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# New approach of fragment charge correlations in 129Xe+natSn central collisions

## 1 Introduction

The search for signals of a liquid-gas phase transition in the nuclear medium is presently a very active field of research (see  and ref. therein). In such a framework, multifragmentation is a key process. A possible scenario is the excursion of the excited system, produced in dissipative heavy-ion collisions, at low densities inside the coexistence region of the nuclear phase diagram (for a general introduction to the subject, see for instance ). There, a volume instability, the so-called spinodal decomposition, leads to a disassembly of the system . Such a behaviour is predicted by microscopic transport calculations based on the nuclear Boltzmann equation and its stochastic extensions . The main idea is to search for fragmentation events in which most fragment atomic numbers are nearly equal as suggested by theoretical works . It is worth noting that surface instabilities, like Rayleigh or sheet instabilities , may produce, in the early compression-expansion stage of the collision, the formation of toroidal and bubble nuclei (depending of the value of the incompressibility constant $`K`$) that may also decay into several nearly equal fragments . In any case, the proportion of this kind of multifragmentation events should be small and a sensitive method, called “higher-order correlations”, has been proposed in Ref.  to search for weak signals in the fragment charge correlation analyses. Following the prescriptions of this method, the question of a possible experimental signature of spinodal decomposition of excited nuclear matter has been examined for 129Xe+natSn central collisions at 32 MeV/n in a previous work .

The analysis relies on two variables. The average fragment charge per event is defined as:

$$<Z>=\frac{1}{M}\underset{i=1}{\overset{M}{}}Z_i$$
(1)
where $`Z_i`$ is the charge of fragment $`i`$ and $`M`$ is the fragment multiplicity. Only fragments with atomic number $`Z_i5`$ are considered. As in Refs , the standard deviation in fragment sizes is defined as:

$$\mathrm{\Delta }Z=\sqrt{\frac{1}{M1}\underset{i=1}{\overset{M}{}}(Z_i<Z>)^2}$$
(2)
The correlation function, $`R`$, is built by considering the ratio of the measured yield $`Y(\mathrm{\Delta }Z,<Z>)`$ versus the “uncorrelated” yield $`Y^{}(\mathrm{\Delta }Z,<Z>)`$. Since events with nearly equal size fragments are associated with low values of $`\mathrm{\Delta }Z`$, any significant enhancement of $`R`$ for small $`\mathrm{\Delta }Z`$ ($`\mathrm{\Delta }Z<1`$) may signal a spinodal decomposition as proposed in . The key question is how to build the uncorrelated yield $`Y^{}`$. This last quantity has been estimated for each class of fragment multiplicities by mixing fragments from different events of the selected sample . In doing so, the initial total charge carried out by the fragments ($`Z_{bound}=_{i=1}^MZ_i=M<Z>`$) and also the average fragment charge $`<Z>`$ are not conserved in building $`Y^{}`$. Consequently, in the absence of correlations the ratio $`R=Y/Y^{}`$ is not equal to unity and depends simultaneously on the $`<Z>`$ and $`\mathrm{\Delta }Z`$ values. Thus, to extract the true correlation one has to determine a background function $`R^{}`$ corresponding to the ratio $`Y/Y^{}`$ for uncorrelated events.

In the present paper, in a first step, we would like to show how the method previously used to generate the charge correlation functions , that we will call $`Z_{bound}`$ mixing method, may generate spurious signals. Then, a new method to build the uncorrelated yield $`Y^{}`$ is presented in Section 3. By applying this method, the fragment charge correlations obtained in the 129Xe+natSn central collisions between 32 and 50 MeV/n are discussed in Section 4. A recently proposed method to build the denominator $`Y^{}`$, called IPM for Intrinsic Probability Method , which has been applied to the same Xe+Sn data set , is commented in Section 5.

## 2 Review of the $`Z_{bound}`$ mixing method

### 2.1 Data selection and previous charge correlation results

The charge correlations were analysed in a set of events associated with a “quasi-fusion” process occurring in central 129Xe+natSn collisions at 32 MeV/n. Only events with the sum $`Z_{tot}`$ of the detected charges greater or equal to 80 were considered, the total charge of the Xe+Sn system being 104. Briefly, the event selection was based on the measurement of the distribution of the preferred emission direction of matter in the centre of mass of the reaction (flow angle). In this work, fragment charge correlation analyses have been performed by selecting events having a flow angle larger than $`60^o`$. It has been shown  that such events ($`\mathrm{\Theta }_{flow}60^o`$) could be interpreted as resulting from the multifragmentation of a thermalised and compact nuclear system (“single source” events). In a previous work , using the same gating condition, the charge correlation functions $`R(\mathrm{\Delta }Z,<Z>)`$ were first built for each fragment multiplicity $`M=`$ 3, 4, 5 and 6. However, the results suffered from a lack of statistics. The numbers of events in the first bin in $`\mathrm{\Delta }Z`$ ($`\mathrm{\Delta }Z<1`$) and for each multiplicity of this selection are shown in the third column of Table 1. As we see, these numbers, summed over all $`<Z>`$, are quite small, specially for multiplicities $`M=`$ 5 and 6. Thus, to increase the statistical significance of the signal, the charge correlations were built by replacing the variable $`<Z>`$ by the sum of the fragment charges $`Z_{bound}`$ (each bin in $`Z_{bound}`$ containing six atomic numbers). Summing over all $`M`$, the resulting correlation functions shown in Fig. 3 of Ref.  were interpreted as an evidence of a significant enhancement of equal-sized fragments associated with fused events in Xe+Sn collisions at 32 MeV/n. However, as we mentioned previously, the charge correlation function cannot be compared to unity but to a specific $`R^{}`$ background function. This function has been estimated in Ref.  by assuming that, in the absence of correlations and for a given $`Z_{bound}`$, $`R^{}=f(\mathrm{\Delta }Z,Z_{bound})`$ is exponentially increasing with $`\mathrm{\Delta }Z`$ in the range $`0<\mathrm{\Delta }Z<8`$. Obviously, the choice of the background estimation is the critical point of this method and in order to test the hypothesis of Ref.  we have performed a charge correlation analysis $`R(\mathrm{\Delta }Z,Z_{bound})`$ from a sample of randomly generated events.

