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# Spin Polarization of the Low Density 3D Electron Gas

## I Introduction

The three dimensional homogeneous electron gas, also known as the fermion one component plasma or jellium, is one of the simplest realistic models in which electron correlation plays an important role. Despite years of active research, the properties of thermodynamic phases of the electron gas are still not known at intermediate densities. In this paper, we study the spin polarization phase transition of the three dimensional electron gas at zero temperature with recently improved quantum Monte Carlo methods.

There has been recent interest in the low density phases spurred by the observation of a ferromagnetic state in calcium hexaboride (CaB6) doped with lanthium. The magnetic moment corresponds to roughly 10% of the doping density. The temperatures (600K) and densities ($`7\times 10^{19}/cm^3`$) of this transition are in rough agreement with the predicted transition in the homogeneous electron gas.. However, to make a detailed comparison, it is necessary to correct for band effects. For example, conduction electrons are located at the X-point of the cubic band structure and thus have a six-fold degeneracy. The effective mass of electrons at this point and the dielectric constant are also changed significantly from their vacuum values. These effects cast doubt on the viability of the electron gas model to explain the observed phenomena. Excitonic models have been proposed to explain the ferromagnetism. Whatever the interpretation of ferromagnetism in $`CaB_6`$, the determination of the polarization energy of the electron gas is important problem because of the importance of the model.

The ground state properties of the electron gas are entirely determined by the density parameter $`r_s=a/a_0`$ where $`4\pi \rho a^3/3=1`$ and $`a_0`$ is the bohr radius, possibly changed from its vacuum value by band effects. In effective Rydbergs, the Hamiltonian is :

$$H=\frac{1}{r_s^2}\underset{i=1}{\overset{N}{}}_i^2+\frac{2}{r_s}\underset{i<j}{}\frac{1}{\left|𝐫_i𝐫_j\right|}+const.$$
(1)
Note that the kinetic energy scales as $`1/r_s^2`$ and the potential energy scales as $`1/r_s`$ so that for small $`r_s`$ (high electronic density), the kinetic energy dominates, and the electrons behave like ideal gas; in the limit of large $`r_s`$, the potential energy dominates and the electrons crystallize into a Wigner crystal. There is a first order freezing transition at $`r_s100`$.

Considering now the spin degrees of freedom, at small $`r_s`$, electrons fill the Fermi sea with equal number of up spin and down spin electrons to minimize the total kinetic energy and thus the total energy; the system is in the paramagnetic state. As the density decreases and before the freezing transition, there is a possibility that the electrons become partially or totally polarized (ferromagnetic). The spin polarization is defined as $`\zeta =\left|N_{}N_{}\right|/N`$, where $`N_{}`$ and $`N_{}`$ are the number of up and down spin electrons, respectively and $`N=N_{}+N_{}`$. For paramagnetic phase $`\zeta =0`$ and for ferromagnetic phase $`\zeta =1`$.

This polarization transition was suggested by Bloch who studied the polarized electronic state within the Hartree-Fock (HF) approximation. He found the ferromagnetic state favored over paramagnetic state for $`r_s>5.45`$, almost within the density of electrons in metals. However, HF is not accurate for $`r_s>0`$.

More accurate energies became available with the development of Monte Carlo methods for many-fermion systems. Ceperley using Variational Monte Carlo with a Slater-Jastrow trial function determined that the transition between the polarized and unpolarized phase occured at $`r_s=26\pm 5`$. Using a more accurate method, diffusion Monte Carlo (DMC), it was estimated that the polarized fluid phase is stable at $`r_s=75\pm 5`$. An extension to this work found the $`\zeta =0.5`$ partially polarized fluid becomes stable at roughly $`r_s20`$ and the completely polarized state never stable.

Recently Ortiz et al. applied similar methods to much larger systems ($`N1930`$) in order to reduce the finite-size error. They concluded the transition from the paramagnetic to ferromagnetic transition is a continuous transition, occurring over the density range of $`20\pm 5r_s40\pm 5`$, with a fully polarized state at $`r_s40`$.

Due to the very small energy differences between states with different polarizations, systematic errors greatly affect the QMC results. Recent progress in the quantum simulation methods makes it possible to reduce these errors. Kwon et al. found that a wavefunction incorporating back-flow and three-body (BF-3B) terms provides a more accurate description: they obtained a significantly lower variational and fixed-node energy. In another advance of technique, twist-averaged boundary conditions (TA) have been shown to reduce the finite-size error by more than an order of magnitude, allowing one to obtain results close to the thermodynamic limit using results for small values of $`N`$. In this paper, we apply these improved methods to the polarization transition in the three dimensional electron gas. We first describe the simulation method, and then, the results.

## II Methods

The most accurate Quantum Monte Carlo (QMC) method at zero temperature is Projector or Diffusion Monte Carlo (DMC): one starts with a trial function and uses $`\mathrm{exp}(tH)`$ to project out the ground state using a branching random walk. Fermi statistics pose a significant problem for the projection method, since exact fermion methods such as transient estimate or release-node QMC suffer an exponential loss of efficiency for large numbers of particles. For this reason, the fixed-node approximation is normally used, obtaining the best upper bound to the energy consistent with an assumed sign of the wave function. The generalization of the fixed-node method to treat complex-valued trial functions is known as the fixed-phase approximation.

In the simpler, but less accurate Variational Monte Carlo method (VMC), one assumes an analytic form for a trial function $`\mathrm{\Psi }_T(R)`$ and samples $`|\mathrm{\Psi }_T(R)|^2`$ using a random walk. An upper bound to the exact ground state energy is the average of the local energy $`E_L(R)=\mathrm{\Psi }_T(R)^1\mathrm{\Psi }_T(R)`$ over the random walk.

The trial wavefunction plays a very important role in these two methods. With a better trial wavefunction, not only is the variational energy lower and closer to the exact energy, but also the variance of the local energy is smaller so that it takes less computer time to reach desired accuracy level. The trial wavefunction is also important in fixed-phase DMC because the solution is assumed to have the same phase as the trial function. One then solves for the modulus. This implies that the DMC energy lies above the exact ground state energy by an amount proportional to the mean squared difference of the phase of the trial function from the exact phase. As this is the only uncontrolled approximation, it is important to carefully optimize the assumed trial wavefunction.

