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# The central part of the young open cluster NGC 6383 Based on observations collected at the European Southern Observatory, La Silla, Chile.

## 1 Introduction

NGC 6383 ($`\alpha _{1950}`$ = 17h31$`\stackrel{m}{.}`$4, $`\delta _{1950}`$ = $``$32°32′) is a relatively small (10 arcmin radius, Hagen 1970) very young open cluster, centered around the bright spectroscopic binary HD 159176 (O7 V + O7 V, $`P`$ = 3.366767 days; Stickland et al. 1993). The weak H$`\alpha `$ emission nebula Stromlo 67 (Gum 1955), also known as S11 (Sharpless 1953) or RCW 132 (Rodgers et al. 1960), is centered approximately on HD 159176, by which it is excited. Together with NGC 6530 and NGC 6531, NGC 6383 belongs to the Sgr OB1 association.

A photoelectric study by Eggen (1961) showed that the stars in NGC 6383 later than A0 lie above the zero-age main sequence (ZAMS) and might therefore still be contracting. A photographic study of stars in a larger area around the cluster by Thé (1965) confirmed Eggen’s results, but failed to find weak H$`\alpha `$ emission line stars of the type found in other very young open clusters, such as NGC 2264, NGC 6530 and NGC 6611.

Fitzgerald et al. (1978) studied stars in the central core (1.25 arcmin radius) of NGC 6383 using photoelectric photometry and derived an average colour excess $`E(BV)`$ = $`0\stackrel{m}{.}33\pm 0\stackrel{m}{.}02`$, a cluster distance $`d`$ of $`1.5\pm 0.2`$ kpc and a cluster age of $`1.7\pm 0.4`$ million years. Luiken-Miller (1982) derived a similar numbers for the $`E(BV)`$: $`0\stackrel{m}{.}31\pm 0\stackrel{m}{.}02`$. However, her cluster distance of $`2.4\pm 0.3`$ kpc deviates considerably from the value by Fitzgerald et al. (1978). Furthermore, Luiken-Miller found a considerable spread in the ages of the stars in NGC 6383, with an average age of 2.2 million years.

The spectral energy distributions of stars in the central core of NGC 6383 were studied by Thé et al. (1985) using photoelectric photometry in the Walraven $`WULBV`$, Cousins $`VRI`$ and Near-IR $`JHKLM`$ photometric systems. They found a considerable infrared excess around three stars located above the ZAMS, probably due to thermal emission of circumstellar dust grains, confirming the pre-main sequence nature of these objects. Thé et al. also derived a colour excess $`E(BV)`$ = $`0\stackrel{m}{.}30\pm 0\stackrel{m}{.}01`$ and a distance of $`1.4\pm 0.15`$ kpc for NGC 6383, in excellent agreement with the values found by Fitzgerald et al. (1978).

However, spectral types of some of the stars studied by Thé et al. (1985) are still uncertain, and previous authors did not take the possibility of anomalous extinction into account while deriving properties of the stars in NGC 6383. Therefore, a new study of the pre-main sequence candidates in this cluster is in place. For this, 14 stars in NGC 6383, mostly located in the core, were selected from the paper by Thé et al. (1985). The stars along with the available data in the literature are listed in Table 1. We shall use the star’s number as given in Fitzgerald et al. (1978) except for the last two stars in Table 1 which are assigned number T17 and T54 following the numbering system by Thé (1965).

## 2 Observations

Low resolution (1.80 Å pix-1) CCD spectra of our programme stars, in the wavelength range of 4200 to 7800 Å, were obtained on the 16th of June 1992 at the European Southern Observatory, La Silla, Chile, using the Boller & Chivens spectrograph mounted on the ESO 1.52 m telescope. Using the MIDAS software package, the spectra were reduced with the usual steps of bias subtraction, flatfielding, background subtraction and spectral extraction, and wavelength and flux calibration. The resulting spectra are shown in Fig. 1.

New $`JHKLM`$ near-IR photometric data of star number 6 in the numbering system by Fitzgerald et al. (1978) were obtained by P.S. Thé in July 1986 with the ESO 1 m telescope at La Silla with the InSb detector attached. These observations were made through a 15″ diaphragm. Sky subtraction was achieved by chopping, with a frequency of 8 Hz, in the east-west direction with a throw of 30″ amplitude. The measurements and their accuracies are listed in Table 2.

## 3 Spectral classification

New spectral classifications for our programme stars were made by comparing our new spectra with the standard MK spectra by Jacoby et al. (1984). The resulting spectral classifications are listed in Table 3. Particularly interesting is the spectrum of star number 4, which shows H$`\alpha `$ in emission and also has the O i 7774 line strongly in absorption. According to the relations obtained by Danks & Dennefeld (1994), the relative strength of this last line indicates that it must be a giant. Furthermore, the Na i$`D`$ lines in this star appear to be somewhat stronger than those in the other spectra shown in Fig. 1, suggesting the presence of circumstellar gas in this object.

Additional spectral classifications were made from the photometric data by Fitzgerald et al. (1978) and by Eggen (1961) by deredenning all programme stars in the $`(UB)`$ versus $`(BV)`$ diagram, assuming a normal extinction law, i.e. $`E(UB)/E(BV)`$ = 0.72. They are listed in Table 3. The adopted final classification, determined by comparing literature classifications with ours is also listed in Table 3. Note that with the exception of star number 4 we do not retrieve the emission-line classification obtained for several programme stars by previous authors. We believe this to be due to the superior background subtraction procedures allowed by our long-slit CCD observations.

