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# Exchange interactions in (ZnMn)Se

## I Introduction

The perspective of using the spin of electrons in the semiconductor devices promises to revolutionize modern electronics. ohno\_science  A necessary component of a spintronic process is the spin-injection into semiconductor. This demand created a need for ferromagnetic materials on the semiconductor basis with strong spin-polarization of the carriers and high Curie temperature. After recent discovery ohno\_gaas  of ferromagnetism in (GaMn)As with Curie temperature as high as 110 K much attention is devoted to the study of the diluted III-V semiconductors as possible sources of the spin-polarized electrons. Also the interest to more traditional II-VI semiconductors has been revived since, first, the theoretical studies shaw that the II-VI systems possess the potential for high Curie temperature diohma\_science ; sato\_rev , second, the study of the II-VI diluted magnetic semiconductors (DMS) deepens understanding of the exchange interactions in other types of DMS kacman\_rev ; dietl\_rev ; sato\_rev  and, third, the II-VI systems, in particular (ZnMn)Se, are used in spin-injection experiments as a source of spin-polarized charge carriers. goscri ; jopabe ; oehuha

In (ZnMn)Se with low Mn concentration no magnetic ordering has been experimentally detected up to very low temperatures. furdyna  However, the application of magnetic field leads to the observation of the so-called giant Zeeman splitting for the states of the semiconductor matrix. Because of this large spin splitting (ZnMn)Se is an efficient source of highly polarized carriers. goscri ; jopabe

A commonly accepted explanation of the giant Zeeman splitting in (ZnMn)Se relies on the following picture. In the system there is a strong exchange interaction between the Mn 3d states and the states of the semiconductor. This interaction does not, however, lead to the ordering of the Mn moments. The application of a magnetic field aligns the Mn moments and results in the observation of a giant spin-splitting. The term ’giant’ arises here from the comparison of two energy scales. The characteristic energy of the magnetostatic interaction of the magnetic field of 1 T with the spin of 1$`\mu _B`$ amounts to 0.004 mRy and is up to five orders of magnitude smaller than the splittings detected experimentally. goscri ; furdyna  The coexistence of a very strong exchange between the Mn 3d and semiconductor states and a very low temperature of the magnetic phase transition makes the II-VI DMS an interesting laboratory for studying the physics of exchange interactions.

Much efforts has been paid to the theoretical studies of the DMS of the II-VI type (see, e.g., reviews furdyna ; kacman\_rev ; dietl\_rev ; sato\_rev ). Most of these studies are based on a model-Hamiltonian approach. \[See, e.g., Ref. dubhwo  for the model of bound magnetic polarons and Refs. dietl\_rev ; feciwa  for the Zener model. The latter can be considered as a continuous-medium limit of the well-known Rudermann-Kittel-Kasuya-Yosida (RKKY) approach. Spalek et al spalek\_86  used Anderson’s approach to superexchange and have shown that few adjustable parameters of the theory are sufficient to describe the interplay between different types of exchange interactions in the system. Reach experimental information (e.g. furdyna\_88  in the case of (ZnMn)Se) is helpful in the selection of the values of the parameters.\]

The developments in the methods of the density functional theory (DFT) accompanied by fast increasing computer power allow now for parameter-free calculation of the electronic properties of very complex systems. In the case of II-VI DMS the number of the DFT studies of the exchange interactions is still very restricted (for exceptions see, e.g., Refs. lahaeh ; wezu ; sato\_rev ). Most of the calculations have been performed with the use of a virtual crystal approximation or a single-site coherent-potential approximation (CPA).lahaeh ; sato\_rev  These schemes are convenient and efficient in the investigation of the systems with varying concentration of impurities. They, however, do not take into account the atomic short-range order and the increasing distance between impurities with decreasing impurity concentration. Therefore it is important to combine the calculations within the virtual-crystal and CPA techniques with the studies making more detailed account for the positions of the impurity atoms. Such studies can be performed with the use of large supercells of the semiconductor crystals. zhao ; sanvito\_rev ; sabr02\_1 ; sabr\_condmat  The aim of this paper is the investigation of the exchange interactions in (ZnMn)Se on the basis of the supercell approach.

An important question concerns the role of the intraatomic correlations in the Mn 3d states. Within the model-Hamiltonian approaches the 3d states are usually considered as atomic-like and strongly correlated. This treatment is rather different from the treatment within LDA. To study the role of the electron correlations in the Mn3d shell we use the LDA+U method LDA+U\_93  designed to take into account the on-site Coulomb interaction $`U`$.

The purpose of this paper is two-fold. On the one hand, by detailed DFT calculation of the electronic properties of (ZnMn)Se we aim to provide deeper insight into the physics of the system. On the other hand, by comparison with experimental data of the calculational results we aim to draw the conclusion which of the two approaches, LDA or LDA+U, provides better description of (ZnMn)Se. Both components of the purpose are of strong importance for future studies of DMS within the DFT.

## II Calculational approach

In the calculations we follow the scheme described in Ref. sabr02\_1 . This scheme is based on the supersell approach where one of the Zn atoms in a supercell of zinc-blende ZnSe is replaced by the Mn atom. The calculations are performed for four values of the concentration $`x`$: 0.25, 0.125, 0.0625, and 0.03125.

The calculations were carried out with the augmented spherical waves wikuge  (ASW) method within the LDA and LDA+U approaches. In all calculations the lattice parameter was chosen to be equal to the experimental lattice parameter of ZnSe. Two empty spheres per formula unit have been used in the calculations. The positions of empty spheres are (0.5, 0.5, 0.5) and (0.75, 0.75, 0.75). Radii of all atomic spheres were chosen to be equal. Depending on the concentration of Mn, the super cell is cubic (x=25%, $`a\times a\times a`$, and x=3.125%, $`2a\times 2a\times 2a`$) or tetragonal (x=12.5%, $`a\times a\times 2a`$ and 6.25%, $`2a\times 2a\times a`$).

The LDA+U calculations were performed with $`U=0.3Ry`$. U\_comment

### II.1 Spin-projected densities of states

The spin splitting of the valence-band states is a result of the interaction between these states and the Mn3d states. The directions of the Mn moments are disordered in the absence of magnetic field and become increasingly ordered with increasing value of the applied field. There are two possible scenarios for the relation between the ordering of the Mn moments and the spin splitting of the valence band states (Fig. 1). First scenario is a mean-field (Stoner-like) type of the relation.

In this case the valence-band states experience an average exchange field of the Mn moments that is proportional to the net magnetization in the Mn subsystem. Complete disordering of the Mn moments leads to the disappearance of the net magnetization and, respectively, of the spin splitting. In the second scenario, the spin of the valence states follows locally the spins of the Mn atoms. Therefore, the spin polarization and exchange splitting do not disappear with disappearance of the net magnetization. An experimental example of the non-Stoner behavior of the exchange splitting is discussed by Kisker kisker  for the case of iron with thermally disordered atomic moments. In (ZnMn)Se the experimental data is treated in favor of the mean-field scenario. furdyna

To study both scenarios within the DFT we will need to calculate densities of states (DOS) projected on different spin-quantization axes. The calculation is performed as follows. The wave function of a given electron state is considered to be two-component spinor $`\left(\begin{array}{c}\psi _1(𝐫)\\ \psi _2(𝐫)\end{array}\right)`$. The spin components $`\psi _1(𝐫)`$ and $`\psi _2(𝐫)`$ are written with respect to a chosen axis. The spin-quantization axis does not change within atomic spheres but can vary from atom to atom. The integral

$$n_{i𝐤\nu }^s=_{\mathrm{\Omega }_\nu }𝑑𝐫|\psi _{i𝐤s}(𝐫)|^2$$
(1)
gives the part of the state $`\psi _{i𝐤}`$ corresponding to atom $`\nu `$ and spin-projection $`s`$. Here k is the wave vector, $`i`$ numbers the energy bands. The integration is carried out over the $`\nu `$th atomic sphere. The wave functions are normalized in the unit cell: $`_{s\nu }n_{i𝐤\nu }^s=1`$. The partial DOS for given $`\nu `$ and $`s`$ is given by formula

$$N_\nu ^s(\epsilon )=\frac{1}{\mathrm{\Omega }_{BZ}}\underset{i}{}_{BZ}𝑑𝐤n_{i𝐤\nu }^s\delta (\epsilon \epsilon _{i𝐤})$$
(2)
where $`\mathrm{\Omega }_{BZ}`$ is the volume of the Brillouin zone (BZ). To calculate the partial DOS with respect to another quantization axis the electron wave functions are subjected to the transformation adv\_phys

$$\left(\begin{array}{c}\psi _1^{}(𝐫)\\ \psi _2^{}(𝐫)\end{array}\right)=U_\nu ^{}\left(\begin{array}{c}\psi _1(𝐫)\\ \psi _2(𝐫)\end{array}\right),𝐫\mathrm{\Omega }_\nu $$
(3)
where $`U_\nu `$ is the spin-$`\frac{1}{2}`$ transformation matrix corresponding to the rotation of the axis of the $`\nu `$th atom. Next, the procedure defined by Eqs. (1-2) is performed for the spinor components of the transformed functions (3).