For a homogeneous system, the non-interacting (NI) wavefunction consists of a Slater determinant of single-electron plane waves orbitals. To incorporate electron correlation, one multiplies the NI wavefunction by a pair wavefunction, obtaining the so-called Slater-Jastrow (SJ) form. To construct a better trial function, one incorporates backflow and three-body effects. The particle coordinates appearing in the determinant become quasi-particle coordinates:

$$𝐱_i=𝐫_i+\underset{ji}{\overset{N}{}}\eta (r_{ij})(𝐫_i𝐫_j).$$
(2)
The Slater determinant is then $`D=det(e^{i𝐤_m𝐱_n})`$ where $`\eta (r_{ij})`$ is a function to be optimized. Then the backflow-three body wavefunction (BF-3B) is:

$$\mathrm{\Psi }_T(R)=D_{}D_{}\mathrm{exp}\left(\underset{i<j}{\overset{N}{}}\stackrel{~}{u}(r_{ij})\frac{\lambda _T}{2}\underset{i=1}{\overset{N}{}}𝐆_i^2\right)$$
(3)
where

$$𝐆_i=\underset{ji}{\overset{N}{}}\xi (r_{ji})(𝐫_j𝐫_i)$$
(4)
and

$$\stackrel{~}{u}(r)=u^{RPA}(r)\lambda _T\xi ^2(r)r^2+\gamma (r).$$
(5)
Here $`D_{}`$ and $`D_{}`$ are determinants for the up spin and down spin electrons, $`\xi (r)`$ is the three-body correlation function, and $`\stackrel{~}{u}`$ is the Jastrow correlation function. For the electron gas an accurate analytic form, $`u^{RPA}(r)`$, has as low an energy as those with optimized parameters. In the presence of three-body correlation, the RPA two-body term is supplemented with an extra Gaussian function $`\gamma (r)`$. Please refer to Kwon et al. for further details concerning this wavefunction. We used optimized Ewald sums  both for the potential and for the correlation factor so as to have the correct long wavelength behavior.

Though the computational cost for BF-3B wavefunction is somewhat greater than the simple SJ wavefunction and there is the added cost of optimization for BF-3B wavefunction, we found accurate trial wavefunctions crucial to compute the small energy differences between different polarization states. We optimized the parameters by minimizing a combination of the energy and the variance for each density and polarization. Figure (1) shows the energy vs. polarization at $`r_s=50`$ using different trial functions and simulation methods. The SJ trial function with VMC has the highest energy for all polarizations and at this level of accuracy finds the fully polarized phase to be stable, in agreement with earlier VMC calculations. However, using the best BF-3B trial function, the variational energies are lowered significantly with the unpolarized energy dropping more than the polarized case so that the polarized phase is no longer stable. DMC calculations confirm this result. Note that the DMC energies determined using the NI phases (or nodes) give energies lower than the BF-3B variational energies confirming the importance of accurate DMC calculations. The use of BF-3B wavefunctions with DMC leads to the lowest ground state energies, hopefully, very close to the exact energy.

After the effect of the nodes, the dependence of the energy on the number of electrons is the largest systematic error. Within periodic boundary conditions (PBC), the phase picked up by the wavefunction as a particle makes a circuit across the unit cell, is arbitrary. General boundary conditions are:

$$\mathrm{\Psi }(𝐫_1+L,𝐫_2,\mathrm{})=e^{i\theta }\mathrm{\Psi }(𝐫_1,𝐫_2,\mathrm{})$$
(6)
where $`L`$ is a lattice vector of the supercell. If the twist angle $`\theta `$ is averaged over, most single-particle finite-size effects arising from shell effects in filling the plane wave orbitals, are eliminated. This is particularly advantageous for polarization calculations since shell effects dominate the polarization energy. The extra effort in integrating over the twist angles is minimal, since the various calculations all serve to reduce the final variance of the computed properties. The effect of boundary conditions is examined in detail in Lin et al.

There is a further size effect in the calculation of the potential energy due to a charge interacting with its correlation hole in neighboring supercells as shown in Fig. (6) of Lin et al.. To correct this, we fit the energies versus $`N`$ using the expansion:

$$E_N=E_{\mathrm{}}+\frac{a_1}{N}+\frac{a_2}{N^2}+\mathrm{}.$$
(7)
For unpolarized systems, the fitted $`E_{\mathrm{}}`$ agrees with the previous non-twist averaged (PBC) result determined using extrapolations based on fermi liquid theory (FLT). As shown in Fig. 2, the correlation hole is only weakly dependent on spin polarization at low density: the peak of $`g(r)`$ only changes from 1.175 to 1.190 as the system goes from unpolarized to polarized. Hence, the potential size-effect hardly changes the spin polarization energy. Fig. 3 shows the polarization energies for $`N=54,108,162`$. With TA boundary conditions, there is a remarkable insensitivity to the number of electrons. Even though the system size is increased threefold, the change in the energy versus polarization is almost undetectable. Considering only the leading $`1/N`$ correction, we estimated $`E_{\mathrm{}}`$ with $`N=54`$ and $`N=108`$.

Also shown in Fig. 3 is the estimate of the polarization energy from Ceperley-Alder. In that work, size effects were estimated with Fermi liquid corrections. Rather than BF-3B wavefunctions, corrections using the potentially exact, release-node method were used. The results with PBC and FN-DMC are in agreement with the present FP-DMC calculations. However, the present results have an error bar more than an order of magnitude smaller than those of Ceperley-Alder, primarily due to increased computer performance.

Though PBC with FLT corrections are adequate for unpolarized and fully polarized systems, the precision is limited for intermediate polarizations. To estimate finite size effects within FLT, one must perform accurate DMC simulations for widely varying system sizes. In Ortiz et al., the simulation size varied from $`725N1450`$. Within DMC it is very time-consuming to ensure uniform accuracy independent of particle number, so that one typically determines size effects within VMC, using the more approximate SJ trial functions. As we have seen in Fig. (1), the SJ trial functions are unreliable at low densities. TA boundary conditions allow a much better way to estimate energies in the thermodynamic limit of partially polarized fermi liquids since the number of electrons can be held fixed as the spin polarization varies. Small system sizes, allowing use of more accurate but expensive trial functions and even exact fermion methods, give precise estimates of the spin polarization energy in the thermodynamic limit.

