text:
# Gapped tunneling spectra in the normal state of Pr2-xCexCuO4

## I Introduction

The nature of the normal state of high-$`T_c`$ superconductors is a matter of great interest because it gives information about the nature of the charge carriers and the pairing mechanism leading to superconductivity. It is now widely accepted that, in cuprate superconductors there is a depletion of the density of states (DOS) at the Fermi level ($`E_F`$) at a temperature $`T^{}`$, which is much higher than the superconducting transition temperature ($`T_c`$). This gap is called the pseudogap (PG). The evidence for this PG has come from various experiments which include angle resolved photoemission spectroscopy (ARPES), optical conductivity and tunneling spectroscopy . For the hole-doped high-$`T_c`$ superconductors (e.g. BSCCO) these measurements show that the superconducting gap ($`\mathrm{\Delta }_{SC}`$) has a similar width as the PG. This leads many to believe that the PG and the $`\mathrm{\Delta }_{SC}`$ have a similar origin. Theories predicting pair correlations above $`T_c`$ have been suggested, which are supported by these experiments. The other important property of the PG is its doping dependence. The PG appears at higher temperatures for the underdoped compounds and is not observed in overdoped compounds . The situation is less clear for other cuprates like the hole-doped system La2-xSrxCuO4 (LSCO). The width of the PG in LSCO from ARPES  and optical conductivity  measurements comes out to be much larger than the width of $`\mathrm{\Delta }_{SC}`$ . These results raise questions about the origin of the PG and more experiments on the normal state of the cuprates are necessary.

A lot of interest has been generated recently by the electron doped counterparts of the high $`T_c`$ cuprates. These materials have the general formula $`RE_{2x}`$CexCuO4 ($`RE`$=Nd, Pr, Sm). These materials were believed to have an $`s`$-wave superconducting gap symmetry but recent results have shown that the gap has a $`d`$-wave symmetry like the hole-doped cuprates . A comparison between the properties of the hole-doped and electron doped systems is needed as input for theories of high-$`T_c`$ superconductivity. In this context it is important to investigate the normal state of the electron-doped materials and check if results similar to the hole-doped cuprates are obtained, e.g. the formation of a PG in the normal state. Transport measurements have shown that there is a metal-insulator crossover as a function of Ce doping in the normal state of the electron-doped cuprate Pr2-xCexCuO4 (PCCO) . Recently tunneling spectroscopy measurements have been reported in the normal state of PCCO and NCCO  These reports give evidence for a normal state gap for fields above the bulk $`H_{c2}`$ and $`T<T_c`$. In ref.  the authors suggest that this normal state gap could be due to the presence of a PG in the normal state of the electron doped superconductors. However the width of this gap is not consistent with other recent measurements using ARPES and optical conductivity which show normal state gaps of 60 meV and wider . Further work is therefore necessary to explain the origin of this normal state gap and the differences between the properties of the hole and electron-doped systems.

In this paper we report our tunneling studies of the normal state of the electron doped cuprate superconductor Pr2-xCexCuO4 for different values of the doping $`x`$. Preliminary work was reported in . For PCCO the $`H_{c2}`$ is of the order of 10 tesla for $`x=0.15`$ at 1.5 K. This makes it possible to obtain the normal state by applying a field greater than $`H_{c2}`$ and to then perform the tunneling studies. In hole-doped cuprates the $`H_{c2}`$ is much higher ($``$ 50 T for optimally doped samples) and the tunneling studies which have been performed in the normal state are for $`T>T_c`$. We find that in the normal state, there is a depletion of the density of states (DOS) near the Fermi level ($`E_F`$). Further investigation reveals that this normal state gap (NSG) closely resembles the correlation gap formed in disordered metals due to enhanced electron-electron interactions. We present data which show that this NSG is not due to residual superconductivity at the surface for fields above the bulk $`H_{c2}`$ and we argue that this is probably not a pseudogap feature. The formation of this NSG gives us new information about the nature of the charge carriers in the normal state and hence about the pairing mechanism.

There have been several tunneling studies reported on the electron-doped cuprates but the results have been inconsistent vis a vis the values of the SC gap, the observation of the zero bias conductance peak formed due to Andreev bound states, etc . The standard techniques used for other cuprates like YBCO, e.g. multilayer junctions, are difficult to use for the electron doped materials because, 1) a-axis oriented superconducting films of PCCO or NCCO have not been grown yet, and 2) the extreme sensitivity of these compounds to the oxygen stoichiometry which makes it difficult to fabricate tunnel junctions without changing the superconductor in some way. In this paper we report tunneling data on three different types of junctions and show that they all give consistent results.

## II Experimental Details

The tunneling studies were performed mainly on $`c`$-axis oriented thin films of PCCO grown using pulsed laser deposition (PLD) on LaAlO3 (LAO) and yttrium stabilized zirconia (YSZ) substrates. Details of the film growth are given in ref. . The films have been optimized for oxygen content by maximizing $`T_c`$ for each cerium concentration. The films were characterized by X-ray, ac susceptibility and resistivity measurements.

We have used three techniques to tunnel into the $`ab`$ plane of $`c`$-axis oriented thin films. In the first technique, a thin film of c-axis oriented PCCO, covered with SiO2, is broken in vacuum to expose the a-b plane while Ag is being evaporated in the vacuum chamber. A junction is thus formed between the freshly exposed PCCO surface and silver. The size of the junction is reduced to about 200 $`\mu `$m. This is a new method of forming junctions to tunnel into the a-b plane of PCCO details of which will be discussed in a future publication. We will call these “break junctions” in the subsequent sections although they are not break junctions in the usual sense. The second technique is very similar to the break junction method. Here the c-axis oriented film is covered with SiO2 and broken in air. Indium was pressed on the freshly exposed side of the film. We used indium to check the quality of the junction by recording the tunneling features of indium. These will be called “pressed junctions”. The third method was the usual point contact junction formed by pressing a gold electrode on the side of a single crystal or a freshly broken thin film such that the direction of current flow is perpendicular to the c-axis.

## III Results and Discussions

We first show the tunneling data on the optimally doped PCCO sample ($`x=0.15`$). Fig. 1a shows

the data using the break junction method. The superconducting gap is clearly visible and results in a bunching of states near $`\pm \mathrm{\Delta }_{SC}`$ (coherence peaks). The value of $`\mathrm{\Delta }_{SC}`$ is about 5 meV which is similar to the values reported in earlier tunneling studies . The conductance ($`G=dI/dV`$) within the gap voltage does not go to zero because of two possible reasons: 1) the junctions have more than one conduction channel i.e. are not tunnel junctions but ballistic point contact junctions and 2) the likely $`d`$\- wave symmetry of the SC gap. The effect of the first point has been discussed in detail in the classic paper by Blonder, Tinkham and Klapwijk (BTK)  for the case of isotropic $`s`$-wave superconductors. In the BTK analysis the junction was parametrized by a quantity $`Z`$ which depends on the scattering at the interface between the metal and the superconductor. High transparency junctions have $`Z0`$ and tunnel junctions have $`Z1`$. For superconductors with an anisotropic gap a modified BTK model has been described in ref. . A detailed fitting of our data to such models is in progress.

However in the following sections we will use these ideas qualitatively. Fig. 1a also shows the variation of the tunneling spectra with temperature. This variation is due to a combined effect of the thermal smearing of the spectra and the variation in the density of states (DOS) of the SC with temperature. The $`\mathrm{\Delta }_{SC}`$ does not change noticeably with temperature. The gap structure disappears above $`T_c`$ and the background conductance of the junction is observed for $`T`$=25 K.

When a magnetic field $`H>H_{c2}`$ is applied to this tunnel junction at $`T=`$ 1.7 K ($`TT_c`$), the SC gap is no longer observed as expected (i.e. the coherence peaks disappear), but surprisingly the gap at the $`E_F`$ persists. However the shape of this gap as a function of energy is quite different (fig. 1b) from the SC gap. We call this unexpected gap the normal state gap (NSG), since resistivity measurements at this magnetic field show that the PCCO film is in the normal state. Before we further analyze this NSG we present data which show that the observation of this NSG does not depend on the type of

tunnel junction. Fig 2a shows data for a pressed junction using an indium counterelectrode. The indium was used to check the quality of the junction. The contribution of the indium density of states is visible in the zero field data, since when a field of about 5000 G was applied to make the indium electrode normal there is a large increase in the zero bias conductance which indicates that the indium has become a normal metal with no superconducting gap (inset fig. 2a). In the superconducting state of indium the $`G`$ at zero bias is not zero which shows that this junction is not in the tunneling limit. We find $`Z0.7`$ according to a rough estimate made from the ratio of the conductance at 20 mV ($`G_{20}`$) and at 0 V ($`G_0`$) . For fields above 5000 G the contributions to the tunneling spectra will be dominated by the DOS features of PCCO. For an applied field of 8.5 T the NSG is clearly seen for this junction too (fig. 2b). In fig. 3a we show the tunneling data obtained from point contact tunnel junctions formed between a gold tip and a PCCO thin film. The zero field data clearly shows the

gap feature for superconducting PCCO. The temperature dependence of the tunneling spectra is similar to that observed for the other two types of junctions. On the application of a magnetic field of 8.5 T we observe the formation of the NSG again (fig. 3b). From these data we conclude that this anomalous NSG is present irrespective of the kind of tunnel junction.

