# Antiferromagnetism in a doped spin-Peierls model: classical and quantum behaviors

## 1 Introduction

The spin-Peierls transition at $`T_{\mathrm{SP}}14`$ K in the inorganic quasi one dimensional spin-Peierls compound CuGeO<sub>3</sub> has attracted much interest . This transition is characterized by the appearance of a finite dimerization in the CuO<sub>2</sub> chains, and the opening of a spin gap. With CuGeO<sub>3</sub>, it became possible to experiment the effect of doping in a spin-Peierls system. An antiferromagnetic (AF) phase was discovered upon replacing a fraction of the Cu ions (with $`S=1/2`$) by magnetic ions with a different spin: Ni  (with $`S=1`$) or Co  (with $`S=3/2`$), or non magnetic ions: Zn  or Mg . Also, the Ge sites (outside the CuO<sub>2</sub> chains) can be substituted with Si , leading to antiferromagnetism at low temperature.

Recent experiments by Manabe et al. have shown the existence of a finite Néel temperature $`25`$ mK, with a doping concentration as low as $`0.12`$ $`\%`$ . The doping dependence of the Néel temperature obtained in these experiments suggests the absence of a critical concentration for the appearance of antiferromagnetism: at low doping the ordering temperature scales like $`\mathrm{ln}T_N1/x`$ .

Early theoretical works  have focussed on the identification of the relevant low energy degrees of freedom. Fukuyama, Tanimoto and Saito  have shown the coexistence between antiferromagnetism and dimerization in a doped spin-Peierls model. The degrees of freedom relevant to the low energy physics are solitonic spin-$`1/2`$ excitations pinned at the impurities . These excitations are the building blocks of the theory in Refs. . These spin-1/2 objects interact via an exchange decaying exponentially with distance. Interchain interactions can be incorporated by considering the existence of a transverse correlation length, approximately one tenth of the longitudinal correlation length, as recently proposed independently by Dobry et al. , and Fabrizio, Mélin and Souletie . Numerical calculations with realistic spin-phonon couplings have provided a link between the microscopic Hamiltonian and the effective model of interacting spin-$`1/2`$ moments . The approach followed in Refs.  and continued in the present work relies on the treatment of disorder in the effective Hamiltonian. This allows to discuss the qualitative physics of large scale systems at a finite temperature, while the numerical methods have so far been limited to the ground state properties . The scope of this article is to analyze the model beyond the percolation approximation used in Ref. , both at the classical and quantum levels. We first show in section 3 that the physics of the quantum Hamiltonian is already present in the classical Ising Hamiltonian, and give a rigorous derivation of mean field theory via a Bethe-Peierls treatment. The second purpose of the article is to show that the quantum Hamiltonian has an antiferromagnetic behavior at low temperature. The quantum model is treated in a cluster renormalization group (RG) calculation in sections 4 and 5.

## 2 The model

We recall the model proposed in Ref. . When impurities are introduced in a dimerized background (for instance non magnetic impurities such as Zn), spin-1/2 solitonic moments are released out of the dimerized pattern. These magnetic moments are pinned at the impurities due to interchain interactions . This picture is in agreement with susceptibility experiments , indicating the release of one spin-$`1/2`$ moment per Zn impurity at low doping. The interaction between two magnetic moments at a distance $`d`$ originates from virtual excitations of the gaped dimerized background, and decays exponentially with distance, with a characteristic length set by the correlation lengths $`\xi _x9`$ c along the chain direction (c-axis) , and $`\xi _y\xi _x/10`$ in the b-axis direction. These exchange interactions as well as the relevance of disorder were identified in Ref.  to play a crucial role in the establishment of antiferromagnetism. The low energy physics of a doped spin-Peierls system is represented by spin-$`1/2`$ solitonic magnetic moments distributed at random with a concentration $`x`$ on a square lattice, and interacting via a Heisenberg Hamiltonian 

$$H=\underset{i,j}{}J_{ij}𝐒_i.𝐒_j,$$
(1)   
the exchange in Eq. 1 being staggered and decaying exponentially with distance:

$$J_{ij}=(1)^{d_x+d_y+1}\mathrm{\Delta }\mathrm{exp}\left(\sqrt{\left(\frac{d_x}{\xi _x}\right)^2+\left(\frac{d_y}{\xi _y}\right)^2}\right),$$
(2)   
with $`\xi _x9`$ c the correlation length along the c-axis and $`\xi _y0.1\times \xi _x`$ the correlation length along the b-axis. Correlations along the a-axis are neglected.