### II.2 Interatomic exchange parameters and Curie temperature

To describe the exchange interactions between Mn moments we use an effective Heisenberg Hamiltonian of classical spins

$$H_{eff}=\underset{ij}{}J_{ij}𝐞_i𝐞_j$$
(4)
where $`J_{ij}`$ is an exchange interaction between two Mn sites $`(i,j)`$ and $`𝐞_i`$ is the unit vector pointing in the direction of the magnetic moment at site $`i`$.

To estimate the parameters of the Mn-Mn exchange interaction we perform calculation for the following frozen-magnon haespe ; nikl  configurations:

$$\theta _i=const,\varphi _i=𝐪𝐑_i$$
(5)
where $`\theta _i`$ and $`\varphi _i`$ are the polar and azimuthal angles of vector $`𝐞_i`$, $`𝐑_i`$ is the position of the $`i`$th Mn atom. The directions of the induced moments in the atomic spheres of Ga and As and in the empty spheres were kept to be parallel to the $`z`$ axis.

It can be shown that within the Heisenberg model (4) the energy of such configurations can be represented in the form

$$E(\theta ,𝐪)=E_0(\theta )\theta ^2J(𝐪)$$
(6)
where $`E_0`$ does not depend on q and $`J(𝐪)`$ is the Fourier transform of the parameters of the exchange interaction between pairs of Mn atoms:

$$J(𝐪)=\underset{j0}{}J_{0j}\mathrm{exp}(i𝐪𝐑_{\mathrm{𝟎}𝐣}).$$
(7)
In Eq. (6) angle $`\theta `$ is assumed to be small. Using $`J(𝐪)`$ one can estimate the energies of the spin-wave excitations comm\_proport :

$$\omega (𝐪)=\frac{4}{M}[J(\mathrm{𝟎})J(𝐪)]=\frac{4}{M}\frac{E(\theta ,𝐪)E(\theta ,\mathrm{𝟎})}{\theta ^2}$$
(8)
where $`M`$ is the atomic moment of the Mn atom. Performing back Fourier transformation we obtain the parameters of the exchange interaction between Mn atoms:

$$J_{0j}=\frac{1}{N}\underset{𝐪}{}\mathrm{exp}(i𝐪𝐑_{\mathrm{𝟎}𝐣})J(𝐪).$$
(9)
The Curie temperature was estimated in the mean-field (MF) approximation

$$k_BT_C^{MF}=\frac{2}{3}\underset{j0}{}J_{0j}$$
(10)
We use rigid band approach to calculate the exchange parameters and Curie temperature for different electron occupations. We assume that the electron structure calculated for a DMS with a given concentration of the 3d impurity is basically preserved in the presence of defects. The main difference is in the occupation of the bands and, respectively, in the position of the Fermi level.

## III Calculational results

### III.1 Densities of states and exchange splittings

#### III.1.1 LDA

We begin the discussion of the calculational results with consideration of the DOS of the ferromagnetic (ZnMn)Se (Fig. 2). Compared with pure ZnSe, the replacement of a Zn atom by a Mn atom adds five 3d spin-up energy bands to the valence band of the system. Since the number of Mn 3d electrons is also five no carriers appear either in the valence band or in the conduction band.

The values of the calculated spin moments are collected in Table 1. The moment in the Mn sphere and the induced moment on the neighboring Se atom are practically independent of the Mn concentration. The moment per supercell is exactly 5$`\mu _B`$ since there are extra five filled spin-up bands compared with the nonmagnetic ZnSe.

At the top of the valence band there is strong negative exchange splitting: the upper edge of the spin-up DOS lies higher in energy than the upper edge of the spin-down DOS ( Fig. 2). The spin splitting increases with increasing Mn concentration. The origin of this splitting can be understood from the analysis of the partial Mn3d DOS (Fig. 3).

Indeed, a higher energy of the spin-up valence-band edge results from the contribution of the Mn3d spin-up states. On the other hand, there is no strong contribution of the Mn spin-down states to the valence band. Unoccupied spin-down Mn3d bands lie in the semiconducting gap, close to the bottom of the conduction band.

The exchange splitting of the states at the top of the valence band of the ferromagnetic (ZnMn)Se is in qualitative agreement with the observation of the giant spin splitting under the application of the magnetic field.

To understand the dependence of the electron structure on the magnetic configuration we performed calculation for the antiferromagnetic configuration of the Mn moments for $`x=3.125\%`$. The antiferromagnetic structure is characterized by the largest angle between the neighboring Mn moments and, therefore, is the state most different from the ferromagnetic one. The comparison of the DOS of the ferromagnetic and antiferromagnetic configurations for $`x=3.125\%`$ (Figs. 2 and 4) shows that they are similar. The main difference in the antiferromagnetic DOS is the appearance of a small energy gap which separates the upper part of the valence-band states from the rest of the valence band. The spin-splitting obtained in the ferromagnetic DOS is present also in the antiferromagnetic DOS as the splitting between the top of the separated (impurity) band and the top of the valence band. Figures 3 and 4 show that the partial DOS of the Mn atoms are only weakly dependent on the magnetic configuration and preserve fully the local spin splitting. Obviously the main features of the LDA-DOS cannot be treated in terms of the Stoner-like mean-field picture (Fig. 1).

To study in more details the relation between the electron structure and magnetic configuration we perform the analysis of the partial DOS of the atoms of the semiconductor matrix. As we show below, the behavior of the DOS of different atoms ranges from a highly non-Stoner one to the behavior well described by the mean-field picture.

In Figs. 5,6 we present the partial DOS for two different Se atoms. The DOS is calculated for magnetic configurations depicted schematically in Fig. 7 where three successive Mn atoms along the $`z`$ axis are shown. The angles between neighboring Mn moments vary from 0 to 180 with a step of 30. Correspondingly, the net magnetization vary from maximal to zero.

First of the two Se atoms, Se-I, is at position $`(\frac{a}{4},\frac{a}{4},\frac{a}{4})`$ and is the nearest neighbor of the Mn impurity situated at (0,0,0). The second atom, Se-II, is at position $`(\frac{3a}{4},\frac{3a}{4},\frac{5a}{4})`$ and belongs to the 4th coordination sphere of Se atoms. (To remind, the supercell in this case is a cube of the size $`2a`$.) The spin-projected DOS is presented with respect to two different quantization axes. The first (local) axis is parallel to the direction of the magnetic moment of the nearest Mn atom. The second (global) axis is directed along the net magnetization. The DOS projected on the local atomic quantization axis provides, in most cases, better insight into the physics of the system. However, in the experiments determining the spin-splittings the spin-quantization axis is usually the global one.

The DOS shown in Figs. 5,6 reveal strong difference between two Se atoms. The spin of the electron states of the Se-I atom follows almost perfectly the spin of the neighboring Mn atom (Fig. 5). This is evidenced by the negligibly small local spin-down DOS. The smallness of the local spin-down DOS holds up to the largest angle between Mn moments. Considered from the viewpoint of the global quantization axis, both spin-up and spin-down DOS of Se-I have similar shape but different weights (amplitudes). The relative weight of the spin-down DOS increases from zero for $`\theta =0^{}`$ to 1 for $`\theta =90^{}`$. Because of the similarity of the form of the global spin-up and spin-down DOS the variation of the DOS with the change of the net magnetization cannot be treated in terms of the varied spin-splitting. The changes in the global DOS take the form of the redistribution of the weight between the spin-up and spin-down DOS. This behavior is principally different from the behavior expected within the mean-field picture.

