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# On “the authentic damping mechanism” of the phonon damping model

## Abstract

Some general features of the phonon damping model are presented. It is concluded that the fits performed within this model have no physical content.

In a recent article d1 , the phonon damping model (PDM) has been applied for a description of the giant dipole resonance (GDR) and pygmy dipole resonance (PDR) in oxygen and calcium chains from double-magic to exotic isotopes. It has been argued that it provides much better agreement with the GDR photoabsorption cross sections (PCS) than more advanced, microscopic, approaches. The main purpose of the present Comment is to understand why it is so.

The PDM is a model in which the mode under discussion, the phonon $`Q`$ (with the excitation energy $`\omega `$) and its coupling to $`N`$ uncorrelated $`1p1h`$ states are described phenomenologically. The $`1p1h`$ spectrum is calculated microscopically. Let us start with the PDM application to double-magic nuclei.

A key starting point of almost all PDM calculations is an approximation that the phonon and any $`1p1h`$ state interact with an equal strength $`f_1`$, a model parameter. From microscopic point of view, this assumption is very far from reality.

The general features of the $`Q`$ fragmentation due its interaction with some other states $`|\alpha `$ may be found in textbooks (see, e.g., Appendix 2D in Boh69 ). Then, the second moment for the phonon distribution in the PDM has a simple analytical form:

$$W_2=\left(f_1\right)^2N.$$
(1)
Equation (1) is exact and independent of the details of the spectrum $`E_\alpha `$. However, the shape of the distribution does depend on it, having the Breit-Wigner (BW) form if the energies $`E_\alpha `$ are equidistant Boh69 . Again, the nature of $`|\alpha `$ (whether they are $`1p1h`$ or n$`p`$n$`h`$ states) is not essential. It is only important that the energy scales of $`\omega `$, $`f_1`$, and $`E_\alpha `$ are of the same order.

This means that the BW form for the GDR within the PDM is a direct consequence of the assumption that the coupling matrix element is the same for all $`1p1h`$ states. When a realistic $`1p1h`$ spectrum is used in the PDM calculations, the BW shape is disturbed. To check how strong is this disturbance in general, the PDM calculations with random values of $`E_\alpha `$ from 0 to 50 MeV have been performed. The purpose of these calculations is to reproduce the Lorentz line for the GDR PCS in some hypothetical nucleus with $`E_0=15.0`$ MeV and $`\mathrm{\Gamma }=4.3`$ MeV by fitting the PDM parameters $`f_1`$ and $`\omega `$. The results of calculations with an additional smearing parameter $`\epsilon =0.5`$ MeV (as in Ref. d1  for the oxygen chain) are represented in Fig. 1 by thick lines. Cross sections are plotted in arbitrary units. For the amplitude adjustment, a free parameter $`c_1`$ is available in the PDM.

The calculations show that the PDM results for the GDR PCS converge rather fast to the Lorentz line as $`N`$ increases, even for a random $`E_\alpha `$ spectrum. To exclude any accidental coincidence, the calculations have been repeated with several different random spectra. Qualitatively, the results are similar. So, any traces of the PDM “microscopy” vanish if $`N`$ is not small.

Adopting the Lorentz shape for the GDR PCS as the model input, it is not surprising that the PDM “describes” the photoabsorption data better than microscopic models in which such physical observable as the GDR width is calculated(!). But, to understand whether there is any physical content behind the PDM fits, one needs to analyze the physical meaning of the PDM parameters and/or check how it describes some independent data.

In microscopic perturbative approaches, the matrix element of the interaction between $`1p1h`$ configurations and a phonon tends to increase when a larger basis of $`1p1h`$ states is employed. This is due to the increase of the phonon’s collectivity. However, in the PDM, the collectivity of $`Q`$ does not depend on the $`1p1h`$ basis, and the strength parameter $`f_1`$ decreases with increasing N. Roughly, it goes as $`f_11/\sqrt{N}`$, since $`W_2`$ in Eq. (1) is more or less fixed by the data to which $`f_1`$ is adjusted. Since $`f_1`$ is determined not according to its physical meaning, but only to fit the data, this procedure leads Dang et al. into a contradiction in principle with rather general arguments on the properties of the system under consideration. Indeed, the strength of the interaction between any configuration $`|\alpha _0`$ and $`Q`$ is determined not by their physical properties but only by the number(!) of other configuration $`|\alpha `$. The authors define it as “microscopic description of damping”?!

Another misleading statement in d1  is that the coupling to higher-order graphs are included effectively in the strength parameter $`f_1`$ of the lowest order graphs. This is not true because these are two different physical processes.

Let us briefly consider the PDM results in Ref. d1 . The physics of the essential difference of the GDR width in 40Ca and 48Ca is still an open question. Dang et al. report an agreement with the data in both nuclei. The agreement for 48Ca is obtained by renormalizing $`f_1`$ by 34% (note, that $`f_1`$ is fitted up to 4 digits). But it is difficult to learn anything from this agreement when the true physical meaning of $`f_1`$ in the PDM model is simply ignored.

The extention of the PDM to open-shell nuclei in d1  by including pairing for the $`1p1h`$ states only stresses the internal PDM problems. The lack of the PCS data for these nuclei, except for 18O, allows Dang et al. to keep $`f_1`$ fixed from 18O to 24O, from 42Ca to 46Ca, and from 50Ca to 60Ca as an assumption. But the data available for 16O and 18O already forces the authors to reduce $`f_1`$ by $`25\%`$ from 18O to 16O to achieve an agreement in both (see, note1 ). They claim that the renormalization is to compensate for the enlargement of the configuration space in 18O due to the pairing. But a smaller configuration space should lead to a larger(!) $`f_1`$ and not vice versa (see, Eq. (1)). Again, considering the physical meaning of $`f_1`$, there are no physical grounds for such renormalization.

The properties of the PDR are considered as independent data for the PDM calculations. Although Dang et al. conclude a “consistent and quantitative description” of this resonance, it is difficult to find any agreement of the calculation with the fine structure of the PCS at low energies presented in Fig. 4 of d1 , especially for 18O. For 40Ca and 48Ca, the high-resolution data below 10 MeV are available Har00 . The PDM results are compared to these data in d1  for 48Ca, but not for 40Ca. Such selective comparison may mislead the reader. The PDM predictions for 40Ca were published before the data in Ref. d3 . We find that the PDR exhausts 0.3% of the EWSR in this nucleus. The same value obtained experimentally equals in 40Ca about 0.007% after the two-phonon candidate $`[2_1^+\times 3_1^{}]_1^{}`$ at 6.950 MeV, which is outside the PDM space, is excluded from consideration. The difference by a factor of 40 cannot be defined as quantitative agreement.

The failure to describe the PDR by the GDR spreading to lower energies, as the PDM does, has been sufficiently discussed in the literature (see, e.g., Har00 ; End00  as latest references). In microscopic models, the PDR is associated with the excitation of the lowest $`1p1h`$ $`1^{}`$ configurations End00 ; Cat97 ; Oro98 ; Vre01 ; Col01 . These configurations are included in the PDM model space but their B($`E1`$) values are set to zero to avoid an obvious PDM problem with double counting.

To conclude, it is not clear what Dang et al. mean by the “consistent and quantitative” description of the GDR within the PDM in d1 . A possibility to fit the PCS by the Breit-Wigner shape, which is the model phenomenologic ad hoc input, is not under question. For those nuclei for which the data is available and presented, the PDM needs different sets of the model parameters which are fitted to the described physical observables (three parameters for three observables). Taken together with the above analysis of the physical meaning of the strength parameter, this makes the physical content of the PDM calculations very doubtful. The predictive power of this model is also doubtful and there is no sense to use it for such purpose. The nature of the PDR in the PDM contradicts the microscopic understanding of this resonance and the conclusion that this model describes the PDR properties on the quantitative level is not justified.

It is not possible to agree that the PDM fits confirm “the authentic damping mechanism of giant resonances” as “the result of coupling between collective phonon and non-collective $`p`$-$`h`$ configurations” (with equal matrix element).

The author thanks Professor J. Weil for a careful reading of the manuscript.


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# Dynamical phase transition in a neural network model with noise: an exact solution

## 1 Introduction

Boolean networks have been used to describe a wide variety of complex systems. They provide a common language for models of associative memory , spin glasses , dynamics of evolution , and cellular automata . A typical Boolean network model consists of a set of binary elements (also called nodes, neurons or spins, depending on the context) which are connected among them to form a net. The value of each element at a given time depends on the value at the previous time step of all the nodes that are connected to it.

The use of common tools of statistical physics has revealed a strong parallel between Boolean networks and dynamical systems. In this context, several authors have studied the non-equilibrium dynamics of deterministic Boolean networks and, in particular, the one of *neural networks* . Their work has unveiled the existence of a variety of possible collective behaviors such as synchronized oscillations or chaos . On a similar perspective, the influence of noise on the dynamics of Boolean networks has been analyzed in . It is shown that, for increasing noise level, the barriers separating different attractors decrease and then disappear.

We are interested in considering the changes in the dynamical properties of a deterministic system in the presence of noise. Following this motivation, we study a simple Boolean network model exhibiting self-organization and analyze its tolerance to the effect of noise. We show analytically that the system undergoes a dynamical second-order phase transition as its amount of randomness is increased.

The paper is organized as follows. In section 2, we describe the neural network model with noise. Section 3 introduces the definition of the order parameter characterizing the network and presents numerical evidence for the phase transition by considering two particular network examples. In section 4 we find the dynamical equation satisfied by the order parameter and compute analytically its fixed points, exhibiting the phase transition. In section 5 we apply these results to the two cases studied in section 3. Finally, section 6 is our conclusion.

## 2 Definition of the model

Consider a neural network composed of $`N`$ elements $`\{\sigma _1,\sigma _2,\mathrm{},\sigma _N\}`$, each of which can only take the values $`\sigma _i=1`$ or $`\sigma _i=+1`$. Every $`\sigma _i`$ is randomly connected to any $`K`$ elements of the network, which define its set of *linkages* $`\{\sigma _{i_j}\}_{j=1,\mathrm{},K}`$ (see Fig.1). The parameter $`K`$ is the *connectivity* of the network. Each linkage $`\sigma _{i_j}`$ is weighted by an independent random variable $`c_{ij}`$ that is chosen with a probability density function (PDF) given by $`\mathrm{P}_c(x)`$. The $`NK`$ connections of a network, and its corresponding weights, remain fixed throughout the evolution of the system.

At every discrete time step, each $`\sigma _i`$ receives a signal $`+1`$ or $`1`$ equal to the *input function*

$$f(c_{i1},\mathrm{},c_{iK};\sigma _{i_1},\mathrm{},\sigma _{i_K})=\text{Sign}\left\{\underset{j=1}{\overset{K}{}}c_{ij}\sigma _{i_j}\right\}.$$
(1)
For the particular case in which we have for all weights $`c_{ij}=1`$, this definition corresponds to the *majority rule*, in which $`f`$ takes the same value as the majority of the linkages.

Using the input function (1), we define a stochastic evolution rule for every $`\sigma _i`$ by introducing a noise intensity $`\eta `$ such that

$$\sigma _i(t+1)=\{\begin{array}{ccc}f(c_{i1}\mathrm{}c_{iK};\sigma _{i_1}(t)\mathrm{}\sigma _{i_K}(t))& \text{with probability}& 1\eta \\ & & \\ f(c_{i1}\mathrm{}c_{iK};\sigma _{i_1}(t)\mathrm{}\sigma _{i_K}(t))& \text{with probability}& \eta .\end{array}$$
(2)
The dynamics can thus be set from purely deterministic to purely random by varying $`\eta `$ between $`0`$ and $`1/2`$. Note that in the case with $`\eta =0`$, the system will typically converge to an ordered state in which all the $`\sigma _i`$ are equal.

