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# JETP Letters, Vol. 75, No. 2, 2002, pp. 93-97. Coherent Tunneling between Elementary Conducting Layers in the NbSe3 Charge-Density-Wave Conductor

## Abstract

Characteristic features of transverse transport along the $`a^{}`$ axis in the NbSe3 charge-density-wave conductor are studied. At low temperatures, the $`I`$-$`V`$ characteristics of both layered structures and NbSe3-NbSe3 point contacts exhibit a strong peak of dynamic conductivity at zero bias voltage. In addition, the $`I`$-$`V`$ characteristics of layered structures exhibit a series of peaks that occur at voltages equal to multiples of the double Peierls gap. The conductivity behavior observed in the experiment resembles that reported for the interlayer tunneling in Bi-2212 high-$`T_c`$ superconductors. The conductivity peak at zero bias is explained using the model of almost coherent interlayer tunneling of the charge carriers that are not condensed in the charge density wave.

It is well known that the crystal structure of BSCCO high-$`T_c`$ superconductors consists of atomically thin superconducting cuprate layers spatially separated by atomically thin insulating layers of BiO and SrO. The corresponding spatial modulation of the superconducting order parameter in the direction across the layers (along the $`c`$ axis) leads to a discrete description of the transverse transport (the Lawrence-Doniach model 1 ) with the neighboring superconducting layers being coupled through Josephson tunneling junctions. The validity of this approach is confirmed by the results of the experiments on natural Bi-2212 layered structures of small lateral size 2 ; 3 . Currently, the study of the interlayer tunneling of Cooper pairs and quasiparticles 4 ; 5  is one of the new original methods for investigating high-$`T_c`$ superconductors.

In this paper, we study the interlayer tunneling in a layered system with an electron condensate of a different type, namely, in a charge-density-wave (CDW) conductor. The material chosen for our experiments is NbSe3. This compound is characterized by two Peierls transitions, which occur at the temperatures $`T_{p1}=`$145 K and $`T_{p2}=`$59 K. In the low-temperature Peierls state, the Fermi surface retains some regions where the nesting conditions are not satisfied (the pockets ) and, hence, the Peierls gap is absent. Therefore, NbSe3 does not undergo transition to the insulating state and retains metallic properties down to the lowest temperatures 6 . From the analysis of both the crystal structure of NbSe3 and the anisotropy of its properties, it follows that this material can be classed with quasi-two-dimensional layered compounds. In fact, its conductivity anisotropy in the ($`bc`$) plane is determined by the chain conductivity along the $`b`$ axis and is estimated as $`\sigma _b/\sigma _c10`$, whereas the conductivity ratio $`\sigma _b/\sigma _a^{}`$ is determined by the layered character of the structure and reaches the values $`10^4`$ at low temperatures 7 ; 8 . Figure 1a shows the crystal structure of NbSe3 in the ($`ac`$) plane. One can see that, in this material, the layered structure is formed as a result of a pairwise coordination of selenium prisms with the predominant orientation of their bases in the ($`bc`$) plane. In Fig. 1b, the shaded areas indicate the elementary conducting layers in which the prisms are rotated and shifted with their edges toward each other. In these layers, the distances between the niobium chains are relatively small, whereas the neighboring conducting layers are separated by an insulating layer formed as a double barrier by the bases of the selenium prisms.

This type of layered structure in combination with the conductivity anisotropy offers the possibility for the CDW condensation in the elementary conducting layers spatially separated by atomically thin insulating layers. In this case, as in layered high-$`T_c`$ superconductors, one can expect that the CDW order parameter will be modulated along the $`a^{}`$ axis, and the transport across the layers will be determined by the intrinsic interlayer tunneling between the elementary layers with the CDW.

To verify these speculations, we carried out an experimental study of the transport across the layers in NbSe3 in the condensed CDW state.

The samples used in the experiment were layered structures with a small area through which the current flows across the layers, $`S=2\times 2`$ $`\mu `$m2, and with the number of elementary layers $``$30 (the overlap junctions). They were made from a thin NbSe3 single crystal by the focused ion beam processing technique developed for fabricating similar structures from Bi-2212 9 . Schematically, the structure under investigation is shown in the inset of Fig. 2. In addition, we studied the characteristics of NbSe3-NbSe3 point contacts oriented in the direction of the $`a^{}`$ axis. The configuration of such a contact is shown in the inset of Fig. 3. The contact was formed directly at low temperature by bringing two NbSe3 whiskers together with high accuracy. In both cases, we performed four-terminal measurements of the $`I`$-$`V`$ characteristics and their derivatives at low temperatures, i.e., below the second Peierls transition $`T_{p2}=59`$ K.

The main results of the experiment are shown in Fig. 2, which, for one of the virtually perfect structures (No. 3), displays the dynamic conductivity along the $`a^{}`$ axis versus the bias voltage $`V`$ at different temperatures from 59.5 to 4.2 K. It can be seen that, for $`T<T_{p2}`$, the differential $`I`$-$`V`$ characteristics are of a tunneling character. When the temperature decreases below $``$35 K, the $`I`$-$`V`$ characteristics begin to exhibit a conductivity peak at zero bias voltage. As the temperature decreases further, this peak becomes a dominant feature. The peak amplitude reaches saturation when the temperature decreases below 6-8 K, and at $`T`$ = 4.2 K, it is almost 20 times as great as the conductivity observed at high bias voltages. Note that this anomaly cannot be attributed to Joule heating. The estimate of the sample heating for a typical value of heat transfer to helium yields a conductivity decrease of less than 10% for the whole range of measured voltages. In addition, the $`I`$-$`V`$ characteristics show a clearly defined set of conductivity peaks that are symmetric about zero voltage and at low temperature correspond to $`|V|=`$50, 100, and 150 mV, i.e., to $`|V|=nV_0`$, where $`V_0=`$ 50 mV and $`n`$= 1,2, 3. As the temperature increases above 25 K, these peaks move to lower energies, and, at the temperature $`T`$59 K corresponding to the second Peierls transition for NbSe3, the values of $`V_n`$ vanish.

The picture described above was observed only for perfect structures. The presence of structure defects, such as a twin boundary, leads to a considerable reduction of the conductivity peak at zero bias and to the appearance of a peak at $`V=`$ 25-27 mV $`V_0/2`$ (curve 2 in Fig. 3). Qualitatively similar dependences were observed for some of the NbSe3-NbSe3 point contacts. Their $`I`$-$`V`$ characteristics also exhibit a conductivity peak at zero bias with an amplitude approximately equal to that observed for defect overlap junctions, as well as a conductivity peak at $`V`$ 25 mV (curve 1 in Fig. 3). Figure 4 presents the temperature dependences of the normalized dynamic conductivity at zero bias voltage for all types of samples studied in the experiment. One can see that, for a perfect overlap junction, the amplitude of the zero bias anomaly is more than three times greater than the amplitudes observed for the defect layered structures and point contacts. Note that the voltage value $`V_0=`$ 50 mV is close to twice the value of the low-temperature energy gap, $`2\mathrm{\Delta }_{p2}/e`$, for NbSe3 10 ; 11 , while the dependence $`V_n(T)/V_n(0)`$ obtained for both overlap junctions and point contacts (Fig. 5) agrees well with the temperature dependence of the energy gap predicted by the BCS theory (the dashed line in Fig. 5). This result suggests that the conductivity features observed in the experiment are governed by a gap mechanism.

It is important to note that all effects described above were observed exclusively for the transport across the layers (along the $`a^{}`$ axis). The extra experiments performed by us on specially fabricated bridges and point contacts oriented along the $`c`$ axis (with the transport across the chains in the layer plane) showed no conductivity peak at $`V=0`$.

Let us first analyze the results obtained for perfect overlap junctions. The most prominent feature of the $`I`$-$`V`$ characteristics of these structures is the strong conductivity peak at zero bias voltage. In addition, the characteristics exhibit a periodic sequence of peaks at $`|V|=nV_0`$, which resembles the series of quasiparticle branches observed in the $`I`$-$`V`$ characteristics of Bi-2212 layered structures when the measurements are performed across the layers 3 . As was noted above, the value $`V_0=`$ 50 mV is close to twice the value of the low temperature CDW gap in NbSe3, and the temperature dependence $`V_0(T)`$ follows the prediction of the BCS theory. However, in contrast to the case of a superconductor, the conductivity observed for NbSe3 at zero bias voltage is finite. This fact suggests that the interlayer conduction at zero bias does not originate from the collective CDW contribution of the Josephson tunneling type.

The conductivity peak observed at zero bias cannot be explained by the regular (incoherent) single-particle tunneling as well. If this were the case, the conductivity peak could be attributed to the energy dependence of the density of states of electrons that are not condensed in the CDW. Then, the conductivity feature under discussion should also be observed for N-I-CDW tunnel junctions. However, no such effects were revealed by the detailed experimental studies of this kind of tunnel junctions oriented along the $`a^{}`$ axis 10 ; 11 .

We believe that the conductivity peak at zero bias is caused by the coherent interlayer tunneling of the charge carriers localized in the pockets of the Fermi surface, and below we thoroughly substantiate this statement.

In the general case, the tunnel current between two nonsuperconducting layers, $`a`$ and $`b`$, is described by the expression 12 :

$$I=\frac{4\pi es}{\mathrm{}}\underset{𝐩,𝐪}{}|t_{ab}(𝐩,𝐪)|^2_{\mathrm{}}^+\mathrm{}𝑑\omega \left(\mathrm{tanh}\frac{\omega }{\text{2T}}\mathrm{tanh}\frac{\omega \text{eV}}{\text{2T}}\right)\mathrm{Im}G_a^R(𝐩,\omega )G_b^R(𝐪,\omega \text{eV}),$$
(1)
where $`G^R`$ is the retarded Green function of an electron with the momentum $`𝐩`$ in the layer $`a`$, $`\mathrm{Im}G^R(𝐩,\omega )`$ is the spectral density of the Green function, $`t_{ab}(𝐩,𝐪)`$ is the matrix element characterizing the tunneling from the state with the momentum $`𝐩`$ in the layer $`a`$ to the state with the momentum $`𝐪`$ in the layer $`b`$, $`V`$ is the voltage between the adjacent layers, and $`T`$ is the temperature.

Note that the contribution of the collective (moving) CDW mode 13  to the interlayer tunneling is absent, because the tunnel current is determined by the Green functions in different layers, whereas the collective mode propagates within the layers.

