SITE DENSITY WAVES VS.

BOND DENSITY WAVES IN THE ONE-DIMENSIONAL IONIC HUBBARD MODEL IN THE HIGH IONICITY LIMIT
FLORIN D. BUZATU1,2, DANIELA BUZATU
2

Institute of Atomic Physics, Mgurele-Bucharest, 077125, Romania Dept. of Theoretical Physics, Horia Hulubei National Institute for Physics and Nuclear Engineering, Mgurele-Bucharest, 077125, Romania 3 Dept. of Physics, Politehnica University, Bucharest, 060040, Romania Received August 30, 2008

We consider a Hubbard chain with an energy difference between the odd and the even sites (ionicity). For a sufficiently large ionicity and electron concentrations less than half-filling, the system can be described by the one-band Hubbard model with a bond-site interaction. We investigate the competition between the density waves localized on sites and on bonds at different band fillings by solving an appropriate Bethe-Salpeter equation. Our results indicate the occurrence of the bond density waves at quarter-filling.

1. INTRODUCTION

The organic charge-transfer (CT) solids are of two types: (i) separate stacks, with donor (D) or acceptor (A) molecules; (ii) mixed stacks with alternating D and A molecules. The CT insulators, which are mixed stacks, are either neutral or ionic, depending on the size of the orbital overlap: neutral at small overlap and ionic at large overlap. Torrance et al. [1] discovered that by increasing the pressure on an organic CT compound, such as TTF-CA (tetrathiafulvalene-chloranil), it could pass from a neutral state to an ionic one, and the transition is reversible. The same effect was observed by decreasing the temperature, with the formation of a coexistence neutral-ionic region [2]. In order to explain the neutral-to-ionic transition, Hubbard and Torrance proposed a microscopic model for TTF - CA with alternating on-site energies [3]. Based on that model, Nagaosa and Takimoto introduced the ionic Hubbard model (IHM) [4]:

H IHM = t
j ,

( cj,c j+1, + H .c.) +

j ,

(1) j n j, + U
j

n j, n j, .

(1)

The first term in the Eq. (1) describes free one-dimensional (1D) electrons in the tight binding approximation, the second one introduces the alternating on-site
Rom. Journ. Phys., Vol. 53, Nos. 9 1 0 , P. 10451052, Bucharest, 2008

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Florin D. Buzatu, Daniela Buzatu

energies of the electrons, and the last one represents the on-site (Hubbard) interaction between the electrons. A slightly modified Hamiltonian was used to describe the displacive-type ferroelectric transition in ferroelectric transition metal oxides such as BaTiO3 [57]. At half-filling and U = 0 the system is obviously a band insulator (BI), characterized by the existence of a gap in both charge and spin excitations; for = 0, the model reduces to the 1D Hubbard model (HM) and at half-filling it is a Mott insulator (MI), with no gap in the spin excitations [8]. In the atomic limit (t 0), the transition is expected to occur at U 2 , a critical line separating two configurations: double-occupied (D) and empty (A) sites for U < 2 and single-occupied sites for U > 2. The interest for the 1D IHM has been renewed once with the work of Fabrizio, Gogolin, and Nersesyan [9], who proved that a two-step transition should take place at half-filling between the BI and MI phases, with the occurrence of an intermediate spontaneously dimerized insulator (SDI) phase. The SDI phase is like the BI phase (with gaps in both charge and spin excitations) in which a bond-charge-density-wave (BCDW)state occurs, with a
non-zero average value of the operator Di = (1)i

( ci,ci+1, + H .c.) .

