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# In Search of the Vortex Loop Blowout Transition for a type-II Superconductor in a Finite Magnetic Field

## I Introduction

In pure extreme type-II superconductors, such as the high $`T_c`$ superconductors, the Abrikosov vortex line lattice melts via a sharp first order phase transitionR1  into a vortex line liquid as the temperature is increased above a critical $`T_m`$. The properties of this vortex line liquid phase have been the subject of considerable investigation. Theoretical argumentsR2  and early simulationsR3 ; R3.1 ; R3.2  suggested that the vortex line liquid might retain superconducting phase coherence parallel to the applied magnetic field, within some temperature interval above $`T_m`$. Later, better converged simulationsR4  found that phase coherence is simultaneously lost in all directions upon melting.

Subsequently, TešanovićR5  has proposed that, for small magnetic fields, there still remains a sharp thermodynamic phase transition at a temperature $`T_\mathrm{\Phi }`$ within the vortex liquid state, associated with diverging fluctuations of closed vortex loops, such as drive the superconducting transition in the zero magnetic field case. Considering the limit of infinite penetration length $`\lambda `$, Tešanović proposed that, in a finite field, the fluctuations of the magnetic field induced vortex lines act to screen the interactions of thermally excited closed vortex loops, in the same way that magnetic field fluctuations screen the vortex loop interactions of a finite $`\lambda `$ model in zero applied magnetic field. Pursuing this argument, he predicted that the proposed vortex loop blowout transition at $`T_\mathrm{\Phi }`$ may be an inverted XY transition, as is the case of the zero field Meissner transition for the finite $`\lambda `$ model.

Following Tešanović’s predictions, Sudbø and co-workersR6 ; R7 ; R8  have carried out numerical simulations of the three dimensional (3D) uniformly frustrated XY model of a type-II superconductor. They claim to find evidence for Tešanović’s transition, which they associate with the formation of a vortex line path that percolates entirely around the system in the direction transverse to the magnetic field.

Most recently, measurementsR9  on high purity YBa2Cu3O7 (YBCO) single crystals have found a step like anomaly in the specific heat at a temperature highter than the melting $`T_m`$, reminiscent of an inverted mean field transition. It has been arguedR9  that this feature may be evidence for Tešanović’s transition $`T_\mathrm{\Phi }`$.

In order to further investigate this issue, we have carried out new simulations on the 3D uniformly frustrated XY model, both repeating the approach of Sudbø and co-workers, and measuring new quantities that make a more direct test of Tešanović’s theory. After correcting certain inconsistencies in the earlier numerical work, we show that whether or not one finds indications of a vortex loop blowout transition depends crucially on how one chooses to resolve vortex line paths at points where two or more lines intersect. Making the choice that favors the blowout interpretation, we find the critical exponent $`\nu 1`$, rather than the value $`2/3`$ expected for an inverted 3D XY transition. Finally, we make high precision measurements of the specific heat, in search of a thermodynamic signature for a blowout transition, but no such signature is found.

## II Model

The model that we use is the 3D uniformly frustrated XY modelR3 ; R3.1 ; R3.2 ; R4 ; R6 ; R7 ; R8 ; R10  which models a type-II superconductor in the limit of infinite magnetic penetration length, $`\lambda \mathrm{}`$, and is given by the Hamiltonian,

$$[\theta _i]=\underset{i,\mu }{}J_\mu \mathrm{cos}(\theta _{i+\widehat{\mu }}\theta _iA_{i\mu }).$$
(1)
Here $`i`$ are the nodes of a cubic grid of sites, $`\mu =x,y,`$ $`z`$, are the directions of the grid axes, and the sum is over all nearest neighbor bonds of the grid. $`\theta _i`$ is the phase angle of the superconducting wavefunction on site $`i`$, $`A_{i\mu }=(2\pi /\mathrm{\Phi }_0)_i^{i+\widehat{\mu }}𝐀𝑑𝐫`$ is given by the integral of the magnetic vector potential $`𝐀`$ across the bond at site $`i`$ in direction $`\widehat{\mu }`$, and $`\mathrm{\Phi }_0=hc/2e`$ is the flux quantum. The argument of the cosine is the gauge invariant phase angle difference across the bond. The circulation of the $`A_{i\mu }`$ around any plaquette of the grid is equal to $`2\pi `$ times number of flux quanta of magnetic field penetrating the plaquette. We take the magnetic field, $`𝐁=\times 𝐀`$, uniform and parallel to the $`\widehat{z}`$ axis, with a fixed density of flux quanta $`f=Ba^2/\mathrm{\Phi }_0`$ per plaquette of area $`a^2`$. The couplings $`J_\mu `$ we take to model an anisotropic system, with $`J_x=J_yJ_{}`$, and $`J_zJ_{}`$.

