text:
# 𝒩=1/2 Wess-Zumino model is renormalizable

## 1 Introduction

It is commonly understood that for a four-dimensional quantum field theory to be renormalizable, every operator appearing in the Lagrangian must have a mass dimension less than or equal to 4. An important assumption in this statement is that the action is real. However, it was recently observed  that in string theory with a constant graviphoton background, the field theory of the string worldsheet suffers a deformation of its superspace coordinates $`\theta ^\alpha `$. These coordinates no longer anticommute, but satisfy a Clifford algebra: $`C^{\alpha \beta }=\{\theta ^\alpha ,\theta ^\beta \}`$. Supersymmetry is reduced by half. It follows too that the action is no longer real. In , it was found that this deformation of superspace effectively adds new terms, of dimension greater than 4, to the Wess-Zumino and Yang-Mills Lagrangians.111This deformation of superspace was considered previously for example in ; recent work on $`𝒩=\frac{1}{2}`$ supersymmetric field theories has appeared in . Initially it was expected that these deformed theories were unrenormalizable, but should simply be treated perturbatively. In this letter we defy intuition by demonstrating the renormalizability of the $`𝒩=\frac{1}{2}`$ Wess-Zumino model to all orders. Our result generalizes the recent work , which proved renormalizability up to two loops.

The classical Lagrangian is

$`{\displaystyle \mathrm{d}^4\theta \overline{\mathrm{\Phi }}\mathrm{\Phi }}+{\displaystyle \mathrm{d}^2\theta (\frac{m}{2}\mathrm{\Phi }^2+\frac{g}{3}\mathrm{\Phi }^3)}+{\displaystyle \mathrm{d}^2\overline{\theta }(\frac{\overline{m}}{2}\overline{\mathrm{\Phi }}^2+\frac{\overline{g}}{3}\overline{\mathrm{\Phi }}^3)}{\displaystyle \frac{g}{3}}det(C)F^3,`$ (1)
where

$`\mathrm{\Phi }(y,\theta )`$ $`=`$ $`A(y)+\sqrt{2}\theta \psi (y)+\theta \theta F(y)`$
$`\overline{\mathrm{\Phi }}(\overline{y},\overline{\theta })`$ $`=`$ $`\overline{A}(\overline{y})+\sqrt{2}\overline{\theta }\overline{\psi }(\overline{y})+\overline{\theta }\overline{\theta }\overline{F}(\overline{y}),`$
and $`y`$ and $`\overline{y}`$ are chiral coordinates. The $`F^3`$ term arising from the deformation of superspace might appear to render the theory unrenormalizable. However, the recent paper  showed that up to two loops it is in fact renormalizable, after adding by hand $`F`$ and $`F^2`$ terms to the Lagrangian. Specifically,  proved the following assertions up to two loops:

* Divergences are at most logarithmic.
* Divergent terms have at most one power of $`det(C)`$.
* Divergent terms are of the form $`F^{\mathrm{}}\overline{G}^k`$, where $`\overline{G}\overline{m}\overline{A}+\overline{g}\overline{A}^2`$.
* Contractions with $`\overline{G}`$ are equivalent to contractions with $`F`$, and thus the counterterms from $`F,F^2,F^3`$ suffice to renormalize the theory.

In this work we prove the same assertions to all orders. We work in terms of component fields, making use of the two $`U(1)`$ (pseudo)symmetries of the theory (see  and the Appendix), as well as Feynman diagram combinatorics, to constrain the form of divergent terms in the effective action.

The reasoning of this kind of renormalizability is discussed in detail in . The essential point is that the higher-dimensional term (like $`F^3`$) acts as a source vertex with no corresponding sink (like $`\overline{F}^3`$ or $`A^3`$), so these vertices do not show up in arbitrarily high order diagrams. This point can be seen clearly in our argument below; for example, the $`F^3`$ term can appear only once in any divergent diagram.

## 2 At most log divergence and one power of $`det(C)`$

In this section we use symmetry arguments to show that the effective action has at most logarithmic divergences, and that the divergent terms have at most one power of $`det(C)`$.

Suppose a general divergent operator appears in the effective action with a coefficient $`\lambda `$:

$`\mathrm{\Gamma }_𝒪=\lambda 𝒪,`$
and that $`\lambda `$ has mass dimension $`d`$ and charges $`q_R=R,q_\mathrm{\Phi }=S`$ under the two global U(1) (pseudo)symmetries, whose action is described in the Appendix. By dimensional analysis and charge considerations, and with an ultraviolet momentum cutoff, we will have

$`\lambda \mathrm{\Lambda }^dg^{x+4zR}\overline{g}^x\left({\displaystyle \frac{m}{\mathrm{\Lambda }}}\right)^y\left({\displaystyle \frac{\overline{m}}{\mathrm{\Lambda }}}\right)^{y+6z+\frac{S3R}{2}}\left(det(C)\mathrm{\Lambda }^2\right)^z`$ (2)
from the loop calculation, where $`x,y,z`$ are nonnegative integers; the nonegative powers of $`m,\overline{m},g,\overline{g}`$ and $`det(C)`$ come from the propagators and vertices.

The most general operator $`𝒪`$ is given by

$`𝒪^pA^{\alpha _1}\overline{A}^{\overline{\alpha }_1}F^{\alpha _2}\overline{F}^{\overline{\alpha }_2}\psi ^{\alpha _3}\overline{\psi }^{\overline{\alpha }_3}.`$
The differential operators are understood to act on the others in all possible combinations; for our purposes it is enough to count the overall dimension. Because the term $`\mathrm{\Gamma }_𝒪`$ must have mass dimension 4 and zero charge, we must have

$`d`$ $`=`$ $`4p(\alpha _1+\overline{\alpha }_1+2\alpha _2+2\overline{\alpha }_2+{\displaystyle \frac{3}{2}}\alpha _3+{\displaystyle \frac{3}{2}}\overline{\alpha }_3)`$
$`R`$ $`=`$ $`\alpha _1+\overline{\alpha }_1+\alpha _2\overline{\alpha }_2`$
$`S`$ $`=`$ $`\alpha _1+\overline{\alpha }_1\alpha _2+\overline{\alpha }_2\alpha _3+\overline{\alpha }_3`$
Thus, the overall power of $`\mathrm{\Lambda }`$ in $`\mathrm{\Gamma }_𝒪`$ is

$`P`$ $`=`$ $`44z2yp2\alpha _14\overline{\alpha }_2\alpha _32\overline{\alpha }_3.`$ (3)
The new operator is superficially divergent iff $`P0`$. Note that this restricts $`z`$, which is the power of $`det(C)`$, to be 0 or 1. (1) If $`z=0`$, it is the ordinary Wess-Zumino case with only the familiar wave function renormalization; we will not discuss it here. (2) If $`z=1`$, then $`y=p=\alpha _1=\overline{\alpha }_2=\alpha _3=\overline{\alpha }_3=0`$, and there is at most a logarithmic divergence. The possibly divergent operators take the form $`\overline{A}^{\overline{\alpha }_1}F^{\alpha _2}`$.

## 3 Finitely many divergent operators

Now we show that there are only finitely many divergent operators, namely

$`\overline{A}^{\overline{\alpha }_1}F^{\alpha _2},\mathrm{for}\overline{\alpha }_1+2\alpha _26\mathrm{and}\alpha _21.`$ (4)
Let us examine the Feynman diagrams that generate a given operator. We introduce the following nonnegative integers to count the number of each type of vertex and propagator that appears in the diagram:

$`a_0:F^3,a_1:\overline{A}^2\overline{F},b_1:\overline{A}\overline{\psi }\overline{\psi },a_2:A^2F,b_2:A\psi \psi ,`$
$`c_1:A\overline{A},c_2:F\overline{F},c_3:AF,c_4:\overline{A}\overline{F},`$
$`d_1:\psi \psi ,d_2:\overline{\psi }\overline{\psi },d_3:\psi \overline{\psi }.`$
Now, by matching powers of the coupling constants, we can specify the exponents in the previous section: $`(x,y,z)=(a_1+b_1,c_4+d_2,a_0)`$. Moreover, restricting to possibly divergent operators, we apply the main result of the previous section to set $`c_4=d_2=0`$ and $`a_0=1`$. By matching the appearances of each field among vertices, contractions and external lines, we can derive six conditions on these integers. One consequence of these conditions is that $`d_1=6\overline{\alpha }_12\alpha _2c_3`$. Because $`d_1`$ is nonnegative, it follows that $`\overline{\alpha }_1+2\alpha _26`$, which is the desired result. The additional condition $`\alpha _21`$ follows from the nonrenormalization of the antiholomorphic superpotential .

