# The influence of correlated hopping on valence and metal-insulator transitions in the Falicov-Kimball model

## Abstract

The extrapolation of small-cluster exact-diagonalization calculations is used to examine the influence of correlated hopping on valence and metal-insulator transitions in the one-dimensional Falicov-Kimball model. It is shown that the ground-state phase diagram as well as the picture of valence and metal-insulator transitions found for the conventional Falicov-Kimball model (without correlated hopping) are strongly changed when the correlated hopping term is added. The effect of correlated hopping is so strong that it can induce the insulator-metal transition, even in the half-filled band case.

PACS nrs.:75.10.Lp, 71.27.+a, 71.28.+d, 71.30.+h

In the past decade, a considerable amount of effort has been devoted to understanding of the multitude of anomalous physical properties of rare-earth and transition-metal compounds. Recent theoretical works based on exact numerical and analytical calculations showed that many of these anomalous features, e.g., mixed valence phenomena, metal-insulator transitions, etc., can be describe very well within different versions of the Falicov-Kimball model (FKM) . For example, it was found that the spinless FKM, in the pressure induced case, can describe both types of intermediate-valence transitions observed experimentally in rare-earth compounds: a discontinuous insulator-insulator transition for sufficiently strong interactions  and a discontinuous insulator-metal transition for weak interactions . In addition, at nonzero temperatures this model is able to provide the qualitative explanation for anomalous large values of the specific heat coefficient and for extremely large changes of electrical conductivity  found in some intermediate-valence compounds (e.g., in SmB<sub>6</sub>). Moreover, very recently the spin-one-half version of the FKM has been used successfully for a description of a discontinuous intermediate-valence transition (accompanied by a discontinuous insulator-metal transition) in SmS  as well as for a description of an anomalous magnetic response of the Yb-based valence-fluctuating compounds .

These results show that the FKM could, in principle, yield the correct physics for describing rare-earth compounds. On the other hand it should be noted that the conventional FKM neglects all nonlocal interaction terms and thus it is questionable whether above mentioned results persist also in more realistic situations when nonlocal interactions will be turned on. An important nonlocal interaction term obvious absent in the conventional FKM is the term of correlated hopping in which the $`d`$-electron hopping amplitudes $`t_{ij}`$ between neighbouring lattice sites $`i`$ and $`j`$ depend explicitly on the occupancy $`(f_i^+f_i)`$ of the $`f`$-electron orbitals. To examine effects of this term on valence and metal-insulator transitions in the FKM we adopt here the following general form for the nearest-neighbour matrix elements

$$\stackrel{~}{t}_{ij}=t_{ij}+t_{ij}^{}(f_i^+f_i+f_j^+f_j),$$
(1)   
which represent a much more realistic type of electron hopping than the conventional hopping ($`t_{ij}=t`$ if $`i`$ and $`j`$ are the nearest neighbours, and zero otherwise).

Thus the spinless FKM in which the effects of correlated hopping are included can be written as

$$H=\underset{<ij>}{}t_{ij}d_i^+d_j+\underset{<ij>}{}t_{ij}^{}(f_i^+f_i+f_j^+f_j)d_i^+d_j+U\underset{i}{}f_i^+f_id_i^+d_i+E_f\underset{i}{}f_i^+f_i,$$
(2)   
where $`f_i^+`$, $`f_i`$ are the creation and annihilation operators for an electron in the localized state at lattice site $`i`$ with binding energy $`E_f`$ and $`d_i^+`$, $`d_i`$ are the creation and annihilation operators of the itinerant spinless electrons in the $`d`$-band Wannier state at site $`i`$.

The first term of (2) is the kinetic energy corresponding to quantum mechanical hopping of the itinerant $`d`$-electrons between the nearest-neighbour sites $`i`$ and $`j`$. The second term is just the correlated hopping term discussed above. The third term is the on-site Coulomb interaction between the $`d`$-band electrons with density $`n_d=\frac{1}{L}_id_i^+d_i`$ and the localized $`f`$-electrons with density $`n_f=\frac{1}{L}_iw_i`$, where $`L`$ is the number of lattice sites. The last term stands for the localized $`f`$ electrons whose sharp energy level is $`E_f`$.