In Fig. 4 we compare the total energy for $`r_s=40`$ calculated with DMC and TA and extrapolated to the thermodynamic limit with the calculation of much larger systems ($`N=725`$) of Ortiz et al.  The BF-3B energies are lower energy and show a different polarization energy: Ortiz’s calculation finds that the polarized or partially polarized phase is stable at this density, while we find the unpolarized phase is stable. This difference is due to the backflow correlations in the trial wavefunction. Although backflow energies are small, they favor the unpolarized state and hence are crucial for accurate determination of the polarization transition.

## III Results

We carried out computations of the spin polarization energies at electronic densities $`40r_s100`$. At each density, we performed DMC calculations with $`N=54`$ and $`N=108`$ electrons using $`10^3`$ twist angles. The time step was adjusted so that the DMC acceptance ratio was in the range $`98\%99\%`$. Note that when calculating the polarization energy, most time step errors will cancel out of the polarization energy. Thus systematic errors in the polarization energy are much smaller than in the total energy. We then extrapolated the energy to the thermodynamic limit using Eq. (7). The energies are given in Table I.

We then fit the energy versus polarization to a quadratic polynomial in $`\zeta ^2`$. The results are shown in figure 5. A polarization transition is evident. At $`r_s=40,`$ the system is still paramagnetic, with the unpolarized phase stable. As the density decreases, at $`r_s50,`$ the system becomes unstable with respect to spin fluctuations. The partially polarized states become stable at $`r_s60.`$ As the electronic density continues to decrease, the fully polarized state has a lower energy with respect to unpolarized state at $`r_s80`$, however, we find that the partially polarized state has an even lower energy.

In Fig. 6 is shown the predicted square of the optimal polarization versus density. We find that the equilibrium polarization is described by $`\zeta ^2=(r_sr_s^{})/62`$ with the critical density $`r_s^{}=50\pm 2`$. As the density decreases, the stable state becomes more and more polarized approach fully polarized at freezing, $`r_s100`$. Quantum critical fluctuations, not present in systems with $`N162`$, could modify the behavior of the spin polarization energy near the critical density.

The quoted error bar on the critical density estimates the statistical errors, not the systematic errors arising from the fixed-phase approximation. The experimental and theoretical results on polarized helium give caution on placing too much confidence in the estimate of the polarization transition. Even using the accurate optimized BF-3B wavefunctions, the magnetic susceptibility in liquid 3He does not agree with experiment at low pressure and the polarized phase is nearly degenerate with the unpolarized phase at the freezing density. The present results also do not preclude the existence of phases with other order parameters such as superfluids, as occurs in ground state of liquid 3He. In fact, it is rather likely that the ground state of the electron gas will have such a phase at the lowest fluid densities.

However, examination of the variance of the trial function suggests that the result for the electron gas may be more reliable than for liquid 3He. Shown in fig. 7 is the variance of the trial function at $`r_s=50`$ for both the SF and BF-3B functions. Although the variance of the SJ trial function depends on spin polarization, that of the BF-3B does not. Such is not the case with liquid 3He. Arguments based on variance extrapolation suggest that the DMC calculations with BF-3B phases should be more reliable than in liquid 3He.

## IV The Phase Diagram

One can use the calculated energies to estimate the finite temperature behavior within the Stoner model, arising in the theory of itinerant magnetism. The Stoner model differs from Hartree-Fock by replacing the Coulomb interaction by a zero range one, a repulsive delta function potential: $`_{i<j}g\delta (r_{ij})`$. One can view this approach as the first step to a full Fermi-liquid description of the quasiparticle interactions, and use the QMC data to determine the strength of those interactions. One expects that the Slater-Jastrow trial function has screened off the long-range interaction leaving only a short-ranged spin-dependent term that can be modeled by a contact interaction.

In the Stoner model, the energy is evaluated within the mean field (Hartree-Fock) approximation using the NI wavefunction. The energy at zero temperature in the thermodynamic limit is:

$$E(1+\zeta )^{5/3}+(1\zeta )^{5/3}+0.054gr_s^2(1\zeta ^2).$$
(8)
For $`gr_s^2<20.5`$ the system has an unpolarized ground state and for $`gr_s^2>24.4`$ the ground state is ferromagnetic. For intermediate couplings, the ground state has a partial spin polarization at zero temperature, similar to the observed behavior of the electron gas at low density.

Although the polarizations are qualitatively correct, the above functional form does not fit well the DMC data (i.e. from Table I.) In addition, assuming $`g`$ does not have a very strong density dependence, the Stoner model predicts that the partially polarized density range should be quite narrow, from $`50r_s54`$, while as the QMC results indicate a much broader density range. Perhaps the assumption of a zero-range interaction of quasiparticles is too restrictive.

Nevertheless, we use this mean field model to make a estimate of the transition temperature of the polarized phase. Fitting the energy to the function given in Eq. (8), we obtain estimates of $`g`$ and the effective mass of the electrons. Then, using the free energy of the ideal spin (1/2) partially polarized fermi gas with the additional spin interaction, we estimate the temperature at which the system becomes polarized by determining when the spin-stiffness of the unpolarized system vanishes. Fig. 8 is the estimated phase diagram of the electron gas. In this diagram, the effective mass and dielectric constant for $`SrB_6`$, a closely related material to $`CaB_6`$, have been used to convert to units of $`K`$ and $`cm^3`$. Note that both the temperatures and densities of our calculated magnetic transition are four orders of magnitude smaller than that found experimentally in $`CaB_6`$. Even assuming errors because of uncertainties in material properties and from the mean field methods to estimate $`T_c`$, these estimates are very difficult to reconcile with experiment, apparently ruling out an electron gas model of ferromagnetism in this material. Also plotted on the phase diagram is the energy difference between the partially polarized fluid and the unpolarized fluid as another estimate of the magnetic transition temperature. Finite temperature QMC calculations would be desirable to confirm the mean field estimate of $`T_c`$. A rough estimate of the limit of stability of the Wigner crystal  is also shown.

Tanaka and Ichimaru have computed the polarization phase diagram of the electron gas both at zero and non-zero temperature using an integral equation method. At zero temperature they obtain a result similar to Ortiz at al., with a continuous transition at $`r_s20`$ and a fully polarized fluid state at a slightly higher density $`r_s22`$. Apparently this approach, built on local field corrections to free fermion response functions, is biased by the initial Hartree-Fock assumption and overemphasizes the tendency for ferromagnetism.

