BB_{3,x}/J=0.1`$ (dashed line, coinciding with the solid line on this scale) and $`0.5`$ (dashed-dotted line), respectively. The time evolution is obtained by numerical integration of the Schrödinger equation. For small $`g\mu _BB_{3,x}\mathrm{\Delta }0.72J`$, the spatially inhomogeneous field rotates $`|0`$ into $`|1`$ with high fidelity. The gate fidelity $`|1|U_{\mathrm{rot}}|0|^2`$ decreases from $`99.8`$% ($`g\mu _BB_x/J=0.1`$) to $`93.4`$% for $`g\mu _BB_x=0.5J`$, where the typical energy scale of $`\widehat{H}^{}`$ becomes comparable to $`\mathrm{\Delta }`$. Here, $`U_{\mathrm{rot}}=\widehat{\mathrm{T}}_t\mathrm{exp}\left(i_0^{t_{max}}𝑑t(\widehat{H}+\widehat{H}^{})/\mathrm{}\right)`$ with $`t_{max}=h/(4|1|\widehat{s}_{x,3}|0|g\mu _BB_x)`$ describes the time evolution during a $`\pi `$-rotation.

The decrease in gate fidelity with increasing $`B_{3,x}`$ can be understood from the local spin densities \[Figs. 3(b), (c), and (d)\]. Although only the central spin is acted on by $`B_{3,x}`$, for $`|g\mu _BB_{3,x}|\mathrm{\Delta }`$ all spins of the spin cluster corotate with the central spin due to the exchange field. The condition $`|g\mu _BB_{3,x}|\mathrm{\Delta }`$ guarantees that the externally induced rotation of the central spin is sufficiently slow that all spins of the chain corotate in phase. For $`|g\mu _BB_{3,x}|`$ of order $`\mathrm{\Delta }`$, the rotation of the central spin induced by $`B_{3,x}`$ is too fast for the remaining spins of the chain to follow in phase \[see, e.g., Fig. 3(c) for short times, $`\varphi 1`$\]. The spins of the chain no longer rotate in phase and magnons are excited \[Fig. 4(b)\]. Quantum gate operation probes the spin dynamics in real time and, hence, may provide new insight into the low energy physics of spin chains. That leakage is controlled by the parameter $`|g\mu _BB_{3,x}|/\mathrm{\Delta }`$ can be traced back to the existence of a ground state doublet.

To illustrate this point, we next contrast our results for a system with antiferromagnetic exchange coupling and a ground state doublet with a ferromagnetic chain with exchange coupling $`J<0`$ in Eq. (4). For the ferromagnetic chain, the ground state has degeneracy $`n_c+1`$. A computational basis could be defined also in terms of a subset of the ground state multiplet for $`J<0`$, e.g., by the states $`|S_z=n_c/2`$ and $`|S_z=n_c/2+1`$. Due to the $`n_c+1`$-fold degeneracy of the ground state multiplet, the system is more prone to leakage than the antiferromagnetic systems considered here because quantum mechanical selection rules no longer prevent transitions from the computational basis to other states in the ground state multiplet.

### II.4 XY-like chains

Our considerations have so far been focused on an isotropic exchange coupling which is found, e.g., for coupled quantum dots. burkard:99  However, spin cluster qubits could not only be realized in such artificial superstructures. Rather, a wide variety of spin–$`1/2`$ chains in which magnetic ions are coupled by an exchange interaction has been synthesized. mikeska:91  The control of single ion spins in a molecule or solid in which the ions are rather closely spaced is even more challenging than the control of a single spin in a quantum dot. Defining a qubit in terms of the collective state of a short spin chain will make it substantially simpler to address qubits. However, in contrast to coupled quantum dots, the exchange coupling in many spin chains found in nature is anisotropic. mikeska:91  Hence, we next turn to a discussion of anisotropic chains, $`J_{}J_z`$.

For odd $`n_c`$, the spectrum still exhibits a ground state doublet of $`\widehat{S}_z`$ eigenstates with eigenvalues $`\pm \mathrm{}/2`$, respectively. However, $`\widehat{𝐒}^2`$ is no longer a good quantum number. Both for $`J_{}J_z`$ (XY-like systems) and $`J_{}J_z`$ (Ising-like systems), $`|0`$ and $`|1`$ can be explicitly constructed.

We first consider the XY model with $`J_z=0`$ in Eq. (3). By the Jordan-Wigner transformation, auerbach:94  the XY chain is mapped onto a system of noninteracting spinless fermions on a lattice with spatially varying hopping amplitudes,

$$\widehat{H}=\frac{J_{}}{2}\underset{j=1}{\overset{n_c1}{}}f_j(\widehat{\psi }_{j+1}^{}\widehat{\psi }_j+\widehat{\psi }_j^{}\widehat{\psi }_{j+1}),$$
(28)
where

$$\widehat{\psi }_j=\mathrm{exp}\left[i\pi \underset{k=1}{\overset{j1}{}}\left(\widehat{s}_{k,z}+\frac{1}{2}\right)\right]\widehat{s}_j^{}$$
(29)
annihilates a Jordan-Wigner fermion at site $`j`$. The problem is thus reduced to calculating the one-particle eigenenergies and eigenstates of Eq. (28). The one-particle Hamiltonian has $`(n_c1)/2`$ pairs of states with negative and positive energy $`E_i`$, respectively, which are related to each other by staggering of the wave function,

$$𝐞_i^\pm =(e_{i,1},\pm e_{i,2},e_{i,3},\pm e_{i,5},\mathrm{}),$$
(30)
where $`e_{i,j}`$ are real numbers. In addition, there is one eigenstate

