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# An effective spin-orbital Hamiltonian for the double perovskite Sr2FeWO6: Derivation of the phase diagram.

## I Introduction.

Transition metal oxides have been the subject of numerous experimental and theoretical studies after the discovery of a variety of novel physical phenomena and a diversity of ordered phases.imada  Their ground state can be insulating, metallic or superconducting, depending on temperature and stoichiometry and their magnetic structure varies from ferromagnetic (FM) to different antiferromagnetic (AFM) types. The insulating behavior is generally attributed to a large Coulomb interaction that localizes the $`d`$-electrons in Mott-Hubbard or charge-transfer regimes.imada  In this case low energy excitations can be described by the spin degrees of freedom through an effective superexchange model. Often, the ground state of the transition metal ion possesses an orbital degeneracy in addition to its that originating from the spin. In such cases, orbital degrees of freedom are also incorporated in the superexchange theory and the system is described by means of an effective spin-orbital model.kugel

The purpose of the present work is to formulate such a superexchange theory and derive a spin-orbital Hamiltonian for the antiferromagnetic insulator Sr2FeWO6. The experimental value of its Nèel temperature $`T_N`$ is quite low and reported in the literature as $`1637`$ K.blasse ; kawanaka ; kobayashi1  Sr2FeWO6 belongs to a family of double perovskite compounds with general formula A2BBO6. It has, however, electronic and magnetic properties which differ significantly from those of the other members of the family. For example, Sr2FeMoO6 and Sr2FeReO6, that have been the subject of the intense studies since the discovery of room temperature magnetoresistance in these compounds,kobayashi2  are half-metallic ferrimagnets with fairly high magnetic transition temperatures. kobayashi2  One of the reason why Sr2FeWO6 is so different from the other members of the group has been suggested by band structure analysis.fang  In this picture, the antibonding W(5d) states are pushed higher in energy by the stronger hybridization with oxygen $`p`$-orbitals.fang ; solovyev  (In the case of Re(5d) states this effect is compensated by the deeper $`5d`$-level of Re ion.) Because of this, 5d-electron prefer to move away from W site, leaving it in a W6+ ($`5d^0`$) configuration, and stay on the Fe $`3d`$-level even at the cost of paying an extra Coulomb energy. As a result, in Sr2FeWO6 iron is in a Fe2+ ($`3d^6`$) valence state,dass  and the moderately large Fe-W charge transfer gap, in the presence of strong Coulomb interaction on Fe sites, causes the insulating behavior.

In the perovskite structure, the octahedral ligand field of oxygens splits d-levels into a low-lying triplet ($`t_{2g}`$) and a higher doublet ($`e_g`$). There are several experimental evidenceskawanaka ; kobayashi1  suggesting that Fe2+ ion is in the high spin configuration $`t_{2g}^4e_g^2`$ with $`S=2`$. As four electrons occupy the threefold degenerate $`t_{2g}`$-levels, the ground state of Fe2+ has a threefold orbital degeneracy. This degeneracy, similarly to the spin one, can be described by pseudospin quantum numbers. The spin $`S=2`$ and pseudospin $`\tau =1`$ are thus the building blocks of an effective theory for insulating Sr2FeWO6. In the double perovskite structure of Sr2FeWO6 Fe and W ions form a rock-salt structure. Each type of ions resides on a face-centered-cubic (fcc) sublattice. The fcc lattice is weakly frustrated and allows ordered anisotropic AFM structures. But weak frustration of the lattice alone can not be responsible for the very low magnetic transition temperature. The reason why $`T_N`$ is low, we believe, is as follows. The superexchange interaction, that couples magnetic moments of Fe ions, is mediated by two types of diamagnetic ions, along the path Fe-O-W-O-Fe, with $`90^{}`$ and $`180^{}`$ angles between Fe and W ions. Because of this, the resulting Fe-Fe exchange is rather weak and the corresponding transition temperature is low. The nearest-neighbor (nn) and next-nearest-neighbor (nnn) Fe moments are coupled, respectively, by $`90^{}`$ and $`180^{}`$ Fe-W-Fe bonds. Depending on values and signs of the nn and nnn exchange energies, different types of AFM structures can be stabilized on the fcc lattice. To our knowledge no experimental determination of the kind of AFM order taking place in Sr2FeWO6 has ever been undertaken.

In this paper we derive an effective spin-orbital model from the Hubbard Hamiltonian of correlated Fe-3d electrons hybridized with uncorrelated 5d electrons of W and determine the magnetic ground-state structure as a function of the model parameters. We assume that oxygen degrees of freedom are integrated out and consider an effective hybridization between Fe and W $`d`$-states. Performing a fourth order perturbation expansion in the hopping parameters around the atomic limit we get an effective $`S=2`$ Hamiltonian for a system with six electrons in five $`d`$ orbitals. It may be worthwhile to note that our derivation is based only on the geometrical structure and electronic configuration of the system. As such it can be applied to a variety of systems presenting the same characteristics: any rock-salt with a high-spin $`t_{2g}^4e_g^2`$ configuration, like, e.g., FeO.

The paper is organized as follows: In the next section we introduce the multi-band Hubbard Hamiltonian, perform the fourth order perturbation expansion and write the effective spin-orbital Hamiltonian in which the orbital degrees of freedom are described in terms of the pseudospin representation. The derivation of the effective Hamiltonian demands a lot of algebra with rather cumbersome expressions. To facilitate the reader, we have tried to use, whenever possible, a pictorial representation of states and processes, relegating both the fourth order perturbation scheme and all the final expressions in the Appendices A and B, correspondingly. In section III the classical ground state phase diagram of the effective spin-orbital model is discussed, as a function of model parameters, within a variational procedure. In the same section we also discuss the range of the external parameters appropriate to the case of Sr2FeWO6 and sketch some results. In section IV we draw our conclusions.

## II Effective Hamiltonian.

Here we introduce the five-band Hubbard Hamiltonian, and perform a perturbative expansion in the hopping parameters up to the fourth order to describe all the low-lying excited states of the Fe-W system in terms of spin and orbital degrees of freedom of iron sites, only.

### II.1 Ground state.

We start from the multi-band Hubbard Hamiltonian:

$$H=H_0+H_{\text{cf}}+H_{0W}+H_t^{},$$
(1)
where $`H_0`$ is the on-site term of the form:

$`H_0`$ $`=`$ $`U_1{\displaystyle \underset{i,\alpha }{}}n_{i\alpha }n_{i\alpha }+{\displaystyle \frac{1}{2}}(U_2J){\displaystyle \underset{i,\sigma ,\alpha \alpha ^{}}{}}n_{i\alpha \sigma }n_{i\alpha ^{}\sigma }`$ (2)
$`+`$ $`U_2{\displaystyle \underset{i,\alpha \alpha ^{}}{}}n_{i\alpha }n_{i\alpha ^{}}+J{\displaystyle \underset{i,\alpha \alpha ^{}}{}}d_{i\alpha }^+d_{i\alpha }^+d_{i\alpha ^{}}d_{i\alpha ^{}}`$
$``$ $`J{\displaystyle \underset{i,\alpha \alpha ^{}}{}}d_{i\alpha }^+d_{i\alpha }d_{i\alpha ^{}}^+d_{i\alpha ^{}},`$
$`U_1`$ and $`U_2`$ are the Coulomb repulsion among electrons in the same and in different orbitals, respectively, and $`J`$ is the Hund’s coupling constant. Due to the cubic symmetry, the relation $`U_1=U_2+2J`$ holds. The annihilation and creation operators, $`d_{i\sigma \alpha }`$ and $`d_{i\sigma \alpha }^{}`$ refer to Fe-3d orbitals at site $`i`$, of type $`\alpha `$ (one of $`x^2y^2`$, $`3z^2r^2`$, $`xy`$, $`xz`$ or $`yz`$) and with spin $`\sigma =,`$, $`n_{i\alpha \sigma }=d_{i\sigma \alpha }^{}d_{i\sigma \alpha }`$.

The octahedral crystal field splitting of d-orbitals into a $`e_g`$-doublet ($`x^2y^2`$ and $`3z^2r^2`$) and a lower-lying $`t_{2g}`$ triplet ($`xy`$, $`xz`$ and $`yz`$) is taken into account for both Fe and W ions by the term:cf

$$H_{cf}=\mathrm{\Delta }_{e_g}\underset{ii^{},\alpha =x^2y^2,3z^2r^2}{}(n_{i\alpha \sigma }+\stackrel{~}{n}_{i^{}\alpha \sigma })$$
(3)
where $`\stackrel{~}{n}_{i^{}\alpha \sigma }`$ counts the electrons on W sites $`i^{}`$. The summation is for all $`i`$ and $`i^{}`$ running over Fe and W sublattices, respectively. Finally, the last term of the local part of the Hamiltonian, $`H_{0W}`$, represents the single particle energy level of the W ion with respect to Fe(6):

$$H_{0W}=\mathrm{\Delta }_{\text{CT}}\underset{i^{}\alpha \sigma }{}\stackrel{~}{n}_{i^{}\alpha \sigma },$$
(4)
where $`\mathrm{\Delta }_{\text{CT}}=E(\text{Fe}^{(5)}\text{W}^{(1)})E(\text{Fe}^{(6)}\text{W}^{(0)})`$ is the charge transfer energy, i.e., the minimum energy needed to remove one electron from Fe(6) ion and put it to an empty W(0) site. Here and below an upper index denotes the number of $`d`$-electrons on a given ion. The kinetic term $`H_t^{}`$ is considered as a perturbation:

$`H_t^{}`$ $`=`$ $`{\displaystyle \underset{ii^{}\sigma \alpha \beta }{}}t_{\alpha \beta }(d_{i\sigma \alpha }^{}\stackrel{~}{d}_{i^{}\sigma \beta }+h.c.)`$ (5)
The summation is over nearest-neighbor Fe-W sites, and all possible spin and orbital indices. Here $`\stackrel{~}{d}_{i^{}\sigma \alpha }^{}`$ ($`\stackrel{~}{d}_{i^{}\sigma \alpha }`$) creates (annihilates) a 5d-electron on W ions, with spin $`\sigma `$ in the orbital $`\alpha `$. In a cubic lattice there is no hopping between $`e_g`$ and $`t_{2g}`$. The transfer matrix $`t_{\alpha \beta }`$ is diagonal in the $`t_{2g}`$ manifold for all the orbitals $`xy`$, $`xz`$, $`yz`$, with non-zero matrix elements $`t`$ only for the bonds laying in the corresponding plane (i.e., along $`x`$ direction, the hopping integral is zero for $`yz`$ orbitals and equal to $`t`$ for the other two). Due to the shape of the $`e_g`$ orbitals, their hybridization is different in the three cubic directions thus leading to direction dependent hopping with the anisotropic transfer matrix elements $`t_{\alpha \beta }`$ ($`\alpha =3z^2r^2`$ and $`\beta =x^2y^2`$) given by:

