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# A doubler-free lattice theory for QCD based on geometric fermions

## 1. Introduction

One of the main problems of lattice gauge theory is the fermion doubling problem. If we use a naive central differences discretization of the Dirac equation, we observe a doubling effect: The large distance limit of the resulting lattice equation does not describe the original single Dirac particle, but, instead, sixteen Dirac particles — a factor two doubling in each spacetime dimension. Such a discretization is inappropriate for quantum computations where the number of degrees of freedom is important.

A partial solution is given by a geometric variant of the Dirac equation — the Dirac-Kähler equation . This equation is defined on the complexified four-dimensional exterior bundle $`\mathrm{\Lambda }(^4)`$. This bundle contains sixteen complex components, and the Dirac-Kähler equation on it is equivalent to the classical Dirac equation for four Dirac bispinors. On the other hand, for this equation exists a doubler-free so-called “staggered” or Kogut-Suskind discretization (, see also ). Instead of sixteen doublers of the naive discretization this gives a lattice equation for four Dirac bispinors. Another solution is to suppress the doublers using some additional terms which give all the doublers except one a large mass. The most famous one is the Wilson mass term , but many different versions of such mass terms have been proposed.

In this paper we consider another variant of geometric fermions. Instead of the bundle $`\mathrm{\Lambda }(^4)`$ we use the three-dimensional exterior bundle $`\mathrm{\Lambda }(^3)`$ and a direction-dependent complex structure on it. The four-dimensional Dirac equation appears as an evolution equation on this bundle. The time $`t`$ is only a parameter of dynamics without geometric meaning. This representation of the Dirac equation describes already a single bispinor.

The main advantage of the geometric Dirac-Kähler fermions remains — there exists a doubler-free “staggered” discretization of the continuous Dirac equation. But now it gives a doubler-free “staggered” discretization of a single bispinor. We find also a remarkable, more symmetric discretization for an octet of bispinors related with the bundle $`(\mathrm{\Lambda }\mathrm{\Lambda })(^3)`$.

Using the standard Wilson approach to lattice gauge fields becomes problematic because the complex structure does not act pointwise. But to put the octet representation of $`SU(3)`$ used in QCD on the lattice we do not need the complex structure: It is equivalent to a real representation. As a consequence we obtain a doubler-free discretization for lattice QCD.

The discretization presented here is closely related with the “space-geometric” interpretation of standard model fermions as sections of the bundle $`(T\mathrm{\Lambda }\mathrm{\Lambda })(^3)`$, or, on curved background with ADM decomposition $`M^4M^3`$, the bundle $`(T\mathrm{\Lambda }\mathrm{\Lambda })(M^3)`$ made in .

## 2. Space-geometric representation of spinors

The classical Dirac algebra is defined by the operators $`\gamma ^i`$ with commutation relations $`\{\gamma ^i,\gamma ^j\}=\eta ^{ij}`$ — the Clifford algebra $`Cl(1,3)`$. But there are also some other operators which play an important role in the standard model: The complex structure, which is defined by the operator $`i`$, and a real structure defined by the operator $`C`$, which is necessary to define Majorana mass terms. The commutation relations of this “extended Dirac algebra” $`\{\gamma ^\mu ,i,C\}`$ are: $`\{\gamma ^\mu ,\gamma ^\nu \}=2\eta ^{\mu \nu }`$, $`[i,\gamma ^\mu ]=0`$, $`[C,\gamma ^\mu ]=0`$, $`\{C,i\}=0`$, $`C^2=1`$, $`i^2=1`$.

The three-dimensional or space-geometric representation of spinors based on the following isomorphism:

###### Theorem 1.

The “extended Dirac algebra” $`\{\gamma ^\mu ,i,C\}`$ is isomorph to the Clifford algebra $`Cl(3,3)`$. The Clifford algebra generators are the $`\gamma ^i`$ for $`i>0`$ and the three operators $`\beta ^i`$ defined by

$`\beta ^1`$ $`=`$ $`C,`$
$`\beta ^2`$ $`=`$ $`Ci,`$
$`\beta ^3`$ $`=`$ $`\gamma ^5=i\gamma ^0\gamma ^1\gamma ^2\gamma ^3.`$
Proof: An explicit check proves that the operators $`\gamma ^i,\beta ^i`$ fulfil the properties required for the generators of $`Cl(3,3)`$ (they anticommute, $`(\beta ^i)^2=(\gamma ^i)^2=1`$). We have already expressed the generators of $`Cl(3,3)`$ in terms of the extended Dirac algebra $`\{\gamma ^\mu ,i,C\}`$. The reverse expressions can be easily found:

(1) $`C`$ $`=`$ $`\beta ^1`$
(2) $`i`$ $`=`$ $`\beta ^1\beta ^2`$
(3) $`\gamma ^0`$ $`=`$ $`\beta ^1\gamma ^1\beta ^2\gamma ^2\beta ^3\gamma ^3`$
It remains to prove that there are no other relations in $`\{\gamma ^\mu ,i,C\}`$. This can be done by an explicit computation of the dimension of the extended Dirac algebra. We have six generators $`\{\gamma ^\mu ,i,C\}`$, for each pair of generators we have one commutation resp. anticommutation rule, the square of all generators is $`\pm 1`$, and there are no other independent relations. Therefore an arbitrary monom may be transformed into a monom where every generator appears at most once. There are $`2^6`$ such monoms, which gives the dimension of $`Cl(3,3)`$. qed.

The Clifford algebra $`Cl(3,3)`$ acts in a natural way on the three-dimensional Clifford bundle $`Cl(^3)`$. This bundle is equivalent to the exterior bundle $`\mathrm{\Lambda }(^3)`$ which consists of inhomogeneous differential forms $`\phi =\phi _\kappa (x)(dx^1)^{\kappa _1}(dx^2)^{\kappa _2}(dx^3)^{\kappa _3}`$, $`\kappa =(\kappa _1,\kappa _2,\kappa _3)(_2)^3`$. The operators $`\gamma ^i`$ act as in standard Hodge theory and define the Hodge theory Dirac operator

(4)
$$D_3=i\gamma ^i_i$$

(see, for example, ). The action of the operators $`\beta ^i`$ follows from the following formula:

(5)
$$(\beta ^i\gamma ^i\phi )_\kappa (x)=(1)^{\kappa _i}\phi _\kappa (x)$$

It is not hard to see the following:

###### Theorem 2.

The representation of the extended Dirac algebra $`\{\gamma ^\mu ,i,C\}`$ on $`\mathrm{\Lambda }(^3)`$ defined by (4), (5) and theorem 1 is equivalent to the standard representation.

Theorem 1 gives now the following four-dimensional Dirac operator:

(6)
$$D_4=i\gamma ^0_0+D_3$$

The definition of the Lagrange formalism simplifies if we use the following variant of the Dirac operator:

(7)
$$D=i\gamma ^1\gamma ^2\gamma ^3D_4=\iota _t+\iota \alpha ^i_i$$

where $`\iota =\beta ^1\beta ^2\beta ^3`$, $`\iota ^2=1`$, $`\{\iota ,\gamma ^i\}=0`$, $`[\iota ,\alpha ^i]=0`$. The equivalence is obvious: $`D\phi =0`$ iff $`D_4\phi =0`$. Now we can use the standard Euclidean scalar product on $`\mathrm{\Lambda }(^3)`$ to define the Langrange formalism as

(8)
$$L=(\phi D\phi )$$

The Dirac operator considered here should not be mingled with the four-dimensional Dirac-Kähler operator defined on the spacetime bundle $`\mathrm{\Lambda }(^4)`$ which has real dimension 32. It defines an evolution equation on the spatial bundle $`\mathrm{\Lambda }(^3)`$ with real dimension 8. Time is only a parameter of dynamics and has no geometric interpretation. Manifest Lorentz invariance is lost. Only the equivalence theorem proves that Lorentz invariance will be recovered for observable effects.

This representation also violates manifest symmetry in space: The complex structure $`i=\beta ^1\beta ^2`$ as well as the operator $`\gamma ^5=\beta ^3`$ depend on a preferred direction in space. The introduction of three generations of fermions associated with the three spatial directions may be used to get rid of this asymmetry.

A similar ”space Clifford” representation of the Dirac equation has been considered by Daviau , see also .

A comparison of space-geometric spinors with standard spinors can be found in . It is shown there that on Minkowski background we have no observable differences, but on curved background we obtain differences which are observable in a graviational analogon of the Bohm-Aharonov experiment.

## 3. Lattice theory for the three-dimensional Dirac operator

Let’s consider at first the naive central differences discretization of the Dirac operator $`D`$ on $`\mathrm{\Lambda }(^3)`$. We use a regular rectangular lattice with lattice functions $`\phi \mathrm{\Omega }:_2^3^4`$ denoted by $`\phi _\kappa (n)`$, $`\kappa =(\kappa _1,\kappa _2,\kappa _3)(_2)^3`$, $`n=(n_0,n_1,n_2,n_3)^4`$. Using the denotations $`h_\mu =(\delta _{0\mu },\delta _{1\mu },\delta _{2\mu },\delta _{3\mu })`$ we define

(9) $`(t_\pm ^\mu \phi )_\kappa (n)`$ $`=`$ $`\phi _\kappa (n\pm h_\mu )`$
(10) $`\mathrm{\Delta }_\mu `$ $`=`$ $`{\displaystyle \frac{1}{2}}(t_+^\mu t_{}^\mu )`$
(11) $`D_h`$ $`=`$ $`\iota \mathrm{\Delta }_0+\iota \alpha ^i\mathrm{\Delta }_i`$
The Lagrange formulation of the lattice theory can be given in the same form as (8), but with the lattice version (11) of the Dirac operator $`D`$:

(12)
$$L=(\phi D_h\phi )$$

### 3.1. Decomposition into sixteen staggered fermions

A well-known problem of lattice gauge theory — the so-called “fermion doubling problem” — is that the naive central differences discretization of the classical Dirac equation does not describe a single Dirac fermion, but sixteen. This doubling problem appears in our naive discretization (11) too. As usual, we obtain sixteen Dirac fermions instead of one. But in our discretization these sixteen doublers decompose in a quite simple way.

###### Theorem 3.

There exists a decomposition

$$\mathrm{\Omega }\underset{\lambda }{}\mathrm{\Omega }^\lambda ,$$

$`\lambda =(\lambda _0,\lambda _1,\lambda _2,\lambda _3)^4`$, $`\lambda _i=\pm 1`$ so that for $`\phi =\phi _\lambda `$, $`\phi _\lambda \mathrm{\Omega }^\lambda `$

$$D_h\phi =0D_h\phi _\lambda =0$$

and the subspaces $`\mathrm{\Omega }^\lambda \mathrm{\Omega }`$ are realized as staggered sublattices.

To see this let’s consider the following lattice operators:

(13) $`(ϵ_0\phi )_\kappa (n)`$ $`=`$ $`(1)^{n_0+n_1+n_2+n_3}\phi _\kappa (n)`$
(14) $`(ϵ_i\phi )_\kappa (n)`$ $`=`$ $`(1)^{k_i+n_i}\phi _\kappa (n)`$
These four operators $`ϵ_\mu `$ commute with each other and fulfil $`ϵ_\mu ^2=1`$. This allows to define common eigenspaces with eigenvalues $`\pm 1`$. Thus, we define the $`\mathrm{\Omega }^\lambda `$ as eigenspaces $`ϵ_\mu \phi =\lambda _\mu \phi `$. It is easy to verify that the $`\mathrm{\Omega }^\lambda `$ define staggered sublattices: They contain only the component defined by $`(1)^{k_i+n_i}=\lambda _i`$ on nodes which fulfil the property $`(1)^{n_0+n_1+n_2+n_3}=\lambda _0`$.

