text:
# Kirwan map and moduli space of flat connections

## Index of notation

| $``$ | Group of relative integers |
| --- | --- |
| $``$ | Field of reals |
| $`g`$ | Integer bigger than $`1`$ |
| $`𝐅`$ | Free group on $`2g`$ generators $`x_1,\mathrm{},x_{2g}`$ |
| $`R`$ | Element in $`𝐅`$ given by $`_{j=1}^g[x_{2j1},x_{2j}]`$ |
| $`𝚷`$ | Quotient of $`𝐅`$ by the relation $`_{j=1}^g[x_{2j1},x_{2j}]`$=1 |
| $`\mathrm{\Sigma }`$ | Closed Riemann surface of genus $`g`$ |
| $`\mathrm{\Sigma }_0`$ | $`\mathrm{\Sigma }`$ with the interior of a disc removed |
| $`K`$ | Simply connected compact Lie group |
| $`Z(K)`$ | Centre of $`K`$ |
| $`K_c`$ | Quotient of $`K`$ by its centre $`Z(K)`$ |

## Acknowledgement

I would like to thank Frances Kirwan for her comments on a preliminary version of this article. I also thank Lisa Jeffrey for sending me a copy of Shulman .

The author was supported by a Marie-Curie Fellowship, EC Contract Ref: HPMF-CT-2002-01850.

## 1. Introduction

All cohomology will have coefficients in $``$.

Let $`\mathrm{\Sigma }`$ be a closed compact Riemann surface of genus $`g`$. Let $`\mathrm{\Sigma }_0`$ be a compact Riemann surface with boundary obtained from $`\mathrm{\Sigma }`$ by removing a small disc.

Let $`K`$ be a compact simply connected Lie group. I denote by $`K_c`$ the quotient of $`K`$ by its centre $`Z(K)`$. In other words, $`K_c`$ is the projectivisation of $`K`$. Let $`\beta `$ be in the centre of $`K`$. Let $`K`$ act on itself by conjugation and on $`K^{2g}`$ by diagonal conjugation. The point $`\beta `$ is fixed by $`K`$. Let $`EKBK`$ be a classifying bundle for $`K`$. If $`M`$ is a topological space acted on by $`K`$, the equivariant cohomology $`H_K^{}(M)`$ of $`M`$ is the singular cohomology of $`M_K=M\times _KEK`$. If $`M`$ is a manifold and it is acted on smoothly by $`K`$, then $`H_K^{}(M)`$ is also the cohomology of the Cartan-de Rham complex $`\mathrm{\Omega }_K^{}(M)`$.

Let $`\mathrm{\Phi }`$ be the equivariant map

$$\begin{array}{ccc}K^{2g}& & K\\ (X_1,\mathrm{},X_{2g})& & _{i=1}^g[X_{2i1},X_{2i}].\end{array}$$

Let $`Y_\beta =\mathrm{\Phi }^1(\beta )`$. The space $`\mathrm{\Phi }^1(\beta )/K`$ is homeomorphic to the moduli space of flat connections on the trivial bundle $`K\times \mathrm{\Sigma }_0\mathrm{\Sigma }_0`$ (all $`K`$ principal bundles over $`\mathrm{\Sigma }_0`$ are trivial) with prescribed holonomy $`\beta `$ around the boundary $`S^1`$ of $`\mathrm{\Sigma }_0`$.

Call $`\kappa `$ the restriction map

$$\kappa :H_K^{}(K^{2g})H_K^{}(Y_\beta ).$$

Let $`b_1,\mathrm{},b_r`$ be primitive elements which generate $`H^{}(K)`$ and let $`c_1,\mathrm{},c_r`$ be their respective transgressions in $`H^{}(BK)`$. One can extend $`b_1,\mathrm{},b_r`$ to equivariant classes $`b_1^K,\mathrm{},b_r^K`$ on $`K`$. Let $`pr_i:K^{2g}K`$ be the projection on the $`i`$-th factor and $`b_{j,i}^K`$ the pull-back of $`b_j^K`$ by $`pr_i`$.

Because $`\mathrm{\Phi }`$ is a moment map on the quasi-Hamiltonian space $`K^{2g}`$ (see ), the paper  gives a way of constructing equivariant classes $`a_1,\mathrm{},a_r`$ on $`Y_\beta `$ (see Equation (1) on page 1) such that $`\{\kappa (c_j),\kappa (b_{j,i}^K),a_j,j=1,\mathrm{},r,i=1,\mathrm{},2g\}`$ generate the $`K`$-equivariant cohomology of $`Y_\beta `$.

Also, one can construct a $`K`$-equivariant $`K_c`$-principal bundle over $`\mathrm{\Sigma }\times Y_\beta `$: the so called universal bundle. The Künneth decomposition of the equivariant characteristic classes of this bundle allows me to construct classes $`\{c_j^{},b_{j,i}^{},a_j^{},j=1,\mathrm{},r,i=1,\mathrm{},2g\}`$ in $`H_K^{}(Y_\beta )`$ (see Equation (2) on page 2). At least when $`K`$ is the special unitary group and $`\beta `$ is a generator of the centre of $`K`$, these classes are known to generate $`H_K^{}(Y_\beta )`$ as a ring. They are the Atiyah-Bott-Biswas-Raghavendra classes111Atiyah and Bott  were the first ones to construct generators of the cohomology of the moduli space. Their classes depended on the choice of a universal bundle which was only defined up to the tensor product with a line bundle. The universal bundle of this article is actually the projectivisation of theirs. It is well-defined and so are the generators constructed from it. This was proved by Biswas and Raghavendra in .

The aim of this paper is to prove the following Theorem.
Theorem 3.2. — Let $`\mathrm{K}`$ be a compact, connected and simply connected Lie group. Let $`\mathrm{\beta }`$ be in the centre of $`\mathrm{K}`$ such that $`\mathrm{K}`$ acts locally freely on $`\mathrm{Y}_\mathrm{\beta }`$. Let $`\mathrm{a}_\mathrm{j}^{},\mathrm{b}_{\mathrm{j},\mathrm{i}}^{},\mathrm{c}_\mathrm{j}^{},\mathrm{a}_\mathrm{j},\mathrm{b}_{\mathrm{j},\mathrm{i}}^\mathrm{K},\mathrm{c}_\mathrm{j}`$ be equivariant classes defined as above. The following relations hold

$$\begin{array}{ccc}c_j^{}& =& \kappa (c_j)\\ b_{j,i}^{}& =& \kappa (b_{j,i}^K).\end{array}$$

Also, the classes $`\{a_j\}`$ depend on certain choices but one can choose them so that

$$a_j^{}=a_j.$$

This article is organised as followed. In Section 2, I recall what  says about the restriction map involved in the reduction of $`K^{2g}`$ at $`\beta `$. I also show how to use this result to construct generators for the $`K`$-equivariant cohomology of $`Y_\beta `$. In Section 3, I describe the construction of equivariant characteristic classes on $`Y_\beta `$ using a universal bundle over $`\mathrm{\Sigma }\times Y_\beta `$. I also outline the proof of Theorem 3.2, leaving the most technical details for Section 4.

## 2. Generators for the equivariant cohomology of $`Y_\beta `$

Let $`𝚷`$ be the fundamental group of $`\mathrm{\Sigma }`$. Fix a presentation

$$𝚷=x_1,\mathrm{},x_{2g};\underset{j=1}{\overset{g}{}}[x_{2j1},x_{2j}]=1.$$

Let $`𝐅`$ be the fundamental group of $`\mathrm{\Sigma }_0`$. Fix a presentation

$$𝐅=x_1,\mathrm{},x_{2g}$$

such that the map

$$𝐅𝚷$$

induced by the inclusion of $`\mathrm{\Sigma }_0`$ in $`\mathrm{\Sigma }`$, is given by the obvious map $`x_kx_k`$.

Let $`\beta `$ be in the centre of $`K`$. Let $`Y_\beta `$ be the subset of $`K^{2g}`$ defined by

$$Y_\beta =\{(X_1,\mathrm{},X_{2g})K^{2g}\underset{j=1}{\overset{g}{}}[X_{2j1},X_{2j}]=\beta \}.$$

The group $`K`$ acts on $`K^{2g}`$ by conjugation. This action restricts to $`Y_\beta `$, since $`\beta `$ is in the centre of $`K`$. The quotient $`_\beta =Y_\beta /K`$ can be identified with a moduli space of flat connections on the trivial principal bundle $`K\times \mathrm{\Sigma }_0\mathrm{\Sigma }_0`$ (because $`K`$ is simply connected, all principal bundles are trivial over $`\mathrm{\Sigma }_0`$), with holonomy $`\beta `$ around the boundary $`\mathrm{\Sigma }_0`$. If $`K`$ acts locally freely on $`Y_\beta `$, then the cohomology of $`_\beta `$ is isomorphic to the $`K`$-equivariant cohomology of $`Y_\beta `$ (recall that cohomology is taken with coefficients in $``$).

Let $`\kappa `$ be the restriction map

$$\kappa :H_K^{}(K^{2g})H_K^{}(Y_\beta ).$$

The space $`K^{2g}`$ has the structure of a quasi-Hamiltonian space (see ) with moment map

$$\begin{array}{cccc}\varphi :& K^{2g}& & K\\ & (X_1\mathrm{},X_{2g})& & _{j=1}^g[X_{2j1},X_{2j}].\end{array}$$

The map $`\varphi `$ is a submersion at any point of $`Y_\beta =\varphi ^1(\beta )`$ if and only if $`K`$ acts locally freely on $`Y_\beta `$. In this nice case, the space $`_\beta `$ is a compact symplectic orbifold since it is the regular reduction of $`K^{2g}`$ at $`\beta `$.

Let $`b_1,\mathrm{},b_r`$ be primitive elements in $`H^{}(K)`$ that generate the cohomology of $`K`$ as a ring

$$H^{}(K)=(\underset{j=1}{\overset{r}{}}b_j).$$

Each $`b_j`$ is of odd degree.

Let $`c_1,\mathrm{},c_r`$ be the transgressions in $`H^{}(BK)`$ of respectively $`b_1,\mathrm{},b_r`$, thus $`\mathrm{deg}c_j=\mathrm{deg}b_j+1`$ and

$$H^{}(BK)=[c_1,\mathrm{},c_r].$$

For each $`K`$-principal bundle $`GX`$, the classes $`c_1,\mathrm{},c_r`$ define characteristic classes $`c_1(G),\mathrm{},c_r(G)`$ in $`H^{}(X)`$.

###### Proposition 2.1.

Let $`EKBK`$ be the classifying bundle for $`K`$. The bundle $`EK\times _KK^nBK`$ is cohomologically trivial as a ring, that is

$$H_K^{}(K^n)H^{}(BK)H^{}(K^n)$$

as rings.

This result is not new. I propose here a proof which is original as far as I know.

Also, because I want to state the principal results as soon as possible, I will make use in the following proof, as well as in others, of Lemma 3.5 even if I haven’t proved it yet.
Proof.  I will prove the case $`n=1`$. The general case is similar, one only has to use Proposition 3.6 instead of Lemma 3.5 (or use the fact that if $`X`$ has an equivariantly formal action of $`K`$ then the diagonal action of $`K`$ on $`X^n`$ is also equivariantly formal).

Let me first prove that $`H_K^{}(K)`$ and $`H^{}(BK)H^{}(K)`$ are isomorphic as $`H^{}(BK)`$ modules. By the Leray-Hirsch Theorem, all I have to do is prove that the homomorphism

$$H_K^{}(K)H^{}(K)$$

is surjective. Let $`b_j`$ be one of the generators of $`H^{}(K)`$. Let $`DS^1\times K`$ be the $`K`$-equivariant $`K`$-principal bundle of Lemma 3.5. As a $`K`$-principal bundle, its characteristic class $`c_j(D)`$ is $`\mathrm{d}tb_j`$ (Lemma 3.5). As an immediate corollary, I deduce that there exists $`b_j^K`$ in $`H_K^{}(K)`$ such that $`c_j(D\times _KEK)=1c_j+\mathrm{d}tb_j^K`$, where $`b_j^K`$ restricts to $`b_j`$. Now, because the $`b_j`$’s generate $`H^{}(K)`$ as a ring, the homomorphism

$$H_K^{}(K)H^{}(K)$$

is surjective and I have proved the existence of a $`H^{}(BK)`$ module isomorphism between $`H_K^{}(K)`$ and $`H^{}(BK)H^{}(K)`$. The existence of a ring isomorphism follows because the cohomology $`H^{}(K)`$ of the fibre in $`K\times _KEKBK`$ is generated by classes of odd degree (see ). $`\mathrm{}`$

###### Remark 2.2.

Let $`s`$ be the section

$$\begin{array}{cccc}s:& BK& & EK\times _KK\\ & [u]& & [u,1].\end{array}$$

Via $`\mathrm{id}\times s:S^1\times BKS^1\times K_K`$, the bundle $`D_KS^1\times K_K`$ pulls back to $`S^1\times EKS^1\times BK`$. Hence $`s^{}b_j^K=0`$.

Let $`n`$ be an integer (I will need it to be either $`1`$ or $`2g`$). Let $`b_{j,i}^K`$ be the pull-back, under the projection on the $`i`$-th factor $`K^nK`$, of $`b_j^K`$.

The following Lemma is a consequence of Proposition 2.1.

###### Lemma 2.3.

The $`K`$-equivariant cohomology of $`K^n`$ is isomorphic as a ring to

$$H_K^{}(K^n)(b_{j,i}^K)[c_1,\mathrm{},c_r].$$

Before stating the result of Bott, Tolman and Weitsman for $`\kappa `$, I need to construct some classes in $`H_K^{}(Y_\beta )`$.

