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# Galactic Center Shells and a Recurrent Starburst Model

## 1 Introduction

The Galactic Center radio-continuum Arc comprises a bunch of highly aligned magnetic fields vertical to the galactic plane. Various thermal features, such as the “Sickle” and “Bridge”, are superposed (Yusef-Zadeh, Morris 1987a,b). Besides the prominent features, several fainter loops with larger diameters are known to be apparently superposed on the Arc (Yusef-Zadeh, Morris 1987b). However, since the radio emission from the Arc dominates, the faint radio features have not been investigated in details. A high-resolution CO-line survey has revealed various-scale molecular shells in the direction of the Radio Arc (Oka et al. 1998).

In the present work, we tried to enhance the concentric shell structures by applying a filtering technique, which removed straight filaments in the Radio Arc. We showed that the enhanced features comprise numerous thermal radio shells, which we call the Galactic-Center Shells (GCS), in positional coincidence with 16–26 $`\mu `$m observed with the MSX (Shipman et al. 1997). We also compared the shells with CO-line morphology around the Arc regions using a high-resolution CO survey of the Galactic Center (Oka et al. 1998), while a direct interaction of the CO clouds with the Radio Arc is still controversial.

Based on the obtained images, we propose a new idea that the GCSs are coherent expanding fronts from a starburst in the GC near the Pistol and Quintuplet stars. Starbursts in the Galactic Center (GC) are among the major interesting topics in the history of the activity of the Milky Way. We discuss the GCS as being a manifestation of the most recent starburst in the GC, where past recurrent bursts yielded various scale shells, such as the North Polar Spur (NPS: Sofue 1977, 1994, 2000) and the Galactic-Center Lobe (GCL: Sofue, Handa 1984). We further propose a recurrent starburst model for the GCS, GCL and NPS.

## 2 Filtering Technique and Data

We used the VLA 20 and 6-cm radio data from Yusef-Zadeh and Morris (1987a,b) with angular resolutions of 16′′ and 2′′, respectively, which are available as an archive in FITS format and are distributed on a CD-ROM (Condon, Wells 1992).

We first applied the radial-relieving method (Sofue 1993), while taking the center at the Sickle (G$`0.180.04`$) position. The radial-relieving method comprises the following procedure. A radio image is slightly enlarged, e.g. by a factor of 1.05, concentric to a position which is supposed to be the center of a shell to be enhanced. The original map is then subtracted from the enlarged map with the center positions coinciding. The difference map gives a relieved residual, enhancing loop-like features concentric to the center position, while other extended features are suppressed. We also used the pressing method (Sofue, Reich 1979) in order to subtract the straight filaments in the Arc, which is the same procedure to as that used remove scanning effects from a radio map, except that the scan-direction is assumed to be parallel to the filaments. We also used a background-filtering technique (Sofue and Reich 1979) in order to subtract the extended background emission, such as that due to the Sgr A halo.

Among the various features abstracted from the data, we have taken those features to be real, only if the amplitudes were significantly greater (e.g. more than 3 times) than the r.m.s. noise of the original image, and the features could be recognized on the original maps as well. Here, the r.m.s. noise was estimated for emissions from the most quiet region in the original map, including the residual interferometer patterns. The radial relieving technique has the potential to enhance artificial concentric patterns. In order to confirm that the enhanced features are real, we cross-checked the result from three different methods: (a) radial relieving to enhance the shell (loop) features, (b) pressing method to remove straight filaments, and (c) background filtering (unsharp masking). The features discussed here are all visible in the three results. They were also confirmed to be visible in the original maps, if their intensities are properly displayed individually.

## 3 Multiple Radio Shells

### 3.1 Open Lotus

The results are shown in figures 1 and 2 in galactic coordinates. Figure 1a shows a radial-relieved 20-cm image (original data from Yusef-Zadeh and Morris 1987b); Figure 1b is a pressed image, where the vertical filaments have been removed by the pressing method. Figure 2a shows the same as figure 1 in a contour form, and figure 2b is the same but in grey scale and smoothed to an angular resolution of 20′′, where we illustrate the positions of the identified radio shells. We name them GCS (Galactic Center Shells) I, II and III. We also mark the Sickle (Yusef-Zadeh and Morris 1987a,b) by S.

— Fig. 1a, b, 2a, b —

These loops are clearly recognized on the original 20-cm image as well as on the 6-cm images. The fact that the same loop features are recognized in the original 6 and 20-cm maps confirms that the loops are not an artifact of the reduction procedure. Note, however, that because their faintest parts are contaminated by various interferometer patterns, we discuss only the global features here.

The most pronounced loop, GCS I, is centered on G$`0.1700.125`$ at $`(l,b)=(0^{}.170,0^{}.125)`$ with a radius of $`4^{}.24`$, which comprises an almost perfectly round loop. At an assumed distance of the Galactic Center of 8 kpc, this radius corresponds to 9.9 pc. The Sickle (S) at G0.192-0.62 with a radius of $`0^{}.95`$ is apparently in touch with GCS I at the north-western inner edge, and the ’Handle’ appears to compose a part of GCS I. The brightest loops, Shells II and III, are coincident with the thermal filaments in the Radio Bridge, which are also concentric to the other loops. In addition to these prominent loop features, there are several segments of loops, or arcs, which are concentric to each other with their centers near to the Sickle and Pistol. They do not necessarily make perfect loops, but are sometimes oval and partial.

Because of their round shapes, these loops are most likely tangential views of multiple shells. The shells appear to compose a coherent structure, suggesting multiple expanding spherical fronts concentric to the Pistol/Sickle region. The galactic-western (negative-longitude) sides of the shells are apparently contacting the halo of Sgr A, and are much brighter than the opposite side. The galactic-eastern sides are less bright, and seem to be expanding more freely with less deformation. As a whole, the shells look like open petals of a lotus bloom with its neck at the Sgr A halo (figures 2a, b). It is interesting to note that the shells appear to have no clear indication of any interaction with the straight nonthermal filaments in the Radio Arc. In fact, GCS I, the almost perfectly round shell, is not deformed by the Radio Arc.

### 3.2 Properties of Radio Emission

Most of the GCS are visible in the 43-GHz map (Sofue et al. 1986). The spectral index of the NE part of GCS II, inferred from the 43 and 1.4 GHz intensities, is about $`0.05`$, indicating a thermal origin due to ionized interstellar gas. The typical brightness temperature on GCS II is $`50`$ K at 20 cm, which yields an emission measure of $`1.2\times 10^5`$ pc cm-6, if the electron temperature is taken to be $`10^4`$ K. Assuming that the thickness of the shell is 0.1 times the radius ($`0.1\times 9.9`$ pc $`1`$ pc), the line-of-sight depth will be about $`4`$ pc.