Below, we consider the coherent tunneling, when the electron momentum in the plane does not change under the tunneling: $`𝐩=𝐪`$. Then, we have

$$I=\frac{es}{\pi \mathrm{}}𝑑𝐩|t_{ab}(𝐩)|^2_{\mathrm{}}^+\mathrm{}𝑑\omega \left(\mathrm{tanh}\frac{\omega }{\text{2T}}\mathrm{tanh}\frac{\omega \text{eV}}{\text{2T}}\right)\mathrm{Im}G_a^R(𝐩,\omega )G_b^R(𝐩,\omega \text{eV})$$
(2)
Taking into account that the scattering in a layer is determined by the collision frequency $`\nu `$, we obtain

$$\mathrm{Im}G^R(𝐩,\omega )=\frac{\gamma }{\pi (\omega ϵ(𝐩)^2+\gamma ^2)}$$
(3)
where $`ϵ(𝐩)`$ is the electron spectrum and $`\gamma =\mathrm{}\nu `$. We can use this expression with $`\gamma =\gamma _{sc}+\gamma _{inc}`$, which takes into account the change in the momentum because of the scattering within the layers and the change due to the tunneling $`\gamma _{inc}=ϵ(𝐩)ϵ(𝐪)`$. In both cases, we take into account the energy uncertainty for the state characterized by the momentum $`𝐩`$. We define the tunneling as almost coherent when $`\gamma _{inc}`$ and $`\gamma `$ are small relative to other energy parameters of the electron system. In our case, such parameters are the Peierls gap and the width of the electron band in the pockets. Replacing $`t_{ab}(𝐩)`$ by the momentum-independent quantity $`t`$ and integrating with respect to $`𝐩`$, we obtain

$$\frac{1}{4\pi ^2}𝑑𝐩|t_{ab}(𝐩)|^2\mathrm{Im}G_a^R(𝐩,\omega )\mathrm{Im}G_b^R(𝐩,\omega \text{eV})=\frac{2\gamma N(0)|t|^2}{e^2V^2+4\gamma ^2}$$
(4)
where $`N(0)`$ is the density of states of electrons in the pockets. Finally, for the interlayer current when $`eV<2\mathrm{\Delta }`$, we obtain the expression

$$I(V)=\frac{eV\gamma N(0)|t|^2}{2\pi ^3(e^2V^2+4\gamma ^2)}$$
(5)
and the dynamic conductivity has the form

$$\frac{\sigma (V)}{\sigma (0)}=4\gamma ^2\frac{4\gamma ^2e^2V^2}{(e^2V^2+4\gamma ^2)^2}$$
(6)
Note that the temperature dependence is present in $`\gamma (T)`$ only. One can see that the dynamic conductivity has a peak of width $`\gamma `$ at $`V`$ = 0 and becomes negative and unstable when $`eV>2\gamma `$. For a thirty-layer structure, the experimentally observed peak width $``$10 mV corresponds to $`\gamma `$ 0.3 meV. For comparison, we estimate the parameter $`\gamma _{sc}`$ characterizing the scattering within the layers. Using the known mobility data $`\mu =e/\nu _{sc}m^{}4\times 10^4`$ cm2/Vs 7 ; 14 , where $`m^{}=0.24m_e`$ 15 , we obtain $`\gamma _{sc}0.13`$ meV; i.e., the changes in the electron momentum because of tunneling are approximately equal to changes caused by the scattering within the layers.

Now, we explain why the interlayer current decreases with increasing voltage V. The electron tunneling between the layers must obey the energy conservation law; i.e., $`ϵ(𝐩)=ϵ(𝐪)eV`$ to within $`2\gamma `$. For coherent tunneling, we have $`ϵ(𝐩)=ϵ(𝐪)`$, and for $`eV\gamma `$, tunneling is possible and we have the conventional Ohm’s law. When $`eV>2\gamma `$, tunneling is impossible up to the voltage $`V`$ reaching $`2\mathrm{\Delta }/e`$. In this case, electrons condensed in the CDW begin to contribute to the interlayer current in the form of a regular tunneling of CDW quasiparticles through the double Peierls gap $`2\mathrm{\Delta }`$. Thus, the interlayer current can be realized by means of only one of the two aforementioned mechanisms. In an actual multilayer structure, because of the geometric nonuniformity of individual layers (the areas of the layers are somewhat different), the voltage value $`V2\gamma /e`$ will not be reached simultaneously for different individual tunneling junctions. When $`V>2\gamma /e`$, some of the junctions can be in the coherent tunneling regime whereas other junctions can be in the regime of single-particle tunneling through the gap. As a result, a sequence of conductivity peaks must appear in the $`I`$-$`V`$ characteristic of the compound under study at the voltages $`V=2n\mathrm{\Delta }_p/e`$, where $`n`$ = 1, 2, $`\mathrm{}`$.

In the presence of defects in an overlap junction or in the case of a point contact, the incoherence of tunneling is enhanced, although in the best structures the tunneling remains almost coherent. Therefore, the $`I`$-$`V`$ characteristics of these structures, along with the conductivity peak at zero bias, contain an additional feature at $`V=\mathrm{\Delta }_p/e`$, which is related to the single-particle tunneling of the N-I-CDW type.

Thus, the results of this study show that the interlayer tunneling in natural layered structures obtained from NbSe3 represents an independent efficient method for investigating the Peierls state in this compound. The tunneling conductivity peak observed at zero voltage can be self-consistently explained by the almost coherent interlayer tunneling of charge carriers that are not condensed in the CDW and are localized in the Fermi surface pockets not covered by the gap. The series of equidistant peaks in the $`I`$-$`V`$ characteristic can be explained by the quasiparticle tunneling through the CDW gap under sequential transitions of individual tunneling junctions to the resistive state. Note that the conductivity peak observed at zero bias is a unique manifestation of coherent single-particle transport in solids.

We are grateful to S.A. Brazovskii, V.A. Volkov, and V.M. Yakovenko for useful discussions. This work was supported by the Russian Foundation for Basic Research (project nos. 99-02-17364, 01-02-16321, and 00-02-22000 CNRS), the state program Physics of Solid Nanostructures (project no. 97-1052), the NWO Russian-Netherlands Project, and the Los Alamos National Laboratory with the support of US DOE.


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# A Steady State Model for Graph Power Laws

## 1 Introduction

The growth of the World Wide Web (WWW) has been explosive and phenomenal. Google  has more than $`2`$ billion pages searched as of February $`2002`$. The Internet Archive  has $`10`$ billion pages archived as of March $`2001`$. The existing growth-based models  are adequate to explain the web’s current graph structure. It would be interesting to know if a different model will be needed as the web’s growth rate slows down  while its link structure continues to evolve.

### 1.1 Why Power Laws?

Barabási et al.  and Medina et al.  stated that preferential connectivity and incremental growth are both required for the power law distribution observed in the web. The importance of the preferential connectivity has been shown by several researchers .

Faloutsos et al.  observed that the internet topology exhibits power law distribution in the form of $`y=x^\alpha `$. When studying web characteristics, the documents can be viewed as vertices in a graph and the hyper-links as edges between them. Various researchers  have independently showed the power law distribution in the degree sequence of the web graphs. Huberman and Adamic  showed a power law distribution in the web site sizes. See  for a summary of works on web graph structure.

Medina et al.  showed that topologies generated by two widely used generators, the Waxman model , and the GT-ITM tool , do not have power law distribution in their degree sequences. Palmer and Steffan  proposed a power law degree generator that recursively partitions the adjacency matrix into an $`80`$-$`20`$ distribution. However, it is unclear if their generator actually emulates other web properties.

The power law distribution seems to be an ubiquitous property. The power law distribution occurs in epidemiology , population studies , genome distribution , various social phenomena , and massive graphs . For the power law graphs in biological systems, the connectivity changes appear to be much more important than growth in size due to the long time-scale of biological evolution.

### 1.2 Properties for Graph Model Comparison

Another important web graph property that has been looked at is diameter. However, there are conflicting results in the published papers. Albert et al.  stated that web graphs have the small world phenomenon , in which the diameter $`\mathrm{\Delta }`$ is roughly $`0.35+2.06\mathrm{lg}n`$, where $`n`$ is the size of the web graph. For $`n=8\times 10^8`$, $`\mathrm{\Delta }19`$. Lu  proved the diameters of random power law graphs are logarithmic function of $`n`$ under the model proposed by Aiello et al. . However, Broder et al.  showed that, over $`75\%`$ of the time, there is no directed path between two random vertices. If there is a path, the average distance is roughly $`16`$ when viewing web graph as directed graph or $`6.83`$ in the undirected case.

Currently, there are few theoretical graph models  for generating power law graphs. There are very few comparative studies that would allow us to determine which of these theoretical models are more accurate models of the web. We only know that the model proposed by Kumar et al.  generates more bipartite cliques than other models. They believe clustering to be an important part of web graph structures that was insufficiently represented in previous models .

### 1.3 New Contributions

In this paper, we show power law graphs do not require incremental growth, by developing a graph model which (empirically) results in power laws by evolving a graph according to a Markov process while maintaining constant size and density.

We also describe an easily computable graph property that can be used to capture cluster information in a graph without enumerating all possible subgraphs. We use this property to compare our model with others and with actual web data.

## 2 Steady State Model

Our $`SteadyState`$ (SS) model is very simple in comparison with other web graph models . It consists of repeatedly removing and adding edges in a sparse random graph $`G`$.

Let $`m`$ be $`\mathrm{\Theta }(n)`$. We generate an initial sparse random graph $`G`$ with $`m`$ edges and $`n`$ vertices, by randomly adding edges between vertices until we have $`m`$ edges. As discussed below, the initial random distribution of edges is unimportant for our model.

We then iterate the following steps $`r`$ times on $`G`$, where $`r`$ is a parameter to our model.

1. Pick a vertex $`v`$ at random. If there is no edge incident upon $`v`$, we repeat this step until $`v`$ has nonzero degree.
2. Pick an edge $`(u,v)G`$ at random.
3. Pick a vertex $`x`$ at random.
4. Pick a vertex $`y`$ with probability proportional to degree.
5. If $`(x,y)`$ is not an edge in $`G`$ and $`x`$ is not equal to $`y`$, then remove edge $`(u,v)`$ and add edge $`(x,y)`$.

One can view our model as an aperiodic Markov chain with some limiting distribution. If we repeat the above steps long enough, the random graphs generated by this model will be close to this limiting distribution, no matter what the initial random sparse graph is. Note that unlike other models , the graphs generated by our model do not contain self-loops nor multiple edges between two vertices.