Now, the $`ϵ_\mu `$ also anticommute with $`D_h`$. This gives the property $`D_h:\mathrm{\Omega }^\lambda \mathrm{\Omega }^\lambda `$. As a consequence, from $`D_h\phi =0`$ follows $`D_h\phi _\lambda =0`$ for all $`\lambda `$.

The decomposition on the level of lattice components suggests to use one of the eigenspaces, say $`\mathrm{\Omega }^{(1,1,1,1)}`$, as a staggered discretization of a single Dirac fermion.

A comparison of such a single staggered fermion with the standard staggered Dirac-Kähler fermions seems interesting: In the classical staggered fermion concept  there remain four doublers (more accurate, already the continuous Dirac-Kähler equation describes four Dirac bispinors, it’s staggered discretization is doubler-free as a discretization of the Dirac-Kähler equation but nonetheless describes four bispinors). Instead, in our approach we have no doublers, but a single Dirac fermion (eight real components). On the other hand, we have to pay for this with two disadvantages: We have no longer manifest, explicit relativistic symmetry, but a special role of the time coordinate. On curved background, such a special role for a time coordinate requires an additional structure — an ADM decomposition.

The other problem is the complex structure. First, it depends on a direction in space. This dependence disappears if we introduce three generations of fermions and associate the three generations with directions in space (see ). A more serious problem is that the complex structure on the lattice is not pointwise: real and imaginary parts of the four complex components of a bispinor are located on different lattice nodes. Especially there is no pointwise operator for multiplication with $`i`$ on our staggered fermion. Now, multiplication with $`i`$ is obviously an important operation in the standard model. Even if we get rid of it in the pure Dirac equation using the form (6) or (7), they reappear in the interaction terms with gauge fields as well as in the mass terms. Fortunately for mass terms it seems sufficient to fix some non-pointwise replacement for $`i`$. For gauge fields, the non-pointwise character of multiplication with $`i`$ seems more problematic.

### 3.2. The geometric octet

To define the standard model (inclusive right-handed neutrinos), we have to consider three octets of Dirac fermions. Now, a straightforward way to do define an octet would be to use eight copies of the staggered fermion defined by $`\mathrm{\Omega }^{(1,1,1,1)}`$. But there is a much simpler and more natural way to obtain an octet of fermions which we name geometric octet: We use the eigenspace $`\widehat{\mathrm{\Omega }}\mathrm{\Omega }`$ defined by $`ϵ_0\phi =\phi `$ which consists of all components on ”even” nodes. The lattice space $`\widehat{\mathrm{\Omega }}`$ has not only a much simpler definition (we don’t even have to define the operators $`ϵ_i,i>0`$ to define $`\widehat{\mathrm{\Omega }}`$), but also a larger symmetry group: While on different lattice nodes in $`\mathrm{\Omega }^{(1,1,1,1)}`$ we have different components $`\phi _\kappa `$, all lattice nodes in $`\widehat{\mathrm{\Omega }}`$ are of the same type: They contain all eight components $`\phi _\kappa `$.

Thus, from point of view of symmetry between lattice nodes, the geometric octet of Dirac fermions seems much more natural than a single Dirac fermion. Let’s consider its geometric nature: The eight doublers $`\mathrm{\Omega }^{(1,i,j,k)}`$ in this octet are connected with each other by translations in space. The components of the continuous limit of the geometric octet therefore should be connected by infinitesimal translations. This gives transformational properties as for the geometric bundle $`(\mathrm{\Lambda }\mathrm{\Lambda })(^3)`$ instead of $`\mathrm{\Lambda }(^3)^8`$.111Of course, as long as we consider only the Minkowski background, as we do in this paper, there is no physical difference between $`(\mathrm{\Lambda }\mathrm{\Lambda })(^3)`$ and $`\mathrm{\Lambda }(^3)^8`$. The difference becomes important on curved background. The consideration of discretizations for curved background we leave to future research.

There is one problem with the reduction $`\mathrm{\Omega }\widehat{\mathrm{\Omega }}`$ — the naive Lagrange formulation (12) is not well-defined on $`\widehat{\mathrm{\Omega }}`$. But there is a simple solution — instead of (12) we can use the following Lagrangian:

(15)
$$L=(\phi t^3D_h\phi )$$

where the translation $`t^3`$ defines a preferred direction in space. This requires the same type of symmetry breaking as the choice of the complex structure $`i=\beta ^1\beta ^2`$, and we can get rid of it if we introduce three fermion generations (see ).

Below we focus our interest on the “geometric” octet.

## 4. Lattice gauge theory

Our lattice Dirac equation for the geometric octet may be connected with gauge fields following the classical Wilson scheme for lattice gauge fields, even with some simplifications. In the Wilson approach, the lattice gauge field for a gauge group $`G`$ is described by gauge transformations $`U_\mu (n)G`$ defined on edges (links) of the lattice. The lattice gauge transformations are defined by functions $`g(n)G`$ on the nodes with values in the gauge group $`G`$. In comparison with standard lattice fermions we have no pointwise operation of multiplication with $`i`$. But if the representation $`T:Ggl(8)`$ which acts on the space spanned by the $`\phi _\kappa (n)`$ is real, we can nonetheless use the standard way to define a gauge-invariant interaction Lagrangian — to replace the difference operators in the Lagrangian by covariant difference operators $`\mathrm{\Delta }_\mu \stackrel{~}{\mathrm{\Delta }}_\mu `$:

(16)
$$(\stackrel{~}{\mathrm{\Delta }}_\mu \phi )_\kappa (n)=\frac{1}{2}(T(U_\mu (n))\phi _\kappa (n+h_\mu )T(U_\mu ^1(nh_\mu ,\mu ))\phi _\kappa (nh_\mu ))$$

The restriction to pointwise gauge transformations (and the resulting restriction to real representations) is is not only prescribed by the standard Wilson approach. It also allows to preserve the reduction $`\mathrm{\Omega }\widehat{\mathrm{\Omega }}`$ and, therefore, allows to define the gauge action not only on the original sixteen doublers $`\mathrm{\Omega }`$ but also on the geometric octet $`\widehat{\mathrm{\Omega }}`$. This gives the Lagrangian

(17)
$$L=(\phi t^3\stackrel{~}{D}_h\phi )+L_{Wilson}(U_\mu (n))$$

for the gauged Dirac operator $`\stackrel{~}{D_h}=\iota \stackrel{~}{\mathrm{\Delta }}_0+\iota \alpha ^i\stackrel{~}{\mathrm{\Delta }}_i`$.

### 4.1. QCD on the geometric octet

Let’s consider now the specific properties of local gauge actions on the geometric octet. To define QCD on the geometric octet we need the appropriate octet representation of the Lie algebra $`su(3)`$ in terms of pointwise operators which commute with the Dirac operator $`D_h`$. For this purpose, let’s consider the following operator algebra:

(18) $`\beta _i`$ $`=`$ $`\beta ^i`$
(19) $`\gamma _i`$ $`=`$ $`\beta _iϵ_i`$
We have $`\beta _i^2=1`$, $`\gamma _i^2=1`$, and all $`\beta _i,\gamma _i`$ anticommute, thus, it is the Clifford algebra $`Cl(3,3)gl(8)`$. The compact subalgebra $`o(8)gl(8)`$ is generated by products $`g`$ of the generators which fulfil $`g^2=1`$.

Moreover, we have simple commutation relations with the Dirac operator: $`[\beta _i,D_h]=0`$, $`\{\gamma _i,D_h\}=0`$. If we require $`[g,D_h]=0`$, we have to restrict ourself to monoms with even number of factors $`\gamma _i`$. This restriction is equivalent to $`[g,\widehat{i}]=0`$ with $`\widehat{i}=\beta _1\beta _2\beta _3`$, $`\widehat{i}^2=1`$. The subalgebra of $`o(8)`$ which fulfills this restriction is equivalent to $`u(4)`$, where $`\widehat{i}`$ plays the role of the related complex unit.

It should be noted that this is a real eight-dimensional representation of $`u(4)`$. A complex unit $`i`$ which acts on single fermions $`\mathrm{\Omega }^{(1,i,j,k)}`$ has not been used here. Such a complex unit $`i`$ should be distinguished from the real operator $`\widehat{i}gl(8)`$ which does not preserve the decomposition into fermions $`\mathrm{\Omega }^{(1,i,j,k)}`$.

As a real representation, this octet representation of $`u(4)`$ would be irreducible. But as a complex octet representation it is reducible: We have an involution operator $`i\widehat{i}`$, $`(i\widehat{i})^2=1`$, $`[g,i\widehat{i}]=0`$ for $`gu(4)`$. This allows to define two invariant subspaces with projectors $`P^\pm =\frac{1}{2}(1\pm i\widehat{i})`$. On these four-dimensional subspaces $`\widehat{\mathrm{\Omega }}_\pm =P^\pm \widehat{\mathrm{\Omega }}`$ we have $`i=\widehat{i}`$.222Note that on the lattice such a decomposition would require a lattice analogon of $`i`$ with exact properties $`i^2=1`$, $`[i,\widehat{i}]=0`$, $`[i,\stackrel{~}{D}_h]=0`$ which does not exist. Thus, this decomposition will not be exact on the lattice. It appears only in the continuous limit. The observable quarks and leptons will be, therefore, linear combinations of pairs of staggered fermions $`\mathrm{\Omega }^{(1,i,j,k)}`$ and $`\mathrm{\Omega }^{(1,i,j,k)}`$ defined by the projectors $`P^\pm `$. It seems natural to identify the pairs $`\mathrm{\Omega }^{(1,i,j,k)}\mathrm{\Omega }^{(1,i,j,k)}`$ with electroweak doublets.

Thus, we obtain two times the defining four-dimensional representation of $`u(4)`$. Restricted to $`su(3)u(4)`$ this gives two times the defining representation of $`su(3)`$ and two times a singlet representation of $`su(3)`$, as required for the QCD action. At least as long as we do not consider weak interaction the two subspaces $`\widehat{\mathrm{\Omega }}_\pm `$ are independent. Therefore the different choice of the sign of the complex structure is a question of convention.

It remains to define an appropriate restriction from $`u(4)`$ to $`su(3)`$. For this purpose we have the interesting symmetric operator

(20)
$$\sigma =\beta _1\gamma _1\beta _2\gamma _2+\beta _2\gamma _2\beta _3\gamma _3+\beta _3\gamma _3\beta _1\gamma _1$$

which defines baryon resp. lepton charge in a natural way. The restriction $`[g,\sigma ]=0`$ defines the subalgebra $`u(1)u(3)u(4)`$. Its generators are:

(21)
$$\widehat{i}=\beta _1\beta _2\beta _3,\delta _i=\beta _i\gamma _j\gamma _k,\omega _i=\beta _j\beta _k\gamma _j\gamma _k,\eta _i=\gamma _i(\beta _j\gamma _j\beta _k\gamma _k),$$

with $`1i3`$, $`j=i+1\text{ mod }3`$, $`k=i+2\text{ mod }3`$. The two-dimensional center of this algebra is generated by the generators $`\widehat{i}`$, $`\delta =\delta _1+\delta _2+\delta _3`$. We obtain $`su(3)`$ as the remaining factor algebra, with the eight generators $`\omega _i`$, $`\eta _i`$, $`\delta _1\delta _2`$, $`\delta _2\delta _3`$.

