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# On the Correlations Between Quantum Entanglement and 𝑞-Information Measures

## Abstract

In the present study we revisit the application of the $`q`$-information measures $`R_q`$ of Rényi’s and $`S_q`$ of Tsallis’ to the discussion of special features of two qubits systems. More specifically, we study the correlations between the $`q`$-information measures and the entanglement of formation of a general (pure or mixed) state $`\rho `$ describing a system of two qubits. The analysis uses a Monte Carlo procedure involving the 15-dimensional 2-qubits space of pure and mixed states, under the assumption that these states are uniformly distributed according to the product measure recently introduced by Zyczkowski et al \[Phys. Rev. A 58 (1998) 883\]. Pacs: 03.67.-a; 89.70.+c; 03.65.Bz

KEYWORDS: Generalized information measures, quantum entanglement, Tsallis entropy, Rényi entropy.

Important tools have been developed in recent years for the systematic exploration of the entanglement properties of composite quantum systems . Quantum entanglement is a physical resource associated with the peculiar nonclassical correlations that may exist between separated quantum systems . Entanglement is indeed the basic resource required to implement quantum information processes . A state of a composite quantum system is called “entangled” if it can not be represented as a mixture of factorizable pure states. Otherwise, the state is called separable. The above definition is physically meaningful because entangled states (unlike separable states) cannot be prepared locally by acting on each subsystem individually. In particular, for bipartite pure states $`|\mathrm{\Psi }_{AB}`$ one finds that they are entangled if their Schmidt number is greater that one. Otherwise, they are separable and their associated reduced density matrices $`\widehat{\rho }_A`$, $`\widehat{\rho }_B`$ are projectors. Any bipartite pure state that cannot be expressed as the direct product $`|\mathrm{\Psi }_{AB}=|\varphi _A|\chi _B`$ is entangled and $`\widehat{\rho }_A`$, $`\widehat{\rho }_B`$ represent mixed states. Two-qubits systems are the simplest quantum mechanical systems exhibiting the entanglement phenomenon and play a fundamental role in quantum information theory. They also provide useful limit cases for testing the behaviour of more involved systems . The concomitant space $`S`$ of mixed states is 15-dimensional. Its entanglement properties being far from trivial, their complete characterization constitutes a currently active field of research .

Considerable attention has been paid in recent years to the application of $`q`$-entropies to the study of quantum entanglement . These entropic measures incorporate both Rényi’s  and Tsallis’  families of information measures as special instances (both admitting, in turn, Shannon’s measure as the particular case associated with the limit $`q1`$). The early motivation for these studies was the development, on the basis of the conditional $`q`$-entropies, of practical separability criteria for density matrices. The discovery by Peres of the partial transpose criteria, which for two-qubits and qubit-qutrit systems turned out to be both necessary and sufficient, rendered that original motivation a bit weaker, once it was realized that it is not possible to find a necessary and sufficient separability criterium on the basis of just the eigenvalue spectra of the three density matrices $`\widehat{\rho }_{AB},\widehat{\rho }_A=Tr_B[\widehat{\rho }_{AB}]`$, and $`\widehat{\rho }_B=Tr_A[\widehat{\rho }_{AB}]`$ associated with a composite system $`AB`$ . Is is clear, however, from the studies reported in , that $`q`$-entropies do play a significant role in the investigation of entanglement phenomena. It is our intention in this Communication to investigate the degree of correlation between (i) the amount of entanglement $`E[\rho _{AB}]`$ exhibited by a two-qubits state $`\rho _{AB}`$, and (ii) the $`q`$-entropies (or $`q`$-information measures) of $`\rho _{AB}`$ (notice that we refer here to the total $`q`$-entropy of the density matrix $`\rho _{AB}`$ describing the composite system as a whole. We shall not consider conditional $`q`$-entropies). It is well known that the amount entanglement and the degree mixture (as measured by the $`q`$-entropies) of a state $`\rho _{AB}`$ are independent quantities. However, there is a certain degree of correlation among them. States with an increasing degree of mixture tend to be less entangled. In point of fact, all two-qubits states with a large enough degree of mixture are separable. We want to explore to what extent does the strength of the alluded to correlation depend upon the parameter $`q`$ characterizing the $`q`$-entropy used to measure the degree of mixture. In particular, we want to find out if there is a special value of $`q`$ yielding a better entropy-entanglement correlation than the entropy-entanglement correlations associated with other values of $`q`$. To such an end, and for the sake of completeness, a few words regarding measures of entanglement are necessary.

A physically motivated measure of entanglement is provided by the entanglement of formation $`E[\widehat{\rho }]`$ . This measure quantifies the resources needed to create a given entangled state $`\widehat{\rho }`$. That is, $`E[\widehat{\rho }]`$ is equal to the asymptotic limit (for large $`n`$) of the quotient $`m/n`$, where $`m`$ is the number of singlet states needed to create $`n`$ copies of the state $`\widehat{\rho }`$ when the optimum procedure based on local operations is employed. For the particular case of two-qubits states Wootters obtained an explicit expression for $`E[\widehat{\rho }]`$ in terms of the density matrix $`\widehat{\rho }`$ . Wootters’ formula reads

$$E[\widehat{\rho }]=h\left(\frac{1+\sqrt{1C^2}}{2}\right),$$
(1)
where $`h(x)=x\mathrm{log}_2x(1x)\mathrm{log}_2(1x)`$, and $`C`$ stands for the concurrence of the two-qubits state $`\widehat{\rho }`$. The concurrence is given by $`C=max(0,\lambda _1\lambda _2\lambda _3\lambda _4)`$, $`\lambda _i,(i=1,\mathrm{}4)`$ being the square roots, in decreasing order, of the eigenvalues of the matrix $`\widehat{\rho }\stackrel{~}{\rho }`$, with $`\stackrel{~}{\rho }=(\sigma _y\sigma _y)\rho ^{}(\sigma _y\sigma _y)`$. The above expression has to be evaluated by recourse to the matrix elements of $`\widehat{\rho }`$ computed with respect to the product basis.

Our investigations will be based upon a Monte Carlo exploration of $`𝒮`$: the set of all states, pure and mixed of a two-qubits system. To do this we need to define a proper measure on $`𝒮`$. The space of all (pure and mixed) states $`\rho `$ of a quantum system described by an $`N`$-dimensional Hilbert space can be regarded as a product space $`𝒮=𝒫\times \mathrm{\Delta }`$ . Here $`𝒫`$ stands for the family of all complete sets of orthonormal projectors $`\{\widehat{P}_i\}_{i=1}^N`$, $`_i\widehat{P}_i=I`$ ($`I`$ being the identity matrix). $`\mathrm{\Delta }`$ is the set of all real $`N`$-uples $`\{\lambda _1,\mathrm{},\lambda _N\}`$, with $`0\lambda _i1`$, and $`_i\lambda _i=1`$. The general state in $`𝒮`$ is of the form $`\rho =_i\lambda _iP_i`$. The Haar measure on the group of unitary matrices $`U(N)`$ induces a unique, uniform measure $`\nu `$ on the set $`𝒫`$ . On the other hand, since the simplex $`\mathrm{\Delta }`$ is a subset of a $`(N1)`$-dimensional hyperplane of $`^N`$, the standard normalized Lebesgue measure $`_{N1}`$ on $`^{N1}`$ provides a natural measure for $`\mathrm{\Delta }`$. The aforementioned measures on $`𝒫`$ and $`\mathrm{\Delta }`$ lead to a natural measure,

$$\mu =\nu \times _{N1},$$
(2)
on the set $`𝒮`$ of quantum states .

In the present investigation we deal with the case $`N=4`$. Our present considerations are based on the assumption that the uniform distribution of states of a two-qubit system is the one determined by the measure $`\mu `$. Thus, in our numerical computations we are going to randomly generate states of a two-qubits system according to the measure $`\mu `$ and study the relation between the entanglement properties of these states, on the one hand, and

* 1) the Tsallis $`q`$-entropy

$$S_q=\frac{1}{q1}\left(1\omega _q\right),\text{with}\omega _q=Tr\left(\widehat{\rho }^q\right),$$
(3)
and
* 2) the Rényi $`q`$-entropy

$$R_q=\frac{1}{1q}\mathrm{ln}[1+(1q)S_q],$$
(4)
on the other one.

Most recent research efforts dealing with the relationship between the degree of mixture and the amount of entanglement focus on the behaviour, as a function of the degree of mixture, of the entanglement properties exhibited by the set of states endowed with a given amount of mixedness. For instance, they consider the behaviour, as a function of the degree of mixture (as measured, for instance, by $`S_2`$), of the average entanglement of those states characterized by a given value of $`S_2`$. Here we are going to adopt, in a sense, the reciprocal (and complementary) point of view. We are going to study the behaviour, as a function of $`C^2`$, of the entropic properties associated with the set of states characterized by a given value of $`C^2`$. This vantage point will enable us to clarify some aspects of the $`q`$-dependence of the entanglement-mixedness correlation. In particular, we want to asses, for different $`q`$-values, how sensitive are the average entropic properties to the value of the entanglement of formation (or, equivalently, to the value of the squared concurrence $`C^2`$).