$$𝐞_0(1,0,\frac{f_1}{f_2},0,\frac{f_1f_3}{f_2f_4},0,\mathrm{},\pm \frac{f_1f_3\mathrm{}f_{n_c2}}{f_2f_4\mathrm{}f_{n_c1}})$$
(31)
with energy eigenvalue $`0`$. The ground state doublet of the XY chain corresponds to the lowest $`(n_c1)/2`$ and $`(n_c+1)/2`$ Jordan-Wigner fermion levels filled. Similarly to the spin chain with isotropic exchange interactions, one-qubit gates can be realized by magnetic fields $`B_z(t)`$ and $`B_x(t)`$. By numerical exact diagonalization of small spin chains ($`n_c=9`$), we have shown that $`|1|\widehat{S}_x|0|`$ remains of order $`1/2`$ for various set of $`f_j`$ \[e.g., $`f_j1`$, $`f_j=\mathrm{sin}(j\pi /n_c)`$\], such that the operation time for the one-qubit rotation gate is only limited by $`\mathrm{}/\mathrm{\Delta }`$. An isotropic interqubit coupling $`\widehat{H}_{}=J_{}(t)\widehat{𝐬}_{n_c}^\mathrm{I}\widehat{𝐬}_1^{\mathrm{II}}`$ for two-qubit gates still translates into the effective Hamiltonian in Eq. (11). With Eqs. (30) and (31), from the completeness relation $`_{i=1}^{(n_c1)/2}(e_{i,j}^{+2}+e_{i,j}^2)+e_{0,j}^2=1`$ for $`j=1,\mathrm{},n_c`$ and $`\widehat{s}_{j,z}=\widehat{\psi }_j^{}\psi _j1/2`$, one can calculate all matrix elements entering the effective coupling Hamiltonian Eq. (11),

$`0|\widehat{s}_{n_c,z}|0`$ $`=`$ $`{\displaystyle \frac{e_{0,1}^2}{2}},`$ (32)
$`|1|\widehat{s}_{n_c,x}|0|`$ $`=`$ $`{\displaystyle \frac{e_{0,1}}{2}},`$ (33)
where $`e_{0,1}`$ is the first component of the normed one-particle eigenstate defined in Eq. (31). In particular, for $`f_j1`$, $`0|\widehat{s}_{n_c,z}|0=1/(n_c+1)`$ and $`|1|\widehat{s}_{n_c,x}|0|=1/\sqrt{2(n_c+1)}`$. Due to the anisotropy of the intrachain exchange coupling, $`\widehat{H}_{}`$ (which is isotropic in the single-spin operators) translates into an effective XXZ-Hamiltonian in the two-qubit product basis. Nevertheless, the CNOT gate can still be realized according to Eq. (14). For the anisotropic chain, a magnetic field applied along an axis $`𝐧`$ translates into a rotation around the axis $`(n_x,n_y,n_z/2|1|\widehat{S}_x|0|)`$ in the Hilbert space spanned by $`\{|0,|1\}`$,

$`\widehat{H}^{}`$ $`=`$ $`g\mu _BB𝐧\widehat{𝐒}`$
$``$ $`g\mu _BB2|1|\widehat{S}_x|0|[n_x(|01|+|10|)/2`$
$`+n_yi(|10||01|)/2]`$
$`+g\mu _BBn_z(|00||11|)/2.`$
A one-qubit rotation around an arbitrary axis, e.g. $`𝐧_1`$ in Eq. (14), hence requires appropriate rescaling of the magnetic fields. meier:02

### II.5 Ising-like chains

In the Ising limit $`J_zJ_{}`$ the ground state doublet

$`|0`$ $`=`$ $`|_1|_2\mathrm{}|_{n_c}+𝒪(J_{}/J_z),`$
$`|1`$ $`=`$ $`|_1|_2\mathrm{}|_{n_c}+𝒪(J_{}/J_z)`$ (35)
is separated from the next excited state by an $`n_c`$-independent $`\mathrm{\Delta }J_z\mathrm{min}(f_j)`$. In perturbation theory in $`J_{}/J_z`$, for $`f_j1`$, the matrix elements

$`|1|\widehat{S}_x|0|`$ $``$ $`{\displaystyle \frac{n_c+1}{4}}\left({\displaystyle \frac{2J_{}}{J_z}}\right)^{(n_c1)/2},`$
$`|1|\widehat{s}_{n_c,x}|0|`$ $``$ $`{\displaystyle \frac{1}{2}}\left({\displaystyle \frac{2J_{}}{J_z}}\right)^{(n_c1)/2}`$ (36)
decrease exponentially with system size because $`\widehat{S}_x`$ and $`\widehat{s}_{n_c,x}`$ only flip one spin within the chain. Expanding the states $`|0`$ and $`|1`$ in powers of $`J_{}/J_z`$ it follows that finite matrix element of $`\widehat{s}_{1,x}`$ and $`\widehat{S}_x`$ between $`|0`$ and $`|1`$ occur only in order $`(n_c1)/2`$ in $`J_{}/J_z`$villain:75  Even for medium sized chains $`n_c9`$ and $`J_{}/J_z<0.2`$, an isotropic inter-qubit coupling Hamiltonian $`\widehat{H}_{}`$ translates into an effective Hamiltonian Eq. (11) of Ising form (Fig. 5). Because of the long gate operation times implied by Eq. (36) for the one-qubit rotation and, in particular, the CNOT gate, only quantum computing schemes which require a small number of such operations raussendorf:01  appear feasible.

In Fig. 5, for a chain with $`n_c=9`$, we compare our analytical results (solid lines) for the matrix elements $`|1|\widehat{S}_x|0|`$ and $`|1|\widehat{s}_{1,x}|0|`$ as functions of anisotropy with exact diagonalization for the chain with $`f_j1`$ (symbols). Because matrix elements of order unity imply quantum gate operation times comparable to single spins, the results in Fig. 5 show that universal quantum computing based on a sequence of one-qubit rotation and CNOT gates is feasible for a wide range of spin cluster qubits.

