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# Scaling of the Coercive Field with Thickness in Thin-Film Ferroelectrics

## Abstract

Motivated by the observed thickness-scaling of the coercive field in ferroelectric films over five decades, we develop a statistical approach towards understanding the conceptual underpinnings of this behavior. Here the scaling exponent is determined by the field-dependence of a known and measured quantity, the nucleation rate per unit area. We end with a discussion of our initial assumptions and point to instances where they could no longer be applicable.

Experimentally the coercive field ($`E_c`$) of a thin-film ferroelectric increases with decreasing sample thickness ($`d`$). Recently we have shown that $`E_c`$ displays a specific thickness-dependence, $`E_cd^{2/3}`$, over five decades ranging from 100 microns down to 1 nanometer. Here we study the conceptual underpinnings of this dramatic scaling behavior. Guided by a set of experimental facts, we develop a statistical approach that yields the expression, $`E_cd^{\frac{1}{\alpha }}`$. In particular we find that this exponent $`\alpha `$ is determined by the field-dependence of another measured quantity, the nucleation rate unit area ($`N(E)`$). Experimentally it is known that $`\alpha =3/2`$, which then leads to the observed scaling relation, $`E_cd^{2/3}`$. Finally we emphasize the necessary conditions for this scaling to occur, indicating situations where it may not be applicable.

The thickness-dependence of the coercive field in ferroelectric films ranging from 100 microns to 200 nanometers has been known to display the relation $`E_cd^{2/3}`$ for some time. However recent measurements of $`E_c`$ for PVDF films down to one nanometer indicate significant deviation from the expected scaling behavior. Elsewhere we have noted that at such small length-scales the imperfect conducting nature of the capacitor electrodes becomes important. More specifically the full charge on each plate does not reside in the plane of the ferroelectric-electrode interface, completely compensating for the spontaneous polarization in the ferroelectric film. Rather it is distributed over a small but finite region in the electrode, and there is incomplete charge conpensation at the interface. Physically this results in a depolarization field in the film which must play a role in the switching process. Since the potential in the imperfect but realistic electrodes results from the induced charge density it will be proportional to the spontaneous polarization $`P_s`$ in the film. In many ferroelectric materials $`P_s`$ is weakly $`d`$-dependent so that the depolarization field will scale roughly inversely with $`d`$; then the associated corrections will be important in films of decreasing thickness.

The presence of a depolarization potential indicates that the switching field measured by the external circuit is not the same as that in the ferroelectric. More specifically the coercive field in the film is

$$E_c=\frac{V+8\pi P_sa}{d+ϵ_f(2a)}$$
(1)
where $`V`$ is the voltage drop across the capacitor, $`a=\frac{\lambda }{ϵ_e}`$ is a normalized screening length ($`\lambda `$) associated with the charge, and $`ϵ_e`$ and $`ϵ_f`$ are the dielectric constants of the metal electrodes and the film respectively. Here we have assumed a Yukawa form for the charge density at the ferrolectric-electrode interface. We observe that when $`a=0`$ we recover the result that the film and the measured fields are identical ($`E_c=\frac{V}{d}`$). For PVDF the addition of such depolarization corrections to the measured coercive fields leads to the recovery of the scaling behavior. We refer the interested reader elsewhere for more details of this treatment. In Figure 1 we present a normalized scaling plot of $`\mathrm{log}\frac{E_c}{C}`$ vs $`\mathrm{log}d`$ where $`C`$ for three distinct material types of ferroelectric films and note that the slope of this line is $`s=0.66`$ for five decades; here $`C`$ is a materials-specific thickness-independent normalization constant. For the PVDF data, we estimated the screening length associated with the aluminum electrodes to be $`a=0.45\AA `$ using a Thomas-Fermi approximation; in the inset of Figure 1 we display the inverse capacitance vs. thickness data for the PVDF films, and note that our fit yields $`a=0.34\pm 0.15\AA `$ so that our estimate is within the bounds set by the experiment.

Motivated by the tremendous success of this semi-empirical scaling relation, $`E_cd^{2/3}`$, we now turn towards understanding its conceptual foundations. First, we recall that an electric field is proportional to a force and thus is usually an intensive quantity. Thus the observation that the coercive field is thickness-dependent indicates the breakdown of standard self-averaging. This raises the possibility that homogenous nucleation might be responsible for the observed $`E_c(d)`$, since here rare fluctuations determine physical quantities. However such processes have been shown to be energetically improbable in ferroelectrics. Furthermore we expect that the probability of having rare fluctuations anywhere in the sample would increase with system size, resulting in a decreasing $`E_c`$ with diminishing thickness in contradiction with observation.

We can posit a voltage drop across a surface layer at the metal-ferroelectric interface; then the coercive field of the entire ferroelectric film is thickness-dependent. However the resulting $`E_c`$ is inversely proportional to $`d`$, which is not in agreement with experiment. Noting the observed scaling behavior, $`E_cd^{2/3}`$, Janovec and later Kay and Dunn developed phenomenological appproaches to the problem that involved the characterization of rare fluctuations at the metal-electrode boundary. Though conceptually appealing, their treatments were logically inconsistent since they applied ideas of homogenous nucleation, with uniform probability of reverse-domain creation throughout the film, to particular sites on the sample boundary. The observed $`d`$-dependence of $`E_c`$ is recovered in these papers, and results from the specific geometry of the critical nucleus, a half prolate spheroid. This conceptual pathway to the scaling law is somewhat surprising given the latter’s broad application to materials with rather different microscopic qualities. Finally it is important to establish the working limits of this scaling behavior; for example, clearly it will not be appropriate for bulk crystals.

The coercive field is a kinetic quantity, and the associated switching involves many complex processes that include the nucleation and growth of a distribution of domains. Clearly any theoretical attempt to recover the observed scaling behavior must be guided by experiment in its choice of initial assumptions. Here we use a statistical approach to model $`E_c`$, restricting our attention to its quasi-static amplitude. Supported by imaging measurements, we argue that the nucleation of “dissident” domains in thin ferroelectric films is most probable at the electrode boundaries. The reversal of the sample’s macroscopic polarization is initiated by the nucleation and subsequent growth of many of these independent domains that develop in parallel (cf. Figure 2). This approach clearly neglects long-range interactions in the system, though it can be adapted to include them at the mean-field level. However we expect that in thin films, the Coulomb force will be screened by charges on the ferroelectric-electrode interfaces. Elastic interactions can have important scale-dependent effects on the transition temperatures in these systems, but they are not expected to contribute to $`E_c(d)`$ since the strain energy is usually weakly dependent on field direction.

We now show that the observed thickness scaling of the coercive field can be recovered from an adapted Kolmogorov-Avrami model of inhomogenous nucleation in a confined geometry. The coercive field is defined by the condition that half the sample is transformed. More specifically the thickness-dependence of $`E_c`$ is determined by the expression $`U(E,d)|_{E=E_c}=\frac{1}{2}`$ where $`U(E,d)`$ is the untransformed sample fraction as a function of applied (quasi-static) field $`E`$ and thickness $`d`$. In a model of nucleation and growth, the rate of transformation of a region at time $`t`$ is governed not only by the nucleation rate there but also by the probability that a domain that was nucleated earlier somewhere else in the sample sweeps into the region in question. As mentioned above, there is strong evidence from experiment that nucleation events occur predominantly at the ferroelectric-electrode interface. For the large electric fields ($`10`$ kV/cm) corresponding to the thin-films of our study, it is known that $`v_f`$, the forward domain velocity, is of the order of the speed of sound. By contrast $`v_l`$, the lateral domain motion is field-dependent and is significantly slower; furthermore it is not expected have a strong dependence on film thickness and should therefore make a neglible contribution to $`E_c(d)`$. In our treatment we will therefore assume that the nucleation rate, known to increase with increasing field strength, is high enough that the film is transformed by large numbers of independent nucleation events, rather than by the slow lateral growth of a few domains (cf. Figure 2); this approximation is supported by a detailed quantitative analysis for PZT films of dimensions comparable to those used in this study.

The rate of change of the untransformed fraction of the sample, $`U(E,d)`$, decreases as a function of increasing time, and is proportional to the product of the material available, $`U(E,d)`$, and the nucleation rate. For the homogenous case, where nucleation is equally probable throughout the sample, this rate is defined as the nucleation per unit volume multiplied by a characteristic volume that the critical nucleus has swept out in a given time. By contrast for the interface-specific inhomogenous nucleation considered here, we are interested in a nucleation rate per unit area, $`N`$, and the lateral area of a domain, $`𝒜`$; experimentally $`N=N(E)`$ is known to be field-dependent. We therefore obtain a simple expression for the time-dependence of $`U(E,d)`$

$$\frac{dU}{dt}UN(E)𝒜$$
(2)
where we implicity assume that the time associated with the domain to propagate across the thickness of the film, $`t_f`$, is shorter than the period of the a.c. driving electric field. This time-scale, $`t_f=\frac{d}{v_f}`$, is roughly a nanosecond for a micron-thick film where the forward domain velocity, $`v_f`$, is of order the speed of sound and is known to be asymptotically independent of field-strength at high fields; we note that the thickness provides a natural time-scale that cuts off the time evolution of the system. The resulting expression for the fraction of the sample untransformed as function of field and thickness, can therefore be taken to be quasi-static for all practical measurements since domain propagation across the film is effectively instantaneous . With the time replaced by the natural time scale $`t_f`$, we have

$$U(E,d)\mathrm{exp}N(E)\left(\frac{𝒜d}{v_f}\right).$$
(3)
It is important to note that within this framework many independent nucleation and growth events occur in parallel, so that the detailed nature of the final state is not crucial (cf. Figure 2). In Figure 2 we assume columnar grains for graphical simplicity; there the shaded regions refer to the untranformed parts of the sample.