Due to the presence of noise and to the randomness in the initial assignment of the linkages, the statistical properties of the dynamics of the network do not change if the connection weights or the linkages are either time-independent or if they are randomly re-assigned at every time step. Using the language of boolean networks, this means that for the model presented here the *annealed* and *quenched* dynamics are equivalent .

## 3 Numerical evidence

In this section we perform a numerical study of the evolution of the neural network model introduced above. We show that the system undergoes a dynamical phase transition (for $`N\mathrm{}`$) from an ordered to a disordered state as the noise intensity $`\eta `$ is increased. The analytical expression for this transition will be deduced in section 4.

Let us define an order parameter that adequately describes the degree of alignment of the elements of the network. We first introduce

$$s(t)=\underset{N\mathrm{}}{lim}\left[\frac{1}{N}\underset{i=1}{\overset{N}{}}\sigma _i(t)\right].$$
(3)
With this definition, $`|s(t)|1`$ for an “ordered” system in which most elements take the same value, while $`|s(t)|0`$ for a “disordered” system in which the elements randomly take values $`+1`$ or $`1`$. For systems where the time-average of $`|s(t)|`$ converges, a time-independent order parameter can now be defined as

$$\mathrm{\Psi }=\underset{T\mathrm{}}{lim}\frac{1}{TT_0}_{T_0}^T|s(t)|𝑑t,$$
(4)
where $`T_0`$ can take any arbitrary finite value without changing $`\mathrm{\Psi }`$.

We computed numerically the evolution of the model for a network with $`N=100000`$ elements, connectivity $`K=11`$, and random initial conditions. In practice, the order parameter $`\mathrm{\Psi }`$ was obtained by integrating $`|s(t)|`$ from $`T_0=1000`$ (to drop the initial relaxation dynamics) until $`T=10000`$. A change to a larger integration time produces negligible variations on the result.

The numerical results presented on Figure 2 show the bifurcation diagram of $`\mathrm{\Psi }`$ as a function of the control parameter $`\eta `$ for the case with $`c_{ij}=1`$, in which all connection weights are equal. The input function (1) then simply becomes the majority rule. It is apparent that the system undergoes a phase transition at $`\eta _c0.32`$. For $`\eta <\eta _c`$, all elements in the system will tend to align either to $`+1`$ or to $`1`$. For $`\eta >\eta _c`$, their values are randomly distributed. The blowup on figure 2 shows the usual finite size effect on the phase transition, which smoothes the curve near $`\eta _c`$.

On figure 3 we present the results for the case of a network with fixed connection weights $`c_{ij}`$ that follow the PDF

$$\mathrm{P}_c(x)=\{\begin{array}{cc}1& \mathrm{if}\mathrm{\hspace{0.17em}\hspace{0.17em}0}x1\\ 0& \mathrm{otherwise}.\end{array}$$
(5)
The phase transition on this system is qualitatively equivalent to the previous one, but the critical noise value is now changed to $`\eta _c0.28`$. The blowup shows again the finite size effects.

## 4 Analytic solution

We will compute here the exact analytic expression that relates the noise intensity control parameter $`\eta `$ and the order parameter $`\mathrm{\Psi }`$ for any given PDF of the connection weights $`\mathrm{P}_c(x)`$.

### 4.1 Dynamics of the order parameter

First, we will relate the probability distribution of the system at a time $`t+1`$ with the one at a time $`t`$. In order to do so, let us define $`\varphi _N(t)`$ as the fraction of elements in the network whose value is $`+1`$ at time $`t`$:

$$\varphi _N(t)=\frac{1}{N}\underset{i=1}{\overset{N}{}}\frac{\sigma _i(t)+1}{2}.$$
(6)
In the thermodynamic limit $`N\mathrm{}`$, the above quantity transforms into the probability that at time $`t`$ any arbitrary node $`\sigma _i`$ acquires the value $`+1`$:

$$\varphi (t)𝐏_t\left\{\sigma _i=+1\right\}=\underset{N\mathrm{}}{lim}\varphi _N(t)$$
(7)
Note that from definition (3), the relation between $`s(t)`$ and $`\varphi (t)`$ is simply given by

$$s(t)=2\varphi (t)1.$$
(8)
Thus, in a fully ordered state we have $`|s(t)|=1`$ and $`\varphi (t)=0`$ or $`1`$, while in a fully disordered state we have $`|s(t)|=0`$ and $`\varphi (t)=1/2`$.

It is useful to define $`\xi _i(t)`$ as the argument of the Sign function appearing in the definition of $`f`$ for the $`i`$-th element at a time $`t`$ (see equation (1)),

$$\xi _i(t)=\underset{j=1}{\overset{K}{}}c_{ij}\sigma _{i_j}(t).$$
(9)
If the linkages of every node are assigned in a sufficiently random way222If the linkages are not assigned randomly, the situation changes. For example if they are chosen among the first neighbors of every element, there is no phase transition and the analysis presented here is not applicable., the products $`c_{ij}\sigma _{i_j}(t)`$ can be considered as independent random variables. Therefore, if we denote by $`\mathrm{P}_{\xi (t)}(x)`$ and $`\mathrm{P}_{c\sigma (t)}(x)`$ the PDF associated to $`\xi _i`$ and to the product $`c_{ij}\sigma _{i_j}`$ respectively, then $`\mathrm{P}_{\xi (t)}(x)`$ is simply given by the $`K`$-fold convolution of $`\mathrm{P}_{c\sigma (t)}(x)`$ with itself:

$$\mathrm{P}_{\xi (t)}(x)=\underset{K\text{times}}{\underset{}{\mathrm{P}_{c\sigma (t)}\mathrm{P}_{c\sigma (t)}\mathrm{}\mathrm{P}_{c\sigma (t)}(x)}}.$$
(10)
In terms of $`\mathrm{P}_{\xi (t)}(x)`$, the probability $`I(t)`$ of having the input function $`f=+1`$ at time $`t`$ can be computed as

$$I(t)𝐏_t\left\{f=+1\right\}=_0^{\mathrm{}}\mathrm{P}_{\xi (t)}(x)𝑑x.$$
(11)
Using the updating rule (2), we can now directly write the probability $`\varphi (t+1)`$ of having $`\sigma _i(t+1)=+1`$ in terms of $`I(t)`$ and $`\eta `$:

$$\varphi (t+1)=I(t)\left[1\eta \right]+\left[1I(t)\right]\eta .$$
(12)
This master equation describes the stochastic dynamics of the network. Its fixed points as a function of $`\eta `$ will generate the bifurcation diagram showing the phase transition.

### 4.2 Probability distribution of the input function

In order to express equation (12) in a closed form, we must find how $`I(t)`$ relates to $`\varphi (t)`$. For this, we first compute $`\mathrm{P}_{\xi (t)}(x)`$ which is in turn determined by $`\mathrm{P}_{c\sigma (t)}(x)`$. In Fourier space, the convolution appearing in (10) acquires the simple form

$$\widehat{\mathrm{P}}_{\xi (t)}(\lambda )=\left[\widehat{\mathrm{P}}_{c\sigma (t)}(x)\right]^K,$$
(13)
where $`\widehat{\mathrm{P}}_{\xi (t)}(\lambda )`$ and $`\widehat{\mathrm{P}}_{c\sigma (t)}(\lambda )`$ are the Fourier transforms of $`\mathrm{P}_{\xi (t)}(x)`$ and $`\mathrm{P}_{c\sigma (t)}(x)`$ respectively.

Since the connection weights $`c_{ij}`$ are distributed according to the probability function $`\mathrm{P}_c(x)`$, and the variables $`\sigma _i(t)`$ evaluate to $`+1`$ with probability $`\varphi (t)`$ and to $`1`$ with probability $`1\varphi (t)`$, it follows that the PDF of the products $`c_{ij}\sigma _{i_j}`$ is given by

$$\mathrm{P}_{c\sigma (t)}(x)=\varphi (t)\mathrm{P}_c(x)+\left[1\varphi (t)\right]\mathrm{P}_c(x).$$
(14)
Taking the Fourier transform of the previous expression, and inserting the result into equation (13), one gets

$$\widehat{\mathrm{P}}_{\xi (t)}(\lambda )=\left[\widehat{\mathrm{P}}_c^{}(\lambda )+\left(\widehat{\mathrm{P}}_c(\lambda )\widehat{\mathrm{P}}_c^{}(\lambda )\right)\varphi (t)\right]^K,$$
(15)
where the ‘’ denotes complex conjugation. From the above expression it is apparent that $`\mathrm{P}_{\xi (t)}(x)`$, and consequently $`I(t)`$, are polynomial functions of $`\varphi (t)`$. Therefore, equation (12) is a polynomial of degree $`K`$ in $`\varphi (t)`$, with solutions that depend on the value of the noise intensity $`\eta `$. As we will see later, the roots of this polynomial will furnish the bifurcation diagram of the order parameter.

For convenience, we will write our results in terms of $`s(t)`$ instead of $`\varphi (t)`$ (see equation (8)). Substituting $`\varphi (t)=\left[s(t)+1\right]/2`$ in expression (15) we get

$$\widehat{\mathrm{P}}_{\xi (t)}(\lambda )=\left[\frac{\widehat{\mathrm{P}}_c(\lambda )+\widehat{\mathrm{P}}_c^{}(\lambda )}{2}+\frac{\widehat{\mathrm{P}}_c(\lambda )\widehat{\mathrm{P}}_c^{}(\lambda )}{2}s(t)\right]^K.$$
(16)
By denoting $`\widehat{g}(\lambda )`$ and $`\widehat{h}(\lambda )`$, the real and imaginary parts of $`\widehat{\mathrm{P}}_c(\lambda )`$ respectively, $`\widehat{\mathrm{P}}_{\xi (t)}(\lambda )`$ can then be written as

$`\widehat{\mathrm{P}}_{\xi (t)}(\lambda )`$ $`=`$ $`\left[\widehat{g}(\lambda )+i\widehat{h}(\lambda )s(t)\right]^K`$
$`=`$ $`{\displaystyle \underset{m=0}{\overset{K}{}}}\left({\displaystyle \genfrac{}{}{0pt}{}{K}{m}}\right)\left[\widehat{g}(\lambda )\right]^{Km}\left[i\widehat{h}(\lambda )s(t)\right]^m,`$
whose inverse Fourier transform is

$$\mathrm{P}_{\xi (t)}(x)=\underset{m=0}{\overset{K}{}}\left\{\frac{i^m}{2\pi }\left(\genfrac{}{}{0pt}{}{K}{m}\right)_{\mathrm{}}^{\mathrm{}}\left[\widehat{g}(\lambda )\right]^{Km}\left[\widehat{h}(\lambda )\right]^me^{i\lambda x}𝑑x\right\}\left[s(t)\right]^m.$$
(17)
We are now in position of computing $`I(t)`$. Using equations (11) and (17), and moving the integrals inside the sum we have

$$I(t)=\underset{m=0}{\overset{K}{}}a_m\left[s(t)\right]^m,$$
(18)
where the $`a_m`$ are constant coefficients that depend only on $`\mathrm{P}_c(\lambda )`$ and are given by

$$a_m=\frac{i^m}{2\pi }\left(\genfrac{}{}{0pt}{}{K}{m}\right)_0^{\mathrm{}}_{\mathrm{}}^{\mathrm{}}\left[\widehat{g}(\lambda )\right]^{Km}\left[\widehat{h}(\lambda )\right]^me^{i\lambda x}𝑑\lambda 𝑑x.$$
(19)
We can formally integrate over $`x`$ by replacing $`e^{i\lambda x}e^{(i\lambda +ϵ)x}`$, computing the new $`x`$-integral, and then evaluating the result at $`ϵ=0`$. Our final formula for the $`a_m`$ coefficients gives

$$a_m=\frac{i^{m+1}}{2\pi }\left(\genfrac{}{}{0pt}{}{K}{m}\right)_{\mathrm{}}^{\mathrm{}}\frac{1}{\lambda }\left[\widehat{g}(\lambda )\right]^{Km}\left[\widehat{h}(\lambda )\right]^m𝑑\lambda .$$
(20)
Note that $`a_m=0`$ for all even values of $`m`$. Indeed, since the function $`\widehat{g}(\lambda )`$ is even and $`\widehat{h}(\lambda )`$ is odd, the integrand will be antisymmetric for any even $`m`$, thus vanishing the integral.