### 2.2 Random break-up simulation

In the Monte Carlo simulation, the following procedure, that we will call random break-up, has been used: for a given fragment multiplicity $`M`$, the charge of the fragments is obtained by breaking $`M1`$ bonds at random in a chain of length $`Z_{bound}`$. Only events for which all fragments have $`Z5`$ were kept. For each multiplicity, the $`Z_{bound}`$ distribution was the experimental one for central Xe+Sn collisions at 32 MeV/n. We have checked that for each multiplicity $`M`$, the ensemble thus generated is equivalent to the one obtained by computing all partitions and their permutations containing $`M`$ fragments with $`Z_i5`$ such that $`_{i=1}^MZ_i=Z_{bound}`$ . The $`Z_{bound}`$ distributions are given in the first column of Fig. 1 as a function of the fragment multiplicity $`M`$. They are gaussian in shape with a centroid which increases from $``$54 for $`M`$=3 to $``$64 for $`M`$=6, whereas their width is practically constant. To minimize statistical effects, twenty times more events were generated in the simulation than in the data. The simulated $`Z`$-distributions (full lines) are compared to the experimental data in the second column of Fig. 1. For multiplicities $`M`$= 5 and 6, the agreement is remarkably good. At lower multiplicities $`M`$= 3 and 4, the simulated distributions are slightly broader than the experimental ones. The last two columns of Fig. 1 compare the simulated $`\mathrm{\Delta }Z`$ distributions (full lines) to the experimental ones with two $`\mathrm{\Delta }Z`$ scales (in order to show the details at low $`\mathrm{\Delta }Z`$). There again for multiplicities 5 and 6, the agreement between the simulation and the data is remarkable. For the lower multiplicities 3 and 4, as for the $`Z`$-distributions, the simulated distributions are broader than the experimental ones. Examination of the last column of Fig. 1 reveals no enhancement over the simulation for $`\mathrm{\Delta }Z<6`$. The numbers of events with $`\mathrm{\Delta }Z<1`$ obtained in the simulation are listed in the second column of Table 1 as a function of multiplicity. We note that the total fraction of events (0.154 $`\pm `$ 0.005 %) in this $`\mathrm{\Delta }Z`$ bin is compatible with the experimental one (0.127 $`\pm `$ 0.020 %).

Fig. 2a shows the ratio between the random break-up yield $`Y_{breakup}`$ over $`Y_{partitions}`$ obtained by calculating analytically all possible partitions  as a function of $`\mathrm{\Delta }Z`$ for each multiplicity $`M`$ and their sum. Except for the low statistics data with large $`\mathrm{\Delta }Z`$ ($`M`$=6), all of the ratio values are consistent with unity. It is worth noting that in the present case, deviations from unity are of statistical origin only. Fig.2b displays the values of $`Y_{breakup}/Y_{partitions}`$ in the bin $`\mathrm{\Delta }Z<1`$ as a fonction of $`<Z>`$. In this bin, the statistics is poor and we observe deviations in excess of one standard deviation ($`\sigma `$). In the following, the random break-up events are analysed using the $`Z_{bound}`$ mixing method .

### 2.3 Application of the $`Z_{bound}`$ mixing method to the random break-up simulation

Firstly, the charge correlation functions $`R(\mathrm{\Delta }Z,<Z>)`$ were built for each multiplicity $`M=3,4,5,6`$, separately. For this purpose, the uncorrelated yield $`Y^{}`$ was built generating $`10^3`$ times more events than in the numerator in order to minimize statistical errors on the denominator. The $`R`$ values corresponding to four ($`M,<Z>`$) pairs chosen in the interval $`48Z_{bound}52`$ are shown in Fig. 3a. They illustrate the general evolution of the function $`R=Y/Y^{}`$. The amplitude and extension in $`\mathrm{\Delta }Z`$ of the function $`R`$ depend on the multiplicity $`M`$ and the average charge $`<Z>`$. However, we note that within statistics, the charge correlation functions decrease with decreasing $`\mathrm{\Delta }Z`$ without any significant enhancement in the first bin in $`\mathrm{\Delta }Z`$, as expected for uncorrelated events. In the absence of correlations other than charge conservation, these results (Fig. 3a) represent the background function $`R^{}`$ discussed above. Large fluctuations and statistical error bars are present in the low $`\mathrm{\Delta }Z`$ bins. Thus, a correct estimate of the function $`R^{}`$ from experimental data, often associated with weaker statistics, appears to be a very difficult task.

Secondly, following , we built the charge correlations $`R(\mathrm{\Delta }Z,Z_{bound})`$. They are displayed in Fig. 3b for six values of $`Z_{bound}=39,45,51,57,63,69`$ as a function of $`\mathrm{\Delta }Z`$ (each bin in $`Z_{bound}`$ regrouping six atomic numbers). The four ($`M,<Z>`$) pairs shown in Fig. 3a are now integrated in the bin $`Z_{bound}=51`$. Obviously, our events being uncorrelated all these correlation functions are the background functions $`R^{}`$. Contrary to what was assumed in  these background functions are not exponential functions of $`\mathrm{\Delta }Z`$ even in the restricted range $`\mathrm{\Delta }Z<8`$. Thus, if as in , one assumes an exponential background in the range $`2<\mathrm{\Delta }Z<8`$ (the lines in Fig. 3b), and extrapolates it down to zero, one creates artificially a signal at low $`\mathrm{\Delta }Z`$. The fragment charge correlations for the bin $`\mathrm{\Delta }Z<1`$ and the corresponding background extracted this way (broken line) are plotted in Fig. 4 (up-left) as a function of $`Z_{bound}`$. This figure is very similar to Fig. 3 of Ref. . This spurious result finds its origin in the mixing of events with different fragment multiplicities $`M=`$ 3, 4, 5 and 6 to build $`Z_{bound}`$ bins. Indeed, the charge correlation functions $`R(\mathrm{\Delta }Z,Z_{bound})`$ combine various functions $`R(\mathrm{\Delta }Z,<Z>)`$ which are multiplicity dependent.

This artificial enhancement of equal-sized fragments is not systematic and depends on the $`Z_{bound}`$ distributions. Xe+Sn central collisions have also been studied with INDRA at 39, 45 and 50 MeV/n . In Ref. , the authors show the disappearence of the charge correlation signal at low $`\mathrm{\Delta }Z`$ when the energy increases. But, the same evolution is obtained by analysing simulated data without charge correlations. By using the $`Z_{bound}`$ mixing method, we show in Fig. 4 the charge correlations in the first $`\mathrm{\Delta }Z`$ bin of four sets of events generated by the random break-up simulations obtained from the $`Z_{bound}`$ distributions of Xe+Sn data at 32, 39, 45 and 50 MeV/n (with 20 times the statistics of the data). This figure, very similar to Fig.2 of Ref. , shows clearly the artificial decreasing of the charge correlation signal when the energy increases. Consequently, the method using the mixing of multiplicities  renders unreliable an estimation of the background $`R^{}`$.