### 4.2. The mass terms

To put various mass terms on the lattice we need lattice versions of the complex unit $`i=\beta ^1\beta ^2`$ as well as of the operators $`C=\beta ^1`$, $`\gamma ^5=\beta ^3`$. These have to be operators which leave the subspaces $`\mathrm{\Omega }^\lambda `$ invariant. Because they are transformations of different components $`\phi _\kappa `$, which are located on different nodes in the staggered subspaces $`\mathrm{\Omega }^\lambda `$, such operators cannot be pointwise operators. As a consequence, it is not possible to preserve all important exact properties of the continuous operators $`i,C,\gamma ^5`$ on the lattice. The question is which of the exact properties are the more important. For example, a variant for $`i`$ which commutes with $`D_h`$ is:

(22)
$$(i_h\phi )_\kappa (n)=(\beta ^1\beta ^2\phi )_\kappa (n+h_1+h_2).$$

But this operator does not define a complex structure, $`(i_h)^21`$ but includes a shift. We can, instead, preserve the property $`i^2=1`$, for example with:

(23)
$$(i_h\phi )_\kappa (n)=(\beta ^1\beta ^2\phi )_\kappa (n+(1)^{n_1}h_1+(1)^{n_2}h_2)$$

In this case $`[i_h,D_h]0`$. Similar variants exist for the operators $`C`$, $`\gamma ^5`$. Which choices for these operators are optimal for the implementation of mass terms has to be left to future research.

## 5. Discussion

We have defined a doubler-free gauge-invariant lattice gauge theory for the $`SU(3)`$ octet action of QCD. Such a discretization is in itself quite useful for applications in lattice QCD: In comparison with the standard approach to lattice QCD we do not have to waste time and memory for the doublers, and we do not have to compute the additional terms to suppress them.

But this discretization seems interesting not only because of these applications. It has been found by consideration of a “space-geometric” interpretation of the whole fermionic sector of the standard model as the bundle $`(T\mathrm{\Lambda }\mathrm{\Lambda })(^3)`$ proposed in . The vector index describes the three fermion generations, and the bundle $`(\mathrm{\Lambda }\mathrm{\Lambda })(^3)`$ is the large distance limit of our geometric octet. The direction-dependent structures of our octet (the complex structure $`i=\beta ^2\beta ^3`$, use of $`t^3`$ in (15)) may be combined into direction-independent structures if we consider all three generations and associate these generations with different preferred directions in space.

On the other hand, there is no simple way to recover manifest relativistic symmetry. In the space-geometric interpretation time is only a non-geometric parameter of evolution. Geometric interpretation is only three-dimensional. This is in conflict with the four-dimensional spacetime interpretation of the gravitational field, but in natural correspondence with the ADM decomposition — a foliation of spacetime into space and time $`M^4M^3`$. In an ADM decomposition the gravitational field is described by a positive-definite three-metric, a three-dimensional vector field, and a positive scalar field. In  we propose to interpret standard model fermions as sections of the bundle $`(T\mathrm{\Lambda }\mathrm{\Lambda })(M^3)`$.

If this discretization really has some fundamental importance, then there should be also a natural possibility to describe electroweak interaction on the geometric octet. The key for understanding chiral gauge fields may be a better understanding of the necessarily non-pointwise lattice approximations of $`i`$, $`C`$, and $`\gamma ^5`$. Note, for example, that the use of an $`i_h`$ which preserves $`(i_h)^2=1`$ like (23) defines a decomposition into two lattice subspaces $`\widehat{\mathrm{\Omega }}_h^\pm `$ which is not exactly preserved by $`D_h`$. A decomposition into exact mass eigenstates on the lattice will give different subspaces which will not be left invariant by the QCD gauge fields. They will coincide only in the continuous limit. What will be the highest order correction terms? It will be some interaction between the mass eigenstates inside the electroweak doublets $`\mathrm{\Omega }^{(1,i,j,k)}\mathrm{\Omega }^{(1,i,j,k)}`$.

Maybe for some appropriate choice of the mass terms this discretization effect gives electroweak interaction or something sufficiently close to it? This hypothesis we leave to future research.


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# Detection of Intergalactic He ii Absorption at Redshift 3.5 Based on observations made with the NASA/ESA Hubble Space Telescope, obtained at the Space Telescope Science Institute, which is operated by the Association of Universities for Research in Astronomy, Inc., under NASA contract NAS 5-26555. These observations are associated with program GO 8582 and 9067.

## 1 INTRODUCTION

Much of the intergalactic hydrogen exists in a highly ionized state as evidenced by the lack of H i Gunn-Peterson troughs in the optical spectra of high-redshift quasars (Gunn and Peterson, 1965). The first presence of a Gunn-Peterson trough was detected in He ii absorption, in a quasar at $`z=3.28`$ (Jakobsen et al., 1994). Follow-up observations at a higher S/N level and spectral resolution (Hogan et al., 1997; Heap et al., 2000) found an average He ii optical depth $`\tau =4.0\pm 0.5`$ at $`z3`$ and at least $`\tau =5`$ at $`z3.2`$. He ii absorption displays significant structure, consisting of unabsorbed void regions and deep absorption troughs (Reimers et al., 1997). When contrasted with the low He ii opacity measured at $`z2.5`$ (Davidsen et al., 1996; Kriss et al., 2001; Zheng et al., 2003) these findings indicate a sudden increase in optical depth. While the large opacity at $`z3.2`$ is conceivably related to a fluctuation in the number of local ionizing sources, it may instead (e.g., if confirmed in multiple additional independent sightlines) more generally signal an epoch in which intergalactic helium is not fully ionized. Recently, a similar pattern for intergalactic hydrogen has been observed in the $`z>6`$ quasars. Becker at al. (2000) and Fan at al. (2002) report a H i optical depth of at least $`\tau =15`$ at $`z6.2`$, signaling the late stages of reionization of the intergalactic medium (IGM). The recent WMAP results (Spergel et al., 2003) suggest that the IGM reionization may have started at $`z17`$, and there may have been a second stage of hydrogen reionization that took place at $`z6`$ (Cen, 2003).

The reionization of intergalactic hydrogen and helium are cosmic milestones. As the early universe cooled and evolved, neutral hydrogen atoms in the IGM gradually became bathed in the ionizing ultraviolet background radiation produced by the first stars and quasars. With increasing UV background radiation, the IGM eventually became fully ionized. Atomic hydrogen and helium are affected by the same ionizing UV radiation in the distant universe – but because the He ii Ly$`\alpha `$ transition is related to the number of ionizing photons at 4 Rydbergs (generally smaller than the number at 1 Rydberg), the the reionization of intergalactic helium is expected to occur later than hydrogen, approximately at $`z35`$ (Haardt and Madau, 1996; Madau at al., 1999; Wyithe and Loeb, 2003). Indirect evidence (Theuns et al., 2002) suggests that the final stage of He ii reionization may take place at $`z3.23.4`$, but only a very small number of independent sightlines have thus far been identified that are suitable to probe He ii even to $`z3`$. Moreover, each such sightline is potentially susceptible to systematic bias; these sightlines are, by selection, the most unobscured of all known quasar sightlines to high redshift. It is therefore important to find additional sightlines (to average over possible systematics in global conclusions), and also to extend He ii studies to higher redshift. Higher redshift sightlines are, of course, potentially the most useful as each such object may provide a measure of He ii absorption spanning the full redshift range likely to be most interest. Our knowledge of the intergalactic helium has been derived from only four lines of sight, and only two are between $`3.0<z<3.3`$. More such examples are needed to establish the statistics and evolution of intergalactic helium at redshift $`z>3`$. The discovery of any bright, UV-unobstructed quasar in this redshift range is therefore interesting.

We report here the detection of a He ii absorption feature in the spectrum of quasar SDSS J234625.67-001600.4 (hereafter abbreviated as SDSSJ2346-0016), the highest redshift He ii feature found to date. This new quasar sightline potentially will allow a measure of He ii absorption from $`z=2.8`$ to $`z=3.5`$ in a single object, efficiently sampling the full redshift range commonly suggested for the epoch of helium reionization. We describe the method of selection, preliminary observations from HST/STIS, and the probability for further discovery of similar objects.

## 2 CANDIDATE SELECTION AND OBSERVATIONS

At redshift $`z\stackrel{>}{}2.8`$ the He ii Ly$`\alpha `$ feature becomes observable with HST. However, the observed UV flux of most high-redshift quasars is strongly suppressed by absorption from intergalactic H i along the line of sight. For objects at $`z3`$, attenuation by individual Ly$`\alpha `$ forest lines is moderate at restframe wavelengths shortward of $`600`$ Å, but Lyman-limit systems (LLSs) can remove significant – and frequently most – of the UV flux in high-redshift quasars (Møller and Jakobsen, 1990). Not until recently have quasar catalogs provided sufficient numbers of bright, high-redshift candidates to begin to outweigh these difficulties. To date extensive searches have revealed only four such quasar sightlines with He ii absorption features. Such a sample is too small to confidently understand the possible systematic uncertainties in the resulting cosmological inferences.

The Sloan Digital Sky Survey (SDSS; York et al., 2000) plans to image a quarter of the sky through five broadband filters (Fukugita et al., 1996) and to obtain spectra of approximately one million galaxies and 100,000 quasars. The survey employs a dedicated 2.5m telescope at Apache Point Observatory to obtain images (Gunn et al., 1998), and automated pipelines (Pier et al., 2003; Smith et al., 2002; Stoughton et al., 2002) process the data. Objects were selected based on their broadband SDSS colors (Hogg et al., 2001). Richards et al. (2002) describe the SDSS quasar selection algorithm. The spectrophotometric calibration includes scaling by wider aperture ”smear” exposures to the photometry from the imaging data. Details regarding the spectroscopic system and analysis pipelines may be found in Stoughton et al. (2002) and Blanton at al. (2003). The Early Data Release (EDR) Quasar Catalog contains 3814 quasars, 3000 discovered by the SDSS (Schneider et al., 2002). The redshift-magnitude distribution of the 302 EDR quasars at $`z>2.5`$ are shown in Figure 1.

The SDSS provides an excellent sample in which to search for quasar candidates with He ii absorption features. We selected a sample of optically bright ($`i<18.5`$) quasars at redshift $`z>2.9`$ for an HST snapshot survey to search for He ii absorption edges in the UV. The snapshot program used the Space Telescope Imaging Spectrograph (STIS); only one out of the 24 candidates observed by the programs exhibited flux at the expected location of He ii absorption.

The optical spectrum of SDSSJ2346-0016 ($`i=17.8`$) was processed using the standard SDSS spectroscopic data reduction pipeline, and is shown in Figure 2. The redshift is measured using the peak of several emission lines: C IV $`\lambda `$1549, O I $`\lambda `$1304, C II $`\lambda `$1334, Si IV+O IV $`\lambda `$1400, and Ly$`\alpha `$, and the averaged value is $`z=3.49\pm 0.03`$. The Ly$`\alpha `$ forest lines set in at $`5476.2`$ Å, corresponding to $`z=3.5047`$.

The ultraviolet HST/STIS spectroscopic snapshot of SDSSJ2346-0016 was performed on 2002 May 18. The data were obtained with the G140L grating and a $`52\mathrm{}\times 0.5\mathrm{}`$ slit. covering the wavelength range of 1150 to 1700 Å. The spectral resolution was approximately 1 Å, and the exposure time was 600 seconds. The HST spectrum extraction was done manually, and processed using the standard STIS pipeline for wavelength and flux calibration. Figure 3 shows the spectrum binned by 9 pixels ($`2.7`$ Å). It was fit with a power-law continuum, a Ly$`\alpha `$ emission line, and an absorption edge. The fitted absorption edge is at $`1369\pm 2`$ Å, with a longward continuum level at $`f_\lambda 10^{16}`$ ergs s-1 cm-2 Å-1. No flux is detected at the wavelengths below 1360 Å. Between 1330 and 1360 Å, the average flux is $`(0.05\pm 0.8)\times 10^{17}`$ ergs s-1 cm-2 Å-1, corresponding to an optical depth of $`6_3^+\mathrm{}`$.