It will be useful for later calculations to compute the value of $`a_0`$. In fact, it turns out that $`a_0=1/2`$ for every $`K`$ and any “well behaved” function $`\mathrm{P}_c(x)`$. This can be readily proven by extending the integral in (20) to the complex plane. The integration path $`𝒞`$ shown on figure 4 contains no poles, therefore

$$_𝒞\frac{1}{z}\left[\widehat{g}(z)\right]^K𝑑z=0.$$
(21)
Since $`\mathrm{P}_c(x)`$ is a PDF, Parseval’s theorem guarantees that its Fourier transform is square integrable, which implies $`_{\mathrm{}}^{\mathrm{}}\widehat{g}^2(\lambda )𝑑\lambda <\mathrm{}`$. Therefore, the contribution of segment $`𝒞_3`$ to the integral in (21) is zero for $`R\mathrm{}`$. On the other hand, being $`\widehat{g}(\lambda )`$ the real part of the Fourier transform of a PDF, one has $`\widehat{g}(0)=1`$ and thus, for any well behaved function it is possible to approximate $`\widehat{g}(r)1`$ over the small segment $`𝒞_1`$. This allows us to compute $`_{𝒞_1}\frac{1}{z}\left[\widehat{g}(z)\right]^K𝑑z=_\pi ^0i𝑑\theta =i\pi `$. Replacing into (21), we obtain the value of the integral in (20) and find that $`a_0=1/2`$ for any $`\mathrm{P}_c(x)`$ and any $`K`$.

### 4.3 Computing the bifurcation diagram

We can now combine the main results of sections 4.1 and 4.2 to find an analytic expression relating $`\eta `$ and $`\mathrm{\Psi }`$. We have shown that $`I(t)`$ is a polynomial of degree $`K`$ in $`s(t)`$. Therefore, in terms of $`s(t)`$, the master equation (12) governing the dynamics of the network becomes

$$s(t+1)=2\left(12\eta \right)\left(a_1s(t)+a_3[s(t)]^3+\mathrm{}+a_K[s(t)]^K\right).$$
(22)
In the limit $`t\mathrm{}`$, $`s(t)`$ will asymptotically approach a fixed point $`s`$ which, from the above equation, obeys

$$s=2\left(12\eta \right)\left(a_1s+a_3s^3+\mathrm{}+a_Ks^K\right).$$
(23)
It is important to point out that if the probability function $`\mathrm{P}_c(x)`$ is symmetric, there is no phase transition. Indeed, if $`\mathrm{P}_c(x)`$ satisfies $`\mathrm{P}_c(x)=\mathrm{P}_c(x)`$, then the imaginary part $`\widehat{h}(\lambda )`$ of its Fourier transform would be identically zero. It follows from equation (20) that $`a_m=0m`$ and, therefore, equations (22) and (23) give the trivial result $`s=0`$ as the only possible solution for the dynamics.

Equation (23) is always satisfied by $`s=0`$. However, as $`\eta `$ is varied, this solution becomes unstable as other ones appear. Discarding the solution $`s=0`$ and solving equation (23) for $`\eta `$, we get

$$\eta =\frac{a_11/2+a_3s^2+\mathrm{}+a_Ks^{K1}}{2(a_1+a_3s^2+\mathrm{}+a_Ks^{K1})}.$$
(24)
By dividing the polynomials and neglecting the terms of order $`s^4`$ and higher in the resulting expression333As it can be seen in figures 2 and 3, the order parameter vanishes continuously when passing from the ordered to the disordered phase. Therefore, in the vicinity of the phase transition $`s0`$., we obtain

$$\eta \eta _c=\frac{a_3}{4a_1^2}s^2$$
(25)
where $`\eta _c`$ is defined as

$$\eta _c=\frac{1}{2}\left(1\frac{1}{2a_1}\right).$$
(26)
Since $`a_3<0`$, equation (25) implies that real non-zero solutions for $`s`$ in (23) only exist if $`\eta <\eta _c`$. For $`\eta >\eta _c`$ the solutions of equation (25) are imaginary and therefore $`s=0`$ is the only acceptable solution of (23). We thus conclude that a phase transition with critical exponent $`1/2`$ will occur at $`\eta =\eta _c`$. The explicit behavior of the order parameter $`\mathrm{\Psi }=|s|`$ near the transition will be

$$\mathrm{\Psi }=\{\begin{array}{ccc}\frac{2a_1}{\sqrt{|a_3|}}\left(\eta _c\eta \right)^{1/2}\hfill & \text{for}& \hfill \eta <\eta _c\\ & & \\ 0\hfill & \text{for}& \hfill \eta >\eta _c\end{array}$$
(27)
## 5 Examples of the analytic solution

In this section we compare our analytic solution with the numerical results presented in section 3.

We consider first the case with $`c_{ij}=1`$ for all connections. The PDF of these connection weights is then $`\mathrm{P}_c(x)=\delta (x1)`$, and we have

$$\widehat{\mathrm{P}}_c(\lambda )=_{\mathrm{}}^{\mathrm{}}\delta (x1)e^{i\lambda x}𝑑x=\mathrm{cos}(\lambda )+i\mathrm{sin}(\lambda ).$$
(28)
Therefore, the coefficients $`a_m`$ are given by

$$a_m=\frac{i^{m+1}}{2\pi }\left(\genfrac{}{}{0pt}{}{K}{m}\right)_{\mathrm{}}^{\mathrm{}}\frac{1}{\lambda }\left[\mathrm{cos}(\lambda )\right]^{Km}\left[\mathrm{sin}(\lambda )\right]^m𝑑\lambda .$$
(29)
For the other case, in which the connection weights are uniformly distributed in the interval $`[0,1]`$ as given in expression (5), we get

$$\widehat{\mathrm{P}}_c(\lambda )=_0^1e^{i\lambda x}𝑑x=\frac{\mathrm{sin}(\lambda )}{\lambda }+i\frac{1\mathrm{cos}(\lambda )}{\lambda },$$
(30)
and the corresponding coefficients $`a_m`$ are given by

$$a_m=\frac{i^{m+1}}{2\pi }\left(\genfrac{}{}{0pt}{}{K}{m}\right)_{\mathrm{}}^{\mathrm{}}\frac{1}{\lambda ^{K+1}}\left[\mathrm{sin}(\lambda )\right]^{Km}\left[1\mathrm{cos}(\lambda )\right]^m𝑑\lambda .$$
(31)
We evaluated the integrals in (29) and (31) for the case $`K=11`$, which was studied in section 3. By replacing them into equation (24) we explicitly obtain $`\eta `$ as a function of $`s`$ for these two particular cases. The solid curves on figures 2 and 3 show the analytic bifurcation diagram that is found through this procedure. The agreement with the results our numerical simulation is excellent, confirming our assumption that all elements can be considered as independent random variables, even if the network connections and weights are kept fixed throughout the evolution of the system.

Once the values of the coefficients $`a_m`$ are obtained, the critical noise value $`\eta _c`$ can be readily calculated by using equation (26). Figure 5 shows a log-log graph of the vanishing value of $`\mathrm{\Psi }`$ as a function of $`\eta _c\eta `$, both for the constant connection weight case ($`\eta _c0.3153`$) and for the uniform distribution weight case ($`\eta _c0.2838`$). These results are the same that were presented in section 3. On the displayed windows, finite-size effects around $`\eta _c`$ are not visible. As can be seen on this figure, the numerical results coincide perfectly with the analytic solution (24) (solid curve) and with the asymptotic behavior given in (27) (dashed line).

Figure 6 shows the critical noise level $`\eta _c`$ as a function of the connectivity $`K`$ for the two particular cases studied. As the connectivity is increased, the phase transition appears at higher levels of noise and it is increasingly hard to disorder the system. As the system becomes more and more correlated, $`\eta _c`$ will asymptotically approach its maximum value of $`1/2`$ (data not shown). For the case in which $`c_{ij}=1`$ for all connections, the majority rule is not well defined for even values of $`K`$, since there can be equal number of elements with $`\sigma _i=+1`$ and $`\sigma _i=1`$. This justifies the degeneracy observed for $`\eta _c`$ with respect to consecutive odd and even values of $`K`$. For $`K=2`$ the system will be disorganized at any $`\eta _c>0`$ and no phase transition occurs.

## 6 Conclusions

We have shown the existence of a noise-driven phase transition in a neural network with random connections. We found an exact analytic solution of the stochastic equation which governs the dynamics of the system. By finding its fixed points as a function of noise we constructed the bifurcation diagram, which shows that the phase transition is of second-order with a critical exponent of $`1/2`$.

Besides the randomness of the network connection, our work was carried out with very few assumptions. One of these was to consider the connection weights as statistically independent variables. This condition, however, is not satisfied by many models of interest such as the Hopfield neural networks . It would therefore be of great interest to generalize our approach to cases in which the connection weights are statistically correlated. Given that these conditions are satisfied, the existence of the phase transition only seems to require that the PDF of the connection weights $`\mathrm{P}_c(x)`$ is a non-symmetric but otherwise arbitrary function, as shown on section 4.3.

The general framework under which the results on this paper were derived leads us to believe that this type of noise-driven phase transitions from an ordered to a disordered state must be a robust feature of systems with elements that are somehow randomly connected .

