text:
# Transport properties of dense fluid argon

(18 September 2003)

## Abstract

We calculate using molecular dynamics simulations the transport properties of realistically modeled fluid argon at pressures up to $`50GPa`$ and temperatures up to $`3000K`$. In this context we provide a critique of some newer theoretical predictions for the diffusion coefficients of liquids and a discussion of the Enskog theory relevance under two different adaptations: modified Enskog theory (MET) and effective diameter Enskog theory. We also analyze a number of experimental data for the thermal conductivity of monoatomic and small diatomic dense fluids.

Many real fluids are very well represented as ensembles of identical molecules interacting through pairwise spherical potentials and, except for more exotic versions of such interactions where molecular dynamics is still a very useful tool rsbs , the thermodynamics of these systems has been well understood for a fairly long time in the context of various statistical mechanics theories tlwlw . The transport properties on the other hand, i.e. self-diffusion coefficient, viscosity, thermal conductivity, are less amenable to accurate theoretical calculation and require computationally intense molecular dynamics simulations, hence the continuing interest in their study md96 ; re99 ; sh03 . Through a natural although ad hoc extension of the dilute gas Boltzmann equation, Enskog transport theory cc  provided the first prediction of the transport coefficients of the hard sphere fluid and opened the way to the calculation of transport properties of real dense fluids. Other, more heuristic theories have been also proposed, relying on general physical concepts such as“free-volume” and “caging” ct ; re02 , and excess-entropy scaling yr77 ; md96 . The predictive capabilities of all these methods are critically affected by both their intrinsec limitations and the additional interpretations required when they are applied to real fluids hmc ; ks81 . The molecular dynamics calculation of the transport coefficients of the hard sphere fluid model agw  has provided important insights on the limitations of the Enskog theory in the high density regime, as well as the connection between microscopics and hydrodynamics. Experimental results on the transport properties of liquids at high pressures, e.g. tens of GPa, are only now becoming available for both molecular fluids asb  and liquid metals dd02 . Here we present molecular dynamics calculations of the transport properties of realistically modeled argon at pressures up to $`50GPa`$ and temperatures up to $`3000K`$. In this context we provide a critique of some newer theoretical predictions for the diffusion coefficients of liquids and a discussion of the Enskog theory relevance under two different adaptations: modified Enskog theory (MET) and effective diameter Enskog theory. We also analyze a number of experimental data for the thermal conductivity of monoatomic and small diatomic dense fluids.

Argon is generally believed to behave as a quintessential classical fluid in a rather wide range of densities and temperatures and it has been often modeled as a Lennard-Jones system vhc . More accurate representations of its interactions are also available, e.g. the Barker-Fisher-Watts (BFW) potential bfw , but they are more complicated and have been tested only at low pressures. A relatively simple pair-interaction that can account very well for the high density, high temperature thermodynamics of argon rmbx  is the Buckingham exponential-6 potential:

$`u(r)=ϵ\left[Ae^{\alpha \frac{r}{r_0}}B\left({\displaystyle \frac{r_0}{r}}\right)^6\right]`$ (1)
with well-depth $`ϵ`$ corresponding to distance $`r_0`$, and $`\alpha `$ a numerical constant: $`A=6e^\alpha /(\alpha 6)`$, $`B=\alpha /(\alpha 6)`$, the general properties of which have been well studied ep98 . In addition to argon the exponential-6 parametrization was shown to yield appropriate thermodynamics for other molecular fluids as well rr80 , e.g. $`N_2`$, $`O_2`$, $`CO_2`$, $`CH_4`$, $`CO`$ etc., particularly in the dense, hot regimes corresponding to shock-waves, detonations or planetary modeling hbl . The understanding of such dynamic processes requires a knowledge of both the thermodynamic and transport properties of these fluids and their mixtures, and we study argon as a representative example. Other molecular fluids and the limitations of exponential-6 modeling for small diatomics are also discussed in connection with available high pressure thermal transport experimental results.

We set $`ϵ/k_B=122K`$, $`r_0=3.85`$Å, $`\alpha =13.2`$ corresponding to argon rmbx , and perform microcanonical (NVE) molecular dynamics simulations with $`500`$ particles (and some with $`864`$ particles) in a cube $`L\times L\times L`$ with periodic boundary conditions. The temperatures studied are $`T=298,1000,3000K`$ and densities from slightly above the critical density ($`\rho _c0.54g/cm^3`$) to just below freezing, i.e. approximately $`1.95g/cm^3`$ at $`300`$K, $`2.75g/cm^3`$ at $`1000K`$ and $`4.05g/cm^3`$ at $`3000K`$ (for comparison the triple point density is $`1.14g/cm^3`$). The corresponding pressures are up to about $`1.3GPa`$, $`9.3GPa`$ and $`52GPa`$, respectively. The transport coefficients $`D`$ \- (self-)diffusion coefficient, $`\eta `$ \- shear viscosity and $`\lambda `$ \- thermal conductivity, are calculated using the Green-Kubo formalism hm . This entails determining the long time behavior of time integrals of auto-correlation functions of appropriate microscopic currents:

$`D=\underset{t\mathrm{}}{lim}D(t)`$ (2a)
$`D(t)={\displaystyle _0^t}v_{ix}(0)v_{ix}(\tau )𝑑\tau `$
$`\eta =\underset{t\mathrm{}}{lim}\eta (t)`$ (2b)
$`\eta (t)={\displaystyle \frac{1}{Vk_BT}}{\displaystyle _0^t}\sigma _{xy}(0)\sigma _{xy}(\tau )𝑑\tau `$
$`\lambda =\underset{t\mathrm{}}{lim}\lambda (t)`$ (2c)
$`\lambda (t)={\displaystyle \frac{1}{Vk_BT^2}}{\displaystyle _0^t}J_x^e(0)J_x^e(\tau )𝑑\tau `$
where $`\widehat{\sigma }`$ and $`𝐉^e`$ are the microscopic stress tensor and energy current, respectively, easily calculated in the course of molecular dynamics simulations:

$`\sigma _{xy}(\tau )={\displaystyle \underset{i}{}}\left[m_iv_{ix}(\tau )v_{iy}(\tau )+y_i(\tau )F_{ix}(\tau )\right]`$ (3a)
$`J_x^e(\tau )={\displaystyle \underset{i}{}}v_{ix}(\tau )\left\{{\displaystyle \frac{1}{2}}m_iv_i^2(\tau )+{\displaystyle \frac{1}{2}}{\displaystyle \underset{ji}{}}V_{ij}\left[r_{ij}(\tau )\right]\right\}`$
$`+{\displaystyle \frac{1}{2}}{\displaystyle \underset{i}{}}{\displaystyle \underset{ji}{}}\left[x_i(\tau )x_j(\tau )\right]𝐯_i(\tau )𝐅_{ij}(\tau )`$ (3b)
The two main sources of errors affecting the molecular dynamics calculation of transport coefficients are the system size - $`L`$ \- and the time limit - $`t_{lim}`$ \- on the calculation of the above time integrals. Finite size effects on the calculation of transport properties have been extensively analyzed and indicate that systems of 500 particles typically yield results within $`23\%`$ of the infinite system size extrapolations aw70 ; ew91 ; sh03 . The effect of an integration time limit $`t_{lim}`$ is more subtle and it has to do with the slow, algebraic decay of the Green-Kubo integrands aw70 . For usual, 3-dimensional systems these integrands behave at long times as $`\rho _\delta (t)k_\delta /t^{\frac{3}{2}}`$ ehl ; yp72 ; $`\delta `$ stands for $`D`$, $`\eta `$ and $`\lambda `$. The factors $`k_\delta `$ have been calculated using the mode-coupling formalism and depend on the system thermodynamics and on the transport coefficients themselves ehl ; yp72 . We set $`t_{lim}=0.95t_c`$, where $`t_c`$ is the time needed for a sound wave to traverse the system, $`t_c=L/c`$, $`c=(p/\rho )_s^{\frac{1}{2}}`$ (adiabatic sound speed), and add the long time contributions to the final values of the transport coefficients. We find that these corrections can be as high as $`12\%`$ for the diffusion coefficient, in agreement with ew91 , up to $`3\%`$ for the viscosity, and smaller than $`1\%`$ for the thermal conductivity. For each thermodynamic point we run the simulations for $`525`$ million time steps, which corresponds, depending on density and temperature, to $`300015000`$ samples in the averaging of the auto-correlation functions.