There is recent work on the low density electron gas in 2D, studying both the Fermi liquid and the Wigner crystal phase. Using QMC similar techniques in the liquid phase, a polarized phase is found to be stable between $`26r_s35`$, though the energy differences are even smaller than in 3D. The partially polarized phase is never stable. In the 2D Wigner crystal, path integral methods were used to derive directly the spin Hamiltonian. It was found that the ground magnetic state is a spin liquid though the ferromagnetic state has only a slightly higher energy at melting. Analogous calculations of the magnetic phase diagram of the WC in 3D are underway.

## V Conclusion

We studied the polarization transition in three dimensional electron gas using twist-averaged boundary conditions and trial functions with backflow and three body correlations. Twist averaged boundary conditions have a much reduced systematic finite-size error, especially for the calculation of polarization energies, enabling size-converged results with fewer electrons. Using relatively small system sizes allows one to use more accurate trial wavefunctions and to fully converge the diffusion Monte Carlo calculations. We find a second order transition to a polarized phase at $`r_s=50\pm 2`$.

In general, methods based on the variational principle such as the fixed-node quantum Monte Carlo method for many-fermion systems, favor phases with a higher symmetry, in this case the Wigner crystal and polarized fluid, over the more complicated unpolarized phase, (effectively a two-component mixture of spin up and down electrons.) Recall that in HF one has a polarization transition because antisymmetry is the only way to correlate electrons, however, the correlation is only between like spins; hence, there is an instability to polarize the system once the potential is dominant. But using a SJ wavefunction both like and unlike electrons are highly correlated. Our results demonstrate that the SJ wavefunctions still preferentially favors the “simple” phases, even using DMC method. This symmetry argument explains the historical tendency for the polarized phase become stable over a more and more restricted range of density and temperature as more accurate methods are used. Our QMC results using the BF-3B wavefunction indicate that there is still an instability for spin polarization at very low density. Although examination of the variance indicates that the polarized and unpolarized BF-3B trial functions are equally inaccurate, it is still not clear if our finding of a polarization transition is an artifact of the assumed trial wavefunction. Calculations with the new methods (TA and BF-3B wavefunctions) but with the exact fermion methods are desirable to resolve the phase of the electron gas at intermediate densities.

###### Acknowledgements.

This research was supported by NSF DMR01-04399, the Department of Physics at the University of Illinois Urbana-Champaign and the CNRS. We acknowledge unpublished data from G. Ortiz shown in fig. (3). Computational resources were provided by the NCSA.


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# Van Hove features in Bi2Sr2CaCu2O8+δ and effective parameters for Ni impurities inferred from STM spectra

(submitted to PRB on 3 May 2002)

## Abstract

We present a detailed quantitative comparison between theoretical calculations of the local density of states and recent experimental measurements of scanning tunneling spectra around Ni impurities in Bi2Sr2CaCu2O8+δ. A double-peak structure on the hole side of the spectrum at the Ni site is identified as the spin-split van Hove singularity in the band structure. The Ni atom induces local changes in hopping matrix elements comparable in size to the induced on-site spin-dependent potential. We find evidence from the measurements of order parameter suppression in the vicinity of the Ni impurity. These extracted impurity parameters can be of use in quantitative calculations of macroscopic response properties, such as the AC conductivity.

The response of a superconductor to impurities can determine several macroscopic electromagnetic properties, such as the magnetic penetration depth and high frequency losses.Tinkham (1995) For high-temperature superconductors it is advantageous to study the impurity problem in real space rather than in momentum space,Flatté and Byers (1999) not only because the impurities destroy the translational invariance, but also because these doped systems are intrinsically inhomogeneous.Pan et al. (2001) High-quality electronic spectra, using the technique of scanning tunneling microscopy (STM), around individual impurity atoms in superconducting Bi2Sr2CaCu2O8+δ have recently become available.Pan et al. (2000); Hudson et al. (2001) Quantitative comparison between calculations of the local density of states (LDOS) and these STM measurements can lead to effective impurity parameters that are useful for calculating macroscopic properties.

A number of theoretical studies of the STM spectra near impurities in $`d`$-wave superconductors have already been carried out by various authors.Byers et al. (1993); Salkola et al. (1996); Flatté and Byers (1998, 1999); Haas and Maki (2000); Flatté (2000); Polkovnikov et al. (2001); Zhu and Ting (2001) These previous studies focused on qualitative features, such as the existence of quasiparticle resonances, the spatial structure of the resonances, and the differences among systems with various pairing symmetries. Often the model for an impurity only consisted of effective potentials at the impurity site, or relied on an unrealistic band structure for the host superconductor. There are still significant quantitative disagreements between the theoretical and experimental LDOS.Flatté (2000); Polkovnikov et al. (2001); Zhu and Ting (2001) Of the types of impurities and defects for which high-quality STM spectra are available, the Ni impurity provides a good opportunity to resolve some of these issues. Because the perturbation to the local environment caused by a Ni impurity is weak,Hudson et al. (2001); Flatté (2001) we find that, with some extensions to the potential model the STM spectra can be well reproduced by our calculations. In addition to the short-ranged potentials at the impurity site, we also include the change of the hopping matrix elements from the impurity site to its nearest neighbors, and the suppression of the order parameter.

We also find an interesting interplay between the underlying band structure and the superconducting coherence peak near a Ni impurity. In the spectrum of the Ni site there is a large peak on the hole side (below the chemical potential), right outside the gap edge. We find that this peak, previously thought as the remnant of the coherence peak, is largely contributed by a density-of-states peak in the underlying band structure. One special and important feature of hole doped cuprate superconductors is that a van Hove singularity is close to the Fermi level. It has been suggested by various authorsHirsch and Scalapino (1986); Lee and Read (1987); Labbé and Bok (1987); Friedel (1989); Markiewicz (1990); Getino et al. (1992); Newns et al. (1992) that the existence of the van Hove singularity could affect the mechanism of superconductivity, and also account for the unusual normal state properties. The existence of such a density-of-states peak has received direct support from experiments using angle-resolved photoemission spectroscopy (ARPES).Shen and Dessau (1995); Ma et al. (1995) Despite this density-of-states peak (aside from the coherence peaks) in the superconducting state has never been directly reported in tunneling experiments. Traces of this feature were suggested to explain the asymmetry of the coherence peaks,Renner and Fischer (1995); Bok and Bouvier (1997) and the sharpness of the coherence peaks. However, no specific qualitative influence of a van Hove peak on the midgap impurity resonances of a particular impurity has been considered.Crisan and Tifrea (1999)

We find that the Ni impurity offers a novel probe of the van Hove peak. The van Hove singularity is likely very close to the Fermi level, therefore, in the superconducting state the van Hove peak cannot be resolved from the coherence peak. The Ni impurity will locally suppress the coherence peak, but only weakly perturb the underlying band structure. As a result, the van Hove peak shows up unmasked in the spectrum at the impurity site.

