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# Finite size scaling approach to dynamic storage allocation problem

## 1 Introduction

Computers are growing rapidly. The first IBM PC had $`64,000`$ bytes of memory, $`160kB`$ of storage and a microprocessor with speed of 4.77 MHz. Today, they have $`10^9`$ bytes of memory and about hundred times more space on their hard disks. They can process billions of instructions just in one second. These numbers are just for a typical desktop PC, while relative values for super computers could be many times greater. At a higher level, computers can be connected to one another to share their information and resources and make a large amount of data available for users on a network like Internet.

These numbers are large enough to encourage us to manipulate them using the tools of statistical physics. These tools can help us to study and to estimate the efficiency and performance of algorithms and methods which are designed to organize and deal with large amounts of data and resources. Some examples of these algorithms are storage allocation algorithms and file systems and search and indexing algorithms.

In this work we will present finite size scaling  as a tool to study dynamic storage allocation algorithms. We are going to use the same terminology of critical phenomena in the present context.

We have chosen a well defined problem  \- a comparison of speed and memory usage among three simple allocation algorithms: first-fit, next-fit and best-fit algorithm. Nevertheless, this can also be done with other algorithms which are applied on a large set of data and can give us a better understanding of what their behaviors are especially when there is not a simple analytical calculation.

First we should give a brief description of storage allocation methods. A storage device such as memory or hard-disk-drive (HDD) is a pool of words (we will call word the smallest addressable unit of memory)  and an integer number, the address, shows the position of each word in the memory.

The goal of a memory allocation routine is to store and organize data in memory in the most efficient manner - to allocate enough memory at any new request, and to restrict access to the allocated memory from other processes until the task requiring memory liberates it.

Since the size of any request is a dynamical variable which is out of storage allocator’s control, it is called dynamic storage allocation and it is a sort of on-line algorithm .

One simple way to allocate memory consists of dividing memory into large and uniform nodes (the smallest part of a data structure including at least one word). Since data sizes can be smaller than the size of the nodes, this method will waste large amount of memory. Alternatively one might divide memory pool into small nodes and use the scheme of the linked-memory: “if there is no room for the information in a given location, put it elsewhere and implant a link to it” . Because many users and applications may need different size blocks of memory and may need them for different periods of time, data will be fragmented after some time. Data fragmentation slows down reading speed especially when the storage device is a hard disk .

It is feasible to allocate space for a given request just in one contiguous block (a set of contiguous memory locations). We can avoid data fragmentation in this fashion, but still have problem with free space fragmentation. Indeed, after the dynamic storage allocation has been in operation for a while, the free areas are broken into many small pieces which might not be large enough for certain requests; therefore, a larger amount of memory is required to run the system in this way. This amount of memory depends on the two main parts of the algorithm - the method of keeping list of free blocks and the selection policy for choosing among the available free blocks of memory. The list of available free blocks can help in their better use. It stores the addresses and sizes of free blocks. Indeed there are many different types of free lists: address-ordered, size-ordered and etc.. The simplest one which we will use, is the address-ordered list. It keeps the free blocks with the order of their address in storage device. in fact, the order of available block in the list is the same as their place in the memory. For example if a free $`b_n`$ starts from word number $`n`$ and another block $`b_m`$ starts from word number $`m`$, in the list of free blocks, block $`b_n`$ is before $`b_m`$, only when $`nm`$.

Given the list of free blocks, we need a decision policy which tells us where a request should be placed. One of the simplest policies is known as first-fit : it tries to find the first available block in the free list that is large enough for the request. The obvious disadvantage of this algorithm is that it might waste a large space for other future requests by putting a small request there. Another issue with the first-fit is that after the system has been working for a while, the available list will be sorted by increasing order of blocks’ size. Thus, for a large request, we have to check almost all of the list of free blocks which slows down the running speed of the algorithm.

If it is desired to reduce memory waste, another method, best-fit algorithm can be applied. This method tries to find the smallest available space, which is large enough for the request; therefore, we can reduce space use at the cost of more searching in the free blocks’ list.

If speed of the algorithm is important for us we can use next-fit algorithm which is a variation of first-fit algorithm. We define a pointer which points to the starting point of the searching in the list. The value of the pointer will be changed after a successful allocation and it will point to the first available block after the free block used for the last allocation. In this way the size distribution of free blocks in the free list will be uniform hence the algorithm will be faster.

There are many other algorithms such as buddy-system, next-fit and indexed-fit algorithms. A particular choice might be dictated by bottlenecks of the storage device, size distribution function of requests or their life span. For example if a large memory is available the buddy-system may be used because it is fast but needs more space to run. In the opposite case when there is shortage of memory, the linked-memory algorithm is more appropriate. However, in most cases there is not any clear way to determine which algorithm is the best. Many attempts have been made; these attempts answer this question and compare different algorithms from different points of view like performance or probability to have the worst case fragmentation.

We aim to study and compare speed and memory usage, using tools of statistical physics like finite size scaling for simple algorithms: the first-fit, next-fit and best-fit algorithms with address-ordered free list.

It is shown that best-fit algorithm is the best in terms of space use while the next-fit algorithm is the worst. From the speed point of view, the results show that next-fit algorithm is the fastest and there is not a significant difference between the speed of the other two.

## 2 Model

The model we will study assumes a storage device such as memory or hard disk of a computer as a set of small nodes. At the $`r`$-th step of simulation, a request of size $`S_r`$ is sent to the allocator, $`S_r`$ being the number of nodes (or words) needed. We have performed a detailed study of the case where the size $`S_r`$ is drawn from a uniform distribution $`1S_rS_{max}`$. Although is straightforward to extend the analysis to other interesting cases the uniform distribution has often been used previously . Furthermore at each step of the simulation each allocated block can be liberated with the probability $`P_d`$. This is a sort of “grand canonical ensemble” where the total number of blocks, $`N_b`$, fluctuates around its average value, $`1/P_d`$.

In order to prevent the rejection of a request due to an overflow, we allow the memory to increase by the necessary amount when needed. In fact in this way, the memory size is a variable which can be measured during the simulation. This is similar to a system with virtual memory .

The simulation runs until the system reaches the stationary state. Then one starts to measure the density of allocated memory on the device and the searching time.

Density, $`d`$, is defined as the ratio of the total amount of allocated memory to the size of our flexible storage device, including empty spaces; therefore wasted space, $`w`$, is simply $`w=1d`$.

The searching time, $`t_s`$, is the time that allocator spends to find a free block and allocate requested memory. The unit of time is the time needed to find a free block and check its size. Thus allocation time is the number of checks which have to be done through the free list to find the appropriate free block which satisfies all dictated constrains by the algorithm. For example, in the first-fit method, if the first block in the list is satisfactory, this value will be one, if the second block is, it will be 2 and so on. The conversion of this time unit to real time depends on the hardware and many other characteristics of the system and it could be studied as an independent problem for particular uses.

Averages of the two quantities $`w`$ and $`t_s`$ are calculated and stored for all three algorithms. All six cases are performed for different value of $`P_d`$ and $`S_{max}`$.

## 3 Results

In the case of wasted memory a scaling ansatz which works rather well in all three methods is

$$w=P_d^{\nu _m}f_m(S_{max}P_d^{\varphi _m}),$$
(1)
with $`f_m(x)`$ being a constant for large value of $`x`$. Similarly to the same form,

$$t_s=P_d^{\nu _t}f_t(S_{max}P_d^{\varphi _t}),$$
(2)
fits the data of searching time.

To have an estimate of the exponents $`\nu _m`$ we ran the simulation for a fix value of $`S_{max}`$ and various $`P_d`$ with $`x=S_{max}P_d^{\varphi _m}`$ being large enough to be sure that $`f_m(x)`$ is constant. The results are plotted in figure 1, which shows the relation between wasted space and $`P_d`$ for three algorithms. The exponents, $`\nu _m`$, are the slopes of the lines.

The same method has been applied to the searching times and results are shown in figure 2. The value of exponents $`\nu _m`$ and $`\nu _t`$ are summarized in table 1.

Once the values of $`\nu _m`$ and $`\nu _t`$ are known, the functions $`f_m(S_{max}P_d^{\varphi _m})`$ and $`f_t(S_{max}P_d^{\varphi _t})`$ can be calculated to get the exponents $`\varphi _m`$ and $`\varphi _t`$. We repeat the simulation for different $`S_{max}`$ for all the algorithms and at least three different values of $`P_d`$.

For a given algorithm and with a properly selected value for the $`\varphi `$ exponent, all the curves collapse. Figure 3 shows the collapse for wasted space and figure 4 for the searching time just for the next-fit algorithms. Similar results hold for the first and best fit. All of these six sets of data collapse fairly well with their own scaling functions and with the exponents reported in table 1.

Interestingly we note that, for the case of best-fit algorithm we obtain two values for $`\varphi `$ whose difference is substantially larger than the errors if we try to collapse wasted space data or searching time data. In critical phenomenon theory, one expects that a unique exponent is associated to each scaling field. However, in the present context we have no explanation for the results that there may be more than one exponent associated with $`P_d`$.

Figure 1 proves that the best-fit algorithm can save more memory when the number of allocated blocks, $`N_b`$, is high (or $`P_d`$ is small). For a smaller number of $`N_b`$, all three algorithms are similar. An important point about best-fit algorithm is that it does not have any characteristic size because $`\varphi _m=0`$ for this case.

On the other hand, for the searching time (FIG.2) the next fit algorithm performs better than the other two, which show a very similar behavior to one another. An interesting point is that the searching time of next-fit grows with root square of $`N_b`$, while the searching time of other two grows linearly.

## 4 Conclusion

These examples can show us how the knowledge of the scaling function and critical exponents of algorithms help us to choose an optimal strategy. Therefore, the illustrated work can be repeated for other storage allocation algorithms and different distributions of requests’ sizes which may be taken out from actual statistics of a particular system. Nonetheless, it might be useful to apply the same method to other complex algorithms, especially in the case that an algorithm should be selected or designed for a large scale system like an Internet search engine. In addition, we can study algorithms from this point of view and classify them and determine whether any universality exists. Finally one might extend this to other applied fields and engineerings to organize data in more efficient way.

## 5 Acknowledgment

I thank Amos Maritan for valuable advice and a careful reading of the manuscript.I thank Muli Safra for his comments.


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# Exact sequences for equivariantly formal spaces

## 1. Introduction

Let $`T=(S^1)^n`$ be a torus of dimension $`n`$ and $`X`$ a “nice” $`T`$-space. Suppose that $`X`$ is *cohomologically equivariantly formal*111It seems that the terminology ‘equivariantly formal’ was coined by \[GKM\]. We add ‘cohomologically’ to avoid confusion with notions in rational homotopy theory. (or *CEF*), which means that its equivariant cohomology $`H_T^{}(X)`$ (with rational coefficients) is free over the polynomial ring $`H^{}(BT)`$. Then the so-called Chang–Skjelbred lemma \[CS, (2.3)\] asserts that the sequence

(1.1)
$$0H_T^{}(X)H_T^{}(X^T)H_T^{+1}(X_1,X^T)$$

is exact, where $`X^TX`$ denotes the fixed point set and $`X_1`$ the union of all orbits of dimension at most $`1`$. In other words, $`H_T^{}(X)`$ coincides, as subalgebra of $`H_T^{}(X^T)`$, with the image of $`H_T^{}(X_1)H_T^{}(X^T)`$. Usually $`X^T`$ and $`X_1`$ are much simpler than $`X`$, so that (1.1) gives an easy method to compute $`H_T^{}(X)`$. This can be used for instance for a short proof of Jurkiewicz’s theorem about the cohomology of smooth projective toric varieties because they are known to be equivariantly formal, see Remark 2.3. There are many other applications of the Chang–Skjelbred lemma in algebraic and symplectic geometry, often with implications for combinatorics.