## 4 Repackaging in terms of $`\overline{G}`$

The arguments of the previous two sections have proved the renormalizability of the $`𝒩=\frac{1}{2}`$ supersymmetric Wess-Zumino model. However, the observation made in  up to two loops is a stronger result: divergent terms can be packaged in terms of $`F`$ and $`\overline{G}\overline{m}\overline{A}+\overline{g}\overline{A}^2`$. We now show that this result applies generally. The divergent terms generated are

$`F,F^2,F^3,F\overline{G},F^2\overline{G},F\overline{G}^2.`$
We then invoke the beautiful argument of , that a contraction of any field with $`\overline{G}`$ is equivalent to its contraction with $`F`$.222Being able to trade $`\overline{G}`$ exactly for $`F`$ is also a consequence of the nonrenormalization of the antiholomorphic superpotential that was shown in . We conclude that the counterterms for $`F,F^2`$ and $`F^3`$ suffice to renormalize the theory.

To begin, we simplify our task by neglecting diagrams with fermion loops. This is allowed, because there will be a corresponding bosonic loop that cancels the contribution at least partially. Since the leading order is already log divergent, partial cancellation gives at most a finite total contribution. So we are free to set $`b_i=d_j=0`$.

We will classify our divergent 1PI diagrams by powers of $`\overline{A}`$ (as external lines) relative to a base diagram with no powers of $`\overline{A}`$. Consider the following operations on diagrams:

* Insertion: Where there is a propagator $`AF`$, the vertex $`\overline{A}^2\overline{F}`$ can be inserted, so that there are now two propagators, $`A\overline{A}`$ and $`F\overline{F}`$, and an additional external line $`\overline{A}`$. It is easy to see that the divergence from the momentum integration is not modified. The replacement can be sketched as $`\overline{m}\overline{g}\overline{A}`$.
* Deletion: Where there is an external line $`\overline{A}`$, it must lead to a vertex $`\overline{A}^2\overline{F}`$, since there are no fermion loops. Because $`c_4=0`$, there are no propagators $`\overline{A}\overline{F}`$. Thus this vertex must be contracted with $`A`$ and $`F`$, via the propagators $`A\overline{A}`$ and $`F\overline{F}`$. The vertex can be cut out of the diagram, and the two propagators replaced by the single propagator $`AF`$. Again, the divergence is not modified.

These two operations are inverse. By applying deletion repeatedly, every diagram can be reduced to a ‘base diagram’ with only $`F`$ on the external lines. To see these two operations more clearly, Figure 1 will be helpful.

We apply insertion to build up all possible diagrams with a given base diagram for $`F^{\mathrm{}}`$. Let $`q`$ be the number of $`AF`$ propagators in the base diagram. From the results in the previous section, we know in fact that $`q=62\mathrm{}`$. Note in particular that $`q`$ is even and $`q4`$.

From this base, there are $`\left(\genfrac{}{}{0pt}{}{q}{k}\right)2^k`$ ways to insert $`k`$ external lines $`\overline{A}`$—namely $`\left(\genfrac{}{}{0pt}{}{q}{k}\right)`$ ways to choose the propagators for insertion, and two choices for the external line from each new vertex $`\overline{A}^2\overline{F}`$. Moreover, each insertion yields a diagram with a relative factor $`\frac{\overline{g}}{\overline{m}}.`$

Relative to the base diagram including its symmetry factor $`S`$, the sum of all the contributions with $`k1`$ is

$`SF^{\mathrm{}}{\displaystyle \underset{k=1}{\overset{q}{}}}\left({\displaystyle \genfrac{}{}{0pt}{}{q}{k}}\right)2^k({\displaystyle \frac{\overline{g}}{\overline{m}}})^k\overline{A}^k,`$ (5)
which is simply

$`SF^{\mathrm{}}\left[(1+2{\displaystyle \frac{\overline{g}}{\overline{m}}}\overline{A})^q1\right].`$
Since $`q=2(3\mathrm{})`$,

$`(1+2{\displaystyle \frac{\overline{g}}{\overline{m}}}\overline{A})^q1=(1+4{\displaystyle \frac{\overline{g}}{\overline{m}^2}}\overline{G})^{(3\mathrm{})}1.`$
Thus the sum over contributions from diagrams with $`k1`$, with a given base diagram, is indeed a polynomial in $`\overline{G}`$, namely

$`SF^{\mathrm{}}{\displaystyle \underset{k=1}{\overset{3l}{}}}\left({\displaystyle \genfrac{}{}{0pt}{}{3l}{k}}\right)4^k({\displaystyle \frac{\overline{g}}{\overline{m}^2}})^k\overline{G}^k.`$ (6)
## 5 No further divergences from $`F`$ and $`F^2`$ vertices

To renormalize the theory, we must add the terms $`F`$ and $`F^2`$ by hand to the tree-level Lagrangian. We choose to parametrize these terms as

$`\lambda _1g^3\overline{m}^4det(C)F+\lambda _2g^2\overline{m}^2det(C)F^2`$ (7)
The advantage of this parametrization is that both $`\lambda _1,\lambda _2`$ are dimensionless and charge neutral under both $`U(1)_R`$ and $`U(1)_\mathrm{\Phi }`$.

It is easy to see that in this general situation, the symmetry argument given in section two still applies. For example, we only need to add $`\lambda _1^{w_1}\lambda _2^{w_2}`$ to equation (2), which does not affect the power counting. We still have following conclusions. (1) A log divergent term has at most one $`det(C)`$ insertion. This means a divergent diagram contains at most one of any of the three vertices $`F,F^2,F^3`$. (2) The only possible divergent operators, with one power of $`det(C)`$, are still

$`\overline{A}^{\overline{\alpha }_1}F^{\alpha _2},\mathrm{for}\overline{\alpha }_1+2\alpha _22\mathrm{},\mathrm{}=1,2,3`$ (8)
where the vertex $`F^{\mathrm{}}`$ is the one appearing in the diagram.

The crucial point is that with two new terms $`F,F^2`$ in the tree level Lagrangian, the insertion and deletion operations are not modified at all. The repackaging of all these divergent terms into $`\overline{G}`$ will go through unmodified. Thus we conclude that the renormalizability proved in the previous sections continues to hold with the terms $`F,F^2`$ in the tree level Lagrangian.

## Acknowledgements

We thank O. Lunin, S. J. Rey, and N. Seiberg for helpful discussions. This work was supported by the NSF grant PHY-0070928.

## Appendix: The two $`U(1)`$ (pseudo)symmetries

For the $`𝒩=\frac{1}{2}`$ Wess-Zumino model, we can identify two global $`U(1)`$ (pseudo)symmetries by treating all coupling parameters, including the nonanticommutativity parameter $`C^{\alpha \beta }`$, as the lowest components of (anti)chiral superfields. They are $`U(1)_\mathrm{\Phi }`$ flavor symmetry and $`U(1)_R`$ R-symmetry. Charge assignment is given as follows .

|  | dim | $`U(1)_R`$ | $`U(1)_\mathrm{\Phi }`$ |  | dim | $`U(1)_R`$ | $`U(1)_\mathrm{\Phi }`$ |
| --- | --- | --- | --- | --- | --- | --- | --- |
| $`\theta `$ | -1/2 | 1 | 0 | $`\overline{\theta }`$ | -1/2 | -1 | 0 |
| $`d\theta `$ | 1/2 | -1 | 0 | $`d\overline{\theta }`$ | 1/2 | 1 | 0 |
| $`A`$ | 1 | 1 | 1 | $`\overline{A}`$ | 1 | -1 | -1 |
| $`\psi `$ | 3/2 | 0 | 1 | $`\overline{\psi }`$ | 3/2 | 0 | -1 |
| $`F`$ | 2 | -1 | 1 | $`\overline{F}`$ | 2 | 1 | -1 |
| $`g`$ | 0 | -1 | -3 | $`\overline{g}`$ | 0 | 1 | 3 |
| $`m`$ | 1 | 0 | -2 | $`\overline{m}`$ | 1 | 0 | 2 |
| $`C^{\alpha \beta }`$ | -1 | 2 | 0 | $`|C|`$ | -2 | 4 | 0 |
| $`\mathrm{\Phi }`$ | 1 | 1 | 1 | $`\overline{\mathrm{\Phi }}`$ | 1 | -1 | -1 |


format: text

text:
# Ferromagnetic Ga1-xMnxN epilayers versus antiferromagnetic GaMn3N clusters

## Abstract

Mn-doped wurtzite GaN epilayers have been grown by nitrogen plasma-assisted molecular beam epitaxy. Correlated SIMS, structural and magnetic measurements show that the incorporation of Mn strongly depends on the conditions of the growth. Hysteresis loops which persist at high temperature do not appear to be correlated to the presence of Mn. Samples with up to 2$`\%`$ Mn are purely substitutional Ga1-xMnxN epilayers, and exhibit paramagnetic properties. At higher Mn contents, precipitates are formed which are identified as GaMn3N clusters by x-ray diffraction and absorption: this induces a decrease of the paramagnetic magnetisation. Samples co-doped with enough Mg exhibit a new feature: a ferromagnetic component is observed up to $`T_c175`$ K, which cannot be related to superparamagnetism of unresolved magnetic precipitates.