First of all, we have randomly generated a large number of states (according to the measure $`\mu `$ given by expression (2)) and plotted them, for several $`q`$-values, in the $`(C^2,R_q)`$-plane. Each point in Fig. 1 correspond to a particular state in the state space $`𝒮`$. The outcome is a series of “bands”, one for each $`q`$. The top band corresponds to $`q=0.5`$. At the bottom we find that for $`q=10`$. The remaining ones arrange themselves in between, in monotonic fashion. One appreciates the fact that, for the different $`q`$-values, we find, given a certain amount of entanglement as measured by $`C^2`$, states of larger and larger entropies $`R_q`$ as $`q`$ diminishes. From the point of view of information theory this would entail that information about our states is lost as $`q`$ decreases. If we now consider averages over all states that share a given concurrence we are led to consider Fig. 2.

We computed, as a function of $`C^2`$, the average value of the Rényi entropy $`R_q`$ associated with the set of states endowed with a given value of the squared concurrence $`C^2`$. The results are exhibited in Fig. 2 (solid lines), where the mean value $`R_q`$ is plotted against $`C^2`$, for $`q=0.5,\mathrm{\hspace{0.17em}1},\mathrm{\hspace{0.17em}2},\mathrm{\hspace{0.17em}10},`$ and $`\mathrm{}`$. As stated, the averages are taken over all the states $`\widehat{\rho }𝒮`$ that are characterized by a fixed concurrence-value. For all $`q`$ the average entropies diminish as $`C`$ grows. This behaviour is consistent with the fact that states of increasing entropy tend to exhibit a decreasing amount of entanglement . As $`q`$ grows, the average entropy decreases, for any $`C^2`$, although the decreasing tendency slows down for large $`q`$-values. Many recent efforts dealing with the relationship between $`q`$-entropies and entanglement were restricted to states $`\rho _{\mathrm{Bell}}`$ diagonal in the Bell basis. For such states, both the $`R_q`$ entropy and the squared concurrence $`C^2`$ depend solely upon $`\rho _{\mathrm{Bell}}`$’s largest eigenvalue, so that $`R_q`$ can be expressed as a function of $`C^2`$. The dashed line in Fig. 2 depicts the functional dependence of the $`R_{\mathrm{}}`$ Rényi entropy, as a function of $`C^2`$, for two-qubits states diagonal in the Bell basis. It is instructive to compare, in Fig. 2, the curve corresponding to states diagonal in the Bell basis with the curve corresponding (with $`q=\mathrm{}`$) to all two-qubit states. It can can be appreciated that these two curves, even if sharing the same qualitative appearance, differ to a considerable extent.

For the sake of comparison, we plotted in Fig. 3 the mean value $`S_q`$ of Tsallis’ entropy, as a function of $`C^2`$, for $`q=0.5,\mathrm{\hspace{0.17em}1},\mathrm{\hspace{0.17em}2},`$ and $`10`$. Again, for each value of $`C^2`$, the entropy’s average was computed over all those states characterized by that particular $`C^2`$-value. Notice that for large $`q`$-values, the Tsallis entropy is approximately constant for all $`C^2`$ values, while the Rényi one seems to be much more sensitive in this respect. Entropies tend to vanish for $`C^21`$, because only pure states can reach the maximum concurrence value. In the inset of Fig. 3 we depict the behaviour of $`S_q_{C^2}`$ as a function of $`1/q`$ for a given value of the concurrence ($`C^2=0.6`$), thus illustrating the fact that the mean entropy is a monotonically decreasing function of $`q`$. For large $`q`$-values the Tsallis entropy cannot discriminate between different degrees of entanglement for states with $`C^2<1`$, while Rényi’s measure can do it. This fact is related to an important difference between the behaviours, as a function of the parameter $`q`$, of Rényi’s $`R_q`$ and Tsallis’ $`S_q`$ entropies. The maximum value $`R_q^{\mathrm{max}}`$ attainable by Rényi’s entropy (corresponding to the equi-probability distribution) is independent of $`q`$,

$$R_q^{\mathrm{max}}=\mathrm{ln}N,$$
(5)
where $`N`$ is the total number of accesible states. On the contrary, the maximum value reachable by $`S_q`$ does depend upon $`q`$,

$$S_q^{\mathrm{max}}=\frac{1N^{1q}}{(q1)}.$$
(6)
Clearly, $`S_q^{\mathrm{max}}0`$ for $`q\mathrm{}`$. One may think that the $`q`$-dependence of $`S_q^{\mathrm{max}}`$ may be appropriately taken into account if one considers (instead of Tsallis’ entropy itself), a normalized Tsallis’ entropy (see Fig. 4),

$$S_q^{}=\frac{S_q}{S_q^{max}},$$
(7)
For instance, in the case of two qubits one has,

$$S_q^{max}=\frac{14^{1q}}{(q1)},$$
(8)
and we deal then with

$$S_q^{}=\frac{1Tr[\widehat{\rho }^q]}{14^{1q}}=\frac{1\{[Tr(\widehat{\rho }^q)]^{1/q}\}^q}{14^{1q}}.$$
(9)
Consider now the limit $`q\mathrm{}`$ for a density matrix $`\widehat{\rho }`$ corresponding to a state of fixed concurrence $`C`$. In such a process one immediately appreciates the fact that $`[Tr(\widehat{\rho }^q)]^{1/q}\lambda _{max}`$, where $`\lambda _{max}`$ is the largest eigenvalue of $`\widehat{\rho }^q`$. Thus, the limiting value we reach is

$$S_q^{}[1(\lambda _{max})^q],$$
(10)
and we see that this is always equal to unity for all $`C^2<1`$ and vanishes exactly if $`C^2=1`$ (see Fig. 4). Consequently, even employing the normalized $`S_q^{}`$, the information concerning the entropy-entanglement correlation tends to disappear in the $`q\mathrm{}`$ limit.

We see that, with regards to the analysis of the entropy-entanglement correlations of quantum bipartite systems (remember that here we are talking about the total entropy of the whole composite system), Tsallis’ and Rényi’s entropies behave in different ways. It is instructive to compare this behaviour of the $`q`$-entropies, to their behaviour with regards to the relationship between separability and conditional $`q`$-entropies. What matters in this last case is the sign of the conditional $`q`$-entropies. If a classical composite system $`A\times B`$ is described by a suitable probability distribution $`\{p_{AB}\}`$ (defined over the concomitant phase space), the $`q`$-information measure (or $`q`$-entropy) associated to the whole system is always equal or greater than that pertaining to its subsystems, i.e., those associated to $`\{p_A\}`$ or $`\{p_B\}`$. In other words, the conditional entropy

$$S_q[A|B]=S_q[p_{AB}]S_q[p_B],$$
(11)
is always positive. This is also the case for separable states $`\widehat{\rho }_{AB}`$ of a composite quantum system $`AB`$ . In contrast, a subsystem of a quantum system described by an entangled state may have an entropy greater than the entropy of the whole system. That is to say, entangled states may have negative conditional $`q`$-entropies. Now, since Rényi’s entropy is a monotonically increasing function of Tsallis’ measure, it is clear that the sign of the conditional Rényi’s entropy associated with a quantum state $`\widehat{\rho }_{AB}`$, $`R_q[A|B]=R_q[\widehat{\rho }_{AB}]R_q[\widehat{\rho }_B]`$, will be the same as the sign of the conditional Tsallis’ entropy, $`S_q[A|B]=S_q[\widehat{\rho }_{AB}]S_q[\widehat{\rho }_B]`$. Hence, as far as the relationship between conditional entropies and separability (which depends only upon the sign of the conditional $`q`$-entropies) is concerned, Tsallis’ and Rényi’s measures are equivalent.

Returning to our discussion of the connection between entanglement and (total) $`q`$-entropies of bipartite quantum systems, we have seen that Rényi’s entropy is particularly well suited for (i) discussing the $`q\mathrm{}`$ limit and (ii) studying the $`q`$-dependence of the entropy-entanglement correlations. For these reasons, in the rest of the present contribution we will focus upon Rényi entropy.

We tackle now the question of the dispersion around these entropic averages. Fig. 5 is a graph of the dispersions

$$\sigma _q^{(R)}=\left[R_q^2R_q^2\right]^{1/2},$$
(12)
as a function of $`C^2`$, for the same $`q`$-values of Fig. 2. We see that the size of the dispersions diminishes rather rapidly as $`C^2`$ increases towards unity. Also, dispersions tend to become smaller as $`q`$ grows. This suggests that, as $`q`$ increases, the correlation between $`R_q`$ and entanglement improves. A similar tendency, but in the case of $`S_q`$, was detected in .

In order to estimate in a quantitative the sensitiveness of the average $`q`$-entropy to changes in the value of $`C^2`$, we computed the derivatives with respect to $`C^2`$ of the average value of Rényi’s entropy associated with states of given $`C^2`$,

$$\frac{dR_q}{d(C^2)}.$$
(13)
In Fig. 6 we plot the above derivatives, against $`C^2`$, for $`q=0.5,1,2,10`$, and $`\mathrm{}`$. These derivatives fall abruptly to zero, in the vicinity of the origin, as $`C^2`$ diminishes. As a counterpart, for all $`q`$, the derivatives exhibit a rapid growth with $`C^2`$ for small values of the concurrence. This growing tendency stabilizes itself and, for $`q`$ large enough, saturation is reached.