###### Lemma 2.4.

For all $`j`$, the pull-back under $`\varphi ^{}`$ of $`b_j^K`$ is zero

$$\varphi ^{}(b_j^K)=0.$$

In their article , the authors already gave this result. I give here a proof using Lemma 3.5.
Proof.  Consider the diagram

where the horizontal map $`m_1`$ is induced by the moment map $`\varphi :K^{2g}K`$ and the vertical map $`m_2`$ is given by the injection of $`S^1`$ as the boundary of $`\mathrm{\Sigma }_0`$. The pull-back of $`D`$ by $`m_1`$ and the pull-back of $`F`$ by $`m_2`$ are isomorphic. Indeed they are both equivariantly isomorphic to the bundle

$$(\times K^{2g}\times K)/S^1\times K^{2g}$$

where the group $``$ acts by

$$\begin{array}{ccc}\times \times K^{2g}\times K& & \times K^{2g}\times K\\ (\lambda ,t,(X_1,\mathrm{},X_{2g}),k)& & (t+\lambda ,(X_1,\mathrm{},X_{2g}),(_{j=1}^g[X_{2j1},X_{2j}])^\lambda k).\end{array}$$

One then deduces the Lemma from Proposition 3.6 and Lemma 3.5 by noticing that the injection of $`S^1`$ as the boundary of $`\mathrm{\Sigma }_0`$ induces the null map in degree $`1`$ cohomology. $`\mathrm{}`$

Let $`\overline{b_1},\mathrm{},\overline{b_r}`$ be equivariant forms representing respectively $`b_1^K,\mathrm{},b_r^K`$.

###### Remark 2.5.

Such forms will be chosen in Section 4 so that their pull-backs by the section $`s`$ of Remark 2.2 vanish.

The preceding Lemma implies there exist equivariant forms $`\overline{a_1},\mathrm{},\overline{a_r}`$ on $`K^{2g}`$ such that

(1) $`\varphi ^{}(\overline{b_j})`$ $`=`$ $`\mathrm{d}\overline{a_j},j.`$
The $`\overline{a_1},\mathrm{},\overline{a_r}`$ are closed when restricted to $`Y_\beta `$. They define classes $`a_1,\mathrm{},a_r`$ in $`H_K^{}(Y_\beta )`$.

###### Theorem 2.6 ( Bott, Tolman and Weitsman ).

The equivariant cohomology $`H_K^{}(Y_\beta )`$ is generated as a ring by the image of $`\kappa `$ and the $`a_1,\mathrm{},a_r`$.

The following Corollary is an immediate consequence.

###### Corollary 2.7.

The equivariant cohomology $`H_K^{}(Y_\beta )`$ is generated as a ring by the classes $`\kappa (c_j),\kappa (b_{j,i}^K),a_j`$ for $`j=1,\mathrm{},r`$ and $`i=1,\mathrm{},2g`$.

## 3. Some classical classes in $`H_K^{}(Y_\beta )`$

Let $`\stackrel{~}{\mathrm{\Sigma }}`$ be the universal cover of $`\mathrm{\Sigma }`$. The group $`𝚷`$ acts on $`\stackrel{~}{\mathrm{\Sigma }}`$. Since I have chosen a presentation for $`𝐅`$, there is a preferred isomorphism

$$\begin{array}{ccc}\mathrm{Hom}(𝐅,K)& & K^{2g}\\ \rho & & (\rho (x_1),\mathrm{},\rho (x_{2g})).\end{array}$$

I will use this isomorphism to identify $`\mathrm{Hom}(𝐅,K)`$ and $`K^{2g}`$. Define an action of $`𝚷`$ on $`\stackrel{~}{\mathrm{\Sigma }}\times Y_\beta \times K_c`$

$$\begin{array}{ccc}𝚷\times (\stackrel{~}{\mathrm{\Sigma }}\times Y_\beta \times K_c)& & \stackrel{~}{\mathrm{\Sigma }}\times Y_\beta \times K_c\\ (p,\sigma ,\rho ,k)& & (p\sigma ,\rho ,\rho (\stackrel{~}{p})k),\end{array}$$

where $`\stackrel{~}{p}`$ is any element in $`𝐅`$ lying above $`p`$. This action is well-defined and free. The quotient $`E`$, together with the projection $`\pi :E\mathrm{\Sigma }\times Y_\beta `$ define a $`K_c`$-principal bundle. The actions of $`K`$ on $`Y_\beta `$ by conjugation and on $`K_c`$ by multiplication on the left, make $`E`$ into a $`K`$-equivariant $`K_c`$-principal bundle over $`\mathrm{\Sigma }\times Y_\beta `$. I call it the universal bundle (this bundle is also constructed in Jeffrey ).

###### Example 3.1.

For $`K=\mathrm{𝐒𝐔}(n)`$ and $`\beta `$ a generator of $`Z(\mathrm{𝐒𝐔}(n))`$, this is the projectivisation of a universal bundle for the moduli space of semi-stable vector bundles of fixed rank and determinant (see  and ).

Because $`K`$ is compact and simply connected, I know that

$$H^{}(BK)H^{}(BK_c).$$

The classes $`c_1,\mathrm{},c_r`$ in $`H^{}(BK_c)`$ define equivariant characteristic classes for the bundle $`E`$ (recall that these are the same as the usual characteristic classes of the $`K`$-principal bundle $`E\times _KEK\mathrm{\Sigma }\times Y_\beta \times _KEK`$). These classes live in $`H_K^{}(\mathrm{\Sigma }\times Y_\beta )H^{}(\mathrm{\Sigma })H_K^{}(Y_\beta )`$. Let $`\alpha _1,\mathrm{},\alpha _{2g}`$ be a basis of $`H^{}(\mathrm{\Sigma })`$, dual to $`x_1,\mathrm{},x_{2g}`$ in $`𝚷=\pi _1(\mathrm{\Sigma })`$. Let $`𝒱`$ be a volume form of volume $`1`$ on $`\mathrm{\Sigma }`$. Using the Künneth decomposition, write

(2) $`c_j(E\times _KEK)`$ $`=`$ $`1c_j^{}+{\displaystyle \underset{i=1}{\overset{2g}{}}}\alpha _ib_{j,i}^{}+𝒱a_j^{}.`$
In Example 3.1, these classes are the known Atiyah-Bott – Biswas-Raghavendra generators of $`H_K^{}(Y_\beta )`$. A natural question is: what is the relation between these classes and the ones of Corollary 2.7? The answer is given in the following Theorem.

###### Theorem 3.2.

Let $`K`$ be compact, connected and simply connected Lie group. Let $`\beta `$ be in the centre of $`K`$. Assume that $`\beta `$ is a regular value of the moment map $`\mathrm{\Phi }`$. Let the $`\{a_j^{},b_{j,i}^{},c_j^{},a_j,b_{j,i}^K,c_j\}`$ be equivariant classes defined as above. The following relations hold

$$\begin{array}{ccc}c_j^{}& =& \kappa (c_j)\\ b_{j,i}^{}& =& \kappa (b_{j,i}^K).\end{array}$$

Also, the classes $`\{a_j\}`$ depend on certain choices but one can choose them so that

$$a_j^{}=a_j.$$

Proof.  Fix $`j`$. I will start by proving the first part of the Theorem, that is I will compute the $`\{c_j^{},b_{j,i}^{}\}`$.

Let $`\stackrel{~}{\mathrm{\Sigma }}_0`$ be the universal covering for $`\mathrm{\Sigma }_0`$. Define an action of $`𝐅=\pi _1(\mathrm{\Sigma }_0)`$ on $`\stackrel{~}{\mathrm{\Sigma }}_0\times K^{2g}\times K`$

$$\begin{array}{ccc}𝐅\times \stackrel{~}{\mathrm{\Sigma }}_0\times K^{2g}\times K& & \stackrel{~}{\mathrm{\Sigma }}_0\times K^{2g}\times K\\ (p,\sigma ,\rho ,k)& & (p\sigma ,\rho ,\rho (p)k).\end{array}$$

This action is free and the quotient $`F`$ is a $`K`$-principal bundle on $`\mathrm{\Sigma }_0\times K^{2g}`$. The action of $`K`$ by conjugation on $`K^{2g}`$ and by multiplication on the left on $`K`$ makes $`F`$ into a $`K`$-equivariant $`K`$-principal bundle. The situation here is somehow confusing since there are two different actions of $`K`$ on $`F`$. In order to clarify the situation, I will call the action that makes $`F`$ a $`K`$-principal bundle the principal action and call the action that makes it $`K`$-equivariant the covering action (‘covering’ because it covers the action of $`K`$ on $`K^{2g}`$).

###### Proposition 3.3.

The projectivisation of $`F_{\mathrm{\Sigma }_0\times Y_\beta }`$ is $`K`$-equivariantly isomorphic to $`E_{\mathrm{\Sigma }_0\times Y_\beta }`$.

Proof.  The proof is easy. $`\mathrm{}`$

Call $`D_n`$ the restriction of $`F`$ to the $`n`$-th circle in the wedge product times the $`n`$-th copy of $`K`$ in $`K^{2g}`$. I identify the circle $`S^1`$ with the quotient $`/`$. I denote by $`t`$ the natural coordinate in $``$, thus $`dt`$ defines a volume form on $`S^1`$.

###### Lemma 3.4.

All the $`D_n`$’s are isomorphic to the same bundle $`DS^1\times K`$. The total space $`D`$ is $`(\times K\times K)/`$ where the action of $``$ is defined by

$$\begin{array}{ccc}\times (\times K\times K)& & \times K\times K\\ (\lambda ,t,k_1,k_2)& & (t+\lambda ,k_1,k_1^\lambda k_2)\end{array}$$

and the projection is

$$\begin{array}{ccc}(\times K\times K)/& & S^1\times K\\ \{t,k_1,k_2\}& & (\{t\},k_1).\end{array}$$

Proof.  Fix an integer $`n`$ between $`1`$ and $`2g`$ and let $`x=x_n`$ be the $`n`$-th generator of $`𝐅`$.
Recall that $`F`$ was defined as a quotient

$$F=(\stackrel{~}{\mathrm{\Sigma }}_0\times K^{2g}\times K)/\pi _1(\mathrm{\Sigma }_0).$$

Let $`h`$ be the group homomorphism

$$\begin{array}{ccc}& & \pi _1(\mathrm{\Sigma }_0)\\ \lambda & & x^\lambda .\end{array}$$

This morphism makes $``$ into a subgroup of $`\pi _1(\mathrm{\Sigma }_0)`$. Choose a point $`\stackrel{~}{\sigma _0}`$ in $`\mathrm{\Sigma }_0`$ lying above the base point $`\sigma _0`$ of $`\mathrm{\Sigma }_0`$. Choose a loop $`S^1\mathrm{\Sigma }_0`$ representing $`x`$. This loop lifts to a map $`\chi :\stackrel{~}{\mathrm{\Sigma }}_0`$ such that $`\chi (0)=\stackrel{~}{\sigma _0}`$ and for $`\lambda `$ an integer $`\chi (t+\lambda )=x^\lambda \chi (t)`$.

The covering action of $`K`$ (the one that covers the action of $`K`$ on $`S^1\times K`$) on $`D_n`$ is induced by the conjugation on the first factor $`K`$ in $`\times K\times K`$ and by multiplication on the left on the second factor $`K`$.

Let $`\iota :KK^{2g}`$ be the injection of the $`n`$-th factor. Define a map

$$\begin{array}{ccc}(\times K\times K)/& & (\stackrel{~}{\mathrm{\Sigma }}_0\times K^{2g}\times K)/\pi _1(\mathrm{\Sigma }_0)\\ [t,X,k]& & [\chi (t),\iota (X),k].\end{array}$$

This map is well-defined since it sends the translated $`[t+\lambda ,X,X^\lambda k]`$ of $`[t,X,k]`$ by $`\lambda `$ to

$$\begin{array}{cc}& [\chi (t+\lambda ),\iota (X),X^\lambda k]\hfill \\ =& [x_n^\lambda \chi (t),\iota (X),X^\lambda k]\hfill \\ =& [\chi (t),\iota (X),k].\hfill \end{array}$$

It is also $`K`$-equivariant because, for $`\mathrm{}`$ in $`K`$, it sends $`[t,\mathrm{Ad}_{\mathrm{}}X,\mathrm{}k]`$ to

$$\begin{array}{cc}& [\chi (t),\iota (Ad_{\mathrm{}}X),\mathrm{}k]\hfill \\ =& [\chi (t),Ad_{\mathrm{}}\iota (X),\mathrm{}k]\hfill \\ =& \mathrm{}[\chi (t),\iota (X),k].\hfill \end{array}$$

The Lemma follows. $`\mathrm{}`$

###### Lemma 3.5.

The characteristic classes of $`D`$ are

$$c_j(D)=dtb_j.$$

Proof.  The proof is to be found in the next Section. $`\mathrm{}`$

The previous Lemma is actually very useful since it can be used to prove Proposition 3.6 which leads to Theorem 3.2, and also Proposition 2.1 and Lemma 2.4.

Now I wish to compute the equivariant characteristic classes of $`F`$. The cohomologies of $`\mathrm{\Sigma }`$ and $`\mathrm{\Sigma }_0`$ are the same in degree $`0`$ and $`1`$ and $`\mathrm{\Sigma }_0`$ has no cohomology in degree $`2`$. I use the same basis $`\alpha _1,\mathrm{},\alpha _{2g}`$ for $`H^1(\mathrm{\Sigma })`$ and $`H^1(\mathrm{\Sigma }_0)`$.

