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# Evidence for a very low-lying 𝑆=9 excited state of the 𝑆=10 single molecule magnet Mn₁₂-acetate

## Abstract

We present a detailed investigation of the temperature and frequency dependence of the anomalous EPR transitions first observed in Mn12-acetate by Hill et al. \[Phys. Rev. Lett. 80, 2453 (1998)\]. The most dominant of these transitions manifest themselves as an extra series of EPR absorption peaks for spectra obtained with the DC field applied within the hard magnetic plane of a single crystal sample. Recent studies by Amigo et al. \[Phys. Rev. B 65, 172403 (2002)\] have attributed these extra peaks to a strain induced transverse quadratic anisotropy which gives rise to distinct Mn12-acetate species, each having a distinct EPR spectrum; on the basis of these measurements, it has been suggested that this transverse anisotropy is responsible for the tunneling in Mn12-acetate. Our temperature and frequency dependent measurements demonstrate unambiguously that these anomalous EPR absorptions vanish as the temperature tends to zero, thereby indicating that they correspond to transitions from an excited state of the molecule. We argue that this low lying excited state corresponds to an $`S=9`$ multiplet having very similar zero-field crystal parameters to the $`S=10`$ state, and lying only about $`1015`$ $`k_B`$ above the $`S=10`$ (M$`{}_{S}{}^{}=\pm 9`$) ground state. These findings also compare favorably with available neutron scattering data.

I. Introduction

Since it was first suggested that macroscopic quantum tunneling of magnetic moments from one easy axis to another should be observable in ensembles of sufficiently tiny magnetic particles,Bean59  the quantum properties of crystals containing identical magnetic molecules with relatively large magnetic moments (so far up to $`26\mu _B`$) $``$ so called single molecule magnets (SMMs)MRS00 ; Angewandte03  $``$ have become the subject of intense research activity. The main feature of magnetic quantum tunneling (MQT) is the following: below a characteristic temperature, called the blocking temperature TB, the magnetic viscosity (relaxation time for magnetization reversal) stays finite and temperature independent, indicating that the moments are able to short-circuit the classical thermally activated relaxation channel.Bean59 ; MRS00 ; Angewandte03 ; TejadaBook  SMMs offer a number of advantages over other types of magnetic nanostructures. Most importantly, they are monodisperse. Consequently, they enable fundamental studies of properties intrinsic to magnetic nanostructures that have previously been inaccessible. For example, the observation of well defined quantum jumps in the low temperature (T $`<`$ TB) hysteresis loops of \[Mn12O12(CH3COO)16(H2O)4\]$``$2CH3COOH$`4`$H2O (Mn12-ac) crystals provided evidence for resonant MQT.MRS00 ; Angewandte03 ; TejadaBook ; Friedman96 ; Thomas96  Since this discovery, Mn12-ac has become the most widely studied SMM.MRS00 ; Angewandte03 ; TejadaBook ; Friedman96 ; Thomas96 ; Hernandez97 ; delBarcoEPL02 ; Hennion97 ; MirebeauPRL99 ; Barra97 ; HillPRL98 ; HillPRB02 ; KPark02a ; KPark02b ; HillPRL03a  The resonant nature of the MQT has enabled very precise studies of the relaxation dynamics,Hernandez97 ; delBarcoEPL02  while neutronHennion97 ; MirebeauPRL99  and electron paramagnetic resonance (EPR)Barra97 ; HillPRL98 ; HillPRB02 ; KPark02a ; KPark02b ; HillPRL03a  experiments have provided fairly detailed spectroscopic information concerning the low-lying quantum energy levels of Mn12-ac. In spite of these extensive investigations, the precise mechanism responsible for the tunneling has remained elusive. An in-depth understanding of MQT is important not only from a fundamental point of view: for example, there has recently been considerable speculation concerning the possible use of SMMs for quantum information processing.LossNature01

The Mn12-ac molecule consists of four Mn4+ ions, each with spin $`S=\frac{3}{2}`$, surrounded by eight Mn3+ ions with spin $`S=2`$.MRS00 ; Angewandte03  The clusters crystallize into a tetragonal lattice, with each molecule having approximate $`S_4`$ site symmetry; the orbital moment is quenched, and a Jahn-Teller distortion produces a strong axial anisotropy. A simplified treatment of the magnetic interactions within the molecule has been developedSessoliJACS93  wherein four strongly antiferromagnetically coupled Mn$`{}_{}{}^{3+}`$Mn4+ dimers, each with spin $`S=2\frac{3}{2}=\frac{1}{2}`$, couple via an effective ferromagnetic interaction to the remaining four $`S=2`$ Mn3+ ions, giving a total spin $`S=10`$. Within this simplified 8-spin scheme, the weaker couplings between the four spin$`\frac{1}{2}`$ dimers and the four spin$`2`$ Mn3+ ions largely determine the low energy excitations within the molecule.Katsnelson99

To lowest order, the magnetic energy levels of a rigid spin $`S=10`$ system can be described by the effective spin Hamiltonian:

$`\widehat{H}=D\widehat{S}_z^2+\mu _B\stackrel{}{B}\stackrel{}{g}\widehat{S}+\widehat{H}^{},(1)`$

where $`D`$ $`(<0)`$ is the uniaxial anisotropy constant, the second term represents the Zeeman interaction with an applied field $`\stackrel{}{B}`$ ($`\stackrel{}{g}`$ is the Land$`\stackrel{´}{e}`$ g tensor), and $`\widehat{H}^{}`$ includes higher order terms in the crystal field ($`\widehat{O}_4^0`$, $`\widehat{O}_2^2`$, $`\widehat{O}_4^2`$, $`\widehat{O}_4^4`$, etc. Hennion97 ; MirebeauPRL99 ; Barra97 ; HillPRL98 ), as well as environmental couplings such as intermolecular dipolar and exchange interactions.HillPRB02 ; KPark02a ; KPark02b  This predominantly Ising-type anisotropy is responsible for the energy barrier to magnetization reversal and the resulting magnetic bistability - factors which lead to magnetic hysteresis at sufficiently low temperatures.MRS00 ; Angewandte03 ; TejadaBook  MQT in zero-field is caused by interactions in $`\widehat{H}^{}`$ which lower the symmetry of the molecule from strictly axial, thereby mixing otherwise degenerate pure ”spin-up” and ”spin-down” states. Tunnel rates depend on the degree of symmetry breaking, which is something which can be determined very precisely via single crystal EPR measurements.Barra97 ; HillPRL98 ; HillPRB02 ; KPark02a ; KPark02b ; HillPRL03a  The only transverse crystal field term (to fourth order) in $`\widehat{H}^{}`$ allowed by the strict $`S_4`$ symmetry of the molecule is $`\widehat{O}_4^4`$. While such an interaction clearly exists,MirebeauPRL99 ; Barra97 ; HillPRL03a  it cannot account for many aspects of the low temperature magnetic relaxation.delBarcoEPL02 ; FriedmanRC98  For this reason, recent theoretical and experimental attention has focused on a quadratic transverse anisotropy induced by disorder.delBarcoEPL02 ; HillPRB02 ; KPark02a ; KPark02b ; HillPRL03a ; ChudnPRL01 ; GaraninPRB02 ; AmigoPRB02 ; ParksPRB01 ; MertesPRL02 ; CorniaPRL02  One particular proposal considers long range strains caused by dislocations.ChudnPRL01 ; GaraninPRB02  However, a more likely scenario involves acetate ligand disorder which would give rise to distinct Mn12-ac variants with local site-symmetry lower than $`S_4`$.delBarcoEPL02 ; HillPRB02 ; HillPRL03a ; CorniaPRL02  Indeed, our recent angle dependent EPR studies show clear evidence for a quadratic anisotropy ($`\widehat{O}_4^2`$) which can be attributed to a discrete disorder associated with the ligand molecules.HillPRL03a  Furthermore, recent magnetic measurements have shown that a narrow distribution of tunnel splittings exists,delBarcoEPL02  a fact which is again consistent with the ligand disorder scenario.CorniaPRL02

In spite of growing acceptance for the role of disorder in the MQT phenomenon, several outstanding questions remain; not least, the absence of a clear parity effect associated with the resonant MQT steps observed in hysteresis experiments.FriedmanRC98  Meanwhile, several recent works have drawn attention to possible inadequacies of the single spin ($`S=10`$) description of Mn12-ac.Hennion97 ; Katsnelson99 ; AcheyPRB01 ; AcheySSC02 ; YamamotoRPL02  For example: a low lying magnetic excitation has been observed in neutron scattering experiments, which cannot be explained within the single spin picture;Hennion97  NMR experiments have demonstrated that the paramagnetic spin density is delocalized over the entire molecule;AcheyPRB01 ; AcheySSC02  and recent calculationsKatsnelson99  have shown that interactions between the $`S=10`$ multiplet and low lying excited multiplets ($`S<10`$) are necessary in order to explain the significant quartic terms in Eq. (1) which are found for Mn12-ac.MirebeauPRL99 ; Barra97 ; HillPRL03a  In this paper, we present high-frequency single crystal EPR data which provide convincing evidence for a low-lying $`S=9`$ state. We compare these findings with available neutron scattering data,Hennion97  and comment on the possible consequences of these findings.

II. Experimental

The $`(2S+1)`$fold quantum energy level structure associated with a large molecular spin necessitates spectroscopies spanning a wide frequency range. Furthermore, large zero-field level splittings, due to the significant crystalline anisotropy (large $`D`$) and large total spin $`S`$, demand the use of frequencies and magnetic fields considerably higher (50 GHz to 1 THz, and up to 10 tesla respectively) than those typically used by the majority of EPR spectroscopists. The high degree of sensitivity required for single crystal measurements is achieved using a resonant cavity perturbation technique in combination with a broad-band Millimeter-wave Vector Network Analyzer (MVNA) exhibiting an exceptionally good signal-to-noise ratio; a detailed description of this instrumentation can be found in ref. \[MolaRSI, \]. The MVNA is a phase sensitive, fully sweepable (8 to 350 GHz), superheterodyne source/detection system. Several sample probes couple the network analyzer to a range of high sensitivity cavities ($`Q`$factors of up to 25,000) situated within the bore of a superconducting magnet. The MVNA/cavity combination has been shown to exhibit a sensitivity of at least $`10^9`$ spins$``$G$`{}_{}{}^{1}`$s-1, which is comparable with the best narrow-band EPR spectrometers. This, coupled with newly acquired sources and a split-pair magnet, allow single crystal measurements at any frequency in the range from 8 to 250 GHz, at temperatures down to 1.2 K $`(\pm 0.01`$ K), and for any geometrical combination of DC and AC field orientations.