## 4 Spectral Energy Distributions

Spectral energy distributions (SEDs) of all programme stars were constructed using photometric data from Thé et al. (1985), Fitzgerald et al. (1978), Eggen (1978), the ANS catalogue (Wesselius et al. 1982), the TD1 catalogue (Thompson et al. 1978) and our new photometry from Table 2. No reliable IRAS data were available for any of our programme stars. The resulting SEDs, shown in Fig. 2, were analyzed by comparing them to Kurucz (1991) models corresponding to their spectral classification, using the method described by van den Ancker et al. (1997). The values for the ratio of total to selective extinction $`R_V`$, which are the result of the application of this procedure are also given in Table 3. No deviation from a normal interstellar extinction law (i.e. $`R_V`$ = 3.1) could be found in any of these stars.

As can be seen from Fig. 2, three of our programme stars (numbers 4, 5 and 6) show large amounts of excess radiation above photospheric levels, similar to those seen in many Herbig Ae/Be stars, in the near-infrared. Two additional stars (numbers 18, 20 and possibly 24) show a modest amount of infrared excess. This probably indicates the presence of circumstellar dust, heated up by the central star, in these systems. Since star number 4 is the only one of our programme stars which also shows H$`\alpha `$ in emission (see Fig. 1), this makes it a new candidate for membership of the Herbig Ae/Be stellar group in our sample.

## 5 Evolutionary status

Again following the method of van den Ancker et al. (1997), luminosities of our programme stars were computed from their SEDs, adopting the distance of $`1.4\pm 0.15`$ kpc towards NGC 6383 obtained by Thé et al. (1985). The computed luminosities are also listed in Table 3. Using these and the temperatures corresponding to the spectral types, a Hertzsprung-Russell diagram was constructed (Fig. 3). In this diagram we also plotted the pre-main sequence evolutionary tracks by Palla & Stahler (1993), as well as their so-called “birthline”, where a star becomes visible for the first time during its evolution towards the main-sequence, for accretion rates of 10-5 and 10-4 M yr-1.

From Fig. 3 we notice that all stars in NGC 6383 fall below both stellar birthlines, and therefore confirm the Palla & Stahler models. Furthermore, the stars we classified spectroscopically with luminosity classes III or IV in Table 3 all seem to be located to the right of the main-sequence, and therefore are probably true pre-main sequence stars. However, no strong correlation between position in the HR diagram and the presence of a near-infrared excess seems to be present within our sample.

## 6 Conclusions

The spectral and extinction properties of 14 pre-main sequence star candidates in the central part of the very young open cluster NGC 6383 were investigated. From fitting of Kurucz (1991) models to their Spectral Energy Distributions, it was concluded that none of these stars shows any evidence for anomalous circumstellar extinction. However, six out of out 14 programme stars do show an infrared excess, indicative of the presence of circumstellar dust, heated up by the central star. No correlation between the infrared excess and the position in the cluster’s HR diagram could be found.

One programme star (number 4), has a large infrared excess, reminiscent of the one displayed by many Herbig Ae/Be stars. Furthermore, it shows H$`\alpha `$ in emission and shows some indications for the presence of circumstellar gas in its spectrum. Therefore it was concluded that this star can be considered as a new Herbig Ae star candidate. A literature search was done for photometric data for this star, but the available data do not show any indications for photometric variability, such as displayed by many Herbig Ae stars.

###### Acknowledgements.

The authors would like to thank an anonymous referee for useful comments. This research has made use of the Simbad data base, operated at CDS, Strasbourg, France.


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# 1 Upper bounds on the mass 𝑚_𝑠 of the sterile neutrino 𝜈_𝑠 as a function of sin²𝜃, 𝜃 being the effective mixing angle to SM neutrinos. The solid line comes from the upper bound on radiative 𝜈_𝑠 decays and is independent of the thermal history of the Universe. The dashed line follows from the requirement that thermal 𝜈_𝑠 relics should not “overclose” the Universe; it has been derived under the assumption that 𝜈_𝑠 was in thermal equilibrium after inflation.

TUM-HEP-378-00

June 2000

New Constraints on “Cool” Dark Matter

Manuel Drees and David Wright

Physik Department, TU München, James Franck Str., D–85748 Garching, Germany

## Abstract

It has been suggested that a sterile neutrino $`\nu _s`$ which mixes with standard neutrinos can form nonthermal “cool” Dark Matter if its mass and mixing angle fall in the ranges 0.1 keV $`\stackrel{<}{}m_s\stackrel{<}{}`$ 10 keV and $`10^{10}\stackrel{<}{}\mathrm{sin}^2\theta \stackrel{<}{}\mathrm{\hspace{0.25em}10}^4`$, respectively. We point out that the required mixing makes these heavy neutrinos unstable. The dominant decay mode is into three light neutrinos, but the most stringent constraint comes from the non-observation of radiative decays into a single light neutrino and a photon. Moreover, we point out that the density of thermal relics of such $`\nu _s`$s would be too high, unless the reheating temperature after inflation was below $``$10 GeV.