Since the discovery of giant magneto-resistance in ferromagnetic metal multilayers , spin-dependent phenomena rapidly appeared as a unique mean to merge information storage and processing, thus rising one of the powerful concepts of a spin-based electronics . Nevertheless, metal-semiconductor interfaces could hinder the injection of a spin-polarized current into a semiconductor , although an additional tunneling barrier is predicted to overcome this issue . Diluted magnetic semiconductors (DMS -see, e.g., -) showing room-temperature ferromagnetism appear as a serious alternative to ferromagnetic metals to ensure an efficient injection and, indeed, high critical temperatures $`T_c`$ were predicted in Mn-doped wide band-gap semiconductors . As a result, there is a growing interest in the search for DMS having both a high $`T_c`$ and a large spin polarization of the carriers, which could then be used as spin polarizers or filters and for spin injection into a nonmagnetic semiconductor (similarly to other DMS which were used at low temperature ). Room-temperature ferromagnetism was previoulsy reported in GaN:Mn thick films , with an extrapolated $`T_c940`$ K . However, these results remain ambiguous: a large additional paramagnetic component is also observed , and ferrimagnetic clusters, such as Mn4N precipitates with the perovskite structure, could be at the origin of a ferromagnetic-like behaviour .

In order to determine the specific features of the pure Ga1-xMnxN phase, we investigated in detail the structural and magnetic properties of GaN:Mn thick epilayers with the wurtzite structure. These were grown by nitrogen-plasma assisted molecular beam epitaxy (MBE) on a GaN buffer layer, previously elaborated by metal-organic chemical vapor deposition on a sapphire substrate. The manganese content was always checked by secondary ion mass spectrometry (SIMS), using an Mn-implanted GaN layer as a reference: depth profiles were homogeneous over the 0.3 micron layer thickness. As discussed below, no evidence of any secondary phase was found for Mn incorporations as large as 2$`\%`$, using extended x-ray absorption spectroscopy (EXAFS) as a local probe of the Mn environment, whereas we give direct evidences for the formation and the nature of antiferromagnetic precipitates with the perovskite structure above 2$`\%`$. Every sample exhibits paramagnetism at low temperature, as well as a smaller hysteretic artefact persisting at high temperature which is not specific to our epilayers. Moreover, the low-field susceptibility also reveals the coexistence of magnetic phases in diluted Ga1-xMnxN epilayers, if substantially co-doped with Mg, a widely used acceptor in GaN. This behaviour is not due to clusters of another phase, and it may suggest the occurence of hole-induced ferromagnetism, but still with a $`T_c`$ lower than 300 K.

We first focus onto the growth of Mn-doped GaN epilayers without any additional doping. The MBE-growth of GaN was previously studied in detail . It was shown that the growth front of GaN strongly depends on the Ga/N flux ratio. Under N-rich conditions, a rough N-terminated surface is formed, which is stable when growth is stopped. Under Ga-rich conditions, a wetting Ga film is formed, which can be evidenced by the dwell time of the reflection high-energy electron diffraction (RHEED) transient signal during the growth interruption: a thorough calibration shows that this dwell time is a measure of the Ga-film desorption . At low Ga excess, the Ga surface coverage increases with the Ga flux. At intermediate Ga flux, a plateau is observed (fig. 1a), which corresponds to the formation of a self-regulated bilayer of Ga at the growth front. This smooth surface stabilizes a 2D growth of GaN within a finite growth window so that, the growth is fairly insensitive to fluctuations of the Ga flux and of the substrate temperature. The addition of a Mn flux reduces both the width of this plateau (fig. 1a), and the growth rate under N-rich conditions (fig. 1b): both effects point to a reduction of the Ga sticking coefficient, which tends to limit the self-regulated 2D growth of Mn-doped GaN epilayers. Finally, at even larger Ga flux, Ga droplets are formed, as evidenced by the increase of the Ga desorption time (fig. 1a). It is important to have a precise knowledge of this diagram (fig. 1a), since the Mn incorporation, for a given Mn flux, strongly depends on the growth regime . A significant amount of manganese, up to 18$`\%`$, was incorporated under N-rich conditions, close to stoichiometry, whereas the incorporation of Mn was reduced under Ga-rich conditions within the self-regulated growth window: for a given, small-enough, Mn flux, the Mn content is found to be ten times smaller under Ga-rich conditions as compared to the N-rich case. This behaviour may come from a decrease of the Mn sticking coefficient when the Ga surface coverage is increased or it may mean that the Ga bilayer acts as a diffusion barrier hindering the incorporation into GaN.

The epilayers structure was studied using a SEIFERD 3003 PTS-HR x-ray diffractometer. The measurements do not show any spurious phase for a Mn content smaller than 2$`\%`$, whereas the formation of additional clusters with the perovskite structure is evidenced at larger doping levels (see fig. 2). These could be either GaMn3N or Mn4N clusters: as these two phases have nearly the same lattice parameter , one can hardly distinguish between them by x-ray diffraction. These precipitates show two crystalline orientations, and most have their  direction (three-fold axis) colinear to the wurtzite $`c`$-axis. Note that, using a vicinal silicon surface ($`4^{}`$ off) as a sample holder to achieve a low background, the large dynamical range allows us to evidence the presence of these oriented clusters for a Mn-content down to about 2$`\%`$ of Mn, instead of 6$`\%`$ in . Although a small amount of tiny clusters cannot be excluded (less than a few percents, because of the measurement accuracy given by our small but finite background), the higher sensitivity of x-ray absorption measurements also allows us to demonstrate the absence of such precipitates below about 2$`\%`$ of Mn.

We performed EXAFS measurements at the Mn K-edge on both our GaN:Mn epilayers and two perovskite powders, at the European Synchrotron Radiation Facility. This analysis was intended, first to completely discard the occurence of any other phase but the purely diluted Ga1-xMnxN one at low-enough Mn contents and, second, to clearly identify the precipitates present at larger Mn incorporations. Indeed, the local environment is much different for a Mn either in GaMn3N or Mn4N clusters, both with the perovskite structure, and for a Mn substituting a Ga in wurtzite GaN: there are 2N as nearest-neighbours in the perovskite instead of 4N in the wurtzite, and the bond lengths are shorter. Moreover, the second neighbours allow one to distinguish GaMn3N (8Mn+4Ga) from Mn4N (12Mn). Two contrasted behaviours in EXAFS oscillations are observed in fig. 3a, at low or high Mn contents, whereas intermediate Mn contents above 2$`\%`$ exhibit a gradual change from one case to the other (not shown). The Fourier transforms of these weighted oscillations (fig. 3b) give distances to the central Mn ion that are in agreement with either the wurtzite or the perovskite structures, respectively.

For a 1.5$`\%`$ Mn-doped GaN epilayer, the measurement can be fitted to a calculation based on a Mn random substitution of Ga in wurtzite GaN, including the first seven shells, which shows that the pure Ga1-xMnxN phase is obtained. The two additional peaks evidenced at large $`R`$ values in fig. 3b can also be reproduced if the first thirteen shells are taken into account in the calculation, but without considering multiple scattering paths. However, these neglected paths contribute to the exact shape of the peaks, so that we only considered the first seven shells for the accurate fit shown in fig. 3b. On the contrary, for a 18$`\%`$ Mn-doped GaN epilayer, EXAFS oscillations are strongly modified and now clearly fit the experimental oscillations of a GaMn3N powder (note that these oscillations are perfectly in phase, up to large $`k`$ values). This demonstrates that most of the manganese ions contribute to this perovskite phase in the high-doping range. Moreover, it is clear from the experimental data (shift and amplitude, see fig. 3a -up-) that the EXAFS oscillations of this 18$`\%`$ Mn-doped GaN epilayer do not fit the ones obtained with a Mn4N powder. This result is also corroborated by x-ray absorption near edge structure (XANES) measurements, showing identical edges for both our highest Mn-doped GaN epilayer and the GaMn3N powder, whereas a shift of about 2 eV is revealed for the Mn4N one (not shown). All these features allow us to clearly identify the perovskite precipitates as due to GaMn3N clusters and not to Mn4N ones. This is particularly important since GaMn3N is antiferromagnetic while Mn4N is ferrimagnetic .