Our calculation is based on the following tight-binding Hamiltonian,

$`H`$ $`=`$ $`{\displaystyle \underset{i,j,\sigma }{}}(t_{ij}+\delta t_{ij})c_{i\sigma }^{}c_{j\sigma }`$ (1)
$`+{\displaystyle \underset{i,j}{}}\left[(\mathrm{\Delta }_{ij}+\delta \mathrm{\Delta }_{ij})c_i^{}c_j^{}+(\mathrm{\Delta }_{ij}^{}+\delta \mathrm{\Delta }_{ij}^{})c_jc_i\right]`$
$`+(V_0+V_S)c_0^{}c_0+(V_0V_S)c_0^{}c_0,`$
where $`i`$ and $`j`$ label sites (the impurity resides at site 0), and $`\sigma `$ labels spin. The hopping matrix elements, $`t_{ij}`$, are taken from a one-band parameterization of the ARPES data.Norman et al. (1995) The numerical values in units of meV are $`148.8`$, $`40.9`$, $`13`$, $`14`$, and $`12.8`$ for the hopping to the first five nearest neighbors. The measured value for the gap maximum $`\mathrm{\Delta }_0`$ at a site away from the impurity is $`28`$ meV.Hudson et al. (2001) The order parameters, $`\mathrm{\Delta }_{ij}`$, are assumed to be real, and to have $`d`$-wave symmetry. They are only non-zero on the bonds between two nearest-neighbor sites, and $`\mathrm{\Delta }_{i,i+\widehat{x}}=\mathrm{\Delta }_{i,i+\widehat{y}}=\mathrm{\Delta }_0/4`$. The momentum-dependent order parameter resulting from a homogeneous system with these $`\mathrm{\Delta }_{ij}`$ is $`\mathrm{\Delta }_𝐤=(\mathrm{\Delta }_0/2)(\mathrm{cos}k_x\mathrm{cos}k_y)`$, where the lattice spacing between two Cu atoms is unity.

Because the experiments were carried out at low temperatures, the spin degree-of-freedom of the magnetic Ni impurity is assumed to be completely frozen. At the Ni site, we use a potential that consists of a magnetic part, $`V_S`$, and a non-magnetic part, $`V_0`$. It is found that the Ni impurity induces a change in the hopping, $`\delta t_{ij}`$, to the nearest neighbor sites, and a suppression of the order parameter magnitudes, $`\delta \mathrm{\Delta }_{ij}`$, on the four bonds connected to the Ni site, and on the other twelve bonds connected to the nearest neighbor sites. A schematic diagram of our model and the fitting parameters used for the Ni impurity are shown in FIG. 1.

Calculations presented here are based on a Koster-Slater technique.Flatté and Byers (1997a, b, 1999) The homogeneous Green’s function, $`𝐠(𝐫_i,𝐫_j,\omega )`$, in the Nambu formalism is first constructed with a $`1`$ meV quasiparticle linewidth. In the presence of an impurity modeled by $`𝐕`$, the Gor’kov equation, $`𝐆=𝐠+\mathrm{𝐠𝐕𝐆}=(𝐈\mathrm{𝐠𝐕})^1𝐠`$, is solved by numerically inverting the matrices. The LDOS is the imaginary part of the Green’s function, $`(1/\pi )\mathrm{Im}\left[𝐆_{11}(𝐫_i,𝐫_i,\omega )𝐆_{22}^{}(𝐫_i,𝐫_i,\omega )\right]`$.

In the following, we will discuss how various parameters influence our calculations. Although six parameters including the chemical potential are introduced in the model, there are particular features in the LDOS spectra associated with each of them. This allows us to determine each parameter largely independently from the others.

Let us first consider the chemical potential. From the ARPES parameterization,Norman et al. (1995) the chemical potential for an optimally doped sample is $`130.5`$ meV. However, we know from STM measurements that the doping concentration is locally varying, and is correlated with the superconducting gap magnitude.Pan et al. (2001) A region with a gap magnitude of $`28`$ meV is overdoped. The fit to STM spectra is optimal if the shift in chemical potential relative to the optimally doped region is about $`25`$ meV. This amount of shift changes the location of the van Hove singularity from $`34`$ meV to $`9`$ meV below the Fermi level, shown in FIG 2(a) for $`\mathrm{\Delta }_{ij}=0`$.Nor  In the superconducting state the van Hove singularity cannot be resolved from the coherence peak at the hole side, shown in FIG 2(b). The chemical potential shift also sharpens the coherence peaks, and contributes to the asymmetry between the two peaks. Although not direct evidence for the van Hove singularity in STM, the agreement between the calculations and the measurements is certainly improved.

We now describe the modeling of the Ni impurity focusing first on the single-site potential model with only the on-site potentials, $`V_0`$ and $`V_S`$. For a weak potential, the main effect of these potential is to set the energies of the resonances. Since the resonance peaks for Ni are at $`9.2`$ and $`18.6`$ meV, and the perturbation from Ni is weak, both $`V_0+V_S`$ and $`V_0V_S`$ should be negative. Our $`V_0`$ does not differ greatly from that found in a simple model.Fehrenbacher (1996) The two on-site parameters, $`V_0`$ and $`V_S`$, are both required to fit the energies of the two resonance peaks.Salkola et al. (1997) Note that we have no control over the peak height or width in the spectra using this simple model. We find, due to extended states within the gap, that the resonance peaks will be broader than the coherence peaks. In the observation, however, the width of the resonance peaks appears comparable, or even sharper, than the coherence peaks.