###### Proposition 3.6.

Using the Künneth decomposition, the equivariant characteristic classes of $`F`$ are

$$c_j(F\times _KEK)=1c_j+\underset{i=1}{\overset{2g}{}}\alpha _ib_{j,i}^K.$$

Proof.  The surface $`\mathrm{\Sigma }_0`$ is homotopic to a wedge product of $`2g`$ circles. As is easily seen, Proposition 3.6 will follow from the computation of the characteristic classes of the restriction of $`F`$ to the $`n`$-th circle in the wedge product times the $`m`$-th copy of $`K`$ in $`K^{2g}`$, that is $`D_n`$. When $`nm`$, the restriction of $`F`$ is trivial. Thus, I only have to do the computation for $`n=m`$. This was done in Lemma 3.5. $`\mathrm{}`$

The first part of the Theorem is a consequence of Proposition 3.3 and Proposition 3.6. Indeed, by Proposition 3.3

$$c_j(E\times _KEK)_{\mathrm{\Sigma }_0\times Y_\beta }=c_j(F\times _KEK)_{\mathrm{\Sigma }_0\times Y_\beta }.$$

But

(3) $`c_j(E\times _KEK)_{\mathrm{\Sigma }_0\times Y_\beta }=1c_j^{}+{\displaystyle \underset{i=1}{\overset{2g}{}}}\alpha _ib_{j,i}^{}`$
and by Proposition 3.6

(4) $`c_j(F\times _KEK)\mathrm{\Sigma }_0\times Y_\beta `$ $`=`$ $`(\mathrm{id}^{}\times \kappa )c_j(F\times _KEK)`$
$`=`$ $`1\kappa (c_j)+{\displaystyle \underset{i=1}{\overset{2g}{}}}\alpha _i\kappa (b_{j,i}^K).`$
The first part of the Theorem follows by comparing Equation (3) and Equation (4).

The second part of Theorem 3.2 is a consequence of the following Lemma and of the definition of the classes $`a_1,\mathrm{},a_r`$.

###### Lemma 3.7.

One can choose representatives $`\overline{b}_j^K`$ and $`\overline{a}_j^{}`$ of respectively $`b_j^K`$ and $`a_j^{}`$ such that $`\overline{a}_j^{}`$ extends to an equivariant class on $`K^{2g}`$ whose differential is $`\mathrm{\Phi }^{}(\overline{b}_j^K)`$.

The proof of this Lemma, together with the proof of Lemma 3.5, is given in the next Section.

This finishes the proof of Theorem 3.2. $`\mathrm{}`$

###### Remark 3.8.

If the group $`K`$ is a torus $`T`$, then it is not simply connected and one can not apply Theorem 3.2 to find generators of the cohomology of the moduli space. Nevertheless, in this case the moduli space is either $`T^{2g}`$ if $`\beta =1`$ or is empty otherwise. Its cohomology is thus very simple. In general, a connected compact Lie group is the quotient by a finite group of a product of a simply connected group and a torus. Combining what I have just said about tori with Theorem 3.2, one can deduce generators for the cohomology of the moduli space.

## 4. Proof of Lemma 3.7 and Lemma 3.5

The aim of this section is to prove Lemma 3.5 and Lemma 3.7.

The proof of Lemma 3.5 goes as follows: in a similar way to Jeffrey, I construct explicitly a map from $`S^1\times K`$ to the fat realisation of $`BK`$ as a simplicial manifold such that the pull-back of $`EK`$ under this map is the principal bundle $`D_n`$. I then use a result of Shulman to prove Lemma 3.5.

I will start by introducing the simplicial realisations of $`EG`$ and $`BG`$ for any group $`G`$ (see ). Let

$$\mathrm{\Delta }^m=\{(t_0,\mathrm{},t_m)[0,1]^{m+1}\underset{i=0}{\overset{m}{}}t_i=1\}$$

be the standard $`m`$-simplex. The simplicial realisation $`\overline{\mathrm{NG}}`$, respectively $`\mathrm{NG}`$, of $`EG`$, respectively $`BG`$, is given by the contravariant functor

$$\{\mathrm{\Delta }^m,m\}\{\text{category of smooth manifolds}\}$$

which to each $`\mathrm{\Delta }_m`$ associates $`\overline{\mathrm{NG}}(m)=G^{m+1}`$, respectively $`\mathrm{NG}(m)=G^m`$. For $`i`$ between $`0`$ and $`m`$, the map $`\overline{ϵ_i}:\overline{\mathrm{NG}}(m)\overline{\mathrm{NG}}(m1)`$, respectively $`ϵ_i:\mathrm{NG}(m)\mathrm{NG}(m1)`$, corresponding to the $`i`$-th face map $`ϵ^i:\mathrm{\Delta }^{m1}\mathrm{\Delta }^m`$ is given by the omission of the $`i`$-th term

$$\overline{ϵ_i}(k_0,\mathrm{},k_m)=(k_0,\mathrm{},\stackrel{ˇ}{k}_i,\mathrm{},k_m),$$

respectively

(8) $`ϵ_i(k_1,\mathrm{},k_m)`$ $`=`$ $`\{\begin{array}{cc}(k_2,\mathrm{},k_m)\hfill & i=0\hfill \\ (k_1,k_2,\mathrm{},k_ik_{i+1},\mathrm{},k_m)\hfill & i=1,\mathrm{},m1\hfill \\ (k_1,\mathrm{},k_{m1})\hfill & i=m.\hfill \end{array}`$
The projection $`\overline{\mathrm{NG}}(m)\mathrm{NG}(m)`$ is the map

$$q_m(k_0,\mathrm{},k_m)=(k_1k_2^1,\mathrm{},k_{m1}k_m^1).$$

I then take $`EG`$, respectively $`BG`$, to be the fat realisation of $`\overline{\mathrm{NG}}`$, resp. $`\mathrm{NG}`$, that is $`EG`$ is the quotient of $`_m\mathrm{\Delta }^m\times \overline{\mathrm{NG}}(m)`$ by the relation

$$(ϵ^i\times \mathrm{id})(t,x)(id\times \overline{ϵ_i})(tx)$$

for $`(t,x)`$ in $`\mathrm{\Delta }^{m1}\times \overline{\mathrm{NG}}(m)`$ and $`BG`$ is the quotient of $`_m\mathrm{\Delta }^m\times \mathrm{NG}(m)`$ by the relation

$$(ϵ^i\times \mathrm{id})(t,x)(id\times ϵ_i)(tx)$$

for $`(t,x)`$ in $`\mathrm{\Delta }^{m1}\times \mathrm{NG}(m)`$. The projection $`q:EGBG`$ is induced by the maps $`q_m`$. The action of $`G`$ on $`EG`$ is induced by the diagonal multiplication of $`G`$ on the right on $`\overline{\mathrm{NG}}(m)=G^{m+1}`$ for each $`m`$. In fact, there is a second action of $`G`$ on $`EG`$, the covering action, which descends to an action of $`G`$ on $`BG`$. This action on $`EG`$ is induced by the diagonal multiplication on the left of $`G`$ on $`\overline{\mathrm{NG}}(m)=G^{m+1}`$, it descends to an action on $`BG`$ induced by the diagonal conjugation on $`\mathrm{NG}(m)=G^m`$.

Notice that

$$\begin{array}{ccc}\hfill S^1& =& B\hfill \\ \hfill \mathrm{\Sigma }& =& B𝚷\hfill \\ \hfill \mathrm{\Sigma }_0& =& B𝐅.\hfill \end{array}$$

In the simplicial models, the injection of $`\mathrm{\Sigma }_0`$ in $`\mathrm{\Sigma }`$ is given by the projections

$$𝐅^n𝚷^n.$$

The surface $`\mathrm{\Sigma }_0`$ is homotopic to the wedge product of $`2g`$ circles. The inclusion of the $`i`$-th circle $`S^1\mathrm{\Sigma }_0`$ is given by

$$\begin{array}{ccc}^n& & 𝐅^n\\ \lambda & & (x_i^\lambda ,\mathrm{},x_i^\lambda ).\end{array}$$

Let $`R=_{j=1}^g[x_{2j1},x_{2j}]`$ be in $`𝐅`$. The inclusion of $`S^1`$ as the boundary of $`\mathrm{\Sigma }_0`$ is the realisation of the simplicial map

$$\begin{array}{ccc}^n& & 𝐅^n\\ \lambda & & (R^\lambda ,\mathrm{},R^\lambda ).\end{array}$$

The classifying map $`f:S^1\times KBK`$ for the bundle $`D`$ is the realisation of the simplicial map

$$\begin{array}{cccc}f:& ^n\times K& & K^n\\ & (k,\lambda _1,\mathrm{},\lambda _n)& & (k^{\lambda _1},\mathrm{},k^{\lambda _n}).\end{array}$$

The homology of $`S^1`$ is the Eilenberg-Mac Lane group homology $`H_{}()`$ of $``$ (see ). Denote by $`x`$ a generator of $``$. A generator of $`H_1()`$ is given by $`x`$.

Since the centre of $`K`$ is finite, on the one hand $`K`$ and $`K_c`$, and on the other hand $`BK`$ and $`BK_c`$ have naturally isomorphic cohomologies. In addition, every $`K`$-principal bundle defines a $`K_c`$-principal bundle in a natural way: one just has to compose the classifying map of the $`K`$-principal bundle with the projection $`BKBK_c`$. The simplicial version of this last projection is given by the maps $`K^nK_c^n`$. Moreover, the characteristic classes of the induced $`K_c`$-principal bundle are the same as the one of the $`K`$-principal bundle.

The cohomology of $`BK_c`$ is the cohomology of a double complex $`\mathrm{\Omega }^{p,q}=\mathrm{\Omega }^p(\mathrm{NK}_c(q))`$ with two differentials: one is the usual differential of forms $`\mathrm{d}:\mathrm{\Omega }^p(\mathrm{NK}_c(q))\mathrm{\Omega }^{p+1}(\mathrm{NK}_c(q))`$ and the other is

$$\begin{array}{c}\delta :\mathrm{\Omega }^p(\mathrm{NK}_c(q))\mathrm{\Omega }^p(\mathrm{NK}_c(q+1))\\ \delta =_{i=0}^{q+1}(1)^i\epsilon _i^{}\end{array}$$

Recall that the maps $`\epsilon _i`$ were defined in (4). The two differentials $`\mathrm{d}`$ and $`\delta `$ commute and the total differential is $`\mathrm{d}+(1)^p\delta `$ on $`\mathrm{\Omega }^{p,q}`$. Shulman  (see also Bott, Shulman and Stasheff ) proved that each class $`c_j`$ in $`H^{2r_j}(BK_c)`$ can be represented by a form $`c_{j,1}+\mathrm{}+c_{j,r}`$ in $`\mathrm{\Omega }^,`$, with $`c_{j,k}\mathrm{\Omega }^{2rk,k}`$. That this form is closed means that

$$\begin{array}{ccc}\hfill \mathrm{d}c_{j,1}& =& 0\hfill \\ \hfill \delta c_{j,k}& =& (1)^k\mathrm{d}c_{j,k+1}\text{ for }1j<r_j\hfill \\ \hfill \delta c_{j,r}& =& 0.\hfill \end{array}$$

Also, the closed form $`c_{j,1}\mathrm{\Omega }^{2r_j1}(K_c)`$ is a representative of $`b_j`$.

Everything in the above paragraph can be done equivariantly. One just has to replace cohomology by equivariant cohomology, the complex $`\mathrm{\Omega }^{p,q}=\mathrm{\Omega }^p(\mathrm{NK}_c(q))`$ by $`\mathrm{\Omega }_K^{p,q}=\mathrm{\Omega }_K^p(\mathrm{NK}_c(q))`$, the differential $`\mathrm{d}`$ by $`\mathrm{d}_K`$, the forms $`c_j`$ by their respective extensions $`c_j^K`$ in $`H_K^{2r_j}(BK_c)`$, and so on. Hence it is clear that the pairing $`x,f^{}c_j`$ is $`b_j^K`$. This together with the fact that the restriction of $`D`$ to $`S^1`$ is trivial proves Lemma 3.5.

I chose $`c_{j,1}^K`$ as a representative $`\overline{b}_j^K`$ of $`b_j^K`$. The section

$$\begin{array}{cccc}s:& BK& & EK\times _KK\\ & [u]& & [u,1]\end{array}$$

is obtained from the inclusion of the identity $`1`$ into $`K`$ by applying the functor, from $`K`$-spaces to spaces,

$$XX\times _KEK.$$

Because the inclusion map $`\{1\}K`$ is constant and because $`c_{j,1}^K`$ is of odd degree, it follows that $`s^{}b_j^K=s^{}c_{j,1}^K=0`$. This proves Remark 2.5.