## 3 Classical Ising model

We consider a model with Ising degrees of freedom, distributed randomly and interacting via the exchange in Eq. 2. The classical antiferromagnet has the same transition temperature as the classical ferromagnet. We consider therefore the ferromagnetic model to calculate the ordering temperature.

### 3.1 One dimensional model

A high temperature expansion leads to the exact form of the correlations in terms of a product over the bonds between the spins at sites $`0`$ and $`L`$: $`\sigma _0\sigma _L=\mathrm{tanh}(\beta J_{i,i+1}).`$ We calculated numerically the disorder average to obtain the correlation length at a finite temperature. As shown on Fig. 1, the average correlation length of the disordered model is larger than the typical correlation length $`\xi =1/[x\mathrm{ln}(\mathrm{tanh}(\beta T^{}))]`$, with $`T^{}=\mathrm{\Delta }\mathrm{exp}(1/(x\xi ))`$ the exchange of the particular disorder realization where the magnetic moments are equally spaced. We calculated in Ref.  the correlation length of the quantum chain and found a similar result: the enhancement of the magnetic correlations above $`T^{}`$ due to disorder does not rely on the quantum nature of the coupling Hamiltonian in spite of a random singlet physics in the quantum chain, not present in the Ising chain.

### 3.2 Determination of the exchange distribution

We consider the exchanges to be drawn independently in a distribution $`P(J)`$ resulting from the combination of randomness in the spatial distribution of the magnetic moments and exponentially decaying interactions, Eq. 2. The relevant exchanges are set by the spins the closest to each other. Therefore, given a spin at site $`(x_0,y_0)`$, we need to determine the probability that one spin is found on the periphery of the ellipse $`[(xx_0)/\xi _x]^2+[(yy_0)/\xi _y]^2=\gamma ^2`$, with no other spin inside the ellipse, and therefore an exchange $`\mathrm{\Delta }\mathrm{exp}(\gamma )`$. We consider a system of total area $`A`$ containing $`n`$ spins. The probability to find no spin inside a subsystem of area $`\delta A`$ is $`P_0=\left(1\frac{\delta A}{A}\right)^n\mathrm{exp}(x\delta A)`$, with $`x=n/A`$ the doping concentration. Now the spacing distribution is

$$P(\gamma )=xL(\gamma )\mathrm{exp}(x\delta A(\gamma )),$$
(3)   
with $`L(\gamma )=d[A(\gamma )]/d\gamma `$. In the one dimensional model, we have $`\delta A(\gamma )=2\gamma \xi _x`$, and $`L(\gamma )=2\xi _x`$. In the two dimensional isotropic model with $`\xi _x=\xi _y=\xi `$, we have $`\delta A(\gamma )=\pi \gamma ^2\xi ^2`$, and $`L(\gamma )=2\pi \gamma \xi `$. In the quasi one dimensional model, $`\delta A(\gamma )=\pi \gamma ^2\xi _x\xi _y`$, and $`L(\gamma )=2\pi \gamma \xi _x\xi _y`$. The distribution $`P(\gamma )`$ of the isotropic and anisotropic two dimensional models is a Wigner distribution with a short scale “distance repulsion”. This repulsion will be shown not to affect the ordering properties.

### 3.3 Bethe-Peierls transition in the infinite coordination limit

We now consider the Bethe-Peierls solution of the Ising model . The lattice has a tree topology, with a forward branching ratio $`z1`$, and we calculate the magnetization of the site with the highest hierarchical level (top spin), in the presence of the other sites. We consider $`z1`$ trees and connect them to obtain a tree with one more generation (see Fig. 2). The recursion of the average magnetization of the top spin reads 

