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# Interaction energy functional for lattice density functional theory: Applications to one-, two- and three-dimensional Hubbard models

## I  Introduction

Density functional theory (DFT) provides a rigorous framework for studying the physics of the many-body problem.hk ; ks ; parr-book ; gross-book  The fundamental concept behind DFT is to replace the conventional dynamical variables that completely define a many-particle state (e.g., the wave function in a quantum mechanical problem, or the particle positions and momenta in a classical system) by considering the particle-density distribution $`\rho (\stackrel{}{r})`$ as the basic variable. For this purpose the energy $`E`$ of the system is expressed as a functional of $`\rho (\stackrel{}{r})`$ separating the various energy terms in two main groups. The first one contains the contributions that depend explicitly on the problem under study, which result from the coupling between $`\rho (\stackrel{}{r})`$ and the external fields $`V_{ext}(\stackrel{}{r})`$. The second one concerns the intrinsic energy of the many-particle system, namely, the kinetic energy $`T`$ and the interaction energy $`W`$ of the particles. These terms are universal functionals of $`\rho (\stackrel{}{r})`$ in the sense that they are independent of the problem under study. While the general functional dependence of $`T[\rho ]`$ and $`W[\rho ]`$ is not known explicitly, they can be formally expressed as the result of integrating out the microscopic degrees of freedom. In the case of ground-state electronic properties, this is achieved by imposing that $`T[\rho ]`$ and $`W[\rho ]`$ correspond to the minimum possible value of $`T+W`$ for a given $`\rho (\stackrel{}{r})`$.parr-book ; gross-book ; levy  These basic notions have general validity and are therefore relevant to a wide variety of situations which may have very different physical origins.

In the present paper the concepts of DFT are applied to investigate the physics of strongly correlated electrons in a narrow energy band. The theoretical description of these systems is usually based on lattice Hamiltonians such as Anderson,andmod  Hubbard,hub  Pariser-Parr-Pople,ppp  and related models which focus on the most relevant electron dynamics at low energies.mb-books ; dagotto ; georges ; imada  The study of many-body lattice models in the framework of DFT seems particularly interesting from various perspectives. On the one side, a detailed understanding of the electronic properties in the strongly correlated limit constitutes an important theoretical challenge. Exact results are rare or numerically very demanding and a variety of elaborate many-body techniques are specifically developed for their study. Therefore, a density functional approach with an appropriate ansatz for $`W`$ should be a useful alternative tool for investigating at least some aspects of this complex problem. On the other side, one would like to extend the range of applicability of DFT to strongly correlated phenomena, like the separation of charge and spin degrees of freedom or the correlation induced localization, where conventional local density approximations (LDAs) or generalized gradient approximations (GGAs) are known to fail systematically. Moreover, the development of DFT on a lattice constitutes an intrinsically inhomogeneous approach, which provides a true alternative to methods relying on the homogeneous electron gas. In this context, investigations on many-body models should open new insights into the properties of the interaction-energy functional that could also be useful for future extensions to more realistic Hamiltonians and first principles calculations.

In past years, a number of density functional studies of lattice models have performed concerning in particular the determination of band-gaps in semiconductors,gunn  the role of off-diagonal elements of the density matrix and the non-interacting $`v`$ representability in strongly correlated systems,godby  or the development of energy functionals of the density matrix with applications to Hubbard and Anderson models.carl  In previous papers we have formulated a lattice density functional theory (LDFT) of many-body models by considering the density matrix $`\gamma _{ij}`$ with respect to the lattice sites $`i`$ and $`j`$ as the fundamental variable.ldftxcfun ; ldftscfer ; ldftdim1D  The interaction energy $`W`$ of the Hubbard model has been calculated exactly as a function of $`\gamma _{ij}`$ for various periodic lattices having $`\gamma _{ij}=\gamma _{12}`$ for nearest neighbors (NNs) $`i`$ and $`j`$. On this basis, a simple general approximation to $`W(\gamma _{12})`$ has been proposed which derives from exact dimer results, the scaling properties of $`W`$, and known limits. Using this ansatz, several ground-state properties of one-dimensional (1D) and two-dimensional (2D) systems have been obtained in good agreement with available exact solutions and accurate numerical calculations.ldftscfer  In addition, applications to dimerized chains provided us with systematic results for the ground-state energy and charge excitation gap of the 1D Hubbard model as a function of hopping alternation and Coulomb repulsion, including the crossover from weak to strong correlations.ldftdim1D  LDFT appears therefore as an efficient method of determining the electronic properties of many-body lattice models, thus encouraging further developments and applications.

The main purpose of this paper is to present a new approximation to the interaction-energy functional $`W[\gamma ]`$ of the Hubbard Hamiltonian and to apply it to determine several electronic properties of this model in the framework of LDFT. In Sec. II the basic formulation of LDFT is briefly reviewed. Different approximations to interaction-energy functional are presented and discussed in Sec. III. First, we analyze the properties of a previously proposed dimer ansatzldftscfer  and discuss its goals and limitations by comparison with known exact results. Some shortcomings of this functional in the limit of strong correlations at half-band filling are pointed out. In order to overcome them, we propose a new approximation based on the scaling properties of $`W`$, which recovers the correct behavior in the limit of strong interactions. In this way a more accurate description of the dependence on $`\gamma _{ij}`$ in different dimensions and lattice structures is obtained. The following sections are mainly concerned with applications to 1D, 2D and 3D Hubbard models. Results for the ground-state energy, charge-excitation gap, and charge susceptibility are presented in Secs. IV, V, and VI, respectively. Comparison is made with the simpler dimer ansatz and with exact analytical or numerical solutions, whenever available, in order quantify the accuracy of the different approximations. Finally, Sec. VII summarizes the conclusions and points out some perspectives of future developments.

## II  Density-functional theory of lattice models

In order to be explicit we focus on the Hubbard model which is expected to capture the main physics of lattice fermions in a narrow energy band. The Hamiltonianhub

$$H=\underset{i,j\sigma }{}t_{ij}\widehat{c}_{i\sigma }^{}\widehat{c}_{j\sigma }+U\underset{i}{}\widehat{n}_i\widehat{n}_i,$$
(1)
includes nearest neighbor (NN) hoppings $`t_{ij}`$, and on-site interactions given by $`U`$ ($`\widehat{n}_{i\sigma }=\widehat{c}_{i\sigma }^{}\widehat{c}_{i\sigma }`$). The hopping integrals $`t_{ij}`$ are defined by the lattice structure and by the range of the single-particle hybridizations (typically, $`t_{ij}=t<0`$ for NN $`ij`$). They specify the system under study and thus play the role given in conventional DFT to the external potential $`V_{ext}(\stackrel{}{r})`$. Consequently, the basic variable in LDFT is the single-particle density matrix $`\gamma _{ij}`$. The situation is similar to the density-matrix functional theory proposed by Gilbert for the study of nonlocal pseudopotentials,gilb  since the hoppings are nonlocal in the sites. A formulation of DFT on a lattice in terms of the diagonal $`\gamma _{ii}`$ alone is possible only if one restricts oneself to models with constant $`t_{ij}`$ for $`ij`$. In this case the functional $`W[\gamma _{ii}]`$ depends on the values of $`t_{ij}`$ for $`ij`$ and in particular on $`U/t`$.gunn

The ground-state energy $`E_{gs}`$ and density-matrix $`\gamma _{ij}^{gs}`$ are determined by minimizing the energy functional

$$E[\gamma ]=E_K[\gamma ]+W[\gamma ]$$
(2)
with respect to $`\gamma _{ij}`$. $`E[\gamma ]`$ is defined for all density matrices that derive from a physical state, i.e., that can be written as

$$\gamma _{ij}=\underset{\sigma }{}\gamma _{ij\sigma }=\underset{\sigma }{}\mathrm{\Psi }|\widehat{c}_{i\sigma }^{}\widehat{c}_{j\sigma }|\mathrm{\Psi },$$
(3)
where $`|\mathrm{\Psi }`$ is an $`N`$-particle state. Such $`\gamma _{ij}`$ are said to be pure-state $`N`$-representable. An extension of the definition domain of $`E`$ to ensemble-representable density matrices $`\mathrm{\Gamma }_{ij}`$ is straightforward following the work by Valone.val ; foot\_ens  The first term in Eq. (2) is the kinetic energy associated with the electronic motion in the lattice. It is given by

$$E_K[\gamma ]=\underset{ij}{}t_{ij}\gamma _{ij},$$
(4)
thus including all single-particle contributions. The second term is the interaction-energy functional given bylevy

$$W[\gamma ]=\underset{\mathrm{\Psi }\gamma }{\mathrm{min}}\left[U\underset{i}{}\mathrm{\Psi }[\gamma ]|\widehat{n}_i\widehat{n}_i|\mathrm{\Psi }[\gamma ]\right],$$
(5)
where the minimization runs over all $`N`$-particles states $`|\mathrm{\Psi }[\gamma ]`$ that satisfy

$$\mathrm{\Psi }[\gamma ]|\underset{\sigma }{}\widehat{c}_{i\sigma }^{}\widehat{c}_{j\sigma }|\mathrm{\Psi }[\gamma ]=\gamma _{ij}$$
(6)
for all $`i`$ and $`j`$. $`W[\gamma ]`$ represents the minimum value of the interaction energy compatible with a given density matrix $`\gamma _{ij}`$. It is a universal functional of $`\gamma _{ij}`$ in the sense that it is independent of $`t_{ij}`$, i.e., of the system under study. However, $`W`$ depends on the number of electrons $`N_e`$, on the structure of the many-body Hilbert space, as given by $`N_e`$ and the number of orbitals or sites $`N_a`$, and on the form of the model interactions.foot\_gen

$`E[\gamma ]`$ is minimized by expressing

$$\gamma _{ij}=\underset{\sigma }{}\gamma _{ij\sigma }=\underset{k\sigma }{}u_{ik\sigma }\eta _{k\sigma }u_{jk\sigma }^{}$$
(7)
in terms of the eigenvalues $`\eta _{k\sigma }`$ (occupation numbers) and eigenvectors $`u_{ik\sigma }`$ (natural orbitals) of $`\gamma _{ij\sigma }`$. Lagrange multipliers $`\mu `$ and $`\lambda _{k\sigma }`$ ($`\epsilon _{k\sigma }=\lambda _{k\sigma }/\eta _{k\sigma }`$) are introduced in order to impose the constraints $`_{k\sigma }\eta _{k\sigma }=N_e`$ and $`_i|u_{ik\sigma }|^2=1`$. Deriving with respect to $`u_{jk\sigma }^{}`$ and $`\eta _{k\sigma }`$ ($`0\eta _{k\sigma }1`$), one obtains the eigenvalue equationsldftscfer ; gilb

$$\underset{i}{}\left(t_{ij}+\frac{W}{\gamma _{ij\sigma }}\right)u_{ik\sigma }=\epsilon _{k\sigma }u_{jk\sigma },$$
(8)
with the subsidiary conditions $`\epsilon _{k\sigma }<\mu `$ if $`\eta _{k\sigma }=1`$, $`\epsilon _{k\sigma }=\mu `$ if $`0<\eta _{k\sigma }<1`$, and $`\epsilon _{k\sigma }>\mu `$ if $`\eta _{k\sigma }=0`$. Self-consistency is implied by the dependence of $`W/\gamma _{ij\sigma }`$ on $`\eta _{k\sigma }`$ and $`u_{ik\sigma }`$. This formulation is analogous to density-matrix functional theory in the continuum.gilb  However, it differs from KS-like approaches which assume non-interacting $`v`$-representability and where only integer occupations are allowed.gunn ; godby  In the present case, the fractional occupations of natural-orbitals play a central role. One may in fact show that in general $`0<\eta _{k\sigma }<1`$ for all $`k\sigma `$. Exceptions are found in very special situations like the uncorrelated limit ($`U=0`$) or the fully-polarized ferromagnetic state in the Hubbard model ($`S_z=\mathrm{min}\{N_e,2N_aN_e\}/2`$). This can be understood from perturbation-theory arguments —none of the $`\eta _{k\sigma }`$ is a good quantum number for $`U0`$— and is explicitly verified by exact solutions of the Hubbard Hamiltonian on finite systems or the 1D chain.lieb-wu  Therefore, all $`\epsilon _{k\sigma }`$ in Eq. (8) must be degenerate and consequently the ground-state density matrix satisfies

$$t_{ij}+\frac{W}{\gamma _{ij\sigma }}=\delta _{ij}\mu .$$
(9)
Notice the importance of the dependence of $`W`$ on the off-diagonal density-matrix elements $`\gamma _{ij}`$ which measure the degree of electron localization. Approximations of $`W`$ in terms of the diagonal $`\gamma _{ii}`$ alone are not applicable in this framework ($`t_{ij}0`$ for NN $`ij`$). Eq. (9) provides a self-consistent scheme to obtain the ground-state $`\gamma _{ij}^{gs}`$ according to the variational principle. In the following section we present and discuss simple explicit approximations to $`W[\gamma ]`$ that are intended to describe the electronic properties of the Hubbard model in different interaction regimes, band-fillings, and lattice structures.