### II.6 Experimental realization

We illustrate the advantages of a spin cluster qubit formed by $`n_c=5`$ spins $`s=1/2`$ in a one-dimensional array of quantum dots with diameter $`d50`$ nm. For realistic parameters burkard:99  ($`J10`$ K$`k_B`$, $`J_{}2.3`$ K$`k_B`$, $`g\mu _BB0.7`$ K$`k_B`$) and a magnetic field which decreases from its maximum values $`B_x`$ at the central site of the chain to $`0.2B_x`$ at sites $`j=2,4`$, the operation time for one-qubit gates increases by a factor $`1/2|1|0.2\widehat{s}_{2,x}+\widehat{s}_{3,x}+0.2\widehat{s}_{4,x}|0|2.2`$ compared to a single spin. The operation time for the square-root of SWAP gate is increased by a factor of $`1/(2|0|\widehat{s}_{1,z}|0|)^24`$ compared to the single-spin qubit. However, the operation time for the CNOT gate as defined in Eq. (14) is mainly determined by the single-qubit operations of the sequence. Hence, for the minimum operation time of the CNOT gate we find $`386`$ ps for spin clusters instead of $`165`$ ps for single spins. The decrease of decoherence time strongly depends on the microscopic origin of decoherence. From the heuristic argument in Sec. II.1 we find that the decoherence rate due to globally fluctuating magnetic fields does not scale with $`n_c`$ and is equal to the one of the single-spin qubit. Decoherence caused by fluctuating local fields scales linearly with $`n_c`$. For a spin cluster qubit with $`n_c=5`$, we estimate that the number of quantum gates which can be performed during the decoherence time decreases by at most a factor of $`10`$ compared to the single-spin qubit. However, in contrast to single-spin qubits, magnetic fields and exchange constants must be controlled only over length scales $`n_cd=250`$ nm and $`2n_cd=500`$ nm, respectively instead of $`d=50`$ nm. This would allow one to control the exchange interaction between neighboring clusters optically. levy:01  Note that, for the small clusters analyzed here, $`\mathrm{\Delta }`$ is so large that neither adiabaticity nor the requirement that the Zeeman energy and $`J_{}`$ be small compared to $`\mathrm{\Delta }`$ provides a serious restriction on quantum gate operation times.

Decoherence due to dipolar interactions is unimportant for electron spins in quantum dots with a typical distance $`d=50100`$ nm, where $`E_{\mathrm{dip}}`$ \[Eq. (21)\] is of order $`10^{11}\mathrm{K}k_B=\mathrm{}/0.25s`$. However, for P dopants in a Si matrix with a typical distance $`d=100`$ Å, $`E_{\mathrm{dip}}=6.2\times 10^7\mathrm{K}k_B=\mathrm{}/12\mu s`$. Recent experiments tyryshkin:03  show that magnetic dipolar interactions are indeed among the most dominant decoherence mechanisms for P dopants in a Si matrix. The characteristic time scale for dephasing by dipolar interactions, $`12\mu s`$, is larger than realistic gate operation times by only a factor $`10^210^3`$koiller:02 ; friesen:02  However, for a spin cluster formed by $`n_c=9`$ spins with a dominant nearest neighbor exchange interaction, the intercluster dipolar interaction energy is reduced compared to the one of single spins by a factor of $`8`$, i.e., the characteristic decoherence time for dipolar interactions increases to $`100\mu s`$.

## III Spin clusters in $`d>2`$

So far, our considerations have been restricted to spin chains. The main ideas discussed above apply to a much larger class of antiferromagnetic systems with uncompensated sublattices. We illustrate next that quantum gates are feasible also if spins $`s=1/2`$ are arranged in a two- or three-dimensional cluster. For definiteness, we restrict our attention to an isotropic exchange interaction $`J>0`$.

### III.1 Bipartite lattice

We first consider an odd number of spins arranged on a bipartite lattice with the number of sublattice sites differing by $`1`$, e.g., a rectangular lattice with $`L_1\times L_2`$ sites, where $`L_{1,2}`$ are odd. This two-dimensional lattice exhibits a ground state doublet lieb:62 . Similarly to the spin chain, the computational basis $`\{|0,|1\}`$ can be defined in terms of the $`\widehat{S}_z`$-eigenstates of the ground state doublet. Here, $`\widehat{𝐒}`$ is the operator of total spin of the two-dimensional array. From a spin-wave ansatz for the elementary excitations, the energy gap $`\mathrm{\Delta }`$ separating the ground state doublet from the next excited state can be estimated as

$$\mathrm{\Delta }\frac{J\pi }{\mathrm{min}(L_1,L_2)}.$$
(37)
Because the characteristic features of the ground state doublet carry over from the one- to the two-dimensional spin cluster qubit, quantum computing with two-dimensional spin arrays on bipartite lattices is possible with the techniques discussed in Sec. II.1. Gate operation times are determined by the matrix elements $`|0|\widehat{s}_{j,z}|0|=|1|\widehat{s}_{j,x}|0|`$. For the $`3\times 3`$-lattice shown in Fig. 6(a), from exact diagonalization we find $`0|\widehat{s}_{j,z}|0=0.15`$ for sites $`j`$ in the center of the edges, $`0|\widehat{s}_{j,z}|0=0.23`$ for sites $`j`$ at the corners, and $`0|\widehat{s}_{j,z}|0=0.17`$ for the central site of the cluster. Similarly to the spin chain, the ground state doublet is robust against a spatial variation in the exchange constants as long as all exchange constants remain antiferromagnetic.

### III.2 Geometrically frustrated systems

For non-bipartite lattices, a ground-state doublet is not guaranteed to emerge. The simplest example is the geometrically frustrated system of three spins $`s=1/2`$ shown in Fig. 6(b),

$`\widehat{H}`$ $`=`$ $`J(\widehat{𝐬}_1\widehat{𝐬}_2+\widehat{𝐬}_1\widehat{𝐬}_3+\widehat{𝐬}_2\widehat{𝐬}_3)`$ (38)
$`=`$ $`{\displaystyle \frac{J}{2}}\left(\widehat{𝐒}^2{\displaystyle \frac{9}{4}}\right),`$
which has a fourfold degenerate ground state with energy eigenvalue $`E=0.75J`$. The eigenstates can be chosen as

$`|0`$ $`=`$ $`(||)/\sqrt{2},`$
$`|1`$ $`=`$ $`(||)/\sqrt{2},`$
$`|2`$ $`=`$ $`(2|||)/\sqrt{6},`$ (39)
$`|3`$ $`=`$ $`(2|||)/\sqrt{6}.`$
As demonstrated in Ref. kempe:01, , these states could still define a logical qubit robust against certain sources of decoherence. However, quantum gate operation would always require control over single exchange interactions or local magnetic fields and exclude quantum computing with control parameters which vary slowly in space.