Since in this spinless version of the FKM without hybridization the $`f`$-electron occupation number $`f_i^+f_i`$ of each site $`i`$ commutes with the Hamiltonian (2), the $`f`$-electron occupation number is a good quantum number, taking only two values: $`w_i=1`$ or 0, according to whether or not the site $`i`$ is occupied by the localized $`f`$ electron. Therefore the Hamiltonian (2) can be written as

$$H=\underset{<ij>}{}h_{ij}(w)d_i^+d_j+E_f\underset{i}{}w_i,$$
(3)   
where $`h_{ij}(w)=\stackrel{~}{t}_{ij}(w)+Uw_i\delta _{ij}`$ and

$$\stackrel{~}{t}_{ij}(w)=t_{ij}+t_{ij}^{}(w_i+w_j).$$
(4)   
Thus for a given $`f`$-electron configuration $`w=\{w_1,w_2\mathrm{}w_L\}`$ defined on a one-dimensional lattice with periodic boundary conditions, the Hamiltonian (2) is the second-quantized version of the single-particle Hamiltonian $`h(w)`$, so the investigation of the model (3) is reduced to the investigation of the spectrum of $`h`$ for different configurations of $`f`$ electrons. Since the $`d`$ electrons do not interact among themselves, the numerical calculations precede directly in the following steps (in the next we consider only the case $`N_f+N_d=L`$, which is the point of the special interest for the mixed-valence phenomena). (i) Having $`w=\{w_1,w_2\mathrm{}w_L\}`$, $`U`$, $`E_f`$ and the nearest-neighbour hopping amplitudes $`t`$ and $`t^{}`$ fixed, (in the following $`t=1`$ and all energies are measured in units of $`t`$) find all eigenvalues $`\lambda _k`$ of $`h(w)`$. (ii) For a given $`N_f=_iw_i`$ determine the ground-state energy $`E(w,U,E_f)=_{k=1}^{LN_f}\lambda _k+E_fN_f`$ of a particular $`f`$-electron configuration $`w`$ by filling in the lowest $`N_d=LN_f`$ one-electron levels. (iii) Find the $`w^0`$ for which $`E(w,U,E_f)`$ has a minimum. Repeating this procedure for different values of $`U,t^{}`$ and $`E_f`$, one can study directly the the ground-state phase diagram and valence transitions (a dependence of the $`f`$-electron occupation number on the $`f`$-level position $`E_f`$) in the FKM with correlated hopping.

The most interesting question that arises for the FKM with correlated hopping is whether the correlated hopping term can change the ground state phase diagram and the picture of valence and metal-insulator transitions found for the conventional FKM ($`t=1`$ and $`t^{}=0`$). The nature of the ground state, its energetic and structural properties and the correlation-induced metal-insulator transitions are subjects of special interest. For the conventional FKM these problems are well understood at least at half-filling ($`E_f=0,n_f=n_d=1/2`$). In this case the localized $`f`$-electrons fill up one of two sublattices of the hypercubic lattice (the charge density wave state) and the corresponding ground state is insulating for all $`U>0`$. Thus, for the finite interaction strength there is no correlation-induced metal-insulator transition in the half-filled band case. Outside half-filling the situation is more complicated since there exist the analytical results only for a restricted class of configurations  and exact-numerical results are limited to small finite clusters . In spite of these restrictions both analytical and numerical results yield the same ground-state phase diagram which consists of only two main domains: the domain of the phase separation and the domain of the most homogeneous configurations. The domain of the phase separation is restricted to a small region of low $`f`$-electron concentrations ($`n_f<1/4`$) and weak Coulomb interactions ($`U<1.2`$). In this domain the ground state are incoherent (metallic) mixtures  of the empty configuration (whose length $`l`$ is at least $`L/2`$) and a configuration $`w`$ (whose length is $`l<L/2`$). Outside this domain the ground states are the most homogeneous configurations, which are insulating for all $`f`$-electron concentrations. The boundary between these two domains is the boundary of correlation-induced metal-insulator transitions.