The equivariant forms $`c_{j,1}^K`$ and $`c_{j,2}^K`$ satisfy $`\mathrm{d}_Kc_{j,2}^K=\delta c_{j,1}^K`$. A classifying map for the $`K`$-equivariant $`K_c`$-principal bundle $`E`$ is the realisation of the equivariant simplicial map

$$\begin{array}{cccc}\mathrm{\Psi }:& Y_\beta \times \mathrm{\Pi }^n& & K_c^n\\ & (\rho ,p_1,\mathrm{},p_n)& & (\rho (p_1),\mathrm{},\rho (p_n)).\end{array}$$

The homology of $`\mathrm{\Sigma }`$ is the Eilenberg-Mac Lane group homology $`H_{}(𝚷)`$. A generator of $`H_2(𝚷)`$ is (see \[6, Proposition 3.9\])

$$c=\underset{i=1}{\overset{2g}{}}\frac{R}{x_i}x_i,$$

where $`\frac{R}{x_i}`$ is the Fox free differential calculus (see \[6, Section 3\]). In fact,

$$\frac{R}{x_i}=\gamma _j^0\gamma _i^1,$$

where $`\gamma _i^\tau 𝐅`$ is

$$\begin{array}{ccc}\gamma _{2i1}^0& =& _{l=1}^{i1}[x_{2l1},x_{2l}],\\ \gamma _{2i1}^1& =& \gamma _{2i1}^0x_{2i1}x_{2i}x_{2i1}^1,\\ \gamma _{2i}^0& =& \gamma _{2i1}^0x_{2i1},\\ \gamma _{2i}^1& =& \gamma _{2i1}^0[x_{2i1},x_{2i}].\end{array}$$

A representative $`\overline{a}_j^{}`$ of $`a_j^{}`$ is given by

$$\begin{array}{ccc}\hfill \overline{a}_j^{}& =& _{i=1}^{2g}\frac{R}{x_i}x_i,\mathrm{\Psi }^{}c_{j,2}^K\hfill \\ & =& _{i=1}^{2g}_{\tau =0,1}(1)^\tau \gamma _i^\tau x_i,\mathrm{\Psi }^{}c_{j,2}^K\hfill \\ & =& _{i=1}^{2g}_{\tau =0,1}(1)^\tau (\mathrm{ev}_{\gamma _i^\tau }\times \mathrm{ev}_{x_i})^{}c_{j,2}^K,\hfill \end{array}$$

where, for $`p𝐅`$, the evaluation map is

$$\begin{array}{cccc}ev_p:& \mathrm{Hom}(𝐅,K_c)& & K_c\\ & \rho & & \rho (p).\end{array}$$

The last line of the above computation of $`\overline{a}_j^{}`$ clearly shows that $`\overline{a}_j^{}`$ extends to a form on $`K^{2g}`$. The differential of this form is

(9) $`\mathrm{d}\overline{a}_j^{}`$ $`=`$ $`{\displaystyle \underset{i=1}{\overset{2g}{}}}{\displaystyle \underset{\tau =0,1}{}}(1)^\tau (\mathrm{ev}_{\gamma _i^\tau }\times \mathrm{ev}_{x_i})^{}\mathrm{d}c_{j,2}^K`$
$`=`$ $`{\displaystyle \underset{i=1}{\overset{2g}{}}}{\displaystyle \underset{\tau =0,1}{}}(1)^\tau (\mathrm{ev}_{\gamma _i^\tau }\times \mathrm{ev}_{x_i})^{}\delta c_{j,1}^K`$
$`=`$ $`{\displaystyle \underset{i=1}{\overset{2g}{}}}{\displaystyle \underset{\tau =0,1}{}}(1)^\tau (\mathrm{ev}_{\gamma _i^\tau }\times \mathrm{ev}_{x_i})^{}{\displaystyle \underset{l=0}{\overset{2}{}}}(1)^l\epsilon _l^{}c_{j,1}^K`$
$`=`$ $`{\displaystyle \underset{i=1}{\overset{2g}{}}}{\displaystyle \underset{\tau =0,1}{}}{\displaystyle \underset{l=0}{\overset{2}{}}}(1)^{\tau +l}(\epsilon _l(\mathrm{ev}_{\gamma _i^\tau }\times \mathrm{ev}_{x_i}))^{}c_{j,1}^K`$
$`=`$ $`{\displaystyle \underset{i=1}{\overset{2g}{}}}{\displaystyle \underset{\tau =0,1}{}}{\displaystyle \underset{l=0}{\overset{2}{}}}(1)^{1+\tau +l}\mathrm{ev}_{z_{i,l}^\tau }^{}c_{j,1}^K,`$
where

$$z_{i,0}^\tau =x_i,z_{i,1}^\tau =\gamma _i^\tau x_i\text{ and }z_{i,2}^\tau =\gamma _i^\tau .$$

Because

$$\begin{array}{ccc}\hfill \mathrm{ev}_{z_{i,0}^0}^{}& =& \mathrm{ev}_{z_{i,0}^1}^{}\hfill \\ \hfill \mathrm{ev}_{z_{2i,1}^1}^{}& =& \mathrm{ev}_{z_{2i1,2}^1}^{}\hfill \\ \hfill \mathrm{ev}_{z_{2i1,1}^0}^{}& =& \mathrm{ev}_{z_{2i,2}^0}^{}\hfill \\ \hfill \mathrm{ev}_{z_{2i,1}^0}^{}& =& \mathrm{ev}_{z_{2i1,1}^1}^{}\hfill \\ \hfill \mathrm{ev}_{z_{2i+1,2}^0}^{}& =& \mathrm{ev}_{z_{2i,2}^1}^{}\hfill \end{array}$$

many terms cancel each other in the expression (9) above. I am left with

$$\mathrm{d}\overline{a}_j^{}=\mathrm{ev}_{z_{2g,2}^1}^{}c_{j,1}^Kev_{z_{1,2}^0}^{}c_{j,1}^K.$$

But $`z_{1,2}^0=1`$ the identity of $`𝐅`$ and hence $`ev_{z_{1,2}^0}`$ is a constant map, whereas $`z_{2g,2}^1=_{j=1}^g[x_{2j1},x_{2j}]`$ and hence $`\mathrm{ev}_{z_{2g,2}^1}^{}=\mathrm{\Phi }^{}`$. Since $`c_{j,1}^K`$ is a representative of $`b_j^K`$, I deduce that on $`K^{2g}`$

$$\mathrm{d}\overline{a}_j^{}=\mathrm{\Phi }^{}\overline{b}_j^K.$$

This proves Lemma 3.7.


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# Low temperature magnetic phase diagram of the cubic non-Fermi liquid system CeIn3-xSnx

## 1 Introduction

The classical description of heavy fermion (HF) metals in terms of a “Fermi liquid” of quasiparticles with a large renormalized mass fails in several Ce, Yb and U systems. During the last decade, many examples of “non-Fermi liquid” (NFL) behaviour have been identified by the anomalous dependences of the low temperature thermodynamic and transport properties. Different scenarios have been proposed for these NFL effects, in particular the case of NFL associated to a quantum critical point (QCP) is nowadays the subject of intensive research, both experimental Stewart01 ; Lohneysen99 ; Steglich00  and theoretical Si01 ; Coleman02 .

A quantum critical point is a singularity in the phase diagram where a second order phase transition is driven to zero temperature by means of a non-thermal control parameter such as pressure, magnetic field or alloying. In HF systems, the QCP results from the competition of the Kondo effect (the screening of local magnetic moments by conduction electrons) and the RKKY interaction between neighboring magnetic moments.Continentino00  The nature of the QCP is a subject of current discussion, but in any case a strong influence of the dimensionality of the spin-fluctuations is expected.Si01  This raises the question of the influence that structural symmetry may have on NFL behaviour.

At present, most of the systems that have been thoroughly investigated in connection with a QCP have tetragonal or lower structural symmetry, and thus, an intrinsic structural anisotropy. In order to avoid this constraint a cubic system should be studied. To our knowledge, no cubic doped system has been studied yet in this context. Because of its FCC structure, CeIn3-xSnx, with a cubic symmetry at the Ce site, can be considered an excellent candidate. Previous research has shown that the antiferromagnetic (AF) order present in CeIn3 at $`T_\mathrm{N}=10.2`$K drops to zero with Sn doping (increasing $`x`$), and $`T_\mathrm{N}`$ was predicted to disappear near $`x_\mathrm{c}0.4`$.Lawrence79  Furthermore, resistivity measurements performed on stoichiometric CeIn3 under pressure reveal NFL behaviour with a non-quadratic temperature dependence of the resistivity ($`\mathrm{\Delta }\rho T^{1.6}`$) close to the critical pressure $`p_\mathrm{c}26`$ kbar where the ordering temperature extrapolates to zero.Mathur98 ; Knebel01

In two short conference contributions Pedrazzini02 ; Pedrazzini03  we have presented low temperature specific heat and resistivity results of our research on CeIn3-xSnx for $`x1`$. Those preliminary results relocate the critical concentration at $`x_\mathrm{c}0.65`$ and show evidence of NFL behaviour and a complex magnetic phase diagram. In this work we present more detailed information on structural, magnetic, transport and thermal measurements around the QCP and we extend the previous study to the non-ordered region of the phase diagram.

## 2 Experimental details and Results

Eighteen polycrystalline samples covering the full concentration range were prepared by arc melting the proper amounts of pure elements in an Argon atmosphere. The starting materials were Ce of grade 5N and In and Sn of grade 6N. In order to insure homogeneity, the resulting buttons were flipped over and remelted several times. At the end of this process the mass loss was found to be negligible (below 0.2 wt.%). Samples were annealed at $`700^\mathrm{o}`$C for 24 hours and then slowly cooled down to $`500^\mathrm{o}`$C within 80 hours. Powder X-ray diffraction confirmed the FCC AuCu3 type structure of all samples and revealed no signs of secondary phases. The magnetic dc-susceptibility ($`\chi `$) was measured between 2 K and 300 K in a commercial SQUID magnetometer under a magnetic field $`H=10`$kOe. Electrical resistivity ($`\rho `$) was measured with the conventional four-contact technique with a Linear Research LR-700 resistance bridge in the 0.5–300 K temperature range. At low temperature ($`T<6`$K) a small (extrinsic) superconducting signal was suppressed by an $`H=10`$kOe magnetic field (this is probably due to tiny amounts of In–Sn segregation at the surface and grain boundaries of the samples Sakurai84Chem ). Specific heat ($`C_\mathrm{P}`$) measurements were performed in a He3 quasiadiabatic calorimeter by the usual heat-pulse technique, between 0.45 K and 20 K.

The lattice parameters of some of the samples are presented in Fig. 1 together with the crystallographic data previously reported in the literature.Lawrence79 ; Maury82 ; Sakurai84  The lattice parameter ($`a`$) of the AuCu3-cubic structure increases monotonously with increasing $`x`$. Between $`x=0`$ and $`x2`$ the data follow the expected Vegard law extracted by comparison between the LaIn3 and LaSn3 lattice parameters. However, a clear deviation from a straight line occurs for $`x>2.2`$. Such a deviation is associated to a change of the Ce-valence on the Sn rich side due to the reduction of the Ce-$`4f`$-level occupancy from $`n_f=1`$ (CeIn3) to $`n_f<1`$ (CeSn3).Lawrence79

The magnetic susceptibility is employed to follow the ordering transition (at low $`x`$) and to study the formation of the intermediate valence (IV) state (for $`x>2`$). Our $`\chi (T)`$ data are plotted in Fig. 2 along with the data of pure CeSn3 (taken from Ref. Sereni80 ). Within our experimental range ($`T2`$K), the AF transition can be observed for $`x<0.45`$. At this Sn concentration, $`x=0.45`$, $`\chi _{2\mathrm{K}}(x)\chi (T=2\mathrm{K},x)`$ reaches its maximum value and then it rapidly decreases for $`x>0.6`$, as shown in the inset of Fig. 2. This decrease is not monotonous because $`\chi _{2\mathrm{K}}`$ shows a weak increase at $`x=2.0`$ with respect to the neighbouring samples ($`x=1.5`$ and 2.5, see the inset of Fig. 2). A weak shoulder around 50 K is observable at low Sn concentration, which becomes more pronounced for the $`x=0.5`$ and $`0.6`$ samples. This deviation from the Curie-Weiss law, already observed below 100 K, is related to the thermal depopulation of the quartet ($`\mathrm{\Gamma }_8`$) excited level. Eventually, the shoulder evolves into a broad maximum centered at $`T_{max}^\chi 40`$K for $`x1`$. Coincidentally with the deviation of the unit-cell volume ($`V`$) from Vegard’s law at $`x2`$, $`T_{max}^\chi `$ shifts to higher temperature for $`x>2`$, indicating the increase of the $`4f`$-conduction state hybridization strength. Once its value exceeds the crystal-field splitting, the system behaves like an IV system, as in pure CeSn3 where $`T_{max}^\chi 140`$ K. Our $`\chi (T)`$ results are in good agreement with those reported in the literature for $`T>10`$K.Dijkman80

Figure 3 displays the electrical resistivity of the studied samples in a logarithmic $`T`$ scale. For the sake of clarity, the data is normalized as $`(\rho (T)\rho _{170\mathrm{K}})/(\rho _{70\mathrm{K}}\rho _{170\mathrm{K}})`$ for $`x0.7`$ in Fig. 3-a, and as $`\rho (T)/\rho _{280\mathrm{K}}`$ for $`x1`$ in Fig. 3-b. The most prominent features extracted from these measurements are: i) the magnetic transition observed in the $`0x<0.6`$ range; ii) a maximum in $`\rho (T)`$ at $`T_{max}^\rho `$ which decreases from 55 K at $`x=0`$ down to 20 K at $`x=0.45`$, and then increases for $`x>0.7`$; iii) a minimum at $`T200`$ K resulting from the decrease of the electron-electron scattering and the increase of electron-phonon scattering as the temperature increases.

As shown in Fig. 3-a, the resistivity of the samples with $`x0.7`$ merges in a common $`\rho (T)`$ dependence at high temperature. Furthermore, such a common temperature dependence extends between $`T_{max}^\rho =20`$K and nearly room temperature for the samples with $`x0.45`$. This fact points to common scattering mechanisms within this range of concentration. At low temperature, the AF transition is characterized by a negative $`\rho (T)`$ slope in a temperature range around $`T_\mathrm{N}`$, followed by the typical decrease in the ordered phase. This effect becomes much weaker at $`x=0.25`$, and is dominated by a sudden drop due to another transition occuring at $`T=T_\mathrm{I}`$ in the $`x=0.3`$, $`0.37`$, $`0.41`$ and $`0.45`$ samples. The observation of both a hysteresis in $`\rho (T)`$ and a peak-like anomaly in $`C_\mathrm{P}(T)`$ have led us to conclude that a first order phase transition occurs at $`T_\mathrm{I}`$.Pedrazzini03  This phase transition is no longer detected in the $`x=0.5`$ sample within our experimental temperature window ($`T>0.5`$K). Instead, a continuous increase in $`\rho (T)`$ is found down to the lowest temperature, which we again associate to an AF ordering. This behaviour, observed in the resistivity around $`T_\mathrm{N}`$ in the $`0.15x0.5`$ concentration range, can be ascribed to the opening of the superzone gap due to the AF order, as reported e.g. in CeSbNiy.Kim01  For $`x=0.6`$ and $`0.7`$, $`\rho (T)`$ decreases monotonously with $`T`$ from their common maximum at 20 K, with a clear sub-quadratic power law behaviour: $`\rho (T)=\rho _0+AT^n`$, with $`n<1.5`$. Resistivity measurements performed down to the milikelvin range confirm an exponent $`n1`$ for the sample with $`x=0.7`$.Custers03

At higher Sn concentration the $`\rho (T)`$ maximum at $`T_{max}^\rho `$ shifts again to a higher temperature, with $`T_{max}^\rho =30`$K for $`x=1`$. No maximum is observed in the samples with $`x=2`$, 2.5 and 3 (see Fig. 3-b), though it appears at a higher temperature once the phonon contribution is substracted. The evolution of $`\rho (T)`$ is clearly broken at $`x=1.5`$, where $`\rho (T)`$ has a monotonous negative slope in the whole temperature range. This unexpected behaviour for a Ce-lattice system was previously reported in the literature at this concentration,Sakurai84 ; Elenbaas80  although in a smaller temperature range that did not include the low temperature saturation value.