$$X=\frac{_{i=1}^{z1}(1+Y_i\mathrm{tanh}(\beta J_i))_{i=1}^{z1}(1Y_i\mathrm{tanh}(\beta J_i))}{_{i=1}^{z1}(1+Y_i\mathrm{tanh}(\beta J_i))+_{i=1}^{z1}(1Y_i\mathrm{tanh}(\beta J_i))},$$
(4)   
where $`Y_i`$, $`i=1,\mathrm{},z1`$ are the magnetizations of the top spins with $`n`$ generations, and $`X`$ the magnetization of the top spin with $`n+1`$ generations. We first consider the artificial situation where the ordering temperature is large compared to the exchange: $`T_{\mathrm{bp}}\mathrm{\Delta }`$, which turns out to be equivalent to assuming a large coordination. Eq. 4 is linearized into $`X=_{i=1}^zY_i\mathrm{tanh}(\beta J_i)`$, leading to the recursion of the magnetization $`X_{n+1}=(z1)\mathrm{tanh}(\beta J)X_n`$, with the subscript $`n`$ labeling the number of generations. This leads to the ordering temperature $`T_{\mathrm{bp}}=(z1)J`$, far above $`\mathrm{\Delta }`$ if $`z1`$, and consistent with the initial assumption. We can calculate the ordering temperature $`T_{\mathrm{bp}}`$ with the different distributions $`P(J)`$ derived in section 3.2. We find:

* with the one dimensional model distribution: $`T_{\mathrm{bp}}=2(z1)x\xi \mathrm{\Delta }/(1+2x\xi )`$;
* with the isotropic two dimensional model distribution: $`T_{\mathrm{bp}}2(z1)\pi x\xi ^2\mathrm{\Delta }`$ in the dilute regime $`x\xi ^2<1`$.
* with the quasi one dimensional model distribution: $`T_{\mathrm{bp}}2(z1)\pi x\xi _x\xi _y\mathrm{\Delta }`$ in the dilute regime $`x\xi _x\xi _y<1`$.

The three limits therefore show a similar behavior $`T_{\mathrm{bp}}(z1)x\mathrm{\Delta }`$, showing that the short distance Wigner repulsion in the spacing distribution Eq. 3 does not affect the ordering properties. Comparing the Bethe-Peierls ordering temperature to the ordering temperature obtained from the Stoner criterion in Ref. , we see that $`z1`$ should be identified with the interchain coupling. The small-$`z`$ regime, relevant to weak interchain correlations, is now discussed in sections 3.4 and 3.5.

### 3.4 Bethe-Peierls transition with a finite coordination: (i) percolation approximation

We now consider the physics at a finite $`z=3`$. In this regime, the Bethe-Peierls method takes into account the inhomogeneities of the magnetization, not included in the Stoner criterion mean field solution in Ref. . We first consider a “percolation approximation” in which we assume the bonds $`JT`$ ($`JT`$) to be set to zero (infinity) in the effective percolation problem. With $`z=3`$, the Bethe-Peierls iteration Eq. 4 reads

$$X=\frac{Y\mathrm{tanh}(\beta J_y)+Z\mathrm{tanh}(\beta J_z)}{1+YZ\mathrm{tanh}(\beta J_y)\mathrm{tanh}(\beta J_z)},$$

and is approximated into: (i) $`TJ_y`$, $`TJ_z`$: $`XY+Z`$; (ii) $`TJ_y`$, $`TJ_z`$: $`XZ`$; (iii) $`TJ_y`$, $`TJ_z`$: $`XY`$; (iv) $`TJ_y`$, $`TJ_z`$: $`X0`$. The recursion of the average magnetization is therefore $`X_{n+1}2\lambda X_n`$, with the percolation parameter

$$\lambda =_T^+\mathrm{}P(J)𝑑J.$$
(5)   
With the one dimensional distribution, we have $`\lambda =1(T/\mathrm{\Delta })^{2x\xi _x}`$, which yields a transition at the temperature

$$T^{}=\mathrm{\Delta }\mathrm{exp}\left(\frac{2\mathrm{ln}2}{x\xi _x}\right),$$
(6)   
exponentially small in $`1/(x\xi _x)`$. This behavior is compatible with Ref.  where we have shown the absence of a true ordering transition in the percolation approximation of a two dimensional anisotropic model, while the model was shown to percolate in a finite size.