## 3 The exchange mixing event method

### 3.1 Description of the method

To get rid of the problematic evaluation of the background, we attempted to build an uncorrelated yield $`Y^{}`$ with the conservation of the total fragment charge ($`Z_{bound}`$). In such a case the charge correlation function can be directly compared to unity. The following procedure has been developed. For an ensemble of events with a given fragment multiplicity, $`M`$, we consider the exchange of two fragments of charges $`Z_1(i)`$ and $`Z_2(i)`$ belonging to the event labelled $`i`$ with two fragments of charges $`Z_1^{}(j)`$ and $`Z_2^{}(j)`$ belonging to the event labelled $`j`$ under the condition that $`Z_1(i)+Z_2(i)=Z_1^{}(j)+Z_2^{}(j)`$. As such, the total fragment charge $`Z_{bound}`$ and the average charge $`<Z>`$ are conserved event by event and then the $`Z_{bound}`$ and the charge distributions of the considered ensemble are conserved. For a given event $`i`$, we performed the substitutions by a random picking of event $`j`$ followed by a random picking of charges inside, respectively, the events $`i`$ and $`j`$. If the condition $`Z_1(i)+Z_2(i)=Z_1^{}(j)+Z_2^{}(j)`$ was verified the charge substitutions were performed, if not we proceeded with a new random picking of event $`j`$, and so on, until all events in the sample has been changed at least once (one iteration). First, 100 iterations are performed to get a mixed sample. Then, the yield $`Y^{}(\mathrm{\Delta }Z,<Z>)`$ is created from this mixed sample by continuing the same iterative procedure $`10^3`$ times and at each time $`Y^{}`$ is incremented in order to make negligible its statistical error (relative to $`Y`$). Accurate tests showing the sensitivity of the exchange method are developed in the next. One can also consider exchanges among the events in which more than two (say $`N`$) fragments are exchanged. In this latter case, the method is obviously restricted to events for which $`M`$ is larger than $`N`$ and in the following we only use $`N=2`$.

### 3.2 Tests of the exchange mixing method

The technique has been tested with the random break-up calculation and the results are plotted in Fig. 5a for each multiplicity and the whole ensemble $`M=3,4,5,6`$. For any multiplicity, the correlation function $`R=f(\mathrm{\Delta }Z)`$ is constant and close to unity (most of the statistical error bars are smaller than the symbol size). Although we performed this simulation with a statistics twenty times larger than the one of the Xe+Sn data at 32 MeV/n (see Table 1), statistical fluctuations are still present, specially, in the first and largest bins in $`\mathrm{\Delta }Z`$ for $`M=`$ 6. The correlation function $`R`$ corresponding to the whole multiplicity set is equal to unity (bottom picture in Fig. 5a) independently of $`\mathrm{\Delta }Z`$. In this latter case, the fact that the correlations $`R=f(\mathrm{\Delta }Z)`$ are multiplicity independent validates the multiplicity regrouping.

However, when this method is applied to the data, the denominator may partially keep the fragment charge correlations present in the experimental sample (numerator). For example, applied on an event sample populated in majority by nearly-equal sized fragments, this method, as any others based on the data, would paradoxally give a weak signal. So, the exchange method may only be relevant in the search of a weak proportion of equal-sized fragment events in the data and it is crucial to test its sensitivity to measure an enhancement of charge correlations precisely in the bin $`\mathrm{\Delta }Z<1`$. In order to do this test, we doubled the number of events populating the first bin in $`\mathrm{\Delta }Z`$ in the random break-up sample and build new uncorrelated yields $`Y^{}`$. The results of the charge correlation analyses of this new sample are displayed in Fig. 5b. As expected, the charge correlations $`R`$ in the first bin, within statistical uncertainties, are twice the ones shown in Fig. 5a, whereas they are unchanged in other bins. By integrating over all multiplicities $`M`$ and $`<Z>`$, the correlation value in the first bin is: $`R=1.941\pm 0.045`$ (bottom picture in Fig. 5b). In this case, the number of events is large and we performed the same analysis with a set of simulated events statistically compatible with the Xe+Sn data at 32 MeV/u. In the first bin, the new correlation value $`R=1.961\pm 0.192`$ is very close to the expected value $`R=2`$ at $`5`$ standard deviations from one. These tests substantiate the good sensitivity of the exchange procedure used to build $`Y^{}`$.

The use of the random break-up simulation is also a powerful tool to evaluate the kind of errors induced by the exchange mixing method. In such a simulation, where no correlation is expected, the deviations from unity should contain a statistical part due to the number of generated events (numerator), called $`\sigma _N`$, and, perhaps, a systematic error due to the method itself. In Fig. 6a, we show the deviations from 1 of all charge correlation values $`R(\mathrm{\Delta }Z,<Z>,M)`$, normalized to their statistical error bar $`\sigma _N`$ (absissa $`x=(R1)/\sigma _N`$), obtained from the simulations previously described and for each multiplicity $`M=3,4,5`$ and 6 (see Fig. 5a). The good superimposition of the $`x`$ distribution with the normal function (see Fig. 6a) shows clearly that the errors associated with the exchange method are purely statistical. As all possible partitions ($`Y_{partitions}`$) have been analytically calculated (see Fig. 2) in the random break-up simulation, the yield $`Y^{}=Y_{partitions}`$ has been used as denominator in Fig. 6b. The remarkable similarity between both $`x`$ distributions in Fig. 6a and 6b indicates that there is no contribution due to the exchange method itself in the fluctuations of $`R`$. In the same manner, we plotted in Fig. 6c, the distribution of $`x`$ obtained from the Xe+Sn data at 32 MeV/n. In this data, the good superimposition of the distribution of $`R(\mathrm{\Delta }Z,<Z>,M)`$ values by the normal function, indicates that all deviations of $`R`$ from unity appear compatible with statistical fluctuations. In the next Section, the fragment charge correlation functions associated to the Xe+Sn data are presented as a function of $`\mathrm{\Delta }Z`$, $`<Z>`$ and $`M`$.