By

increasing U from zero at half-filling, the transition between the BI and the SDI is given by the place where the charge gap vanishes (it opens again in the SDI phase) and Di takes some finite value; by increasing U further, the system undergoes the transition to the MI phase where both the spin gap and Di become (and remain) zero [9]. This scenario was confirmed by numerical studies [10] and exact results for an effective model [11]. It is worth mentioning that the occurrence of the BCDW phase is also predicted for the 1D extended Hubbard model (on-site and inter-site interactions) at half-filling [12, 13]. In the present work we investigate the competition between the site density waves (charge CDW, spin SDW) and the bond density waves (charge BCDW, spin BSDW) in the ground-state of the 1D IHM at high ionicities (| U |< 2 , t 2 / 2 1) and for electron densities less than half-filling.
2. EFFECTIVE MODEL AT HIGH IONICITIES

It was shown in the Ref. [14] that the Hamiltonian composed of the first two terms in the Eq. (1)

H 0 = 2t
k ,

cos ak e iak / 2 ak , bk , + H .c. + 2

k ,

( ak, ak, bk, bk , ) ,

(2)

where the Fermi operators in the Bloch representation a(b) correspond to the even (odd) lattice sites, can be easily diagonalized by the following canonical transformation:

One-dimensional ionic Hubbard model

1047

(3)

with

A(k ) = 1 1 + ( k ) 2 B( k ) = 1 1 ( k ) 2 and

1 2

1 2

(4)

( k ) = 2 + 4t 2 cos2 (ak / 2) .

(5)

The result is a two-band model and the last term in the Eq. (1) introduces both intra-band and inter-band electron-electron interactions. In the high ionicity limit | U |< 2, t 2 / 2 1 (6)

and for electron concentrations less than half-filling, it was also shown in the Ref. [14] that we can restrict the considerations to a one-band model with the same dispersion law as for free electrons in an usual non-alternating chain

(k ) 2 t cos(ak ), and the following two-particle interaction

2 t t 2

(7)

V1 ( k1 ,.., k4 ) U + 4 X [ cos(ak1 ) + cos(ak3 )] with

(8)

(9)

In the high ionicity regime and below half-filling, the 1D IHM can be thus approximated by a one-band model with a narrower bandwidth, a reduced onsite interaction, and a small bond-site coupling term proportional to the on-site interaction and with opposite sign. The model is know as the 1D (t, U, X)-model [15] and it is relevant to quasi-1D materials with large bandwidth like conducting polymers. The ground-state instabilities (charge and spin density waves, singlet superconductivity) of the 1D (t, U, X)-model have been analyzed in a mean-field-like approach in the Ref. [16].

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Florin D. Buzatu, Daniela Buzatu 3. SITE DENSITY WAVES VS. BOND DENSITY WAVES

In investigating the competition between the site and the bond density waves in the 1D IHM, we use the same method applied to determine the groundstate phase diagrams of the 1D (t, U, X)-model [16] and 1D Penson-KolbHubbard model [17]. Without going into details, the recipe is the following: (i) start with the Bethe-Salpeter equation in the particle-hole channel in the simplest approximation; (ii) find the solution (K, ); (iii) fix the total momentum K = 2 k F ; (iv) take of the form Eexc + T with the excitation

energy Eexc = 0; (v) find Tc corresponding to the poles of (Tc1 giving the relaxation time of the unstable ground-state); (vi) determine the regions where the instabilities can occur from the well-behavior condition Tc 0 at no-interaction; (vii) find the dominant instability in the new ground-state, i.e., that one with the shortest relaxation time. The method amounts to a mean-fieldtype approach to the ground state instabilities for 1D Hubbard-like models. In the case of an alternating chain, the relevant operators in investigating the occurrence of the density wave instabilities are (we use the notation DW for the site density waves and BDW for the bond density waves):
DW ( j, t )

a, (t )a j, (t ) b, (t )b j, (t ) j j H .c. b, (t )a j +1, (t ) + H .c. j

(10)

BDW ( j, t )

{a

j , (t )b j , (t ) +

(11)

where
ci, c j, ci, c j, ci, c j, , = 1 charge sector +1 spin sector (K , t )
( K , 0)

(12) ; in

We look now for the poles of the response function the high ionicity limit,

(K , t )

( K , 0)

