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# Metal-insulator transitions in systems with electron-phonon and Coulomb interactions

## I Introduction

The alkali-doped fullerenes, AnC60 (A= K, Rb), raise many interesting problems due to the important role played by both the electron-electron and the electron-phonon interaction. For $`n=3`$ and $`n=4`$ each alkali atom is assumed to donate about one electron into a six-fold degenerate $`t_{1u}`$ band. A3C60 are metals and superconductors, while A4C60 are insulators. The $`t_{1u}`$ orbital is only partly filled for both systems, and band structure calculations predict both systems to be metallic. A4C60 must then be an insulator due to interaction effects neglected in band structure calculations. Under pressure A4C60 becomes metallic, while some fullerenes at normal pressure and with the doping $`n=3`$ (NH3K3C60, Cs3C60) are not superconductors and probably insulators, but become superconductors under pressure. This suggest that these systems are relatively close to a metal-insulator transition. A metal-insulator transition is usually discussed in terms of the ratio between the Coulomb interaction $`U`$ between two electrons on the same molecule and the one-particle band width $`W`$. For A3C60 and A4C60 this ratio is, however, almost identical. It is then interesting to ask which factors determine whether a system is on the metallic or insulating side.

These systems have been studied in a Hubbard-like model, and it was found that the three-fold degeneracy of the $`t_{1u}`$ orbital plays an important role by increasing the ratio $`U/W`$ where the metal-insulator transition takes place. It was furthermore found that the lattice structure is important for the difference between A3C60 (fcc) and A4C60 (bct). Hubbard-like models predict, however, that A4C60 is an anti-ferromagnetic insulator, while it is known experimentally that there are no moments in A4C60. The electrons in AnC60 have a relatively strong interaction with Jahn-Teller intramolecular phonons with Hg symmetry and a weaker interaction with Ag phonons. The interaction with the Jahn-Teller phonons favor a low spin state and might lead to a nonmagnetic insulator. At the same time there is, however, a Hund’s rule coupling, which favors a high spin state. This leads to an interesting competition between the Jahn-Teller effect and the Hund’s rule coupling. The purpose of this paper is therefore to study the influence of the Jahn-Teller effect and the Hund’s rule coupling on the metal-insulator transition. We do this in the context of the Fullerenes, but similar effects also occur in many other systems, e.g., transition metal compounds.

In this paper we study a model of AnC60 which includes the electron-phonon coupling and the electron-electron interaction. In AnC60 partly occupied orbital $`t_{1u}`$ couples to two nondegenerate phonons of Ag symmetry and to eight five-fold degenerate (Jahn-Teller) phonons of Hg symmetry. For AnC60 the important coupling is believed to be to the Hg phonons, and we therefore study a model with a coupling to one Hg phonon. To see the effect of having a Jahn-Teller phonon, we also compare with a model containing an Ag phonon. The models are solved in the dynamical mean-field theory (DMFT) or by using exact diagonalization. To interprete the results we also study analytically a single molecule and a simple two-site model. A brief summary of some aspects of this work are published elsewhere.

In Sec. II we present results for a free molecule and in Sec. III we discuss the typical parameter range. We present results for a two-site model in Sec. IV and describe the DMFT calculation in Sec. V. The results are given in Sec. VI and discussed in Sec. VII.

## II Isolated molecule

We first study an isolated molecule. We consider the case of the coupling to an Ag phonon and two cases of coupling to Jahn-Teller phonons, namely the $`E\times E`$ case, where a two-fold degenerate level couples to a two-fold degenerate phonon, and the $`T\times H`$ case, where a three-fold degenerate level couples to a five-fold degenerate phonon. The $`E\times E`$ case is the simplest model with a Jahn-Teller effect, and the $`T\times H`$ case is a simple model of a C60 molecule. Thus we consider the Hamiltonian

$`H_{\mathrm{el}\mathrm{ph}}`$ $`=\epsilon _0{\displaystyle \underset{m}{}}{\displaystyle \underset{\sigma }{}}c_{m\sigma }^{}c_{m\sigma }+\omega _0{\displaystyle \underset{\nu }{}}b_\nu ^{}b_\nu `$ (2)
$`+g{\displaystyle \underset{\nu }{}}{\displaystyle \underset{\sigma }{}}{\displaystyle \underset{m}{}}{\displaystyle \underset{m^{^{}}}{}}V_{mm^{^{}}}^{(\nu )}c_{m\sigma }^{}c_{m^{^{}}\sigma }(b_\nu +b_\nu ^{}),`$
where the first term describes the electronic level, the second the phonon and the third the electron-phonon coupling. The coupling matrices $`V^{(\nu )}`$ are determined by symmetry and they are given in, e.g., Ref. . For the coupling to an Ag phonon $`V^{(1)}`$ is diagonal with all the diagonal elements equal to unity, $`V_{mm^{^{}}}^{(1)}=\delta _{mm^{^{}}}`$. For the $`E\times E`$ case

$$V^{(1)}=\left(\begin{array}{cc}1& 0\\ 0& 1\end{array}\right)\mathrm{and}V^{(2)}=\left(\begin{array}{cc}0& 1\\ 1& 0\end{array}\right)$$
(3)
and for the $`T\times H`$ case

$`V^{(1)}={\displaystyle \frac{1}{2}}\left(\begin{array}{ccc}1& 0& 0\\ 0& 1& 0\\ 0& 0& 2\end{array}\right)V^{(2)}={\displaystyle \frac{1}{2}}\left(\begin{array}{ccc}\sqrt{3}& 0& 0\\ 0& \sqrt{3}& 0\\ 0& 0& 0\end{array}\right)`$ (10)
$`V^{(3)}={\displaystyle \frac{\sqrt{3}}{2}}\left(\begin{array}{ccc}0& 1& 0\\ 1& 0& 0\\ 0& 0& 0\end{array}\right)V^{(4)}={\displaystyle \frac{\sqrt{3}}{2}}\left(\begin{array}{ccc}0& 0& 1\\ 0& 0& 0\\ 1& 0& 0\end{array}\right)`$ (17)
$`V^{(5)}={\displaystyle \frac{\sqrt{3}}{2}}\left(\begin{array}{ccc}0& 0& 0\\ 0& 0& 1\\ 0& 1& 0\end{array}\right)`$ (21)
The overall coupling strength is determined by $`g`$. In a metallic molecular solid with narrow bands, there is a simple relation between $`g`$ and the dimensionless coupling $`\lambda `$

$$\lambda _H=\frac{5}{3}N(0)\frac{g^2}{\omega _0}$$
(22)
for the $`T\times H`$ case and

$$\lambda _E=2N(0)\frac{g^2}{\omega _0}$$
(23)
for the $`E\times E`$ case. Here $`N(0)`$ is the electron density of states per spin. We also define a Jahn-Teller energy

$$E_{JT}=\frac{g^2}{\omega _0}.$$
(24)
In addition we include the Coulomb interaction

$`H_\mathrm{U}=`$ $`U_{xx}{\displaystyle \underset{m}{}}n_mn_m+U_{xy}{\displaystyle \underset{\sigma \sigma ^{^{}}}{}}{\displaystyle \underset{m<m^{^{}}}{}}n_{\sigma m}n_{\sigma ^{^{}}m^{^{}}}`$ (25)
$`+`$ $`{\displaystyle \frac{1}{2}}K{\displaystyle \underset{\sigma \sigma ^{^{}}}{}}{\displaystyle \underset{mm^{^{}}}{}}\psi _{m\sigma }^{}\psi _{m^{^{}}\sigma ^{^{}}}^{}\psi _{m\sigma ^{^{}}}\psi _{m^{^{}}\sigma }`$ (26)
$`+`$ $`{\displaystyle \frac{1}{2}}K{\displaystyle \underset{\sigma }{}}{\displaystyle \underset{mm^{^{}}}{}}\psi _{m\sigma }^{}\psi _{m\sigma }^{}\psi _{m^{^{}}\sigma }\psi _{m^{^{}}\sigma },`$ (27)
where $`n_{m\sigma }=\psi _{m\sigma }^{}\psi _{m\sigma }`$ is an occupation number, $`U_{xx}`$ and $`U_{xy}`$ are the Coulomb interactions between equal and unequal orbitals, respectively and $`K`$ is an exchange integral. The Coulomb integrals are related via

$$U_{xy}=U_{xx}2K.$$
(28)
For Ag phonons and a free molecule, the electron-phonon problem is reduced to a displaced oscillator, and we can easily obtain the electron-phonon contribution to the ground-state energy

$$E^{A_g}(N)=N^2E_{JT}.$$
(29)
where $`E(N)`$ is the energy of a free molecule with $`N`$ electrons. The Jahn-Teller case is more complicated and cannot be solved exactly. We therefore focus on the lowest order contribution to $`E(N)`$. For the Coulomb interaction this contribution is of first order in $`K`$ and for the electron-phonon interaction it is of second order in $`g`$. The results are shown in Table I for the $`E\times E`$ case and in Table II for the $`T\times H`$ case. We have subtracted an average Coulomb energy,

$$\stackrel{~}{E}(N)E(N)\frac{1}{2}N(N1)U_{av}(k),$$
(30)
where $`U_{av}(k)`$ is the average interaction for the ground-state in a full shell with $`2k`$ electrons and the orbital degeneracy $`k`$. By definition, $`\stackrel{~}{E}(N)`$ is then zero for a full shell. Results for the low spin state (singlet or doublet) and the high spin state (triplet or quartet) are shown in Table I.