Barabási et al.  also proposed a non-growth model, which failed to produce a power law distribution. Both models have preferential connectivity features. However, there are several differences between our model and theirs. First, our edge set is fixed and the initial graph is generated via classical random graph models . Second, our model has “rewiring” feature similar to one in the small world model .

### 2.1 Simulation Results

We simulated our model on graphs of different sizes, $`(500n5000)`$, and densities $`\frac{m}{n}`$, $`(1\frac{m}{n}3)`$. We repeated each simulation $`5`$ times, and performed $`r=10000000`$ edge deletion/insertion operations on each graph. The vertices’ degree distributions appear to converge to power law distributions as the number of edge deletion/insertion operations increases. Some of our simulation results are shown in Figures 1 \- 4. Figures 1 and 3 show degree distributions at various stage of simulations. Figures 2 and 4 show degree distributions for graphs with different densities $`\frac{m}{n}`$.

## 3 Cluster Information

Given a subgraph $`S`$ of $`G`$, $`d_S(v)`$ is the degree for vertex $`v`$ in $`S`$. Here we examine the maximum degree $`d_{\mathrm{m}ax}`$ in all subgraphs, which is defined as

$$d_{\mathrm{m}ax}=\mathrm{m}ax_S\mathrm{m}in_{vS}d_S(v).$$

We use $`d_{\mathrm{m}ax}^M`$ to denote the value obtained under graph model $`M`$.

To compute $`d_{\mathrm{m}ax}`$ for a graph $`G`$, we perform the following steps until $`G`$ becomes empty:

1. Select a minimum degree vertex $`v`$ from $`G`$.
2. Set $`d_{\mathrm{m}ax}`$ to $`d(v)`$ if $`d(v)>d_{\mathrm{m}ax}`$.
3. Remove vertex $`v`$ and its edges from $`G`$.

The above steps correctly compute $`d_{\mathrm{m}ax}`$ because we cannot remove any vertices of $`S`$ until the degree of the current subgraph reaches $`d_{\mathrm{m}ax}`$. The minimal degree elimination sequence for graph in Figure 5 will be $`B,C,A,D,`$ and $`E`$. The degrees when those vertices got eliminated are $`1,1,2,1,`$ and $`1`$. $`d_{\mathrm{m}ax}`$ is $`2`$ since $`\mathrm{m}ax\{1,1,2,1,1\}=2`$ .

###### Observation 1

For any model $`M`$ that constructs a graph by adding a vertex at a time, and for which each newly added vertex has the same degree $`d=\frac{m}{n}`$, $`d_{\mathrm{m}ax}^M=d`$.

Thus the Barabási and Albert model (BA)  or the linear growth copying model in  have the same value for $`d_{\mathrm{m}ax}`$ for graphs of all sizes once $`d=\frac{m}{n}`$ is fixed.

###### Observation 2

The web graph generated by the linear model has minimum vertex degree of $`d=\frac{m}{n}`$.

Hence, the linear model may not encapsulate all the crucial properties in a web graph if there are significant numbers of vertices with degree less than $`\frac{m}{n}`$.

### 3.1 Web Crawl and Simulation Data

We performed a web crawl on various Computer Science department web sites. We then used the $`ACL`$ model  to generate new graphs from degree sequences in the actual web graphs. We also ran the $`SS`$ model using $`n`$ and $`m`$ values from the actual web graphs with $`10000000`$ edge insertion/deletion steps. For each graph, we run both models $`5`$ times. The following table shows the means $`\mu `$ and the standard deviations $`\sigma `$ for $`d_{\mathrm{m}ax}`$ values using the $`ACL`$ model and the $`SS`$ model.

| Site | $`n`$ | $`m`$ | $`d_{\mathrm{m}ax}`$ | $`\mu _{ACL}`$ | $`\sigma _{ACL}`$ | $`\mu _{SS}`$ | $`\sigma _{SS}`$ |
| --- | --- | --- | --- | --- | --- | --- | --- |
| arizona | 5315 | 16892 | 15 | 10 | 0 | 8 | 0 |
| berkeley | 2826 | 22957 | 45 | 21.6 | 0.547 | 16 | 0 |
| caltech | 622 | 4830 | 7 | 5.8 | 0.447 | 12.8 | 0.447 |
| cmu | 2052 | 23821 | 57 | 37.2 | 0.447 | 20 | 0.707 |
| cornell | 7145 | 14919 | 17 | 19.4 | 0.547 | 6 | 0 |
| harvard | 915 | 9327 | 21 | 12.6 | 0.894 | 16.4 | 0.547 |
| mit | 4861 | 15360 | 31 | 24.4 | 0.547 | 7 | 0 |
| nd | 1913 | 16328 | 33 | 29.2 | 0.447 | 15.4 | 0.547 |
| stanford | 2553 | 25693 | 27 | 14.6 | 0.547 | 18.4 | 0.547 |
| ucla | 2718 | 19755 | 22 | 16.6 | 0.547 | 14.2 | 0.447 |
| ucsb | 5236 | 10338 | 22 | 13.8 | 0.447 | 5 | 0 |
| ucsd | 553 | 3885 | 15 | 7.2 | 0.447 | 11.8 | 0.447 |
| uiowa | 1410 | 12258 | 8 | 8.8 | 0.447 | 15.2 | 0.447 |
| uiuc | 5623 | 28872 | 29 | 21 | 0 | 11.8 | 0.836 |
| unc | 1465 | 5446 | 17 | 9.8 | 0.447 | 8 | 0 |
| washington | 7001 | 24901 | 17 | 12 | 0 | 9 | 0 |

Table $`1`$: $`d_{\mathrm{m}ax}`$ from Actual Web Crawl and Model Simulation

In general, the $`ACL`$ model and the $`SS`$ model are generating less clustered graphs than what we see on actual web graphs. This implies that we need a more detailed model of web graph clustering behavior.

## 4 Conclusion and Open Problems

Previously, researchers have conjectured that preferential connectivity and incremental growth are necessary factors in creating power law graphs. In this paper, we provide a model of graph evolution that produces power law without growth. Our $`SteadyState`$ model is very simple in comparison with other graph models . It also does not require prior degree sequences as in the $`ACL`$ model .

The difficulty in comparing various models  is that each model has different parameters and inputs. Here we provide a simple graph property $`d_{max}`$ that captures the clustering behavior of graphs without complicated subgraph enumeration algorithm. It can be useful in gauging the accuracy of various models.

From our web crawl data, we know that the linear models such as Barabási’s  are not the best ones to use when considering $`d_{\mathrm{m}ax}`$. Both $`ACL`$ and $`SS`$ models are not generating dense-enough subgraphs when comparing against the actual web graphs. Thus, we need a better web graph model that mimics actual web graph clustering behavior.

Here are some of our open problems:

1. Can one prove theoretically that the SS method actually has a power law distribution?
2. How long does it take for our model to reach a steady state?
3. What are other simple web graph properties that we can use to determine the accuracy of various models?
4. Are there any technique such as graph products that we can use to generate realistic massive web graphs in relatively short times?


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# Anisotropic transport in unidirectional lateral superlattice around half-filling of the second Landau level

Also at \]CREST, JST Corporation.

## Abstract

We have observed marked transport anisotropy in short period ($`a`$=92 nm) unidirectional lateral superlattices around filling factors $`\nu `$=5/2 and 7/2: magnetoresistance shows a sharp peak for current along the modulation grating while a dip appears for current across the grating. By altering the ratio $`a/l`$ (with $`l`$=$`\sqrt{\mathrm{}/eB_{}}`$ the magnetic length) via changing the electron density $`n_e`$, it is shown that the $`\nu `$=5/2 anisotropic features appear in the range 6.6$``$$`a/l`$$``$7.2 varying their intensities, becoming most conspicuous at $`a/l`$$``$6.7. The peak/dip broadens with temperature roughly preserving its height/depth up to 250 mK. Tilt experiments reveal that the structures are slightly enhanced by an in-plane magnetic field $`B_{}`$ perpendicular to the grating but are almost completely destroyed by $`B_{}`$ parallel to the grating. The observations suggest the stabilization of a unidirectional charge-density-wave or stripe phase by weak external periodic modulation at the second Landau level.

It has been known for some time that the second ($`N`$=1) Landau level (LL) exhibits enigmatic even denominator fractional quantum Hall effect (FQHE) Willett et al. (1987); Sarma and Pinczuk (1997) at half-filling (filling factors $`\nu `$=5/2 and 7/2). Interestingly, the state at these filling factors is qualitatively different either from that for the lowest ($`N`$=0) or for the higher ($`N`$$``$2) LL’s. The state at the half-filled lowest LL ($`\nu `$=1/2, 3/2) is now well established to be described by the Fermi sea of composite Fermions.Sarma and Pinczuk (1997) On the other hand, the ground state of higher LL’s near half-filling is predicted to be a unidirectional charge-density-wave (CDW) or stripe phase by Hartree-Fock calculations,Koulakov et al. (1996); Fogler et al. (1996); Moessner and Chalker (1996) which has been supported by a number of recent theories.Rezayi et al. (1999); Maeda (2000); Shibata and Yoshioka (2001) Experimentally, ultrahigh mobility ($`\mu `$$``$1000 m2/Vs) two-dimensional electron gas (2DEG) at low temperatures ($`T`$$``$ 150 mK) displays strong transport anisotropy at $`\nu `$=9/2, 11/2, 13/2,…, between $``$110$``$ and $``$1$`\overline{1}`$0$``$ axes of the host crystal.Lilly et al. (1999a); Du et al. (1999) It is now widely believed that the transport anisotropy is related to CDW phase, although the key factor connecting the stripe and the crystal axes still remains to be uncovered.Willett et al. (2001); Cooper et al. (2001)

Returning back to the second LL, $`\nu `$=5/2 (and 7/2) FQHE is known to be quite fragile, having a small activation energy gap, observable only for 2DEG with reasonably high mobility at very low temperatures ($`T`$$``$100 mK) Willett et al. (1987); Eisenstein et al. (1990); Pan et al. (1999a) and to collapse in tilted magnetic fields.Eisenstein et al. (1988, 1990) Moreover, it has recently been reported that an in-plane magnetic field $`B_{}`$ turns the *isotropic* FQHE state into an anisotropic state similar to those observed at higher LL’s, with current parallel to $`B_{}`$ giving the resistivity maxima.Pan et al. (1999b); Lilly et al. (1999b) The role played by $`B_{}`$ in the drastic transition of the $`\nu `$=5/2 and 7/2 states is not exactly established yet. The most probable picture however seems to be alteration by $`B_{}`$ of Haldane’s pseudopotential components.Morf (1998); Rezayi and Haldane (2000) (Zeeman effect has been experimentally shown to make only small, if any, contribution.Pan et al. (2001)) Whatever the role may be, the effect of $`B_{}`$ on 2DEG is generally believed to be not so large. Therefore the two states are expected to have only small energy difference. (Two-dimensional hole system exhibits anisotropic transport at $`\nu `$=5/2 without tilting,Shayegan et al. (2000) demonstrating the subtleness of the difference.) This in turn suggests the possibility of an alternative way to the transition.