The advantages of a narrow band cavity perturbation technique, and the ability to study single crystals, have recently been discussed in ref. \[HillPRB02, \]. In particular, such a scheme enables faithful extraction of the intrinsic EPR lineshapes (both the real and imaginary components), free from instrumental artifacts. Consequently, any raw data displayed in this paper constitutes pure absorption. Single Mn12-ac crystals were grown using literature methods.Lis80  All measurements were performed in the standard EPR configuration with the AC excitation field transverse to the DC field. The two samples (A and B) used in this study were needle shaped, having approximate dimensions $`1\times 0.1\times 0.1`$ mm3. Orientation of the crystals was relatively straightforward due to the shape of the samples, with the needle axis defining the easy axis. All of the presented data were obtained with the DC magnetic field aligned within the samples’ hard magnetic $`(x,y)`$ plane (easy axis data are presented in ref. \[HillPRB02, \]). Low field data $`(<7`$ T) were obtained using a superconducting solenoid, while higher field data were obtained in the resistive magnets at the National High Magnetic Field Laboratory (NHMFL).

III. Background

In our earlier single crystal investigations of Mn12-ac, we first pointed out that EPR spectra obtained with the field perpendicular to the easy-axis revealed a number of anomalous EPR transitions;HillPRL98  these transitions were labeled $`\beta `$ and $`\gamma `$ in ref. \[HillPRL98, \], as opposed to the $`\alpha `$-resonances which nicely fit the accepted $`S=10`$ Hamiltonian for Mn12-ac (see Fig. 1 and Table 1, which adopts this same labeling scheme). These earlier studies were conducted at moderate fields $`(B<11`$ T), and at relatively low frequencies compared to the powder studies by Barra et al.Barra97  In the high-field limit, one expects 20 transitions within the $`2S+1`$ $`(S=10)`$ multiplet; the $`\alpha `$-resonances in ref. \[HillPRL98, \] and Fig. 1 comprise half of this total (corresponding to transitions from M$`{}_{S}{}^{}=`$ even-to-odd integers, see Table 1). One should eventually expect to see an additional 10 EPR peaks, in between the $`\alpha `$-resonances (corresponding to transitions from M$`{}_{S}{}^{}=`$ odd-to-even integers), but only in the high-field/frequency limit; Fig. 2 illustrates the origin of these transitions. We previously tentatively ascribed the $`\beta `$-resonances to the expected high-field resonances. However, the M$`{}_{S}{}^{}=`$ odd-to-even transitions should become EPR silent below about 95 GHz (due to avoided level crossings, see Fig. 2b), yet they persist down to at least 45 GHz. Indeed, all attempts to fit the $`\beta `$-resonances to the accepted Mn12-ac Hamiltonian (Eq. 1) have failed quite spectacularly. We should point out that we have since carried out single crystal studies on simpler $`S=\frac{9}{2}`$ Mn4 SMMs (corresponding to the core of the Mn12 SMM), with the same $`S_4`$ symmetry, which behave absolutely as expected according to Eq. 1.SB4Poly02

More recently, several other groups have reported extra EPR peaks for both single crystal studies with the field perpendicular to the easy axis, and from powder measurements. Amigo et al.AmigoPRB02  ascribe the extra peaks to a strain or disorder induced transverse anisotropy (caused by dislocations in the sample, see ref. \[ChudnPRL01, ; GaraninPRB02, \]), which gives rise to different species of molecule within the crystal. In this model, the extra peaks arise due to the fact that one expects equal numbers of molecules having their hard axes along a particular direction in the hard plane, and at $`90^{}`$ to this direction. Matters are complicated further due to the fact that their model includes a rather broad distribution of transverse anisotropies. Thus, it is unlikely that one would observe distinct splittings in such a case, but rather a broadening of the resonance linewidths, with an EPR lineshape that reflects the distribution. Cornia et al. have also recently published data which show a splitting of the $`\alpha `$-resonances (the $`\beta `$ resonances are also seen in their 95 GHz spectra).CorniaPRL02  However, this splitting is more subtle, since it is only clearly observed using field modulation, or by taking derivatives of absorption spectra.HillPRL03a  We also see this effect in the $`\alpha `$-resonances (this is the subject of a separate publicationHillPRL03a ). Cornia et al. propose a mechanism for this splitting involving disorder associated with the acetic acids of crystallization. Like Amigo’s model, this ligand disorder induces a transverse anisotropy which varies from one molecule to the next.

We believe that the EPR splittings observed by Amigo et al.,AmigoPRB02  and by Cornia et al.,CorniaPRL02  have quite different origins. The latter almost certainly are associated with ligand disorder, as we have recently confirmed,HillPRL03a  whereas the distinct absorptions observed by Amigo et al. correspond to the same $`\beta `$-resonances that we observed in our original single crystal investigations.HillPRL98  Although Amigo et al. claim that the anomalous peaks are only observed upon stressing their samples, there is clear evidence for such resonances even in their unstressed samples (see Fig. 2 in ref. \[AmigoPRB02, \]\]. Furthermore, we have seen these extra peaks in all of the samples that we have studied, as have Barra et al.Barra97  and Cornia et al.CorniaPRL02  There do, however, appear to be noticeable differences in the positions and intensities of anomalous EPR peaks obtained by different groups. Since transverse EPR spectra are notoriously sensitive to field alignment,HillPRL03a  minor differences in sample orientation may easily explain these differences, as could solvent loss from the samples.

IV. Results and discussion

Figure 1 shows data obtained for sample A at four different frequencies from 44 GHz up to 111 GHz; the temperature is 10 K for each sweep. The dips in absorption are due to EPR transitions, and these have been labeled according to the original scheme in ref. \[HillPRL98, \]. The $`\alpha `$-resonances correspond to transitions within the Zeeman split energy levels which, in zero-field, correspond to M$`{}_{S}{}^{}=\pm m`$ states $`(m=`$ integer, and $`0mS`$) as depicted in Fig. 2a; in this representation, the quantization axis is defined by the uniaxial crystal field tensor, and is along $`z`$. In the high-field limit, the quantization axis points along the applied field vector; in this limit, the ten $`\alpha `$-resonances correspond to transitions from M$`{}_{S}{}^{}=`$ even-to-odd $`m`$, e.g. M$`{}_{S}{}^{}=10`$ to $`9`$ (again, this situation is illustrated in Fig. 2a). Because the $`\alpha `$-resonances originate from pairs of levels which are (approximately) degenerate in zero field, one expects the resonance frequencies, when plotted against field, to tend to zero as the field tends to zero; this can be seen in Fig. 2b.

In the high field limit, one expects ten additional resonances corresponding to M$`{}_{S}{}^{}=`$ odd-to-even $`m`$, e.g. M$`{}_{S}{}^{}=9`$ to $`8`$. Indeed, we do see these transitions at high fields (see below). However, if one follows these transitions to the zero-field limit, it is clear that the resonance frequency should go through a minimum, tending to one of the zero-field splittings in this limit; this is illustrated in Fig. 2a and by the dashed curves in Fig. 2b. Consequently, such EPR transitions should become ”EPR silent” below some characteristic cut-off frequency determined by the point of closest approach for the two levels involved in the transition. The dominant interaction responsible for this level repulsion is simply the Zeeman term in Eq. 1 and is, therefore, more-or-less insensitive to the other transverse terms in Eq. 1. For Mn12-ac, this cut-off frequency is about 95 GHz for the three highest field odd-to-even $`m`$ transitions (see Fig. 2b, which uses realistic parameters for Mn12-ac).MirebeauPRL99 ; HillPRL03a  For this reason, below 95 GHz, the $`\beta `$-resonances observed in Fig. 1 cannot be attributed to the high-field odd-to-even $`m`$ transitions. However, it is noticeable that the strength of the $`\beta `$-resonances increases dramatically between the 77.4 GHz trace and the 111.1 GHz trace, i.e. above 95 GHz, there is a pronounced increase in the strength of the $`\beta `$-resonance. We shall comment more on this below.

Next, we turn to the temperature dependence of the data obtained in Fig. 1, with particular attention being paid to the highest field $`\beta `$-resonance ($`\beta 10`$), and a much weaker $`\gamma `$-resonance. Fig. 3 shows data for three frequencies below the cut-off of 95 GHz. In all of these traces, the $`\beta 10`$ resonance diminishes in intensity as T $`0`$, becoming more-or-less invisible at the lowest temperature. This fact proves beyond any doubt that the $`\beta 10`$ resonance originates from an excited state of the Mn12-ac molecule, thereby ruling out any likelihood that it corresponds to a different Mn12-ac species, as proposed by Amigo et al.AmigoPRB02  We will discuss the possible origin of this excited state further below. Meanwhile, we note that the weak $`\gamma `$-resonance exhibits a very similar temperature dependence to the $`\alpha 10`$ resonance, which corresponds to the transition from the accepted $`S=10`$ ground state of the molecule, i.e. the $`\gamma `$ and $`\alpha 10`$ peaks continue to grow as T $`0`$. Therefore, there is every likelihood that the $`\gamma `$ peak does signify a small minority ($`1`$ to $`2\%`$) of molecules having a different ground state from the majority. We speculate that this peak may correspond to the well known faster relaxing species of Mn12-ac, which has one of its Jahn-Teller axes tilted with respect to the $`z`$-axis of the molecule.Sun99 ; Aubin01  This peak has only been observed for some samples, a fact which is also consistent with the faster relaxing species. The faster relaxing Mn12-ac Jahn-Teller isomer is believed to have an $`S=9`$ ground state, a reduced axial anisotropy constant ($`D`$-value) and an appreciable transverse quadratic anisotropy.ChristouPC  All of these factors can explain the fact that the $`\gamma `$-resonance is observed at lower fields than the $`\alpha 10`$ resonance. However, the shift appears to be rather large, implying a $`30\%`$ reduction in $`D`$ over the majority species; further studies on pure samples of the faster relaxing species are planned in the near future in order to resolve this issue. A similar weak lower lying peak has been observed in neutron scattering experiments where, again, the authors attribute this to the faster relaxing Mn12-ac species.MirebeauPRL99  It is interesting to note that the ratios of the frequencies of the presumed fast and slow relaxing peaks observed here, and from neutron scattering are quite similar,MirebeauPRL99  as are the relative intensities.