Roughly at the same time as Chang and Skjelbred, Atiyah proved a much more general theorem in the context of equivariant $`K`$-theory \[A, Ch. 7\]. Bredon \[Br\] then observed that it applies equally to cohomology. In the context of toric varieties an Atiyah-like theorem was proven by Barthel–Brasselet–Fieseler–Kaup for cohomology and intersection homology \[BBFK, Thm. 4.3\]. Recently Goertsches and Töben \[GT\] made the very interesting observation that the Cohen–Macaulay property, which Atiyah used in an essential way, gives generalizations also for fixed-point-free actions.

The principal aim of this note is to present a generalized cohomological version of Atiyah’s theorem. Our proof in Section 2 will be a modification of his, adapted to cohomology and with a special emphasis on coefficient rings $`R`$ other than the rationals, namely on subrings of $``$ and on prime fields. As a corollary, we get an integral version of the Chang–Skjelbred lemma with certain restrictions on the isotropy groups. We also extend the Goertsches–Töben result to the same coefficient rings and to more general spaces than compact $`T`$-manifolds.

###### Acknowledgements.

The authors thank Winfried Bruns, Jean-Claude Hausmann, Lex Renner and Sue Tolman for helpful discussions. We are also indebted to the anonymous referee for suggesting improvements to the presentation of the paper.

## 2. The Atiyah–Bredon sequence

We use Alexander–Spanier cohomology, cf. \[M, Ch. 8\]. Coefficients are taken in a subring $`R`$ of $``$ or in the finite field $`R=_p`$. Here the letter $`p`$ denotes a prime, as it does in the rest of the paper. All topological spaces will be assumed to be paracompact and Hausdorff. Recall that on locally contractible spaces Alexander–Spanier cohomology and singular cohomology coincide.

Let $`T=(S^1)^n`$ be a torus and $`X`$ a $`T`$-space. (Note that its Borel construction $`X_T`$ is again paracompact Hausdorff.) We assume $`X`$ to be finite-dimensional, with only finitely many orbit types and such that $`H^{}(X^K)`$ is finitely generated over $`R`$ for all closed subgroups $`K`$ of $`T`$.222These assumptions can be weakened, cf. \[AP, Sec. 3.2\]. For example, $`X`$ can be finitistic instead of finite-dimensional, and, for $`R=`$, must only have finitely many *connected* orbit types. For example, $`X`$ may be a finite $`T`$-CW complex, a compact topological $`T`$-manifold or a complex algebraic variety with an algebraic action of $`(^\times )^nT`$.

Denote by $`X_i`$, $`1in`$, the equivariant $`i`$-skeleton of $`X`$, i. e., the union of all orbits of dimension $`i`$. In particular, $`X_1=\mathrm{}`$, $`X_0=X^T`$ and $`X_n=X`$. Since $`X`$ is Hausdorff with only finitely many orbit types, each $`X_i`$ is closed in $`X`$. The maximal $`p`$-torus $`T_pT`$ is the subgroup of all elements of order $`p`$ (together with $`1T`$). It is isomorphic to $`_p^n`$. The $`T_p`$-equivariant $`i`$-skeleton $`X_{p,i}`$ of $`X`$ is the set of all $`T_p`$-orbits consisting of at most $`p^i`$ points. One clearly has $`X_iX_{p,i}`$.

The inclusion of pairs $`(X_i,X_{i1})(X,X_{i1})`$ gives rise to a long exact sequence

(2.1)
$$\mathrm{}H_T^{}(X,X_i)H_T^{}(X,X_{i1})H_T^{}(X_i,X_{i1})\stackrel{\delta }{}H_T^{+1}(X,X_i)\mathrm{},$$

and likewise $`(X_{i+1},X_{i1})(X_{i+1},X_i)`$ gives maps

(2.2)
$$H_T^{}(X_i,X_{i1})H_T^{+1}(X_{i+1},X_i).$$

###### Theorem 2.1.

Let $`X`$ be a $`T`$-space such that $`H_T^{}(X)`$ is a free $`H^{}(BT)`$-module. Suppose in addition that for all $`i`$

(2.3a) $`X_{p,i}`$ $`=X_i`$
if $`R=_p`$, or, in case $`R`$,
(2.3b) $`X_{p,i1}`$ $`X_i`$
for all $`p`$ not invertible in $`R`$. Then the following “Atiyah–Bredon sequence” is exact:

(2.4)
$$0H_T^{}(X)H_T^{}(X_0)H_T^{+1}(X_1,X_0)\mathrm{}H_T^{+n}(X_n,X_{n1})0.$$

More generally, if condition (2.3a) or (2.3b) holds for all $`ik`$, then one still has exactness for

(2.5)
$$0H_T^{}(X)H_T^{}(X_0)H_T^{+1}(X_1,X_0)\mathrm{}H_T^{+k}(X_k,X_{k1}).$$

The content of the Chang–Skjelbred lemma is just exactness of the Atiyah–Bredon sequence at the first terms. Rephrasing Theorem 2.1 for $`k\{0,1\}`$ and integer coefficients, we get:

###### Corollary 2.2.

Assume $`R=`$ and let $`X`$ be a $`T`$-space such that $`H_T^{}(X)`$ is free over $`H^{}(BT)`$. Then

$$0H_T^{}(X)H_T^{}(X_0)$$

is exact. If in addition the isotropy group of each $`xX_1`$ is contained in a proper subtorus of $`T`$ (i. e., if condition (2.3b) holds for $`i1`$), then the following sequence is exact:

$$0H_T^{}(X)H_T^{}(X_0)H_T^{+1}(X_1,X_0).$$

The injectivity of the map $`H_T^{}(X)H_T^{}(X_0)`$ is an immediate consequence of the localization theorem in equivariant cohomology, see Lemma 4.4 below.

The above “proper subtorus condition” is violated in the counterexample given by Tolman–Weitsman \[TW, Sec. 4\] because there all orbits of dimension $`2`$ have isotropy group $`_2\times _2S^1\times S^1`$. The full condition (2.3b) can be stated analogously: For $`R=`$ the isotropy group $`T_x`$ of any $`xX`$ must be contained in a subtorus of dimension $`dimT_x+1`$.

###### Remark 2.3.

In some cases general criteria guarantee the freeness of $`H_T^{}(X)`$ over $`H^{}(BT)`$, for instance if $`H^{}(X)`$ is free over $`R`$ and concentrated in even degrees (Leray–Hirsch). Assume that $`H^{}(X)`$ is free over $`R`$. Then $`H_T^{}(X)`$ is free over $`H^{}(BT)`$ if $`X`$ is a compact Kähler manifold with $`X^T\mathrm{}`$ (for example, a smooth projective $`(^\times )^n`$-variety) \[Bl, Thm. II.1.2\] or if $`X`$ is a compact Hamiltonian $`T`$-manifold \[F\]. If all isotropy groups of $`X`$ are connected, then the exactness of the Atiyah–Bredon sequence with integer coefficients can be characterized by a homological condition on $`H_T^{}(X)`$, see \[FP\].

## 3. Isotropy groups

Before proving Theorem 2.1, we want to reformulate the conditions (2.3a) and (2.3b) on the equivariant skeletons in algebraic terms. In the sequel, we will refer to (2.3a) and (2.3b) together as condition (2.3). Notice that this condition is always satisfied for $`R=`$.

For any closed subgroup $`T^{}T`$ there is an isomorphism $`T(S^1)^n`$ and a divisor chain $`m_q\left|m_{q1}\right|\mathrm{}|m_1`$ such that $`T^{}`$ corresponds to the subgroup

(3.1)
$$_{m_1}\times \mathrm{}\times _{m_q}\times (S^1)^r(S^1)^n.$$

(To see this, consider the inverse image of $`T^{}`$ under the exponential map $`\mathrm{exp}:𝔱T`$ and compare it with the lattice $`\mathrm{exp}^1(1)`$.)

Recall that the dimension of a module $`M`$ over a ring $`S`$ is the Krull dimension of $`S/\mathrm{Ann}M`$, that is, the length of a maximal chain $`𝔭_0𝔭_1\mathrm{}`$ of prime ideals in $`S`$, all containing the annihilator $`\mathrm{Ann}M`$ of $`M`$. We denote the dimension of $`R`$ over itself by $`d`$. Hence, $`d=0`$ if $`R`$ is a field, and $`d=1`$ if $`R`$. Since $`R`$ is a PID, the dimension of a polynomial ring $`R[t_1,\mathrm{},t_s]`$ is $`d+s`$ \[S, Prop. III.13\].

###### Lemma 3.1.

Let $`T^{}T`$ be a closed subgroup and let $`s`$ be the number of $`m_j`$’s in the decomposition (3.1) which are not invertible in $`R`$. Then

$$dim_{H^{}(BT)}H^{}(BT^{})=\{\begin{array}{cc}r+s\hfill & \text{if }R\text{ is a field or }s>0\text{,}\hfill \\ r+1\hfill & \text{if }R\text{ and }s=0\text{.}\hfill \end{array}$$

###### Proof.

The $`H^{}(BT)`$-action on $`H^{}(BT^{})`$ comes from the algebra map induced by the inclusion $`T^{}T`$. Hence, the dimension of the $`H^{}(BT)`$-module $`H^{}(BT^{})`$ is equal to the Krull dimension of the (evenly graded) image $`A`$ of $`H^{}(BT)`$ in $`H^{}(BT^{})`$.

We choose isomorphisms $`H^2(BS^1)R[t]`$ and $`H^2(B_m)R[t]/mt`$ such that the map $`H^2(BS^1)H^2(B_m)`$ corresponds to the canonical quotient map $`R[t]R[t]/mt`$. By the Künneth theorem for cohomology, we find

$`A`$ $`H^2(B_{m_1})\mathrm{}H^2(B_q)H^2(BS^1)^r`$
$`R[t_1,\mathrm{},t_q,t_1^{},\mathrm{},t_r^{}]/(m_1t_1,\mathrm{},m_qt_q)`$
$`=R[t_1,\mathrm{},t_s,t_1^{},\mathrm{},t_r^{}]/(m_1t_1,\mathrm{},m_st_s)`$
since $`m_{s+1}`$, …, $`m_q`$ are invertible in $`R`$.

$`R`$, a field or $`s=0`$: then $`AR[t_1,\mathrm{},t_s,t_1^{},\mathrm{},t_r^{}]`$, so the assertion is clear.

$`R`$ and $`s>0`$: An ascending chain of prime ideals in $`A`$ of length $`k`$ is the same as an ascending chain $`𝔭_0\mathrm{}𝔭_k`$ of prime ideals in $`B=R[t_1,\mathrm{},t_s,t_1^{},\mathrm{},t_r^{}]`$ with $`(m_1t_1,\mathrm{},m_st_s)𝔭_0`$. Since one can clearly find such a chain of length $`r+s`$, we have to show that there are no longer chains. If $`𝔭_0`$ contains some prime factor $`p`$ of $`m_s`$, then $`B/𝔭_0`$ is a quotient of $`_p[t_1,\mathrm{},t_s,t_1^{},\mathrm{},t_r^{}]`$, which is of dimension $`r+s`$. Otherwise, $`t_s𝔭_0`$ and $`B/𝔭_0`$ is a quotient of $`R[t_1,\mathrm{},t_{s1},t_1^{},\mathrm{},t_r^{}]`$, which by induction has again dimension $`r+s`$. In any case, we find that $`kr+s`$. ∎

###### Proposition 3.2.

The conditions (2.3) for all $`ik`$ are equivalent to the conditions

(3.2)
$$xXdim_{H^{}(BT)}H^{}(BT_x)d+nixX_i$$

for all $`ik`$.

###### Proof.

$`R=`$: Since the dimension of $`H^{}(BT_x)`$ is just the rank of $`T_x`$, condition (3.2) holds for all spaces, as does (2.3).

$`R=_p`$: By Lemma 3.1, condition (3.2) means that the rank of the maximal $`p`$-torus contained in $`T_x`$ equals the dimension of $`T_x`$ for $`xX_k`$, and differs by at most $`ik1`$ for $`xX_iX_{i1}`$, $`i>k`$. This is equivalent to $`X_{p,i}=X_i`$ for $`ik`$.