The period $`a_{\mathrm{CDW}}`$ of CDW is theoretically predicted to be about 4$``$8 times the magnetic length $`l=\sqrt{\mathrm{}/eB_{}}`$ depending on the Landau index $`N`$.Fogler et al. (1996); Koulakov et al. (1996); Jungwirth et al. (1999); Stanescu et al. (2000) In the magnetic field range of interest, $`a_{\mathrm{CDW}}`$$``$ 30$``$150 nm. If a 2DEG has a tendency toward spontaneously forming CDW with a period $`a_{\mathrm{CDW}}`$, it will undoubtedly show strong response to the external modulation having a period close to $`a_{\mathrm{CDW}}`$.Rezayi et al. (1999) Along the same line of thought, we investigated the behavior around $`\nu `$=9/2 of unidirectional lateral superlattices (LSL) with periods $`a`$=92 and 115 nm.Endo and Iye (2001) We identified small anisotropic features in magnetoresistance traces, which possibly reflect the response of CDW to the modulation. However the observed features were too small to be decisive. In the present paper, we focus on the second LL. We report qualitatively similar, but much more intense, anisotropic features at $`\nu `$=5/2 (and 7/2) for $`a`$=92 nm LSL (see, e.g., Fig. 1). We have also observed sharp peaks at higher LL’s up to $`\nu `$=25/2 for current along the grating (qualitatively similar as regard the direction of the current and grating), which will be reported in detail elsewhere. In the case of the $`N=1`$ LL, the expected role of external modulation is two-fold: to make the anisotropic state energetically favorable than the isotropic state noe  — the role played by $`B_{}`$ in the case of ultrahigh mobility plain 2DEG —, and to assist the CDW to form and/or align itself, which would otherwise be obstructed by the impurities in moderate-mobility 2DEG. The observation of anisotropic transport features suggests that the external modulation *do* play the expected roles. The observed peaks/dips are much more distinct than before Endo and Iye (2001) due presumably to optimization of the ratio $`a/l`$ and also to the expansion of energy scale by larger magnetic field. Two new attempts are made in the present study: (1) samples with square geometry are used instead of Hall bars and (2) the ratio $`a/l`$=$`a\sqrt{2\pi n_e/\nu }`$ for a given $`\nu `$ is tuned by varying the electron density $`n_e`$ through infrared LED illumination. Square geometry has an advantage of allowing measurement of anisotropy within a *single* LSL sample. This is quite important since it is nearly impossible to prepare two exactly identical Hall bars differing only in the orientation of the grating;Endo and Iye (2001) the smallest disparity in $`n_e`$ can deteriorate the strict comparison. To achieve maximum response, it is desirable to make $`a`$ as close to $`a_{\mathrm{CDW}}`$ as possible. Since $`a`$ is fixed once a sample is prepared, we tuned $`l`$=$`\sqrt{\nu /2\pi n_e}`$ instead, to which $`a_{\mathrm{CDW}}`$ is predicted to be related.

The lower inset of Fig. 1 depicts the schematic of the sample. A square mesa (40$`\times `$40 $`\mu `$m2) with eight arms (width 4 $`\mu `$m) is lithographically defined out of conventional GaAs/AlGaAs single heterostructure 2DEG ($`\mu `$$``$75 m2/Vs and $`n_e`$$``$1.97$`\times `$1015 m-2 before illumination). A grating ($`a`$=92 nm) of electron-beam resist was placed on the square to introduce potential modulation through strain-induced piezoelectric effect as before.Endo et al. (2000); Endo and Iye (2001); Endo et al. (2001) The modulation amplitude is estimated from the low-field commensurability magnetoresistance oscillation to be $``$0.015 meV,Endo et al. (2001) which is quite small but still much larger than the native anisotropy energy of $``$1 mK per electron estimated in ultrahigh mobility plain 2DEG.Cooper et al. (2001) It can readily be seen that $`I_{15}`$-$`V_{24}`$ or $`I_{15}`$-$`V_{86}`$ ($`I_{37}`$-$`V_{28}`$ or $`I_{37}`$-$`V_{46}`$) mainly measures resistivity component parallel (perpendicular) to the grating, where $`I_{ij}`$-$`V_{kl}`$ denotes the probe configuration using arms $`i,j`$ as source/drain and $`k,l`$ as voltage probes. It has been pointed out that the square geometry exaggerates the anisotropy due to current-path effect.Simon (1999); Endo and Iye (2002) However, since it is not our purpose to quantify the anisotropy, the property is rather advantageous bringing small anisotropy into light. The grating is placed with their stripes parallel either to $``$110$``$ or to $``$1$`\overline{1}`$0$``$ axis in order to maximize the piezoelectric effect.Skuras et al. (1997) Although we mainly discuss the former arrangement in the following, both directions of the grating give the consistent results not  confirming that the transport is ruled by the external modulation, and the crystallographic axes do not play major role.

The main panels of Fig. 1 show magnetoresistance traces between $`\nu `$=2 and 3 at three different temperatures from our base temperature ($``$20 mK) up to 250 mK. The traces are taken after slight illumination ($`n_e`$=2.20$`\times `$1015 m-2). Near $`\nu `$=5/2, a sharp peak is observed for current parallel to the grating, which is replaced by a dip for the perpendicular current. The peak/dip broadens with temperature almost symmetrically in $`B^1`$ hence in $`\nu `$ (see the upper inset), but their height/depth does not change very much in the measured temperature range. The measurements were done by ordinary ac (13 Hz) lock-in technique. The peak/dip was rather insensitive also to the measurement current in the range $`I`$=1–20 nA, although peak broadening attributable to the heating was seen for larger currents. Measurements with $`I`$=2 or 5 nA are shown throughout this paper where broadening was almost negligible. The temperature dependence is quite dissimilar from that of ultrahigh mobility plain 2DEG: in the latter, the peak height strongly depends on the temperature but the width is almost temperature insensitive, and the anisotropy vanishes at the temperature as low as 150 mK.Lilly et al. (1999a); Du et al. (1999) Moreover, the width of our peak/dip is much narrower ($`\mathrm{\Delta }\nu _{\mathrm{FWHM}}`$$``$0.007 at the lowest temperature and $``$0.024 even at 250 mK), accounting for only small fraction of the region between two successive integer QHE, while in ultrahigh mobility plain 2DEG, the peak spans major part of the region ($`\mathrm{\Delta }\nu _{\mathrm{FWHM}}`$$``$0.3–0.4). In a nutshell, our anisotropy occurs only when much severer condition for $`\nu `$ (or $`a/l`$) is met, but once it takes place, it is much more robust. The robustness of the observed anisotropic features against temperature and also against impurities does not in itself defy the interpretation by CDW. We believe low temperature and extremely high mobility are required for plain 2DEGs in order for the very small built-in anisotropy of unknown origin to be operative. In fact, theories predict rather high ($``$ 1 K) onset temperature of the anisotropic transport (with sufficient anisotropy energy), Jungwirth et al. (1999) or melting temperature for CDW even in the presence of rather large disorder. Stanescu et al. (2000)

The first step toward interpreting the observed transport anisotropy in terms of unidirectional CDW or stripe would be to specify the orientation of the stripe. However, this turns out to be not straightforward. Intuitively one would expect (i) the stripe aligns with the external modulation, and (ii) the low resistivity axis is along the stripe. This implies a dip for current along the grating in contradiction to the observation, suggesting that either (i) or (ii) is incorrect. Recent calculations Ishikawa and Maeda ; Yoshioka (2001); Aoyama et al.  show that for external modulation with a period much larger than $`a_{\mathrm{CDW}}`$, the stripe tends to orient itself orthogonal to the external modulation. This counterintuitive prediction challenges the firmness of (i). We believe, however, the period $`a`$ of our modulation is close to $`a_{\mathrm{CDW}}`$. The expectation (ii) is generally believed to be valid in the interpretation of experimental data on ultrahigh mobility plain 2DEG. However, it is based on the assumption that the CDW is pinned by impurities and that the current is mainly carried by the stripe edge,MacDonald and Fisher (2000); von Oppen et al. (2000) which probably requires to be examined more carefully. In addition, the situation may be different between our LSL and ultrahigh mobility plain 2DEG.

To gain more insight into the orientation of the stripe, the behavior of the peak/dip under tilted magnetic fields is investigated. Fig. 2 shows traces for current along the grating. By the tilt, $`B_{}`$ is introduced either perpendicular (left) or parallel (right) to the grating. As highlighted in the insets, the effect of $`B_{}`$ perpendicular to the grating is small, slightly enhancing the peak height, while the parallel $`B_{}`$ profoundly affect the peak, almost destroys the peak by $`\theta `$=60, shifting it to higher $`B_{}`$. For current across the grating (not shown), basically the same trend is observed with a peak replaced by a dip. The effect of $`B_{}`$ on the stripe is theoretically calculated to be quite subtle:Jungwirth et al. (1999); Stanescu et al. (2000) for 2DEG with small enough thickness ($`6`$ nm), the stripe prefers to be oriented perpendicular to $`B_{}`$, but the trend is reversed for thicker 2DEG. The theories are consistent with experiments on ultrahigh mobility plain 2DEG, if one assumes the aforementioned (ii).Pan et al. (1999b); Lilly et al. (1999b); Pan et al. (2000) Our 2DEG is expected to be thinner than ultrahigh mobility 2DEG owing to higher concentration of unintentionally doped acceptors in the GaAs channel of our triangular confinement potential. In fact, a self-consistent calculation for $`n_e`$=2.2$`\times `$1015 m-2 and estimated acceptor concentration $`N_A`$=1.5$`\times `$1020 m-3 shows rms thickness of 4.8 nm. This means, according to the theories, our stripe prefers to be oriented perpendicular to $`B_{}`$, which in turn suggests, in conjunction with Fig. 2, (i) mentioned above is valid and (ii) must be discarded. Considering the subtleness of thickness dependence of the calculated anisotropy energy, apparently more pieces of information are necessary to be more decisive.