Neglecting the Coulomb interaction ($`U`$ and $`K`$) the results for the $`T\times H`$ case can be written as

$$E_H^{WC}(N)=\frac{5}{2}C(N)E_{JT},$$
(31)
where

$$C(N)=\{\begin{array}{ccc}1& \mathrm{for}& N=1,5\\ 4& \mathrm{for}& N=2,4\\ 3& \mathrm{for}& N=3\end{array}$$
(32)
This is a weak-coupling result for the case when $`\lambda `$ (or $`g`$) is small. For the strong-coupling case

$$E_H^{SC}(N)=C(N)E_{JT}.$$
(33)
In the strong-coupling case the prefactor in front of $`C(N)E_{JT}`$ has been reduced by a factor of $`5/2`$.

From tables I and II it follows that the low spin state is lower in energy for $`K<2E_{JT}`$ in the $`E\times E`$ case and for $`K<\frac{3}{2}E_{JT}`$ in the $`T\times H`$ case. The results illustrate the competition between the Jahn-Teller effect and the Hund’s rule coupling. According to Hund’s first rule, it is favorable to form a high spin state to minimize the Coulomb energy. On the other hand, the Jahn-Teller effect favors a low spin state. For instance, if the first phonon ($`\nu =1`$) of $`E`$ symmetry (the left matrix in Eq. (3)) is excited, it is favorable to put two electrons (with opposite spins) in the level $`m=2`$, resulting in a singlet. The tables show that in the low spin state the energy $`\stackrel{~}{E}(N)`$ is lowered by the electron-phonon coupling but is increased by the exchange integral $`K`$. In the high spin state, on the other hand, the exchange coupling lowers the energy, while the electron-phonon interaction lowers the energy less than in the low spin state or not at all.

This can be further illustrated by considering the case of two electrons in the $`E\times E`$ system. For $`K<2E_{JT}`$, the important states are

$$|1=\psi _1^{}\psi _1^{}|\mathrm{vac}|2=\psi _2^{}\psi _2^{}|\mathrm{vac}.$$
(34)
These states couple directly via the exchange interaction and indirectly via the electron-phonon interaction. Thus we also include states where one phonon has been excited. In the corresponding Hamiltonian matrix the part corresponding to the states with one phonon are “folded” into the part corresponding to $`|i`$, $`i=1`$ or 2, and we obtain the matrix

$$\left(\begin{array}{cc}U_{xx}6E_{JT}& 2E_{JT}+K\\ 2E_{JT}+K& U_{xx}6E_{JT}\end{array}\right)$$
(35)
If $`K<2E_{JT}`$ the corresponding energy is

$$U_{xx}6E_{JT}+(2E_{JT}+K)=U_{av}(2)8E_{JT}+\frac{8}{3}K,$$
(36)
which clearly shows the competition between the Jahn-Teller coupling and the Hund’s rule coupling. For $`K>2E_{JT}`$ a triplet state of the type $`\psi _1^{}\psi _2^{}|\mathrm{vac}`$ with the energy $`U_{av}(2)4K/3`$ becomes the lowest state.

## III Parameter range

It is now important to establish the parameter range appropriate for AnC60. In particular, the relative size of $`g`$ and $`K`$ is important, since this determines whether the Jahn-Teller effect or the Hund’s rule coupling wins. The exchange integral $`K`$ has been estimated from an ab initio SCF calculation. From the calculated multiplet splitting the result $`K=0.11`$ eV was obtained. Correlation effects are expected to reduce this number, since correlation effects in particular lower the energies of the low spin states. The difference in Coulomb energy between the low spin states and the high spin states is then reduced and the effective $`K`$ becomes correspondingly smaller. For instance, for some atomic multiplets, correlation effects were found to reduce the multiplet splitting by about 25 $`\%`$. The electron-phonon coupling constants have been estimated from photoemission experiments for a free molecule. Here we replace the eight Hg modes by one effective mode. The frequency of this mode is chosen as the logarithmically averaged frequency

$`\lambda ={\displaystyle \underset{\nu =1}{\overset{8}{}}}\lambda _\nu ;\lambda \mathrm{ln}\omega _0={\displaystyle \underset{\nu =1}{\overset{8}{}}}\lambda _\nu \mathrm{ln}\omega _\nu `$ (37)
where $`\lambda _\nu `$ and $`\omega _\nu `$ are the electron-phonon couplings and frequencies, respectively. We have calculated the energies of the lowest singlet and triplet states for a free C60 molecule. The results are shown in Fig. 1. Experimentally it is found that the low spin state wins for both A3C60 and A4C60, A4C60 being a nonmagnetic insulator and NH3K3C60 being antiferromagnetic with a moment (0.7 $`\mu _B`$ per molecule) which corresponds to a spin 1/2 system. For A4C60 the triplet-singlet splitting is estimated to be 0.1 eV. In Fig. 1 this splitting is obtained for $`K0.07`$ eV. As expected this value is smaller than the value $`K=0.11`$ eV deduced from the HF calculation. We observe that a change in the estimate of $`g`$ of course would also lead to a change in this empirical number of $`K`$. Since, however, the present estimate of $`K`$ seems reasonable relative the the HF value, this calculation also gives some support for the value of $`g`$ deduced from PES.

## IV A two-site model

In this section we study a two-site model to gain understanding of a) the different influences of an Ag and a Jahn-Teller phonon on the metal-insulator transition and b) the competition between the Jahn-Teller effect and the Hund’s rule coupling. We therefore compare the case of an Ag phonon coupling to a two-fold degenerate level ($`A\times E`$ problem) with the Jahn-Teller $`E\times E`$ problem. Thus we study the model

$$H=\underset{i=1}{\overset{2}{}}[H_{\mathrm{el}\mathrm{phon}}(i)+H_\mathrm{U}(i)]+H_{\mathrm{hop}},$$
(38)
where $`H_{\mathrm{el}\mathrm{phon}}(i)`$ (Eq. (2)) describes the electron-phonon interaction on site $`i`$, $`H_\mathrm{U}(i)`$ (Eq. (25)) describes the Coulomb interaction on site $`i`$, and

$$H_{\mathrm{hop}}=t\underset{m=1}{\overset{2}{}}\underset{\sigma }{}(\psi _{1m\sigma }^{}\psi _{2m\sigma }+\psi _{2m\sigma }^{}\psi _{1m\sigma }),$$
(39)
describes the hopping between the two sites. We have assumed that there is only hopping between equal $`m`$-quantum numbers.

The band gap $`E_g(n)`$ for the filling $`n`$ is given by

$$E_g(n)=E(2n1)+E(2n+1)2E(2n)$$
(40)
for a two-site model, where $`E(N)`$ is the ground-state energy of a system with $`N`$ electrons. It is useful to consider $`E_g`$ in the limit when $`U`$ is very large, and then to extrapolate to intermediate values of $`U`$. The limit of a large $`U`$ is particular transparent, allowing for simple calculations and a qualitative understanding, but it is still relevant for the intermediate values of $`U`$ where the metal-insulator transition takes place. The the metal-insulator transition happens when $`E_g=0`$, i.e., we find the critical value of $`U`$ for which this condition is satisfied. The two-site system is much too small for obtaining reliable quantitative estimates of the critical $`U`$ and the extrapolation of the large $`U`$ results is questionable. Nevertheless, this approach can give a qualitative understanding of more realistic calculations. We consider the limit

$`g<<\omega _0<<W<<U`$ (41)
$`K{\displaystyle \frac{g^2}{\omega _0}}E_{JT}<<W,`$ (42)
where the electron-phonon coupling and the exchange integral are just weak perturbations to the hopping and to the Coulomb interaction.

We first study the case of an Ag phonon and calculate the gap for the filling $`n=1`$. It is then convenient to transform the coupling term to the form

$$g\underset{i=1}{\overset{2}{}}(n_i1)(b_i+b_i^{}),$$
(43)
where $`n_i=_{m\sigma }\psi _{im\sigma }^{}\psi _{im\sigma }`$ and we have neglected an irrelevant term $`(g^2/\omega _0)_i(2n_i1)`$. For a system with two electrons and in the limit of a large $`U`$, hopping is almost completely suppressed, and each site has almost exactly one electron. The term (43) then has essentially zero coupling to this state, and we obtain

$$E^{A_g}(2)0.$$
(44)
Since there is only one electron per site, there are no multiplet effects. To obtain the energy of a system with one electron, it is convenient to transform to bonding and antibonding operators, e.g., $`\psi _{\pm m\sigma }=(\psi _{1m\sigma }\pm \psi _{2m\sigma })`$. This gives the interaction term

$`{\displaystyle \frac{g}{\sqrt{2}}}[`$ $`(\psi _{+m\sigma }^{}\psi _{+m\sigma }+\psi _{m\sigma }^{}\psi _{m\sigma })(b_++b_+^{})`$ (45)
$`+`$ $`(\psi _{+m\sigma }^{}\psi _{m\sigma }+\psi _{m\sigma }^{}\psi _{+m\sigma })(b_{}+b_{}^{})].`$ (46)
The bonding level is then occupied by one electron, giving the kinetic energy $`t`$. The leading contribution to the energy due to the electron-phonon interaction is $`\frac{1}{2}E_{JT}`$, giving

$$E^{A_g}(1)=t\frac{1}{2}E_{JT}.$$
(47)
In the limit studied here ($`\omega _0<<W`$), the phonons react to the average electronic charge, which gives rise to the factor $`\frac{1}{2}`$.