1 N

V2 (k , k ; K )
k ,k ck K / 2, (t )ck + K / 2, (t )ck K / 2, (0)ck + K / 2, (0) ,

(13)

where V2 is the potential generated by the site/bond response function and has the form
2 VDW (k , k ; K ) = 1 t 2 sin(aK / 2) 2 cos(aK / 2) + cos ak + cos ak 2

(14)

One-dimensional ionic Hubbard model

1049

for the site density waves, or

(15)

for the bond density waves. When t/ 0, VDW 1 and VBDW 0, as for a regular (non-alternating) chain. The approximate Bethe-Salpeter equation for the investigated instabilities has the following form:
(k , k ; K , ) = i V ( k , k ; K ) + 2 with V (k , k ; K ) = V1 (k , k ; K )V2 (k , k ; K ). (17) V1 in the Eq. (17) is given by the Eq. (8) but in the new variables k = k1 + K / 2 and k = k3 + K / 2 : V1 ( k , k ; K ) = U + 4 X cos( aK / 2) ( cos ak + cos ak ) , V2 is either VDW or VBDW from above, and ( k ; K , ) = i 2
+

V (k , k ; K )G (k ; K , )(k , k ; K , )
k

(16)

(18)

(k ; K , ) has the form

dG 0 k + K , + G 0 k K , . 2 2 2 2

) (

(19)

In the second order of t/ , the potential V given by the Eq. (17) becomes V (k , k ; K ) where
2 U ( K ) U 1 t 2 (2 + sin aK ) 2 2 X ( K ) U t 2 [sin(aK / 2) + cos(aK / 2)] 8

U ( K ) + 4 X ( K ) ( cos ak + cos ak ) , DW 4t 2 U sin 2 ( aK / 2) cos ak cos ak , 2 BDW

(20)

(21) (22)

The approximate Bethe-Salpeter equation (16) ca be solved exactly. The poles of are given by the zeros of
2 1 + c0 U + 8c1 X + 16(c1 c0 c2 ) X2 , DW t t t D ( K , ) = U c sin 2 (aK / 2), 8 BDW 2 2

(23)

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Florin D. Buzatu, Daniela Buzatu

where

cn ( K , ) t N

cos j ak (k ; K , ),
k

n = 0, 1, 2

(24)

can be calculated by elementary integrations. For T :

0 T
2

(25)

DW (26) BDW

ln | cos ak F | U 2 = + 1 sin ak F 1 + (1 + sin 2ak F ) , DW 4 2 2 sin 2 ak F 4 U sin 2 ak F ,

(27)

BDW

(28)

gF = ( 2 sin ak F ) ,

(29)

gF / t being the density of states at the Fermi level. The transition to an ordered state occurs for / < 0 at
Tc =| 0 | exp gF (30)

which has the same form as the BCS critical temperature. The competition between the site and bond density waves for the 1D IHM in the high ionicity regime can be visualized in the phase diagram from Fig. 1. In the validity range of the used approximations, at half-filling (akF = ) only site density waves occur. Going away from half-filling, the bond density waves also occur but the site density waves are still dominant. By decreasing the density further, the bond density waves become dominant in an increasing area and, approaching the quarter-filling, a separation | U | / -line appears between the

One-dimensional ionic Hubbard model

1051

site and the bond spin (charge) density waves for U > 0 (U < 0). At exactly quarter-filling, only bond density waves occur in the ground-state of the system. It can be also remarked in Fig. 1 the spin-charge symmetry of the phase diagram when U changes its sign.

Fig. 1 Site density waves vs. bond density waves for the 1D IHM at high ionicities.

In conclusion, our results show that, for the 1D IHM in the high ionicity limit, the bond density waves are likely to occur for a quarter-filled band. Although the 1D IHM was much less investigated away from half-filling, some interesting properties have been reported in this case [18, 19].
Acknowledgments. This work was supported by the Romanian research project CERES C4-163.

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Florin D. Buzatu, Daniela Buzatu REFERENCES

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