Now let us assume that we know the value of the entropy $`R_q[\rho ]`$ of certain state $`\rho `$. How useful is this knowledge in order to infer the value of $`C^2`$?. In other words, how good is $`R_q`$ as an “indicator” of entanglement? It has been suggested that $`q=\mathrm{}`$ provides a better “indicator” of entanglement than other values of $`q`$ . There are two ingredients that must be taken into account in order to determine the $`q`$-value yielding the best entropic “indicator” of entanglement. On the one hand, the sensitivity of the entropic mean value $`R_q`$ to increments in $`C^2`$, as measured by the derivative $`dR_q/d(C^2)`$. On the other hand, the dispersion $`\sigma _q^{(R)}`$, given by (12). A given $`q`$-value would lead to a good entropic “indicator” if it corresponds to (i) a large value of $`dR_q/d(C^2)`$, and (ii) a small value of $`\sigma _q^{(R)}`$. These two factors are appropriately taken into account if we compute the ratio

$$r=\left|\frac{\sigma _q^{(R)}}{dR_q/d(C^2)}\right|,$$
(14)
between the dispersions depicted in Fig. 5 and the derivative of Fig. 6. The ratio $`r`$ provides a quantitative measure for the strength of the entropic-entanglement correlations. The quantity $`r`$ constitutes an estimate of the smallest increment $`\mathrm{\Delta }C^2`$ in the squared concurrence which is associated with an appreciable change in $`R_q`$. In order to clarify this last assertion, an analogy with the uncertainty associated with the measurement of time in quantum mechanics can be established. Let us assume that we can measure an observable $`\widehat{A}`$. Then, the time uncertainty $`\mathrm{\Delta }t`$ depends upon two quantities, (i) the time derivative of the expectation value of the observable, $`d\widehat{A}/dt`$, and (ii) the uncertainty of the observable, $`\mathrm{\Delta }\widehat{A}=[\widehat{A}^2\widehat{A}^2]^{1/2}`$. The time uncertainty is given by

$$\mathrm{\Delta }t=\frac{\mathrm{\Delta }\widehat{A}}{d\widehat{A}/dt}$$
(15)
The above expression for $`\mathrm{\Delta }t`$ gives an estimation of the smallest time interval that can be detected from measurements of the observable $`\widehat{A}`$. In the analogy we want to establish, $`C^2`$ plays the role of $`t`$, and $`R_q`$ plays the role of the observable $`A`$. The ratio $`r`$ is depicted in Fig. 7, as a function of $`C^2`$, for $`q=1`$ and $`q=\mathrm{}`$. The two upper curves in Fig. 7 correspond to the $`r`$-values obtained when all the states in the two-qubits state-space $`𝒮`$ are considered. On the other hand, the lower curves are the ones obtained when the computation of $`r`$ is restricted to states diagonal in the Bell basis. When all states in $`𝒮`$ are considered, the values of $`r`$ associated with $`q=\mathrm{}`$ are seen to be smaller than the values corresponding to $`q=1`$, which can be construed as meaning that the $`q`$-entropies with $`q=\mathrm{}`$ can indeed be regarded as better “indicators” of entanglement than the $`q`$-entropies associated with finite values of $`q`$, as was previously suggested in . Alas, the results depicted in Fig. 7 indicate that this improvement of the entropy-entanglement correlation associated with $`q=\mathrm{}`$ is not considerable. The usefulness of $`q`$-entropies with $`(q\mathrm{})`$ as an “indicator” of entanglement was proposed in  on the basis of the behaviour of states diagonal in the Bell basis. As already mentioned, the squared concurrence $`C^2`$ of states $`\rho _{\mathrm{Bell}}`$ diagonal in the Bell basis can be expressed as a function of $`R_{\mathrm{}}`$, since both these quantities depend solely on the largest eigenvalue $`\lambda _m`$ of $`\rho _{\mathrm{Bell}}`$ (in particular, $`R_{\mathrm{}}=\mathrm{ln}\lambda _m`$). This means that, as pointed out in , for states diagonal on the Bell basis there is a perfect correlation between $`C^2`$ and $`(q=\mathrm{})`$-entropies (and, consequently, $`r`$ vanishes). This implies that, when restricting our considerations only to states diagonal in the Bell basis, the entropy-entanglement correlation is much more strong for $`q=\mathrm{}`$ than for other values of $`q`$. States diagonal in the Bell basis are important for many reasons, but their properties are by no means typical of the totality of the state-space $`𝒮`$. See for instance, as depicted in Fig.7, the behavior of $`r`$ (for $`q=1`$) associated with (i) all states in $`𝒮`$ and (ii) states diagonal in the Bell basis. There are remarkable differences between the two cases.

We thus find ourselves in a position to assert that the relationship between the $`q`$-entropies and the amount of entanglement exhibited by the family of states diagonal in the Bell basis does not constitute a reliable guide to infer the typical behavior of states in the two-qubits state-space $`𝒮`$. When considering the complete state-space $`𝒮`$, the $`q=\mathrm{}`$-entropies turn out to be only a slightly better, as entanglement “indicators”, than the entropies associated with other values of $`q`$.

We summarize now our present considerations. By recourse to a Monte Carlo procedure we have studied the $`q`$-dependence of the correlations exhibited by two-qubits states between (i) the amount of entanglement and (ii) the $`q`$-entropies. It was previously conjectured by other researchers, on the basis of the study of states diagonal in the Bell basis, that the $`q`$-entropies associated with $`q=\mathrm{}`$ are better “indicators” of entanglement than the entropies corresponding to finite values of $`q`$. In other words, it was suggested that the $`q`$-entropy with $`q=\mathrm{}`$ exhibits a stronger correlation with entanglement than the other $`q`$ entropies. By a comprehensive numerical survey of the complete (pure and mixed) state-space of two-qubits, we have shown here that the alluded to conjecture is indeed correct. However, when globally considering the whole state-space the advantage, as an entanglement indicator, of $`(q=\mathrm{})`$-entropy turns out to be much smaller than what can be inferred from the sole study of states diagonal in the Bell basis. This constitutes an instructive example of the perils that entails trying to infer typical properties of general two-qubits states from the study of just a particular family of states, such as those diagonal in the Bell basis.

###### Acknowledgements.

This work was partially supported by the MCyT grant BFM2002-03241 (Spain), and by CONICET (Argentine Agency). One of us (ARP) thanks financial support from the MECyD grant SAB2001-0106.

FIGURE CAPTIONS

Fig.1- Rényi entropy $`R_q`$ vs. the squared concurrence $`C^2`$ for all two-qubits states and several $`q`$ values. All depicted quantities are dimensionless.

Fig.2- Average value of the Rényi entropy $`R_q`$ of all states with a given squared concurrence $`C^2`$, as a function of $`C^2`$, and for several $`q`$-values (solid lines). The dashed line depicts the functional dependence of the $`R_{\mathrm{}}`$ Rényi entropy, as a function of $`C^2`$, for two-qubits states diagonal in the Bell basis. All depicted quantities are dimensionless.

Fig.3- Average value of the Tsallis’ entropy $`S_q`$ of all states with a given squared concurrence $`C^2`$, as a function of $`C^2`$, and for several $`q`$-values. The inset shows $`S_q`$ vs. $`1/q`$ for the particular value of the squared concurrence $`C^2=0.6`$. All depicted quantities are dimensionless.

Fig.4- Average value of the normalized Tsallis entropy $`S_q/S_{q\mathrm{max}}`$ vs. $`C^2`$, for several $`q`$-values. All depicted quantities are dimensionless.

Fig.5- Dispersion of the Rényi entropy $`\sigma _q^{(R)}=\left[R_q^2R_q^2\right]^{1/2}`$ for all qubits states with a given $`C^2`$, as a function of $`C^2`$, and for several $`q`$-values. All depicted quantities are dimensionless.

Fig.6- The derivative $`dR_q/d(C^2)`$, as a function of the squared concurrence $`C^2`$, for several values of the $`q`$-parameter. All depicted quantities are dimensionless.

Fig.7- The absolute value of the quotient $`r=\left|\frac{\sigma _q^{(R)}}{dR_q/d(C^2)}\right|`$, as a function of the squared concurrence $`C^2`$, for $`q=1`$ and $`q=\mathrm{}`$. The two upper curves correspond to all states in the two-qubit state-space $`𝒮`$. The lower curves correspond to states diagonal in the Bell basis. All depicted quantities are dimensionless.


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# Radio galaxies: unification and dust properties

## 1 Introduction

Unification of active galaxies combines the mechanisms of relativistic beaming in radio jets (when present – the radio-loud objects) with anisotropy due to dust shadowing or non-spherical optically thick emission; key parameter is the aspect angle. These geometric effects, in interplay with source evolution – youth, adulthood, seniority, as well as duty cycle – provide the full framework in which we seek to explain the active galaxy populations.

In case of Seyfert galaxies, an optically thick torus was invoked in the mid 1980’s to explain the apparent differences (strength of continuum and emission line radiation) between Seyfert’s of Types 1 and 2. As for the radio-loud population of radio galaxies and quasars such tori were postulated in combination with relativistic effects in their radio jets. The model whereby quasars and BLLac objects are favourably oriented radio galaxies has drawn considerable interest: the unification church still has many members. The review articles by Antonucci (1993) and Urry & Padovani (1995) provide excellent accounts of these models. Increased attention has been paid in the last decade to the subject of life-time evolution of active galaxies and AGN: some of that work will be dealt with here, while Biretta et al. (2002) provide an excellent full account. For a nice up-to-date summary of the general aspects of unification studies we refer to the Proceedings of the Elba workshop ”Issues in Unification of AGN” (Maiolino et al., 2002).