Figure 4 shows the temperature dependence of the 111.1 GHz data from Fig. 2. At this frequency, which is above the cut-off for odd-to-even $`m`$ high-field transitions, the $`\beta 10`$ resonance shows a marked increase in intensity over the lower frequency data. Indeed, it exceeds the intensity of the $`\alpha 10`$ resonance at temperatures above about 4.2 K. Furthermore, $`\beta 10`$ is clearly visible at the lowest temperatures investigated. A similar trend may be noted for $`\beta 9`$. We suspect that this pronounced enhancement of $`\beta 10`$ (and $`\beta 9`$) is caused by the switching on of the anticipated high-field M$`{}_{S}{}^{}=9`$ to $`8`$ ($`7`$ to $`6`$) transition within the $`S=10`$ state of Mn12-ac (see Fig. 2 and Table 1); the fact that it is difficult to distinguish these transitions from the anomalous low frequency transitions will be discussed further below. EPR spectra obtained with the field applied parallel to the easy ($`z`$-) axis show no additional anomalous peaks,HillPRB02  i.e. no EPR absorptions which cannot be explained within the framework of the $`S=10`$ picture. Easy axis data obtained over a wider frequency range (40 to 200 GHz) compared to our earlier studies (ref. \[HillPRL98, \]) have recently been published in ref. \[HillPRB02, \].

Recent hard axis measurements for a second sample (B), covering a wider frequency range compared to our original investigations,HillPRL98  have enabled a complete determination of the Hamiltonian parameters for Mn12-ac up to fourth order.HillPRL03a  Further details of our fitting procedure are published elsewhere.HillPRL03a  Fig. 5 shows the results of such a fit, along with the obtained parameters. As can be seen, the solid curves $`(S=10`$ picture) lie beautifully on the $`\alpha `$-resonance data (open circles). However, as already discussed, the $`\beta `$-resonances (solid squares) only match the $`S=10`$ curves at the highest frequencies investigated; below 95 GHz, a dramatic departure from the expected behavior can be seen. It is impossible to force the $`S=10`$ fits through these low frequency $`\beta `$-resonance data points, since it is apparent that they belong to curves which approach zero frequency as the field tends to zero; for an $`S=10`$ system, the high-field odd-to-even $`m`$ transitions tend to finite frequency offsets in the low field limit (see Fig. 2). We therefore speculate that, at low frequencies, the $`\beta `$-resonances correspond to transitions within an excited state of Mn12-ac. For comparison, Fig. 5 includes curves corresponding to the $`S=9`$ state, which were generated using precisely the same parameters as obtained from the $`S=10`$ fit. For an odd total spin state, the low field limiting behavior of odd-to-even $`m`$ and even-to-odd $`m`$ transitions is the reverse of that for an even total spin state. Consequently, one does expect the frequency of the M$`{}_{S}{}^{}=9`$ to $`8`$ transition to go to zero in the low field limit for $`S=9`$. Although not perfect, the low frequency $`\beta `$-resonance data lie quite close to the $`S=9`$ curves. At higher frequencies, the $`\beta `$-resonances lie somewhat in between the $`S=9`$ and $`S=10`$ curves while, in the high frequency limit, they lie nicely on the $`S=10`$ curves.

Having noted the possible connection between the $`\beta `$-resonances and an $`S=9`$ state, one has to ask whether such an assignment is consistent with other published results. Based on the limited temperature dependence of $`\beta 10`$ (Fig. 3), we can estimate the approximate activation energy to the state from which $`\beta 10`$ is excited, i.e. the presumed $`S=9`$ state. This analysis is complicated somewhat by the broad asymmetric $`\alpha 10`$ resonance, and due to the fact that the $`\beta 10`$ resonance saturates at temperatures as low as $`46`$ K. Nevertheless, a crude analysis yields a very low activation energy of 10-15 $`k_B`$. Incredibly, this implies that the supposed $`S=9`$ (M$`{}_{S}{}^{}=\pm 9`$) state lies very close to the first excited state of the $`S=10`$ multiplet! Even looking by eye at the data in Fig. 3, one can see that the temperature dependence of $`\beta 10`$ and $`\alpha 9`$ are quite similar, so it is clear that the activation energy to the $`S=9`$ state is of a similar order to the low lying $`S=10`$ levels. An energy of $`10`$ $`k_B`$ corresponds precisely to 0.2 THz, where a very strong finite $`Q`$ (1.18 $`\AA ^1`$) mode has been observed from neutron scattering experiments.Hennion97  The momentum dependence of the intensity of this mode indicates that it has a magnetic origin (its intensity tends to zero as $`Q0`$), suggesting spins that are coupled on a local scale. Indeed, from an analysis of the neutron data, one can conclude that this mode may be related to the antiferromagnetic coupling within a Mn$`{}_{}{}^{3+}`$Mn4+ dimer within the framework of the Mn12 molecule.Hennion97

Recent theoretical studies of the spin excitations within Mn12-ac treat the molecule as a system of four strongly antiferromagnetically coupled Mn$`{}_{}{}^{3+}`$Mn4+ dimers, each with spin $`S=2\frac{3}{2}=\frac{1}{2}`$ which, in the ground state, are coupled via an effective ferromagnetic interaction to the four remaining Mn3+ ions, each having $`S=2`$.SessoliJACS93 ; Katsnelson99 ; YamamotoRPL02  Within this simplified scheme, the weaker couplings between the four spin$`\frac{1}{2}`$ dimers and the four spin$`2`$ Mn3+ ions largely determine the low energy excitations within the molecule. While these calculations do not reproduce the 0.2 THz neutron mode,Hennion97  this 8 spin model provides a basis for comparison with the present data. In particular, one could imagine an excitation within a spin$`\frac{1}{2}`$ dimer leading to a reversal of this moment, and to an overall $`S=9`$ state for the molecule. It was previously speculated that the 0.2 THz mode originates from dissipative interactions between the Mn12 clusters and their environment.Katsnelson99  The present work seems to indicate that this is not the case, and that the 0.2 THz mode corresponds to a distinct finite $`Q`$ excitation of the molecule to a well defined (probably $`S=9)`$ state. We hope that these findings will stimulate further theoretical work on this problem.

While our measurements do not provide definitive proof that the low lying excitation within the molecule corresponds to an $`S=9`$ state, such an explanation for the observed trends in the single crystal EPR data is quite appealing. Furthermore, it is apparent that the $`S=9`$ and $`S=10`$ data become indistinguishable in the high frequency limit, which would explain why other researchers have successfully simulated most aspects of their high-field powder EPR data using an $`S=10`$ model.Barra97 ; AmigoPRB02  A summary of the tentative assignments of the resonances is presented in Table 1. In order to simplify the ensuing discussion, we shall assume that the observed excited state does, in fact, correspond to $`S=9`$. The fact that the $`\beta `$ resonances merge smoothly into the $`S=10`$ model at high frequencies suggests that the parameters describing the $`S=9`$ state of the molecule are quite similar to those describing the $`S=10`$ state. To a first approximation, this is not so unrealistic since this merely corresponds to the reversal of the moment of one of the dimers. Consequently, one would expect excitations within the $`S=9`$ and $`S=10`$ multiplets to be virtually indistinguishable for fields parallel to the easy axis, since there is no distinction between even-to-odd $`m`$ and odd-to-even $`m`$ transitions for this orientation. This fact, again, appears to be consistent with our experimental findings. Minor mismatches in the parameters could give rise to temperature dependent line shapes and widths. In particular, one could expect some line narrowing upon depopulating the $`S=9`$ state at low temperatures. Such behavior has been observed, and explained very well in terms of inter-molecular dipolar interactions.HillPRB02 ; KPark02a ; KPark02b  Without more precise data for the $`S=9`$ state, it is not possible to say whether this picture needs to be re-evaluated.

Due to the finite momentum separating the $`S=9`$ and $`S=10`$ states, it is clear that there could be no direct evidence for the 0.2 THz excitation from optical studies, i.e. no direct optical transitions from the $`S=10`$ ground state, to the low-lying $`S=9`$ state. Indeed, no such transitions ($`0.2`$ THz) have been reported. However, excitations within each manifold ($`S=10`$ and $`S=9`$) are allowed, as appears to be the case from these EPR investigations. Furthermore, the finite momentum separation would tend to minimize any interaction between these two states, thereby explaining why the $`S=10`$ picture explains so many low-temperature experimental observations with such precision, including most EPR data. Nevertheless, even very weak interactions between these states could have crucial implications as far as the tunneling is concerned in Mn12-ac. Clearly further theoretical studies are required.