## III  Interaction-energy functional in the Hubbard model

The general functional $`W[\gamma ]`$, valid for all lattice structures and for all types of hybridizations, can be simplified at the expense of universality if the hopping integrals are short ranged. For example, if only NN hoppings are considered, the kinetic energy $`E_K`$ is independent of the density-matrix elements between sites that are not NNs. Therefore, the constrained search in Eq. (5) may be restricted to the $`|\mathrm{\Psi }[\gamma ]`$ that satisfy Eq. (6) only for $`i=j`$ and for NN $`ij`$. This reduces significantly the number of variables in $`W[\gamma ]`$ and renders the determination and interpretation of the functional dependence far simpler. In particular for periodic lattices the ground-state $`\gamma _{ij}^{gs}`$ is translational invariant. Therefore, in order to determine $`E_{gs}`$ and $`\gamma _{ij}^{gs}`$, one may set $`\gamma _{ii}=n=N_e/N_a`$ for all sites $`i`$, and $`\gamma _{ij}=\gamma _{12}`$ for all NN pairs $`ij`$. In this case the interaction energy can be regarded as a simple function $`W(\gamma _{12})`$ of the density-matrix element between NNs. This is certainly a great practical advantage. However, it should be noted that restricting the minimization constraints in Eqs. (5) and (6) to NN $`\gamma _{ij}`$ also implies that $`W`$ loses its universal character, since the NN map and the resulting dependence of $`W`$ on $`\gamma _{12}`$ are in principle different for different lattice structures.

The difficulties introduced by the lack of universality can be overcome by taking advantage of the scaling properties $`W(\gamma _{12})`$. Recent numerical studiesldftxcfun  have in fact shown that $`W`$ is nearly independent of system size $`N_a`$, band filling $`n=N_e/N_a`$ and lattice structure, if W is measured in units of the Hartree-Fock energy $`E_{\mathrm{HF}}=Un^2/4`$ and if $`\gamma _{12}`$ is scaled within the relevant domain of representability $`[\gamma _{12}^{\mathrm{}},\gamma _{12}^0]`$. Here, $`\gamma _{12}^0`$ stands for the largest possible value of the NN bond order $`\gamma _{12}`$ for a given $`N_a`$, $`n`$, and lattice structure. It represents the maximum degree of electron delocalization and corresponds to the uncorrelated limit. On the other side, $`\gamma _{12}^{\mathrm{}}`$ refers to the strongly correlated limit of $`\gamma _{12}`$, i.e., to the largest NN bond order that can be obtained under the constraint of vanishing $`W`$. For half-band filling $`\gamma _{12}^{\mathrm{}}=0`$, while for $`n1`$, $`\gamma _{12}^{\mathrm{}}>0`$.nonbip  Physically, the possibility of scaling the interaction energy means that the relative change in $`W`$ associated to a given change in the degree of electron localization $`g_{12}=(\gamma _{12}\gamma _{12}^{\mathrm{}})/(\gamma _{12}^0\gamma _{12}^{\mathrm{}})`$ can be regarded as nearly independent of the system under study. This pseudo-universal behavior of $`W/E_{\mathrm{HF}}`$ as a function of $`g_{12}`$ can be exploited to obtain good general approximations to $`W(\gamma _{12})`$ by applying such a scaling to the functional dependence derived from a simple reference system or from known limits.

In a previous paper we have proposed an approximation to the interaction energy $`W`$ of the Hubbard model by extracting the functional dependence from the exact result for the Hubbard dimer, which is given byldftscfer

$$W^{(2)}=E_{\mathrm{HF}}\left(1\sqrt{1g_{12}^2}\right).$$
(10)
This very simple expression satisfies several general properties of the exact $`W(\gamma _{12})`$:
(i) For $`\gamma _{12}=\gamma _{12}^0`$, $`W^{(2)}=E_{\mathrm{HF}}`$ since the underlying electronic state $`\mathrm{\Psi }[\gamma _{12}^0]`$ is a single Slater determinant. Moreover, one observes that $`W^{(2)}/\gamma _{12}=\mathrm{}`$ for $`\gamma _{12}=\gamma _{12}^0`$. This is a necessary condition in order that $`\gamma _{12}^{gs}<\gamma _{12}^0`$ already for arbitrary small $`U/t0`$, as expected from perturbation theory.
(ii) $`W^{(2)}(\gamma _{12})`$ decreases monotonously with decreasing $`\gamma _{12}`$ reaching its lowest possible value, $`W=0`$, for $`\gamma _{12}=\gamma _{12}^{\mathrm{}}`$. In other words, a reduction of the interaction energy is obtained at the expense of electron delocalization.
(iii) In the strongly correlated limit ($`\gamma _{12}\gamma _{12}^0`$) one observes that $`W^{(2)}\gamma _{12}^2`$. Therefore, for $`U/t1`$, $`\gamma ^{gs}t/U`$ and $`E_{gs}t^2/U`$, a well known result in the Heisenberg limit of the half-filled Hubbard model.mb-books
A correct description of these basic properties and of the dependence of $`W/E_{HF}`$ on $`g_{12}`$ are at the origin of the remarkable performance of this simple dimer ansatz in the description of several ground-state properties of the Hubbard model.ldftscfer

In order to discuss the strongly correlated limit of Eq. (10) in more detail we expand $`W^{(2)}`$ to lowest order in $`\gamma _{12}`$. At half-band filling one obtains

$$W^{(2)}=(1/8)\alpha _2U\gamma _{12}^2+𝒪(\gamma _{12}^4)$$
(11)
with $`\alpha _2=(\gamma _{12}^0)^2`$. The exact interaction-energy $`W_{ex}`$ is also proportional to $`U\gamma _{12}^2`$ in the limit of small $`\gamma _{12}`$. Therefore, $`W_{ex}`$ can be expanded in the same form as Eq. (11) but with a somewhat different coefficient $`\alpha _{ex}`$. Notice that in the case of the Hubbard dimer, we have $`\gamma _{12}^0=1`$ and $`\alpha _2^{dim}=1`$, which coincides of course with the exact result. Considering for example the 1D chain, the 2D square lattice, and the 3D simple-cubic lattice one finds that the leading coefficients resulting from Eq. (10) are $`\alpha _2^{1D}=(\pi /2)^22.47`$, $`\alpha _2^{2D}=6.09`$, and $`\alpha _2^{3D}=9.30`$. These can be compared with the corresponding exact result derived from the Bethe-ansatz solution of the 1D Hubbard chain,lieb-wu  or with perturbation-theory calculations for the square and simple-cubic lattices,taka  which are given by $`\alpha _{ex}^{1D}=2/\mathrm{ln}22.89`$, $`\alpha _{ex}^{2D}=6.91`$, and $`\alpha _{ex}^{3D}=10.94`$. One observes that Eq. (10) reproduces correctly the trends in $`\alpha `$ with increasing dimensions. However, there is also a systematic underestimation of the interaction energy of the order of $`12`$$`15`$%. These quantitative discrepancies have direct consequences on the predicted properties, since the behavior of $`W`$ for small $`\gamma _{12}`$ determines the ground-state density matrix $`\gamma _{12}^{gs}`$ and energy $`E_{gs}`$ in the strongly correlated limit. In fact, approximating $`W`$ as in Eq. (11), writing the kinetic energy as $`E_K=zt\gamma _{12}`$, where $`z`$ is the coordination number, and using Eq. (9), one obtains $`\gamma _{12}^{gs}=(4z/\alpha )(t/U)`$ and $`E_{gs}=(2z^2/\alpha )(t^2/U)`$. Thus, an inaccuracy in $`\alpha `$ results in a similar relative error in $`\gamma _{12}^{gs}`$ and $`E_{gs}`$ for $`U/t1`$.

To overcome these shortcomings more flexible approximations to the interaction-energy functional are needed, which allow one to go beyond Eq. (10). Therefore, we propose a general ansatz of the form

$$W^{(n)}=E_{\mathrm{HF}}\left(1\sqrt{P_n(g_{12})}\right),$$
(12)
where $`P_n(g_{12})`$ is a function of $`g_{12}=(\gamma _{12}\gamma _{12}^{\mathrm{}})/(\gamma _{12}^0\gamma _{12}^{\mathrm{}})`$, thus incorporating the scaling properties of $`W`$ without loss of generality. $`P_n(g_{12})`$ is approximated by an $`n`$-order polynomial $`P_n(g_{12})=_{k=0}^na_kg_{12}^k`$. This is justified by the fact that $`(WE_{HF})^2`$ is in general a well-behaved function of $`g_{12}`$, even in the uncorrelated limit where $`W/\gamma _{12}`$ diverges ($`g_{12}=1`$). The coefficients $`a_k`$ are to be determined from known properties of $`W`$. First of all, one observes that at half-band filling, and for bipartite lattices in general, the sign of $`\gamma _{12}`$ can be changed without altering $`W`$. Thus, $`P_n(g_{12})`$ is an even function of $`g_{12}`$ and $`a_k=0`$ for odd $`k`$ ($`\gamma _{12}^0=\gamma _{12}^{0+}`$ and $`\gamma _{12}^{\mathrm{}}=\gamma _{12}^\mathrm{}+`$). In non-bipartite lattices away from half-band filling one may also set for simplicity $`a_k=0`$ for odd $`k`$, since the dependence on $`g_{12}`$ is very similar for positive and negative $`\gamma _{12}`$, once the different domains of representability are scaled.ldftxcfun ; nonbip

The uncorrelated and fully-correlated limits of $`W`$ ($`W=E_{HF}`$ for $`g_{12}=1`$, and $`W=0`$ for $`g_{12}=0`$) impose two simple conditions on the $`a_k`$, namely, $`P_n(1)=_ka_k=0`$ and $`P_n(0)=a_0=1`$. This defines the second-order approximation $`W^{(2)}`$ completely. In this case, $`P_2(g_{12})=1g_{12}^2`$, which coincides with the above discussed dimer ansatz \[Eq. (10)\]. The two approaches are therefore consistent. The dimer ansatz can be regarded as the simplest polynomial-based approximation of $`W`$, as given by Eq. (12), that satisfies the obvious limits.