$`t_{\alpha \beta }^{x,y}=t_e(\begin{array}{cc}1/4& \sqrt{3}/4\\ \sqrt{3}/4& 3/4\end{array}),t_{\alpha \beta }^z=t_e(\begin{array}{cc}1& \mathrm{\hspace{0.33em}\hspace{0.33em}0}\\ 0& \mathrm{\hspace{0.33em}\hspace{0.33em}0}\end{array})`$ (10)
In constructing the effective Hamiltonian we also assume that the Hund’s coupling $`J`$ is strong enough to win the competition with the crystal field splitting $`\mathrm{\Delta }_{e_g}`$. This implies that Fe2+-ion in the ground state is in the high-spin configuration $`t_{2g}^4e_g^2`$ with total spin $`S=2`$, and justifies the exclusion from our zeroth order of the low-spin state, $`t_{2g}^6e_g^0`$ ($`S=0`$) and of the intermediate-spin state, $`t_{2g}^5e_g^1`$ ($`S=1`$), both higher in energy. We can write the ground state as a collection of atomic states $`|\alpha _j`$, each characterized by two quantum numbers: the spin $`\stackrel{}{S}`$ and pseudospin $`\stackrel{}{\tau }`$. This latter describes the orbital occupation, namely the position of double occupied orbital in the $`t_{2g}`$-manifold. Since there are three possibilities to put the double occupied orbital in the manifold, we can describe it by $`\stackrel{}{\tau }=1`$, with the same algebra of the usual spin operator. The orbital quantization axis can be selected arbitrarily, and we choose the following convention which pictorially can be presented as:

In this notation, the upper boxes represent the $`e_g`$ orbital doublet, $`e_g^{(1)}=3z^2r^2`$ (left upper box) and $`e_g^{(2)}=x^2y^2`$ (right upper box). The lower boxes refer to the three-fold degenerate $`t_{2g}`$ orbitals. with $`t_{2g}^{(1)}=xy`$ (left box), $`t_{2g}^{(2)}=yz`$ (central box) and $`t_{2g}^{(3)}=xz`$ (right box). The atomic ground state energy is $`E_g^{(6)}=15U_28J+2\mathrm{\Delta }_{e_g}`$. Because of the three-fold orbital and the five-fold spin degeneracies, the ground state is 15-fold degenerate. Such a degeneracy is then lifted by the hopping term, $`H_t^{}`$, as detailed below.

### II.2 Excited states and perturbation theory.

In this subsection we briefly describe the perturbation scheme and classify the excited states according to their total spin $`S`$, their $`S_z`$ projection and orbital configurations. Since we are interested in describing the superexchange interactions between iron sites, we need to go beyond second order perturbation theory in the hopping Hamiltonian $`H_t^{}`$ and deal with fourth-order perturbative expansion. In fact, we neglect the direct Fe-Fe hopping and consider only the hopping through the W sites. The explicit form of $`H_t^{}`$ is such that the fourth order eigenvalue equation simplifies to (see Appendix A):

$`\left|{\displaystyle \underset{mln}{}}{\displaystyle \frac{\alpha |H_t^{}|\beta _m\beta _m|H_t^{}|\beta _l\beta _l|H_t^{}|\beta _n\beta _n|H_t^{}|\alpha ^{}}{(E_\alpha E_{\beta _m})(E_\alpha E_{\beta _l})(E_\alpha E_{\beta _n})}}E\right|=0`$ (11)
where $`|\alpha `$ and $`|\alpha ^{}`$ are two possible ground-states for $`H_0`$ (all the Fe2+-ions in the $`t_{2g}^4e_g^2`$ configuration, all 5d W-orbitals empty), while $`|\beta _{m(l,n)}`$ denotes all possible intermediate excited states, as imposed by $`H_t^{}`$. The first and third step states, $`|\beta _{m(n)}`$, must have five electrons on one Fe-ion and one electron in an adjacent W-ion ($`\mathrm{Fe}^{(5)}\mathrm{W}^{(1)}`$), while the second-step state, $`|\beta _l`$, must be of the kind $`\mathrm{Fe}^{(5)}\mathrm{W}^{(0)}\mathrm{Fe}^{(7)}`$ or $`\mathrm{Fe}^{(5)}\mathrm{W}^{(2)}\mathrm{Fe}^{(5)}`$ on the three sites involved in the hopping process (see Fig. 1). Our aim is to find out a representation of the effective Hamiltonian, leading to this same eigenvalue equation, in terms of the spin and orbital degrees of freedom of iron only. We consider the full multiplet structure of the intermediate states with five and seven electrons which can be grouped according to their energies and the total value of the spin. Moreover, depending on the orbital occupation of Fe(6) ion in the ground state and the orbital symmetry ($`e_g`$ or $`t_{2g}`$) of the hopping electron, different intermediate configurations can be reached. As already stated, in the cubic symmetry the hopping is allowed only within $`t_{2g}`$-manifold and $`e_g`$-manifold, separately.

Consider the excited states which involve $`t_{2g}`$ hopping, first. The intermediate atomic states with seven electrons Fe$`{}_{t}{}^{}{}_{}{}^{(7)}`$ have total spin $`S=3/2`$. The manifold is 12-fold degenerate (4(spin)$`\times `$3(orbital)) and one of the possible states can be depicted as:

The three-fold orbital degeneracy arises from the $`t_{2g}`$ unpaired electron. The energy of this state is $`E_t^{(7)}=21U_27J+2\mathrm{\Delta }`$.

The intermediate states with five electrons split over a manifold with different values of total spin and energies.

The excited states with maximum spin configuration have $`S=5/2`$ and no orbital degeneracy. The 6-fold degeneracy is entirely due to the spin. The state with maximum $`S_z`$ is:

The energy is $`E_a^{(5)}=10U_210J+2\mathrm{\Delta }`$, the minimum excitation energy of $`\text{Fe}^{(5)}`$ states.

All the other $`\text{Fe}^{(5)}`$ states with all orbitals singly occupied have total spin $`S=3/2`$ and can be pictured as:

Each of these states is 4-fold degenerate because of the spin (only the states with maximum $`S_z`$ are shown). They give the same contribution to the effective Hamiltonian and below, for convenience, we denote them with the common notation $`\text{Fe}_b^{(5)}`$. Their energy is $`E_b^{(5)}=10U_25J+2\mathrm{\Delta }`$.

Finally, there are the states with one unoccupied orbital. They have total spin $`S=3/2`$ and the global degeneracy is 24 (4(spin)$`\times `$6(orbital)).

The energies of these states are $`E_{c_+}^{(5)}=10U_25J+2\mathrm{\Delta }`$ and $`E_c_{}^{(5)}=10U_23J+2\mathrm{\Delta }`$.

Now we consider the intermediate states which can be reached by $`e_g`$ hopping. Those with seven electrons have spin $`S=3/2`$ and can be presented as the following :

Their degeneracy is 4(spin)$`\times `$3(orbital $`t_{2g}`$)$`\times `$2(orbital $`e_g`$)=24. Their energy is: $`E_e^{(7)}=21U_27J+3\mathrm{\Delta }`$.

The states with five electrons arising from the $`e_g`$ hopping have also total spin $`S=3/2`$ and can be drawn as

where the normalization factors are defined as $`N_\pm =\frac{J^2+\mathrm{\Delta }_\pm ^2}{\mathrm{\Delta }_\pm ^2}`$, $`\alpha =\frac{1}{\sqrt{2}}\sqrt{1+\frac{\mathrm{\Delta }}{\sqrt{J^2+\mathrm{\Delta }^2}}}`$, and $`\mathrm{\Delta }_\pm =\mathrm{\Delta }\pm \sqrt{J^2+\mathrm{\Delta }^2}`$. These states have energy $`E_{d_\pm }^{(5)}=10U_24J+2\mathrm{\Delta }\sqrt{J^2+\mathrm{\Delta }^2}`$ and their degeneracy is 4(spin)$`\times `$3(position of doubly occupied orbital)$`\times `$2(position of hole)=24.

### II.3 Classification of virtual processes and derivation of the spin-orbital Hamiltonian.

In order to derive the effective spin-orbital Hamiltonian in the simplest way it is useful to classify all the allowed hopping processes depending on the specific geometry of the fcc lattice. It becomes then possible to select the orbital dependence for each process and for a given projection of the spin coupling (whether FM or AFM) along the direction $`ij`$ of the bond. The general form for the Hamiltonian turns out to be:

$`H_{\mathrm{eff}}={\displaystyle \underset{ij}{}}\left[\stackrel{}{S}_i\stackrel{}{S}_j+6\right]O_{ij}^{(F)}+\left[\stackrel{}{S}_i\stackrel{}{S}_j4\right]O_{ij}^{(A)}`$ (12)
where $`ij`$ denote the summation over both nn and nnn Fe-ions of the fcc lattice. The terms $`O_{ij}^{(F(A))}`$ are the orbital, energy-dependent, contributions to the effective Hamiltonian for FM or AFM bonds $`ij`$, respectively, which are explicitly given in Appendix B. The two spin-dependent terms are projectors over $`\stackrel{}{S}_i+\stackrel{}{S}_j=4`$ (FM coupling) and $`\stackrel{}{S}_i+\stackrel{}{S}_j=0`$ (AFM coupling), respectively. Below we clarify the procedure adopted to derive the spin-orbital Hamiltonian (12). We try to avoid as much as possible formulas and present the derivation in a pictorial way. Following Fig. 1 we consider four types of processes (from $`A`$ to $`D`$), according to the way the intermediate states can be reached.