The match between the redshifts of H i Ly$`\alpha `$ and the He ii Ly$`\alpha `$ features strongly suggests, at a 98% level, that the observed UV absorption edge is not merely coincidental. The 2% probability is based on the expected number of LLSs per redshift interval (Storrie-Lombardi et al., 1994). If this observed break is a LLS, the restframe cutoff wavelength is at 920 Å or longer, due to the combined effect of high-order Lyman-series lines. Such a system would be at $`z0.49`$, and a pair of Mg II lines may be expected around 4163.7/4174.4 Å. Between 4160 and 4180 Å there are three absorption lines in the SDSS spectrum: 4180.6 Å(EW$`2.4`$ Å), 4167.3 Å (EW$`1.5`$ Å) and 4161.9 Å (EW$`4.4`$ Å). If any of them is Mg II 2803 Å, a counterpart feature is expected approximately at the wavelength 10.5 Å shortward. No such lines are identified within 2 Å at the expected wavelength and within 30% of the expected intensity (50%).

## 3 IMPLICATIONS

The study of He ii absorption in this new unobscured quasar sightline (and others extending to similarly high redshifts) will allow significant progress in IGM studies. For example, if helium in the IGM is not fully ionized at $`z=3.50`$, the high He ii opacity would result in a damping profile, which may be detected even at low spectral resolution (Miralda-Escudé et al., 1998). This profile is characterized by a redward wavelength shift of a trough from the expected position of He ii Ly$`\alpha `$ emission, on the order of 2-10 Å. The limited signal-to-noise level of our detection spectrum is insufficient to accurately measure such a feature; future observations with STIS or COS (Cosmic Origins Spectrograph) with significantly longer exposures may establish conclusive evidence. The diagnosis of such a feature may be complicated by the proximity effect (Madau and Rees, 2001), and residual infall of matter into the deep potential well of the quasar host galaxy may also give rise to such absorption feature (Barkana and Loeb, 2002). However, previous observations of He ii absorption in other $`z>3`$ quasars suggest that these effect may not be always present, as high-opacity clouds near the quasar may block the ionizing radiation from the quasar itself (Heap et al., 2000).

Should future observations of this object reveal the proximity effect, the data are useful to estimate the intensity of the metagalactic UV background radiation (Zheng et al., 2003; Miralda-Escudé et al., 1998) and the baryon density of the IGM (Hogan et al., 1997; Anderson et al., 1999). It is known that He ii absorption at $`z>3`$ is represented by high opacity of $`\tau >3`$. The wavelength baseline between 1050 and 1370 Å in a HST spectrum will be the longest to reveal the ionization history of intergalactic helium.

This detection strengthens our confidence in future discoveries of similar features at higher redshifts. Model simulations of the IGM (Møller and Jakobsen, 1990) suggest a success rate of approximately 7% in finding a $`z>3`$ quasar whose flux at 300 Å (restframe) may be detected. This appears to be consistent with our detection rate of 4% (one in 24 objects) and that of a similar program (HST GO 8287, one detection in 26 objects). While the lines of sight towards objects at even higher redshifts will encounter more intervening LLSs, these additional systems will not affect the He ii detection in a significant manner – they set in at long wavelengths ($`\stackrel{>}{}4100`$ Å), and their optical depths recover quickly with $`\tau \lambda ^3`$. Therefore, the effect on He ii detection at $`z>3.5`$ is determined mainly by the LLSs at $`z<3.5`$. The large number of SDSS quasars should provide several hundreds of quasars at $`z>3.5`$ that are sufficiently bright for future study. The cases confirmed to be unobscured will be studied with HST’s STIS and/or Cosmic Origins Spectrograph (COS) with significantly higher sensitivity.

The large span in IGM redshift accessible to He ii studies in each such suitable high redshift quasar will provide critical information on the reionization history of the IGM. The anticipated large sample size will allow assessment of, and averaging over, potential systematic biases that may be present in the current critically small sample, as well as the cosmological inferences obtained therefrom.

Funding for the creation and distribution of the SDSS archive has been provided by the Alfred P. Sloan Foundation, the Participating Institutions, the National Aeronautics and Space Administration, the National Science Foundation, the U.S. Department of Energy, the Japanese Monbukagakusho, and the Max Planck Society. The SDSS Web site is http://www.sdss.org/. The SDSS is managed by the Astrophysical Research Consortium (ARC) for the Participating Institutions. The Participating Institutions are The University of Chicago, Fermilab, the Institute for Advanced Study, the Japan Participation Group, The Johns Hopkins University, Los Alamos National Laboratory, the Max-Planck-Institute for Astronomy (MPIA), the Max-Planck-Institute for Astrophysics (MPA), New Mexico State University, University of Pittsburgh, Princeton University, the United States Naval Observatory, and the University of Washington. Support for this research was provided by NASA through grants 8582 and 9067 from the Space Telescope Science Institute, which is operated by the Association of Universities for Research in Astronomy, Inc., under NASA contract NAS 5-26555.


text:
# Again on the non-existence of gravitational waves and of black holes

## Abstract.

Very straightforward arguments proving the physical non-existence of GW’s and of BH’s. They are so simple that even the members of the Wheelerian establishment will understand them.

In course of publication on *Spacetime & Substance*
*An obvious premise*: in (the exact, i.e. non-approximate ) general relativity (GR) only the concepts and the results that are independent of the choice of the system of *general* co-ordinates have a physical meaning.

*i*) Let us consider any solution of the Einstein field equations of GR which has – in a given co-ordinate system – a definite undulatory character, i.e. that represents a gravitational wave (GW). Now, through a *finite* sequence of co-ordinate transformations, endowed with suitable undulating properties, the primary wave character of our solution can be fully *obliterated*. Thus, this character has no *physical* meaning, it is only a mathematical property of the original co-ordinate system. *Q*.*e*.*d*. –

*i*’) A first proof of the physical non-existence of the GW’s was given in 1917 by Tullio Levi-Civita . Other proofs have been published in recent years by the present writer .

*ii*) As it was remarked by Eddington , the solution of the problem of the Einsteinian gravitational field generated by a point mass $`M`$ (at rest) is given – if $`r`$, $`\vartheta `$, $`\phi `$ are spherical polar co-ordinates – by the following spacetime interval:

(1)
$$\text{d}s^2=\left[1\frac{2m}{f(r)}\right]c^2\text{d}t^2\left[1\frac{2m}{f(r)}\right]^1\left[\text{d}f(r)\right]^2\left[f(r)\right]^2\left[\text{d}\vartheta ^2+\mathrm{sin}^2\vartheta \text{d}\phi ^2\right],$$

where $`mGM/c^2`$, and $`G`$ is the gravitational constant; $`f(r)`$ is *any* regular function of $`r`$.

Now, the invention of the black holes (BH’s) is due to a (mis)interpretation of that form of solution (1) for which $`f(r)r`$: it is the so-called *standard* solution, erroneously named “Schwarzschild solution”. In reality, Karl Schwarzschild chose $`f(r)[r^3+(2m)^3]^{1/3}`$, see ; this *original* Schwarzschildean form is singular only at the spatial point $`r=0`$. Thus, the notion of BH does *not* have a physical meaning, it is only a (fictive) by-product of a very particular choice of the function $`f(r)`$. *Q*.*e*.*d*. –

APPENDIX

All the (erroneous) *loci communes* concerning the GW’s and the BH’s are respectively illustrated in the review articles by Schutz  and by Celotti *et alii* .

*“Truth is aristocratic”.*

Howleglas


text:
# Cooperative Jahn-Teller Distortion in PrO2

## I Introduction

In recent years there has been a resurgence of interest in phenomena associated with orbital degrees of freedom, Tokura and Nagaosa (2000) such as orbital ordering, orbital waves (“orbitons”) Saitoh et al. (2001) and unusual spin-orbital liquid ground states. Khaliullin and Maekawa (2000); Khaliullin (2001) Much of the work has been stimulated by studies of the perovskite-based transition-metal oxides, e.g. the colossal magnetoresistance manganites, whose properties can be strongly influenced by the extent to which orbital degrees of freedom are quenched by Jahn-Teller distortions of the lattice or coupled to other electronic degrees of freedom.

Jahn-Teller and orbital phenomena also occur in compounds containing localized 4$`f`$ and 5$`f`$ electrons. Among the simplest of these, the fluorite-structure actinide dioxides UO2 and NpO2 have been investigated for many years, Santini et al. (1999); Paixão et al. (2002) and are now understood to exhibit complex ordered phases at low temperatures involving coupled electric and magnetic multipoles as well as (in the case of UO2) a lattice distortion.

Unusual magnetic effects have also been found in the fluorite-structure lanthanide dioxide PrO2. Some years ago, PrO2 was found to have an anomalously small ordered moment in the antiferromagnetic phase. Kern et al. (1984) Very recently, we discovered a broad continuum in the magnetic excitation spectrum of PrO2 probed by neutron inelastic scattering, which we ascribed to Jahn-Teller fluctuations involving the orbitally-degenerate 4$`f`$ ground state and dynamic distortions of the lattice. Boothroyd et al. (2001) In a separate neutron diffraction experiment Gardiner et al. (2002) we found evidence that the antiferromagnetic structure contains a component with twice the periodicity of the accepted type-I magnetic structure. Kern et al. (1984)

In this paper we follow up our previous work Boothroyd et al. (2001); Gardiner et al. (2002) with further experimental results on the electronic and magnetic behaviour of PrO2. Our main results come from neutron and x-ray diffraction measurements of the crystallographic and magnetic structure of PrO2 in the temperature range 2–300 K. These reveal the existence of an internal distortion of the fluorite structure below $`T_\mathrm{D}=120`$ K and a related distortion of the antiferromagnetic structure below $`T_\mathrm{N}=13.5`$ K. We also report measurements of the magnetic susceptibility, the specific heat capacity, and the electrical conductivity of PrO2, which allow us to determine the effective paramagnetic moment of the Pr ion, the degeneracy of the 4$`f`$ electron ground state, and the activation energy of the charge carriers.

## II Sample preparation

Measurements were made on single crystal and polycrystalline samples of PrO2. The single crystals used for the neutron diffraction and conductivity measurements were taken from a batch prepared several years ago by a hydrothermal procedure. McKelvy and Eyring (1983) The sample used for neutron diffraction was the largest of the batch, with a mass of $`1`$ mg, while the sample used for the conductivity measurements was somewhat smaller. Both were irregularly shaped. Polycrystalline samples were used for the x-ray diffraction, magnetic susceptibility and specific heat capacity measurements. These were prepared by oxidation of commercially obtained Pr6O11. The starting powder was first baked in air at 1000C for $``$ 11 hours, then annealed in flowing oxygen at 280C for 30 days. The powder was reground approximately once a week during the annealing. Synchrotron x-ray diffraction showed that the final product contained $`1`$% of residual Pr6O11.

## III Structural Investigation

We investigated the crystallographic and magnetic structure of PrO2 by performing a neutron diffraction study on a single crystal sample. The experiment was carried out on the D10 four-circle diffractometer at the Institut Laue-Langevin. We used an Eulerian cradle for crystal orientation and a position sensitive detector. The latter was kept in the scattering plane at all times. The diffractometer configuration was as follows: vertically curved pyrolytic graphite (002) or Cu (200) monochromator, no collimators, circular aperture of diameter 6 mm before the sample and rectangular aperture of dimensions 20 mm $`\times `$ 25 mm before the detector. We used incident neutron wavelengths of 2.3575 Å ($`\lambda _1`$) and 1.2579 Å ($`\lambda _2`$) from the pyrolytic graphite and Cu monochromators respectively, with a pyrolytic graphite filter for the former to reduce the half-wavelength contribution. The larger wavelength provided greater flux, while the smaller provided greater coverage of reciprocal space.

The single crystal sample was mounted on a thin aluminium pin and aligned such that the \[1$`\overline{1}`$0\] direction lay along the axis of the pin. The pin was attached to the Eulerian cradle inside a helium flow cryostat.

### III.1 Measurements

The quality of the crystal was checked by performing crystal rotation scans ($`\omega `$-scans) of the strongest structural Bragg reflections at room temperature. The peak widths were found to be within the experimental resolution.