The 4th-order approximation $`W^{(4)}`$ introduces the aimed additional flexibility that can be exploited to reproduce the strongly correlated limit of $`W`$ exactly. Expanding Eq. (12) to second-order in $`\gamma _{12}`$ one observes that at half-band filling this is achieved when $`a_0=1`$, $`a_2=\alpha _{ex}(\gamma _{12}^0)^2=\alpha _{ex}/\alpha _2`$, and $`a_4=(a_0+a_2)`$. Thus, the 4th-order approximation to $`W`$ is given by

$$W^{(4)}=E_{\mathrm{HF}}\left(1\sqrt{1\kappa g_{12}^2+(\kappa 1)g_{12}^4}\right),$$
(13)
where $`\kappa =\alpha _{ex}/\alpha _2>0`$ is the ratio between the small-$`\gamma _{12}`$ expansion coefficients of $`W^{ex}`$ and $`W^{(2)}`$. The value of $`\kappa `$ depends on the lattice structure or system dimensions. At half-band filling it can be determined by applying perturbation-theory to the Heisenberg limit of the Hubbard model.taka  For instance, for the 1D chain, 2D square lattice, and 3D simple-cubic lattice one obtains, respectively, $`\kappa _{1D}=8/(\pi ^2\mathrm{ln}2)=1.169`$, $`\kappa _{2D}=1.135`$, and $`\kappa _{3D}=1.176`$. Notice that $`\kappa `$ depends rather weakly on the lattice structure and that it is not very far from the dimer value $`\kappa =1`$, for which Eq. (13) reduces to Eq. (10). Therefore, the 4th-order term appears as a relatively small correction to the 2nd-order approximation. Higher-order polynomial approximations to $`W`$ could be derived in an analogous way, provided that reliable information is available on the following terms of the small-$`\gamma _{ij}`$ expansion of $`W^{ex}`$. This gives the possibility of further improving the accuracy of the results by incorporating a more detailed description of the strongly correlated limit.

In Fig. 1 the approximate interaction energies $`W^{(2)}`$ and $`W^{(4)}`$ of the half-filled 1D Hubbard chain are compared with the corresponding exact result $`W_{ex}`$, as derived from the Bethe-Ansatz solution.lieb-wu  As already observed,ldftscfer  even the simplest dimer ansatz $`W^{(2)}`$ follows $`W_{ex}(\gamma _{12})`$ quite closely all along the crossover from weak to strong correlations. In this case the interaction energy is always underestimated, and the absolute value of the relative error $`ϵ=|WW^{ex}|/W^{ex}`$ increases monotonously as $`\gamma _{12}`$ decreases, reaching about 15% for $`\gamma _{12}/\gamma _{12}^0<0.4`$. The 4th-order approximation provides a significant advance, not only for $`\gamma _{12}/\gamma _{12}^01`$ but in the complete domain of representability. For $`W^{(4)}`$ the relative error $`ϵ`$ is reduced to less than 1% for $`\gamma _{12}/\gamma _{12}^0<0.4`$ ($`ϵ0`$ for $`\gamma _{12}0`$). The largest discrepancies are found for $`\gamma _{12}/\gamma _{12}^00.8`$$`0.9`$, where $`ϵ`$ reaches only 3%. An appreciable improvement in the accuracy of the derived properties can be therefore expected. In the following sections, Eqs. (10) and (13) are applied in the framework of LDFT to determine several electronic properties of the Hubbard model in 1D, 2D, and 3D periodic lattices.

## IV  Ground state energy

In Fig. 2 the ground-state energy $`E_{gs}`$ of the half-filled 1D Hubbard model is given as a function of the Coulomb repulsion strength $`U/t`$. Comparison between LDFT and the Bethe-Ansatz exact solution shows that 4th-order approximation improves significantly the already good results derived using the dimer ansatz.ldftscfer  This concerns not only the strongly correlated limit where, as expected, $`W^{(4)}`$ recovers the exact result, but the complete range of $`U/t`$. The largest quantitative discrepancies between exact and 4th-order results are in fact very small. They amount to less than 3% and are found for intermediate interaction strengths ($`U/t4`$). In contrast, the relative error in the dimer ansatz increases monotonously with $`U/t`$ reaching about 17% for $`U/t=\mathrm{}`$ (see the inset of Fig. 2). It is interesting to note that in both cases no artificial symmetry breaking is required in order to describe correctly the electron localization induced by correlations and the resulting dependence of $`E_{gs}`$ on $`U/t`$, as it is often the case in other mean-field approaches.

The higher performance obtained with the 4th-order correction originates in an improved accuracy of both kinetic and Coulomb contributions to the ground-state energy. As shown in Fig. 3, the kinetic energy $`E_K<0`$ increases monotonously with increasing $`U/t`$, first rather slowly up to $`U/t4`$, and then more rapidly when electron localization starts to set in. For $`U/t4`$, the values of $`E_K`$ obtained using $`W^{(2)}`$ and $`W^{(4)}`$ are very close to the exact result (typically $`|E_K^{(2)}E_K^{ex}|/E_K^{ex}2.6\%`$ and $`|E_K^{(4)}E_K^{ex}|/E_K^{ex}2.0\%`$). For $`U/t>4`$ the dimer ansatz shows some limitations while the 4th-order approximation remains very accurate (for example, for $`U/t=12`$, $`|E_K^{(2)}E_K^{ex}|/E_K^{ex}13\%`$ and $`|E_K^{(4)}E_K^{ex}|/E_K^{ex}2.4\%`$). The Coulomb energy $`E_C`$ shows the usual non-monotonous behavior, first increasing with $`U/t`$ in the weakly correlated regime and then decreasing as the strongly-correlated limit is approached. This behavior is correctly described by both 2nd- and 4th-order approximations. However, one finds that it is in general more difficult to accurately describe $`E_C`$ as compared to $`E_K`$. The 2nd-order $`E_C^{(2)}`$ underestimates (overestimates) $`E_C^{ex}`$ appreciably for $`2<U/t<5`$ ($`U/t>5`$). The 4th-order correction provides a clear improvement over the dimer ansatz, by increasing $`E_C`$ in one case ($`U/t5`$) and reducing it in the other ($`U/t10`$). As for $`E_{gs}`$, the remaining differences with the exact results are quite small and correspond to intermediate $`U/t`$. Summarizing, one may observe that the accuracy of the calculated $`E_{gs}`$ is not the result of a strong compensation of errors, since a very good performance is achieved for the kinetic and Coulomb energies separately.

In Fig. 4 results are given for $`E_{gs}`$ of the 2D square lattice and 3D simple cubic lattice at half-band filling. For $`U/t3`$ the 2nd-order and 4th-order results are almost indistinguishable, while for $`U/t>4`$ the 4th-order approximation yields somewhat higher values ($`E_{gs}^{(2)}<E_{gs}^{(4)}<0`$). These trends are very similar to those observed in the 1D chain. The LDFT calculations for 2D and 3D systems compare well with far more demanding quantum Monte Carlo (QMC) studiesQMC-2D ; QMC-3D  (see Fig. 4). Furthermore, the reliability of the LDFT results is confirmed by comparison with exact Lanczos diagonalizations on small clusters, for example, on a $`N_a=3\times 4`$ cluster of the square lattice with periodic boundary conditions. In this case, like in 1D, the overall performance is very good, with the largest quantitative discrepancies being observed for intermediate values of $`U/t`$. For instance, for $`U/t=4`$ one obtains $`|E_{gs}^{(4)}E_{gs}^{ex}|/|E_{gs}^{ex}|=4.2\times 10^2`$, and for $`U/t=16`$ $`|E_{gs}^{(4)}E_{gs}^{ex}|/|E_{gs}^{ex}|=3.2\times 10^2`$. In conclusion, LDFT using Eq. (13) for the interaction energy $`W`$ yields an accurate description of the ground-state energy of the Hubbard model in different dimensions.foot-comp

## V  Charge excitation gap

The charge-excitation or band gap

$$\mathrm{\Delta }E_c=E_{gs}(N_e+1)+E_{gs}(N_e1)2E_{gs}(N_e)$$
(14)
is a property of considerable interest, which measures the low-energy excitations associated to changes in the number electrons $`N_e`$, and which is very sensitive to the degree of electronic correlations. It can be related to the discontinuity in the derivative of the ground-state kinetic energy $`E_K`$ and correlation energy $`E_{corr}=E_CE_{\mathrm{HF}}`$ with respect to band-filling $`n`$. For $`N_a\mathrm{}`$ and $`n=1`$, it is given by

$$\mathrm{\Delta }E_c=(\epsilon /n)|_{1^+}(\epsilon /n)|_1^{},$$
(15)
where $`\epsilon =(E_K+E_{corr})/N_a`$. The determination of $`\mathrm{\Delta }E_c`$ is in general a more difficult task than the calculation of ground-state properties like $`E_{gs}`$, $`E_K`$, and $`E_C`$. In fact, the band-gap in semiconductors has been an important problem which motivated numerous works in the context of DFT in the continuum. Therefore, $`\mathrm{\Delta }E_c`$ appears as a particularly interesting property to investigate with the present lattice density-functional formalism.

In the half-filled Hubbard model on bipartite lattices, $`\mathrm{\Delta }E_c`$ increases with increasing $`U/t`$ ($`\mathrm{\Delta }E_c=0`$ for $`U/t=0`$) and approaches the limit $`\mathrm{\Delta }E_c(Uw_b)`$ for $`U/t\mathrm{}`$, where $`w_b`$ is the width of the single-particle band ($`w_b=4t`$, $`8t`$, and $`12t`$ for the 1D, 2D square, and 3D simple-cubic lattices, respectively). Fig. 5 presents LDFT results for $`\mathrm{\Delta }E_c`$ in 1D, 2D, and 3D Hubbard models ($`n=1`$). Comparison with the exact Bethe-Ansatz solution for the 1D chainlieb-wu  and with available QMC calculations for the squareQMC-2D  and simple cubicQMC-3D  lattices shows a good overall agreement. It should be however noted that in the 1D case the gap is significantly overestimated for $`U/t1`$. Here we obtain $`\mathrm{\Delta }E_\mathrm{c}(U/t)^2`$, while in the exact solution $`\mathrm{\Delta }E_\mathrm{c}`$ increases much more slowly, namely, exponentially in $`t/U`$. This discrepancy concerns both the 2nd-order and the 4th-order approximations, which are nearly indistinguishable for $`U/t<2`$$`4`$. Consequently, it is possible that the results for 2D and 3D lattices shown in Fig. 5 also overestimate the gap for small $`U/t`$. In any case, the accuracy of LDFT improves rapidly with increasing $`U/t`$, as electron localization starts to set in, and the error in $`\mathrm{\Delta }E_\mathrm{c}`$ tends to zero for large $`U/t`$. Therefore, the development of a Mott insulator in the strongly correlated limit is correctly described.