### 3.5 Bethe-Peierls transition with a finite coordination: (ii) beyond the percolation approximation

We now solve the Ising model beyond the percolation approximation. We take into account the iteration of small exchanges to lowest order, with the following approximate iteration: (i) $`TJ_y`$, $`TJ_z`$: $`XY+Z`$; (ii) $`TJ_y`$, $`TJ_z`$: $`X\beta J_yY+Z`$; (iii) $`TJ_y`$, $`TJ_z`$: $`XY+\beta J_zZ`$; (iv) $`TJ_y`$, $`TJ_z`$: $`X\beta J_yY+\beta J_zZ`$. The dominant contribution originates from the region (iv) of the couplings: $`X_{n+1}(2/T)\mu (1\lambda )X_n`$, with $`\lambda `$ in Eq. 5, and $`\mu =_0^TJP(J)𝑑J`$. With the one dimensional distribution for $`P(J)`$, we have $`\mu 2x\xi \mathrm{\Delta }`$ and therefore the same critical temperature $`T_{\mathrm{bp}}=4x\xi \mathrm{\Delta }`$ as in the model with a large connectivity $`z`$ (with $`z=3`$ in this calculation). It is remarkable that the correct treatment of the small exchanges restores a transition temperature $`x\xi \mathrm{\Delta }`$. This shows the relevant role played by energy scales smaller than the temperature.

The main unsolved question regarding the classical model behavior is to determine whether the finite dimensional model has a true thermodynamic transition at a temperature $`x\xi \mathrm{\Delta }`$. The Bethe-Peierls solution orders at a temperature $`x\xi \mathrm{\Delta }`$ because of the strong short range correlations. This does not necessarily mean that the finite dimensional model also has a true thermodynamic transition at this temperature. Instead, we believe it possible that the classical model has a cross-over to a Griffiths physics at a temperature $`x\xi \mathrm{\Delta }`$ and a true thermodynamic transition with a diverging correlation length at a temperature $`T^{}`$, which would also be a behavior compatible with a low temperature antiferromagnetic susceptibility. At the present stage, we cannot make the distinction between these two behaviors.

## 4 Quantum isotropic model

We first consider the artificial situation where the correlation lengths are identical in the two directions: $`\xi _x=\xi _y=\xi =9`$. The tendency to ordering in this isotropic model is overestimated compared to the anisotropic model with $`\xi _x=9`$, $`\xi _y=0.1\times \xi _x`$. We are lead to consider the class of interactions

$$J_{ij}=(1)^{d_x+d_y+1}\mathrm{\Delta }\mathrm{exp}\left(\left[\left(\frac{d_x}{\xi _x}\right)^2+\left(\frac{d_y}{\xi _y}\right)^2\right]^{\alpha /2}\right),$$
(7)   
decaying faster than the interactions in Eq. 2 if $`\alpha >1`$. The cluster RG (see the Appendix) generates large energy scales in the parameter range $`\alpha <\alpha _01.2`$. It turns out that $`\alpha _0<1`$ in the model with anisotropic exchanges, and we therefore consider only the regime $`\alpha >\alpha _01.2`$ in the isotropic model.

The gap distribution is shown on Fig. 3 for decreasing temperatures. It is visible that the RG produces gaps of order of the temperature $`T`$ unlike in the case of the infinite randomness fixed point where the opposite occurs (see Ref.  for the one dimensional Heisenberg chain with an infinite randomness, random singlet behavior; see Ref.  for the infinite randomness behavior in the two dimensional Ising model in a transverse field). As in the Ising model analysis, we calculate the susceptibility in two ways: (i) we assume a paramagnetic behavior of the set of effective moments; (ii) we incorporate the correlations induced by exchanges $`\mathrm{\Delta }T`$, in which case an antiferromagnetic behavior in the susceptibility is restored.

### 4.1 Infinite randomness calculation

We first consider all the exchanges $`J<T`$ to be set to zero: the set of effective spins is viewed as a paramagnet with a susceptibility

$$\chi =\frac{1}{TL^2}\underset{i=1}{\overset{N^{(\mathrm{eff})}}{}}S_i^{(\mathrm{eff})}(S_i^{(\mathrm{eff})}+1),$$
(8)   
where $`N^{(\mathrm{eff})}`$ the number of effective spins. We have discarded a prefactor $`1/3`$ in Eq. 8, not relevant to the present calculation. The low temperature susceptibility is therefore controlled by two quantities: (i) the density of free spins $`n_{\mathrm{eff}}=N^{(\mathrm{eff})}/(xL^2)`$; and (ii) the magnitude of the effective spin.