We next consider the system with three electrons. The wave function for $`g=0`$ and $`K=0`$ is

$`|0={\displaystyle \frac{1}{\sqrt{6}}}(\psi _{11}^{}\psi _{11}^{}\psi _{22}^{}+\psi _{11}^{}\psi _{21}^{}\psi _{12}^{}+\psi _{21}^{}\psi _{11}^{}\psi _{12}^{}`$ (48)
$`+`$ $`\psi _{21}^{}\psi _{21}^{}\psi _{12}^{}+\psi _{21}^{}\psi _{11}^{}\psi _{22}^{}+\psi _{11}^{}\psi _{21}^{}\psi _{22}^{})|\mathrm{vac}.`$ (49)
The corresponding energy is $`0|H|0=2t`$. For a general lattice and for a state which is half-filled apart from one electron or one hole, we expect the hopping to be enhanced by roughly a factor $`\sqrt{N_{\mathrm{deg}}}`$, where $`N_{\mathrm{deg}}`$ is the orbital degeneracy. However, for the two-site system this enhancement is $`N_{\mathrm{deg}}`$. The effects of the electron-phonon coupling are now included in perturbation theory. For the parameter range considered here ($`\omega _0<<W`$), there is only coupling to the states $`b_i^{}|0`$. Furthermore, the Coulomb energy is given by $`0|H_\mathrm{U}|0`$, since there are no states with the kinetic energy -$`2t`$ which couple to $`|0`$ via $`H_\mathrm{U}`$. The energy is therefore

$$E^{A_g}(3)=U_{xx}2t\frac{1}{2}E_{JT}\frac{5}{3}K.$$
(50)
The corresponding band gap is given in Table III ($`A\times E`$), which also shows the result for the filling $`n=2`$. The table shows that the band gap is reduced by the electron-phonon coupling. Extrapolating to intermediate values of $`U`$ then suggests that the electron-phonon coupling increases the critical value of $`U`$ where the metal-insulator transition takes place. The reason is that the electron-phonon interaction in the model (43) is not effective for integer filling in the large $`U`$ case, since the charge fluctuations are then suppressed. For the states with an extra electron or hole, on the other hand, there is a fluctuating charge due to the hopping of the electron or hole and a corresponding lowering of the energy due to the electron-phonon coupling.

The multiplet effects trivially reduce the gap for $`n=1`$, since they are effective for the state with three electrons but not for the other two states. For $`n=2`$, however, they increase the gap. The reason is that in the integer occupation case ($`N=4`$), hopping plays no role for a large $`U`$ and the state can adjust to use the multiplet effects optimally. This is not possible for the case of an extra hole ($`N=3`$) or an extra electron ($`N=5`$), since then the states first of all adjusts to optimize hopping, and only in the second place adjust to optimize the multiplet effects. The increase of the gap due to the exchange integral has been observed earlier.

We next consider the Jahn-Teller case of two-fold degenerate phonons. We first calculate the energy of the state with one electron per site in the large $`U`$ limit. Perturbation theory shows that each phonon contributes an energy $`E_{JT}`$. Since there are two phonons per site and two sites, the energy is

$$E^{E_g}(2)=4E_{JT},$$
(51)
where Eg labels the Jahn-Teller case. Although charge fluctuations are completely suppressed in this case, the system can still gain energy by introducing a (dynamical) Jahn-Teller distortion. This is in strong contrast to the Ag phonons, which only couple to the net charge on a given site. In perturbation theory, the energies of the states with an extra electron or hole are

$`E^{E_g}(1)=tE_{JT}`$ (52)
$`E^{E_g}(3)=U_{xx}2tE_{JT}{\displaystyle \frac{5}{3}}K.`$ (53)
The electron-phonon interaction lowers the energy twice as much as in the Ag case (Eqs. (47) and (50)), simply because the phonon is two-fold degenerate and the coupling therefore is to twice as many phonons as in the Ag case. The corresponding gap is shown in Table III, which also shows the gap for the filling $`n=2`$.

For $`n=2`$ and $`K<E_{JT}`$ the Jahn-Teller effect dominates over the Hund’s rule coupling. In this case as well as for $`n=1`$ the gap is then increased by the electron-phonon interaction, while in the Ag case it is decreased. The reason is similar as for the multiplet effects in the Ag case, discussed in the second paragraph below Eq. (50). For the parameter range (Eq. (41)) we are considering and for integer filling, the hopping is very efficiently suppressed, and the Jahn-Teller system can therefore adjust efficiently to the electron-phonon interaction. With an extra electron or hole, however, the system cannot take advantage of the electron-phonon interaction to the same extent, since the wave function primarily optimizes the hopping of the electron or hole. According to Eq. (40), this leads to an increase of the gap. In the Ag case, on the other hand, the system cannot couple to the phonons in the integer filling case, and therefore even the reduced coupling to the phonons in the case of an extra electron or hole is sufficient to reduce the gap.

Table III furthermore illustrates the competition between the Jahn-Teller effect and the Hund’s rule coupling. For $`K<2E_{JT}`$ and $`n=2`$ an increase of $`K`$ leads to a reduction of the gap. As $`K`$ is further increased, the system instead tends to go into high spin states, and the gap is increased as K is increased.

It is interesting to compare the results with a different approach. We can calculate an effective on-site $`U_{eff}(n)`$ for the filling $`n`$ as

$$U_{eff}(n)=E(n+1)+E(n1)2E(n),$$
(54)
where $`E(N)`$ now refers to the energy of a free molecule, calculated in Sec. II. For $`K<2E_{JT}`$ and for the $`E\times E`$ case, we then obtain

$`U_{eff}(1)=U_{av}(2)4E_{JT}+{\displaystyle \frac{8}{3}}K`$ (55)
$`U_{eff}(2)=U_{av}+12E_{JT}{\displaystyle \frac{16}{3}}K.`$ (56)
It is then tempting to assume that for the filling $`n=1`$ and $`n=2`$ the gap is given by $`U_{eff}(1)3t`$ and $`U_{eff}(2)4t`$, respectively. Comparison with Table III shows that this is incorrect in the limit studied here (Eq. (41)). In particular, for $`n=1`$, this approach would even predict the wrong sign for the the electron-phonon contribution to the gap. The reason is that Eq. (54) assumes that the electron-phonon and Hund’s rule couplings can adjust to the instantaneous occupation of a given site. As we have seen above, this is not possible in the limit (Eq. (41)) for the states with an extra electron or hole. $`U_{eff}(2)`$ may instead become relevant in the limit when the exchange coupling $`K`$ and the Jahn-Teller energy $`E_{JT}`$ are much larger than the hopping energy.

In a similar way we have calculated the gap for the $`T\times H`$ two-site problem. The results are shown in Table IV. These results also illustrate the competition between the Jahn-Teller effect and the Hund’s rule coupling.

## V Dynamical mean-field calculations

We now consider the $`T\times H`$ problem in the dynamical mean-field theory (DMFT). We formulate the infinite dimensional limit on the Bethe lattice, where the nearest-neighbor hopping integral $`t_{im,jm^{}}`$ is rescaled as $`t^{}/\sqrt{z}`$ with the connectivity $`z`$ going to infinity. We further simplify the hopping by setting $`t_{im,jm^{}}\delta _{mm^{}}`$ only allowing the diagonal hopping. The unit of energy is chosen such that the bandwidth, $`W`$, is set to 2. The Jahn-Teller phonons embedded at each lattice sites of the bath can be easily incorporated into the effective medium of the impurity Anderson model, since they are Einstein phonons without direct intersite couplings between them. Therefore the lattice contribution of phonons is implicitly included in the medium electron Green’s function.

We here focus on the problem where the exchange integral $`K=0`$. The effective impurity Anderson model is solved using the quantum Monte Carlo (QMC) technique with the Fye-Hirsch algorithm, which has only mild “fermion sign-problems” with our Hamiltonian. Here we treat fully quantum mechanically the phonon fields which are updated together with the fermion auxiliary fields in each Monte Carlo step. Details of the implementation of the QMC technique in the DMFT can be found elsewhere in the literature. We have used the discretization step for the Trotter breakup, $`\mathrm{\Delta }\tau =1/3`$, throughout this paper unless mentioned otherwise and more than one million Monte Carlo sweeps are taken for each iteration of the self-consistency loop. For the case where the exchange integral $`K>0`$ the QMC method has a serious “sign-problem”, and this case is treated in Sec. VID using exact diagonalization.

## VI Results

We study how the metal-insulator transition depends on the parameters, e.g., the ratio $`U/W`$ for different strengths of the electron-phonon coupling $`\lambda `$ and the exchange integral. When the system becomes insulating a gap is opened up in the electron spectral function $`A(\omega )`$. This shows up in the electron Green’s function $`G(\tau )`$ calculated for imaginary times $`\tau `$. For instance if

$$A(\omega )=0\mathrm{f}\mathrm{o}\mathrm{r}|\omega |<\mathrm{\Delta },$$
(57)
we obtain

$$G(\tau =\beta /2)e^{\mathrm{\Delta }\beta /2},$$
(58)
where $`\beta =1/T`$. Thus $`G(\beta /2)`$ decays exponentially with $`\beta `$ for an insulator. We therefore use the behavior of $`G(\beta /2)`$ as a measure whether the system is a metal or an insulator. It is also interesting to study the charge fluctuation $`(nn_0)^2`$, which is an average of $`(n_in_0)^2`$ and where $`n_0`$ is the average occupancy per site. This quantity is expected to become small but nonzero at the metal-insulator transition.