On the other hand, for Se-II we get a strong dependence of the local DOS on the magnetic configuration of the Mn moments (Fig. 6). With increasing angle between Mn moments the contribution of the spin-down DOS increases. This happens because the spin of the states of Se-II deviates increasingly from the spin of the nearest Mn atom responding to the influence of other Mn atoms. Now, the shape of the spin-up and spin-down DOS calculated with respect to the global quantization axis differ strongly. To characterize this difference in terms of the spin-splitting we calculated the centers of gravity for both spin-DOS in the energy region at the top of the valence band (Fig. 6).

In a good approximation the spin-splitting is proportional to the net magnetization (Fig. 8). Therefore the properties of the electron structure of Se-II can be described within the mean-field picture.

Since the relation between the exchange splitting and net magnetization varies from atom to atom, in experiments probing different parts of the electron structure this relation can appear different.

Important role in the experimental determination of the strength of the exchange interaction between the Mn moments and valence band states in DMS is played by the magneto-optical measurements of the spin splitting at the top of the valence band ($`\mathrm{\Gamma }`$ point of the Brillouin zone). furdyna  In Fig. 9 we show the calculated dependence of the splitting on Mn concentration. The LDA results for the exchange splitting at the $`\mathrm{\Gamma }`$ point disagree with experiment in two respects. First, the mean-field picture which assumes proportionality between the exchange splitting and the net magnetization in the system does not apply to the LDA results. The LDA-splitting is well described by a linear function with a finite value in the limit of $`x0`$. Such form of the dependence is the result of the presence of the Mn3d states at the Fermi level. Second, the exchange splitting is substantially larger than the splitting obtained experimentally. Since the LDA results cannot be described within the mean-field picture the use of the formula

$$J_{pd}=\frac{\mathrm{\Delta }E}{Sx}$$
(11)
gives values of the $`J_{pd}`$ parameter that depend on concentration $`x`$. For illustration, the value of $`J_{pd}`$ obtained for $`x=0.125`$ according to Eq. (11) is about two times larger than the experimental value. In Eq. (11), $`\mathrm{\Delta }E`$ is the exchange splitting and $`S`$ is the atomic spin moment of Mn.

#### III.1.2 LDA+U

Introducing of the Hubbard-U into calculational scheme results in a strong shift of the Mn3d spin-up states to lower energies (Fig. 10,11).

At the top of the valence band there is still an admixture of the Mn3d states. It is, however, very weak, especially for the spin-up states. Nevertheless, one can notice the hybridizational repulsion of the valence-band spin-down states from the spin-down Mn3d states lying in the semiconductor gap. This repulsion is an important factor leading, in agreement with experiment, to negative exchange splitting at the top of the valence band. Note that in the LDA calculation the negative exchange splitting has different origin: the presence of the spin-up Mn3d states at the top of the valence band.

To study the relation between net magnetization and exchange splitting we performed calculation for the antiferromagnetic configuration of the Mn moments for $`x=3.125\%`$ (Fig. 12).

In contrast to LDA (Fig. 4), no exchange splitting of the states at the top of the valence band is obtained in the antiferromagnetic case. This property is in agreement with the mean-field picture (Fig. 1). To investigate this property further we performed the LDA+U calculation of the exchange splitting at the $`\mathrm{\Gamma }`$ point of the BZ as a function of the Mn concentration $`x`$ (Fig. 9). The result obtained within the LDA+U scheme is in very good agreement with experiment concerning both the mean-field character of the dependence and the magnitude of the exchange parameter $`J_{pd}`$. Summarizing the study of the exchange interaction between Mn3d and valence band states we draw the conclusion that the LDA+U approach provides for this property much better agreement with experiment than the LDA approach.

### III.2 Interatomic exchange interactions

Now we turn to the discussion of the exchange interactions between Mn moments and address the question why large Mn moments and strong $`p`$-$`d`$ exchange do not result in the case of (ZnMn)Se with low Mn content in a sizable magnetic phase-transition temperature. To get deeper insight into formation of the interatomic exchange interactions in the system we performed calculations for different band occupations (Fig. 13). The number of electrons varied from $`n=2`$ (two electrons per supercell less) to $`n=0`$. Negative values of the Curie temperature in Fig. 13 indicate an instability of the ferromagnetic state due to dominating antiferromagnetic interactions. The calculations have been performed within both LDA and LDA+U approaches. In Fig. 14 we show, for $`x=3.125\%`$, the dependence of the main interatomic exchange parameters as a function of the valence-band occupation.

We begin with the discussion of the features common for both LDA and LDA+U calculations. Analysis of the calculated $`T_C^{MF}`$ ( Fig. 13) shows that in the case of completely filled valence band and empty conduction band ($`n=0`$) the main exchange interactions are antiferromagnetic. The antiferromagnetic character of the interaction agrees with the commonly excepted picture that the interatomic exchange interaction between magnetic atoms in an insulating system is dominated by the antiferromagnetic superexchange. This interaction is considered to be mediated by the states of the intermediate nonmagnetic atoms magnetism\_anderson  or the states of the completely filled bands. lahaeh

Remarkable, however, is very small value of the exchange interactions for $`n=0`$. With decreasing number of the holes the absolute value of all interatomic exchange interactions becomes very small. This result is in good correlation with the failure to experimentally detect the spin-ordering up to very low temperatures. furdyna  It is also in agreement with the perturbative calculation by Larsen et al for Cd<sub>1-x</sub>Mn<sub>x</sub>Te. lahaeh

The calculations show that the appearance of holes results in increasing ferromagnetic interactions. This is reflected by the property that the minimum of the estimated $`T_C`$ is at $`n=0`$ (Fig. 13) and correlates with experimental observation of the ferromagnetism with small Curie temperature in p-doped (ZnMn)Te. feciwa

Although both LDA and LDA+U give very weak negative exchange interactions for completely filled valence band the form of the dependence of the interatomic exchange parameters and correspondingly Curie temperature on the number of holes differs strongly for these two techniques (Figs. 13,14). Comparison of the calculated exchange parameters shows that the main difference between LDA and LDA+U concerns parameter $`J_{022}`$ that describes the exchange interaction between the Mn atoms separated by vector (022): the LDA predicts much stronger increase of the ferromagnetic interaction than LDA+U. The strength of the ferromagnetic interactions obtained within LDA seems to be strongly overestimated since the large values of the LDA-$`T_C`$ (Fig. 13) does not correlate with the experimental data available. On this basis, we draw the conclusion that the LDA+U scheme gives better description of the character of the dependence of the interatomic exchange interactions on the number of holes.

This last conclusion might seem to be expected since in Sec. III.1 we have seen that the value of the $`J_{pd}`$ parameter playing an important role in the mediation of the ferromagnetism is overestimated by LDA. The situation is, however, more complex since a larger $`J_{pd}`$ parameter is accompanied, in the case of LDA, by a stronger spatial localization of the valence-band hole states about the Mn atom. Increased localization of the holes produces the trend to decreasing $`T_C`$. Which of two factors, $`J_{pd}`$ or hole-localization, prevails depends on the peculiar interplay of the details of the electron structure of the specific system studied. The calculations for various III-V DMS show that the account for Hubbard-U can lead to both increase and decrease of the Curie temperature. sandratskii\_unpubl

To complete the consideration of the exchange interactions in (ZnMn)Se we discuss the physical reason for a very weak interatomic exchange interactions for undoped (ZnMn)Se ($`n=0`$ in Fig. 13). To remind, this result is common for both LDA and LDA+U and is very important for understanding of the failure to experimentally detect any magnetic phase transition up to very low temperatures. Note, that the behavior of the II-VI DMS is different from that obtained for the III-V DMS (GaMn)As. In (GaMn)As, the same calculational scheme gives sabr\_condmat  for the completely filled valence band and $`x=3.125\%`$ interatomic antiferromagnetic interactions that are about 20 times larger that in (ZnMn)Se (Fig. 13).