The number of effective moments scales like $`N_{\mathrm{eff}}(T/\mathrm{\Delta })xL^2`$, as it is visible on Fig. 4. The squared effective moment shows two regimes:

* High temperature regime: The high temperature average squared effective moment scales like $`[S^{\mathrm{eff}}]^2\mathrm{\Delta }/T`$ (see Fig. 5). The susceptibility per unit volume is $`\chi x/T`$.
* Low temperature percolation regime: At low temperature, the squared effective moment scales like $`S^2axL^2`$, with $`a`$ some constant (see the insert Fig. 5). The susceptibility per unit volume is $`\chi (ax^2L^2)/\mathrm{\Delta }`$. In this regime, a cluster has percolated through the finite size system. Its magnetization results from summing $`xL^2`$ variables $`S_i^z=\pm 1/2`$, corresponding to the two sublattices magnetizations. Therefore, $`S\sqrt{xL^2}`$, and $`S^2xL^2`$.

The cross-over between these regimes occurs at the temperature scale $`T_{\mathrm{co}}=(\mathrm{\Delta }/a)(xL^2)^1`$, which decreases to zero when the system size is increased. Therefore in the thermodynamic limit, only the high temperature paramagnetic behavior survives while in a finite size, a low temperature tail is present in the susceptibility (see Fig. 6). Now the situation changes when correlations between spins coupled by exchanges of order $`T`$ are included.

### 4.2 Finite randomness calculation

To schematically incorporate the correlations at energy scales of order of the temperature, we consider as frozen the spins connected by an exchange with a gap between $`T/2`$ and $`T`$. This freezing results in a staggered magnetization because the set of effective moments is unfrustrated (see the Appendix). The resulting susceptibility is shown on Fig. 7. It is visible that $`\chi T`$ is linear in $`T`$ at small $`T`$, with therefore a finite susceptibility at zero temperature. This shows qualitatively how an antiferromagnetic behavior can be restored because of the correlations at energy scales $`\mathrm{\Delta }T`$.

## 5 Quantum anisotropic model

### 5.1 One dimensional model

In one dimension, the RG equations of a model in which only AF nearest neighbor exchanges are retained can be solved exactly (see Ref. ). We note $`x=J/[\text{Max}(J)]`$ the exchange normalized to the maximal exchange. The distribution of the variable $`x`$ is $`P(x)=(\overline{f}/\mathrm{\Gamma })x^{\overline{f}/\mathrm{\Gamma }1}`$, with $`\mathrm{\Gamma }=\mathrm{ln}(\mathrm{\Delta }/\text{Max}(J))`$, and $`\overline{f}/\mathrm{\Gamma }=x\xi /(1+\mathrm{\Gamma }x\xi )`$. The weight on the strongest exchanges $`x1`$ is $`x\xi `$ above the cross-over temperature $`T^{}=\mathrm{\Delta }\mathrm{exp}(1/x\xi )`$, and decreases to zero at temperatures below $`T^{}`$, where the system has crossed over to the random singlet fixed point. As a test of our program, we considered the cluster RG of a one dimensional model, with the exchanges not restricted to nearest neighbors (see Eqs. 12). For any practical temperature above $`T^{}`$, the weight on energy scales of order $`T`$ is found to remain constant as the system is renormalized, with therefore the same behavior as in the one dimensional model with AF nearest neighbor exchanges only.

### 5.2 Anisotropic model

We show on Fig. 8 the evolution of the gap distribution as the system is scaled down, with the parameters $`\xi _x=9`$, $`\xi _y=0.1\times \xi _x`$, relevant to CuGeO<sub>3</sub>. As in the isotropic model, energy scales of order $`T`$ are generated upon renormalizing the system. To qualitatively include the effects of correlations at energy scales $`\mathrm{\Delta }T`$, we consider the spins connected by an exchange with a gap between $`T/2`$ and $`T`$ to be frozen, and obtain a low temperature power-law Curie susceptibility, $`\chi T^\alpha `$, with $`\alpha =0.7`$ if $`x=0.01`$ (see Fig. 9). The low temperature susceptibility diverges slower than a Curie law, which is a behavior characteristic of an antiferromagnet. We did not succeed to obtain $`\alpha >0`$ as it is the case in doped CuGeO<sub>3</sub>. Therefore, we cannot rigorously conclude on whether antiferromagnetism is long ranged or associated to a zero temperature transition. A precise discussion of this point is an open question, and would require the correlations at energy $`\mathrm{\Delta }T`$ to be incorporated beyhond our present treatment. For instance the cluster RG could be used to renormalize the high energy physics and the low energy effective Hamitonian could be treated by exact diagonalizations.