To examine the crystallographic structure of PrO2, as many structural Bragg reflections as possible were measured by $`\omega `$-scan at the accessible positions in reciprocal space satisfying the selection rules for the fluorite structure ($`h`$, $`k`$ and $`l`$ all even or all odd). This set of reflections was measured at $`\lambda _1`$ at temperatures of 2 K, 20 K, 90 K, 150 K and 300 K. At some temperatures the full set was measured at both neutron wavelengths ($`\lambda _1`$ and $`\lambda _2`$).

The intensities of the strongest reflections (e.g. (220), (400)) were found to change rapidly with temperature. The temperature dependence of these reflections was measured more carefully by performing $`\omega `$-scans at 2 K intervals between 2 K and 130 K, then at 5 K intervals between 130 K and 300 K. Figure 1 shows the integrated intensity of the scan as a function of temperature. A sharp rise in intensity can be seen below 120 K. We found that the rise was greatest for the strongest reflections and more pronounced at the larger wavelength $`\lambda _1`$, suggesting a sudden reduction in extinction. A possible explanation for this observation is a reduction in grain size caused by the strain associated with a structural distortion.

The temperature dependence of the lattice parameter, estimated from the variation of the Bragg angle with temperature for the (400) reflection, also shows a sharp change at $``$ 120 K (see Fig. 2: closed circles). Although the absolute value of the lattice parameter obtained by this method is inaccurate, as it relies on the crystal being perfectly aligned, the data nevertheless give a good qualitative indication of the way the lattice parameter changes with temperature. It is seen to decrease linearly from 300 K to $`120`$ K, below which it becomes approximately constant, dipping slightly at $`18`$ K. The open circles in Figure 2 show data taken from a high-resolution x-ray powder diffraction study on PrO2 performed at the Swiss-Norwegian Beamline BM1B at the European Synchrotron Radiation Facility (ESRF). There are fewer points in this plot, but the absolute value of the lattice parameter is much more accurate because it has been obtained by Rietveld refinement of the diffraction pattern. The temperature variation found by x-ray diffraction is consistent with that found by neutron diffraction.

To probe the magnetic structure, as many magnetic Bragg reflections as possible were measured by $`\omega `$-scan at the accessible positions in reciprocal space satisfying the selection rules for the antiferromagnetic (AFM) type-I magnetic structure ($`h`$, $`k`$ and $`l`$ a mixture of even and odd). This set of reflections was measured at temperatures of 2 K and 20 K (below and above $`T_\mathrm{N}`$) using only the larger wavelength $`\lambda _1`$, since this provided higher flux.

In addition to the above measurements we also performed $`\omega `$-scans at a number of positions in reciprocal space with half-integer Miller indices. The object of these measurements was to search for peaks seen previously in a powder diffraction experiment. Gardiner et al. (2002) The scans were performed at temperatures of 2 K, 20 K and 150 K.

At $`T`$ = 2 K, we found reflections at positions satisfying the selection rule $`h=n+1/2`$, $`k`$ = odd, $`l`$ = even, where $`n`$, $`k`$ and $`l`$ are integers, and $`h`$, $`k`$ and $`l`$ can be commuted. At $`T=20`$ K (above $`T_\mathrm{N}`$), we found reflections at exactly the same positions, except that those with $`l=0`$ were no longer present. The strongest half-integer reflection we observed was $``$1% of the intensity of the strongest fluorite reflection. At $`T=150`$ K, all the half-integer reflections had disappeared. Figure 3 shows $`\omega `$-scans of the $`\left(\frac{1}{2}10\right)`$ and $`\left(\frac{1}{2}14\right)`$ reflections. These are typical of the two observed sets of half-integer reflections: those with $`l=0`$ and those with $`l0`$.

We measured the temperature dependence of the $`\left(\frac{1}{2}10\right)`$ reflection by counting at the peak centre at a series of temperatures between 2 K and 20 K. The temperature dependence of the stronger $`\left(\frac{1}{2}14\right)`$ reflection was measured by performing $`\omega `$-scans at a series of temperatures between 2 K and 150 K.

Figure 4 compares the temperature dependence of the $`\left(\frac{1}{2}10\right)`$ reflection with that of the magnetic reflection (100). To within experimental uncertainty, both reflections disappear at the antiferromagnetic ordering temperature $`T_\mathrm{N}`$. We were able to determine $`T_\mathrm{N}`$ for both reflections by fitting the data using order parameter curves of the form

$$I(T_\mathrm{N}T)^{2\beta },$$
(1)
where $`I`$ is the peak count and $`\beta `$ is the critical exponent. For the (100) reflection we found $`T_\mathrm{N}=13.41\pm 0.04`$ K, while for the $`\left(\frac{1}{2}10\right)`$ reflection we found $`T_\mathrm{N}=13.5\pm 0.2`$ K. Since these are in excellent agreement, it is likely that both reflections are magnetic in origin and belong to the same magnetic phase. The existence of half-integer magnetic Bragg reflections indicates that the magnetic unit cell is doubled along one crystal axis.

Figure 5 shows the temperature-dependence of the $`\left(\frac{1}{2}14\right)`$ reflection. It is found to disappear at $`T_\mathrm{D}=120\pm 2`$ K, which is the same as the temperature below which we observed a sharp rise in the intensities of the large structural reflections. This strongly suggests that the $`\left(\frac{1}{2}14\right)`$ reflection is structural in origin. The existence of half-integer structural reflections indicates that the crystallographic unit cell is also doubled along one crystal axis.

A re-examination of previous data taken with a powder sample on the POLARIS diffractometer at the ISIS facility Gardiner et al. (2002) has now also revealed half-integer structural reflections. Although two of the magnetic half-integer reflections had been seen previously, the structural reflections had not been noticed, due to the nearby presence of other peaks of similar intensity, which were probably due to scattering from the sample environment. The x-ray powder diffraction study mentioned above also confirms the presence of half-integer structural reflections.

### III.2 Structure analysis

To identify the nature of the crystallographic structure below $`T_\mathrm{D}=120`$ K and the magnetic structure below $`T_\mathrm{N}=13.5`$ K, we performed a detailed analysis of the intensities of the observed integer and half-integer structural and magnetic reflections at low temperatures.

After background subtraction, each $`\omega `$-scan was integrated using the extended trapezoidal rule Press et al. (1992) (a simple method of numerical integration), corrected for the Lorentz factor, normalised to the monitor count and the intensity of the (311) reflection, and multiplied by a wavelength-dependent scale factor to enable direct comparison between the intensities of the observed structural reflections and their calculated structure factors. The (311) reflection was used for normalisation because it was one of the weakest reflections accessible at both wavelengths, so it was little affected by extinction. In addition, its structure factor contained no contribution from the oxygen ions, so it was unaffected by the distortion. Finally, the corrected and scaled intensities were averaged over symmetry-equivalent reflections to guard against the possibility that a chance uneven distribution in symmetry-equivalent structural or magnetic domain populations might affect the measured intensity of any given reflection (although this was unlikely since the majority of the symmetry-equivalent reflections were equal in intensity to within experimental uncertainty).

We then considered distortions of the fluorite crystallographic structure and the type-I antiferromagnetic structure which would give rise to structure factors in agreement with the relative intensities and selection rules of the observed reflections. Such structures were identified by trial and error. However, in the case of the crystallographic structure we were guided by the results of the x-ray diffraction study, which revealed no splitting of the reflections caused by the fluorite structure. This indicated that the Pr lattice remained undisturbed, and any distortion must therefore be due to an internal rearrangement of the oxygen atoms.

Once a suitable distorted crystallographic structure was found, we refined the overall magnitude of the oxygen displacements by a least squares method to achieve the best possible agreement between the structure factors and peak intensities. For the magnetic structure we used the ratio of the peak intensity to the magnetic structure factor for each reflection to obtain a value for the ordered moment $`\mu `$ of the Pr ion.

The structure factors of the structural reflections are given by

$$|F_\mathrm{N}(𝐐)|^2=\left|\underset{j}{}\overline{b}_j\mathrm{e}^{\mathrm{i}𝐐.𝐫_j}\mathrm{e}^{W_j(Q,T)}\right|^2$$
(2)
where the summation index $`j`$ runs over all the atoms in the unit cell, $`\overline{b}_j`$ is the nuclear scattering length of the $`j`$th atom averaged over all of its isotopes, $`𝐫_j`$ is the position of the $`j`$th atom within the unit cell, and $`\mathrm{e}^{W_j(Q,T)}`$ is the Debye-Waller factor (we set this equal to 1, since the measurements were made at low temperatures) and $``$ denotes an average over all symmetry-equivalent structural domains. The scaled, integrated intensities of the structural reflections are equal to $`|F_\mathrm{N}(𝐐)|^2`$. The structure factors of the magnetic reflections are given by

$$|F_\mathrm{M}(𝐐)|^2=\underset{\alpha \beta }{}\left(\delta _{\alpha \beta }\widehat{Q}_\alpha \widehat{Q}_\beta \right)F_\mathrm{M}^\alpha (𝐐)F_\mathrm{M}^\beta (𝐐),$$
(3)
where the summation indices $`\alpha `$ and $`\beta `$ run over the cartesian co-ordinates $`x,y`$ and $`z`$, $`\delta _{\alpha \beta }`$ is the Kronecker delta, * denotes the complex conjugate, $`\widehat{Q}_\alpha `$ is the $`\alpha `$-component of the unit scattering vector and $``$ denotes an average over all symmetry-equivalent magnetic domains. In the dipole approximation $`F_\mathrm{M}^\alpha (𝐐)`$ is given by

$$F_\mathrm{M}^\alpha (𝐐)=f(𝐐)\underset{j}{}\widehat{\mu }_j^\alpha \mathrm{e}^{\mathrm{i}𝐐.𝐫_j}\mathrm{e}^{W_j(Q,T)},$$
(4)
where the summation index $`j`$ runs over all the magnetic atoms in the magnetic unit cell, $`\widehat{\mu }_j^\alpha `$ is the $`\alpha `$-component of a unit vector in the direction of the magnetic moment of the $`j`$th magnetic atom, $`𝐫_j`$ is the position of the $`j`$th magnetic atom within the magnetic unit cell, $`f(𝐐)`$ is the magnetic form factor of the Pr4+ ion and $`\mathrm{e}^{W_j(Q,T)}`$ is the Debye-Waller factor (set equal to 1). The scaled, integrated intensities of the magnetic reflections are proportional to $`\left(\frac{\gamma r_0}{2}\right)^2\left(\frac{\mu }{\mu _\mathrm{B}}\right)^2|F_\mathrm{M}(𝐐)|^2`$, where $`\left(\frac{\gamma r_0}{2}\right)^2=72.4`$ mb ($`=7.24`$ fm2) and $`\mu _\mathrm{B}`$ is the Bohr magneton.

For reference we note the structure factors of the fluorite structure here:

$$|F_\mathrm{N}(𝐐)|^2=\{\begin{array}{cc}\text{336\hspace{0.17em}fm}^2,\hfill & h\text{}k\text{}l\text{ all odd}\hfill \\ \text{791\hspace{0.17em}fm}^2,\hfill & h+k+l=2n\hfill \\ \text{4194\hspace{0.17em}fm}^2,\hfill & h+k+l=4n.\hfill \end{array}$$
(5)
These were computed using the fluorite unit cell, which contains four Pr ions and eight O ions. For the half-integer reflections (both structural and magnetic) we used a unit cell that was doubled along one axis, thus containing eight Pr ions and sixteen O ions. In order to allow direct comparison with the structure factors of the fluorite structure we divided the structure factors $`F_\mathrm{N}(𝐐)`$ and $`F_\mathrm{M}(𝐐)`$ of the half-integer reflections, calculated in the doubled cell, by 2.