We now discuss the nature of this NSG in more detail. First we look at the behavior of this gap as the temperature is increased upto and beyond $`T_c`$. The $`T_c`$ for our optimally doped PCCO films is about 21 K. We see that the NSG becomes indistinguishable from the background for $`T>T_c`$ (figs. 1b, 2b and 3b). This could be interpreted as evidence for the NSG being due to some residual superconductivity (even for $`H>H_{c2}`$) which goes away for $`T>T_c`$. However we have to consider that the width of the NSG is $``$ 7 meV and a temperature of 25 K can smear out features of about 5 meV in the tunneling spectra. To check if the NSG closes around $`T=T_c`$ just due to thermal smearing we have made a simple estimate of the role of thermal smearing in the temperature evolution of the $`Gvs.V`$ curves using the following equation for the tunneling current :

$`I(V,T)`$ $`=`$ $`c{\displaystyle _{\mathrm{}}^{\mathrm{}}}n\left(E+{\displaystyle \frac{eV}{2}}\right)`$ (2)
$`\times \left[f(E+{\displaystyle \frac{eV}{2}},T)f(E{\displaystyle \frac{eV}{2}},T)\right]dE`$
where $`n(E)`$ is the DOS of the PCCO sample at zero temperature, $`f(E,T)`$ is the Fermi function at a temperature $`T`$, and V is the junction bias. For $`n(E)`$ we have taken the $`G(V)vs.V`$ curve at 1.6 K and smeared it using eqn. 1 for a temperature $`T`$. We have assumed that the density of states of the counterelectrode gold is a constant for the relevant energy range and so is the tunneling barrier for this range of energies both of which are included in the constant $`c`$. The results of these calculations are shown in fig. 4. It shows that thermal smearing alone cannot explain the disappearance of the NSG for $`T`$ 20 K. This means that the NSG has a significant thermal dependence of its own. With this analysis we have shown that although the thermal smearing of the tunneling spectra has a significant influence on their evolution with temperature the NSG does indeed become smaller with increasing temperature. This thermal dependence of the NSG could be due to residual SC, or it could be that there is no residual SC and the NSG has its own thermal dependence.

To study the possible contribution to the NSG of residual SC at the interface and/or the tunnel barrier, we formed a high transparency point contact junction between a gold tip and an $`x=0.13`$ thin film of PCCO. Fig. 5a shows the $`GV`$ data at various applied fields for such a junction, at 1.6 K. The peak formed at zero bias (for $`H<H_{c2}`$) is due to Andreev reflection which is observed in high transparency junctions. At $`H=0`$ the width of the feature is about $`2\mathrm{\Delta }_{SC}`$ ($``$ 10 meV) and $`G(0)/G_N`$ is 1.62 (fig. 5a inset), where $`G_N`$ is the value of $`G(V)`$ for $`eV>\mathrm{\Delta }`$. These are clear signatures of Andreev reflection (AR) occurring at the interface between gold and PCCO. This also shows that for this junction $`Z0`$. We chose the $`x=0.13`$ composition because it has a low $`T_c`$ of 12 K and therefore we get a good temperature range to operate in before thermal smearing washes out the features in the $`G(V)vs.V`$ curves. When a magnetic field is applied on this junction, the AR feature reduces in height and also shrinks in width and when the superconductivity is destroyed, disappears completely. This is a clear indication that there is no residual SC at the interface in our $`GV`$ curves. However, the NSG is clearly visible! In fact for intermediate values of $`H`$ the normal state density of states reveals itself at higher $`V`$ while at the same time there is peak at zero bias due to Andreev reflection, as shown in fig 5b. Since this is a high transparency junction, the junction barrier has negligible effect on the shape of the curve. This is clear from fig. 5a since for $`H=0`$ the $`GV`$ curve is almost flat (independent of $`V`$) for $`eV>\mathrm{\Delta }`$.

The other test to check if the NSG is truly a feature of the normal state is to increase the temperature beyond $`T_c`$ and observe the evolution of the $`G(V)vs.V`$ curves. Fig. 5c shows that removing SC by increasing the temperature has an evolution similar to that of increasing $`H`$ beyond $`H_{c2}`$ (for $`T<T_c`$). However, the presence of the NSG is less clear for $`T>T_c`$ due to thermal smearing. This strongly suggests that the NSG is indeed a normal state feature. We should add here that the high transparency junctions are not tunnel junctions but point contact junctions with more than one channel for conduction. However we are still in the ballistic region i.e. the junction size, given by a radius $`a`$, is smaller than the elastic mean free path of the electron, $`l_e`$ (the Sharvin

limit). We know this must be the case because at $`T`$ 20 K, $`G(V)`$ has a minimum at $`V=0`$ . If the junction were in the diffusive limit ($`a>l_e`$) then the curvature of the tunneling spectra in the normal state would change and there would be a maximum in the $`GV`$ curve at $`V=0`$. Hence the features observed in the $`GV`$ curves in the normal state do reflect the DOS features of the normal state. From this experiment we thus draw two important conclusions: 1) the NSG is definitely a normal state feature and 2) it can be observed for $`H>H_{c2}`$ as well as for $`T>T_c`$.

What is the origin of this NSG? Such features in the density of states have been observed before in various systems like disordered metallic films  and perovskite oxides like LaNiO3-δ  using tunneling spectroscopy. The appearance of these features in the density of states of these materials is due to electron-electron Coulomb interactions which are enhanced due to disorder in the materials. Such effects lead to anomalies in the DOS, $`n(E)`$, near $`E_F`$. For three-dimensional systems this anomaly is of the form $`n(E)=n(0)[1+\sqrt{E/\mathrm{\Delta }}]`$ where $`\mathrm{\Delta }`$ is called the correlation gap. For two-dimensional systems the electron-electron interaction leads to decrease in the DOS near $`E_F`$ given by $`\delta n/nln(E/E_0)`$ . These anomalies are the precursors of the insulating phase “Coulomb gap” which is formed at $`E_F`$ when the disorder is increased and the states near $`E_F`$ are localized.

To check if such effects are the reason for the formation of the NSG we look at the properties of the NSG is more detail. Fig 6 shows a plot of the $`G(V)`$ as a function of $`logV`$ ($`V>0`$) taken at $`T=1.6`$ K using a gold and PCCO point contact junction. $`G(V)`$ is a linear function of $`logV`$ for a large range of V (for $`V<1`$ mV, $`G(V)`$ deviates from the straight line due to thermal smearing). This behavior follows closely the abovementioned signature of a 2D correlation gap . In ref.  it is shown that as the sheet resistance of the film is increased, the logarithmic anomaly at zero bias becomes deeper. We want to verify if a similar trend is observed in the normal state of PCCO as in the case of disordered metal films. The sheet resistance in the normal state of PCCO increases as $`x`$ is lowered . Moreover, the field induced normal state in PCCO has a metallic behavior for overdoped samples ($`x>0.15`$) and the resistivity shows an upturn at low temperatures for optimally doped and underdoped samples ($`x0.15`$) . A suggested mechanism for this transition was the onset of weak localization below a certain doping. This transition suggests an increase in the electron-electron interactions as $`x`$ is decreased. If our hypothesis about effect of interactions on the DOS is correct then the tunneling data should reflect this transition. The inset of fig. 6 shows the point contact tunneling data for an $`x=0.17`$ sample of PCCO ($`T=1.6`$ K). At zero field the superconducting gap is clearly seen. At 8.5 T the SC gap gives way to the NSG. The NSG in this case is smaller than the one found for $`x=0.15`$. Fig. 6 also shows the $`G_{norm}logV`$ plots for the $`x=0.17`$ (at $`T=1.6`$ K) and $`x=0.13`$ (at $`T=1.61`$ K) samples. The deepening of the NSG with lowering of $`x`$ is clearly indicated by the increase of the slope of the $`G_{norm}vs.logV`$ curves and is similar to the trend observed in metallic films with different amounts of disorder . Therefore our tunneling data shows that in the underdoped region there are strong electron-electron interactions which results in a larger NSG. As the doping is increased the effect of the interactions is lowered and a trend towards a more conventional Fermi liquid like normal state is obtained as seen from a much smaller NSG. It has been conjectured that for some value of $`x`$ there is quantum critical transition in the normal state of cuprate superconductors . The gradual disappearance of the NSG is an indication that the physical properties of the cuprates are going through a gradual crossover with increasing $`x`$, probably due to their proximity to this quantum critical point.

The data discussed above show that there is a NSG in the normal state of PCCO. This gap shows the properties of a 2D correlation gap and is related to the position of the material in the PCCO phase diagram i.e. it depends on the doping. The pseudogap (PG) is a gap in the normal state of cuprate superconductors and it also depends on the doping . In fact the other similarity between the NSG observed here and the PG is that the gap becomes smaller for the overdoped compounds. But is our observed NSG the same as the pseudogap (PG)? In ref.  the authors claim that the NSG they observe in PCCO and NCCO is the pseudogap and they also estimate field values at which this NSG is suppressed. However there is serious discrepancy in the energy scale of the pseudogap observed in ref.  and in our experiments with that observed in other experiments. Optical conductivity data on LSCO (a hole-doped cuprate superconductor similar to PCCO) show a PG of about 500 cm-1 i.e. about 62 meV . New optical conductivity data on e-doped NCCO gives a large pseudogap width of about 600 cm-1 which survives even above room temperature . Recent ARPES data also shows evidence of a pseudogap larger than 50 meV . In non-superconducting NCCO pseudogaps of about 200 meV have been observed from optical conductivity measurements . These gaps are at least an order of magnitude larger than the NSG we observe. For high $`T_c`$ compounds like BSCCO the PG observed from the tunneling spectra agree quite well with other experiments like ARPES and optical conductivity . Hence, it is unlikely that the NSG we found in our tunneling experiments in PCCO and the pseudogap observed in other experiments on PCCO and NCCO are the same.

There is only a small variation of the NSG with magnetic field in our experiment and for the maximum field values that we applied ($``$ 9 T) the NSG was still prominent. The small variation that we see with the magnetic field is most likely due to the change in $`ee`$ correlations on the application of a magnetic field . However, further experiments are necessary to determine accurately the variation of the NSG with $`T`$ and $`H`$.