Recently Shi and Fuller suggested  a new particle physics candidate for the Dark Matter in the Universe. They note that, if a significant lepton-antilepton asymmetry $`\mathrm{\Delta }L`$ existed in the early Universe and was reflected in a net neutrino number, and if there is a sterile neutrino species $`\nu _s`$ with an appropriate mass and mixing angles, the standard neutrino excess is converted into a sterile neutrino excess via resonant interactions with the thermal plasma at a temperature of $``$10 MeV. Since neutrinos with the lowest energy will be converted first, until $`\mathrm{\Delta }L`$ is essentially used up, the resulting sterile neutrinos, while mostly relativistic, will be significantly “colder” than the standard neutrinos. More exactly, their energy distribution will be nonthermal, with average energy a fraction of that of the parent (standard) neutrinos. This nonthermal ensemble of sterile neutrinos $`\nu _s`$ would survive to this day, and constitutes a suitable Dark Matter candidate for mass and mixing angle parameters in the ranges 0.1 keV $`\stackrel{<}{}m_s\stackrel{<}{}`$ 10 keV and $`10^{10}\stackrel{<}{}\mathrm{sin}^2\theta \stackrel{<}{}\mathrm{\hspace{0.25em}10}^4`$, respectively. Such “cool” Dark Matter might be compatible with studies of structure formation, while hot Dark Matter seems to be excluded. An explicit realization of this idea, where $`\nu _s`$ is a supersymmetric axino, has been suggested by Chun and Kim .

The authors of refs.  seem to have overlooked the fact that the mixing of $`\nu _s`$ with standard neutrinos will cause the $`\nu _s`$ to decay, and will induce interactions between $`\nu _s`$ and the thermal plasma. Obviously, $`\nu _s`$ can only form Dark Matter if it is sufficiently long-lived. In addition, it will only form cool Dark Matter if the density of thermal $`\nu _s`$ relics is sufficiently small. We find that the first condition imposes a significant constraint on parameter space that is independent of the thermal history of the Universe. The second condition excludes the model altogether, if the post-inflationary Universe was ever hot enough for $`\nu _s`$ to have been in thermal equilibrium. Even for the smallest mixing angle $`\mathrm{sin}^2\theta 10^{10}`$ compatible with efficient conversion of a lepton asymmetry $`\mathrm{\Delta }L`$ into $`\nu _s`$s, the $`\nu _s`$ freeze-out temperature only amounts to $``$ 10 GeV. “Cool” Dark Matter would thus require the reheating temperature after inflation to be below this value.

We start our discussion with an analysis of $`\nu _s`$ decays. Since we are interested in sterile neutrinos with mass $`m_s\stackrel{<}{}\mathrm{\hspace{0.25em}10}`$ keV, the only possible tree-level decay is the one into three light Standard Model (SM) neutrinos, $`\nu _s3\nu `$, which proceeds through the exchange of a $`Z`$-boson. The $`Z\nu _s\overline{\nu }`$ coupling is simply $`\mathrm{sin}\theta `$ times the $`Z\nu \overline{\nu }`$ coupling of the SM, where $`\theta `$ is the $`\nu \nu _s`$ mixing angle. The corresponding partial width is given by

$$\mathrm{\Gamma }(\nu _s3\nu )=\frac{G_F^2m_s^5}{192\pi ^3}\mathrm{sin}^2\theta ,$$
(1)
where $`G_F`$ is the Fermi constant, and we have summed over all three generations of SM neutrinos. $`\mathrm{sin}^2\theta =_i\mathrm{sin}^2\theta _i`$, where $`\theta _i`$ is the mixing angle between $`\nu _s`$ and $`\nu _i`$, is the effective mixing angle to standard model neutrinos.

An obvious constraint on any particle physics candidate for Dark Matter is that its lifetime should exceed the age of the Universe, $`\tau (\nu _s)\stackrel{>}{}\mathrm{\hspace{0.25em}5}10^{17}`$ sec. However, in the case at hand a stronger constraint can be derived, since the mixing between $`\nu _s`$ and the light neutrinos also induces radiative decays at the one–loop level, with branching ratio

$$B(\nu _s\nu \gamma )=\frac{27\alpha _{\mathrm{em}}}{8\pi }810^3,$$
(2)
where $`\alpha _{\mathrm{em}}`$ is the fine structure constant. These decays would add a monochromatic line at energy $`E=m_s/2`$ to the diffuse background of hard UV or soft X-ray photons. There are stringent observational bounds on such anomalies , leading very conservatively to the requirement***This constraint is weaker than the corresponding one in ref.  by a factor of the branching ratio (2). Note also that we assume $`\nu _s`$ to form all Dark Matter, independently of $`m_s`$; this can be arranged by an appropriate choice of $`\mathrm{\Delta }L`$. As a result, our limit (3) is independent of $`m_s`$, since the neutrino density $`n_s`$ and the observational upper bound on the photon flux both scale like $`1/m_s`$.

$$\tau (\nu _s)>10^{22}\mathrm{sec}.$$
(3)
This implies

$$\mathrm{sin}^2\theta <2.910^3\left(\frac{1\mathrm{keV}}{m_s}\right)^5,$$
(4)
where we have used eq. (1). This condition imposes a nontrivial new constraint for $`m_s\stackrel{>}{}\mathrm{\hspace{0.25em}2}`$ keV. Note that this constraint does not depend on the thermal history of the Universe prior of the conversion of the lepton asymmetry into sterile neutrinos. It is depicted by the solid line in Fig. 1.

The constraint (3) has been derived  under the conservative assumption that Dark Matter is distributed uniformly throughout the Universe. A simple estimate shows that the contribution from the dark halo of our galaxy alone yields a comparable bound. The best strategy would probably be to search for the emission of monoenergetic photons from regions that are known to be rich in Dark Matter, but have few background sources in the relevant frequency band. One example might be (the centers of) dwarf galaxies.