The equation (3) is valid with the implicit underlying assumption that nucleation dominates over lateral growth. In order to obtain a more quantitative condition for the validity of this expression, we can do a direct comparision of these two different rates. More specifically, the change in time of the transformed fraction by lateral growth is proportional to the number of transformed domains $`(\frac{1U}{𝒜})`$ and their lateral velocity ($`\frac{d𝒜}{dt}`$) which results in

$$\frac{d(1U)}{dt}=(1U)\frac{d\mathrm{ln}𝒜}{dt}.$$
(4)
An expression for a similar change due to nucleation is simply proportional to the untransformed fraction and the nucleation rate and is

$$\frac{d(1U)}{dt}=UN𝒜.$$
(5)
Then in order for lateral growth to be less important than nucleation we must have

$$\frac{d\mathrm{ln}𝒜}{dt}<<N𝒜$$
(6)
where we take $`U\frac{1}{2}`$ since this is its value when $`EE_C`$. Therefore (6) is our working premise for the validity of equation (3) and all that follows from it. We note that recent atomic force microscopy studies of switching in thin ferroelectric films support our contention that it is dominated by domain forward growth processes.

For field-strengths greater than $`10kV/cm`$, relevant for the thin-films studied here, the nucleation rate per unit area is known to have a power-law dependence on applied field. If we accordingly put $`N(E)E^\alpha `$ in (3), the expression for the thickness-dependence of the coercive field, $`U(E_c,d)=\frac{1}{2}`$, becomes $`E_c^\alpha d1`$; this then yields

$$E_cd^{\frac{1}{\alpha }}.$$
(7)
Experimentally and theoretically, it is known from switching kinetics that $`\alpha =\frac{3}{2}`$ over a broad range of fields; this value of $`\alpha `$ then leads to the result $`E_cd^{2/3}`$. We note that the scaling of $`E_c`$ with thickness follows directly from the field-dependence of the density of nucleation sites, $`N(E)`$, which is a statistical quantity that could plausibly have similar behavior for materials with different microscopic features.

We have therefore successfully recovered the observed thickness scaling of the coercive field using a statistical approach that is not dependent on particular sample specifics. It is important to be clear about our underlying assumptions, and to point to situations where they could break down. First of all, we have assumed that nucleation of new reverse-polarization domains occur solely at the ferroelectric-electrode interface. Next we have considered situations where the transformation of the new polarization domains occurs predominantly by nucleation and not by lateral growth of preexisting “dissident” ones. Finally we assume that, once formed, the new domains grow unimpeded to the other side of the film. Clearly these assumptions will not be valid for all ferroelectric capacitors. For example it is known that for thicker samples than those considered here, the switching process is dominated by lateral growth. The specific length-scale where this occurs depends on material-specific quantities. Similarly in disordered and granular films, grain boundaries and charge vacancies could act as nucleation centers away from the sample edges. Finally defects in the ferroelectric could obstruct the motion of domains, and then again we would not expect the scaling relation discussed here to be appropriate.

In summary, we have presented a statistical model that leads to a specific thickness-dependence of the coercive field. This scaling behavior is observed over five decades of length-scale in several different materials. Guided by a number of experimental observations, we recover the observed scaling by assuming that nucleation at the electrode interface dominates the switching process, and that the resulting “dissident” domains propagate uninhibited across the film’s thickness. The exponent associated with the functional form of $`E_c(d)`$ is related to another known and measured exponent, that associated with the field-dependence of the nucleation rate per unit area. We emphasize that $`N(E)`$ is a quantity that is not dependent on sample microscopics, and thus our result is compatible with experimental findings. We note that there remain a number of unresolved theoretical issues associated with this derivation of $`E_c`$ that include the calculation of realistic energy barriers and the determination of the absolute rather than the relative magnitude of $`E_c`$. Finally we would like to study the behavior of the coercive field at finite-frequency, and in this case it may not be possible to neglect the long-range elastic and Coulomb interactions as we have done here.

We thank K. Rabe for discussions.

Figure Captions

1. (Main Figure) The normalized corrected log coercive field vs. log thickness which indicates scaling over five decades of length-scale. The slope is $`0.66\pm 0.02`$, in agreement with the theoretical value of $`\frac{2}{3}`$. (Inset) Inverse-capacitance vs. thickness of PVDF data where the y-intercept is related to the screening length used in the depolarization correction.
2. A schematic of the statistical approach to the scaling law. The sample is originally poled (a). Application of a small electric field leads to a number of nucleation events at the electrodes, $`N(E)`$, which then grow across the same. For $`E<E_c`$, the fraction of the sample that is untransformed (shaded regions), $`U(E)`$, is more than one-half. The nucleation density of reverse-polarization domains increases with increasing applied field, $`N(E)E^\alpha `$. For $`E=E_c`$, one-half of the system remains untransformed. Details of the domain structure of the final state are not important, and the thickness-dependence of $`E_c`$ is determined by the field-dependence of the nucleation density.

Fig. 1

Fig. 2


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# Spin Fluctuations and the Magnetic Phase Diagram of ZrZn2

## Abstract

The magnetic properties of the weak itinerant ferromagnet ZrZn2 are analyzed using Landau theory based on a comparison of density functional calculations and experimental data as a function of field and pressure. We find that the magnetic properties are strongly affected by the nearby quantum critical point, even at zero pressure; LDA calculations neglecting quantum critical spin fluctuations overestimate the magnetization by a factor of approximately three. Using renormalized Landau theory, we extract pressure dependence of the fluctuation amplitude. It appears that a simple scaling based on the fluctuation-dissipation theorem provides a good description of this pressure dependence.

The physics of metals near ferromagnetic quantum critical points (QCPs) has attracted renewed interest following several recent discoveries of materials with unusual still poorly understood transport and thermodynamic properties, as well as unusual low-temperature states, particularly superconductivity coexisting with ferromagnetism.  From a generic, qualitative point of view, the phenomena are understood as being connected with renormalization, scattering and pairing due to strong fluctuations in the ferromagnetic order parameter (i.e., spin fluctuations) as the critical point is approached. Besides the mentioned superconducting transition, in clean samples of many weak itinerant ferromagnetic metals the magnetic transition near the QCP crosses over from the second order to the weakly first order, although whether this happens in ZrZn2 is not yet established. The physics of this cross-over is not clear yet. In any case, quantitative, material specific understanding of these phenomena is still lacking.

ZrZn2 is a prototypical example of a weak itinerant (Stoner) ferromagnet. Very small magnetic moments (0.12 to 0.23 $`\mu _B`$) have been reported. These do not saturate even at fields up to 35 T, indicating softness of the magnetic moment amplitude and suggesting existence of soft longitudinal spin fluctuations. The Curie temperature, $`T_C`$ drops approximately linearly with pressure, starting at $`29`$ K at $`P=0`$ and decreasing to $`4`$ K at $`P=16`$ kbar,  which extrapolates to a QCP at $`P=1820`$ kbar. The discovery of superconductivity in the ferromagnetic (FM) phase  resulted in renewed interest in this compound, including several theoretical studies (Refs.  and others). The relative structural simplicity of this compound and the availability of high quality experimental data as functions of $`H`$, $`T`$ and $`P`$ on clean samples suggest this material as a test case for developing understanding of quantum critical phenomena in ferromagnetic metals. Here we focus on the magnetic properties, in particular the renormalization of LDA results due to fluctuations.

Density functional theory is in principle an exact ground state theory. It should, therefore, correctly describe the spin density of magnetic systems. This is usually the case in actual state of the art density functional calculations. However, common approximations to the exact density functional theory, such as the LDA, may miss important physics and indeed fail to describe some materials. A well know example is in strongly Hubbard correlated systems, where the LDA treats the correlations in an orbitally averaged mean field way and underestimates the tendency towards magnetism. Overestimates of magnetic tendencies, especially in the LDA, are considerably less common, the exceptions being materials near magnetic QCPs; here the error comes from neglect of low energy quantum spin fluctuations. Indeed, the LDA is parameterized based on the uniform electron gas at densities typical for atoms and solids. However, the uniform electron gas at these densities is stiff against magnetic degrees of freedom and far from magnetic QCP’s. Thus, although the LDA is exact for the uniform electron gas, and therefore does include all fluctuation effects in the uniform electron gas, its description of magnetic ground states in solids and molecules is mean field like. This leads to problems such as the incorrect description of singlet states in molecules with magnetic ions as well as errors in solids when spin fluctuation effects beyond the mean field are important. In solids near a QCP, the result is an overestimate of the magnetic moments and tendency toward magnetism (i.e. misplacement of the position of the critical point) due to neglect of the quantum critical fluctuations.  Examples include Sc3In,  ZrZn2,  and Sr3Ru2O7 (Ref. ). Sr3Ru2O7 displays a novel metamagnetic quantum critical point,  while, as mentioned, ZrZn2 shows coexistence of ferromagnetism and superconductivity. The effects of such quantum fluctuations can be described on a phenomenalogical level using a Ginzburg-Landau theory, in which the magnetic properties defined by the LDA fixed spin moment curve are renormalized by averaging with an assumed (usually Gaussian) function describing the beyond LDA critical fluctuations.  Although a quantitative theory allowing extraction of this function from first principles calculations has yet to be established, one can make an estimate based on the LDA fixed spin moment curves as compared with experiment.

LDA calculations of the magnetic properties of ZrZn2 (Refs. ) are found to be sensitive to shape approximations, possibly because of the very small energy scales involved. In particular, atomic sphere approximations result in smaller magnetizations than those found by more accurate full potential methods.  In fact, it was found that full potential calculations produce a Stoner factor of $`1.16,`$ as opposed to 1.01 in the atomic sphere calculations, indicating a stronger tendency to magnetism in the full-potential calculations.

Our full potential LDA calculations for ZrZn2 at its experimental volume yield a magnetization of 0.72 $`\mu _B`$ per formula unit – 3 to 4 times larger than experiment, reflecting an crucial role for the renormalization of the magnetization due to beyond LDA fluctuations, presumably associated with the QCP.

As mentioned, one can incorporate such fluctuations into LDA calculations by renormalizing the Landau expansion for the free energy with Gaussian spin fluctuations of a given r.m.s. amplitude (see Refs.  and references therein). The latter can be obtained empirically, or estimated from the parameters of the band structure with an ansatz to separate spin fluctuations included in the LDA from those neglected, as discussed in Ref. . Here we report renormalized Landau functional calculations where one parameter, the r.m.s. amplitude of the beyond LDA fluctuations at $`P=0`$ is taken as an adjustable parameter, determined by comparison with the experimental $`P=0`$ magnetization, and use it to describe, without further empirical parameters, the pressure and field dependence of the magnetic properties of ZrZn2.