As mentioned, we would like to compare the simulation results with available theoretical estimates. Among them the Enskog theory cc  is perhaps the best known; its predictions for the transport coefficients of the hard sphere system are:

$`{\displaystyle \frac{D_E}{D_B}}={\displaystyle \frac{\rho b_{hs}}{y_{hs}}}`$ (4a)
$`{\displaystyle \frac{\eta _E}{\eta _B}}=\rho b_{hs}\left({\displaystyle \frac{1}{y_{hs}}}+{\displaystyle \frac{4}{5}}+0.7614y_{hs}\right)`$ (4b)
$`{\displaystyle \frac{\lambda _E}{\lambda _B}}=\rho b_{hs}\left({\displaystyle \frac{1}{y_{hs}}}+{\displaystyle \frac{6}{5}}+0.7574y_{hs}\right)`$ (4c)
where $`b_{hs}=2\pi \sigma ^3/3`$, $`y_{hs}=p/\rho k_BT1`$ and the pressure $`p`$ can be accurately calculated using the Carnahan-Starling equation hm : $`p/\rho k_BT=(1+\varphi +\varphi ^2\varphi ^3)/(1\varphi )^3`$. The right-hand-side of the above equations depends only on the hard sphere packing fraction $`\varphi =\pi \rho \sigma ^3/6`$, while the left-hand-side contains the Boltzmann transport coefficients $`D_B`$, $`\eta _B`$ and $`\lambda _B`$, obtained in the limit of low densities cc :

$`D_B=1.019{\displaystyle \frac{3}{8\rho \sigma ^2}}\left({\displaystyle \frac{k_BT}{\pi m}}\right)^{\frac{1}{2}}`$ (5a)
$`\eta _B=1.016{\displaystyle \frac{5}{16\sigma ^2}}\left({\displaystyle \frac{mk_BT}{\pi }}\right)^{\frac{1}{2}}`$ (5b)
$`\lambda _B=1.025{\displaystyle \frac{75}{64\sigma ^2}}\left({\displaystyle \frac{k_B^3T}{\pi m}}\right)^{\frac{1}{2}}`$ (5c)
with $`\rho =N/V`$ the number density, $`\sigma `$ the hard sphere diameter and $`m`$ the molecular mass.

The application of these results to real dense fluids requires suitable interpretation, and the so-called modified Enskog theory (MET) hmc  has been widely used. The MET ingredients as applied to real fluids are i) the replacement of $`y_{hs}`$ with the “thermal pressure” of the fluid in question, $`y=(p/T)_\rho /\rho k_B1`$, which is then required to equal that of the hard sphere fluid, $`y=y_{hs}`$, and therefore leads by invoking the low density limit to ii) the identification of $`b_{hs}`$ with the second virial coefficient of the real fluid and its temperature derivative, $`d[Tb(T)]/dT`$, and iii) the replacement of $`D_B`$, $`\eta _B`$ and $`\lambda _B`$ with the real dilute gas transport coefficients of the fluid considered, $`D_0`$, $`\eta _0`$ and $`\lambda _0`$. The comparison of the MET predictions with experimental results for a variety of fluids up to densities about twice the critical density is rather favorable hmc . However, a number of MET inconsistencies have been pointed out ks81 , and it is not clear if this approach would continue to be useful as the density is increased. For our MET estimates we recall that the transport coefficients of a dilute gas of molecules interacting through some general potential such as that defined in Eq. 1 can be written in the first Enskog approximation as cc :

$`D_0={\displaystyle \frac{3}{8\rho r_0^2}}\left({\displaystyle \frac{k_BT}{\pi m}}\right)^{\frac{1}{2}}{\displaystyle \frac{1}{\mathrm{\Omega }^{(1,1)}(T^{})}}`$ (6a)
$`\eta _0={\displaystyle \frac{5}{16r_0^2}}\left({\displaystyle \frac{mk_BT}{\pi }}\right)^{\frac{1}{2}}{\displaystyle \frac{1}{\mathrm{\Omega }^{(2,2)}(T^{})}}`$ (6b)
$`\lambda _0={\displaystyle \frac{75}{64r_0^2}}\left({\displaystyle \frac{k_B^3T}{\pi m}}\right)^{\frac{1}{2}}{\displaystyle \frac{1}{\mathrm{\Omega }^{(2,2)}(T^{})}}`$ (6c)
where $`\mathrm{\Omega }^{(m,n)}(T^{})`$, $`m,n=1,2`$ are dimensionless collision integrals fk  depending on the interaction potential and reduced temperature $`T^{}=k_BT/ϵ`$, that we evaluate numerically.

A different interpretation of the Enskog theory for real fluids has been advocated in ks81 , based on the use of a state-dependent hard sphere diameter directly in the Enskog relations Eqs. 4. The success of statistical mechanics theories in predicting the thermodynamics of simple fluids bh76  is largely due to the idea of equivalent hard sphere diameters, which embody the dominant effect of short range repulsions on the structure and dynamics of liquids, particularly at high densities. The appeal of using the same diameter to calculate both the thermodynamic and transport properties of fluids lies therefore both in its simplicity and physical consistency. In the present work we adopt the definition of effective diameter provided by the Mansoori-Canfield variational method bh76 , which uses the fact that the first order perturbation theory approximation for the free energy of a system interacting through potential $`u(r)`$ is an upper bound for the free energy of the system. Using the hard sphere fluid as a reference this translates into:

$`f_u(\rho ,T)f_{hs}(\varphi ,T)+12\varphi {\displaystyle _1^{\mathrm{}}}s^2g_{hs}(s;\varphi )u(\sigma s)𝑑s`$ (7)
where $`g_{hs}(s;\varphi )`$, $`s=r/\sigma `$, is the pair-correlation function of the hard sphere fluid. The optimal approximation for the free energy per particle $`f_u`$ (the interaction potential dependence is explicitly indicated for clarity) is obtained by minimizing the right hand side of Eq. 7 with respect to $`\sigma `$, which provides at fixed density and temperature an effective hard sphere diameter. Thermodynamics is then derived in the usual way by taking the appropriate derivatives. A straightforward modification of the variational procedure Eq. 7 mr79  further improves its accuracy for dense fluids tlwlw  and we use it for the calculation of the “thermal pressure” necessary for the MET estimates.