In order to reduce the coupling to the extended states and increase the localization of the resonance states, we then assume that the hopping to the nearest neighbor sites, $`\delta t_{01}`$, is reduced. With only a $`20\%`$ change in the nearest-neighbor hopping, we can reproduce the linewidth of the resonance peaks. $`V_0`$ and $`V_S`$ must be adjusted slightly when $`\delta t_{01}`$ is introduced in order to keep the resonances at the fixed energies. Our calculations show that the magnitudes of the on-site potentials change to even weaker values, and characterize an even weaker impurity potential. Using these three parameters for calculating the effect of a Ni impurity in the normal state (shown in FIG 2(c)), one can see that the band structure is not highly distorted. The van Hove peak remains reasonably sharp, and splits into two spin components. Comparing 2(c) to the superconducting state, shown in FIG 2(d), we can identify the two peaks on the hole side, right outside the gap edge, as the spin-split van Hove peaks. A similar connection between the normal state electronic structure and an impurity’s influence on the superconducting state has been identified in calculations for impurities in s-wave superconductors.Flatté and Byers (1997a, b) Another distinction between the midgap resonances and the van Hove peaks is that the spin splitting of the resonance peaks inside the gap remains independent of distance from the impurity site. The spin splitting of the van Hove singularity, however, decreases as the distance increases.

Once the large peak at the hole side was identified as the van Hove peak, a noticeable disagreement between the calculation and the data became apparent. The calculated relative energy difference between the resonance peaks and the van Hove peaks is somewhat larger than the observed value if the gap maximum is constant everywhere. In the $`d`$-wave superconducting state, the position of the van Hove peak is dominated by the gap edge. One cannot increase the agreement by tuning $`V_0`$ because that shifts all peaks almost an equal amount of energy. We could obtain good agreement if the gap maximum were about $`22`$ meV instead of $`28`$ meV. In principle using self-consistent calculations can account for the effect, however, the self-consistency conditions involve the pairing mechanism, which is controversial. Taking a phenomenological approach, we can identify the suppression of the order parameter around the impurity from the data. This then becomes a constraint on pairing theory. We find that the parameter is locally suppressed more than $`50\%`$ (See FIG. 1).

So far, we were only fitting the spectrum right at the Ni site. Nevertheless, good agreement in spatial structure is also obtained. Detailed comparisons for the spectra on neighboring sites are shown in FIG. 2(e)–(h), the spatial decay of the resonance peaks is shown in FIG. 3, and the spatial maps at given energies are shown in FIG. 4. These are direct comparisons with the data in FIGs. 2–4 in Ref. 5.

Two key additional features are found from the spatial structure. The first one is that the hole component of the resonance has $`d`$-wave symmetry.Flatté and Byers (1999); Flatté (2001) The second is that the perturbation, due to the van Hove singularity, is strongest along the diagonals of the lattice. At given energy, the secondary peaks are always located at the next-nearest rather than the nearest neighbor sites relative to the main peaks. This is because, around the Fermi level, the saddle points that give rise to the van Hove singularity in the density of states are near the $`(\pm \pi ,0)`$ and $`(0,\pm \pi )`$ points in momentum space. The main contribution to the real space Green’s function largely comes from these high density-of-states regions,

$$𝐠(𝐫_i,𝐫_j,\omega )=\frac{d^2𝐤}{(2\pi )^2}e^{i𝐤(𝐫_i𝐫_j)}𝐠(𝐤,\omega ).$$
(2)
For $`𝐫_i𝐫_j=(\pm 1,\pm 1)`$ the four regions add up constructively, while for $`(\pm 1,0)`$ or $`(0,\pm 1)`$, the contributions from $`(\pm \pi ,0)`$ cancel with those from $`(0,\pm \pi )`$. As a result, $`|𝐠((1,1),(0,0),\omega )||𝐠((1,0),(0,0),\omega )|`$ for energies near the chemical potential. This is also consistent with the larger spin splitting of the van Hove peak at the second nearest neighbors compared to the nearest neighbors.

In this study we have assumed that the STM spectra are directly related to the electronic structure of the Cu–O plane regardless of the presence of the intermediate Bi–O plane. As was argued in Ref. 5, the energies and linewidths of the resonances should be the same. We find the principal effect of a $`d`$-wave filterMartin et al. (2002) on our parameterization is to (roughly) change the sign of $`V_0`$. Therefore, the evidence for the reduction of hopping, and suppression of the order parameter are still clear.

In summary, the presence of a Ni atom on the Cu–O plane produces a weak perturbation to the system. We show direct evidence for a density-of-states peak in the STM measurements and local suppression of the order parameter. The suppression of the order parameter can constrain the self-consistency condition and thus the pairing mechanism.

We thank E. W. Hudson and J. C. Davis for providing data shown in FIGs. 23 from Ref. 5. This work is supported by ONR Grant No. N00014-99-0313.


text:
# Experimental Quantum Cloning of Single Photons

(28 March 2002)

## Abstract

Although perfect copying of unknown quantum systems is forbidden by the laws of quantum mechanics, approximate cloning is possible. A natural way of realizing quantum cloning of photons is by stimulated emission. In this context the fundamental quantum limit to the quality of the clones is imposed by the unavoidable presence of spontaneous emission. In our experiment a single input photon stimulates the emission of additional photons from a source based on parametric down-conversion. This leads to the production of quantum clones with near optimal fidelity. We also demonstrate universality of the copying procedure by showing that the same fidelity is achieved for arbitrary input states.

No device is capable of producing perfect copies of an unknown quantum system. This statement, known as the “no-cloning theorem” wootters:82 ; dieks:82 , is a direct consequence of the linearity of quantum mechanics, and constitutes one of the most significant differences between classical and quantum information. The impossibility of copying quantum information without errors is at the heart of the security of quantum cryptography gisin:02 . If one could perfectly copy arbitrary quantum states, this would make it possible to exactly determine the state of an individual quantum system, which - in combination with quantum entanglement - would even lead to superluminal communication herbert:82 . Thus the no-cloning principle also ensures the peaceful coexistence of quantum mechanics and special relativity.

Given that perfect cloning is impossible, it is natural to ask how well one can clone. This question was first addressed in buzek:96 , and initiated a large amount of theoretical work. In particular, bounds on the maximum possible fidelity of the clones produced by universal cloning machines were derived bruss:98 . A universal cloning machine produces copies of equal quality for all possible input states. Following the work of buzek:96 , quantum cloning was discussed mainly in the language of quantum computing, where its realization was envisaged in the form of a certain quantum logical network, consisting of a sequence of elementary quantum gates. An implementation of the cloning network based on NMR has recently been reported cummins:01 , but uses ensemble techniques and thus does not constitute true cloning of individual quantum systems. In another experiment the polarization degree of freedom of a single photon was approximately copied onto an external degree of freedom of the same photon huang:01 . Although formally this is a realization of a quantum cloning network, only a single particle is involved in the whole process.