### A Jahn-Teller Hg phonons

We first study the Jahn-Teller Hg phonons and consider the case of half-filling, i.e., three electrons per site. Fig. 2 shows $`G(\beta /2)`$ as a function of $`U/W`$ for different values of $`\lambda `$. The figure illustrates that for a given $`\lambda `$, $`G(\beta /2)`$ is reduced as $`U`$ is increased and at some critical value $`U_c`$, $`G(\beta /2)`$ becomes very close to zero (not exactly equal to zero due to the finite temperature), where a metal insulator transition takes place. The figure also illustrates that the charge fluctuations $`(n3)^2`$ are strongly reduced in the insulating state. The critical $`U_c/W`$ is reduced as $`\lambda `$ grows. The reason for this was discussed extensively in Sec. IV.

It is interesting that $`U_c`$ as a function of $`\lambda `$ initially is reduced very strongly as $`\lambda `$ is increased, while for larger values of $`\lambda `$ the decrease is slower. This can be understood in terms of the results in Eq. (31, 33) for the Jahn-Teller energy in the weak- and strong-coupling limits. This shows that the electron-phonon energy increases much faster with $`\lambda `$ (by a factor of $`5/2`$) in the weak-coupling limit than in the strong-coupling limit. This is particularly relevant for the large $`U`$ integer filling case, where the electron-phonon interaction has a similar effect as in the free molecule, and it gives a qualitative explanation for the dependence of $`U_c`$ on $`\lambda `$.

### B Ag versus Jahn-Teller Hg phonons

We next compare the Jahn-Teller Hg phonons with Ag phonons. Fig. 3 shows $`G(\beta /2)`$ in a system with coupling to Ag phonons as a function of $`U`$ for $`\lambda =0`$ and for $`\lambda =0.8`$. Comparing the results for $`\lambda =0`$ and $`\lambda =0.8`$, we can see that the coupling to Ag phonons increases the critical $`U_c`$ where the metal-insulator transition takes place, while in the case of Hg phonons this value is decreased (see Fig. 2). The reason for this change was discussed extensively in Sec. IV.

It is interesting to observe that both the electron-phonon interaction and the electron-electron interaction by themselves would tend to reduce $`G(\beta /2)`$. In a weak-coupling theory where we simply add the lowest order contribution to the self-energy from each interaction, we would then predict that the two interactions work together in reducing $`G(\beta /2)`$. This is indeed what is found in Fig. 3 for $`U/W=0.5`$. Not too surprisingly, the arguments presented below Eq. (52) and assuming the large $`U`$ limit are incorrect for $`U/W=0.5`$. It is not surprising that these arguments become correct for large values of $`U/W`$, but it is important that they are qualitatively correct already for $`U/W1.5`$, which is on the metallic side of the metal-insulator transition.

For a system with only a Coulomb interaction $`U`$, the metal-insulator transition can be thought of as resulting from the competition between kinetic and potential energy. When the coupling to the phonons is introduced the hopping of the electrons is reduced, since an electron tends to drag a cloud of phonons along its path. It is then tempting to assume that the coupling to phonons will move the metal-insulator transition towards smaller values of $`U`$. Our results show that for the parameter range considered here, the effect is the opposite for the case of coupling to Ag phonons.

The coupling to the Ag phonons in A3C60 is weak, and the Ag phonons should not play an important role. There is, however, a strong coupling to a charge carrying plasmon derived from the $`t_{1u}`$ electrons. This plasmon couples in the same way as the Ag phonons. Its energy (0.5eV) is larger than the phonon energies. However, whether we consider the plasmon energy to be small or large we arrive at the conclusion that it increases $`U_c`$. For small values of the plasmon energy this follows from the study of the Ag phonons, and for large energies of the plasmon, we can introduce an effective $`U_{eff}`$ as in Eq. (54). The coupling to the plasmon reduces $`U_{eff}`$ and therefore the metal-insulator transition happens for a larger bare $`U`$.

### C A3C60 versus A4C60

Fig. 4 shows $`G(\beta /2)`$ for A4C60. The figure illustrates that $`U_c`$ is smaller at filling four than filling three (see Fig. 4). This is not surprising in view of Eq. (31-33) and Table IV, since the energy is lowered more by the electron-phonon coupling for filling four than for filling three. According to Eq. (40) this increases the gap of the insulating state more for filling four than for filling three, i.e., it makes $`U_c`$ smaller for filling four. As discussed in the next section, this result is, however, modified by the Jahn-Teller coupling.

### D Competition between Jahn-Teller and Hund’s rule coupling

We finally discuss the competition between the Jahn-Teller effect and the Hund’s rule coupling. Since there is a sign-problem in the dynamical mean-filed calculations if we use the full multiplet coupling in Eq. (25), we use an exact diagonalization technique. This requires that the system size is small. Therefore we consider a system with just four sites and we consider the $`E\times E`$ problem (Eq. (3)). We furthermore limit the Hilbert space by not allowing more than two phonons per site. To reduce the discreteness of the one-particle spectrum for such a small system, we pick the hopping integrals randomly. We calculate the gap according to Eq. (40) and add some finite size corrections

$$E_g^{red}(U_{xx})=E_g\frac{U_{av}(2)}{N_{site}}E_g^{U=0},$$
(59)
where $`U_{av}(2)/N_{site}`$ is a contribution to the gap from the electrostatic energy of a finite system, $`N_{site}`$ is the number of sites and $`E_g^{U=0}`$ is the gap of a system without any Coulomb interaction. Both these corrections go to zero for a large system. Assuming that that $`E_g^{red}`$ grows linearly with $`U_{xx}`$, we can then use

$$U_{xx}E_g^{red}(U_{xx})$$
(60)
as a crude estimate of the critical $`U_{xx}`$. This quantity is shown in Fig. 5. The results can be qualitatively understood from the results in Table III for a two-site system, although the parameter range considered here is outside the range where the results in the table are valid. For $`\lambda =0`$, the critical value of $`U_{xx}`$ is reduced as $`K`$ is increased, as expected. However, as $`\lambda `$ is increased, the competition between the Jahn-Teller and Hund’s rule effects leads to an increase of the critical $`U_{xx}`$. This is in agreement with Table III, although the increase is faster than for the parameter range of this table. For a particular value of $`\lambda `$, the critical $`U_{xx}`$ becomes comparable to the value for $`K=\lambda =0`$. As $`\lambda `$ is further increased, the Jahn-Teller effect becomes dominating and the critical value of $`U_{xx}`$ decreases again. This critical value is, however, larger than for $`K=0`$, due to the competition between the Jahn-Teller and Hund’s rule coupling.

## VII Discussion

It is interesting to discuss these results in the context of AnC60. Considering just the Hubbard $`U`$ ($`g=K=0`$), it is found that the metal-insulator transition in A3C60 takes place at the upper range of what is believed to be physical values of $`U/W`$, while for A4C60 this happens at the lower range of these parameters. This agrees nicely with the fact that A3C60 is a metal but A4C60 is an insulator. However, to explain why A4C60 is not antiferromagnetic, we need to include the coupling to the Jahn-Teller Hg phonons. This substantially lowers the critical $`U_c`$ for both systems, and it puts $`U_c/W`$ of A3C60 at the lower range of the physical parameters. This puts our understanding of A3C60 being a metal into question. We find, however, that the competition between the Jahn-Teller effect and the Hund’s rule coupling increases $`U_c`$ again. The coupling to the $`t_{1u}`$ plasmons in A3C60 should lead to an additional increase of $`U_c`$ in this system. This makes it understandable that A3C60 can be a metal.

## VIII Acknowledgements

This work has been supported by the Max-Planck-Forschungspreis.


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# 𝑆𝑂(10) Unification of Color Superconductivity and Chiral Symmetry Breaking ?

## Acknowledgements

We are indebted to D. H. Friedan for extremely helpful advice and to D. Kaplan and K. Rajagopal for clarifying and stimulating discussions. We also like to thank M. Alford and S.-C. Zhang for interesting discussions about color and high-temperature superconductivity. We gratefully acknowledge the hospitality of the INT in Seattle where this work was done. Our work is supported in part by funds provided by the U.S. Department of Energy (D.O.E.) under cooperative research agreements DE-FC02-94ER40818 and DE-FG02-96ER40945. U.-J. W. also acknowledges the support of the A. P. Sloan foundation.


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# 1 Preparations

## 1 Preparations

Let $`X`$ be a compact Kähler manifold. Then $`𝒦_XH^{1,1}(X,)`$ denotes the Kähler cone, i.e. the open set of all Kähler classes on $`X`$. For a class $`\alpha H^{1,1}(X,)`$ we usually denote by $`\stackrel{~}{\alpha }𝒜^{1,1}(X)_{}`$ a closed real $`(1,1)`$-form representing $`\alpha `$. Let us recall the following version of the Aubin-Calabi-Yau theorem

###### Theorem 1.1

— Let $`X`$ be an $`N`$-dimensional compact Kähler manifold with a given volume form $`\mathrm{vol}𝒜^{N,N}(X)_{}`$. For any Kähler class $`\omega 𝒦_X`$ there exists a unique Kähler form $`\stackrel{~}{\omega }𝒜^{1,1}(X)_{}`$ representing $`\omega `$, such that $`\stackrel{~}{\omega }^N=c\mathrm{vol}`$, with $`c`$.