To understand the weakness of the calculated superexchange in (ZnMn)Se and the difference between (ZnMn)Se and (GaMn)As we invoke a tight-binding model of noncollinear magnetic configurations. We consider helical configurations of the atomic moments and study the dependence of the band energy of the system on magnetic structure. The helical structures are defined by the formula

$$𝐞_n=(\mathrm{cos}(𝐪𝐑_n)\mathrm{sin}\theta ,\mathrm{sin}(𝐪𝐑_n)\mathrm{sin}\theta ,\mathrm{cos}\theta )$$
(12)
where $`𝐑_n`$ are the lattice vectors, $`𝐪`$ is the wave vector of the helix, $`𝐞_n`$ is the unit vectors in the direction of the magnetic moment at site $`𝐑_n`$, polar angle $`\theta `$ gives the deviation of the moments from the $`z`$ axis. The helical structures allow to describe broad range of magnetic configurations from collinear ferromagnetism ($`\theta =0`$ or $`𝐪=\mathrm{𝟎}`$) to collinear antiferromagnetism ($`𝐪=\frac{1}{2}𝐊`$ and $`\theta =90^{}`$, $`𝐊`$ is a reciprocal lattice vector).

The tight binding method for spiral structures was discussed in its general form in Ref. sand86 . By neglecting the difference in the spatial dependence of the basis functions with opposite spin projections and by preserving only the single-center matrix elements of the exchange potential we arrive at the following simple form of the secular matrix $`H(𝐤)`$ sakuv :

$$H(𝐤)=\left(\begin{array}{cc}\mathrm{cos}^2\frac{\theta }{2}H_{}+\mathrm{sin}^2\frac{\theta }{2}H_+\frac{1}{2}\mathrm{\Delta }& \frac{1}{2}\mathrm{sin}\theta (H_{}H_+)\\ \frac{1}{2}\mathrm{sin}\theta (H_{}H_+)& \mathrm{sin}^2\frac{\theta }{2}H_{}+\mathrm{cos}^2\frac{\theta }{2}H_++\frac{1}{2}\mathrm{\Delta }\end{array}\right)$$
(13)
where $`H_{}=H_{}(𝐤\frac{1}{2}𝐪)`$, $`H_+=H_{}(𝐤+\frac{1}{2}𝐪)`$, and matrix $`H_{}(𝐤)`$ describes spin-degenerate bands of a non-magnetic crystal; $`\mathrm{\Delta }`$ is the diagonal matrix of the on-site exchange splittings. In LDA+U scheme $`\mathrm{\Delta }`$ includes also $`\frac{U}{2}`$. Secular matrix (13) describes a many-band system and takes into account the hybridization between the states of different atoms. Through the hybridization between the Mn states and the states of the semiconductor matrix the spin polarization is transmitted to the nonmagnetic atoms. Note, that in contrast to the two-band model used in Ref. sabr\_condmat  the matrix (13) includes all relevant bands. In particular the Mn3d states are assumed to be included. This makes model (13) conceptually similar to our ASW calculations.

The property of the secular matrix (13) that is important for us reads

$$_{\mathrm{BZ}}𝑑𝐤Sp[H(𝐤)]=2_{\mathrm{BZ}}𝑑𝐤H_{}(𝐤)$$
(14)
that is the trace of the matrix $`H(𝐤)`$ does not depend on the magnetic configuration. The variation of the magnetic structure changes the energy of individual electron states. The changes of different states, however, compensate. In the case the trace of the secular matrix represents the total energy of the system the invariance with respect to the magnetic configuration means that all effective interatomic exchange interactions are negligible.

The property given by Eq. (14) applies to the total energy of a system if all bands described by the tight-binding secular matrix (13) are occupied. This condition can be fulfilled only in the case that the hybridization between the occupied and empty states is weak and can be neglected. The weakness of the hybridization allows to include into the secular matrix the occupied states only.

An attempt to use Eq. (14) for the explanation of the weakness of the superexchange in (ZnMn)Se leads immediately to the following difficulty. According to Eq. (13) both spin-up and spin-down Mn 3d states must be included into the secular matrix to fulfill Eq. (14). Since only the spin-up Mn 3d states are occupied, the inclusion of the spin-down Mn 3d states, apparently, does not allow to relate the trace of the matrix to the energy of the system. In the case of (ZnMn)Se this difficulty can, however, be overcome if we notice that the spin-down Mn 3d states form very narrow energy bands lying in the semiconducting gap of ZnSe (Figs. 2,10). For example, the estimation for the LDA case shows that the states of these bands are strongly localized about the Mn atoms: more than 76% is located in the Mn spheres and more than 88% within the first coordination sphere of the Zn atoms. These states can be treated as evanescent states that are unable to mediate efficiently the exchange interaction between Mn atoms (Fig. 13). The evanescent character of the empty Mn 3d states allows to approximately consider their contribution into the trace of the secular matrix \[Eq. (14)\] as being independent of the magnetic configuration. This has as a consequence that the contribution of the occupied states is also approximately independent of the magnetic configuration resulting in weak effective interatomic exchange interactions.

This consideration allows us to also explain the difference between DMS on the GaAs and ZnSe bases. The semiconducting energy gap is substantially larger in the case of ZnSe. In the case of GaAs the influence of empty states is stronger and they must be included into the secular matrix (13). Therefore, the property described by Eq. (14) does not apply to the occupied states that results in stronger superexchange.

Some further comments are worth making here. First, the relation between the value of the semiconducting gap and the spatial extent of the exchange interactions has been many times discussed in the scientific literature within the framework of the perturbative treatment involving virtual transitions between the occupied states of the valence band and empty states of the conduction band (see. e.g., Ref. blro  for an early publication on this topic. See also an interesting comment on the relation between the range of the exchange interaction and an imaginary Fermi vector in recent paper by Pajda et al pakutu ). The model considered above captures basically the same physics by taking into account, in a non-perturbative manner, the hybridization between occupied and empty states. Only in the case the contribution of this hybridization into the response of the valence band states on the change of magnetic configuration is small the interatomic exchange interactions are weak. An important feature of model (13) is that it reflects the properties of the non-perturbative technique we used in the calculation of the exchange interactions and, therefore, provides additional understanding of the calculational results.

## IV Conclusions

One of the remarkable properties of the II-VI diluted magnetic semiconductor (ZnMn)Se is the giant spin splitting of the valence band states under application of the magnetic field (giant Zeeman splitting). This splitting reveals strong exchange interaction between Mn moments and semiconductor states. On the other hand, no magnetic phase transition has been observed for systems with small Mn content up to very low temperatures. The latter property shows weakness of the exchange interaction between Mn moments. In this paper, the local density approximation (LDA) and the LDA+U techniques are employed to study exchange interactions in (ZnMn)Se. Supercell and frozen-magnon approaches applied earlier to III-V diluted magnetic semiconductors are used. It is found that both LDA and LDA+U describe successfully the combination of the strong Zeeman splitting and weak interatomic exchange. However, the physical pictures provided by two techniques differ strongly. A detailed analysis shows that LDA+U method provides the description of the system which is much closer to the experimental data.

###### Acknowledgements.

The author profited much from the discussions with Patrick Bruno and Tomasz Dietl. The financial support of Bundesministerium für Bildung und Forschung is acknowledged.


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# New abundances of planetary nebulae in the Galactic BulgeBased on observations made at the European Southern Observatory (Chile) and Laboratório Nacional de Astrofísica (Brasil)

## 1 Introduction

In the past few years, many papers have been published dealing with the kinematics and abundances of the galactic bulge. Most of these works on bulge abundances are concerned with heavy elements produced by supernovae, so that light elements such as helium and nitrogen have had a smaller share of attention.

Planetary nebulae (PN) constitute an important tool in the study of the chemical evolution of the bulge, providing accurate determinations of the abundances of light elements produced by progenitor stars of different masses. In fact, PN offer the possibility of studying both light elements produced in low mass stars, such as He and N, and also heavier elements which result from the nucleosynthesis of large mass stars, such as oxygen, sulfur and neon, which are present in the interstellar medium at the stellar progenitor formation epoch.

Previous determinations of chemical abundances of bulge PN have shown that, on average, these objects have abundances similar to disk planetary nebulae (Escudero & Costa 2001, Liu et al. 2001, Cuisinier et al. 2000, Costa & Maciel 1999, Ratag et al. 1997). However, the total number of bulge PN with accurate abundances is still small; furthermore, a correlation between the chemical abundances and bulge kinematics is still to be determined, in contrast with the observed properties of the galactic disk.