V. Summary and conclusions

Detailed single crystal EPR investigations of Mn12-ac reveal several transitions in the hard axis spectra which do not fit the accepted $`S=10`$ picture; indeed, the deviations of these EPR peaks from the $`S=10`$ theory are quite dramatic. Temperature dependent studies indicate that the anomalous transitions originate from an excited state of the molecule which lies only about $`1015`$ $`k_B`$ above the $`S=10`$, M$`{}_{S}{}^{}=\pm 10`$ ground state, i.e. approximately coincident with the first excited state of the $`S=10`$ multiplet. These observations conflict with the recent suggestion by Amigo et al. that the anomalous peaks correspond to unique disorder-induced ground states of Mn12-ac.AmigoPRB02

Independent evidence for a low-lying ($`1015`$ $`k_B`$) excitation to something other than the standard $`S=10`$ state has been known for some time from neutron scattering experiments.Hennion97  The present EPR investigations show, unambiguously, that this low-lying state is very real; indeed, both studies agree on the activation energy. Based on extensive frequency dependent measurements, we argue that the excited state corresponds to an $`S=9`$ multiplet having very similar zero-field crystal field parameters to the $`S=10`$ state. While our measurements do not provide definitive proof for such an $`S=9`$ state, this assignment would explain why there is little evidence for its existence in most other EPR and optical studies published to date. The effects of this low-lying $`S=9`$ state on the low-temperature quantum properties of Mn12-ac are not known, and we hope these investigations will stimulate further theoretical studies.

VI. Acknowledgements

We thank Andy Kent, George Christou and David Hendrickson for useful discussion. This work was supported by the NSF (DMR0103290, DMR0196430 and DMR0239481); the NHMFL is supported by the State of Florida and the NSF under DMR0084173. S. H. would like to thank the Research Corporation for financial support.

Figure captions

FIG. 1. Frequency dependence of the hard axis EPR spectra for Mn12-ac (sample A); the temperature and the frequencies are indicated in the figure. The $`\alpha `$-resonances behave as expected for a spin $`S=10`$ easy axis system. The anomalous $`\beta `$-resonances increase in intensity with increasing frequency, becoming particularly prominent at the highest frequency; these transitions are indicated with dots ($`\beta 10`$) and arrows ($`\beta 9`$). Assignments of the various resonances are listed in Table 1, and Fig. 2 illustrates the possible spin $`S=10`$ transitions.

FIG. 2. The upper panel shows the energy level diagram for Mn12-ac for a field applied within the hard plane; this simulation was made using accepted Hamiltonian parameters for Mn12-ac ($`D=0.454`$ cm-1, $`B_4^0=2.0\times 10^5`$ cm-1, $`B_4^4=\pm 3.0\times 10^5`$ cm-1).MirebeauPRL99 ; HillPRL03a  The vertical bars illustrate the origin of the $`\alpha `$-resonances (even-to-odd MS transitions), while the filled circles represent the high frequency odd-to-even MS transitions. The quantum state labels on the left hand side of the figure correspond to the spin projection along $`z`$ (low-field limit), while the labels on the right hand side correspond to the spin projection along the applied field direction (high-field limit). The lower panel plots the expected transition frequencies, as a function of magnetic field, for the transitions labeled in the upper panel. The main point to note is the fact that the odd-to-even MS transition frequencies (dashed lines) go through a minimum. Therefore, these transitions should not be observable below a cut-off frequency which is about 95 GHz for the first few resonances in Mn12-ac.

FIG. 3. Temperature dependence of the hard axis EPR spectra obtained at three frequencies below the hard axis cut-off frequency (see Fig. 2 for explanation) for sample A; the temperatures and frequencies are indicated in the figure. The main point to note is that only the $`\alpha `$\- and $`\gamma `$-resonances persist as T $`0`$; the intensities of the $`\beta `$-resonances, on the other hand, go to zero as T $`0`$. Consequently, only the $`\alpha `$\- and $`\gamma `$-peaks can be attributed to ground states of Mn12-ac \- see main text for further discussion.

FIG. 4. Temperature dependence of the hard axis EPR spectra obtained above the hard axis cut-off frequency (see Fig. 2 for explanation) for sample A; the temperature and the frequencies are indicated in the figure. In contrast to Fig. 3, the $`\beta `$-resonance shows appreciable intensity, even at the lowest temperature while, at the highest temperature, it is by far the strongest peak.

FIG. 5. Fits of the frequency dependence of hard axis spectra obtained for sample B. Details of this analysis are published elsewhere.HillPRL03a  The $`\alpha `$-resonances (open circles) fit the $`S=10`$ model (solid lines) exceptionally well. The $`\beta `$-resonances (solid squares), on the other hand, only fit the $`S=10`$ picture at higher frequencies. It is not possible to force the $`S=10`$ fits through the $`\beta `$ resonance data points observed below 95 GHz. However, it is found that these low-frequency points lie quite close to the behavior expected for $`S=9`$ (dashed curves). The inset depicts the orientation of the applied field relative to the sample, and the obtained quadratic and quartic Hamiltonian parameters are indicated in the figure.


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# ON THE ACTIVE GRAVITATIONAL MASS OF A NON–SPHERICAL SOURCE LEAVING HYDROSTATIC EQUILIBRIUM

## 1 Introduction

One of the most remarkable aspect of general relativity, is the very special status that this theory confers to the spherical symmetry. This situation is particularly well illustrated by the Israel theorem.

Indeed, as is well known , the only static and asymptotically-flat vacuum space-time possessing a regular horizon is the Schwarzschild solution. For all the others Weyl exterior solutions , the physical components of the Riemann tensor exhibit singularities at $`r=2m`$. Therefore, it is intuitively clear that for high gravitational fields, the evolution of sources of Weyl space-time should drastically differ from the evolution of spherical sources . It is important to keep in mind that the sharp difference in the behaviour of both types of sources (for very high gravitational fields) will exist independently on the magnitude of multipole moments (higher than monopole) of the Weyl source. This is so because, as the source approaches the horizon, any finite perturbation of the Schwarzschild space-time becomes fundamentally different from any Weyl solution, even when the latter is characterized by parameters whose values are arbitrarily close to those corresponding to the spherical symmetry. This point has been stressed before , but usually it has been overlooked.

Notwithstanding, spherical symmetry is a common assumption in the study of compact self-gravitating objects (white dwarfs, neutron stars, black holes ) , furthermore in the specific case of non-rotating black holes, spherical symmetry should be“absolute”, according to Israel theorem. Therefore it is pertinent to ask, how do small deviations from this assumption, related to any kind of perturbation (e.g. fluctuations of the stellar matter, external perturbations, etc), affect the dynamics of the system?.

In a recent work  it was shown that for a non–spherical source (even in the case of slight deviations from spherical symmetry), the speed of entering the collapse regime decreases substantially, as compared with the exactly spherically symmetric case. Also, the sensitivity of the trajectories of test particles in the $`\gamma `$ spacetime, to small changes of $`\gamma `$, for orbits close to $`2m`$, has been brought out .

It is the purpose of this work to study further the behaviour of axysymmetric sources for very high gravitational fields. This will allow us to put in evidence the role played by the non sphericity (however small) of the source, on the outcome of evolution. To do so we shall obtain an expression for the active gravitational mass of the source, immediately after its departure from equilibrium. Here “immediately” means on a time scale of the order of (or smaller than) hydrostatic time scale -see section 4 for more details.

As initial configurations, we shall consider two interior metrics. These ones were found some years ago by Stewart et al. , following a prescription given by Hernández  allowing to obtain sources of Weyl space time, from known spherically symmetric interior solutions.

The configurations to be considered are sources of the so-called gamma metric ($`\gamma `$-metric) , . This metric, which is also known as Zipoy-Vorhees metric , belongs to the family of Weyl’s solutions, and is continuously linked to the Schwarzschild space-time through one of its parameters. The motivation for this choice is twofold. On one hand the exterior $`\gamma `$-metric corresponds to a solution of the Laplace equation (in cylindrical coordinates) with the same singularity structure as the Schwarzschild solution (a line segment ). In this sense the $`\gamma `$-metric appears as the “natural” generalization of Schwarzschild space-time to the axisymmetric case. On the other hand, the two interiors considered have reasonable physical properties and generalize important and useful sources of the Schwarzschild space-time, namely the interior Schwarzschild solution (homogeneous density) and the Adler solution . All this having been said, we would like to emphasize that our main goal here is not to model the behaviour of a specific type of compact object, but to illustrate the effects of slight deviations from spherical symmetry, on the source.

As we shall see, the value of active gravitational mass of the source evaluated just after the departure from equilibrium, will be seriously affected by slight deviations from spherical symmetry.

On the other hand, we are well aware of the fact that the $`\gamma `$ metric is not the only possible description for the exterior of a compact objetc and, of course, the two equations of state considered here do not exhaust the list of possible candidates for the equation of state of the stellar matter. However, in view of the properties of the $`\gamma `$ metric and the two equations of state considered here, mentioned above, it is fair to say that the case for the relevance of small deviations from spherical symmetry in the dynamics of compact objects has been further strengthened. This suggests that any conclusion on the structure and evolution of a compact object, derived on the assumption of spherical symmetry should be carefully checked against small deviations from that assumption, whenever the boundary of the source is close to the horizon.

## 2 The Space-time

### 2.1 The exterior space-time

As it has been mentioned above, our initial matter configuration is the source of an axially symmetric and static space-time ($`\gamma `$-metric). In cylindrical coordinates, static axisymmetric solutions to Einstein equations are given by the Weyl metric

$$ds^2=e^{2\lambda }dt^2e^{2\lambda }\left[e^{2\mu }\left(d\rho ^2+dz^2\right)+\rho ^2d\phi ^2\right],$$
(1)
with

$$\lambda _{,\rho \rho }+\rho ^1\lambda _{,\rho }+\lambda _{,zz}=0$$
(2)
and

$$\mu _{,\rho }=\rho \left(\lambda _{,\rho }^2\lambda _{,z}^2\right)\mu _{,z}=2\rho \lambda _{,\rho }\lambda _{,z}.$$
(3)
Observe that (2) is just the Laplace equation for $`\lambda `$ (in the Euclidean space).