It is important to remark, in the context of metal-insulator transitions in three dimensions, that our calculations on the SC lattice yield a finite gap $`\mathrm{\Delta }E_c>0`$ for $`n=1`$ and all $`U/t>0`$. This is consistent with previous results on 3D bipartite lattices, which are expected to be antiferromagnetic (AF) insulators for all $`U/t>0`$.georges ; imada  The functionals $`W^{(2)}`$ and $`W^{(4)}`$ reproduce correctly this behavior, as well as the formation of local moments $`S_i^2=3(12\widehat{n}_i\widehat{n}_i)/4`$, without involving a spin-density-wave symmetry breaking. This can be understood be recalling that they are based on the exact functional of the Hubbard dimer which, being a bipartite cluster, incorporates AF correlations ($`n=1`$). However, the properties change qualitatively if frustrations become important (e.g., in non-bipartite lattices or if second NN hopping are significantly large). In this case it has been shown that the half-filled Hubbard model is a metal with $`\mathrm{\Delta }E_c=0`$ for small $`U>0`$ and that a metal-insulator transition takes place at a finite interaction strength $`U_c`$, which is of the order of the single-particle band width $`w_b`$.georges  This behavior is not reproduced by the functionals $`W^{(2)}`$ and $`W^{(4)}`$, even if they are applied to compact lattices (e.g., the face-centered cubic lattice), since they are free from any singularities throughout the domain of representability (except for $`g_{12}=1`$) and since the resulting $`\gamma _{ij}^{gs}`$ are smooth functions of $`U/t`$. Notice that the exact functional $`W_{ex}`$ may show a far more complex behavior, particularly if the nature of the state $`|\mathrm{\Psi }[\gamma ]`$ yielding the minimum of Eq. (5) changes as a function of $`\gamma `$. This is expected to be the case at a metal-insulator transition, where a discontinuous decrease of $`\widehat{n}_i\widehat{n}_i`$ occurs. Finally, let us point out that the results derived from Eqs. (10) and (13) for large $`U/t`$ ($`U>U_c`$) are consistent with previous studies. This concerns not only the presence of a finite gap $`\mathrm{\Delta }E_c`$, but also the fact that the number of double occupations does not vanish on the insulating side of the transition.georges ; imada

Comparing 2nd- and 4th-order approximations for $`U/t>2`$$`4`$ one observes that the charge gap is always somewhat smaller in the latter case. For the 1D chain, the reduction of $`\mathrm{\Delta }E_\mathrm{c}`$ due to the 4th-order correction improves the agreement with the exact solution appreciably (e.g., $`|\mathrm{\Delta }E_\mathrm{c}^{(4)}\mathrm{\Delta }E_\mathrm{c}^{ex}||\mathrm{\Delta }E_\mathrm{c}^{(2)}\mathrm{\Delta }E_\mathrm{c}^{ex}|/2`$ for $`U/t>10`$). In the considered 2D and 3D lattices, the differences between 2nd- and 4th-order results are similar to those observed in the 1D chain. Comparison with QMC calculations shows a good overall agreement although some quantitative differences can be noted. For example, as shown in Fig. 5, our values for $`\mathrm{\Delta }E_\mathrm{c}`$ are somewhat smaller than the QMC ones for the 2D (3D) lattice with $`U/t=4`$ ($`U/t=8`$) and somewhat larger for $`U/t=8`$ ($`U/t=12`$). In summary, the ensemble of 1D, 2D and 3D results shows that LDFT provides a very simple and efficient method of calculating the charge excitation energies of the Hubbard model in different dimensions and interaction regimes. However, the proposed approximations to $`W`$ are still not quite satisfactory in the weakly-correlated limit and deserve to be improved.

## VI  Charge susceptibility

The charge susceptibility $`\chi _c`$ is defined by

$$\chi _c=\frac{dn}{d\mu },$$
(16)
where $`n=N_e/N_a`$ is the number of electrons per site and $`\mu `$ the chemical potential. It represents the many-body density of electronic states at the Fermi energy $`\mu `$ and thus provides very useful information on the low-energy charge-excitation spectrum as a function of band filling. In Figs. 68 $`\chi _c`$ is given as a function of $`\mu `$ for 1D, 2D, and 3D Hubbard models on bipartite lattices for representative values of $`U/t`$. The LDFT calculations reported in these figures were performed using the dimer ansatz for $`W`$ given by Eq. (10). As it will be discussed below, the 4th-order approximation \[Eq. (13)\] yields very similar results. In the case of the 1D chain comparison is made with the exact $`\chi _c(\mu )`$, which is obtained from the Bethe ansatz solution.lieb-wu  For the 2D square lattice, we also show ground-state QMC resultsQMC-2D  for $`U/t=4`$. Notice that in bipartite lattices, as those considered here, electron-hole symmetry implies that $`\chi _c`$ is the same for band fillings $`n`$ and $`n^{}=2n`$, and therefore $`\chi _c(\mu )=\chi _c(\mu ^{}=U\mu )`$.

In the absence of interactions $`\chi _c`$ coincides with the single-particle density of states of the corresponding lattices ($`U=0`$). These are gapless and show the usual van Hove singularities at the band edges $`\mu =\pm w_b/2`$ and at some points within the bands of the square and simple-cubic lattices. For finite $`U`$ a gap $`\mathrm{\Delta }E_c=\mu (n=1^+)\mu (n=1^{})`$ opens at half-band filling which increases monotonously with $`U`$, as discussed in the previous section. Thus, the two so-called lower and upper Hubbard bands start to be distinguished, which correspond to hole and electron doping respectively. The separation of the bands becomes particularly clear for $`Uw_b`$, when $`\mathrm{\Delta }E_c`$ reaches values of the order of single-particle band width $`w_b`$ (see Figs. 68). At the same time the width of the lower and upper bands increases with $`U`$, from $`w_b/2`$ for $`U=0^+`$, to $`w_b`$ for $`U=+\mathrm{}`$. These qualitative features are common to bipartite lattices in all dimensions and are correctly described by LDFT.

In the 1D case, where a detailed comparison with the exact solution is possible, we observe that our results are very accurate except close to half-band filling and for small or moderate values of $`U/t`$ (see Fig. 6). The nature of the discrepancies close to $`n=1`$ is basically twofold. First, we find again the overestimation of the band gap $`\mathrm{\Delta }E_c`$ which is relatively important for small $`U/t`$ (see also Sec. V). Consequently, the band edges $`\mu (n=1^{})`$ and $`\mu (n=1^+)`$ are not precisely reproduced in this limit, even if the absolute error $`ϵ=|\mu \mu ^{ex}|`$ always remains reasonably small. The largest inaccuracies are found for $`U/t3`$ and amount to $`ϵ/w_b=8.1\times 10^2`$. Nevertheless, this problem disappears as $`U/t`$ increases, since $`ϵ`$ tends rapidly to zero in the strongly correlated limit (e.g., $`ϵ/w_b=1.2\times 10^4`$ for $`U/t=16`$). The second limitation concerns the shape of $`\chi _c`$ close to half-band filling. The exact solution of the 1D chain shows sharp divergences in $`\chi _c`$ at the gap edges $`\mu (n=1^{})`$ and $`\mu (n=1^+)`$ for $`U>0`$, which we fail to reproduce. For small and moderate $`U/t`$, for example $`U/t=1`$ or $`4`$, we obtain a nearly constant $`\chi _c`$ for $`\mu \mu (n=1^\pm )`$, while the exact result is $`\chi _c+\mathrm{}`$ (see Fig. 6). Notice, however, that the increase and divergence of $`\chi _c^{ex}`$ are sharply localized in a narrow range of $`\mu `$, particularly for small $`U/t`$. The divergence of $`\chi _c`$ for $`n1`$ could be reproduced by considering broken symmetry solutions of the LDFT equations, like in the AF Hartree-Fock approximation. Even so, it would be more interesting to describe this effect without involving a symmetry breaking, which is known to be artificial, and which could affect the results on the kinetic, Coulomb, and total energies, particularly in the case of finite systems.maol  As we approach the strongly correlated limit the LDFT results for $`\chi _c`$ develop peaks at the gap edges, which height increases with $`U/t`$, thus approaching asymptotically the exact result. Still, $`\chi _c`$ always remains finite for all finite $`U/t`$ (see Fig. 6 for $`U/t=16`$ and $`64`$). The very good performance for large $`U/t`$ can be understood by recalling that for $`U/t=+\mathrm{}`$, the LDFT results correspond to the fully-polarized or Nagaoka state,nagaoka  which is the exact ground-state in 1D for all $`n`$ ($`U/t=+\mathrm{}`$).lieb-wu  In higher dimensions it is possible that our calculations yield a finite-height peak for $`n1`$, where a true divergence of $`\chi _c`$ could be present. This seems to be the case in the 2D square lattice where we observe narrow peaks in $`\chi _c`$ at the band edges. In fact ground-state QMC calculations on the square lattice with $`U/t=4`$ predict a divergent $`\chi _c`$ at half-band filling (see Fig. 7). In contrast, no such peaks are found in our calculations of $`\chi _c`$ for the 3D simple-cubic lattice (see Fig. 8).

As already discussed in the previous section, it is important to remark that the results presented in Fig. 8 are representative of bipartite lattices which at the half-band filling show an AF insulating behavior for all $`U/t>0`$. In this case of our results are in good qualitative agreement with previous studies. The obtained simple Hubbard-approximation-like structure of $`\chi _c`$, with a lower and upper Hubbard bands, also applies to frustrated lattices or to paramagnetic phases provided that $`U/t`$ is sufficiently large to bring the system on the insulating side of the metal-insulator transition ($`U>U_c`$).georges ; imada  However, it has been shown that the presence of frustrations drives the system into an AF metallic state at small $`U/t`$ which contrasts with the AF insulator found in the absence of frustrations.georges  In this case the spectral density presents —in addition to a progressive development of lower and upper Hubbard bands with increasing $`U/t`$— a Kondo-like resonance at half-band filling ($`\mu U/2=0`$) characterized by a constant-height peak having a width that decreases with increasing $`U/t`$ and that vanishes at $`U_c`$, i.e., at the transition to the insulating state (see Ref. georges, ). The functionals $`W^{(2)}`$ or $`W^{(4)}`$ fail to reproduce this kind of behavior, even when applied to compact structures (e.g., fcc lattice). This limitation does not seem surprising, since Eqs. (10) and (13) were derived from the properties of a bipartite system, and since the extensions presented in this paper, while achieving an accurate $`W`$ in the strongly correlated limit at half-band filling, do not aim a precise description at small $`U/t`$ and as a function of $`n`$. Exploring the functional dependence of $`W`$ in frustrated structures, particularly close to $`n=1`$ and $`g_{12}1`$, should provide very useful clues in view of developing practical approximations capable of describing these remarkable effects.

Let us finally point out that we have also determined $`\chi _c`$ using $`W^{(4)}`$ as approximate interaction energy \[Eq. (13)\] and found that the results are very similar to those obtained using $`W^{(2)}`$ and shown in Figs. 68. In both cases the results are extremely good away from half-band filling, nearly indistinguishable from the 1D exact solution. Close to $`n=1`$, the 4th-order calculations yield smaller $`\mathrm{\Delta }E_c`$ and thus perform slightly better for $`U/t4`$. However, the divergences of $`\chi _c`$ at the gap edges are not reproduced. Therefore, the 4th-order corrections do not provide a significant improvement over the dimer ansatz concerning $`\chi _c`$ of the 1D chain. This is probably related to the simple form considered for $`W^{(4)}`$ which uses a coefficient $`\kappa `$ that is independent of $`n`$ \[see Eq. (13)\]. While this approximation seems satisfactory for applications that concern a fixed band filling, it appears as a limitation for properties like $`\mathrm{\Delta }E_\mathrm{c}`$ or $`\chi _c`$, where a precise description of the dependence of $`W`$ on $`n`$ is crucial. For 2D and 3D lattices the 4th-order results for $`\chi _c`$ are also very similar to those shown in Figs. 7 and 8.