This yields an electron density of $`1.7\times 10^2`$ cm-3, and a total mass of the ionized hydrogen $`5\times 10^3M_{}`$. The thermal energy would, then, be $`1\times 10^{49}`$ erg. However, the southern part appears to have a steeper spectrum as inferred from 20 and 6 cm maps, although the present data are not sufficiently accurate to derive spectral indices in such faint features. Thus, we cannot exclude the possibility that the shell comprises nonthermal emission, such as a supernova remnant.

### 3.3 Far-Infrared Shells

GCS I coincides in positions with the most prominent far-infrared loop observed by the MSX experiment at 16–26 $`\mu `$m (Shipman et al. 1997). The MSX image also shows many other shells, coincident with the other GCSs. In figures 3 we compare the radio shells with the MSX image. The association of the FIR emission may indicate that the shells are predominantly thermal, consistent with the radio spectrum, and contain warm dust and probably molecular gas. It is interesting to note that the Arc is not visible in the FIR at all. Thus, the MSX FIR image appears to be very similar to the radio image after subtracting of the Arc filaments.

— Fig. 3 —

### 3.4 Molecular Shells

The association of molecular gas with the radio Arc and Bridge has been discussed in details by Serabyn and Guesten (1987). Numerous CO-line shells and arcs are found toward the presently identified GCSs, whereas no clear CO feature is associated with the Arc. Figure 4a shows an unsharp-masked total CO intensity map, and figure 4b is a superposition on the radio continuum image from figure 1a. Figure 5 shows channel maps of the CO emission. Here, the CO map has been produced using the data cube of the Galactic Center CO survey by Oka et al. (1998). In figure 4a, we indicate GCS I, II, III, and the Sickle (S) by full lines.

— Fig. 4, 5 —

Oka et al. (1998) noticed an expanding shell at 50 km s-1 with a radius and thickness of $`9`$ and $`4`$ pc, respectively, centered on $`(l,b)=(15^{},4^{})`$. We illustrate this shell by the dotted circle in figures 4a and 5. The CO intensity is roughly $`10^2`$ K km s-1, yielding a molecular mass of $`2\times 10^4M_{}`$ for a conversion factor of $`1.0\times 10^{20}`$ H2 \[K km s-1\]-1 (Arimoto et al. 1996). The shell is expanding at 25 km s-1, which yields a kinetic energy of $`1.4\times 10^{50}`$ erg, and an age of $`3.5\times 10^5`$ yr.

Besides this expanding shell, there are several arc-features in the channel maps, some of which appear to be spatially coincident with the GCS positions. GCS I appears to be associated with a CO arc at 10 to 30 km s-1. GCS II is associated with a dense CO arc at 60 to 70 km s-1. The galactic-northern part of GCS III is associated with an extended CO arc at $`10`$ to $`20`$ km s-1. However, no conclusive physical association can be derived from these coincidences at the present resolution, and we cannot exclude the possibility of a chance coincidence.

### 3.5 X-ray Sources in GCS I

The ASCA Galactic Center survey has revealed several bright X-ray sources in the 6.4 keV iron-line (Maeda 1998). The brightest source coincides with Sgr B. The second-strongest source coincides with the Radio Bridge, with which GCS II and III are associated. Most interestingly, the third-strongest source, associated with the Arc region, coincides with the center of GCS I, which is toward the hole in the FIR 16–26 $`\mu `$m emission. An extended continuum X-ray source at 0.7–10 keV is also found near to the center of GCS I.

## 4 Discussion

### 4.1 GCS Energetics

The concentric distribution of the GCSs suggests that they have a common origin, most likely due to mass loss or explosions associated with active star formation near to the Pistol and Sickle. In fact, intense star-forming activity has been observed as the Pistol star and Quintuplet stars (Figer et al. 1998, 1999; Lang et al. 1999). Figer et al. (1999) estimate the mass-loss rate and duration to be $`10^4M_{}\mathrm{yr}^1`$ and 6000 yr with a wind velocity of 2000 km s-1, which yields a total kinetic energy of $`2.4\times 10^{49}`$ erg. This is comparable to the thermal energy of a single GCS and the kinetic energy of an associated CO shell.

If such giant stars, or an ensemble of massive stars, like the Quintuplet, were born recurrently in the past, they would have produced multiple ionization shells, which expanded to sizes as large as several to tens of parsecs. Interactions with and/or the accumulation of background interstellar gas and molecular clouds would decelerate the expansion velocity to several tens of km s-1, as observed in the GCS. Hence, the GCSs would be shells in the evolved phases of similar nebulae to the Pistol. If the total energy $`E`$ is conserved, the expansion velocity $`v`$ and radius $`r`$ are related as $`E\frac{2\pi }{3}\rho r^3v^2`$, where $`\rho `$ is the background gas density. Taking $`E2.4\times 10^{49}`$ erg, and $`v25`$ km s-1, the averaged ISM density is required to be $`\rho 20\mathrm{H}_2\mathrm{cm}^3`$. The age is of the order of $`tr/v4\times 10^5`$ yr.

The total energy of the Pistol, Sickle and all the GCSs identified here is of the order of $`10^{51}`$ erg. The age of the outermost shell (GCS III) is estimated to be $`10^6`$ years from their radii of $`9^{}20`$ pc, and the assumed expansion velocity is 20 km s-1. We may, thus, suppose that recurrent mini-bursts have occurred near the Pistol/Sickle region in the past million years. The burst centers were within several parsecs of the center of GCS II.

### 4.2 GCS Morphology

GCS I is almost perfectly round, suggesting that they have not been disturbed very much by the surrounding ISM. However, the outer shells, GCS II and III, are significantly deformed, particularly on their SW side, where they become concave with respect to the shell centers. This fact suggests an interaction with the Sgr A halo. On the contrary, the galactic-eastern sides of GCS II and III, are more open, where the shells appear to be torn off into several segments. One prominent segment is indicated by an arc in figure 2b.

If we assume that GCS II, III and the other segments (as in figure 2) are a coherent structure, they may be parts of a large shell, which is elongated in the direction perpendicular to the galactic plane, with the galactic-western sides being interrupted by the Sgr A halo and the eastern sides expanding more freely. If the GCSs are expanding shells in the GC gas disk, the vertical elongation is a natural consequence due to the background gas-density distribution. The lopsidedness observed in most of the GCSs will be due to interactions with an inhomogeneous ISM, such as the Sgr A halo and neighboring molecular clouds.

### 4.3 GCS Origin: Recurrent Starbursts Model

We have proposed a bipolar hyper shell (BHS) model due to an intense energy release, such as starbursts at the GC in order to explain the large-scale radio shell structures associated with the GC (Sofue 1977, 1984, 1994, 2000). This model can be applied to smaller scale shells, such as the GCSs. BHS simulations have shown that an expanding shell is round in the early phase, when the shell radius is smaller than the disk thickness. GCS I may be in such an early phase. Then, the shell becomes elongated in the direction perpendicular to the disk when the radius becomes comparable to the disk thickness. GCS II and III would be in such a phase. Hence, GCSs would manifest sequential phases of evolution of an expanding shell originating around the Pistol.