Geometrical frustration does, however, not in general rule out the existence of a ground state doublet. In the more generic case that geometrically frustrated bonds are part of a larger system \[Fig. 6(c)\] or the exchange constants in Fig. 6(b) are not all equal, a ground state doublet emerges. In this case, the logical states of the spin cluster qubit again can be defined in terms of the $`\widehat{S}_z`$ eigenstates of the ground state doublet and quantum gate operation is possible with magnetic fields and exchange constants varying slowly over the cluster. For systems as shown in Fig. 6(c), in which some bonds are frustrated, $`\mathrm{\Delta }`$ is usually smaller than in the case of bipartite lattices. For example, for Fig. 6(c), $`\mathrm{\Delta }=0.157J`$ compared to $`\mathrm{\Delta }=0.991J`$ for Fig. 6(a). According to the adiabaticity requirement, the small gap limits gate operation times more severely for the system in Fig. 6(c).

### III.3 Experimental realization

Because spin cluster qubits emerge also in two-dimensional regular spin arrays, spin cluster qubits can be arranged in a plane if the positions of single spins can be controlled as, e.g., for lateral quantum dots \[Fig. 6(a)\]. For a spin cluster qubit formed by $`L\times L=n_c`$ quantum dots, $`\mathrm{\Delta }1/L`$. Decoherence due to globally fluctuating fields does not increase with $`n_c`$, whereas independent local Gaussian white noise gives rise to a decoherence rate $`1/\tau _\varphi n_c`$. Two-dimensional spin cluster qubits are hence particularly interesting for qubits in which decoherence is induced mainly by global rather than local fluctuating fields.

More importantly, a spin cluster qubit can be defined even for a wide range of systems in which the positions and exchange constants cannot be accurately controlled. For P atom electron spins in a Si matrix, because of rapid oscillations of the exchange coupling between atoms at large distances, placement of atoms with lattice spacing precision is required for single-spin qubits. koiller:02  Without this precision, the exchange interaction at large distances vanishes with a probability of $`50`$%. In contrast, for spin cluster qubits formed by a small number (e.g. three) of P dopants located close to each other, the spin defining the logical state of the qubit is delocalized over the cluster. The effective exchange coupling between neighboring qubits obtained by integration of the exchange interaction over the clusters is finite with a high probability. Because the intracluster exchange interaction at small distances varies strongly with distance, koiller:02  for a random arrangement of three spins, the exchange couplings will differ with high probability and the system is not frustrated.

## IV Larger spins

So far, our considerations have been restricted to clusters formed by spins $`s=1/2`$. We next consider antiferromagnetic systems with larger spins $`s>1/2`$.

### IV.1 Antiferromagnetic molecular clusters

Only very recently it has been shown theoretically that Grover’s algorithm can be implemented with ferromagnetic molecular magnets using a unary encoding. leuenberger:01 ; leuenberger:02  In view of universal quantum computing, ferromagnetic clusters such as the molecular magnets Mn<sub>12</sub> and Fe<sub>8</sub> (Ref. gatteschi:94, ) suffer from the large net spin which usually means large matrix elements coupling the spin to the environment and, hence, short decoherence times.

In contrast, in antiferromagnetic systems, such as various ring compounds, gatteschi:94  the spins couple such that they form a small total magnetic moment. Antiferromagnetic clusters which have unequal sublattice magnetization, will in general have a ground state multiplet rather than the singlet found for systems with compensated sublattice spins. meier:01  Several antiferromagnetic molecular magnets comprised of spins with quantum numbers larger than $`1/2`$ have been synthesized to date taft:94 ; caneschi:96 ; waldmann:99 ; waldmann:01 ; slageren:02  including several compounds with uncompensated sublattice spins. larsen:03  As a paradigm, we consider systems with isotropic exchange interaction $`J`$, but allow for an easy or hard axis single-spin anisotropy,

$$\widehat{H}=J\widehat{𝐬}_1\widehat{𝐬}_2+k_z(\widehat{s}_{1,z}^2+\widehat{s}_{2,z}^2).$$
(40)
Here, $`s_1`$ and $`s_2=s_1\pm 1/2`$ are the spin quantum numbers of the two sublattices, respectively, $`J>0`$ is an effective exchange constant, and $`k_z`$ the single ion anisotropy. Equation (40) has a ground state doublet $`\{|0,|1\}`$ of $`\widehat{S}_z=\widehat{s}_{1,z}+\widehat{s}_{2,z}`$ eigenstates with eigenvalues $`\pm \mathrm{}/2`$, respectively. Because $`[\widehat{S}_z,\widehat{H}]=0`$ for the Hamiltonian Eq. (40), the logical qubit basis states have an expansion of the form (for $`s_2=s_11/2`$)

$`|0`$ $`=`$ $`{\displaystyle \underset{m_1=s_1+1}{\overset{s_1}{}}}\alpha _{m_1}|m_1,1/2m_1`$
$`=`$ $`\alpha _{s_1+1}|s_1+1,s_11/2`$
$`+\alpha _{s_1+2}|s_1+2,s_13/2+\mathrm{}`$
$`+\alpha _{s_1}|s_1,s_1+1/2`$
in terms of the spin product basis. For $`s_{1,2}1`$, analytical expressions can be derived both for the action of a magnetic field (one-qubit rotation gate) and for the action of an interqubit coupling Hamiltonian (two-qubit gates) between clusters I and II,

$$\widehat{H}_{}=J_{}(t)\widehat{𝐬}_2^\mathrm{I}\widehat{𝐬}_1^{\mathrm{II}},$$
(42)
within a coherent state path integral formalism. klauder:79 ; auerbach:94  We only state the main results of our calculations here. Further details are given in Appendix C.