Since $`\stackrel{~}{\omega }^N`$ is harmonic with respect to $`\stackrel{~}{\omega }`$, this can be equivalently expressed by saying that any Kähler class $`\omega `$ can uniquely be represented by a Kähler form $`\stackrel{~}{\omega }`$ with respect to which the given volume form is harmonic. Note that the constant $`c`$ can be computed as $`c=_X\omega ^N/\mathrm{vol}(X)`$.

###### Definition 1.2

— For a given volume form $`\mathrm{vol}𝒜^{N.N}(X)_{}`$ we let $`\stackrel{~}{𝒦}_X𝒜^{1,1}(X)_{}`$ be the set of Kähler forms $`\stackrel{~}{\omega }`$ with respect to which $`\mathrm{vol}`$ is harmonic.

By the Aubin-Calabi-Yau theorem the natural projection $`\stackrel{~}{𝒦}_X𝒦_X`$ is bijective. But, in general, $`\stackrel{~}{𝒦}_X`$ is not an open subset of a linear subspace of $`𝒜^{1,1}(X)`$ (cf. 2.1). Let $`\stackrel{~}{\omega }\stackrel{~}{𝒦}_X`$. The tangent space of $`\stackrel{~}{𝒦}_X`$ at $`\stackrel{~}{\omega }`$ can be computed as follows. Firstly, we may write $`\stackrel{~}{𝒦}_X=_+\times \stackrel{~}{𝒦}_X^c`$, where $`\stackrel{~}{𝒦}_X^c=\{\stackrel{~}{\omega }𝒦_X|\stackrel{~}{\omega }^N=c\mathrm{vol}\}`$. Secondly, the infinitesimal deformations of $`\stackrel{~}{\omega }`$ in the direction of $`\stackrel{~}{𝒦}_X^c`$ are of the form $`\stackrel{~}{\omega }+\epsilon \stackrel{~}{v}`$, where $`\stackrel{~}{v}`$ is a closed real $`(1,1)`$-form and such that $`(\stackrel{~}{\omega }+\epsilon \stackrel{~}{v})^N=\stackrel{~}{\omega }^N`$. The latter condition gives $`\stackrel{~}{\omega }^N+\left(\genfrac{}{}{0pt}{}{N}{2}\right)\epsilon \stackrel{~}{\omega }^{N1}\stackrel{~}{v}=\stackrel{~}{\omega }^N`$, i.e. $`\stackrel{~}{v}`$ is primitive. As any closed primitive $`(1,1)`$-form is harmonic, this shows that the tangent space of $`\stackrel{~}{𝒦}_X^c`$ at $`\stackrel{~}{\omega }`$ is the space $`^{1,1}(\omega )_{,prim}`$ of real $`\stackrel{~}{\omega }`$-primitive $`\stackrel{~}{\omega }`$-harmonic $`(1,1)`$-forms. Thirdly, the $`_+`$-direction corresponds to the scaling of $`\stackrel{~}{\omega }`$ and this tangent direction is therefore canonically identified with $`\stackrel{~}{\omega }`$. Altogether, one obtains that $`T_{\stackrel{~}{\omega }}\stackrel{~}{𝒦}_X=^{1,1}(\stackrel{~}{\omega })_{}`$ is the space of real $`\stackrel{~}{\omega }`$-harmonic $`(1,1)`$-forms. In particular, $`\stackrel{~}{𝒦}_X`$ is a smooth connected subset of $`𝒜^{1,1}(X)_{}`$. To make this approach rigorous, one completes $`𝒜^{1,1}(X)`$ in the $`L^2`$-topology. The projection of the closed forms to cohomology is a differential map (use e.g. Hodge theory, cf. ). The lifted Kähler cone $`\stackrel{~}{𝒦}_X`$ is the intersection of the space of closed $`L^2`$-forms with the space of sections of the submanifold of the bundle of $`(1,1)`$-forms that consists of those positive forms whose top exterior power equals (a scalar multiple of) the given $`(N,N)`$-form at every point.

###### Definition 1.3

— Let $`X`$ be a compact Kähler manifold with a given volume form. Then one associates to a given Kähler class $`\omega 𝒦_X`$ the space $`^{p.q}(\omega ):=^{p,q}(\stackrel{~}{\omega })`$ of $`(p,q)`$-forms that are harmonic with respect to the unique $`\stackrel{~}{\omega }\stackrel{~}{𝒦}_X`$ representing $`\omega `$.

Note that two different Kähler forms $`\stackrel{~}{\omega }_1`$ and $`\stackrel{~}{\omega }_2`$ representing the same Kähler class $`\omega _1=\omega _2`$ always have different spaces of harmonic $`(1,1)`$-forms. Indeed, $`\stackrel{~}{\omega }_1`$ and $`\stackrel{~}{\omega }_2`$ are $`\stackrel{~}{\omega }_1`$-harmonic respectively $`\stackrel{~}{\omega }_2`$-harmonic. Since any class, in particular $`\omega _1=\omega _2`$, is represented by a unique harmonic form and $`\stackrel{~}{\omega }_1\stackrel{~}{\omega }_2`$, this yields $`^{1,1}(\stackrel{~}{\omega }_1)^{1,1}(\stackrel{~}{\omega }_2)`$. One might ask more generally what the relation is between the spaces of harmonic forms with respect to different Kähler forms not representing the same Kähler class. It is quite interesting to observe that the dependence of $`^{1,1}(\stackrel{~}{\omega })`$ on the Kähler class $`\omega `$ is related to the problem discussed in the introduction. We will try to make this more explicit in the next section.

## 2 How ‘harmonic’ depends on the Kähler form

Let us begin with the following fact which relates the shape of $`\stackrel{~}{𝒦}_X`$ to the dependence of $`^{1,1}(\omega )`$ on $`\omega `$.

###### Proposition 2.1

— The subspace $`^{1,1}(\omega )𝒜^{1,1}(X)`$ is independent of $`\omega `$ if and only if $`\stackrel{~}{𝒦}_X`$ spans an $``$-linear subspace of dimension $`h^{1,1}(X)`$.

Proof. Let $`^{1,1}(\omega )𝒜^{1,1}(X)`$ be independent of $`\omega 𝒦_X`$. Since for any $`\omega 𝒦_X`$ the unique $`\stackrel{~}{\omega }\stackrel{~}{𝒦}_X`$ representing it is $`\stackrel{~}{\omega }`$-harmonic, the assumption immediately yields $`\stackrel{~}{𝒦}_X^{1,1}(\omega )_{}`$ for any $`\omega 𝒦_X`$.

Conversely, if $`\stackrel{~}{𝒦}_X`$ spans an $``$-linear subspace of dimension $`h^{1,1}(X)`$, then this subspace coincides with the tangent space of $`\stackrel{~}{𝒦}_X`$ at every point $`\stackrel{~}{\omega }\stackrel{~}{𝒦}_X`$. But the latter was identified with $`^{1,1}(\omega )_{}`$. Hence, the linear subspace equals $`^{1,1}(\omega )_{}`$ for any $`\omega 𝒦_X`$ and $`^{1,1}(\omega )`$, therefore, does not depend on $`\omega `$. $`\mathrm{}`$

###### Remark 2.2

— The assertion might be rephrased from a slightly different point of view as follows. The bijective map $`\stackrel{~}{𝒦}_X𝒦_X`$ can be used to define a differentiable map $`𝒦_X𝒜^2(X)`$ (in the $`L^2`$-topology). The proposition then just says that this map is linear if and only if the Gauss map is constant. It might be instructive to rephrase some of the results later on in this spirit, e.g. Prop. 3.2.

The next proposition states that the ‘global’ change of $`^{1,1}(\omega )`$ for $`\omega 𝒦_X`$ is determined by the ‘harmonic’ behaviour with respect to a single $`\omega 𝒦_X`$.

###### Proposition 2.3

— Let $`X`$ be a compact Kähler manifold of dimension $`N`$ with a fixed Kähler form $`\stackrel{~}{\omega }_0`$ and volume form $`\stackrel{~}{\omega }_0^N/N!`$. Then the following statements are equivalent:

i) The linear subspace $`^{1,1}(\omega )𝒜^{1,1}(X)_{}`$ does not depend on $`\omega 𝒦_X`$.

ii) For all $`\alpha ^{1,1}(\omega _0)`$ one has $`\alpha ^N^{N,N}(\omega _0)`$.

Proof. Let us assume i). By the previous lemma the lifted Kähler cone $`\stackrel{~}{𝒦}_X`$ spans the $``$-linear subspace $`^{1,1}(\omega _0)`$. Since $`\stackrel{~}{𝒦}_X`$ is open in $`^{1,1}(\omega _0)_{}`$ and all $`\alpha \stackrel{~}{𝒦}_X`$ satisfy the $``$-linear equation

$$\alpha ^N=(_X\alpha ^N/_X\omega _0^n)\omega _0^N$$
(1)
which is an algebraic condition, in fact all $`\alpha ^{1,1}(\omega _0)`$ satisfy (1). Hence, for all $`\alpha ^{1,1}(\omega _0)`$ the top exterior power $`\alpha ^N`$ is harmonic, i.e. ii) holds true.