The LDA calculations were done using the general potential linearized augmented planewave (LAPW) method. Local orbital extensions were included to accurately treat high lying core states and avoid linearization errors.  The Hedin-Lundqvist exchange correlation function was used with von-Barth-Hedin spin scaling.  The valence and Zr semicore $`p`$ states were treated in a scalar relativistic approximation, while the core states were treated fully relativistically. LAPW sphere radii $`R`$=2.1 a0 were employed with a dimensionless basis set cutoff $`RK_{max}`$=9. Brillouin zone samplings were done using the special k-points method, with 182 points in the irreducible $`1/48`$ wedge of the zone. Convergence tests were done, showing that these parameters were adequate. For example, fixed spin moment calculations at the experimental lattice parameter were done using up to 1300 points in the wedge, with very slight changes of less than 0.01 $`\mu _B`$ in the magnetization. Calculations at the experimental lattice parameter were also done with a different sphere radius, $`R`$=2.45 a0, again with negligible changes in magnetization.

In order to construct the Landau expansion, we did fixed spin moment calculations, determining the total energy as a function of magnetic moment an volume, using seven lattice parameters from 13.0 $`a_0`$ to 13.9 $`a_0`$ plus the experimental lattice parameter of 13.9358 $`a_0`$.  The variation of the energy with volume yields a bulk modulus, $`B`$=1.0 Mbar, which we use to set the pressure scale,  since there is no experimental value in the literature to our knowledge. Using this value, the QCP at $`P=1820`$ corresponds to a volume compression of 1.7-1.9%.

We now turn to the magnetic properties in the LDA. As shown in Fig.1, the magnetization drops slowly from 0.72 $`\mu _B`$ at zero pressure ($`V`$=338 a$`{}_{}{}^{3}{}_{0}{}^{}`$) to 0.68 $`\mu _B`$ at $`V`$= 299 a$`{}_{}{}^{3}{}_{0}{}^{}`$, $`P=161`$ kbar (all volumes and magnetizations are given per formula unit). At this pressure the ground state becomes nonmagnetic and the moment suddenly collapses to zero. The ferromagnetic state remains metastable until $`V`$=290 a$`{}_{}{}^{3}{}_{0}{}^{}`$, $`P=`$212 kbar. Thus, the LDA predicts not a QCP, but a first order transition at a pressure of $`P`$ 161 kbar. Leaving aside the question of the order of the transition, the LDA strongly overestimates the magnetization, and has a much higher transition pressure than experiment, implying an overestimate of $`T_C`$ as well. Additionally, the LDA yields very weak $`P`$ dependence of the moment up to the transition pressure, while experiment finds moments that decrease considerably with $`P`$ until at least $`P16`$ kbar.

To proceed, we use the fluctuation-renormalized Landau theory. A large literature exists on this subject, for instance, the review of Ref. . The basis of this theory is that the main omission in LDA calculations is from long-range ferromagnetic spin fluctuations, which are important near a QCP. One writes the Landau expansion of the LDA total energy as

$$E_{LDA}(M)=a_0+\underset{n1}{}\frac{1}{2n}a_{2n}M^{2n},$$
(1)
and then introduces additional Gaussian zero-point fluctuations of an r.m.s. magnitude $`\xi `$ for each of the $`d`$ components of the magnetic moment (for a 3D material $`d=3`$). After averaging over these, one obtains a fluctuation-corrected functional. The general expression  reads

$`E_{renormalized}(M)=a_0+`$ $`{\displaystyle \underset{n1}{}}`$ $`{\displaystyle \frac{1}{2n}}\stackrel{~}{a}_{2n}M^{2n},`$ (2)
$`\stackrel{~}{a}_{2n}={\displaystyle \underset{i0}{}}C_{n+i1}^{n1}a_{2(n+i)}\xi ^{2i}`$ $`\mathrm{\Pi }_{k=n}^{n+i1}`$ $`(1+{\displaystyle \frac{2k}{d}}).`$ (3)
Two approaches are, in principle, possible at this point: one is to evaluate $`\xi `$ using the fluctuation-dissipation theorem,

$$\xi ^2=\frac{4\mathrm{}}{\mathrm{\Omega }}d^3q\frac{d\omega }{2\pi }\frac{1}{2}Im\chi (𝐪,\omega ),$$
(4)
however, this requires some knowledge of the susceptibility $`\chi (𝐪,\omega )`$, and a choice for the cutoff in the integration. This choice gives the separation between the fluctuations accounted for in LDA from those missing. In the most pessimistic view it converts one unknown parameter, $`\xi `$, into another, though it should be said that the cutoff may be much less material and pressure dependent than $`\xi `$ itself. The other approach is to treat $`\xi `$ as an adjustable parameter. Here we are interested in the magnetic phase diagram of ZrZn2 in a pressure range corresponding to that where magnetism is observed experimentally, so it is possible to adjust $`\xi `$ to reproduce the magnetic moment at ambient pressure and then use it for the whole pressure range. The fluctuation-dissipation theorem, though not used directly, is used implicitly to construct an ansatz for the $`P`$ dependence of $`\xi ^2`$: the lowest-order expansion of the bare susceptibility $`\chi _0(𝐪,\omega )`$,

$$\chi _0(𝐪,\omega )=N(E_F)aq^2+ib\omega /q$$
(5)
gives rise, near a QCP, to the formula (see, e.g., Refs. ),

$`\xi ^2={\displaystyle \frac{bv_F^2N(E_F)^2}{8a^2\mathrm{\Omega }}}[Q^4\mathrm{ln}(1+Q^4)+\mathrm{ln}(1+Q^4)]`$

where $`Q=q_c\sqrt{a/bv_F},`$ $`q_c`$ is a cutoff in the momentum space, $`\mathrm{\Omega }`$ is the Brillouin zone volume, and $`v_F`$ and $`N(E_F)`$ are the Fermi velocity and the density of states, respectively. The expression in the square brackets depends on its argument logarithmically, so the main volume dependence comes from the prefactor. Following the arguments of Ref. , this prefactor scales with $`V`$ as $`V^1`$ in the effective mass approximation. Thus, in the first approximation we write $`\xi ^2(V)=\xi ^2(V_0)V_0/V`$.

In order to ensure stable fits, we have chosen the minimal power in the expansion 1, $`n=6`$. Fig.2 shows the quality of the fits, which is quite good. The value of $`\xi (V_0)`$ that yields the experimental value of the magnetic magnetization, $`M=0.17`$ $`\mu _B`$, is then found to be $`\xi (V_0)=0.5`$ $`\mu _B`$. Although the resulting dependence of $`\xi `$ on $`V`$ is relatively weak, its effect on the phase diagram is large: In Fig. 3 we show the (zero-temperature) equilibrium magnetization in zero field, as a function of volume. One can see that neglecting the volume dependence of $`\xi `$ leads to a QCP at $`P_c29`$ kbar, while using the above scaling, one gets nearly exact value $`P_c15`$ kbar. We should recall, however, that this is the idealized phase diagram in zero field, while actual measurements are performed in a small, but finite field. Near a QCP even a small field can change magnetization drastically, as Fig.4 illustrates. It is interesting to note that the metamagnetism present in the bare LDA calculations disappears when the renormalization is included account and as a result a QCP appears. In reality, it may be that symmetry breakings other than uniform ferromagnetism occur near the QCP and change the transition to first order. It would be very interesting to experimentally investigate whether this in fact is the case, and if so how close to the transition it occurs and what the relevant order parameter is.

In summary, we report LDA calculations of the magnetic energy of ZrZn2 under pressure. Our results demonstrate that the LDA substantially overestimates the tendency to magnetism in the whole experimentally studied pressure range. This is an indication of strong quantum spin fluctuations, associated with the QCP. Using fluctuation-renormalized Landau theory, we find that spin fluctuations with an r.m.s. amplitude of 0.5 $`\mu _B`$ are needed at $`P`$=0 to obtain agreement with the experimental magnetization. We further find that using a simple scaling based on the fluctuation-dissipation theorem we are able to describe the phase diagram up to the critical pressure with a good accuracy.

We are grateful for helpful discussions with G.G. Lonzarich, C. Pfleiderer and S.S. Saxena. We thank C. Pfleiderer for discussion of experimental data prior to publication. Work at the Naval Research Laboratory is supported by the Office of Naval Research. The DoD-AE code and computing time from the DoD ASC and ARL centers were used for some of the calculations.


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# On a small cancellation theorem of Gromov

## 1 Statement and discussion

Let $`S`$ be a finite set which is the disjoint union of two sets $`S^{}`$ and $`S^{\prime \prime }`$, with a bijection from $`S^{}`$ to $`S^{\prime \prime }`$ called *being inverse*. The elements of $`S`$ are called *letters*.

A *word* is a finite sequence of letters. The inverse of a word is the word made of the inverse letters put in reverse order.

A word is called *reduced* if it does not contain a letter immediately followed by its inverse.

A *labelled complex* is a finite unoriented $`2`$-complex in which each oriented edge bears a letter, such that opposite edges bear inverse letters. (Each unoriented edge is considered as a couple of two oriented edges.) Thus each face defines a word (up to inversion and cyclic permutation) read on its boundary. We require a map of labelled complexes to preserve labels (but it may change orientation of faces, sending a face to a face with inverse boundary label — this amounts to considering maps between the corresponding oriented complexes).

A *labelled graph* is a $`1`$-dimensional labelled complex.

A labelled complex is said to be *reduced* if there is no pair of oriented edges arising from the same vertex and bearing the same letter.

Note that a word can be seen as a (linear) labelled graph, which we will implicitly do from now on. The word is reduced if and only if the labelled graph is.

A *doublet* of a labelled complex is a word which has two different immersions in the labelled complex. (An immersion is a locally injective map of labelled complexes. Two immersions are considered different if they are different as maps of $`2`$-complexes.) This is analogue to the traditionnal “piece” of small cancellation theory.

A *standard family of cycles* for a graph is a set of paths in the graph, generating the fundamental group, such that there exists a maximal subtree of the graph such that, when the subtree is contracted to a point (so that the graph becomes a bouquet of circles), the set of generating cycles is exactly the set of these circles. There always exists some.

We are now in a position to state the theorem.

Theorem 1 (M. Gromov) –  Let $`\mathrm{\Gamma }`$ be a reduced labelled graph. Let $`R`$ be the set of words read on all cycles of $`\mathrm{\Gamma }`$ (or on a generating family of cycles). Let $`g`$ be the girth of $`\mathrm{\Gamma }`$ and $`\mathrm{\Lambda }`$ be the length of the longest doublet of $`\mathrm{\Gamma }`$.