Depending on the kind and number of ions involved in the intermediate steps, it is possible to distinguish the following processes:

$`A\text{processes}:`$
$`\mathrm{Fe}^{(6)}\mathrm{W}^{(0)}\mathrm{Fe}^{(6)}\mathrm{Fe}^{(5)}\mathrm{W}^{(1)}\mathrm{Fe}^{(6)}\mathrm{Fe}^{(5)}\mathrm{W}^{(0)}\mathrm{Fe}^{(7)}`$
$`\mathrm{Fe}^{(5)}\mathrm{W}^{(1)}\mathrm{Fe}^{(6)}\mathrm{Fe}^{(6)}\mathrm{W}^{(0)}\mathrm{Fe}^{(6)}`$
$`B/C\text{processes}:`$
$`\mathrm{Fe}^{(6)}\mathrm{W}^{(0)}\mathrm{Fe}^{(6)}\mathrm{Fe}^{(5)}\mathrm{W}^{(1)}\mathrm{Fe}^{(6)}\mathrm{Fe}^{(5)}\mathrm{W}^{(2)}\mathrm{Fe}^{(5)}`$
$`\mathrm{Fe}^{(5)}\mathrm{W}^{(1)}\mathrm{Fe}^{(6)}\mathrm{Fe}^{(6)}\mathrm{W}^{(0)}\mathrm{Fe}^{(6)}`$
$`D\text{processes}:`$
$`\mathrm{Fe}^{(6)}\mathrm{W}^{(0)}\mathrm{W}^{(0)}\mathrm{Fe}^{(6)}\mathrm{Fe}^{(5)}\mathrm{W}^{(1)}\mathrm{W}^{(0)}\mathrm{Fe}^{(6)}`$
$`\mathrm{Fe}^{(5)}\mathrm{W}^{(1)}\mathrm{W}^{(1)}\mathrm{Fe}^{(5)}\mathrm{Fe}^{(6)}\mathrm{W}^{(0)}\mathrm{W}^{(1)}\mathrm{Fe}^{(5)}`$
$`\mathrm{Fe}^{(6)}\mathrm{W}^{(0)}\mathrm{W}^{(0)}\mathrm{Fe}^{(6)}`$
where the upper index denotes the number of electrons on each ion. A first basic distinction is easily drawn between the $`A`$-process and all the others. The former involve the formation of a Fe(7) state at the second step, while none of the latter type processes does.

On the contrary, all $`B`$-, $`C`$\- and $`D`$-processes are characterized by a Fe(5) state for both iron ions involved in a virtual process. The difference among them lies in the way these states are reached. For $`B`$\- and $`C`$-processes there is only one intermediate W ion with two electrons on it, differently from the the $`D`$-process, where two distinct W ions are involved. Finally, the difference between $`B`$\- and $`C`$-processes lies in the behavior of the two virtual electrons. In the first case they go back to the original Fe-ion where they came from. On the contrary for C-processes there is an exchange of the two electrons, as shown in Fig. 1, and each of them moves toward the other Fe ion. For the sake of clarity it should be reminded that we are considering the specific case of the fcc sublattice of Fe ions in Sr2FeWO6: this allows some simplifications in the derivation of the effective spin-orbital Hamiltonian, $`H_{\text{eff}}`$. In particular, it is possible to build the following table, where we list the contributions to $`H_{\text{eff}}`$ depending on the characteristics of each single term.
$`A`$ $`B`$ $`C`$ $`D`$    $`aa`$ FM AFM (T1) FM (T2,nnn) FM (T1,nn)  $`bb`$ AFM AFM (T1) FM (T2,nnn) FM (T1,nn)  $`cc`$ AFM AFM (T1) FM (T2,nnn) FM (T1,nn)  $`dd`$ AFM AFM (T1) FM (T2,nnn) FM (T1,nn)  $`ac`$  FM (T1) AFM (T2,nnn) AFM (T1,nn)  $`bc`$  AFM (T1) FM (T2,nnn) FM (T1,nn)  $`ab`$  FM (T1) AFM (T2,nnn) AFM (T1,nn)
Each column in the table represents one of the four possible processes drawn in Fig. 1. Each row represents the states of the Fe(5)-ion reached at the second step of the virtual process. For example, for $`B`$-, $`C`$\- and $`D`$-processes, $`aa`$ means that the virtual intermediate state is made of both Fe$`{}_{a}{}^{}{}_{}{}^{(5)}`$, while $`ac`$ indicates one Fe$`{}_{a}{}^{}{}_{}{}^{(5)}`$-state and one Fe$`{}_{c\pm }{}^{}{}_{}{}^{(5)}`$-state. In the case of the A process, only one Fe(5)-state is present and “$`aa`$” refers to this single Fe$`{}_{a}{}^{}{}_{}{}^{(5)}`$-state, while $`ac`$ has no meaning. The table gives us the magnetic character of the bond $`ij`$ involved in the process (whether FM or AFM), if it requires a nn or a nnn contribution, and its orbital signature. In this respect T$`1`$ means that only one type of orbital is allowed in the process (ie, a contribution proportional to $`t_{xy}^4`$), while T$`2`$ means that there must be two different orbitals (for example a contribution proportional to $`t_{xy}^2t_{xz}^2`$). If there are no orbital or neighbors specifications, it means that both kinds are allowed. With this in mind, the derivation of the orbital part reported in Appendix B follows quite straightforward.

As an example, we show how to derive the term (B) (see Appendix B), corresponding to the A-process towards states $`c_\pm `$. In order to have a state $`c_\pm `$ on a Fe(5)-ion, the electron that jumps to the W-site and then forms the Fe$`{}_{t}{}^{}{}_{}{}^{(7)}`$ state, must belong to one of the singly occupied t2g-states of the original Fe(6)-ion. Only in this case, in fact, the Fe(5)-ion is left with one doubly occupied, one singly occupied and one vacant $`t_{2g}`$-state. The electron is free to jump on W site, that is empty, and it has some restriction to hop to the next Fe(6) ion, because of the Pauli principle. Only some jumps are allowed and they do depend on the relative orbital occupations of the two Fe(6)-ions involved in the process. It is worthwhile to note that, if the spins of the two Fe(6)-ions involved were ferromagnetically coupled, no hopping processes could have taken place because of the Pauli principle: the hopping electron would find all the singly occupied orbitals of the final Fe(6)-ion filled with the same spin projection. Thus, superexchange between c± states can take place only when the two Fe(6) ions are coupled antiferromagnetically, as shown in the previous table.

Let us now analyze the orbital dependence. For simplicity we consider two specific configurations, of those that we called T1 and T2 in the table, e.g., the term depending on t$`{}_{}{}^{4}{}_{xy}{}^{}`$ and that depending on t$`{}_{}{}^{2}{}_{xy}{}^{}`$t$`{}_{}{}^{2}{}_{xz}{}^{}`$. The first hopping process is allowed only when $`\tau _{iz}1`$ and $`\tau _{jz}1`$, i.e. $`xy`$-orbital states are singly occupied at both $`i`$ and $`j`$ Fe-sites involved. The second is active only when both $`\tau _{iz}`$ and $`\tau _{jz}`$ are either 1 or -1, i.e. either $`xy`$\- or $`xz`$-orbital states are doubly occupied at both sites. During this process both orbital quantum numbers are either reduced or increased by two, respectively. In the case of a doubly occupied $`xy`$-orbital, the $`xz`$-electron hops leaving a hole in this orbital state. The resulting state is not an eigenstate of the Hamiltonian (2) and is then projected over an eigenstate $`c_\pm `$ given by the superposition of states with $`xy`$\- and $`xz`$-holes. Therefore, an electron from the doubly occupied $`xy`$-orbital of Fe(7) can hop back to Fe(5) ion. This changes the initial orbital configuration $`\tau _{iz}=\tau _{jz}=1`$ to the final $`\tau _{iz}=\tau _{jz}=1`$ form. In terms of the pseudospin quantum numbers, the two contributions are:

$`t_{xy}^4\left[(1\tau _{iz}^2)+{\displaystyle \frac{1}{2}}\tau _{iz}(\tau _{iz}1)\right]\left[(1\tau _{jz}^2)+{\displaystyle \frac{1}{2}}\tau _{jz}(\tau _{jz}1)\right]`$
$`\pm {\displaystyle \frac{1}{4}}t_{xy}^2t_{xz}^2\left[\tau _i^+\tau _i^+\tau _j^+\tau _j^++\tau _i^{}\tau _i^{}\tau _j^{}\tau _j^{}\right],`$
where $`\pm `$ depends on which of the c± states are considered. These terms enter into Eq. (11) with a weight taking into account both spin (through Clebsch-Gordan coefficients) and orbital projection of the single Slater determinant into the correlated state c±. The weight, or normalization coefficient (see the Table in Appendix B), of a given process is obtained by equating the matrix elements of the Hamiltonian (12) to the corresponding ones obtained directly using the perturbation theory (11). To calculate the weight of the proccess under consideration, for simplicity, we conider diagonal matrix elements of $`H_{\text{eff}}`$ in the spin subspace over the bond configuration $`S_i^z=2`$ and $`S_j^z=2`$. The $`SU(2)`$ spin symmetry of the problem guarantees that consideration of the nondiagonal matrix elements in the spin subspace, i. e. processes that involve spin flips, will lead to the same result. For the present process this weight is $`\gamma _A^{cc}=\frac{1}{16}=\frac{1}{8}\left(\frac{1}{\sqrt{2}}\right)^2`$, where the factor $`1/8`$ normalizes $`|\stackrel{}{S}_i\stackrel{}{S}_j4|=8`$ for the bond we consider and the remaining $`\left(\frac{1}{\sqrt{2}}\right)^2`$ is due to the projection of the single Slater determinant into the states c±. The square power is due to the fact that the virtual state, not eigen-state of the local Hamiltonian, is projected twice into the corresponding eigenstate in Eq. (11).

All the other contributions, detailed in Appendix B, have been found in a similar way.