Let us now assume ii). If $`\alpha ^{1,1}(\omega _0)`$, such that its cohomology class $`\omega :=[\alpha ]`$ is a Kähler class, let $`\stackrel{~}{\omega }\stackrel{~}{𝒦}_X`$ denote the distinguished representing Kähler form of $`\omega `$. If $`\alpha `$ itself is strictly positive definite, then the unicity of $`\stackrel{~}{\omega }`$ and ii) imply $`\alpha =\stackrel{~}{\omega }`$. Thus, the intersection of the closed subset $`^{1,1}(\omega _0)_{}`$ with the open cone of strictly positive definite real $`(1,1)`$-forms is contained in $`\stackrel{~}{𝒦}_X`$. This intersection is non-empty, as it contains $`\stackrel{~}{\omega }_0`$. Since $`\stackrel{~}{𝒦}_X`$ is a closed connected subset of this open cone of the same dimension as $`^{1,1}(\omega _0)_{}`$ this yields $`\stackrel{~}{𝒦}_X^{1,1}(\omega _0)_{}`$. By Prop. 2.1 one concludes that $`^{1,1}(\omega )`$ does not depend on $`\omega 𝒦_X`$. $`\mathrm{}`$

## 3 The positive cone

The next proposition is a first step towards a geometric understanding of the failure of harmonicity of $`\alpha ^N`$ for a harmonic form $`\alpha `$. To state it we recall the following notation.

###### Definition 3.1

— For a compact Kähler manifold $`X`$ the positive cone $`𝒞_XH^{1,1}(X,)`$ is the connected component of $`\{\alpha H^{1,1}(X,)|_X\alpha ^N>0\}`$ that contains the Kähler cone.

Note that by definition $`𝒦_X𝒞_X`$.

###### Proposition 3.2

— If $`X`$ is a compact Kähler cone such that $`𝒦_X`$ is strictly smaller than $`𝒞_X`$, then for any Kähler form $`\stackrel{~}{\omega }`$ there exists a $`\stackrel{~}{\omega }`$-harmonic $`(1,1)`$-form $`\alpha `$ such that $`\alpha ^N`$ is not $`\stackrel{~}{\omega }`$-harmonic.

Proof. Assume that there exists a Kähler form $`\stackrel{~}{\omega }_0`$ such that for all $`\alpha ^{1,1}(\stackrel{~}{\omega }_0)`$ also $`\alpha ^N`$ is $`\stackrel{~}{\omega }_0`$-harmonic. We endow $`X`$ with the volume form $`\stackrel{~}{\omega }_0^N/N!`$. By Prop. 2.3 the lifted Kähler cone $`\stackrel{~}{𝒦}_X`$ is contained in $`^{1,1}(\stackrel{~}{\omega }_0)`$. Since $`𝒦_X`$ is strictly smaller than $`𝒞_X`$ there exists a sequence $`\omega _t𝒦_X`$ converging towards a $`\omega 𝒞_X𝒦_X`$. As $`\stackrel{~}{𝒦}_X`$ is contained in the finite-dimensional space $`^{1,1}(\stackrel{~}{\omega }_0)`$ the lifted Kähler forms $`\stackrel{~}{\omega }_t\stackrel{~}{𝒦}_X`$ will converge towards a form (!) and not only a current $`\stackrel{~}{\omega }^{1,1}(\stackrel{~}{\omega }_0)\stackrel{~}{𝒦}_X`$. As a limit of strictly positive definite forms $`\stackrel{~}{\omega }`$ is still semi-positive definite. Moreover, $`\stackrel{~}{\omega }`$ is strictly positive definite at $`xX`$ if and only if $`\stackrel{~}{\omega }^N`$ does not vanish at $`x`$. By assumption $`\stackrel{~}{\omega }^N=c\stackrel{~}{\omega }_0^N`$ with $`c=_X\omega ^N/_X\omega _0^N`$. Since $`\omega 𝒞_X`$, the scalar factor $`c`$ is strictly positive. Hence, $`\stackrel{~}{\omega }^N`$ is everywhere non-trivial. Thus $`\stackrel{~}{\omega }`$ is strictly positive definite. This yields the contradiction.$`\mathrm{}`$

The interesting thing here is that the proposition in particular can be used to determine the positivity of a class with positive top exterior power just by studying the space of harmonic forms with respect to a single given, often very special Kähler form:

###### Corollary 3.3

— Let $`X`$ be a compact Kähler manifold with a given Kähler form $`\stackrel{~}{\omega }_0`$. If for all $`\stackrel{~}{\omega }_0`$-harmonic $`(1,1)`$-forms $`\alpha `$ the top exterior power $`\alpha ^N`$ is also $`\stackrel{~}{\omega }_0`$-harmonic, then any class $`\omega 𝒞_X`$ is a Kähler class.$`\mathrm{}`$

We conclude this section with a few examples, where the assumption of the corollary is met a priori. In the later sections we will discuss examples where $`𝒦_X`$ is strictly smaller than $`𝒞_X`$ and where Prop. 3.2 can be used to conclude the ‘failure’ of harmonicity.

###### Examples 3.4

i) If $`X`$ is a complex torus and $`\omega `$ is a flat Kähler form, then harmonic forms are constant forms and their products are again constant, hence harmonic. In particular, one recovers the fact that on a torus the Kähler cone and the positive cone coincide.

ii) If for two Kähler manifolds $`(X,\stackrel{~}{\omega })`$ and $`(X^{},\stackrel{~}{\omega }^{})`$ with $`b_1(X)b_1(X^{})=0`$ the top exterior power of any harmonic $`(1,1)`$-forms on $`X`$ or on $`X^{}`$ is again harmonic, then the same holds for the product $`(X\times X^{},\stackrel{~}{\omega }\times \stackrel{~}{\omega }^{})`$. The additional assumption on the Betti-numbers is necessary as the product of two curves shows. Indeed, any $`\phi H^{1,0}(X)`$, for a curve $`X`$, is harmonic, but $`\phi \overline{\phi }`$ is not. Hence, $`\alpha =\phi \times \overline{\phi }+\overline{\phi }\times \phi `$ is a harmonic $`(1,1)`$-form on $`X\times X^{}`$ with non-harmonic $`\alpha ^2`$.

iii) If $`X`$ is a Kähler manifold, such that $`^{1,1}(\omega )`$ does not depend on $`\omega `$, then the same holds for any smooth finite quotient of $`X`$.

iv) For hermitian symmetric spaces of compact type it is known that the space of harmonic forms equals the space of forms invariant under the real form. As the latter space is invariant under products, the Kähler cone of an irreducible hermitian symmetric space coincides with the positive cone.

## 4 K3 surfaces

As indicated earlier the behaviour of the Kähler cone is closely related to the geometry of the manifold. We shall study this in more detail for K3 surfaces. The next proposition follows directly from the description of the Kähler cone of a K3 surface.

###### Proposition 4.1

— Let $`X`$ be a K3 surface containing a smooth rational curve. Then for any Kähler form $`\stackrel{~}{\omega }`$ there exists an $`\stackrel{~}{\omega }`$-harmonic form $`(1,1)`$-form $`\alpha `$ such that $`\alpha ^2`$ is not harmonic.

Proof. If $`X`$ contains a smooth rational curve, then $`𝒦_X`$ is strictly smaller than $`𝒞_X`$ and we apply Prop. 3.2. Indeed, a smooth rational curve $`CX`$ determines a $`(2)`$-class $`[C]`$, whose perpendicular hyperplane $`[C]^{}`$ cuts $`𝒞_X`$ into two parts and $`𝒦_X`$ is contained in the part that is positive on $`C`$.$`\mathrm{}`$

If the harmonicity of the top exterior powers fails for a Kähler manifold with a given Kähler form $`(X,\stackrel{~}{\omega })`$ then it should do so for any small deformation of $`(X,\stackrel{~}{\omega })`$. For a Ricci-flat Kähler structure on a K3 surface the argument can be reversed and one can use the existence of rational curves on arbitrarily near deformations to prove the above proposition on any K3 surface.

###### Corollary 4.2

— Let $`X`$ be an arbitrary K3 surface. If $`\stackrel{~}{\omega }`$ is any hyperkähler form on $`X`$, then there exists a $`\stackrel{~}{\omega }`$-harmonic $`(1,1)`$-form $`\alpha `$ such that $`\alpha ^2`$ is not $`\stackrel{~}{\omega }`$-harmonic.

Proof. Let $`H^0(X,\mathrm{\Omega }_X^2)=\sigma `$. Then

$$\begin{array}{ccc}\hfill ^2(\stackrel{~}{\omega })& =& ^{1,1}(\stackrel{~}{\omega })^{2,0}(\stackrel{~}{\omega })^{0,2}(\stackrel{~}{\omega })\hfill \\ & =& ^{1,1}(\stackrel{~}{\omega })\sigma \overline{\sigma }\hfill \end{array}$$

As the space of harmonic forms only depends on the underlying hyperkähler metric $`g`$, $`^{1,1}(\stackrel{~}{\omega })\sigma \overline{\sigma }`$ contains $`^{1,1}(\stackrel{~}{\omega }_{aI+bJ+cK})`$ for all $`(a,b,c)S^2`$. Here, $`I,J,`$ and $`K`$ are the three complex structures associated with the hyperkähler metric $`g`$.