If $`\mathrm{\Lambda }<g/6`$ then the presentation $`SR`$ defines a group $`G`$ enjoying the following properties.

1. It is hyperbolic, torsion-free.
2. If the rank of the fundamental group of $`\mathrm{\Gamma }`$ is greater than the number of generators, $`G`$ is infinite and not quasi-isometric to $``$.
3. Any presentation of $`G`$ by the words read on a standard family of cycles of $`\mathrm{\Gamma }`$ is aspherical (hence the cohomological dimension of $`G`$ is at most $`2`$).
4. The shortest relation in $`G`$ is of length $`g`$.
5. For any reduced word $`w`$ equal to $`e`$ in $`G`$, some cyclic permutation of $`w`$ contains a subword of a word read on a cycle of $`\mathrm{\Gamma }`$, of length at least $`(13\mathrm{\Lambda }/g)>\frac{1}{2}`$ times the length of this cycle.
6. The natural map from the labelled graph $`\mathrm{\Gamma }`$ into the Cayley graph of $`G`$ is an isometric embedding.

If $`\mathrm{\Gamma }`$ is a disjoint union of circles, this theorem almost reduces to ordinary $`1/6`$ small cancellation theory. The “almost” accounts for the fact that the length of a shared doublet between two relators is supposed to be less than $`1/6`$ the length of the smallest of the two relators in ordinary small cancellation theory, and less than $`1/6`$ the length of the smallest of all relators in our case. But it is clear from the proof below that the assumption in the theorem can be replaced by the following slightly weaker one: for each doublet, its length is less than $`1/6`$ the minimal length of the cycles of the graph on which the doublet appears. With this assumption, the theorem reduces to ordinary small cancellation when the graph is a disjoint union of circles.

The group obtained is not always non-elementary: for example, if there are three generators $`a,b,c`$ and the graph consists in two points joined by three edges bearing $`a`$, $`b`$ and $`c`$ respectively, one obtains the presentation $`a,b,ca=b=c`$ which defines $``$. However, since the cohomological dimension is at most $`2`$, it is easy to check (computing the Euler characteristic) that if the rank of the fundamental group of $`\mathrm{\Gamma }`$ is greater than the number of generators, then $`G`$ is non-elementary.

This theorem is not stated explicitly in \[Gro2\] in the form we give but using a much more abstract formalism of “rotation families of groups”. In the vocabulary thereof, the case presented here is when this rotation family contains only one subgroup of the free group (and its conjugates), namely the one generated by the words read on cycles of the graph with some base point; the corresponding “invariant line” $`U`$ is the universal cover of the labelled graph $`\mathrm{\Gamma }`$ (viewed embedded in the Cayley graph of the free group). Reducedness of the labelling ensures quasi-convexity.

In \[Gro2\], this theorem is applied to a random labelling (or rather a variant of this theorem given below, in which reducedness is replaced with quasi-geodesicity). It is not difficult, using for example the techniques described in \[Oll\], to check that a random labelling satifies the small cancellation and quasi-geodesicity assumptions.

## 2 Proof

We now give some more definitions which are useful for the proof.

A *tile* is a planar labelled complex with only one face and no other edge than the boundary edges of this face (but not necessarily simply connected). By our definition of maps between labelled complexes, a tile is considered equal to the tile bearing the inverse word.

Convention: A tile may bear a word which is not simple (i.e. is a power of a smaller word). In this case the tile has a non-trivial automorphism. Say that on each boundary component of a tile we mark a starting point and that a map between tiles has to preserve marked points. This is useful for the study of torsion because with this convention asphericity of a presentation implies torsion-freeness and asphericity of the Cayley complex. Note that our definition of asphericity is thus slightly stronger than the one in \[LS\].

The *length* of a tile is the length of its boundary.

A *tile of a labelled complex* is any of its faces.

A *doublet* with respect to a set of tiles is a word which has immersions in the boundary two different tiles, or two distinct immersions in the boundary of one tile.

A *puzzle* with respect to a set of tiles is a planar labelled complex all tiles of which belong to this set of tiles (the same tile may appear several times in a puzzle).

A puzzle is said to be *minimal* if it has the minimal number of tiles for a given boundary word.

A puzzle is said to be *van Kampen-reduced* if there is no pair of adjacent faces such that the words read on the boundary of these two faces are inverse and the position (with respect to the marked point) of the letter read at a common edge of these faces is the same in the two copies of the boundary word of these faces (in other words, there is no trivial gluing). This corresponds to reduced van Kampen diagrams (see \[LS\]). (Incidentally, a reduced puzzle is van Kampen-reduced, though the converse is not necessarily true.)

Proof of the theorem – Let $`\mathrm{\Gamma }`$ be a reduced labelled graph. $`\mathrm{\Gamma }`$ defines a presentation $`R`$ by taking all the words read along its cycles. The group presented by $`SR`$ will be the same if we take not all cycles but only a generating set of cycles.

Note that the assumption on doublets implies that no two distinct cycles of $`\mathrm{\Gamma }`$ bear the same word. We will implicitly use this fact below for unicity of lifts to $`\mathrm{\Gamma }`$.

The fundamental group of the graph $`\mathrm{\Gamma }`$ is a free group. Let $`𝒞`$ be a finite generating set of $`\pi _1(\mathrm{\Gamma })`$ (maybe not standard). Let $`R`$ be the set of words read on the cycles in $`𝒞`$.

Add $`2`$-faces to $`\mathrm{\Gamma }`$ in the following way: for each cycle in $`𝒞`$, glue a disk bordering this cycle.

Note $`\mathrm{\Gamma }`$ again this $`2`$-complex. As the cycles in $`𝒞`$ generate all cycles, $`\mathrm{\Gamma }`$ is simply connected. If $`𝒞`$ is taken standard, $`\mathrm{\Gamma }`$ has no homotopy in degree $`2`$.

Let $`D`$ be a simply connected puzzle with respect to the tiles of $`\mathrm{\Gamma }`$. We are going to show that there exists a constant $`C>0`$ such that for any $`D`$, if $`D`$ is van Kampen-reduced, then $`D`$ satisfies a linear isoperimetric inequality $`\left|D\right|C\left|D\right|`$ where $`\left|D\right|`$ is the boundary length of $`D`$ and $`\left|D\right|`$ is the number of faces of $`D`$. This implies hyperbolicity (see for example \[Sh\]).

We can safely assume that all edges of $`D`$ lie on some face (there are no “filaments”). Indeed, filaments only improve isoperimetry. Generally speaking, in what follows we will never mention the possible occurrence of filaments, their treatment being immediate. In particular, we suppose that all vertices of $`\mathrm{\Gamma }`$ are adjacent to at least two edges (or, equivalently, that any edge is adjacent to some face).

Let $`e`$ be an internal edge of $`D`$, between faces $`f_1`$ and $`f_2`$. As $`D`$ is a puzzle over the tiles of $`\mathrm{\Gamma }`$, there are faces $`f_1^{}`$ and $`f_2^{}`$ of $`\mathrm{\Gamma }`$ bearing the same boundary word as $`f_1`$ and $`f_2`$ respectively (maybe up to inversion). (Note that these faces are unique, since no two faces of $`\mathrm{\Gamma }`$ can bear the same word as it would contradict the $`1/6`$ condition on doublets.)

The edge $`e`$ belongs to $`f_1`$ and $`f_2`$ and thus can be lifted in $`\mathrm{\Gamma }`$ either in $`f_1^{}`$ or in $`f_2^{}`$. Say $`e`$ is an *edge originating from $`\mathrm{\Gamma }`$* if these two lifts coincide, so that in $`\mathrm{\Gamma }`$, the two faces at play are adjacent along the same edge as they are in $`D`$.

Any labelled complex with respect to the tiles of $`\mathrm{\Gamma }`$, all edges of which originate from $`\mathrm{\Gamma }`$, can thus be lifted to $`\mathrm{\Gamma }`$ by lifting each of its edges.

Note that $`D`$ is van Kampen-reduced if and only if there is no edge $`e`$ originating from $`\mathrm{\Gamma }`$ and adjacent to faces $`f_1`$, $`f_2`$ such that $`f_1^{}=f_2^{}`$.

We work by first proving the isoperimetric inequality for puzzles having all edges originating from $`\mathrm{\Gamma }`$. Second, we will decompose the graph $`D`$ into parts having all their edges originating from $`\mathrm{\Gamma }`$ and show that these parts are in $`1/6`$ small cancellation with each other. Then we will use ordinary small cancellation theory to conclude.

We begin by proving what we want for some particular choice of $`R`$.

Lemma 2 –  Let $`\mathrm{\Delta }=\mathrm{diam}(\mathrm{\Gamma })`$. Suppose that $`R`$ was chosen to be the set of words read on closed paths embedded in $`\mathrm{\Gamma }`$ of length at most $`3\mathrm{\Delta }`$. Then, for any closed path in $`\mathrm{\Gamma }`$ labelling a reduced word $`w`$, there exists a simply connected puzzle with boundary word $`w`$, with tiles having their boundary words in $`R`$, all edges of which originate from $`\mathrm{\Gamma }`$, and with at most $`3\left|w\right|/g`$ tiles.

Proof of Lemma 2 – If $`w2\mathrm{\Delta }`$ then by definition of $`R`$ there exists a one-tile puzzle spanning $`w`$, and as $`\left|w\right|g`$ the conclusion holds. Show by induction on $`n`$ that if $`\left|w\right|n\mathrm{\Delta }`$ there exists a puzzle $`D`$ spanning $`w`$ with at most $`n`$ pieces. This is true for $`n=2`$. Suppose this is true up to $`n\mathrm{\Delta }`$ and suppose that $`2\mathrm{\Delta }\left|w\right|(n+1)\mathrm{\Delta }`$.