The electronic contribution to the specific heat of the alloys included in the antiferromagnetic region (i.e. $`x0.7`$) is depicted in Fig. 4 in a logarithmic $`T`$ scale after phonon subtraction. The $`x=0.15`$ sample shows a jump in $`C_{\mathrm{el}}(T)`$ at the Néel temperature: $`\mathrm{\Delta }C_{\mathrm{el}}(T_\mathrm{N})12`$J/mol K2, as expected for a mean-field like transition. As $`x`$ increases, the transition first broadens (for $`x=0.25`$, 0.3 and 0.37) and then (for $`x=0.41`$, $`0.45`$, $`0.47`$, $`0.5`$ and $`0.55`$) $`\mathrm{\Delta }C_{\mathrm{el}}`$ becomes sharper again, being much smaller and followed at $`T>T_\mathrm{N}`$ by a nearly logarithmic tail. At $`x=0.6`$ no transition is observed within our accessible temperature range. However, $`C_{\mathrm{el}}(T)`$ measurements performed down to lower temperature confirm the existence of a transition at $`T_\mathrm{N}=0.40`$K,Custers03  with similar characteristics to those observed in the $`x=0.55`$ sample. Above $`T_\mathrm{N}`$, the $`x=0.6`$ sample displays a logarithmic $`C_{\mathrm{el}}(T)`$ dependence within more than a decade of temperature, which can be described by the function $`C_{\mathrm{el}}(T)/T=0.50\mathrm{log}(16/T)`$J/mol K2. A similar type of behaviour has been observed in other cerium systems, in particular in the doping-induced NFL CeCu6-yAuy (see for example references Lohneysen99  and Sereni02 ). The $`x=0.7`$ sample also shows a logarithmic $`T`$ dependence, although $`C_{\mathrm{el}}(T)/T`$ flattens at low temperature. Specific heat measurements presented in Ref. Custers03  show that this curvature extends down to lower temperature with a $`C_{\mathrm{el}}(T)/T\gamma _0b\sqrt{T}`$ dependence (after the substraction of a hyperfine nuclear contribution due to In). This behaviour is expected for a three dimensional antiferromagnet.Moriya95  We also include in Fig. 4 the $`C_{\mathrm{el}}(T)`$ results for the $`x=1`$ sample, which show a drastic decrease of $`C_{\mathrm{el}}/T(T0)`$. Using a Kondo-impurity model,Desgranges82  the $`\gamma `$ value extracted from this measurement corresponds to $`T_\mathrm{K}=45`$K.

The specific heat data of the samples with $`x1`$ are presented in Fig. 5, together with the data corresponding to the LaIn2Sn sample which serves as phonon reference in this concentration range. The low temperature $`C_\mathrm{P}/T`$ values of these samples are strongly reduced when compared to those in the In-rich region. There is also a flattening of the curves at low temperatures, indicating the recovery of Fermi-liquid behaviour. However, a weak increase of $`C_\mathrm{P}(T)/T`$ is still present in the $`x=1`$ sample below 5 K. The Sommerfeld coefficient in this region has a maximum value at $`x=2`$, where it reaches $`\gamma =270`$mJ/mol K2, and then decreases monotonously down to 73 mJ/mol K2 for CeSn3.Ikeda82  These results are in agreement with the $`\gamma `$ values reported in the literature,Elenbaas80  though no $`C_\mathrm{P}(T)/T`$ dependences were given there.

## 3 Discussion

These experimental results indicate that the CeIn3-xSnx cubic-binary system is suitable for a detailed study of a magnetic to non-magnetic transformation which involves a quantum critical point. Because of the variety of properties to be considered, we will first discuss the high temperature results and low temperature ones will be discussed in the second part of this section.

Previous research performed by neutron scattering has shown that a precise estimation of the crystalline field splitting is difficult in this system because In is a strong neutron absorber which makes experiments rather difficult.Loewenhaupt  Taking profit of the simple CF level scheme of a cubic system, we can use our $`\chi (T)`$ data to estimate the crystal field splitting $`\mathrm{\Delta }_{\mathrm{CF}}`$ between the $`\mathrm{\Gamma }_7`$ doublet ground state (GS) and the excited $`\mathrm{\Gamma }_8`$ quartet by fitting the measurements in the low-$`x`$ samples. In this fitting, we take into account the effects of a molecular field by introducing a $`\lambda `$-parameter and a temperature independent non-$`4f`$ contribution $`\chi _0`$:

$$\chi (T)=\frac{\chi _{\mathrm{CF}}(T)}{1+\lambda \chi _{\mathrm{CF}}(T)}+\chi _0.$$
(1)
In this equation $`\chi _{\mathrm{CF}}(T)`$ corresponds to Van Vleck’s formula, which in a cubic symmetry is a function of a single parameter, $`\mathrm{\Delta }_{\mathrm{CF}}`$.Lueken79  By fitting the data of several samples above $`10`$K, we have calculated a mean value for the splitting: $`\mathrm{\Delta }_{\mathrm{CF}}=130`$K, which coincides with the result of neutron scattering experiments performed on CeIn3 ($`\mathrm{\Delta }_{\mathrm{CF}}12\mathrm{meV}=130`$K Murani93 ).

The evolution of $`\chi (T)`$ with Sn concentration (see Fig. 2) can be separated into three regions. One close to $`x=0`$, where $`\chi (T)`$ is well described by equation 1. Already at $`x=0.7`$ it is not possible to fit the $`\chi (T)`$ data with such a simple expression, probably due to the effect of the increasing Kondo temperature. In the intermediate region ($`0.7<x<2`$) the magnetic susceptibility $`\chi _{2\mathrm{K}}`$ drops down from its maximum at $`x=0.45`$ ($`\chi _{2\mathrm{K}}17\times 10^3`$emu/mol) by around 50% due to a reduction of the moment of the Ce-doublet ground state ($`\mathrm{\Gamma }_7`$). This crossover region ends with a weak increase of $`\chi _{2\mathrm{K}}(x)`$ at $`x=2`$. The concentration at which this relative maximum occurs coincides with the already quoted deviation of $`V(x)`$ from a linear behaviour (Vegard law), with the observation of a maximum in the $`\gamma (x)`$ dependence and with the beginning of a strong growth of $`T_{\mathrm{max}}^\chi `$. All these features have been related to a strong increase of hybridization effects as the system approaches the unstable valence state.Sereni95

Concerning the resistivity measurements, the continuous reduction of $`T_{\mathrm{max}}^\rho `$ between CeIn3 and $`x0.37`$, from $`55`$K down to $`20`$K, indicates a decrease of the temperature at which the coherence sets in. This strong decrease cannot be attributed to a reduction of the $`4f`$-conduction state hybridization because the Kondo temperature $`T_\mathrm{K}`$ (extracted from the entropy evolution, see below) increases, nor to a change in the crystal field splitting which would have to decrease by a $`2.5`$ factor between $`x=0`$ and $`0.37`$. This reduction of $`T_{\mathrm{max}}^\rho (x)`$ close to the stoichiometric compound could be produced by the disorder introduced in the alloying process, though it becomes concentration independent in the range $`0.37x0.7`$. At higher Sn concentration, $`T_{max}^\rho `$ increases indicating a steeper increase of $`T_\mathrm{K}`$.

From the low temperature resistivity measurements, one observes that the $`\mathrm{\Delta }\rho =AT^2`$ dependence is not detected above the critical concentration ($`x_\mathrm{c}0.7`$) within our experimental temperature range. This sub-quadratic power law behaviour of the resistivity is broken at $`x=1.5`$, with a low temperature $`\mathrm{\Delta }\rho (T)=\rho _0[1(T/T_\mathrm{K})^2]`$ dependence which indicates an impurity (instead of a lattice) behaviour of the magnetic moments. The $`T_\mathrm{K}50`$K value extracted from this formula is comparable to the one extracted for the $`x=1`$ sample (see the discussion of the entropy results in the following paragraph). However, in the high temperature region, the expected $`\rho (T)\mathrm{log}(T)`$ is not strictly observed, probably due to the crystal field excited level and phonon contributions. Although the low temperature coherent regime is recovered for $`x>1.5`$, it is only at $`x=3`$ where the $`T^2`$ dependence is clearly observed at least up to $`40`$K with $`A=1.6\times 10^3\mu \mathrm{\Omega }\mathrm{cm}/\mathrm{K}^2`$. The $`n<2`$ exponent observed in the resistivity for $`x>x_\mathrm{c}`$ may be due to the doping-induced disorder. However, we stress that the $`n1`$ exponent observed for $`xx_\mathrm{c}`$ should be associated to an intrinsic feature around the antiferromagnetic QCP, since the $`\mathrm{\Delta }\rho T^2`$ temperature dependence is recovered under applied magnetic field.Custers03

The evolution of the entropy with increasing concentration provides valuable information on the variation of the low energy spectrum of excitations along the phase diagram. The entropy gained by the electronic system ($`S_{\mathrm{el}}(T)`$) is plotted in Fig. 6 for the samples with $`x1`$. At low Sn concentration the transition at $`T_\mathrm{N}`$ results in a change of slope of $`S_{\mathrm{el}}(T)`$, as expected for a second-order phase transition. For $`x=0.15`$, the entropy above $`T_\mathrm{N}=9.1`$K is $`S_{\mathrm{el}}(T_\mathrm{N},x=0.15)=0.8\mathrm{R}\mathrm{ln}(2)`$. This value can be compared with $`S_{\mathrm{el}}(T_\mathrm{N},x=0)0.87\mathrm{R}\mathrm{ln}(2)`$, given for CeIn3 in Ref. Elenbaas80 . These results confirm that the doublet $`\mathrm{\Gamma }_7`$ is involved in the magnetic order, lying well below the $`\mathrm{\Gamma }_8`$ quartet. The deviation of the calculated entropy when compared to the expected value ($`\mathrm{R}\mathrm{ln}2`$) is probably due to a weak Kondo effect. As $`x`$ increases, less entropy is collected at some fixed temperature, meaning that the characteristic Kondo temperature is increasing. To estimate the evolution of $`T_\mathrm{K}(x)`$ we have calculated $`\mathrm{\Delta }S_{\mathrm{el}}^{12\mathrm{K}}S_{\mathrm{el}}(T=12\mathrm{K})`$, plotted in the inset of Fig. 6. Between $`x=0.15`$ and $`x=1`$ this quantity diminishes continuously from $`0.87\mathrm{R}\mathrm{ln}(2)`$ down to $`0.33\mathrm{R}\mathrm{ln}(2)`$. By means of a Kondo impurity model Desgranges82  $`T_\mathrm{K}(x)`$ can be computed. We found that $`T_\mathrm{K}(x=0.15)3`$K and $`T_\mathrm{K}(x=1)45`$K. The value $`\mathrm{\Delta }S_{\mathrm{el}}^{12\mathrm{K}}`$ for $`x=1.5`$ (also included in the inset of Fig. 6), corresponds to $`T_\mathrm{K}(x=1.5)40`$K. This value almost coincides with the Kondo temperature extracted from the fitting of the low temperature resistivity data. Such a constant behaviour of $`T_\mathrm{K}`$ between $`x=1`$ and $`x=1.5`$ is not expected within the Doniach diagram, where $`T_\mathrm{K}`$ rises exponentially with increasing hybridization. At that concentration, the eventual contribution of the excited quartet $`\mathrm{\Gamma }_8`$ may explain this “anomalous” evolution of $`T_\mathrm{K}`$.

The $`T_\mathrm{N}(x)`$ dependence we observe indicates that the antiferromagnetic order disappears at a quantum critical point near $`x0.7`$. However, instead of a monotonous trend with negative curvature, our results indicate a complex behaviour around $`x0.3`$ (see Fig. 7). This change of regime is reflected in the specific heat as a deviation of $`\mathrm{\Delta }C_{\mathrm{el}}(T_\mathrm{N})`$ from a mean field type behaviour and the formation of a long $`C_{\mathrm{el}}/T`$ tail at $`T>T_\mathrm{N}`$. The broadening of the $`C_{\mathrm{el}}(T)`$ anomaly around $`T_\mathrm{N}`$ can be characterized by comparing the temperatures $`T_{\mathrm{max}}(x)T_\mathrm{N}(x)`$, at which $`C_{\mathrm{el}}/T`$ has its maximum, and $`T_{\mathrm{slope}}(x)T_\mathrm{N}(x)`$ where the largest (negative) slope of $`C_{\mathrm{el}}/T`$ is detected, see Fig. 7. Above $`x=0.41`$, $`T_\mathrm{N}(x)`$, $`T_{\mathrm{max}}(x)`$ and $`T_{\mathrm{slope}}(x)`$ merge again, decreasing linearly down to $`T_\mathrm{N}=0.1`$ at $`x=0.65`$. The new information obtained from the present study, together with the low temperature data from reference Custers03 , relocate the critical concentration around $`x_\mathrm{c}0.7`$ instead of $`x=0.4`$, extrapolated by J. Lawrence from higher temperatures.Lawrence79

In coincidence with the change of regime near $`x=0.3`$, a second transition (in this case, with first order character) develops at $`T_\mathrm{I}<T_\mathrm{N}`$ within the $`0.30x0.45`$ range. The temperature $`T_\mathrm{I}`$ evolves in a non-monotonous manner: it increases up to 2.1 K for $`x=0.37`$ (almost merging the $`T_{\mathrm{max}}(x)`$ curve) and then it decreases down to $`T_\mathrm{I}(x=0.45)0.8`$K at $`x=0.45`$. No signs of $`T_\mathrm{I}`$ where found in the $`x=0.47`$ sample within our temperature range. The merging of both transition lines around $`x=0.4`$ raises the possibility of a tetracritical point around this concentration as discussed in Ref. Pedrazzini03 .