## Acknowledgements

We would like to thank Leo Kadanoff for his encouragement and valuable scientific discussions. This work was supported in part by the MRSEC Program of the National Science Foundation under award number 9808595, and by the NSF DMR 0094569. M. Aldana also acknowledges CONACyT-México for a postdoctoral grant and the Santa Fe Institute of Complex Systems for partial support through the David and Lucile Packard Foundation Program in the Study of Robustness.


text:
# The stochastic resonance mechanism in the Aerosol Index dynamics

## I Introduction

Over the last two decades, much attention has been devoted to study stochastic resonance (SR) as a model for many kinds of physical phenomena. The term ”stochastic resonance” describes a phenomenon whereby a weak signal can be amplified and optimized by the presence of noise. Stochastic resonance was introduced by Benzi et al. benzi ; benzi1983  and Nicolis nicolis  in the field of the physics of atmosphere to explain the periodic recurrent ice ages. They used the two levels Budyko-Sellers potential Budyko  for describing the incoming and outcoming radiation and added to it a weak periodic forcing, representing the small modulation of the Earth’s orbital eccentricity and a noise corresponding to variations on small time-scale respect to eccentricity. They found that the presence of the noise amplifies the periodic component, facilitating the jump of the system between the two levels synchronously with the periodical forcing. So they obtained ice ages as a peak, in the power spectrum of a temperature record, centered around the $`100000`$ year period and characterized by the correct amplitude. Since then, stochastic resonance has been observed in a large variety of physical systems, including bistable ring lasers, semiconductor devices, chemical reactions and neurophysiological systems gammaitoni . In the atmospheric field, only recently it appears another application of the SR. In fact, in 1994 El-Niño-Southern-Oscillation has been modeled with stochastic resonance with a periodic forcing of five years Tziperman ; Stone  i.e. stochastic resonance is conjectured to have some relevance also at local climate scale. From these works, however, it seems to be a strong link between the fluctuations in the atmospheric medium (humidity, temperature, wind speed and direction, industrial emission and urban pollution) and the dynamics, that describes the atmospheric behavior on larger spatial and temporal scales. In this paper, we want to reconsider the relevance of SR on global climate scale but on smaller time scale, considering that periodic behaviours of Earth motion could induce stochastic resonance. In this study, we consider time-series representing distribution of tropospheric aerosols that surely are affected by Earth’s revolution and rotation motions. Actually much attention is devoted to a better understanding of the aerosol role in the radiation budget Andreae . The aerosol effect on climate is quantified in terms of radiative forcing, namely the net variation of radiation flux at the top of the atmosphere due only to radiative aerosol effects. A cooling effect of some aerosol (ash and sulfate aerosols) is well-documented Charlson1987 , while other types absorb solar radiation (dust, carbonic and silicaceous aerosols). At present, there are many activities addressed to study the optical properties of anthropogenic aerosols, for determining their influence on the radiative forcing Tegen1996 ; Charlson . The finding of SR into time series from troposheric aerosol should give some new insight on this topic.

## II Datasets

We extracted time-series to analyze from the archive of TOMS (Total Ozone Mapping Spectrometer) Aerosol Index (AI hereafter). In particular we use the data retrieved from the measurements effected by Nimbus 7, an eliosynchronous satellite orbiting around the Earth from November 1978 to May 1993. The AI was determined using the backscattered radiances $`(I_{340},I_{380})`$ measured by TOMS at 340 and 380nm in the following way:

$`AI=100\left[log\left({\displaystyle \frac{I_{340}}{I_{380}}}\right)_{meas}log\left({\displaystyle \frac{I_{340}}{I_{380}}}\right)_{theor}\right]`$
where the subscripts meas and theor indicate respectively measured and theoretically computed quantities Torres1998 . This parameter gives an information on the aerosol optical depth and strongly depends on aerosol layer height and on the optical properties of the aerosols Hsu1999 . The AI is defined in such a way that it is positive for UV absorbing aerosols and negative for no absorbing ones, even if it assumes small negative values when absorbing aerosols are near the Earth’s surface, up to 1.5 km Hsu1999 . It is important to underline that the clouds are characterized by a null AI, but their influence on the measurements is not negligible. In fact the presence of clouds can act as a screen for the detection operations, at least in the case of clouds covering large areas Torres1998 . The data have a spatial resolution of $`1^o`$ latitude x $`1.25^o`$ longitude (corresponding to 50km x 50km) and temporal resolution of one sample a day. At this time, we consider only a restricted area relative to Italy with the following geographical coordinates $`(718^oE;3647^oN)`$. To reduce the clouds contribution on our data, we used the reflectivity data from TOMS as parameter to distinguish the case of obscuring clouds from not one. If the reflectivity exceeds a threshold of $`25\%`$, we consider the AI as corrupted by clouds and we corrected this sample replacing the experimental value with the previous one plus a quantity chosen randomly among $`0`$, $`0.1`$ and $`0.1`$, where $`0.1`$ is the instrumental error. The physical hypothesis underlying this correction is the small variability of the aerosol content in two days on a area of 50km x 50km. Moreover we have to take into account that the Nimbus 7 stability period started from the 1984, so we consider time-series extended from January 1984 up to May 1993 Herman .

## III Analysis

The first step in examining AI data is to use standard linear and nonlinear analysis techniques to prove that we are in presence of a dynamics intrinsically stochastic. In fig. 1 we can see one scalar time-series and its power spectrum. The power spectrum shows two evident peaks: the principal peak corresponds to an annual period, while the second one is related to a period of about 6 days.

For upgrading our knowledge about the dynamics generating these signals, as a first step, we apply the Independent Component Analysis (ICA) (Hyvarinen1999  and reference therein). It is a well established method, based on Information Theory, to extract, from a recorded signal, independent dynamical systems also non linear, but linearly superposed Acernese2000 . The ICA separates also noise.

As we can observe looking at Fig.2, the application of ICA to our signals has not been able to separate noise contribution from deterministic one. So we may conclude that the periodic part of the signal is intrinsically tied to the fluctuations, i.e. our signals are generated by a genuine stochastic dynamics. Another confirmation of the stochastic nature of the dynamics can be derived from estimating embedding dimension. This estimate is made applying the False Nearest Neighbors method Kennel1992  to a single record: we obtain that up to dimension equal to 10 the algorithm does not converge as in the case of a stochastic process. In conclusion analyzing time series, it seems to be plausible to conjecture the presence of a mechanism of SR acting between the stochastic noise and the annual periodicity. It is important stressing that, if we conjecture SR as a global mechanism, it is also true that the parameters that rules the SR (local radiation budget and insolation) are characteristic of the site location. So it is clear that these parameters, as well as the noise level, depend on the width of the investigated area. In this first step, we focalize our attention on Italy $`(718^oE;3647^oN)`$: we choose this particular area for investigating the contributes of both antrophic and natural aerosol sources and their mutual influence. Thus we have extracted 99 recorded series considering each one of them as a realization of the same stochastic process in a different spatial point. Since a comparison between two stochastic process can be made only on average, we have to extract the average series of experimental data that will be compare with that derived from the model. In this first analysis we devote our attention only to the dominant annual peak, so we execute a pass-band linear filter in the range of $`10^910^6`$ Hz. Successively, we eliminate from the signal a trend that can be ascribed to a residual trace of the satellite instability, obtaining the time-series represented in Fig.3. Now, finally, we have the experimental average time-series to be compared with the one derived from a simulated model.

## IV Modelling

We have to mark two goals, the first is to numerically prove that our physical system can be effectively described with a resonance model, the second one is to make the best fit of the involved parameters and to give a physical interpretation of them. In the framework of the model used by Benzi et al. benzi ; benzi1983 , we described our physical system by means of the following equation:

$`dx=\left[\left(x{\displaystyle \frac{x^3}{a}}\right)+Acos(\omega t)\right]dt+\nu `$
So we have considered a double well potential representing the radiative balance of incoming and outcoming radiation at the top of the atmosphere, that should be directly correlated with the different height of the aerosol layers in winter and summertime. This potential is completely characterized by the gap between them (gap that we indicate with a). The periodical component has a frequency of $`3.210^{}8`$ Hz, corresponding to the annual peak, and amplitude $`A`$. This term is included to take into account the change of daily insolation with the solar declination angle. Because the short period disturbances can be described as a random walk hasselmann , the noise has been included as a Wiener process multiplied for a diffusion coefficient $`\nu `$. The estimate of parameters will give us the noise level, the amplitude of periodic forcing and then the estimate of difference between the two levels. Bearing in mind that, in regime of SR, the oscillation amplitude is equal to a, we fix this parameter in agree with the experimental average at the value of $`0.3636`$. So we have reduced the problem to determine the value of two parameters to better approximate our experimental signal.

Tuning the parameters we realize the time scale conditions gammaitoni  finding the values that give us a maximum correlation integral between the mean value of the simulated stochastic process (obtained from 100 realizations for each value of the parameters) and the averaged experimental signal. In this way we find a maximum correlation integral of 0.71 corresponding to a dimensionless level noise of about 0.06 and an amplitude of periodic forcing equals to $`43710^4`$. The last quantity corresponds to the 10 percent of insolation variation over Italy, respect to the clear day solar insolation (estimated as $`1000W/m^2`$). With this simulation, we have the estimation of the parameters describing our system and we can also reconstruct the Signal to Noise Ratio (SNR) behavior as function of the noise strength. The SNR curve represented in Fig.4 is characteristic of the stochastic resonance gammaitoni : this confirms us that the AI dynamics can be described with a SR mechanism. Moreover the best approximating signal corresponds to a noise level of $`\nu `$=0.06, so in this curve of resonance we are around the maximum.

## V Conclusions

The stochastic nature of the atmospheric medium is a well-established reality, but the enhancing function of this component is a no-trivial one. In this paper, we have proved that the Aerosol Index dynamics over Italy can be described through a stochastic resonance model and in addition we have found that we are effectively in stochastic resonance regime. This is an important aim, because it is the first time that SR is observed in atmospheric physics on human time scale. Surely this could be a fundamental tool for a better understanding of atmospheric dynamics, in particular for what concerns the links between the mechanism of global circulation and the local processes of aerosolic production and distribution. Moreover the presence of an atmospheric SR mechanism on a small time scale for the Aerosol Index has certainly some direct and indirect effects on other relevant atmospheric parameters such as the water vapor and precipitable water atmospheric contents, because of the aerosol’s role as condensation nuclei.


text:
# Conditional entropies and their relation to entanglement criteria

## I Introduction

Entanglement has always been a key issue in the ongoing debate about the foundations and interpretation of quantum mechanics since Einstein EPR  and Schrödinger Sch  expressed their deep dissatisfaction about this astonishing part of quantum theory. Whereas for the long period from 1935 to 1964, until Bell Bell  published his famous work, discussions about entanglement were purely meta-theoretical, nowadays quantum information theory has established entanglement as a physical resource and key ingredient for quantum computation and quantum information processing. This led to a dramatic increase of general structural knowledge about entanglement in the last few years, and the resource point of view often led to results that are reminiscent of those known from thermodynamics: free entanglement is distinguished from bound entanglement BE , irreversibility can be observed in the process of preparing and distilling entangled states irrev  and entanglement itself is defined in a way that it must not increase by means of local operations and classical communication (LOCC). Moreover, there is recent effort in order to quantify quantum correlations through heat engines heatengines .

Entropies lay at the heart of both theories, thermodynamics and entanglement theory. Concerning the latter it was shown that few reasonable assumptions lead to a unique measure of entanglement unique  for pure bipartite quantum states, which is just the von Neumann entropy of the reduced state. Hence, it is obvious that the two subsystems of a pure entangled state exhibit more disorder as the system as a whole, such that the respective conditional entropy is negative. This is a remarkable property of entangled states, which is impossible for classical systems (i.e. classical random variables).

The present paper is primarily devoted to settling the relationship between the negativity of conditional Rényi and Tsallis entropies and other entanglement properties. We will in particular show how the property of having a positive conditional entropy enters into the known implication chain of entanglement resp. separability criteria.

In the second part we will then follow the result of Nielsen and Kempe Nielsen  and give examples of entangled states having the property that their entanglement can neither be detected by entropic criteria nor by any other spectral criterion. Sec.IV shows that this is indeed the case for symmetric Werner states (in odd dimensions), which play a crucial role in entanglement theory.

## II Preliminaries on separability criteria

To fix ideas we will start by recalling some of the basic notions and previous results concerning separability resp. entanglement criteria.