In the present paper, we report new observations and derive chemical abundances for a sample of 57 bulge PN. These results are compared with previous data from our own group and other groups as well, both regarding the galactic bulge and other galactic systems, such as the galactic disk and halo.

In section 2 we present our new observations for a sample of bulge PN and comment on the reduction procedure. In section 3 we present our method to derive the chemical abundances. A discussion of the main uncertainties of the physical parameters is given in section 4. A comparison of our results with published data is given in section 5, and in section 6 we discuss our results an present our main conclusions.

## 2 Observations and data reduction

### 2.1 Observations

In this work we present results for 57 new PNe, extending and completing a previous paper (Escudero & Costa 2001), in which we have presented our results for a sample of 45 objects toward the galactic bulge.

The objects were selected according to their distances, taken from the literature (Schneider & Buckley 1996, van de Steene & Zijlstra 1995 and Zhang 1995), adopting as probable bulge objects those with heliocentric distances greater than 5 kpc. In spite of the sometimes larger uncertainties for these distances, this is still the best homogeneous criterion to define the sample. Other criteria like diameters, H$`\beta `$ or radio fluxes are even less reliable. It should be noted that in this paper we did not use the same criterion used by Escudero & Costa (2001), where all objects towards the bulge from Beaulieu et al. (1999) and Kohoutek (1994) were observed. These objects do not have distance determinations, but as most of them have diameters smaller than 20”, they should be at or near the bulge according to the criteria of Gathier et al. (1983).

Adopted distances are listed in table 3. We divided our sample in two samples: those with heliocentric distances greater than 5 kpc (Sample 1), and those with heliocentric distancies smaller than 5 kpc or unknown (Sample 2). Figure 1 displays the distance distribution for our Sample 1 objects, combined with objects chosen from the literature (see section 5 for detailed references). Adopting these distances and the criteria mentioned above we would expect some 80 % of the sample to be in the galactic bulge, a fraction similar to the estimates given by Pottasch (1990), to which the reader is refered for a detailed discussion on the characterization of galactic bulge PN.

The program objects were observed with two telescopes: 1.60m LNA (Laboratório Nacional de Astrofísica, Brasópolis - Brasil), and 1.52m ESO (European Southern Observatory). Each object was observed at least twice in order to secure good final spectra. We selected the exposure time for each object in order to have a good S/N in the region of the H$`\gamma `$ line, due to the importance of the \[OIII\]$`\lambda `$4363 line in the temperature diagnostics.

For all objects, we used the long slit of 2 arcsecs width. At LNA we used a 300 l/mm grid with 4.4 A/pix dispersion, and at ESO the used grid was 600 l/mm with 2.4 A/pix dispersion. Each night at least three spectrophotometric standard stars were observed to improve the flux calibration.

Table 1 list the PN G designation (first column), the usual names of the observed objects (column 2), equatorial coordinates for epoch 2000 (columns 3 and 4), date of observation (column 5), observatory (column 6) and the exposure time in seconds (last column). For some objects, spectra were taken with different exposure times: a short exposure to measure the Balmer series lines (and therefore to derive interstellar extinction), and a longer exposure (usually with H$`\alpha `$ saturated) to measure the fluxes of lower intensity lines.

Table 2 (available electronically) display the line fluxes of the reddened lines. For the cases where the line blend \[OII\]$`\lambda \lambda `$7319,7330 was impossible do separate, their intensities are added in the \[OII\]$`\lambda `$7319 column.

Figure 2 shows typical spectra from our sample. The upper panel shows M 3-26, an object with well defined lines, and the other shows KFL 4, a poorer object, observed with lower resolution.

### 2.2 Interstellar Extinction

The application of the extinction curve of Fitzpatrick (1999) had better results than the use of the curve of Cardelli et al. (1989) (CCM), when we compared the predicted H$`\gamma `$/H$`\beta `$=0.47, (adopting Osterbrock’s case B) with the calculated values after interstellar extinction correction. A small difference between the two curves in the H$`\gamma `$ and H$`\alpha `$ regions (see fig. 6 of Fitzpatrick 1999) results in a significant discrepancy with respect to the recombination values when we use the CCM curve. Using the Fitzpatrick (1999) curve this difference is considerably reduced. These results are displayed in figure 3, where both distributions are plotted. Is easy to see that the distribution of H$`\gamma `$/H$`\beta `$ ratios calculated with the Fitzpatrick curve is narrower and that its center is closer to the theoretical value of 0.47.

In order to bring the value of H$`\gamma `$ closer to the recombination value using the CCM curve, it would be necessary to use a value of the ratio of total to selective absorption RV higher than 6.0, which is extremely large and inconsistent with the value determined by Stasińska et al. (1992). The main consequence for the poor interstellar correction in the H$`\gamma `$ region is the poor determination of the electron temperature for O++. High O\[III\]$`\lambda `$4363 values would result in overestimated temperatures and low abundance values, as shown by other authors (Köppen et al. 1991, Stasińska et al. 1998) who expected that some of the objects lacking O\[III\]$`\lambda `$4363 might be the most metal rich.

In this work we have used the Fitzpatrick (1999) extinction curve, deriving E(B-V) from the observed Balmer ratio H$`\alpha `$/H$`\beta `$ and adopting the theoretical value H$`\alpha `$/H$`\beta `$ = 2.85, with RV = 3.1.

Figure 4 displays the distribution of E(B-V) derived for Sample 1 (see section 2.1) compared with data from the literature and from Escudero & Costa (2001). It can be seen that the distribution for the present data agrees well with our previous work, and is in reasonable agreement with data from the literature, which are on average nearer the galactic center.

## 3 Determination of chemical abundances

### 3.1 Physical parameters

The quality of the physical parameters is crucial for a good derivation of chemical abundances, as line emissivities of the ions are extremely sensitive to the electron temperature and density of the nebulae.

For the determination of electron temperatures we used the following line ratios for oxygen and nitrogen: \[OIII\]$`\lambda \lambda `$4363,5007 and \[NII\]$`\lambda \lambda `$5755,6584, from which we can obtain estimates of the electron temperature for high and low ionization regions. The electron density was derived from the sulfur line ratio \[SII\]$`\lambda \lambda `$6716,6731, giving therefore an average value for the whole nebula. Excitation classes were also defined for the object following the Webster (1988) criterium. For each nebula the H$`\beta `$ surface flux was calculated using the derived H$`\beta `$ flux and the fraction of the nebula within the slit.

In table 3 we give the observed (column 2) H$`\beta `$ intensities and corrected by interstellar extinction (in erg cm-2 s-1) (column 3), diameters in arcsecs from Acker et al. (1991) (column 4), H$`\beta `$ surface flux (in erg cm-2 s-1 arcsec-2), the interstellar extinction E(B-V) (column 6), the electron density in 103cm-3 (column 7), the electron temperatures in 104 K (columns 8 and 9), excitation class (column 10) and heliocentric distances in kpc (column 11).

### 3.2 Ionic abundances

In order to calculate abundances for the ions N+, O0, O+, O++, S+, S++, Ar++, Ne++, we have used the fits by Alexander & Balick (1997) that show a good agreement with ionic abundances obtained from statistical balance equations. For the helium ions (He+, He++) we used the recombination coefficients from Péquignot et al. (1991), with the coefficients for He+ collisional excitation correction derived by Kingdon & Ferland (1995). Only for Cl++, not present in the Alexander & Balick (1997) tables, we used the statistical balance equation for the \[ClIII\]$`\lambda \lambda `$5518+5538 lines.

In particular, the O+ abundance can be derived from two pairs of lines: $`\lambda `$3727+29 and $`\lambda `$7319+30. There is however a systematic difference between the resulting values, with some tendency to higher abundances for the red pair. These differences are shown in figure 2. In this figure, the dashed line is a linear fit for our sample. To explain this difference, observed also by other authors, we raised four alternatives: interstellar extinction, data reduction, electron temperature and density variations, and O++ recombination.

\- Interstellar Extinction: one of the factors that could cause this difference is a poor interstellar extinction correction. To check this, we corrected all spectra with two interstellar extinction laws (Fitzpatrick 1999 and CCM 1989) using two extreme values for RV: 2.1 e 5.9. The results do not imply a significant variation of the O++ abundance in any case. The only possibility to invoke extinction to explain such a difference would be a new, totally distinct interstellar extinction law, which seems unrealistic, since most of the extinction comes from the disk

\- Data reduction: as the two line pairs are in opposite regions of the spectrum, poor flux calibration could affect the final data. However, it is unlikely that this effect could affect all data. Furthermore, this effect appears also in other, independent works (Stasińska et al. 1998).