## 4 Application of the exchange mixing method to the Xe+Sn data

In the Xe+Sn central collisions, the multifragmentation process is present at 32, 39, 45 and 50 MeV/n and complete events ($`Z_{tot}80`$) selected with $`\mathrm{\Theta }_{flow}60^o`$ have been considered to arise from the multifragmentation of single nuclear sources . For a given fragment multiplicity, the number of events with $`\mathrm{\Delta }Z<1`$ at respectively 39, 45 and 50 MeV/n bombarding energies are listed in columns 4 to 6 of Table 1. The production of near equal-sized fragment events increases with the incident energy and reaches $`2`$% at 50 MeV/n. This trend is a result of charge conservation. The multiplicity of light charged particles and fragments ($`Z4`$) is increasing with the incident energy . Hence, the average total fragment charge ($`Z_{bound}`$) decreases. Thus for a given fragment multiplicity, the size of the fragments decreases and the probability to measure equal-sized fragment events naturally increases. The analyses of the charge correlations for these “single source” samples have been performed, using the exchange mixing procedure to generate $`Y^{}`$. The charge correlations $`R`$ have been built at each energy. First, we show in Fig. 7 the charge correlation functions $`R=Y/Y^{}`$, summed over all $`<Z>`$, as a function of $`\mathrm{\Delta }Z`$ for each multiplicity $`M=`$ 3, 4, 5 and 6 (the first four rows) and for each incident energy (columns). The bottom row of Fig. 7 corresponds, at each bombarding energy, to the whole experimental data (summed over $`M`$) and benefits from enhanced statistics. All values of $`R`$ are close to unity. To be more quantitative, Fig. 8 displays the quantity $`(R1)/\sigma `$ as a function of $`\mathrm{\Delta }Z`$ for random break-up (with analytical background) simulated events (first column) and for the experimental data from 32 to 50 MeV/n (columns 2 to 5), for multiplicities $`M=3`$ to 6 (rows 1 to 4) and for all multiplicities (last row). For convenience, we have drawn dotted lines corresponding, respectively, to one and two standard deviations. We note that the fluctuations around zero are about of the same amplitude in the simulation and in the data over the whole range in $`\mathrm{\Delta }Z`$. The fluctuations for small $`\mathrm{\Delta }Z`$ (as well as for large $`\mathrm{\Delta }Z`$) are not particularly larger than in any other $`\mathrm{\Delta }Z`$ bins. Nevertheless, following theoretical predictions  the overproduction of equal-sized fragments should specifically concern a narrow range in $`Z1015`$. If true, the summing over all $`<Z>`$ to determine the correlation functions may reduce significantly the importance of the “signal”. For this reason, we show in Fig. 9 the $`R`$ values corresponding to this first bin as a function of $`<Z>`$ for each multiplicity $`M=`$ 3, 4, 5 and 6 (the first four rows), for all multiplicities (last row) and for each incident energy (columns). All $`<Z>`$ bins populated with more than one event have been plotted in Fig. 9. This choice induces the absence of data point at 32 MeV/n for $`M=`$5 and 6. Notice that experimental error bars are statistical only. All values of $`R`$ are within $`2\sigma `$ of 1. It has to be emphasized that the $`R`$ values (Fig. 9) for each multiplicity corresponding to the energies 45 and 50 MeV/n are particularly close to the $`R=1`$ line and associated with small statistical fluctuations. On the other hand, at 32 MeV/n and 39 MeV/n, we are dealing with large statistical errors. The, perhaps, systematic enhancements of $`R`$ at 39 MeV/n for multiplicity 4 in the range $`<Z>=711`$, are compatible with 1 within $`1.2\sigma `$ which is poorly significant (less than 80% of confidence level). Finally, we do not observe any significant enhancement of equal-sized fragments in the Xe+Sn central collisions between 32 and 50 MeV/n.

## 5 Comparison between methods

Recently, an alternative method, called IPM , has been proposed to build the denominator $`Y^{}`$ using the independent emission hypothesis constrained by the charge conservation. Basically, it is assumed that the probability to observe a given partition ($`n_z:(n_1,\mathrm{},n_{Z_{tot}})`$) with a multiplicity $`M`$ of a nucleus of charge $`Z_{tot}`$ is given by the multinomial formula

$$P(\{n_z\})=\alpha M!\frac{(P_z)^{n_z}}{n_z!}\text{ with }\underset{z}{}P_z=1$$
(3)
where $`\alpha `$ is the normalization constant ($`_{n_z}P(\{n_z\})=1`$), $`P_z`$ is the intrinsic probability for emitting the charge $`z`$, $`n_z`$ the number of charges $`z`$ in the partition ($`Z_{tot}=_zn_zz`$) and $`M`$ the multiplicity of the partition ($`M=_zn_z`$). We note that in the case of a fully random break-up, the partitions are weighted by the factor $`M!/n_z!`$. Thus, in that particular case the quantity $`(P_z)^{n_z}`$ is a constant. For large $`Z_{tot}`$, the normalization condition implies $`P_z=2^z`$ . Any other laws for the $`P_z`$ will imply a departure from random break-up and the partitions thus generated might not be free from correlations. In the IPM method, the probabilities $`P_z`$ are determined by fitting the partition probabilities $`P(\{n_z\})`$ of the numerator and, as a consequence, they may keep memory of the experimental correlations. In other words, the IPM method may measure charge correlation deviations from the independent emission hypothesis but the absence of charge correlations in the denominator $`Y^{}`$ is not obvious. Moreover, as the IPM method relies upon a fit to the statistical weights associated with each fragment partition, it washes partly out statistical fluctuations. In Ref. , the IPM method has been applied to the Xe+Sn data and the deviations of $`R`$ from unity are distributed according to a law which is narrower than a normal distribution. However what should be this law is unknown. Thus, the fact that the fluctuations of $`R`$ around unity are narrower in the case of the IPM method compared with the exchange mixing method does not guarantee that the former method is more sensitive. The question of sensitivity has been accurately discussed for the exchange mixing method by performing several tests from simulated event samples in which the amplitudes of charge correlations in the bin $`\mathrm{\Delta }Z<1`$ were precisely known (see Section 3.2).