#### III.2.1 Distorted crystallographic structure

One of the simplest structures that possesses structure factors in agreement with the intensities of the half-integer structural reflections is shown in Fig. 6(a). The Pr lattice is undisturbed, but the oxygen ions are each displaced by an amount $`d`$ in a direction perpendicular to that along which the unit cell is doubled (in Fig. 6 the doubling is along the $`x`$-direction and the displacements are along the $`y`$-direction). The oxygen cubes in the two halves of the doubled unit cell are sheared in opposite senses, so we will refer to this structure as the “sheared” structure. The space group is Imcb (a variant of Ibam, space group 72), with the origin shifted by $`\frac{1}{4}`$ of the unit cell length along the orthorhombic $`a`$-direction (the $`x`$-direction in Fig. 6).

A simple least squares refinement of the oxygen displacement $`d`$, based on comparison of the domain-averaged structure factors111Averaging over symmetry-equivalent domains in Equation (2) means that we compare the observed intensity $`I(hkl)_{\mathrm{obs}}`$ with the calculated intensity $`\frac{1}{6}[I(hkl)_{\mathrm{calc}}+I(klh)_{\mathrm{calc}}+I(lhk)_{\mathrm{calc}}+I(\overline{h}lk)_{\mathrm{calc}}+I(\overline{k}hl)_{\mathrm{calc}}+I(\overline{l}kh)_{\mathrm{calc}}]`$, where $`h`$, $`k`$ and $`l`$ are in the cubic cell. This accounts for three-fold twinning around the cubic $`111`$ direction and reflection across the cubic $`(01\overline{1})`$ plane. and the observed intensities of the half-integer reflections, yielded $`d=0.0726(54)`$ Å. The structure factors and observed intensities at $`T=20`$ K are listed in Table 1, and a plan view of the structure with displacements to scale is shown in Fig. 6(b). A full crystal structure refinement using the Cambridge Crystallography Subroutine Library (CCSL) yielded $`d=0.0664(17)`$ Å.

An identical shearing of the oxygen cube was originally proposed for an internal distortion observed in UO2, Faber and Lander (1976) although in that compound there was no evidence for a doubling of the unit cell. In UO2 the oxygen ions are displaced by 0.014 Å from their fluorite structure sites, so the oxygen displacements in PrO2 are five times as large, and this is reflected in the high value of the transition temperature. It is now accepted that the oxygen configuration in UO2 forms a triple-$`𝐪`$ structure. Burlet et al. (1986) However, there is currently no reason to assume that the same is true in PrO2.

It is interesting to note that there are two distinct Pr sites in the sheared structure, each of which occurs with equal frequency. The two sites have different surrounding oxygen configurations, which are shown in Fig. 7. At one site the oxygens form a parallelohedron (a polyhedron with two square faces, two rectangluar faces and two parallelogram faces), while at the other they form a polyhedron with four parallelogram faces and four triangular faces.

Although the distorted structure described above is consistent with the intensities of the observed reflections, it is not the only such structure. For example, a superposition of two structures identical to the sheared structure, but with oxygen displacements of 0.0511 Å in mutually perpendicular directions, gives similar agreement between the calculated structure factors and observed intensities. The overall displacement of each oxygen ion in that case is $`\sqrt{2}\times 0.0511=0.0722`$ Å.

The “chiral” structure shown in Fig. 8 is also consistent with the intensities of the observed reflections, and has the additional advantages of having a lower Jahn-Teller energy Jensen  and a single Pr site. A chiral model is adopted for the oxygen displacement vector, but the structure factors and the magnitude of the oxygen displacement are almost identical to that of the sheared structure (a simple least squares refinement yielded $`d=0.0726(54)`$ Å, whereas a full crystal structure refinement using CCSL yielded $`d=0.0663(16)`$ Å). The space group is I4(1)/acd (space group 142), with Pr at positions $`8a`$ $`(0,\frac{1}{4},\frac{3}{8})`$ and O at positions $`16e`$ $`(\frac{1}{4}+d,0,\frac{1}{4})`$, where the origin is chosen to be at the centre of inversion, and $`c`$ is the unique axis.

#### III.2.2 Doubled magnetic structure

The presence of half-integer magnetic reflections alongside stronger integer magnetic reflections indicates that the magnetic structure consists of two components: a primary component with the same unit cell as the fluorite structure and a secondary component with a unit cell that is doubled along one crystal axis. This picture fits well with the model of the distorted crystallographic structure, in which the Pr lattice remains unchanged, but the oxygen sublattice undergoes an internal distortion which gives rise to a component of the structure with a doubled unit cell.

The easiest way to analyse the magnetic structure is to consider the two components separately, so that the overall structure can be visualised by performing a vector addition of the two components of the magnetic moment for each Pr ion in the doubled unit cell.

The primary component of the magnetic structure is the AFM type-I structure, shown in Fig. 9. This gives rise to the integer magnetic reflections. Under ambient conditions it is not possible to distinguish between the three multi-$`𝐪`$ structures shown in the figure, but in view of the fact that the structural distortion doubles the unit cell along one crystal axis only, the single-$`𝐪`$ structure seems the most likely candidate.

The configuration of the magnetic moments in the secondary component of the magnetic structure was deduced using a technique similar to that for the structural distortion. In our search for possible configurations we found it impossible to conceive of a magnetic structure that would give rise to reflections at $`l=0`$ alone. Symmetry requires that if a structure gives rise to reflections at $`l=0`$ it will also give rise to reflections at all positions with $`l=`$ even. This means that many of the magnetic half-integer reflections coincide with the structural ones. However, since little change was observed in the intensities of the structural half-integer reflections below $`T_\mathrm{N}`$ (see Fig. 3), it can be assumed that the magnetic intensities at these positions are much smaller than the structural intensities. We have therefore made no attempt to analyse the magnetic contribution at these positions. Our analysis of the secondary component of the magnetic structure is based solely on the half-integer reflections observed at $`l=0`$.

The number of possible magnetic structures consistent with the observed half-integer intensities is quite large. Two of the simplest possible structures are shown in Fig. 10. Both possess identical magnetic structure factors, shown in Table 2. Figure 10(a) corresponds to the chiral model for the structural distortion shown in Fig. 8, whereas Fig. 10(b) corresponds to the model shown in Fig. 6. The moments of the Pr ions in both magnetic structures point along directions perpendicular to the direction along which the unit cell is doubled. Similar structures in which some or all of the moments point along the doubling direction give poorer agreement with the relative intensities of the observed reflections. It should be mentioned that the $`\left(\frac{5}{2}10\right)`$ reflection had a high and rather sloping background, due to its proximity in reciprocal space to an aluminium powder line, so its intensity is somewhat unreliable.

The magnetic moment of the Pr ion can be calculated for each of the two components of the magnetic structure as follows:

$$\frac{\mu }{\mu _\mathrm{B}}=\sqrt{\frac{I_\mathrm{M}(𝐐)|F_\mathrm{N}(𝐐^{})|^2}{\left(\frac{\gamma r_0}{2}\right)^2I_\mathrm{N}(𝐐^{})|F_\mathrm{M}(𝐐)|^2}},$$
(6)
where $`\mu `$ is the magnetic moment of the Pr ion in one component of the magnetic structure, $`I_\mathrm{M}(𝐐)`$ is the integrated intensity of a magnetic reflection with reciprocal lattice vector $`𝐐`$, $`|F_\mathrm{M}(𝐐)|^2`$ is the magnetic structure factor of this reflection, $`I_\mathrm{N}(𝐐^{})`$ is the integrated intensity of a nuclear reflection with reciprocal lattice vector $`𝐐^{}`$ and $`|F_\mathrm{N}(𝐐^{})|^2`$ is the nuclear structure factor of this reflection.

For each of the magnetic reflections we calculated the magnetic moment of the Pr ion from the observed magnetic intensity and the intensity of the (311) nuclear reflection. The resulting values of the Pr moment were averaged to reduce the uncertainty. For the primary (AFM type-I) component of the magnetic structure we obtained $`\mu _1=(0.65\pm 0.02)\mu _\mathrm{B}`$. This is in good agreement with a previous value of $`(0.68\pm 0.07)\mu _\mathrm{B}`$ Gardiner et al. (2002) obtained by neutron diffraction from the same single crystal sample. Previous powder diffraction experiments have yielded values of $`(0.6\pm 0.1)\mu _\mathrm{B}`$ Kern et al. (1984) and $`(0.572\pm 0.012)\mu _\mathrm{B}`$, Gardiner et al. (2002) but it is likely that these are in error, since in both cases the Rietveld refinement assumed the crystallographic structure to be fluorite at low temperatures, and therefore took no account of the structural distortion. For the secondary (doubled) component of the magnetic structure we obtained $`\mu _2=(0.35\pm 0.04)\mu _\mathrm{B}`$ (we disregarded the unreliable $`\left(\frac{5}{2}10\right)`$ reflection when averaging the values of $`\mu _2`$ obtained from the half-integer reflections). The uncertainties on our values of $`\mu _1`$ and $`\mu _2`$ are dominated by the uncertainty on the magnetic form factor of Pr4+.

## IV Bulk properties

We now present measurements of some of the bulk properties of PrO2: magnetic susceptibility, specific heat capacity and electrical conductivity. These provide support for the findings of the neutron diffraction experiments described above, and reveal clues as to the origin of the structural distortion.

### IV.1 Magnetic susceptibility

We measured the magnetic susceptibility of PrO2 using a commercial SQUID magnetometer, with a powder sample of mass 270 mg. The measurements were made using the reciprocating sample option (RSO), with an applied field of $`H=1`$ T. Data were taken while cooling in steps from $`T=350`$ K to $`T=2`$ K, with a delay to allow temperature equilibriation at each step. A plot of the molar susceptibility (per mole Pr) is shown in Fig. 11. The inset shows the inverse molar susceptibility. Three features are evident. First, there is a peak at $`T=14`$ K, due to antiferromagnetic ordering. Second, there is a change in gradient at $`T=122\pm 2`$ K which is seen most clearly in the inverse susceptibility. Following our structural investigation we can identify this with the internal distortion at $`T_\mathrm{D}`$. This anomaly had not been noticed in previous measurements, Kern (1964); MacChesney et al. (1964) due to the intrinsic noise present. Third, there is an upturn in the susceptibility below $`T6`$ K which is due to the presence of a small amount of Pr6O11 in the sample. We demonstrate this in Figure 12, which shows a plot of the magnetic susceptibility of Pr6O11 measured by AC susceptometry with a powder sample of mass 327 mg. Between 1.5 K and 2.5 K there is evidence for a magnetic transition with glassy characteristics. At 2 K the molar susceptibility (per mole Pr) of Pr6O11 is $`100`$ times that of PrO2, so the upturn below 6 K in the PrO2 susceptibility is consistent with the 1% Pr6O11 impurity known to be present in the sample. There is no feature in the Pr6O11 susceptibility at $`T_\mathrm{D}`$.

We used our measurement of the PrO2 susceptibility to calculate the effective paramagnetic moment of the Pr ion at various temperatures, assuming that the susceptibility obeys the Curie-Weiss law for an antiferromagnet above $`T_\mathrm{N}`$:

$$\chi ^{\mathrm{mol}}=\frac{\mu _{\mathrm{𝑒𝑓𝑓}}^2N_\mathrm{A}}{30k_\mathrm{B}(T+\theta )},$$
(7)
where $`\chi ^{\mathrm{mol}}`$ is the molar magnetic susceptibility, $`\theta `$ is the Weiss constant, $`N_\mathrm{A}`$ is Avogadro’s number, $`k_\mathrm{B}`$ is Boltzmann’s constant and $`\mu _{\mathrm{𝑒𝑓𝑓}}`$ is the effective paramagnetic moment of the Pr ion. $`\chi ^{\mathrm{mol}}`$ is in cgs units (emu \[mol Pr\]-1), as dictated by convention, whereas the quantities on the right hand side of Equation (7) are in SI units. The conversion factor from SI to cgs units is incorporated into the right hand side.