It is worth noting that the effective hard sphere diameter approach is not necessarily tied to the use of the Enskog theory, and can be interpreted more generally as a test of single-variable scaling for the transport properties of fluids modeled by realistic pair interactions. Similar ideas have been considered for the particular case of inverse power-law potentials ah75 . Perhaps even more importantly, this can also be viewed in the larger context of trying to uncover universal features of the transport properties of real fluids by mapping them into those of a reference system, e.g. hard sphere fluid. Using a so-called “entropy packing fraction” suggested by the variational method Eq. 7, a connection between transport coefficients and thermodynamic properties, specifically excess entropy (with respect to the ideal gas) per particle $`s_e`$,

has been proposed more than 20 years ago yr77 . Another version of the excess entropy idea for the particular case of diffusion has been more recently suggested md96 , and we would like to analyze it here for the case of dense argon.

The relationship between the diffusion coefficient and excess entropy postulated in md96  is:

$`D^{}={\displaystyle \frac{D}{\sigma ^2\mathrm{\Gamma }_E}}=C\mathrm{exp}(s_e/k_B)`$ (8)
where the hard sphere diameter $`\sigma `$ and the Enskog collision frequency $`\mathrm{\Gamma }_E=4\sigma ^2g(\sigma )\rho \sqrt{\pi k_BT/m}`$ are assumed to be the relevant length and time scale respectively, and $`C`$ is believed to be an universal constant. A certain definition for $`\sigma `$ and the contact value of the pair correlation function $`g(\sigma )`$, along with an approximation for $`s_e`$ has also been suggested for real systems md96 . Here we use the definition of $`\sigma `$ provided by Eq. 7 and the values for $`s_e`$ and $`g(\sigma )`$ (which we denote by $`g_c(\varphi )`$ to make explicit the dependence on $`\varphi `$) obtained from the Carnahan-Starling equation of state hm :

$`{\displaystyle \frac{s_e}{k_B}}={\displaystyle \frac{4\varphi 3\varphi ^2}{(1\varphi )^2}}`$ (9a)
$`g_c(\varphi )={\displaystyle \frac{2\varphi }{2(1\varphi )^3}}`$ (9b)
Using this scaling the argon simulation results at the three temperatures studied are presented in Fig. 1 together with the diffusion coefficient of the hard sphere system ew91 ; the universal curve proposed in md96 , i.e. Eq. 8, is also shown.

We find that single-variable scaling based on the effective hard sphere diameter of Eq. 7 holds rather well, and the agreement with he hard sphere fluid diffusion coefficient is also reasonable. However, Eq. 8 appears to be valid only in a limited range of excess entropies $`s_e`$, as already remarked in cr00 ; jb02 .

The discrepancy at lower (in absolute value) $`s_e`$, i.e. smaller packing fractions $`\varphi `$, is severe and somewhat troublesome given that the Enskog theory, upon which the proposed relationship is loosely based, performs well precisely in that domain. To understand the problem with the scaling introduced in Eq. 8 we note that the left-hand-side of that equation can be written up to a multiplicative constant as $`D/D_Bg_c(\varphi )\varphi ^2`$. Therefore, in the limit of a dilute system, $`\varphi 0`$, this term will diverge as $`1/\varphi ^2`$, while the right-hand-side of Eq. 8 will go to the constant $`C`$. This behavior, which is observed in Fig. 1, should be expected for any reasonable definition of $`\sigma `$ and $`g(\sigma )`$ and $`s_e`$ approximation.

In order to avoid this pathology we could for example replace $`\sigma `$ as the preferred length scale with $`l1/\rho \sigma ^2`$, the Boltzmann mean-free path. The new relationship is then:

$`D^{}={\displaystyle \frac{D}{D_Bg_c(\varphi )}}=\mathrm{exp}(C_0s_e/k_B)`$ (10)
where we introduced a different constant $`C_0`$. The test of this suggested dependence is shown in Fig. 2. The hard sphere results are very well represented by the new equation with $`C_0=0.80`$, while for the argon results a better fit is $`C_0=0.83`$. It may be interesting to test the validity of Eq. 10 for other systems as well, e.g. liquid metals has ; dd02 . We also show for comparison the predictions of the effective diameter Enskog theory. The disagreement with the simulation results is similar with the one observed for the hard sphere fluid ew91 , and it is even bigger for MET (not shown).

The diffusion theory of Cohen and Turnbull ct  builds upon the physical concept of “free-volume” $`v_f`$ available for a molecule, originally introduced by Van der Waals to account for the effect of short range repulsive forces between molecules. The diffusion coefficient is written as:

$`D=ga(v^{})v_T\mathrm{exp}(\gamma v^{}/v_f)`$ (11)
where $`g`$ is a geometric factor, $`a(v^{})`$ is roughly the diameter of the neighbor-induced “cage” inhabited by a molecule, $`v_T`$ is the thermal velocity and $`v^{}`$ is essentially proportional with the molecular volume $`v_0=\pi \sigma ^3/6`$ and can be identified with it with a suitable rescaling of the constant $`\gamma `$. This theory has been recently recast in a more transparent form as an Arrhenius theory of activation re02 . The transformation is done by recognizing first that in the limit of large free volumes relative to the molecular volume, $`v_fv_0`$, the Boltzmann result for the diffusion coefficient should be recovered. Second, the free volume $`v_f`$ is expressed in terms of an effective pressure $`p_r`$ that includes only the repulsive (excluded volume) contributions, in the spirit of the Van der Waals theory: $`p_rv_f=k_BT`$. The proposed relation for $`D`$ is:

$`{\displaystyle \frac{D}{D_B}}=\mathrm{exp}(\zeta W/k_BT)`$ (12)
where $`\zeta `$ is a constant and $`W=p_rv_0`$ is interpreted as the work necessary to create a void of volume $`v_0`$ in the liquid under the effective pressure $`p_r`$, to be occupied by the diffusing molecules. The ambiguity in defining this pressure is solved by recasting the usual pressure equation for a liquid into a generalized Van der Waals form re02 . There remains the task of defining a suitable hard core diameter $`\sigma `$, which can be avoided for the scaling factor by using $`D_0`$ instead of $`D_B`$, but it is required for $`v_0`$. Eq. 12 has therefore been applied only to systems modelled by interactions that explicitly include a hard core, e.g. hard sphere with an attractive square well re02 . We note that in fact Eq. 12 is unambiguously defined for a hard sphere fluid:

$`{\displaystyle \frac{D}{D_B}}=\mathrm{exp}(\zeta W_0/k_BT)`$ (13)
where $`W_0/k_BT=pv_0/k_BT=\varphi (1+\varphi +\varphi ^2\varphi ^3)/(1\varphi )^3`$ and we used the Carnahan-Starling equation for the pressure. This can then be easily applied to typical Van der Waals-like potentials,

e.g. that of Eq. 1, by using the hard sphere effective diameter given by Eq. 7. The scaled argon simulation results are shown in Fig. 3 as a function of $`W_0/k_BT`$. The data is well fitted by $`\zeta =0.45`$; a better representation is obtained with an additional prefactor, i.e. $`A_0\mathrm{exp}(\zeta W_0/k_BT)`$, for both argon and the hard sphere fluid, albeit with different $`\zeta ^{}s`$. Nevertheless, as seen for example in Fig. 2, the mapping of the argon diffusion constant into that of the hard sphere fluid is more accurate than the Enskog theory except in a very narrow domain of intermediate densities.