A bipartite quantum state described by its density matrix $`\rho `$ acting on a Hilbert space $`=^{(A)}^{(B)}`$ is said to be separable, unentangled or classically correlated if it can be written as a convex combination of tensor product states Werner89

$$\rho =\underset{j}{}p_j\rho _j^{(A)}\rho _j^{(B)},$$
(1)
where the positive weights $`p_j`$ sum up to one and $`\rho ^{(A)}`$ ($`\rho ^{(B)}`$) describes a state on $`^{(A)}`$ ($`^{(B)}`$). This means in particular that pure states are separable if and only if they are product states. Moreover, all entanglement properties of pure states, which can always be written in their Schmidt form (cf. Schmidt ) as $`|\mathrm{\Psi }=_i\sqrt{\lambda _i}|i|i,`$ are completely determined by the eigenvalues $`\{\lambda _i\}`$ of the reduced state $`\rho _A=\mathrm{tr}_B|\mathrm{\Psi }\mathrm{\Psi }|`$. The unique measure of entanglement for pure states is then given by the von Neumann entropy of the reduced state:

$$S_1(\rho _A)=\mathrm{tr}\left(\rho _A\mathrm{log}\rho _A\right).$$
(2)
For mixed quantum states however, the situation is much more difficult and deciding whether a state is entangled or separable is not yet feasible in general. Currently, the most efficient necessary criterion for separability is the positivity of the partial transpose (PPT), i.e., the condition that $`\rho ^{T_A}`$ has to be a positive semi-definite operator Peres . The partial transpose of the state is thereby defined in terms of its matrix elements with respect to some basis by $`kl|\rho ^{T_A}|mn=ml|\rho |kn`$. For the smallest non-trivial systems with $`2\times 2`$ resp. $`2\times 3`$ dimensional Hilbert spaces and a few other special cases the PPT-criterion also turned out to be sufficient HHH . In higher dimensional systems, however, so called bound entangled states exist, which satisfy the PPT-condition without being separable BE .

Another well known condition is given by the reduction criterion red ; red2

$$\rho _A\mathrm{𝟏}\rho 0,\text{and}\mathrm{𝟏}\rho _B\rho 0,$$
(3)
which is implied by the PPT-criterion but nevertheless an important condition since its violation implies the possibility of recovering entanglement by distillation (which is yet unclear for PPT violating states). For the case of two qubits (and $`2\times 3`$) the reduction criterion is also known to be sufficient for separability red ; red2 . Moreover, it was shown in lowrank  that Eq.(3) implies that the rank of the reduced state has to be smaller or equal than the rank of $`\rho `$. The general line of implication is then:

$$\begin{array}{c}\rho \text{ separable}\\ \\ \rho ^{T_A}0\\ \\ \rho \text{ undistillable}\\ \\ \rho _A\mathrm{𝟏}\rho 0\mathrm{𝟏}\rho _B\rho 0\\ \\ \mathrm{max}[\text{rank}(\rho _A),\text{rank}(\rho _B)]\text{rank}(\rho )\end{array}$$
(4)
The last condition we want to mention was recently derived by Nielsen and Kempe Nielsen  and is based on majorization. However, it is yet not known how the majorization criterion enters into the above implication chain. Since it is closely related to conditional entropies we will discuss it in more detail in the following section.

## III Conditional Entropies

The idea to use entropic inequalities as separability resp. entanglement criteria for mixed states goes back to the mid nineties when Cerf and Adami Cerf  and the Horodecki family HHHalpha  recognized that certain conditional Rényi entropies are non-negative for separable states, and it was recently resurrected by several groups Abe1 ; Abe2 ; Lloyd ; Vidiella ; Rajagopal ; Tsallisrecent  in the form of conditional Tsallis entropies.

The quantum Rényi entropy depending on the entropic parameter $`\alpha \text{ }\text{R}`$ is given by

$$S_\alpha (\rho )=\frac{\mathrm{log}\mathrm{tr}(\rho ^\alpha )}{1\alpha },$$
(5)
where $`S_0,S_1,S_{\mathrm{}}`$ reduces to the logarithm of the rank, the von Neumann entropy and the negative logarithm of the operator norm respectively. For the case of separable states it was shown in Cerf ; HHHalpha ; lowrank  that the conditional entropy secondred :

$$S_\alpha (B|A;\rho ):=S_\alpha (\rho )S_\alpha (\rho _A)$$
(6)
is non-negative for $`\alpha =0,\mathrm{}`$ and $`\alpha [1,2]`$.

In Ref. Abe1 ; Lloyd  essentially the same criterion was expressed in terms of the Tsallis entropy

$$T_\alpha (\rho )=\frac{1\mathrm{tr}(\rho ^\alpha )}{\alpha 1},$$
(7)
which is non-negative, concave (convex) for $`\alpha >0`$ ($`\alpha <0`$) and becomes the von Neumann entropy in the limit $`\alpha 1`$. The conditional Tsallis entropy defined in Abe1  reads

$$T_\alpha (B|A;\rho ):=\frac{\mathrm{tr}(\rho _A^\alpha )\mathrm{tr}(\rho ^\alpha )}{(\alpha 1)\mathrm{tr}(\rho _A^\alpha )}.$$
(8)
Concerning positivity, however, the two conditional entropies are equivalent, i.e.

$$T_\alpha (B|A;\rho )0S_\alpha (B|A;\rho )0,$$
(9)
which is in turn equivalent to $`\mathrm{tr}(\rho _A^\alpha )\mathrm{tr}(\rho ^\alpha )`$ for $`\alpha >1`$, $`\mathrm{tr}(\rho _A^\alpha )\mathrm{tr}(\rho ^\alpha )`$ for $`0\alpha <1`$, and the positivity of the conditional von Neumann entropy for $`\alpha =1`$.

Obviously, for pure states the conditional entropies are negative if and only if the state is entangled.

### III.1 Monotonicity counterexample

It was conjectured in Lloyd  that $`T_\alpha (B|A;\rho )`$ is monotonically decreasing in $`\alpha `$, such that it would be sufficient to calculate $`T_{\mathrm{}}(B|A;\rho )`$ in order to decide positivity. However, monotonicity does not hold in general and can most easily be ruled out by low rank examples like

$$\rho =\frac{1}{2}\left(|\mathrm{\Phi }_+\mathrm{\Phi }_+|+|0101|\right),|\mathrm{\Phi }_+=\frac{1}{\sqrt{2}}\left(|00+|11\right),$$

for which the reduced state has eigenvalues $`\frac{1}{4},\frac{3}{4}`$ and therefore $`T_0=T_{\mathrm{}}=0T_2=\frac{1}{5}`$. We note that similar counterexamples can be found for the monotonicity of the conditional Rényi entropy as well. Fortunately, however, monotonicity is not necessary for proving the positivity of the conditional Tsallis/Rényi entropies for separable states for other values than $`\alpha =0,\mathrm{}`$, $`\alpha [1,2]`$ wrongproof .

### III.2 Majorization and convex functions

Majorization turned out to be a powerful tool in the discussion of quantum state transformations by means of LOCC operations (cf.majotrafo ) and it was recently proven to yield the strongest separability criterion, which is based on the spectra of a state and one of its reductions. It was proven in Ref. Nielsen  that any separable state $`\rho `$ acting on $`\text{ }\text{C}^d\text{ }\text{C}^d`$ is majorized by its reduced state $`\rho _A`$:

$$\rho _A\rho \text{ i.e. }kd:\underset{i=1}{\overset{k}{}}\lambda _i^{(A)}\underset{i=1}{\overset{k}{}}\lambda _i,$$
(10)
where $`\{\lambda _i\}`$ and $`\{\lambda _i^{(A)}\}`$ are the decreasingly ordered eigenvalues of $`\rho `$ respectively $`\rho _A`$.

It is a well known result in the theory of majorization that $`xy`$ iff $`\mathrm{tr}\left(f(x)\right)\mathrm{tr}\left(f(y)\right)`$ for all convex functions $`f:\text{ }\text{R}\text{ }\text{R}`$ Bhatia . Since $`f(x)=x^\alpha `$ is convex for $`\alpha 1`$, concave on $`\text{ }\text{R}^+`$ for $`0\alpha 1`$ and the von Neumann entropy is concave (needed for $`\alpha =1`$), this immediately implies:

Theorem 1 Let $`\rho `$ be a bipartite quantum state, which is majorized by its reduction $`\rho _A\rho `$, then for every $`\alpha 0`$ the conditional Tsallis/Rényi entropies of $`\rho `$ are non-negative, i.e.:

$$S_\alpha (B|A;\rho )0\text{and}T_\alpha (B|A;\rho )0.$$
(11)
The result of Nielsen and Kempe implies that this holds in particular for any separable state.

It is yet not known how the majorization criterion (10) is related to other separability criteria like PPT, undistillability and the reduction criterion. However, we will show in the next subsection how the positivity of conditional entropies is related to these properties.

### III.3 Conditional Entropies and the Reduction Criterion

Positivity of the conditional entropies for $`\alpha =0`$ reduces to the rank criterion in the implication chain (4). The following theorem will show, however, that all the other properties stated in (4) in turn imply positivity of the conditional entropies for every value of the entropic parameter $`\alpha `$.

Theorem 2 Let $`\rho `$ be a bipartite quantum state satisfying the reduction criterion $`\rho _A\mathrm{𝟏}\rho `$. Then for every $`\alpha 0`$ the conditional Tsallis/Rényi entropies are non-negative:

$$S_\alpha (B|A;\rho )0\text{and}T_\alpha (B|A;\rho )0.$$
(12)
We note that Thm.2 implies in particular, that states with negative conditional entropies are distillable.

Proof:  We will divide the proof into three steps depending on the value of the entropic parameter.

For $`\alpha >1`$ the proof is essentially based on the Golden-Thompson inequality (cf.Petz ) stating that

$$\mathrm{tr}\left(e^Ae^B\right)\mathrm{tr}\left(e^{A+B}\right)$$
(13)
for hermitian matrices $`A,B`$. Utilizing the definition of the reduced state, i.e.,

$$P0:\mathrm{tr}\left(\rho (P\mathrm{𝟏})\right)\mathrm{tr}\left(\rho _AP\right)$$
(14)
this leads to:

$`\mathrm{tr}\left(\rho _A^\alpha \right)`$ $`=`$ $`\mathrm{tr}\left[\rho (\rho _A^{\alpha 1}\mathrm{𝟏})\right]`$ (15)
$`=`$ $`\mathrm{tr}\left[\mathrm{exp}\left(\mathrm{ln}\rho \right)\mathrm{exp}\left((\alpha 1)\mathrm{ln}(\rho _A\mathrm{𝟏})\right)\right]`$
$``$ $`\mathrm{tr}\left[\mathrm{exp}\left(\mathrm{ln}(\rho )+(\alpha 1)\mathrm{ln}(\rho _A\mathrm{𝟏})\right)\right]`$
At this point we need two monotonicity properties in order to exploit the validity of the reduction criterion. First of all we use the fact that the logarithm is operator monotone KL , i.e.

$$AB\mathrm{ln}A\mathrm{ln}B.$$
(16)
Thus, for $`\alpha >1`$ the reductions criterion $`\rho _A\mathrm{𝟏}\rho `$ implies

$`\mathrm{ln}(\rho )+(\alpha 1)\mathrm{ln}(\rho _A\mathrm{𝟏})`$ $``$ $`\mathrm{ln}(\rho )+(\alpha 1)\mathrm{ln}(\rho )`$ (17)
$`=`$ $`\alpha \mathrm{ln}(\rho ).`$
In the second step we utilize the fact that the exponential function is monotone under the trace. This can be seen by noting that for any $`A`$ hermitian, $`P0`$ and $`B=(A+ϵP)`$ with $`ϵ0`$:

$$\frac{}{ϵ}\mathrm{tr}\left(e^B\right)=\mathrm{tr}\left(e^BP\right)0.$$
(18)
Hence $`\mathrm{tr}\left(e^B\right)\mathrm{tr}\left(e^A\right)`$ is implied by $`BA`$. Together with Eq. (17) this leads to:

$`\mathrm{tr}\left(\rho _A^\alpha \right)(\text{15})`$ $``$ $`\mathrm{tr}\left[\mathrm{exp}\left(\alpha \mathrm{ln}\rho \right)\right]=\mathrm{tr}\left(\rho ^\alpha \right).`$ (19)
For $`0\alpha <1`$ the reduction criterion can immediately be applied since $`f(A)=A^r`$ is an operator decreasing function for $`1r0,A0`$ (cf.MO ) and thus

$$\mathrm{tr}\left(\rho _A^\alpha \right)=\mathrm{tr}\left[\rho (\rho _A^{\alpha 1}\mathrm{𝟏})\right]\mathrm{tr}\left(\rho ^\alpha \right).$$
(20)
For the case $`\alpha =1`$ we hav to look at the conditional von Neumann entropy $`S_1(\rho )S_1(\rho _A)`$, for which positivity is directly implied by the reduction criterion and the operator monotonicity of the logarithm:

$`S_1(\rho _A)`$ $`=`$ $`\mathrm{tr}\rho _A\mathrm{log}\rho _A`$ (21)
$`=`$ $`\mathrm{tr}\rho \mathrm{log}\rho _A\mathrm{𝟏}`$ (22)
$``$ $`\mathrm{tr}\rho \mathrm{log}\rho `$ (23)
$`=`$ $`S_1(\rho ),`$ (24)
which completes the proof.