In this short review we will discuss new evidence from the past decade in favour or against unification of active galaxies. Furthermore, we will examine the infrared properties of active galaxies, in order to gain insight in the physical behaviour of the dusty toroid.

## 2 Status of radio-loud unification models

Aspect being the key parameter in geometric unification, how do we know the aspect angle to or the inclination of an active galactic nucleus? Here radio-loudness helps because the fractional radio core strength (radio core strength normalized with total radio or extended radio luminosity) – obviously taken from kpc-resolution radio images – provides a reasonably good orientation indicator. As pointed out by Wills & Brotherton (1995), the optical core luminosity normalized with the total radio luminosity provides an additional, improved orientation indicator. In addition, radio-loud objects provide us with a radio (jet) axis: radio images permit determination of the projected source axis so only the inclination angle w.r.t. this jet axis is unknown. While radio-quiet objects occasionally display optical cone emission yielding the optical axis, that axis is generally less well constrained.

As such, unification models for radio-loud objects are further developed and encompass more seemingly different classes. Within the framework of this radio-loud meeting we will concentrate on the radio-loud populations, but mention results for radio-quiet objects where relevant.

### 2.1 FR I unification

The model whereby Fanaroff & Riley Class I radio galaxies at small inclination manifest themselves as BL Lacertae objects has gained considerable support from HST observations of the former. Ultraviolet/optical cores in FR I host galaxies were found to correlate with their radio cores arguing for a common, beamed synchrotron origin (Capetti et al., 2002). No evidence for slower milli-arcsec scale jets in comparison to FR II radio galaxies was found: FR I jets – or their relativistic spines – must slow down from the parsec to the kiloparsec scale (e.g., Giovannini et al., 2001). Dust disks are often observed in FR I hosts galaxies: their optical depth is much lower as compared to the opaque circumnuclear tori postulated in FR II radio galaxies (Chiaberge et al., 2002). Added to the apparent absence of broad line emission in FR I radio galaxies (at least: luminous BLR – see e.g., Corbett et al., 2000), this may mark an important distinction between the Fanaroff & Riley classes, but the distinction is blurred (e.g., Blundell & Rawlings, 2001). Further evidence is provided by the far-infrared SEDs: FR I’s are generally less far-infrared-bright than FR II’s at comparable radio luminosity (Heckman et al., 1994), by a moderate factor of $``$4. Note that the broadband optical photometric host properties differ little or nothing (Ledlow et al., 2002) and that the masses of the central black holes have no connection to radio luminosity whatsoever (e.g., Woo & Urry, 2002) – it is most likely the accretion mechanism itself that will determine the FR nature of the radio galaxy.

Backyard FR I Centaurus A was studied in quite some detail and found to conform to the unification model (e.g., Capetti et al., 2000; Chiaberge et al., 2001). Whysong & Antonucci (2002) did however point out differences between archetypal FR I’s Centaurus A and Virgo A (M 87).

### 2.2 FR II unification

Barthel (1993) found substantial supportive evidence for the favourable orientation of all radio-loud quasars; most of this evidence has become stronger. This is however not equivalent with the picture whereby all FR II radio galaxies contain a QSO hidden from direct view. In fact, the evidence for the existence of a population of FR II pure-radio-galaxies – without a big blue bump – has grown. Such a population of optically ”dull” FR II radio galaxies, in which the nuclear accretion activity is currently switched off or at a low level, together with the astrophysically attractive model of a receding torus (e.g., Simpson in these Proceedings) may well account for the reported number density and linear size incompatibilities between FR II radio galaxies and quasars.

Investigations into possible orientation invariants, à la Hes et al. (1996) and Baker (1997) continue to be important. Relatively weak \[OIII\] emission may be due to obscuration but also to a weak ionizing spectrum (e.g., Tadhunter et al., 1998). With regard to the invariance issue, the mid- and far-infrared emission remains controversial. It is still not clear to what extent this emission is suitable to test and/or constrain unification models (e.g., van Bemmel et al., 2000); see Sect. 5. The multi-component, partly anisotropic nature of the far-infrared radiation nevertheless does not provide major inconsistencies with unification models; it is however likely that a cool dust component, related to host star-formation activity plays a significant additional role.

Beautiful radiation cones have been reported, in objects varying from the nearest Seyfert galaxies to high redshift radio galaxies. These provide clear evidence for anisotropic nuclear radiation fields, with an added component of jet driven star-formation (of difficult to determine magnitude). The strength of the latter is – not surprisingly – related to the size of the radio source (e.g., Best et al., 2000). However, in the powerful radio galaxy Cygnus A there is solid evidence that the ionization cones seen in optical images are generated by an outflow, driven by the radiation pressure of the central quasar (van Bemmel, 2002).

As for the host galaxies, the HST studies carried out by the Edinburgh group have yielded strong support for the FR II unification, and also the K($`z`$) behaviour provided consistency – see the contribution by McLure in these Proceedings. HST and ground-based studies of radio galaxy hosts by de Vries and collaborators provide in addition consistency with evolutionary models for the growth of radio sources; see Sect. 3.

Obscured AGN are required by the X-ray background: this was already pointed out in the late 1980’s and the evidence is still strong (e.g., Comastri et al., 1995). X-ray spectra will soon yield the cosmologically evolving obscuration, including the contribution from highly obscured AGN (Fabian, in Maiolino et al., 2002).

Spectropolarimetry provides the tool to proof unification. Following up on the beautiful early work by Miller, Antonucci c.s., both the Caltech and the Hatfield group obtained these proofs, for an as yet small number of objects. Polarization and obscuration/reddening appear to go hand-in-hand, cf. the models (e.g., Young et al., 1996; Cohen et al., 1999).

Observations of the archetypal FR II narrow-line radio galaxy Cygnus A were wonderfully revealing: its radiation cones were imaged with HST (e.g., Jackson et al., 1998; Tadhunter et al., 1999) whereas the hidden BLR was detected with spectropolarimetry (Ogle et al., 1997). We stress however that ultraluminous backyard radio source Cygnus A harbours a QSO of only moderate strength!

## 3 Effects of source evolution

Considerable effort was spent to study the nature of compact radio sources. These objects, of the Gigahertz-Peaked Spectrum (GPS) and Compact Steep-Spectrum (CSS) classes, are now thought to represent the progenitors of the large classical doubles. Whereas the latter display radio structure of supergalactic ($`>100`$kpc) dimensions, the former are subgalactic – typically a few tens of kpc for the CSS and a few tens of pc for the GPS class. See also the contribution by Snellen in these Proceedings. Noteworthy is the determination of the spectral ages of several CSS objects (Murgia et al., 1999) which appear in agreement with their postulated youth. Cold H I gas has been detected in several CSS radio galaxies (e.g., the contribution by Vermeulen in these Proceedings); the CSS quasar class displays pronounced associated CIV absorption (Baker et al., 2002). Combined with the fact that some CSS radio galaxies and quasars radiate unusually strong far-infrared emission this has been postulated to imply a young evolutionary stage with strong star-formation (Baker et al., 2002). Well-known CSS quasar 3C 48 provides an excellent example (Canalizo & Stockton, 2000). It is likely that the radio jets, trying to find their way through the circumnuclear ISM play an important role (e.g., O’Dea et al., 2002). True (proper motion) expansion velocities, of order 100 km/sec, for compact radio galaxies have been measured, arguing for their very young ages (e.g., Owsianik et al., 1999) and a nice case of a reborn GPS in a large double lobed radio galaxy was recently reported (Marecki et al., 2002). Radio source number density data require an increasing expansion speed and/or decreasing radio luminosity with age – to tie this down, the evolutionary models for extragalactic radio sources are currently being investigated with larger samples. Overall, the global host galaxy properties of compact and large scale radio galaxies do not show inconsistencies with the evolutionary models (de Vries et al., 2000).

Support for the occurrence of recurrent nuclear activity (duty cycle ?) is slowly accumulating (e.g., Schoenmakers et al., 2000). Given the general occurrence of massive black holes in luminous galaxies (e.g., Magorrian et al., 1998), such repetitive activity triggered by repetitive fueling is not unexpected. A multi-wavelength approach including deep optical imaging seems at order.

Broad-line radio galaxies make up an important subset of the radio galaxy population. Their nature is most likely composite: the class encompasses low-luminosity QSRs, possibly with different torus opening angles as compared to high luminosity QSRs, as well as radio galaxies with somewhat transparent, porous tori (Tadhunter et al., 1998; Dennett-Thorpe et al., 2000). van Bemmel & Barthel (2001) point out that BLRGs are characterized by the absence of star-formation: one explanation could be that some BLRG represent old, dying radio galaxies. The absence of optical synchrotron (jet) components in some BLRGs (Chiaberge et al., 2002) may be consistent with that view.

## 4 Very dusty sources

Intriguing recent development is the detection in X-rays of active nuclei in seemingly non-active galaxies, apart from their dusty starburst nature: NGC4945 (e.g., Guainazzi et al., 2000) and NGC6240 (Iwasawa & Comastri, 1998). Such highly obscured AGN are important in the possible evolutionary connection between starburst galaxies and AGN and may be important contributors to the X-ray background – ongoing Chandra and XMM-Newton investigations will undoubtedly shed light on these issues.