## IV Summary and Conclusions

In this paper we have shown that the density of states of the normal state of PCCO shows a depletion of states near the Fermi level $`E_F`$. This normal state gap can be treated as a correlation gap which is formed due to electron correlations. Such gaps have been seen in disordered metals using tunneling spectroscopy. We have argued that this gap is probably not the pseudogap mainly due to a difference of an order of magnitude in their values. We have shown that the nature of the NSG depends on the doping i.e. it depends on the position in the phase diagram. We conjecture that this NSG is linked with a quantum phase transition which most probably occurs in the normal state of the cuprates for a certain value of hole or electron doping.

## ACKNOWLEDGMENTS

P. F. acknowledges the support of the Canadian Institute of Advanced Research and the Foundation Force of the Universite de Sherbrooke. We thank Hamza Balci and Z. Y. Li for some of the thin film samples. This work was supported by NSF DMR 97-32736


format: text

text:
# Gordian unknots

## Abstract

Numerical simulations indicate that there exist conformations of the unknot, tied on a finite piece of rope, entangled in such a manner, that they cannot be disentangled to the torus conformation without cutting the rope. The simplest example of such a gordian unknot is presented.

Knots are closed, self-avoiding curves in the 3-dimensional space. The shape and size of a knot, i.e. its conformation, can be changed in a very broad range without changing the knot type. The necessary condition to keep the knot type intact is that during all transformations applied to the knot the curve must remain self-avoiding. From the topological point of view, all conformations of a knot are equivalent but if the knot is considered as a physical object, it may be not so. Let us give a simple example. Take a concrete, knotted space curve $`K`$. Imagine, that $`K`$ is inflated into a tube of diameter $`D`$. If $`K`$ is scaled down without scaling down $`D`$, then there is obviously a minimum size below which one cannot go without changing the shape of $`K`$. Diminishing, in a thought or computer experiment, the size of a knot one arrives to the limit below which in some places of the knot the impenetrability of the tube on which it has been tied would be violated.

Consider a knot tied on a piece of a rope. If the knot is tied in a loose manner, one can easily change its shape. However, the range of transformations available in such a process is much more narrow than in the case of knots tied on an infinitely thin rope. Limitations imposed on the transformations used to change the knot shape by the fixed thickness and length of the rope may make some conformations of the knot inaccessible from each other. The limitations can be in an elegant manner represented by the single condition that the global curvature of the knot cannot be larger than $`2/D`$ . That it is the case we shall try to demonstrate in the most simple case of the unknot. The knot is a particular one since we know for it the shape of the ideal, least rope consuming conformation . The simplest shape of the unknot is obviously circular. If the knot is tied on the rope of diameter $`D`$ the shortest piece of rope one must use to form it has the length $`L_{min}=\pi D`$. If one starts from the circular conformation of the unknot tied on a longer piece of rope, the length of the rope can be subsequently reduced without changing the circular shape until the $`L_{min}`$ value is reached.

Consider now a different, entangled conformation of the unknot tied on a piece of rope having the length $`L>L_{min}`$. Can it be disentangled to the canonical circular shape? Are there such conformations of the unknot, which cannot be disentangled to a circle without elongating the rope? For obvious reasons we propose to call such conformations gordian. In what follows we shall report results of numerical experiments suggesting existence of the gordian conformations of the unknot.

Imagine that the entangled conformation of the unknot is tied on piece the ideal rope of diameter $`D`$ and length $`L>Lmin`$. The ideal rope is perfectly flexible but at the same time perfectly hard. Its perpendicular cross-sections remain always circular. The diameters of all the cross-sections are equal $`D`$. None of the circular cross-sections overlap. The surface of the rope is perfectly slippery. In such conditions one may try to force the knot to disentangle itself just by shortening the rope length. Such a process, in which the knot is tightened, can be easily simulated with a computer. The details of SONO (Shrink-On-No-Overlaps), the simulation algorithm we developed, are described elsewhere. As shown in , SONO disentangles some simple conformations of the unknot. See Fig.1. It manages to cope also with the more complex conformation proposed by Freedman  disentangled previously by the Kusner and Sullivan algorithm minimizing the Möbius energy .

The steps of the construction of the Freedman conformation, are as follows :

1. Take a circular unknot and splash it into a flat double rope band.

2. Tie overhand knots on both ends of the band and tighten them. (From the point of view of the knot theory, the overhand knots are open trefoil knots.)

3. Open and slip the end loops over the bodies of the overhand knots, so that they meet in the central part of the band.

4. Move the rope through both overhand knots so that the loops become smaller.

In what follows we shall refer to the conformation as $`F(3_1,3_1)`$. To disentangle $`F(3_1,3_1)`$, one must slip the loops back all around the bodies of the overhand knots, which is difficult, since the move needs first making the loops bigger.

How the SONO algorithm copes with this task is shown in Fig.2, where consecutive stages of the disentangling process are shown. Tightening the $`F(3_1,3_1)`$ conformation SONO algorithm brings it to the very compact state, which seems at the first sight to be impossible to disentangle. The end loops are very tight and they seem to be too small to slip back over the bodies of the overhand knots. However, as the computer simulations prove, there exists a path in the configurational space of the knot along which the loops slowly become bigger and one of them slips over the body of the overhand knot. Then, the disentangling process proceeds without any problems. Results of the computer experiments we performed suggest strongly, that the $`F(3_1,3_1)`$ conformation is not gordian.

The construction of original Freedman entanglement may be modified making it more difficult to disentangle. The simplest way of doing this is to change the end trefoil knots to some more complex knots. For the sake of brevity we will use $`F(K^{(1)},K^{(2)})`$ symbols to indicate with what kind of the Freedman conformation of the unknot we are dealing with. Results of computer simulations we performed prove that the $`F(4_1,4_1)`$ conformation is also disentangled in the knot tightening process. However, the $`F(5_1,5_1)`$ conformation proves to be resistant to SONO algorithm. Fig.3 shows consecutive stages of the tightening process. The initial conformation, is loose, it becomes tight soon. Then the evolution process slows down and eventually stops. The final conformation is proves to be stable. The gordian conformation has been reached.

Eperimenting with knots tied on real, macroscopic ropes or tubes is by no means easy . First of all, the surface of any real rope is never smooth and strong friction often stops the walk within the configurational space of a knot tied on such a rope. The role of friction was exposed by Kauffman . Friction can be significantly reduced, however, when a knot is tied on a smooth nanoscopic filament, e.g. a nanotube, or on a thermally fluctuating polymer molecule . There exists another, less obvious, factor which makes laboratory experiments on knots difficult: the Berry’s phase , to be more precise, its classical counterpart - the Hannay’s angle . Modern ropes are often constructed in the following manner: a parallel bundle of smooth filaments is kept together by a tube-like, plaited cover. As easy to check, such ropes are much easier to bend than to twist. Forming a knot on a rope, one has to deform it. In view of what was said above, the deformation applied is rather bending than twisting. Avoiding the twist deformations one follows the procedure known as the parallel transport. As a result, when at the final stage of the knot tying procedure the ends of the rope meet, they are in general rotated in relation to each other: the misfit angle $`A`$ is the Hannay’s angle. As shown in  and , the Hannay’s angle $`A`$ stays in a simple relation,

$$1+Wr=(A/2\pi )\mathrm{m}od2$$

with the writhe $`Wr`$ of the knot into which the rope has been formed. Splicing the ends of the rope one fixes the misfit angle $`A`$. Consequently, the writhe value $`Wr`$ becomes fixed as well. As a result, any further changes of the conformation of the knot become very difficult and are basically restricted to the manifold of constant writhe. (The specific construction of the Freedman conformations makes them achiral . Their writhe is equal zero.)

The natural question arises, if the impossibility of disentangling the gordian conformation does not stem from the described above friction and writhe factors. We feel emphasize, that it is not the case. The rope simulated by the SONO algorithm is perfect: it is frictionless and utterly flexible. It has no internal, parallel bundle structure and it accepts any twist. Problems with disentangling the gordian conformations are purely steric. Tightening the $`F(5_1,5_1)`$ Freedman conformation SONO brings it into a cul-de-sac of what mathematicians call thickness energy . To get out of it, one needs elongate the rope. By how much? We do not know yet the answer to this question.

We thank Jacques Dubochet, Giovanni Dietler, Kenneth Millett, Robert Kusner, Alain Goriely, Eric Rawdon, Jonathan Simon, Gregory Buck and Joel Hass for helpful discussions and correspondence. PP thanks the Herbette Foundation for financial support during his visit in LAU. This work was carried out under Project KBN 5 PO3B 01220.


text:
# 1 Introduction

## 1 Introduction

Quantum corrections can qualitatively change the analytic structure of the Green function or the symmetry properties of a classical field-theoretical system. Qualitatively new features compared to the tree level picture may emerge already at finite orders of perturbation theory for Green functions while some effects can only appear as a result of summing up an infinite number of perturbative terms. An effect of non-conservation of the Abelian axial current reveals itself at leading order as a result of the calculation of an one-loop triangle diagram  while spontaneous symmetry breaking or bound state formation cannot be observed at any finite order of perturbation theory and requires an infinite summation of relevant subsets of diagrams. For problems related to an investigation of the symmetry properties of quantum systems, such an infinite summation can be readily done by introducing an effective action for the system and calculating it as a loop expansion series. Such an approach reorders the perturbation series with respect to the lines of diagrams related to external fields and allows one to take into account the entire dependence on external fields exactly within a given order of the loop expansion. An effective action can be considered as a generating functional for the vertex (one-particle irreducible, or proper) Green functions (see e.g. Ref. ). The treatment of external fields beyond finite order of expansion was done in Ref. . The efficient method of calculating the effective action is based on the Legendre transform of the generating functional for connected Green functions and heavily uses the functional techniques . One can also use a practical calculation technique by substituting the shifted fields in the original Lagrangian of the system . The part of the effective action which is constructed from the constant field is usually called an effective potential and is used to analyze the fundamental symmetry properties of the theory beyond the plain perturbation theory where the effect of the external fields is resummed to all orders. The expansion leading to the effective potential is, in fact, an expansion in Planck’s constant $`\mathrm{}`$, i.e. the correction accounts for the deflection from the classical limit. Therefore new effects which are absent in the classical approximation may appear within such an approach. An example for this kind of new quantum effects is the light-by-light scattering which emerges as a quantum correction to the photon dynamics due to the interaction with virtual electrons. In the low-energy limit it can be seen as a nonlinearity of the equations for the strong electromagnetic fields in the vacuum. The behaviour of the electromagnetic fields with such a correction can be described by the Euler-Heisenberg Lagrangian . The generalization to non-Abelian fields is discussed in Ref. . The effective potential is also a powerful tool for investigating effects of spontaneous symmetry breaking by quantum corrections  and for analyzing the properties of particle systems at finite temperature and density .