The change of the $`T_\mathrm{N}(x)`$ dependence at $`x0.4`$ could be related to the onset of NFL behaviour, clearly before reaching the critical concentration. Such a behaviour is reflected in the almost logarithmic tail of the specific heat, in the drastic change of the $`C_{\mathrm{el}}/T`$ anomaly associated to the AF order and in the onset of a linear dependence of $`T_\mathrm{N}(x)`$. Whether the simultaneous observation of a first order transition is related to this fact cannot be established with the available experimental data.

The effect of Sn doping on CeIn3 is to be contrasted with that produced by hydrostatic pressure, $`p`$. Although in both cases the weakening of the $`4f`$ moments with increasing control parameter ($`p`$ or $`x`$) is observed, the unit-cell volume $`V(p)`$ and $`V(x)`$ have opposite slopes. This fact implies that Sn doping substantially modifies the electronic structure of CeIn3 as the electron-count changes. As a consequence, both phase diagrams show striking differences besides a continuous reduction of $`T_\mathrm{N}`$: no evidence of superconductivity appears in the alloy despite the low temperature to which $`T_\mathrm{N}`$ was detected. On the other hand, the first order transition at $`T=T_\mathrm{I}`$ has not been observed in CeIn3 under pressure. Moreover, the features observed in $`\rho (T)`$ around $`T_\mathrm{N}`$ or the exponent of the $`\rho (T)T^n`$ dependence close to the critical region are quite different when controlling the two different parameters.Knebel01

## 4 Conclusions

This study shows that the low temperature magnetic phase diagram of CeIn3-xSnx is much richer than expected from previous works. Although the ordering temperature decreases continuously with increasing Sn content towards $`T_\mathrm{N}=0`$K at $`x_\mathrm{c}0.7`$, the evolution of the antiferromagnetic state is not monotonous. Instead, our results indicate that around $`x0.4`$ there are clear changes in the concentration dependencies of the ordering temperature, specific heat anomaly and electrical resistivity. Those changes also affect the paramagnetic phase, where the logarithmic behaviour $`C_{\mathrm{el}}/T\mathrm{log}(T)`$ at $`T>T_\mathrm{N}(x)`$ extends even above the Néel temperature of stoichiometric CeIn3, $`T_\mathrm{N}(x=0)=10`$K. For $`x>0.4`$, $`T_\mathrm{N}(x)`$ decreases linearly down to $`T_\mathrm{N}=0.4`$K at $`x=0.6`$. The decrease of $`T_\mathrm{N}(x)`$ over more than an order of magnitude in temperature (i.e., from 10 K down to 0.4 K), exceeds the temperature range of $`T_\mathrm{N}(p)`$ observed in stoichiometric CeIn3 under hydrostatic pressure.Knebel01 ; Kawasaki02  To our knowledge, the decrease of $`T_\mathrm{N}`$ in such an extended temperature range has not previously been reported. This fact indicates that in CeIn3-xSnx the disorder introduced by doping is not the dominant factor in the evolution of the characteristic parameters such as the magnetic exchange or the Kondo screening. As a consequence, the CeIn3-xSnx phase diagram up to $`x=1`$ can be described within the Doniach scheme.

Due to the cubic point symmetry at the Ce site, this research proves that structural anisotropy is not determinant for the appearance of NFL behaviour. In spite of this, the $`T`$ dependences observed in this research (almost linear $`\rho (T)`$ and logarithmic $`C_{\mathrm{el}}/T`$ for $`T>0.4`$K) would imply a low dimensional scenario for this NFL. Eventhough the low temperature measurements suggest the expected $`C_{\mathrm{el}}/T\sqrt{T}`$ at lower temperatures, the $`\rho (T)T`$ observed in Ref. Custers03  differs with the temperature dependence expected by current models for a three dimensional antiferromagnet.

Around $`x=2`$, the anomalous concentration dependence of the lattice parameter, of $`\chi _{2\mathrm{K}}`$ and $`C_{\mathrm{el}}/T`$ (at $`T=0.5`$K) can be explained by a non-monotonous evolution of the hybridization strength with concentration as suggested in Ref. Lawrence79 , and by the evolution of the system towards the formation of the IV state.Sereni95  In this limit the ground state degeneration is expected to involve the six fold $`J=5/2`$ level. Further progress on the knowledge of the nature of the AF phase close to the critical concentration and the phase formed below $`T_\mathrm{I}`$ requires microscopic measurements, which are presently under way.

###### Acknowledgements.

This work was supported by a DAAD (Germany) and F. Antorchas (Argentina) cooperation program (Pr. Nr. 13740/1-88). The authors P. P., M. G. B. and J. G. S. are affiliated to CONICET.


text:
# Magnetic fluctuations in frustrated Laves hydrides R(Mn1-xAlx)2Hy

## I Introduction

There is now a growing interest in studying magnetic fluctuations in the paramagnetic phase of strongly correlated electron systems. An original behavior in the dynamical susceptibility, where the magnetization density does not follow the single exponential decay predicted by Landau-Fermi theory is often observed. In itinerant magnets, non Fermi-liquid behavior is often associated with temperature anomalies of the thermodynamical properties, like specific heat and resistivity. In Heavy-Fermions and superconductors, it could be the precursor a quantum phase transition around zero temperature.

In paramagnets with localized spins, a non Fermi liquid behavior of the dynamical susceptibility could be also expected due to strong magnetic disorder, since magnetic inhomogeneities associated with disorder and frustration yield a distribution of relaxation times. However, in usual spin glasses with localized spins, although such distribution indeed exists, the excitation spectrum in the paramagnetic phase usually remains much narrower than in itinerant magnets, yielding typical energies of the fluctuating spins below 1 meV.

The intermetallic Laves compounds RMn2 have two main characteristics : i) they are at the frontier between localized and itinerant magnetism, the instability of the Mn spins being governed by the distance between first neighbor Mn pairs, and ii) they show a topological frustration of the pyrochlore Mn lattice for antiferromagnetic first neighbor Mn-Mn interactions. When R is a magnetic rare earth, the diamond-like R lattice interacts with the frustrated Mn lattice. Varying Mn-Mn interatomic distance d allows one to encompass the critical distance d0 between localized and itinerant Mn magnetism. For d $`>`$ d0, spontaneous Mn moments are present and the frustrated Mn-Mn interactions dominate, whereas for d $`<`$ d0 Mn moments are induced by rare earth moments and the topological frustration is suppressed. Changing interatomic distances is realized by chemical substitution or by applying pressure .

Introducing hydrogen in interstitial sites also modifies the magnetic properties . In Laves compounds, hydrogen expands the lattice, favoring the localization of the Mn moments, but also modifies the frustration by making Mn-Mn interactions nonequivalent. Therefore, ordered H atoms release the topological frustration, yielding long range ordered magnetic structures . On the other hand, H disorder induces a random variation of the exchange interactions and therefore magnetic disorder.

In Y(Mn1-xAlx)2Hy and Y(Mn1-xFex)2Hy, we studied such phases by magnetic neutron diffraction. Surprisingly, and in contrast with usual spin glasses, we found that these disordered magnetic phases combine short spin correlation lengths (around 10-20 Å) with high transition temperatures (100-250 K), in the same range as in the ordered parent compound. The behavior of the short range order parameter was intermediate between that expected for a canonical Edwards-Anderson spin glass, and the Brillouin curve for a non frustrated magnet.

Up to now the study of the spin fluctuations and magnetic transition in such topologically disordered phases has received little attention. A previous study of Y(Mn0.9Al0.1)2 single crystal by inelastic neutron scattering , where interatomic Mn distances are close to the instability threshold, revealed very interesting features with regards to canonical spin glasses. Namely, it pointed out the existence of a large energy range of the magnetic fluctuations (up to about 40 meV), well above the typical fluctuation energy in spin glasses, and close to that observed in other itinerant magnets . This large energy range was attributed to the influence of both topological frustration and itinerant character of the Mn moments, without any way to clear up their respective roles.

Studying the magnetic excitations yields precious information about the microscopic nature of the magnetic ground state and ordering transition. Especially, it could help to explain why the transition temperature remains high in spite of the strong disorder. Inelastic neutron scattering is the most straightforward way to probe such excitations. We have studied the spin fluctuations in R(Mn1-xAlx)Hy compounds (R = Y or Tb) by time of flight neutron scattering, together the steady-state correlations by neutron diffraction, and the low field susceptibility by static magnetization measurements. In all compounds, H disorder was achieved by substituting a small amount of Al on the Mn sites. By choosing appropriate compounds, we checked the influence of magnetic moments on the R sites, hydrogen concentration and hydrogen disorder. The results suggest an original picture of a ‘cluster glass’ magnetic state.

## II Sample description

Powdered samples of R(Mn1-xAlx)2Dy, with (R = Y, Tb), Al content $`x`$=0.09, and different deuterium contents were prepared using the technique described in Ref. , and characterized by X-ray diffraction. All samples showed a single chemical phase, besides a very small amount of RH3 impurity phase in some cases. We mostly studied three disordered samples, Tb(Mn0.9Al0.1)2Dy, ($`y`$=1 and $`y`$=4), and Y(Mn0.9Al0.1)2Dy ($`y`$=4). Exact D contents are given in Table I. In most cases, the deuterium isotope was chosen instead of hydrogen to decrease the incoherent background. The small Al content induces hydrogen disorder and breaks down the long range magnetic order . The Tb ion with high magnetic moment yields a strong enhancement of the magnetic fluctuations (by about a factor 10), yielding an excellent precision on the lineshape of the dynamical susceptibility. The influence of this second magnetic ion on the spin correlations and spin dynamics was checked in comparison with Y(Mn0.9Al0.1)2D4 where Y is non magnetic. The amount of hydrogen (or deuterium) introduced ($`y`$=1 or $`y`$=4) allows to vary interatomic distances in a large range. In this range, the dMn-Mn distance (2.77 Å for Tb(Mn0.9Al0.1)2D1, and 2.87 Å for Tb(Mn0.9Al0.1)2D4) remains above the magnetic instability threshold for the Mn moments (d0$``$2.66 Å).

In comparison with the disordered compounds we studied the spin fluctuations in ordered TbMn2D4, TbMn2H4, and YMn2H4. Their simple long range antiferromagnetic structure, which is determined by the H superstructure , is a reference to check the influence of hydrogen or deuterium disorder on the spin fluctuations.

## III Neutron diffractiion measurements

We studied the magnetic correlations on the powder diffractometer G6-1 of the reactor Orphée (with an incident neutron wavelength of 4.734 Å). Temperature varied between 350 K and 10 K. A spectrum measured in the paramagnetic range was subtracted to extract the magnetic correlations. The magnetic spectra of the Al substituted samples show diffuse magnetic peaks, corresponding to short range antiferromagnetic correlations (Fig. 1). The peak positions are indexed with the same propagation vector as in the ordered parent compound RMn2D4. Using the Fullprof program , we refined the data assuming short range ordered antiferromagnetic regions of diameter Lc with ordered moments $`\mu _\mathrm{R}`$ and $`\mu _{\mathrm{Mn}}`$, keeping the same type of order as in Ref.. Results are given in Table I. We find correlated regions of extension Lc between 15 and 30 Å. Lc is temperature independent, but varies with H content and R substitution. The presence of magnetic Tb ions increases Lc with respect to non magnetic Y. It also induces ferromagnetic correlations on a shorter length scale (about 6 Å). These ferromagnetic correlations, shown by an increase of the magnetic scattering at low angles coexist with the antiferromagnetic ones. The short range ordered moments remain well below the moments in the long range ordered samples ($`\mu _{\mathrm{Mn}}`$=4 $`\mu _B`$ and $`\mu _{\mathrm{Tb}}`$=9 $`\mu _B`$ in ordered TbMn2D4 for instance). In spite of the strong magnetic disorder, the transition temperatures TSRO towards the short range ordered state are in the range 100-250 K, therefore not much decreased with respect to the Néel temperature of the long range ordered state (TN =300 K in TbMn2D4 and 330 K in YMn2D4). This was also the case of other disordered hydrides previously studied . A detailed description of the short range magnetic order in the R(Mn0.9Al0.1)2Hy family will be given later.