Noting that dust obscuration lies at the heart of unification models, we proceed by reviewing the status of torus models.

## 5 Modelling the toroid in AGN

### 5.1 Introduction

Key to the unification model is the obscuring torus, creating an angle and wavelength dependent anisotropy in active galaxies. The soft X-ray and UV emission from the central engine is reprocessed to infrared wavelengths by the dust in the torus. In 1983 IRAS was the first satellite to detect infrared emission from the relatively distant active galaxies. Soon after, several groups started to model this reprocessing using radiative transfer codes. Among the first to present their models are Pier & Krolik (1992), hereafter PK92. A few years later they are followed by Granato & Danese (1994), hereafter GD94 and Efstathiou & Rowan-Robinson (1995), hereafter ER95, and recently models have appeared by Nenkova et al. (2002) and van Bemmel & Dullemond (2003), hereafter BD03. The ISO satellite provided a wealth of additional data, however, only for the Seyfert galaxies these allow a good constraint of the models. For the radio-loud AGN population only few objects have a well defined broad-band SED, e.g. Cygnus A.

### 5.2 The early models: PK92, GD94 and ER95

To ease the radiative transfer calculations, all groups assume azimuthal symmetry, but the actual torus geometries differ among the different groups. PK92 define a so-called pill-box geometry, where the thickness of the torus is constant with radius, and the inner walls are perpendicular to the plane of the toroid. GD94 use a similar geometry, but with the possibility of having a conical hole in the center, instead of perpendicular walls. They also allow for different dust mixtures to be present in the torus. ER95 use three different geometries: a conical disk, where the thickness of the disk increases linearly with radius, an anisotropic sphere, and a pillbox with a conical hole. In all their models, the torus has a constant inner radius, causing the central opening to be circular (the opposite of the GD94 central cavity). All these ’early’ models assume Galactic dust properties.

### 5.3 The silicate problem

All three groups predict significant 10 $`\mu `$m silicate emission in type 1 active galaxies, which is not observed. The more powerful radio-loud population still lacks proper spectra, but the absence of 10 $`\mu `$m emission is well established by the ISO spectrometers for the Seyfert type AGN. GD94 postulate depletion of small grains by shocks in order to explain the lack of 10 $`\mu `$m emission in type 1’s. Only one of the ER95 pill-box model does not predict 10 $`\mu `$m emission.

This leads several groups to the conclusion that AGNs do not contain standard Galactic dust. The grain size distribution might differ significantly from the Galactic distribution, in the sense that AGN toroid dust is dominated by larger grains. This is first recognized by Laor & Draine (1993), and several groups have brought forth explanations for this. From UV spectra it becomes clear that also the 2200 Å absorption is shallower than expected in many AGN, consistent with the lack of small grains (Maiolino et al., 2001a).

Small grains are easily destroyed in the strong radiation field of an active nucleus. However, they should survive in the regions shielded by the torus. Several reasons have been presented in literature for the lack of small grains in AGN: most recently a clumping theory is presented by Maiolino et al. (2001b). The grains are swept up by the radiation pressure, and clump together to form larger grains.

### 5.4 The width problem

The early models encounter a second problem in explaining the full width of the broad-band SED observed in all types of active galaxies. Although the results from the models are generally broader than a single grey body, due to the temperature gradient in the dust, most of them are not yet broad enough. PK92 recognize this problem, and both GD94 and ER95 have tried to improve, but did not succeed.

### 5.5 A second component?

To deal with these issues, recent models have appeared in which the dust is no longer smooth, but clumpy (Nenkova et al., 2002), or has a non-Galactic grain size distribution (BD03). Both sets of models can produce the full observed width of the infrared SED of active galaxies, and both manage to circumvent significant 10 $`\mu `$m emission in models at small inclinations.

However, observational evidence is mounting that not all the infrared emission in active galaxies arises from the compact torus (see e.g., Spinoglio et al., 2002; Prieto et al., 2001). There must be a significant contribution from a second dust component, which seems to be related to star-formation in the host galaxy, i.e. at scales much larger than the radius at which the AGN can influence the dust. So far, all papers have ignored this possibility, except BD03. Such a second component may well provide a solution to the width problem in the early models. BD03 provide colour-colour diagrams for their models, showing that the observed 25–60 and 60–100 $`\mu `$m colours are not well fitted by single component torus models, and demand an additional dust component.

This secondary dust component might also be responsible for the lack of silicate emission observed in type 1 AGN; if the torus does produce 10 $`\mu `$m emission but this passes through a colder layer of dust, the resulting spectrum shows no 10 $`\mu `$m emission, or even a shallow absorption. However, this would require a large scale, spherical dust screen that covers all viewing angles to the nuclear regions. In the case of NGC 1068 there is no evidence of large scale silicate absorption: the nucleus seems to be the main source of the absorption. However, in this object the star-formation provides only a marginal fraction of the total infrared luminosity (Marco & Brooks, 2003), whereas it is thought to contribute at least 50% to the far-infrared emission in powerful radio sources.

For a proper understanding of dust in the nuclear regions of AGN the relative contributions of large and small scale dust need to be assessed. Decomposition will result in a better understanding of the behaviour of dusty tori in active galaxies, but also of the properties of the dust associated with star-formation in the host galaxies. Although the current generation of models is roughly consistent with observations, many important issues need to be solved. For this purpose, deep SIRTF low resolution spectroscopy data will be most welcome.

## 6 Conclusions

Good progress has been made during the past decade regarding aspect angle unification of radio-loud objects. The basic picture is correct, but the distinction between various classes appears somewhat blurred. The actual torus, big blue bump, and jet set-up, connected to source power and lifetime evolution, is not yet understood. The infrared might provide valuable clues, but we first need to understand how the various components contribute to the overall SED.

Acknowledgements
We acknowledge expert reading by healthy Ski Antonucci noting in passing that he fell ill just before the Workshop, leading the SOC to request the present reviewers to take over Ski’s review talk at 48h notice ….. The authors realize that this review is far from complete and does no justice to many active workers in the field. Apologies to those outside the review cone ….


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# Titanium additions to 𝑀𝑔𝐵₂ conductors

## I Introduction

Shortly after the discovery of superconductivity in $`MgB_2`$, small wire segments of this compound were prepared by reacting commercial $`B`$ fibers in a $`Mg`$ vapor. Typically these wire segments of pure $`MgB_2`$ will carry current densities, $`J_c`$, in the range of a few hundred thousand $`A/cm^2`$ in self field and $`5K`$. Fully reacted wire segments were consistently found to show critical current densities, $`J_c`$ ranging from $`100kA/cm^2`$ to $`500kA/cm^2`$ at $`5K`$ and magnetic fields in the range of $`0.1T`$ with a drop by a factor of about $`100`$ as the magnetic field increases to $`3T`$.

In light of the early success of the $`Mg`$ vapor diffusion method of sample preparation, a more detailed study of the of the $`MgB_2`$ growth processwas undertaken and has shown that as $`Mg`$ diffuses into $`B`$, a wall of $`MgB_6`$ sweeps across the boron fiber, followed by a wall of $`MgB_4`$, and finally a wall of $`MgB_2`$. Energy dispersive spectra ($`EDS`$) in a scanning electron microscope ($`SEM`$) have shown that the $`Mg`$ content is rather uniform across any given phase and rises abruptly at the phase boundary. For example, in a region containing both $`MgB_4`$ and $`MgB_2`$, the $`Mg`$ concentration as measured by a $`1\mu m`$ diameter EDS beam is rather uniform in the $`MgB_4`$ region and then rises abruptly at the interface between the $`MgB_4`$ and $`MgB_2`$ regions within the resolution of the $`EDS`$ probe of $`1`$ to $`2\mu m`$. Then, it is again rather uniform through the $`MgB_2`$ region.

Very successful $`Ti`$-doping experiments were reported by Zhao et al. using a solid state reaction method in which powders of $`Mg`$, $`Ti`$, and $`B`$ were mixed, pressed, and reacted on an $`MgO`$ plate in flowing $`Ar`$ gas. Best results were found for a $`Ti/Mg`$ ratio of about $`0.1`$ which showed $`J_c2\times 10^6A/cm^2`$ at $`5K`$ and zero field. Another recent paper by Wang et al. shows that $`Y_2O_3`$ nano-particles can greatly enhance the irreversibility field and $`J_c`$ performance of $`MgB_2`$ in the $`34T`$ range for samples prepared by a powder-in-tube method. In an alternate approach, Komori et al. have used a pulsed laser deposition method to prepare $`0.5\mu m`$ thick films of $`MgB_2`$ on a buffered flexible substrate that carry about $`100,000A/cm^2`$ at $`4.2K`$ and $`10T`$. These thick films are special because the grain size is in the nanometer range and $`J_c`$ remains high out to $`10T`$.

The purpose of the work reported here is to explore the use of continuous $`CVD`$ methods to dope the $`MgB_2`$ phase. It is important to increase both the upper critical field, $`H_{c2}`$ and the critical current densities in high field by shortening the mean-free-path of the electrons and by adding suitable pinning centers for the superconducting vortices. Impurities tend to suppress the transition temperature, $`T_c`$, so it is important to find a trade-off such that the $`T_c`$ is not reduced too much, but the critical field and critical current are substantially improved. The goal is to find suitable impurities and convenient methods to uniformly disperse them so that the $`J_c`$ values increase with relatively little suppression of $`T_c`$. Emphasis is on chemical vapor deposition processing of the $`B`$ and vapor diffusion of $`Mg`$ to form the $`MgB_2`$ conductor.