A special advantage of using the external field technique in gauge theories is an explicit gauge invariance of the effective action that allows to drastically simplify the computation and to reduce the number of necessary diagrams . It is generally believed that in non-Abelian gauge theories the nonperturbative fluctuations (instantons)  create a complex vacuum structure that eventually explain (or is responsible for) the low-energy observable spectrum of particles . The technique of calculating in external fields was heavily used for the calculation of quantum corrections to the effective action of gauge fields in the classical instanton background . In practical applications to QCD the complex vacuum structure could explain a phase transition from the quark-gluon representation of Green functions at high energies to the hadron picture at low energies. While the problem of a full description of this transition remains unresolved, Wilson’s operator product expansion which is one of the key tools for calculating the correlation functions at short distances is used for describing hadronic properties at low energies in a semiphenomenological way using sum rule techniques . The external field technique provides a convenient way for practical calculations within the sum rule method based on a semiphenomenological account for the condensates of the local operators .

In the present paper we calculate the low-energy limit of heavy quark current correlators within the $`1/m`$ expansion where $`m`$ is a heavy quark mass. The induced low-energy currents corresponding to the heavy quark initial operators are obtained from an effective action for gauge fields of the $`SU(N_c)U(1)`$ model in the one-loop approximation at leading order of both the coupling constant and the $`1/m`$ expansion. Our results for the effective action for vector and tensor currents are presented in Sec. 2. Using the external field technique as a convenient framework for practical calculations of the induced currents in this model, in Sec. 3 we present these induced currents. In Sec. 4 we show phenomenological applications, and in Sec. 5 we deal with the consequences encountered for calculating arbitrary moments.

## 2 The effective action

While the technique is standard, we are aiming at concrete results for further phenomenological applications to sum rules for the vacuum polarization functions of heavy quarks. Therefore we briefly outline the calculation and the related issues. Further details can be found in Refs. . The Lagrangian of a heavy fermion field $`\psi `$ interacting with a gauge field $``$ of the gauge group $`SU(N_c)U(1)`$ reads

$$L=\overline{\psi }\left(i\gamma ^\mu _\mu +\gamma ^\mu _\mu m\right)\psi $$
(1)
where $`_\mu =eA_\mu +g_sB_\mu `$. Here $`A_\mu `$ is a gauge field of the $`U(1)`$ subgroup (photon) with the coupling constant $`e`$ and $`B_\mu `$ is a gauge field of the $`SU(N_c)`$ subgroup (gluon) with the coupling constant $`g_s`$. The matrix notation for the non-Abelian gauge field potentials is used, $`B_\mu =t_aB_\mu ^a`$, $`t_a`$ are generators of the gauge group $`SU(N_c)`$. A generating functional $`W[J]`$ of connected Green functions is given by a functional integral with the sources $`J`$,

$`Z[J]`$ $`=`$ $`\mathrm{exp}(iW[J])={\displaystyle [d\overline{\psi }d\psi ]\mathrm{exp}\left(iL^J(x)d^4x\right)}`$ (2)
$`=`$ $`{\displaystyle [d\overline{\psi }d\psi ]\mathrm{exp}\left(i\left(\overline{\psi }(i\gamma ^\mu _\mu +\gamma ^\mu _\mu m)\psi +J^\mu _\mu \right)d^4x\right)}`$
where the product $`J^\mu _\mu `$ implies a trace with respect to the representation of $`SU(N_c)U(1)`$. A proper gauge fixing is implied as well. The effective action $`\mathrm{\Gamma }[\overline{}]`$ for the gauge field is then given by the Legendre transform

$$\mathrm{\Gamma }[\overline{}]=W[J]J\overline{},\overline{}=\frac{\delta W[J]}{\delta J}.$$
(3)
It was shown that this procedure is equivalent to the more direct calculation in external fields (see e.g. Ref. ). It is also a generalization of results obtained for constant external fields . Up to leading order in $`\mathrm{}`$ the effective action constructed with a Legendre transform can also be found through

$$\mathrm{exp}(i\mathrm{\Gamma }[])=[d\overline{\psi }d\psi ]\mathrm{exp}\left(i\overline{\psi }(i\gamma ^\mu _\mu +\gamma ^\mu _\mu m)\psi d^4x\right)=det\left(i\gamma ^\mu _\mu +\gamma ^\mu _\mu m\right)$$
(4)
where $``$ is now a classical gauge field (integration over $`d^4x`$ is implied for expressions of the action). By using the identity $`detM=\mathrm{exp}(\mathrm{tr}(\mathrm{ln}M))`$ for an operator $`M`$ one continues with

$$i\mathrm{\Gamma }[]=\mathrm{tr}\left[\mathrm{ln}\left(i\gamma ^\mu _\mu +\gamma ^\mu _\mu m\right)\right].$$
(5)
### 2.1 Results for the effective action

A straightforward calculation of the functional determinant gives a correction to the effective low-energy action of the gauge fields within $`SU(N_c)U(1)`$. We calculate the leading nontrivial contribution in the $`1/m`$ expansion. The functional determinant in loop expansion can be represented by Feynman diagrams. A diagram which gives a correction to the effective action due to a heavy quark loop is shown in Fig. 1.

Two-gluon transitions are forbidden according to a generalization of Farry’s theorem to non-Abelian theories . We are interested in the behaviour of the amplitude associated with the diagram in Fig. 1 at low energies and, therefore, take the limit of a very heavy quark. Formally the limit $`m\mathrm{}`$ is taken which in physical terms means that $`m`$ is much larger than all momenta of external legs of the diagram in Fig. 1, namely the three gluons and the photon. A straightforward calculation of the diagram presented in Fig. 1 gives the one-loop result for the correction to the effective action induced by a heavy quark loop at leading order of the $`1/m`$ expansion. It reads

$$\mathrm{\Delta }\mathrm{\Gamma }_{\mathrm{QCD}}=\frac{eg_s^3d_{abc}}{180m^4(4\pi )^2}\left[14\mathrm{t}\mathrm{r}(FG^aG^bG^c)5\mathrm{t}\mathrm{r}(FG^a)\mathrm{tr}(G^bG^c)\right]$$
(6)
where $`F_{\mu \nu }`$ is a field strength tensor for the $`U(1)`$ subgroup, $`G_{\mu \nu }=t_aG_{\mu \nu }^a`$ is the field strength tensor for the $`SU(N_c)`$ subgroup, and $`d_{abc}`$ are the totally symmetric $`SU(N_c)`$ structure constants defined by the relation $`d_{abc}=2\mathrm{t}\mathrm{r}(\{t_a,t_b\}t_c)`$. The trace in Eq. (6) is understood as a trace with respect to the Lorentz indices of the fields, i.e. one considers the strength tensors of gauge fields as matrices for which $`\mathrm{tr}(FG^a)=F^{\mu \nu }G_{\nu \mu }^a`$. This makes the formulae shorter and more transparent. Before we proceed to the calculation of the induced current in the next section, we compare the result with the corresponding expression in QED.

### 2.2 Comparison with QED

The effective action within QED corresponding to Eq. (6) is known as Euler-Heisenberg Lagrangian ,

$$\mathrm{\Delta }\mathrm{\Gamma }_{\mathrm{QED}}=\frac{2\alpha ^2}{45m^4}\left[(\stackrel{}{E}^2\stackrel{}{H}^2)^2+7(\stackrel{}{E}\stackrel{}{H})^2\right],\alpha =\frac{e^2}{4\pi }$$
(7)
which can be obtained from Eq. (6) by replacing $`d_{abc}`$ by $`1`$ and $`G_{\mu \nu }^a`$ by $`F_{\mu \nu }`$, supplemented by the obvious substitution $`g_se`$. Using the definitions for the electric field $`\stackrel{}{E}`$ and the magnetic field $`\stackrel{}{H}`$,

$$F^{0j}=F_{0j}=E_j,F^{i0}=F_{i0}=E_i,F^{ij}=F_{ij}=ϵ_{ijk}H_k$$
(8)
one finds

$`\mathrm{tr}(F^2)=2(\stackrel{}{E}^2\stackrel{}{H}^2),`$ $`\mathrm{tr}(F^4)=2(\stackrel{}{E}^2\stackrel{}{H}^2)^2+4(\stackrel{}{E}\stackrel{}{H})^2,`$
$`\mathrm{tr}(F\stackrel{~}{F})=4(\stackrel{}{E}\stackrel{}{H}),`$ $`\mathrm{tr}(F\stackrel{~}{F}F\stackrel{~}{F})={\displaystyle \frac{1}{2}}(\mathrm{tr}(F^2))^2+\mathrm{tr}(F^4)=4(\stackrel{}{E}\stackrel{}{H})^2`$ (9)
where

$$\stackrel{~}{F}_{\mu \nu }=\frac{1}{2}ϵ_{\mu \nu \rho \sigma }F^{\rho \sigma }.$$
(10)
Note for further use and convenience that in order to rewrite the expressions from one form to another there is one more relation between the fourth-order monomials of the electromagnetic field strength tensor $`F_{\mu \nu }`$,

$$(F\stackrel{~}{F})^2=2(F^2)^2+4F^4$$
(11)
with

$$F\stackrel{~}{F}=F^{\mu \nu }\stackrel{~}{F}_{\mu \nu },F^2=F^{\mu \nu }F_{\mu \nu },F^4=F^{\mu \nu }F_{\nu \alpha }F^{\alpha \beta }F_{\beta \mu }.$$
(12)
Therefore the correspondence between Eq. (6) and its QED counterpart in Eq. (7) is established.