Magnetisation measurements were performed using a MPMS-Quantum Design SQUID magnetometer, with an improved accuracy achieved using the reciprocating sample technique, the magnetic field being applied within the layer plane. We paid much attention to accurately subtract the large diamagnetic contribution of the substrate. This is particularly difficult at low temperature for the small paramagnetic signals measured. Therefore, we mainly ruled out any significant non linear contribution from the substrate and used the saturated magnetisation, as observed in high fields below $`T5`$ K, to subtract the diamagnetic component.

As above, we first concentrate on the two extreme cases involving either a low Mn content (that is, below or around 2$`\%`$), for which only the pure diluted Ga1-xMnxN phase is obtained, or the highest Mn incorporation showing a large amount of GaMn3N precipitates. Fig. 4a shows the magnetic behaviour of a Ga1-xMnxN epilayer grown under Ga-rich conditions with $`x0.3\%`$, that is, being far away from the smaller concentration at which additional precipitates were evidenced. Similarly to any other sample, a temperature-dependent paramagnetic contribution, being clearly observed at low temperature and in high fields, is superimposed to a nearly temperature-independent hysteretic component (see fig. 4b). The saturated magnetisation at 4 K, of about 5 emu/cm3, gives the right order of magnitude for a Mn localized magnetic moment, that is close to 5 $`\mu _B`$, but does not allow to conclude quantitatively about the valence state. Contrary to the low Mn content case, the magnetic moment per Mn is found to be strongly reduced in a GaN:Mn epilayer containing a much larger amount of manganese ions ($`18\%`$), giving less than 0.5 $`\mu _B`$/Mn at low temperature (solid line in fig. 4a). Reduced paramagnetism shows that most of the manganese ions ($`90\%`$) now incorporate into GaMn3N precipitates, thus corroborating EXAFS measurements, and it demonstrates that these clusters are large enough to have a bulk-like antiferromagnetic behaviour .

More complicated results are expected at intermediate manganese compositions, when GaMn3N precipitates are small enough to also contribute to the whole magnetisation, due to deviations from long-range antiferromagnetic ordering. This could lead to an optimum in the magnetisation , with some low-temperature hysteresis related to the coexistence of both Ga1-xMnxN and very small GaMn3N precipitates with a finite magnetisation. For instance, the early formation of such small precipitates, which cannot be resolved by x-ray analysis, is evidenced below about 10 K by a slow magnetic relaxation component in a $`1.7\%`$ Mn-doped GaN epilayer and at higher intermediate Mn contents. Nevertheless, this contribution of the freezing of small superparamagnetic clusters remains rather small compared to any other component, and it is absent for $`x<1.7\%`$, within the magnetisation measurement accuracy (in this case less than $`0.1\%`$ of Mn ions incorporate into GaMn3N clusters).

The high-temperature hysteresis loop shown in fig. 4b, which behaves as an in-plane ferromagnetic contribution, was not found to be specific to Mn-doped GaN epilayers. Indeed, a systematic investigation of the saturated magnetisation at room temperature over a broad Mn-incorporation range does not give any significant dependence with the Mn content. This high-temperature hysteretic artefact was carefully checked not to be due to the apparatus nor to the sample holder, but to the measured sample itself. Therefore, in most cases, the low-field susceptibility consists of a 1/$`T`$ variation with temperature, adding to an offset which is reminiscent of the artefact.

However, the susceptibility of samples co-doped with Mn and Mg reveals an important new feature: a clear anomaly is observed near 175 K at large enough Mg contents, as shown in fig. 4c. This anomaly remains very similar for Mn contents much higher than 2.8$`\%`$ (that is, when a large amount of GaMn3N clusters is formed), as if the Mn incorporation in the diluted phase saturates (not shown). Note that the ferromagnetic component is observed up to $`T_c175`$ K. Such a value of $`T_c`$ is large enough not to be due to unresolved magnetic precipitates, mainly because large blocking temperatures are ruled out in tiny clusters with a small anisotropy. All large manganese nitride clusters are either antiferromagnets or highly compensated ferrimagnets, which could explain the small amplitude of the magnetisation measured in our experiments. Nevertheless, the small change in the susceptibility anomaly at large Mn incorporations suggests that large clusters with the perovskite structure do not contribute significantly to the magnetisation. In addition, the associated Néel temperatures are much different than the observed values of $`T_c`$. The low-field magnetisation remains rather small at low temperature, as compared to a metallic Ga1-xMnxAs epilayer, and most of Mn impurities still remain in the paramagnetic state, which points to the occurence of inhomogeneous magnetic properties. Finally, the anomaly in the susceptibility is also independent of the artefact hysteresis loop and, as a Mg impurity usually acts as an acceptor in GaN, it suggests the possible occurence of hole-mediated ferromagnetism.

To sum up, this study shows that diluted Ga1-xMnxN epilayers which do not contain any secondary phase, exhibit a ferromagnetic behaviour below room temperature, when introducing a significant amount of additional non-magnetic impurities, which usually act as acceptors in GaN. Further investigations of the exact role of the Mn and Mg doping levels are still required to control both the ordering temperature and to make ferromagnetism more homogeneous. In Ga1-xMnxAs, the coexistence of magnetic phases is usually attributed to a random distribution of localized Mn-impurities exchange-coupled to each other by a spatially-inhomogeneous carrier density, which can be expected in a system close to its Mott transition. Yet, an inhomogeneous distribution of Mn ions cannot be excluded. Note, however, that large band-gap ferromagnetic semiconductors are quite different from previously studied materials, since the $`3d`$-band as well as the Fermi energy are expected to lie within the gap , and not within the valence band. Therefore, a better understanding of the carrier and Mn ion spatial distributions is necessary to highlight the origin of ferromagnetism in wide band-gap DMS. Finally, the conductivity of GaN:Mn layers is often found to be of $`n`$-type, instead of $`p`$-type as usually required, and previous claims for room-temperature ferromagnetism in such samples must be considered with caution, because of uncontrolled but reproductive hysteretic artefacts when small magnetisations of thin films are measured.

Acknowledgements

We thank Y. Genuist for his technical assistance, P. Hollinger, O. Kaitasov and the PROBION company for the SIMS measurements, and O. Proux and J.-L. Hazemann for their support at the ESRF. J.-F. Jacquot is acknowledged for his support with SQUID measurements. SK thanks the Japanese Overseas Research Fellow sponsored by Monbukagakush . This work was supported by the EC FENIKS project G5RD-CT-2001-00535.

LIST OF FIGURES CAPTIONS

* Growth of Mn-doped GaN epilayers. (a), Ga flux dependence of the Ga desorption time, after the growth of GaN (filled squares) and Mn-doped GaN for two values (open triangles and circles) of the Mn-beam equivalent pressure (BEP), the N2 flow and the substrate temperature being kept constant (surface stoichiometry is achieved close to 0.27 ML/s). (b), Specular RHEED intensity obtained during the growth of both GaN and Ga1-xMnxN (with $`x1.7\%`$), under N-rich conditions with a Ga flux of 0.23 ML/s. The indicated growth rate is deduced from the RHEED oscillations.
* (a), X-ray $`\theta `$–2$`\theta `$ diffraction patterns of GaN:Mn epilayers. For a 18$`\%`$ Mn-doped GaN epilayer, the presence of oriented clusters with the perovskite structure is revealed. An additional AlN buffer layer was also grown for transport measurements. (b), Observation of perovskite clusters at Mn contents larger than about 2$`\%`$, which are shown to be GaMn3N precipitates by x-ray absorption.
* Mn local environment in GaN:Mn epilayers. (a), EXAFS oscillations as measured in the two extreme cases, that is, for a Mn content either below 2$`\%`$ or as large as 18$`\%`$. The latter case is compared with EXAFS oscillations obtained in GaMn3N and Mn4N powders, with the perovskite structure. (b), Fourier transforms of the weighted EXAFS oscillations shown in (a), within the $`k`$-range \[4.25, 11.7\] Å-1. Using the FEFITT routine package, the calculation based on wurtzite GaN, with a central Ga atom substituted by a Mn atom, takes every interferences paths into account. Including the first seven shells, an accurate fit is obtained, without any additional contribution but a slight change of about 2$`\%`$ in the Mn-N bound length to the first 4N neighbours (see also ).
* (a), Paramagnetic behaviour in Ga1-xMnxN with $`x0.3\%`$. A limited magnetisation is observed at $`T=5`$ K in our 18$`\%`$ Mn-doped sample (see solid line). (b), A nearly temperature-independent hysteretic artefact is superimposed at low fields to the paramagnetic component. (c), Temperature dependence of the field-cooled magnetisation ($`H=100`$ Oe) in samples co-doped with Mg impurities. For a large enough Mg content, an anomaly is evidenced near 175 K.


text:
# The resistible effects of Coulomb interaction on nucleus-vapor phase coexistence

## Abstract

We explore the effects of Coulomb interaction upon the nuclear liquid vapor phase transition. Because large nuclei ($`A>60`$) are metastable objects, phases, phase coexistence, and phase transitions cannot be defined with any generality and the analogy to liquid vapor is ill-posed for these heavy systems. However, it is possible to account for the Coulomb interaction in the decay rates and obtain the coexistence phase diagram for the corresponding uncharged system.

preprint: LBNL-53344

Since the birth of the liquid drop model, which occurred more than 60 years ago, nuclei have been recognized as charged drops of a van der Waals like fluid. Soon after, the concept of cold uncharged, symmetric nuclear matter was introduced. The characterization of its properties, such as its phase diagram and equation of state has been and remains still perhaps the most eminent goal of nuclear physics.