## 6 Conclusions

We have shown that the physics of the quantum Hamiltonian Eqs. 12 was already present at the level of the classical Ising model. A Bethe-Peierls treatment of the classical model has been given in which a transition at a temperature $`x\xi \mathrm{\Delta }`$ was found. The quantum Hamiltonian has been treated in a cluster RG. The model was shown to have a finite randomness behavior. We have shown at a qualitative level how a low temperature antiferromagnetic susceptibility can be obtained.

Two questions are left open:

* The Bethe-Peierls solution orders at a temperature $`x\xi \mathrm{\Delta }`$. We do not know whether the two dimensional model has also a thermodynamic transition at a temperature $`x\xi \mathrm{\Delta }`$, or whether this temperature scale corresponds to a cross-over to a Griffith physics. Both behaviors would be a priori compatible with the existence of a maximum in the susceptibility of the antiferromagnet at a temperature $`x\xi \mathrm{\Delta }`$.
* The quantum model susceptibility shows an antiferromagnetic behavior at low temperature due to correlations at energies $`\mathrm{\Delta }T`$. The isotropic model shows a finite susceptibility at low temperature while the quasi one dimensional has a susceptibility diverging slower than a Curie law. A precise investigation of the low temperature susceptibility would require a treatment going beyond our present analysis, for instance by treating the low energy effective Hamiltonian by exact diagonalizations.

Two other proposals to explain antiferromagnetism in doped in CuGeO<sub>3</sub> have been made: Fukuyama, Tanimoto and Saito  and Mostovoy, Khomskii, and J. Knoester . These proposals are quite different from ours, and we have exposed previously why we think they our model is more relevant . The inclusion of interchain interaction in our model in Ref.  and the present work, points strongly towards an compatibility with experiments.

## Acknowledgements

The author thank M. Fabrizio and J. Souletie for numerous fruitful discussions, their encouragements, and for useful comments on the manuscript. M. Fabrizio pointed out to me the possibility of cluster RG calculations as well as the proof that the effective problem remains unfrustrated as the system is scaled down. J. Souletie suggested the existence of a similar physics in the classical and quantum models. The cluster RG calculations have been performed on the CRAY T3E supercomputer of the Centre Grenoblois de Calcul Vectoriel of the Commisariat à l’Energie Atomique.

## Appendix A Renormalization equations

We use a cluster RG to renormalize the quantum Hamiltonian Eqs. 12. The method relies on a perturbative expansion in the inverse of the largest exchange, and was originally proposed by Dasgupta and Ma  in the context of disordered Heisenberg chains. The cluster RG was applied by Bhatt and Lee  to a model of phosphorus doped silicon. Fisher used the method to solve exactly the random singlet fixed point . The cluster RG was also used to investigate the low energy physics of disordered spin chains: the dimerized Heisenberg chain with random exchanges ; the spin-one chain with random exchanges ; Heisenberg chains with random ferromagnetic and antiferromagnetic couplings . Recently, Motrunich et al.  shown the existence of an infinite randomness fixed point in two dimensions in the Ising model in a transverse field. At such a fixed point, inhomogeneities in the disorder grow indefinitely as the system is scaled down, as in the random singlet fixed point in one spatial dimension. We now give a short derivation of the RG equations.

We isolate two spins $`𝐒_1`$ and $`𝐒_2`$ coupled by an exchange $`J_{12}`$. This sets an energy scale given by the gap between the ground state and the first excited multiplet: if $`J_{12}>0`$ is antiferromagnetic, the ground state has a spin $`S=|S_1S_2|`$ and the first excited multiplet has $`S=|S_1S_2|+1`$, with a gap $`\mathrm{\Delta }_{12}=|J_{12}|(|S_1S_2|+1)`$. If $`J_{12}<0`$ is ferromagnetic, the ground state has $`S=S_1+S_2`$ and the first excitated multiplet has $`S=S_1+S_21`$, with a gap $`\mathrm{\Delta }_{12}=|J_{12}|(S_1+S_2)`$. Among all possible pairs of spins, we consider the one with the strongest gap $`\mathrm{\Delta }_{12}`$. This energy scale is identified to the system temperature. If $`𝐒_1`$ and $`𝐒_2`$ are coupled ferro ($`J_{12}<0`$) , the two spins $`𝐒_1`$ and $`𝐒_2`$ are replaced by an effective spin $`S=S_1+S_2`$. If they are coupled antiferro, they are replaced by an effective spin $`S=|S_1S_2|`$. $`S_1=S_2`$ with an AF coupling $`J_{12}`$ leads to singlet formation while a residual moment is formed otherwise.