## 3 The induced current

An expression for the induced electromagnetic current $`J^\mu `$ as being an effective electromagnetic current for the low-energy effective theory describing the interaction of photons and gluons is given by the derivative of the effective action with respect to the external Abelian gauge field,

$$eJ^\mu =\frac{\delta \mathrm{\Gamma }[]}{\delta A_\mu }=\mathrm{tr}\left[ie\gamma _\mu \frac{1}{i\gamma ^\mu ^{}_\mu ^{}+\gamma ^\mu ^{}_\mu ^{}m}\right].$$
(13)
The derivative with respect to $`A_\mu `$ can be replaced by a derivative with respect to $`F_{\mu \nu }=_\mu A_\nu _\nu A_\mu `$,

$$eJ^\mu (x)=\frac{\delta F_{\mu ^{}\nu ^{}}}{\delta A_\mu }\frac{\delta \mathrm{\Gamma }[]}{\delta F_{\mu ^{}\nu ^{}}}=2_\nu \frac{\delta \mathrm{\Gamma }[]}{\delta F_{\nu \mu }}.$$
(14)
### 3.1 Results for the induced vector current

With the explicit expression for the effective action given in Eq. (6) we obtain

$$J^\mu =_\nu 𝒪^{\mu \nu },𝒪^{\mu \nu }=\frac{g_s^3d_{abc}}{90m^4(4\pi )^2}[14(G^aG^bG^c)^{\mu \nu }5(G^a)^{\mu \nu }\mathrm{tr}(G^bG^c)].$$
(15)
Note that the current conservation $`_\nu J^{\mu \nu }=0`$ is automatically guaranteed because the operator $`𝒪^{\mu \nu }`$ is antisymmetric, $`𝒪^{\mu \nu }+𝒪^{\nu \mu }=0`$. Higher order corrections in the coupling constant $`\alpha `$ of the $`U(1)`$ subgroup are omitted. The induced electromagnetic current in Eq. (15) is a correction of order $`1/m^4`$ in the inverse heavy quark mass which vanishes in the limit of an infinitely heavy quark. Corrections in the inverse heavy quark masses are important for tests of the standard model at the present level of precision and have been already discussed in various areas of particle phenomenology .

### 3.2 Other types of induced currents

Expressions for the induced currents with quantum numbers other than that of the electromagnetic current $`J^{PC}=1^{}`$ can be obtained in a similar way. The axial current of fermions naturally appears in the standard model as a result of an axial-vector interaction of fermions with $`W`$ and $`Z`$ bosons. The corresponding induced current can be obtained as a derivative of the respective effective action with respect to the $`Z`$ boson field. The leading order diagram, however, contains only two external legs and is UV divergent. In case of massless fermions this diagram leads to the anomalous non-conservation of the axial current that also requires a strict definition of the corresponding operator $`\overline{\psi }\gamma _\mu \gamma _5\psi `$ within perturbation theory because its renormalization is not dictated by the Ward identities any more. The leading corrections to the anomaly of the axial current for massless fermions due to strong interactions were considered in Refs.  where implications of the Adler-Bardeen no-go theorem (non-renormalizability) were discussed also for dimensional regularization and different definitions of the axial current at the tree level. Higher order corrections were analyzed in Ref. . Explicit high order corrections to the expression for the anomaly depend on the renormalization prescription for the composite operator $`\overline{\psi }\gamma _\mu \gamma _5\psi `$ within perturbation theory.

The scalar current $`\overline{\psi }\psi `$ appears in an interaction vertex for the Higgs boson and was intensively studied. The decay $`H\gamma \gamma `$ is described by the effective interaction

$$\mathrm{\Delta }L_H=g_S\alpha HFF$$
(16)
with the parameter $`g_S`$ (remark the different to $`g_s`$, $`S`$ stands for the scalar current) given by the corresponding one-loop diagram with two external photons. Here $`H`$ is an interpolating field for the Higgs boson. The decay of the Higgs boson into two photons is calculated up to high orders of perturbation theory and mass expansion . The application of the effective potential technique to the analysis of the correlators of the scalar gluonic currents which emerge in the decay of the Higgs boson into hadrons was considered in Ref. .

### 3.3 Results for the induced tensor current

In the context of the effective action we consider a tensor current of the form

$$J^{\mu \nu }=\overline{\psi }\sigma ^{\mu \nu }\psi ,\sigma ^{\mu \nu }=\frac{i}{2}[\gamma ^\mu ,\gamma ^\nu ]$$
(17)
and calculate its low-energy limit induced by a heavy quark loop. The properties of this current are rather similar to those of the electromagnetic current. Note that the classical vector mesons ($`\rho `$, $`\omega `$, $`\varphi `$) interact with this current and can be produced by it. We introduce an interaction

$$\mathrm{\Delta }L_T=g_T\overline{\psi }\sigma ^{\mu \nu }\psi F_{\mu \nu }$$
(18)
in the Lagrangian of heavy quarks and readily find the effective action for gauge fields induced by such a vertex. The low-energy limit at the one-loop order reads

$$\mathrm{\Gamma }_T=\frac{g_Tg_s^3d_{abc}}{180m^3(4\pi )^2}\left(32\mathrm{t}\mathrm{r}(FG^aG^bG^c)15\mathrm{t}\mathrm{r}(FG^a)\mathrm{tr}(G^bG^c)\right)$$
(19)
with the same notations as in Eq. (6). According to the form of the effective interaction in Eq. (18) the induced current $`J_{\mu \nu }`$ is given by a derivative

$$g_TJ^{\mu \nu }=\frac{\delta \mathrm{\Gamma }_T}{\delta F_{\mu \nu }}$$
(20)
and explicitly reads

$$J^{\mu \nu }=\frac{g_s^3d_{abc}}{180m^3(4\pi )^2}\left(32(G^aG^bG^c)^{\mu \nu }15(G^a)^{\mu \nu }\mathrm{tr}(G^bG^c)\right).$$
(21)
Note the lower power of the heavy quark mass in Eq. (21) as compared to Eq. (15).

## 4 Phenomenological applications

High precision tests of the standard model remain one of the main topics of particle phenomenology . The recent observation of a possible signal from the Higgs boson may complete the experimentally confirmed list of the standard model particles . Because experimental data are becoming more and more accurate, the determination of numerical values of the parameters of the standard model Lagrangian will require more accurate theoretical formulae. Recently an essential development in high-order perturbation theory calculations has been observed. A remarkable progress has been made in the heavy quark physics where a number of new physical effects have been described theoretically with high precision. The cross section of top–antitop production near the threshold has been calculated at the next-to-next-to-leading order of an expansion in the strong coupling constant and velocity of a heavy quark with an exact account for Coulomb interaction (as a review, see Refs. ). This theoretical breakthrough allows for the best determination of a numerical value of the top quark mass from experimental data. The method of Coulomb resummation resides on a nonrelativistic approximation for the Green function of the quark-antiquark system near the threshold and has been successfully used for the heavy quark mass determination within sum rule techniques . Being applied to quarkonium systems this method is considered to give the best estimates of heavy quark mass parameters . Technically an enhancement of near-threshold contributions to sum rules is achieved by considering integrals of the spectral density of the heavy quark production with weight functions which suppress the high-energy tail of the spectrum. The integrals with weight functions $`1/s^n`$ for different positive integer $`n`$, $`s=E^2`$, where $`E`$ is the total energy of the quark-antiquark system, are called moments of the spectral density and are most often used in the sum rule analysis . The interest in the precision determination of the $`c`$-quark mass is especially high because this parameter introduces the largest uncertainty to the theoretical calculation of the running electromagnetic coupling constant at $`M_Z`$ which is one of the key quantities for the constraints to the Higgs boson mass . We stress that in the corresponding determination of the running electromagnetic coupling constant at $`M_Z`$ based on direct integration of experimental data over the threshold region, the sensitivity of the results to the $`c`$-quark mass is much weaker .

For phenomenological applications of our results one therefore has to compute the two-point correlation functions of induced currents. In the following we show that there is a strong constraint on the order $`n`$ of the moment that can be used in heavy quark sum rules. Because of the contribution of low-energy gluons, only the first few moments exist if the theoretical expressions for the correlators include the $`O(\alpha _s^3)`$ order of perturbation theory.

### 4.1 The spectrum for the induced vector current correlator

First we discuss the case of the vector current where the data are obtained from $`e^+e^{}`$ annihilation experiments and are rather precise. The basic quantity for the analysis of a vector current $`j^\mu =\overline{q}\gamma ^\mu q`$ of a heavy fermion $`q`$ within sum rules is the vacuum polarization function

$$12\pi ^2iTj_\mu (x)j_\nu (0)e^{iqx}d^4x=(q_\mu q_\nu g_{\mu \nu }q^2)\mathrm{\Pi }(q^2).$$
(22)
With the spectral density $`\rho (s)`$ defined by the relation

$$\rho (s)=\frac{1}{2\pi i}(\mathrm{\Pi }(s+i0)\mathrm{\Pi }(si0)),s>0,$$
(23)
the dispersion representation

$$\mathrm{\Pi }(q^2)=\frac{\rho (s)ds}{sq^2}$$
(24)
holds. A necessary regularization and subtraction is assumed in Eq. (24). The normalization of the vacuum polarization function $`\mathrm{\Pi }(q^2)`$ in Eq. (22) is chosen such that one obtains the high-energy limit $`lim_s\mathrm{}\rho (s)=1`$ for a lepton. For the quark in the fundamental representation of the gauge group $`SU(N_c)`$ the high-energy limit of the spectral density reads $`\rho (\mathrm{})=N_c`$. The integral in Eq. (24) runs over the whole spectrum of the correlator in Eq. (22) or over the whole support of the spectral density $`\rho (s)`$ in Eq. (23).