Simulations are carried out varying the $`\theta _i`$ according to a usual Monte Carlo scheme; the $`A_{i\mu }`$ are held fixed. That the $`A_{i\mu }`$ do not fluctuate, and that they give a uniform magnetic field, are the consequences of the $`\lambda \mathrm{}`$ approximation. Simulations are carried out on $`L_z\times L_{}^2`$ cubic grids, using periodic boundary conditions. Except where otherwise noted, our runs are typically for $`1/4`$ to $`1/2\times 10^6`$ Monte Carlo passes through the entire lattice.

While we simulate in the phase angle degrees of freedom, $`\theta _i`$, our interest will be in the behavior of the vorticity in these phase angles. Let $`s`$ denote the dual sites of the original grid; these are the sites at the centers of the unit cells of the grid. Denote by $`(s,\mu )`$ the plaquette which is the face of the unit cell centered on dual site $`s`$ with normal in the $`\widehat{\mu }`$ direction, $`\mu =x,y`$, $`z`$. We define the integer vorticity $`n_{s\mu }`$ piercing plaquette $`(s,\mu )`$ by computing the circulation of the gauge invariant phase angle differences around the plaquette,

$$\underset{(s,\mu )}{}[\theta _{i+\widehat{\sigma }}\theta _iA_{i\sigma }]=2\pi (n_{s\mu }f\delta _{z\mu }),$$
(2)
where the sum is counterclockwise around all bonds forming the boundary of plaquette $`(s,\mu )`$, and the gauge invariant phase angle differences are restricted to the interval $`[\pi ,\pi )`$. In a constant magnetic field, the condition that the total energy density remains finite can be shown to yield the “neutrality” constraint (see section III.A),

$$\underset{s}{}n_{s\mu }=fL_{}^2L_z\delta _{z\mu },$$
(3)
i.e. the total vorticity piercing any plane at constant $`z`$ is $`fL_{}^2`$; these are the magnetic field induced vortex lines. The total vorticity in the transverse directions $`x`$ and $`y`$ is zero.

Taking the vorticity $`n_{s\mu }`$ as the directed bond of the dual grid, emanating from site $`s`$ in direction $`\widehat{\mu }`$, the vorticity so defined is divergenceless, forming continuous lines that, due to the periodic boundary conditions, must ultimately close upon themselves. We will label such a closed vortex path by the index $`\alpha `$, and define the vector $`𝐑_\alpha `$ as the net displacement one travels upon following the path $`\alpha `$ from a given starting point until returning back to that point as the line closes back on itself. If $`𝐑_\alpha =0`$, then the vortex line path is a closed loop of finite extent that exists as a thermal fluctuation. If $`R_{z\alpha }=mL_z`$, $`m`$ integer, then such a vortex line path represents $`m`$ of the $`fL_{}^2`$ field induced vortex lines; these $`m`$ lines are mutually connected to each other via the periodic boundary conditions in the $`z`$ direction.R3.1  For $`m>1`$, we can say that the $`m`$ field induced lines are geometrically entangled with each other. If $`R_{x\alpha }=mL_{}`$ or $`R_{y\alpha }=mL_{}`$, then the vortex line path winds $`m`$ times around the system transversely to the applied magnetic field. We will be particularly interested in vortex line paths for which $`R_{z\alpha }=0`$, but $`R_{x\alpha }`$ or $`R_{y\alpha }0`$. Henceforth, we will refer to as the “lines”, the set of vortex line paths $`\{\alpha \}`$ for which all $`R_{z\alpha }>0`$; these are the field induced vortex lines. All other vortex paths we will refer to as the “loops”.

In order to trace out vortex line paths, one needs to know how to treat intersections. An intersection is when there is more than one vortex line entering and exiting a give unit cell of the grid, and it is therefore ambiguous which entering segment to connect to which exiting segment. It was previously shownR11  by one of us that the method chosen to resolve such intersections can have a dramatic effect on the statistics of closed thermally excited loops in the zero field $`f=0`$ model. Here, for the $`f>0`$ model, we consider two different schemes, which we henceforth refer to as method (i) and method (ii):

(i) At each intersection we choose randomly, with equal probability, which entering segment connects to which exiting segment. In the $`f=0`$ model this scheme was found to give results closest to theoretical expectations.R11

(ii) Motivated by Sudbø and co-workers,R6 ; R7 ; R8  we first searchR11.1  through all possible connections to find a path $`\alpha `$ with $`R_{z\alpha }=0`$ and $`R_{x\alpha }`$ or $`R_{y\alpha }0`$. Such a path winds around the system transverse to the field, without ever winding around the system parallel to the field. If one such path is found, it is selected as a path $`\alpha ^{}`$ contributing to the “loops”, and we then repeat the proceedure applied to all remaining vortex paths. When all such transverse paths are found, the remaining vortex line intersections are resolved randomly, as in method (i).