## II Experiment

A variety of methods have been used to introduce both point defects and small precipitates that will both shorten the electronic mean free path and provide small precipitates. To produce $`Ti`$ impurites, the $`Ti`$ and $`B`$ are co-deposited in a reel-to-reel CVD chamber. Two different substrates were used for the co-deposition of $`B`$ and $`Ti`$. In some experiments, the substrate is a $`W`$ wire. A $`15\mu m`$ diameter $`W`$ continuous filament enters the $`CVD`$ chamber in which a mixture of $`BCl_3`$ and $`H_2`$ are flowing. The conductor is electrically heated to peak temperatures of $`1100^{}C`$ and either pure $`B`$ or $`B`$-$`Ti`$ mixtures can be deposited. Titanium is added by bubbling the hydrogen component through $`TiCl_4`$ held at a temperature near $`0^{}C`$. The resulting partial pressure of $`TiCl_4`$ is approximately $`2\times 10^3`$ bar. The $`Ti`$ level is set by the temperature of the $`TiCl_4`$. In other experiments, the substrate for boron deposition was a $`75\mu m`$ diameter $`SiC`$ filament coated with several micrometers of glassy carbon known commercially as $`SCS9a`$. The $`CVD`$ coated fibers were spooled continuously on emerging from the reactor. After co-deposition of $`B`$ and $`Ti`$, X-ray patterns show both $`TiB`$ and $`TiB_2`$ in the fibers. The boron is transformed to $`MgB_2`$ by immersion in $`Mg`$ vapor as previously reported.. For the $`Ti`$-doped samples, more details of the structure and $`Ti`$ distribution has been presented elsewhere.

Critical current values were determined from magnetization hysteresis loops using the Bean Model for cylindrical geometry by

$$J_c=\frac{1.5\mathrm{\Delta }M}{r_o[1r_i^3/r_o^3]}$$
$`1`$
where $`\mathrm{\Delta }M`$ in A/m is the difference in magnetization for field increasing and field decreasing, $`r_o`$ is the outer radius of the superconductor, and $`r_i`$ is the inner radius measured in m. Magnetization measurements were made in a Quantum Designs SQUID magnetometer. Both $`MvsT`$ and the $`MvsH`$ hysteresis loops were measured sequentially on the same sample.

## III Results and discussion

To compare relative performance of various samples, a reference sample of pure $`MgB_2`$ sample was made by reacting $`100\mu m`$ diameter $`CVD`$ boron fibers in a $`Ta`$ container at $`950^{}`$C for $`2h`$. The resulting magnetization curve in an applied field of $`50Oe`$, is illustrated in the inset of Fig. 1 and shows the onset of superconductivity at $`39.2K`$ and a transition width of a few tenths of a Kelvin. In a separate control measurement, a sample with a pure boron layer $`25\mu m`$ thick was deposited on a carbon coated $`SiC`$ fiber and reacted in $`Mg`$ vapor as above. As reported elsewhere, the $`J_cvs.H`$ curves of this sample are identical to the sample with pure $`B`$ deposited on $`W_2B_5`$ to a thickness of $`100\mu m`$. Changing the substrate from $`W_2B_5`$ to carbon coated $`SiC`$ and changing the thickness from the $`25\mu m`$ to $`100\mu m`$ does not change the $`J_cvs.H`$ behavior of pure $`MgB_2`$. These results would appear to imply that $`C`$ is not diffusing from the $`C`$ substrate into the $`MgB_2`$ during reaction at $`950^{}`$C for $`2h`$ to a level that will have a significant effect on $`J_c`$.

### A Heavy $`Ti`$-doping

Doping with $`Ti`$ has been done at both the $`50\%`$ and $`5\%`$ levels. To get a broad perspective, a sample with a high $`Ti`$ level was prepared.and converted to $`MgB_2`$ by reacting at $`950^{}`$C for $`2h`$. This high $`Ti`$ level sample was deposited on a $`15\mu m`$ $`W`$ substrate similar to the standard pure $`MgB_2`$, but the diameter was $`80\mu m`$ rather than $`100\mu m`$ as in the pure sample. The resulting sample had a $`Mg/Ti`$ ratio of about 1 as determined by the $`EDS`$. , As shown by the upper curve in the inset of Fig. 1, the low field magnetization has a small diamagnetic drop at $`38K`$ and a larger drop in the region of $`25K`$. An energy dispersive X-ray (EDS) study in the scanning electron microscope (SEM) showed comparable amounts of $`Ti`$ and $`Mg`$ which is consistent with the Meissner screening fraction of about $`25G`$ in an external field of $`50Oe`$. As shown by the solid squares of Fig. 1, the pure $`MgB_2`$ sample at $`5K`$ shows $`J_c650,000A/cm^2`$ at zero field and $`J_c10,000A/cm^2`$ at $`1.5T`$. At $`25K`$, shown by the solid triangles, $`J_c300,000A/cm^2`$ at zero field and $`J_c10,000A/cm^2`$ at $`0.7T`$. For the $`B/Ti`$ ratio approximately equal to 1 sample, $`J_c`$ values at $`5K`$ are about $`200,000A/cm^2`$ at zero applied field, but drop below $`10,000A/cm^2`$ in just a few tenths of a Tesla. This sample clearly has far too much $`Ti`$.

### B Light $`Ti`$-doping

Samples with nominally a $`Ti/B`$ ratio of $`0.05`$ were all deposited onto $`SiC`$ substrates coated with glassy carbon so these samples have both $`Ti`$ and possibly some small amount of $`C`$ impurities. A series of $`EDS`$ measurements in the $`SEM`$ show that different samples with boron thicknesses of $`4`$, $`6`$, and $`10\mu m`$ have somewhat different $`Ti`$ concentrations. These $`EDS`$ studies with a sampling beam diameter of $`1\mu m`$ indicate that the $`4\mu m`$, the $`6\mu m`$, and the $`10\mu m`$ thick samples have $`Ti`$ contents roughly in the ratio of $`2:1.5:1`$. The $`10\mu m`$ thick sample has roughly $`9`$% as many $`Ti`$ atoms as $`Mg`$ atoms. The $`Ti`$ and $`Mg`$ peaks are strong and isolated so the result is relatively easy to measure. A systematic study of the causes for the variation in the $`Ti`$ content with $`B`$ thickness has not yet been undertaken, but it is most likely related to the fact that the temperature dependence of $`Ti`$ is deposition differs from the temperature dependence of $`B`$ deposition.

Low field magnetization characteristics at $`50Oe`$ are shown in the inset of Fig. 2 for the $`4\mu m`$ thick sample that has been reacted in $`Mg`$ vapor at $`950^{}`$C for $`1h`$ and $`2h`$. The onset of Meissner screening is systematically suppressed to values near $`36K`$ and crosses $`50Oe`$ at about $`33K`$. For these samples with a few micrometers of superconductor on a $`75\mu m`$ diameter $`SiC`$ substrate, there is some difficulty determining both the mass of superconductor present. In addition, the reacted samples are not completely straight or really well aligned with the magnetic field so the demagnetizing factor for the sample has some uncertainty. Thus, the absolute magnitude of the $`4\pi M`$ values could be in error by $`30`$ to $`40`$ percent. All samples were treated in the same manner, however, so sample to sample comparisons are more reliable than the absolute value of the magnetization. The pure $`MgB_2`$ sample of Fig. 2 and Fig. 3 is a $`100\mu m`$ diameter boron fiber on a $`15\mu m`$ diameter $`W_2B_5`$ substrate that has been reacted in $`Mg`$ vapor at $`950^{}C`$ for $`2h`$.

The semi-logarithmic plot of $`J_c`$ vs field for these two samples at $`5K`$ are a factor of $`8`$ higher than pure $`MgB_2`$ at low field. Both the $`1h`$ reaction and the $`2h`$ reaction samples have essentially the same $`J_c`$ dropping from about $`5,000,000A/cm^2`$ at $`0.1T`$ to about $`50,000A/cm^2`$ at $`3T`$ as shown in Fig. 2. Above $`2T`$, the improvement is very substantial.

Because short reaction times are usually desirable in any commercial process, a series of samples ranging in thickness from $`410\mu m`$ were deposited on a $`C`$ substrate and reacted at $`1100^{}`$C for $`15min`$. The transition temperature again is suppressed to about $`35K`$ as shown in the inset of Fig. 3. With these reaction conditions, the value of $`J_c`$ in zero applied field systematically drops from about $`4,000,000A/cm^2`$ for a $`4\mu m`$ thick layer to about $`2,000,000A/cm^2`$ for a $`10\mu m`$ thick layer as shown in Fig. 3. If these data are plotted on a semi-logarithmic scale to emphasize the lower $`J_c`$ values at high magnetic field, this trend with thickness is reversed. In the region of $`3T`$, the $`10\mu m`$ thick sample shown by the solid triangles in Fig. 4 carries more than $`100,000A/cm^2`$ and the $`4\mu m`$ thick sample shown by the solid squares carries about $`10,000A/cm^2`$. If the temperature is raised to $`25K`$, the $`10\mu m`$ thick sample has $`J_c600,000A/cm^2`$ in zero applied field and about $`J_c10,000A/cm^2`$ at $`1.3T`$ as shown on Fig. 4. .