Assume $`\alpha ^2`$ is $`g`$-harmonic for all $`\alpha ^{1,1}(\stackrel{~}{\omega })`$. Since $`\sigma =\stackrel{~}{\omega }_J+i\stackrel{~}{\omega }_K`$ (up to a scalar factor) and since the product of a harmonic form with the Kähler form is again harmonic, also $`\sigma \overline{\sigma }`$ is harmonic. This implies that $`\alpha ^2`$ is harmonic for all $`\alpha ^2(\omega )`$, as $`\sigma ^2=\overline{\sigma }^2=\alpha \sigma =\alpha \overline{\sigma }=0`$ for $`\alpha ^{1,1}(\stackrel{~}{\omega })`$. Thus, $`\alpha ^2`$ is $`g`$-harmonic for all $`\alpha ^{1,1}(\stackrel{~}{\omega }_{aI+bJ+cK})`$ and all $`(a,b,c)S^2`$. On the other hand, it is well-known that for a non-empty (dense) subset of $`S^2`$ the K3 surface $`(X,aI+bJ+cK)`$ contains a smooth rational curve. Indeed, if $`eH^2(X,)`$ is any $`(2)`$-class, then the subset of the moduli space of marked K3 surfaces for which $`e`$ is of type $`(1,1)`$ is a hyperplane section. This hyperplane section, necessarily, cuts the complete curve given by the base $`^1=S^2`$ of the twistor family. Hence, on one of the K3 surfaces $`(X,aI+bJ+cK)`$ the class $`e`$ represents a smooth rational curve. Contradiction.$`\mathrm{}`$

###### Remark 4.3

— What are the bad harmonic $`(1,1)`$-forms? Certainly $`\stackrel{~}{\omega }^2`$ is harmonic and for any harmonic form $`\alpha `$ also $`\stackrel{~}{\omega }\alpha `$ is harmonic. So, if there is any bad harmonic $`(1,1)`$-form there must be also one that is $`\stackrel{~}{\omega }`$-primitive. Most likely, it is even true that the square of any primitive harmonic form is not harmonic. The proof of it should closely follow the arguments in the proof of Prop. 3.2, but there is a slight subtlety concerning the existence of sufficiently many $`(2)`$-classes, that I cannot overcome for the moment. We sketch the rough idea: Assume there exists a $`\stackrel{~}{\omega }`$-harmonic $`\stackrel{~}{\omega }`$-primitive real $`(1,1)`$-form $`\alpha `$ such that $`\alpha ^2`$ is $`\stackrel{~}{\omega }`$-harmonic. As a $`\stackrel{~}{\omega }`$-harmonic $`\stackrel{~}{\omega }`$-primitive $`(1,1)`$-form $`\alpha `$ is also of type $`(1,1)`$ with respect to any complex structure $`\lambda =aI+bJ+cK`$ induced by the hyperkähler metric corresponding to $`\stackrel{~}{\omega }`$ (see Prop. 7.5 ). Moreover, $`\alpha `$ is also primitive with respect to all Kähler forms $`\stackrel{~}{\omega }_\lambda `$. Assume that there exists a complex structure $`\lambda S^2`$, such that $`𝒞_X[\alpha ]\omega _\lambda `$ is not contained in $`𝒦_X`$. This condition can be easily rephrased in terms of $`(2)`$-classes and thus becomes a question on the lattice $`3U2(E_8)`$. It looks rather harmless, but for the time being I do not know a complete proof of it. Under this assumption, we may even assume that in fact $`\lambda =I`$. Since $`\alpha ^2`$ is harmonic, in fact $`\beta ^2`$ is harmonic for all $`\beta \alpha \stackrel{~}{\omega }^{1,1}(\omega )`$. Going back to the proof of Prop. 3.2, we see that the second part of it can be adapted to this situation and shows that $`\psi ^1(𝒦_X[\alpha ]\omega )\alpha \stackrel{~}{\omega }`$, where $`\psi :\stackrel{~}{𝒦}_X𝒦_X`$. The space $`\psi ^1(𝒦_X[\alpha ]\omega )`$ is the space of the distinguished Kähler forms whose classes are linear combinations of $`[\alpha ]`$ and $`\omega `$. Therefore, all these forms are harmonic and linear combinations of $`\alpha `$ and $`\stackrel{~}{\omega }`$ themselves. To conclude, we imitate the proof of Prop. 3.2 and choose a sequence $`\omega _t𝒦_X[\alpha ]\omega `$ converging towards $`\omega ^{}𝒞_X𝒦_X`$. The corresponding sequence $`\stackrel{~}{\omega }_t\stackrel{~}{𝒦}_X`$ is contained in $`\alpha \stackrel{~}{\omega }`$ and converges towards a form(!) $`\stackrel{~}{\omega }^{}`$. As in the proof of Prop. 3.2 this leads to a contradiction.

## 5 Hyperkähler manifolds

We will try to improve upon Prop. 3.2 in the case of hyperkähler manifolds. In particular, we will replace the question whether the top exterior power $`\alpha ^N`$ of an harmonic form $`\alpha `$ is harmonic by the corresponding question for the square of $`\alpha `$. The motivation for doing so stems from the general philosophy that hyperkähler manifolds should be treated in almost complete analogy to K3 surfaces and that instead of the top intersection pairing one should consider the Beauville-Bogomolov  form as the higher dimensional analogue of the intersection pairing for K3 surfaces.

Let us begin by recalling some notations and basic facts. By a compact hyperkähler manifold $`X`$ we understand a simply-connected compact Kähler manifold, such that $`H^0(X,\mathrm{\Omega }^2)=\sigma `$, where $`\sigma `$ is an everywhere non-degenerate holomorphic two-form. A Ricci-flat Kähler form $`\stackrel{~}{\omega }`$ turns out to be a hyperkähler form (cf. ), i.e. there exists a metric $`g`$ and three complex structures $`I`$, $`J`$, and $`K:=IJ`$, such that the corresponding Kähler forms $`\stackrel{~}{\omega }_{aI+bJ+cK}`$ are closed for all $`(a,b,c)S^2`$, such that $`I`$ is the complex structure defining $`X`$, and such that $`\stackrel{~}{\omega }=\stackrel{~}{\omega }_I`$. One may renormalize $`\sigma `$, such that $`\sigma =\stackrel{~}{\omega }_J+i\stackrel{~}{\omega }_K`$. In particular, multiplying with $`\sigma `$ maps harmonic forms to harmonic forms, for this holds true for the Kähler forms $`\stackrel{~}{\omega }_J`$ and $`\stackrel{~}{\omega }_K`$.

The positive cone $`𝒞_XH^{1,1}(X,)`$ is a connected component of $`\{\alpha H^{1,1}(X,)|q_X(\alpha )>0\}`$, where $`q_X`$ is the Beauville-Bogomolov form (cf. ).

###### Proposition 5.1

— Let $`X`$ be a $`2n`$-dimensional compact hyperkähler manifold with a fixed hyperkähler form $`\omega _0`$ and the unique holomorphic two-form $`\sigma `$. Then $`\alpha ^2(\sigma \overline{\sigma })^{n1}`$ is harmonic for all $`\alpha ^{1,1}(\omega _0)`$ if and only if the linear subspace $`^{1,1}(\omega )𝒜^{1,1}(X)`$ does not depend on $`\omega 𝒦_X`$.

Proof. Assume that for all $`\alpha ^{1,1}(\omega _0)`$ also $`\alpha ^2(\sigma \overline{\sigma })^{n1}`$ is harmonic. If $`\alpha `$ is in addition strictly positive definite and $`\stackrel{~}{\omega }\stackrel{~}{𝒦}_X`$ with $`[\alpha ]=\omega `$, then $`\alpha ^2(\sigma \overline{\sigma })^{n1}=\stackrel{~}{\omega }^2(\sigma \overline{\sigma })^{n1}`$. We adapt Calabi’s classical argument to deduce that in this case $`\alpha =\stackrel{~}{\omega }`$: If $`\alpha ^2(\sigma \overline{\sigma })^{n1}=\stackrel{~}{\omega }^2(\sigma \overline{\sigma })^{n1}`$, then $`(\alpha \stackrel{~}{\omega })(\alpha +\stackrel{~}{\omega })(\sigma \overline{\sigma })^{n1}=0`$. Since $`\alpha `$ and $`\stackrel{~}{\omega }`$ are strictly positive definite, also $`(\alpha +\stackrel{~}{\omega })`$ is strictly positive definite. By Lemma 6.1 of  also $`(\alpha +\stackrel{~}{\omega })(\sigma \overline{\sigma })^{n1}`$ is strictly positive. As $`[\alpha ]=\omega =[\stackrel{~}{\omega }]`$, the difference $`\alpha \stackrel{~}{\omega }`$ can be written as $`dd^c\phi `$ for some real function $`\phi `$. But by the maximum principle the equation $`(\alpha +\stackrel{~}{\omega })(\sigma \overline{\sigma })^{n1}dd^c\phi =0`$ implies $`\phi const`$. Hence, $`\alpha =\stackrel{~}{\omega }`$.