Of course, these searches can only be expected to be successful if $`\nu _s`$ does indeed form (most of) the Dark Matter in the Universe. We will now show that the requirement of thermal nonequilibration, the second condition mentioned above, imposes a severe constraint on the thermal history of the Universe if Dark Matter is indeed “cool”. This constraint follows from the requirement that the present density of thermal relic $`\nu _s`$s, which contribute to hot Dark Matter, should be sufficiently small. Since $`\nu _s`$ was relativistic when it decoupled its contribution to the present mass density of the Universe can be obtained by simple scaling from the contribution of massive SM neutrinos :

$$\mathrm{\Omega }_s^{\mathrm{thermal}}h^2\frac{m_s}{100\mathrm{eV}}\frac{10.75}{g_{}(T_F)},$$
(5)
where $`h`$ is today’s Hubble constant in units of 100 km$`/`$(sec$``$Mpc), and $`g_{}`$ is the number of relativistic degrees of freedom at the temperature $`T_F`$ where $`\nu _s`$ decoupled from the plasma of SM particles. This temperature is defined by the condition that the rate of reactions that change the number density $`n_s`$ of $`\nu _s`$ should be equal to the Hubble expansion rate $`H`$ at that temperature:

$$n_s(T_F)v\sigma (\nu _sf\nu f)(T_F)=H(T_F).$$
(6)
Here $`f`$ stands for any SM fermion or antifermion and $`\nu `$ for an active neutrino. The symbol $`\mathrm{}`$ denotes the thermal average.

During the radiation dominated era, the Hubble expansion rate was

$$H(T)=\frac{\pi T^2}{M_{Pl}}\sqrt{\frac{g_{}}{90}},$$
(7)
where $`M_{Pl}=2.410^{18}`$ GeV is the reduced Planck mass. Since by assumption $`\nu _s`$ was in equilibrium for $`TT_F`$, $`n_s`$ in eq. (6) can be replaced by the equilibrium density

$$n_s=n_s^{\mathrm{eq}}=\frac{3\xi (3)}{2\pi ^2}T^3=0.183T^3.$$
(8)
Here we have conservatively assumed that $`\nu _s`$ effectively has only two degrees of freedom (left-handed $`\nu _s`$ and right-handed $`\overline{\nu }_s`$); if $`\nu _s`$ is a Dirac particle, this amounts to the assumption that interactions which change the chirality of $`\nu _s`$ are not in equilibrium at $`TT_F`$.

We estimate the cross section appearing in eq. (6) from the $`\nu _\mu e^{}\nu _\mu e^{}`$ scattering cross section. This is again conservative, since it ignores charged current contributions to the cross section; moreover, electrons have the smallest (vector) couplings to the $`Z`$ among all SM fermions. This gives

$$v\sigma (\nu _sf\nu f)=\mathrm{sin}^2\theta \frac{G_F^2}{12\pi }\left(312\mathrm{sin}^2\theta _W+16\mathrm{sin}^4\theta _W\right)s,$$
(9)
where $`\theta _W`$ is the weak mixing angle. We have ignored the momentum dependence of the $`Z`$ propagator, since $`T_F^2M_Z^2`$ for all cases of interest. Moreover, when computing the thermal average, we ignore the Fermi blocking in the final state. The thermal average of the squared center-of-mass energy $`s`$ is then given by

$$s=2E_1E_2=2T^2\left[\frac{_0^{\mathrm{}}𝑑xx^3/(1+\mathrm{e}^x)}{_0^{\mathrm{}}𝑑xx^2/(1+\mathrm{e}^x)}\right]^2=19.8T^2,$$
(10)
where $`E_1`$ and $`E_2`$ are the energies of the two particles in the initial state in the co-moving frame. Putting everything together, we have

$$T_F2.2\mathrm{MeV}\left(\mathrm{sin}^2\theta \right)^{1/3}\left[g_{}(T_F)\right]^{1/6}.$$
(11)
The factor $`\left[g_{}(T_F)\right]^{1/6}`$ varies between 1.5 for $`T_F10`$ MeV and 2.1 for $`T_F10`$ GeV. Note that $`T_F\stackrel{<}{}\mathrm{\hspace{0.25em}10}`$ GeV for $`\mathrm{sin}^2\theta \stackrel{>}{}\mathrm{\hspace{0.25em}10}^{10}`$.

The dashed line in Fig. 1 shows the upper bound on $`m_s`$ that follows from eqs.(5) and (11) by requiring that $`\nu _s`$ should not “overclose” the Universe, $`\mathrm{\Omega }_s^{\mathrm{thermal}}h^2<0.5`$. The drop at $`\mathrm{sin}^2\theta =310^5`$ occurs since for larger mixing angles $`T_F`$ falls below the temperature of the QCD phase transition, which we conservatively assumed to be 150 MeV; this leads to a significant decrease of $`g_{}(T_F)`$ in eq. (5). Note that the upper bound on $`m_s`$ should be lowered by at least another factor of five if $`\nu _s`$ is to form mostly cool Dark Matter, i. e. if thermal (hot) relics are to form only a minor fraction of today’s $`\nu _s`$ relic density. The upper bound on $`m_s`$ that follows from the upper bound on the density of thermal $`\nu _s`$ relics would then fall slightly below the lower bound on $`m_s`$ of $``$0.1 keV derived in ref. .