### IV.2 Hard axis systems

For strong hard axis anisotropy, $`k_z>0`$ and $`k_zs_{1,2}^2/J1`$, the spins $`𝐬_1`$ and $`𝐬_2`$ lie close to the $`x`$-$`y`$ plane for both states of the ground state doublet. A large contribution in the expansion Eq. (IV.1) comes from the states $`|m_1=0|m_2=1/2`$ and $`|m_1=0|m_2=1/2`$, respectively. For illustration, for $`s_1=3`$, $`s_2=5/2`$, and $`k_z/J=0.2`$, by numerical diagonalization of Eq. (40), we find

$`|0`$ $`=`$ $`0.25|3,{\displaystyle \frac{5}{2}}0.41|2,{\displaystyle \frac{3}{2}}`$
$`+0.52|1,{\displaystyle \frac{1}{2}}0.52|0,{\displaystyle \frac{1}{2}}`$
$`+0.42|1,{\displaystyle \frac{3}{2}}0.24|2,{\displaystyle \frac{5}{2}}.`$
The state $`|1`$ is obtained by $`|m_1,m_2|m_1,m_2`$ on the right hand side of Eq. (IV.2). In agreement with the semiclassical theory, a major contribution to $`\{|0,|1\}`$ comes from states with small $`m_1`$ and $`m_2`$.

In the following, we restrict our attention to systems with large anisotropy, $`k_z(s_1^2+s_2^2)/J1`$. Then, $`\mathrm{\Delta }J`$ (Appendix C) and

$`|1|\widehat{S}_x|0|`$ $`=`$ $`1/4,`$
$`|1|\widehat{s}_{1,x}|0|`$ $`=`$ $`s_1/2,`$ (44)
$`|1|\widehat{s}_{2,x}|0|`$ $`=`$ $`s_2/2.`$
In particular, Eq. (42) translates into the effective Hamiltonian

$`\widehat{H}_{}`$ $`=`$ $`J_{}|0|\widehat{s}_{1,z}|0||0|\widehat{s}_{2,z}|0|\left(\begin{array}{cccc}1& 0& 0& 0\\ 0& 1& 0& 0\\ 0& 0& 1& 0\\ 0& 0& 0& 1\end{array}\right)`$ (54)
$`+{\displaystyle \frac{J_{}s_1s_2}{2}}\left(\begin{array}{cccc}0& 0& 0& 0\\ 0& 0& 1& 0\\ 0& 1& 0& 0\\ 0& 0& 0& 0\end{array}\right)`$
in the two-qubit product basis. As discussed in Sec. II.1, the CNOT gate can be realized with a unitary time evolution governed by this effective qubit coupling of the XXZ-form.

Matrix elements of order unity in Eq. (44) show that, e.g., a magnetic field $`B_x`$ efficiently rotates the state $`|0`$ into $`|1`$. This is not a priori evident given the rather complicated representation of the ground state doublet in the single-spin product basis \[Eq. (IV.1)\]. The large matrix elements arise because, for both $`|0`$ and $`|1`$, the spins lie close to the $`x`$-$`y`$ plane in the hard axis system.

### IV.3 Easy axis systems

For $`k_z<0`$, configurations with spins aligned along the z-axis are energetically favorable. We restrict our attention to systems with large anisotropy, $`4|k_z|(s_1^2+s_2^2)/J1`$. Because a transition from $`|0`$ to $`|1`$ requires a rotation of both spins through a large energy barrier, from the theory of spin quantum tunneling in antiferromagnetic systems barbara:90 ; krive:90  we find that $`|1|\widehat{S}_x|0|,|1|\widehat{s}_{1,x}|0|,|1|\widehat{s}_{2,x}|0|\mathrm{exp}(\sqrt{8|k_z|(s_1^2+s_2^2)/J})1`$ are exponentially small. Similarly to a spin chain in the Ising limit \[Sec. II.5\], the easy axis system is a candidate for quantum computing schemes as suggested in Ref. raussendorf:01, .

The analytical results for the matrix elements discussed here are compared with numerical exact diagonalization for $`s_1=7`$ in Fig. 7. We find good agreement with our semiclassical results.

### IV.4 Experimental realization

Single molecule electrical switches ball:00 ; collier:99 ; gittins:00 ; joachim:00  have nourished hopes that, in the future, it will be possible to down-scale computers to the level at which bits or qubits are represented by single molecules. The results in Secs. IV.2 and IV.3 show that, in such bottom-up approaches aiming at a universal quantum computer, control is not required at the level of single atom spins but only on the scale of molecule spins. In particular, molecular magnetic clusters with an effective spin $`S=1/2`$ define a qubit. One-qubit quantum gates could be effected, for example, by a magnetic tip as used in magnetic force microscopy. rugar:90  The spatial resolution of these techniques currently lies in the range of $`10100`$ nm (Ref. liu:02, ) and approaches the typical size of molecular magnetic clusters. gatteschi:94

Control of the exchange interaction between molecules is challenging. As has been demonstrated recently, collier:99 ; gittins:00  the electrical conductivity of individual molecules can be switched between two states in a controlled way. By connecting molecular magnetic clusters by reversible redox switches one could also switch intercluster exchange paths. Alternatively, if the relative position of molecular magnetic clusters can be controlled, the intercluster exchange interaction can be switched on and off via the overlap of electron orbital wave functions by moving clusters relative to each other.