## IV magnetic measurements

The magnetization was measured with a SQUID magnetometer, under static magnetic field of 10 Oe, in the zero field cooling (zfc) and field cooling (fc) conditions. Typical curves are shown in Fig. 2. In all disordered samples, magnetic irreversibilities start around 230-280 K, namely above TSRO. In the Y-samples, where only Mn sublattice is magnetic, the fc curve continuously increases with decreasing temperature, well above the zfc curve, which shows a broad maximum then flattens or decreases. The magnetization of the two Y-samples have the same order of magnitude in the paramagnetic regime, but in the irreversibility region, the magnetization is much smaller for the sample with low hydrogen content. The temperature dependence of both fc and zfc curves is reminiscent of the behavior in cluster glasses , where magnetic order occurs within spatially limited regions, and the relative orientations of the superparamagnetic-like spin clusters depend on the cluster interaction field, anisotropy field, and thermal activation . In the Tb-samples with two magnetic sublattices, this cluster glass behavior is superimposed on a global paramagnetic component, with a variation close to 1/T. This second component should be related with the strong thermal fluctuations of the Tb moments, which become progressively polarized by the Tb-Mn exchange field as temperature decreases . In all the short range ordered samples, anomalies are observed in the low temperature range (30-50 K), as shown by a small maximum in the zfc curve, and an upturn of the fc curve. Similar anomalies were predicted and observed in some cluster glasses, when the local anisotropy fields start to be significant . They suggest the presence of small superparamagnetic clusters which could fluctuate down to low temperatures, having their anisotropy fields perpendicular to the interaction fields. In Y(Mn0.9Al0.1)2D4, the low temperature anomalies result in a plateau on the fc curve. This plateau, whose origin is unexplained, reaches only about 3 $`\%`$ of the maximum expected due to demagnetization effect.

In comparison with the short range ordered compounds, the magnetization of YMn2D4 and TbMn2D4 with long range antiferromagnetic order is shown in the insets. In both samples, the magnetic irreversibilities start abruptly at the Néel temperature TN measured by neutrons . In YMn2D4, a magnetization plateau is observed below TN, with a value of about 3 $`\%`$ of the demagnetization value. This plateau, rather unusual for an antiferromagnet, is presumably connected with the first order character of the transition, yielding a spin blocking induced by hydrogen order and ordered antiferromagnetic moment which remains close to saturation almost up to TN. TbMn2D4 shows a similar behavior, with an additional paramagnetic component. In both samples, the low temperature anomalies observed in the short range ordered samples are absent.

## V Inelastic neutron scattering

### A experimental set up and data analysis

The experiments were performed in the time of flight spectrometer Mibemol of the reactor Orphée, with an incident wavelength of 5 Å (incident energy of 3.27 meV). The energy resolution (FWHM=0.15 meV) and the efficiency of the detectors were determined by measuring a vanadium standard of the same plate-like shape as the samples. After background and absorption corrections, the neutron cross sections were calibrated in absolute scale using the vanadium spectrum. Measurements were performed versus temperature, using either a closed cycle nitrogen flow cryo-oven (between 350 K and 100 K) or a helium flow cryostat (between 300 K and 20 K). The maximum temperature of 350 K was chosen to avoid any decomposition of the samples due to hydrogen migration. The temperature range allowed us to study the spin fluctuations in the paramagnetic range, and to follow their evolution below the transition. The range of the elastic scattering vector is the same as in the diffraction measurements.

The scattering cross section for magnetic quasielastic neutron scattering can be expressed in a general form

$$S(q,\omega )=\frac{1}{\pi }n(\omega )\chi _q^{\prime \prime }(\omega )$$
(1)
where $`n(\omega )`$ is the Bose factor taking into account the thermal population factor of the fluctuations, and $`\chi _q^{\prime \prime }(\omega )`$ the dynamical susceptibility yielding the response of the system. Within linear response theory, $`\chi _q^{\prime \prime }(\omega )`$ is the product of the static transverse susceptibility $`\chi `$(q,$`\omega `$=0), and the spectral function $`F(\omega )`$. In the simplest case of a single exponential decay (SED), there is a single energy $`\mathrm{\Gamma }`$ (or equivalently a single relaxation rate $`\tau `$=1/2$`\pi \mathrm{\Gamma }`$, taking $`\mathrm{}`$=1) for the magnetic fluctuations, so that the spectral function is expressed as $`F(\omega )=\frac{1}{\pi }\frac{\mathrm{\Gamma }}{\mathrm{\Gamma }^2+\omega ^2}`$. In classical spin glasses like CuMn, the spectral response was expressed by a distribution of Lorentzians correspondig to a distribution of relaxation rates . Still, the quasielatic scattering cross section in the experimental energy range was well fitted by a single Lorentzian lineshape.

This simple model could not account for our data, yielding strong misfits even in the paramagnetic range. Therefore we considered explicitely an energy distribution in the spectral lineshape. We took two limiting forms for this distribution, namely a bimodal distribution (model 1) and a uniform distribution (model 2). Model 1 assumes two typical energies $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$ ($`\mathrm{\Gamma }_1`$$`<`$$`\mathrm{\Gamma }_2`$) for the spin fluctuations. It was used previously to analyze the spin dynamics in cluster glasses . Model 2 assumes that the energies of the spin fluctuations are distributed with an equal probability between lower and higher energy bounds $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$. It was recently proposed by Bernhoeft  within a general model of the dynamical phase inhomogeneities in non Fermi liquid systems.

The quasielastic neutron cross section is written

\- within model 1:

$$S(q,\omega )=\frac{\omega }{e^{\omega /kT}1}\left(F_1(\omega )\chi _1(q)+F_2(\omega )\chi _2(q)\right)$$
(2)
where $`\chi _1`$ and $`\chi _2`$ are the static susceptibilities of the two quasielastic contributions and the spectral functions are respectively

$$F_1(\omega )=\frac{1}{\pi }\frac{\mathrm{\Gamma }_1}{\mathrm{\Gamma }_1^2+\omega ^2}F_2(\omega )=\frac{1}{\pi }\frac{\mathrm{\Gamma }_2}{\mathrm{\Gamma }_2^2+\omega ^2}$$
(3)
with $`\mathrm{\Gamma }_1`$, $`\mathrm{\Gamma }_2`$ being the corresponding energy linewidths. The static susceptibility is defined as $`\chi `$=$`\chi _1`$+$`\chi _2`$.

\- within model 2:

$$S(q,\omega )=\frac{\omega }{e^{\omega /kT}1}F(\omega )\chi (q)$$
(4)
where $`\chi `$ is the static susceptibility and $`F(\omega )`$ the spectral function written as

$$F(\omega )=\frac{1}{\pi }\frac{1}{\mathrm{ln}(\mathrm{\Gamma }_2)\mathrm{ln}(\mathrm{\Gamma }_1)}\frac{1}{\omega }\left(\mathrm{arctan}(\frac{\omega }{\mathrm{\Gamma }_1})\mathrm{arctan}(\frac{\omega }{\mathrm{\Gamma }_2})\right)$$
(5)
where $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$ are respectively the low and high energy limits of the energy distribution.

In the above expressions, $`\omega `$$`>`$0 corresponds to a neutron energy gain. The prefactors in equations (3) and (5) normalize to unity the energy integration of the spectral function. Therefore, in the high temperature limit $`\omega `$$``$kT (valid here in the paramagnetic range and down to about 50 K), the quantity T$`\chi `$ is equal to the energy-integrated intensity of the quasielastic signal. The fitted energy widths do not depend on the normalisation factor.

In the limit of a Curie-Weiss behavior, the neutron susceptibility is related to the effective fluctuating moment by the expression: $`\chi `$(q=0,T)=$`A\frac{m_{eff}^2\mu _B^2}{3kT}`$. $`A`$ corresponds to the calibration of the neutron cross section in absolute scale. This expression provides an effective moment value, to be compared with the value from bulk magnetic measurement.

The total cross section is written as

$$S^{\mathrm{total}}(q,\omega )=c_{el}\delta (\omega )+S(q,\omega )$$
(6)
The neutron intensity $`I`$ detected versus time of flight $`t`$ at the scattering angle $`2\theta `$ is proportional to the quantity:

$$I(\theta ,t)\frac{1}{t^4}S^{\mathrm{total}}(q,\omega )$$
(7)
The neutron intensity was convoluted with the experimental resolution and fitted to each individual time of flight (TOF) spectrum, with $`c_{el}`$ (intensity of the elastic peak), $`\mathrm{\Gamma }_1`$, $`\mathrm{\Gamma }_2`$, and $`\chi _1`$, $`\chi _2`$ (model 1) or $`\chi `$ (model 2) as parameters. A very small linear background was also added in the fit. The fit was performed in the energy range (-20, 2) meV, where the phonon contribution is small and could be neglected.

### B results

a) short range ordered samples

We first show the results in Tb(Mn0.9Al0.1)2Dy ($`y`$=1 and $`y`$=4). In spite of their different D contents, ordering temperatures and magnetic correlations lengths, the behavior of the magnetic fluctuations is the same for the two samples. Typical TOF spectra are shown in Figs. 3 and 4 for temperatures respectively above and below TSRO. Note that due to the $`t^4`$ factor of equation (7), the maxima of the quasielastic signals are shifted with respect to the elastic one. In spite of this distortion, the time dependent plot were preferred to the energy dependent ones (in inset), since they provide a better estimation of the fit quality at low energies.

Whatever the model chosen for the spectral function, the general evolution with temperature can be described as follows. Above TSRO, the susceptibility follows a Curie law, and the quasielastic integrated intensity T$`\chi `$ is temperature independent (Fig. 5). Below TSRO, we observe a gradual transfer of intensity from the quasielastic signal to the elastic one, the sum of the two contributions being conserved with temperature. The high energy signal of width $`\mathrm{\Gamma }_2`$ dominates, with a weight of 80$`\%`$ of the suceptibility at high temperature. The energy linewidths have a rather original behavior (Fig. 6). Above TSRO, $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$ are temperature independent. Below TSRO, the small linewidth $`\mathrm{\Gamma }_1`$ starts to decrease whereas the large linewidth $`\mathrm{\Gamma }_2`$ increases with decreasing temperature. This behavior is the same for all q values. In the paramagnetic regime, the quasielastic cross section is well fitted by the two models. Below TSRO, model 1 still yields very good fit of the data, whereas model 2 starts to show some misfits. They occur mainly below 80 K where the linewidths $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$ are very different. We have therefore restricted the use of model 2 to temperatures above 80 K, where this model was meaningful. In the paramagnetic range, the two models give an energy linewidth in the same energy range, with $`\mathrm{\Gamma }_1`$ around 0.1 meV, and $`\mathrm{\Gamma }_2`$ around 3-5 meV.

The q dependence of the susceptibility and quasielastic widths is shown in Fig. 7. The susceptibility $`\chi `$ shows a weak and broad modulation with respect to the form factor of the free ion. This modulation remains the same below TSRO. The magnetic correlations observed below TSRO by neutron diffraction correspond to a modulation of the elastic component. The energy linewidths are almost q-independent, both above and below TSRO. The Tb(Mn0.9Al0.1)2D1 sample, where the magnetic correlations are enhanced, shows the same behavior.

In Y(Mn0.9Al0.1)2D4, the magnetic signal coming from Mn ions only is much smaller, but still shows the complex lineshape described above. The main difference with the Tb samples concerns the temperature dependence of the large energy linewidth $`\mathrm{\Gamma }_2`$, which now strongly decreases below TSRO (Fig. 8). This is observed whatever the model used to describe the spectral function.

b) long range ordered samples

In comparison, we show the magnetic fluctuations in TbMn2D4, TbMn2H4, and YMn2H4 where long range magnetic order occurs at TN through a first order magnetostructural transition. Above TN, the magnetic fluctuations are very similar in the ordered and in the disordered samples. The main effect of the LRO is a strong suppression of the quasielastic intensity below TN. For example, at T= TN/2 the intensity of the magnetic fluctuations is decreased by a factor 3 with respect to its value in the paramagnetic state in the ordered Tb samples, and by a factor 5 in ordered YMn2H4, whereas it decreases by 30$`\%`$ in disordered Tb(Mn0.9Al0.1)2D1 and only 8$`\%`$ in Y(Mn0.9Al0.1)2D4. The second important difference is the occurence of a well defined localized excitation in the ordered Tb samples below TN.

In Fig. 9, we show two typical TOF spectra for TbMn2D4 at 340 K and 160 K, namely above and below TN. At 340 K, the spectral lineshape is well fitted by a bimodal distribution (model 1), with typical energy widths of 0.5 and 2 meV, therefore comparable to the energy widths of the disordered samples at the same temperature. Below TN, a purely inelastic signal appears in the TOF spectra, coexisting with the quasielastic one. This new component was fitted by a Gaussian lineshape, of energy E0 and width $`\mathrm{\Gamma }_{\mathrm{inel}}`$. Its intensity (fig. 10a) shows a broad maximum versus temperature. The energy E0 slightly increases from 6 to 7 meV when temperature decreases (Fig 10b), with constant energy width $`\mathrm{\Gamma }_{\mathrm{inel}}`$ of 2 meV. The quasielastic signal strongly decreases just below TN, but still persist in the ordered state. The large energy width $`\mathrm{\Gamma }_2`$ increases with decreasing T, whereas the small energy width $`\mathrm{\Gamma }_1`$ is about temperature independent. The sum of the three contributions (elastic, quasielastic and inelastic) is conserved with temperature.

In TbMn2H4, the inelastic and quasielastic signals are the same as in the TbMn2D4. The elastic component is enhanced by about a factor 10 in TbMn2H4, due to the large incoherent contribution of the hydrogen isotope. As expected from previous inelastic neutron studies of Laves hydrides , the dynamics of hydrogen ordering cannot be resolved in the present experiment. In other words, hydrogen (or deuterium) is frozen at the time scale of the neutron experiment (t=9$`\times `$$`10^{12}`$s), and there is no interference between H or D diffusion and the magnetic fluctuations.

Finally, in ordered YMn2H4 (Fig 11), the quasielastic signal above TN also consists of two components. Below TN, it becomes very small but can still be detected down to 100 K. The energy width in the paramagnetic state are about the same as in the disordered Y(Mn0.9Al0.1)2D4, but here they do not vary much with temperature. The inelastic localized mode observed in the ordered Tb samples was not observed.