### III.4 Negative entropic parameters

So far we have only discussed conditional entropies for non-negative values of the entropic parameter $`\alpha `$. For these cases we know that they can become negative for entangled states, the simplest examples being pure entangled states. However, for $`\alpha <0`$ (and states of full rank) the sign of the conditional entropy contains no information:

Theorem 3 Let $`\rho `$ be a bipartite quantum state of full rank. Then for every $`\alpha <0`$ the conditional Tsallis/Rényi entropies are non-negative:

$$\alpha <0:S_\alpha (B|A;\rho )0\text{and}T_\alpha (B|A;\rho )0.$$
(25)
Proof:  Let $`\{|a\}`$ be an eigenbasis of $`\rho _A`$. Then:

$`\mathrm{tr}\left(\rho _A^\alpha \right)`$ $`=`$ $`{\displaystyle \underset{a}{}}a|\rho _A|a^\alpha `$ (26)
$`=`$ $`{\displaystyle \underset{a}{}}\left[{\displaystyle \underset{i}{}}ai|\rho |ai\right]^\alpha `$ (27)
$``$ $`{\displaystyle \underset{a,i}{}}ai|\rho |ai^\alpha \mathrm{tr}\left(\rho ^\alpha \right),`$ (28)
where Eq.(27-28) uses that $`\left(_ib_i\right)^\alpha _ib_i^\alpha `$ holds for $`b_i0,\alpha 0`$, and the last inequality is implied by the convexity of negative powers on $`\text{ }\text{R}^+`$.

## IV Isospectral states

The fact that positivity of conditional entropies is implied by the reduction criterion (Thm.2) shows already that such an entropic criterion cannot be sufficient for separability. In fact, it was shown in Ref. Nielsen  that no spectral property is capable of distinguishing any entangled state from separable ones.

We will in this section follow the idea of Ref. Nielsen  and construct particular examples of states, such that their entanglement cannot be detected by any spectral criterion, since there exist separable states having the same spectrum and the same reductions.

Werner states Werner89  have always played an important and paradigmatic role in quantum information theory. Their characteristic property is that they commute with all unitaries of the form $`UU`$ and they can be expressed as

$$\rho (p)=(1p)\frac{P_+}{r_+}+p\frac{P_{}}{r_{}},0p1,$$
(29)
where $`P_+`$ ($`P_{}`$) is the projector onto the symmetric (antisymmetric) subspace of $`\text{ }\text{C}^d\text{ }\text{C}^d`$ and $`r_\pm =\mathrm{tr}[P_\pm ]=\frac{d^2\pm d}{2}`$ are the respective dimensions. Werner showed that these states are entangled iff $`p>\frac{1}{2}`$ independent of the dimension $`d`$. The following shows however, that none of these entangled states for odd dimension $`d`$ can be detected by any separability criterion, which is based on the spectrum of the state and its reductions.

Theorem 4 Any entangled state in $`\text{ }\text{C}^d\text{ }\text{C}^d`$ with maximal chaotic reductions and eigenvalues having multiplicities which are multiples of $`d`$, has a separable isospectral counterpart, which is locally undistinguishable as it has the same reductions.

Proof:  Let us consider a special basis of maximally entangled states in $`\text{ }\text{C}^d\text{ }\text{C}^d`$ W2 :

$$|\mathrm{\Psi }_{jk}=\frac{1}{\sqrt{d}}\underset{n=1}{\overset{d}{}}\mathrm{exp}\left(\frac{2\pi i}{d}jn\right)|n,nk,$$
(30)
where $`j,k=1,\mathrm{},d`$ and $``$ means addition modulo $`d`$. Any equal weight combination of all states of the form (30), which belong to the same value of $`k`$, is then a projector onto a separable state since

$`P_k`$ $`=`$ $`{\displaystyle \underset{j=1}{\overset{d}{}}}|\mathrm{\Psi }_{jk}\mathrm{\Psi }_{jk}|`$
$`=`$ $`{\displaystyle \frac{1}{d}}{\displaystyle \underset{j,n,m=1}{\overset{d}{}}}\mathrm{exp}\left[{\displaystyle \frac{2\pi i}{d}}j(nm)\right]|n,nkm,mk|`$
$`=`$ $`{\displaystyle \underset{n=1}{\overset{d}{}}}|nn||nknk|`$
is an equal weight combination of product states. Here we have used that $`\frac{1}{d}_{j=1}^d\mathrm{exp}\left[\frac{2\pi i}{d}j(nm)\right]=\delta _{n,m}`$. Moreover, the reductions of the respective states $`P_k/d`$ are maximally chaotic, i.e. $`\rho _A=\mathrm{𝟏}/d`$, just as the reductions of any maximally entangled state.

If we now have a state with multiplicities being multiples of $`d`$ we can replace the projectors onto its eigenspaces with sufficiently many projectors of the form $`P_k`$. The resulting state will then be again a convex combination of product states, i.e., separable, having the same spectrum and maximal chaotic reductions.

For the case of Werner states we note that the unitary invariance of the state $`\rho (p)`$ in Eq. (29) implies that its reductions are $`\rho _A=\mathrm{𝟏}/d`$. Moreover $`\rho (p)`$ has two eigenvalues $`(1p)/r_+`$ and $`p/r_{}`$ with multiplicities $`r_+`$, $`r_{}`$ which are indeed multiples of $`d`$ in odd dimensions.

Following Proposition 2 we can now construct a state

$$\rho ^{}(p)=\frac{(1p)}{r_+}\underset{k=1}{\overset{r_+/d}{}}P_k+\frac{p}{r_{}}\underset{l=1}{\overset{r_{}/d}{}}P_{l+r_+/d},$$
(32)
which has then both, the same spectrum and the same reductions as $`\rho (p)`$. However, as convex combination of separable states it is itself separable for any $`0p1`$.

## V Conclusion

We discussed conditional Rényi and Tsallis entropies and the relation between their positivity and other separability properties. We showed in particular that states having a negative conditional entropy are distillable since they violate the reduction criterion.

Conditional entropies are a special instance of criteria using just the spectra of a state and its reductions. Concerning the detection of entanglement, it was shown in Ref.Nielsen  that majorization is the strongest spectral criterion, which uses the spectra of a state and just one of its reductions. Its relation to other separability criteria is yet not known. The present result and numerical evidence may indicate that majorization is also implied by the reduction criterion. However, the proof presented in Sec.III.3 does not work for arbitrary convex functions and in fact majorization is not implied by the conditional entropy criteria.

Concerning separability the most efficient criterion is still the PPT criterion, which is also a spectral criterion, however, for the partially transposed state. One interesting question in this context would therefore be: how can other (easy calculable) invariants provide information about the separability of a state, which is not yet encoded in the smallest eigenvalue of its partial transpose?

## Acknowledgement

The authors would like to thank R.F. Werner for useful discussions and M.A. Nielsen for bringing the relation to majorization to their attention. Funding by the European Union project EQUIP (contract IST-1999-11053) and financial support from the DFG (Bonn) is gratefully acknowledged.


text:
# Rheological aging and rejuvenation in solid friction contacts

## 1 Introduction

Surfaces of macroscopic solids in general present some degree of roughness on the small — typically micrometric — scale. For this reason, most extended interfaces between two nominally flat solids are of the multicontact type, i.e. composed of a sparse set of real contacts between load-bearing asperities (Fig.1). Their typical size lies in the 1–10 $`\mu `$m range, and they bear average normal stresses $`\overline{p}`$ of the order of the yield stress $`Y`$ of the weaker bulk material BT .

In frictional sliding, it is in the nanometer-thick region — the “joint” — where the two surfaces come into molecular contact and feel the short-range adhesive interactions, that shear localizes, which indicates that the joint is mechanically weaker than the cohesive bulk PRB2 .

Following Tabor BT , the solid friction force $`F`$ needed to slide one solid against the other at relative velocity $`\dot{x}`$ reads:

$$F=\sigma _s\mathrm{\Sigma }_r$$
(1)
with $`\mathrm{\Sigma }_r`$ the total real area of contact, and $`\sigma _s`$ the shear stress within microcontacts.

It is now well established that, at low velocities, the variations of the friction force are governed by the competition between two effects:

(i) Geometric aging: since $`\overline{p}Y`$, the load-bearing asperities creep plastically, hence $`\mathrm{\Sigma }_r`$ increases quasi-logarithmically with contact duration $`\mathrm{\Phi }`$, which may thus be termed “geometric age”. When the interface is at rest, $`\mathrm{\Phi }=t`$. When motion starts, contacts get gradually destroyed, after a lifetime or age $`\mathrm{\Phi }`$, and replaced by fresh ones. So, while the interface sits still, it ages (strengthens), when it slides, it rejuvenates (weakens). This is reflected in the so-called static friction peak observed when setting the system into motion by loading it at constant velocity PRB1 .

(ii) Velocity dependence of the sliding stress $`\sigma _s`$: For various types of such rough/rough multicontact interfaces (polymer glasses PRB2 , rocks nakatani ; scholz , paper PRE94 ) the analysis of the sliding dynamics has led to conclude that, for $`\dot{x}`$ typically in the 1–100 $`\mu `$m.s-1 range, and up to experimental accuracy:

$$\sigma _s(\dot{x})\sigma _{s0}\left(1+\alpha \mathrm{ln}\frac{\dot{x}}{V_0}\right)$$
(2)
with $`V_0`$ some reference velocity in this range. For most systems $`\alpha `$ lies in the $`10^2`$ range. This rheology can be interpreted as resulting from thermally activated “depinning” dissipative events occurring within the adhesive joint and involving activation volumes in the (nm)3 range PRB2 ; persson .

This is consistent with the following qualitative description of adhesive solid friction joints:

(i) A joint is a molecularly disordered, quasi-$`2D`$ medium with thickness $`h`$ of nanometric order. This is obviously the case when the bulk solids themselves are amorphous. It should also be so for a vast majority of solids ordered in the bulk, due to nanometric surface roughnesses, defects in the bulk, atomic misorientation between surfaces, and the frequent presence of adsorbates robbins .