Simply put, “cool” Dark Matter as discussed in refs.  cannot exist if $`\nu _s`$ ever was in thermal equilibrium. The “cool” Dark Matter model is therefore only viable if the reheating temperature $`T_R`$ after inflation is (well) below the temperature (11). For example, certain models of $`D`$-term inflation have $`T_R1`$ GeV ; this would leave some parameter space with $`\mathrm{sin}^2\theta <10^7`$. Note, however, that the density of thermally produced $`\nu _s`$ can be significant even if $`\nu _s`$ never was in thermal equilibrium. This is analogous to the case of gravitinos with mass $`\stackrel{>}{}\mathrm{\hspace{0.25em}1}`$ keV in supergravity models. For a given $`T_R<T_F`$ and a given $`\mathrm{sin}^2\theta `$, a nontrivial upper bound on $`m_s`$ may therefore still result. Of course, the requirement of a very low reheating temperature may also make it difficult to explain the large lepton asymmetry that is required by the model.

In summary, we have shown that the requirement that the sterile neutrino be sufficiently long-lived imposes a significant constraint on the allowed combinations of mass $`m_s`$ and mixing angle $`\theta `$ with ordinary (active) neutrinos. Loop induced radiative $`\nu _s\nu \gamma `$ decays play a crucial role here. This constraint is independent of the thermal history of the Universe. Furthermore, the $`\nu _s`$ can only form cool Dark Matter if, after the end of inflation, it never was in thermal equilibrium. This imposes a very stringent constraint on the reheating temperature; e. g., $`T_R<10`$ GeV (1 GeV) for $`\mathrm{sin}^2\theta =10^{10}(10^7)`$. These constraints, together with the requirement of a lepton asymmetry that is several orders of magnitude larger than the observed baryon asymmetry, make this model rather unattractive.

Acknowledgements:
We thank Subir Sarkar for pointing out the importance of radiative $`\nu _s`$ decays. This work was supported in part by the “Sonderforschungsbereich 375–95 für Astro–Teilchenphysik” der Deutschen Forschungsgemeinschaft.


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# 1 The density of states in SrB6 for two types of interband hybridization (a) isotropic excitonic gap, bold line, and (b) anisotropic crystal-field mixing Eq. (1), thin line.

Comment on “Electronic fine structure in
the electron-hole plasma of SrB6

In a recent Letter , Rodriguez et al. addressed the origin of the high-temperature weak ferromagnetism found in doped hexaborides  by calculating details of the band structure of SrB6 in the vicinity of the X-point in the Brillouin zone. They conclude that crystal field induced electron-hole mixing has an important effect on the density of states (DOS) and suggest nesting between electron Fermi pockets as an alternative explanation to the excitonic ferromagnetism . We would like to question several conclusions in this work .

(i) Rodriguez et al. claim that the two bands cross only along the symmetry lines $`(\xi ,0,0)`$ and $`(\frac{\pi }{a},\xi ,0)`$. This result contradicts a previous band structure study, which found band crossing in all symmetry planes passing through the X-point . The latter conclusion has a simple symmetry interpretation. At the X-point the valence and conduction bands belong to different irreducible representations of the small group: $`X_3`$, basis function $`yz`$, and $`X_3^{}`$ symmetry, basis function $`x(y^2z^2)`$, respectively. The band mixing occurs away from the X-point and is given by the product $`X_3\times X_3^{}`$

$$\mathrm{\Delta }_{\mathrm{cryst}}E_bk_xk_yk_z(k_y^2k_z^2)/b^5,$$
(1)
where $`E_b`$ is a bandwidth and $`b=\frac{2\pi }{a}`$ is a reciprocal lattice vector. The crystal field hybridization is strongly suppressed by the high power of momentum in Eq. (1) ($`k_F0.1b`$). Therefore, not only is the hybridization more anisotropic than suggested in Ref. , but also it is very weak on the scale of the band overlap. Our TB-LMTO calculations  as well as FLAPW method  yield an extremely small band mixing for a general direction in the Brillouin zone in agreement with Eq. (1).

(ii) Even for a strong hybridization, the DOS is quite different from the results of Ref. . Fig. 1 shows the DOS for two parabolic bands with anisotropic effective masses , band overlap $`E_G=100`$ meV, and two angular dependences for the mixing matrix element: isotropic, which models an excitonic gap , and anisotropic given by Eq. (1). The amplitudes were chosen to give the same maximum splitting of $`2\mathrm{\Delta }_{\mathrm{max}}=15`$ meV. Because of the anisotropic dispersion the DOS is slightly reduced at the Fermi level. The true gap in the DOS opens only for a sufficiently large excitonic gap $`\mathrm{\Delta }>0.16E_G`$. Note that the tetrahedron method for DOS does not allow for crossing of bands, which are numbered in increasing order of energy at every k-point, and, therefore, may lead to spurious peaks  due to artificial anticrossings.

(iii) Correlation effects in the $`e`$-$`h`$ plasma lead to a forbidden range for the band overlap values in the hexaborides . At the first order metal-insulator transition a semiconductor jumps into a dense plasma with $`r_s1`$. Rodriguez et al. have estimated $`r_s=2.5`$ for the band overlap $`E_G=100`$ meV in SrB6, a value lying within the forbidden range. The real overlap must be larger. Therefore, the conclusion that 0.5 % doping fills hole Fermi pockets in SrB6 , which is based on the above underestimated value of $`E_G`$, is by no means reliable and does not exclude electron-hole pairing at this doping level.