## VII  Discussion

A new approximation to the interaction-energy functional $`W[\gamma ]`$ of the Hubbard model has been proposed in the framework of lattice density functional theory, which exactly recovers the limit of strong electron correlations at half-band filling. The simpler ansatz which was derived from the functional dependence of $`W`$ in the Hubbard dimerldftscfer  is thereby extended and improved. A more accurate description of $`W`$ is achieved throughout the domain of representability of $`\gamma _{ij}`$ including the crossover from weak to strong correlations. Several properties have been determined by applying this functional to one-, two-, and three-dimensional lattices. Ground state energies, as well as kinetic and Coulomb energies, were successfully determined in all dimensions and interaction regimes. Very good results are also obtained concerning the charge-excitation gap $`\mathrm{\Delta }E_c`$ and the charge susceptibility $`\chi _c`$ of bipartite lattices, except very close to half-band filling ($`n=1`$) and for small values of the Coulomb repulsion strength ($`U/t4`$). This reveals some limitations in the description of the band-filling dependence of $`W`$ for $`n1`$ and $`\gamma _{12}\gamma _{12}^0`$, which deserve more detailed investigations. Further insight on the origin of this problem could be obtained, for example, by analyzing the properties of the exact $`W`$ as derived from the Bethe ansatz exact solution of the 1D chain and from Lanczos diagonalizations in finite 2D clusters with periodic boundary conditions. Moreover, the functional dependence of $`W`$ could be determined in the limit of large $`\gamma _{12}`$ (i.e., $`\gamma _{12}\gamma _{12}^0`$ corresponding to the weak correlations) by applying perturbation theory for small $`U/t`$. In this way, more accurate approximations to $`W`$ could be developed in order to improve the results on $`\mathrm{\Delta }E_c`$ and $`\chi _c`$ in this limit, particularly concerning the differences between bipartite and non-bipartite lattices.

Besides these methodological aspects, the accuracy of the results and the simplicity of the calculations encourage new applications of the present approach to related problems of current interest like dimerized one-dimensional chains and ladders, the 2D square lattice with competing first and second nearest-neighbor hoppings, the properties of $`\pi `$ electrons in doped fullerenes and nanotubes in the framework of Hubbard or PPP models, or the connection with the continuum’s DFT using minimal basis sets. In this way, a novel density-functional route to the physics of strongly correlated fermions is opened.

###### Acknowledgements.

This work has been supported by CONACyT Mexico through Grant No. J-41452 and Millennium Initiative W-8001. Computer resources were provided by IDRIS (CNRS, France).


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# Orthogonality of Biphoton Polarization States

## Abstract

Orthogonality of two-photon polarization states belonging to a single frequency and spatial mode is demonstrated experimentally, in a generalization of the well-known anti-correlation ’dip’ experiment.

Orthogonality, one of the basic mathematical concepts, plays an important role in physics, especially quantum physics and, in particular, quantum optics. A well-known example including both classical and quantum cases is orthogonality of two polarization modes of electromagnetic radiation. Physically, orthogonality of two arbitrary polarization states means that if light is prepared in a certain (in the general case, elliptic) polarization state it will not pass through a filter selecting the orthogonal state. (A filter selecting an arbitrary polarization state can be made of a rotatable quarter-wave plate and a rotatable linear polarization filter Shurkliff .) Orthogonality of polarization states has an explicit representation on the Poincaré sphere where each polarization state is depicted by a point. The state orthogonal to a given one is shown by a point placed on the opposite side of the same diameter. Examples are states with vertical and horizontal linear polarization, right- and left- circularly polarized states, and any two elliptically polarized states with opposite directions of rotation and inverse axis ratios. This concept of orthogonality relates to both classical polarization states of light and single-photon quantum states of polarized light kljetp . Mathematically, orthogonality of two polarization states means that the scalar product of two corresponding Jones vectors Shurkliff  is equal to zero. In quantum optics, this corresponds to zero scalar product of polarization state vectors, for instance, state vectors of single-photon states. This is a particular case of the general rule: orthogonality of quantum states means that their scalar product is equal to zero.

However, in addition to single-photon states there are other types of nonclassical light. In quantum optics, one of the central roles is played by two-photon states, which are most easily generated via spontaneous parametric down-conversion (SPDC) photons . In a two-photon state, radiation consists of photon pairs, often called biphotons, that are correlated in frequency, wavevector, moment of birth, and polarization. Focusing on the case of collinear frequency-degenerate SPDC, here we will discuss the so-called single-mode biphotons. Although even in the frequency-degenerate collinear case SPDC has a finite frequency and angular spectrum, under certain experimental conditions such biphotons can be treated as relating to a single frequency and angular mode.

One can show that the polarization state of a single-mode biphoton burkl  can be described as a qutrit, a three- state quantum system. Using qutrits instead of qubits for the transmission of quantum information has been previously discussed trits , in particular, in connection with ternary cryptography protocols bechmann bruss peres . The general case of a qutrit represented by a biphoton in an arbitrary pure polarization state is given by the state vector

$$|\psi =c_1|2,0+c_2|1,1+c_3|0,2,$$
(1)
where $`c_i`$ are complex amplitudes satisfying the normalization condition, $`|c_1|^2+|c_2|^2+|c_3|^2=1`$, and $`|n,m`$ denotes a two-photon ($`n+m=2`$) state with $`n`$ photons polarized horizontally and $`m`$ photons polarized vertically indistinguishable . In quarkobzor , it is shown that the state (1) allows an explicit representation on the Poincaré sphere. It can be written in the form of two arbitrarily polarized correlated single-photon states,

$$|\psi =\frac{a^{}(\theta ,\varphi )a^{}(\theta ^{},\varphi ^{})|\mathrm{vac}}{a^{}(\theta ,\varphi )a^{}(\theta ^{},\varphi ^{})|\mathrm{vac}}.$$
(2)
Here, $`a^{}(\theta ,\varphi )`$ and $`a^{}(\theta ^{},\varphi ^{})`$ are operators of photon creation in arbitrary polarization modes given by the coordinates $`\theta ,\varphi `$, $`\theta ^{},\varphi ^{}`$ on the Poincaré sphere:

$$a^{}(\theta ,\varphi )=\mathrm{cos}(\theta /2)a_H^{}+\mathrm{e}^{i\varphi }\mathrm{sin}(\theta /2)a_V^{},$$
(3)
where $`a_{H,V}^{}`$ are photon creation operators in the horizontal and vertical linear polarization modes, and similarly for $`a^{}(\theta ^{},\varphi ^{})`$. Axial angles $`\theta ,\theta ^{}`$ and azimuthal angles $`\varphi ,\varphi ^{}`$ angles  are in one-to-one correspondence with the four parameters describing the state (1), which are, for instance, $`d_1=|c_1|`$, $`d_3=|c_3|`$, $`\varphi _1=\mathrm{arg}(c_1)\mathrm{arg}(c_2)`$, $`\varphi _3=\mathrm{arg}(c_3)\mathrm{arg}(c_2)`$. Representation (2) means that a biphoton of arbitrary polarization can be shown as a pair of points on the Poincaré sphere. It turns out that the Stokes vector of a biphoton is simply a normalized sum of the Stokes vectors of photons forming it (’biphoton halves’), and the polarization degree $`P`$ of the pair is given by the angle $`\sigma `$ at which the pair can be seen from the sphere center.

A question arises: what does orthogonality of two biphoton polarization states mean? As usually in quantum mechanics, it means that the product of their state vectors is equal to zero. For instance, orthogonality of two biphotons $`\psi _{ab}\frac{a^{}b^{}|\mathrm{vac}}{a^{}b^{}|\mathrm{vac}}`$ and $`\psi _{cd}\frac{c^{}d^{}|\mathrm{vac}}{c^{}d^{}|\mathrm{vac}}`$, with the operators of photon creation in arbitrary polarization modes denoted now by $`a^{},b^{},c^{},d^{}`$, means that

$$\mathrm{vac}|cda^{}b^{}|\mathrm{vac}=0.$$
(4)
What does orthogonality of two biphotons mean from the viewpoint of physics? This question was answered in orthogonality  where an operational criterion of orthogonality for arbitrarily polarized biphotons was formulated. Namely, orthogonality of two biphotons can be tested using a simple setup consisting of a non-polarizing beamsplitter, two detectors installed in its two output ports, with an arbitrary polarization filter inserted at the input of each detector, and a coincidence circuit. A biphoton is registered if there is a coincidence of photocounts from the two detectors. Let a biphoton $`|\psi _{ab}`$ be at the input and the filters in the output ports of the beamsplitter select polarization states corresponding to photon creation operators $`c^{},d^{}`$. Then orthogonality of $`|\psi _{ab}`$ and $`|\psi _{cd}`$ is equivalent to the absence of coincidences absence  in such a setup. Note that orthogonality of any two polarization states among $`a^{}|\mathrm{vac}`$, $`b^{}|\mathrm{vac}`$, $`c^{}|\mathrm{vac}`$, $`d^{}|\mathrm{vac}`$ is not required.

Such an experiment is the most general case of the well-known anticorrelation experiment hong . Earlier, a particular case of this polarization version of anticorrelation experiment has been performed for type-II SPDC typeiianti . The absence of coincidences in the anticorrelation experiment typeiianti  can be interpreted as orthogonality of the states $`|HVa_H^{}a_V^{}|\mathrm{vac}`$ and $`|D\overline{D}a_{45}^{}a_{45}^{}|\mathrm{vac}`$, a pair of photons polarized linearly at angles $`\pm 45^{}`$ to the vertical axis. Similarly, in ternary , orthogonality of the states $`|HV`$ and $`|D\overline{D}`$ to the state of right- and left polarized photons, $`|RL`$, has been demonstrated. In both cases, orthogonal biphotons had zero polarization degree, which means that they were pairs of orthogonally polarized photons. Another example of a basis formed by three mutually orthogonal biphotons with zero polarization degree was demonstrated in trifonov .

Several examples of orthogonal biphotons of other polarization degrees are shown in Fig.1. Fig.1a shows three mutually orthogonal states $`|HV`$, $`|D\overline{D}`$, $`|RL`$ of biphotons with zero polarization degree studied in typeiianti  and ternary . All three states are biphotons consisting of two orthogonal photons; at the same time, no photon forming a biphoton is orthogonal to any photon of the other two biphotons. Three biphotons shown in Fig.1a form an orthogonal basis.

Whenever a biphoton is fixed (two points are fixed on the Poincaré sphere), there are infinitely many biphotons orthogonal to it. Replacing the Poincaré sphere by the globe, one can pick two spots denoting a biphoton to be, for instance, Moscow (Russia) and Turin (Italy). Then, one should make a choice for the third point. Let it be Baltimore(MD, USA). Then the fourth point is found from Eq. (4), and it turns out to be near New Zealand and the Bounty isles. So, the biphoton ’Moscow - Turin’ is orthogonal to the biphoton ’Baltimore - Bounty’!

The idea of our experiment was to prepare some arbitrary input biphoton state, to make the registration part select the state orthogonal to it, and to demonstrate orthogonality by scanning the parameters of the input and registered states around the minimum of coincidence counting rate. We chose the input biphoton state to be a pair of photons polarized linearly at the opposite angles to the horizontal direction, the polarization degree being $`P=0.5`$. On the Poincaré sphere, this is shown as two points on the equator placed symmetrically at the angles $`\pm 74.5^{}`$ with respect to the ’H’ axis, which corresponds to photons polarized linearly at the angles $`37.25^{}`$ to the horizontal axis. For the reasons that we will explain later, it is convenient to make one of the polarization filters in the registration part select the state polarized linearly at the angle $`45^{}`$ to the horizontal axis. The other filter, as one can easily find, should then select linear polarization at the angle $`60^{}`$ to the horizontal axis. This configuration, which is used in one of our experiments, is shown in Fig.1b. Finally, Fig.1c gives an example of two orthogonal biphotons with polarization degree $`P=0.5`$ in a ’non-plane’ configuration. This time, the points denoting the biphoton ’ab’ are placed on the ’Greenwich meridian’, if we follow the globe terminology. Again, one of the polarizers selects the state polarized linearly at $`45^{}`$. However, the position of the other polarizer is changed: now, it should select linear polarization at the angle $`60^{}`$ to the horizontal axis. Under each Poincaré sphere in Fig.1, the corresponding polarization states are shown schematically. In all these examples, there is no orthogonality between separate photons, or ’halves of biphotons’.