The $`\gamma `$-metric is defined by

$$\lambda =\frac{\gamma }{2}\mathrm{ln}\left[\frac{R_1+R_22m}{R_1+R_2+2m}\right],$$
(4)
$$e^{2\mu }=\left[\frac{\left(R_1+R_2+2m\right)\left(R_1+R_22m\right)}{4R_1R_2}\right]^{\gamma ^2},$$
(5)
where

$$R_1^2=\rho ^2+(zm)^2R_2^2=\rho ^2+(z+m)^2.$$
(6)
It is worth noticing that $`\lambda ,`$ as given by (4), corresponds to the Newtonian potential of a line segment of mass density $`\gamma /2`$ and length $`2m,`$ symmetrically distributed along the $`z`$ axis. The particular case $`\gamma =1,`$ corresponds to the Schwarzschild metric.

It will be useful to work in Erez-Rosen coordinates , given by

$$\rho ^2=(r^22mr)\mathrm{sin}^2\theta z=(rm)\mathrm{cos}\theta ,$$
(7)
which yields the line element as

$$ds^2=Fdt^2F^1\left\{Gdr^2+Hd\theta ^2+\left(r^22mr\right)\mathrm{sin}^2\theta d\phi ^2\right\},$$
(8)
where

$`F`$ $`=`$ $`\left(1{\displaystyle \frac{2m}{r}}\right)^\gamma ,`$ (9)
$`G`$ $`=`$ $`\left({\displaystyle \frac{r^22mr}{r^22mr+m^2\mathrm{sin}^2\theta }}\right)^{\gamma ^21},`$ (10)
and

$$H=\frac{\left(r^22mr\right)^{\gamma ^2}}{\left(r^22mr+m^2\mathrm{sin}^2\theta \right)^{\gamma ^21}}$$
(11)
Now, it is easy to check that $`\gamma =1`$ corresponds to the Schwarzschild metric.

The total mass of the source is  $`M=\gamma m,`$ and the quadrupole moment is given by

$$Q=\frac{\gamma }{3}m^3\left(1\gamma ^2\right).$$
(12)
So that $`\gamma >1`$ ($`\gamma <1`$) corresponds to an oblate (prolate) spheroid.

### 2.2 The interior space-time

The metric within the matter distribution bounded by the surface

$$r=r_\mathrm{\Sigma }$$
(13)
is given by

$`g_{tt}`$ $`=`$ $`f^{2\gamma }`$
$`g_{rr}`$ $`=`$ $`f^{2(1\gamma )}\mathrm{\Delta }^{\gamma ^22}\mathrm{\Sigma }^{1\gamma ^2}`$
$`g_{\theta \theta }`$ $`=`$ $`r^2f^{2\gamma (\gamma 1)}\mathrm{\Phi }^{1\gamma ^2}`$
$`g_{\phi \phi }`$ $`=`$ $`r^2f^{2(1\gamma )}\mathrm{sin}^2\theta `$ (14)
where $`f,`$ $`\mathrm{\Delta },`$ $`\mathrm{\Sigma }`$ and $`\mathrm{\Phi }`$ are functions whose specific form depends on the model under consideration.

The two cases to be considered here are reported in , namely

1. The modified constant density Schwarzschild solution

$`f(r)`$ $`=`$ $`{\displaystyle \frac{3}{2}}\sqrt{1{\displaystyle \frac{r_\mathrm{\Sigma }^2}{B^2}}}{\displaystyle \frac{1}{2}}\sqrt{1{\displaystyle \frac{r^2}{B^2}}}`$ (15)
$`\mathrm{\Delta }(r)`$ $`=`$ $`1{\displaystyle \frac{r^2}{B^2}}`$ (16)
$`\mathrm{\Sigma }(r,\theta )`$ $`=`$ $`1{\displaystyle \frac{r^2}{B^2}}+{\displaystyle \frac{r^4}{4B^4}}\mathrm{sin}^2\theta `$ (17)
$`\mathrm{\Phi }(r,\theta )`$ $`=`$ $`f^2+{\displaystyle \frac{r^4}{4B^4}}V(r)\mathrm{sin}^2\theta `$ (18)
with

$$V(r)=1+\frac{6}{r}_\mathrm{\Sigma }\left(r_\mathrm{\Sigma }r\right),$$
(19)
and

$$B^2=\frac{3}{8\pi \rho _{ss}},$$
(20)
where $`\rho _{ss}`$ denotes the energy density in the spherically symmetric limit ($`\gamma =1`$)
2. The modified Adler solution

$`f(r)`$ $`=`$ $`A+Br^2`$ (21)
$`\mathrm{\Delta }(r)`$ $`=`$ $`1+{\displaystyle \frac{Cr^2}{\left(A+3Br^2\right)^{2/3}}}`$ (22)
$`\mathrm{\Sigma }(r,\theta )`$ $`=`$ $`1+{\displaystyle \frac{Cr^2}{\left(A+3Br^2\right)^{2/3}}}+{\displaystyle \frac{C^2r^4}{4\left(A+3Br^2\right)^{4/3}}}\mathrm{sin}^2\theta `$ (23)
$`\mathrm{\Phi }(r,\theta )`$ $`=`$ $`\left(A+Br^2\right)^2+{\displaystyle \frac{C^2r^4V(r)}{4\left(A+3Br^2\right)^{4/3}}}\mathrm{sin}^2\theta `$ (24)
with

$$V(r)=1+\frac{6}{r}_\mathrm{\Sigma }\left(1\frac{5m}{3r_\mathrm{\Sigma }}\right)\left(1\frac{m}{r}_\mathrm{\Sigma }\right)^1\left(r_\mathrm{\Sigma }r\right)$$
(26)
and

$`A`$ $`=`$ $`{\displaystyle \frac{1\frac{5m}{2r_\mathrm{\Sigma }}}{\left(1\frac{2m}{r_\mathrm{\Sigma }}\right)^{1/2}}}`$
$`B`$ $`=`$ $`{\displaystyle \frac{m}{2r_\mathrm{\Sigma }^3\left(1\frac{2m}{r_\mathrm{\Sigma }}\right)^{1/2}}}`$
$`C`$ $`=`$ $`{\displaystyle \frac{2m\left(1\frac{m}{r_\mathrm{\Sigma }}\right)^{2/3}}{r_\mathrm{\Sigma }^3\left(1\frac{2m}{r_\mathrm{\Sigma }}\right)^{1/3}}}`$ (27)

Before closing this section, two remarks are in order:

1. Since we are considering the source described in (14) as an initial state, the time derivatives of functions $`f,`$ $`\mathrm{\Delta },`$ $`\mathrm{\Sigma }`$ and $`\mathrm{\Phi }`$ will be in principle different from zero.
2. Junction (Darmois) conditions are satisfied at the boundary $`r=r_\mathrm{\Sigma }`$ -see  for details.

## 3 The energy momentum tensor

In order to give physical meaning to the components of the energy momentum tensor in coordinates ($`t,`$ $`r,`$ $`\theta ,`$ $`\phi `$), we shall develop a procedure similar to that used by Bondi  in his study of non static spherically symmetric sources. Thus, we introduce purely local Minkowski coordinates ($`\tau ,`$ $`x,`$ $`y,`$ $`z`$) (alternatively one may introduce a tetrad field associated with locally Minkowskian observers) defined by

$`d\tau `$ $`=`$ $`f^\gamma dt`$ (28)
$`dx`$ $`=`$ $`f^{1\gamma }\mathrm{\Delta }^{1+\gamma ^2/2}\mathrm{\Sigma }^{(1\gamma ^2)/2}dr`$ (29)
$`dy`$ $`=`$ $`rf^{\gamma (\gamma 1)}\mathrm{\Phi }^{(1\gamma ^2)/2}d\theta `$ (30)
$`dz`$ $`=`$ $`r\mathrm{sin}(\theta )f^{1\gamma }d\phi .`$ (31)
Next, since we are assuming that our source does not dissipate energy, then the covariant components of the energy momentum tensor, as measured by a local Minkowskian and comoving with the fluid observer, will be

$$\widehat{T}_{\mu \nu }=\left(\begin{array}{cccc}\rho & 0& 0& 0\\ 0& p_{xx}& p_{xy}& 0\\ 0& p_{yx}& p_{yy}& 0\\ 0& 0& 0& p_{zz}\end{array}\right),$$
(32)
where $`\rho `$ is the energy density and in general $`p_{xx}p_{yy}p_{zz}`$ and $`p_{xy}=p_{yx}.`$ We may write (32) in the form

$$\widehat{T}_{\mu \nu }=\left(\rho +p_{zz}\right)\widehat{U}_\mu \widehat{U}_\nu p_{zz}\eta _{\mu \nu }+\left(p_{xx}p_{zz}\right)\widehat{k}_\mu \widehat{k}_\nu +\left(p_{yy}p_{zz}\right)\widehat{l}_\mu \widehat{l}_\nu +2p_{xy}\widehat{k}_{(\mu }\widehat{l}_{\nu )},$$
(33)
where $`\eta _{\mu \nu }`$ denotes the flat space-time metric and

$`\widehat{U}_\mu `$ $`=`$ $`\left(\begin{array}{cccc}1,& 0,& 0,& 0\end{array}\right)`$ (35)
$`\widehat{k}_\mu `$ $`=`$ $`\left(\begin{array}{cccc}0,& 1,& 0,& 0\end{array}\right)`$ (37)
$`\widehat{l}_\mu `$ $`=`$ $`\left(\begin{array}{cccc}0,& 0,& 1,& 0\end{array}\right)`$ (39)
The components of the energy-momentum tensor $`T_{\mu \nu }`$ in ($`t,`$ $`r,`$ $`\theta ,`$ $`\phi `$) coordinates are linked to (33) by

$$T_{\mu \nu }=\mathrm{\Lambda }_\mu ^\alpha \mathrm{\Lambda }_\nu ^\beta L_\alpha ^\gamma L_\beta ^\delta \widehat{T}_{\gamma \delta },$$
(40)
where the non vanishing components of $`\mathrm{\Lambda }_\mu ^\nu `$ are

$`\mathrm{\Lambda }_t^\tau `$ $`=`$ $`f^\gamma `$ (41)
$`\mathrm{\Lambda }_r^x`$ $`=`$ $`f^{1\gamma }\mathrm{\Delta }^{1+\gamma ^2/2}\mathrm{\Sigma }^{(1\gamma ^2)/2}`$ (42)
$`\mathrm{\Lambda }_\theta ^y`$ $`=`$ $`rf^{\gamma (\gamma 1)}\mathrm{\Phi }^{(1\gamma ^2)/2}`$ (43)
$`\mathrm{\Lambda }_\phi ^z`$ $`=`$ $`r\mathrm{sin}(\theta )f^{1\gamma }.`$ (44)
and the Lorentz matrices $`L_\mu ^\nu `$ are given by

$$L_t^t=\mathrm{\Gamma }L_i^t=L_t^i=\mathrm{\Gamma }w_iL_j^i=L_i^j=\delta _j^i+\frac{(\mathrm{\Gamma }1)w_iw_j}{w^2},$$
(45)
where

$$w^2=w_x^2+w_y^2\mathrm{\Gamma }=\frac{1}{\sqrt{1w^2}},$$
(46)
and $`w_x`$ and $`w_y`$ denote, respectively, the velocity of a fluid element along the $`x`$ and $`y`$ ($`r`$ and $`\theta `$) directions, as measured by our local Minkowskian observer as defined by (28)–(31). Observe that we are considering the case $`w_z=0,`$ which means that the system preserves the reflection symmetry (besides the axial symmetry).