(iv) Nesting of electron pockets between inequivalent X-points was suggested in Ref.  as another source of CDW and SDW instabilities, which does not involve holes from the valence band. This suggestion is physically incorrect. The nesting condition refers to a sign change under translation in momentum space: $`ϵ(k+Q)ϵ(k)`$. Only in such a case can repulsive $`e`$-$`e`$ interaction produce a density-wave instability in $`e`$-$`h`$ channel, see e.g. .

Lastly, the interpretation of the de Haas-van Alphen measurements quoted in  seems to us to be problematic in view of the high values of the low temperature resistivity reported for SrB6  and its strong dependence on stoichiometry. Further information is required before a definitive conclusion can be made.

We thank R. Monnier for many useful discussions.

M. E. Zhitomirsky,1 T. M. Rice,1 and V. I. Anisimov2
1Theoretische Physik, ETH-Zürich, Switzerland
2Institute of Metal Physics, Ekaterinburg, Russia

PACS numbers: 71.10.Hf, 71.18.+y, 75.10.Lp, 75.30.-m


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# An electron paramagnetic resonance study of Pr0.6Ca0.4MnO3 across the charge ordering transition

## Abstract

We report the first electron paramagnetic resonance studies of single crystals and powders of Pr0.6Ca0.4MnO3 in the 300-4.2 K range, covering the charge ordering transition at $``$ 240 K and antiferromagnetic transition (TN) at $``$ 170 K. The asymmetry parameter for the Dysonian single crystal spectra shows anomalous increase at Tco. Below Tco the g-value increases continuously, suggesting a gradual strengthening of orbital ordering. The linewidth undergoes a sudden increase at Tco and continues to increase down to TN. The intensity increases as the temperature is decreased till Tco due to the renormalization of magnetic susceptibility arising from the build up of ferromagnetic correlations. The value of the exchange constant, $`J`$, is estimated to be 154 K.

PACS numbers: 76.30.-v, 75.70.Pa, 72.80.Ga, 71.30.+h

today

Recent investigations of rare earth manganites and related systems exhibiting colossal magnetoresistance has led to the discovery of interesting phenomena related to charge, spin and orbital ordering in these materials . Phase diagrams of these systems as a function of doping and temperature are therefore very interesting showing regimes of varied magnetic and electrical properties. These manganites of general composition $`A_{1x}A_x^{}MnO_3`$ where $`A`$ is a trivalent rare earth ion (e.g La, Pr, Nd etc) and $`A^{}`$ is a divalent ion (e.g Ca, Sr, Pb etc) show a rich phase diagram  depending on the tolerance factor and the amount of doping x which, in turn, controls the ratio of Mn3+ to Mn4+. The end members of this series i.e x=0 and x=1 are A type and G type antiferromagnetic insulators (AFI), respectively. For 0.17 $`<`$ x $`<`$ 0.5 the system undergoes a metal to insulator (MI) transition as the temperature is increased. This MI transition also coincides with the magnetic transition from the ferro to the paramagnetic state. Electronic properties of these systems are understood qualitatively in terms of the Zener’s double exchange interaction  (DEX). In DEX there is a strong Hund’s coupling between the 3 $`t_{2g}`$ electrons whose spins are parallel and constitute a core spin of 3/2 and the lone $`e_g`$ spin. This $`e_g`$ electron can hop from one Mn3+ site to adjacent Mn4+ site via the intermediate oxygen when the core spins are parallel which also implies that metallicity coincides with ferromagnetism. To explain the resistivity data, Millis et al  invoked the localization of charge carriers above Tc due to polaron formation. In the case of systems where the weighted average A site cation radius is small, the system also shows charge ordering (CO) i.e real space ordering of Mn3+ and Mn4+ ions, as a function of temperature. The CO state becomes stable when the repulsive Coulomb interaction between carriers is dominant over the kinetic energy. In these types of cases there is a strong competition between the double exchange interaction which favours ferromagetism and CO which favours antiferromagnetism. The smaller size of A site cation leads to a deviation in the Mn-O-Mn bond angle from 180 resulting in lowering of the transfer integral. This in turn implies a lower band width of the $`e_g`$ electron and hence higher electronic correlations in the system. The stability of the CO state depends on the commensurability of the carrier concentration with the periodicity of the crystal lattice and is stable for x=0.5.

Pr1-xCaxMnO3 shows a rich phase diagram as a function of doping and temperature and is well studied using a variety of probes like resistivity , magnetization , neutron diffraction studies  and transmission electron microscopy . For x=0.4, the sample is insulating at all temperatures in zero field. The resistivity changes by more than six orders of magnitude from 300 K to 50 K. There is a perceptible change in slope at around TCO $``$ 240 K signifying the onset of charge ordering. In the temperature range T $`>`$ Tco (240 K) the system is a paramagnetic insulator. In dc magnetic susceptibility, a large peak is observed at Tco followed by a relatively small peak at TN. The peak at Tco is attributed to ferromagnetic correlations . The system further undergoes a transition at 170 K to a CE type AFI. The pseudo CE type structure for x $`<`$ 0.5 is different than the CE structure present in systems with x = 0.5. In this so called ”pseudo CE” structure the zig-zag FM chains in the ab plane are FM aligned along the c axis . This is unlike the CE structure where the layers in the ab plane are aligned antiferromagnetically along c. Further lowering of temperature below 50 K leads to another transition which can be understood either as a canted antiferromagnetic state  or as a mixture of ferromagnetic domains or clusters in an antiferromagnetic background. In this paper we report our EPR study of single crystals as well as powders of Pr0.6Ca0.4MnO3 as a function of temperature from 300 K to 4.2 K. Although several EPR studies on the manganites have been reported recently across the metal-insulator transition , to our knowledge, there has been no study across the CO transition. The dynamics of spins in the charge ordered state as studied by EPR is expected to throw some light on the controversial magnetic structure between the charge ordering transition and the Neel temperature.