$`R`$: Here condition (3.2) translates into the following: for each non-invertible prime $`p`$ the rank of the maximal $`p`$-torus in $`T_x`$ differs by at most $`1`$ from the dimension of $`T_x`$ for $`xX_k`$, and by at most $`ik`$ for $`xX_iX_{i1}`$, $`i>k`$. This is the same as saying $`X_{p,i1}X_i`$ for all $`ik`$. ∎

Note that conditions (3.2) are always true in $`K`$-theory (see \[A, (7.1)\]), essentially because the representation ring of a finite group is a finitely generated $``$-module.

## 4. Proof of Theorem 2.1

Before starting in earnest, we remark that our assumptions on $`X`$ imply that all $`R`$-modules $`H^{}(X_j,X_i)`$, $`ji`$, are finitely generated, hence so are the $`H^{}(BT)`$-modules $`H_T^{}(X_j,X_i)`$. (Use the usual long exact sequences for the first claim. For equivariant cohomology, the proof given in \[AP, (3.10.1)\] for $`R=`$ still applies.)

The sequences (2.4) and (2.5) are exact if and only if for all $`i0`$ (respectively $`0ik`$) the sequence (2.1) splits into short exact sequences

(4.1)
$$0H_T^{}(X,X_{i1})H_T^{}(X_i,X_{i1})H_T^{+1}(X,X_i)0,$$

i. e., if and only if the inclusion of pairs $`(X,X_{i1})(X,X_i)`$ induces the zero map in cohomology. (See \[FP, Lemma 4.1\].)

Let $`M`$ be a graded $`H^{}(BT)`$-module. Then any prime ideal associated with $`M`$ is homogeneous, i. e., generated by its homogeneous elements \[BH, Lemma 1.5.6\], hence contained in some maximal homogeneous ideal $`𝔪`$. This implies $`M=0`$ if and only if $`M_𝔪=0`$ for all maximal homogeneous ideals $`𝔪H^{}(BT)`$. It suffices therefore to prove exactness after localizing at such an ideal $`𝔪`$. Note that it always contains $`H^{>0}(BT)`$. From now on all localized modules will be over the regular local ring $`A=H^{}(BT)_𝔪`$, whose maximal ideal we denote by $`𝔪_A`$.

By induction on $`i0`$ (resp. $`0ik`$), we show:

###### Claim 4.1.

The sequence (4.1) is exact, and $`H_T^{}(X,X_i)_𝔪`$ is zero or a Cohen–Macaulay module of dimension $`d+ni1`$.

Recall that the *depth* of a finitely generated $`A`$-module $`M`$ is the maximal length of an $`M`$-regular sequence in the maximal ideal $`𝔪_A`$. An $`M`$-regular sequence is a sequence $`a_1`$, …, $`a_l𝔪_A`$ such that $`(a_1,\mathrm{},a_l)MM`$ and such that $`a_j`$ is not a zero divisor on $`M/(a_1,\mathrm{},a_{j1})M`$ for all $`jl`$. One always has

(4.2)
$$\mathrm{depth}MdimM;$$

if $`M0`$ and

(4.3)
$$\mathrm{depth}M=dimM,$$

then $`M`$ is called *Cohen–Macaulay*. (We use \[S\] and \[BH\] as references for commutative algebra. The reader might also find the summary of results in \[AP, App. A\] helpful. They were compiled with applications in equivariant cohomology in mind.)

We start the proof with several lemmas. The first two are standard.

###### Lemma 4.2.

Let $`0UMN0`$ be an exact sequence of $`A`$-modules. Then

$$\mathrm{depth}N\mathrm{min}\{\mathrm{depth}U1,\mathrm{depth}M\}.$$

###### Proof.

Since

$$\mathrm{depth}M=inf\{i:\mathrm{Ext}^i(K,M)0\},$$

where $`K`$ denotes the residue field of $`A`$, the assertion follows from the long exact sequence

$$\mathrm{}\mathrm{Ext}^i(K,U)\mathrm{Ext}^i(K,M)\mathrm{Ext}^i(K,N)\mathrm{Ext}^{i+1}(K,U)\mathrm{}.\mathit{}$$

###### Lemma 4.3.

Let $`M`$ be a Cohen–Macaulay $`A`$-module. If $`UM`$ is a non-zero submodule, then $`dimU=dimM`$.

###### Proof.

Choose a prime ideal $`𝔭`$ associated to $`U`$, hence also to $`M`$. Since $`M`$ is Cohen–Macaulay, we have $`dimA/𝔭=dimM`$ by \[S, Prop. IV.13\]. On the other hand, $`dimA/𝔭dimUdimM`$. ∎

###### Lemma 4.4.

For all $`ik`$ one has $`dimH_T^{}(X,X_i)d+ni1`$.

###### Proof.

This follows from the localization theorem in equivariant cohomology: For a prime ideal $`𝔭H^{}(BT)`$, define $`X^𝔭=\{xX:𝔭\mathrm{Ann}H^{}(BT_x)\}.`$ The localization theorem asserts that the inclusion $`X^𝔭X`$ induces an isomorphism

$$H_T^{}(X)_𝔭=H_T^{}(X^𝔭)_𝔭,$$

see for example \[AP, Sec. 3.2\]. An analogous formula holds for relative cohomology.

Now assume that $`dimH_T^{}(X,X_i)d+ni`$. This means that there is a prime ideal $`𝔭\mathrm{Ann}H_T^{}(X,X_i)`$ such that $`dimH^{}(BT)/𝔭d+ni`$. Hence $`dimH^{}(BT_x)d+ni`$ for any $`xX^𝔭`$. By Proposition 3.2, this implies $`xX_i`$, i. e., $`X^𝔭X_i`$. The localization theorem now gives

$$H_T^{}(X,X_i)_𝔭=H_T^{}(X^𝔭,X_i^𝔭)_𝔭=H_T^{}(X^𝔭,X^𝔭)_𝔭=0.$$

But this is impossible because for any prime ideal $`𝔭`$ one has $`𝔭\mathrm{Ann}H_T^{}(X,X_i)`$ if and only if $`H_T^{}(X,X_i)_𝔭0`$ \[S, Prop. I.3\]. (Here we are using that $`H_T^{}(X,X_i)`$ is finitely generated over $`H^{}(BT)`$.) Hence $`dimH_T^{}(X,X_i)d+ni1`$. ∎

###### Lemma 4.5.

For all $`i0`$ one has $`\mathrm{depth}H_T^{}(X_i,X_{i1})_𝔪ni`$.

###### Proof.

Each $`xX_iX_{i1}`$ is fixed by exactly one $`(ni)`$-dimensional torus $`T_\alpha T`$. Because $`X`$ has only finitely many orbit types, we can write $`X_iX_{i1}`$ as the disjoint union of finitely many subsets $`Y_\alpha =(X_iX_{i1})^{T_\alpha }`$. Since $`\overline{Y}_\alpha Y_\alpha X_{i1}`$, a Mayer–Vietoris argument gives

$$H_T^{}(X_i,X_{i1})=\underset{\alpha }{}H_T^{}(\overline{Y}_\alpha ,\overline{Y}_\alpha X_{i1}).$$

(Recall that with respect to Alexander–Spanier cohomology, the Mayer–Vietoris sequence is exact for all pairs of closed subspaces, cf. \[M, Sec. 8.6\].)

We have

$$M:=H_T^{}(\overline{Y}_\alpha ,\overline{Y}_\alpha X_{i1})=H_{T/T_\alpha }^{}(\overline{Y}_\alpha ,\overline{Y}_\alpha X_{i1})_RH^{}(BT_\alpha )$$

because $`\overline{Y}_\alpha `$ is fixed by $`T_\alpha `$. A sequence of generators $`x_1`$, …, $`x_{ni}H^2(BT_\alpha )𝔪`$ clearly is $`M_𝔪`$-regular. Hence

$$\mathrm{depth}M_𝔪ni.$$

The description of depth via $`\mathrm{Ext}`$ (cf. the proof of Lemma 4.2) shows that the depth of a direct sum is the minimum of the depths of the summands. This gives the result. ∎

We now prove Claim 4.1 by induction on $`i`$, assuming that $`H_T^{}(X,X_{i1})_𝔪`$ is zero or a Cohen–Macaulay module of dimension $`d+ni`$. For $`i=0`$ this is true because we assume $`H_T^{}(X,X_1)=H_T^{}(X)`$ to be free over the regular ring $`H^{}(BT)`$.

In the case $`H_T^{}(X,X_{i1})_𝔪=0`$ the sequence (2.1) splits into short exact sequences for trivial reasons. Suppose therefore that $`H_T^{}(X,X_{i1})_𝔪`$ is non-zero and Cohen-Macaulay of dimension $`d+ni`$. Since

(4.4)
$$dimH_T^{}(X,X_i)_𝔪dimH_T^{}(X,X_i)d+ni1$$

by Lemma 4.4 and $`dimH_T^{}(X,X_{i1})_𝔪=d+ni`$, the image of $`H_T^{}(X,X_i)_𝔪`$ in $`H_T^{}(X,X_{i1})_𝔪`$ has lower dimension than the target module, hence is zero by Lemma 4.3. In other words, (4.1) is exact in this case as well.

Lemma 4.2 now gives

(4.5)
$$\mathrm{depth}H_T^{}(X,X_i)_𝔪d+ni1$$

since $`\mathrm{depth}H_T^{}(X_i,X_{i1})_𝔪ni`$ by Lemma 4.5 and $`\mathrm{depth}H_T^{}(X,X_{i1})_𝔪=d+ni`$ (or infinity if $`H_T^{}(X,X_{i1})_𝔪=0`$).

Comparing (4.4) and (4.5) with the inequality (4.2) finishes the proof.

## 5. Actions without fixed points

The Atiyah–Bredon sequence (2.4) can never be exact if $`T`$ acts without fixed points (unless $`X=\mathrm{}`$). Yet there are interesting fixed-point-free actions. In the context of compact differentiable $`T`$-manifolds and real coefficients, Goertsches and Töben \[GT\] observed that one can modify (2.4) to accommodate for this case. We briefly comment on such a generalization in our setting.

###### Proposition 5.1.

Let $`k`$ be the minimal dimension of the $`T`$-orbits in $`X`$. If $`X`$ satisfies condition (2.3), then $`dimH_T^{}(X)=d+nk`$.

###### Proof.

Since $`X_{k1}=\mathrm{}`$, we have $`dimH_T^{}(X)d+nk`$ by Lemma 4.4.

For the reverse inequality, pick an $`xX_k`$, say with isotropy group $`T^{}`$. The map $`H^{}(BT)H^{}(BT^{})`$ factors through the map $`H_T^{}(X)H_T^{}(Tx)=H^{}(BT^{})`$ induced by the inclusion $`TxX`$. This implies $`\mathrm{Ann}H_T^{}(X)\mathrm{Ann}H^{}(BT^{})`$, hence $`dimH_T^{}(X)dimH^{}(BT^{})`$. But, under condition (2.3), Lemma 3.1 gives $`dimH^{}(BT^{})=d+nk`$. ∎

A finitely generated graded module $`M`$ over $`H^{}(BT)`$ is called *Cohen–Macaulay* if $`M_𝔪`$ is Cohen–Macaulay over $`H^{}(BT)_𝔪`$ for all maximal ideals $`𝔪\mathrm{Supp}M`$. If $`M`$ is free over $`H^{}(BT)`$, then it is Cohen–Macaulay of maximal dimension $`d+n`$ (cf. the proof of Claim 4.1). We remark in passing that the converse holds as well, even if $`R`$ is not a field: The Auslander–Buchsbaum formula \[BH, Thm 1.3.3\] together with \[S, Cor. IV.C.2\] implies that $`M`$ is projective; freeness then follows from the (comparatively easy) analogue of the Quillen–Suslin theorem for finitely generated *graded* modules over polynomial rings with coefficients in a PID \[L, Cor. 4.7\].