As mentioned earlier, LED illumination is employed to vary $`n_e`$ and hence the ratio $`a/l`$. $`n_e`$ is varied step by step over the range 1.97–2.84$`\times `$1015 m-2.amp  Magnetoresistance traces between $`\nu `$=2 and 3 are displayed in Fig. 3, for both current directions. The anisotropic features appear in a narrow $`n_e`$ range: they are observed only in traces from a1 to a7 ($`n_e`$=2.11–2.29$`\times `$1015 m-2), and traces d and a8 to a14 are featureless. In trace a1 very small structures begin to emerge, followed by the most conspicuous peak/dip at $`a/l`$$``$6.7 in trace a2. The peak/dip shifts to higher field ($`a/l`$$``$6.8) and at the same time becomes smaller in trace a3, and starts to split preserving its position at trace a4, splits into several peaks/dips and becomes complicated in traces a5 and a6. Finally in trace a7, the dip and peak interchange their positions: a dip (peak) appears in the trace with current along (across) the grating at $`a/l`$$``$7.0.rep  In terms of $`\nu `$, the peaks/dips move in a non-monotonic way around $`\nu `$=5/2$`\pm `$0.1.acc

The observation that the peak/dip is most prominent at $`a/l`$$``$6.7 suggests that 6.7$`l`$ represents a certain optimum length scale of the 2DEG. The simplest idea is to identify 6.7$`l`$ with $`a_{\mathrm{CDW}}`$. However, theoretically estimated $`a_{\mathrm{CDW}}`$$`=`$4.443$`l`$ for $`N`$=1 LL of zero-thickness 2DEG Jungwirth et al. (1999); Lag  is much smaller. Inclusion of the effect of finite thickness will presumably make the estimate larger by softening the short range repulsive force, but at present we are not sure whether the present discrepancy is reconciled with this inclusion. Yos  Since 6.7$`l`$ is very close to 1.5$`\times `$4.443$`l`$=6.66$`l`$, another possibility arises that the observed “resonance” signifies $`a`$=1.5$`a_{\mathrm{CDW}}`$. In that condition, external modulation provides 2DEG with wave vector commensurate to the CDW and at the same time every other minimum in the potential modulation experiences the maximum and the minimum of charge density, respectively, which will make translational motion of CDW easier. Since, as mentioned earlier, our tilted-field experiment favors the alignment of the stripe parallel to the grating, sliding motion of the stripe is consistent with a resistivity minimum for the current across the grating. The insensitiveness to the measurement current suggests the lack in our case of the nonlinear I-V characteristics observed in ultrahigh mobility plain 2DEGs, Lilly et al. (1999a) which is also consistent with the picture that the CDW is not pinned. However, this sliding motion picture is no more than a crude speculation at present. Away from the “resonant” condition, the peak/dip probably try to survive making compromise among the optimum conditions for $`a/l`$, $`\nu `$ and so forth. On an occasion when multiple conditions come closer in energy together, splitting may result. The interchange in trace a7 of the peak and dip implies, if one assumes one-to-one correspondence between appearance of peak/dip and the orientation of the stripe, the stripe has turned its direction around. A recent theory Aoyama et al. ; Zhu  suggests the possibility of such turnaround. Since the orientation of the stripe is expected to be reflected in its response to $`B_{}`$, we have conducted tilt experiment also for a7. For $`B_{}`$ parallel to the grating (to be compared with the right panel in Fig. 2), the dip/peak is observed to be more robust, consistent with the turnaround. Owing to the smallness of the observed features that makes quantitative evaluation difficult, however, it seems to be going too far to take this as evidence of the turnaround.

Around $`\nu `$=7/2, similar peaks/dips are observed, although with much less distinctness, over the entire range of $`n_e`$ available in the present experimental setup. The behavior is rather complicated to allow simple analysis.

To summarize, we have observed anisotropic features around $`\nu `$=5/2 (and 7/2) in 2DEG subjected to weak external modulation having a period comparable to the theoretically calculated period $`a_{\mathrm{CDW}}`$. The advantage of the present study is that the source of the anisotropy is well-defined. Nevertheless the interpretation of the transport anisotropy in terms of CDW requires further study.

###### Acknowledgements.

The authors acknowledge D. Yoshioka for discussion on calculated $`a_{\mathrm{CDW}}`$ and the effect of finite thickness. This work was supported in part by a Grant-in-Aid for Encouragement of Young Scientist (13740177) and for COE Research (#12CE2004 “Control of Electronics by Quantum Dot Structures and Its Application to Advanced Electronics”) from the Ministry of Education, Culture, Sports, Science and Technology.


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# Evidence for a generic novel quantum transition in high-𝑇_𝑐 cuprates

## Abstract

We study the low-energy spin fluctuations and superfluid density of a series of pure and Zn-substituted high-$`T_c`$ superconductors (HTS) using the muon spin relaxation and $`ac`$-susceptibility techniques. At a critical doping state, $`p_c`$, we find (i) simultaneous abrupt changes in the magnetic spectrum in the superconducting ground state and (ii) that the slowing down of spin fluctuations becomes singular at $`T=0`$. These results provide experimental evidence for a novel quantum transition that separates the superconducting phase diagram of HTS into two distinct ground states.

Quantum phase transitions occur at zero-temperature at a critical electron density separating distinct ground states. Near a quantum critical point electrons in metals are highly correlated and the diverging fluctuations may induce unconventional superconductivity . For example, in certain heavy fermion compounds a “bubble” of superconductivity occurs around the quantum critical point at which itinerant antiferromagnetism is suppressed by applied pressure . The search for an underlying quantum phase transition in HTS is motivated by the potential for quantum fluctuations to bind electronic carriers into superconducting Cooper pairs and also to cause the celebrated linear temperature dependence of their electrical resistivity . HTS exhibit a common generic phase diagram in which the superconducting transition temperature, $`T_c`$ rises to a maximum at an optimal doping of approximately 0.16 holes per planar copper atom and then falls to zero on the overdoped side. In addition the underdoped normal state exhibits correlations, which introduce a gap in the density of states that strongly affects all physical properties. There is no phase transition associated with the opening of this gap and so it is called a pseudogap. Analysis of specific heat data, for example, suggests that the pseudogap energy decreases with doping and falls to zero at a critical doping of $`p_c`$ $``$ 0.19, just beyond optimal doping , a behaviour rather analogous to the quantum-critical heavy-fermion materials .

Many fundamental physical quantities such as the superconducting condensation energy , the superfluid density , and the quasiparticle lifetime , show abrupt changes as $`p`$ $``$ $`p_c`$. While compelling in their totality , none of the results can be considered as evidence of a quantum transition. In particular there is no evidence for an associated order parameter and slowing down of the relevant fluctuations. With this in mind we examined the evolution with doping of the low-energy spin fluctuation spectrum using muon spin relaxation ($`\mu `$SR) combined with low-field $`ac`$-susceptibility measurements of the superfluid density.

The samples studied were: (i) La2-xSrxCu1-yZnyO4 (LSCO) ($`x`$=0.03-0.24 and $`y`$=0, 0.01 and 0.02). Samples were synthesised using solid-state reaction and where necessary followed by quenching and subsequent oxygenation. They were characterised by powder x-ray diffraction as well as extensive transport and thermodynamic measurements $`e.g.`$ refs  and found to be phase pure. Their $`T_c`$ values and lattice parameters were also in good agreement with published data, where available . (ii) Bi2.1Sr1.9Ca1-xYxCu2O8+y (Bi-2212) ($`x`$=0, 0.3, 0.5 and appropriate values of $`y`$ to achieve the desired carrier concentration). Underdoped samples were prepared by deoxygenation and the samples were fully characterised using also thermoelectric power to determine the doping state. (Note that deoxygenation actually removes disorder in this system.) We note that in LSCO $`x=p`$ and to avoid confusion in the rest of the paper we refer to the carrier concentration as $`p`$.

Zero-field (ZF) and transverse-field (TF) $`\mu `$SR studies were performed at the pulsed muon source, ISIS Facility, Rutherford Appleton Laboratory. Spectra were collected down to as low as 40mK thus allowing the temperature dependence of slow spin fluctuations to be studied to high doping. In a $`\mu `$SR experiment, $`100\%`$ spin- polarised positive muons implanted into a specimen precess in their local magnetic environment. Random spin fluctuations will depolarise the muons provided they do not fluctuate much faster than the muon precession. The muon decays with a life-time $`2.2\mu s`$, emitting a positron preferentially in the direction of the muon spin at the time of decay. By accumulating time histograms of such positrons one may deduce the muon depolarisation rate as a function of time after implantation. The muon is expected to reside at the most electronegative site of the lattice. In both HTS families studied here it is the O-2 nearest to the planes  so the results reported here are dominated by the magnetic correlations in the CuO2 planes. As we show below this is confirmed by results in samples doped with Zn, which substitutes for Cu in the CuO2 planes.

The superfluid density, $`\lambda _{ab}^2`$, results shown here are for pure La2-xSrxCuO4 ($`y=0`$) and were determined from measurements of the in-plane magnetic penetration depth $`\lambda _{ab}`$ using the low-field $`ac`$-susceptibility technique at 1G and 333Hz for grain-aligned powders . In total, 16 samples were investigated for each doping content. The values of $`\lambda _{ab}(0)^2`$ for samples with $`p0.15`$ were also confirmed by standard TF $`\mu `$SR experiments performed on unaligned powders at 400G .

Figure 1 shows the typical time dependence of the ZF muon asymmetry  for pure La2-xSrxCuO4 with $`x=p`$=0.08 ($`T_c`$=21K) at (a) low and (b) high temperatures. In all samples the high-temperature form Fig. 1b of the depolarisation is Gaussian and temperature independent, consistent with dipolar interactions between the muons and their near-neighbour nuclear moments. This was verified by applying a 50G longitudinal field, which completely suppressed the depolarisation. Here the electronic spins in the CuO2 planes fluctuate so fast that they do not affect the muon polarisation. At low enough temperatures Fig. 1a, typical of other spin glass systems , there is a fast relaxation due to a static distribution of random local fields, followed by a long-time tail with a slower relaxation resulting from remnant dynamical processes within the spin glass. At very low temperatures oscillations in the asymmetry were observed for $`p0.08`$ and by decoupling experiments in a longitudinal field we confirmed the static nature of the magnetic ground state. For $`p>0.08`$ oscillations were not observed and, as discussed below, the data were better represented by an exponential relaxation indicating either a very strongly disordered static field distribution or rapid fluctuations. Between the high and low temperature limits the spin correlations slow down through the experimental $`\mu `$SR time window and modify the depolarisation process in a distinctive fashion.