As in the proof of Prop. 3.2 this shows that the intersection of the closed subset $`^{1,1}(\omega _0)_{}`$ with the open cone of strictly positive definite forms in $`𝒜^{1,1}(X)_{}`$ is contained in $`\stackrel{~}{𝒦}_X`$ and one concludes that $`\stackrel{~}{𝒦}_X^{1,1}(\omega _0)_{}`$.

Hence, $`𝒦_X`$ spans a linear subspace of the same dimension and, by Lemma 2.1 this shows that $`^{1,1}(\omega )`$ is independent of $`\omega 𝒦_X`$.

Conversely, let $`^{1,1}(\omega )`$ be independent of $`\omega 𝒦_X`$. Then $`\stackrel{~}{𝒦}_X^{1,1}(\omega )_{}`$ for any $`\omega 𝒦_X`$. Therefore, $`\alpha ^2(\sigma \overline{\sigma })^{n1}=c(\sigma \overline{\sigma })^n`$ with $`c`$ for $`\alpha `$ in the Zariski-dense open subset $`\stackrel{~}{𝒦}_X^{1,1}(\omega )_{}`$. Hence, $`\alpha ^2(\sigma \overline{\sigma })^{n1}`$ is harmonic for any $`\alpha ^{1,1}(\omega )`$ (cf. proof of Prop. 2.3). $`\mathrm{}`$

Of course, as for K3 surfaces one expects that $`^{1,1}(\omega )`$ does in fact depend on $`\omega `$. This would again follow from the existence of rational curves in every nearby hyperkähler manifold. But it would actually be more interesting to reverse the argument: Assume that $`X`$ is a hyperkähler manifold, such that for any small deformation $`X^{}`$ of $`X`$ the Kähler cone $`𝒦_X^{}`$ equals $`𝒞_X^{}`$. I expect that this is equivalent to saying that $`^{1,1}(\omega )`$ does not depend on $`\omega `$. If for some other reason than the existence of rational curves as used in the K3 surface case this can be excluded, then one could conclude that there always is a nearby deformation $`X^{}`$ for which $`𝒦_X^{}`$ is strictly smaller than $`𝒞_X^{}`$. The latter is expected to imply the existence of rational curves on $`X^{}`$. Along these lines one could try to attack the Kobayashi conjecture, as the existence of rational curves on nearby deformations would say that $`X`$ itself cannot be hyperbolic. Unfortunately, I cannot carry this through even for K3 surface.

## 6 Various other examples

Here we collect a few examples where algebraic geometry predicts the failure of harmonicity of the top exterior power of harmonic two-forms. In all examples this is linked to the existence of rational curves.

Varieties of general type. Let $`X`$ be a non-minimal smooth variety of general type. As I learned from Keiji Oguiso this immediately implies that the Kähler cone is strictly smaller than the positive cone. His proof goes as follows: By definition the canonical divisor $`K_X`$ is big and by the Kodaira Lemma (cf. ) it can therefore be written as the sum $`K_X=H+E`$ of an ample divisor $`H`$ and an effective divisor $`E`$ (with rational coefficients). Consider the segment $`H_t:=H+tE`$ with $`t[0,1)`$. If all $`H_t`$ were contained in the positive cone $`𝒞_X`$, then $`K_X`$ would be in the closure of $`𝒞_X`$. If the Kähler cone coincided with the positive cone $`𝒞_X`$, then $`K_X`$ would be nef, contradicting the hypothesis that $`X`$ is not minimal. Hence $`t_0:=sup\{t|H_t𝒞_X\}(0,1)`$. If $`H_{t_0}`$ is not nef, then $`𝒦_X`$ is strictly smaller than $`𝒞_X`$. Thus, it suffices to show that $`H_{t_0}`$ is not nef. If $`H_{t_0}`$ were nef then all expressions of the form $`H_{t_0}^{Ni}.H^{i1}.E`$ would be non-negative. Then $`0=H_{t_0}^N=H_{t_0}^{N1}(H+t_0E)=H_{t_0}^{N1}.H+t_0H_{t_0}^{N1}.E`$, so both summands must vanish. In particular, $`0=H_{t_0}^{N1}.H=H^2.H_{t_0}^{N2}+t_0H.H_{t_0}^{N2}.E`$ Again this yields the vanishing of both terms and in particular $`0=H^2.H_{t_0}^{N2}`$. By induction we eventually obtain $`0=H^{N1}.H_{t_0}`$ and, furthermore, $`0=H^{N1}.H_{t_0}=H^N+t_0H^{N1}.E`$. But this time $`H^N>0`$ yields the contradiction. Therefore, for a non-minimal variety of general type one has $`𝒦_X𝒞_X`$ and hence there exist harmonic (with respect to an arbitrary Kähler metric) two-forms with non-harmonic top exterior power. Note that a non-minimal variety contains rational curves. As the reader will notice, the above proof goes through on an arbitrary manifold $`X`$ that admits a big, but not nef line bundle $`L`$ (replacing the canonical divisor). Also in this case the positive cone and the Kähler cone differ.

Birational Calabi-Yau. Let $`X`$ and $`X^{}`$ be birational Calabi-Yau manifolds, i.e. $`K_X`$ and $`K_X^{}`$ are trivial, then the birational map extends to an isomorphism or there exist harmonic $`(1,1)`$-forms on $`X`$, such that their top exterior power is not harmonic. Again, a non-trivial birational correspondence produces rational curves. As one expects for hyperkähler manifolds that $`^{1,1}(\omega )`$ does depend on the hyperkähler form even when $`X`$ does not contain a rational curve, e.g. for K3 surfaces, it would be interesting to see an example of a simply-connected Calabi-Yau manifold (in particular not a torus), where it does not.

The same argument could be applied to the case of different birational minimal models (minimal models are not unique!). This shows that in the previous example the Kähler cone could be strictly smaller than the positive cone, even when $`K_X`$ is nef or ample.

Blow-ups. This example is very much in the spirit of the previous two. Let $`X`$ be a non-trivial blow-up of a projective variety $`Y`$. Then $`𝒦_X`$ is strictly smaller than $`𝒞_X`$ and, therefore, for any Kähler structure on $`X`$ there exist harmonic $`(1,1)`$-forms with non-harmonic maximal exterior power. Indeed, if $`L`$ is an ample line bundle on $`Y`$ then $`f^{}(L)`$ is nef, but not ample, and it is contained in the positive cone. Hence, $`f^{}(L)𝒞_X𝒦_X`$. Note that also the first example could be proved along these lines. By evoking the contraction theorem one shows that any non-minimal projective variety $`X`$ admits a non-trivial contraction to a projective variety $`Y`$. The above argument then yields that $`𝒦_X`$ and $`𝒞_X`$ are different.

## 7 Chern forms

Let $`X`$ be a compact Kähler manifold with a Ricci-flat Kähler form $`\stackrel{~}{\omega }`$. If $`F`$ denotes the curvature of the Levi-Cevita connection $``$, then the Bianchi identity reads $`F=0`$. The Kähler-Einstein condition implies $`\mathrm{\Lambda }_\omega F=0`$. The last equation can be expressed by saying that $`F`$ is $`\stackrel{~}{\omega }`$-primitive. Analogously to the fact that any closed primitive $`(1,1)`$-form is in fact harmonic, one has that for $`F`$ with $`F=0`$ the primitivity condition $`\mathrm{\Lambda }_{\stackrel{~}{\omega }}F=0`$ is equivalent to the harmonicity condition $`F=0`$. As for untwisted harmonic $`(1,1)`$-forms one might ask for the harmonicity of the product $`F^m`$. Slightly less ambitious, one could ask whether the trace of this expression, an honnest differential form, is harmonic. This trace is, in fact, a scalar multiple of the Chern character $`ch_m(X,\stackrel{~}{\omega })`$.

Question. — Let $`(X,\stackrel{~}{\omega })`$ be a Ricci-flat Kähler manifold. Are the Chern forms $`ch_m(X,\stackrel{~}{\omega })`$ harmonic with respect to $`\stackrel{~}{\omega }`$ ?

By what was said about K3 surface we shall expect a negative answer to this question at least in this case:

Problem. — Let $`X`$ be a K3 surface with a hyperkähler form $`\stackrel{~}{\omega }`$. Let $`c_2A^2(X)`$ be the associated Chern form. Show that $`c_2`$ is not harmonic with respect to $`\stackrel{~}{\omega }`$ !

So, this should be seen in analogy to the fact that $`\alpha ^2`$ is not harmonic for any primitive harmonic $`(1,1)`$-form $`\alpha `$. Here, $`\alpha `$ is replaced by the curvatue $`F`$ and $`\alpha ^2`$ by $`trF^2`$. It is likely that the non-harmonicity of $`c_2`$ can be shown by standard methods in differential geometry, in particular by using the fact that $`c_2`$ is essentially $`F\stackrel{~}{\omega }^2`$ (see ), but I do not know how to do this.

Furthermore, it is not clear to me what the relation between the above question and the one treated in the previous sections is. I could imagine that the non-harmonicity of $`ch_m`$ in fact implies the existence of harmonic $`(1,1)`$-forms with non-harmonic top exterior power.

Acknowledgements. I wish to thank U. Semmelmann for his interest in this work and M. Lehn and D. Kaledin for making valuable comments on a first version of it. I am most grateful to Keiji Oguiso for its enthusiastic help with several arguments.