\- Temperature and density variations: this can be an important factor in abundance calculations (Viegas & Clegg 1994). Regions with high density in the inner part of a planetary nebula contribute to the intensity of $`\lambda `$7319+30, but not to $`\lambda `$3727 (Mathis et al. 1998). With respect to the density, as the intensity of the \[SII\] line relative to H$`\beta `$ depends on the density (Alexader & Balick 1997), this value will represent preferentially lower density regions, and this effect would be more evident for bulge objects due to their smaller angular sizes. For disk objects, the slit would cover only the central part of a planetary nebula and the effect is not as important as for bulge nebulae.

\- Recombination of O++: For nebulae with low density and electron temperature, dielectronic recombination of O++ may play an important role (Rubin 1986, Aller & Keyes 1987), leading to differences in the derived ionic abundances.

Figure 5 displays a comparison between the O+ ionic abundance derived from the blue (3726+29) and the red (7320+30)lines, both for our sample and that from Stasinska et al. (1998). In the figure, the continuous line is a y=x plot and the dashed line is a linear fit for all the points. As can be seen, there is a small discrepacy between both determinations, with a tendency for higher abundances when the red lines are used. The same effect appears for both samples. As the final explanation is still an open issue, we adopted the blue pair to derive the O+ abundance like most of the other works in the literature:

$$log(\mathrm{O}_{3727}^+/\mathrm{H}^+)=(0.1\pm 0.3)+(1.06\pm 0.08)\mathrm{log}(\mathrm{O}_{7325}^+/\mathrm{H}^+)$$

The derivation of sulfur abundance requires both S+ and S++ ions. For those objects where S++ was not available we adopted the same technique used by Kingsburgh & Barlow (1994), deriving the S++ abundance from the relation between ratios S++/S+ and O++/O+. This relation was derived from our data, as can be seen in figure 6. In the figure, filled and open circles represent the points included in the fit, and crosses are abundances poorly determined, which were not included. The dotted line is a y=x relation and the continuous line is the best fit represented by the relation:

$$log(\mathrm{S}^{++}/\mathrm{S}^+)=(0.21\pm 0.08)+(0.73\pm 0.06)\mathrm{log}(\mathrm{O}^{++}/\mathrm{O}^+)$$

### 3.3 Elemental abundances

The final abundances are listed in table 4. The objects separated by an horizontal line in the final of table 4 and also in table 3 are those from our Sample 2 (see section 2.1). In the discussion on the abundance distribution (see section 5) we do not include these objects.

Since it is not possible to get the chemical abundances of all ions of a given element, we use the ICF method (Ionization Corrections Factors) to derive the elemental abundances, as in our previous works. For details, see Escudero & Costa (2001), Costa et al. (1996) and references therein.

The adopted ICF for oxygen and nitrogen are those suggested by Peimbert & Torres-Peimbert (1977); for sulfur and neon we used the ICF provided by Kingsburgh & Barlow (1994), except for those objects for which S++ is not available; in this case we adopted the value derived by the relation given in the last section. For argon we used the ICF provided by Freitas Pacheco et al. (1993). These ICFs are listed below.

$$\frac{\mathrm{He}}{\mathrm{H}}=\frac{\mathrm{He}^+}{\mathrm{H}^+}+\frac{\mathrm{He}^{++}}{\mathrm{H}^+}$$

$$\frac{\mathrm{O}}{\mathrm{H}}=(\frac{\mathrm{O}^{++}}{\mathrm{H}^+}+\frac{\mathrm{O}^+}{\mathrm{H}^+})\frac{\mathrm{He}}{\mathrm{He}^+}$$

$$\frac{\mathrm{N}}{\mathrm{H}}=\frac{\mathrm{N}^+}{\mathrm{H}^+}\frac{\mathrm{O}}{\mathrm{O}^+}$$

$$\frac{\mathrm{S}}{\mathrm{H}}=(\frac{\mathrm{S}^+}{\mathrm{H}^+}+\frac{\mathrm{S}^{++}}{\mathrm{H}^+})(1(1\frac{\mathrm{O}^+}{\mathrm{O}})^3)^{1/3}$$

$$\frac{\mathrm{Ar}}{\mathrm{H}}=1.34\frac{\mathrm{Ar}^{++}}{\mathrm{H}^+}\frac{\mathrm{O}}{\mathrm{O}^{++}}$$

$$\frac{\mathrm{Ne}}{\mathrm{H}}=\frac{\mathrm{Ne}^{++}}{\mathrm{H}^+}\frac{\mathrm{O}}{\mathrm{O}^{++}}$$

## 4 Errors in the physical parameters and chemical abundances

In Escudero & Costa (2001) typical errors were derived through a Monte Carlo simulation, based on the line intensities and their errors, which requires the same exposure time for all measurements. This is not the case for the present work, so we examined the effect of these uncertainties on the abundances.

From Escudero & Costa (2001), we have estimated average errors to the abundances of 0.023, 0.18, 0.17, 0.24 and 0.19, respectively for He, N, O, S and Ar. However, it should be remembered that errors are highly affected by interstellar extinction, in the sense that objects that have higher extinction should have greater errors in the abundances, on the average, depending also on the exposition time and the size of the telescope. Therefore, abundances of bulge objects, that have high extinction, typically have higher errors than disk objects, so that we can estimate the uncertainties in the abundances of bulge nebulae to be roughly 0.2 dex, apart from He/H.

### 4.1 Physical parameters

One of the main error sources in the chemical abundances are the uncertainties in electron temperatures and densities, as discussed previously. Low S/N in weaker diagnostic lines, as well as internal variations in the physical parameters certainly affect the final abundances. As discussed in section 3.2, electron densities derived from \[SII\] can be underestimated since the emissivity of this line depends on density.

### 4.2 Helium

The main factors that affect the helium abundance are the uncertainties in densities and electron temperatures. Depending on these parameters, the correction due to collisional excitation can reach 50%. Therefore, errors in the physical parameters would considerably affect the chemical abundances. The existence of neutral helium would also have an influence on the derived abundances. This was tested on the basis of the criterion proposed by Torres-Peimbert & Peimbert (1977), according to which objects with log O+/O $`>`$ -0.4 seem to have a substantial contribution of neutral helium. For this sample, 11 objects fit this criterion, indicating that their derived helium abundance should be taken cautiously.

### 4.3 Abundances from collisionally excited lines

In addition to observational errors and those resulting from the inhomogeneity of the nebulae, the use of ionization correction factors (ICF) to estimate elemental abundances for the elements with collisionally excited lines will include additional error sources.

For nitrogen, O+ is used as ICF, and small variations in its abundance will affect the nitrogen abundance. The use of O$`{}_{3727}{}^{}{}_{}{}^{+}`$ or O$`{}_{7325}{}^{}{}_{}{}^{+}`$ ionic abundances will imply differences of 0.0 to 0.7 dex in the nitrogen abundance.

The same effect occurs for sulfur, in whose ICF O+ is also present. Two observational effects affect the sulfur abundance: the dependence of S+ emissivity with density, and the weak intensity of the line \[SIII\]$`\lambda 6312`$, which will result in a poor determination of the S++ abundance. Therefore, the present sulfur abundances should be taken cautiously.

For oxygen, argon and neon, whose lines are normally intense in planetary nebulae, the main error sources are the uncertainties in the physical parameters.

## 5 Data from the literature

To compare our data, we collected objects from 5 recent works in the literature: Stasińska et al. (1998), Cuisinier et al. (2000), Cuisinier et al. (1996), Samland et al. (1992) and Köppen et al. (1991). We use only those objects with distances already determined (Schneider & Buckley 1996, van de Steene & Zijlstra 1995 and Zhang 1995), and with heliocentric distances greater than 5 kpc.

In figure 7 we show the distribution of chemical abundances of He, N and O from the literature and our data.