###### Theorem 5.2.

Let $`k`$ be the minimal dimension of the $`T`$-orbits in $`X`$. If $`H_T^{}(X)`$ is Cohen–Macaulay over $`H^{}(BT)`$ and $`X`$ satisfies condition (2.3), then the following sequence is exact:

$$0H_T^{}(X)H_T^{}(X_k)H_T^{+1}(X_{k+1},X_k)\mathrm{}H_T^{+n}(X_n,X_{n1})0.$$

The only change to the proof of Theorem 2.1 is that the induction now starts at $`i=k`$, which is the dimension of $`H_T^{}(X)`$ by Proposition 5.1.


text:
# Magnetic Properties of Yb2Mo2O7 and Gd2Mo2O7 from rare earth Mössbauer Measurements

## I Introduction

In the rare earth pyrochlores R2T2O7 (R is a trivalent rare earth, T a tetravalent transition or sp metal ion), each of the two cationic sublattices forms a network of corner sharing tetrahedra . For this arrangement, each sublattice is prone to geometrically derived magnetic frustration , with the behaviour in each particular compound depending on the sign, size and anisotropy of the interionic couplings. The main signatures of magnetic frustration are the absence of long range order and the persistence of dynamic short range magnetic correlations as $`T0`$.

The rare earth molybdates R2Mo2O7 may be formed with the rare earths from Nd3+ to Lu3+. For R from Nd to Gd, they show metallic-like behaviour, whereas for R from Dy to Lu (and with Y), they show semiconducting behaviour with an activation energy of the order of 15 meV . The change in behaviour (“metal-semiconductor crossover”) is chiefly linked with changes within the Mo-O subsystem and it has been related to variations in the Mo-O bond lengths associated with the changing lattice parameter (lanthanide contraction)  and in the Mo-O-Mo bond angles . The metal-semiconductor crossover also leads to profound changes in the magnetic properties. In the semiconducting compounds, the Mo intra-sublattice coupling is antiferromagnetic , whereas in the metallic compounds, it is ferromagnetic .

In the R2Mo2O7, the dominant exchange interaction is that within the d-ion sublattice. The next most important interaction is the inter-sublattice exchange with the interaction within the f-ion sublattice the weakest of the three. For the d-ion sublattice, the dominant exchange mechanism is different either side of the metal-semiconductor crossover. In the semiconducting compounds, antiferromagnetic superexchange prevails whereas in the metallic compounds, the direct ferromagnetic coupling involving the Mo 4d-spin density at the Fermi level dominates . An important feature controlling the properties of most of the R3+ ions and the way they are magnetised through coupling with the Mo4+ sublattice is the crystal field interaction, which fashions the wave functions of the R3+ ground state. This consideration does not concern the S-state Gd3+ ion which is essentially immune to the influence of crystal fields.

In Y2Mo2O7 , as in the other semiconducting molybdates, the Mo-Mo interaction is antiferromagnetic. A magnetic irreversibility occurs at 22 K evidencing a spin-glass-like transition . This was a surprising result for a compound which seemed to be crystallographically ordered. Recent structural studies have shown, however, that the Mo-Mo (and some of the Y-O) bond lengths are disordered , raising the possibility that the spin-glass-like transition is linked to the disorder and frustration. 89Y nuclear magnetic resonance measurements have confirmed the presence of lattice disorder . Magnetic frustration is clearly operative in Y2Mo2O7: the spin fluctuations associated with the short range correlated Mo spins do not die out as T $``$ 0, but rather tend to a temperature independent rate  and neutron scattering measurements have shown that the spin-glass-like transition occurs mainly in the frequency domain . In Gd2Mo2O7, as in the other metallic molybdates, the Mo-Mo interaction is ferromagnetic. A transition occurs with a temperature that depends on the sample ($`T_C55`$ K in Refs. and $``$ 65 K in Ref.), and it is accompanied by a magnetic irreversibility. Little information is available concerning the possible influence of frustration in this compound although specific heat measurements down to $``$ 1.8 K have suggested that the low energy tail of the density of magnetic excitations does not tend to zero .

We present a study of semiconducting Yb2Mo2O7 and metallic Gd2Mo2O7 based chiefly on rare earth Mössbauer measurements (respectively using the isotopes 170Yb and 155Gd) down to $``$ 30 mK. Magnetic measurements were also made for the two compounds, and 172Yb perturbed angular correlation (PAC) were carried out for Yb2Mo2O7 up to $``$ 1000 K. We obtain information concerning the static and dynamic magnetic properties of the rare earths and concerning the ordering and spin-dynamics of the Mo4+ sub-lattice and its coupling with the R3+ sublattices. Making use of the microscopic nature of the Mössbauer probes, we discuss the information obtained concerning local symmetry lowering and bond disorder in the two compounds, which are a priori expected to be crystallographically ordered.

After outlining some background properties of the two samples in section II, we present the results concerning Yb2Mo2O7 in section III and concerning Gd2Mo2O7 in section IV. Section V contains the summary and discussion.

## II Samples and background rare earth single ion properties.

The polycrystalline samples of Yb2Mo2O7 and Gd2Mo2O7 were prepared by first reacting Mo and MoO3 in a sealed container to form MoO2 which was then reacted under argon with the R2O3. Room temperature X-ray diffraction measurements show both samples are single phase and provide the cubic lattice parameter: 10.146Å (Yb2Mo2O7) and 10.366Å (Gd2Mo2O7).

The cubic pyrochlore structure (space group Fd$`\overline{3}`$m) contains eight formula units per unit cell. The R3+ ions situated at the 16b sites (point symmetry: $`\overline{3}`$m), form a network of corner sharing tetrahedra. Each of the four R3+ making up a tetrahedron has its local symmetry axis along one of the  directions. The Mo4+ situated at the 16d sites (point symmetry: $`\overline{3}`$m), also form a network of corner sharing tetrahedra which is displaced by (1/2,1/2,1/2) relative to that of the R3+.

Yb3+ (4f13) has 8 sublevels in its spin-orbit derived ground state (2F7/2). The degeneracy is partially lifted by the crystal electric field to leave four Kramers doublets. In an isomorphous pyrochlore (Yb2Ti2O7), the total energy separation of the four doublets is about 1000 K and the well isolated ground state Kramers doublet has planar anisotropy with the easy magnetisation plane lying perpendicular to the appropriate local  direction .

Gd3+ (4f7) is an S-state ion (8S7/2). Both its anisotropy and the amount of crystal field degeneracy lifting within the 8 sublevels of the ground state are quite small. In the context of the present study, this ground state can be taken to be an initially degenerate S=7/2 state, whose degeneracy is lifted only by a molecular or applied magnetic field.

## III Yb2Mo2O7

### A Susceptibility and magnetisation measurements.

The magnetic susceptibility of Yb2Mo2O7 was measured from 300 to 2 K. Both the field cooled (FC) and zero field cooled (ZFC) variations change monotonically as the temperature is lowered and there is a small irreversibility with an onset in the range 16 - 18 K (Fig.1).

To obtain a more accurate value for the irreversibility temperature $`T_{irr}`$, we measured the thermo-remanent magnetisation (TRM) after field cooling with 5 T down to 2 K (Fig.1). We then obtain $`T_{irr}`$ = 17.0 K. The size of the low field irreversibility as evidenced by the difference between the the FC and ZFC branches, is quite small and it is somewhat different to that observed in Y2Mo2O7. The question then arises as to the nature of the transition occurring at $`T_{irr}`$. We first note that cases are known where antiferromagnetic (AF) ordering takes place without giving rise to an anomaly in the magnetic susceptibility (see for instance, Ref. for the case of the Yb pnictides). Thus, the fact that there is no strong anomaly does not in itself represent evidence against the existence of low temperature magnetic order or correlations. In fact, as is described in section III B, at temperatures below $`T_{irr}`$, the 170Yb Mössbauer data evidence Yb3+ magnetic hyperfine fields and Yb3+ magnetic moments which are produced through Mo-Yb exchange. $`T_{irr}`$ could then correspond to a change in the length scale and/or in the fluctuation rate of the correlations within the Mo sublattice.

The value of $`T_{irr}`$ can be linked to one of two possible scenarios. First, that frustation does not play a major role so that $`T_{irr}`$ directly corresponds to the strength of the molecular field interaction within the Mo4+ sublattice. Second, that frustration is operative and in common with the typical behaviour of frustrated compounds, the temperature of the transition ($`T_{irr}`$) is much smaller than the temperature equivalent to the strength of the Mo-Mo coupling. We examine the two possibilities in turn. For the first case, we analyse the inverse susceptibility 1/$`\chi `$ between 20-100 K (Fig.2) in terms of the molecular field approximation. In this temperature range, 1/$`\chi `$ shows a quasi-linear thermal dependence, with a small background curvature due to the influence of the three Yb3+ Kramers doublet excited crystal field levels which have energies up to $``$ 1000 K (see section III C). Below 100 K, only the ground crystal field Yb3+ doublet is appreciably populated and it is described by an effective spin 1/2 and a crystal field derived spectroscopic g-tensor. As Yb2Mo2O7 is an insulator, an ionic description for the Mo4+ ion, i.e. S=1 and a g-factor close to 2, should be adequate. We assume the following hierarchy of exchange interactions: a dominant Mo-Mo coupling which is AF and a smaller Mo-Yb exchange, with a molecular field constant $`\lambda `$. For a two magnetic sublattice system in the paramagnetic region, the molecular field theory leads to a ferrimagnetic-like inverse susceptibility:

$$\frac{1}{\chi }=\frac{T(T+T_N)\lambda ^2C_{Mo}C_{Yb}}{T(C_{Mo}+C_{Yb})+2\lambda C_{Mo}C_{Yb}+C_{Yb}T_N},$$
(1)
where $`C_{Mo}`$ and $`C_{Yb}`$ are the Curie constants respectively of Mo4+ and Yb3+. Setting $`T_N=T_{irr}=17`$ K, expression (1) reproduces the main features of the thermal variation of 1/$`\chi `$ (solid line in Fig.2) with a Mo4+ g-value of 1.9(1) (close to the ionic value appropriate for a high spin Mo4+ ion) and an average Yb3+ g-value of 3.2(2). This latter value is coherent with the average saturated magnetic moment of 1.7 $`\mu _B`$ measured by 170Yb Mössbauer spectroscopy (see section III B). The Mo-Yb exchange constant $`\lambda `$ derived from this analysis is antiferromagnetic, and its value lies in the range from $`0.82`$ to $`2.20`$ T/$`\mu _B`$. This yields a mean saturated molecular field acting on the Yb3+ ion of 2.75 T and a mean Yb-Mo exchange energy of about 3 K. In agreement with this analysis, the direct extrapolation of the inverse susceptibility (Fig.2) leads to a paramagnetic Curie-Weiss temperature with a value in the range -5 to -10 K (AF interaction). The AF nature of the correlations is confirmed by two aspects of the magnetisation measurements which are shown in the inset of Fig.2 : the increase of the moment with applied field is relatively slow and at 2 K, saturation is not achieved in a field of 5 T.

The possibility that the strength of the Mo - Mo sublattice interaction is very much bigger than that corresponding to $`T_{irr}`$ is based, for the moment, only on the analogy with the situation in Y2Mo2O7. In this case, muon spin relaxation ($`\mu `$SR) , neutron diffraction  and unpublished high temperature susceptibility measurements quoted in Ref.  all point to the presence of a Mo - Mo interaction which is much bigger than that corresponding to $`T_{irr}`$. It is not feasible to access the Mo - Mo interaction in Yb2Mo2O7 from high temperature susceptibililty measurements because of the temperature dependent contribution coming from the Yb3+ excited crystal field levels. To our knowledge, no $`\mu `$SR or neutron diffraction measurements have yet been carried out on Yb2Mo2O7.