We now turn to the discussion of the collective transport coefficients shear viscosity $`\eta `$ and thermal conductivity $`\lambda `$ using the same effective diameter approach. The Boltzmann-scaled simulation results for the argon viscosity, $`\eta /\eta _B`$, are shown in Fig. 4 as a function of the effective packing fraction $`\varphi `$. Similarly with diffusion, single-variable scaling appears to hold rather well and the behavior of the viscosity largely mirrors that of the hard sphere fluid (not shown). Given that the Enskog theory strongly underestimates the hard sphere values at

high densities agw ; sh03 , it is not surprising that both adaptations of the theory, effective diameter Enskog and modified Enskog (MET), fail to capture the steep rise of $`\eta `$ as the system moves closer to freezing. Nevertheless, there are significant differences between the two approaches. The modified Enskog theory appears to work well at lower densities, as observed in hmc , and slightly better than the effective diameter version. This however reverses quickly as the density increases, with the effective diameter method emerging as a much better estimator than MET at high densities. Although it may be interesting to pinpoint the origin of this different behavior, which also occurs for the thermal conductivity, this is difficult due to the convoluted nature of MET. It suffices perhaps to remark that a large part of the difference between the two procedures at high densities is due to a smaller $`y`$ (see Eqs. 4 and below) in the MET approach, which is proportional with the Enskog theory collision frequency. The rapid increase of $`\eta `$ at large packings may be better reproduced by assuming that the diffusion constant is inversely proportional with the shear viscosity, i.e. the Einstein relation, $`D=k_BT/c\eta \sigma `$ agw . We find that the ’slip’ boundary condition $`c=2\pi `$ provides a reasonably good match to the $`\eta `$ dependence on $`\varphi `$ in the dense region erd , in agreement with agw .

Among the transport properties of the hard sphere system the thermal conductivity is most accurately predicted by the Enskog results up to the liquid-solid transition agw ; sh03 . It is therefore important to assess if the success of the theory can also be transferred to fluids well described by Van der Waals-type potentials, e.g. argon. As shown in Fig. 5 the effective hard sphere diameter allows again a very good single-variable representation of the thermal conductivity for all temperatures studied. Moreover, the use of this diameter in the Enskog relation is successful in modeling the simulation results over the entire range of densities simulated. The modified Enskog theory (MET) on the other hand yields increasing discrepancies as the density rises and it is therefore not appropriate at high pressures.

Finally, it would be desirable to test the above methods for the calculation of transport coefficients against real dense fluids experimental data. Unfortunately, these are somewhat scarce. For example, only thermal transport measurements have been performed up to GPa pressures tn80 ; ngt , and recently extended to tens of GPa just for the case of oxygen asb . We limit ourselves therefore to the available high pressure thermal conductivity data and consider here argon ($`Ar`$), neon ($`Ne`$), nitrogen($`N_2`$) and oxygen ($`O_2`$). The first two of these are monoatomic fluids naturally modeled by isotropic potentials. The last ones are small diatomics, but a spherical interaction approximation turns out to be very successful in predicting the thermodynamics of these molecular systems in

a wide domain of temperatures and pressures rr80 ; sjh ; br00 . All are well described by Buckingham exponential-6 potentials with $`\alpha =13.2`$; the other parameters are: ($`ϵ^{Ar}/k_B=122K`$, $`r_0^{Ar}=3.85`$Å) rmbx  \- also used in simulations, ($`ϵ^{Ne}/k_B=42K`$, $`r_0^{Ne}=3.18`$Å) vsyr , ($`ϵ^{N_2}/k_B=101.9K`$, $`r_0^{N_2}=4.09`$Å) rr80 , ($`ϵ^{O_2}/k_B=125K`$, $`r_0^{O_2}=3.86`$Å) vtr . The experimental results that we use for comparison are the ones of tn80 ; ngt ; asb  and also hmr82 . The calculation of the effective diameters is done as before with the use of Eq. 7 and results are shown in Fig. 6.

The success of single-variable scaling for both monoatomic and small diatomic molecules through the use of the effective hard sphere diameter is remarkable. The resulting master curve is also in very good agreement with the Enskog prediction in a large domain of packing fractions, which appears to roughly coincide with the equilibrium hard sphere fluid region that extends up to $`\varphi 0.494`$. While a comparison between systems described by different types of interactions or at least Buckingham potentials with different $`\alpha `$’s would be a more stringent test of the existence of an universal curve for the scaled thermal conductivity, the agreement with the Enskog theory lends very good support to this idea for fluids that are well modeled by classical Van der Waals-like potentials.

The disagreement at the largest $`\varphi `$’s is rather interesting, particularly because the Enskog theory is known to slightly underestimate the thermal conductivity of the hard sphere system in the dense regime agw ; sh03 . The corresponding experimental data have been recently obtained for dense oxygen asb . Since the oxygen molecule is in fact anisotropic the observed discrepancy, where the effective diameter Enskog prediction significantly overestimates the experimental values, could be reasonably attributed to a breakdown of the spherical potential approximation at high densities. The fact that most calculated effective packing fractions lie in the metastable region of the hard sphere liquid, which is unexpected for an equilibrium fluid if it is fully modeled by Van der Waals-type interactions, also seems to support this idea note . This breakdown however appears to be rather subtle because the thermodynamics based on Eq. 7 and the Buckingham exponential-6 potential still reproduces very well, within approximately $`2\%`$, all oxygen densities measured in the experiments.

Molecular dynamics calculations of the transport properties of hard ellipsoids, which should be a better approximation for the $`O_2`$ molecule at high densities, indicate that if the system is dense even a small molecular anisotropy decreases the thermal conductivity compared to the hard sphere system btae . This can be understood intuitively as follows: for very dense systems the collisional contribution to thermal conduction is dominant eucken , but the energy transfer in collisions is less “efficient” for hard anisotropic bodies than for isotropic ones. This “efficiency” is even further reduced for molecules such as $`O_2`$ that also posses vibrational degrees of freedom. For example, the energy exchange between translations and vibrations can involve exceedingly long relaxation times compared to those typical for translations alone cgp . Such effects severely limit the usefulness of the hard sphere system as a reference for the description of transport properties of dense systems with multiple - translational, rotational, vibrational - degrees of freedom, even when that may still be appropriate for thermodynamics. This would also suggest that in this case, in addition to thermodynamics, structural properties may become increasingly important in determining dynamical behavior at high densities. With respect to the Enskog approach, the assumption of a single relaxation time appears already to be its major drawback for such systems, even when the anisotropy, for example, is partly accounted for btae .

The preceding analysis indicates that the thermal conductivity of nitrogen ($`N_2`$), whose molecular size is comparable to that of $`O_2`$, will likely exhibit a similar behavior at high pressures when described in terms of an effective diameter, while even larger deviations should be expected for more anisotropic molecules, e.g. $`CO_2`$. Moreover, the above discussion should also apply to the viscosity mutatis mutandis btae . High pressure experimental data on the transport properties of these or similar molecular systems, although difficult to obtain asb , would help in understanding the interplay between thermodynamic and structural properties on the one hand, and transport behavior on the other, for very dense fluids.