A correlator of the induced vector current $`J^\mu `$ has the general form

$$TJ^\mu (x)J^\nu (0)=_\alpha _\beta T𝒪^{\mu \alpha }(x)𝒪^{\nu \beta }$$
(25)
where an explicit expression of the current as a derivative of the antisymmetric operator $`𝒪^{\mu \nu }`$ has been employed. The resulting correlator $`T𝒪^{\mu \alpha }(x)𝒪^{\nu \beta }`$ in Eq. (25) contains only gluonic operators. Such correlators were considered previously in the framework of perturbation theory . In leading order of perturbation theory the correlator in Eq. (25) has a topological structure of a sunset diagram, as it is shown in Fig. 2(a).

Technically, a convenient procedure of computing the sunset-type diagrams is to work in configuration space . We find

$$TJ_\mu (x)J_\nu (0)=\frac{34d_{abc}d_{abc}}{2025\pi ^4m^8}\left(\frac{\alpha _s}{\pi }\right)^3\left(_\mu _\nu g_{\mu \nu }^2\right)\frac{1}{x^{12}}.$$
(26)
A Fourier transform of the correlator in Eq. (26) gives the vacuum polarization function in momentum space which reads

$$12\pi ^2iTJ_\mu (x)J_\nu (0)e^{iqx}d^4x=(q_\mu q_\nu g_{\mu \nu }q^2)\mathrm{\Pi }(q^2)$$
(27)
where at small $`q^2`$ ($`q^2m^2`$)

$$\mathrm{\Pi }(q^2)|_{q^20}=C_g\left(\frac{q^2}{4m^2}\right)^4\mathrm{ln}\left(\frac{\mu ^2}{q^2}\right),C_g=\frac{17d_{abc}d_{abc}}{243000}\left(\frac{\alpha _s}{\pi }\right)^3.$$
(28)
For QCD with the colour group $`SU(3)`$ one has $`d_{abc}d_{abc}=40/3`$. The spectral density of the vacuum polarization function $`\mathrm{\Pi }(q^2)`$ in Eq. (27) is given at small values for $`s`$ by

$$\rho (s)|_{s0}=C_g\left(\frac{s}{4m^2}\right)^4.$$
(29)
Note that the spectral density in Eq. (29) can be found without an explicit calculation of its Fourier transform. Instead one can use a spectral decomposition (dispersion representation) in configuration space which was heavily employed for the analysis of sunset diagrams in Ref. . In this particular instance the spectral representation of the correlator in configuration space reads

$$\frac{i}{x^{12}}=\frac{\pi ^2}{2^8\mathrm{\Gamma }(6)\mathrm{\Gamma }(5)}_0^{\mathrm{}}s^4D(x^2,s)𝑑s$$
(30)
with $`D(x^2,s)`$ being the propagator of a scalar particle of mass $`\sqrt{s}`$,

$$D(x^2,m^2)=\frac{im\sqrt{x^2}K_1(m\sqrt{x^2})}{4\pi ^2(x^2)}$$
(31)
where $`K_1(z)`$ is the McDonald function (a modified Bessel function of the third kind, see e.g. Ref. ). $`\mathrm{\Gamma }(z)`$ is Euler’s gamma function.

An asymptotic behaviour of the spectral density of the corresponding contribution for large energies (where the limit of massless quarks can be used) enters the expression for the ratio $`R(s)`$ of $`e^+e^{}`$ annihilation into hadrons and has been known since long ago . This term is usually called light-by-light (lbl) contribution and reads

$$R^{\mathrm{lbl}}(s)=\left(\frac{\alpha _s}{\pi }\right)^3\frac{d_{abc}d_{abc}}{1024}\left(\frac{176}{3}128\zeta (3)\right).$$
(32)
Here $`\zeta (z)`$ is the Riemann $`\zeta `$ function with $`\zeta (3)=1.20206\mathrm{}`$ The contribution to the spectral density given in Eq. (32) is negative while our result given in Eq. (29) is positive as it should be the case for the spectral density of the electromagnetic current as a Hermitean operator.

### 4.2 The spectrum for the induced tensor current correlator

The results for the correlator of the tensor current given in Eq. (21) are slightly more complicated. The correlator reads

$`12\pi ^2i{\displaystyle Tj_{\mu \nu }(x)j_{\alpha \beta }(0)e^{iqx}d^4x}=(g_{\mu \alpha }g_{\nu \beta }g_{\mu \beta }g_{\nu \alpha })\mathrm{\Pi }_g(q^2)`$ (33)
$`+(g_{\mu \alpha }q_\nu q_\beta g_{\mu \beta }q_\nu q_\alpha g_{\nu \alpha }q_\mu q_\beta +g_{\nu \beta }q_\mu q_\alpha )\mathrm{\Pi }_q(q^2)`$
where two scalar amplitudes are possible now. One finds

$$\mathrm{\Pi }_g(q^2)=\frac{q^2}{2}\mathrm{\Pi }_q(q^2)=\frac{61d_{abc}d_{abc}}{729000}\left(\frac{\alpha _s}{\pi }\right)^3\frac{q^2}{4}\left(\frac{q^2}{4m^2}\right)^3\mathrm{ln}\left(\frac{\mu ^2}{q^2}\right).$$
(34)
The physical content of the amplitudes $`\mathrm{\Pi }_g(q^2)`$ and $`\mathrm{\Pi }_q(q^2)`$ is related to contributions of the states with $`J^{PC}=1^{}`$ and $`J^{PC}=1^+`$, resp. Note that the sum rule analysis for the mesons with quantum numbers $`J^{PC}=1^+`$ has been done in Ref.  with quark interpolating currents. From the present results we also see a possibility to use gluonic currents as interpolating operators for such mesons. The validity of such a description depends strongly on the strength of the interaction of the meson in question with the corresponding interpolating operator which is difficult to estimate independently.

Note that there are only two independent gluonic operators to construct the induced currents under consideration. The electromagnetic current is given by a derivative of a special linear combination of these operators while the tensor current is given by a linear combination of operators themselves. There is one more current relevant to the situation. It originates from the Gordon decomposition of the electromagnetic current (see e.g. Ref. )

$$2m\overline{\psi }\gamma ^\mu \psi =_\nu (\overline{\psi }\sigma ^{\mu \nu }\psi )+\overline{\psi }i\stackrel{}{D}{}_{}{}^{\mu }\psi .$$
(35)
This relation retains for the induced currents as well. The left hand side and the right hand side of Eq. (35) have different parity as for the number of Dirac $`\gamma `$-matrices between spinor fields which is reflected in an additional factor $`m`$ at the left hand side of Eq. (35). In the massless limit these types of currents are alien and can never mix. At the level of induced currents the Dirac structure of the initial heavy quark currents is reflected in different degrees of suppression by the heavy quark mass $`m`$.

### 4.3 The spectrum for a mixed current correlator

Having both currents at hand, one can study a mixed correlator of the form

$$12\pi ^2iTJ_\mu (x)J_{\alpha \beta }(0)e^{iqx}d^4x=i(g_{\mu \alpha }q_\beta g_{\mu \beta }q_\alpha )\mathrm{\Pi }_M(q^2)$$
(36)
with a single scalar amplitude $`\mathrm{\Pi }_M(q^2)`$. Such mixed correlators are useful in sum rule applications . One finds

$$\mathrm{\Pi }_M(q^2)=\frac{67d_{abc}d_{abc}}{972000}\left(\frac{\alpha _s}{\pi }\right)^3\frac{q^2}{4m}\left(\frac{q^2}{4m^2}\right)^3\mathrm{ln}\left(\frac{\mu ^2}{q^2}\right)$$
(37)
The physical content of the amplitude is given by the $`J^{PC}=1^{}`$ resonance, i.e. by the $`\mathrm{{\rm Y}}`$-family in case of $`b`$ quarks.

## 5 Moments of the spectral density

As mentioned earlier, the moments of the spectral density $`\rho (s)`$ of the form

$$_n=\frac{\rho (s)ds}{s^{n+1}}$$
(38)
are usually studied within the sum rule method for heavy quarks . These moments are related to the derivatives of the vacuum polarization function $`\mathrm{\Pi }(q^2)`$ at the origin,

$$_n=\frac{1}{n!}\left(\frac{d}{dq^2}\right)^n\mathrm{\Pi }(q^2)|_{q^2=0}.$$
(39)
Such moments are chosen in order to suppress the high energy part of the spectral density $`\rho (s)`$ which is not measured accurately in the experiment. Within the sum rule method one assumes that the moments in Eq. (38) can be calculated for any $`n`$ or, equivalently, that the derivatives in Eq. (39) exist for any $`n`$. The existence of moments seems to be obvious because one implicitly assumes that the spectral density $`\rho (s)`$ of the heavy quark electromagnetic currents vanishes below the two-particle threshold $`s=4m^2`$ which means that the vacuum polarization function $`\mathrm{\Pi }(q^2)`$ of heavy quarks is analytic in the whole complex plane of $`q^2`$ except for the cut along the positive real axis starting from $`4m^2`$. This assumption about the analytic properties of the vacuum polarization function $`\mathrm{\Pi }(q^2)`$ is known to be wrong if a resummation of Coulomb effects to all orders of perturbation theory is performed: as a result of such a resummation the Coulomb bound states appear below the perturbation theory threshold $`s=4m^2`$.