## III Ground state phase diagram.

In this section we discuss the classical ground state phase diagram of the spin-orbital model, Eq. (12). We factorize spin and orbital degrees of freedom and perform a mean-filed type analysis of the possible ordered phases. The factorization is justified because of the two different energy scales governing these degrees of freedom: spins are coupled by virtual processes that involve both $`e_g`$ and $`t_{2g}`$ electron transfers, while only the latter electrons generate the coupling between the orbital degrees of freedom, as $`e_g`$ orbitals are half-filled. The ratio of spin and orbital exchange energies thus scales approximately as $`t_e^4/t^4`$ and is much larger than unity in the situation of interest. Therefore, it is reasonable to average out spin degrees of freedom, first, by considering all possible ordered magnetic structures on a fcc centered cubic lattice and then for each type of magnetic ordering find an orbital configuration, that minimizes the total energy by means of a variational procedure.

We consider the following magnetic structures that are possible ordered states for a nn and a nnn Heisenberg Hamiltonian on a fcc latticesmart :

i) Ferromagnetic state (FM);

ii) Type-I antiferromagnetic (AFM-I) ordering, which consists of ferromagnetic {110} planes stacked antiferromagnetically in the third direction;

iii) Type-II antiferromagnetic (AFM-II) structure, consisting of ferromagnetic {111} planes, each being antiferromagnetically coupled to adjacent layers. This magnetic structure is presented in Fig. 2, where only the Fe atoms are shown.

### III.1 Minimization procedure.

The trial wave function can be written in general as follows:

$$|\mathrm{\Psi }=\mathrm{\Pi }_i|\mathrm{\Psi }_i=\mathrm{\Pi }_i|\psi _i^o|\varphi _i^s$$
(13)
where $`|\psi _i^o`$ and $`|\varphi _i^s`$ refer to orbital and spin states at site $`i`$ , respectively. Since $`H_{\mathrm{eff}}`$ factors into an orbital $`H_{\mathrm{eff}}^o`$ and a spin $`H_{\mathrm{eff}}^s`$ part and its action involves two sites at a time, its average value over the above state takes the form:

$`\begin{array}{c}\mathrm{\Psi }_i|\mathrm{\Psi }_j|H_{\mathrm{eff}}|\mathrm{\Psi }_j|\mathrm{\Psi }_i=\\ \psi _i^o|\psi _j^o|H_{\mathrm{eff}}^o|\psi _j^o|\psi _i^o\times \varphi _i^s|\varphi _j^s|H_{\mathrm{eff}}^s|\varphi _j^s|\varphi _i^s\end{array}`$ (16)
The orbital part of the variational wave function can be written as

$`\psi _i^o=\mathrm{cos}\theta _i|0_i+\mathrm{sin}\theta _i(\mathrm{cos}\psi _i|1_i+\mathrm{sin}\psi _i|1_i).`$ (17)
allowing all three orbital states $`|\tau _z=0_i`$, $`|\tau _z=1_i`$ and $`|\tau _z=1_i`$ with a relative weight determined by the minimization procedure with respect to the variational parameters $`\theta _i`$ and $`\psi _i`$. The expectation values of $`H_{\mathrm{eff}}^o`$ over the trial orbital wave function for both ferromagnetic and antiferromagnetic bonds are then expressed in terms of variational parameters $`\theta _i`$ and $`\psi _i`$ and are quite lengthy. On the contrary, the average of spin variables is straightforward in a mean field treatment. For a ferromagnetic bond $`\stackrel{}{S}_i\stackrel{}{S}_j+6=10`$ and for an antiferromagnetic bond $`\stackrel{}{S}_i\stackrel{}{S}_j4=8`$ in the classical ground state.

The energy per Fe atom, $`E^{\text{Fe}}`$, is given by the sum of the energy contributions from all the bonds contained in the cell, divided by the number of atoms (each Fe-ion has 12 nn and 6 nnn). AFM-II phase has the biggest cell, with eight Fe atoms (see Fig. 2), and for generality we consider it as the unit cell for both FM and AFM-I phases, too. Hence, we have sixteen variational parameters ($`\theta _{18}`$ and $`\psi _{18}`$ for the eight sites of the unit cell). We have then performed a numerical minimization of the ground state energy with respect to all the sixteen independent angular variational angles $`\theta _i`$ and $`\psi _i`$. By taking the absolute minimum we determine the orbital configuration that minimizes the total energy of the system for a given magnetic order. The ground state magnetic and orbital structure are determined by selecting the state with the lowest energy. The results are presented below.

### III.2 Model parameters

In order to proceed further with the ground state phase diagram of $`H_{\text{eff}}`$, we fix below the values of the parameters that have already been estimated in the literature and we try to give a reasonable guess for the remainings.

* Crystal field splitting $`\mathrm{\Delta }_{e_g}`$: The value of the $`e_g`$$`t_{2g}`$ splitting $`\mathrm{\Delta }_{e_g}1.24`$ eV has been estimated for Fe2+ ion in Ref. anderson,  and we take this value in our analysis.
* Exchange parameter $`J`$: The exchange part of Coulomb energy is known to be little screened in solids. It can thus be estimated trough the atomic values of Racah parameters B and C ($`J=5/2B+C`$). Given the values of $`B`$ and $`C`$ from Ref. bocquet, , one obtains $`J0.78`$ eV.
* Coulomb energy $`U_2`$: Intra-atomic Coulomb repulsion is generally considerably screened in solids and can not be simply related to its atomic value. The estimates reported in the literature suggest that $`U_2=57`$ eV (Refs. anderson, ; bocquet, ; takahashi, ), however we also consider variation of $`U_2`$ in a wider range.
* Transfer integrals $`t`$ and $`t_e`$: We fix, in most of the cases, the ratio of $`e_g`$ and $`t_{2g}`$ transfer integrals to be $`t_e/t=3`$ as suggested by the Muffin-Tin Orbital theory.harrison  We are not aware of any estimates of absolute values of the transfer integrals between Fe and W ions. However $`t_{2g}`$ hopping amplitude has been estimated to be $`t0.25`$ eV for Fe-Re bond.millis  We may consider the same value of $`t_{2g}`$ transfer for Fe-W bond too, since for both Re and W ions this transfer involves $`5d`$-shell.
* Charge-transfer gap $`\mathrm{\Delta }_{\text{CT}}`$: We can estimate a lower boundary for the charge transfer gap between the high spin state of Fe(6) and W ions in two possible ways as follows. First, the difference in $`\mathrm{\Delta }_{\text{CT}}`$ for Re and W based systems can be approximately taken equal to the energy mismatch of $`5d`$-levels of these ions: $`\mathrm{\Delta }_{\text{CT}}(\text{W})\mathrm{\Delta }_{\text{CT}}(\text{Re})=E^{(5d)}(\text{W})E^{(5d)}(\text{Re})`$. The latter mismatch is of the order of $`1.4`$ eV.harrison  A lower estimate of $`\mathrm{\Delta }_{\text{CT}}(\text{W})`$ is then obtained by putting $`\mathrm{\Delta }_{\text{CT}}(\text{Re})=0`$ for the metallic Re based compound. We get $`\mathrm{\Delta }_{\text{CT}}>1.4`$ eV for the W based compound. Second, the insulating behavior of the system implies that the charge-transfer gap is larger than the bandwidth of those electrons that are involved in the lowest energy charge-transfer.zaanen ; aligia  Taking the above reported value for $`t_{2g}`$ transfer one obtains the even more strict constraint $`\mathrm{\Delta }_{\text{CT}}>2`$ eV.

### III.3 Results and discussion

In Fig. 3 we show the ground state phase diagram of the spin-orbital model (12) in $`\mathrm{\Delta }_{\text{CT}}U_2`$ plane. We fix the other parameters as discussed above and take $`t_e/t=3`$. Because of this ratio, $`e_g`$ superexchange, which is antiferromagnetic, overwhelms the superexchange due to the $`t_{2g}`$ hopping. Therefore the ground state is always antiferromagnetic and it turns out to be of type-II.

Given this magnetic structure, orbitals order in such a way to further reduce the ground state energy. The type of orbital ordering depends on whether $`2\mathrm{\Delta }_{\text{CT}}U_2`$ (orbital ordering of type-II, OO-II) or $`2\mathrm{\Delta }_{\text{CT}}U_2`$ (orbital ordering of type-I, OO-I). In the former case virtual processes with singly occupied W-states (A-processes) become dominant. Instead in the latter case it is energetically more favorable to create doubly occupied W states rather than to pay a Coulomb energy at Fe sites (B-, C-, D-processes). In Table 1 we list the types of orbital orderings together with the corresponding structure. The numbers from 1 to 8 label the eight atoms of the unit cell shown in Fig. 2. The ket-vectors denote the type of doubly occupied $`t_{2g}`$ orbital at each atom for each orbital ordering.

To understand the orbital structure of the AFM-II state it is convenient to divide the fcc lattice of Fe ions, in four simple cubic sublattices. These four sublattices are generated by the pairs of nonequivalent atoms of the unit cell: (1,5), (2,6), (3,7), and (4,8) (see Fig. 2). Each sublattice is AFM and the moments are coupled only by nnn exchange, while the coupling between sublattices is due to the nn exchange. If we denote by $`J_1`$ and $`J_2`$ the nn and nnn exchange constants of Fe spins, respectively, and consider only spin degrees of freedom, then the ground state energy in the AFM-II phase depends only on $`J_2`$, because there is an equal number of nn ferro- and antiferro-bonds. Therefore the contributions from $`J_1`$ to the ground state energy are canceled out. However, in the present case, due to the orbital part of the effective Hamiltonian (12), inter-sublattice couplings (i.e. nn spin-orbital couplings) also contribute to the ground state energy. The antiferromagnetic superexchange for a given sublattice is maximized when $`t_{2g}`$ orbitals are ordered ferromagnetically and all equally populated. Switching on the inter-sublattice coupling does not affect the ferromagnetic-type orbital order within each sublattices. However, the type of occupied orbital state changes, in order to minimize the contribution of nn energy to the ground state. As a result, there are two types of orbitally ordered ground states (OO-I and OO-II), depending on the parameters (see Fig. 3). The structure of these orbital states is explicitly given in Table 1.