The experimental characterization of cold nuclear matter began by setting the surface, symmetry, and Coulomb terms of the liquid drop expression to zero and retaining just the volume term. This, together with the independent measurement of nuclear radii (already inferable from the surface and Coulomb coefficients), defined the fundamental properties of cold symmetric nuclear matter, namely its binding energy and density at saturation.

Thus, the Coulomb interaction was reasonably eliminated from the picture in order to dispose of what was perceived as a troublesome inessential divergence, while, for better or worse, it remains all pervasive in the experimental realm.

The experimental extension to higher temperatures was hampered both by the lack of a suitable container which became necessary to accommodate the vapor phase (shown to exist by the the soon discovered neutron and proton evaporation) and by the not obviously generalizable finite size effects.

In this paper we consider the problem of the Coulomb interaction and the problem of the container, and we present a simple and natural solution to both. This solution also gives a good indication of how to deal with finite size with maximum generality.

The nuclear liquid vapor phase transition, or more properly, the liquid vapor coexistence is being discussed intensely in literature Elliott et al. (2002, 2003); Berkenbusch et al. (2002); Natowitz et al. (2002); Gulminelli and Chomaz (1999); Moretto et al. (2002a); Pochodzalla et al. (1995); D’Agostino et al. (2000). Theoretically, a great deal of attention has been given to the effects of the nuclear finite size Moretto et al. (2002b). Experimentally, discovery and characterization has been claimed from various quarters Elliott et al. (2002, 2003); Moretto et al. (2002a); Berkenbusch et al. (2002); Natowitz et al. (2002); D’Agostino et al. (2000); Pochodzalla et al. (1995), although doubts remain regarding the validity of some approaches and the consistency of the results.

Many of the theoretical approaches have been based upon numerical simulations of finite lattice systems. From these studies negative heat capacities have been claimed to be the signal of the phase transitions in nuclei and other finite systems D’Agostino et al. (2000). From our part we found it more productive to use a simple extension of thermodynamics which incorporates the finiteness of the nuclear system through the surface and other liquid drop terms Moretto et al. (2002b).

We showed that a negative heat capacity can be trivially expected in terms of the change of the droplet (nuclear) binding energy with the decreasing size of the evaporating droplet (nucleus). This can be seen most clearly in the case of an isobaric transition:

$$dp=\frac{p}{A}|_TdA+\frac{p}{T}|_AdT=0$$
(1)
or

$$\frac{T}{A}|_p=\frac{\frac{p}{A}|_T}{\frac{p}{T}|_A}.$$
(2)
Since from the Clapeyron equation

$$\frac{p}{A}|_T\frac{p}{T}\frac{\mathrm{\Delta }H_m}{A}|_T$$
(3)
and

$$\frac{p}{T}|_Ap\frac{\mathrm{\Delta }H_m}{T^2}$$
(4)
we can obtain the desired result for the isobaric dependence of the transition temperature on the size of the system

$$\frac{T}{A}|_p=\frac{T}{\mathrm{\Delta }H_m}\frac{\mathrm{\Delta }H_m}{A}|_T$$
(5)
or

$$\frac{T}{A}|_p=T\frac{\mathrm{log}\mathrm{\Delta }H_m}{A}|_T.$$
(6)
In all the above, $`A`$ is the size of the system, $`\mathrm{\Delta }H_m`$ is the molar enthalpy of vaporization ($`\mathrm{\Delta }H_mB(A)+T`$), and $`B(A)`$ is the binding energy per particle of a cluster of size $`A`$.

In a droplet of a van der Waals liquid, $`\mathrm{\Delta }H_m`$ increases with increasing size $`A`$ and saturates for the infinite systems. This is of course due to the droplet molar surface energy which decreases and asymptotically vanishes with increasing droplet size. Thus Eq. (6) says that, at fixed pressure $`p`$ the coexistence temperature decreases as the droplet (nucleus) evaporates. This implies a sloping downwards of the caloric curve in the transition region and a negative heat capacity in the same region. An example of the droplet size dependent heat capacity is given in Fig. 1 as the slope in the temperature-enthalpy correlation at constant pressure for different drop sizes.

However, as we pointed out elsewhere Moretto et al. (2002b), in nuclei surface effects are not the only ones to be considered. Coulomb effects become progressively more important with increasing $`A,Z`$ and eventually, at about $`A`$=60 they reverse the surface trend prevailing at small $`A`$ values. Above $`A`$ 60 where the binding is at a maximum the binding and thus $`\mathrm{\Delta }H_m`$ progressively decreases with increasing $`A`$. The inescapable conclusion is that, within the scope of the Clapeyron equation, no negative heat capacities should be observed for $`A>60`$, in contradiction with claims to the contrary D’Agostino et al. (2000).

The above result is predicated upon the dominant emission of monomers (neutrons, protons), or, at any rate, very small clusters. Should the nucleus statistically breakup into large fragments, the $`A`$ 60 upper limit for the observation of negative heat capacities would be correspondingly displaced upwards. However, not only are large fragments rare at low temperature but they never dominate at any temperature (below the critical temperature). In Ising models, finite or not, the average cluster size in the “gas phase” hardly rises above unity. The same holds true in experimental data Elliott et al. (2002, 2003). It truly seems impossible to escape these thermodynamic conclusions.

However, one may question whether the role of the Coulomb interaction is merely that of decreasing the binding energy. The long range nature of this force may compel us to analyze its role in more detail in first order phase transitions. As will be shown below, the problems are quite serious and threaten our ability to define a true first order phase transition with any generality in the presence of such a force.

Let us begin with a premise. In typical first order phase “coexistence”, the two phases (liquid and vapor) do not have to be in actual physical contact. The contact surface is irrelevant as is the short range interaction between the two phases. In other words the equilibrium regime depends exclusively on the properties of each of the two phases, as if the other were not there. Equilibrium exists when the chemical potentials of the two phases are equal, be they in contact or not.

Let us now introduce the Coulomb interaction in the problem of a drop and its vapor.

The Coulomb interaction can be split into three parts: 1) the drop self energy; 2) the drop-vapor interaction energy; and 3) the vapor self energy.

The drop self energy, for a finite bound or metastable drop, is easily calculated and does not constitute a problem.

For the drop-vapor interaction, we consider a probe cluster which we can carry from the interior of the drop to infinity. The potential energy experienced in the process depends upon the particle’s charge/mass and is shown schematically in Fig. 2.

If the particle has zero charge (top panel), a step is observed at the droplet radius equal to the particle binding energy. For charges greater than zero, a maximum $`B_c`$ is observed at the approximate distance of the two droplets in contact. From there the potential decreases according to the Coulomb law and settles down at infinity to a value equal to the binding energy of the particle, $`Q`$.

In this case, where we assume that any particle of any size is bound ($`Q<0`$) and we forget about problem 3), there is no difficulty in defining a gas phase in equilibrium with the droplet at infinity constituted by particles of all sizes whose abundance is controlled by the respective binding energies in the standard way. The intervening Coulomb barrier $`B_c`$ does not alter the equilibrium, although it may slow its achievement. In this case the vapor is constituted mainly of monomers and the coexistence pressure described by the Clapeyron equation

$$\frac{dp}{dT}=\frac{\mathrm{\Delta }H_m}{T\mathrm{\Delta }V_m}$$
(7)
with the molar enthalpy $`\mathrm{\Delta }H_m`$ suitably accounting for both surface and Coulomb terms, is completely adequate to describe the liquid to vapor transition and coexistence ($`\mathrm{\Delta }V_m`$ is the molar volume).