Over the temperature range $`T=250`$–350 K we obtained $`\mu _{\mathrm{𝑒𝑓𝑓}}=2.32\mu _\mathrm{B}`$. This is close to the value of $`2.54\mu _\mathrm{B}`$ expected for a free Pr4+ ion. Below $`T_\mathrm{D}`$ the gradient of the inverse susceptibility first decreases then increases, causing $`\mu _{\mathrm{𝑒𝑓𝑓}}`$ to decrease. This indicates a reduction in the number of magnetic degrees of freedom, which is probably caused by a lifting of the degeneracy of the crystal field ground state by the structural distortion (it is generally accepted that the ground state is a $`\mathrm{\Gamma }_8`$ quartet in the fluorite phase). Kern et al. (1984); Boothroyd et al. (2001)

Although an anomaly at $`T=122`$ K had not been noticed in previous measurements, the curvature of the susceptibility trace below this temperature had been noticed previously by Kern. Kern (1964) When attempting a crystal field analysis he found that his data could not be fitted well with a crystal field of cubic symmetry. He proposed that the oxygen ions surrounding the Pr ion did not in fact form a cube, but that the two at opposite ends of the body diagonal were displaced outwards along the (111) direction, causing a splitting of the $`\mathrm{\Gamma }_8`$ crystal field level into two doublets. Using this modified structure he obtained a good fit to his data over the whole temperature range 0–300 K. He calculated the splitting of the $`\mathrm{\Gamma }_8`$ level to be 28.8 meV.

The significance of this result was later dismissed MacChesney et al. (1964) because the sample used did not exhibit a clear antiferromagnetic transition. Although a discontinuity was observed at 14 K, the susceptibility continued to rise at lower temperatures. The sample had been prepared from a starting material of Pr6O11 by annealing at a temperature of 360C under 5 atmospheres of oxygen pressure. These conditions lie close to the border, on a temperature-pressure diagram, of the regions in which the PrO2 and Pr6O11 phases are stable, so it is likely that the sample was not single phase PrO2. However, x-ray diffraction showed that it had a lattice parameter of $`5.393\pm 0.007`$ Å, which agrees well with the accepted value for PrO2 of $`5.393\pm 0.001`$ Å, and is much less than the value for Pr6O11 of 5.468 Å. Eyring and Baenziger (1963) This suggests that the sample was mostly PrO2, but contained enough of the Pr6O11 phase to obscure partially the antiferromagnetic transition. By adding proportions of our susceptibility data for Pr6O11 and PrO2, and comparing the results with the data obtained by Kern, we estimate that his sample contained $``$ 20% Pr6O11.

Since we believe that Kern’s sample was predominantly PrO2, and we have now obtained direct evidence for an internal distortion of the oxygen sublattice below $`T_\mathrm{D}=120`$ K, we believe that his original crystal field analysis, in particular the 28.8 meV splitting of the $`\mathrm{\Gamma }_8`$ crystal field ground state is still of some relevance below $`T_\mathrm{D}`$.

### IV.2 Specific heat capacity

We measured the specific heat capacity of PrO2 by the relaxation method Bachmann et al. (1972) using a laboratory-built calorimeter. The sample was a disc-shaped pressed pellet of PrO2 powder of diameter 10 mm, thickness 1 mm and mass 83 mg, which was mounted on the sapphire sample platform of the calorimeter using a small amount of Apiezon grease (high thermal conductivity grease).

The measurements were made over a temperature range 2.4 K to 23 K. We measured the heat capacity of the sapphire platform first, then the heat capacity of the sample and platform combined. We obtained the heat capacity of the sample alone by subtracting the former from the latter. Finally, we obtained the specific heat capacity of the sample by dividing by the sample mass.

Figure 13 shows a plot of the specific heat capacity of PrO2 versus temperature. The experimental uncertainty is estimated to be $``$ 5%. A lambda anomaly due to the antiferromagnetic ordering is observed at $`13.5`$ K. This is superimposed on the contribution to the specific heat from vibrations of the crystal lattice.

The specific heat capacity of a pressed pellet of CeO2 powder (commercially obtained) was also measured. This sample had mass 81 mg and was of similar shape to the PrO2 sample. Since CeO2 is non-magnetic, but has the same crystal structure, a similar lattice parameter and similar formula mass to PrO2, it provides a good estimate of the contribution of the crystal lattice to the PrO2 specific heat. The CeO2 data is plotted with the PrO2 data in Fig. 13.

To determine the degeneracy of the crystal field ground state in PrO2, we used our measurement of the specific heat capacity to calculate the change in magnetic entropy on passing through the magnetic transition. The specific entropy is related to the specific heat capacity by the formula

$$s(T)=_0^T\frac{c}{T}dT,$$
(8)
where $`c`$ is the specific heat and $`s`$ is the change in specific entropy between $`T`$ = 0 and a finite temperature $`T`$. The total specific entropy of PrO2 (magnetic entropy $`+`$ lattice contribution) was obtained from the specific heat data by dividing by $`T`$, then integrating by the extended trapezoidal rule. Press et al. (1992) This gave

$$\mathrm{\Delta }s_{\mathrm{total}}=_0^{23}\frac{c(\mathrm{PrO}_2)}{T}dT=\mathrm{\hspace{0.33em}32.9}\mathrm{JK}^1\mathrm{kg}^1.$$
(9)
To obtain the change in magnetic entropy it was necessary to subtract off the lattice contribution. This was estimated using the CeO2 data:

$$\mathrm{\Delta }s_{\mathrm{lattice}}=_0^{23}\frac{c(\mathrm{CeO}_2)}{T}dT=\mathrm{\hspace{0.33em}1.7}\mathrm{JK}^1\mathrm{kg}^1.$$
(10)
By subtracting (10) from (9) we obtained the change in magnetic entropy:

$$\mathrm{\Delta }s_{\mathrm{magnetic}}=\mathrm{\Delta }s_{\mathrm{total}}\mathrm{\Delta }s_{\mathrm{lattice}}=\mathrm{\hspace{0.33em}31.2}\mathrm{JK}^1\mathrm{kg}^1.$$
(11)
From Boltzmann’s law,

$$\mathrm{\Delta }s_{\mathrm{magnetic}}=nk_\mathrm{B}\mathrm{ln}g,$$
(12)
where $`n`$ is the number of magnetic ions per unit mass (for PrO2, $`n=3.48\times 10^{24}`$ kg-1) and $`g`$ is the degeneracy of the ground state above $`T_\mathrm{N}`$ (below $`T_\mathrm{N}`$ the degeneracy is lifted). The entropy changes predicted for a quartet ($`g=4`$) and a doublet ($`g=2`$) ground state are 66.7 JK-1kg-1 and 33.3 JK-1kg-1 respectively. The measured change (11) suggests that the ground state is a doublet. This finding supports a distortion of the crystal structure, which would lift the degeneracy of the $`\mathrm{\Gamma }_8`$ quartet below $`T_\mathrm{D}`$. An extension of the specific heat capacity measurement up to room temperature, to look for an anomaly near 120 K, would be eminently worthwhile.

### IV.3 Electrical conductivity

We measured the electrical conductivity of PrO2 as a function of temperature using a simple probe designed for use with a helium cryostat. Two thin gold wires were attached to opposite sides of the single crystal sample using silver conducting paint (attempts to attach four wires to the tiny crystal were unsuccessful, due to the difficulty in achieving good electrical contact while keeping the contacts separate). The crystal was glued to the copper base of the probe with GE varnish to ensure good thermal contact.

Four-terminal measurements were made of the resistance of the sample + gold wires (this was justified, since the resistance of the crystal was much greater than the resistance of the gold wires) over a temperature range from 5.8 K to 288 K. The temperature was increased in steps, allowing the sample to equilibriate at each new setpoint. Figure 14 shows a plot of current against temperature at a voltage of 3 V. Below $`T`$ 180 K the current became too small to measure reliably. We were unable to determine the absolute value of the electrical conductivity because the shape of the crystal was irregular and its dimensions were not known exactly.

The inset to Fig. 14 shows that the conductivity has an activated behaviour, at least over the temperature range 180–288 K. To determine the activation energy we fitted our data using the Arrhenius form:

$$I=I_0\mathrm{exp}\left(\frac{E_\mathrm{a}}{k_\mathrm{B}T}\right),$$
(13)
where $`I`$ is the current and $`E_\mathrm{a}`$ is the activation energy. We extracted $`E_\mathrm{a}`$ from several runs, each measured at a different constant voltage (between $`5`$ V and $`+5`$ V), and took the mean of these values to obtain $`E_\mathrm{a}`$ = 0.262 $`\pm `$ 0.003 eV for the temperature range 180–288 K. This is much smaller than the band gap of $`2.5`$ eV predicted by band structure calculations, Koelling et al. (1983) and is also smaller than the activation energies of other PrOx materials, which have been reported in the range 0.4–1 eV. Eyring (1979); Subba Rao et al. (1970); Arakawa et al. (1986)

Possible mechanisms for electrical conductivity in PrO2 are (i) ionic conductivity, (ii) intrinsic electronic conductivity due to hopping between Pr sites, (iii) extrinsic electronic conductivity due to impurities. Compounds with the fluorite structure often exhibit ionic conduction when vacancies caused by Schottky or Frenkel defects allow the oxygen ions to hop from site to site. However, at room temperature the number of thermally induced defects is very small, so ionic conductivity in PrO2 is unlikely to be important in this temperature range. It has been suggested that ionic conductivity in PrOx materials is significant only above $`900`$ K. Subba Rao et al. (1970); Arakawa et al. (1986) Therefore, it is most likely that the conductivity in PrO2 is electronic. Given the small activation energy found here, the mechanism warrants further investigation.

## V Discussion and conclusions

We have presented neutron diffraction experiments on single crystal PrO2, which reveal an internal distortion of the oxygen sublattice at $`T_\mathrm{D}=120\pm 2`$ K and a related component of the magnetic structure below $`T_\mathrm{N}=13.5\pm 0.2`$ K. The displacements of the oxygen ions are five times as large as those observed in UO2, Faber and Lander (1976) and this is reflected in the high value of the transition temperature. The observation that both the distorted crystallographic structure and the related component of the magnetic structure have a unit cell that is doubled along one crystal axis with respect to the fluorite structure suggests that the displacement of the oxygen ions affects the magnetic ordering of the Pr sublattice.

Our measurement of the specific heat capacity indicates that the crystal field ground state of the Pr 4$`f`$ electron is a doublet, consistent with the lowering of the local symmetry of the Pr site. This raises the question of what mechanism drives the structural distortion. The most obvious answer is that the electronic energy is reduced by a collective Jahn-Teller distortion at the expense of a small penalty in elastic energy. Another possibility is that the distortion is a consequence of a quadrupolar ordering of the Pr 4$`f`$ orbitals. Intuitively this would seem an unlikely mechanism, since the coupling between electric quadrupoles would be expected to be too weak to cause an orbital ordering at a temperature as high as 120 K. Nevertheless, there is evidence for a degree of Pr 4$`f`$—O 2$`p`$ hybridisation in PrO2, Karnatak et al. (1987); Bianconi et al. (1988) and such a covalency effect could provide a mechanism for aligning the 4$`f`$ orbitals.

The splitting of the ground state could also partly explain the observation of an ordered magnetic moment smaller than that associated with the $`\mathrm{\Gamma }_8`$ quartet ground state of cubic symmetry. On the other hand, we have previously reported a broad continuum of magnetic scattering in the excitation spectrum of PrO2, which we believe arises from a strong magnetoelastic coupling. Boothroyd et al. (2001) This coupling would tend to quench magnetic degrees of freedom and reduce the size of the ordered moment by the dynamic Jahn-Teller mechanism. From the experimental evidence available so far it seems likely that both the static and dynamic Jahn-Teller effects are important in PrO2, but it is not clear which of the two is dominant at low temperatures.

In work that we will report elsewhere, Gardiner et al. (2004) we have found that the application of a magnetic field in the distorted phase at $`T<T_\mathrm{D}`$ produces striking hysteresis effects in both the magnetic structure and the magnetisation. The totality of results that have emerged in recent years suggests that a strong interplay between electronic and lattice degrees of freedom exists in PrO2 and influences its properties, perhaps in unexpected ways.