In , the IPM method has been applied to a set of partitions generated by the Brownian One-Body (BOB) dynamical model which supports the spinodal decomposition of hot and dilute finite nuclear systems . This calculation, performed for head-on Xe+Sn collisions at 32 MeV/n, has been shown to reproduce quite well the experimental fragment multiplicity and charge distributions . Of the 1% of events in the bin $`\mathrm{\Delta }Z<1`$, a percentage of 0.36% of events has been evaluated in excess of the background with the IPM method which represents a correlation value $`R1.5`$ . The charge correlation function of the same BOB event sample has been also determined by using the exchange mixing method proposed in this work and, inside the statistical error bars, no enhancement of equal-sized fragments was visible . This contradictory result is really puzzling. Indeed, from the simulated event sample obtained from the $`Z_{bound}`$ distribution of the Xe+Sn data at 32 MeV/n (see Section 3.2), with a statistics comparable to the BOB calculation one, we increased the number of events in the first $`\mathrm{\Delta }Z`$ bin by 50%. We analysed, by taking the definition $`\mathrm{\Delta }Z=\sqrt{\frac{1}{M}_i(Z_i<Z>)^2}`$ used in Ref. , the fragment charge correlations of this new set of events with the exchange method. In the first $`\mathrm{\Delta }Z`$ bin the charge correlation value, integrated over all $`M`$ and $`<Z>`$, was: $`R=1.450\pm 0.121`$, which is compatible with the expected value $`R=1.5`$ at $`3.7\sigma `$ from $`R=1`$. Once more, we conclude about the good ability of the exchange method to exhibit a correlation signal with a low rate of overproduction of equal-sized fragment events. In fact, in the BOB calculation equal-sized fragment events are produced early in the collision when the system goes through the spinodal region of the phase diagram of the nuclear matter. Then, subsequent steps like coalescence to form heavier fragments, thermal desexcitation and detection filtering, coupled with the finite size of the system, deeply blur the original picture of the partitions . Thus, it seems difficult to use BOB calculation as a reference to assess the sensitivity of the various correlation methods.

We note that, applied to the same Xe+Sn data analysed in this work, the IPM method shows an enhancement of equal-sized fragment production at 32, 39 and 45 MeV/n , in contradiction with our results.

## 6 Conclusions

We have developed a two-step analysis to address the issue of charge correlations in nuclear collisions. First, we have shown, by using a simulation which randomly generates fragments, how the extrapolation to low values of the $`\mathrm{\Delta }Z`$ distribution as performed in  may induce a spurious enhancement of the correlation function at small $`\mathrm{\Delta }Z`$. We have underlined the difficulties to make a quantitative analysis of the charge correlations when the total fragment charge ($`Z_{bound}`$) is not conserved in building the uncorrelated yield $`Y^{}`$. Then, to avoid such a problem, we have discussed a new method to build the yield $`Y^{}`$ by mixing events under the constraints of the conservation of the total charge of the fragments and the invariance of charge distributions for a given fragment multiplicity. This method has been successfully tested with a random break-up simulation and is sensitive to any statistically significant deviation from a pure uncorrelated fragmentation process. Finally, it has been applied in multifragmentation samples of the 129Xe+natSn central collisions at energies between 32 and 50 MeV/n. All charge correlation functions at low $`\mathrm{\Delta }Z`$ are equal to unity within two standard deviations and we conclude that no significant enhancement of equal-sized fragments has been observed. These results are in agreement with those obtained in the reactions Xe+Cu and Ar+Au at 50 MeV/n  but at variance with other analyses of the Xe+Sn data using different estimations of the uncorrelated yield $`Y^{}`$ . In view of these contradictory results, caution should be taken before giving any definite conclusion on a signature of spinodal decomposition in nuclear systems by charge correlation measurements.

The experiments 129Xe+natSn were performed at GANIL by the INDRA collaboration.


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# Current Noise in ac-Driven Nanoscale Conductors

## Abstract

The theory for current fluctuations in ac-driven transport through nanoscale systems is put forward. By use of a generalized, non-Hermitian Floquet theory we derive novel explicit expressions for the time-averaged current and the zero-frequency component of the power spectrum of current fluctuations. A distinct suppression of both the zero-frequency noise and the dc-current occurs for suitably tailored ac-fields. The relative level of transport noise, being characterized by a Fano factor, can selectively be manipulated by ac-sources; in particular, it exhibits both characteristic maxima and minima near current suppression.

Recent experimental successes in the coherent coupling of quantum dots Blick1996a  and in the reproducible measurement of electronic currents through molecules Cui2001a ; Reichert2002a  have given rise to renewed theoretical interest in the transport properties of nanoscale systems Nitzan2001a ; Hanggi2002a . Thereby, new ideas in order to exploit the quantum coherence of such systems for the construction of novel electronic devices Hanggi2002a  have emerged. One possible construction element is based on the manipulation of quantum dots or single molecules by use of an oscillating gate voltage or an infrared laser, respectively. A prominent effect of such ac-fields consists in the adiabatic Thouless1983a ; Brouwer1998a ; Altshuler1999a ; Switkes1999a  and nonadiabatic Wagner1999a ; Wang2002a  pumping of electrons. Moreover, laser irradiated molecular wires provide novel devices such as coherent quantum rectifiers Lehmann2002b  and optically controlled transistors Lehmann2002c . However, such time-dependent control schemes can be valuable in practice only if they operate at tolerable noise levels. Thus, the question whether noise properties of nanoscale systems can be selectively manipulated becomes of foremost interest.

Electron transport through time-independent, mesoscopic systems is commonly described within the framework of a scattering formalism. Both the average current Datta1995a  and the transport noise characteristics Blanter2000a ; Chen2002a  can be expressed in terms of the quantum transmission coefficients for the corresponding transport channels. By contrast, the theory for driven quantum transport is much less developed. Expressions for the spectral density of the current fluctuations have been derived for the low-frequency ac-conductance Pedersen1998a  and the scattering by a slowly time-dependent potential Lesovik1994a . However, the situation becomes more opaque in the presence of rapidly varying time-dependent fields. Within a Green function approach, a formal expression for the current through a time-dependent conductor has been presented in Refs. Datta1992a ; Jauho1994a . Here, we derive explicit expressions for both the current and the noise properties of electron transport through a nanoscale conductor under the influence of time-dependent forces at arbitrary frequency and strength. The dynamics of the electrons is solved by integrating the Heisenberg equations of motion for the electron creation/annihilation operators within a generalized Floquet approach. We then use the resulting expressions to explore the possibility of an a priori control of the dc-current and the zero-frequency noise by the influence of an ac-field.