According to BHS simulations, the shell expands further into the halo, while becoming more elongated and opened to form a bipolar $`\mathrm{\Omega }`$ shape or an hour-glass shape. In fact, radio observations have shown an $`\mathrm{\Omega }`$-shaped feature above the Galactic Center, called the Galactic Center Lobe (GCL), which requires energy of the order of $`10^{54}`$ erg and an age of $`10^6`$ yr (Sofue 1985). If the energy scale is greater, the $`\mathrm{\Omega }`$-shaped shell expands into the halo, forming a larger scale BHS. In fact, in our Galaxy an extremely large shell has indeed been observed in radio and X-rays as the North Polar Spur (NPS), for which the BHS model has been successfully applied; the simulation requires an input energy of $`10^{55}`$ erg and an age of $`1.5\times 10^7`$ yr (Sofue 1977, 1984, 1994, 2000). Similar BHS or hyper-wind phenomena have also been observed in starburst galaxies (Heckman et al. 1990), for which a number of numerical simulations have been successfully applied (Tomisaka, Ikeuchi 1988; Suchkov et al. 1994; Strickland, Stevens 2000; Sofue, Vogler 2002).

We, thus, propose a recurrent-starburst model in our Galactic Center. The most recent mini-burst, which occurred some $`10^5`$ years ago, produced the inner GCSs, while the outer GCSs were created by previous ones $`10^{56}`$ years ago. Each energy scale of these mini-bursts was of the order of $`10^{51}`$ erg. A stronger burst a million years ago produced the Galactic Center Lobe, for which an energy of $`10^{54}`$ erg is required. A much bigger burst with $`10^{55}`$ occurred 15 million years ago, and produced the North Polar Spur. Their energy scales are diverse from $`10^{51}`$ to $`10^{55}`$ erg. The large, long-living shells, like the GCL and NPS, would not necessarily be due to a single event, but due to the accumulation of succeeding mini-bursts of GCS scale and bursts of GCL scale, respectively.

The radio continuum data were taken from the VLA public images, courtesy Drs. F. Yuzef-Zadeh and M. Morris, distributed by J. J. Condon and D. Wells by a CD-ROM. The author thanks Dr. T. Oka for the CO-line survey in FITS format.

References

Arimoto, N., Sofue, Y., & Tsujimoto, T. 1996, PASJ, 48, 275

Condon, J. J., & Wells, D. 1992, Images from the Radio Universe (CD-ROM), NRAO

Figer, D. F., Najarro, F., Morris, M., McLean, I. S., Geballe, T. R., Ghez, A. M., & Langer, N. 1998, ApJ, 506, 384

Figer, D. F., Morris, M., Geballe, T. R., Rich, R. M., Serabyn, E., McLean, I. S., Puetter, R. C., & Yahil, A. 1999, ApJ, 525, 759

Heckman, T. M., Armus, L., & Miley, G. K., 1990, ApJS, 74, 833

Lang, C. C., Figer, D. F., Goss, W. M., & Morris, M. 1999, AJ, 118, 2327

Maeda, Y. 1998, PhD Thesis, Kyoto University (ISAS Research Note No. 653)

Oka, T., Hasegawa, T., Sato, F., Tsuboi, M., & Miyazaki, A. 1998, ApJS, 118, 455

Serabyn, E, & Guesten, R. 1987, A&A, 184, 133

Shipman, R. F., Egan, M. P., & Price, S. D. 1997, Galactic Center News, ed. A. Cotera and H. Falcke, Vol 5, 3

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Figure Captions

Fig. 1a. Radial-relieved image of the Galactic Center Arc region observed with the VLA at 20 cm (1.446 GHz: original data from Yusef-Zadeh, Morris 1987a). Numerous loop features are prominent.

Fig. 1b. Pressed VLA 20-cm map, where straight Arc filaments have been removed by the pressing method. Extended emissions were also subtracted by a background-filtering technique.

Fig. 2a. Same as figure 1a in a contour form. Contours are drawn at 1, 2, 4, 8, 16, 32, 64 mJy/(16′′ Beam).

Fig. 2b. Same as figure 2a, but smoothed to a resolution of $`20^{\prime \prime }`$. The Galactic-Center Shells I to III and the Sickel (S) are indicated by the full lines. Contours are drawn at 1, 2, 4, 8, 16, 32, 64 mJy/(16′′ Beam).

Fig. 3. Comparison of the radio GCS (left) with the MSX 16–26 $`\mu `$m image (right: Shipmann et al. 1997).

Fig. 4. Unsharp-masked CO integrated-intensity map produced by using the CO survey by Oka et al. (1998). Contour levels are at 6.33$`\times `$(1, 2,…, 10) K km s-1. The GCS I, II, III and the Sickle (S) are indicated by full lines, and the expanding shell of Oka et al. is indicated by a dotted circle (ES+50km).

Fig. 5. CO intensity channel maps from Oka et al. (1998) at $`V_{\mathrm{lsr}}=60`$ to 130 km s-1 at 10 km s-1 interval. The contour levels are at 1.11$`\times `$(1, 2,…, 10) K km s-1. The GCSs are indicated by full lines, and the expanding CO shell by the dotted circle.


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# Negative virial coefficients and the dominance of loose packed diagrams for 𝐷–dimensional hard spheres

## 1 Introduction

The question of the possible negativity of virial coefficients $`B_k`$ in the low density expansion

$$\frac{P}{k_BT}=\rho +\underset{k=2}{\overset{\mathrm{}}{}}B_k\rho ^k$$
(1)
of the system of hard spheres with diameter $`\sigma `$ in $`D`$ dimensions specified by the two body pair potential

$$U(𝐫)=\{\begin{array}{c}+\mathrm{}\\ 0\end{array}\begin{array}{c}|𝐫|<\sigma \\ |𝐫|>\sigma \end{array}$$
(2)
has been an unresolved problem of outstanding importance since it was first proposed by Temperley  in 1957. For dimensions $`D5`$ all currently available information is summarized in Table 1 where it is seen that all $`B_k`$ are positive. However it was first shown  in 1964 for $`D8`$ that $`B_4`$ is indeed negative. The best available current results for $`B_4`$ as a function of dimension are shown in Table 2.

Most of our intuition and physical insight into the low density (fluid) phase of hard spheres in 3 dimensions comes from the 8 term virial expansion of Table 1. Over the years this data has been used to produce many approximate equations of state . These approximates all incorporate the feature of positive virial coefficients and they all have the feature that they have a radius of convergence which is greater than the packing fraction $`\eta _f=0.49`$ at which freezing has been seen to occur in computer experiments  where the packing fraction $`\eta `$ is related to the density $`\rho `$ by $`\eta =B_2\rho /2^{D1}.`$ This analyticity at the freezing density is incorporated into most phenomenological theories of freezing  as a homogeneity or mean field approximation which ignores the fluctuations at phase coexistence between the fluid and solid phases .