The experimental setup is shown in Fig.2. Collinear frequency-degenerate SPDC is generated in two similar type-I lithium iodate crystals of length 1 cm, cw radiation of argon laser at wavelength 351 nm used as the pump. The optic axis of the first crystal is in the vertical plane while the optic axis of the other crystal is in the horizontal plane. The two-photon state generated after the crystals is of the form (1), with $`c_2=0`$, the amplitudes $`d_1`$ and $`d_3`$ can be varied by rotating the $`\lambda /2`$ plate in the pump beam, and the phase $`\mathrm{\Delta }\varphi \varphi _3\varphi _1`$ can be varied by tilting the two quartz plates QP, whose optic axes are oriented in the vertical plane. The pump after the crystals is cut off by a UV mirror UVM. Spatial and frequency filtering of the SPDC radiation is performed by a pinhole P and an interference filter IF with $`702`$ nm central wavelength and $`3`$ nm bandwidth. The right-hand side of the setup shows the registration part (the Brown-Twiss interferometer). It includes a non-polarizing beamsplitter BS and two detectors (photomultiplier tubes) D1, D2 inserted in its output ports. At the input of each detector, there is a polarization filter consisting of a rotatable quarter-wave plate QWP1,2 qp  and a rotatable polarizer P1,2. Coincidences between the photocounts of the detectors are registered using a coincidence circuit with a resolution $`T_c=5.5`$ ns.

The measurements were performed for two configurations shown in Figs 1b,c. The plates QP were tilted so that the phase $`\mathrm{\Delta }\varphi `$ was equal to $`\pi `$. Then the angle $`\chi `$ of the $`\lambda /2`$ plate was scanned from $`0^{}`$ to $`90^{}`$. As a result, the two points corresponding to the produced biphoton state travelled on the Poincaré sphere: first, from the ’VV’ point ($`\chi =0^{}`$) to the ’HH’ point ($`\chi =45^{}`$) symmetrically along the opposite sides of the equator, then again to the ’VV’ point ($`\chi =90^{}`$) but this time, along the opposite sides of the ’Greenwich meridian’. This way, both cases shown in Fig.1b,c were realized. In the first run, the polarizer P1,2 orientations were fixed as in Fig.1b: $`\zeta _1=45^{}`$ and $`\zeta _2=60^{}`$. In the dependence of coincidence counting rate on $`\chi `$ (Fig.3a), the minimum was at $`\chi =30^{}`$, which corresponded to $`d_1^2/d_3^2=3`$. For this point, the ratio $`d_1^2/d_3^2`$ was measured using the tomography procedure developed in tomography ; this ratio turned out to be $`3.4\pm 0.8`$. The $`45^{}`$ orientation of P1 is convenient since in this case, rotation of the half-wave plate in the pump beam does not lead to the variation of D1 single counting rate $`R_1`$.

In the next run, the orientations of P1, P2 were fixed as in Fig.2c: $`\zeta _1=45^{}`$ and $`\zeta _2=60^{}`$. In this case, the minimum was achieved for $`\chi =60^{}`$ (Fig.3b), corresponding to $`d_1^2/d_3^2=1/3`$.

Finally, orthogonality of two biphoton states was checked by fixing all parameters ($`\chi `$, $`\zeta _{1,2}`$, $`\mathrm{\Delta }\varphi `$) in the configuration shown in Fig.1b and then scanning them around their optimal values. The plot in Fig.4 shows the dependence of the coincidence counting rate on the orientation of polarizer P1, with the other polarizer fixed at $`60^{}`$ and the half-wave plate in the pump beam fixed at $`\chi =30^{}`$. Similar dependencies were obtained for scanning $`\zeta _2`$ and $`\mathrm{\Delta }\varphi `$.

Two important notes should be made about the measurement procedure. First, when the angle $`\chi `$ is scanned with fixed positions of the two polarizers (Fig.3a), a considerable modulation in the singles counting rate $`R_2`$ of detector D2 is observed (Fig.5). This is quite natural since in the course of $`\chi `$ variation the state of biphoton light changes from being vertically polarized through completely non-polarized state (at $`\chi =22.5^{}`$) to being horizontally polarized. With the polarizer P1 oriented at $`\pm 60^{}`$, the intensity of transmitted light should vary three times, as it indeed does in Fig.5. However, the minimum of the coincidence counting rate $`R_c`$ does not correspond to the point where $`R_2`$ is minimal; according to the calculation, it occurs at $`\chi =30^{}`$. The second remark is that in all kinds of anticorrelation experiments, the coincidence counting rate in the minimum is given by the level of accidental coincidence counting rate, which corresponds to the normalized second-order Glauber’s correlation function $`g^{(2)}=1`$. To demonstrate this, instead of the coincidence counting rate, in all plots we present $`g^{(2)}`$ g2  instead of $`R_c`$.

To find the dependence of the coincidence counting rate $`R_c`$ on all parameters, one can write

$$R_c|\mathrm{vac}|cda^{}b^{}|\mathrm{vac}|^2.$$
(5)
The operators $`a^{}`$, $`b^{}`$, $`c`$, $`d`$ are substituted in (5) in the form (3), with the angles $`\varphi `$ taking the values $`0,\pi ,0,0`$, respectively. The axial angles for $`a,b`$ can be expressed as functions of $`\chi `$ via the relations given in orthogonality  and the formulas $`d_1=\mathrm{sin}(2\chi )`$, $`d_3=\mathrm{cos}(2\chi )`$. The axial angles for $`c,d`$ can be calculated as functions of $`\zeta _{1,2}`$, the angles of P1,P2 orientations. Then we obtain the coincidence counting rate,

$$R_c\left[\mathrm{cos}\zeta _1\mathrm{cos}\zeta _2\mathrm{sin}(2\chi )\mathrm{sin}\zeta _1\mathrm{sin}\zeta _2\mathrm{cos}(2\chi )\right]^2,$$
(6)
and the single-photon counting rate in detector 2,

$$R_2\mathrm{cos}^2\zeta _2\mathrm{sin}^2(2\chi )+\mathrm{sin}^2\zeta _2\mathrm{cos}^2(2\chi ).$$
(7)
Equations (6,7) were used to plot the theoretical dependencies shown in Figs.3,4.

To conclude, we have experimentally demonstrated orthogonality of two biphotons having polarization degree between $`0`$ and $`1`$. Our experiment is a generalization of the ’anti-correlation dip’ experiment to the case of arbitrarily polarized photon pairs. The observed effect can find applications in ternary quantum cryptography protocols cryptography .

This work was supported in part by the Russian Foundation for Basic Research grants #02-02-16664,#03-02-16444, INTAS grant #01-2122, and the Russian program of scientific school support (#166.2003.02)


text:
# The 𝑟-process: recent progress and needs for nuclear data

## 1 INTRODUCTION

The dominant mechanism for producing nuclei beyond the Fe group is neutron capture. In particular, the rapid neutron capture process, or the $`r`$-process, is responsible for approximately half the solar abundances of nuclei with mass numbers $`A>70`$. The relative abundances of $`r`$-process nuclei in the solar system are shown in Figure 1. This solar $`r`$-process abundance pattern ($`r`$-pattern) has two prominent peaks at $`A130`$ and 195, respectively, and provides an important basis for studying the $`r`$-process.

By definition, neutron capture occurs much more rapidly than $`\beta `$ decay during the $`r`$-process. With many neutrons available for capture by each seed nucleus, the nuclear flow quickly moves toward the neutron-drip line. At some point, the separation energy of the next neutron to be captured becomes so small that it will be quickly disintegrated by the photons in the $`r`$-process environment. At this so-called “waiting point,” the nuclear flow is characterized by a tug of war between neutron capture and photo-disintegration. Heavier nuclei cannot be produced until the waiting-point nucleus $`\beta `$ decays to its daughter with a higher proton number. Then the tug of war repeats at the next waiting point. Through such a series of neutron capture and $`\beta `$ decay, very neutron-rich nuclei far from stability are produced. Clearly, at a given proton number $`Z`$, the abundance is concentrated in the corresponding waiting-point nucleus. The more slowly this nucleus $`\beta `$ decays, the more abundant it is. As nuclei with magic neutron numbers $`N=82`$ and 126 have (relatively) very slow $`\beta `$-decay rates, abundance peaks are produced at these nuclei. After neutron capture ceases, these nuclei successively $`\beta `$ decay to stability and give rise to the peaks at $`A130`$ and 195 in the solar $`r`$-pattern (see Fig. 1).

## 2 WAITING-POINT APPROXIMATION AND NUCLEAR PROPERTIES

The tug of war between neutron capture and photo-disintegration during the $`r`$-process results in a so-called “$`(n,\gamma )(\gamma ,n)`$ equilibrium,” for which the abundances $`Y(Z,A+1)`$ and $`Y(Z,A)`$ of two neighboring nuclei $`(Z,A+1)`$ and $`(Z,A)`$ in the same isotopic chain satisfy (see e.g., )

$`{\displaystyle \frac{Y(Z,A+1)}{Y(Z,A)}}`$ $`=`$ $`{\displaystyle \frac{n_nv\sigma _{n,\gamma }(Z,A)}{\lambda _{\gamma ,n}(Z,A+1)}}`$ (1)
$`=`$ $`n_n\left({\displaystyle \frac{2\pi \mathrm{}^2}{m_ukT}}\right)^{3/2}\left({\displaystyle \frac{A+1}{A}}\right)^{3/2}{\displaystyle \frac{G(Z,A+1)}{2G(Z,A)}}\mathrm{exp}\left[{\displaystyle \frac{S_n(Z,A+1)}{kT}}\right],`$
where $`n_n`$ is the neutron number density of the $`r`$-process environment, $`v\sigma _{n,\gamma }(Z,A)`$ denotes the product of neutron velocity and capture cross section averaged over a thermal distribution of temperature $`T`$, $`\lambda _{\gamma ,n}(Z,A+1)`$ is the photo-disintegration rate at the same temperature, $`\mathrm{}`$ is the Planck constant, $`m_u`$ is the atomic mass unit, $`k`$ is the Boltzmann constant, $`G(Z,A)`$ is the nuclear partition function, and $`S_n(Z,A+1)`$ is the neutron separation energy. If $`S_n`$ monotonically decreases with increasing $`A`$ over an isotopic chain, then Equation (1) indicates that the most abundant nucleus in this chain is the nucleus with an $`S_n`$ approximately equal to

$`\overline{S}_n`$ $`=`$ $`kT\mathrm{ln}\left[{\displaystyle \frac{2}{n_n}}\left({\displaystyle \frac{m_ukT}{2\pi \mathrm{}^2}}\right)^{3/2}\right]`$ (2)
$`=`$ $`\left({\displaystyle \frac{T}{10^9\mathrm{K}}}\right)\left\{2.79+0.198\left[\mathrm{log}\left({\displaystyle \frac{10^{20}\mathrm{cm}^3}{n_n}}\right)+{\displaystyle \frac{3}{2}}\mathrm{log}\left({\displaystyle \frac{T}{10^9\mathrm{K}}}\right)\right]\right\}\mathrm{MeV}.`$
However, pairing leads to odd-even staggering superposed on a general trend of decreasing $`S_n`$ with increasing $`A`$ for an isotopic chain. In contrast, the behavior of the two-neutron separation energy $`S_{2n}`$ is essentially monotonic. Consequently, the most abundant nucleus in an isotopic chain has an even $`N`$ and a two-neutron separation energy $`S_{2n}2\overline{S}_n`$ . As $`\overline{S}_n`$ only depends on $`n_n`$ and $`T`$ of the $`r`$-process environment, it can be seen that the abundances in $`(n,\gamma )(\gamma ,n)`$ equilibrium are concentrated in a set of even-$`N`$ nuclei that have approximately the same two-neutron separation energy $`S_{2n}2\overline{S}_n`$. These are the waiting-point nuclei.