### B 170Yb Mössbauer measurements.

The 170Yb Mössbauer absorption measurements were made over the temperature range 95 to 0.036 K using a source of TmB12 and a triangular velocity sweep. For 170Yb, the ground nuclear state has a spin Ig = 0, the excited nuclear state has a spin Iex = 2 and a quadrupole moment $`Q=2.11`$ b, and Eγ = 84.3 keV and 1 cm/s corresponds to 680 MHz.

In the upper part of the examined temperature range, the spectra are well described in terms of quadrupole hyperfine interactions, showing that in this region, the Yb3+ ions are paramagnetic. As exemplified by the data at 50 K on Fig. 3, we find that an acceptable data fit cannot be obtained if the quadrupole hyperfine interaction is taken to have the axial symmetry that is characteristic of the rare earth site in the standard pyrochlore structure. To obtain a good quality data fit, it is necessary both to introduce an asymmetry parameter ($`\eta `$) and to allow the principal component $`V_{ZZ}`$ of the electric field gradient tensor to show a distribution. We find $`\eta `$ = 0.6 and with a Gaussian shaped distribution, we obtain a mean value: eQVZZ/8 = 1.3 mm/s and a root mean square deviation: $`\sigma `$ 0.4 mm/s. The microscopic Mössbauer probe measurements thus identify two aspects of the local structure of Yb2Mo2O7: the point symmetry at the Yb site is non-axial and there is a distribution of environments indicating that significant disorder is present. Lattice disorder has previously been evidenced in the isomorphous semiconducting compound Y2Mo2O7 by X-ray absorption edge  and 89Y nuclear magnetic resonance  measurements. There was no evidence of any significant departure from full oxygen stoichiometry nor of site exchange and it was suggested that the disorder principally involved the Mo-Mo pair distances with also some modest disorder in the Y-O(1) distances . It seems likely that an analogous situation will also pertain in Yb2Mo2O7 and that the anomalous characteristics of the quadrupole hyperfine interaction reported here are linked to lattice disorder involving some of the bond lengths and angles.

At low temperatures, magnetic hyperfine splittings are visible (Fig.3). Such splittings appear when the Yb3+ moments are either long or short range magnetically correlated and when any fluctuation of the correlated moments occurs at frequencies of the order of or below the 170Yb Mössbauer threshold value $``$ 3.0 $`\times `$108 s-1. We first consider the data at 0.036 K. The overall shape of the spectrum and in particular the inhomogeneous broadenings of the 5 lines, point to the presence of a distribution in hyperfine field and quadrupolar coupling parameter values. This is coherent with the analysis of the data in the paramagnetic region, which evidenced a distribution of quadrupole hyperfine interactions. Both distributions can be linked to distribution in the Yb3+ ground state wave functions which results from the local disorder. In presence of random disorder, it can be shown that the distributions in the hyperfine field and quadrupolar parameters are linearly correlated . Using linearly correlated distributions, we obtain good data fits (Fig.3) and these provide the mean 170Yb hyperfine field and the root mean square deviation of the distribution. The saturated values at 0.036 K are respectively 175 T and 45 T. The mean saturated Yb3+ magnetic moment value is therefore 1.7 $`\mu _B`$, using the standard 170Yb3+ relation: 1$`\mu _B`$ corresponds to 102 T.

The spectra become less resolved as the temperature increases (Fig.3). Reliable fits in terms of a distribution of hyperfine fields are possible only up to 10 K. The thermal variation of the mean Yb3+ moment is shown on Fig.4. The theoretical curve is obtained assuming that the Yb3+ ground doublet, with effective spin 1/2 and spectroscopic factor g, is polarised by the molecular field $`H_{ex}`$ due to Mo-Yb exchange. In order to calculate Hex(T), which is proportional to the Mo moment within a molecular field model, we assume that the thermal variation of the Mo moment follows the mean field law for S=1. Then the reduced exchange field $`\sigma (T)=H_{ex}(T)/H_{ex}(0)`$ is obtained by solving the self-consistent equation:

$`\sigma (T)=_1\left({\displaystyle \frac{3S}{S+1}}{\displaystyle \frac{\sigma (T)}{\tau }}\right),`$ (2)
where $`_1`$ is the Brillouin function for S = 1 and $`\tau =T/T_N`$. The solid line in Fig.4 is obtained with TN = 17 K and $`H_{ex}(0)=3`$ T, corresponding to an exchange energy of 3.4 K. This value is in good agreement with that derived from the analysis of the susceptibility data (section III A).

Although no reliable values can be obtained for the hyperfine field as the temperature is increased above $``$ 10 K, it is clear that correlated Yb3+ magnetic moments are still present. In fact, the lineshapes also show that some correlations persists above 17 K. Both just above and just below the irreversibility temperature, the Mössbauer line shapes are compatible with the presence of dynamic magnetic correlations.

### C 172Yb perturbed angular correlation (PAC) measurements.

The PAC measurements provide the thermal dependence of the absolute value of the quadrupole hyperfine interaction at the 172Yb nucleus . They were made over the range 34 to 965 K, that is at temperatures above the range where magnetic correlations are present. Three examples of the spectra are shown in Fig. 5.

The strong damping of the $`R(t)`$ oscillations visible in Fig. 5 is very characteristic of a hyperfine interaction which is distributed in size. The spectra cannot be fitted in terms of a single quadrupole interaction at any temperature and it is necessary to allow for a distribution of the fitted electric field gradient. This observation reinforces the same conclusion obtained from the 170Yb Mössbauer analysis.

It turns out that in presence of this distribution, the PAC data are not very sensitive to the asymmetry parameter $`\eta `$. The PAC technique thus cannot provide independent evidence confirming the conclusion of the 170Yb Mössbauer analysis that this parameter is non-zero. The thermal variation of the mean absolute value of $`V_{ZZ}`$ and of $`\sigma `$ the width of its Gaussian distribution are shown in Fig. 6. The total interaction is made up of two parts, one which is temperature dependent arising from the Yb3+ 4f shell, and one which is essentially temperature independent arising from the lattice charges. At low temperatures, the 4f electron contribution dominates whereas at high temperatures, the total 4f contribution tends to zero and the lattice contribution dominates.

At the lowest measurement temperature, the mean value for $`|V_{ZZ}|`$ agrees with that obtained from the 170Yb Mössbauer analysis. This latter technique also provides the sign of the gradient showing that in the low temperature limit $`V_{ZZ}`$ = -135 V/$`\AA ^2`$. The two techniques also provide essentially the same value for $`\sigma `$, the root mean square deviation of the distribution.

As shown on Fig.6, the electric field gradient also evidences a distribution in the high temperature region of the measurement range. Since the electric field gradient in this region is due chiefly to the surrounding lattice charges, the observation of a distribution directly evidences the presence of lattice disorder. We attribute the fact that the size of the distribution of the electric field gradient is much bigger at low temperatures to the fact that the disorder gives rise to a distribution in the Yb3+ crystal field parameters and wave functions and this leads to an enhanced distribution in the part of the quadrupolar hyperfine interaction linked with the 4f-shell.

Because of the local symmetry lowering, it is impossible to carry out a crystal field analysis of the thermal variation of $`V_{ZZ}`$, such as was done for Yb2Ti2O7. The values for this latter compound, also shown in Fig.6, are different from those in Yb2Mo2O7 showing there are some differences between the Yb3+ crystal field properties of the two compounds. The temperature range over which the gradient continues to vary is however similar in the two cases suggesting the overall crystal field splittings are of comparable magnitudes ($``$ 1000 K) in the two compounds.

## IV Gd2Mo2O7.

### A Susceptibility and magnetisation measurements.

The magnetic susceptibility $`\chi (T)`$ and magnetisation $`m(H)`$ measurements are shown in Fig.7. The sharp rise in $`\chi (T)`$ that occurs at $``$ 80 K (previously observed at $``$ 55 K  and at $``$ 65 K ) suggests the onset of ferromagnetic ordering of the Mo4+ moments. The specific heat shows only a broad anomaly near the temperature of the susceptibility rise, , suggesting the ordering is short range. An irreversibility between the FC and ZFC branches (reported previously ) is observed below 75 K. It is probably chiefly related to the pinning of domain walls by defects.

The rapid initial rise of the magnetisation curves (inset of Fig.7) measured below 60 K also evidences ferromagnetic interactions. At 2.5 K, the quasi-saturated value of the high field magnetisation of 15.8(4) $`\mu _B`$ per formula unit (dashed line in the inset of Fig.7) shows the Gd-Mo coupling is ferromagnetic. The two Gd3+ ions contribute a saturated moment of 14 $`\mu _B`$, and thus each Mo4+ ion carries a moment of 0.9(2) $`\mu _B`$, parallel to that of the Gd3+, as reported previously . This value for the Mo4+ moment is much smaller than that expected assuming a ionic description in terms of high spin 4d2, t2g state with S=1 and g$``$2 ($`2\mu _B`$). Furthermore, our attempts to fit the magnetisation curves within a self-consistent molecular field model assuming an ionic description for Mo4+ as well as for Gd3+ failed even allowing the Mo g-factor to be adjustable. The magnetic properties of the Mo in metallic Gd2Mo2O7 thus appear to be associated rather with exchange coupled 4d electrons with some metallic character.

### B 155Gd Mössbauer measurements.

The 155Gd Mössbauer absorption measurements were made over the temperature range 80 to 0.027 K using a source of SmPd3. The isotope 155Gd has a ground nuclear state with spin Ig = 3/2 and quadrupole moment Q=1.31 barn, and an excited nuclear state with spin Iex = 5/2 and very small quadrupole moment. The transition energy is Eγ = 86.5 keV, and 1 mm/s corresponds to 69.8 MHz. Spectra at some selected temperatures are shown in Fig. 8.

At 80 K, in the paramagnetic phase, the absorption takes the form of a nearly symmetric doublet. It corresponds to a quadrupole hyperfine interaction, with a quadrupolar splitting $`\frac{eQV_{ZZ}}{2}(1+\frac{\eta ^2}{3})^{1/2}5.1`$ mm/s (the negative sign is obtained from the analysis of the line shapes at low temperatures when a hyperfine field is also present and $`\eta `$ is included to allow for possible local symmetry lowering). For the S-state Gd3+ ion, the quadrupole hyperfine interaction is due only to the neighbouring lattice charges. As in other Gd pyrochlores , the interaction is quite large in keeping with the important local structural anisotropy of the rare earth site.

A hyperfine field, proportional to the Gd3+ moment, appears when the temperature is lowered below $``$ 75 K, and this confirms the magnetic transition evidenced by the susceptibility data. In Gd2Mo2O7, the magnetic hyperfine interaction is much smaller than the quadrupole interaction, and the hyperfine field acts only to broaden each of the two absorption lines. At 0.027 K, the saturated hyperfine field is: $`H_{hf}(0)`$19.8 T, which is markedly smaller than that usually found in insulating Gd compounds ($``$30 T). The reduced value of $`H_{hf}(0)`$ in this metallic compound is probably linked to the exchange polarisation of $`s`$-type conduction electrons, which contributes a hyperfine field opposite to that arising from the polarisation of the core $`s`$-electrons by the 4f shell moment. At 0.027 K, the relative intensity of the two absorption lines is different from that at 4.2 K even though the value of the hyperfine field remains essentially the same. The change in the relative intensity at very low temperatures is related to changes in the populations of the sublevels of the 155Gd nuclear ground state and these will be discussed at more length in section IV C.

The asymmetry parameter of the electric field gradient tensor ($`\eta `$) can only be obtained from a 155Gd Mössbauer measurement when a magnetic hyperfine interaction is present. From the 0.027 K spectrum, we obtain $`0.0\eta 0.4`$. Thus, although it is possible that $`\eta `$ is zero as expected for the axially symmetric rare earth site of the standard pyrochlore structure, we cannot discount the possibility (clearly established above for Yb2Mo2O7) that $`\eta `$ is not exactly zero in which case local symmetry lowering is present. Over the whole temperature range, i.e., in both the paramagnetic and magnetically correlated regions, we find the line widths of the individual transitions are $``$ 20% larger than in the compound Gd2Sn2O7 where $`\eta `$ is essentially zero . We attribute the background line broadening in Gd2Mo2O7 to indicate the quadrupolar hyperfine interaction shows a small distribution. Since this interaction arises solely from the electric field gradient created by the lattice charges, the presence of a distribution directly provides evidence for local disorder.