Let $`w=w^{}w^{\prime \prime }`$ where $`\left|w^{}\right|=2\mathrm{\Delta }`$. As the diameter of $`\mathrm{\Gamma }`$ is $`\mathrm{\Delta }`$, there exists a path in $`\mathrm{\Gamma }`$ labelling a word $`x`$ joining the endpoints of $`w^{}`$, with $`\left|x\right|\mathrm{\Delta }`$. So $`w^{}x^1`$ is read on a cycle of $`\mathrm{\Gamma }`$ of length at most $`3\mathrm{\Delta }`$, hence (its reduction) belongs to $`R`$. Now $`xw^{\prime \prime }`$ is a word read on a cycle of $`\mathrm{\Gamma }`$, of length at most $`\left|w\right|\mathrm{\Delta }n\mathrm{\Delta }`$. So there is a puzzle with at most $`n`$ tiles spanning $`xw^{\prime \prime }`$. Gluing this puzzle with the tile spanning $`w^{}x^1`$ along the $`x`$-sides provides the desired puzzle. (Note that this gluing occurs in $`\mathrm{\Gamma }`$, so that edges of the resulting puzzle originate from $`\mathrm{\Gamma }`$.)

So for any $`w`$ we can find a puzzle spanning it with at most $`1+\left|w\right|/\mathrm{\Delta }`$ tiles. As $`\mathrm{\Delta }g/2`$ and as $`\left|w\right|g`$, we have $`1+\left|w\right|/\mathrm{\Delta }1+2\left|w\right|/g3\left|w\right|/g`$. $`\mathrm{}`$

Corollary 3 –  For any choice of $`R`$, there exists a constant $`\alpha `$ such that any minimal simply connected puzzle $`D`$ with respect to the tiles of $`\mathrm{\Gamma }`$ all internal edges of which originate from $`\mathrm{\Gamma }`$ satisfies the isoperimetric inequality $`\left|D\right|\alpha \left|D\right|`$.

Proof of Corollary 2 – Indeed, the existence of an isoperimetric constant does not depend on the presentation. $`\mathrm{}`$

The second lemma is just ordinary small cancellation theory (see for example the appendix of \[GH\], or \[LS\]), stated in the form we need. We include a short proof here for completeness.

Lemma 4 –  Let $`R`$ be a set of simply connected reduced tiles. Suppose that any doublet with respect to two tiles $`t,t^{}R`$ is a word of length at most $`\lambda `$ times the smallest boundary length of $`t`$ and $`t^{}`$, for some constant $`\lambda <1/6`$.

Then any simply connected van Kampen-reduced puzzle $`D`$ with respect to the tiles of $`R`$ satisfies the following properties.

1. The reduction $`w`$ of the boundary word of $`D`$ contains a subword of some tile $`t`$ with length at least $`(13\lambda )>\frac{1}{2}`$ times the boundary length of $`t`$.
2. The word $`w`$ is not a proper subword of the boundary word of some tile.
3. The boundary length $`\left|D\right|`$ is at least $`16\lambda `$ times the sum of the lengths of the faces of $`D`$, and at least the boundary length of the largest tile it contains.

The value $`1/6`$ is optimal, as a hexagonal tiling shows.

Proof – Let $`D`$ be a van Kampen-reduced puzzle w.r.t. $`R`$. We can suppose that its boundary word is reduced (isoperimetry for the reduction implies isoperimetry for $`D`$ a fortiori). It is a planar graph. Define a metric graph $`D^{}`$ as follows: start with $`D`$, but for each pair of adjacent faces, replace all consecutive edges between these two faces by a single edge. Define the length of this new edge as the number of edges it replaces. So $`D^{}`$ is a metric planar graph having the same faces as $`D`$ but in which every vertex is of degree at least $`3`$. The small cancellation assumption states that the length of any edge in $`D^{}`$ is at most $`\lambda `$ times the smallest boundary length of the two adjacent faces.

Let $`V`$, $`E`$ and $`F`$ denote the number of vertices, edges and faces of $`D^{}`$, respectively. Let $`E_i`$ and $`E_e`$ denote the number of internal and external edges, and $`F_i`$, $`F_e`$ the number of internal faces and faces adjacent to the boundary. Let $`F_e^1`$ and $`F_e^2`$ denote the number of external faces with exactly one, or at least two, external edges, respectively.

As every vertex has degree at least $`3`$, we have $`E3V/2`$. By definition we have $`E_eF_e^1+2F_e^2`$. Since $`\lambda <1/6`$, any internal face has at least $`6`$ edges.

We now prove that there are at least two external faces with exactly one external edge and at most three internal edges (this will prove the first assertion of the lemma). Let $`F_e^{}`$ and $`F_e^{\prime \prime }`$ be the number of external faces with exactly one external edge and, respectively, at most three or at least four internal edges. Since any internal face has at least six internal edges, and since any external face with two external edges has at least two internal edges, we get $`E_i\frac{1}{2}\left(F_e^{}+4F_e^{\prime \prime }+2F_e^2+6F_i\right)`$.

The Euler formula writes

$`1`$ $`=`$ $`VE+F=V{\displaystyle \frac{2}{3}}E{\displaystyle \frac{1}{3}}E+F`$
$``$ $`0{\displaystyle \frac{1}{3}}E_i{\displaystyle \frac{1}{3}}E_e+F_e+F_i`$
$``$ $`{\displaystyle \frac{1}{6}}\left(F_e^{}+4F_e^{\prime \prime }+2F_e^2+6F_i\right){\displaystyle \frac{1}{3}}\left(F_e^{}+F_e^{\prime \prime }+2F_e^2\right)+F_e^{}+F_e^{\prime \prime }+F_e^2+F_i`$
$`=`$ $`{\displaystyle \frac{1}{2}}F_e^{}`$
Hence there exist at least two faces with exactly one external edge and at most three internal ones.

By the small cancellation assumption, the internal edges of such a face have cumulated length at most $`3\lambda `$ times the length of this face. This proves the first assertion of the lemma.

The second assertion is easy. Suppose that the boundary word of some puzzle is a proper subword $`w`$ of the boundary word $`x`$ of some tile $`t`$. We know that $`w`$ contains a subword which contains a proportion at least $`(13\lambda )>1/2`$ of the boundary word of some tile $`t^{}`$. If $`\left|w\right|\left|x\right|/2`$ we have $`t^{}t`$, so $`t`$ and $`t^{}`$ share a common subword of length more than one half the boundary length of $`t^{}`$, which contradicts the small cancellation assumption. If $`\left|w\right|>\left|x\right|/2`$, then define a new puzzle by gluing the inverse tile $`t^1`$ to the original puzzle (and reducing the resulting puzzle): the new puzzles now contains the reduction of the word $`wx^1`$, which is at least one half of the boundary word of $`t^1`$; use the same argument.

Isoperimetry follows immediately. Let $`F`$ be a external face of $`D^{}`$ with at most three internal edges. Let $`\mathrm{}`$ be the length of $`F`$. Let $`D^{\prime \prime }`$ be the (maybe non connected) graph obtained from $`D^{}`$ by removing $`F`$. We have $`\left|D^{}\right|=\left|D^{\prime \prime }\right|+\mathrm{}2\left|FD^{\prime \prime }\right|\left|D^{\prime \prime }\right|+(16\lambda )\mathrm{}`$ hence the conclusion by backwards induction on the number of faces.

The fact that the boundary length of $`D`$ is at least the boundary length of the largest face is trivial if $`D`$ has only one face, and otherwise follows from the fact that there are two external faces having at least a proportion $`13\lambda >\frac{1}{2}`$ of their length on the boundary. Remove such a face (but not the largest one): this decreases the boundary length. Iterate this process up to a diagram containing only the largest face. $`\mathrm{}`$

Corollary 5 –  Let $`R`$ be a set of (not necessarily simply connected) reduced tiles. Suppose that any doublet with respect to two tiles $`t,t^{}R`$ is a word of length at most $`\lambda `$ times the smallest length of the boundary component of $`t`$ and $`t^{}`$ it immerses in, for some constant $`\lambda <1/6`$.

Then, any simply connected puzzle with respect to this set of tiles contains only simply connected tiles.

Proof of the corollary – Let $`D`$ be a simply connected puzzle with respect to $`R`$. Let $`t`$ be a non-simply connected tile in $`D`$. Consider the subdiagram $`D^{}`$ of $`D`$ filling one of the holes of $`t`$. We can suppose that $`D^{}`$ contains only simply connected tiles (otherwise, take again a non-simply connected tile in $`D^{}`$ and a diagram filling one of its holes, and repeat this operation as many times as necessary).

By the previous lemma, the boundary word $`w`$ of $`D^{}`$ contains a subword $`w^{}`$ of the boundary word $`w_t^{}`$ of some tile $`t^{}`$ of $`D^{}`$, with $`\left|w^{}\right|\left|w_t^{}\right|/2`$. But as all tiles are reduced, the boundary word of $`D^{}`$ is the word read on the boundary component of $`t`$ spanning $`D^{}`$. So $`t^{}`$ and $`t`$ have in common a word of length at least one half the boundary length of $`t^{}`$, which contradicts the assumption. $`\mathrm{}`$

Back to our simply connected puzzle $`D`$ with tiles in $`\mathrm{\Gamma }`$. A puzzle is built by taking the disjoint union of all its tiles and gluing them along the internal edges.

First, define a (maybe not connected) puzzle $`D^{}`$ by taking the disjoint union of all tiles of $`D`$ and gluing them along the internal edges of $`D`$ originating from $`\mathrm{\Gamma }`$. All internal edges of $`D^{}`$ originate from $`\mathrm{\Gamma }`$.

As $`D`$ is van Kampen-reduced, $`D^{}`$ is as well.

Let $`D_i`$, $`i=1,\mathrm{},n`$ be the connected components of $`D^{}`$. They form a partition of $`D`$. The puzzle $`D`$ is obtained by gluing these components along the internal edges of $`D`$ not originating from $`\mathrm{\Gamma }`$.

It may be the case that the boundary word of some $`D_i`$ is not reduced. This means that there is a vertex on the boundary of $`D_i`$ which is the origin of two (oriented) edges bearing the same vertex. We will modify $`D`$ in order to avoid this. Suppose some $`D_i`$ has non-reduced boundary and consider two edges $`e_1,e_2`$ of $`D`$ responsible for this: $`e_1`$ and $`e_2`$ are two consecutive edges with inverse labels. These edges are either boundary edges of $`D`$ or internal edges. In the latter case this means that $`D_i`$ is to be glued to some $`D_j`$. We treat only this latter case as the other one is even simpler.