If $`(n,\gamma )(\gamma ,n)`$ equilibrium is indeed obtained during the $`r`$-process, then there is no need to follow neutron capture and photo-disintegration reactions in an $`r`$-process calculation. This so-called “waiting-point approximation” is valid only when the rates of neutron capture and photo-disintegration are much faster than those of $`\beta `$ decay for the nuclei involved in the $`r`$-process. The photo-disintegration rate for nucleus $`(Z,A+1)`$ is related to the neutron capture cross section for nucleus $`(Z,A)`$ by detailed balance as described in Equation (1). Based on a range of theoretical input for neutron capture cross sections, nuclear masses, and $`\beta `$-decay rates, it was estimated that the waiting-point approximation is valid for $`n_n\stackrel{>}{}\mathrm{\hspace{0.25em}10}^{20}`$ cm-3 at $`T=2\times 10^9`$ K and for $`n_n\stackrel{>}{}\mathrm{\hspace{0.25em}10}^{28}`$ cm-3 at $`T=10^9`$ K .

The derivation of the constraints on $`n_n`$ and $`T`$ can be illustrated by considering production of the peak at $`A195`$. The expected waiting-point nuclei giving rise to this peak should include 195Tm with $`N=126`$. For 195Tm to be a waiting-point nucleus at least requires

$$\lambda _{\gamma ,n}({}_{}{}^{195}\mathrm{Tm})>\lambda _\beta ({}_{}{}^{195}\mathrm{Tm}),n_nv\sigma _{n,\gamma }({}_{}{}^{195}\mathrm{Tm})>\lambda _\beta ({}_{}{}^{195}\mathrm{Tm}),$$
(3)
where $`\lambda _\beta ({}_{}{}^{195}\mathrm{Tm})`$ is the $`\beta `$-decay rate of 195Tm. Calculations give $`v\sigma _{n,\gamma }({}_{}{}^{194}\mathrm{Tm})=4\times 10^{19}`$ cm3 s-1, $`v\sigma _{n,\gamma }({}_{}{}^{195}\mathrm{Tm})=7\times 10^{22}`$ cm3 s-1 , $`S_n({}_{}{}^{195}\mathrm{Tm})=4.2`$ MeV, and $`\lambda _\beta ({}_{}{}^{195}\mathrm{Tm})=10`$ s-1 . Based on these theoretical results, the waiting-point approximation may be used for production of the $`A195`$ peak when $`T>1.4\times 10^9`$ K and $`n_n>1.4\times 10^{22}`$ cm-3.

Clearly, the validity of the waiting-point approximation depends on both astrophysical conditions in the $`r`$-process environment and nuclear properties. If valid, this approximation greatly simplifies $`r`$-process calculations and reduces the needs for cross sections of neutron capture on neutron-rich nuclei far from stability. In view of this nice feature, it is crucial that the validity of the waiting-point approximation be established by experimental data. For example, the constraints on $`n_n`$ and $`T`$ for applying the waiting-point approximation to production of the $`A195`$ peak discussed above should be rederived based on measurements of the neutron capture cross sections for 194Tm and 195Tm and the neutron separation energy and $`\beta `$-decay rate for 195Tm.

## 3 $`r`$-PATTERN RESULTING FROM CLASSICAL CALCULATIONS AND STRENGTH OF CLOSED NEUTRON SHELLS

Classical $`r`$-process calculations  assume $`(n,\gamma )(\gamma ,n)`$ equilibrium, which selects a set of waiting-point nuclei with $`S_{2n}2\overline{S}_n`$. The value of $`\overline{S}_n`$ is determined by $`n_n`$ and $`T`$ of the $`r`$-process environment \[see Eq. (2)\]. The relative abundances of the waiting-point nuclei are controlled by their $`\beta `$-decay rates and the duration of the $`r`$-process $`t_r`$. A specific abundance pattern is produced for a set of $`n_n`$, $`T`$, and $`t_r`$ based on the nuclear physics input of two-neutron separation energies and $`\beta `$-decay rates for the relevant nuclei. The goal of classical $`r`$-process calculations is to reproduce the solar $`r`$-pattern by a superposition of patterns produced with a range of $`n_n`$, $`T`$, and $`t_r`$. This approach succeeds in reproducing the gross features of the solar $`r`$-pattern, especially the peaks at $`A130`$ and 195. However, most such calculations severely underproduce the nuclei below these peaks (see e.g., ). These deficiencies can be traced to the astrophysical conditions and nuclear physics input assumed in such calculations.

To produce a component of the solar $`r`$-pattern, classical calculations assume a fixed set of $`n_n`$ and $`T`$, which then choose a fixed set of waiting-point nuclei with approximately the same $`S_{2n}`$. As the waiting-point nuclei are far from stability, $`S_{2n}`$ has to be calculated from a mass formula for essentially all these nuclei. The waiting-point nuclei with $`S_{2n}5.8`$ MeV corresponding to $`n_n=3.16\times 10^{23}`$ cm-3 and $`T=1.35\times 10^9`$ K are shown as open and crossed squares in Figure 2 along with the stable nuclei shown as filled squares. It can be seen that there is a large mass gap for the waiting-point nuclei below the magic number $`N=126`$. This can be understood as follows. In general, at a given $`N`$, $`S_{2n}`$ increases with increasing $`Z`$ while at a given $`Z`$, it decreases with increasing $`N`$. Typical mass formulae predict that $`S_{2n}`$ decreases very slowly as $`N`$ increases toward the magic numbers. Consequently, when $`Z`$ increases from 59 to 60, $`N`$ has to increase from 108 to 118 in order to reach the same $`S_{2n}5.8`$ MeV. This results in a gap of 11 mass units for the waiting-point nuclei below the magic number $`N=126`$ and causes the severe underproduction below the $`A195`$ peak. The deficiency below the $`A130`$ peak can be similarly explained.

The severe underproduction of nuclei below the peaks at $`A130`$ and 195 in classical calculations suggest that the mass formulae used in these calculations may be inadequate or that the astrophysical conditions are not treated properly by these calculations. For example, these deficiencies can be alleviated by quenching the strength of closed neutron shells in the mass formulae . On the other hand, $`n_n`$ and $`T`$ decrease with time during a realistic $`r`$-process. So the waiting-point nuclei are not fixed as assumed in classical calculations. It was shown that the deficiency below the $`A195`$ peak can be removed by taking into account the time evolution of $`n_n`$ and $`T`$ . Clearly, to fully understand the cause for the underproduction of nuclei below the peaks at $`A130`$ and 195 in classical calculations, we need both accurate mass measurements for nuclei far from stability and detailed description of the $`r`$-process environment.

## 4 $`r`$-PROCESS SITE AND EFFECTS OF NEUTRINO INTERACTION

The $`r`$-process is commonly associated with core-collapse supernovae or neutron star mergers. In the supernova model, neutrinos emitted from a nascent neutron star drives a wind by heating the material above the neutron star. The wind material is initially composed of neutrons and protons. As it expands away from the neutron star and cools, neutrons and protons combine to produce seed nuclei. If many neutrons are left over for each seed nucleus produced, then an $`r`$-process can occur in this neutrino-driven wind (see e.g., ). However, this model currently has sever difficulty in producing the nuclei with $`A>130`$ (see e.g., ). In the neutron star merger model, the $`r`$-process is supposed to occur in the ejecta from an old neutron star that is disrupted during the merger. By treating the neutron-richness of the ejecta as a free parameter, it was shown that an $`r`$-process can occur to produce the nuclei with $`A>130`$ . In fact, when such nuclei are produced in the neutron star merger model, the heaviest nucleus fissions, thereby providing fission fragments as new seed nuclei to capture neutrons. This results in fission cycling with major production of $`A>130`$ nuclei only .

The above summary of $`r`$-process models appears to suggest that supernovae produce the nuclei with $`A\stackrel{<}{}\mathrm{\hspace{0.25em}130}`$ while neutron star mergers produce those with $`A>130`$. However, observations of abundances of Fe and $`r`$-process elements in old stars show that supernovae rather than neutron star mergers are the major source for $`r`$-process nuclei with $`A>130`$. Only supernovae can contribute Fe to stars. If supernovae also contribute $`r`$-process elements with $`A>130`$ such as Eu, then Eu should be observed along with Fe in old stars. In contrast, if neutron star mergers are the major source for Eu, then Eu should not be observed in very old stars that received Fe contributions from only a small number of supernovae. This is because neutron star mergers are $`10^3`$ times less frequent than supernovae in the Galaxy. Many supernovae must have already occurred to provide Fe to old stars before neutron star mergers could provide Eu. As $`r`$-process elements with $`A>130`$ such as Eu have been observed in stars with Fe abundances corresponding to contributions from very few supernovae, neutron star mergers can be ruled out as the major source for $`r`$-process nuclei with $`A>130`$ .

The above discussion leads to a rather unsatisfactory situation: observations favor supernovae as the major source for $`r`$-process nuclei with $`A>130`$ but current supernova models have difficulty in producing these nuclei. A crucial step in resolving this dilemma is to find some independent observational signatures that also support supernovae as the major source for these nuclei. For example, interaction of supernova neutrinos with the nuclei produced by the $`r`$-process may have left some signatures in the $`r`$-pattern. Supernova neutrinos have average energies of 10–25 MeV. So neutrino interaction can highly excite the neutron-rich $`r`$-process nuclei, which can then deexcite through neutron emission. It was shown that the solar $`r`$-process abundances of the nuclei with $`A=183`$–187 can be completely accounted for by neutrino-induced neutron emission from the nuclei in the $`A195`$ peak (see Fig. 3) . In addition, supernova neutrinos may induce fission of the $`r`$-process nuclei in and above the $`A195`$ peak. This would produce fission fragments below and above $`A=130`$ but very few fragments with $`A130`$, which can account for the $`r`$-patterns observed in two old stars .

## 5 CONCLUSIONS

In conclusion, a full understanding of the $`r`$-process depends on a lot of nuclear physics input. Neutron separation energies and capture cross sections and $`\beta `$-decay rates for some key nuclei such as 195Tm are needed to establish the validity of the waiting-point approximation. Accurate mass measurements for extremely neutron-rich nuclei are needed to quantify the effects of neutron shell strength on production of the nuclei below the $`A130`$ and 195 peaks. Finally, branching ratios of neutron emission and fission and fission yields for highly-excited neutron-rich nuclei are needed to understand the effects of supernova neutrinos on the $`r`$-pattern.


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# Antilocalization in gated 2D quantum well structures with composition gradient

## I Introduction

An asymmetry of the quantum well leads to splitting of the energy spectrum due to spin-orbit interaction. The inversion asymmetry of the crystal field results in linear and cubic in quasimomentum terms in the energy spectrum and thus leads to so called Dresselhaus spin-orbit splitting.Mindress  The dispersion law for the heterostructure grown in  direction looks in this case as follows

$$E(k,\phi )=\frac{k^2}{2m}\pm \sqrt{\mathrm{\Omega }_1^2+\mathrm{\Omega }_3^2+2\mathrm{\Omega }_1\mathrm{\Omega }_3\mathrm{cos}(4\phi )},$$
(1)
where $`\mathrm{\Omega }_1=\gamma k\left(k_z^2k^2/4\right)`$, $`\mathrm{\Omega }_3=\gamma k^3/4`$, $`k^2=k_x^2+k_y^2`$, $`\mathrm{tan}\phi =k_x/k_y`$, $`k_z^2`$ is the mean square of electron momentum in the direction perpendicular to 2D plane, and $`\gamma `$ is the constant of spin-orbit interaction, which depends on the band parameters of the bulk material.