However, if there are negative virial coefficients for hard spheres in $`D=3`$ then no conclusion on the radius of convergence of the virial expansion based on Table 1 can be considered as reliable.

The most striking effect of negative viral coefficients will occur if the signs oscillate with some period as $`k\mathrm{}`$ because this will give a radius of convergence which is not on the positive real axis. If this radius is less than the freezing density then it will be impossible to reliably learn anything about the freezing transition from a knowledge of a finite number of virial coefficients.

It is thus most significant that the sixth and seventh virial coefficients for parallel hard cubes  were shown to be negative in 1962, and even more important that for an exactly solved hard squares model  and the hard hexagon model  the radius of convergence is limited by a singularity at complex density thus resulting in virial coefficients that oscillate in sign.

The purpose of this paper is to extend the results of Tables 1 and 2 and examine as closely as possible the question of whether or not the virial coefficients $`B_k`$ of the hard sphere gas in $`D`$ dimensions have negative virial coefficients. The method we shall use is Monte-Carlo evaluations of the integrals in the Ree-Hoover expansion. In Section 2 we review the formalism of the Ree-Hoover expansion to establish our notation. In Section 3 we compute the virial coefficients $`B_5`$ and $`B_6`$ for dimensions up to $`D=50`$. We find that $`B_5`$ is not monotonic but is in fact always positive. More importantly we find that $`B_6`$ is negative for all $`D6.`$ Our numerical results are given in Table 3. For higher virial coefficients the number of contributing diagrams rapidly increases. Consequently in this study we restrict our attention to various classes of diagrams which are studied in Section 4 where we are able to determine the class of diagrams which are dominant for large $`k.`$ In Section 5 we use our results to form estimates of the radius of convergence to the virial series and we conclude in Section 6 with an evaluation of the various approximate equations of state for hard spheres.

## 2 Ree–Hoover expansions

The original graphical expansion for the virial series is due to Mayer and Mayer , in which each bond represents the function

$$f(𝐫)=\mathrm{exp}\left(U(𝐫)/k_BT\right)1$$
(3)
where r is the distance between the two vertices. A useful re-summation was performed by Ree and Hoover  by introducing the function

$$\stackrel{~}{f}(𝐫)=1+f(𝐫)=\mathrm{exp}\left(U(𝐫)/k_BT\right)$$
(4)
and then expanding each Mayer graph by substituting $`1=\stackrel{~}{f}f`$ for pairs of vertices not connected by $`f`$ bonds. This method was previously used by Percus and Yevick  in comparing the exact values of the fourth and fifth virial coefficients with coefficients obtained from the Percus–Yevick equation, and by Percus  in discussing the derivation of the Percus–Yevick equation.

The fourth virial coefficient may then be written as

$$B_4=\frac{1}{8}\text{}\frac{3}{4}\text{}\frac{3}{8}\text{}=\frac{1}{4}\mathrm{}\frac{3}{8}\text{}=\frac{1}{4}\text{}\frac{3}{8}\text{}$$
(5)
where the first expression is the expansion in Mayer graphs, the second is the expansion in Ree-Hoover graphs with the $`\stackrel{~}{f}`$ bonds indicated by dotted lines and the third shows the equivalent Ree-Hoover graphs with the $`f`$ bonds indicated by solid lines. In the second expression the graph with no $`\stackrel{~}{f}`$ bonds is represented by $`\mathrm{}`$. In the case of hard spheres, the potential is given by Eq. 2 so $`f(𝐫)`$ and $`\stackrel{~}{f}(𝐫)`$ are particularly simple:

$`f(𝐫)`$ $`=`$ $`\{\begin{array}{c}\hfill 1\\ \hfill 0\end{array}\begin{array}{c}|𝐫|<\sigma \hfill \\ |𝐫|>\sigma \hfill \end{array}`$ (10)
$`\stackrel{~}{f}(𝐫)`$ $`=`$ $`\{\begin{array}{c}\hfill 0\\ \hfill +1\end{array}\begin{array}{c}|𝐫|<\sigma \hfill \\ |𝐫|>\sigma \hfill \end{array}`$ (15)
The virial coefficient $`B_k`$ is given in terms of the Ree-Hoover diagrams of $`k`$ points of which $`m`$ are the end points of $`\stackrel{~}{f}`$ bonds $`S_k[m,i]`$ and a combinatorial factor $`C_k[m,i]`$ as

$$B_k=\underset{m,i}{}B_k[m,i]$$
(16)
with

$$B_k[m,i]=C_k[m,i]S_k[m,i]$$
(17)
where the index $`i`$ labels the graphs in the class with fixed $`k,m.`$ The combinatorial factor is expressed as

$$C_k[m,i]=\frac{k1}{k!}s_k[m,i]\stackrel{~}{a}_k[m,i]$$
(18)
with

$$s_k[m,i]=k!/\mathrm{}\mathrm{Aut}S_k[m,i]$$
(19)
where $`\mathrm{}\mathrm{Aut}S_k[m,i]`$ is the cardinality of the automorphism group of the diagram $`S_k[m,i]`$ and $`\stackrel{~}{a}_{m,l}[k]`$ is the “star content” as defined by Ree and Hoover . We will let $`S_k[m,i]`$ represent both the Ree-Hoover graph and the value of the corresponding integral. The $`k`$ dependence of $`C_k[m,i]`$ is calculated by using the following relation for the star content .

$$\stackrel{~}{a}_k[m,i]=(1)^{k1}(k2)\stackrel{~}{a}_{k1}[m,i]$$
(20)
The diagram $`S_k[m,i]`$ has $`km`$ points that are connected to all other points by $`f`$ bonds and are therefore indistinguishable, leading to the relation

$`\mathrm{}\mathrm{Aut}S_k[m,i]`$ $`=`$ $`(km)!\mathrm{}\mathrm{Aut}S_m[m,i]`$ (21)
to obtain for $`k>m`$

$$C_k[m,i]=(1)^{k(k1)/2}\left(\genfrac{}{}{0pt}{}{k1}{m1}\right)C_m[m,i]$$
(22)
where we note that for the complete star diagram $`B_k[0,1]`$ we have $`C_k[0,1]=1/k.`$

For arbitrary $`D`$ the number of Mayer graphs grows asymptotically as $`k\mathrm{}`$ as

$$N(k)\frac{2^{k(k1)/2}}{k!}$$
(23)
However, when the Ree-Hoover transformation is made many diagrams have zero star content and hence do not contribute to the virial coefficient. From Table 4 it appears that the ratio of contributing Ree-Hoover diagrams to the number of Mayer diagrams is bounded below, and so it is reasonable to suppose that

$$\underset{k\mathrm{}}{lim}N_{RH}(k)/N(k)>0$$
(24)
In addition Ree-Hoover graphs may be zero for geometrical reasons. The number of non-zero graphs for $`D=2`$ are taken from , and listed in Table 4, where the value in parentheses excludes diagrams found to be negligible but which were not proven to be zero. For $`D=1`$ only one graph in the Ree-Hoover expansion is non-zero for each $`k`$, namely the complete star, but for $`D2`$ it is an open question as to how many non-zero graphs there are at order $`k`$.