We have also evaluated $`J_1`$ and $`J_2`$ averaged over the bond directions. The transition temperature $`T_N`$ can be directly linked to the nnn exchange energy $`J_2`$ by the formula: $`T_N=2S(S+1)zJ_2/3`$ where $`z=6`$ is a number of next-nearest neighbors. For $`S=2`$ and the experimental values of $`T_N1637`$ K one obtains $`J_20.060.15`$ meV. Fixing $`t_e/t=3`$, $`U_2=5`$ eV and varying $`\mathrm{\Delta }_{\text{CT}}`$ in the range $`27`$ eV we obtain the following range of $`J_2`$: $`J_2=0.030.14`$ meV for $`t=0.20`$ eV and $`J_2=0.080.35`$ meV for $`t=0.25`$ eV. The exchange energy scales as the forth power of the transfer integrals and is thus very sensitive to the variation of $`t`$, nonetheless we can conclude that the superexchange theory gives the correct order of magnitude of the experimental transition temperature. It is worth mentioning that $`t_{2g}`$ electrons contribute approximately only to one-tenth of the value of $`J_2`$. Our analysis also suggests that $`J_1`$ is antiferromagnetic as well, but around half of $`J_2`$. Next-nearest neighbor spins are thus coupled stronger than nearest-neighbor ones.

To complete the discussion on the ground state properties of the spin-orbital Hamiltonian (12), in the following we relax the constraint $`t_e/t=3`$, fixing $`t=0.25`$ eV and $`U_2=5`$ eV, and consider the phase diagram in $`t_e`$ and $`\mathrm{\Delta }_{\text{CT}}`$ parameter plane. The result is presented in Fig. 4. For small values of $`e_g`$ hopping, a ferromagnetic phase is stabilized. Its orbital ordering (OO-III) is shown in Table 1. In this configuration the system maximizes the nn ferromagnetic exchange, $`J_1>0`$. The exchange between nnn neighbors is always antiferromagnetic, $`J_2<0`$, and increases with $`t_e`$. At some critical value of the $`e_g`$ transfer, at which $`J_1+J_2=0`$, the FM ordering becomes unstable and a transition to the AFM-II state takes place (see filled circles in Fig. 4). For smaller values of the Coulomb energy, $`U_2`$, the phase space for ferromagnetic ordering is enlarged and the transition to the AFM-II state occurs for larger values of $`t_e`$. The FM–AFM-II phase boundary for $`U_2=2.5`$ eV is shown as open circles in Fig. 4.

## IV Summary

To summarize, we have developed a superexchange theory for insulating double-perovskite compounds such as Sr2FeWO6. The superexchange interaction, that couples the magnetic moments of Fe2+ ions through the diamagnetic W6+ ions, takes place on Fe-W-Fe bonds with $`90^{}`$ and $`180^{}`$ angles. The theory has been implemented in an effective spin-orbital Hamiltonian formulated in terms of spin ($`S=2`$) and orbital pseudo-spin ($`\tau =1`$) degrees of freedom of the iron ion only, arising from the threefold degeneracy of $`t_{2g}`$-levels. We have studied magnetically and orbitally ordered states and constructed the classical ground state phase diagram of the effective Hamiltonian. We have shown that for realistic values of the model parameters the ground state is antiferromagnetic, as experimentally observed. Our results suggests, that the antiferromagnetic order is of type-II, i.e., $`\{111\}`$ ferromagnetic planes stacked antiferromagnetically. This prediction can be tested by means of polarized neutron experiments. We have evaluated the exchange energies for these magnetic structure and showed that the theory gives an estimate of the transition temperature which is compatible with the experimental value. The magnetic structure is accompanied by an orbital ordering in which each cubic-sublattice of iron ions shows a ferro-type orbital ordering. The type of occupied orbital states changes from one sublattice to the other. The energy scale of orbital degrees of freedom is one order of magnitude smaller than the spin one. The is due to the fact that orbitals are coupled by $`t_{2g}`$ electrons, only, while both $`e_g`$ (with larger transfer amplitude) and $`t_{2g}`$ virtual processes lift the spin degeneracy. Finally, we note that in the present paper we have just dealt with the electronic mechanisms to lift the ground state orbital degeneracy.

However, there are two other possible mechanisms, not discussed here, that can lift the orbital degeneracy, such as the lattice distortion, or Jahn-Teller (JT) effect, and the spin-orbit coupling. The latter breaks the rotational spin invariance and opens a spin gap: Therefore a correct order of magnitude for this effect could be obtained by the experimental measurement of the spin-wave gap. As for the lattice mechanism, it should support the orbital ordering that minimizes the electronic energy of the system and thus enlarge the stability range of the orbital order, because the JT effect in this compound is mainly governed by the physics of isolated clusters rather than by cooperative effects. In fact, the oxygen octahedra surrounding Fe ions are independent one another, as they do not share any common oxygen-ion. Therefore JT distortions are not correlated as far as change in the electronic energy is concerned: Distortions of the octahedra around W ions with empty $`5d`$-level do not cause any considerable change in the electronic energy.

In conclusion, if the electronic mechanism dominates the other two, then the orbital order can be stabilized only at very low temperatures, much lower than the magnetic transition temperature and in between the system is magnetically ordered but orbitally disordered. In order to clarify which of the above mechanism is dominant further experimental studies of the magnetic and structural properties of the system are necessary.

###### Acknowledgements.

We would like to thank C. R. Natoli for a critical reading of the manuscript. G. J. acknowledges kind hospitality at the theory group of the LNF-INFN, Frascati.

## Appendix A Derivation of the fourth order energy correction.

Consider the Hamiltonian:

$`H=H_0+\lambda H^{}`$ (18)
where $`H_0`$ is exactly solvable ($`H_0\psi _0=E_0\psi _0`$) and $`\lambda =`$ is some “small” non-dimensional parameter. Following, for example Ref.bransden, , it is straightforward to write the coupled equations to get eigenvalue and eigenvector corrections to $`E_0`$ and $`\psi _0`$ up to the fourth order in $`\lambda `$:

$`(H_0E_0)\psi _0=0,(H^{}E_1)\psi _0+(H_0E_0)\psi _1=0,(H^{}E_1)\psi _1+(H_0E_0)\psi _2E_2\psi _0=0,`$
$`(H^{}E_1)\psi _2+(H_0E_0)\psi _3E_2\psi _1E_3\psi _0=0,`$
$`(H^{}E_1)\psi _3+(H_0E_0)\psi _4E_2\psi _2E_3\psi _1E_4\psi _0=0.`$
Multiplying scalarly all equations by $`(\psi _0)^{}`$ and solving with respect to the fourth order energy correction, $`E_4`$, we get:

$`E_4`$ $`=`$ $`{\displaystyle \underset{lk}{}}{\displaystyle \underset{mk}{}}({\displaystyle \underset{nk}{}}{\displaystyle \frac{H_{kl}^{}H_{lm}^{}H_{mn}^{}H_{nk}^{}}{(E_kE_l)(E_kE_m)(E_kE_n)}}{\displaystyle \underset{nk}{}}{\displaystyle \frac{H_{kl}^{}H_{lm}^{}\delta _{mn}H_{nk}^{}H_{kk}^{}}{(E_kE_l)(E_kE_m)(E_kE_n)}}`$
$``$ $`{\displaystyle \frac{H_{kl}^{}H_{lk}^{}H_{km}^{}H_{mk}^{}+H_{kl}^{}H_{lm}^{}H_{mk}^{}H_{kk}^{}H_{kl}^{}\delta _{lm}H_{mk}^{}H_{kk}^2}{(E_kE_m)(E_kE_l)^2}})`$
where we use notation: $`H_{km}^{}=\psi _k|H^{}|\psi _m`$. Given the form of $`H_t^{}`$, Eq. (5), it follows that $`H_{kk}^{}=0`$, ie, the second, fourth and fifth terms do not contribute. Also the third term can be neglected, because it does not give rise to an effective exchange between Fe-sites, being the product of two second-order processes. This justifies our formula (11) in Sec.II.A.

## Appendix B Orbital terms and energy denominators.

Here we write explicitly the orbital contributions to the effective Hamiltonian (12).

First we consider virtual processes with $`t_{2g}`$-electrons involved. All orbital contributions $`O_{ij}^{(F(A))}`$ for a bond $`ij`$ can be written in the following general form:

$`O_{ij}^{(F(A))}={\displaystyle \underset{P,ll^{}}{}}O_{ij,P}^{ll^{}},\text{where}O_{ij,P}^{ll^{}}={\displaystyle \frac{\gamma _P^{ll^{}}}{D_P^{ll^{}}}}\stackrel{~}{O}_{ij,P}^{ll^{}}`$ (20)
and $`D_P^{ll^{}}`$ denotes an energy denominator, $`\stackrel{~}{O}_{ij,p}^{ll^{}}`$ is an orbital contribution expressed by means of the pseudospin operators, $`\gamma _P^{ll^{}}`$ are normalization factors, which are given in the Table at the end of the Appendix B, $`P`$ denotes one of the four virtual hopping processes $`A`$, $`B`$, $`C`$, and $`D`$, depicted in Fig. 1, and $`l`$ and $`l^{}`$ are the kind of excited states involved in the hopping process (i.e. $`a`$, $`b`$, and $`c`$ introduced in Sec. II.B).

In the following, we list all the terms, classified for the kind of process.

$`A`$-process: For processes involving excited states of $`a`$\- and $`b`$\- type the orbital contributions differ only because of the energy denominators:

$`D_A^{aa(bb)}=\mathrm{\Delta }_{\text{CT},a(b)}^2\left[E_t^{(7)}+E_{a(b)}^{(5)}2E_g^{(6)}\right],`$ (21)
here and below $`\mathrm{\Delta }_{\text{CT},l}`$ denotes energy needed for an electron transfer from Fe(6) to W(0) when iron ion is left in a Fe$`{}_{l}{}^{}{}_{}{}^{(5)}`$ state. This energy is given by $`\mathrm{\Delta }_{\text{CT},l}=\mathrm{\Delta }_{\text{CT}}+E_l^{(5)}E_a^{(5)}`$. The state $`a`$ is the lowest energy configuration of Fe(5) and $`\mathrm{\Delta }_{\text{CT}}=\mathrm{\Delta }_{\text{CT},a}`$ is the lowest energy necessary for the $`\text{Fe}^{(6)}\text{W}^{(0)}`$ charge transfer.