An asymmetry of smooth electrostatic potential in the perpendicular to the 2D plane direction due to Schottky barrier or due to asymmetry in disposition of doping layers gives linear term or, so called, the Rashba term:Bychkov

$$E(k)=\frac{k^2}{2m}\pm \mathrm{\Omega }_R,$$
(2)
where $`\mathrm{\Omega }_R=\alpha |k|`$. The value of parameter $`\alpha `$ can be found within framework of $`kP`$-formalism:

$$\alpha =\frac{P^2}{3}\mathrm{\Psi }(z)\left|\frac{d}{dz}\left(\frac{1}{E_FE_{\mathrm{\Gamma }_7}(z)}\frac{1}{E_FE_{\mathrm{\Gamma }_8}(z)}\right)\right|\mathrm{\Psi }(z),$$
(3)
where $`\mathrm{\Psi }(z)`$ is the wave function for the confined electrons, $`P`$ is the momentum matrix element, $`E_F`$ is the Fermi energy, and $`E_{\mathrm{\Gamma }_7}(z)`$ and $`E_{\mathrm{\Gamma }_8}(z)`$ are the positions of the band edges energies for $`\mathrm{\Gamma }_7`$ and $`\mathrm{\Gamma }_8`$ valence bands, respectively, at position $`z`$.

As seen from Eq. (3) an appropriate disposition of the doping layers and quantum well, in principle, gives a possibility to engineer the value of the spin splitting. Another way to change the splitting is a variation of composition within the quantum well in the growth direction.

One of suitable way to study the spin splitting of the energy spectrum at zero-magnetic field is analysis of the weak antilocalization. This paper is devoted to experimental study of the low magnetic field positive magnetoresistance caused by the spin relaxation in GaAs/InxGa1-xAs/GaAs quantum wells.

## II Experimental details

The quantum well GaAs/InxGa1-xAs/GaAs heterostructures were grown by metal-organic vapor phase epitaxy on semi-insulator GaAs substrate. Two types of heterostructures were measured.

Asymmetric heterostructure 3635 consists of a 0.3 $`\mu `$m-thick undoped GaAs buffer layer, a 30 nm InxGa1-xAs well, a 15 nm spacer of undoped GaAs, a Si $`\delta `$-layer and 200 nm cap layer of undoped GaAs. The concentration of In within the quantum well varies from $`0.1`$ to $`0.6`$ from the buffer to cap as $`0.6/[60.17(z+245)]`$, where $`z`$ is the coordinate perpendicular to the quantum well plane, measured in nanometers \[upper panel in Fig. 1(a)\]. The energy diagram calculated for this structure is presented in lower panel in Fig. 1(a) The electron density $`n`$ and mobility $`\mu `$ are the following: $`n=8\times 10^{15}`$ m-2, $`\mu =2.4`$ m2/Vs.

Heterostructures 3512 and Z76 are symmetric. The heterostructure 3512 consists of 0.5 mkm-thick undoped GaAs epilayer, a Sn $`\delta `$-layer, a 9 nm spacer of undoped GaAs, a 8 nm In0.2Ga0.8As well, a 9 nm spacer of undoped GaAs, a Sn $`\delta `$-layer, and a 300 nm cap layer of undoped GaAs. The electron density and mobility are the following: $`n=9.5\times 10^{15}`$ m-2, $`\mu =1.4`$ m2/Vs. The energy diagrams for structure 3512 is presented in Fig. 1(b). The structure Z76 is analogous. The only difference is thickness of spacer between the Sn $`\delta `$-layers and quantum well, which is 12 nm. The parameters of this structure are $`n=6.2\times 10^{15}`$ m-2 and $`\mu =2.4`$ m2/Vs.

The samples were mesa etched into standard Hall bars and then an Ag or Al gate electrode was deposited by thermal evaporation onto the cap layer through a mask. Varying the gate voltage $`V_g`$ we were able to control the density and conductivity of electron gas in the quantum well. The low field magnetoresistance was measured with step $`10^2`$ mT within the temperature range $`0.455.0`$ K.

## III Results and discussion

Figure 2 shows the low-field magnetoconductivity $`\sigma (B)=\rho _{xx}^1(B)`$ measured for the structure 3635 as a function of magnetic field $`B`$ for different temperatures. The antilocalization minimum in low fields, which magnitude decreases with temperature increase, is clearly seen.

The data treatment was performed using the model developed by Iordanskii, Lyanda-Geller, and Pikus (ILP),ILP  which took into account both linear and cubic in $`k`$ terms in the energy spectrum. Within framework of this theory four characteristic magnetic fields describe the behavior of interference induced magnetoresistance in the presence of spin relaxation. They are two standard parameters: $`B_{tr}=\mathrm{}/(4eD\tau )`$ and $`B_\varphi =\mathrm{}/(4eD\tau _\varphi )`$, where $`D`$ is the diffusion coefficient, $`\tau `$ and $`\tau _\varphi `$ are the momentum and phase relaxation time, respectively, and two additional parameters relevant to spin relaxation: $`B_{so}=\mathrm{}/(4eD\tau _s)`$ and $`B_{so}^{}=\mathrm{}/(4eD\tau _s^{})`$ with $`\tau _s=\left(2\mathrm{\Omega }^2\tau _1+2\mathrm{\Omega }_3^2\tau _3\right)^1`$, and $`\tau _s^{}=\left(2\mathrm{\Omega }^2\tau _1\right)^1`$. Here, $`\mathrm{\Omega }`$ is equal to $`\mathrm{\Omega }_R`$ or $`\mathrm{\Omega }_1`$, and $`\tau _1`$ and $`\tau _3`$ are the transport relaxation times introduced as $`\tau _i^1=(1\mathrm{cos}i\theta )W(\theta )𝑑\theta `$, where $`W(\theta )`$ is the probability of the scattering per angle $`\theta `$ per unit time (note, $`\tau _1=\tau `$). The value of $`B_{tr}`$ was found in the ordinary way using the results of Hall and conductivity measurements. The other three parameters are in principle free and can be used as the fitting ones. However, our analysis shows that the experimental data for structure 3635 are in excellent agreement with ILP-expression under the condition $`B_{so}=B_{so}^{}`$ \[see Fig. 2\]. The temperature dependences of $`\tau _\varphi `$ and $`\tau _s`$ for $`V_g=0`$ are presented in Fig. 3(a). It is seen that the fitting parameter $`\tau _s`$ is independent of $`T`$ that corresponds to the Dyakonov-Perel mechanism of spin relaxation.MinDP  The temperature dependence of $`\tau _\varphi `$ is close to the $`T^1`$-law predicted by conventional theory for the temperature dependence of the phase relaxation time when the dephasing is caused by inelasticity of electron-electron interaction. Such a natural behavior of $`\tau _s`$ and $`\tau _\varphi `$ with temperature allows us to believe that we have experimentally obtained the phase and spin relaxation times.

The fact that the fitting procedure does not fail at $`B_{so}=B_{so}^{}`$ means that the main contribution to antilocalization comes from the linear in $`k`$ term. In order to understand what mechanism, Rashba or Dresselhaus, is responsible for the energy splitting resulting in the spin relaxation, we have performed self-consistent calculations of the electron energy spectrum within framework of $`kP`$-model.

Let us start with consideration of the Rashba mechanism. It is not so difficult to obtain rather reliable theoretical results in this case because the heterostructure geometry and all the material parameters are known. Figure 3(b) shows the electron density dependences of the energy splitting obtained experimentally as $`\mathrm{\Delta }=\mathrm{}/\sqrt{2\tau \tau _s}`$ together with the results of calculations of $`\mathrm{\Omega }_R`$. It is seen that the theoretical values of the splitting is strongly less than experimental ones in whole electron density range. From the first sight it seems unnatural because the structure 3635 was grown with strong In-gradient within the quantum well. However our analysis shows that the contribution of inclined part of the well (see Fig. 1(a)) to the splitting is compensated by that of the right-side abrupt InGaAs/GaAs interface. This effect takes place due to insufficient height of the right-side barrier that results in strong penetration of the wave function into it. Thus, we conclude that not Rashba effect is responsible for the antilocalization in the structure 3635.

To calculate the energy splitting caused by the Dresselhaus effect one needs to know the value of parameter $`\gamma `$. This parameter is expressed through seven (!) band parameters of the volume material.Knap  Not all of them are known with high enough accuracy, therefore, we have obtained the parameter $`\gamma `$ experimentally. For this purpose we have used the experimental results obtained for the structures Z76 and 3512. For these structures it was impossible to fit satisfactorily the experimental $`\sigma `$-versus-$`B`$ curves by ILP-formula under the condition $`B_{so}=B_{so}^{}`$. This means that both linear and cubic in $`k`$ terms contribute to antilocalization in these structures. To simplify the fitting procedure in this case we did not consider the parameters $`B_{so}`$ and $`B_{so}^{}`$ as independent ones. We supposed that they were interrelated via the energy spectrum and scattering anisotropy in accordance with their definition: $`B_{so}/B_{so}^{}=1+\mathrm{\Omega }_3^2\tau _3/(\mathrm{\Omega }^2\tau _1)`$, where $`\mathrm{\Omega }`$ stands for $`\mathrm{\Omega }_1`$ or $`\mathrm{\Omega }_R`$. The ratio $`\mathrm{\Omega }_3/\mathrm{\Omega }`$ was chosen equal to that found from the calculation of the energy spectrum. The ratio $`\tau _3/\tau _1`$ was from the range $`0.5\mathrm{}0.7`$ depending on the scattering anisotropy which in its turn depended on the electron density. The best fit of $`\sigma `$-versus-$`B`$ curves has been achieved when $`\mathrm{\Omega }=\mathrm{\Omega }_1`$ that points to the fact that the main contribution to the spin relaxation comes from the Dresselhaus effect. The final results of such a data processing for structures Z76 and 3512 are shown in Fig. 4(a) by symbols. Comparing the experimental and calculated electron density dependences of $`\mathrm{\Omega }_1`$ and $`\mathrm{\Omega }_3`$ we have found that the best agreement between theory and experiment is achieved for $`\gamma =18`$ eV Å3 (lines in Fig. 4(a)). An overall error in determination of $`\gamma `$ can be estimated as $`\pm 2`$ eV Å3. Finally we can return to the results obtained for the structure 3635. Figure 4(b) demonstrates satisfactory agreement between experimental data and results calculated with just the same value of $`\gamma =18`$ eV Å3.

Comparing Figs. 4(a) and 4(b) one can see that the $`\mathrm{\Omega }_3`$ to $`\mathrm{\Omega }_1`$ ratio is close for both symmetric and asymmetric structures. The reasonable question arises in this connection: why does not the cubic in $`k`$ splitting contribute to the antilocalization in structure 3635? From our point of view one of possible reason is that the doped layer is more spaced from the quantum well in this structure as compared to the other structures. This results in smoother scattering potential and stronger scattering anisotropy which in its turn determines the relative contribution of cubic and linear terms in antilocalization via $`\tau _3`$ to $`\tau _1`$ ratio.

## IV Conclusion

We have investigated the antilocalization caused by the spin-orbit interaction in GaAs/InxGa1-xAs/GaAs quantum wells with and without gradient of indium content in growth direction. It has been found that the Dresselhaus effect is responsible for antilocalization in both types of the heterostructures. The comparison of experimental data with the results of self-consistent calculations allows us to determine reliably the value of $`\gamma `$ parameter: $`\gamma =(18\pm 2)`$ eVÅ3.

This work was supported in part by the RFBR through Grants No. 01-02-17003, No. 03-02-16150, and No. 03-02-06025, the INTAS through Grant No. 1B290, the CRDF through Grant No. REC-005, the Program University of Russia through Grant No. UR.06.01.002.