### 2.1 Close packed diagrams

The $`\stackrel{~}{f}`$ graph form used by Ree and Hoover (e.g. in ) has the property that a single graph represents the sequence of diagrams $`B_k[m,i]`$ with $`m`$ fixed where the ($`k+1`$)th order diagram is obtained from the $`k`$th by adding an additional point connected to all other points by an $`f`$ bond. For example, all complete star diagrams of order $`k`$ may be represented by the same symbol $`\mathrm{}`$. We call such graphs with $`m<k`$ close packed because no two points can be further apart than $`2\sigma .`$

We find from Eq. 22 that the sign of $`B_k[m,i]`$ for fixed $`m,i`$ is independent of $`k.`$ We further obtain from Eq. 22 for $`k`$ large and $`m,i`$ fixed that

$$C_k[m,i]=C_m[m,i]\left(\frac{k^{m1}}{(m1)!}+O(k^{m2})\right)$$
(25)
### 2.2 Loose packed diagrams

For diagrams in the class $`B_k[k,i]`$ there are no points which are connected to all other points by $`f`$ bonds and therefore there exist sequences of diagrams which have the property that the size of the configuration grows as $`k\mathrm{}.`$ We refer to this class of diagrams as “loose packed”. For these graphs the $`f`$ bond notation is more convenient.

The simplest loose packed diagram in $`B_k[k,i]`$ is the simple ring of $`k`$ of the $`f`$ bonds. We denote this diagram by the symbol $`𝖱`$. More generally we consider graphs where a point is replaced by a diagram. We call such diagrams insertion diagrams and when we wish to make the type of insertion visually apparent we use the notation $`𝖱()`$ to represent a ring with a point replaced by a diagram. We also find it useful to label insertion diagrams by $`𝖱_{n,l}[k]`$ where the index $`n`$ is the number of points in the inserted diagram of $`k`$ total points and $`l`$ labels the diagrams with given $`k`$ and $`n.`$ All four and five point insertions were found by starting with all four and five point Mayer graphs, and adding an extra point that is connected to two points by $`f`$ bonds. A canonical labeling for this graph was found using “nauty”, a program due to B. McKay , and matched with the five and six point graphs of Ree and Hoover  to find the star content. All insertions with non-zero star content are given in Table 5 along with the size of their automorphism group and over all combinatorial factor. From Eq. 22 we find the insertion diagrams have the alternating sign property that $`(1)^k𝖱_{n,l}[k]`$ has a sign which depends only on $`n`$ and $`l`$ but is independent of $`k.`$

Multiple insertions are also possible when $`k`$ is sufficiently large. We denote such a graph with $`n`$ insertions as $`𝖱_{\{n_1,i_i\},\mathrm{},\{n_m,i_m\}}^{(m)}`$ where the subscripts indicate the types of insertions. For $`B_6`$ we see in Table 8 that there are three graphs which may be interpreted as being composed of two 4-point insertions.

We give in Tables 68 the Ree-Hoover graphs and their associated combinatorial factors for $`k=4,5,6.`$ We here give both the representation of the graphs in terms of $`\stackrel{~}{f}`$ and $`f`$ bonds. For the class of loose packed graphs in $`B_k[k,i]`$ we indicate the interpretation in terms of insertion diagrams with either multiple insertions or with a ring of one point and two bonds. In three cases the identification is not unique.

The labeling index $`i`$ in $`B_k[m,i]`$ is chosen such that in $`D=2`$ the magnitude of the contribution decreases with increasing $`i`$. If the diagram is identically zero for $`D=2`$ then the ordering obtained from $`D=3`$ is used when possible.

## 3 Monte-Carlo Calculation of $`B_k`$ for $`Dk1`$.

When $`Dk1`$ the integral $`S_k[m,i]`$ can be written in a form where the dimension $`D`$ appears as a simple power in the integrand. Hence the Monte-Carlo procedure can simultaneously calculate the given Ree-Hoover diagram in an arbitrary set of dimensions, including non-integer values. The key advantage of this method over that of  used in Section 4 is that we obtain fast convergence for high dimensions. We first present the details of the Monte-Carlo method and then the results for $`B_4`$, $`B_5`$, and $`B_6`$.

We believe that all Ree-Hoover diagrams are non-zero for $`Dk1`$ as it is possible to obtain a configuration for any diagram. We can see this by starting with a configuration where the distance between each point is exactly one, and then since each bond can be independently varied in length by a small amount we are able to satisfy the constraints imposed by $`f`$ and $`\stackrel{~}{f}`$ bonds of any graph.

### 3.1 Monte-Carlo method

In order to do the Monte-Carlo integration we need an appropriate measure for calculating Ree-Hoover diagrams in $`D`$-dimensional Euclidean space, where we wish to integrate out coordinates to leave ourselves with the lowest dimensional integral possible. The integrand is a product of $`f`$ and $`\stackrel{~}{f}`$ functions; for central potentials this leaves only the inter-particle distances as appropriate degrees of freedom. These form an independent set of $`k(k1)/2`$ coordinates provided that $`Dk1`$, where $`k`$ is the order of the diagram and hence the number of points in the configuration. After taking the infinite volume limit, for an arbitrary diagram $`S_k[m,i]`$ we thus need to calculate integrals of the form

$$I=\underset{i=1}{\overset{k1}{}}d^D𝐫_𝐢𝐅(r_{ij})=\left(\underset{i=1}{\overset{k1}{}}\mathrm{\Omega }_{Di}\right)\underset{i<j}{}da_{ij}[V(\{a_{ij}\})]^{Dk}𝐅(r_{ij})$$

where $`\mathrm{\Omega }_{D1}2\pi ^{D/2}/\mathrm{\Gamma }(D/2)`$, $`a_{ij}=|𝐫_𝐢𝐫_𝐣|^2=a_{ji}`$, $`V`$ is the volume of the parallel-piped defined by these distances in $`^{k1}`$, and $`𝐅(r_{ij})`$ is an arbitrary function of the inter-particle distances. As shown for example in  $`V`$ may be expressed by the Cayley-Menger determinant:

$$V(\{a_i\})=\left[\frac{(1)^k}{2^{k1}}\left|\begin{array}{cccccc}0& 1& 1& 1& \mathrm{}& 1\\ 1& 0& a_{12}& a_{13}& \mathrm{}& a_{1k}\\ 1& a_{21}& 0& a_{23}& \mathrm{}& a_{2k}\\ 1& a_{31}& a_{32}& 0& \mathrm{}& a_{3k}\\ \mathrm{}& \mathrm{}& \mathrm{}& \mathrm{}& \mathrm{}& \mathrm{}\\ 1& a_{k1}& a_{k2}& a_{k3}& \mathrm{}& 0\end{array}\right|\right]^{\frac{1}{2}}$$
(26)
An overall scale factor can be taken out of Eq. 26 by taking $`a_{12}`$ to be the largest value, and then setting $`a_{ij}^{}=a_{ij}/a_{12}`$, so that

$`I`$ $`=`$ $`{\displaystyle \frac{1}{2}}k(k1)\left({\displaystyle \underset{i=1}{\overset{k1}{}}}\mathrm{\Omega }_{Di}\right){\displaystyle _0^{\mathrm{}}}𝑑a_{12}a_{12}^{(k1)D/21}`$ (27)
$`\times \left[{\displaystyle \underset{i<j2}{}}{\displaystyle _0^1}𝑑a_{ij}^{}\right]V(\{a_{12}1,a_{ij}^{}\})^{Dk}𝐅(r_{ij})`$
A formula similar to Eq. 3.1 was previously obtained by Percus , in which the integration of $`p`$ vectors in dimension $`D`$ is reduced to an integration of $`p`$ vectors in $`p`$ dimensions.