I would like to thank E. Abramson for kindly providing the data published in asb . This work was performed under the auspices of the U. S. Department of Energy by University of California Lawrence Livermore National Laboratory under Contract No. W-7405-Eng-48.


format: text

text:
# An Analytical Expression for the Non-Singlet Structure Functions at Small 𝑥 in the Double Logarithmic Approximation

## Acknowledgments

The author is very grateful to Jochen Bartels for reading of the manuscript and for the fruitful collaboration in Ref.  which lead to the observation reported in this paper.
The author would like to thank Andrei Kataev for a very informative and stimulating discussion.
The valuable comments from Johannes Bluemlein, Boris Ermolaev and Yura Kovchegov are greatly acknoledged.


text:
# New optical spectra and general discussion on the nature of ULX’s

## 1 Introduction

Numerous X-ray sources have been found in the central regions of nearby galaxies such as M 31 and succesfully attributed to the presence of X-ray binary stars (e.g. Supper et al. 1997). A number of objects with much greater luminosities in the range $`L_X=10^{39}`$ to $`10^{41}`$ erg s-1 have also been found in nearby galaxies. In that case they are designated “Ultra Luminous X-ray sources” (ULX’s). It has been proposed that they are exceptionally massive black hole binaries. If, however, at the distance of the parent galaxy a source has an X-ray luminosity exceeding about $`L_X=10^{38.5}`$ erg s-1, it needs to be more massive than a normal stable star (Pakull & Mirioni 2002 quote an Eddington limit as the upper bound on the luminosity of an accreting star as $`L_X=10^{38.1}M/M_o`$ erg s-1 and Foschini et al. (2002a) quote $`L_X=10^{38.3}`$ ergs-1 as the most luminous X-ray binaries in M 31). Other explanations have been proposed in terms of black holes in globular clusters (Angelini et al. 2001), or associations with HII regions (Roberts et al. 2003, Pakull & Mirioni 2002, Wang 2002, Gao et al. 2003). Alternative explanations have been proposed in terms of non-isotropic emission of the radiation (King et al. 2001; Körding et al. 2002). But, as discussed here, an important fraction of the ULX’s which have been so far spectroscopically observed have higher redshift than the parent galaxy. So currently, the nature of these objects remains unexplained, and it is necessary to rexamine the assumption that they are physically associated with the galaxies in which they are found.

The most extensive catalog of ULX’s is the one presented by Colbert & Ptak 2002 (CP02 hereafter) in which 87 ULX’s in the near field of 54 RC3 galaxies with $`cz5000`$ km s-1 are compiled. However, these authors have filtered out known quasars and X-ray supernova. We think this is unjustified until the true nature of the ULXs become clear. In this paper we do not remove such objects, use only the $`L_X`$ criterion to define ULX objects and change slightly the range in X-luminosity to define ULXs, $`L_X10^{38.5}`$ erg s-1. To disentangle the nature of these objects it is necessary to find their possible optical counterparts and identify their characteristic optical spectral features. However, this is not an easy task (see Foschini et al. 2002b) due to the uncertainties in the X-ray coordinates and the faintness of many of these objects. In this paper we present the optical identification and spectroscopic observations of three ULX’s, two of them (IXO1 and IXO2 according to the notation used in CP02) in the field of the galaxy NGC 720 and one (IXO5) around NGC 1073.

## 2 Observations and data reduction

We found probable optical counterparts in the Digital Sky Survey (DSS) plates for objects IXO1 and 2 around NGC 720 (the existence of the optical counterparts of these two objects was pointed out by CP02) and IXO5 around NGC 1073. Figure 1 shows DSS plates centered on NGC 720 and NGC 1073, and the position of the possible optical counterparts of the IXO objects. We obtained long-slit spectroscopy of these three objects with the WHT111The William Herschel Telescope (WHT) is operated by the Isaac Newton Group and the IAC in Spain’s Roque de los Muchachos Observatory. on 28 -29 Dec. 2002. We used the red arm of the ISIS spectrograph with the grism R158R. The slitwidth was 1 arcsec. This provides a sampling of 1.62 Å pixel-1 and a resolution of 8 Å. For each object we took a single image with a exposure time of 1800 sec. The data were reduced using IRAF222IRAF is the Image Reduction and Analysis Facility, written and supported by the IRAF programming group at the National Optical Astronomy Observatories (NOAO) in Tucson, Arizona.. Further details of the observing conditions and data reduction can be found in López-Corredoira & Gutiérrez (2003).

The extracted spectra of the three objects are presented in Figure 2. All of them are emission line objects. It is evident from the optical spectra that objects IXO1 and IXO2 around NGC 720 are normal appearing quasars. From the main spectral features indicated in Figure 2, we obtain redshifts of $`z`$ = 2.216 and $`z`$ = 0.964 for IXO1 and IXO2 respectively. Given the paucity of quasars and the fact these have strong X-ray emission, we think the identification of these objects is unequivocal.

The optical object that we have identified with IXO5 has strong narrow emission lines. From the position of the main lines we measure a redshift of $`z=0.0040`$ or in velocity 1200 km s-1. According to the ratio of OIII(5007)/H$`\beta `$ and H$`\alpha `$/NII(6584), this object should be a HII region. Its redshift is similar to that quoted in NED for the galaxy NGC 1073 and it is in a region close to one of the spiral arms. The abundance of HII regions in the spiral arms makes the identification of the optical counterpart of the X-ray emission not as clear as for the objects IXO1 and IXO2 (furthermore there are a much fainter optical sources near this HII region as can be seen in Figure 1). In any case, if the identification is correct, IXO5 would be associated with ionized gas, with the X-ray photons of the ULX as the possible source of ionization. Gao et al. (2003) have found more than a dozen of ULX’s apparently associated to the outer, active star-forming ring in the Cartwheel ring galaxy.

## 3 A compilation of ULX’s identified as quasars

In Table 1 we present a compilation from the literature of objects which fit the definition of ULX’s and have been spectroscopically identified. Three of the objects (the ones denoted as IXO1, 2 and 43) are listed as ULX’s in CP02. The rest of the objects, although they fit the observational criteria of classification as ULX, were not included in the above catalog apparently because they were known quasars with higher redshift than the parent galaxy. The parameters quoted in this table are:

Column 1: The designation ULX (or IXO in the CP02 catalog) is based on a $`\mathrm{log}L_X38.5`$ erg s-1 as estimated in Col. 5.

Column 2 and 3: The Right Ascension and declination of each object (epoch 2000).

Column 4: The X-ray counts/ks measured whenever possible from the ROSAT HRI detector in order to match as closely as possible the CP02 flux criteria. In a few cases outside the HRI field they were estimated from PSPC observations.

Column 5: The X-ray luminosity $`(\mathrm{log}L_X)`$ if the ULX’s are at the same distance as the associated low-redshift galaxies (see discussion below). If the ULX’s were not at the same distance, the real luminosities would have to be multiplied roughly by $`\left(\frac{d_{\mathrm{ULX}}}{d_{\mathrm{galaxy}}}\right)^2`$. Except for the IXO’s, most of these values have been calculated by the relation between the HRI counts/ks and the CP02 luminosities.

Most of the galaxies have redshift $`0.003z0.005`$ where the contribution to this redshift from their peculiar velocities could be significant. Therefore, except for NGC 720, NGC 4168 and NGC 4258 the distances used for the ULX’s in Table 1 are the distance to the associated Local Supercluster, 15.3 Mpc. (Hubble Key Project, Freedman et al. 2001). The flux calculations vary somewhat from hard to soft bands and the raw counts are subject to variability in most sources. We have only attempted to get the calculated luminosities approximately on the scale of other catalogs.

Column 6: The redshift ($`z_Q`$) measured for the object which has been optically identified with the X-ray source.

Column 7: The apparent magnitude is in the V band but in a few cases in other bands as individually noted in Véron-Cetti and Véron (2000).

Column 8 and 9: The name and redshift ($`z_G`$) of the host or parent galaxy.

Column 10: The radial distance ($`r`$), in arcmin, from the center of the galaxy to the position of the ULX. This usually is about 4 - 5 arcmin for IXO identifications but we have included a few here with slightly larger acceptance distances as individually noted.

Column 11: The absolute optical magnitude (see above note in column 7).

Column 12: A note to indicate BL Lac type objects.