The lead-wire model.—The entire setup of our nanoscale system is described by the time-dependent Hamiltonian $`H(t)=H_{\mathrm{wire}}(t)+H_{\mathrm{leads}}+H_{\mathrm{contacts}}`$, where the different terms correspond to the driven wire (or coupled quantum dots), the leads, and the wire-leads coupling, respectively. In order to go beyond merely formal considerations, we herewith focus on the regime of coherent quantum transport where the main physics at work occurs on the wire itself. In doing so, we neglect other possible influences stemming from driving induced hot electrons in the leads, dissipation on the wire and, as well, electron-electron interaction effects. Then, the wire Hamiltonian reads in a tight-binding approximation with $`N`$ orbitals $`|n`$

$$H_{\mathrm{wire}}(t)=\underset{n,n^{}}{}H_{nn^{}}(t)c_n^{}c_n^{}^{}.$$
(1)
The fermion operators $`c_n`$, $`c_n^{}`$ annihilate and create, respectively, an electron in the orbital $`|n`$. The influence of an applied ac-field with frequency $`\mathrm{\Omega }=2\pi /𝒯`$ results in a periodic time-dependence of the Hamiltonian: $`H_{nn^{}}(t+𝒯)=H_{nn^{}}(t)`$. The leads are modeled by ideal electron gases, $`H_{\mathrm{leads}}=_qϵ_q(c_{Lq}^{}c_{Lq}^{}+c_{Rq}^{}c_{Rq}^{})`$, where $`c_{Lq}^{}`$ ($`c_{Rq}^{}`$) creates an electron in the state $`|Lq`$ ($`|Rq`$) in the left (right) lead. The tunneling Hamiltonian

$$H_{\mathrm{contacts}}=\underset{q}{}\left(V_{Lq}c_{Lq}^{}c_1^{}+V_{Rq}c_{Rq}^{}c_N^{}\right)+\mathrm{h}.\mathrm{c}.$$
(2)
establishes the contact between the sites $`|1`$, $`|N`$ and the respective lead, as sketched in Fig. 1. Below, we shall assume within a so-termed wide-band limit that the coupling strengths $`\mathrm{\Gamma }_{\mathrm{}}=2\pi _q|V_\mathrm{}q|^2\delta (ϵϵ_q)`$, $`\mathrm{}=L,R`$, are energy independent. To specify fully the dynamics, we choose as an initial condition for the left/right lead a grand-canonical electron ensemble at temperature $`T`$ and electro-chemical potential $`\mu _{L/R}`$, respectively. An applied voltage $`V`$ maps to a chemical potential difference $`\mu _R\mu _L=eV`$, where $`e`$ is the electron charge.

We shall focus on two central transport quantities: the time-dependent electrical currents through the two contacts and their fluctuations. The current operators are given by the negative time variation of the electron numbers in the leads, multiplied by the electron charge $`e`$, $`I_{\mathrm{}}(t)=ie[H(t),N_{\mathrm{}}]/\mathrm{}`$, where $`N_{\mathrm{}}=_qc_\mathrm{}q^{}c_\mathrm{}q^{}`$ denotes the electron number in lead $`\mathrm{}`$.

Generalized Floquet approach.—For the evaluation of correlation functions, we work in the Heisenberg picture and derive the annihilation operators at long times by a Floquet ansatz Grifoni1998a . From the Hamiltonian $`H(t)`$ follow the Heisenberg equations for the lead operators, with the wire operators appearing in an inhomogeneity. In an integrated form they read

$$c_{Lq}(t)=c_{Lq}(t_0)e^{iϵ_q(tt_0)/\mathrm{}}\frac{iV_{Lq}}{\mathrm{}}\underset{0}{\overset{tt_0}{}}𝑑\tau e^{iϵ_q\tau /\mathrm{}}c_1(t\tau )$$

and $`c_{Rq}(t)`$ accordingly. Inserting this into the Heisenberg equations for the wire operators yields

$`\dot{c}_{1/N}=`$ $`{\displaystyle \frac{i}{\mathrm{}}}{\displaystyle \underset{n^{}}{}}H_{1/N,n^{}}(t)c_n^{}{\displaystyle \frac{\mathrm{\Gamma }_{L/R}}{2\mathrm{}}}c_{1/N}+\xi _{L/R}(t),`$
$`\dot{c}_n=`$ $`{\displaystyle \frac{i}{\mathrm{}}}{\displaystyle \underset{n^{}}{}}H_{nn^{}}(t)c_n^{},n=2,\mathrm{},N1.`$ (3)
Owing to the wide-band limit, the dissipative terms are memory free. Within the chosen grand canonical ensembles the operator-valued Gaussian noise $`\xi _{\mathrm{}}(t)=(i/\mathrm{})_qV_\mathrm{}q^{}e^{iϵ_q(tt_0)/\mathrm{}}c_\mathrm{}q(t_0)`$ obeys

$`\xi _{\mathrm{}}(t)=`$ $`0,`$ (4)
$`\xi _{\mathrm{}}^{}(t)\xi _{\mathrm{}^{}}(t^{})=`$ $`\delta _{\mathrm{}\mathrm{}^{}}{\displaystyle \frac{\mathrm{\Gamma }_{\mathrm{}}}{2\pi \mathrm{}^2}}{\displaystyle 𝑑ϵe^{iϵ(tt^{})/\mathrm{}}f_{\mathrm{}}(ϵ)},`$ (5)
where $`f_{\mathrm{}}(ϵ)=(1+\mathrm{exp}[(ϵ\mu _{\mathrm{}})/k_BT])^1`$ denotes the Fermi function at temperature $`T`$ and chemical potential $`\mu _{\mathrm{}}`$, $`\mathrm{}=L,R`$. The current operator then assumes the form

$$I_L(t)=\frac{e}{\mathrm{}}\mathrm{\Gamma }_Lc_1^{}(t)c_1(t)e\left\{c_1^{}(t)\xi _L(t)+\xi _L^{}(t)c_1(t)\right\}.$$
(6)
Before solving the inhomogeneous set of equations (3), let us first analyze the corresponding homogeneous equations. They are linear and possess time-dependent, $`𝒯`$-periodic coefficients. Thus, it is possible to construct a complete solution with the help of the Floquet ansatz $`|\psi (t)=\mathrm{exp}[(iϵ_\alpha /\mathrm{}\gamma _\alpha )t]|u_\alpha (t)`$. The Floquet states $`|u_\alpha (t)=_k|u_{\alpha k}\mathrm{exp}(ik\mathrm{\Omega }t)`$ obey the time-periodicity of the differential equations and fulfill in a Hilbert space that is extended by a periodic time coordinate the eigenvalue equation