The corresponding pseudospin part is:

$`\stackrel{~}{O}_{ij,A}^{aa(bb)}={\displaystyle \frac{t_{xy}^4}{2}}\tau _{iz}(\tau _{iz}+1)\left[{\displaystyle \frac{1}{2}}\tau _{jz}(\tau _{jz}1)+(1\tau _{jz}^2)\right]+{\displaystyle \frac{t_{xz}^4}{2}}\tau _{iz}(\tau _{iz}1)\left[{\displaystyle \frac{1}{2}}\tau _{jz}(\tau _{jz}+1)+(1\tau _{jz}^2)\right]+t_{yz}^4(1\tau _{iz}^2)\tau _{jz}^2`$
$`+{\displaystyle \frac{t_{xy}^2t_{xz}^2}{4}}\left[\tau _i^{}\tau _i^{}\tau _j^+\tau _j^++\tau _i^+\tau _i^+\tau _j^{}\tau _j^{}\right]+{\displaystyle \frac{t_{xy}^2t_{yz}^2}{2}}\left[\tau _i^{}\tau _{iz}\tau _{jz}\tau _j^++\tau _{iz}\tau _i^+\tau _j^{}\tau _{jz}\right]+{\displaystyle \frac{t_{xz}^2t_{yz}^2}{2}}\left[\tau _{iz}\tau _i^{}\tau _j^+\tau _{jz}+\tau _i^+\tau _{iz}\tau _{jz}\tau _j^{}\right]`$
(22)
If the excited state is Fe$`{}_{c\pm }{}^{}{}_{}{}^{(5)}`$ then the purely orbital contribution can be written as:

$`\stackrel{~}{O}_{ij,A}^{cc}`$ $`=`$ $`t_{xy}^4\left[(1\tau _{iz}^2)+{\displaystyle \frac{1}{2}}\tau _{iz}(\tau _{iz}1)\right]\left[(1\tau _{jz}^2)+{\displaystyle \frac{1}{2}}\tau _{jz}(\tau _{jz}1)\right]`$
$`+`$ $`t_{xz}^4\left[(1\tau _{iz}^2)+{\displaystyle \frac{1}{2}}\tau _{iz}(\tau _{iz}+1)\right]\left[(1\tau _{jz}^2)+{\displaystyle \frac{1}{2}}\tau _{jz}(\tau _{jz}+1)\right]+t_{yz}^4\tau _{iz}^2\tau _{jz}^2`$
$`\pm `$ $`{\displaystyle \frac{t_{xy}^2t_{xz}^2}{4}}\left[\tau _i^+\tau _i^+\tau _j^+\tau _j^++\tau _i^{}\tau _i^{}\tau _j^{}\tau _j^{}\right]\pm {\displaystyle \frac{t_{xy}^2t_{yz}^2}{2}}\left[\tau _{iz}\tau _i^+\tau _{jz}\tau _j^++\tau _i^{}\tau _{iz}\tau _j^{}\tau _{jz}\right]\pm {\displaystyle \frac{t_{xz}^2t_{yz}^2}{2}}\left[\tau _{iz}\tau _i^{}\tau _{jz}\tau _j^{}+\tau _i^+\tau _{iz}\tau _j^+\tau _{jz}\right]`$
where $`c`$ can be either $`c_+`$ or $`c_{}`$, and respectively, either upper or lower sign should be taken in Eq. B. Corresponding energy denominator is given by:

$`D_A^{cc}=\mathrm{\Delta }_{\text{CT},c}^2\left[E_t^{(7)}+E_c^{(5)}2E_g^{(6)}\right].`$ (24)
$`B`$-process: It has only diagonal orbital contributions, as shown in the Table of section II. If $`aa`$-, $`bb`$-, $`ab`$\- excited states are involved then the pure orbital part is the same, and can be written as:

$`\stackrel{~}{O}_{ij,B}^{ll^{}}={\displaystyle \frac{t_{xy}^4}{4}}\tau _{iz}(\tau _{iz}+1)\tau _{jz}(\tau _{jz}+1)+{\displaystyle \frac{t_{xz}^4}{4}}\tau _{iz}(\tau _{iz}1)\tau _{jz}(\tau _{jz}1)+t_{yz}^4(1\tau _{iz}^2)(1\tau _{jz}^2)`$ (25)
For $`cc`$-hopping processes the orbital contribution $`\stackrel{~}{O}_{ij,B}^{cc}`$ is equal to diagonal part of $`\stackrel{~}{O}_{ij,A}^{cc}`$ and reads as

$`\stackrel{~}{O}_{ij,B}^{cc}`$ $`=`$ $`t_{xy}^4\left[(1\tau _{iz}^2)+{\displaystyle \frac{1}{2}}\tau _{iz}(\tau _{iz}1)\right]\left[(1\tau _{jz}^2)+{\displaystyle \frac{1}{2}}\tau _{jz}(\tau _{jz}1)\right]`$
$`+`$ $`t_{xz}^4\left[(1\tau _{iz}^2)+{\displaystyle \frac{1}{2}}\tau _{iz}(\tau _{iz}+1)\right]\left[(1\tau _{jz}^2)+{\displaystyle \frac{1}{2}}\tau _{jz}(\tau _{jz}+1)\right]+t_{yz}^4\tau _{iz}^2\tau _{jz}^2`$
As for $`ac`$\- and $`bc`$\- processes, their orbital part are equal to the diagonal part of $`\stackrel{~}{O}_{ij,A}^{aa(bb)}`$ (22) given by

$`\stackrel{~}{O}_{ij,B}^{ac(bc)}={\displaystyle \frac{t_{xy}^4}{2}}\tau _{iz}(\tau _{iz}+1)\left[{\displaystyle \frac{1}{2}}\tau _{jz}(\tau _{jz}1)+(1\tau _{jz}^2)\right]+{\displaystyle \frac{t_{xz}^4}{2}}\tau _{iz}(\tau _{iz}1)\left[{\displaystyle \frac{1}{2}}\tau _{jz}(\tau _{jz}+1)+(1\tau _{jz}^2)\right]+t_{yz}^4(1\tau _{iz}^2)\tau _{jz}^2`$
(27)
The general form for B-processes energy denominators is

$`D_B^{ll^{}}=\mathrm{\Delta }_{\text{CT},l}\mathrm{\Delta }_{\text{CT},l^{}}\left[\mathrm{\Delta }_{\text{CT},l}+\mathrm{\Delta }_{\text{CT},l^{}}\right]`$ (28)
$`C`$-process: In this process two electrons with the same spin directions are exchanged between iron sites. The intermediate step involves the formation of a doubly occupied W site. This implies that two different orbitals must participate to the hopping process because of Pauli principle. The orbital contributions are thus only non-diagonal. They are the same for all processes of the kind $`aa`$, $`bb`$, $`cc`$, and $`ab`$:

$`\stackrel{~}{O}_{ij,C}^{ll^{}}`$ $`=`$ $`\pm {\displaystyle \frac{t_{xy}^2t_{xz}^2}{4}}\left[\tau _i^{}\tau _i^{}\tau _j^+\tau _j^++\tau _i^+\tau _i^+\tau _j^{}\tau _j^{}\right]`$ (29)
$`\pm `$ $`{\displaystyle \frac{t_{xy}^2t_{yz}^2}{2}}\left[\tau _i^{}\tau _{iz}\tau _{jz}\tau _j^++\tau _{iz}\tau _i^+\tau _j^{}\tau _{jz}\right]\pm {\displaystyle \frac{t_{xz}^2t_{yz}^2}{2}}\left[\tau _{iz}\tau _i^{}\tau _j^+\tau _{jz}+\tau _i^+\tau _{iz}\tau _{jz}\tau _j^{}\right],`$
where the lower sign should be taken only when $`l=c_{}`$ and $`l^{}=c_+`$. These processes differ one another only by the energy denominators.

For $`ac`$\- and $`bc`$\- processes we have

$`\stackrel{~}{O}_{ij,C}^{ac(bc)}`$ $`=`$ $`\pm {\displaystyle \frac{t_{xy}^2t_{xz}^2}{4}}(\tau _i^+\tau _i^+\tau _j^+\tau _j^++\tau _i^{}\tau _i^{}\tau _j^{}\tau _j^{})`$ (30)
$`\pm `$ $`{\displaystyle \frac{t_{xy}^2t_{yz}^2}{2}}(\tau _{iz}\tau _i^+\tau _{jz}\tau _j^++\tau _i^{}\tau _{iz}\tau _j^{}\tau _{jz})\pm {\displaystyle \frac{t_{xz}^2t_{yz}^2}{2}}(\tau _{iz}\tau _i^{}\tau _{jz}\tau _j^{}+\tau _i^+\tau _{iz}\tau _j^+\tau _{jz})`$
where upper sign $`(+)`$ and lower sign $`()`$ correspond to $`c=c_+`$ and $`c=c_{}`$, respectively.

We note that along $`90^{}`$ Fe-W-Fe bond (nn Fe ions) hopping is allowed only for one kind of orbital. Therefore, being orbitally nondiagonal, $`C`$-processes are effective only for $`180^{}`$ bond (nnn Fe ions), as shown in the Table of Sec. II.C. Energy denominators for all orbital contributions have the following common form:

$`D_C^{ll^{}}=\mathrm{\Delta }_{\text{CT},l}\mathrm{\Delta }_{\text{CT},l^{}}\left[\mathrm{\Delta }_{\text{CT},l}+\mathrm{\Delta }_{\text{CT},l^{}}\right].`$ (31)
$`D`$-process: This type of processes is effective only for $`90^{}`$ Fe-W-Fe bonds by definition \[see Fig. 1\] and thus can only be orbitally diagonal. All orbital contributions and energy denominators are equal to the corresponding ones of B-processes \[see Eqs. 25-28\].

Now we consider $`e_g`$ hopping processes. The contributions to the Hamiltonian from such processes does not depend on the orbital degree of freedom:

$`O_{ij,P}^{dd}={\displaystyle \frac{\gamma _P^{dd}}{D_P^{dd}}}t_e^4.`$ (32)
Here the extra factors, which depend on the type of process, and appear due to the anisotropic form of $`e_g`$ transfer (10), are included in normalization factors $`\gamma _P^{dd}`$ given in the Table below.