Column 13: References

### 3.1 Comments on Individual objects

* NGC 720: These two IXO’s lie very close to a bright ($`B_T=11.15`$ mag) E galaxy. The galaxy is a very strong ROSAT X-ray source which emits 148 cts/ks. Moreover, there is a strong, “twisted”, X-ray jet/filament which curves southward as it emerges from the nucleus (Buote and Canizares 1996). In addition to the two ULX’s, X-ray quasar candidates of similar apparent magnitude are conspicuous at larger radial separations from NGC 720 (see “Catalogue of Discordant Redshift Associations”, Arp 2003).
* NGC 1073: In the CP02 catalog there are two X-ray sources in this galaxy which are at about the same distance from the nucleus and much brighter in X-rays than the source which they designated IXO 5 (this is associated to a HII region if our identification was correct, as said). These two were not include in the IXO CP02 catalog because it was known that they were quasars (Arp and Sulentic 1979; Burbidge et al. 1979). But clearly these fit the definition of ULX’s and are listed in Table 1. Also included in Table 1 is the third known quasar in NGC 1073 since it has $`\mathrm{log}L_X=38.7`$ erg s-1 only slightly above the general criterion for ULX’s. The strong X-ray quasar with $`z`$ = 1.411 is also a strong radio source. Since high redshift compact objects which are strong in both X-ray and radio are generally now regarded as BL Lac type objects it is noted in the last column of Table 1.
* NGC 1365: This is a well known Seyfert Galaxy in the Fornax Cluster. About 12 arcmin to the SE in the direction of its extended spiral arm lies a very strong X-ray BL Lac (Arp 1998, p. 49). The distance to the Fornax Super Cluster is about the same as to the Virgo Super Cluster in the opposite direction in the sky, or about 15 Mpc (or see Arp 2002 for a Cepheid distance of 18 Mpc). With this distance to NGC 1365, the BL Lac object comes within the acceptance radius of the IXO Catalog and is included in Table 1.

Closer in radial separation on the other side of NGC 1365 is a strong X-ray source with $`z`$= 0.904 (La Franca et al. 2002).
* NGC 3628: This starburst/low level AGN exhibits extensive outgassed plumes of neutral hydrogen and is apparently ejecting X-ray material along its minor axis. Point X-ray sources might be associated with this ejected material and a number have already turned out to be quasars (Arp et al. 2002). We lists 7 of these quasars which have $`\mathrm{log}L_X`$ between 38.8 and 39.6 erg s-1. Column 10 shows that six of these quasars fall within the same radial distances as most of the ULX’s in this Table. The seventh, which has the strongest, $`\mathrm{log}L_X=39.6`$ erg s-1, falls at a greater distance, very similar to the radial distance of the bright BL Lac from NGC 1365.
* NGC 4151: There is a powerful X-ray source only 4.9 arcmin N of this active Seyfert galaxy. It is also a strong radio source (de Ruiter, Arp, Willis 1977) but, surprisingly, quite faint optically. Later it was shown that there was an X-ray filament apparently linking this $`z`$= 0.615 BL Lac quasar to the nucleus of NGC 4151 (Arp 1997, Fig. 17). The object should have been included in the CP02 catalog but they centered their field to the SW of NGC 4151, just leaving it out of their frame. As a result this important BL Lac object was not listed as an IXO.

A very interesting object SW of NGC 4151 was, however, listed as IXO 43. It turns out to be a galaxy on the end of a chain of seven or eight galaxies (Arp 1977). This end galaxy on the chain has an emission spectrum of about z = 0.239 and is apparently the identification of the Ultra Luminous X-ray Source (IXO 43). Three other members of the chain have redshifts near $`z`$= 0.160 and there are indications of absorption redshifts of $`z`$= 0.04 to 0.06.
* NGC 4168: A faint AGN galaxy at redshift $`z=0.217`$ is the ULX close to this Seyfert 1 galaxy which has $`z=0.0076`$ (Masetti et al. 2003). It is similar to the objects found in the filament from the Seyfert NGC 7603 (López-Corredoira and Guitiérrez 2002, 2003). Masetti et al. title their paper ”Yet another galaxy identification for an ultraluminous X-ray source”.
* NGC 4203: A remarkably similar object to the $`z`$= 0.615 BL Lac object near NGC 4151, is the strong X-ray source only 2.1 arcmin from NGC 4203. It has a redshift of $`z`$= 0.614. This is another source which was not included in the CP02 catalog due to previously known high redshift.

NGC 4203 is a liner type AGN with broad Balmer lines. It is also a strong X-ray source and an IRAS infrared source. IXO 45 is just W of the BL Lac, Tonanzintla 1480, and optically identified with a blue quasar candidate. Chandra snapshots of this field show the galaxy X-ray emission and the strong emission of the adjacent ULX’s (Terashima and Wilson 2003).
* NGC 4258 is a Seyfert II galaxy with ”anomalous” spiral arms. The distance used to compute the X-ray emission is 6.4 Mpc. More details can be found in Vogler & Pietsch 1999.
* NGC 4319: This is an unusually disrupted spiral with a well known quasar/AGN, Markarian 205, only 40 arc sec south of its nucleus. As Table 1 shows this ULX is exceptionally strong in X-rays, the strongest in the Table at $`\mathrm{log}L_X=41.5`$ erg s-1, if it were at the redshift distance of NGC 4319, and much larger luminosity if the redshift were cosmological.
* NGC 4374: This is a large radio galaxy. The close X-ray source has long been known as a quasar of z=1.25. Again, this was not included in the CP02 catalog just because its known high redshift.
* NGC 4698: The central galaxy here is a bright nearby Seyfert 2 galaxy. Foschini et al. (2002c) identified a ULX within only 73 arcsec of the nucleus of the galaxy. If it was an object at the same distance as the galaxy it would have a luminosity of $`\mathrm{log}L_X=39.5`$ erg s-1. This ULX, however, turned out to be a quasar of $`z`$= 0.43. In fact it turned out to be a pure absorption line BL Lac quasar which is a very rare type of object. Its apparent magnitude was quite red, $`B`$ = 21.3 and $`R`$ =19.6 mag. In order to get it roughly on the $`V`$ system we take a mean of these and get an absolute magnitude of $`M_{abs}=10.4`$ mag, corresponding roughly to the lower limit of the optical luminosities of the ULX/quasars in Table 1.

Note It is perhaps significant that almost exactly on a line through the nucleus of NGC 4698, extended beyond the BL Lac, is another, stronger X-ray source, 1RXS J124828.2+083103. It has a redshift of $`z`$ = 0.120. Extended further beyond that is a line of fainter galaxies of unknown redshift (Forschini et al. 2002c). It is very similar to the lines of galaxies extending from active low redshift galaxies that were found in (Arp 2001b).

## 4 Discussion

Data available so far and compiled in Table 1 indicates that at least an important fraction of the ULX’s are quasars. However, there is one respect in which the ULX quasars are different from the general run of quasars. Out of the 10 galaxies listed in Table 1, six have strong BL Lac objects associated with them as ULX’s. A further case was recently discovered: in a recent Chandra investigation of the multiple interacting nuclei of NGC 4410 a possible population of ULX sources were investigated. Nowak et al. (2003) reported: “One of these sources is clearly associated with a radio point source, whereas another source (in fact the brightest in the system), may also be associated with radio emission”.