## VI Discussion

### A paramagnetic regime

In the high temperature range where the samples show a Curie-Weiss behavior, the effective moments deduced from the integration of the quasielastic neutron cross section agree with the value deduced from magnetization (table II). This means that most of the spin fluctuations are probed by the experimental time window, and rules out the presence of high energy spin fluctuations (in the 50 meV range or above), similar to that observed in YMn2 , Y(Mn0.9Al0.1)2  or other itinerant systems. Therefore, all samples are in the localized moment limit, even at low H(D) content, and the wide energy distribution seen in both Tb and Y samples should be connected with peculiar features of the magnetic disorder. At high temperature, for localized spins coupled by near neighbor interactions, the energy linewidth of the magnetic fluctuations is related to the values of the exchange constants . This is the case of the present samples, where the anisotropy energy is much smaller than the exchange energy . Within molecular approximation, the lineshape of the response function is expected to be intermediate between Gaussian and Lorentzian, and its second moment, which measures the quasielastic width is given for a polycrystalline sample by

$$\overline{\omega ^2}=(8/3)S(S+1)\underset{i}{}J^2(\mathrm{R}_i)(1\mathrm{sin}(\mathrm{qR}_i)/(\mathrm{qR}_i))$$
(8)
In this model, the energy linewidth $`\sqrt{\overline{\omega ^2}}`$ is temperature independent, in agreement with experiment, and in contrast with the behavior of itinerant systems where the linewidth increases linearly with temperature (Korringa behavior). Assuming first neighbor interactions only (R1=2.86 Å), the smooth variation of the linewidth predicted by equation (8) above 1 Å-1 is also consistent with experiment (Fig. 7b), although the expected decrease at low q values is not seen.

The distribution of linewidths may be connected with a distribution of exchange constants, induced by the frozen hydrogen or deuterium disorder. As discussed previously for the ordered compounds YMn2D4, the presence of a H(D) atom near a Mn-Mn pair modifies the amplitude, and even the sign, of the first neighbor exchange interaction . The various environments of the Mn atoms having zero or one H(D) atom nearby the Mn pairs should be at the origin of the linewidth distribution. In the Tb samples, the magnetic fluctuations are dominated by the Tb moments of much larger magnitude. The distribution of linewidths therefore mostly measures the distribution of Tb-Mn interactions, showing that they are also sensitive to the number of H(D) near neighbors atoms. This is also consistent with the analysis of the ordered structure. Taking $`S_{\mathrm{Mn}}`$=2, and summing equation (8) over the 6 first neighbors of a Mn ion, we obtain from the two energy widths in Y(Mn0.9Al0.1)2D4, low and high limits for the Mn-Mn exchange constant $`\sqrt{\overline{J^2}_{\mathrm{Mn}\mathrm{Mn}}}`$ equal to 0.03 and 0.3 meV. A similar evaluation for Tb(Mn0.9Al0.1)2D4 ($`S_{\mathrm{Tb}}`$=3) yields limit values for the the Tb-Mn exchange constant $`\sqrt{\overline{J^2}_{\mathrm{Tb}\mathrm{Mn}}}`$ equal to 0.03 and 0.1 meV.

### B ordering transition

In the long range ordered compounds, the transition is of first order, whereas in the short range ordered compounds, it is close to second order. As shown previously, H(D) order is the key parameter which controls the frustration. In the LRO samples, the first order transition is directly connected with the formation of H(D) superstructure which relieves the frustration of the Mn lattice. In contrast, in the disordered samples, the second order transition occurs in a range of temperature where the slowing down the H(D) diffusion yields a more progressive change from thermal to frozen disorder. In both cases, the present results show that the transition is characterized by a deep change in the magnetic fluctuations, namely, i) a transfer of intensity from the quasielastic to elastic signal connected with the onset of static correlations, and ii) a change in the behavior of the quasielastic widths, which start to vary with temperature.

The transition temperature TSRO remains in the range 100-250 K, therefore is not much decreased with respect to the Néel temperature of the ordered compounds (300-330 K). Such high transition temperature is often observed in cluster glasses . It contrasts with classical spin glasses where the spin glass temperature is typicallty ten times smaller than the transition temperature of the ordered parent compound. The average exchange constant $`J_{\mathrm{Mn}\mathrm{Mn}}`$ deduced from TN in the mean field approximation (TN=$`_i`$$`\frac{2}{3}J_{\mathrm{Mn}\mathrm{Mn}}S_{\mathrm{Mn}}(S_{\mathrm{Mn}}+1)`$, summing over the 6 first neighbors of a Mn ion) yields $`J_{\mathrm{Mn}\mathrm{Mn}}`$=0.9 meV, which is about 3 times higher than the upper limit for $`\sqrt{\overline{J^2}_{\mathrm{Mn}\mathrm{Mn}}}`$ deduced from the linewidths in the paramagnetic regime. Obviously, such evaluations only provide an order of magnitude of the exchange constant since they neglect the influence of inhomogeneity and frustation.

A simple picture in terms of a cluster glass can account for the observed decrease of TN with respect to the ordered state. One assumes clusters of diameter Lc (where Lc is the correlation length) consisting of an ordered core surrounded by a disordered layer of thickness d (where d=2.8Å is the first neighbor distance). In first approximation, the decrease of TN is given by the percentage disordered spins, assuming that they do not contribute to the average exchange interaction. For the Tb samples (TN=300K in ordered TbMn2D4), this simple picture yields short range ordering temperatures of 112K (y=4) and 161K (y=1), in relatively good agreement with the experimental values (135K and 200K respectively). A better evaluation would require to define different inter and intracluster exchange interactions, as proposed in mean fields models of cluster glasses .

The coexistence of highly frustrated and low frustrated spins yields a large distribution of energy barriers, as observed in cluster glasses or inhomogeneous superparamagnets. The magnetization data support this qualitative picture, showing that some spins could freeze either above TSRO (up to the Néel temperature of the ordered compound), or well below TSRO down to the low T range.

### C spin dynamics below the transition

As temperature decreases, more and more spins freeze and contribute to the static clusters. The fluctuating spins remain almost uncorrelated like in the paramagnetic regime. In Y(Mn0.9Al0.1)2D4, the decrease of the two quasielastic widths suggests that these uncorrelated spins relax between several metastable configurations, with typical times ($`\tau `$=1/2$`\pi \mathrm{\Gamma }`$) increasing with decreasing temperature.

In the Tb samples, the formation of the static clusters is associated with the emergence of two types of spin dynamics : a relaxation process involving weakly coupled and almost uncorrelated spins, as shown by the decrease of the small quasielastic width $`\mathrm{\Gamma }_1`$, and an excitation process as shown by the increase of the large quasielastic width $`\mathrm{\Gamma }_2`$. Here the magnetic signal is dominated by the Tb spins. In ordered TbMn2D4, a local mode of energy E0 is clearly observed below TN, and is attributed to local fluctuations of the Tb spins in the static Mn molecular field. Such mode is predicted and observed in ordered RFe2 or RAl2 Laves phases . Its energy is expected to increase smoothly with temperature like the ordered Mn moment(E0 $``$ $`J_{\mathrm{Tb}\mathrm{Mn}}`$ $`S_{\mathrm{Mn}}`$). In the short range ordered Tb compounds, one should also expect a similar inelastic mode, but broadened by the distribution of exchange interactions and situated at a lower energy, due to the lower value of the short range ordered Mn moment. Therefore, this mode could be hidden by the large quasielastic signal. In order to check this assumption, we have performed for Tb(Mn0.9Al0.1)2D4 the same fit as for ordered TbMn2D4. It yields a slight improvement of the fit quality, with an inelastic contribution of about 10$`\%`$ of the quasielastic one. The energy E0 is smaller than in TbMn2D4 and increases more rapidly with decreasing temperature (from 3 to 5 meV), as expected from a simple model. The quasielastic widths, especially the low energy width $`\mathrm{\Gamma }_1`$ are not much affected.

This analysis points out the strong similarities between the spin fluctuations in the short range and long range ordered Tb compounds. It also suggests that the large quasielastic signal and the inelastic one have the same nature, and we note that their characteristic energies E0 and $`\mathrm{\Gamma }_2`$ vary in the same way with temperature. The onset of short range order weakens the energy of the inelastic mode, and changes the balance between the two contributions. The persistence of a quasielastic signal in the ordered state, which is not observed in RFe2 Laves phases, is presumably related to the influence of hydrogen or deuterium. The lowering of symmetry due to the H(D) superstructure might create lower energy levels which cannot be distinguished from the quasielastic scattering. The residual disorder, since one H(D) site is halfly occupied, could also play a role. Whatever the exact mechanism, we have observed local excitations of low energy which develop as soon as a static magnetic order freezes in, and are almost insensitive to the correlation length. A better analysis of these excitations would require higher resolution measurements on a single crystal.

## VII Conclusion

In the Laves compounds R(Mn0.9Al0.1)2Dy with deuterium or hydrogen disorder, a transition towards short range magnetic order is probed by neutron scattering. It is shown by the occurrence of static clusters of a few tens of Angstroms, with a size independent of temperature. The transition temperature TSRO is high in spite of the small cluster size, and the transition is close to second order, in contrast with the first order transition in the long range ordered compounds. In the paramagnetic range, the complex lineshape of the spectral function suggests a distribution of exchange constants, possibly related to the onset of nonequivalent magnetic bonds and the influence of frozen H(D) configurations. Below TSRO, several types of fluctuations are observed, depending on the presence of the Tb magnetic ion. They are attributed either to the relaxation of almost uncorrelated spins, or to local spin excitations within the frozen clusters. The spin fluctuations in the short range and long range ordered compounds show strong similarities. The overall behavior and the macroscopic magnetic properties are interpreted in terms of a cluster glass, where short range ordered regions with local H(D) order and low frustration coexist with strongly frustrated and uncorrelated spins. It would be interesting to know if the observed spin fluctuations arise from the peculiar coupling of hydrogen and magnetic lattices, or if they could be observed in other cluster glasses or disordered magnets with topological frustration.

###### Acknowledgements.

We thank N. Bernhoeft, M. Hennion, P.A. Alekseev and J.C. Gómez Sal for many interesting discussions. P. C.-P. is supported by Fundação para a Ciência e a Tecnologia, Portugal, through the research grant PRAXIS XXI/BD/20334/99. This work was partly supported by the Russian foundation for Basic Research, Grant N. 02-02-06085,and the Russian State Program ’Neutron Investigations of Condensed Matter’.

Figure captions

Fig.1: Magnetic neutron diffraction spectra at 10 K for Tb(Mn0.9Al0.1)2Dy ($`y`$=4 and $`y`$=1) and Y(Mn0.9Al0.1)2D4, measured on G6-1 diffractometer ($`\lambda `$ =4.734 Å). A spectrum measured in the paramagnetic range was subtracted to extract the magnetic contribution. For Tb(Mn0.9Al0.1)2D4, the first antiferromagnetic peak is not observed since magnetic moments are along direction $`<`$111$`>`$. Solid lines are fits of the data, yielding the short range ordered magnetic moments and correlations lengths given in Table 1.

Fig.2: Low field magnetization in Tb(Mn0.9Al0.1)Dy ($`y`$=4 and $`y`$=1), and in Y(Mn0.9Al0.1)Dy ($`y`$=4 and $`y`$=1), measured in a static field H=10 Oe, using zero field cooling (zfc) and field cooling (fc) conditions. Insets: low field magnetization of the long range ordered YMn2D4 and TbMn2D4 compounds. The transition temperature TSRO towards short range order is shown by arrows. Other arrows point out the low temperature anomalies.

Fig.3: Time of flight (TOF) spectrum of Tb(Mn0.9Al0.1)D4 at 250 K (paramagnetic range), focusing on the quasielastic region. Spectra were regrouped for detectors within an angular range 23.5–63.1 degrees. Fits with model 1 (a) and model 2 (b) are shown by solid lines. Inset: the corresponding neutron cross section versus energy transfer, and a schematic drawing of the distribution of energy widths for each model.

Fig.4: TOF spectrum of Tb(Mn0.9Al0.1)D4 at 80 K (below TSRO), in an angular range 23.5–63.1 degrees. Fits with model 1 (a) and model 2 (b) are shown by solid lines. Inset: the corresponding neutron cross section versus energy transfer and a schematic drawing of the distribution of energy widths for each model.

Fig.5: Elastic, quasielastic intensity T$`\chi `$, and sum of the two contributions versus temperature in Tb(Mn0.9Al0.1)2D4. TOF spectra have been regrouped within an angular range 23.5–63.1 degrees. Models 1 and 2 give equivalent results.

Fig.6: Quasielastic widths $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$ versus temperature in Tb(Mn0.9Al0.1)2D4, obtained by fitting the data with model 1 (a) and model 2 (b).

Fig.7: Results obtained in Tb(Mn0.9Al0.1)2D4 with model 1. a) Quasielastic intensity versus q for two temperatures, 200 K and 80 K, above and below TSRO respectively. Solid lines correspond to the squared magnetic form factors of Tb and Mn ions. Dotted lines are guides to the eye. b) Quasielastic widths $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$ versus q at 200 K. Solid lines are fits with the equation (8) described in text. c) Quasielastic widths versus q at 80 K.

Fig.8: Quasielastic widths $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$ versus temperature in Y(Mn0.9Al0.1)2D4, obtained with model 1.

Fig.9: TbMn2D4 : TOF spectra at 340 K and 160 K, (TN =300 K). In inset, the corresponding neutron cross section versus energy transfer. Solid lines are fits with model 1, adding an inelastic contribution below TN.

Fig.10: TbMn2D4 : a) variation of the integrated intensities versus temperature, b) quasielastic widths $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$ and energy E0 of the inelastic signal versus temperature.

Fig.11: YMn2H4 : a) variation of the integrated intensities versus temperature, b) quasielastic widths $`\mathrm{\Gamma }_1`$ and $`\mathrm{\Gamma }_2`$ versus temperature.

Table captions