Let us now consider the case in which the probe particle becomes unbound to the droplet above some $`Z`$ value, due to the Coulomb interaction. Now the situation becomes as depicted in Fig. 3. In this case the droplet is not stable and the ground state of the system may consist of two or more pieces of the original drop at infinity. This is naturally true already at $`T=0`$. Thus it is not possible to speak properly of this drop in statistical equilibrium with its vapor, since the drop itself is metastable. For a nucleus like gold, the ground state is at least as complicated as three fragments of approximately size 60 nucleons at infinity. This “true” ground state is hundreds of MeV below the mass of the gold nucleus. In any statistical calculation, at any reasonable temperature, one can expect a liquid-like phase consisting of a configuration similar to the true ground state in equilibrium with some vapor. A metastable gold-like drop is an immensely improbable configuration because of the great energy chasm mentioned above. The probability of such a configuration can be surmised from the Boltzmann factor $`P=\mathrm{exp}(\mathrm{\Delta }E/T)`$ where $`\mathrm{\Delta }E`$ is the energy difference between the metastable state and the ground state. Estimating $`\mathrm{\Delta }E`$ 135 MeV and a temperature of 4 MeV we obtain $`Pe^{34}`$ or approximately $`2\times 10^{15}`$.

One might argue that our point is made from energetic rather than free energy considerations and that it may in fact be incorrect. After all, equilibria work both ways, and typically one of the phases is at a lower energy than the other.

Let us consider, then, the transition from a condensed phase (liquid-like) to a dilute phase (vapor-like). For an infinitesimal isothermal transfer, the variation of the free energy must be zero

$$\mathrm{\Delta }F=\mathrm{\Delta }ET\mathrm{\Delta }S=0.$$
(8)
As we go from liquid to vapor, $`\mathrm{\Delta }E>0`$ for a typical fluid, but this energy increase is compensated by an equivalent increase in entropy, due just to the increase in molar volume.

However, if $`\mathrm{\Delta }E`$ is negative, due to the Coulomb effect, we need a decrease in entropy which is hardly compatible with expansion.

The conclusion is that a statistical equilibrium first order phase coexistence and phase transition is not definable for any droplet that has unbound channels. Of course, the transition of the metastable droplet to its “true” complex ground state does not qualify as a statistical phase transition.

This Coulomb effect seems truly devastating since it does not allow one to define nuclear phase transitions much above $`A60`$.

However there may be a solution to this difficulty. If we consider the emission of particles with a sizable charge, we notice that a large Coulomb barrier $`B_c`$ is present. For $`T<<B_c`$ these channels may be considered effectively closed. Consequently the unbound channels may not play a role on a suitably short time scale. Then a phase transition may still be definable in an approximate way. But, of course, we reach again the previous conclusion that for $`A>60`$ heat capacities must be positive and therefore claims of negative heat capacities for large nuclei D’Agostino et al. (2000); Gulminelli and Chomaz (2003) find here a most serious objection.

Let us consider now part 3) of the Coulomb energy, namely the vapor self energy. As we said above, it diverges for an infinite amount of vapor. For a dilute vapor, we could consider a small portion such that the intrinsic self energy/nucleon is much less than the temperature $`T`$. Alternatively, we could consider a finite box containing a finite system. Unfortunately, at any other distance smaller than infinity the result depends annoyingly on the size (and shape!) of the container and on whether the drop is confined or not in a specified location of the container; a rather inelegant and non-general situation leading to confusing questions about true equilibrium. In any case, it is clear that overall, the Coulomb term makes the definition of phase coexistence and phase transition intractable and ill-posed.

A solution to these difficulties can be arrived at only by asking a slightly different question: is there a way to obtain experimentally the signal and characterization of the phase diagram (transition) of a nucleus as if the Coulomb interaction were not there?

As mentioned above, any attempt to define and characterize both phases in the presence of the Coulomb interaction depends (at the very least) on the shape and size of a confining volume applied from without. This seems artificial and lacks a desirable generality. But nature actually provides this “confining volume” for us. Any particle trying to leave the nucleus is “boxed in” by a barrier ($`B_s`$) which depends on the particle under consideration and on the residual nucleus (or the “complement”). The top of this potential barrier is close in shape to the potential of two objects, particle and complement, in near contact. The tops of these barriers are actually conditional saddle points Moretto (1975), conditional in the sense that the mass asymmetry is considered frozen.

According to standard transition state theory all these saddles are in statistical equilibrium with the droplet and the decay rates give direct information on their population which is naturally controlled by a Boltzmann factor $`\mathrm{exp}(B_s/T)`$. In particular for large enough $`B_s`$ the observed experimental abundances are directly related to first chance emission and thus to the transition state rate.

Now $`B_s`$ is composed by

$$B_s=E_{\mathrm{surface}}^sE_{\mathrm{surface}}^{gs}+E_{\mathrm{Coul}}^sE_{\mathrm{Coul}}^{gs}.$$
(9)
where $`E_{\mathrm{surface}}^s`$ and $`E_{\mathrm{surface}}^{gs}`$ are the surface energies of the saddle and ground state respectively, and $`E_{\mathrm{Coul}}^s`$ and $`E_{\mathrm{Coul}}^{gs}`$ are the Coulomb energies for the same two configurations. Since the Coulomb energies can be easily estimated assuming a two touching spheres configuration for the saddle and one sphere configuration for the droplet (see Fig. 4), we can correct the rates by dividing away the Boltzmann factor containing the Coulomb terms and be left with only the rates/abundances pertaining to the decay of an uncharged drop, for which all channels are bound by the extra surface energy $`Q_{\mathrm{surface}}=E_{\mathrm{surface}}^sE_{\mathrm{surface}}^{gs}`$ (see Fig. 5). These rates are now independent of distance and are proportional to the effective partial concentration of the hypothetical gas in equilibrium. We speak of a virtual gas phase because it is not and it need not be present. This picture of a free evaporation of a droplet in vacuum neatly bypasses also the need for a physical presence of the vapor. The resulting situation is very much that described by the Fisher droplet model Fisher (1969) for the composition of a saturated vapor in equilibrium with a liquid droplet. The Fisher droplet model can be directly co-opted to describe the (first chance) fragment abundances of a nuclear physics experiment after correction for Coulomb effects. From it, it is easy to obtain the coexistence diagram for any nuclear system deprived of the Coulomb interaction Elliott et al. (2002, 2003). This is in the same spirit as in nuclear matter calculations in which neutrons and protons are considered as distinct particles, but without any Coulomb interaction.

In summary, we have illustrated the difficulties brought about by the Coulomb interaction in the problem of the nuclear heat capacities. We have shown that for systems with bound decay channels, negative specific heats, if definable at all, are allowed only for $`A`$ 60. For unbound channels, namely nuclei metastable to breakup into two or more large fragments, no phase description or phase coexistence with the normal thermodynamic generality is possible. However, we have shown that decay transition rates can be corrected for the Coulomb interaction in a natural way and the phase diagram for the corresponding chargeless system can be easily obtained.


text:
# Low-energy quasiparticle excitations in dirty d-wave superconductors and the Bogoliubov-de Gennes kicked rotator

## Abstract

We investigate the quasiparticle density of states in disordered d-wave superconductors. By constructing a quantum map describing the quasiparticle dynamics in such a medium, we explore deviations of the density of states from its universal form ($`E`$), and show that additional low-energy quasiparticle states exist provided (i) the range of the impurity potential is much larger than the Fermi wavelength \[allowing to use recently developed semiclassical methods\]; (ii) classical trajectories exist along which the pair-potential changes sign; and (iii) the diffractive scattering length is longer than the superconducting coherence length. In the classically chaotic regime, universal random matrix theory behavior is restored by quantum dynamical diffraction which shifts the low energy states away from zero energy, and the quasiparticle density of states exhibits a linear pseudogap below an energy threshold $`E^{}\mathrm{\Delta }_0`$.

In recent years, considerable attention has been focused on the low-energy properties of the quasiparticle spectrum of disordered cuprate superconductors Hirsch02 ; Altland02 . Because many of the cuprate superconductors are randomly chemically doped insulators and disorder is a pair-breaker for d-wave superconductors, the role of nonmagnetic impurities is particularly important for an understanding of the d-wave superconducting state, its quasiparticle spectral and transport properties. Of special interest is the low-energy behavior of the single-particle Density of States (DoS) $`\rho (E)`$.