### 4.1 Excess of X-ray quasars around active galaxies

A first observation is that almost every one of the galaxies which have associated ULX’s in Table 1 are Seyfert, starburst, radio or AGN active galaxies. One might argue that these are selectively the most X-ray observed class of galaxies, nevertheless it is striking that there is not even one, normal quiescent galaxy among the group. A systematic study of the kinds of galaxies most associated with quasars and ULX’s would be useful. Apparently this is in disagreement with the paper by Humphrey et al. (2003) which states that they found, with Chandra, 22 ULX’s in a sample of 13 normal galaxies. However the 7 galaxies from which those 22 ULX’s actually come, include a Liner/AGN, a Seyfert, an X-ray cluster, an interacting radio X-ray pair (Arp 281) and a strong radio ejecting galaxy in the center of the Fornax Cluster (NGC 1399). For their five least active galaxies only one candidate ULX was found. So, it seems that in fact the active galaxies do preferentially produce the ULX’s.

In their study of X-ray sources in fields around bright Seyfert galaxies, Radecke (1997) and Arp (1997) showed that there was an overdensity of bright, point X-ray sources compared to control fields at a significance level of $`7.5\sigma `$. According to the present paper, these X-ray sources consistently turn out to be mostly quasars of a normal range in redshift. The radii from the central galaxy within which these X-ray quasars were found was roughly 5 to 50 arcmin (from the outer edges of the galaxies to the field limit of the PSPC, ROSAT detector). In the present case of the ULX’s, the majority are found within about 5 arcmin of the central galaxy. Roughly speaking, there is a difference of about 100 in the areas concerned so that the chance of finding unrelated background sources is roughly 1/100 of the probability in the larger area in which the $`7.5\sigma `$ association was found. When some ULX’s turned out to be much higher redshift, each of these was relegated, on an individual basis, to be a background source. Now, however, we have about 20 cases, all turning out to be quasars but not one with a binary stellar spectrum.

Of the 24 Seyferts investigated in Radecke (1997) and Arp (1997) only four had BL Lac’s associated. But it should be noted that those BL Lac’s were the most significant associations with the surveyed active galaxies. Just by themselves the chance of finding those four was $`2\times 10^9`$. Here in Table 1 we see two of those previous BL Lacs (with NGC 1365 and NGC 4151) but in addition, four new ones, four of which are extremely close, between 2.1 and 1.2 arcmin of the host galaxy so the probability to have them as background sources is much lower. The question then is: why would BL Lacs be more closely associated than ordinary quasars with Seyfert, starburst, radio or AGN galaxies?

### 4.2 Very bright, off nuclear, Chandra ULX’s

Active galaxies like NGC 3628, Arp 220 and M 82 are now known to have very bright, ULX sources very close to their nuclei. Because these are generally even more X-ray luminous than the ones discussed here it would be especially important to attempt optical identifications with high resolution telescopes. For instance in NGC 3628 a source $`\mathrm{log}L_X=40`$ only 20 arcsec from the nucleus is reported as violently variable (Strickland et al. 2001). Arp 220 has a source $`\mathrm{log}L_X=40.6`$ erg s-1 only 7 arcsec off nucleus (Clements et al. 2002). NGC 7319, the Seyfert Galaxy in Stephan’s Quintet has a ULX only 8 arcsec S of its nucleus.(Trinchieri et al. 2003); it is identified with a stellar appearing object at $`B`$ = 21.78 mag (Galianni & Arp in preparation). M 82 has its most luminous X-ray source variable between $`\mathrm{log}L_X40`$ to 41 erg s-1 (Matsumoto et al. 2001) lying within 8 arcsec of the M82 nucleus, but no optical identifications have been made so it can only be surmised that it would turn out to be like, or a precursor of, the ULX’s for which we have spectra in the present paper.

### 4.3 Possible interpretation

Arp (1987,1998) suggested that quasars emerge from the nuclei of galaxies. In that model the quasars or proto quasars must pass out from the nucleus and out through the body and immediate environments of the galaxy before arriving at the distances where they have been shown to be physically associated. In this case they must pass through the region in which the present ULX’s have been identified. It was therefore predicted that we should observe quasar-like objects in just the region in which observers are reporting ULX’s (see Burbidge, Burbidge and Arp 2003a). Seyfert, starburst, radio or AGN active galaxies would be the parent ejecting galaxies. Rare cases such as the ULX in NGC 4698 (see Table 1), where there are no optical emission lines would represent a recent or strong internal burst or external interaction which removed even the usual gaseous, optical emission regions leaving only the core of absorption line stars. This model also gives a possible evolutionary connection between recent observations of HII and other narrow line galaxies and the ejection of quasars. Several high or medium redshift emission line objects apparently emerging from low redshift active galaxies either in or entraining luminous filament/arms are given in the literature: NGC 4151 (Arp 1977, 2003), NGC 1232 (Arp 1982, 2003), NGC 7603 (López-Corredoira & Gutiérrez 2002, 2003), NEQ3 (Arp 1977, Gutiérrez & López-Corredoira 2003), NGC 1365 (Roy & Walsch 1997), NGC 3628 (Arp et al. 2002), 53W-003 (Arp 1999b), NGC 2639 (Arp, Burbidge and Zibetti, A&A submitted), etc. Many of these systems are known to have ULX’s. Obviously deeper multi-color images and Chandra333It must be noted, however, that an application to make an observation of NGC 7603 with Chandra was turned down; as a consequence we do not know if the two HII galaxies in the bridge are X-ray sources nor do we know what else this active Seyfert contains. X-ray observations should yield important results on all of these objects.

Another suggested explanation for these association of galaxies and quasars with different redshift is mesolensing by King objects. In López-Corredoira & Gutiérrez (2003) this is discussed in more detail.

## 5 References

Angelini, L. et al. 2001. ApJ, 557, L35

Arp, H. 1977, ApJ, 218, 72

Arp, H. 1982, ApJ, 263, 54

Arp, H. 1987, Quasars, Redshifts and Controversies 1987, Interstellar Media, Berkeley

Arp, H. 1997, A&A, 319, 33

Arp, H.C. 1998, ”Seeing Red”(Apeiron, Montreal)

Arp, H. 1999b, ApJ, 525, 594

Arp, H. 2001b, ApJ, 549, 802

Arp, H. 2002, ApJ, 571, 615

Arp, H. 2003, ”A Catalogue of discordant Redshift Associations”, Apeiron, Montreal, in press

Arp, H., & Sulentic, J. 1979, ApJ, 229, 496

Arp, H., Burbidge, E. M., Chu, Y., Flesch, E., Patat, F., & Rupprecht, G. 2002, A&A, 391, 833

Buote, D., & Canizares, C. 1996, ApJ 468, 184

Burbidge, E.M., Junkkarinen, V., & Koski, A. 1979, ApJ 233, 97

Burbidge, E.M., Burbidge, G.R., & Arp H.C. 2003, A&A, 400, L17

Clements, D. et al. 2002, ApJ, 581, 974

Colbert, E. & Ptak, A. 2002, ApJS, 143, 25

de Ruiter, H., Arp, H., & Willis, A. 1977, A&AS, 28, 211

Foschini, L., Di Cocco, G., Ho, L. C., et al. 2002a, A&A, 392, 817

Foschini, L., et al. 2002b, astro-ph/0209298

Foschini, L., Ho, L., Masetti, N., et al. 2002c, A&A, 396, 787

Freedman, W., Madore, B., Gibson, B. et al. 2001, ApJ, 553, 47.