One can expect, on the base of simple arguments, that the ground-state phase diagram of the FKM with correlated hopping will be fully different from one discussed above for the conventional FKM. Indeed, the following selection of hopping matrix amplitudes $`t=1`$ and $`t^{}>0`$ may favor the segregated configuration $`\{11\mathrm{}100\mathrm{}0\}`$ since the itinerant $`d`$ electrons have the lower kinetic energy in this state. This mechanism could lead, for example, to the instability of the CDW state $`\{10\mathrm{}10\}`$ that is the ground state for $`t^{}=0`$ and thereby to a metal-insulator transition, even in the half-filled band case. To verify this conjecture we have performed an exhaustive study of the model on finite clusters (up to 32 sites) for a wide range of parameters $`t^{}`$ and $`U`$. The results of numerical calculations are summarized in Fig. 1 in the form of the $`t^{}`$-$`U`$ phase diagram. In addition to the alternating configuration $`w_1=\{10\mathrm{}10\}`$ that is the ground state at $`t^{}=0`$ for all nonzero $`U`$ we found two new phases that can be the ground states of the model, and namely, the alternating configuration $`w_2=\{1100\mathrm{}1100\}`$ with double period and the segregated configuration $`w_3=\{11\mathrm{}100\mathrm{}0\}`$. Thus at nonzero $`t^{}`$ the configuration $`w_1`$ becomes unstable against the transition to $`w_2`$ and $`w_3`$. The transition from $`w_1`$ to $`w_2`$ is the insulator-insulator transition since both $`w_1`$ and $`w_2`$ configurations have the finite gaps $`\mathrm{\Delta }`$ at the Fermi energy  for nonzero values of $`U`$ (see the inset in Fig. 1). On the other hand the segregated configuration $`w_3`$ is metallic ($`\mathrm{\Delta }=0`$) for all nonzero $`U`$ and so the transition from $`w_1`$ to $`w_3`$ (as well as from $`w_2`$ to $`w_3`$) is the insulator-metal transition. Thus we arrive to the very important conclusion, and namely, that the correlated hopping term can induce the insulator-metal transition, even in the half-filled band case.

The fact that the correlated hopping plays the important role in stabilizing the ground state indicates that the picture of valence and metal-insulator transitions found in our previous papers within the conventional FKM  could be dramatically changed if finite values of $`t^{}`$ will be considered. To verify this conjecture we have performed the study of the model for two representative values of $`U`$ ($`U=1.5`$ and $`U=4`$) and a selected set of $`t^{}`$ values. The results of numerical calculations obtained for $`U=1.5`$ on finite clusters (up to 32 sites) can be summarized as follows: (i) For sufficiently small values of $`t^{}`$ ($`t^{}0.3`$) the ground states are the most homogeneous configurations for all $`f`$-electron concentrations. (ii) For intermediate values of $`t^{}`$ ($`t^{}0.6`$) the ground states are the segregated configurations for $`n_f<0.5`$ and the most homogeneous configurations for $`n_f0.5`$. (iii) For large values of $`t^{}`$ ($`t^{}>0.8`$) the ground states are only the segregated configurations. Since no significant finite-size effects have been observed on clusters up to 32 sites we suppose that these results can be satisfactory extrapolated on large systems and used for a study of effects of correlated hopping on valence and metal-insulator transitions. Typical valence transitions obtained on the extrapolated set of configurations are presented in Fig. 2. For $`t^{}=0.3`$ the valence transition holds all characteristic features found in our previous papers for $`t^{}=0`$. The basic structure of the transition is formed by the most homogeneous configurations with the smallest periods ($`n_f=1/5,1/4,1/3,1/2,2/3,3/4,4/5`$). This primary structure is independent of $`L`$ while the secondary structure corresponding to remaining configurations strongly depends on $`L`$ and forms the gradual transition between two valence states from the primary structure. The correlated hopping term reduces considerably the width of the primary structure, especially for $`n_f0.5`$, but it does not change the nature of the ground state. The ground states for $`t^{}=0.3`$ are the most homogeneous configurations which are insulating (see the inset in Fig. 2) and thus there is no insulator-metal transition induced by external pressure for small values of $`t^{}`$. (It is generally supposed that in the pressure induced case $`E_f`$ is proportional to pressure.) From this point of view the situation looks more hopeful for intermediate values of $`t^{}`$. As was mentioned above for this case the ground states are the segregated (metallic) configurations (for $`n_f<0.5`$) and thus one could expect the pressure induced insulator-metal transition at $`E_f=E_c`$ (corresponding to $`n_f=n_c=0.5`$), of course if the segregated configurations persist as the ground states on some finite region of $`E_f`$ values. Fig. 2 illustrates that such a situation indeed becomes. For $`t^{}=0.6`$ the segregated configurations are the ground states in the wide region above $`E_c=0.02`$ and the valence transition in this region is continuous. Below $`E_c`$ the ground states are the most homogeneous (insulating) configurations. In this region the primary structure is practically fully suppressed and only the intermediate valence states with $`n_f=1/2`$ and $`n_f=2/3`$ have the finite regions of stability. At $`E_f=E_c`$ the FKM exhibits a discontinuous insulator-metal transition that is apparently induced by correlated hopping. This result shows how crucial role plays the correlated hopping in the mechanism of valence and insulator-metal transitions. Already relatively small values of $`t^{}`$ can fully destroy the picture of valence and metal-insulator transitions found for the conventional FKM and therefore the correlated hopping term cannot be neglected in the correct description of valence and metal-insulator transitions. Of course, for large values of $`t^{}`$ we can expect the largest deviations from $`t^{}=0`$ case, since the ground states in this region are only the segregated configurations which contrary to the most homogeneous configurations are metallic. The inset in Fig. 2 confirms this conjecture. The valence transitions for large values of $`t^{}`$ are only continuous and fully differ from $`t^{}=0`$ case.