One might look for more natural ways of realizing quantum cloning. In the first papers on the topic a connection to the process of stimulated emission was made and it was suggested that stimulated emission might allow perfect copying herbert:82 . It was subsequently pointed out mandel:83 ; milonni:82  that perfect cloning is frustrated by spontaneous emission. Recently it was proposed simon:00  that optimal quantum cloning, where the quality of the copies saturates the fundamental quantum bounds, could be realized for photons using stimulated emission in parametric down-conversion. First indications of the effect were reported in demartini:00 , but neither universality nor optimality were demonstrated. We present a demonstration of universal cloning for individual quantum systems, realizing the proposal of simon:00  and achieving a quality of the clones that is close to optimal.

Universal cloning by stimulated emission proceeds by sending a single input photon into an amplifying medium capable of spontaneously emitting photons of any polarization with equal probability. This rotational invariance of the medium ensures the universality of the cloning procedure simon:00 . As a result of stimulated emission, the medium is more likely to emit an additional photon of the same polarization as the input photon than to spontaneously emit a photon of the orthogonal polarization. The probabilities for stimulated and spontaneous emission are always proportional, making it impossible to suppress spontaneous emission without also affecting the stimulated process. Thus, it is spontaneous emission that limits the achievable quality of the quantum cloning and ensures that the no-cloning theorem is not violated simon:00 ; mandel:83 ; milonni:82 .

The principle of our experiment is illustrated in Fig. 1. A strong pump light pulse propagates through a non-linear crystal, where, with low probability, photons from the pump pulse can split into two photons of lower frequency (parametric down-conversion). Under suitable conditions and for certain specific directions of emission the two created photons are entangled in polarization kwiat:95 . The situation can be described by a simplified interaction Hamiltonian

$$H=\kappa (a_v^{}b_h^{}a_h^{}b_v^{})+h.c.,$$
(1)
where $`\kappa `$ is a coupling constant, and $`a^{}`$ and $`b^{}`$ are creation operators for photons in the spatial modes corresponding to two different directions of emission (Fig. 1). The subscripts $`v`$ and $`h`$ refer to vertical and horizontal polarization. The Hamiltonian can be shown to be invariant under joint identical polarization transformations in modes $`a`$ and $`b`$, ensuring that the cloning will be equally good in every polarization basis.

The input photon arrives in mode $`a`$ passing through the non-linear crystal (Fig. 1). Because of the rotational invariance of the Hamiltonian, it is sufficient to consider one particular initial polarization state, for example $`a_v^{}|0=|1,0_a`$, where we have introduced the notation $`|k,l_a`$ for a state containing $`k`$ vertically and $`l`$ horizontally polarized photons in mode $`a`$. Its time evolution is obtained by applying the operator $`e^{iHt}`$. For small values of $`\kappa t`$, corresponding to the experimental situation, this can be expanded into a Taylor series. The zeroth order term corresponds to the case where no additional photons are produced. This emphasizes that our cloning machine has a probabilistic aspect, sometimes it will just output the input photon. The first order term leads to the following (unnormalized) three-photon state

$`i\kappa t(a_v^{}b_h^{}a_h^{}b_v^{})a_v^{}|0`$
$`=i\kappa t(\sqrt{2}|2,0_a|0,1_b|1,1_a|1,0_b).`$ (2)
Recall that $`|2,0_a|0,1_b`$ is the (normalized) state with 2 photons in mode $`a_v`$ and one photon in mode $`b_h`$, while $`|1,1_a|1,0_b`$ has one photon each in modes $`a_v`$, $`a_h`$ and $`b_v`$. Note the factor $`\sqrt{2}`$, which shows that the additional emitted photon in mode $`a`$ is more likely by a factor of 2 to be of the same polarization as the input photon than of the orthogonal polarization. In this way the information about the input photon polarization is imprinted on the down-converted photon.

The two photons in mode $`a`$ are the clones. Note that in the present ideal case the input photon and the additional photon created in the process have identical space-time wave functions and are thus completely indistinguishable from each other. Therefore the two photons are both approximate copies of the input photon with the same fidelity. Operationally, the fidelity is defined by picking one of the two photons in mode $`a`$ and determining with which probability its polarization is identical to that of the input photon. Inspection of the output state Eq. 2 shows that with a probability of 2/3 both photons are vertically polarized, i.e. they are perfect clones, while with a probability of 1/3 the photons have opposite polarization, so that in this case the probability of picking a vertical photon is just 1/2. Therefore the overall fidelity of the clones is given by

$$F=\frac{2}{3}\times 1+\frac{1}{3}\times \frac{1}{2}=\frac{5}{6},$$
(3)
which has been shown to be the optimal achievable fidelity for the universal cloning of a single photon bruss:98 . Note that because of the rotational invariance of the Hamiltonian Eq. 1 every other input polarization is copied with the same fidelity.

The stimulation effect only occurs when there is overlap between the incoming photon and the photon produced by the source. In our experiment we use photons created in short pulses. By changing the relative delay between the input photon and the photon created in the down-conversion process, we can continuously vary the degree of distinguishability. Suppose that the state of the incoming photon, $`\stackrel{~}{a}_v^{}|0`$, does not overlap with the down-conversion mode $`a`$. Then the same calculation as above leads to a three-photon state

$`i\kappa t(a_v^{}b_h^{}a_h^{}b_v^{})\stackrel{~}{a}_v^{}|0`$
$`=i\kappa t(|1,0_a|1,0_{\stackrel{~}{a}}|0,1_b|0,1_a|1,0_{\stackrel{~}{a}}|1,0_b),`$ (4)
If $`\stackrel{~}{a}`$ differs from $`a`$ only by a time delay that is small compared to the time resolution of the detectors (which is of the order of 1 ns), then they are practically, though not fundamentally, indistinguishable. In this case the state in Eq. 4 will be experimentally indistinguishable from the state $`i\kappa t(|2,0_a|0,1_b|1,1_a|1,0_b)`$. Note that there is an important distinction with respect to Eq. 2, namely the factor $`\sqrt{2}`$ in the first term has disappeared, which means that the additional emitted photon is now equally likely to be vertically or horizontally polarized. There is no stimulation effect.