### 5.1 Infrared singular behaviour of the moments

The qualitatively new feature of effective currents given in Eqs. (15) and (21) is that they are expressed through massless fields. Therefore the spectrum of the two-point correlators of these currents start at zero energy. This feature drastically changes the analytic structure of the two-point correlators of these currents and, in particular, their infrared (IR) or small $`s`$ behaviour because of the branching point (cut) singularity of $`\mathrm{\Pi }(q^2)`$ at the origin $`q^2=0`$. This new feature of having a nonvanishing spectrum below the formal tree-level two-particle threshold which appears at the $`O(\alpha _s^3)`$ order of perturbation theory for induced current correlators has important phenomenological consequences. Indeed, such a change of the analytic structure of induced current correlators affects strongly the theoretical expressions for some observables usually employed in heavy quark physics for the precision determination of the parameters of heavy quarks and their interactions.

Because of the low-energy gluon contributions, the large $`n`$ moments of the spectral density in Eq. (38) do not exist and cannot be used for phenomenological analyses. Caused by the factor $`(s/4m^2)^4`$ in Eq. (38) the moments become IR singular for $`n4`$ in case of the induced vector current. This can already be seen by looking at the factor $`1/m^4`$ in the induced vector current in Eq. (15). For the induced tensor current the corresponding moments start to diverge earlier because of a weaker suppression by the heavy quark mass, the corresponding factor in Eq. (21) is $`1/m^3`$ instead of $`1/m^4`$. Therefore, in this case the moments become IR singular already for $`n3`$. Note that in early considerations of sum rules quite large $`n`$ were used. For instance, the numerical value of the gluon condensate was extracted from sum rules for the moments with $`n10÷20`$ . In view of our result on the low-energy behaviour of the spectral density, one has either to limit the accuracy of theoretical calculations for the moments to the $`O(\alpha _s^2)`$ order of perturbation theory which seems insufficient for a high precision analysis of quarkonium systems (especially if the Coulomb resummation to all orders is performed) or to use only a few first moments. For small $`n`$, however, the high-energy contribution, which is not known experimentally with a reasonable precision, is not sufficiently suppressed and introduces a large quantitative uncertainty into the sum rules for the moments. An analysis based on finite energy sum rules is free from such a problem and can be used in phenomenological applications .

Note in passing that there is no low-energy gluon contribution (and therefore no low-energy divergence problem) for correlators of the currents containing only one heavy quark with mass $`m`$. The spectrum of such correlators starts at $`m^2`$ and there are no massless intermediate states contributing to the correlator in perturbation theory (see e.g. Ref. ). The theoretical expressions for such correlators can be used for high precision tests of theoretical predictions when the accuracy of experimental data in corresponding channels will improve in the future.

### 5.2 An infrared safe moment definition

The infinite-integration sum rules with large $`n`$ can be retained at high orders of perturbation theory if an appropriate cutoff at small energies is introduced. This can be readily achieved by calculating the moments (or derivatives) at some Euclidean point $`q^2=\mathrm{\Delta }`$ . Indeed, for the regularized moments

$$_n(\mathrm{\Delta })=\frac{1}{n!}\left(\frac{d}{dq^2}\right)^n\mathrm{\Pi }(q^2)|_{q^2=\mathrm{\Delta }}=\frac{\rho (s)ds}{(s+\mathrm{\Delta })^{n+1}}$$
(40)
there is no divergence at small $`s`$. However, the regularization parameter $`\mathrm{\Delta }`$ cannot be arbitrary small. The reason is that the resulting correlator of gluonic currents in Eq. (25) is essentially normalized at $`\mu ^2=\mathrm{\Delta }`$ when radiative corrections are taken into account, like the diagram shown in Fig. 2(b). The corrections are known to be large and, therefore, $`\mathrm{\Delta }`$ is much larger than the expected IR scale in quark channels . This observation makes the phenomenological analysis based on the regularized sum rules in Eq. (40) unprecise even for reasonably large $`n`$ because the continuum contribution to moments is not suppressed for large values of $`\mathrm{\Delta }`$. The suppression of the high-energy tail can be enhanced by constructing a more special kind of moments which exploit the explicit behaviour of the spectral density at low energy. The IR safe moments with a more efficient suppression of high-energy tail for the induced vector current have the form

$$\stackrel{~}{}_n(\mathrm{\Delta })=\frac{\rho (s)ds}{s^3(s+\mathrm{\Delta })^{n+1}}$$
(41)
It seems that even in such an optimized form these moments cannot be used for the $`c\overline{c}`$-system, i.e. for analyzing $`J/\psi `$ resonances because the suppression is insufficient for achieving the precision goals necessary for the $`c`$-quark mass determination. For the $`b\overline{b}`$-system, i.e. for the analysis of $`\mathrm{{\rm Y}}`$-resonances the dependence on the cutoff $`\mathrm{\Delta }`$ is numerically essential for moments at large $`n`$ and for $`\mathrm{\Delta }`$ as large as $`\mathrm{\Delta }=1÷2\mathrm{GeV}^2`$ which is still small according to the estimates of radiative corrections in gluonic channels. We would like to remind the reader that Coulomb poles which are essential for the analysis of the $`\mathrm{{\rm Y}}`$-resonance and $`b\overline{b}`$-production near threshold give contributions which are formally of the $`O(\alpha _s^3)`$ order (for the value of the Coulombic wave function at the origin see e.g. Ref. ), an order which coincides with the order of corrections considered here (see Eq. (28)). The theoretical expressions for the correlators in the scalar channel where below threshold corrections start at the $`O(\alpha _s^2)`$ order are more sensitive to these special below threshold contributions. However, data in the scalar channel are considerably worse than those in the vector channel and there is no possibility of a high precision analysis on the scalar channel at present.

## 6 Conclusions

We have presented corrections to the heavy quark currents induced by a virtual heavy quark loop and expressed through the gluon operators. We have considered the electromagnetic current and the tensor current closely related to it. Heavy quark loop induced corrections first appear at $`O(\alpha _s^3)`$ order of perturbation theory and are given by the $`1/m^4`$ term of the mass expansion in case of the electromagnetic current and by the $`1/m^3`$ term in case of the tensor current. The spectra of the correlators of such induced currents start at zero energy. This fact makes impossible the standard analysis of the moment sum rules at $`O(\alpha _s^3)`$ order of perturbation theory for $`n4`$ in case of the electromagnetic current and for $`n3`$ in case of the tensor current.

### Acknowledgements

The work is partially supported by the Russian Fund for Basic Research under contracts 99-01-00091 and 01-02-16171. A.A. Pivovarov is an Alexander von Humboldt fellow. S. Groote acknowledges a grant given by the Deutsche Forschungsgemeinschaft, Germany.


text:
# Surface Magnetic Phase Diagram of Tetragonal Manganites

## I Introduction

Over the last half a decade, the perovskite colossal magnetoresistive (CMR) manganites have attracted intensive attention due to the remarkably rich variety of structural, magnetic, transport and optical properties  and are regarded as potentially important materials for the next generation technology. Such possibility may be a strong motivation for the study of thin films and superlattices  of the manganites and the related materials. In these systems surfaces and interfaces will play important roles. However, even without appealing to thin films and superlattices, surfaces and interfaces are involved in various aspects. The enhanced low-field magnetoresistance has been reported in the polycrystalline samples due to the spin-dependent behaviors across the grain boundaries . The photoemission data , which provide evidence for the half-metallicity, and the scanning tunneling spectroscopy (STS)  or microscopy (STM) , which provide evidence for the spatial phase-separation , are all surface sensitive. Therefore, the basic understanding of the surfaces of doped manganites is an urgent and challenging problem. It is already established that one of the most important implications in the physics associated with the CMR manganites is the key roles of orbital degrees of freedom (ODF) , which couple strongly with the lattice, charge and magnetic degrees of freedom (MDF). We expect that the ODF will play even more important roles on the surfaces due to the lowering in symmetry and dimensionality.

Detailed experimental and theoretical studies on the surfaces of CMR manganites have started only very recently  and the results obtained so far are not yet sufficient to establish any general picture about the surface phase diagram. In the experimental side, it is still difficult to prepare well defined surfaces. In the theoretical side, on the other hand, only some limited phase space and limited conditions have been taken into account. Although it is not possible to consider the complete phase space and all possible complications conceivable in real systems, it is very important to construct a general qualitative picture for the surface phase diagram by taking account of possible phases and some important experimental conditions. This is what we aim in the present work by taking La1-xSrxMnO3 (LSMO) as a canonical system of doped manganites .

First, since it is possible to control the terminations by chemical treatment of the surface  or by controlling the chemical potential , consideration of two possible terminations of (001) surface is important. It is natural to expect that the surface effect will be strong for the MnO2 termination, but weak for the (La, Sr)O termination, due to the loss of part of the ligand of Mn in former case. Although the expectation is qualitatively true, the change in the electrostatic potential for SrO termination can also produce significant change in the electronic structure. Second, the lattice deformation induced by the substrates can produce cooperative stabilization of orderings in ODF and MDF, leading to strong anisotropy in the thin film . Therefore, in the present work, we will present a general surface phase diagram of LSMO, for both the (La, Sr)O and MnO2 terminated (001) surfaces, as functions of the hole doping $`x`$ and the bulk tetragonal distortion $`c/a`$ ratio induced by the substrates. We found that the (La, Sr)O terminated surface shows strong tendency toward the A-type antiferromagnetic (AF) state, while the surface phases of MnO2 termination are dominated by the C-type AF state. The basic physics behind is the ordering in the surface ODF of Mn $`e_g`$ states. Third, we found that the Sr atoms should seriously segregate towards the surfaces due to the electrostatic interaction. The general tendency of surface segregation will further favor the surface AF states.