Make the following transformation of $`D`$: do not glue any more edge $`e_1`$ of $`D_i`$ with edge $`e_1`$ of $`D_j`$, neither edge $`e_2`$ of $`D_i`$ with edge $`e_2`$ of $`D_j`$, but rather glue edges $`e_1`$ and $`e_2`$ of $`D_i`$, as well as edges $`e_1`$ and $`e_2`$ of $`D_j`$, as in the following picture. This is possible since by definition $`e_1`$ and $`e_2`$ bear inverse labels.

This kind of operation has been studied and termed *diamond move* in \[CH\].

Since $`\mathrm{\Gamma }`$ is reduced, the lifts to $`\mathrm{\Gamma }`$ of the edges $`e_1`$ and $`e_2`$ of $`D_i`$ are the same edge of $`\mathrm{\Gamma }`$. This shows that the transformation above preserves the fact that all edges of $`D_i`$ and of $`D_j`$ originate from $`\mathrm{\Gamma }`$.

The resulting diagram (denoted $`D`$ again) has the same number of faces as before, and no more boundary edges. Thus, proving isoperimetry for the modified diagram will imply isoperimetry for the original one as well. So we can safely assume that the boundary words of the $`D_i`$’s are reduced.

Now consider $`D`$ as a puzzle with the $`D_i`$’s as tiles. Note that these tiles are not necessarily simply connected.

These tiles satisfy the condition of Corollary 2. Indeed, suppose that the two tiles $`D_i`$, $`D_j`$ are to be glued along a common (reduced!) word $`w`$. By definition of the $`D_i`$’s, the edges making up $`w`$ do not originate from $`\mathrm{\Gamma }`$.

As the edges of $`D_i`$ originate from $`\mathrm{\Gamma }`$, there is a lift $`\phi _i:D_i\mathrm{\Gamma }`$ (as noted above). Consider the two lifts $`\phi _i(w)`$ and $`\phi _j(w)`$. As the edges making up $`w`$ do not originate from $`\mathrm{\Gamma }`$, these two lifts are different. As $`w`$ is reduced these lifts are immersions. So $`w`$ is a doublet. By assumption the length of $`w`$ is at most $`\mathrm{\Lambda }<g/6`$.

Now as $`D_i`$ lifts to $`\mathrm{\Gamma }`$, any boundary component of $`D_i`$ goes to a closed path in the $`1`$-skeleton of $`\mathrm{\Gamma }`$. This proves that the length of any boundary component of $`D_i`$ is at least $`g`$.

So the tiles $`D_i`$ satisfy the small cancellation condition with $`\lambda =\mathrm{\Lambda }/g<1/6`$. As they are tiles of a simply connected puzzle, by Corollary 2 they are simply connected.

Then by Lemma 2, the boundary of $`D`$ is at least $`16\lambda `$ times the sum of the boundary lengths of the $`D_i`$’s. Since $`D`$ is minimal, each $`D_i`$ is as well, and as $`D_i`$ is simply connected, by Corollary 2 it satisfies the isoperimetric inequality $`\left|D_i\right|\alpha \left|D_i\right|`$. So

$$\left|D\right|(16\lambda )\left|D_i\right|\alpha (16\lambda )\left|D_i\right|=\alpha (16\lambda )\left|D\right|$$

which shows the isoperimetric inequality for $`D`$, hence hyperbolicity.

For asphericity and the cohomological dimension (hence torsion-freeness), suppose that $`R`$ is standard (so that $`\mathrm{\Gamma }`$ is aspherical) and that there exists a van Kampen-reduced spherical diagram $`D`$. Define the $`D_i`$’s as above. As we shown above that the boundary length of $`D`$ (which is $`0`$) is at least the boundary length of any $`D_i`$, this means that the boundary length of all the $`D_i`$’s is $`0`$. Hence each $`D_i`$ is a spherical diagram itself. But by definition $`D_i`$ lifts to $`\mathrm{\Gamma }`$. We conclude with the following lemma.

Lemma 6 – Suppose that the set of paths read along faces of $`\mathrm{\Gamma }`$ is standard. Let $`D`$ be a non-empty spherical puzzle all edges of which come from $`\mathrm{\Gamma }`$. Then $`D`$ is not reduced.

Proof of the lemma – Let $`T`$ be a maximal tree of the $`1`$-skeleton of $`\mathrm{\Gamma }`$ witnessing for standardness of the family of cycles. Homotope $`T`$ to a point. This turns $`\mathrm{\Gamma }`$ into a bouquet of circles with a face in each circle. Similarly, homotope to a point any edge of $`D`$ coming from a suppressed edge of $`\mathrm{\Gamma }`$. This way we turn $`D`$ into a spherical van Kampen diagram with respect to the presentation of the fundamental group of $`\mathrm{\Gamma }`$ (i.e. the trivial group) by $`c_1,\mathrm{},c_nc_1=e,\mathrm{},c_n=e`$. But there is no reduced spherical van Kampen diagram with respect to this presentation, as can immediately be checked. $`\mathrm{}`$

The last affirmations of the theorem follow easily from the last affirmations of Lemma 2. The smallest relation in the group presented by $`SR`$ is the boundary length of the smallest puzzle, which by Lemma 2 is at least the smallest boundary length of the $`D_i`$’s, which is at least $`g`$. Similarly, any reduced word representing the trivial element in the group is the boundary of a reduced diagram, thus contains as a subword at least one half of the boundary word of some $`D_i`$.

For the isoperimetric embedding of $`\mathrm{\Gamma }`$ in the Cayley graph of the group, suppose that some geodesic path in the graph labelling a word $`x`$ is equal to a shorter word $`y`$ in the quotient. This means that there exists a puzzle with boundary word $`xy^1`$, made up of tiles with cycles of $`\mathrm{\Gamma }`$ as boundary words. Now (if $`\mathrm{\Gamma }`$ contains no filaments) $`x`$ is part of some cycle labelled by $`w=xz`$ of the graph. Since the path $`x`$ is of minimal length, we have $`\left|x\right|\left|z\right|`$. So $`\left|xy^1\right|<\left|w\right|`$ and in particular, the puzzle bordering $`xy^1`$ cannot contain a tile with boundary word $`w`$. Glue a tile with boundary word $`(xz)^1`$ to the puzzle $`xy^1`$ along the subwords $`x`$ and $`x^1`$. This results in a (reduced) puzzle bordering $`z^1y^1`$, containing a tile $`z^1x^1`$. This is impossible as by assumption $`\left|y\right|<\left|x\right|`$.

Non-elementariness in case the rank of the fundamental group of $`\mathrm{\Gamma }`$ is large enough follows immediately from a computation of the Euler characteristic, using that the cohomological dimension is at most $`2`$.

This proves the theorem. $`\mathrm{}`$

## 3 Further remarks

Remark 7 – The proof above gives an explicit isoperimetric constant when the set of relators taken is the set of all words read on cycles of the graph of length at most three times the diameter: in this case, any minimal simply connected puzzle satisfies the isoperimetric inequality

$$\left|D\right|g(16\mathrm{\Lambda }/g)\left|D\right|/3$$

This explicit isoperimetric constant growing linearly with $`g`$ (i.e. “homogeneous”) can be very useful if one wants to apply such theorems as the local-global hyperbolic principle, which requires the isoperimetric constant to grow linearly with the sizes of the relators.

Remark 8 – The assumption that $`\mathrm{\Gamma }`$ is reduced can be relaxed a little bit, provided that some quasi-geodesicity assumption is granted, and that the definition of a doublet is emended.

Redefine a *doublet* to be a couple of words $`(w_1,w_2)`$ such that both immerse in $`\mathrm{\Gamma }`$ and such that $`w_1=w_2`$ in the free group. The *length* of a doublet $`(w_1,w_2)`$ is the maximal length of $`w_1`$ and $`w_2`$.

There are trivial doublets, for example if $`w_1=w_2`$ and both have the same immersion. However, forbidding this is not enough: for example, if a word of the form $`aa^1w`$ immerses in the graph, then $`(aa^1w,w)`$ will be a doublet.

A *trivial doublet* is a doublet $`(w_1,w_2)`$ such that there exists a path $`p`$ in $`\mathrm{\Gamma }`$ joining the beginning of the immersion of $`w_1`$ to the beginning of the immersion of $`w_2`$ such that $`p`$ is labelled with a word equal to $`e`$ in the free group.

The new theorem is as follows.

Theorem 9 (M. Gromov) –  Let $`\mathrm{\Gamma }`$ be a labelled graph. Let $`R`$ be the set of words read on all cycles of $`\mathrm{\Gamma }`$ (or on a generating family of cycles). Let $`g`$ be the girth of $`\mathrm{\Gamma }`$ and $`\mathrm{\Lambda }`$ be the length of the longest non-trivial doublet of $`\mathrm{\Gamma }`$.

Suppose that $`\lambda =\mathrm{\Lambda }/g`$ is less than $`1/6`$.

Suppose that there exist a constant $`A>0`$ such that any word $`w`$ immersed in $`\mathrm{\Gamma }`$ of length at least $`L`$ satisfies $`wA(\left|w\right|L)`$ for some $`L<(16\lambda )g/2`$.

Then the presentation $`SR`$ defines a hyperbolic, infinite, torsion-free group $`G`$, and (if $`R`$ is standard) this presentation is aspherical (hence the cohomological dimension of $`G`$ is at most $`2`$). Moreover, the natural map of labelled graphs from $`\mathrm{\Gamma }`$ to the Cayley graph of $`G`$ is a $`(1/A,AL)`$-quasi-isometry. The shortest relation of $`G`$ is of length at least $`Ag/2`$, and any reduced word equal to $`e`$ in $`G`$ contains as a subword the reduction of at least one half of a word read on a cycle of $`\mathrm{\Gamma }`$.

(In the notation of \[GH\], by a $`(\lambda ,c)`$-quasi-isometry we wean a map $`f`$ such that $`d(x,y)/\lambda cd(f(x),f(y))\lambda d(x,y)+c`$.)

Remark 10 – The same theorems hold if we use the $`C(7)`$ condition instead of the $`C^{}(1/6)`$ condition, but in this case there is no control on the radius of injectivity.

Remark 11 – Using the techniques in \[Del\] or \[Oll\], the same kind of theorem holds starting with any torsion-free hyperbolic group instead of the free group, provided that the girth of the graph is large enough w.r.t. the hyperbolicity constant, and that the labelling is quasi-geodesic.