So far, the third photon that is produced into mode $`b`$ has played no role in our discussion. However, it serves an important purpose in the experiment as a trigger. As the down-conversion photons are created in pairs, the detection of the photon in mode $`b`$ means that a clone has indeed been produced in mode $`a`$. For our experimental setup, the mere detection of two photons in mode $`a`$ doesn’t ensure that cloning has indeed occurred, because both photons could have been contained in the input pulse. Because the input pulse has an average photon number of only 0.05 and the down-conversion process occurs only with a probability of the order of 1/1000, total photon numbers larger than 3 are exceedingly unlikely. The possible presence of more than one photon in the input pulse leads to a slight overestimation of the cloning fidelity (by about 0.003). However, this effect is negligible compared to the experimental and statistical errors. It is worth noting that, as a consequence of the anti-correlation in polarization between the photons in modes $`a`$ and $`b`$, the photon in mode $`b`$ is actually an optimal anti-clone of the input photon buzek:99 ; simon:00 . Even if the phase between the two terms in the Hamiltonian Eq. 1 is not fixed, such that the entanglement between modes $`a`$ and $`b`$ is reduced, the cloning procedure will still be universal and work with optimal fidelity, as long as the source emits photons of any polarization with equal probability. However, the quality of the anti-clones will steadily decrease as the quantum correlations are lost.

In the experiment, the polarization of the photons in spatial mode $`a`$ is analyzed triggered by the detection of a photon in mode $`b`$, while varying the overlap between the input photon and the photon created in the crystal. The polarization analysis is performed in the following way. For linear polarizations a $`\lambda /2`$ waveplate is used to select the measuring basis; a polarizing beam splitter (PBS) is used to measure the events in which the two photons in mode $`a`$ have different polarizations ($`N(1,1)`$), while a polarizer followed by an ordinary beam splitter (BS) is used to probabilistically detect the presence of two identical photons in mode $`a`$ ($`N(2,0)`$). For the case of circular polarization, a $`\lambda /4`$ plate is used to convert circular to linear polarization and subsequently the same method is used. In practice, the PBS is effectively changed into a BS by introducing an additional $`\lambda /4`$ to introduce minimum changes to the experimental setup.

According to our above discussion and comparing Eqs. 2 and 4, an enhancement of the rate $`N(2,0)`$ of events where both photons have the same polarization is expected, as soon as the input photon and the produced photon overlap. On the other hand, for the rate $`N(1,1)`$ of detections where the two photons have orthogonal polarizations, there should be no enhancement (because the amplitude is always $`i\kappa t`$). Moreover, the stimulation effect should be equally strong for all incoming polarizations.

These expectations are fulfilled in the experiment. Fig. 2 shows our experimental quantum cloning results. One sees a clear increase in the $`N(2,0)`$ count rate in the overlap region. This increase is observed for three complementary input polarizations (linear $`0^{}`$, linear $`45^{}`$ and circular left-handed), thus demonstrating universality. It should be noted that far away from the overlap region the probabilities $`p(2,0)`$ and $`p(1,1)`$ are actually the same. This is due to the rotational invariance of the source, which has been verified independently. The measured values for the $`N(2,0)`$ and $`N(1,1)`$ base levels in Fig. 2 are different because the two identically polarized photons in the $`N(2,0)`$ case can be detected only probabilistically by observing coincident counts behind a beam splitter. About half of the time, the two photons will choose the same output port of the beam splitter and no coincidence will be observed.

The average fidelity of the clones can be directly deduced from Fig. 2 by taking the ratio, $`R`$, between the maximum and base values in the $`|2,0`$ curves. The flatness of the $`|1,1`$ curves demonstrates that the observed peaks are indeed due to stimulation. From the above discussion it follows that this is equal to the ratio between $`p(2,0)`$ and $`p(1,1)`$. Therefore the relative probability for the two photons to have equal polarization is $`R/(R+1)`$, while the probability for them to have orthogonal polarizations is $`1/(R+1)`$. As a consequence, the average fidelity of the individual clones is

$$F=\frac{R}{R+1}\times 1+\frac{1}{R+1}\times \frac{1}{2}=\frac{2R+1}{2R+2},$$
(5)
in analogy with Eq. (3). The observed values of $`R`$ from Fig. 2 have uncertainties of the order of $`3\%`$ and lead to values for the fidelity $`F`$ of $`0.81\pm 0.01`$, $`0.80\pm 0.01`$ and $`0.81\pm 0.01`$ for the three complementary polarization directions linear vertical, linear at $`45^o`$ and circular left-handed respectively. The experimental values are close to the optimum value of $`5/6=0.833`$ for a universal symmetric cloning machine. Note that strictly speaking the clones are equally good only for perfect overlap. For imperfect overlap, one can in principle distinguish the input photon from the photon produced by down-conversion with a finite probability.

The absolute number of counts in Fig. 2 is determined by several factors: the pump pulse repetition rate (80 MHz), the probability for each input pulse to contain a photon ($`5\times 10^2`$), the probability of producing a down-converted pair ($`10^3`$) and the overall detection efficiency ($`0.10`$ per photon). Multiplication of all these factors leads to the observed levels.

The limiting factor for the quality of the clones in our experiment is the difference in (temporal) width between the input photons and the photons produced in the down-conversion process, leading to imperfect mode overlap. There are two reasons for this. First, the input photon goes through several additional optical elements which stretch the wavepacket, cf. Fig. 1. Second, the down-conversion process intrinsically has a shorter coherence time than the input pulse. This is largely compensated by using 5 nm bandwidth interference filters in front of the detectors.

Another important practical point for the experiment is the compensation for the effects of birefringence, which is achieved by the three compensation crystals (Fig. 1). Birefringence leads to a time delay between vertical and horizontal polarization, which, without compensation, would considerably affect the overlap and thus the stimulating effect for $`45^o`$ linear and circular polarization. The fact that the stimulation effect for these polarizations is comparable to the vertical case (see Fig. 2) indicates that the compensation is effective.

An interesting property of universal quantum cloning machines is that they constitute the optimal attack on certain quantum cryptography protocols bechmann:99 . Applications of cloning in a quantum computing context were suggested in galvao:00 . From a more fundamental point of view, quantum cloning by stimulated emission shows how a basic quantum information procedure can be implemented in a natural way.