### A.1 Residual moment formation

Let us first consider the case where a residual moment is formed corresponding to (a) and (b) on Fig. 10. We specialize a spin $`𝐒_3`$ among the other spins and denote by $`J_{ij}`$ the exchange between spins $`i`$ and $`j`$, with $`i,j=1,\mathrm{},3`$. The coupling Hamiltonian between the spins $`𝐒_1`$ and $`𝐒_2`$ is $`H_{12}=J_{12}𝐒_1.𝐒_2`$ while the remaining couplings

$$H_I=J_{13}𝐒_1.𝐒_3+J_{23}𝐒_2.𝐒_3$$
(9)   
are treated in a first order perturbation. This leads to the renormalized coupling Hamiltonian $`H_I=\stackrel{~}{J}_3𝐒_3.𝐒`$, with the renormalized exchange

$$\stackrel{~}{J}_3=J_{13}c(S_1,S_2,S)+J_{23}c(S_2,S_1,S),$$
(10)   
with

$$c(S_1,S_2,S)=\frac{S(S+1)+S_1(S_1+1)S_2(S_2+1)}{2S(S+1)}$$

derived in Ref. . The sublattice on which the residual spin is placed is determined as follows: if $`S_1>S_2`$, the residual spin $`S`$ is placed on the same sublattice as $`S_1`$ while it is placed on the sublattice of $`S_2`$ if $`S_1<S_2`$.

### A.2 Singlet formation

We now consider singlet formation, with $`S_1=S_2`$ coupled AF. The renormalized couplings are obtained in a second order perturbation theory. Generalizing the calculation in Ref.  to the coupling Hamiltonian (9), we find the renormalized exchange

$$\stackrel{~}{J}_{34}=J_{34}+\frac{2S_1(S_1+1)}{3J_{12}}(J_{13}J_{23})(J_{24}J_{14}),$$
(11)   
where $`S_1=S_2`$ denote the spins at site $`1`$ and $`2`$. In the 1D limit $`J_{23}=J_{14}=0`$ Eq. 11 reproduces the result in Ref. , and the spin-1/2 limit $`S_1=1/2`$ reproduces the result in Ref. .

### A.3 Absence of frustration

We show that frustration is not generated by the RG procedure. We assume an unfrustrated starting Hamiltonian, and show that the different RG operations are compatible with the sublattice structure. We distinguish three cases:

* $`S_1`$ and $`S_2`$ belong to different sublattices and are coupled antiferro. We assume $`S_1>S_2`$ and the effective spin $`S=S_1S_2`$ replaces the spin $`S_1`$. The renormalized coupling to another spin $`S_3`$ in Eq. 10 is

$$\stackrel{~}{J}_3=J_{13}+(J_{13}J_{23})\frac{S_2}{S+1}.$$

$`J_{13}>0`$ and $`J_{23}<0`$ leads to $`\stackrel{~}{J}_3>0`$. $`J_{13}<0`$ and $`J_{23}>0`$ leads to $`\stackrel{~}{J}_3<0`$. The renormalized coupling $`\stackrel{~}{J}_3`$ has thus a sign compatible with the sublattice structure.
* $`S_1`$ and $`S_2`$ belong to the same sublattices and are coupled ferro. $`J_{13}`$ and $`J_{23}`$ have the same sign. We have $`c(S_1,S_2,S)>0`$ and $`c(S_2,S_1,S)>0`$. The renormalized coupling $`\stackrel{~}{J}_3`$ has the same sign as $`J_{13}`$ and $`J_{23}`$, compatible with the sublattice structure.
* $`S_1=S_2`$ are coupled antiferro and a singlet is formed. If $`S_3`$ and $`S_4`$ are coupled ferro and in the same sublattice, $`\stackrel{~}{J}_{34}<0`$ in Eq. 11. If $`S_3`$ and $`S_4`$ are coupled antiferro and in the opposite sublattice, $`\stackrel{~}{J}_{34}>0`$ in Eq. 11. The singlet formation is thus compatible with the sublattice structure.