In early work REF:nerseyan , the self consistent $`T`$-matrix approximation was shown to break down for 2-dimensional d-wave superconductors. This led to a series of papers using nonperturbative methods, which predicted (at first sight) contradictory results: vanishing REF:nerseyan ; REF:Senthil ; REF:Bocquet ; REF:Altland , constant REF:Ziegler98 ; REF:Huckenstein , and diverging REF:Pepin ; Ada02  DoS as $`E0`$. On the numerical side, several investigations also predicted both vanishing Ghos00 ; Atkinson01 , and diverging REF:detofdisord ; REF:zhu  DoS at zero energy. It was soon argued, based on numerical analysis, that the reason behind these contradicting predictions is the fact that the microscopic details of disorder (i.e. details beyond the transport mean free path $`\mathrm{}`$, such as the density of scatterers or the correlation length $`\zeta `$ of the impurity potential) as well as the symmetries of the clean Hamiltonian matter both qualitatively and quantitatively REF:detofdisord ; REF:Yashenkin01  (see also Chamon01 ). An important feature shared by the numerics of Refs. Ghos00 ; Atkinson01 ; REF:detofdisord ; REF:zhu ; REF:Yashenkin01  is that the disorder is introduced via isolated point-like scatterers. Long-wavelength disorder, which may arise due to chemical doping away from $`\mathrm{CuO}_2`$ planes, or can be induced via ion radiation techniques REF:ionrad  or via a STM tip REF:Yazdani , is thus ignored. Effects of long-wavelength disorder are expected to become dominant when the $`\mathrm{CuO}_2`$ planes have almost no atomic disorder REF:clean ; they are the main focus of this paper.

It has recently been realized, in the context of mesoscopic physics and weak localization, that $`\zeta `$ and $`\mathrm{}`$, together with the Fermi wavelength $`\lambda _F`$, define two classes of complex quantum systems: quantum disordered systems where $`\lambda _F\mathrm{}/\zeta ^2>1`$ and quantum chaotic systems for which $`\lambda _F\mathrm{}/\zeta ^2<1`$ Alarkin . The latter class is characterized by the emergence of a new diffractive scattering time scale, $`\tau _E=\nu ^1\mathrm{ln}[\zeta /\lambda _F]`$, defined as the time it takes for the classically chaotic dynamics (with Lyapunov exponent $`\nu `$) to stretch a wavepacket of minimal initial extension $`\lambda _F`$ to a length $`\zeta `$. In contrast to quantum disordered systems, quantum chaotic systems exhibit nonuniversal properties due to their short-time classical (i.e. deterministic) dynamics. In particular, significant deviations from Random Matrix Theory (RMT) emerge, as was recently found by Adagideli et al. Ada02  in the context of impurities in d-wave superconductors. These authors used a semiclassical approach to calculate the low energy DoS for a collection of extended scatterers (a quantum chaotic system) and found an asymptotic behavior $`\rho (E)1/E|\mathrm{ln}E^2|^3`$ as $`E0`$. They nevertheless argued that the RMT predictions of a linear pseudogap would be restored at lower energy $`E<E^{}`$, i.e. that the singularity in the DoS would be cut off at an energy $`E^{}`$ related to $`\tau _E`$, by diffractive (nonclassical) scattering occurring at larger times $`\tau >\tau _E`$. The purpose of the present paper is to investigate the modifications that the DoS undergoes as the correlation length of the impurity potential increases and $`\tau _E`$ becomes relevant. We will focus our attention on (i) providing for numerical checks of the theory of Adagideli et al. in the case of long-wavelength disorder Ada02 ; (ii) finding out whether for some $`E^{}`$ the DoS is suppressed for $`E<E^{}`$, in agreement with RMT predictions REF:Senthil ; REF:Bocquet ; REF:Altland , (this could also reconcile the above mentioned contradictory predictions); and (iii) investigate the transition region between extended and pointlike disorder.

We start by introducing a quantum map model for quasiparticle states in disordered d-wave superconductors. The main motivation behind this model is to investigate discrepancies (in low-energy DoS) between point-like vs. extended disorder as well as the transition region, i.e. the regime in which the impurity size is intermediate. To the best of our knowledge no disorder model which includes extended impurities as well as pointlike in d-wave superconductors has been studied numerically so far. This map has two additional advantages: First, as both the density and correlation length of impurities can be tuned independently, it is possible to interpolate between the two extreme regimes of strong disorder: unitary disorder (i.e. disorder due to dilute, pointlike scatterers REF:Pepin ; Chamon01 ; REF:Yashenkin01 ; REF:Altland , viz. quantum disorder) and quasiclassical disorder Ada02  (i.e. disorder due to extended scatterers, viz. quantum chaotic). Second, from a numerical point of view, it allows for the investigation of very large system sizes, i.e. lattice sizes of up to $`256\times 256`$, which are necessary for both variations of the disorder correlation length and the numerical extraction of the parametric behavior of the DoS. Our reasons why a dynamical model is relevant are: (i) In absence of superconductivity, many properties of quasiparticles in disordered media (such as Anderson localization) are correctly described by 1-D maps Fish82 . In fact it has been shown by Altland and Zirnbauer that one of those maps, the 1-D kicked rotator, and quasi-one-dimensional metallic wires are described by the same effective field theory Alt96 . Recent numerical investigations in $`D=2`$ suggest that this is also true in higher dimensions Ossi02 . (ii) In presence of superconductivity, Andreev maps based on the kicked rotator have recently been shown to adequately describe quantum dots in contact with a superconductor Jac03 .

We first briefly discuss generic properties of quantum maps for uncoupled quasiparticles. The dynamics corresponds to a succession of free propagations, interrupted by sudden kicks of period $`\tau _0`$, i.e. instantaneous perturbations. Quantum maps are conveniently represented by a unitary, Floquet operator $`F`$, giving the time-evolution after $`p`$ kicks as $`u(p)=F^pu(0)`$, for an initial wavefunction $`u(0)`$. The matrix $`F`$ has eigenvalues $`\mathrm{exp}(i\epsilon _m)`$, which define quasi-energies $`\epsilon _m(\pi ,\pi )`$ (energies and quasi-energies are expressed in units of $`\mathrm{}/\tau _0`$). While the energy is not conserved, the periodicity of the kick still preserves quasi-energies, much in the same way as a periodic potential breaks translational symmetry, but still preserves quasi-momentum. Time evolution of hole excitations (being the time-reversed of electronic excitations) is given by $`v(p)=(F^{})^pv(0)`$. Specializing to the $`D`$-dimensional kicked rotator, we write the Floquet operator as Izr90

$`F`$ $`=`$ $`\mathrm{exp}\left(i{\displaystyle \frac{KI}{\mathrm{}\tau _0}}\mathrm{\Pi }_{j=1}^D\mathrm{cos}r_j\right)\mathrm{exp}\left(i{\displaystyle \frac{\mathrm{}\tau _0}{2I}}\stackrel{}{}^2\right).`$ (1)
It describes the free motion of a particle with dimensionless coordinates $`\{r_j\}`$ (e.g. expressed in units of a lattice constant), which is interrupted at periodic time intervals $`\tau _0`$ by a kick of strength $`K\mathrm{\Pi }_{j=1}^D\mathrm{cos}r_j`$. $`I`$ is the moment of inertia of the particle, and $`K`$ is the kicking strength. For $`D=1`$ and 2, increasing $`K`$ makes the classical dynamics evolve from integrable ($`K=0`$) to fully chaotic \[$`K7`$, with Lyapunov exponent $`\lambda \mathrm{ln}(K/2)`$\]. For $`0<K<7`$ stable and unstable motion coexist (a so-called mixed phase space) Izr90 . Increasing $`K`$ is thus tantamount to increasing the amount of disorder, the fully chaotic regime corresponding to a finite density of impurities.