Then, (40) readily gives

$`T_{tt}`$ $`=`$ $`f^{2\gamma }\mathrm{\Gamma }^2\left(\rho +p_{xx}w_x^2+p_{yy}w_y^2+2p_{xy}w_xw_y\right)`$ (47)
$`T_{tr}`$ $`=`$ $`f\mathrm{\Delta }^{1+\gamma ^2/2}\mathrm{\Sigma }^{(1\gamma ^2)/2}\mathrm{\Gamma }\times `$ (48)
$`\left(\mathrm{\Gamma }w_x\rho +p_{xx}w_x\mathrm{\Lambda }_x+p_{yy}w_y\mathrm{\Lambda }+p_{xy}\left[w_x\mathrm{\Lambda }+w_y\mathrm{\Lambda }_x\right]\right)`$
$`T_{t\theta }`$ $`=`$ $`rf^{\gamma ^2}\mathrm{\Phi }^{(1\gamma ^2)/2}\mathrm{\Gamma }\times `$ (49)
$`\left(\mathrm{\Gamma }w_y\rho +p_{xx}w_x\mathrm{\Lambda }+p_{yy}w_y\mathrm{\Lambda }_y+p_{xy}\left[w_y\mathrm{\Lambda }+w_x\mathrm{\Lambda }_y\right]\right)`$
$`T_{rr}`$ $`=`$ $`f^{22\gamma }\mathrm{\Delta }^{\gamma ^22}\mathrm{\Sigma }^{1\gamma ^2}\times `$ (50)
$`\left(\mathrm{\Gamma }^2w_x^2\rho +p_{xx}\mathrm{\Lambda }_x^2+p_{yy}\mathrm{\Lambda }^2+2p_{xy}\mathrm{\Lambda }\mathrm{\Lambda }_x\right)`$
$`T_{r\theta }`$ $`=`$ $`rf^{(\gamma 1)^2}\mathrm{\Delta }^{1+\gamma ^2/2}\mathrm{\Phi }^{(1\gamma ^2)/2}\mathrm{\Sigma }^{(1\gamma ^2)/2}\times `$ (51)
$`\left(\mathrm{\Gamma }^2w_xw_y\rho +\mathrm{\Lambda }\left[p_{xx}\mathrm{\Lambda }_x+p_{yy}\mathrm{\Lambda }_y\right]+p_{xy}\left[\mathrm{\Lambda }^2+\mathrm{\Lambda }_x\mathrm{\Lambda }_y\right]\right)`$
$`T_{\theta \theta }`$ $`=`$ $`r^2f^{2\gamma (\gamma 1)}\mathrm{\Phi }^{1\gamma ^2}\times `$ (52)
$`\left(\mathrm{\Gamma }^2w_y^2\rho +p_{xx}\mathrm{\Lambda }^2+p_{yy}\mathrm{\Lambda }_y^2+2p_{xy}\mathrm{\Lambda }\mathrm{\Lambda }_y\right)`$
$`T_{\phi \phi }`$ $`=`$ $`r^2f^{2(1\gamma )}\mathrm{sin}^2(\theta )p_{zz},`$ (53)
with

$`\mathrm{\Lambda }`$ $``$ $`{\displaystyle \frac{\left(\mathrm{\Gamma }1\right)w_xw_y}{w^2}},`$ (54)
$`\mathrm{\Lambda }_x`$ $``$ $`1+{\displaystyle \frac{\left(\mathrm{\Gamma }1\right)w_x^2}{w^2}},`$ (55)
$`\mathrm{\Lambda }_y`$ $``$ $`1+{\displaystyle \frac{\left(\mathrm{\Gamma }1\right)w_y^2}{w^2}},`$ (56)
So that

$$T_{\mu \nu }=\left(\rho +p_{zz}\right)U_\mu U_\nu p_{zz}g_{\mu \nu }+\left(p_{xx}p_{zz}\right)k_\mu k_\nu +\left(p_{yy}p_{zz}\right)l_\mu l_\nu +2p_{xy}k_{(\mu }l_{\nu )},$$
(57)
where $`U_\mu `$, $`k_\mu `$ and $`l_\mu `$ are obtained after applying the boost velocity (45) and (41)–(44) to (35)–(39),

$$U_\mu =\mathrm{\Gamma }\left(\begin{array}{cccc}f^\gamma ,& w_xf^{1\gamma }\mathrm{\Delta }^{1+\gamma ^2/2}\mathrm{\Sigma }^{(1\gamma ^2)/2},& w_yrf^{\gamma (\gamma 1)}\mathrm{\Phi }^{(1\gamma ^2)/2},& 0\end{array}\right),$$
(58)
$$k_\mu =\left(\begin{array}{cccc}\mathrm{\Gamma }w_xf^\gamma ,& f^{1\gamma }\mathrm{\Delta }^{1+\gamma ^2/2}\mathrm{\Sigma }^{(1\gamma ^2)/2}\mathrm{\Lambda }_x,& rf^{\gamma (\gamma 1)}\mathrm{\Phi }^{(1\gamma ^2)/2}\mathrm{\Lambda },& 0\end{array}\right),$$
(59)
$$l_\mu =\left(\begin{array}{cccc}\mathrm{\Gamma }w_yf^\gamma ,& f^{1\gamma }\mathrm{\Delta }^{1+\gamma ^2/2}\mathrm{\Sigma }^{(1\gamma ^2)/2}\mathrm{\Lambda },& rf^{\gamma (\gamma 1)}\mathrm{\Phi }^{(1\gamma ^2)/2}\mathrm{\Lambda }_y,& 0\end{array}\right).$$
(60)
In the static case $`w_x=w_y=\mathrm{\Lambda }=0`$ and $`\mathrm{\Gamma }=\mathrm{\Lambda }_x=\mathrm{\Lambda }_y=1`$. The same holds after the system departs from equilibrium, on a time scale of the order of (or smaller than) the hidrostatic time scale (see Section 2.4).

## 4 The Tolman mass and departure from equilibrium

We shall now find an expression for the Tolman mass of the source described in the previous section, an then we shall evaluate it just after its departure from equilibrium, on a time scale of the order of (or smaller than) the hydrostatic time scale. Also, since we are interested in the effects produced by small deviations from spherical symmetry, it will be assumed further that the source is quasi–spherical, and therefore we shall put $`\gamma =1+ϵ`$ and will neglect terms of order $`O(ϵ^2)`$ or smaller.

### 4.1 The Tolman mass

The Tolman mass is given by

$`m_T`$ $`=`$ $`{\displaystyle _0^{r_\mathrm{\Sigma }}}{\displaystyle _0^\pi }{\displaystyle _0^{2\pi }}\sqrt{g}(T_0^0T_1^1T_2^2T_3^3)𝑑r𝑑\theta 𝑑\varphi `$ (61)
$`+`$ $`{\displaystyle \frac{1}{8\pi }}{\displaystyle \sqrt{g}g^{\alpha \beta }\frac{}{t}\left[\frac{}{((\sqrt{g}g^{\alpha \beta })/t)}\right]𝑑r𝑑\theta 𝑑\varphi }`$
where $``$ denotes the usual gravitational lagrangian density (eq.(10) in ). Although Tolman’s formula was introduced as a measure of the total energy of the system, with no commitment to its localization, we shall define the mass for any value of $`r`$, smaller or equal to $`r_\mathrm{\Sigma }`$, as

$`m_T`$ $`=`$ $`{\displaystyle _0^r}{\displaystyle _0^\pi }{\displaystyle _0^{2\pi }}\sqrt{g}(T_0^0T_1^1T_2^2T_3^3)𝑑r𝑑\theta 𝑑\varphi `$ (62)
$`+`$ $`{\displaystyle \frac{1}{8\pi }}{\displaystyle \sqrt{g}g^{\alpha \beta }\frac{}{t}\left[\frac{}{((\sqrt{g}g^{\alpha \beta })/t)}\right]𝑑r𝑑\theta 𝑑\varphi }.`$
This extension of the global concept of energy to a local level  is suggested by the conspicuous role played by $`m_T`$ as the “active gravitational mass”.

Indeed, it can be easily shown  that the gravitational acceleration $`a`$ of a test particle, instantaneously at rest in a static gravitational field, as measured with standard rods and coordinate clock is given by

$$a=\frac{m_T}{r^2}.$$
(63)
A similar conclusion can be obtained by inspection of the equation of hydrostatic equlibrium (TOV) (in the static or quasi-static, spherically symmetric case case) .

Even though these properties of Tolman’s definition of mass are only valid in the spherically symmetric and static case, it is reasonable to assume that for small deviations from these conditions, the same role of active gravitational mass may be assigned to our expression.