$$\left((t)i\mathrm{\Sigma }i\mathrm{}\frac{d}{dt}\right)|u_\alpha (t)=(ϵ_\alpha i\mathrm{}\gamma _\alpha )|u_\alpha (t),$$
(7)
where $`(t)=_{n,n^{}}|nH_{nn^{}}(t)n^{}|`$ and $`2\mathrm{\Sigma }=|1\mathrm{\Gamma }_L1|+|N\mathrm{\Gamma }_RN|`$. Because the eigenvalue equation (7) is non-Hermitian, its eigenvalues $`ϵ_\alpha i\mathrm{}\gamma _\alpha `$ are generally complex valued and the (right) eigenvectors are not mutually orthogonal. Therefore, we need to solve also the adjoint Floquet equation yielding again the same eigenvalues but providing the adjoint eigenvectors $`|u_\alpha ^+(t)`$. It can be shown that the Floquet states $`|u_\alpha (t)`$ together with the adjoint states $`|u_\alpha ^+(t)`$ form at equal times a complete bi-orthogonal basis: $`u_\alpha ^+(t)|u_\beta (t)=\delta _{\alpha \beta }`$ and $`_\alpha |u_\alpha (t)u_\alpha ^+(t)|=\mathrm{𝟏}`$ on\_orthonormal . For $`\mathrm{\Gamma }_{L/R}=0`$, both $`|u_\alpha (t)`$ and $`|u_\alpha ^+(t)`$ reduce to the usual Floquet states.

The Floquet states $`|u_\alpha (t)`$ allow to write the general solution of Eq. (3) in closed form. In the asymptotic limit $`t_0\mathrm{}`$, it reads

$$\begin{array}{cc}\hfill c_n(t)=\underset{\alpha }{}\underset{0}{\overset{\mathrm{}}{}}& d\tau n|u_\alpha (t)e^{(iϵ_\alpha /\mathrm{}\gamma _\alpha )\tau }u_\alpha ^+(t\tau )|\hfill \\ & \times \left\{|1\xi _L(t\tau )+|N\xi _R(t\tau )\right\}.\hfill \end{array}$$
(8)
To obtain the current $`I_L(t)`$, we insert the operator (8) into Eq. (6) and use the expectation values (5). We then find that the current assumes the commonly expected “scattering form” Datta1995a  but with time-dependent transmission probabilities and, as well, an additional contribution that accounts for a $`𝒯`$-periodic charging of the wire. The latter does not contribute to the time-averaged current $`\overline{I}=_0^𝒯𝑑tI_L(t)/𝒯`$ so that we obtain as a first result

$$\overline{I}=\frac{e}{2\pi \mathrm{}}\underset{k}{}𝑑ϵ\left\{T_{LR}^{(k)}(ϵ)f_R(ϵ)T_{RL}^{(k)}(ϵ)f_L(ϵ)\right\}.$$
(9)
Owing to charge conservation it equals the average current through the right contact. The coefficients

$$T_{LR}^{(k)}(ϵ)=\mathrm{\Gamma }_L\mathrm{\Gamma }_R\left|G_{1N}^{(k)}(ϵ)\right|^2$$
(10)
can be interpreted as the probability that an electron with energy $`ϵ`$ is transmitted from the right lead to the left lead under the absorption of $`k`$ photons, respectively the emission of $`k`$ photons when $`k<0`$. Note that the sum runs over all integers $`k`$ corresponding to different conduction channels that contribute independently to the average current $`\overline{I}`$. The retarded Green function

$$G_{nn^{}}^{(k)}(ϵ)=\underset{\alpha ,k^{}}{}\frac{n|u_{\alpha ,k^{}+k}u_{\alpha ,k^{}}^+|n^{}}{ϵ(ϵ_\alpha +k^{}\mathrm{}\mathrm{\Omega }i\mathrm{}\gamma _\alpha )}$$
(11)
describes the propagation of an electron from orbital $`|n^{}`$ to orbital $`|n`$. We emphasize that generally $`|G_{1N}^{(k)}(ϵ)||G_{N1}^{(k)}(ϵ)|`$ for a driven system. An expression for the time averaged current similar to Eq. (9) has been proposed in Ref. Datta1992a  without providing an explicit form for the Green function in terms of generalized Floquet states.

Next, we address the main topic of this work, namely the current noise given by the auto-correlation function $`S_L(t,\tau )=\frac{1}{2}[\mathrm{\Delta }I_L(t),\mathrm{\Delta }I_L(t+\tau )]_+`$ of the current fluctuation operator $`\mathrm{\Delta }I_L(t)=I_L(t)I_L(t)`$. It can be shown that $`S_L(t,\tau )=S_L(t+𝒯,\tau )`$ shares the time-periodicity of the driving. Therefore, it is possible to characterize the noise level by the time-averaged noise power at zero frequency, $`\overline{S}_L=𝑑\tau _0^𝒯𝑑tS_L(t,\tau )/𝒯`$. Since the total charge is conserved, the zero-frequency noise is identical at both the left and the right contact, i.e. $`\overline{S}_L=\overline{S}_R=\overline{S}`$. After some extensive algebra we obtain our central result