###### Acknowledgements.

We would like to thank P. Santini for insightful discussions, and D. Prabhakaran and F. Wondre for help with sample preparation and characterisation. We would also like to thank J. Jensen for suggesting the chiral model for the distorted crystal structure and making many other helpful comments. We are also grateful to M. Enderle and K. Kiefer for advice on the design of the calorimeter. Financial support and provision of a studentship for CHG by the EPSRC is acknowledged.


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# Untitled Document

Light deflection by photonic crystals

Chao-Hsien Kuo and Zhen Ye

Wave Phenomena Laboratory, Department of Physics, National Central University, Chungli, Taiwan 320, Republic of China.

> When propagating through periodically structured media, i. e. photonic crystals, optical waves will be modulated with the periodicity. As a result, the dispersion of waves will no longer behave as in a free space, and so called frequency band structures appear. Under certain conditions, waves may be prohibited from propagation in certain or all directions, corresponding to partial and complete bandgaps respectively. Here we report a new fascinating phenomenon associated with the partial gaps, that is, deflection of optical waves. This phenomenon will render novel applications in manipulating light flows.

The band phenomenon was first investigated for electrons in solids. The well-known Bloch theorem has been proposed and led to successful explanation of some important properties of solids such as conducting, semi-conducting, and insulating states. Applying these concepts to electromagnetic waves started and flourished with the seminal papers published in 1987 Yab . Not only all the phenomena previously observed or discussed for electronic systems are successfully transplanted to classical systems, but many more significant and novel ideas, and applications have well gone beyond expectation, and are so far reaching that a fruitful new field called photonic crystals has come into existence, signified by the establishment of a comprehensive webpage web .

Photonic crystals (PCs) provide a new possibility in designing optoelectronic devices. Up to date, most applications have mainly relied on the existence of complete bandgaps. This includes, for example, cavity laser, optical fibers, and optical waveguides Opto . Here we demonstrate a new property of PCs, which is associated with partial bandgaps, referring to the situation in which waves are prohibited from propagation along certain directions.

We show that partial bandgaps can give rise to a fascinating phenomenon: deflection of optical waves. This phenomenon would allow for better optical steering, bending and beam collimating. It may also help explain some recent mysteries about the negative refraction or left-handed-material (LHM) behavior and the amphoteric refraction revealed by PCs PRB ; exp ; Chuang ; Zhang .

The systems considered here are two dimensional photonic crystals made of arrays of parallel dielectric cylinders placed in a uniform medium, which we assume to be air. Such systems are common in both theoretical simulations or experimental measurements of two dimensional PCsPRB ; McCall . For brevity, we only consider the E-polarized waves, that is, the electric field is kept parallel to the cylinders. The following parameters are used in the simulation. (1) The dielectric constant of the cylinders is 14, and the cylinders are arranged to form a square lattice. (2) The lattice constant is $`a`$ and the radius of the cylinders is 0.3$`a`$; in the computation, all lengths are scaled by the lattice constant. (3) The unit for frequency is $`2\pi c/a`$.

The band structure is plotted in Fig. 1, and the qualitative features are similar to that obtained for a square array of alumina rods in air. A complete band gap is shown between frequencies of 0.22 and 0.28. Just below the complete gap, there is a regime, sandwiched by two horizontal lines, of partial band gap in which waves are not allowed to travel along the $`\mathrm{\Gamma }X`$ or  direction.

We wish to examine the properties of the energy flow of the eigenmodes which correspond to the frequency bands shown in Fig. 1. Differing from the common approaches which mainly rely on the curvatures of frequency bands to infer the energy flow, we consider the genuine definition of the energy flow. By Bloch’s theorem, the eigenmodes corresponding to the frequency bands of PCs can be expressed as $`E_\stackrel{}{K}(\stackrel{}{r})=e^{i\stackrel{}{K}\stackrel{}{r}}u_\stackrel{}{K}(\stackrel{}{r})`$, where $`\stackrel{}{K}`$ is the Bloch vector, as the wave vector, and $`u_\stackrel{}{K}(\stackrel{}{r})`$ is a periodic function with the periodicity of the lattice. When expressing $`E_\stackrel{}{K}(\stackrel{}{r})`$ as $`|E_\stackrel{}{K}(\stackrel{}{r})|e^{i\theta _\stackrel{}{K}(\stackrel{}{r})}`$, the corresponding energy flow is derived as $`\stackrel{}{J}_\stackrel{}{K}(\stackrel{}{r})|E_\stackrel{}{K}(\stackrel{}{r})|^2\theta _\stackrel{}{K}(\stackrel{}{r})`$; clearly $`\theta _\stackrel{}{K}`$ combines the phase from the term $`e^{i\stackrel{}{K}\stackrel{}{r}}`$ and the phase from the function $`u_\stackrel{}{K}(\stackrel{}{r})`$, making the determination of the phase and group velocities in PCs less obvious, or even perhaps not so useful. To explore the characteristics of the partial bandgap, we have computed the eigen-field $`E_\stackrel{}{K}(\stackrel{}{r})`$ and also the energy flow of the eigenmodes. The results are shown in Fig. 2.

A significant discovery from Fig. 2 is that the energy flow of eigenmodes does not always follow the direction of the Bloch vectors. As evidenced by Fig. 2 (b2), the energy tends to flow into the direction of $`\mathrm{\Gamma }M`$, i. e the  direction, while the Bloch vector points to an angle of 22.5o that lies exactly between $`\mathrm{\Gamma }X`$ and $`\mathrm{\Gamma }M`$. This feature, however, cannot be inferred from the field pattern in (b1), i. e. the main wave front is more or less perpendicular to the direction of the Bloch vector rather than that of the energy flow, implying that it is not appropriate to determine the energy flow purely from the field pattern. For the other two Bloch vectors along $`\mathrm{\Gamma }X`$ and $`\mathrm{\Gamma }M`$ respectively, the net energy flows and the normals of the wave fronts follow the directions of the Bloch vectors, as shown by Figs. 2(a) and (c). From (a1), (b1) and (c1), we see that the eigenmodes have also periodic structures perpendicular to the direction of the propagation. The feature in (b2) can be explained in the context of partial bandgaps. In Fig. 2 (b), the frequency 0.185 lies within the partial bandgap in the $`\mathrm{\Gamma }X`$ direction. Since waves are not allowed to propagate along $`\mathrm{\Gamma }X`$ and the directions perpendicular to $`\mathrm{\Gamma }X`$, we may expect from the symmetry consideration that the energy flow will be tilted towards $`\mathrm{\Gamma }M`$ for waves whose Bloch vectors make an angle to $`\mathrm{\Gamma }X`$. Note here that in Fig. 2, the frequency corresponding to the Bloch vector along $`\mathrm{\Gamma }X`$ is outside the partial gap.

The deviation of the energy flow from the direction of the Bloch vector, serving as the wave vector, suggests an intriguing phenomenon, that is, the light deflection. Consider a plane wave propagation in a uniform medium. When it encounters an perpendicular interface of PCs with the normal of the interface being along the direction exactly between $`\mathrm{\Gamma }X`$ and $`\mathrm{\Gamma }M`$, what can be expected to happen? In the conventional thought, the wave would keep going straight, and the wave vectors on both sides of the interface will point to the same direction, as there are no components in the tangent direction. However, according to Fig. 2, the flow of the energy will be deflected into the direction of $`\mathrm{\Gamma }M`$. This is a surprising finding. To confirm this, we have carried out further simulations. For example, first, when we chose frequencies that lie outside the partial gap region, the deflection phenomenon disappears.

We have also studied the transmission properties. In Fig. 3, we plot the transmission of EM waves across two slabs of photonic crystals with two different lattice orientations: one is along the diagonal direction $`\mathrm{\Gamma }M`$, and the other is along the direction making an equal angle to the $`\mathrm{\Gamma }X`$ and $`\mathrm{\Gamma }M`$ directions. The incidence is normal to the slab interface. In the simulation, we have employed the standard multiple scattering method MST  to compute the transmitted intensity, which is usually the quantity to be measured in experiments. The frequencies chosen correspond to those in Fig. 2. We have used three types of sources in the simulations: (1) plane waves; (2) collimated waves by guiding the wave propagation through a window before incidence on the slabs; (3) a line source. The results from these three scenarios are similar. Here, we see that when the incidence is along the $`\mathrm{\Gamma }M`$ direction, the transmission follows a straight path inside the slab. For the second case in Fig. 3, the transmission direction inside the slab is deflected towards the $`\mathrm{\Gamma }M`$ direction. Fig. 3 clearly indicates that there are some favorable directions for waves to travel, fully in agreement with the above light deflection picture and in consistency with the results in Fig. 2. We also note that there is relatively small transmission along the \[1-1\] direction; by symmetry, this direction is also a probable passing path for the waves.

The light deflection in the presence of partial bandgaps can be important in a number of occasions. First, it may help designing novel optoelectronic devices in controlling optical flows. Compared to applications based on complete bandgaps, there is no reflection loss because the light deflection occurs in the passing bands, allowing for efficient wave transmission. Second, the mechanism of the light deflection discussed here may help understand the recent puzzles about the negative refraction PRB  or LHM behaviorChuang  and the amphoteric refraction revealed by PCs Zhang . To elaborate, we consider the slab shown in Fig. 3 (b). Assume that a plane wave is incident on the slab with a tilt angle. We can expect from the above results that as long as the tilt angle is not too large, the energy flow will be deflected towards the direction of $`\mathrm{\Gamma }M`$, no matter the incidence is positive or negative. Consequently, an amphoteric refraction may prevail and is conceptually illustrated by Fig. 4.

Correspondence and requests for materials should be addressed to Z.Y. (e-mail: zhen@shaw.ca).

Figure Captions

The band structure of a square lattice of dielectric cylinders. The lattice constant is $`a`$ and the radius of the cylinders is $`0.3a`$. $`\mathrm{\Gamma }M`$ and $`\mathrm{\Gamma }X`$ denote the  and  directions respectively. A partial gap is between the two horizontal lines.

Left panel: the field pattern of eigenmodes. Right panel: the energy flow of the eigenmodes. The eigenmodes along three directions are considered: (a) $`\stackrel{}{K}=(0.9\pi /a,0)`$, i. e. along $`\mathrm{\Gamma }X`$; the corresponding frequency is 0.175; (b) $`\stackrel{}{K}=(0.9\pi /a,0.37\pi /a)`$, i. e. along an angle of 22.5o exactly between $`\mathrm{\Gamma }X`$ and $`\mathrm{\Gamma }M`$ directions; the corresponding frequency is 0.185; (c) $`\stackrel{}{K}=(0.7\pi /a,0.7\pi /a)`$, i. e. along $`\mathrm{\Gamma }M`$; the corresponding frequency is 0.192. The direction of the Bloch vectors are denoted by the blue arrows, while the red arrows denote the local energy flow including the direction and the magnitude. The circles refer to the cylinders. Both frequencies in (b) and (c) lie within the partial gap. Due to the periodicity, we only plot the energy flow within one unit cell. Note that although the features shown by (b) also hold for other Bloch vectors for which the corresponding frequencies lie within the partial gap regime, we only plot here for the case of 22.5o

The imaging fields for slabs of photonic crystal structure. Two lattice orientations are considered: (a) The slab measures as about 56$`\times 10`$ and the incidence is along the  direction; (2) the slab measures as 50$`\times 13`$ and the incidence is along the direction that makes an equal angle to the  and  directions. The main lobes in the transmitted intensities are shown. There is a gap along the  direction.

Conceptual illustration of amphoteric refraction due to partial bandgaps, or perhaps better termed as amphoteric deflection. Depending on the incident angle, the deflection may not exactly follow the direction of $`[11]`$.