The results from the first paper of this series are also shown (solid irregular lines). In order to homogenize the results, we rederived the elemental abundances for those data, using the same ionic abundances but adopting the improvements used here: sulfur ICF from Kingsburgh & Barlow (1994); O+ abundance derived preferentially from the blue doublet, and S++ derived acording the procedure described in section 3.2, when necessary.

These results have been obtained using the same instruments and procedures as in the present paper, so that both samples are expected to present a large degree of homogeneity. This fact can be observed in fig. 7, as the abundance distributions of both samples are similar. Small differences observed at the low end of the He and N abundances can be attributed to the incompleteness of the samples. It can be seen that our abundances show a good similarity to all other data. The nitrogen abundances, that reflect the progenitor mass, show a little more scattering from our objects than the data from literature. This was expected to occur because our objects are more widely distributed in angular position than the literature objects (see Escudero & Costa 2001).

## 6 Discussion and conclusions

Our results are in agreement with those from other works (see for example Escudero & Costa 2001, Cuisinier et al. 2000), indicating that bulge PNe have mean abundances similar to those from disk objects, however displaying higher dispersion.

Figure 8 displays the relation between excitation classes and helium abundances (panel a) and oxygen abundances (panel b). The data distribution in panel (a) shows no correlation between the helium abundances and the excitation class; the only exception is that some objects with very low abundances are preferably associated with the lowest excitation classes, which possibly indicates the presence of neutral helium for these objects. On the other hand, the absence of correlation in panel (b) also indicates that our abundance analysis is unbiased with respect to the excitation of the nebulae.

Figure 9 displays several abundance correlations for our sample which are distance independent, combined with data from Escudero & Costa (2001) and the literature.

Oxygen and nitrogen are two key elements for the diagnostics of PNe. Due to strong lines, oxygen abundances are normally very well determined, giving the abundance of the interstellar medium at the progenitor formation epoch. It was already noted that more massive, younger objects like type-I PNe progenitors have oxygen abundance lower than the Sun or type-IIa PNe progenitors (see Costa et al. 1996). The same effect appears in stellar evolution yields (van den Hoek & Groenewegen 1997, Marigo 2001), however for the majority of the lower mass stars, oxygen remains unchanged and can be used to trace the chemical evolution of the interstellar medium.

Nitrogen, on the other hand, has two possible origins: it reflects the abundance of the interstellar medium at the progenitor formation epoch, combined with the material produced by nucleosynthesis during the evolution of the PN progenitor star. Typical yields as a function of the stellar mass are given by van den Hoek & Groenewegen (1997) and Marigo (2001).

Examining the O vs. N diagram displayed in fig. 9a, a positive correlation between O/H and N/H can be observed. As for the correlation between log(N/O) and O/H (figure 9b), this is less evident. We can see that objects with high N/O can have higher or lower oxygen abundances. Those with higher oxygen abundances are similar to the disk type-I PNe, while those with lower abundances are similar to halo objects. On the other hand, objects with low N/O are usually oxygen-rich, which is consistent with the correlation shown in fig. 9a. Some of these objects may be type-III PNe in the inner disk (see also Maciel 1999) and with the abundances of metal rich bulge giants (Rich 1988). This dispersion in the abundances suggests that the chemical evolution of the bulge cannot be explained in a single formation scenario, so that a composite scenario is required instead.

Another important diagram for the diagnostics of PNe abundances is He x log(N/O), which reflects the chemical enrichment during the stellar evolution of the progenitor. From figure 9c it can be seen that there is a reasonably well defined correlation between He/H and log(N/O), in the sense that helium-rich nebulae are are usually also nitrogen rich, which probably reflects an increasing progenitor mass. A small group of objects apparently have very low He abundances, while their N abundances are normal. This can be explained either by the fact that their progenitor star had smaller masses, which characterizes them as type IIa nebulae, or their He abundances may have been underestimated owing to the presence of neutral helium.

Figures 9d, 9e and 9f display the correlation between the alpha-elements; as they are produced mainly in type II supernovae their correlation reflects the chemical evolution of the interstellar medium from which the progenitor stars are formed. From these figures one can see that lower oxygen abundances imply also lower sulfur, argon and neon abundances.

###### Acknowledgements.

We thank E.L. Fitzpatrick for providing his extintion curves. We thank also A. Acker, referee of this work, for her comments and suggestions. This work was partly supported by the Brazilian agencies *FAPESP* and *CNPq*. A.V.E. acknowledges *FAPESP* for his graduate fellowship (Process 00/12609-0). Observations at ESO/Chile were possible through the *FAPESP* grant 98/10138-8.


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# Comparing Chemical Abundances of the Damped Ly𝛼 Systems and Metal-Poor Stars

## 1. Introduction

I wish to first acknowledge the wisdom of the organizers for bringing the damped Ly$`\alpha `$ and metal-poor stellar abundance communities together in a Joint Discussion aimed at heightening communication and collaboration between the two fields. While previous conferences on chemical abundances have included members of each group, talks were generally organized such that we have talked to one another instead of with one another. From the perspective of a DLA researcher, the proceeding 50 years of stellar abundance research is invaluable to drawing interpretations on nucleosynthesis from DLA observations. I suspect that as DLA abundance studies become a mature field, the stellar community will similarly gain from observations of these young, metal-poor galaxies.

The organizers charged me with reviewing the fields to open the JD. In Sydney, I briefly compared the observations, techniques of analysis, and major systematic uncertainties in each field. I then described a few areas of research where the fields clearly intersect and where a joint analysis impacts theories of chemical evolution, nucleosynthesis, and galaxy formation. In this proceeding I present an even more brief summary.

## 2. Observations and Analysis

Presently, the data for damped Ly$`\alpha `$ and metal-poor stellar abundance research is acquired with the same telescopes on the same instruments and with comparable spectral resolution. Ionic transitions are analysed in a similar fashion: integrated equivalent widths or column densities are derived from isolated, ’clean’ lines while spectra synthesis or line-profile fitting techniques are applied to blended and crowded regions. The derivation of elemental abundances from the ionic measurements, however, follows different paths. For stellar abundances, one introduces a stellar atmosphere derived from the spectroscopic and/or photometric observations of the star. The atmosphere is typically parameterized by three parameters – temperature, gravity, and microturbulence – and one solves the radiative transfer equations to predict equivalent widths and/or spectral profiles. The uncertainties attributed to this modeling (e.g. non-LTE corrections; see Apslund’s contribution) generally dominate the statistical errors associated with the observations.

With the DLA systems, one must consider ionization corrections to convert the measured ionic column densities into elemental abundances. In practice, the corrections are generally assumed to be small. This assumption is supported by theory and observation, although with exception (see Vladilo et al. 2001; Prochaska et al. 2002). The most important systematic error in the DLA analysis is dust depletion; the DLA observations provide gas-phase abundances which may significantly underestimate the true abundances of refractory elements like Fe, Cr, and Ni which deplete from the gas-phase onto dust grains (e.g. Jenkins 1987). This effect dominates the uncertainty of DLA abundance studies and plays a central role in nearly all interpretation drawn from the observations.

## 3. Age-Metallicity Relation (AMR)

One research area where the two fields nicely complement each other is in describing an age-metallicity relation (AMR). Stellar research has focused primarily on Galactic disk stars and therefore probes the chemical enrichment history of a single galaxy over the past $`10`$ Gyr. Because of the uncertainties of isochrone fitting, it is difficult to determine absolute ages with meaningful precision for ages $`>10`$ Gyr. In contrast, the DLA observations reveal the AMR of the population of high $`z`$ galaxies which dominate the H I content of the universe. Therefore, the DLA trace the ‘cosmic’ mean metallicity in neutral gas (e.g. Prochaska et al. 2003). The ages of the DLA systems are precisely calculated by combining their cosmological redshift with the ‘concordance cosmology’ (e.g. Spergel et al. 2003). The challenge with DLA studies is pursuing the AMR to $`z<1.7`$ because space-bourne UV observations are required to observe the Ly$`\alpha `$ profile. Therefore, the DLA and stellar abundance measurements complement one another both temporally (spanning nearly the entire history of the universe) and spatially (examining a single galaxy to a population of galaxies).