(ii) At rest under zero shear stress, this highly confined medium is a solid. Indeed it is found to respond elastically to a small amplitude shear force.

(iii) When this force reaches the static friction threshold, $`F_s=\mu _sW`$ (with $`W`$ the normal load and $`\mu _s`$ the static friction coefficient), sliding sets in.

Such a phenomenology entails that frictional sliding can be understood as plastic flow of this $`2D`$ confined medium sheared at a deformation rate $`\dot{x}/h`$ proportional to the interfacial sliding velocity. The static threshold then corresponds to what is usually called, in the language of bulk plasticity, the yield stress.

Recent theoretical sollich1 ; sollich2 ; kurchan ; lequeux1  and experimental bonn ; cloitre ; derec  developments in the rheology of complex fluids and (e.g. soft) glasses, have brought to light the important fact that the main characteristics of such rheologies can be interpreted as resulting from the interplay between:

(i) Glass-like aging: As a quenched amorphous structure relaxes down its glassy energy landscape, the system becomes mechanically stronger. This age-strengthening is usually roughly logarithmic.

(ii) Rejuvenation by motion: In the plastic regime, dissipative events, instead of being solely due to activation by (thermal or dynamical) noise, are accelerated by the stress-induced biasing of the energy landscape. The “young”, shallow energy states which were depopulated as aging pushed the system into “older”, deeper ones, thus get repopulated: The sheared soft glass rejuvenates.

If the characterization of solid friction proposed above is truly relevant, it should therefore be possible to evidence structural aging vs rejuvenation effects in the rheology of adhesive joints. If such effects are present, a more direct — hence accurate — experimental study of the fine variations of the frictional stress should reveal that $`\sigma _s`$ not only depends on the instantaneous deformation rate $`\dot{x}/h`$, but also on the previous history of the joint.

In this article we show, on the basis of a detailed experimental study of the frictional dynamics of a {rough PMMA/float glass} interface, that such is indeed the case. The use of such a configuration, in which the microcontacts permanently retain their identity, enables us to get rid of the geometric aging/rejuvenation effects which are predominant for rough/rough interfaces. We are thus able to show that, while an adhesive joint strengthens quasi-logarithmically as it ages at rest, it rejuvenates when sliding. Moreover, we report experiments in which the joint ages under a finite shear stress below the static threshold. They clearly demonstrate that, the larger this applied stress, the faster the aging dynamics of the joint. All this phenomenology proves that a frictional joint can be considered as a confined 2D soft glass.

In section 2 we describe the system and measurement setup, and the experimental procedures. Section 3 reports the experimental results, which are discussed in section 4.

## 2 Experimental setup and system preparation

### 2.1 Sample preparation

The system consists of a slider and a track. The slider is a poly(methyl methacrylate) \[PMMA\] block, with thickness $`10`$ mm and a nominal area $`20\times 70`$ mm2, sliding along its longer dimension. The sliding surface is roughened by hand-lapping against a flat reference glass plate with SiC powder (GRIT $`400`$). The resulting r.m.s. roughness is $`1.3\mu `$m. After lapping, the surface is thoroughly rinsed with distilled water an dried by an Ar flux.

The track is a float soda lime glass $`120\times 120`$ mm2 plate, of thickness $`10`$ mm, with subnanometric roughness on the micrometer scale. Its surfaces are prepared as follows :

(i) Cleaning

The plate, degreased with methanol, ethanol and acetone, is sonicated first in a $`2\%`$ solution of RBS detergent for $`15`$ minutes at $`50^{}`$C, then in ultrapure milli-Q water. After drying it by a N2 flux, ultimate cleaning is performed in a UV-ozone reactor for $`2`$ hours under the steady O2 flux $`0.5`$ l/min, both surfaces being successively exposed to the UV light.

We thus obtain what we will call “bare” glass. In the cases where we use it as such, the plate is immediately transferred from the clean room into the glove box in which all experiments are performed.

(ii) Silanization

Most track samples are silanized before use, with the short molecule (1,1,1,3,3,3) hexamethyl disilazane, in a vacuum chamber. Prior to silanization, the plate is exposed for $`12`$ hours to a saturated water vapor in order to maximize the number of reactive Si-OH surface sites. After pumping out this vapor, the evacuated chamber and the flask containing 1 ml of silane are separately heated up to $`90^{}`$C, then put in communication, which results in total silane evaporation. The reaction is carried on at $`90^{}`$C for either 1 (D1 tracks) or 5 days (D5 tracks).

After cooling, the samples are transferred to the glove box, where we maintain a small Ar overpressure, in the presence of a desiccant resulting in 8–10% relative humidity. All experiments are performed at temperature $`20^{}`$C, well below the PMMA glass transition temperature ($`T_g110^{}`$C.

### 2.2  Measurement setup

The mechanical setup has been described in detail elsewhere PRB1 . It is schematized on Figure 1. The normal load on the interface is provided by the slider dead weight, $`W=7.7`$ N. The slider is driven by a stepping motor through a loading spring of stiffness $`K=8\times 10^2`$ N/$`\mu `$m, the elongation of which, measured with the help of a capacitive sensor, yields the tangential force to within $`10^4`$ N. Driving velocities range between $`10^1`$ and $`10^2\mu `$m/s.

### 2.3 Preparing an interface of constant $`\mathrm{\Sigma }_r`$

In a preliminary series of experiments, the slider and track are brought into contact at an initial instant $`t=0`$. We then measure the dynamic friction coefficient $`\mu _d=F/W`$ in stationary sliding at $`V_0=10\mu `$m/s, at successive times $`t_i`$ ranging from $`10`$ to $`10^5`$ seconds. In between two measurements, the driving is stopped. After such a stop, the slider slows down, and ultimately stops (after a few seconds; see Figure 3) at a finite force level $`F_{stop}`$ where no creep motion is detectable any longer. As shown on Figure 2, $`\mu _d(V_0)`$ is found to increase quasi-logarithmically with the time $`t`$ elapsed from the moment of first contact. We have checked that $`\mu _d(V_0t)`$ is independent of the number and distribution of the $`t_i`$’s.

This result can be attributed to the geometric aging of a population of contacts which retain their identity during sliding, in agreement with observations from optical imaging DK  of the sliding interface Kpc . Indeed, in this case, the geometric age of the microcontacts simply reads $`\mathrm{\Phi }=t`$, and :

$$\mathrm{\Sigma }_r(t)=\mathrm{\Sigma }_0[1+m\mathrm{ln}(1+\frac{t}{\tau })]$$
(3)
For PMMA at room temperature, $`\tau `$ has been estimated PRB1  to be at most of order $`10^2`$ s, and $`m10^2`$.

The measured logarithmic slope, $`d\mu _d(V_0t)/d(\mathrm{ln}t)=\mathrm{2.3\hspace{0.17em}10}^2`$, yields a time evolution of $`\mathrm{\Sigma }_r`$ compatible with that deduced from the increase with waiting time of the static friction coefficient of a {rough/rough} PMMA interface: $`d\mu _s/d(\mathrm{ln}t)=1.7\times 10^2\pm 4\times 103`$.

The situation encountered here is to be contrasted with the rough/rough configuration, in which sliding permanently destroys the microcontacts and replaces them by fresh ones. The use of a rough/flat system enables us to take advantage of the quasi-saturation associated with logarithmic growth, by performing experimental runs of limited duration $`\mathrm{\Delta }t`$ on an interface of geometric age $`\mathrm{\Phi }>>\mathrm{\Delta }t`$. Typically, for all the results presented below, $`\mathrm{\Phi }`$ ranges from $`10^4`$ to $`10^5`$ s, while $`\mathrm{\Delta }t<1`$ hour. $`\mathrm{\Sigma }_r`$ variations are then negligible, giving us access to the fine variations of the “rheological stress” $`\sigma _s`$.

## 3 Experimental results

### 3.1 Friction force level versus silanization

A first, rough characterization of the effect of the physico-chemical state of the glass surface is provided by the value $`\overline{\mu }`$ of $`\mu _d`$ measured at some fixed $`V_0`$. Indeed, the friction force variations to be described below, which provide insight into the frictional joint dynamics, are always quite small as compared with the average level.

First of all, as can be expected for such a highly wettable surface, bare glass tracks yield highly scattered $`\overline{\mu }`$-levels, ranging between $`0.4`$ and $`0.7`$

Silanization results in a sizeable decrease of both the average friction level and its scatter. Namely, for D1 tracks, $`\overline{\mu }`$ lies between $`0.25`$ and $`0.36`$. For more thoroughly silanized, D5 samples, $`\overline{\mu }`$ ranges from $`0.13`$ to $`0.2`$ – a very low level for unlubricated friction BT .

It is worth mentioning that contact angle measurements performed with pure water drops hardly permit to distinguish between D1 and D5 surfaces. The contact angle for both types of tracks is $`85^{}\pm 5^{}`$, compatible with previous measurements for short chain silanes JMB . This points towards the high sensitivity of solid friction as a probe of small scale chemical inhomogeneity of extended surfaces.

In view of the poor reproducibility of the results on nominally bare surfaces, clearly resulting from the presence of uncontrolled adsorbates, most of the results reported below have been obtained with D1 and D5 silanized glass tracks.

### 3.2 Static friction peak as a proof of structural aging

We prepare an “old” interface, with geometric age $`t_0`$, on which we then perform a set of “stop-and-go” experiments. That is, starting from steady sliding at velocity $`V_0`$, the drive is stopped, and the slider left at rest under its self-selected tangential force $`F_{stop}`$ (see 3). After waiting a time $`t_w`$ after the drive has been stopped, loading is resumed at the same $`V_0`$. The corresponding force record, shown on Figure 3, exhibits a so-called static friction peak. Namely :

(i) In a first regime, $`F`$ increases linearly, at the rate $`KV_0`$ corresponding to the elastic loading of the non sliding system. The interface is pinned.

(ii) This static regime ends at the peak value $`F_s=\mu _sW`$, which defines the static friction coefficient $`\mu _s`$.

Note that, strictly speaking, due to the finite loading stiffness $`K`$, sliding starts (depinning occurs) at a slightly lower force level. Indeed, when the peak is reached, necessarily, the instantaneous sliding velocity $`\dot{x}`$ equals the driving one since, inertia being negligible, $`K(V_0\dot{x})=dF/dt=0`$ at this point. Close inspection of the $`F`$-trace indeed reveals, in the immediate vicinity of $`F_s`$, a small rounding off.

(iii) Beyond the static threshold, a rapid force drop is observed, and $`F`$ reaches the steady state plateau value $`\mu _d(V_0|t_0)W`$.

Moreover, when varying the waiting time $`t_w`$ over more than two decades, we observe (fig.4) that $`\mu _s`$ increases quasi-logarithmically with $`t_w`$: as time lapses, the interfacial pinning strength of the non moving system increases. Since this occurs at constant $`\mathrm{\Sigma }_r`$, we must conclude that, when at rest, the adhesive joints experience structural aging.

A second important conclusion results from the presence of the post-peak stress drop in the transient characteristics. Indeed, this decrease of the interfacial strength indicates that, conversely, when sliding sets in, the “structural age” $`\phi `$ decreases from its initial value, reached after waiting $`t_w`$, to the smaller value $`\phi (V_0)`$ , reached when steady motion is established : motion rejuvenates the adhesive joints.

Structural aging is a robust phenomenon, which we have observed with all interface samples, involving either bare or silanized glass tracks.