Thanks to Thomas Delzant for having brought the problem to my attention and to Étienne Ghys and Pierre Pansu for helpful discussions and comments on the manuscript.


text:
# Proton-neutron interaction near closed shells

## I Introduction

Odd-odd nuclei around double shell closures provide the best testing ground for the matrix elements of the proton-neutron interaction between valence nucleons. In this context, of special interest are nuclei in the close vicinity to 208Pb, 132Sn and 100Sn, which show strong shell closures for both protons and neutrons. From the experimental point of view, the 208Pb neighbors have been extensively investigated and a large amount of data is available for them. On the other hand, the 132Sn and 100Sn neighbors lie well away from the valley of stability, which makes it very difficult to obtain information on their spectroscopic properties. In recent years, however, substantial progress in the development of spectroscopic techniques has opened the way to the exploration of nuclear structure in the regions of shell closures off stability. This has led to new experimental data for the immediate odd-odd neighbors of both 132Sn and 100Sn. The information presently available for nuclei of this kind, although still rather scanty, is of great value for the understanding of the effective proton-neutron interaction in these two regions as well as for a comparison with the proton-neutron interaction in the 208Pb region.

During the past several years, we have studied a number of nuclei around 208Pb, 132Sn and 100Sn within the framework of the shell model employing realistic effective interactions derived from modern nucleon-nucleon ($`NN`$) potentials. In most of these studies, however, we have been concerned with nuclei having few identical valence particles or holes. A summary of the results obtained through 2000 is given in Ref. cov1 .

More recently cor02a ; cov03a , we have turned our attention to nuclei with unlike valence nucleons to try to gain information on the neutron-proton effective interaction. The main aim of this paper is to report on some selected results of our current work along these lines, which we have obtained starting from the CD-Bonn free $`NN`$ potential machl01 . In particular, we consider the six odd-odd nuclei 208Bi, 210Bi, 132Sb, 134Sb, 98Ag and 102In, and focus attention on the particle-hole and particle-particle multiplets, which offer the opportunity to test directly the matrix elements of our calculated realistic effective interaction.

To place this study in its proper perspective, it should be mentioned that the particle-hole multiplets in the 208Pb region were the subject of great theoretical and experimental interest ersk64 ; alf68 ; kuo68 ; moin69  some thirty-five years ago. In particular, the spectrum of 208Bi was extensively studied through pick-up and stripping reactions and several proton-neutron hole multiplets were identified ersk64 ; alf68 . The pattern exhibited by the observed multiplets was well reproduced by the shell-model calculations of Ref. kuo68 , where particle-hole matrix elements derived from the Hamada-Johnston $`NN`$ potential ham62  were used.

Despite these early achievements in the understanding of the effective proton-neutron interaction around closed shells, little work along the same lines has been done during the last three decades. The new data which are becoming available in the 132Sn and 100Sn regions, as well as the prospect of spectroscopic studies of unstable nuclei opened up by the development of radioactive ion beams, has motivated us to undertake the present study and perform shell-model calculations making use of a modern $`NN`$ potential and improved many-body methods for deriving the effective interaction.

The outline of the paper is as follows. In Sec. II we give a brief description of our calculations. Our results are presented and compared with the experimental data in Sec. III, where we also discuss the effects of the core polarization. In Sec. IV we draw the conclusions of our study.

## II Calculations

In our calculations for the Bi isotopes we assume that 208Pb is a closed core and let the valence proton and neutron hole occupy the six single-particle levels $`0h_{9/2}`$, $`1f_{7/2}`$, $`0i_{13/2}`$, $`1f_{5/2}`$, $`2p_{3/2}`$ and $`2p_{1/2}`$ of the 82-126 shell, while for the valence neutron the model space includes the seven orbits $`1g_{9/2}`$, $`0i_{11/2}`$, $`0j_{15/2}`$, $`2d_{5/2}`$, $`3s_{1/2}`$, $`1g_{7/2}`$, and $`2d_{3/2}`$. Similarly, for the Sb isotopes we assume that the valence proton and neutron hole occupy the five single-particle levels $`0g_{7/2}`$, $`1d_{5/2}`$, $`1d_{3/2}`$, $`2s_{1/2}`$ and $`0h_{11/2}`$ of the 50-82 shell, while the valence neutron outside the 132Sn core occupies the orbits of the 82-126 shell. As regards 98Ag and 102In, we assume that the valence neutrons outside the 100Sn core occupy the orbits of the 50-82 shell, while for the proton holes the model space includes the four orbits $`0g_{9/2}`$, $`1p_{1/2}`$, $`1p_{3/2}`$ and $`0f_{5/2}`$ of the 28-50 shell.

As regards the choice of the single-particle and single-hole energies, we have proceeded as follows. For the Bi isotopes we have taken them from the experimental spectra nndc  of 209Bi, 209Pb and 207Pb. In the same way, for the Sb isotopes we have made use of the experimental spectra of 133Sb sanch99 , 133Sn hoff96  and 131Sn nndc . In the spectra of the two former nuclei, however, some single-particle levels are still missing. More precisely, this is the case of the proton $`2s_{1/2}`$ and neutron $`0i_{13/2}`$ levels, whose energies have been taken from Refs. andr97  and cor02b , respectively, to which we refer for details. As regards the neutron hole energy $`ϵ_{h_{11/2}}`$ in 131Sn, we have adopted the value of 0.100 MeV which has been recently suggested in Ref. gen00 . This is somewhat smaller than that reported in Ref. nndc . For 98Ag and 102In the single-particle and single-hole energies cannot be taken from experiment, since no spectroscopic data are yet available for 101Sn and 99In. Therefore, we have taken them from Ref. andr96  and Ref. cor00 , where they have been determined by an analysis of the low-energy spectra of the Sn isotopes with $`A111`$ and of the N=50 isotones with $`A89`$. For completeness, our adopted values for the single-particle and single-hole energies are reported in Tables I-III.

As already mentioned in the Introduction, in our shell-model calculations we have made use of a realistic effective interaction derived from the CD-Bonn free nucleon-nucleon potential machl01 . This high-quality $`NN`$ potential, which is based upon meson exchange, fits very accurately ($`\chi ^2`$/datum $`1`$) the world $`NN`$ data below 350 MeV available in the year 2000.

The shell-model effective interaction $`V_{\mathrm{eff}}`$ is defined, as usual, in the following way. In principle, one should solve a nuclear many-body Schrödinger equation of the form

$$H\mathrm{\Psi }_i=E_i\mathrm{\Psi }_i,$$
(1)
with $`H=T+V_{NN}`$, where $`T`$ denotes the kinetic energy. This full-space many-body problem is reduced to a smaller model-space problem of the form

$$PH_{\mathrm{eff}}P\mathrm{\Psi }_i=P(H_0+V_{\mathrm{eff}})P\mathrm{\Psi }_i=E_iP\mathrm{\Psi }_i.$$
(2)
Here $`H_0=T+U`$ is the unperturbed Hamiltonian, $`U`$ being an auxiliary potential introduced to define a convenient single-particle basis, and $`P`$ denotes the projection operator onto the chosen model space,

$$P=\underset{i=1}{\overset{d}{}}|\psi _i\psi _i|,$$
(3)
$`d`$ being the dimension of the model space and $`|\psi _i`$ the eigenfunctions of $`H_0`$. The effective interaction $`V_{\mathrm{eff}}`$ operates only within the model space $`P`$. In operator form it can be schematically written kuo80  as

$$V_{\mathrm{eff}}=\widehat{Q}\widehat{Q^{}}\widehat{Q}+\widehat{Q^{}}\widehat{Q}\widehat{Q}\widehat{Q^{}}\widehat{Q}\widehat{Q}\widehat{Q}+\mathrm{},$$
(4)
where $`\widehat{Q}`$, usually referred to as the $`\widehat{Q}`$-box, is a vertex function composed of irreducible linked diagrams, and the integral sign represents a generalized folding operation. $`\widehat{Q^{}}`$ is obtained from $`\widehat{Q}`$ by removing terms of first order in the interaction. Once the $`\widehat{Q}`$-box is calculated, the folded-diagram series of eq. (4) can be summed up to all orders by iteration methods, as, for instance, the Lee-Suzuki one lee80 ; suz80 .

A main difficulty encountered in the derivation of $`V_{\mathrm{eff}}`$ from any modern $`NN`$ potential is the existence of a strong repulsive core which prevents its direct use in nuclear structure calculations. This difficulty is usually overcome by resorting to the well known Brueckner $`G`$-matrix method. Here, we have made use of a new approach bogn02  which has proved to be an advantageous alternative bogn02 ; cov02 ; cor03  to the use of the above method. The basic idea underlying this approach is to construct a low-momentum $`NN`$ potential, $`V_{\mathrm{low}\mathrm{k}}`$, that preserves the physics of the original potential $`V_{NN}`$ up to a certain cut-off momentum $`\mathrm{\Lambda }`$. In particular, the scattering phase shifts and deuteron binding energy calculated by $`V_{NN}`$ are reproduced by $`V_{\mathrm{low}\mathrm{k}}`$. The latter is a smooth potential that can be used directly as input for the calculation of shell-model effective interactions. A detailed description of our derivation of $`V_{\mathrm{low}\mathrm{k}}`$ can be found in Ref. bogn02 , where a criterion for the choice of the cut-off parameter $`\mathrm{\Lambda }`$ is also given. We have used here the value $`\mathrm{\Lambda }=2.1`$ fm-1.

Once the $`V_{\mathrm{low}\mathrm{k}}`$ is obtained, the calculation of the matrix elements of the effective interaction is carried out within the framework of the folded-diagram method outlined above. The key feature of this approach is that there is no need for $`G`$-matrix procedures to eliminate the effects of a strongly repulsive core, since the $`V_{\mathrm{low}\mathrm{k}}`$ can be used directly in the calculation of the vertex function $`\widehat{Q}`$-box. The calculation of $`\widehat{Q}`$, which is in principle an infinite sum of irreducible diagrams, can only be made approximately by selecting certain classes of diagrams. In our calculations we have included in $`\widehat{Q}`$ all the 1-body and 2-body diagrams up to second order in $`V_{\mathrm{low}\mathrm{k}}`$. For instance, for the particle-particle case these are precisely the diagrams shown in Ref. jian92 . In this connection, it should be pointed out that the proton-neutron matrix elements for 208Bi, 132Sb, 98Ag and 102In have been explicitly derived in the particle-hole formalism. A description of the derivation of the particle-hole effective interaction is given in Ref. cor02a .