Let us now evaluate expression (62). After some lengthy calculations one finds:

$`m_T`$ $`=`$ $`2\pi {\displaystyle _0^r}{\displaystyle _0^\pi }r^2\mathrm{sin}\theta f^{\gamma ^22\gamma +2}\mathrm{\Delta }^{\gamma ^2/21}\mathrm{\Sigma }^{(1\gamma ^2)/2}\mathrm{\Phi }^{(1\gamma ^2)/2}`$ (64)
$`\times `$ $`[\mathrm{\Gamma }^2\rho (1+\omega _x^2+\omega _y^2)+p_{xx}(\mathrm{\Gamma }^2\omega _x^2+\mathrm{\Lambda }_x^2+\mathrm{\Lambda }^2)+p_{yy}(\mathrm{\Gamma }^2\omega _y^2+\mathrm{\Lambda }_y^2+\mathrm{\Lambda }^2)`$
$`+p_{zz}+2p_{xy}(\mathrm{\Gamma }^2\omega _x\omega _y+\mathrm{\Lambda }(\mathrm{\Lambda }_x+\mathrm{\Lambda }_y))]drd\theta `$
$`+`$ $`{\displaystyle \frac{1}{4}}{\displaystyle _0^r}{\displaystyle _0^\pi }r^2\mathrm{sin}\theta f^{\gamma ^24\gamma +2}\mathrm{\Delta }^{\gamma ^2/21}\mathrm{\Sigma }^{(1\gamma ^2)/2}\mathrm{\Phi }^{(1\gamma ^2)/2}`$
$`\times `$ $`[2(23\gamma +\gamma ^2){\displaystyle \frac{\ddot{f}}{f}}+(\gamma ^22){\displaystyle \frac{\ddot{\mathrm{\Delta }}}{\mathrm{\Delta }}}+(1\gamma ^2){\displaystyle \frac{\ddot{\mathrm{\Phi }}}{\mathrm{\Phi }}}+(1\gamma ^2){\displaystyle \frac{\ddot{\mathrm{\Sigma }}}{\mathrm{\Sigma }}}`$
$`+2\gamma (1\gamma ^2)(\gamma ^2+2\gamma 3)\left({\displaystyle \frac{\dot{f}}{f}}\right)^2+{\displaystyle \frac{1}{2}}(\gamma ^22)(\gamma ^24)\left({\displaystyle \frac{\dot{\mathrm{\Delta }}}{\mathrm{\Delta }}}\right)^2`$
$`{\displaystyle \frac{1}{2}}(1\gamma ^2)(\gamma ^2+1)\left(\left({\displaystyle \frac{\dot{\mathrm{\Phi }}}{\mathrm{\Phi }}}\right)^2+\left({\displaystyle \frac{\dot{\mathrm{\Sigma }}}{\mathrm{\Sigma }}}\right)^2\right)+(\gamma ^22)(23\gamma ){\displaystyle \frac{\dot{f}}{f}}{\displaystyle \frac{\dot{\mathrm{\Delta }}}{\mathrm{\Delta }}}`$
$`+(1\gamma ^2)(23\gamma ){\displaystyle \frac{\dot{f}}{f}}{\displaystyle \frac{\dot{\mathrm{\Sigma }}}{\mathrm{\Sigma }}}+\gamma (1\gamma ^2)(2\gamma 3){\displaystyle \frac{\dot{f}}{f}}{\displaystyle \frac{\dot{\mathrm{\Phi }}}{\mathrm{\Phi }}}`$
$`+(1\gamma ^2)(\gamma ^22){\displaystyle \frac{\dot{\mathrm{\Delta }}}{\mathrm{\Delta }}}{\displaystyle \frac{\dot{\mathrm{\Sigma }}}{\mathrm{\Sigma }}}]drd\theta `$
We shall now evaluate this last expression at the very moment the system leaves the equilibrium, and for small non–sphericity.

### 4.2 Departure from equilibrium

Let us now consider that our source, once submitted to perturbations, departs from equilibrium without dissipation. We shall then evaluate the system after such departure, on a time scale such that $`w_x`$ and $`w_y`$ remain vanishingly small, whereas their time derivatives though small, will be different from zero.

Thus, just after leaving the equilibrium, the following conditions hold

$$w_x=w_y=w_{x,i}=w_{y,i}0,(i=r,\theta ,\phi )$$
(65)
$$\dot{w}_x,\dot{w}_y0(\text{small})$$
(66)
where dots denote derivative with respect to $`t`$.

From now on, unless otherwise stated, all equations are evaluated at the moment the system starts to deviate from equilibrium.

Then from (47)–(53), we obtain using (65)

$$T_{t\theta }=T_{tr}=0$$
(67)
which implies, because of field equations (see  for details)

$$\dot{\mathrm{\Delta }}=\dot{f}=\dot{\mathrm{\Sigma }}=\dot{\mathrm{\Phi }}=0$$
(68)
where for simplicity we write $`0`$ for $`𝒪(\omega )`$ (as we shall do hereafter).

Obviously, spatial derivatives of the above quantities will be also vanishingly small on the time scale under consideration.

Also, from evaluation of the $`t`$-component of the conservation law $`T_{\nu ;\mu }^\mu =0`$, we get (see ).

$$\dot{\rho }=0$$
(69)
Then, in the approximation above, the expression for the Tolman mass becomes

$`m_T`$ $`=`$ $`2\pi {\displaystyle _0^r}{\displaystyle _0^\pi }r^2\mathrm{sin}\theta f^{(\gamma ^22\gamma +2)}\mathrm{\Delta }^{(\gamma ^2/21)}\mathrm{\Sigma }^{(1\gamma ^2)/2}\mathrm{\Phi }^{(1\gamma ^2)/2}`$
$`\times `$ $`(T_0^0T_1^1T_2^2T_3^3)drd\theta d\varphi `$
$`+`$ $`{\displaystyle \frac{1}{4}}{\displaystyle _0^r}{\displaystyle _0^\pi }r^2\mathrm{sin}\theta f^{(\gamma ^24\gamma +2)}\mathrm{\Delta }^{(\gamma ^2/21)}\mathrm{\Sigma }^{(1\gamma ^2)/2}\mathrm{\Phi }^{(1\gamma ^2)/2}`$
$`\times `$ $`\left[2(\gamma ^23\gamma +2){\displaystyle \frac{\ddot{f}}{f}}+(\gamma ^22){\displaystyle \frac{\ddot{\mathrm{\Delta }}}{\mathrm{\Delta }}}+(1\gamma ^2)\left({\displaystyle \frac{\ddot{\mathrm{\Sigma }}}{\mathrm{\Sigma }}}+{\displaystyle \frac{\ddot{\mathrm{\Phi }}}{\mathrm{\Phi }}}\right)\right]drd\theta d\varphi `$
We shall now write $`\gamma =1+ϵ`$, then assuming that non–sphericity is small (quasi–spherical approximation), the expression above reads:

$`m_T`$ $`=`$ $`2\pi {\displaystyle _0^r}{\displaystyle _0^\pi }r^2\mathrm{sin}\theta f\mathrm{\Delta }^{(ϵ1/2)}\mathrm{\Sigma }^ϵ\mathrm{\Phi }^ϵ\times (T_0^0T_1^1T_2^2T_3^3)𝑑r𝑑\theta 𝑑\varphi `$
$`+`$ $`{\displaystyle \frac{1}{4}}{\displaystyle _0^r}{\displaystyle _0^\pi }r^2\mathrm{sin}\theta f^{(1+2ϵ)}\mathrm{\Delta }^{(ϵ1/2)}\mathrm{\Sigma }^ϵ\mathrm{\Phi }^ϵ`$
$`\times `$ $`\left[{\displaystyle \frac{\ddot{\mathrm{\Delta }}}{\mathrm{\Delta }}}+2ϵ\left({\displaystyle \frac{\ddot{f}}{f}}+{\displaystyle \frac{\ddot{\mathrm{\Delta }}}{\mathrm{\Delta }}}{\displaystyle \frac{\ddot{\mathrm{\Sigma }}}{\mathrm{\Sigma }}}{\displaystyle \frac{\ddot{\mathrm{\Phi }}}{\mathrm{\Phi }}}\right)\right]drd\theta d\varphi `$
Within our two approximations (quasi–spherical and (65)–(68)) it follows from (47)–(56) that:

$$T_0^0T_1^1T_2^2T_3^3=\rho +p_{xx}+p_{yy}+p_{zz}$$
(72)
Also within these approximations, the time derivative of the $`tr`$ component of the Einstein equations $`G_{rt}=8\pi T_{rt}`$, yields

$``$ $`{\displaystyle \frac{1}{r}}{\displaystyle \frac{\ddot{\mathrm{\Delta }}}{\mathrm{\Delta }}}+2ϵ\left[{\displaystyle \frac{\ddot{\mathrm{\Phi }}^{}}{2\mathrm{\Phi }}}+{\displaystyle \frac{\mathrm{\Phi }^{}}{2\mathrm{\Phi }}}{\displaystyle \frac{\ddot{\mathrm{\Delta }}}{2\mathrm{\Delta }}}+{\displaystyle \frac{1}{r}}\left({\displaystyle \frac{\ddot{\mathrm{\Delta }}}{\mathrm{\Delta }}}{\displaystyle \frac{\ddot{\mathrm{\Sigma }}}{\mathrm{\Sigma }}}{\displaystyle \frac{\ddot{f}}{f}}+{\displaystyle \frac{\ddot{\mathrm{\Phi }}}{2\mathrm{\Phi }}}\right){\displaystyle \frac{\ddot{\mathrm{\Phi }}}{2\mathrm{\Phi }}}\left({\displaystyle \frac{f^{}}{f}}+{\displaystyle \frac{\mathrm{\Phi }^{}}{\mathrm{\Phi }}}\right)\right]`$ (73)
$`=`$ $`8\pi f\mathrm{\Delta }^{(ϵ1/2)}\mathrm{\Sigma }^ϵ\left[\dot{\omega }_x(\rho +p_{xx})+\dot{\omega }_yp_{xy}\right].`$
Feeding back (72) and (73) into (LABEL:mtse), one obtains after some rearrangements