The energy denominators for different processes can be written in the following forms. For A-process

$`D_A^{dd}=\mathrm{\Delta }_{\text{CT},d}^2\left[E_e^{(7)}+E_d^{(5)}2E_g^{(6)}\right],`$ (33)
and for B-, C- and D-processes

$`D_C^{ll^{}}=\mathrm{\Delta }_{\text{CT},l}\mathrm{\Delta }_{\text{CT},l^{}}\left[\mathrm{\Delta }_{\text{CT},l}+\mathrm{\Delta }_{\text{CT},l^{}}\right].`$ (34)
where $`d`$ and $`d^{}`$ can be either $`d_+`$ or $`d_{}`$ excited states.

In the following Table we list all normalization coefficients $`\gamma _P^{ll^{}}`$:

|  | $`aa`$ | $`bb`$ | $`cc`$ | $`dd`$ | $`ac`$ | bc | ab |
| --- | --- | --- | --- | --- | --- | --- | --- |
| $`A`$ | $`1/10`$ | $`1/10`$ | $`1/16`$ | $`1/8N_\pm `$ |  |  |  |
| $`B`$ | $`1/8`$ | $`2/25`$ | $`1/32`$ | $`1/(8N_\pm ^2)`$ | $`1/20`$ | $`1/20`$ | $`2/25`$ |
| $`C`$ | $`1/10`$ | $`8/125`$ | $`1/40`$ | $`1/(10N_\pm ^2)`$ | $`1/16`$ | $`1/25`$ | $`1/10`$ |
| $`D`$ | $`1/10`$ | $`8/25`$ | $`1/40`$ | $`1/(10N_\pm ^2)`$ | $`1/16`$ | $`1/25`$ | $`1/10`$ |


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# Inverse Compton X–rays from the radio galaxy 3C 219

## 1 Introduction

It is well known that diffuse non–thermal X–ray emission from the radio lobes is a unique tool to constrain the spectrum and the energetics of the relativistic electrons and possibly the acceleration mechanisms at work in radio galaxies.

Diffuse X–rays from the lobes of radio galaxies and quasars are produced by inverse Compton (hereinafter IC) scattering of Cosmic Microwave Background (CMB) photons (e.g. Harris & Grindlay 1979), and/or nuclear photons (Brunetti, Setti & Comastri 1997). In the first case they are sampling the relativistic electrons with Lorentz factor $`\gamma `$ 103, while the X–rays from IC scattering of the nuclear far–IR/optical photons are mainly powered by $`\gamma 100300`$ electrons whose synchrotron emission typically falls in the undetected hundred kHz frequency range.

Non–thermal X–ray emission from the radio lobes has been discovered by ROSAT and ASCA in a few nearby radio galaxies, namely Fornax A (Feigelson et al. 1995; Kaneda et al. 1995; Tashiro et al. 2001), Cen B (Tashiro et al. 1998), 3C 219 (Brunetti et al. 1999) and NGC 612 (Tashiro et al. 2000). The analysis of the spatially coincident X–ray and radio flux densities has allowed to estimate magnetic field strengths which are close, but on average lower than the values derived under equipartition conditions. However these results are affected by significant uncertainties arising from the low X–ray counting statistics in the diffuse component and the insufficient angular resolution of the instruments.

The superb capabilities of the Chandra X–ray observatory make now possible to image, on arcsec scale, the radio lobes of powerful radio galaxies and quasars and to disentangle the non–thermal emission from the thermal and from the nuclear component. Non–thermal emission from the radio lobes of relatively compact and powerful objects has been successfully detected with Chandra in the case of the radio galaxy 3C 295 (Brunetti et al., 2001) and, possibly, in a few high redshift radio galaxies (Carilli 2002), and in the counter lobes of the radio loud quasars 3C 207 (Brunetti et al. 2002) and 3C 179 (Sambruna et al. 2002). These observations are well interpreted as IC scattering of IR photons from the corresponding nuclear source, thus providing a clear evidence for the presence of low energy electrons ($`\gamma `$ 100) in the radio volumes. On the other hand, the detection of X–ray emission from the radio lobes of giant radio galaxies is best explained by IC scattering of the CMB photons (Hardcastle et al. 2002; Isobe et al. 2002; Grandi et al. 2002).

In this paper we report on the Chandra observation of the nearby, powerful, double–lobed FRII radio galaxy 3C 219. $`H_0=50`$ km s-1 Mpc-1 and $`q_0=0.5`$ are used throughout.

## 2 3C 219 and the radio data

The radio galaxy 3C 219 at $`z`$=0.1744 is a prototype of the FR–II class of powerful radio sources. Its projected angular size is about 180 arcsec (Clarke et al. 1992) corresponding to a projected liner size of about 680 kpc. The optical counterpart of the nuclear radio source is a cD galaxy with M$`{}_{V}{}^{}=21.4`$ (Taylor et al. 1996) in a non-Abell cluster (Burbidge & Crowne 1979). The radio structure is characterized by a relatively weak core, a straight jet $`20^{\prime \prime }`$ long (75 kpc) pointing towards the SW, and a weak blob on the counterjet side. Two almost symmetric hot-spots are present, the one in the south–west lobe being aligned with the jet axis. The two lobes account for most of the radio emission at all frequencies below 15 GHz.
The overall radio spectrum is best fitted with a slope $`\alpha `$ 0.8 (S$`\nu ^\alpha `$) between 178 and 750 MHz (Laing et al. 1983) which steepens to $`\alpha `$ 1 above about 1 GHz (see Fig. 3).
By assuming the standard equipartition recipe, which corresponds to integrate the synchrotron spectrum between the fixed range of frequencies 10 MHz – 100 GHz (Pacholczyk 1970), the magnetic field in the lobes, considered as homogeneous emitting regions, is $``$ 7.6 $`\mu `$G. If we assume instead that low energy electrons down to $`\gamma _{min}50`$ are present, the magnetic field increases to $``$ 10.4 $`\mu `$G.

### 2.1  The VLA observations

The radio images at 1.4 GHz were obtained by combining archival VLA data: A-configuration observations were carried out on May 18, 1986 for a total integration of 6.5 hours, while B-configuration data were taken on September 6, 1986 for a total of about 7 hours on source. The total bandwidth is 25 MHz for each dataset. We carried out the data reduction in a standard way by means of the NRAO Astronomical Image Processing System (AIPS). We first processed the B-configuration data, and then used the final image to start the phase self-calibration of the shortest spacings of the A-configuration data for which the source structure is resolved out in the latter dataset. Then we combined the A and B configuration observations and the final image obtained has a resolution of 1.74 $`\times `$ 1.64 arcsec in p.a. $`13^{}`$; the off-source r.m.s. noise level in the image plane is 40 $`\mu `$Jy/beam. The total flux density accounted for 3C219 in our image is 8.525 Jy.
A more detailed analysis of the radio data will be presented elsewhere, where further VLA observations at various frequencies and configurations will be discussed (Dallacasa et al. in preparation).

## 3 X–ray observations

### 3.1 Imaging

The target was placed at about 40” from the nominal aimpoint of the back illuminated ACIS S3 chip onboard Chandra and observed on 2000 October 11th. Although the observation was performed using a subarray configuration the nuclear source is affected by photon pile-up and will not be considered any further. The raw level 1 data were re–processed using the latest version 2.2 of the CXCDS CIAO software and filtered using a standard grade selection. There is evidence for an increased background count rate towards the end of the observation. The corresponding time intervals were filtered out leaving about 16.8 ksec of useful data. In order to study the morphology of the extended emission all the counts within a region of 5 arcsec radius centered on the nuclear source and those in the read–out streaks have been subtracted. The full band (0.5–7 keV) X–ray image smoothed with a fixed size gaussian (FWHM of 10′′) is reported in Fig. 1. The radio contours obtained from the 1.4 GHz radio image smoothed on the same scale are also overplotted.

The detection of extended X–ray emission almost coincident with the radio lobes emission strongly favour the non–thermal IC nature for the high energy radiation as previously suggested by Brunetti et al. (1999) on the basis of lower resolution ROSAT HRI data.

The bright clump at the boundary of the northern radio lobe is characterized by a soft X–ray spectrum and is most likely due to a previously unknow group of galaxies at z$``$ 0.4 (see section 3.2.3). The relatively faint diffuse emission coincident with the radio lobes shows a brightness increment in the innermost part of the northern lobe. Extended X–ray emission to the east from the nucleus not spatially coincident with the radio contours is also evident (Fig. 1). Finally, there is also a jetted X–ray emission at about 10–30 arcsec south of the nucleus which appears to be spatially coincident with the two radio knots of the main jet (Fig. 2).

### 3.2 Spectroscopy

Given that we are interested in the study of the origin of the faint diffuse X–ray emission from the radio lobes the background subtraction is an important issue.

In order to obtain the best estimate of the total background we rely on a technique which allows to significantly reduce the particle background for those observations carried out in the Very Faint Mode. 111$`\mathrm{http}://\mathrm{cxc}.\mathrm{harvard}.\mathrm{edu}/\mathrm{cal}/\mathrm{Links}/\mathrm{Acis}`$ $`/\mathrm{acis}/\mathrm{Cal}_\mathrm{p}\mathrm{rods}/\mathrm{vfbkgrnd}/\mathrm{index}.\mathrm{html}`$ We have employed this technique (hereinafter VF) with the recommended choice of parameters. As a result the quiescent background is reduced up to 30% depending on the energy range. Source spectra have been extracted using appropriate response and effective area functions taking into account the source extension and weighing the detector response and effective area according to the source spectrum. The instrument response has been also corrected for the degradation in the ACIS quantum efficiency using the latest version of the ACISABS tool.

#### 3.2.1 The lobes spectra

The Chandra spectrum of the entire extended emission (Fig. 3), including the jet knot, but excluding the background cluster (see below), is best fitted with a power law with $`\mathrm{\Gamma }=1.74\pm 0.17`$ plus Galactic absorption ($`N_H=1.55\times 10^{20}`$ cm-2) fully consistent with the radio spectrum. The 0.5–7 keV flux of 2.4 $`\times `$ 10-13 erg cm-2 s-1 corresponds to a rest–frame luminosity of about 3 $`\times `$ 1043 erg s-1. Even though the counting statistics (about 570 net counts) does not allow to statistically discriminate between a power law and a thermal model the latter returns a slightly worse fit ($`\mathrm{\Delta }\chi ^2`$ 3 for the same number of parameters) with a best fit temperature of about 4 keV (greater than 3 keV at the 90% confidence level). Besides the fact that the observed 0.5–7 keV luminosity is about an order of magnitude lower than that expected from the $`L_X`$–T relation for clusters of galaxies (e.g., Arnaud & Evrard 1999), the observed morphology and the extremely good agreeement between the X–ray and radio spectral slopes strongly rules out a thermal origin for the diffuse X–rays.