For the hard sphere fluid, the integrand is either zero or $`\pm 1`$. In order to calculate $`S_k[m,i]`$ with $`m`$ $`\stackrel{~}{f}`$ bonds and $`[k(k1)/2m]`$ $`f`$ bonds, we may then proceed as follows. Generate a set of $`[k(k1)/21]`$ values uniformly distributed between 0 and 1. Partition these values in two sets, where the largest $`m1`$ values along with 1 represent $`\stackrel{~}{f}`$ bonds and the other $`[k(k1)/2m1]`$ values are $`f`$ bonds, and then randomly assign these values to edges in the diagram. Check that these values of the edge lengths squared can be embedded as a simplex in $`^{k1}`$, and if this is the case one can calculate the volume of the simplex and perform the $`a_{12}`$ integral, making a contribution to the Monte-Carlo integral of

$$\frac{k}{D}\left(a_m^{(k1)D/2}a_{m+1}^{(k1)D/2}\right)\left(\underset{i=1}{\overset{k1}{}}\mathrm{\Omega }_{Di}\right)V(\{a_{12}1,a_{ij}^{}\})^{Dk}$$
(28)
where $`a_m`$ and $`a_{m+1}`$ are the $`m`$th and $`(m+1)`$th largest values of $`a_{ij}`$ respectively.

We have used this procedure to compute $`B_4`$, $`B_5`$, and $`B_6.`$ For $`B_4`$ and $`B_5`$ 500 batches of $`5\times 10^6`$ configurations were used, while for $`B_6`$ 20 batches of $`2\times 10^9`$ configurations were generated. Uncertainties were calculated using

$$\mathrm{Error}=\left[\underset{j=1}{\overset{q}{}}\frac{(<I_j><I>)^2}{q(q1)}\right]^{\frac{1}{2}}$$
(29)
where there are $`q`$ independent batches with value $`I_j`$.

### 3.2 Results

The values of the individual contributions $`B_k[m,i]`$ to the virial coefficients $`B_k`$ for $`k=4,5,6`$ are given in Appendix A in Tables 1214, for many values of $`D50.`$ The values of the virial coefficients $`B_k/B_2^{k1}`$ for $`D50`$ are given in Table 3.

The most important feature of the virial coefficients in Table 3 are the sign changes in $`B_4`$ and $`B_6.`$ A previous estimate for the dimension at which $`B_4`$ becomes negative of $`D7.8`$ was obtained by Luban and Baram  by means of a linear interpolation of the results of Ree and Hoover , and also by an independent calculation. We further note the existence of a local minimum in $`B_5`$ which confirms the tentative prediction of Loeser et al. . To obtain accurate values for these zeros, minima and maxima as a function of $`D`$ the data were fitted with cubic splines, and all of these values are summarized in Table 9. Note that the error estimates were made by fitting, for example, $`B_4+\mathrm{\Delta }B_4`$ and $`B_4\mathrm{\Delta }B_4`$ with cubic splines to obtain a confidence interval for where $`B_4`$ becomes negative. A least squares fit was not used because the error in values at different dimensions are not independent, as they are calculated simultaneously and not as independent samples.

It is most important that $`B_6`$ becomes negative at a lower dimension than $`B_4.`$ If this trend continues, we may expect that for $`B_{2k}`$ the dimension at which the coefficient becomes negative will decrease for higher orders and it is not unreasonable to expect that $`B_8`$ will be negative for $`D=5`$ and possibly even $`D=4.`$ In addition, even though $`B_5`$ is always positive, the existence of a local minimum at $`D=6.87`$ shows that the increasing number of contributing diagrams results in more complex dimensional dependence.

To obtain further insight into the structure of the virial coefficients we examine the individual contributions in Tables 1214. There we see by examining the dependence of the contributions on $`D`$ that by the time $`D=50`$ the Ree-Hoover ring diagram $`𝖱`$ is several orders of magnitude greater than all other diagrams. We therefore make the following conjecture:

###### Conjecture 1

$$\underset{D\mathrm{}}{lim}B_k(D)/𝖱(D)=1$$
(30)
In particular it follows from this conjecture that for each $`k`$

$$(1)^{k1}B_k(D)>0\mathrm{for}\mathrm{sufficiently}\mathrm{large}D.$$
(31)
A similar conjecture in terms of Mayer diagrams was made by Frisch and Percus  in the course of their examination of Mayer diagrams at high dimensionality.

We find further for $`D=50`$ that not only does the Ree-Hoover ring diagram dominate but that the largest diagram in each $`B_k[m,i]`$ has the property that if $`m>m^{}`$ then

$$B_k[m,i]_{\mathrm{max}}>>B_k[m^{},i]_{\mathrm{max}}.$$
(32)
We refer to this ordering as the principle of “loose packed dominance”.

We also note that within the loose packed class $`B_k[k,i]`$ that the ordering of the magnitude of the diagrams at $`D=2`$ and at $`D=50`$ is drastically different. For example we note that the diagram $`𝖱_{4,1}`$ which vanishes identically in $`D=2`$ is the second largest diagram for $`D=50.`$ More generally we find for $`D=50`$ that the contributions in $`B_6[6,i]`$ are ordered in magnitude as

$$𝖱>𝖱_{4,1}>𝖱_{4,2}>𝖱_{5,4}>𝖱_{5,5}>𝖱_{5,3}>𝖱_{5,2}=𝖱_{\{4,1\},\{4,1\}}^{(2)}$$
(33)
where we use the labeling of insertion diagrams in Tables 5 and 8. We make the observation that these insertion diagrams are the largest in the class $`B_k[k,i]`$, and refer to this as “insertion graph dominance”.