### C Optimization of $`Ti`$-doped samples

Optimization of the $`J_c`$ performance as a function of reaction times was performed at two different temperatures of $`1100^{}C`$ and $`950^{}C`$. Here, the $`25K`$ data for $`J_c`$ are shown because this is the most likely operating temperature. As shown in Fig. 5a, the optimum reaction time at $`1100^{}C`$ is in the range of $`15`$ to $`30`$ minutes, and the samples show $`J_c10,000A/cm^2`$ at $`1.2T`$. As shown in Fig. 5b, the optimum reaction time at $`950^{}C`$ is about $`2h`$, and the samples show $`J_c10,000A/cm^2`$ at $`1.3T`$. Our assumption has been that the degradation of $`J_c`$ and $`T_c`$ at long times may arise from the diffusion of carbon from the substrate into the $`MgB_2`$. It is difficult, however, to determine the carbon content in these layers of $`MgB_2`$ that are $`4`$ to $`10\mu m`$ thick and are on a $`C`$ substrate. The $`EDS`$ carbon peak is a shoulder on the $`B`$ peak and is small compared to the $`Ti`$ peak for all temperature and times studied for the $`10\mu m`$ thick sample. If you were very optimistic about the data interpretation, the carbon shoulder may grow to a value of $`10`$ percent of the titanium peak for the sample reacted at $`1100^{}C`$ and $`45min`$ where there is significant degradation of $`J_c`$. This degradation of $`J_c`$, however, may also come from a rearrangement of the $`Ti`$ as well. Further work needed to improve the determination of the carbon content and the causes for the observed changes in $`J_c`$ of the superconductor.

## IV Conclusions

Titanium impurities co-deposited with the boron in a $`CVD`$ process is a very effective method to raise the critical current performance in the range $`3T`$ at $`5K`$ and in the range of $`1.3T`$ at $`25K`$. The value of $`T_c`$ is suppressed only $`2K`$ or $`3K`$ and there is a very substantial enhancement of $`J_c`$. These $`CVD`$ methods are an effective way to distribute the $`Ti`$ impurities and can be used to produce conductors with $`J_c`$ values in the range of $`10,000A/cm^2`$ at $`25K`$ and $`1.3T`$.

## V Acknowledgments

Work is supported by the U.S. Department of Energy, Basic Energy Sciences, Office of Science, through the Ames Laboratory under Contract No. W-7405-Eng-82.


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# Reply to comment on “A simple explanation of the non-appearance of physical gluons and quarks”

## Abstract

This is the reply to a comment by Andreas Aste on a previous article of mine in Can.J.Phys. The counter-arguments used by Aste utilize a mathematical limit without physical meaning. We still contend that in QCD, the particles “gluons” and “quarks” are merely artifacts of an approximation method (the perturbative expansion) and are simply absent in the exact theory.

The critique of my previous article  by Aste  centers on scattering theory (S-matrix) and plane wave solutions to the evolution equation

$`(\delta _{ab}^\mu +g_sf_{abc}A_c^\mu )(_\mu A_\nu ^b_\nu A_\mu ^b+g_sf_{bde}A_\mu ^dA_\nu ^e)=0,`$ (1)
for color fields without quark sources.

The definition of the scattering matrix is that it transforms free states (harmonic oscillator mode excitations = particles) at $`t=\mathrm{}`$ into free states at $`t=+\mathrm{}`$. In other words one has to pre-suppose the existence of asymptotic states, i.e. plane waves (which of course can be quantized in the usual manner). Also the interaction Hamiltonian, $`H_I`$, is (iteratively) made up of such free field operators.

The eight different uncoupled gluons (eq.(3) in Aste’s paper ) resulting from plane wave solutions to eq.(1) above, is solely a result of an unphysical mathematical limit. These asymptotic states are never physically realized, as it either demands that the coupling is identically zero ($`g_s0`$) leading to a non-dynamical theory, or that $`Q^2\mathrm{}`$ where perturbative quantization is feasible through asymptotic freedom. The latter, however, does not imply physical particles observable in the lab. (This should be contrasted to the case in QED, where asymptotic, and physical, states are reached as $`Q^20`$.) The sterile character of the solutions can also be seen directly from the linear plane wave form of eq.(3) in , as it is well known that linear waves do not interact. A more technical way of saying the same thing is that this special solution demands the absence of local gauge invariance (“the color of the gluon field is held constant throughout the space” ) which implies non-interacting fields.

However, why introduce these unphysical states at the start and then, unsuccessfully, try to get rid of them in the end (to explain “confinement”), when they do not appear in the full non-perturbative theory?

Hence, the counter-arguments in  are not physical, and we still contend that the nonappearance of physical gluons and quarks is a direct consequence of QCD, as shown in .


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# Unbiased simulation of structural transitions in calmodulin

## 1 Introduction

The biological functions of many proteins result from their *folded-state* dynamics, and in particular, from conformational changes among meta-stable states. Motor proteins perform their vital functions based upon structural transitions, and additionally, such transitions often accompany ligand-binding and catalysis events: those occurring in calmodulin and in adenylate kinase upon ligand binding are textbook examples  among numerous others. However, little is known about the detailed dynamics of these large-scale transitions. How cooperative are the changes? Do meta-stable intermediate states often occur? How many reaction pathways play an important role? Do any generic kinetic or dynamical features appear, especially in light of the expectation that nature tunes barrier heights to a few times the thermal energy scale $`k_BTRT`$?

Calmodulin (CaM), a 148-residue calcium-binding and signalling protein, is an ideal test system because of its modest size and because it has been the subject of intensive experimental scrutiny (e.g., ). CaM undergoes large scale conformational transitions both within and between its two domains. CaM has also been studied computationally, for instance by the García and Kuczera groups , but these all-atom molecular dynamics studies have been limited to nsec timescales.

Many approaches have been developed for the general problem of determining reaction pathways — including both “static,” “quasi-dynamic,” and “ensemble” approaches. We term “static” those approaches which yield a single, presumably optimal pathway (e.g., ). The so-called static picture, by definition, does not account for inherent thermal fluctuations or the possibility of multiple pathways, though Elber and Shalloway modelled the effect of temperature in a static picture . Biased molecular dynamics approaches, like targeted and steered dynamics  attempt to include more realistic aspects of the true dynamics; such methods typically generate a small number of potentially dominant dynamical pathways in protein systems, rather than a full ensemble.

“Ensemble” approaches attempt to generate suitably distributed sets of reacting trajectories. The pioneering work of Pratt employing the Metropolis approach  was applied by Chandler and coworkers to a variety of problems (e.g., ). Elber and coworkers developed the stochastic difference equation approach, which generates approximate reactive trajectories without high-frequency motions . Woolf and Zuckerman purused a non-Metropolis ensemble approach , as did Mazonka *et al.* ; see also the work of Eastman *et al.* . A notable, independent approach for studying rare events is the “weighted-ensemble Brownian dynamics” of Huber and Kim , which is conceptually related to the earlier work of Harvey and Gabb .

One recent study pursued similar goals to the present investigation for a cubic-lattice toy model. Specifically, Borovinskiy and Grosberg studied the design of cubic-lattice “protein” models capable of undergoing conformational transitions .

Here we introduce an unbiased methodology to study large-scale structural transitions in folded proteins, and we use it to perform an initial examination of the structural dynamics in the N-terminal domain of calmodulin. The method builds on two existing computational strategies. The first, due to Panagiotopoulos and Kumar , is a general discretization approach which involves the use of a fine grid (with lattice spacing much less than the particle or atom size) to mimic continuum calculations. Atoms or particles are only permitted to occupy grid sites, and interaction energies or forces are computed in advance for all necessary inter-particle displacements; see Fig. 1. Panagiotopoulos and Kumar found that critical and coexistence properties of fluids could be reproduced very precisely with a speed gain of one to two orders of magnitude . The notion of using a fine grid to simulate biomolecules also conceptually draws from coarse-grained lattice simulations of proteins , particulularly the high coordination lattice studies by Kolinski, Skolnick, and coworkers.

The second principal computational precursor to the present work is the Gō model , which represents proteins in solely a structural way, without reference to the underlying chemistry. In particular, the Gō model employs a chain of residue “beads”, each of which only reacts favorably with other residues which are nearby in the *native* structure. Non-native contacts are penalized. This simple model was developed to study the dynamics of protein folding and it is still widely used for that end . Note that the Gō model is trivially generalized to other levels of chemical detail — e.g., to all-atom simulation .

While the present approach is not restricted to simplified models, we use a highly reduced (residue-level) model both because it is easier to implement and because residue-level models have already provided meaningful bio-macromolecular results. Reduced models of proteins have often been used in the past, particularly to study protein folding dynamics and thermodynamics (e.g., ), “ab initio” protein strucutre prediction (e.g., ), and coarse-grained dynamics (e.g., ); see also a review of structure-based potentials . Moreover, it has been shown conclusively that even models which do not distinguish among atom or amino acid types can capture intermediate scale (i.e., alpha carbon fluctuations) and large scale motions (i.e., the slowest modes) .