## V Conclusion

In conclusion, we have shown that quantum computing is possible with a wide variety of clusters assembled from antiferromagnetically coupled spins which form an effective total spin $`S=1/2`$. For arrays of spins $`s=1/2`$, the existence of a spin cluster qubit requires little control over the placement and intracluster coupling of the spins and the spatial dimension of the array. This remains true for a wide range of systems with uncompensated sublattice spins differing by $`1/2`$. We have shown explicitly that, for the spin cluster qubit, initialization, quantum gate operation, and readout are possible with the techniques proposed and analyzed for single spins. The scaling of the decoherence time with system size strongly depends on the microscopic decoherence mechanism. Spin cluster qubits are particularly promising in situations where decoherence is induced mainly by globally fluctuating fields during quantum gate operation and the decoherence rate of the spin cluster qubit is comparable to that of a single-spin qubit or for systems in which magnetic dipolar interactions are the dominant decoherence mechanism. The main advantage of spin clusters compared to single spins is that requirements on local control of magnetic fields and exchange interactions can be traded for longer gate operation times. We have illustrated the feasibility and advantages of spin cluster qubits for arrays of quantum dots, P dopants in a Si matrix, and molecular magnetic clusters.

In contrast to single spins, spin clusters are not intrinsically two-state systems and leakage during quantum gate operation must be accounted for. For the one-qubit rotation gate, we have shown that leakage is small if the magnetic field which induces the rotation is switched on and off adiabatically or if the Zeeman energy remains small compared to $`\mathrm{\Delta }`$.

Finally, we note that, because any qubit can be mapped onto a spin $`s=1/2`$, the results of this work do not only apply to quantum computing proposals based on spin degrees of freedom but to any quantum computing scheme. More specifically, for any qubit for which methods for initialization, quantum gate operation, quantum error correction, and readout have been identified, a cluster qubit can be formed by coupling several qubits. For the cluster qubit, initialization, quantum gate operation, quantum error correction, and readout are possible using the same techniques as for the original qubit.

###### Acknowledgements.

This work was financially supported by the EU TMR network MOLNANOMAG, no. HPRN-CT-1999-00012 (FM and DL), DARPA SPINS and QuIST (JL and DL), the Swiss NCCR Nanoscience (DL), and the Swiss NSF (DL). We acknowledge discussions with G. Burkard, V. Cerletti, W. Coish, H. Gassmann, F. Marquardt, and P. Recher.
## Appendix A Effective exchange Hamiltonian

Here, we derive explicitly the effective coupling Hamiltonian in Eq. (11) from Eq. (10). The first and second term in Eq. (11) result from $`J_{}(t)\widehat{𝐬}_{n_c}^\mathrm{I}\widehat{𝐬}_1^{\mathrm{II}}`$ in the microscopic coupling. Decomposing $`\widehat{𝐬}_{n_c}^\mathrm{I}\widehat{𝐬}_1^{\mathrm{II}}=\widehat{s}_{n_c,z}^\mathrm{I}\widehat{s}_{1,z}^{\mathrm{II}}+(\widehat{s}_{n_c}^{\mathrm{I}+}\widehat{s}_1^{\mathrm{II}}+\widehat{s}_{n_c}^\mathrm{I}\widehat{s}_1^{\mathrm{II}+})/2`$ in terms of spin ladder operators, one can readily evaluate the matrix elements in the two-qubit product basis. Because, by definition, $`\widehat{S}_z|0=(\mathrm{}/2)|0`$ and $`\widehat{S}_z|1=(\mathrm{}/2)|1`$ and $`\widehat{s}_{n_c,z}^\mathrm{I}\widehat{s}_{1,z}^{\mathrm{II}}`$ conserves the $`z`$-component of total spin in each cluster separately it follows that

$${}_{\mathrm{I}}{}^{}0|_{\mathrm{II}}1|\widehat{s}_{n_c,z}^\mathrm{I}\widehat{s}_{1,z}^{\mathrm{II}}|1_\mathrm{I}|0_{\mathrm{II}}^{}=0.$$
(55)
Similarly, all other off-diagonal elements of $`\widehat{s}_{n_c,z}^\mathrm{I}\widehat{s}_{1,z}^{\mathrm{II}}`$ vanish. Because of

$${}_{\mathrm{I}}{}^{}0|\widehat{s}_{n_c}^{\mathrm{I}\pm }|0_{\mathrm{I}}^{}=_\mathrm{I}1|\widehat{s}_{n_c}^{\mathrm{I}\pm }|1_\mathrm{I}=0,$$
(56)
the transverse exchange interaction $`J_{}(t)(\widehat{s}_{n_c}^{\mathrm{I}+}\widehat{s}_1^{\mathrm{II}}+\widehat{s}_{n_c}^\mathrm{I}\widehat{s}_1^{\mathrm{II}+})/2`$ has finite matrix elements only between the states $`|0_\mathrm{I}|1_{\mathrm{II}}`$ and $`|1_\mathrm{I}|0_{\mathrm{II}}`$. This completes the proof that the intercluster exchange term $`J_{}(t)\widehat{𝐬}_{n_c}^\mathrm{I}\widehat{𝐬}_1^{\mathrm{II}}`$ leads to the first and second term in Eq. (11).

It remains to show that a possible change in intracluster exchange interaction constants during two-qubit gate operation, $`J_{}(t)_{j=1}^{n_c1}(v_j^\mathrm{I}\widehat{𝐬}_j^\mathrm{I}\widehat{𝐬}_{j+1}^\mathrm{I}+v_j^{\mathrm{II}}\widehat{𝐬}_j^{\mathrm{II}}\widehat{𝐬}_{j+1}^{\mathrm{II}})`$, only leads to a term proportional to $`\mathrm{𝟏}`$ in Eq. (11). This term conserves all components of the total spin of clusters I and II,

$$[\widehat{S}_\alpha ^\mathrm{I},\underset{j=1}{\overset{n_c1}{}}v_j^\mathrm{I}\widehat{𝐬}_j^\mathrm{I}\widehat{𝐬}_{j+1}^\mathrm{I}]=0,$$
(57)
for $`\alpha =x,y,z`$, and similarly for II. Hence, all off-diagonal matrix elements such as $`{}_{\mathrm{I}}{}^{}1|v_j^\mathrm{I}\widehat{𝐬}_j^\mathrm{I}\widehat{𝐬}_{j+1}^\mathrm{I}|0_{\mathrm{I}}^{}`$ vanish. Finally, because $`|1_\mathrm{I}=\widehat{S}^\mathrm{I}|0_\mathrm{I}=2\widehat{S}_x^\mathrm{I}|0_\mathrm{I}`$, with Eq. (57),