## 4 Monte-Carlo Calculation of High Order Diagrams

The observation and conjecture of the dominance of the Ree-Hoover ring diagram at large dimensions demonstrates that negative virial coefficients in the hard sphere fluids is a common occurrence. However it says nothing about the minimum dimension at which the coefficient $`B_k`$ will become negative for fixed $`k`$ nor does it give any indication of whether or not virial coefficients of odd order can ever be negative. Ideally this question should be studied by computing further viral coefficients beyond those in Table 1 for large $`k.`$ Here we will begin this program by examining selected classes of diagrams $`B_k[m,i]`$ for values of $`k`$ up to 17. In particular we examine the conjecture that the features of loose packed dominance and insertion graph dominance found for large $`D`$ and fixed $`k`$ holds also for fixed $`D`$ and large $`k`$.

### 4.1 Method

The Monte-Carlo procedure used for this study is the same as that used by Ree and Hoover (e.g. in ). Random configurations are generated by placing one point at the origin of some arbitrary coordinate system, then the next is randomly placed within a $`D`$-dimensional unit sphere centered on the first point, and so on. The final configuration is then tested to see if it satisfies the requirements imposed on distances by the diagram being calculated. For each diagram we used batches of $`10^6`$ configurations, with enough batches to give accuracy better than two percent up to a maximum of $`10000`$ batches, and errors were calculated using Eq. 29.

### 4.2 Results

The evaluations of the following diagrams are presented in Tables 1522 of Appendix B for values of $`k`$ up to 17 and values of $`D`$ up to 7; $`B_k[0,1],B_k[4,1],B_k[5,1],𝖱[k],𝖱_{4,2}[k],𝖱_{4,1}[k],𝖱_{5,5}[k]`$, and the “pinwheel diagram” in $`B_k[k1,1]`$ obtained by adding one point which is connected by $`f`$ bonds to all points in the Ree-Hoover ring $`𝖱[k1].`$ We note that for $`k=5`$ the pinwheel is $`B_5[4,1]`$ and for $`k=6`$ it is $`B_6[5,2].`$

To investigate the conjecture of loose packed dominance for fixed $`D`$ and large $`k`$ we use the tables of Appendix B to find for each $`k`$ and $`D`$ which diagram of this set is the largest. This is shown in Table 10. We also use Tables 15 and 18 to compute the ratio $`𝖱/B_k[0,1].`$, and display the results in Table 11. From this table we see that for $`D3`$ the Ree-Hoover ring $`𝖱`$ quickly dominates the complete star diagram as $`k`$ increases. However, for $`D=2,`$ even though the ratios are monotonically increasing for $`k6`$ the ring has not dominated the complete star at $`k=17.`$ If we extrapolate the increasing ratios in Table 11 for $`D=2`$ we can estimate that the ring will be larger for approximately $`k22`$.

Further information is obtained from the ratios of $`B_k[4,1]/B_k[0,1]`$ and $`B_k[5,1]/B_k[0,1]`$ plotted in Figs. 1 and 2 of Appendix C. In these figures it is seen that the ratios $`B_k[4,1]/B_k[0,1]`$ and $`B_k[5,1]/B_k[0,1]`$ increase linearly with $`k.`$ Thus while for the values of $`k`$ studied the ratios only rarely exceed one it appears that if we extrapolate to sufficiently large $`k`$ that the inequalities in Eq. 32 will be satisfied for $`m,m^{}=0,4,5.`$

The relative size of diagrams in the class $`B_k[k,i]`$ and $`B_k[k1,i]`$ is studied by comparing the Ree-Hoover ring diagram $`𝖱[k]`$ of Table 18 with the corresponding pinwheel diagram of Table 22. It is clear that in each dimension that for sufficiently large $`k`$ the pinwheel diagram will vanish, and although this can’t be shown numerically one can see the ratio of the pinwheel to the ring $`𝖱[k]`$ decreases rapidly as $`k`$ increases.

We conclude this discussion of results by examining the relative magnitudes of insertion diagrams in $`B_k[k,i].`$ In Figs. 3, 4, and 5 of Appendix C we plot the ratios $`𝖱_{4,2}/𝖱`$, $`𝖱_{4,1}/𝖱`$, and $`𝖱_{5,5}/𝖱`$ as a function of $`k`$ for various $`D.`$ We see that for sufficiently large $`k`$ all three ratios have a linear increase with respect to $`k`$. We also note that even though the ratio $`𝖱_{4,1}/𝖱_{4,2}`$ is small in low dimensions, it approaches a non-zero constant as $`k\mathrm{}`$, and for sufficiently large $`D`$ the ratio is in fact greater that unity.

The examination of all available data supports the following conjectures

###### Conjecture 2

The loose packed diagrams in $`B_k[k,i]`$ dominate all other diagrams for large $`k`$ when $`D3`$.

In connection with this conjecture we note that the three largest diagrams for $`B_6`$ in $`D=5,6`$ are $`𝖱_{5,5}`$, $`𝖱_{4,1}`$, and $`𝖱`$ and that the sum of these three largest diagrams shares the property with $`B_6`$ itself of changing sign between $`D=5`$ and $`D=6.`$ We restrict the conjecture to dimensions $`D3`$ because at this stage there is not yet enough data to support the case for $`D=2`$.

###### Conjecture 3

The insertion diagrams all have the same exponential rate of growth as the Ree-Hoover ring.

## 5 Estimates of the radius of convergence

The dominance of loose packed diagrams for fixed $`D3`$ and large $`k`$ may be used to discuss the question of sign change in the virial coefficients and the radius of convergence of the virial expansion. Of greatest importance is the relation of the radius of convergence to the packing fractions $`\eta _f`$ at which freezing occurs which have been numerically determined as $`\eta _f=0.49`$ in $`D=3`$ , $`\eta _f=0.31`$ in $`D=4`$ and $`\eta _f=0.19`$ in $`D=5`$ as obtained from .

It may be that there are sequences of loose packed diagrams that grow faster than the ring, but for low order the largest diagrams can be characterized as insertion diagrams and these appear to have the same exponential rate of growth as the ring. Hence we will concentrate on the Ree-Hoover ring $`𝖱`$. We first note that the absolute value of this diagram must be strictly less than the absolute value of the corresponding Mayer diagram where all $`\stackrel{~}{f}`$ bonds are replaced by unity. The resulting Mayer ring diagram has been long ago evaluated  in terms of Bessel functions of the first kind $`J_{D/2}(x)`$ and thus we obtain

$$(1)^{k1}𝖱[k]/B_2^{k1}\frac{(k1)(2\pi )^{kD/2}}{2k\mathrm{\Omega }_{D1}^{k2}}_0^{\mathrm{}}𝑑xx^{D1}\left[\frac{J_{D/2}(x)}{x^{D/2}}\right]^k$$
(34)
The large $`k`$ behavior of this integral is easily obtained by steepest descents by noting that the maximum value of $`J_{D/2}(x)/x^{D/2}`$ occurs at $`x=0.`$ Thus we have as $`k\mathrm{}`$

$$(1)^{k1}𝖱[k]/B_2^{k1}\frac{(k1)(1+D/2)^{D/2}}{k^{1+D/2}\mathrm{\Gamma }(1+D/2)}\mathrm{\hspace{0.25em}2}^{k2}$$
(35)
and hence $`𝖱[k]`$ satisfies the bound

$$|𝖱[k+1]/(B_2𝖱[k])|2.$$
(36)
This leads to a packing fraction at the radius of convergence of the sum of Ree-Hoover diagrams of $`\eta _{rh}=2^D`$ which is substantially greater than the lower bound $`0.145/2^D`$ of Lebowitz and Penrose  but which is still much smaller than the freezing densities $`\eta _f.`$ This value of $`\eta _{rh}`$ is of the same order of magnitude as the lower bounds on the termination density due to Baram and Fixman  which are $`\eta _t>0.25838`$ for $`D=2`$ and $`\eta _t>0.12681`$ for $`D=3`$.This is compatible with the pressure being analytic for positive values of $`\eta `$ less than $`\eta _f`$ because the alternations of sign of $`𝖱[k]`$ puts the leading singularity on the negative $`\eta `$ axis.