Electron and hole excitations inside a superconductor are however coupled by a nonvanishing pair-potential. Accordingly we extend the kicked rotator of Eq. (1) to a Bogoliubov-de Gennes form. We discuss this construction for the case $`D=2`$. First, we replace the free quasiparticle motion by a coupled electron and hole dynamics,

$`_0`$ $`=`$ $`\mathrm{exp}(i\tau _0/\mathrm{}),`$ (2a)
$``$ $`=`$ $`H\sigma _z+\mathrm{\Delta }\sigma _x.`$ (2b)
Here, $`H=(\mathrm{}^2\stackrel{}{}^2/2I)E_F`$, with $`E_F`$ the Fermi energy, $`\sigma _{x,z}`$ are Pauli matrices acting in particle-hole space, and $`\mathrm{\Delta }`$ is the superconducting pair potential. Second, the coupled quasiparticle motion is followed by a kick

$`_K`$ $`=`$ $`\mathrm{exp}(i_K/\mathrm{}),`$ (3a)
$`_K`$ $`=`$ $`{\displaystyle \frac{KI}{\tau _0}}\mathrm{cos}x\mathrm{cos}y\sigma _z.`$ (3b)
Exponentiating the Pauli matrices, we end up with the Bogoliubov-de Gennes-Floquet (BdGF) operator

$``$ $`=`$ $`_K_0,`$ (4a)
$`_0`$ $`=`$ $`\mathrm{cos}\sqrt{(H^2+\mathrm{\Delta }^2)(\tau _0/\mathrm{})^2}`$ (4b)
$`+`$ $`{\displaystyle \frac{i\mathrm{sin}\sqrt{(H^2+\mathrm{\Delta }^2)(\tau _0/\mathrm{})^2}}{\sqrt{H^2+\mathrm{\Delta }^2}}}[H\sigma _z+\mathrm{\Delta }\sigma _x],`$
$`_K`$ $`=`$ $`\mathrm{cos}\left[{\displaystyle \frac{KI}{\mathrm{}\tau _0}}\mathrm{cos}x\mathrm{cos}y\right]`$ (4c)
$`+`$ $`i\mathrm{sin}\left[{\displaystyle \frac{KI}{\mathrm{}\tau _0}}\mathrm{cos}x\mathrm{cos}y\right]\sigma _z,`$
with $``$, the identity matrix in particle-hole space. For $`\mathrm{\Delta }=0`$, Eq. (4) describes uncoupled electron and hole excitations in a disordered 2$`D`$ metal. Once this metal becomes superconducting, $`\mathrm{\Delta }`$ couples these excitations during their free propagation, while it is neglected during the instantaneous kick. As in the case of a BdG eigenproblem, the $`2M`$ quasienergies \[with average spacing $`\delta \epsilon _{m+1}\epsilon _m=\pi /M`$\] of the BdGF equation $`\varphi _m=\mathrm{exp}(i\epsilon _m)\varphi _m`$, come in pairs with opposite sign $`\epsilon _m=\epsilon _{2Mm+1}`$, similarly to the spectral properties of a BdG Hamiltonian. These considerations establish the correspondence between the map of Eq. (4) and quasiparticles in a dirty superconductor.

We next quantize the phase space on a $`4`$-torus $`\{x,y;p_x,p_y\}`$, with dimensionless momentum $`p_{x,y}=i\mathrm{}_{\mathrm{eff}}/(x,y)(0,2\pi )`$ Izr90 . The effective Planck constant $`\mathrm{}_{\mathrm{eff}}\mathrm{}\tau _0/I_0`$ takes on values $`\mathrm{}_{\mathrm{eff}}=2\pi /M`$, with integer $`M=L_xL_y`$, in term of the real-space linear system sizes $`L_{x,y}`$ (also expressed in units of a lattice spacing), and the impurities have a spatial extension $`\zeta =O(L_x,L_y)`$. The BdGF operator is then a $`2M\times 2M`$ unitary matrix, and we consider the two cases of d-wave $`[\mathrm{\Delta }(p_x,p_y)=\mathrm{\Delta }_0(p_x^2p_y^2)/(p_x^2+p_y^2)]`$ and extended s-wave $`[\mathrm{\Delta }(p_x,p_y)=\mathrm{\Delta }_0|p_x^2p_y^2|/(p_x^2+p_y^2)]`$ pair potentials, for which $`_0`$ is diagonal in momentum representation. Noting that $`_K`$ is diagonal in real space representation, we rewrite $``$ as

$`_{\stackrel{}{p}\stackrel{}{p}^{}}`$ $`=`$ $`(\left[𝒰_K𝒰^{}\right]_0)_{\stackrel{}{p}\stackrel{}{p}^{}},`$ (5)
where $`𝒰=U`$, and $`U`$ is the unitary matrix of the 2$`D`$ Fourier transform between real space and momentum coordinates, $`U_{\stackrel{}{p}\stackrel{}{p}^{}}=M^{1/2}\mathrm{exp}[(2\pi i/M)\stackrel{}{p}\stackrel{}{p}^{}]`$. We numerically extract the quasienergy DoS from the eigenvalues $`\mathrm{sin}\epsilon _m`$ of the hermitean matrix $`\frac{1}{2i}(^{})`$, which we diagonalize using the Lanczos algorithm Ket99 .

In Fig. 1 we show the quasienergy DoS for d-wave and extended s-wave pair potentials away from half filling ($`E_F=2\pi ^2/5<\pi ^2/2`$), as the kicking strength increases. In the clean case ($`K=0`$) the two DoS are the same. The gap singularity at $`E/\mathrm{\Delta }_0=1`$ gets washed out as $`K`$ increases in both cases, however, a peak emerges in the d-wave DoS around $`E=0`$, while $`\rho (E)=0`$ in the extended s-wave case. This is in agreement with Ref. Ada02 ; Ada99 , i.e. the existence of low-energy states requires a change in the sign of the pair potential. In the extended s-wave case, the low energy peak is shifted by an energy corresponding to the gap averaged over all momenta mixed by the impurity potential.

We focus on the d-wave symmetry from now on. A closer look at the DoS in the fully chaotic regime with $`K=8.`$ is provided in Fig. 2. It indicates that the characteristic semiclassical singularity exhibited by the DoS as $`E0`$ is cut off at an energy $`E^{}\mathrm{\Delta }_0`$, where a sharp drop occurs and $`\rho (E)0`$. RMT predicts such a drop to occur over an energy scale given by the Thouless energy Altland02 , which in our case is however significantly larger than $`\mathrm{\Delta }_0`$ caveat . We thus attribute this drop to the emergence of diffractive scattering at times larger than $`\tau _E`$ Alarkin  as follows. According to Ref. Ada02 , the DoS corresponding to low energy semiclassical states can be estimated from a mapping onto a tight-binding chain with random hoppings, for which the eigenfunctions are localized with an energy-dependent localization length $`\xi (E)`$ Eggarter . At low energies, $`\xi `$ exceeds the diffractive scattering length $`v_F\tau _E`$, ($`v_F`$ is the Fermi velocity) in which case hoppings between otherwise uncoupled tight-binding chains (corresponding to different classical trajectories) have to be taken into account. The emergence of these processes signals the breakdown of semiclassics and the restoration of RMT. One thus expects the vanishing of the DoS below a threshold energy given by the condition $`\xi (E^{})v_F\tau _E`$. Since $`\xi (E)`$ is bounded by the superconducting coherence length, $`\xi (E)\mathrm{}v_F/\mathrm{\Delta }_0`$ Ada02 , the observation of the semiclassical peak in the DoS requires a long enough diffractive scattering length $`v_F\tau _E>\mathrm{}v_F/\mathrm{\Delta }_0`$. While preliminary results corroborate this argument, a detailed investigation of $`E^{}`$ will be presented elsewhere Jacada03 .

In the inset to Fig. 2 we show the asymptotic behavior of the DoS on a log-log scale. Once abstraction is made of the drop in the DoS below $`E^{}`$, the semiclassical data exhibit a singular behavior slightly below $`E^1`$ (black circles) which is in qualitative agreement with the prediction $`\rho (E)E^1|\mathrm{ln}E|^3`$ of Ref. Ada02 .

Having established the validity of semiclassical predictions in the quantum chaotic regime, we next decrease the range of the disorder and enter the quantum disordered regime. We accomplish this via the inclusion of higher harmonics to the kicking potential, and replace Eq. (3) by

$$_K=\frac{KI}{N_H^2\tau _0}\underset{l,m=1}{\overset{N_H}{}}\mathrm{cos}[lx]\mathrm{cos}[my]\sigma _z.$$
(6)
The typical impurity size decreases as $`\zeta N_H^1`$. Fig. 3 shows the disappearance of the low-energy peak in the DoS as $`N_H`$ increases. For the set of parameter considered, once $`N_H27`$ is reached, the DoS vanishes at $`E=0`$. Note that the resolution used in Fig. 3 does not allow to see the opening of the RMT gap below $`E^{}`$. A more precise look at the DoS for $`N_H=27`$ is provided on the inset to Fig. 2 (empty diamonds). The data clearly indicate the expected RMT linear suppression of the DoS.

Our results thus clarify the competition between RMT Altland02  and semiclassics Ada02 . The next step is to investigate the transport properties and to explore the parametric dependence of $`E^{}`$. Work along those lines is in progress Jacada03 .

This work was supported by the Dutch Science Foundation NWO/FOM and the Swiss National Science Foundation. We thank I. Gornyi, A. Yashenkin, M. Vojta, N. Trivedi, and P. M. Goldbart for interesting discussions and comments.