For very different reasons, the AMR’s measured from Galactic stars and the DLA systems have had controversial histories. Indeed, my own studies have contributed to the controversy surrounding the AMR derived for the DLA systems (see also Kulkarni, this proceedings). In this case, the analysis has been limited by uncertainty relating to small sample size; even with 50 DLA systems there was no statistically significant evolution in the cosmic metallicity. Similarly, the AMR of the Galactic disk remains a point of great debate with competing groups arguing for and against any trend of metallicity with age (Edvardsson et al. 1993; Rocha-Pinto et al. 2000; Feltzing, Holmberg, & Hurley 2001; Ibukiyama & Arimoto 2002). It remains unclear to me whether the debate revolves around sample bias or age determinations.

These uncertainties aside, it is illustrative to compare AMR’s taken from the two fields of research. In Figure 1, I present a census of DLA age-metallicity observations overplotted with one estimate of the Galactic AMR (Rocha-Pinto et al. 2000) and rough estimates for the age and metallicity of the Galactic bulge, thick disk, and halo stellar components. Clearly, the DLA systems at $`z>2`$ are distinct in both metallicity and age from the Galactic disk AMR. As first noted by Pettini et al. (1997), the majority of DLA metallicities lie between the peaks of the distributions for the thick disk and halo populations. This indicates the majority of gas associated with the DLA systems at $`z>2`$ may feed the formation of the thick disk and halo populations but has insufficient metallicity at these epochs to produce the majority of disk stars.

As the AMR’s are refined and extended to include additional stellar populations and local galaxies as well DLA systems at $`z<1`$, one will gain further insight into the nature of the DLA systems and their connection to modern galaxies. Future surveys will reveal whether a sample of metal-rich DLA exist at $`z1.5`$ which can be identified as the gas reservoirs of spiral disk formation. The identification of this gas is an important aspect of tracing the history of disk formation. In addition, age-metallicity measurements for high $`z`$ galaxies (e.g. LBG, ERO’s) will allow comparisons with the DLA and stellar populations, illuminating the processes of galaxy enrichment during the early universe.

## 4. DLA systems, dwarf galaxies, and the Galactic halo

One of the most exciting aspects of connecting the fields of DLA and stellar abundance research is to draw comparisons between abundance patterns of local stellar populations and those observed in the early universe. Indeed, this was the focus of several talks and posters of this JD (e.g. Tolstoy, Bonifacacio, Dessauges-Zavadsky). A principal challenge to drawing such comparisons is uncertainty in the DLA abundance patterns related to differential depletion. This point is well illustrated by Figure 2 where I present gas-phase Si/Fe ratios against metallicity for a sample of 56 DLA systems with echelle observations. As noted by Prochaska & Wolfe (2002), the metal-poor DLA systems exhibit \[Si/Fe\] values comparable to the Galactic halo with remarkably small scatter (particularly given that each data point represents a unique galaxy with its own specific chemical enrichment history). This Si/Fe plateau suggests the metal-poor DLA systems have been predominantly enriched by Type II supernovae, perhaps in the same manner as the Galactic halo. At higher metallicity, however, the Si/Fe ratios increase, in contradiction with any empirical or theoretical trends of chemical evolution. The rise in Si/Fe is explained by differential depletion; higher metallicity DLA systems have significant dust-to-gas ratios and a substantial fraction of their Fe is locked into dust grains. If one explains the rising Si/Fe ratios in terms of differential depletion, it raises the possibility that the enhancement of Si/Fe at all metallicity is dominated by differential depletion. Presumably, this interpretation would require an uncomfortable degree of fine-tuning to reproduce a \[Si/Fe\] plateau at \[Si/H\] $`<1`$ which matches the nucleosynthetic enhancement of Si/Fe observed for the Galactic halo, yet more peculiar coincidences exist.

Presently, the majority of both communities favor imposing significant depletion corrections to the observed DLA abundances (e.g. Vladilo 2002). To estimate the corrections, one must assume the intrinsic value for the relative abundance of a refractory and non-refractory element and also assume a differential depletion pattern. Standard practice is to adopt an empirical depletion pattern based on ISM observations (e.g. Savage & Sembach 1996) and to assume \[Zn/Fe\] $`0`$ intrinsically (i.e. attribute any departures from solar as depletion). Under this assumption, one finds that the majority of the DLA systems show nearly solar relative abundances at nearly all metallicity and redshift where Zn is observed. This leads to the conclusion that the relative abundances of the metal-poor DLA do not match Galactic metal-poor stars, specifically the enhanced $`\alpha `$/Fe ratios observed for these stars (note the contradiction with my interpretation of Figure 2). Instead, these researches argue the DLA abundance patterns more closely resemble recent results for dSph and dIrr galaxies (e.g. Shetrone et al. 2001; Venn et al. 2003; Tolstoy et al. 2003).

At first glance, the correspondence between the DLA systems and dwarf galaxies is a comforting picture. In hierarchical cosmology, galaxies at $`z2`$ are actively merging to build-up our present-day galaxies. The DLA systems are identified with ‘protogalactic clumps’ within dark matter halos (Haehnelt et al. 1998; Maller et al. 2001) whose masses might be comparable to modern dSph and dIrr galaxies. For the following reasons, however, I contend that connecting the DLA systems to modern dwarf galaxies is premature and potentially in great conflict with hierarchical cosmology. Consider:

$``$ In hierarchical cosmology, the majority of DLA systems will not evolve into present-day dwarf galaxies.

In order to explain the kinematic characteristics observed for the DLA systems (Prochaska & Wolfe 1997) within the paradigm of hierarchical cosmology, the ‘protogalactic clumps’ identified as DLA systems must arise predominantly in galaxies with $`v_c>125`$ km/s (e.g. Maller et al. 2001). Furthermore, these clumps are actively merging with one another to build up the central galaxy of the dark matter halo. In this scenario, only a small fraction of the DLA population (presumably the low mass tail) could serve as the progenitors of present-day dwarfs; the majority will be merged into larger galaxies by $`z1`$. Therefore, any correspondence between the abundance patterns of the $`z2`$ DLA systems and present-day dwarfs may have to be considered a coincidence.

$``$ Where is the gas enriched by Type II SN?

An important challenge raised by observers studying the elemental abundances of dSph in the Local Group is that these stars exhibit abundances which are very different from those measured for the Galactic halo (specifically, the Galactic halo within a few kpc of the Sun). This apparently contradicts the favored scenario for the formation of the Galactic halo in hierarchical cosmology, i.e., it formed from the accretion of dwarf satellites during the first few Gyr of the universe. One possible (and fashionable) resolution of this problem is that the dwarf galaxies which exist today (i.e. those which have not yet merged with the Milky Way) have had different chemical enrichment histories from those which merged to form the Galactic halo. As noted above, however, in CDM cosmology it is the DLA systems which correspond to the merging dwarfs. This identification leads to a more significant conflict regarding the origin of Galactic metal-poor stars. If we interpret the DLA abundance patterns as matching present-day dwarf galaxies, one is left with the problem: “Where is the gas enriched by Type II SN in the early universe which fueled the formation of the metal-poor stars of the Milky Way?”

$``$ Ages, SFR, Zn, etc.

There are a number of other issues which may contradict or at least complicate the dwarf/DLA connection: (1) the ages of the DLA galaxies are too young to be consistent with the slow, steady SFH generally associated with dIrr galaxies; (2) SFR’s derived for the DLA systems from the C II absorption are typical of those expected for spiral disk galaxies (Wolfe, this proceedings); (3) the DLA galaxies are gas-rich whereas the dSph galaxies are gas-poor. To link the two populations, one may require that the duty cycle for star formation in the dSph galaxies was significantly longer than the starburst behavior suggested by their stellar populations; and (4) the reported agreement between DLA and dwarf abundance patterns hinges on the assumption that \[Zn/Fe\]=0 intrinsically. If \[Zn/Fe\] is even $`+0.2`$ dex, then the DLA observations would be in good agreement with the Galactic halo abundance patterns. I note that several new issues related to the \[Zn/Fe\]=0 presumption were raised at the JD by Nissen, Apslund, and Israelian.

These issues aside, comparisons of the DLA and metal-poor stellar abundance patterns offer a powerful and insightful means of studying nucleosynthesis and galaxy formation. I am confident that ongoing studies of stellar populations in the Milky Way and Local Group as well as more comprehensive analysis of the DLA systems (e.g. Prochaska, Howk, & Wolfe 2003; Dessauges-Zavadsky, this proceeding) will lead to new puzzles and discoveries over the next years.

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