The single crystal used for the experiment was prepared by the float zone technique and characterized using dc magnetic susceptibility which shows a large peak at 240 K (Tco) and a relatively small peak at 170 K (TN). The measurements on single crystals were done with magnetic field parallel to (100) axis. Powder of the material was dispersed in paraffin wax for study. The EPR measurements were carried out at 9.2 GHz (X band) with a Bruker spectrometer ( model 200 D) equipped with an Oxford Instruments continous flow cryostat ( model ESR 900), with a temperature accuracy of $`\pm `$ 2 K.

Fig. 1 shows the EPR spectra at a few temperatures in the range 300 K to 180 K recorded in the heating run for a single crystal (fig. 1(a)) and a powder sample (fig. 1(b)). The ESR signal could be observed only above 180 K. The observed signals are very broad. The spectra from the single crystal are Dysonian in shape and were fitted (solid lines in Fig. 1(a)) to a functional form similar to the one used by Ivanshin et al  for La1-xSrxMnO3. The field derivative of the power absorbed given by

$$\frac{dP}{dH}\frac{d}{dH}(\frac{\mathrm{\Delta }H+\alpha (HH_{res})}{(HH_{res})^2+\mathrm{\Delta }H^2}+\frac{\mathrm{\Delta }H+\alpha (H+H_{res})}{(H+H_{res})^2+\mathrm{\Delta }H^2})$$
(1)
incorporates responses to both the circular components of the exciting linearly polarised microwave field. The above equation also includes both absorption and dispersion. $`\alpha `$, the asymmetry parameter is a measure of dispersion-to-absorption ratio. The spectra from powder samples are symmetrical and were well fitted with Lorentzians as shown in Fig. 1(b).

Careful EPR measurements in doped manganites by Causa et al  and Lofland et al  show that that both Mn3+ and Mn4+ contribute to the EPR signal. The bottleneck model used by Shengalaya et al  also shows that the EPR intensity is proportional to the total susceptibility of the Mn4+ and Mn3+ spins. We will first discuss our results on temperature dependence of EPR lineshape parameters of single crystals.

Fig. 2 shows the temperature dependence of the lineshape parameters of the signals obtained by fitting to equation (1). Fig. 2(a) shows the temperature dependence of the linewidth ( $`\mathrm{\Delta }`$ H). The linewidth decreases as the temperature is lowered from 300 K upto just above Tco and then nearly doubles across the charge ordering transition. This increase is somewhat similar to that observed  in LaCaMnO3 across the paraamgnetic insulator to ferromagnetic metal transition, thereby implying a buildup of spin-correlations at Tco. The increase in linewidth above Tco can be interpreted in terms of spin-lattice relaxation or even as an opening up of the “bottleneck” as the temperature is raised . Fig. 2(c) shows the variation of the integrated intensity as a function of temperature. We have tried to analyse the temperature dependence of intensity in terms of the bottleneck model . In this picture, the EPR signal originates from both Mn4+ and Mn3+ ions and the intensity is proportional to the total susceptibility. Here the spin-spin relaxation rates between the exchange coupled Mn3+ and Mn4+ ions are much larger than the spin-lattice relaxation rates. In this regime the ferromagnetic correlations will renormalize the spin susceptibility given by

$$I\chi _{total}=\chi _s+\chi _\sigma $$
(2)
where $`\chi _s`$ and $`\chi _\sigma `$ are the renormalised static susceptibilities and are given by

$$\chi _s=\chi _s^o\frac{1+\lambda \chi _\sigma ^o}{1\lambda ^2\chi _\sigma ^o\chi _s^o},\chi _\sigma =\chi _\sigma ^o\frac{1+\lambda \chi _s^o}{1\lambda ^2\chi _\sigma ^o\chi _s^o}$$
(3)
where $`\chi _s^o`$ = bare spin susceptibility of Mn4+ and $`\chi _\sigma ^o`$ = bare spin susceptibilty of Mn3+. The parameter $`\lambda =zJ/Ng_sg_\sigma \mu _B^2`$ , where $`J`$ is the exchange coupling constant between Mn4+ and Mn3+ spins, $`g_s`$ ($`g_\sigma `$) is the g factor of Mn4+ (Mn3+) ions ,$`N`$ is the number of spins per cm3, $`z`$ number of nearest neighbours and $`\mu _B`$ is the Bohr magneton. We can get some estimate of $`J`$ by fitting Eqs. 2 and 3 to the data in Fig 2(c). Taking $`g_s`$ = $`g_\sigma `$ = 2, $`z`$ = 6 and assuming that the bare susceptibility of Mn4+ ions is given by Curie law $`\chi _s^o`$ = Cs/T while that of Mn3+ follows a Curie-Weiss law Cσ/(T-$`\mathrm{\Theta }`$), where $`\mathrm{\Theta }`$, the negative Curie Weiss temperature is taken to be the same as that in undoped LaMnO3 ($`\mathrm{\Theta }`$ = -100 K). The solid line shows the fit to the intensity data above Tco yielding an estimate of $`J`$ 154 $`\pm `$ 1.24 K. This value is of the same order of magnitude as the value obtained for $`J`$ ( $``$ 70 K) in doped manganites by EPR measurements , neutron scattering  and Brillioun scattering experiments . At this stage we would also like to point out that though all spins contribute to the EPR intensity, the temperature dependence is qualitatively different from the dc susceptibility data (as shown in inset of Fig2(c) ) . This could be due the fact that the resistivity of the sample is increases by two orders of magnitude in the temperature regime of 300-180 K which will enhance the penetration depth and hence the volume of sample seen by the microwave field is changing with temperature. Fig 2(b) shows the temperature variation of g value. Since internal field effects can influence the single crystal data, we will focus our attention on temperature variation of g only in the powder data.