In the strong coupling region ($`U=4`$) the ground states are either the most homogeneous configurations (for small and intermediate $`t^{}`$) or the segregated configurations (for large $`t^{}`$). Thus for small and intermediate values of $`t^{}`$ the strong coupling picture of valence and metal-insulator transitions will be the same as one for $`t^{}=0`$. All ground states are insulating and the valence transitions, for both conventional FKM and FKM with correlated hopping consist of a few discontinuous valence transitions which number is reduced with increasing $`U`$. Only one difference between valence transitions obtained within these two models is that the width of the valence transition in the FKM with correlated hopping is reduced due to finite $`t^{}`$. Fig. 3 illustrates that the effect is very strong even for relatively small values of $`t^{}`$. This indicates that the correlated hopping plays important role also in the strong coupling limit although unlike the weak-coupling limit now small values of $`t^{}`$ do not change qualitatively the picture of valence and metal-insulator transitions. In order to change qualitatively the picture of valence and metal-insulator transitions in the strong coupling limit, larger values of $`t^{}`$ should be considered. For example, we have found that for $`U=4`$ and $`t^{}=1.2`$ the ground states are the segregated (metallic) configurations for all $`f`$-electron concentrations and the corresponding valence transition is continuous.

The exactly opposite effect on valence transitions in the strong coupling limit has the correlated hopping term with negative values of $`t^{}`$. As shown in Fig. 4. the correlated hopping with $`t^{}<0`$ stabilizes the insulating intermediate-valence states corresponding to the most homogeneous configurations with the smallest periods (which are the ground states in this region) and this effect is very strong even for relatively small values of $`t^{}`$. This again leads to conclusion that the correlated hopping must be taken into account in the correct description of valence and metal-insulator transitions.

This work was supported by the Slovak Grant Agency VEGA under grant No. 2/4177/97. Numerical results were obtained using computational resources of the Computing Centre of the Slovak Academy of Sciences.

Figure Captions

Fig. $`1.`$ $`t^{}`$-$`U`$ phase diagram of the FKM with correlated hopping at half-filling ($`E_f=0,n_f=n_d=0.5`$). Three different phases correspond to the alternating configuration $`w_1=\{10\mathrm{}10\}`$, the alternating configuration $`w_2=\{1100\mathrm{}1100\}`$ with double period and the segregated configuration $`w_3=\{1\mathrm{}10\mathrm{}0\}`$. For $`L=24`$ the phase diagram has been obtained over the full set of $`f`$-electron configurations, while for $`L=600`$ only the restricted set of configurations $`w_1,w_2`$ and $`w_3`$ has been used to determine the phase boundaries. The inset shows $`t^{}`$-dependence of energy gaps corresponding to the ground state configurations for different values of $`U`$.

Fig. $`2.`$ Dependence of the $`f`$-electron occupation number $`n_f`$ on the $`f`$-level position $`E_f`$ for different values of correlated hopping $`t^{}`$ at $`U=1.5`$. The upper inset shows energy gaps corresponding to the most homogeneous configurations that are ground states for $`t^{}=0.3`$ (for all $`f`$-electron concentrations) and $`t^{}=0.6`$ (for $`n_f0.5`$). The lower inset shows examples of $`n_f(E_f)`$ behaviour for large values of $`t^{}`$.

Fig. $`3.`$ Dependence of the $`f`$-electron occupation number $`n_f`$ on the $`f`$-level position $`E_f`$ for different values of correlated hopping $`t^{}`$ at $`U=4`$. The inset shows energy gaps corresponding to the most homogeneous configurations that are ground states for all $`f`$-electron concentrations for $`t^{}=0.4`$ and $`U=4`$

Fig. $`4.`$ Dependence of the $`f`$-electron occupation number $`n_f`$ on the $`f`$-level position $`E_f`$ for different values of correlated hopping $`t^{}0`$ at $`U=4`$. The inset shows energy gaps corresponding to the most homogeneous configurations that are ground states for all $`f`$-electron concentrations for $`t^{}=0.2`$ and $`t^{}=0.4`$.