In principle, the analysis of the Mössbauer absorption provides the angle $`\theta `$ between the direction of the magnetic moment and the principal local axis of the electric field gradient tensor (a  direction). The best fit yielded $`\theta `$55 but only marginally poorer quality fits were obtained if $`\theta `$ was assumed to be distributed at random. The reduced sensitivity of the data fits to the direction of the hyperfine field is linked to the fact that the magnetic hyperfine interaction is much smaller than the quadrupole hyperfine interaction. Since the Gd3+ ion is essentially isotropic, the direction of the hyperfine field corresponds to the direction of the exchange field coming from the Mo4+ sublattice. The choice of a unique angle $`\theta `$55 is compatible with a magnetic structure where the Gd3+ and the Mo4+ moments are both aligned close to a  axis. To our knowledge, Gd2Mo2O7 has not been studied by neutron diffraction. Such measurements are, in fact, difficult due to the high neutron absorption cross section of non-enriched Gd. They would be useful in order to check if the moments are aligned towards a  direction and also, in fact, to establish whether the magnetic correlations are short or long range. We recall that a specific heat analysis in Gd2Mo2O7 suggested that there is no long range order  and that in in Nd2Mo2O7, which is also metallic, neutron diffraction measurements showed the magnetic order is long range  and the ferromagnetically coupled Mo4+ moments are aligned close (from 6 to 9) to a  direction.

In their analysis of the magnetic specific heat in Gd2Mo2O7, the authors of Ref. assume that even at very low temperatures, the exchange field experienced by the Gd3+ ion is distributed in size, with a finite weight at zero field. We tried to check this assumption by simulating spectra with such a distribution but no clear conclusion could be reached.

Fig.9 shows the thermal variation of the Gd3+ 4f shell magnetic moment, obtained from the hyperfine field value by scaling, using the relation that the measured saturated hyperfine field of 19.8 T corresponds to a saturated Gd3+ moment of 7 $`\mu _B`$. In order to analyse these data, we assume the usual hierarchy of exchange interactions, in decreasing order: Mo-Mo, responsible for the transition at 75 K, Mo-Gd, responsible for the Gd3+ polarisation below 75 K, and Gd-Gd, which we will neglect here. Then, the Gd3+ magnetic moment at a temperature T is given by:

$`M_{Gd}(T)=M_{Gd}(0)_{7/2}\left({\displaystyle \frac{M_{Gd}(0)H_{ex}(T)}{k_BT}}\right),`$ (3)
where $`_{7/2}`$ is the Brillouin function for S = 7/2 and Hex(T) is the Mo derived exchange field which is obtained by solving Eqn.2 with $`\tau =T/T_C`$ and $`T_C=75`$ K, the Mo4+ ordering temperature. The solid line on Fig.9, which provides a good fit to the experimental data, is obtained with a Mo-Gd exchange field Hex(0) = 5.5 T. The Mo-Gd exchange energy can then be estimated as: $`E_{ex}=M_{Gd}(0)H_{ex}(0)26`$ K. This is smaller than $`T_C`$ and so a posteriori justifies the approximations made in the above calculation. The mean size of the Mo4+ derived field acting on the Gd3+ obtained here is $`30\%`$ lower than that estimated from a specific heat analysis . The fact that a mean field law is able to account for the thermal variation of the Gd moment, whereas it fails to reproduce the magnetisation curves (Fig.7, inset), probably stems from the fact that MGd(T) is not very sensitive to the exact shape of Hex(T), and that for Gd3+ an ionic description is valid.

### C 155Gd Mössbauer evidence for persisting T $``$ 0 magnetic fluctuations.

The evidence for the persistence of the magnetic fluctuations is based on the analysis of the relative intensities of the Mössbauer absorption lines of the 27 mK data on Fig.8. We have described this approach previously  for the case of the pyrochlore Gd2Sn2O7 and recall the main features. For the values of the saturated magnetic and quadrupole hyperfine interactions established above, the four hyperfine levels of the 155Gd I = 3/2 ground state span an energy range of 20 mK. Below $``$ 100 mK, the relative populations of these levels will differ from the equipopulated values that pertain at higher temperatures and this leads to changes in the relative intensities of the absorption lines. By measuring these relative intensities on the low temperature spectrum, it is possible to obtain the effective temperature of the hyperfine levels, which in conventional magnetically ordered magnetic compounds corresponds to the temperature of the sample. We find an effective hyperfine level temperature of 47(8) mK (full line fit on Fig.8) which is significantly higher than the measurement probe temperature (27 mK), i.e the lattice temperature of the sample (dashed line on Fig.8). In other words, the steady state populations of the hyperfine levels are not those corresponding to thermal equilibrium. This indicates that at 27 mK, there is a finite Gd3+ spin flip time which is of the same magnitude as the nuclear relaxation time. This approach cannot provide quantitative information concerning the rate of the spin fluctuations since the nuclear relaxation time is unknown. We recall that the good quality data fits on Fig.8 were made with the assumption of a “static” hyperfine field, i.e. a hyperfine field (or Gd3+ magnetic moment) which appears static on the scale of the 155Gd hyperfine Larmor frequency ($``$1.2$`\times 10^8`$ s-1). The low temperature Gd3+ spin fluctuations that are evidenced by the anomalous hyperfine level populations thus occur with frequencies below this value. Since the fluctuations of the Gd3+ moments are driven by the fluctuations of the Mo4+ derived exchange field, this shows the correlated moments of the Mo4+ sublattice also continue to fluctuate at 27 mK.

## V Summary and Discussion.

We have studied the pyrochlore compounds Yb2Mo2O7 and Gd2Mo2O7 by microscopic hyperfine techniques (170Yb, 155Gd Mössbauer and 172Yb perturbed angular correlation spectroscopies) and bulk magnetic measurements and we have obtained information concerning three aspects of their properties : crystallographic disorder, the magnetic interactions and the role of magnetic frustration.

In Yb2Mo2O7, the Yb3+ site symmetry is lower than that of the rare earth site in the standard pyrochlore structure. The distortions are local, since the room temperature X-ray diffraction spectra indicate that the overall cubic lattice symmetry is preserved. In addition, there is considerable lattice disorder. In Gd2Mo2O7, there is no definite evidence of local symmetry lowering but this cannot be excluded and there is some evidence of local disorder.

In semi-conducting Yb2Mo2O7, the Mo-Mo exchange coupling is dominated by an interaction which is antiferromagnetic as is the case in semi-conducting Y2Mo2O7. Based on the analysis of the magnetic susceptibility in the low temperature paramagnetic phase within a molecular field model, the strength of this coupling is of the same order of magnitude as the irreversibility temperature ($`T_{irr}`$ = 17 K). In this case, the Mo-Mo exchange in Yb2Mo2O7 is much smaller than that in Y2Mo2O7. It is possible however, that the Mo-Mo coupling is much bigger than than that correponding to $`T_{irr}`$. Additional studies (for example, in field 57Fe Mössbauer, $`\mu `$SR or neutron diffraction measurements) are needed to investigate this point. At low temperatures, the Yb3+ are magnetically polarised by the field coming from the Mo4+ sublattice. The mean value of the saturated field reaching a Yb3+ is 3 T and the mean value of the saturated Yb3+ moment is 1.7$`\mu _B`$. In metallic Gd2Mo2O7, ferromagnetic correlations dominate, as shown by the saturation of the magnetisation at 2 K and by the sharp rise in the susceptibility at 80 K. Below this latter temperature, the Gd3+ are magnetically polarised by the field coming from the Mo4+ sublattice and the saturated value of this field is 5.5 T.

In Y2Mo2O7, Mo spin fluctuations are known to persist as T $``$ 0 . It seems likely that such fluctuations will also be present in Yb2Mo2O7. Because the hyperfine fields in Yb2Mo2O7 appear static on the 170Yb Mössbauer frequency scale of $``$ 3.0 $`\times `$ 108 s-1, any fluctuations that occur must take place at frequencies that are lower than this value. In Gd2Mo2O7, we find that Gd3+ and Mo4+ spin fluctuations persist as T $``$ 0 so evidencing spin liquid behaviour. The continued influence of frustration is somewhat surprising for it concerns a case where the coupling is ferromagnetic and where no important single ion anisotropy is involved. It is possible that the frustration is linked to the role of further neighbour interactions which are antiferromagnetic.

For both a semi-conducting pyrochlore where the dominant Mo-Mo interaction is anti-ferromagnetic (Y2Mo2O7) and a metallic pyrochlore (Gd2Mo2O7, present results) where the dominant interaction is ferromagnetic, the spin fluctuations persist as T$``$ 0.


text:
# The Chemical Evolution of Magnesium Isotopic Abundances in the Solar Neighbourhood

## 1 Introduction

Magnesium is one of the few elements for which the stellar abundance of individual isotopes can be reliably measured. The relative abundances of Mg isotopes provide a useful probe into the nucleosynthesis history of the Milky Way because they have their origin in different classes of stars. According to standard theories of stellar evolution, most of the Mg isotopes originate from massive stars. The heavy Mg isotopes behave as secondary elements inside massive stars and their production scales with the number of initial “seed” nuclei. Consequently, very little $`{}_{}{}^{25,26}\mathrm{Mg}`$ is synthesised by massive stars until an initial \[Fe/H\] of $``$ $``$1 is reached, whereas the generation of 24Mg operates fairly independently of initial metallicity.

25Mg and $`{}_{}{}^{26}\mathrm{Mg}`$ are detected in metal-poor stars in higher proportions than one would expect if these neutron-rich isotopes originated exclusively from massive stars (Gay & Lambert 2000). Detailed models of the evolution of Mg isotopic ratios find that massive stars alone are insufficient to account for the values of $`{}_{}{}^{25,26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ at low \[Fe/H\], hinting at an additional production site (Timmes et al. 1995; Alibes et al. 2001; Goswami & Prantzos 2000).

Karakas & Lattanzio (2003a,b) have shown that 25Mg and 26Mg production is substantial in metal-poor intermediate-mass stars (IMS). In the low-metallicity regime, asymptotic giant branch (AGB) stars are believed to generate $`{}_{}{}^{25}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$ from alpha capture onto 22Ne triggered by He-shell thermal pulsing. More massive AGB stars (4 $`<`$ $`m`$/M $`<`$ 6) are less common than lower mass stars but may be a significant production site for $`{}_{}{}^{25}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$. Temperatures at the base of the convective envelope in these stars can be high enough to burn $`{}_{}{}^{24}\mathrm{Mg}`$ via hot bottom burning (HBB) as well as synthesise large amounts of $`{}_{}{}^{25}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$. We explore the possibility that AGB stars produce sufficient quantities of 25Mg and 26Mg to resolve the discrepancy between observations and previous model predictions.

## 2 The Chemical Evolution Model

The temporal and radial evolution of the isotopic abundances in the Milky Way was calculated under the assumption that the Galaxy formed via the accretion of gas at a rate decreasing exponentially with time. For the sake of simplicity, we assumed only a single episode of primordial gas accretion, with a timescale of 7 Gyr at the solar radius. However the results were not significantly different for a two-phase accretion model. We traced the chemical elements through the ongoing cycles of star formation, nucleosynthesis, and ejection into the interstellar medium (ISM) via supernovae (SNe) explosions and stellar winds. In order to precisely monitor the abundances of isotopes with different production sites, mass- and metallicity-dependent stellar lifetimes and yields were employed.

The rate of star formation in this model varies with the square of the gas surface density and inversely with Galactocentric radius. This type of radially-dependent law is motivated by the idea that spiral arm patterns trigger star formation (e.g. Prantzos & Silk 1998). The mass distribution of each new generation of stars was governed by the Kroupa, Tout & Gilmore (1993) three-component initial mass function (IMF), with lower and upper mass limits of 0.8 and 100 M, respectively.