To study the doping dependence of this slowing down we determine two characteristic temperatures. (i) The temperature, $`T_f`$, where the spin correlations first enter the $`\mu `$SR time window i.e., where the muon asymmetry first deviates from Gaussian behaviour and (ii) the temperature, $`T_g`$, at which these correlations freeze into a glassy state thus causing an initial rapid decay in the asymmetry. $`\mu `$SR is sensitive to spin fluctuations within a time window of $`10^9`$s to $`10^6`$s  and we may therefore associate $`T_f`$ and $`T_g`$, respectively, with these lower and upper thresholds. In general the relaxation data may be fitted to the form $`G_z(t)=A_1exp(\gamma _1t)+A_2exp((\gamma _2t)^\beta )+A_3`$ where the first term is the fast relaxation in the glassy state (i.e., at higher temperatures $`A_1=0`$), the second stretched-exponential term is the slower dynamical term and $`A_3`$ accounts for a small time-independent background arising from muons stopping in the silver backing plate. As in other spin glass systems, in the high-temperature Gaussian limit $`\beta `$=2.0 . Consequently, any departure below $`\beta `$=2.0$`\pm 0.06`$ is taken as the onset temperature, $`T_f`$, at which spin fluctuations slow down sufficiently to enter the time scale of the muon probe ($`10^9`$s). A typical temperature dependence for $`\beta `$ for Sr=0.08 is shown in Fig. 2a. (As a further check on the assignment of $`T_f`$ we fitted the high-temperature data to the full Kubo-Toyabe function $`G_z(t)=A_1exp(\alpha t^2)exp(\gamma t)+A_2`$ and values of the relaxation rate $`\gamma `$ are plotted in Fig. 2b. $`\gamma `$ is found to rise from zero at the same temperature at which the exponent $`\beta `$ departs from 2, indicating the entrance of the spin correlations into the experimental time window.) At low temperatures the exponent $`\beta `$ falls rapidly towards the value 0.5. We identify $`T_g`$ as the temperature at which $`\beta `$=0.5$`\pm 0.06`$ . This “root exponential” form for the relaxation function is a common feature of spin glasses, and in the present samples the temperature $`T_g`$ coincided with a maximum in the longitudinal relaxation rate $`\gamma `$ (see Fig. 2b) and the appearance of the fast relaxation. Other methods of analysis may still be possible and a different choice might affect the magnitude of the $`T_g`$ values but not the trends. Our values for $`T_g`$ agree with published data, where available .

We first discuss the data for pure LSCO (i.e., $`y=0`$ in Fig. 3). Values of $`T_g`$ and $`T_f`$ summarised in Fig. 3 indicate that the spin-glass phase persists beyond $`p=0.125`$. In fact the onset of the spin glass phase for $`p=0.125`$ occurs at a higher temperature than that for $`p=0.10`$. This may be due to the formation of strongly-correlated antiferromagnetic stripe domains in this range of doping . For $`p=0.15`$ and 0.17, $`T_g`$ becomes very small (less than 45mK) and $`T_f`$ is approximately 8K and 2K, respectively. For $`p0.20`$, there are no changes in the depolarisation function to the lowest temperature measured (40mK).

Figure 3 clearly shows that although the freezing of spins occurs at very low temperatures, low-frequency spin correlations enter the experimental time window at significantly higher temperatures. Both $`T_g`$ and $`T_f`$ are found to decrease with increasing doping and tend to zero at $`p0.19`$. Their behaviour resembles that of the pseudogap  which vanishes at the same doping. The LSCO results are reproduced in the Bi-2212 system (Fig. 3), which shows precisely the same trend with $`T_g`$ and $`T_f`$ $``$ 0 as $`p`$ $``$ 0.19. This observation is not to discount any effects of stripes on our LSCO data. Indeed such effects are clearly seen in the figure where the anomaly seen in LSCO at the hole concentration of 0.125 is clearly absent or diminished in the Bi-2212 data. We also know from a couple of data points  that the YBa2Cu3O7-δ system trends in the same way as LSCO and Bi-2212. Similar slowing down of spin fluctuations has also been observed in the most ordered of all HTS namely the underdoped YBa2Cu4O8 . Furthermore, the doping dependence of $`T_g`$ seen here has also been found in Y1-yCayBa2Cu3O6.02 up to 0.09 holes per planar copper atom . These observations indicate that the behaviour shown in Fig. 3 is common to all HTS. They also indicate that the observed trends are not a consequence of a structural transition or inhomogeneity peculiar to a specific HTS family.

Earlier spectroscopic studies have shown that substitution with Zn slows down the spin correlations . This, as depicted in Fig. 3, enhances the muon depolarisation rate at low temperatures and causes an increase in both $`T_g`$ and $`T_f`$. The striking result which Fig. 3 summarises is the apparent convergence of both $`T_g(p)`$ and $`T_f(p)`$ to zero, for all Zn concentrations, at the critical doping $`p_c0.19`$. While this effect is not so obvious for the pure LSCO samples it is very clear in the two Zn-substituted series. The fact that $`T_f(p)`$ $``$ 0 as $`p`$ $``$ $`p_c`$ for all Zn concentrations suggests that spin correlations within the upper $`\mu `$SR time threshold of $`10^9`$s die out abruptly beyond $`p_c`$ leaving only short-lived fluctuations (or none at all) beyond $`p_c`$. The fact that $`T_f`$ and $`T_g`$ both vanish as $`p`$ $``$ $`p_c`$ implies that the rate of slowing down $`diverges`$ at $`p_c`$, (i.e. the characteristic time changes from $`10^9`$s to $`10^6`$s in smaller and smaller temperature intervals as $`p_c`$ is approached). In the absence of evidence for long-range order in the normal-state, the present observations indicate the existence of a quantum glass transition at $`p_c`$. We note that if the observed quantum glass transition is a conventional spin glass transition, then the glass transition at $`T=0`$ is indeed a quantum critical point . The present behaviour could alternatively be driven by the existence of a quantum metal-insulator transition as has been observed in La2-xSrxCuO4 near $`Sr`$=0.18 . For $`p>p_c`$ spin-flip scattering associated with mobile holes could reduce the lifetime of the spins sufficiently to prevent freezing. Either way, the present results demonstrate the disappearance of short-range magnetic order at $`p_c`$ and a clear link between a quantum transition, the essential physics of superconductivity and the pseudogap in HTS.

This link is further underscored by our detailed measurements of the doping dependence of $`\lambda _{ab}^2(0)`$ for pure LSCO shown in Fig. 4. The superfluid density remains constant above $`p_c`$ but falls abruptly below $`p_c`$. A similar doping dependence of the superfluid density has also been observed in Bi-2212 . This confirms again that this phase behaviour is generic to HTS. Furthermore, recent penetration depth measurements in LSCO and HgBa2CuO4+δ showed that the $`c`$-axis zero-temperature superfluid density $`\lambda _c^2(0)`$ exhibits similar behaviour . The apparent competition between quasi-static magnetic correlations and superconductivity thus results in a crossover to weak superconductivity characterised by a strong suppression of the superfluid density. This suppression in the underdoped region can also be directly linked to the strong reduction in entropy and condensation energy associated with the pseudogap . It is therefore evident here that the onset of short-range magnetic correlations at the critical point $`p_c`$ coincides with an abrupt change in the superconducting ground state properties in HTS. It separates the phase diagram into two distinct regions: (i) below $`p_c`$ where $`T_g`$, $`T_f`$ increase rapidly with underdoping and the superfluid density is rapidly suppressed, and (ii) above $`p_c`$ where $`T_g`$, $`T_f`$ =0 and the superfluid density is almost constant, indicating a transition from weak to strong superconductivity, respectively. Moreover, it is at $`p_c`$ where other fundamental properties such as the superconducting condensation energy and quasiparticle life-time, change abruptly, the resistivity follows its unusual linear temperature dependence to the lowest temperature and the pseudogap extrapolates to zero . These features all indicate that the quantum transition identified here is connected with the fundamental physical properties of HTS.

In general terms our results complement a growing body of work pointing to an intimate relation between slow magnetic correlations and superconductivity that seems mutually co-operative in some experiments  and competitive in others (present work and ref. . In the superconducting state an energy gap is observed in the spin spectrum  but its $`d`$-wave nature ensures that low energy spin fluctuations may still be present, as observed here. Inelastic neutron scattering  and NMR  experiments show that Zn substitution slows spin fluctuations and suppresses long range order. They are consistent with our observation that Zn doping enhances spin glass behaviour. These studies provide a context for the present work but the key new result here is the observation of a quantum transition at a critical doping with an associated change in the superconducting ground state. It follows from our work that the elusive physics of HTS may reduce to the known generic physics of materials near a quantum transition, thus explaining many of their unconventional properties .

In conclusion we have performed a comprehensive study of low-energy spin fluctuations and of the superfluid density in several HTS. We found that both low-energy spin fluctuations and the spin-glass state disappear abruptly at a critical doping $`p_c`$ at zero temperature. Moreover, the rate of slowing of these fluctuations is found to diverge at this point. This provides the first evidence for a $`quantum`$ $`glass`$ $`transition`$ in HTS and indicates quantum critical fluctuations and associated dynamical crossovers may dominate the essential physics of high temperature superconductivity. The identified critical point shows that there are two distinct ground states in the superconducting phase, manifested in a crossover from strong superconductivity for $`p>p_c`$ to weak superconductivity for $`p<p_c`$. The identified transition bears a close resemblance to the locally-critical two dimensional quantum phase transitions described recently by Si $`et`$ $`al`$  in which the magnetic correlations are localised in space but have unlimited range in time.