Gao, Y., Wang, Q. D., Appleton, P. N., & Lucas, R. A. astro-ph/0309253

Gutiérrez, C. M, & López-Corredoira, M. 2003, A&A, submitted (letter)

Humphrey, P., Fabbiano, G., Elvis, M., Church, M., Balucinska-Church, M. 2003, astro-ph/0305345

King, A. R., Davies, M. B., Ward, M. J., Fabbiano, G., & Elvis, M. 2001, ApJ, 552, L109

Körding, E., Falcke, H., & Markoff, S. 2002, A&A, 382, L13

La Franca, F.; Fiore, F.; Vignali, C., Antonelli, A., Comastri, A., Giommi, P., Matt, G., Molendi, S., Perola, G., Pompilio, F. 2002, ApJ 570, 100

López-Corredoira, M., & Gutiérrez, C. M. 2002, A&A, 390, L15

López-Corredoira, M., & Gutiérrez, C. M. 2003, A&A, submitted

Masetti, N. et al. 2003, ApJ, 406, L27

Matsumoto, H., Tsuru, T., & Koyama, K., 2001, ApJ, 547, L25

Nowak, M., Smith, B., Donahue, M., & Stocke, J. 2003, AAS Head Meeting 35, 13.16

Pakull, M.W. and Mirioni, L. 2002, astro-ph/0202488

Radecke, H.-D. 1997, A&A 319, 33

Roberts, T. P., Goad, M. R., & Warwick, R. S. 2003, MNRAS, 342, 709

Roy, J.-R., & Walsh, J. 1997, MNRAS, 288, 715

Strickland, D., Colbert, E., Heckman, T., et al. 2001, ApJ, 560, 707

Supper, R., Hasinger, G., Pietsch, W., et al. 1997, A&A, 317, 328

Terashima, Y., & Wilson, A. 2003, ApJ, 583, 145

Trinchieri, G., Sulentic, J., Breitschwerdt, D., Pietsch, W. 2003, A&A, 402, 73

Véron-Cetty, M.P. and Véron P. 2000, A Catalogue of Quasars and Active Nuclei, 11th Edition. A&A 2003 (in press)

Vogler, A. & Pietsch, W. 1999, A&A 352, 64

Wang, Q. D. 2002, MNRAS, 332, 764

| ID | RA | Dec | cts/ks | log (LX) | $`z_Q`$ | mag | Host galaxy | Z$`z_G`$ | r | Mabs | Type | Refs. |
| --- | --- | --- | --- | --- | --- | --- | --- | --- | --- | --- | --- | --- |
|  | (hh mm ss) | (deg mm ss) |  |  |  |  |  |  | (arcmin) |  |  |  |
| IXO1 | 01 52 49.7 | -13 42 11 | 0.50 | 39.1 | 2.216 | 20.6 | NGC 720 | 0.006 | 3.4 | -11.3 |  | 1 |
| IXO2 | 01 53 02.9 | -13 46 53 | 1.77 | 39.7 | 0.964 | 19.2 |  |  | 2.7 | -12.7 |  | 1 |
| ULX | 02 43 39.4 | 01 21 09 | 1.2 | 39.2 | 1.400 | 20.0 | NGC 1073 | 0.004 | 1.4 | -10.9 | BL Lac | 2 |
| ULX | 02 43 39.5 | 01 22 20 | 0.4 | 38.7 | 1.945 | 19.8 |  |  | 1.8 | -11.1 |  | 2 |
| ULX | 02 43 33.3 | 01 21 36 | 3.0 | 39.6 | 0.599 | 18.8 |  |  | 2.1 | -12.1 |  | 2 |
| ULX | 03 34 07.1 | -36 04 00 | 3.6 | 39.8 | 0.904 | 19.7 | NGC 1365 | 0.005 | 7.7 | -11.2 |  | 3 |
|  | 03 33 12.2 | -36 19 48 | 38.8 | 40.9 | 0.308 | 18.0 |  |  | 12.4 | -12.9 | BL Lac | 3 |
| ULX | 11 20 14.7 | 13 32 28 | 0.83 | 38.8 | 0.995 | 20.1 | NGC 3628 | 0.003 | 3.0 | -10.8 |  | 4 |
|  | 11 20 11.9 | 13 31 23 | 1.39 | 39.0 | 2.15 | 19.5 |  |  | 4.2 | -11.4 |  | 4 |
|  | 11 20 06.2 | 13 40 24 | 2.50 | 39.3 | 0.981 | 19.2 |  |  | 5.5 | -11.7 |  | 4 |
|  | 11 20 39.9 | 13 36 20 | 0.83 | 38.8 | 0.408 | 19.6 |  |  | 5.6 | -11.3 |  | 4 |
|  | 11 20 41.6 | 13 35 51 | 0.83 | 38.8 | 2.43 | 19.9 |  |  | 6.0 | -11.0 |  | 4 |
|  | 11 19 46.9 | 13 37 59 | 1.67 | 39.1 | 2.06 | 19.6 |  |  | 7.9 | -11.3 |  | 4 |
|  | 11 21 06.1 | 13 38 25 | 6.11 | 39.6 | 1.94 | 18.3 |  |  | 12.3 | -12.6 |  | 4 |
| IXO43 | 12 10 07.9 | 39 23 12 | 0.88 | 39.3 | 0.239 | 18.4 | NGC 4151 | 0.003 | 5.0 | -12.5 |  | 5 |
|  | 12 10 26.7 | 39 29 09 | 63-106 | 40.6-41.9 | 0.615 | 20.3 |  |  | 4.9 | -10.6 | BL Lac | 5 |
| ULX | 12 12 14.6 | 13 12 48 | 4.0 | 39.4 | 0.217 | 18.7 | NGC 4168 | 0.0076 | 0.75 | -13.9 |  | 6 |
| ULX | 12 15 09.2 | 33 09 55 | 38.4 | 40.7 | 0.614 | 17.5 | NGC 4203 | 0.004 | 2.1 | -13.4 | BL Lac | 7 |
| ULX | 12 19 23.6 | +47 09 38 | 3.9 | 38.9 | 0.398 | 20.4 | NGC 4258 | 0.0015 | 8.6 | -8.6 |  | 8 |
| ULX | 12 21 44.0 | 75 18 38 | 255 | 41.5 | 0.071 | 15.2 | NGC 4319 | 0.005 | 0.7 | -15.7 | BL Lac | 9 |
| ULX | 12 25 12.0 | 12 21 53 | 5.6 | 39.8 | 1.25 | 18.5 | NGC 4374 | 0.004 | 2.4 | -12.4 |  | 10 |
| ULX | 12 48 25.9 | 08 30 20 |  | 39.5 | 0.43 | 18.9, 21.9 | NGC 4698 | 0.003 | 1.2 | -12.0, -9.0 | BL Lac | 11 |

References: 1 This work; 2 Arp, H. & Sulentic, J. 1979, ApJ, 229, 496; 3 F. La Franca, F., Fiore, F., Vignali, C., et al. 2002, ApJ, 570, L100; 4 Arp, H., Burbidge, E. M., Chu, Y., Flesch, E., Patat, F., & Rupprecht, G. 2002, A&A, 391, 833; 5 Arp, H. 1977 ApJ, 218,70; 6 Masetti, N. et al. 2003, ApJ, 406, L27; 7 Knezek, P. M., & Bregman, J. N. 1998, AJ, 115, 1737;- 8 Vogler, A. & Pietsch, W. 1999, A&A, 352, 64;- 9 Stocke, J. T. et al. 1991, ApJS, 76, 813; 10 Burbidge, G., Hewitt, A., Narlikar, J. V. & Das Gupta, P. 1990, ApJS, 74, 675; 11 Foschini, L., Ho, L., & Masetti, N. et al. 2002, A&A, 396, 787