Three basic models were constructed, differing only in the adopted nucleosynthesis prescriptions. Firstly, *LSC + AGB* refers to a combination of low and intermediate-mass stellar yields from Karakas & Lattanzio (2003a,b) and a grid of mass and metallicity dependent (Z = 0, 10-3 & 0.02) massive star yields provided by Limongi (2001, unpublished), calculated using the FRANEC code described in Limongi, Straneiro & Chieffi (2000) and Limongi & Chieffi (2002). The second model, *LSC no AGB*, is identical to the first model but ignores the AGB contribution to 25Mg and 26Mg production. Finally, the model *WW no AGB* replicates *LSC no AGB* but using metallicity-dependent Woosley & Weaver (1995) yields for massive stars. All models adopt yields for Type Ia SNe from the W7 model of Iwamoto et al. (1999). The SNe Ia contribution to chemical evolution was calculated following the method from Matteucci & Greggio (1986). It was assumed that 3% of binaries culminate in SNe Ia, since this fraction provides a good fit to the present-day SNe Ia rate (e.g. Alibes et al. 2001). For stars whose metallicity lies below (above) the range covered by the nucleosynthesis models we estimate their yields by extrapolating from the two lowest (highest) metallicity grids.

The Karakas & Lattanzio (2003a,b) stellar models comprise a grid of Mg isotopic yields covering a range of low to intermediate stellar mass (1 $``$ $`m`$/M $``$ 6) and a variety of compositions (Z = 0.004, 0.008 & 0.02, supplemented by an unpublished 0.0001 grid calculated with the same code) that is well-suited for chemical evolution models. These models have been evolved from the pre-main sequence to near the end of the thermal-pulsing AGB phase. The nucleosynthesis calculations are performed separately to determine the production of the isotopes.

## 3 Results & Discussion

Figure 1 shows the predicted evolution of magnesium isotopic ratios with \[Fe/H\] from the models *LSC + AGB* (*solid line*) and *LSC no AGB* (*dotted line*) for the solar region. $`{}_{}{}^{25}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ are shown in the upper and lower panels, respectively, along with measured abundance ratios in local dwarfs from Gay & Lambert (2000) and cool subdwarfs from Yong (2003). Representative observational errors are indicated by the large crosses. Although the quoted errors for 25Mg and 26Mg are identical in both studies, 26Mg is expected to be more accurately determined than 25Mg because the 26MgH line is less blended with 24MgH. Both models shown in Figure 1 predict ratios larger than solar (indicated by squares) but consistent with the data of Gay & Lambert. It is not surprising that the models reach similar present-day values irrespective of whether AGBs are included, because massive stars are responsible for most of the neutron-rich Mg isotopes in the present-day ISM. In this model 10% of 26Mg present in the ISM at \[Fe/H\] = 0 comes from AGB stars compared with $``$ 70% at \[Fe/H\] = $``$1 and nearly 90% at \[Fe/H\] = $``$2.

The dotted lines reveal that below \[Fe/H\] $``$ $``$1, massive stars alone seriously under produce 25Mg and 26Mg with respect to $`{}_{}{}^{24}\mathrm{Mg}`$. Much better agreement is obtained by including the contribution from AGB stars. In particular, most of the heavy Mg isotopic abundance at low metallicity is controlled by the 4-6 M stars that undergo hot bottom burning and whose He-shells are hot enough to trigger the $`{}_{}{}^{22}\mathrm{N}`$e($`\alpha ,n`$)$`{}_{}{}^{25}\mathrm{Mg}`$ and $`{}_{}{}^{22}\mathrm{N}`$e($`\alpha ,\gamma `$)$`{}_{}{}^{26}\mathrm{Mg}`$ reactions (Karakas & Lattanzio 2003a,b). These stars typically have lifetimes between 60 and 170 Myr.

The high abundances of 25Mg and 26Mg from the Yong (2003) data-set pose more of a challenge and are difficult to reconcile with our models, even with an AGB contribution. These stars were selected by their large transverse velocities as part of an effort to compile a sample of metal-poor unevolved subdwarfs (Yong & Lambert 2003). Based on their high reduced proper motion, it is likely that most of the sample is distinct from the thin disk, belonging instead to the halo at low metallicities or the thick disk at higher metallicities. One might expect that stars enhanced in 25Mg and 26Mg are also either 1) rich in s-process elements if they have been heavily contaminated by AGB stars; or 2) $`\alpha `$-enhanced if they belong to the halo/thick disk. Yong (2003) reports that there does not appear to be an obvious relationship between high values of $`{}_{}{}^{25,26}\mathrm{Mg}`$ and the abundance of s-process or $`\alpha `$-elements.

The predicted trend of $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ with \[Fe/H\] is plotted in Figure 2 at different Galactic radii for the *LSC + AGB* model. The dotted curve corresponds to the innermost radius of the model (4 kpc) and the dashed curve to the outermost radius (16 kpc). The exponential timescale for infalling gas was assumed to increase linearly with radius, taking on a value of 7 Gyr at the solar radius. Due to this “inside-out” accretion scenario and the radially-dependent star formation law, the timescale of SF is much longer in the outer disk. Only $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ is plotted because the $`{}_{}{}^{25}\mathrm{Mg}`$H line is less reliably determined than the $`{}_{}{}^{26}\mathrm{Mg}`$H line due to more severe blending with the $`{}_{}{}^{24}\mathrm{Mg}`$H feature (Gay & Lambert 2000). This model predicts a greater spread in $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ in metal-poor stars versus metal-rich stars throughout the Galaxy. The dispersion in the metal-poor regime reflects the dependence of 25Mg and 26Mg abundance on the timescale of star formation. Since the lowest metallicity AGB models predict the highest 25Mg and 26Mg yields, environments such as the outer disk, with protracted star formation and slowly increasing metallicity over time, encourage generations of IMS to elevate $`{}_{}{}^{25}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$. The inner Galaxy by contrast, is believed to have experienced intense star formation very early in its history, rapidly enriching the ISM with metals. Once \[Fe/H\] exceeds about $``$1, massive stars begin to surpass IMS as the chief source of neutron-rich Mg isotopes. The spread becomes smaller for \[Fe/H\] $`>`$ $``$1, at which point metallicity rather than star formation history drives $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$.

Figure 3 illustrates the lack of dispersion across different radii for the *LSC no AGB* model. There is some scatter in $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ at high \[Fe/H\] that stems from the delayed release of iron from Type Ia SNe. As most of the ejecta from SNe Ia is in the form of iron, these events increase \[Fe/H\] to a greater extent than overall metallicity. A consequence of the characteristic SNe Ia time delay of about 1 Gyr is that *for the same abundance of iron*, the inner disk is expected to be $`\alpha `$-enhanced and therefore have greater total abundance of nuclei than the outer disk. With more seed nuclei, the inner disk for a given value of \[Fe/H\] should see higher values of $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ than the outer disk. Precisely this effect is revealed in Figure 3.

For the sake of comparing how robust our results are to explosive SNe yields from different authors, we plot in Figure 4 the predicted evolution of $`{}_{}{}^{25}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ for the solar neighbourhood for the *LSC no AGB* and *WW no AGB* models. There is excellent agreement between the two models, although Woosley & Weaver’s (1995) nucleosynthesis models predict about 20% less 25Mg than 26Mg , while Limongi et al. (2000,2002) produce these isotopes in roughly equal numbers. The Mg isotopic yields depend on the adopted $`{}_{}{}^{12}\mathrm{C}`$($`\alpha `$,$`\gamma `$)$`{}_{}{}^{16}\mathrm{O}`$ rate (Imbriani et al. 2001). Specifically, lowering the value of $`{}_{}{}^{12}\mathrm{C}`$($`\alpha `$,$`\gamma `$)$`{}_{}{}^{16}\mathrm{O}`$ leads to higher final yields of $`{}_{}{}^{24}\mathrm{Mg}`$ but leaves the heavier Mg isotopes relatively uneffected. The Limongi et al. yields employed in this Milky Way model use a large $`{}_{}{}^{12}\mathrm{C}`$($`\alpha `$,$`\gamma `$)$`{}_{}{}^{16}\mathrm{O}`$ rate, hence producing low $`{}_{}{}^{24}\mathrm{Mg}`$ yields. The $`{}_{}{}^{25}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ ratios could be decreased with a lower $`{}_{}{}^{12}\mathrm{C}`$($`\alpha `$,$`\gamma `$)$`{}_{}{}^{16}\mathrm{O}`$ value such as that from Kunz et al. (2002) which is used in the latest version of the FRANEC code (Limongi & Chieffi 2003). In this case, the Mg isotopic ratios could be reconciled with solar values, but at the expense of obtaining a good fit to the Gay & Lambert (2000) data.

One of the greatest uncertainties in the model concerns the precise form of the stellar IMF. While most elemental yields are fairly robust to changes in the slope and limits of the IMF, this is not the case for the heavy Mg isotopes, whose production in solar metallicity massive stars rises very sharply with stellar mass. Thus, the most massive stars play a crucial role in determining $`{}_{}{}^{25}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ despite being vastly outnumbered by lower mass stars. Figure 5 displays the yield of 26Mg relative to 24Mg as a function of initial mass for the solar metallicity models of Karakas & Lattanzio (2003a,b) and Limongi et al. (2000,2002) (*solid line*). The solar metallicity massive star yields extend only as far as 35 M and were linearly extrapolated up to 100 M. The largest mass in the AGB models is 6 M. For most elements, including Fe and $`{}_{}{}^{24}\mathrm{Mg}`$, the yields between 6-8 M were derived by extrapolating up from the AGB models. However we conservatively assumed that the 6-8 M stars eject the same quantity of 25Mg and 26Mg as the 6 M star. This causes a dip in $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ at 8 M. Superimposed on the same figure are IMFs from Salpeter (1955) (*dotted line*) and Kroupa, Tout & Gilmore (1993) (*dashed line*) normalized over the mass range 0.08-100 M. The Salpeter IMF has the form of a single slope power-law (this model uses an index of 1.31) and places a higher proportion of the mass of a stellar generation into both the lower and upper extremes of the mass distribution when compared with the Kroupa et al. (1993) IMF. It is apparent that the role of stars between 0.3 $``$ $`m`$/M $``$ 6 is emphasised by adopting a Kroupa et al. IMF, whereas the frequency of high mass stars is increased with the Salpeter IMF.

One can anticipate that a Kroupa et al. (1993) IMF would give rise to more AGB stars than a Salpeter (1955) function, leading to higher values of $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ at low metallicity. At metallicities approaching solar however, the Salpeter IMF should generate the highest $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ ratios, since it favours the birth of massive stars when compared with the Kroupa et al. law. The influence of the IMF can be seen by comparing the results presented in Figure 6, which were derived using the Salpeter function, with those from Figure 2. A ratio of $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ $``$0.3 at \[Fe/H\] = 0 is obtained with a Salpeter IMF. This is $``$ 50% higher than in the Kroupa et al. case and over twice the solar value. Owing to the production of fewer AGB stars, $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ at \[Fe/H\] = $``$2 in the Salpeter case is about half the value derived with the Kroupa IMF. The Kroupa et al. model is in better agreement with the Gay & Lambert (2000) data set. Although the large values of $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ measured by Yong (2003) in higher metallicity stars could be attained by increasing the role of massive stars, this comes at the expense of satisfying observations at low \[Fe/H\]. Multi-component IMFs with steeper slopes at high mass are favoured over the Salpeter single power law on both observational and theoretical grounds (e.g. Kroupa et al. 1993; Scalo 1986).

It has been suggested that the mass distribution of a stellar generation is influenced by factors including the thermal energy and chemical composition of the star-forming gas (Larson 1998). Accordingly, the IMF might be expected to evolve over time. There are theoretical arguments that the IMF of primordial gas would be biased toward higher mass stars, while higher metallicity environments would form relatively more low-mass stars (Kroupa 2001). If the IMF followed this trend then the fit between our model predictions and empirical constraints would worsen. At present however, the observational evidence for a variable IMF is not overwhelming.