$`{}_{\mathrm{I}}{}^{}1|_{\mathrm{II}}0|J_{}(t){\displaystyle \underset{j=1}{\overset{n_c1}{}}}v_j^\mathrm{I}\widehat{𝐬}_j^\mathrm{I}\widehat{𝐬}_{j+1}^\mathrm{I}|1_\mathrm{I}|0_{\mathrm{II}}^{}`$
$`=_\mathrm{I}0|_{\mathrm{II}}0|2\widehat{S}_x^\mathrm{I}J_{}(t){\displaystyle \underset{j=1}{\overset{n_c1}{}}}v_j^\mathrm{I}\widehat{𝐬}_j^\mathrm{I}\widehat{𝐬}_{j+1}^\mathrm{I}2\widehat{S}_x^\mathrm{I}|0_\mathrm{I}|0_{\mathrm{II}}`$ (58)
$`=_\mathrm{I}0|_{\mathrm{II}}0|J_{}(t){\displaystyle \underset{j=1}{\overset{n_c1}{}}}v_j^\mathrm{I}\widehat{𝐬}_j^\mathrm{I}\widehat{𝐬}_{j+1}^\mathrm{I}(2\widehat{S}_x^\mathrm{I})^2|0_\mathrm{I}|0_{\mathrm{II}}`$
$`=_\mathrm{I}0|_{\mathrm{II}}0|J_{}(t){\displaystyle \underset{j=1}{\overset{n_c1}{}}}v_j^\mathrm{I}\widehat{𝐬}_j^\mathrm{I}\widehat{𝐬}_{j+1}^\mathrm{I}|0_\mathrm{I}|0_{\mathrm{II}}.`$
In the second line of Eq. (58) we have invoked that $`\{|0_\mathrm{I},|1_\mathrm{I}\}`$ belong to one spin-$`1/2`$ doublet, the third line then follows from Eq. (57). With a similar argument it can be shown that all diagonal matrix elements in the two-qubit product basis are equal and $`J_{}(t)_{j=1}^{n_c1}(v_j^\mathrm{I}\widehat{𝐬}_j^\mathrm{I}\widehat{𝐬}_{j+1}^\mathrm{I}+v_j^{\mathrm{II}}\widehat{𝐬}_j^{\mathrm{II}}\widehat{𝐬}_{j+1}^{\mathrm{II}})`$ translates into a term $`J_o(t)\mathrm{𝟏}`$ in the effective coupling Hamiltonian Eq. (11).

Finally, we prove Eq. (13) which implies that, for isotropic intracluster exchange interactions, the effective two-qubit Hamiltonian is also of Heisenberg form. For simplicity, we omit the label I of the spin cluster qubit in the following. In order to formally calculate $`0|\widehat{s}_{n_c,z}|0`$ and $`|1|\widehat{s}_{n_c,x}|0|`$, we define the spin operators

$$\widehat{S}_\alpha ^{}=\widehat{S}\widehat{s}_{n_c,\alpha }=\underset{j=1}{\overset{n_c1}{}}\widehat{s}_{j,\alpha }$$
(59)
of all but the outermost spin $`j=n_c`$ of the cluster. Generally, $`|0`$ can be expanded as

$$|0=a|\mathrm{\Psi }|+b|\mathrm{\Phi }|,$$
(60)
where $`|\mathrm{\Psi }`$ and $`|\mathrm{\Phi }`$ describe the normed states of the leftmost $`n_c1`$ spins in the array and $`a`$ and $`b`$ are real numbers. Because $`\widehat{S}_z|0=(\mathrm{}/2)|0`$, $`|\mathrm{\Psi }`$ and $`|\mathrm{\Phi }`$ are eigenstates of $`\widehat{S}_z^{}`$ with eigenvalues $`0`$ and $`\mathrm{}`$, respectively. $`\widehat{S}_x|0=(\mathrm{}/2)|1`$ is an $`\widehat{S}_z`$ eigenstate with eigenvalue $`(\mathrm{}/2)`$, such that $`b|\mathrm{\Phi }=a\widehat{S}_+^{}|\mathrm{\Psi }`$, and

$`|0`$ $`=`$ $`a(|\mathrm{\Psi }|\widehat{S}_+^{}|\mathrm{\Psi }|),`$
$`|1`$ $`=`$ $`a(\widehat{S}_{}^{}|\mathrm{\Psi }|(1\widehat{S}_{}^{}\widehat{S}_+^{})|\mathrm{\Psi }|),`$
$`a`$ $`=`$ $`{\displaystyle \frac{1}{\sqrt{1+\mathrm{\Psi }|\widehat{S}_{}^{}\widehat{S}_+^{}|\mathrm{\Psi }}}}.`$ (61)
From Eq. (61) we calculate

$`0|\widehat{s}_{n_c,z}|0=1|\widehat{s}_{n_c,z}|1={\displaystyle \frac{1}{2}}{\displaystyle \frac{1\mathrm{\Psi }|\widehat{S}_{}^{}\widehat{S}_+^{}|\mathrm{\Psi }}{1+\mathrm{\Psi }|\widehat{S}_{}^{}\widehat{S}_+^{}|\mathrm{\Psi }}},`$
$`1|\widehat{s}_{n_c,x}|0={\displaystyle \frac{1}{2}}{\displaystyle \frac{1\mathrm{\Psi }|\widehat{S}_{}^{}\widehat{S}_+^{}|\mathrm{\Psi }}{1+\mathrm{\Psi }|\widehat{S}_{}^{}\widehat{S}_+^{}|\mathrm{\Psi }}},`$ (62)
which proves Eq. (13).