’Asymmetry parameter’, $`\alpha `$ of the signals, from single crystal data is shown in Fig. 3. The ratio remains practically constant from 300 K to Tco where it discontinously increases from $``$ 2.5 to $``$ 4.5. Further cooling results in a decrease of $`\alpha `$ value towards unity as is to be expected from the decrease in conductivity at lower temperatures (resistivity  shown in inset of Fig. 3). The discontinous increase of $`\alpha `$ at Tco is interesting because normally one would have expected a decrease following the decrease in conductivity. However as shown by Dyson  and Feher and Kip  the value of $`\alpha `$ depends also on the ratio of the time $`T_D`$ taken by the electrons to diffuse through the skin depth and the spin-spin relaxation time $`T_2`$. The sudden increase in $`\alpha `$ therefore indicates a sudden dip in the value $`T_D`$/$`T_2`$. This implies that the value of $`T_2`$ increases at Tco to offset the increase in $`T_D`$ due to decrease in the conductivity. However, this is contrary to the observed increase in the linewidth at Tco. At present, we do not have a satisfactory explaination of this result.

Fig 4 shows the temperature dependence of the lineshape parameters for the powder sample extracted by fitting derivative of the Lorentzian function yielding temperature dependence of the linewidth ($`\mathrm{\Delta }H`$), resonance field ($`H_o`$ ) and area under the curve. Fig. 4(b) shows the temperature dependence of the g factor, estimated from the resonance field. In all the earlier EPR reports in manganites, the value of g was observed to be close to or less than that of free electron ( = 2.0023). Earlier EPR studies on Mn3+ and Mn4+ dilutely doped in diamagnetic hosts have given  g $``$ 1.98. However our experiments give a g value higher than that for the free electrons for all temperatures. A speck of DPPH ( g = 2.0036) was used as a g-marker and the centre resonance field was obtained from the fit to the Lorentzian. This procedure gives confidence in our measurements of temperature dependence of g. Since the internal field effects are expected to average out in powdered samples, we believe that the increase in g for T $`<`$ Tco is intrinsic in nature. One possible reason can be the changes in the spin-orbit coupling. It is known that geff = g\[1 $`\pm `$ $`\kappa `$/ $`\mathrm{\Delta }`$\], where the spin orbit interaction energy is $`\kappa \stackrel{}{L}.\stackrel{}{S}`$ and $`\mathrm{\Delta }`$ is the appropriate crystal field splitting . A recent transmission electron microscopy study  of Pr0.5Ca0.5MnO3 has shown that the incommensurate to commensurate charge ordering is coincident with paramagnetic to antiferromagnetic transition at 180 K. The physical picture is that for TN $`<`$ T $`<`$ Tco, orbital ordering is partial inspite of complete charge ordering. This orbital ordering builds up and is complete at TN. Therefore for T $`<`$ Tco a gradual buildup of the orbital ordering can change the spin-orbit coupling and lead to an increase in the value of g as the temperature is lowered. This may also be the reason for the sign of g shift with respect to the free electron g which is opposite to that expected for Mn3+ and Mn4+ ions ( less than half filled d-shells). It will be very interesting to theoretically calculate the value of g, incorporating orbital ordering. Fig. 4(a) shows the temperature variation of the full width at half maximum of the Lorentzian, $`\mathrm{\Delta }H`$. For T $`>`$ Tco, the width decreases linearly as the temperature is lowered from 300 to 240 K similar to that observed in single crystal data. Below Tco till 180 K, the width increases significantly (almost by a factor of 2). It is remarkable that the width increases sharply from $``$ 1600 G at 240 K to $``$ 2200 G at 228 K. This sharp increase can be due to magnetic fluctuations which are also responsible for the peak in the dc magnetic susceptibility. The further increase in $`\mathrm{\Delta }H`$ as temperature is lowered can arise due to build up of magnetic correlations preceeding the transition to the long range antiferromagnetic ordering at 170 K. Fig. 4(c) shows the temperature dependence of the intensity which is qualitatively similar to that of single crystal data.

In summary, we have reported for the first time EPR measurements on charge-ordered Pr0.6Ca0.4MnO3. The lineshape parameters reveal a rich temperature dependence across Tco as well as at lower temperatures approaching TN. The intensity variation above Tco is considered to be due to the renormalization of spin susceptibility due to ferromagnetic (FM) correlations. Such FM correlations in the paramagnetic insulating phase have been invoked to understand the origin of the peak in magnetic susceptibility near Tco and of dynamical spin fluctuations above Tc in doped manganites . The formation of magnetic polarons to localize the carriers has been suggested by Varma et al . The value of exchange coupling constant $`J`$ is estimated to be about 154 K. The fluctuations in the magnetic correlations near the transition temperatures lead to a large increase in the linewidth. The temperature dependence of the g factor suggests a need to carry out theoretical calculations of g invoking orbital ordering.

SVB and AKS thank the Department of Science and Technology for financial assistance. We thank Prof. B. S. Shastry for his suggestion to do the EPR experiments and for useful discussions.