## 4 Conclusions

Thermally-pulsing AGB stars are shown to be excellent candidates for the additional production site of neutron-rich Mg isotopes needed to account for observations at low metallicities. The failure of previous chemical evolution models to match $`{}_{}{}^{25}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ observed in local metal-poor stars may be resolved if intermediate-mass stars produce 25Mg and 26Mg in quantities given by the calculations of Karakas & Lattanzio (2003a,b).

According to the chemical evolution model presented in this paper, massive stars are responsible for most of the heavy Mg isotopes in the present-day ISM, but played a secondary role to 4-6 M AGB stars at earlier epochs. A consequence of this model is that the spread in $`{}_{}{}^{25}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ should be greater at low metallicities across the Milky Way, although this conclusion was shown to be sensitive to the adopted initial mass function. While the high ratios of $`{}_{}{}^{25}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ and $`{}_{}{}^{26}\mathrm{Mg}`$/$`{}_{}{}^{24}\mathrm{Mg}`$ in Yong’s (2003) halo and thick disk sample remain a mystery and warrant further investigation, our model provides an excellent match to the measurements of local stars from Gay & Lambert (2000).

## Acknowledgments

The financial support of the Australian Research Council (through its Large Grant, Discovery Project, and Linkage International schemes) and the Victorian Partnership for Advanced Computing (through its Expertise Grants scheme) is acknowledged.

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text:
# References

Experimental limit on Spontaneous Parametric Up Conversion

G.Brida, M.Genovese 111 genovese@ien.it. Tel. 39 011 3919253, fax 39 011 3919259, M. Gramegna, C.Novero 222 Dedicated to the memory of our beloved friend and collaborator Carlo Novero.

Istituto Elettrotecnico Nazionale Galileo Ferraris, Str. delle Cacce 91,I-10135 Torino.

Abstract

We present a first experimental test of the existence of Spontaneus Parametric Up Conversion predicted in Ref. . The measurement has been made using a ccd camera on the emission of a $`LiIO_3`$ crystal pumped by a 351 nm and/or a 789 nm lasers. We obtain an upper limit of 160 times on the ratio between intensity of Spontaneus Parametric Up Conversion and Spontaneous Parametric Down conversion.

Keywords: parametric down conversion, non-locality, hidden variable theories

Parametric Down Conversion is a phenomenon where a pump laser converts into pairs of highly correlated photons fulfilling the condition, known as phase matching condition, that the produced pair is such that the sum of frequencies of the produced photons is equal to the frequency of the pump photon and the vectorial sum of wave vectors of the produced photons is equal to the wave vector of the pump photon. A quantum theory of this effect  exists reproducing well all the results of the many experiments performed up to now.

The photon pair produced in PDC is an optical state with clear quantum properties and has often been used for tests of local realism .

However, a classical description based on the use of Wigner function, which is positive for the states produced in PDC, is possible and has been developed recently in a series of papers , where PDC is treated as the interaction of a pumping laser wave and the zero-point vacuum waves inside a non-linear crystal.

The existence of such models, compatible with the nowadays experiments about Bell inequalities , shows that a classical local hidden variable model cannot be excluded completely yet. This is due to the well known detection loophole  that affects all the experiments about local realism performed up to now. This loophole derives from the fact that, because of low detection efficiencies, one needs a further additional hypothesis, stating that the observed sample of particles pairs is a faithful subsample of the whole 333A recent experiment  performed using Be ions has reached very high detection efficiencies (around 98 %), but in this case the two subsystems (the two ions) are not really separated systems during measurement and the test cannot be considered a real implementation of a detection loophole free test of Bell inequalities, even if it represents a relevant progress in this sense. .

A very interesting point of the model of Ref.  is that it presents various predictions which can be tested experimentally . In particular, an interesting prediction of this model, which is elaborated in Ref. , is that a completely new phenomenon, dubbed Spontaneous Parametric Up Conversion, should exist.

In synthesis, in the model of Ref.  spontaneous PDC derives by the interaction inside a non-linear crystal of the high frequency $`\omega _0`$ (usually ultraviolet) pump laser with the zeropoint field in the vacuum (e.g. the one originating Casimir effect) which originates two photons of lower frequencies ($`\omega _2,\omega _3`$) such that the equation

$$\omega _0=\omega _2+\omega _3$$
(1)
for the frequencies and the equation

$$\stackrel{}{k}_0=\stackrel{}{k}_2+\stackrel{}{k}_3$$
(2)
for the wave vectors are satisfied.

If another laser of lower frequency $`\omega _1`$ is injected, with the right angle (see figure 1), a stimulated emission, with frequency $`\omega _3`$, is produced satisfying the equations

$$\omega _0\omega _1=\omega _3$$
(3)
and

$$\stackrel{}{k}_0\stackrel{}{k}_1=\stackrel{}{k}_3$$
(4)
According to Ref.  a fluorescence is emitted also if the high frequency pump laser is turned off and only the second laser (the one with frequency $`\omega _1`$) remains. This phenomenon, due to the interaction of this laser with the zeropoint field (the vacuum), has been dubbed Spontaneous Parametric Up Conversion and is a peculiar prediction of this model, which does not have equivalent in the traditional quantum optics description of SPDC. Therefore the search for this fluorescence represents a determinant test of the model.

The numerical calculations of Ref.  shows that the intensity of this fluorescence should be a factor 2-3 smaller than PDC, but with a different angular distribution. If the incident laser (with frequency $`\omega _1`$) is normal to the non-linear crystal, the SPUC rainbow forms incomplete rings off-centre respect to the pump (see figure 3 of quant-ph 0203042 ), with frequencies ranging from $`\omega _1`$ and the UV. On the other hand, also in a configuration where a UV laser ($`\omega _0`$ in figure 1) was normally incident on a non-linear crystal originating a stimulated emission ($`\omega _3`$ in figure 1) by interacting with a second laser at a lower frequency ($`\omega _1`$ in figure 1), when the UV laser is turned off a SPDUC should appear. This emission should be distributed, because of phase matching conditions, on incomplete circles, of which the one with frequency $`\omega _0`$ passes through the point where the UV pump laser was and the one with frequency $`\omega _3`$ through the point where the stimulated emission was. The remaining emission, with frequency varying from $`\omega _0`$ and $`\omega _3`$, lies between these two points. As in this case the region of emission is perfectly defined by the emission observed in stimulated PDC, this configuration is particularly well suited for an experimental search of SPUC.

In this paper we present a first experimental test of this prediction, which gives severe constraints on the existence of SPUC.

More in details, we have pumped a Lithium iodate crystal, cut at the phase-matching angle of $`51^o`$, with an argon laser at 351 nm. A diode laser at 789 nm, with a power of 50 mW, was injected at the right angle for producing a stimulated emission (see figure 2).

Parametric down conversion was easily observed on a screen, even by naked eye, with a power of the argon laser lowered up to 50 mW (the maximum power of this argon laser is 500 mW). If the IR laser was turned on an evident stimulated emission, at 633 nm, was visible (see figure 2), certifying that this second laser was entering the crystal with the right angle. According to the prediction of Ref. , turning off the argon laser, a strong Parametric Up Conversion, produced by the interaction of the IR laser with zeropoint field, should be observed. In particular an emission with frequency ranging between $`\omega _0`$ (where the pump laser was) and $`\omega _3`$ (where the stimulated emission was) should be present. Thus the use of this experimental configuration allows an easy identification of the region where SPUC should be emitted and of the spatial distribution of frequencies. As the spectral response of our ccd camera, based on silicon sensitive elements, is centred in the visible region (with a quantum efficiency above 10 $`\%`$, in the whole visible region and near UVA and IR) an eventual SPUC emission should therefore be easily observed. Nevertheless, no signal of this emission appeared in our experiment.

In order to obtain an upper limit to the ratio between SPUC and SPDC intensities, we have shot the SPDC with a ccd camera, which measures the time integral of the irradiance coming from the source. The image of SPDC was very evident even with a shot time as short as 1/10 of second and a 2.8 stop (the argon laser was eliminated by an anti-UV filter after the crystal). Then we turned off the argon laser and we searched for SPUC. No fluorescence appeared on the pictures even with long time exposures. In figure 3 we present a 16 seconds exposure (the longest time exposure available on our camera) on a ccd camera opened with a 2.8 stop when only the I.R. laser is injected into the non-linear crystal. Dark frame has been subtracted (even if this contribution is rather unimportant). Due to the long time of the exposure some diffused light of the laser into the crystal appears, but no SPUC is observed.

Considering that the response of a ccd camera is linear with the intensity of incident light (as we operate far from saturation regime), this means that the ratio between SPUC and SPDC intensities is lower than 160 times.

In order to give a further confirmation of the absence of SPUC we have also taken some long time exposure on an ordinary camera film. In this case the response is non-linear, due to reciprocity effect, and thus no ratio between SPUC and SPDC can be derived. However rather a strong indication about the non-existence of SPUC can be obtained: in fact even with a 10 minutes exposure at 1.7 stop with a 1600 ISO film no signal of SPUC appears.

With the purpose of performing a second test of the presence of SPUC, we have injected into the crystal a Nd-YAG laser at 1064 nm and a power of 0.51 W, when entering into the crystal, as well. Also in this case we have tuned the entrance angle in order to observe a well visible stimulated emission at 524 nm when both the UV and IR laser are turned on. We have then repeated the same procedure as before: whilst PDC was observable even with a 1/30 of second exposure at 2.8 stop with the argon laser power tuned to 0.48 W, no SPUC appeared up to a 1/2 second exposure with the same stop and the 1064 nm laser at the same power. Unluckily in this case the high-power Nd-YAG laser strongly diffuses into the crystal and creates a strong background for longer exposures: thus we were not able to derive more stringent limits on the ratio between SPUC and SPDC intensities in this case.

Finally, also repeating the experiments with normal incidence of the laser no SPUC has been observed (with the same limits as before).

Altogether these experimental limits give a severe constraint on the model of Ref.  and substantially excludes the very existence of Spontaneous Parametric Up Conversion.

In conclusion we have performed a first experimental test of existence of Spontaneous Parametric Up Conversion predicted in the model of Ref. . The test was performed comparing the emission observed by a ccd camera when SPDC is present and when SPUC is expected. No SPUC was observed up to a ratio of 160 times (with the 789 nm laser) respect to the intensity of SPDC produced at the same laser power.

Acknowledgements We would like to acknowledge support of Italian Space Agency under contract LONO 500172.

Figure Captions

-Figure 1 Sketch of the source of PDC. NLC is a $`LiIO_3`$ crystal cut at the phase-matching angle of $`51^o`$. U.V. identifies the pumping radiation at 351 nm ($`\omega _0`$). The infrared beam (I.R.) at 789 nm ($`\omega _1`$) is generated by a diode laser. The dashed line identifies the stimulated radiation at 633 nm ($`\omega _3`$).

\- Figure 2 Picture of the parametric down conversion produced by an argon laser injected into a $`LiIO_3`$ crystal. A second laser at 789 nm is injected as well. The spot of this second laser and the stimulated emission at 633 nm appear clearly in the picture. The first one corresponds to the larger spot bleached because of saturation of ccd pixels. The second one corresponds to the spot on the other side respect to the centre of the emission. The concentric circles of different colours are the spontaneous emissions at different wavelengths. In absence of the 789 nm injected laser, exactly the same spontaneous emission appears, but of course the stimulated spot is missing.

\- Figure 3 Picture obtained with a 16 seconds exposure on a ccd camera with a 2.8 stop when only the I.R. laser is injected into the non-linear crystal. The field is the same of Figure 2. Due to long time of the exposure some diffused light of the laser into the crystal and thermal noise of ccd elements appear, but no SPUC is observed. The scale is the same of figure 2.