The present, unbiased approach should also prove useful in the refinement of the biased “ensemble” methods discusssed above. Because the ensemble methods have not been fully vetted in protein systems, the present approach can usefully contribute “perfect” ensembles of *unbiased* large-molecule transition trajectories which can serve as “gold standards” for comparison with biased methods. In particular, unbiased ensembles can help shift the focus to a number of biologically and methodologically important questions regarding intermediates: (i) can their lifetimes be estimated accurately? (ii) do intermediates introduce a very wide variation in the durations of transition events? (iii) are multiple pathways typically observed?

In outline, the next section, 2, describes the simulation approach used here. We emphasize that our method is not tied to the choice of model (i.e., forcefield), which is highly simplified for this initial study and is described in Sec. 3. Sec. 4 presents the simulation results, and highlights the straightforward observation of stable intermediates. Our concluding discussion is given in Sec. 5.

## 2 Methodology

### 2.1 Fine-grid simulation

The fine-grid simulation methodology is adopted directly from Panagiotopoulos and Kumar . The idea is to allow particles (here, residues) to occupy only discrete positions on a grid. Interaction energies are then stored in arrays, rather than computed at each dynamics step.

More specifically, a “fine” grid is used — i.e., one in which the grid spacing is much smaller than the particle size — in an attempt to mimic continuum results. This point bears emphasizing: the grid approach is adopted solely as a means to reproduce continuum results at greater computational speed; the errors or artifacts resulting from using a fine grid are expected to be negligible due to the small size of the grid spacing. Indeed, the central result of Panagiotopoulos and Kumar  is that very sensitive liquid-vapor coexistence curves and critical points could be determined quite accurately within the grid approach. A rough rule of thumb from Panagiotopoulos’ work is that a lattice spacing of $`1/5`$ the particle size is sufficient for practical computations.

How fine a grid spacing is necesary in the present context? Owing to the crudeness of the models used here (see Sec. 3), we do not require high precision. However, to implement a dynamic Monte Carlo scheme (see below) with a sufficient acceptance ratio, a small grid spacing is required. In the simulations discussed here, the lattice spacing was 0.13 Å, which may be compared with residue-residue interaction distances of 4 - 8 Å. In other words, a very fine grid is employed here.

### 2.2 Dynamic Metropolis Monte Carlo

In this initial implementation, we have chosen to use dynamic Monte Carlo (DMC) dynamics, which is a common, current choice for simulations of protein folding dynamics (e.g., ). While DMC dynamics were chosen because of the relative ease of implementation, they may be justified on two grounds. (i) Because only small, local trial moves will be considered — see below — and accepted with a Boltzmann-factor-preserving probability, DMC may be considered a variant of overdamped Brownian dynamics. Brownian dynamics have a well-understood physical basis . (ii) Further, due to the highly simplified nature of the models used here (see Sec. 3), one can expect the simulated dynamics — of any kind — only to give a qualitative picture. This qualitative description should not be sacrificed by Brownian-like dynamics embodied in DMC.

The dynamic Monte Carlo is designed to make highly local moves in a trivial way: at every time step, a randomly chosen residue makes a trial move with uniform probability to one of the 26 lattice sites on the surface of the $`3\times 3\times 3`$ cube centered at its present location. The move is accepted or rejected according to the usual Metropolis criterion: accept if and only if the energy decreases or a random number $`R_u`$ chosen uniformly from the interval $`0<R_u1`$ is less than $`\mathrm{exp}(\mathrm{\Delta }U/RT)`$, where $`\mathrm{\Delta }U`$ is the change in the total energy (Hamilitonian) of the system.

### 2.3 Hardware, Software, and Computer Time

The results reported below are based on a computer program written in the C language and compiled with the “gcc” compiler on Linux machines. Simulations were run on Intel processors of both 2.4 and 2.8 GHz, which permitted approximately 3 - 4 $`\times 10^8`$ Monte Carlo steps per hour. All the trajectories discussed here were obtained in less than one week of of processor time.

## 3 Model

The residue-level model describes a highly reduced protein without any true chemistry, following the spirit of many previous workers . Nevertheless, the model does include the essential toplogical features of calmodulin: residue connectivity and sterics, as well as the attractive interactions found in both *apo* and *holo* strucrures. Only the N-terminal domain was included — specifically the 72 residues numbered 4 - 75 in PDB structures 1cfd (*apo*, unbound) and 1cll (*holo*, bound to calcium ions).

The model of the N-terminal domain of calmodulin is specified by covalent, steric, and attractive interactions; see Fig. 2. Consectutive residues are “covalently” connected by an infinitely deep, attractive square well centered on the native-state separation distance of structure 1cfd; the well width was taken to be 10% of the native separation ($`\pm `$5%). Sterically, each residue excludes other residues from its hard-core exclusion zone, a sphere with radius set to 47.5% (i.e., 95%/2) of the minimum distance to other non-consecutive residues in the 1cfd native state. Finally, Gō-like attractive interactions are represented by square wells (of uniform depth $`ϵ`$) centered at residue separation distances ($`\pm `$5%) of less than 8 Å from *either* of the native structures (i.e., PDB codes 1cfd or 1cll). All simulations were performed at a temperature given by $`k_BT=0.6ϵ`$.

The double-well, attractive interactions depicted in Fig. 2 merit further justification. At first glance, such a potential may seem unnatural, particularly to those readers familiar with the distinction between the pair potential energy and potential of mean force (see, e.g., ): for a simple fluid consisting of spherical particles, it is well known that a single-well potential gives rise to a multi-well potential of mean force. However, amino acids are not spherical, and if one insists on a point-residue model (as here), the only way to represent direct interactions of differing orientations is for the potential to possess more than one well. A second, perhaps facile, justification comes from the results: the double well potential accomplishes the principal aim of stabilizing two distinct conformational states. Indeed, it requires roughly a day of computer time to generate a fluctuation sufficiently large as to jump to the second state. A third justification is more pragmatic: when more realistic potentials (e.g., ) are discretized with the find-grid approach, presumably the “unnatural” double-Gō interactions can be reduced to minimal levels required to stabilize the distinct states.

## 4 Results

In this preliminary report, all the results are depicted in Figs. 4 \- 7, and described in the figure captions. To summarize, sample transition events are shown (Fig. 4), and traces of the helix angles confirm that the transition are genuine and sustained (Fig. 5). Next, long-lived intermediates are readily visualized using compound variables which simply measure distances between helix ends (Fig. 6), and finally the dynamical evolution of individual residue contacts is examined (Fig. 7).

## 5 Summary and Conclusions

We have introduced an approach for studying the long-time dynamics of large-scale conformational transitions in proteins. The technique was tested on a highly reduced, residue-level model of the N-terminus of calmodulin, which undergoes a dramatic rearrangement of its four helices upon the (un)binding of calcium ions. Such rearrangements were observed approximately once per day on a single processor in *unbiased* dynamic Monte Carlo simulation. The scheme is quite promising because it proved capable of spanning the range of timescales from that for inter-residue vibrations to the “waiting time” between transition events — i.e., the inverse rate.

The approach is readily extendable in two important ways. First, it is embarrassingly parallelizable, so an inexpensive, modest-sized Beowulf cluster can readily improve upon the single-processor output by an order of magnitude or more. Second, the fine-grid discretization approach  — which simply mimics continuum calculations — lends itself to more complex potentials: while the addition of particles (e.g., “beads”) to any model entails a cost, the use of a more chemically realistic potential will require minimal additional overhead. Furthermore, other models — reduced or atomistic — can be stabilized in experimentally determined structural states using the same Gō-like interactins employed here.

Despite the apparent simplicity of the model employed here, the simulated structural transitions in calmodulin exhibited highly complex behavior. Distinct transition pathways and quasi-stable intermediate states could be readily identified, as could critical residues. The transition details identified in the present study cannot immediately be identified with expectations for experimental outcomes because of the simplicity of the model. Nevertheless, the results should capture those aspects of the dynamics governed by sterics and connectivity, in analogy with the success of network-like models in predicting large-scale fluctuations .

Future studies with more chemically realistic models (e.g., ) implemented in the rapid, fine-grid approach should suggest testable experimental hypotheses. Note that the effects on dynamics of varying forcefields have recently been addressed by Freed and coworkers . A related question, which also can be addressed directly in the present scheme, regards the effects of *dynamics type* — e.g., Metropolis, Langevin, molecular dynamics — on transition events.

The future determination of reaction pathways and dynamics in a hierarchy of models will also address a question both scientifically and methodologicallly critical: *What is the minimal model necessary to capture residue-level features of structural transitions in proteins?* From the “scientific” perspective, a minimal model will suggest which interactions govern the transition events, while optimal methods should use that model which is least costly, computationally.

Finally, it is appropriate to ask what the unbiased transitions observed in the present study presage for the use of the biased “ensemble” methods discussed in the introduction. The observation of multiple pathways and widely disparate transition event durations suggests that great care will be required in any biased effort to generate ensembles of transition trajectories. Nevertheless, the present approach should provide critical input for testing biased methods in protein systems — namely, unbiased trajectories to be used for comparison. From a practical standpoint, a set of reduced-model transition events may also provide useful starting points to sidestep the potential for trapping associated with the Pratt approach.

## Acknowledgments

The author has benefitted greatly from discussions with many scientists: Ivet Bahar, David Deerfield, Jeffery Evanseck, William Furey, Hagai Meirovitch, Robert Swendsen, Dror Tobi. Special thanks are due Professor Bahar for her invaluable advice, support, and encouragement.