However the ratios $`\left|𝖱[k+1]/(B_2𝖱[k])\right|`$ obtained from Table 18 are substantially below the bound Eq. 36. In fact we see from each $`D4`$ that there is some value of $`k`$ such that for all greater values of $`k`$ the values of $`𝖱/B_2^{k1}`$ increase. The order $`k`$ must surely be greater than this value before it can be claimed that the asymptotic regions has been achieved. If we use that maximum ratios as obtained from Table 18 we estimate that for $`D=4`$ we have $`\eta _{rh}0.12`$ and for $`D=5`$ we have $`\eta _{rh}0.052.`$ In $`D=3`$ if we assume that the data of Table 18 extrapolates to a constant as $`k\mathrm{}`$ then the radius of convergence of the Ree-Hoover ring is $`\eta _{rh}=0.25`$. At most the ratios are bounded below by $`0.91`$ which leads to $`\eta _{rh}=0.27`$. All of these estimated radii of convergence are substantially less than the freezing densities $`\eta _f.`$

In order for the radius of convergence of the virial series to be larger than these estimates obtained from the Ree-Hoover ring there must be cancellations between diagrams in the class $`B_k[k,i].`$ Such cancellations can occur because, for example, the diagrams $`𝖱_{4,2}[k]`$ and $`𝖱_{5,5}[k]`$ which have magnitudes comparable to $`𝖱[k]`$ have signs opposite to $`𝖱[k].`$ Furthermore from Table 1 we see that $`B_k`$ is indeed less in magnitude than $`𝖱[k]`$ for $`k=6,7,8.`$ What cannot be inferred from the existing data is whether or not when $`k`$ is sufficiently large that the diagrams are in their asymptotic region that the cancellation is severe enough to reduce the exponential rate of growth of the ratios $`B_{k+1}/B_k.`$ Unless the cancellation becomes sufficiently great for the radius of convergence to be larger than the freezing density then the leading singularity cannot be on the real $`\eta `$ axis and there must be oscillation in the signs of the virial coefficients.

## 6 Approximate equations of state for hard spheres

For over 40 years the eight virial coefficients of Table 1 have been used to inspire many approximate equations of state for the low density phase of hard spheres. These approximates may be grouped by the location of their leading singularity into the following three classes:

1: High order poles at $`\eta =1`$

Examples of these are the proposals of Thiele

$$Pv/k_BT=\frac{1+2\eta +3\eta ^2}{(1\eta )^2},$$
(37)
Reiss, Frisch, and Lebowitz , and Wertheim

$$Pv/k_BT=\frac{1+\eta +\eta ^2}{(1\eta )^3},$$
(38)
Guggenheim

$$Pv/k_BT=\frac{1}{(1\eta )^4},$$
(39)
and the proposal of Carnahan and Starling

$$Pv/k_BT=\frac{1+\eta +\eta ^2\eta ^3}{(1\eta )^3}.$$
(40)
We do note that Torquato  proposes an equation of state which agrees with Eq. 40 for $`\eta <\eta _f`$ but which is of a different form for $`\eta >\eta _f`$.

2: Simple poles at  or near the packing fraction $`\eta _{cp}=0.74048\mathrm{}`$ of closest packed hard spheres

In particular the Padé analysis made in  has simple poles at

$$\eta =(1.22\pm 0.09i)\eta _{cp}$$
(41)
which leads to sign oscillations beginning with $`B_{45}`$.

3: A fractional power law divergence at or near the “random close packed” density $`\eta _{rcp}=0.64`$ as defined by

These approximates are obtained from a D-log Padé analysis and are (generalizations) of the form

$$Pv/k_BT=A(\eta \eta _{rcp})^s$$
(42)
As an example $`s`$ is estimated as 1 in  as $`0.678`$ in  and $`0.76`$ in . In  other values of $`\eta _{rcp}`$ are chosen and the values of $`s`$ lie in the range $`0.6s0.9`$ depending on the approximation used.

All these approximate equations of state share the feature that their leading singularity is at a value of $`\eta `$ which is greater than the freezing density $`\eta _f=0.49`$ and indeed is even greater than the solid end of the phase transition $`\eta _s=0.542.`$ This fact has lead to the assumption that the virial expansion is analytic at the freezing transition $`\eta _f`$ and this qualitative feature is incorporated into most of the phenomenological theories used to describe freezing . It is therefore of great importance that the estimates of the radius of convergence made above on the basis of loose packed dominance and the assumption of no cancellation estimated the radius of convergence at no more than $`0.27`$.

The estimate of the radius of convergence relies on values of $`k`$ beyond the first eight virial coefficients used to obtain the approximate equations of state. Therefore it is fair to say that none of the approximates incorporates the true large $`k`$ behavior of the virial coefficients. Thus even if there is cancellation for large $`k`$ for the set of close packed diagrams none of the approximates is based on computations which can observe these cancellations and hence no known approximate equation of state can be considered reliable. We therefore conclude that at present there exists no evidence to support the claim that the virial expansion has a radius of convergence greater than the freezing density $`\eta _f.`$

## Appendix A Individual diagram contributions for $`B_4`$, $`B_5`$, and $`B_6.`$

In this appendix we tabulate the contributions of the individual Ree-Hoover diagrams to the virial coefficients for $`B_4`$, $`B_5`$, and $`B_6.`$

## Appendix B Numerical values of selected diagrams to high order.

In this appendix we tabulate the results of Monte-Carlo evaluations of selected diagrams $`B_k[m,i]`$ to orders up to $`k=17`$.

## Appendix C Graphs of the ratio of selected diagrams to high order.

In this appendix we graph the ratios $`B_k[4,1]/B_k[0,1]`$, $`B_k[5,1]/B_k[0,1]`$, $`𝖱_{4,2}/𝖱`$, $`𝖱_{4,1}/𝖱`$, and $`𝖱_{5,5}/𝖱`$ to orders up to $`k=17`$.

Acknowledgments: This work was supported in part by the National Science Foundation under DMR-0073058. We thank Prof. R. J. Baxter and Prof. G. Stell for useful discussions.