$`\overline{S}={\displaystyle \frac{e^2}{2\pi \mathrm{}}}\mathrm{\Gamma }_L\mathrm{\Gamma }_R{\displaystyle \underset{k}{}}{\displaystyle }dϵ\{`$ $`\mathrm{\Gamma }_L\mathrm{\Gamma }_R\left|{\displaystyle \underset{k^{}}{}}G_{N1}^{(k^{}k)}(ϵ+k\mathrm{}\mathrm{\Omega })G_{N1}^{(k^{})}(ϵ)^{}\right|^2f_L(ϵ)\overline{f}_L(ϵ+k\mathrm{}\mathrm{\Omega })`$
$`+`$ $`|G_{1N}^{(k)}(ϵ+k\mathrm{}\mathrm{\Omega })+i\mathrm{\Gamma }_L{\displaystyle \underset{k^{}}{}}G_{1N}^{(k^{}k)}(ϵ+k\mathrm{}\mathrm{\Omega })G_{11}^{(k^{})}(ϵ)^{}|^2f_L(ϵ)\overline{f}_R(ϵ+k\mathrm{}\mathrm{\Omega })\}`$ (12)
$`+\text{same terms with the replacement }(L,1)(R,N),`$
where we have defined $`\overline{f}_{L/R}=1f_{L/R}`$. The key results (9) and (12) contain as special cases prior findings: In the absence of any driving, the Floquet eigenvalues $`ϵ_\alpha i\mathrm{}\gamma _\alpha `$ reduce to the complex-valued eigenenergies; this implies $`G_{nn^{}}^{(k)}=0`$ for all $`k0`$, yielding the transmission probability for an electron with energy $`E`$ of $`T(E)=\mathrm{\Gamma }_L\mathrm{\Gamma }_R|G_{N1}^{(0)}(E)|^2`$. Thus, the quantities $`\overline{I}`$ and $`\overline{S}`$ agree with the well-known expressions obtained within the time-independent, non-driven scattering approach Blanter2000a . In the limit of a weak system-lead coupling but arbitrary driving strength, the average current (9) coincides also with the corresponding result of a recent master equation approach Lehmann2002b .

Current and noise suppression.—As a simple, yet nontrivial application, we consider a wire composed of $`N`$ orbitals as sketched in Fig. 1. Each orbital is coupled to its nearest neighbors by a hopping matrix element $`\mathrm{\Delta }`$. The on-site energies are modulated by the influence of the ac-field, $`H_{nn}(t)=E_nA\mathrm{cos}(\mathrm{\Omega }t)(N+12n)/2`$, $`n=1,\mathrm{},N`$. The energy $`A`$ equals the electric field strength multiplied by the electron charge $`e`$ and the distance between two neighboring sites. The wire is assumed to couple equally to both leads, $`\mathrm{\Gamma }_L=\mathrm{\Gamma }_R=\mathrm{\Gamma }`$, and the laser frequency is far off resonance, $`\mathrm{\Omega }=5\mathrm{\Delta }/\mathrm{}`$. For a molecular wire, a typical value for the hopping matrix element $`\mathrm{\Delta }`$ and the coupling strength $`\mathrm{\Gamma }`$ is $`0.1`$eV leading to a current unit $`e\mathrm{\Gamma }/\mathrm{}25\mu \mathrm{A}`$, while the laser frequency lies in the optical regime. For a distance of $`2`$Å between two neighboring sites, a driving amplitude $`A=\mathrm{\Delta }`$ corresponds to an electric field strength of roughly $`5\times 10^6\mathrm{V}/\mathrm{cm}`$. For the evaluation of the current $`\overline{I}`$ and the noise $`\overline{S}`$, we restrict ourselves to zero temperature. Then, the Fermi functions turn into step functions and the energy integrals in Eqs. (9) and (12) can be carried out analytically. This limit is physically well justified for molecular wires at room temperature and for quantum dots at helium temperature since in both cases, thermal electron excitations do not play a significant role.

Figure 2a depicts the dc-current and the zero-frequency noise for a wire with $`N=3`$ sites with equal on-site energies and a relatively large applied voltage. As a remarkable feature, we find that for certain values of the field amplitude $`A`$, the current drops to a value of some percent of the current in the absence of the field Lehmann2002c . A perturbation theory for the Floquet equation (7) for $`\mathrm{\Delta },\mathrm{\Gamma }\mathrm{}\mathrm{\Omega }`$ yields that the driving results in a renormalized hopping matrix element $`\mathrm{\Delta }\mathrm{\Delta }_{\mathrm{eff}}=\mathrm{\Delta }J_0(A/\mathrm{}\mathrm{\Omega })`$, where $`J_0`$ denotes the zeroth-order Bessel function. Then, $`G_{1N}`$ and $`G_{N1}`$ vanish if the condition $`J_0(A/\mathrm{}\mathrm{\Omega })=0`$ is fulfilled Grossmann1992a . Consequently, the dc-current (9) and the zero-frequency noise (12) also vanish.

The relative noise strength can be characterized by the so-called Fano factor $`F=\overline{S}/e|\overline{I}|`$ depicted in Fig. 2b. Interestingly enough, we find that the Fano factor exhibits as a function of the driving amplitude $`A`$ both a sharp maximum at current suppression and two pronounced minima nearby. For a sufficiently large voltage, the Fano factor assumes at the maximum the value $`F1/2`$. Once the driving amplitude is of the order of the applied voltage, however, the Fano factor becomes much larger. The relative noise minima are distinct and provide a typical Fano factor of $`F0.15`$. Reducing the coupling to the leads renders these phenomena even more pronounced since then the suppressions occur in a smaller interval of the driving amplitude, cf. Fig. 2b. The overall behavior is robust in the sense that approximately the same values for the minima and the maximum are also found for larger wires, different driving frequencies, different coupling strengths, and slightly modified on-site energies, provided that $`\mathrm{\Delta },\mathrm{\Gamma },E_n\mathrm{}\mathrm{\Omega }`$ and that the applied voltage is sufficiently large. The qualitative behavior can again be understood within a perturbative approach. With increasing driving amplitude, a crossover from $`\mathrm{\Delta }_{\mathrm{eff}}\mathrm{\Gamma }`$ to $`\mathrm{\Delta }_{\mathrm{eff}}\mathrm{\Gamma }`$ at the current suppression occurs. Both limits correspond to the transport through a symmetric double barrier and, therefore, are characterized by $`F1/2`$ Blanter2000a . At the crossover $`\mathrm{\Delta }_{\mathrm{eff}}\mathrm{\Gamma }`$ the effective barriers vanish and, consequently, the Fano factor assumes its minimum.

In summary, we have put forward with Eqs. (9) and (12) new and appealing expressions for the time-averaged current and the zero-frequency noise for the electron transport through ac-driven nanoscale systems. A main finding is that in molecular wires and coherently coupled quantum dots, the influence of an ac-field can be used to selectively suppress both the current and its noise. Investigating the relative noise level characterized by the Fano factor has revealed that the current suppression is accompanied by a noise maximum and two remarkably low minima. These phenomena can be used to devise novel current sources with a priori controllable noise levels.

We thank G.-L. Ingold for helpful discussions. This work has been supported by the Volkswagen-Stiftung under Grant No. I/77 217, a Marie Curie fellowship of the European community program IHP under contract No. HPMF-CT-2001-01416 (S.C.), and the DFG Sonderforschungsbereich 486.