## Appendix B Isotropic chain with spatially varying exchange interaction

The local spin density in the energy eigenstates of Eq. (3) depends sensitively on spatial variations of the exchange interaction \[Fig. 2(d)\]. Whereas for $`f_j1`$ (solid lines) the magnetization density in each of the sublattices increases toward the center of the chain, eggert:92  the opposite behavior is observed for an exchange interaction $`f_j=\mathrm{sin}(j\pi /n_c)`$ (dashed lines). In the limit $`f_1=f_{n_c1}\mathrm{min}_{j=2,\mathrm{},n_c2}f_j`$, the increase of local spin density toward the ends of the chain can be understood quantitatively. The ground state doublet of the spin cluster qubit can be constructed explicitly from the ground state doublet $`\{|0_{n_c2},|1_{n_c2}\}`$ of the chain with the outermost spins removed. For $`Jf_1`$ much smaller than the energy gap $`\mathrm{\Delta }_{n_c2}`$ of the chain formed by the $`n_c2`$ central spins, the coupling of the outermost spins can be treated perturbatively. For the chain with centrosymmetric exchange couplings, $`f_j=f_{n_cj}`$, from the ansatz

$`|0`$ $`=`$ $`\alpha _1||1_{n_c2}|+\alpha _2||0_{n_c2}|`$ (63)
$`+\alpha _3||0_{n_c2}|+𝒪(Jf_1/\mathrm{\Delta }_{n_c2}),`$
we find $`(\alpha _1,\alpha _2,\alpha _3)=(2,1,1)/\sqrt{6}`$ for the ground state of the chain with $`n_c`$ spins and, hence,

$$\underset{f_1=f_{n_c1}0}{lim}|0|\widehat{s}_{1,z}|0|=1/3.$$
(64)
## Appendix C Large spins

The matrix elements in Eq. (44) can be calculated from coherent state spin path integrals. klauder:79  We focus on strong easy plane systems, $`k_z>0`$ and $`k_z(s_1^2+s_2^2)/J1`$. Following the standard approach for antiferromagnetic systems, the partition function of the two-spin system is expressed as path integral over the Néel vector $`𝐧`$ and homogeneous magnetization $`𝐥`$ defined by $`𝐬_1=s_1𝐧+𝐥`$ and $`𝐬_2=s_2𝐧+𝐥`$, where $`𝐧𝐥=0`$. Integrating out $`𝐥`$ in a saddle point approximation and parametrizing

$$𝐧=\left(\begin{array}{c}\mathrm{sin}\theta \mathrm{cos}\varphi \\ \mathrm{sin}\theta \mathrm{sin}\varphi \\ \mathrm{cos}\theta \end{array}\right),$$
(65)
the Euclidean action of the system can be written as barbara:90 ; krive:90

$`L_E={\displaystyle \frac{\mathrm{}^2}{2J}}\left(\dot{\theta }^2+\mathrm{sin}^2\theta \dot{\varphi }^2\right)+k_z(s_1^2+s_2^2)\mathrm{cos}^2\theta `$
$`+i\mathrm{\Delta }s\mathrm{}\dot{\varphi }(1\mathrm{cos}\theta ),`$ (66)
where the last factor accounts for the difference $`\mathrm{\Delta }s=s_2s_1`$ of the spin quantum numbers and $`\dot{\varphi }=_\tau \varphi `$ is the imaginary time derivative. In the limit of strong anisotropy, $`k_z(s_1^2+s_2^2)/J1`$, Eq. (66) can be expanded to second order in $`\theta \pi /2`$ and the fluctuations are integrated out, leading to

$$Z=𝒟\varphi \mathrm{exp}\left(_0^\mathrm{}\beta 𝑑\tau L_E[\varphi ]/\mathrm{}\right)$$
(67)
with an effective Euclidean Lagrangean

$$L_E[\varphi ]=\frac{\mathrm{}^2\dot{\varphi }^2}{2J}+i\mathrm{\Delta }s\mathrm{}\dot{\varphi }.$$
(68)
After continuation to real time, by a canonical transformation we obtain the Hamiltonian of the system in terms of the Néel vector operator,

$$\widehat{H}=\frac{J}{2\mathrm{}^2}\left(\widehat{p}_\varphi \mathrm{}\mathrm{\Delta }s\right)^2,$$
(69)
where

$$\widehat{𝐧}=\left(\begin{array}{c}\mathrm{cos}\widehat{\varphi }\\ \mathrm{sin}\widehat{\varphi }\\ 0\end{array}\right),\widehat{𝐥}=\frac{1}{2}\left(\begin{array}{c}0\\ 0\\ \widehat{p}_\varphi /\mathrm{}\mathrm{\Delta }s\end{array}\right),$$
(70)
and $`\widehat{p}_\varphi `$ is the momentum operator conjugate to the in-plane polar angle $`\varphi `$, $`[\widehat{p}_\varphi ,\widehat{\varphi }]=i\mathrm{}`$. By inspection of Eq. (69), we find that the spin system Eq. (40) has been mapped onto the Hamiltonian of a particle on a ring threaded by a magnetic flux $`\mathrm{\Delta }s`$. In particular, for half-integer $`\mathrm{\Delta }s`$, the Hamiltonian has a ground state doublet $`\{|0,|1\}`$ with wave functions $`\psi _0(\varphi )=\mathrm{exp}(i(m+1)\varphi )/\sqrt{2\pi }`$ and $`\psi _1(\varphi )=\mathrm{exp}(im\varphi )/\sqrt{2\pi }`$, where $`m=\mathrm{\Delta }s`$. From $`\widehat{s}_{1,x}s_1\mathrm{cos}\widehat{\varphi }`$ and $`\widehat{s}_{2,x}s_2\mathrm{cos}\widehat{\varphi }`$, one immediately obtains Eq. (44).