In order to search for possible spectral differences between the northern and southern lobe (excluding the jet region) we have considered the X–ray spectra of the two regions separately. We find that the two regions have approximately the same spectral shape, which now is rather poorly constrained with a marginal indication of a slightly harder spectrum ($`\mathrm{\Delta }\alpha `$ 0.25) in the southern lobe.

#### 3.2.2 The jet knot

There is significant evidence of an excess of X–ray emission in the region coincident with the southern radio jet and in particular with the brightest knot (Fig. 2). Although only 12 net counts are detected in the 0.5–7 keV energy range, the band ratio H/S $``$ 2 (where H are the counts in the 2–7 keV and S in the 0.5–2 keV bands, respectively) folded through the ACIS–S spectral response corresponds to a power law spectrum with $`\mathrm{\Gamma }`$ 0 or to an intrinsic absorption column density of about 1022 cm-2 if $`\mathrm{\Gamma }=1.7`$ is assumed. However taking into account the errors associated with small numbers statistic (Gehrels 1986) the spectral slope could be as steep as $`\mathrm{\Gamma }2`$ (90 % confidence) and the absorption fully consistent with the Galactic value. A deeper exposure of 3C219 is needed to confirm the hardness of the X–ray jet and thus constrain the emission mechanism.

#### 3.2.3 The background cluster

A R–band observation retrieved from the HST archive shows the presence of an excess of optical galaxy counts at the position of the north west clump, possibly indicating the presence of a cluster/group. We have obtained the spectrum of the most luminous galaxy of the group with the 3.5m Telescopio Nazionale Galileo (TNG) and identify it with an elliptical galaxy at $`z`$=0.389. The X–ray spectrum of the north west clump (about 115 net counts) is well fitted by a thermal model with a relatively low temperature, $`kT2.1`$ keV plus Galactic absorption. The 0.5–2 keV flux is about 2 $`\times 10^{14}`$ erg cm-2 s-1 and the corresponding luminosity is about 1.2 $`\times 10^{43}`$ erg s-1 which is within a factor of $`2`$ of that expected from the $`L_X`$–T relationship.

## 4 Discussion

The morphology and scale of the faint diffuse X–ray emission is very similar to that of the radio lobes thus suggesting a non–thermal mechanism due to IC scattering of CMB and nuclear photons. The latter would dominate at distances from the nucleus:

$$R_{\mathrm{kpc}}<70\times L_{46}\left(1\mu \right)^2\left(1+z\right)^2$$
(1)
where $`L_{46}`$ is the isotropic nuclear luminosity in units of $`10^{46}`$ erg s-1 in the far–IR to optical band and $`\mu `$ is the cosine of the angle between the direction of the nuclear seed photons and the scattered photons (approximated with the angle between radio axis and line of sight with $`\mu `$ negative for the far lobe and positive for the near one). Since we detect diffuse X–ray emission coincident with the radio lobes out to a distance of $``$300 kpc from the nucleus with a roughly constant and symmetric brightness (Fig. 1), we conclude that the IC scattering of CMB photons is the process which accounts for the majority of the observed X–rays. In addition, we note the presence of enhanced X–ray brightness in the innermost $``$ 15–20 arcsec (projected size $``$ 70 kpc) of the northern (counter) lobe. Although the modest number of counts in this region does not allow to prove the non–thermal origin of this excess, we point out that it would be naturally explained by an additional contribution from IC scattering of nuclear photons which, indeed, is expected to be stronger in the counter lobe (Brunetti et al. 1997). In particular, assuming an angle between the radio axis and the plane of the sky of 30o (appropriate for one–sided jet FR II radio galaxies), Eq.(1) yields a far–IR to optical luminosity of the hidden quasar of $`6\times 10^{45}`$ erg s-1 which is only a factor of $`2`$ lower than that estimated by Brunetti et al. (1999) by making use of a quasar SED normalized to the nuclear X–ray flux. We stress that the present estimate does not depend on the energy densities of the electrons and of the magnetic field in the radio lobes.

From Fig. 1 the X–ray brightness distribution of the enhanced central region appears to be somewhat inclined toward north east with respect to the radio axis. Although we cannot exclude that thermal emission could be responsible for a fraction of the X–ray flux in this region, the observed misalignement indicates an offset between the radio axis and the axis of the pattern of the nuclear photons. We also note that this emission extends further on toward east than the radio pattern, while the diffuse X–ray emission in the lobes is generally well confined within the radio isophotes. This effect finds a straightforward explanation in the model of IC scattering of the nuclear photons because the X–rays from IC scattering of the nuclear photons are emitted by $`\gamma `$ 100-300 electrons which have radiative life–times at least 10 times longer (depending on the importance of Coulomb losses) than the $``$ GHz radio emitting electrons. The oldest population of relativistic electrons in the radio lobes may not be visible anymore in the 1.4 GHz image but still sampled by the Chandra image. As an indication in favour of this possibility it should be noted that the 74 MHz radio observations, which sample electrons with lower energies ($`\gamma `$ 2000) than those synchrotron emitting at 1.4 GHz, also show a slightly larger extension of the radio lobes in the same region with respect to the higher frequency observations (Blundell, Kassim & Perley 2000). In addition, we note that the innermost radio contours in the northern lobe are asymmetric with respect to the radio axis and that they seem to trace a back flow which point in the direction of the X–ray brightness excess region.

The lobes broad band emission (Fig. 4) has been computed by assuming a relativistic electron spectrum with a slope $`\delta =2.5`$. The corresponding synchrotron break ($`\mathrm{\Delta }\delta =1`$) and high frequency cut–off are constrained by the radio data at 1010 and $``$1013 Hz respectively. The observed X–ray emission is accounted for by IC scattering of CMB photons if $`B3.1\mu `$G. Such a value is a factor $`2.5`$ lower than that would be obtained with the standard equipartition formulae (e.g., Packolczyk, 1970) and about a factor 3.3 lower if the equipartition formulae are based on a reasonable choice 222We assume a ratio between protons and electron energy density $`k=1`$ and a filling factor $`\varphi =1`$ of the low energy cut–off in the electron spectrum ($`\gamma _{\mathrm{low}}=50`$; Brunetti et al. 1997). We have also tried to measure the magnetic field across the source by making use of the synchrotron and IC fluxes of both the southern and northern radio lobes. We obtain $`B2.9\mu `$G and $`B3.6\mu `$G for the northern and southern lobe, respectively. These values imply that, depending on the adopted equipartition formulae, the electron energy density is a factor 40–100 and 20–70 larger than that of the average magnetic field in the northern and southern radio lobes, respectively. We remind that the equipartition magnetic field strength would increase if the assumption on the $`\varphi `$ and $`k`$ values are relaxed. These results confirm our previous findings (Brunetti et al. 1999) reached on the basis of ROSAT and ASCA data.

The departure from equipartition of 3C 219 is similar to that found in the lobes of other giant radio galaxies and quasars which emit X–rays via IC of CMB photons (e.g., Cen B, Tashiro et al. 1998; 3C 351, Hardcastle et al. 2002; 3C 452, Isobe et al. 2002; Pictor A, Grandi et al. 2003). On the other hand, despite the poor statistics, the lobes of smaller radio sources, where the effects of IC scattering of the nuclear photons dominates, seem to be closer to minimum energy conditions (e.g., 3C 295, 3C 207; Brunetti et al. 2001,2002). Finally the X–ray emission of 3C 219 does not appear to extend all the way to the end of the radio lobes (Fig. 1), possibly suggesting an amplification of the magnetic field in these external regions as also found in other IC/CMB radio galaxies (e.g., Cen B, Tashiro et al. 1998; 3C 452, Isobe et al. 2002).

## 5 Conclusions

The relatively short (16.8 ksec) Chandra observation of the radio galaxy 3C 219 has successfully detected diffuse X–ray emission from the radio lobes and X–rays associated with the main radio jet. The morphology, extension and spectrum of the diffuse emission strongly support a non–thermal origin, most likely IC scattering of CMB photons. In addition, the net brightness increment observed in the innermost $`70`$ kpc of the northern radio lobe (the far lobe) suggests an additional contribution from IC scattering of nuclear photons for a reasonable far–IR to optical isotropic luminosity of the hidden quasar of $`6\times 10^{45}`$ erg s-1. This implies that the electron spectrum extends to much lower energies (at least $`\gamma `$ 100) than sampled by the radio emission.

From the distribution of the central X–ray emission we deduce that the radiation pattern of the hidden quasar (molecular torus axis) makes an angle of several tens degrees with the radio axis and that the oldes population of the relativistic electrons may occupy a much larger volume than indicated by the radio contours.

By comparing the radio synchrotron and IC emissions from the lobes we obtain an average magnetic field strength approximately a factor $`3`$ lower than the equipartition value.

Additional data from a deeper Chandra observation would allow to perform detailed, spatially resolved X–ray spectroscopy of the diffuse emission and to compute $`B`$-field intensity structure and relativistic electrons’ distribution, if combined with the available radio data.

Finally, the relatively bright X–ray clump at north west on the border of the northern radio lobe (Fig.1) is well fitted by thermal emission from a relatively cold plasma ($`2`$ keV) in a cluster/group of galaxies at $`z=0.389`$.

## 6 Acknowledgments

This research has made use of the NASA/IPAC Extragalactic Database (NED) which is operated by the Jet Propulsion Laboratory, California Institute of Technology, under contract with the National Aeronautics and Space Administration. This letter is based on observations made with the Italian national telescope Galileo Galilei (TNG). We thank Cristian Vignali for a careful reading of the manuscript and the anonymous referee for the useful comments and suggestions. The authors acknowledge partial support by the ASI contracts I/R/113/01 and I/R/073/01 and the MURST grant Cofin–01–02–8773.