We are grateful to A.D. Taylor of the ISIS Facility, Rutherford Appleton Laboratory for the allocation of muon beam time. Thanks are due to B. Ingham for synthesising some of the Zn-doped samples. C.P. thanks C. Bernhard, J.I. Budnick, S. Chakravarty, A. Chubukov, S.A. Kivelson W.Y. Liang, J.W. Loram, A.J. Millis, Ch. Niedermayer, D. Pines, S. Sachdev, J. Schmalian and C.M. Varma for useful discussions and The Royal Society for a University Fellowship. J.L.T. acknowledges financial assistance from the New Zealand Marsden Fund and T.X. from the National Natural Science Foundation of China.

$`Correspondence`$ $`should`$ $`be`$ $`addressed`$ $`to`$ $`C.P.`$ (cp200@hermes.cam.ac.uk).

FIGURE CAPTIONS

FIG. 1. Typical zero-field $`\mu `$SR spectra of La2-xSrxCuO4 for $`Sr=0.08`$ measured at (a) 1.3K and (b) 29K. The solid line in (b) is a fit to a stretched exponential, discussed in the text. In (a) the solid line is a fit to a Lorentzian, describing the initial rapid drop of asymmetry, plus a stretched exponential, describing the long-time tail.

FIG. 2. The temperature dependence of (a) the (stretched-exponential) exponent $`\beta `$ and (b) the relaxation rate, $`\gamma `$, within the Kubo-Toyabe function obtained by fitting muon depolarisation data for La2-xSrxCuO4 ($`Sr`$=0.08).

FIG. 3. The doping dependence of the crossover temperatures $`T_f`$ (open symbols) where the spin fluctuations enter the $`\mu `$SR time window and $`T_g`$ (closed symbols) where the spin fluctuations leave the $`\mu `$SR time window. Below $`T_g`$ the fluctuations freeze out into a spin glass. Black, red and blue data are for La2-xSrxCu1-yZnyO4 with $`y=0`$, $`y=0.01`$ and $`y=0.02`$, respectively. The green symbols are $`T_f`$ (open) and $`T_g`$ (closed) values, determined in the same way, for Bi2.1Sr1.9Ca1-xYxCu2O8+y. The $`T_c`$ values for all samples are shown as crosses in the respective colours. $`T_c`$ for Bi-2212 have been divided by 2 for clarity.

FIG. 4. Doping dependence of the inverse square of the zero temperature in-plane penetration depth for pure ($`y`$=0) La2-xSrxCuO4 measured by the $`ac`$\- susceptibility technique.


text:
# On the spin, parity and nature of the Ξ(1620) resonance

## Acknowledgments

E. O. and C. B. wish to acknowledge the hospitality of the University of Barcelona and A. R. and C. B. that of the University of Valencia, where part of this work was done. This work is also partly supported by DGICYT contract numbers BFM2000-1326, PB98-1247, by the EU-TMR network Eurodaphne, contract no. ERBFMRX-CT98-0169, and by the US-DOE grant DE-FG02-95ER-40907.


text:
# Does ohmic heating influence the flow field in thin-layer electrodeposition?

## I Introduction

The electrochemical deposition of metals from aqueous solutions in quasi-two-dimensional geometries has proven to be a valuable test bed to examine concepts of interfacial growth like fractal growth Argoul et al. (1988); Kuhn and Argoul (1995), morphological transitions Fleury et al. (1991); Kuhn and Argoul (1994); Lòpez-Salvans et al. (1997) or dendritic growth Barkey et al. (1995); Argoul et al. (1996). The properties of the evolving deposit are in many cases sensitive to the presence of convection currents in the solution Jorne et al. (1987); López-Tomàs et al. (1993); Barkey et al. (1994); Lòpez-Salvans et al. (1996); Rosso et al. (1999); Schröter et al. (2002). There are two well-known origins of convection rolls: a) on small scales, spatial inhomogeneities of the ionic charge distribution can trigger electro-convection Fleury et al. (1992, 1993); Huth et al. (1995); b) density inhomogeneities due to concentration changes at the electrodes induce large scale gravity-driven convection rolls Rosso et al. (1994); Barkey et al. (1994); Huth et al. (1995); Linehan and de Bruyn (1995); Chazalviel et al. (1996); Argoul et al. (1996); Dengra et al. (2000); Schröter et al. (2002).

However there is another potential source of density changes: due to the small cell volume of typically $``$ 1 $`\mathrm{cm}^3`$, the dissipated electric energy can be the source of a significant heating. If the cell were completely thermally insulated, a solution exposed to an electrical power of 500 mW would start to boil after 500 s. While thermal conduction will confine the overall temperature increase to smaller values, considerable temperature gradients might arise and generate density driven convection.

Thermally induced convection rolls have been thoroughly studied in thin-layer geometries heated from below (for a recent review see Bodenschatz et al. (2000)) and the side Cormack et al. (1974); Imberger (1974); Patterson and Imberger (1980); Boehrer (1997); Delgado-Buscalioni (2001). In contrast, the role of thermal effects was previously not examined in electrodeposition. In order to quantify the possible temperature gradients, a high spatial resolution of the temperature field is necessary. We present here measurements of the temperature field at both electrodes performed by use of an infrared camera. The so determined evolution of the temperature field can be related to the development of the concentration field, which is known from interferometric measurements Argoul et al. (1996); Léger et al. (2000). The remainder of the paper is organized as follows: Section II describes our experimental setup, section III presents the measurement results, which will be discussed in sec. IV.

## II Experimental Setup

The measurements are performed with the infrared camera Varioscan 3021-ST from InfraTec, which contains a Stirling-cooled HgCdTe-detector with 360 $`\times `$ 240 pixel. Using its macro we observe an area of 5.0 $`\times `$ 3.4 $`\mathrm{cm}^2`$, which yields a spatial resolution of 140 $`\mu `$m. The maximal image capturing frequency is 1.1 Hz, the thermal resolution $`\pm `$ 30 mK.

While the sensor is sensitive for wavelengths in the range of 8-12 $`\mu `$m, glass plates, which are normally used as top and bottom plate of the cell, are opaque in this region. Therefore the upper cell cover was realized using a polyethylene foil stretched over an aluminium frame. Due to the flexibility of the polyethylene foil and a small overpressure necessary to fill the cell, the plate separation of about 0.5 mm is not well defined. The bottom plate of the cell consists of a block of Teflon, because this material has a low reflectivity in the infrared. This reduces the so called narcissism: the response of the cooled detector to its own mirror image. The electrodes are parallel zinc wires (Goodfellow 99.99%) of 0.25 mm diameter and separated by a distance of 4 cm. Fig.1 shows an image of the cell during an experiment.

The cell is filled with an 0.1 M $`\mathrm{ZnSO}_4`$ solution prepared from Merck p.a. chemicals in nondeaerated ultrapure $`\mathrm{H}_2\mathrm{O}`$. The measurements are performed at a constant potential of 20 $`\pm `$ 0.003 V. Due to the current increase during the electrodeposition process, the average electrical power feed $`\dot{Q}_{\mathrm{el}}`$ increases from 470 mW at the beginning of the experiment to 650 mW after 500 s.

Because of the modified cell construction, the question of comparability with experiments performed in standard electrodeposition cells could be raised. Therefore we calculate the heat-flux $`k_iA_i`$ for the confining plates, where $`A_i`$ and $`k_i`$ are the area and the heat transfer coefficient of the plate. It is important to keep in mind, that $`1/k_i`$ is equivalent to $`1/\alpha _1+1/\alpha _2+\mathrm{\Delta }z_i/\lambda _i`$. Here $`\alpha _1`$ and $`\alpha _2`$ are the heat transition numbers from solution to plate resp. plate to air, $`\lambda _i`$ is the heat conductivity and $`\mathrm{\Delta }z_i`$ the thickness of the plate.

Inserting the material parameters of our setup James and Lord (1992); Lindner (1989) and using only the area between the two electrodes, we derive a $`k_iA_i`$ of 16.2 mW per Kelvin temperature difference for the polyethylene foil and 11.5 mW/K for the Teflon plate, while a typical glass plate (Schott BK 7, 6.3 mm thick) yields 16 mW/K. So in a first approximation our setup is thermally equivalent to a standard electrodeposition cell.

## III Experimental Results

Fig. 1 shows the growing deposit at the cathode, which belongs to the homogenous morphology Sagués et al. (2000). It is characterized by tip-splitting but retaining a growing front parallel to the cathode. After 500 s a Hecker transition Kuhn and Argoul (1994) takes place and the growth front breaks up into more spatially localized zones of active development.

Immediately before each experiment the infrared camera takes a zero image, which is then subtracted from all images taken during the experiment. Therefore the thermographies solely depict the temperature increase. Fig. 2 gives an example of such a thermography after 280 s, the scale at the right describes the temperature increase with respect to the beginning of the experiment. The white line marks the position of the anodic zinc wire. The temperature decrease at the left hand side of the image is caused by the thermal conductivity of the aluminium frame, the warm “island” in the middle is due to the inhomogeneity of the cell thickness.

In order to improve the signal to noise ratio, zones of spatial homogeneity and a width of 9.1 mm are chosen by visual inspection. Such a zone is depicted in Fig. 2 with two parallel black lines. Inside this zone all rows are averaged, yielding a temperature increase $`\mathrm{\Delta }T(y,t)`$, which is only a function of distance to the cathode $`y`$ and time.

Fig. 3 shows the evolution of $`\mathrm{\Delta }T`$ in the neighborhood of the anode. It is clearly visible that the temperature increase at the anode itself lags behind with respect to the one observed in the middle of the cell.

Fig. 4 illustrates the evolution of the temperature field at the cathode. The most prominent feature is the existence of a local temperature maximum, denoted with small arrows. This maximum moves towards the middle of the cell, where a plateau of spatially constant temperature is located.

In order to characterize the heating process in the cell, we pick the temperature at a distance of 25.6 mm to the cathode (this is approximately the location, where the two convection rolls emerging from the electrodes finally meet, as will be discussed in Section IV.2). Referring to this point, we will speak of the bulk in the following. In Fig. 5 this temperature increase $`\mathrm{\Delta }T_{\mathrm{bulk}}`$ is given for the two experiments presented in Fig. 3 and 4. The fact that the two measurements are almost identical reflects the reproducibility of the experiment. The solid line is a fit to an exponential function, which is motivated in detail in Section IV.3.

The arrows in Fig. 3 represent the location, where the temperature is 20 mK smaller than $`\mathrm{\Delta }T_{\mathrm{bulk}}`$. The distance of these points with respect to the anode is denoted $`L_a(t)`$ and is shown in Fig. 6 (a). Its monotonous increase with time is fitted by a power law, which will be explained in Section IV.1. Correspondingly, Fig. 6 (b) shows the growth of the distance $`L_c(t)`$ between the the location of the temperature maximum in Fig. 4 and the cathode. The straight line is a fit to all data with $`t>`$ 100 s, which will be motivated in Sec. IV.2.