## II Calculation Methods

The present work is based on the first-principles electronic structure calculations, which adopt the PBE version  of generalized gradient approximation (GGA). The Kohn-Sham equation is solved by using the pseudopotential technique. The Mn(3d) and the O(2p) states are treated by the ultra-soft pseudopotential , while the norm-conserving scheme  is used for other states. The cutoff energies for the plane-wave expansions of wavefunction and charge density are 30 Ry and 200 Ry respectively. LaxSr1-x is treated as a virtual atom by the virtual crystal approximation (VCA) . In present systems, the valence electronic states near and below the Fermi level are contributed mostly by Mn and O, the states coming from La and Sr are far above the Fermi level. Therefore, the simple VCA can provide a reasonable description of the systems. The validity of these techniques was well demonstrated in our previous calculations for the bulk . We use a repeated slab geometry, which includes five MnO2 layers with mirror symmetry in the central MnO2 layer. As the MnO2 layer and the (La, Sr)O layer are stacked alternately along the surface normal, i.e., $`z`$-axis, nine and eleven atomic layers in total are included in the unit cell for the MnO2 and (La, Sr)O terminations, respectively. A vacuum region of $`1213`$Å is included to separate the slabs. Several magnetic states, i.e., ferromagnetic (FM), A-type AF and C-type AF states, are calculated in the present study. In the A-type AF state, the magnetic moment of Mn are aligned ferromagnetically in the $`ab`$-plane (slab plane) and these FM layers are coupled antiferromagnetically along the $`c`$ direction (surface normal). In the C-type AF state, on the other hand, the FM chains along the $`c`$ direction are coupled antiferromagnetically. In the surface phase diagrams in Fig.1, the above definition is applied to the slab. A simple schematic description about the spin configurations of surface A- and C-type AF states can be found in Fig.2. To accommodate the C-type AF states, we use the planar c(2x2) unit cell. The atomic positions and magnetic states are fully optimized for each of given $`ab`$-plane lattice constants, which define the bulk $`c/a`$ ratio since the bulk volume is given for each doping $`x`$. By choosing the lowest energy state among FM, A-type AF and C-type AF states for each $`ab`$-plane lattice constant and each doping $`x`$, we can construct the surface phase diagram.

## III Results and discussion

We show the calculated surface phase diagrams in Fig. 1 compared with the bulk phase diagram which was obtained in our previous calculations . The surface phase diagrams for the (La, Sr)O and MnO2 terminations are indicated by the red and green lines respectively. Clearly for the MnO2 termination, the surface phases are dominated by the C-type AF state for a wide range of doping $`x`$ and $`c/a`$ ratio, except a tiny FM region in the very small $`c/a`$ ratio and low doping case. On the other hand for the (La, Sr)O termination, the surface shows rich phases similar to the bulk case but with a significant shift. Compared with the bulk phase diagram (indicated by black lines and characters), the main change for the surfaces is the up- and downward shifts of the phase boundaries for (La, Sr)O and MnO2 termination respectively. It should be noted that, since non-equal numbers of (La, Sr)O and MnO2 layers are included in our unit cell, the effective doping $`x_{\mathrm{eff}}`$ of the central MnO2 layer is slightly different from the formula doping $`x`$. By calculating the number of $`e_g`$ electrons, we estimate that the $`x_{\mathrm{eff}}`$ is smaller (larger) than $`x`$ by about 0.04 (0.05) for (La, Sr)O (MnO2) termination. For the sampling point ($`x=0.5`$ and $`c/a=1.0`$, indicated by the blue star in Fig. 1), the calculated total energies and some physical parameters are summarized in Tables I and II. It should be also noted here that the presence of interfaces between the surface and bulk regions may modify our calculated phase diagram slightly. If the penetration of the perturbation in the magnetic state on surface is deeper than half of the slab thickness, the surface phase diagram may depend on the slab thickness. In order to check these effects, we performed calculations in which the spin structures of the central MnO2 layer are constrained to be the bulk ones. We found that the spin structures in the first two surface layers (of both sides of the slabs) are little affected by the constraint in the central layer. We should also point out that the possible non-collinear magnetic configurations are not taken into account in the present calculation. However, even if we confine ourselves to collinear spin configurations, we can still gain important valuable insights into the basic trend in surface magnetic states by our calculated phase diagram.

The occupation imbalance between two $`e_g`$ orbitals, namely $`3z^2r^2`$ and $`x^2y^2`$ orbitals in doped manganites, is the key concept to understand the rich phase diagrams . On the surfaces, the orbital polarization is certainly very important because of the change in crystal field, hybridization and surface lattice relaxation. For the (La, Sr)O termination, the environment of the 2nd surface Mn changes only from the 2nd nearest neighbor layer, which is negatively charged MnO2 layer. Missing of this layer in the vacuum side produces an attractive potential leading to downward shift of the 2nd surface Mn $`3d`$ bands. However, the strengthened $`pd\sigma `$ hybridization due to the missing Mn atom on top of the surface O atom will cause the upward shift of the $`3z^2r^2`$ state compared with the $`x^2y^2`$ state. Although the surface relaxation in the interlayer distance, which is very small, will modify the details quantitatively, it will not affect the qualitative features. For the sampling structure in Fig. 1, the Mn-O bond length between the 1st and 2nd layers changes only by $`0.2\%`$ (see Table II). For the MnO2 termination, the most dramatic effect is the significant downward shift of the $`3z^2r^2`$ state due to the reduction in $`pd\sigma `$ hybridization caused by the missing ontop oxygen. For other orbitals, missing of the positively charged (La, Sr)O layer produces repulsive potential. In this case, the surface relaxation is very large because of the loss of ligand oxygen atoms. However, the atoms are relaxed in such a way that the topmost Mn-O bond length along surface normal direction is elongated to further push down the $`3z^2r^2`$ orbital. Therefore the net effect of surface orbital polarization is that the occupation of the $`x^2y^2`$ ($`3z^2r^2`$) orbital is enhanced for (La, Sr)O (MnO2) termination. The orbital population ratio $`n_{3\mathrm{z}^2\mathrm{r}^2}/n_{\mathrm{x}^2\mathrm{y}^2}`$ for the sampling structures in Fig. 1 are estimated as 0.74 and 2.16 for the surface Mn sites of (La, Sr)O and MnO2 terminations respectively. The surface orbital polarization of MnO2 termination is much stronger than that of (La, Sr)O termination. Figure 2 shows the charge distributions (from the Fermi level to 0.8 eV below) for two different terminations of the sampling point. The surface orbital polarizations are clearly seen in each case.

The change in occupation will change the competition between the double exchange (DE) and the superexchange (SE). For the less than half-filled majority-spin $`e_g`$ bands, the more (less) populated are the orbitals, the stronger (weaker) are the DE interactions among these orbitals. Therefore, the region of the A-type (C-type) AF state becomes wider for the (La, Sr)O (MnO2) termination because of higher population of the $`x^2y^2`$ ($`3z^2r^2`$) orbital. A. Filippetti and W. E. Pickett  studied the magnetic properties of MnO2 terminated (001) surface of La1-xCaxMnO3 (LCMO) with particular doping $`x`$ (=0.5). Their observation of the stability of the FM state is due to the use of the (1x1) surface unit cell. Our calculations for LSMO with the same doping ($`x=0.5`$, $`c/a=1.0`$) give the same order of total energy difference between the surface FM and A-type AF states (Table I). However, the surface C-type AF state has much lower energy compared with the above two states.

On the real surfaces of CMR manganites, the surface segregation on the perovskite A-sites may be another important factor. It was experimentally suggested that the Ca content in the surface layers of LCMO is dramatically enhanced  for both terminations. The basic questions here are: 1)why does surface segregation happen? 2)how will it affect our phase diagram? In the analysis of surface segregation, we need the bulk part as a particle reservoir. The present type slab calculation has, therefore, rather severe restriction in this context. In the following, we will do a simple analysis in order to gain insight into the fundamental aspects of the problem. We artificially locate a pure SrO layer at different positions in our unit cell keeping the Sr content $`x`$ in all other (La, Sr)O layers as a given value and calculate the total energy as a function of the SrO layer position. The calculated results shown in Fig. 3 clearly suggest that the stable position of the SrO layer is the surface for the (La, Sr)O termination or the 2nd surface for the MnO2 termination. The result is qualitatively consistent with the experimental observation for LCMO . The main reason for the stability of the surface (or subsurface) SrO layer is the electrostatic interaction. SrO layer is nominally charge neutral, while the nominal charge of LaO is +1. In the bulk the ionized object is stabilized by the electrostatic interaction with the counter ions. This stability mechanism is weakened on the surface. Therefore, the neutral object tends to be located on the surface keeping the charged objects inside the bulk. For the MnO2 termination, the presence of SrO layer at the 2nd surface will make the surface MnO2 layer nearly neutral also. In Fig. 3(b), we show that the contribution coming from the electrostatic energy is responsible to the stability of the SrO layer at the surface. As the nominal doping $`x`$ increases, the effect of Sr segregation should be weakened as is actually demonstrated in Fig. 3. Although the present analysis is only for limited configurations in which one particular layer of the system has full Sr segregation. Nevertheless, the above consideration about the mechanism of the stability of surface SrO layer clearly suggests a rather general tendency of surface segregation of the neutral objects. By taking account of the surface segregation of Sr, the effective doping on the surface becomes larger than the bulk doping. This will again lead to stronger stability of surface AF ordering.

## IV Summary

In summary, we calculated the surface magnetic phase diagram of tetragonal manganite LSMO as functions of hole doping $`x`$ and the bulk tetragonal distortion $`c/a`$. The (001) surfaces of tetragonal manganites show clear tendency towards A-type and C-type AF states for (La, Sr)O and MnO2 terminations respectively though the surface A-type AF state may be hard to distinguish experimentally from the surface FM state. The basic physics governing the phase diagram is explained in terms of the orbital polarization induced by surface effects. Strong surface segregation of Sr atoms is caused by the electrostatic interaction and further favors the tendency to surface antiferromagnetism.

## V Acknowledgments

The authors thank Professors Y. Tokura, E. W. Plummer, M. Kawasaki and R. Matzdorf for valuable comments and for providing us with their experimental data. The present work is partly supported by NEDO.