The aging dynamics can be characterized by the value of the logarithmic slope $`\beta _s=d\mu _s/d(\mathrm{ln}t_w)`$. This is found to lie in the range $`1.5\times 10^3`$$`5\times 10^3`$. Although this level of dispersion is well above experimental uncertainty, no correlation can be evidenced between $`\beta _s`$ values and $`\overline{\mu }`$ levels.

### 3.3 Dependence of aging on shear stress level at rest

In the stop-and-go experiments described above, the system ages at rest under the finite shear force $`F_{stop}=\mu _{stop}W`$ at which its self decelerating creep becomes immeasurably slow. This “jamming force level” is found to lie at most $`10\%`$ below the steady one $`\mu _dW`$ (see for example Figure 3).

The question then naturally arises of whether the shear stress level at rest affects the aging dynamics. For this purpose we have extended the standard stop-and-go protocol as follows. At time $`t=0`$ the drive is reversed, so as to unload the system down to the desired “waiting” level $`\mu _wW`$, with $`0\mu _w<\mu _{stop}`$. After waiting $`t_w`$, we measure the height of the static peak $`\mu _s(t_w|\mu _w)`$.

Figure 4 shows the variations with waiting time of $`\mu _s(t_w|\mu _{stop})`$ and $`\mu _s(t_w|0)`$ for a D5 sample. The corresponding logarithmic slopes are respectively $`\beta _s(\mu _{stop})=6.2\times 10^3`$ and $`\beta _s(0)=3.7\times 10^3`$. Clearly, the aging dynamics is markedly accelerated by the presence of the shear stress. This effect is observed with all samples.

It can be further qualified by measuring $`\mu _s`$, for a given waiting time $`t_w`$, at various $`\mu _w`$ levels. The result of such a set of experiments, performed with four different silanized surfaces, is shown on Figure 5 for $`t_w=10`$ s. In view of the spread of average friction levels, we have plotted, for the sake of comparison, the drop $`\mathrm{\Delta }\mu `$ associated with the post peak stress drop, versus $`(\mu _{stop}\mu _w)`$. It is seen that:

* To a good approximation, all data collapse on a single curve – indicating, again, a very weak correlation between aging dynamics and average friction level.
* The structural age reached at $`t_w`$ decreases very rapidly as the waiting stress level decreases below the jamming one.

Note that some data correspond to $`\mathrm{\Delta }\mu =0`$, meaning that, in such cases, no static peak was observable after waiting $`t_w=10`$ s. In these cases, upon loading, the end of the static regime is revealed by a break in the slope of the $`F(t)`$ trace. For these samples at such low $`\mu _w`$, the static peak starts developing only for larger $`t_w`$ (see Figure 6). Systematic investigations at $`\mu _w=0`$ reveal that the corresponding “latency time” is strongly sample-dependent. We have observed values ranging from less than $`10`$ s to more than $`2000`$ s.

### 3.4 Velocity dependence of the steady sliding friction coefficient

We have also systematically measured the $`\mu _d(V)`$ characteristics of our geometrically old interfaces. A typical result is shown on Figure 7. $`\mu _d(V)`$ exhibits a minimum $`\mu _{min}`$ at $`V=V_{min}`$. For this D5 sample, $`V_{min}1\mu `$m/s.

The velocity weakening observed for $`V<V_{min}`$ provides another evidence that the structural age $`\phi `$ decreases with $`V`$, i.e. that the system rejuvenates when sliding.

For $`V>V_{min}`$, $`\mu _d`$ exhibits clearly a logarithmic increase, reminiscent of that found for rough/rough (e.g. PMMA) interfaces. It has been shown that this effect can be attributed to thermally activated premature depinning of bistable centers with a volume on the order of a cubic nanometer. These centers would thus be the basic dissipative units within the sheared adhesive joint. It is this mechanism, which should also be at work here, which yields the $`V`$-dependence of the sliding stress given by equation (2). For PMMA at $`300`$K, the dimensionless parameter appearing in this equation $`\alpha 5\times 10^2`$.

For the sake of comparison, we have rescaled our $`\mu _d(V)`$ data by $`\mu _{min}`$. The result, for five different (D1 and D5) samples is plotted on Figure 8, in which $`V`$ has also been scaled by $`V_{min}`$. It is seen that, for $`V/V_{min}>1`$, all data then collapse on a single curve. The common reduced logarithmic slope in the velocity-strengthening regime is $`5\times 10^2\pm 6\times 10^3`$, in full agreement with the previously evaluated $`\alpha `$ for PMMA/PMMA.

From this, one may also conclude that, already rather close above $`V_{min}`$, the sliding induced rejuvenation effect is quasi-saturated (which justifies a posteriori our choice of $`\mu _{min}`$ for the rescaling).

Note that, while the $`\mu `$-levels for the various samples differ at most by a factor of $`2`$, $`V_{min}`$ values span more than two decades (from $`0.1`$ to $`30\mu `$m/s). This considerable scatter must certainly be related to the fact that aging/rejuvenation is associated with activated “jumps” above the barriers of a glass-like energy landscape. Hence, roughly speaking, an exponential sensitivity to variations of this landscape.

Velocity-weakening is well known to promote stick-slip instabilities. Indeed, we did observe stick-slip oscillations for silanized samples, but only for of few of the D1 ones, and in the lower part of their $`V`$-weakening regime. Let us recall that, as long as the rejuvenation mechanism responsible for weakening is non-instantaneous, a negative $`d\mu _d/dV`$ does not necessarily entail stick-slip, the presence of which is governed by the detailed dynamics of the age variable and by the external control parameters, e.g. the external loading stiffness.

It is worth mentioning that, with bare glass tracks, we always observe stick-slip, up to a strongly sample-dependent velocity threshold, ranging from $`10\mu `$m/s to $`>100\mu `$m/s. That is, as a rule of thumb, the higher the average friction level, the stronger the trend towards destabilization of steady sliding. However, the poor reproducibility of systems involving bare glass does not permit to make this statement more quantitative.

### 3.5 Long lasting transients

While, for D5 tracks, the transient behavior only consists of the above described static peaks, for D1 systems a more complicated dynamics emerges. Indeed (see Figure 9), in most cases, the force traces also exhibit long lasting post-peak bump shaped transients. Comparison of data for various driving velocities spanning about a decade enable us to assert that this slow transient is not governed by a characteristic time but, rather, by a slid length lying in the 100 – 300 $`\mu `$m range. This must be contrasted with the distance slid during an initial stress drop, which never exceeds 1 $`\mu `$m, indicating that the associated mechanisms are of a different nature.

Moreover, the bump amplitude is found to increase markedly as the waiting stress level is decreased (Figure 9).

These elements lead us to associate long lasting transients with anelastic evolution of the slider PMMA molecules forming the joints: when the stress level is stepped down, as occurs during a stop, they are likely to experience strain recovery. Upon reloading, this process is reversed, and the corresponding work must be provided by the external force.

That this mechanism is attributable to conformational evolution of the surface region of the slider is proved by the fact that these long transients are most pronounced when using freshly lapped PMMA surfaces. Bump heights then decrease gradually with cumulated slid distance, on scales of the order of tens of centimeters. Large bumps reappear after relapping. This suggests that repeated stress cycling leads to irreversible alignment of the polymer molecules – an effect documented already long ago by Tabor et al tabor2 , in particular with PTFE, for which it is most pronounced.

## 4 Discussion

The set of experimental results reported in Section 3 leads us to assert that the nanometer-thick adhesive joints in which frictional sliding localizes can be considered in all respects as a confined 2D soft glass medium, or, equivalently, threshold fluid. Namely :

(i) Below a static threshold, it responds elastically: it is pinned in a disordered solid state induced by confinement under the normal stress.

(ii) This static threshold increases logarithmically with the waiting time : when at rest, the joint ages.

(iii) When sliding starts, the stress drops until reaching its (lower) stationary level : motion rejuvenates the joint.

(iv) This rejuvenation corresponds to the existence of a velocity-weakening regime for dynamic friction. As $`V`$ increases, rejuvenation saturates and friction becomes velocity-strengthening.

Moreover, we find that the (logarithmic) aging rate increases markedly with the shear stress applied to the system at rest. This influence on aging of stress during waiting is akin to the recent results obtained by Viasnoff et al lequeux2  with a colloidal glass. They have shown that applying to this system, aging under stress-free conditions, an oscillating shear stress of finite duration does result in a strong perturbation of the aging process.

In our stop-and-go experiments, the whole aging process takes place under constant shear below the static threshold. This situation is reached after performing a “mechanical quench”, during which sliding decelerates and stops at the prescribed level. Note that the duration $`\mathrm{\Delta }t`$ of the quench depends on the final stress level : for the largest one, corresponding to the jamming level $`\mu _{stop}`$, it is determined by the sliding dynamics itself, and is typically a few seconds. When we unload below $`\mu _{stop}`$, $`\mathrm{\Delta }t`$ is controlled by the unloading time – at most $`1`$ second. For some samples at $`\mu _w=0`$, no static peak is observed for a finite latency period. This indicates that, in these experiments (i) unloading has been fast enough for the joints to be quenched at the initial age $`\phi (V_0)`$ they had when sliding; (ii) the subsequent aging dynamics is slow enough that the peak growth is too small to be measured up to the latency time.

The aging rate increase with waiting stress level is most likely ascribable to the associated biasing of the energy landscape and to the corresponding decrease of “trap depths” sollich1 ; sollich2 . This effect might be responsible in part for the observation by Berthoud et al PRB1  that the logarithmic growth rate of the static peak height of a {rough/rough} PMMA interface is larger under jamming than under stress-free conditions. It would be of interest that analogous studies be performed with 3D threshold fluids such as colloidal glasses.

While the above described phenomenology of friction exhibits all the main qualitative features of soft glass rheology, when inspected more closely, our results lead to two further questions.

(i) The logarithmic velocity dependence of the dynamic friction coefficient $`\mu _d`$ in the strengthening regime is fully compatible with a description in terms of premature depinning events induced by the thermal noise, as discussed in references PRB2 ; persson . Existing theories of sheared glasses sollich1 ; sollich2 ; kurchan  and of plasticity of amorphous media argon ; langer  lead to the idea that, while thermal noise should be relevant at low shear rates, beyond some crossover, the dynamical noise associated with the depinning events themselves should take over. No prediction is available for the moment about the position of this crossover.

In our experiments, the $`V`$-strengthening regime corresponds to shearing rates $`\dot{\gamma }=V/h10^3`$$`10^5`$. This seems to indicate that, for frictional joints, the $`\dot{\gamma }`$ crossover value would be at least that huge. Whether this rather surprising result is of some degree of generality, or is due to possible screening of elastic interactions related with the confinement of our 2D medium remains an open question.

(ii) Average friction levels are highly sensitive to the chemical differences between surfaces obtained under nominally identical silanization conditions. This is most probably related with the fact that defects in the silane coverage, however small their scale, leave non passivated high energy, strong pinning sites on the glass surface. These lead to strong corrugations of the confining potential, hence of the glass-like energy landscape. The impossibility to correlate our $`\beta _s`$ and $`\overline{\mu }`$ data leads us to suspect that, while $`\overline{\mu }`$ measures an average pinning strength, $`\beta _s`$ might be sensitive to much finer details of the landscape. Numerical modelling would probably be very helpful to shed light on this question.

###### Acknowledgements.

We are indebted to J.M. Berquier and P. Silberzan for advice about glass silanization. We thank L. Leger, L. Cugliandolo and J. Kurchan for illuminating discussions.