$`m_T`$ $`=`$ $`2\pi {\displaystyle _0^r}{\displaystyle _0^\pi }r^2\mathrm{sin}\theta f\mathrm{\Delta }^{(ϵ1/2)}\mathrm{\Sigma }^ϵ\mathrm{\Phi }^ϵ\times (\rho +p_{xx}+p_{yy}+p_{zz})𝑑r𝑑\theta `$
$`+`$ $`2\pi {\displaystyle _0^r}{\displaystyle _0^\pi }r^3\mathrm{sin}\theta f^{2ϵ}\mathrm{\Delta }^{(2ϵ1)}\mathrm{\Sigma }^{2ϵ}\mathrm{\Phi }^ϵ\left[\dot{\omega }_x(\rho +p_{xx})+\dot{\omega }_yp_{xy}\right]𝑑r𝑑\theta `$
$``$ $`{\displaystyle \frac{3}{4}}ϵ{\displaystyle r^2\mathrm{sin}\theta f^{(1+2ϵ)}\mathrm{\Delta }^{(ϵ1/2)}\mathrm{\Sigma }^ϵ\mathrm{\Phi }^ϵ\frac{\ddot{\mathrm{\Phi }}}{\mathrm{\Phi }}drd\theta }`$
$``$ $`{\displaystyle \frac{1}{4}}ϵ{\displaystyle r^3\mathrm{sin}\theta f^{(1+2ϵ)}\mathrm{\Delta }^{(ϵ1/2)}\mathrm{\Sigma }^ϵ\mathrm{\Phi }^ϵ}`$
$`\times `$ $`\left[{\displaystyle \frac{\ddot{\mathrm{\Phi }}^{}}{2\mathrm{\Phi }}}+{\displaystyle \frac{\mathrm{\Phi }^{}}{2\mathrm{\Phi }}}{\displaystyle \frac{\ddot{\mathrm{\Delta }}}{2\mathrm{\Delta }}}+{\displaystyle \frac{1}{r}}\left({\displaystyle \frac{\ddot{\mathrm{\Delta }}}{\mathrm{\Delta }}}{\displaystyle \frac{\ddot{\mathrm{\Sigma }}}{\mathrm{\Sigma }}}{\displaystyle \frac{\ddot{f}}{f}}+{\displaystyle \frac{\ddot{\mathrm{\Phi }}}{2\mathrm{\Phi }}}\right){\displaystyle \frac{\ddot{\mathrm{\Phi }}}{2\mathrm{\Phi }}}\left({\displaystyle \frac{f^{}}{f}}+{\displaystyle \frac{\mathrm{\Phi }^{}}{\mathrm{\Phi }}}\right)\right]drd\theta `$
### 4.3 The spherically symmetric case

Before entering into the discussion of (LABEL:mtf), it is quite instructive to analyze the spherically symmmetric situation. In this case one easily obtains from (LABEL:mtf)

$`m_T`$ $`=`$ $`4\pi {\displaystyle _0^r}r^2f\times (\rho +p_{xx}+p_{yy}+p_{zz})𝑑r`$ (75)
$`+`$ $`4\pi {\displaystyle _0^r}r^3\mathrm{\Delta }^1\left[\dot{\omega }_x(\rho +p_{xx})\right]𝑑r`$
with $`p_{yy}=p_{zz}`$. Now, the first term in (75) correspond to the active gravitational mass of the core of radius $`r`$ interior to $`r_\mathrm{\Sigma }`$ before the system leaves the equilibrium. Let us now assume that the system leaves the equilibrium and starts to collapse (expand), then $`\dot{\omega }_x<0`$ ($`\dot{\omega }_x>0`$) decreasing (increasing) the value of the Tolman mass with respect to its value at equilibrium. Thus the second term in (75) tends to stabilize the system, opposing any departure from equilibrium (contraction or expansion). This result was already known .

Let us now get back to the non–spherical case to see how small non–sphericities change the whole picture.

### 4.4 The non–spherical case

Let us now turn back to (LABEL:mtf), to infer what happens in the non-spherical case (i.e. $`\epsilon 0`$), even though $`\epsilon <<1.`$ Then neglecting higher order terms on $`\epsilon `$, and keeping only the leading terms, we get

$`m_T`$ $`=`$ $`2\pi {\displaystyle _0^r}{\displaystyle _0^\pi }r^2\mathrm{sin}\theta f\mathrm{\Delta }^{(ϵ1/2)}\mathrm{\Sigma }^ϵ\mathrm{\Phi }^ϵ\times (\rho +p_{xx}+p_{yy}+p_{zz})𝑑r𝑑\theta `$
$`+`$ $`2\pi {\displaystyle _0^r}{\displaystyle _0^\pi }r^3\mathrm{sin}\theta f^{2ϵ}\mathrm{\Delta }^{(2ϵ1)}\mathrm{\Sigma }^{2ϵ}\mathrm{\Phi }^ϵ\left[\dot{\omega }_x(\rho +p_{xx})\right]𝑑r𝑑\theta `$
In order to extract more information from (LABEL:och) it is necessary to specify the source under consideration. We shall use the two configurations mentioned in section 2. In both cases, $`f`$ vanishes at the central region for $`r_\mathrm{\Sigma }>2m`$. Thus, in the Schwarzschild-like models we have $`f(0)=0`$, if $`2m/r_\mathrm{\Sigma }=8/9`$. Since we know that any spherically symmetric static configuration with constant $`\rho _{ss}`$ and locally isotropic pressure should satisfy the constraint $`n2M/r_\mathrm{\Sigma }<8/9`$ we may assume that the system leaves the equilibrium for values of $`n`$ close to $`8/9`$. Then, an inspection of (LABEL:och) shows that (if $`\epsilon >0`$), for values of $`n`$ approaching $`8/9`$, the second term incresases due to the factor $`f^{2ϵ}`$.

We may now use Einstein equations to elucidate that for negative values of $`\epsilon `$ the system may be unphysical. If $`n`$ takes values close to the limit allowed by the model (8/9 for Schwarzschild-type model and 4/5 for Adler-type model), the critical values ($`f0`$) appear close to $`r=0`$. Outside of this region the system is basically composed by an spherical incompressible fluid plus a perturbation in $`\epsilon `$. Thus, the physical or unphysical character of the model is determined by its behaviour close to these two limits.

The energy density, in the limit $`r0`$, for the Schwarzschild-type model and Adler-type model is given by expresions see ( for details)

$$\rho =\frac{m}{2\pi r_\mathrm{\Sigma }^3}f^{2\epsilon }\left[\frac{3}{2}+\epsilon \left(1+\frac{1}{3\sqrt{1\frac{2m}{r_\mathrm{\Sigma }}}1}\right)\right]$$
(77)
and

$$\rho =\frac{3m}{4\pi r_\mathrm{\Sigma }^3\left(12m/r_\mathrm{\Sigma }\right)^{1/3}}\left(\frac{15m/2r_\mathrm{\Sigma }}{\sqrt{12m/r_\mathrm{\Sigma }}}\right)^{2\epsilon 2/3}\left[\left(1m/r_\mathrm{\Sigma }\right)^{2/3}+\frac{\epsilon }{\left(15m/2r_\mathrm{\Sigma }\right)^{1/3}}\right]$$
(78)
respectively. From these ones, it is easy to show that if $`\epsilon <0`$, the energy density becomes negative as the system approaches to $`n8/9`$ (Schwarzschild case) or $`n4/5`$ (Adler case) and positive for $`\epsilon 0`$. Therefore, in both cases, positive energy conditions impose $`\epsilon 0`$, and for very compact objects (close to the limit allowed by the model) the “stabilizying”term in the expression for the active gravitational mass substantially increases in the central region, close to, but before, the maximum allowed value of $`n`$.

## 5 Conclusions

We have seen so far that (as expected), for high gravitational fields, important differences appear in the way that the spherical and non-spherical systems depart from equilibrium. This conclusion being true even for small non-sphericity.

In the two models considered above, a factor multiplying the stabilizying term in the expression for the active gravitational mass, brings out those differences. Although for the two examples considered here, we have considered $`\epsilon >0,`$ it is obvious that there exist models with $`\epsilon <0,`$ in which case the stabilizying term may become very small, leading to highly unstable situations. In fact, it is worth noticing that important differences between the two cases ($`\epsilon >0`$ and $`\epsilon <0`$) appear also in the behaviour of the exterior $`\gamma `$-metric (, )

Thus, on the basis of presented results we may conclude that whatever the model and the sign of $`\epsilon `$ would be, any source of Weyl metric would evolve quite differently from the corresponding spherical source, as critical values of $`n`$ are considered.

In particular, in the examples examined, the departure from equilibrium appears to be affected by a sharp modification in the stabilyzying term of the active gravitational mass, as $`n`$ approaches its maximum allowed value. This change makes the system more stable, hindering its departure from equilibrium.

Before concluding, the following remarks are in order:

1. Observe that all results above are valid only on a time scale of the order of (or smaller than) hydrostatic time scale. Within this time scale, the general form of the metric and the components of the energy–momentum tensor, is the same as in the static case (of course in the former case time dependence of variables has to be taken into account when taking time derivatives of such components)
2. In  it is shown that the two interiors described in Section 2.2, match smoothly (on $`r_\mathrm{\Sigma }`$) with the $`\gamma `$ metric, in the static case. That this is also the case after the system departs from equilibrium (on a time scale of the order of, or smaller than, hydrostatic time scale) is apparent from (68) and comments after equation (57) and in the point 1 above. Of course in the fully dynamic case (beyond the hydrostatic time scale), (68) does not longer hold, and matching conditions have to be established. But this is out of the scope of this paper.

## acknowledgements

LH acknowledges financial assistance under grant BFM2000-1322 (M.C.T. Spain).