To summarize, there are three main steps in our derivation of $`V_{\mathrm{eff}}`$. We first derive the low-momentum $`V_{\mathrm{low}\mathrm{k}}`$ from the CD-Bonn potential, then calculate the $`\widehat{Q}`$-box including diagrams up to second order in $`V_{\mathrm{low}\mathrm{k}}`$, and finally obtain $`V_{\mathrm{eff}}`$ by summing up the folded diagram series (4) by means of the Lee-Suzuki iteration method.

## III Results and comparison with experiment

In this section, the results of our calculations for the proton-neutron multiplets around 208Pb, 132Sn, and 100Sn are presented and compared with the experimental data. In the first two mass regions, both proton-neutron hole and proton-neutron multiplets are considered by studying 208,210Bi and 132,134Sb. These nuclei, all having only two valence nucleons, are the most appropriate ones to study the effects of the proton-neutron interaction. As regards doubly magic 100Sn, the two immediate odd-odd neighbors for which some experimental information is presently available are 98Ag and 102In, both with four valence nucleons. We have therefore considered these two nuclei to study the proton hole-neutron multiplets in this region. We present our results separately for each mass region in the three following subsections. All calculations have been performed using the OXBASH shell-model code OXBASH .

### III.1 208Pb region: 208Bi and 210Bi

The particle-hole multiplets in 208Bi were long ago found to exhibit a peculiar behavior ersk64 ; alf68 , namely the states with the minimum and maximum $`J`$ have the highest excitation energy, while the state with next to highest $`J`$ is the lowest one. As mentioned in the Introduction, the results of the shell-model calculations of Ref. kuo68  turned out to be consistent with this pattern.

In Fig. 1 our results for three multiplets are reported and compared with the experimental data nndc . Note that the energies are relative to the $`5^+`$ ground state, which is a member of the doublet $`\pi h_{9/2}\nu p_{1/2}^1`$. We see that the calculated energies account for the pattern of the experimental multiplets, the quantitative agreement being remarkably good with discrepancies well below 100 keV for almost all the states. It should be pointed out that our calculations give a better description of the experimental data than the early realistic calculations of Ref. kuo68 .

Let us now come to 210Bi. In Fig. 2 the calculated $`\pi h_{9/2}\nu g_{9/2}`$ multiplet (represented by open circles) is shown and compared with the experimental data nndc . This multiplet shows a breakdown of the Nordheim strong rule nord50  in that the $`1^{}`$ state is the ground state while the $`0^{}`$ one lies at about 50 keV excitation energy. We see that our calculation predicts for the ground state $`J^\pi =0^{}`$ with the $`1^{}`$ state at about 150 keV excitation energy. This is, however, the most significant discrepancy, all other experimental excitation energies being reproduced within few tens of keV. As a whole, the pattern of this multiplet as compared to that of the particle-hole multiplets is still parabolic, but concave downward. Of course this stems from the fact that the interaction changes from repulsive to attractive.

It should be pointed out that the behavior of all the multiplets considered above is directly related to the proton-neutron effective interaction since their members are of almost pure configuration. In this context, it is quite interesting to study the renormalization of the effective interaction, which we have taken into account through second-order diagrams in $`V_{\mathrm{low}\mathrm{k}}`$. By way of illustration, we report in Tables IV and V the diagonal matrix elements of the effective interaction for the particle-hole $`\pi h_{9/2}\nu f_{5/2}^1`$ and particle-particle $`\pi h_{9/2}\nu g_{9/2}`$ configuration, respectively. In both tables we also show the corresponding matrix elements of $`V_{\mathrm{low}\mathrm{k}}`$ and $`<V_{\mathrm{ph}}>`$, the latter representing the contribution of the particle-hole core-polarization diagram, the so-called “bubble”. Here, we do not consider the contributions coming from either other second-order diagrams or folded diagrams, both of which we have found irrelevant for the present discussion. From Table IV, we see that the matrix elements of $`V_{\mathrm{ph}}`$, although not very large in magnitude, are quite relevant in determining the pattern of the considered particle-hole multiplet. In fact, they are repulsive for states with minimum and maximum $`J`$ and attractive for $`J=J_{\mathrm{max}}1`$. It is worth noting that the repulsive contribution to the $`J_{\mathrm{max}}`$ state is essential to place it above the state with $`J=J_{\mathrm{min}}+1`$. For the particle-particle case, Table V shows that the core-polarization contribution is essentially repulsive, except for the $`J^\pi =1^{}`$ state. This goes in the right direction, as it reduces the spacing between the $`1^{}`$ and $`0^{}`$ states. However, as is evident from Fig. 2, it is not sufficient to produce the inversion of these two states.

On these grounds, we have found it interesting to modify our effective interaction for 210Bi by simply increasing the diagonal matrix elements of $`V_{\mathrm{ph}}`$ for the $`\pi h_{9/2}\nu g_{9/2}`$ configuration. It turns out that all the calculated energies go in the right direction, a factor of 2.6 being sufficient to give the correct ground state. The results of this calculation (represented by open squares) are shown in Fig. 2. It can be seen that they practically overlap the experimental ones.

### III.2 132Sn region: 132Sb and 134Sb

The particle-hole and particle-particle nuclei 132Sb and 134Sb play in the 132Sn region the role played by 208Bi and 210Bi in the 208Pb region. In this connection, it is worth mentioning that the resemblance between the spectroscopy of these two regions has been emphasized in several recent papers forn01 .

The nucleus 132Sb has been the subject of our study of Ref. cor02a , to which we refer for details. Some multiplets have been also reported in Ref. garg03  together with some results for 134Sb. For completeness, we report in Fig. 3 the $`\pi g_{7/2}\nu d_{3/2}^1`$ and $`\pi g_{7/2}\nu h_{11/2}^1`$ multiplets in 132Sb while Fig. 4 shows our results for the $`\pi g_{7/2}\nu f_{7/2}`$ multiplet in 134Sb. Note that these multiplets are just the counterparts of those considered above for 208Bi and 210Bi (aside from the doublet $`\pi g_{9/2}\nu p_{1/2}^1`$). Comments on the behavior of the multiplets as well as on the quality of agreement between theory and experiment can be found in Refs. cor02a ; garg03 . In the latter paper, the diagonal matrix elements of $`V_{\mathrm{eff}}`$, $`V_{\mathrm{low}\mathrm{k}}`$, and $`V_{\mathrm{ph}}`$ for the $`\pi g_{7/2}\nu d_{3/2}^1`$ and $`\pi g_{7/2}\nu f_{7/2}`$ configurations are reported. We emphasize here that the particle-hole and particle-particle matrix elements of the effective interaction in the 132Sn region show the same features as those evidenced above for the 208Pb region. In particular, we have found that also in this case the core-polarization plays a significant role, but it is not sufficient to give the right spacing between the $`0^{}`$ and $`1^{}`$ states in the particle-particle multiplet of 134Sb (see Fig. 4). We have then modified the effective interaction by multiplying the diagonal matrix elements of $`V_{\mathrm{ph}}`$ for the $`\pi g_{7/2}\nu f_{7/2}`$ configuration by the same factor used for 210Bi. The corresponding results are represented by open squares in Fig. 4, where we see that they are in excellent agreement with experiment.

### III.3 100Sn region: 98Ag and 102In

In the 100Sn region the counterpart of 208Bi and 132Sb is 100In, which until now has not been accessible to spectroscopic studies. We have therefore considered the two neighboring odd-odd isotopes 98Ag and 102In , focusing attention on the $`\pi g_{9/2}^1\nu d_{5/2}`$ multiplet for which some experimental information is available. The members of the calculated multiplet in both nuclei have been identified as those dominated by this configuration with the two remaining valence nucleons forming a zero-coupled pair. In Figs. 5 and 6 we report the results of our calculations for 98Ag and 102In, respectively, and compare them with the experimental data nndc . We see that the agreement between experiment and theory is of the same quality as that obtained in the 208Pb and 132Sn regions, the largest discrepancy being 130 keV for the $`5^+`$ state in 98Ag. The pattern of the calculated multiplets turns out to be similar to that of the multiplets in 208Bi and 132Sb. However, we find that the percentage of components other than those we have considered to characterize the multiplet is rather large. For instance, it reaches about 60% for the $`7^+`$ state in 102In. A detailed discussion of the structure of the calculated states will be included in a forthcoming publication.

The diagonal matrix elements of the effective interaction for the proton hole-neutron particle $`\pi g_{9/2}^1\nu d_{5/2}`$ configuration are reported in Table VI, where we see that their behavior is quite similar to that occurring in the heavier-mass regions.

## IV Summary and conclusions

We have presented here some results of a shell-model study of odd-odd nuclei in the close vicinity to doubly magic 208Pb, 132Sn and 100Sn, where use has been made of realistic effective interactions derived from the CD-Bonn $`NN`$ potential.

The main aim of this work has been to gain insight into the effects of the proton-neutron interaction on the pattern of the particle-hole and particle-particle multiplets. To this end, we have made a detailed comparison between the calculated results and the available experimental data as well as an analysis of the proton-neutron matrix elements of our effective interaction. It has turned out that the core polarization is essential for the effective interaction to produce a good description of all considered nuclei. In this context, we have found out that some discrepancies for the particle-particle multiplets in both 210Bi and 134Sb are removed when the core polarization contribution is increased by a factor of 2.6. This is likely to be traced to the coupling of the single-particle motion to the octupole excitation in 208Pb and 132Sn.

A relevant outcome of our calculations is that for all the particle-hole multiplets the $`J_{\mathrm{min}}`$ and $`J_{\mathrm{max}}`$ states have the highest excitation energy, while the state with next to the highest $`J_{\mathrm{max}}`$ is the lowest, in agreement with the predictions of the Brennan-Bernstein coupling rule bren60 .

In summary, we may conclude that the results of the present study show that realistic shell-model calculations are able to describe with quantitative accuracy the effects of the proton-neutron interaction around closed shells, which gives confidence in their predictive power. This is of particular value for nuclei in the 132Sn and 100Sn regions, for which it is of utmost importance to gain more experimental information.

###### Acknowledgements.

This work was supported in part by the Italian Ministero dell’Istruzione, dell’Università e della Ricerca (MIUR).