## IV Discussion and conclusions

In principle, the energy balance involves three contributions: the electrical energy feed into the cell, the dissipated ohmic heat and the chemical reaction energy. However the short calculation presented in the appendix supports the assumption that the chemical energy contribution is mostly irrelevant.

The ohmic heat dissipated at some position in the cell will be proportional to the local resistivity $`\rho (y,t)`$ in a one-dimensional model, while $`\rho `$ will depend on the local ion concentration $`c(y,t)`$. In the next three subsections we will compare the evolution of the temperature field at the anode, at the cathode and in the bulk with the development of the concentration field, which is known from interferometric measurements Argoul et al. (1996); Léger et al. (2000).

### IV.1 Evolution of the temperature field at the anode

At the anode $`\mathrm{Zn}^{2+}`$ ions go into solution, increasing the local concentration and therefore density. While this denser solution sinks down to the bottom plate, it gets replaced by less dense bulk solution. This mechanism drives a convection roll of size $`L`$ Huth et al. (1995); Chazalviel et al. (1996); Schröter et al. (2002). According to the fluid dynamical description there are two growth regimes: Initially during the so called immiscible fluid regime $`L`$ will grow with $`t^{0.8}`$, while after some time there will be a crossover to the diffusion hindered spreading regime with a $`t^{0.5}`$ growth law. Chazalviel et al. Chazalviel et al. (1996) showed, that both the fluid velocity $`v`$ and the ion concentration decrease with increasing distance to the electrode. The distance, where $`v`$ has dropped to zero and coincidently $`c`$ has fallen to $`c_{\mathrm{bulk}}`$, defines $`L`$.

Figure 3 shows that the temperature increase in the region between the anode and the arrows lags behind the one observed in the bulk. As $`c>c_{\mathrm{bulk}}`$ translates into reduced ohmic heating, we identify the position of the arrows with the end of the anodic convection roll. A fit to its length with:

$$L_\mathrm{a}(t)=at^b$$
(1)
is presented in Fig 6 (a). It yields: a = 0.13 $`\pm `$ 0.01 mm and b = 0.78 $`\pm `$ 0.01, which indicates that the convection roll is in the immiscible fluid regime for the whole run of the experiment. According to the scaling analysis presented in Ref. Schröter et al. (2002), this corresponds to an average plate separation of about 650 $`\mu `$m.

### IV.2 Evolution of the temperature field at the cathode

Due to the growing deposit, there is a zone of ion depletion in the vicinity of the cathode, the size of which will be affected by the convection roll driven by the occuring density difference. As the decreased $`c`$ leads to higher dissipation, the increased temperature denoted by the arrows in Fig. 4 is qualitatively explained. The distance of the arrows to the initial cathode position $`L_\mathrm{c}(t)`$ should correspond to the actual size of the deposit. Therefore we perform a linear fit with:

$$L_\mathrm{c}(t)=v_\mathrm{c}t+l_\mathrm{c}$$
(2)
which is shown in Fig. 6 (b). We derive $`v_\mathrm{c}`$ = 21.2 $`\pm `$ 0.4 $`\mu `$m/s, which agrees well with 20.7 $`\pm `$ 0.8 $`\mu `$m/s front velocity determined from photographs of the deposit.

$`l_\mathrm{c}`$ is found to be 2 $`\pm `$ 0.1 mm. This finite distance can be explained by the absence of heat production in the metallic deposit because of its low resistivity and the fact that its heat conductivity is 190 times higher than water. So the deposit is an effective heat sink, the resulting heat flux shifts the temperature maximum into the cell.

If the cathodic convection roll, apart from the fact that it starts at the actual front of the deposit, grows in the same way as the anodic roll, they meet 450 s after the beginning of the experiment at a distance of 25 mm to the cathode. This corresponds to the observed change in morphology after that time.

### IV.3 Temperature evolution in the bulk

The temperature increase observed in Fig. 5 can be modeled, if we assume, that the whole cell shares the constant bulk properties $`c`$ and $`\rho `$ and therefore $`T`$. The supplied electrical power $`\dot{Q}_{\mathrm{el}}`$ would then be compensated by the heating of the system with heat capacity $`C`$ and the heat flow $`\dot{Q}_{\mathrm{flow}}`$:

$$\dot{Q}_{\mathrm{flow}}=(TT_0)\underset{i}{}k_iA_i$$
(3)
where $`T_0`$ represents the ambient temperature and $`T`$ the temperature inside the electrolyte. If we assume $`\dot{Q}_{\mathrm{el}}`$ to be constant, the corresponding differential equation:

$$\dot{Q}_{\mathrm{el}}=(TT_0)\underset{i}{}k_iA_i+C\frac{T}{t}$$
(4)
has the straightforward solution:

$$(TT_0)=T_{\mathrm{final}}\left(1e^{t/\tau }\right)$$
(5)
Here $`T_{\mathrm{final}}=\dot{Q}_{\mathrm{el}}/_ik_iA_i`$ denotes the finally reached temperature difference and $`\tau =C/_ik_iA_i`$ is the time constant of the heating up. A fit of Equation 5 to the experimental data is displayed in Fig. 5. It yields: $`T_{\mathrm{final}}`$ = 9 $`\pm `$ 0.2 K. This translates to an overall heat-flux $`_ik_iA_i`$ of 60 mW per K temperature difference. A comparison of this result with the values of $`k_iA_i`$ calculated in Sec. II shows that about 50% of the heat flux takes place through the top and the bottom plate of the cell. The heat flux through the side walls, the electrodes and the plate area beyond the electrodes accounts for the rest.

### IV.4 Influence of the temperature gradients on the convection rolls

In order to estimate the influence of the temperature gradients on the concentration driven convection currents, we plot in Fig. 7 the difference between $`\mathrm{\Delta }T_{\mathrm{bulk}}`$ and a) the cathodic temperature maximum and b) the anode. These temperature gradients result in a down-flow at the anode and an up-flow at the growth front, so they act as an additional driving.

For a more quantitative determination of their contribution, the temperature dependency of the density was measured for different concentrations. The applied density measurement instrument DMA 5000 from Anton Paar has an accuracy better than 50 $`\mu `$g/$`\mathrm{cm}^3`$.

After 400 s the temperature of the 0.1 M $`\mathrm{ZnSO}_4`$ bulk solution has reached about 30  C which corresponds to a density of 1012.3 mg/$`\mathrm{cm}^3`$. In accordance with the measurements presented in Ref. Argoul et al. (1996) and the theory in Ref. Chazalviel et al. (1996), we estimate $`c`$ at the anode for that time as 0.25 M. This corresponds to a density of 1036.4 mg/$`\mathrm{cm}^3`$ for $`T`$ = 30  C and 1037.4 mg/$`\mathrm{cm}^3`$ for the actually measured $`T`$ 27  C. So the contribution of the temperature gradient to the overall density difference at the anode is about 4% as visualized in Fig. 8.

At the cathode $`c`$ has reached zero at that time, $`\rho `$ of $`\mathrm{H}_2\mathrm{O}`$ is 995.68 mg/$`\mathrm{cm}^3`$ for $`T`$ = $`30^{}`$ C and 995.38 mg/$`\mathrm{cm}^3`$ for the $`T`$ = $`31^{}`$ C at the maximum. This results in a 2% contribution of the temperature gradient to the total density contrast.

As our applied potential is above average for standard electrodeposition experiments, we conclude that temperature inhomogeneities will only weakly contribute to the density driven convection rolls. This result justifies with hindsight the use of the theoretical description of Chazalviel et al.Chazalviel et al. (1996). Finally it should be remarked that morphologies like stringy Trigueros et al. (1992), where the zone of active growth is restricted to few small spots with very high local current densities, may differ substantially from our results.

###### Acknowledgements.

We want to thank Jürgen Fiebig from InfraTec for his friendly support. We are also grateful to Niels Hoppe and Gerrit Schönfelder from IMOS, Universität Magdeburg for their assistance with the density measurements. This work was supported by the Deutsche Forschungsgemeinschaft under the project FOR 301/2-1. Cooperation was facilitated by the TMR Research Network FMRX-CT96-0085: Patterns, Noise & Chaos.

## V appendix

The standard enthalpy of formation $`\mathrm{\Delta }_\mathrm{b}H^{}`$ of $`\mathrm{Zn}^{2+}`$ ions in an infinitely diluted solutions is $`153.89`$ kJ/mol Atkins (1990). It contains three different contributions: 1) the energy necessary to liberate an atom from the surrounding lattice, 2) the energy needed to ionize the atom and 3) the hydration energy, which is set free when the water dipoles surround the ion. Only the last term depends on the concentration of the solution, decreasing with the number of ions already dissolved.

As the reaction rate at the electrodes is directly proportional to the electrical current $`I`$, so is the chemical power $`\dot{Q}_{\mathrm{chem}}`$ :

$$\dot{Q}_{\mathrm{chem}}=\frac{\mathrm{\Delta }_\mathrm{b}H^{}}{Fz}I$$
(6)
where $`F`$ is the Faraday constant (96485 As/mol) and $`z`$ the charge number. For zinc we derive $`\dot{Q}_{\mathrm{chem}}/I`$ = -0.8 mW/mA. In the vicinity of the anode this number leads to additional heating due to the transformation of chemical energy. At the cathode the chemical energy stored in the newly produced zinc has to be subtracted from the overall heat production, but does not lead to a direct cooling of the cathode.

With our experimental conditions an average current of 30 mA feeds an electrical power of 600 mW into the cell. Compared to that $`\dot{Q}_{\mathrm{chem}}`$ is 24 mW which is about 4% of the electrical power.

At the cathode the ion concentration drops fast to zero, which justifies the approximation of an infinitely diluted solution. At the anode the ion concentration increases during the whole run of the experiment. Therefore the hydration energy of the newly produced $`\mathrm{Zn}^{2+}`$ ions decreases and in consequence the heat, which is released from the chemical reaction decrease as well. So the overall heat production from chemical energy at the anode is smaller than estimated here and therefore mostly irrelevant for the energy balance. This conclusion agrees with the fact that the anode is the coldest point of the cell as clearly shown in Fig 3, in spite of this extra heat production there.