Using either method (i) or method (ii) we thus decompose the vorticity of any given configuration into disjoint closed vortex line paths, consisting of a set $`\{\alpha \}`$ of “lines” and a set $`\{\alpha ^{}\}`$ of “loops”.

## III Winding of Field Induced Vortex Lines

We first attempt a direct test of Tešanović’s theory of the $`T_\mathrm{\Phi }`$ transition within the liquid phase. A summary of his arguments for the existence of this transition is as follows.

### III.1 Summary of Tešanović’s Theory

First, a duality transformationR12 ; R12.1 ; R12.2  from the XY model of Eq. (1) gives the interaction between vortices as,

$$[n_{s\mu }]=\frac{1}{2}\underset{s,s^{},\mu }{}[n_{s\mu }f\delta _{z\mu }]V^\mu (𝐫_s𝐫_s^{})[n_{s^{}\mu }f\delta _{z\mu }]$$
(4)
where $`V^\mu (𝐫)`$ is the appropriate anisotropic generalization of the Coulomb interaction, with Fourier transform $`V_q^\mu q^2`$. It is this singularity of $`V_q^\mu `$ as $`q0`$ that yields the constraint of Eq. (3).

Next, one imagines decomposing the total vorticity of the system into lines and loops,

$$n_{s\mu }=n_{s\mu }^{\mathrm{lines}}+n_{s\mu }^{\mathrm{loops}}.$$
(5)
If we define,

$$b_{s\mu }n_{s\mu }^{\mathrm{lines}}f\delta _{z\mu }$$
(6)
then $`_sb_{s\mu }=0`$ and the Hamiltonian of Eq. (4) can be rewritten as,

$$=\frac{1}{2}\underset{s,s^{},\mu }{}[n_{s\mu }^{\mathrm{loops}}b_{s\mu }]V^\mu (𝐫_s𝐫_s^{})[n_{s^{}\mu }^{\mathrm{loops}}b_{s^{}\mu }].$$
(7)
Tešanović then argues that a coarse graining of vortex fluctuations, in the vortex line liquid phase, leads to an effective hydrodynamic Hamiltonian on long length scales which has the same interaction piece as Eq. (7), but which has a new additive term proportional to $`_{s\mu }b_{s\mu }^2`$. The resulting long length scale Hamiltonian then has exactly the same form as that of a zero field superconductor with thermally fluctuating vortex loops, $`n_{s\mu }^{\mathrm{loops}}`$, and a thermally fluctuating magnetic field $`b_{s\mu }`$ whose average is zero, i.e. the zero field superconductor with a finite penetration length $`\lambda `$. In other words, in this infinite $`\lambda `$ theory at finite magnetic field, the long wave length fluctuations of the field induced vortex lines $`n_{s\mu }^{\mathrm{lines}}`$ screen the interaction between the vortex loops $`n_{s\mu }^{\mathrm{loops}}`$ in exactly the same manner as magnetic field fluctuations screen the interactions between vortex loops in a finite $`\lambda `$ model at zero magnetic field.

The Meissner transition at $`T_c`$ in the zero field, finite $`\lambda `$, model is an inverted 3D XY transition.R12  The high temperature phase $`T>T_c`$ has vortex loops on all length scales and breaks a global $`U(1)`$ symmetry associated with a disorder parameter;R12.3  the low temperature phase $`T<T_c`$ has no vortex loops on sufficiently long length scales. The correlation length $`\xi `$ and renormalized magnetic penetration length $`\lambda _R`$ both divergeR13  as $`|t|^\nu `$, with $`\nu 2/3`$ and $`tTT_c`$.

We have earlier carried out numerical simulationsR13  of this zero field, finite $`\lambda `$, Meissner transition. We demonstrated that, in this model, magnetic field fluctuations obey the finite size scaling relation,

$`F(t,q,L)`$ $``$ $`b_\mu (q\widehat{\nu })b_\mu (q\widehat{\nu })/L^3`$ (8)
$``$ $`L^1F(tL^{1/\nu },qL,1)`$
where in the above $`\widehat{\mu }\widehat{\nu }`$ and $`b_\mu (q\widehat{\nu })=_se^{iq\widehat{\nu }𝐫_s}b_{s\mu }`$ is the Fourier transform of of the magnetic flux density $`b_{s\mu }`$. As $`L\mathrm{}`$, and $`q0`$,

$$F(t,0,\mathrm{})\{\begin{array}{cc}0\hfill & t<0\hfill \\ 1/\xi \hfill & t>0\hfill \end{array},$$
(9)
hence $`F(t,0,\mathrm{})`$ vanishes below the transition, and increases continuously from zero as one goes above the transition.

In the present case of a finite magnetic field, if Tešanović’s mapping is correct, the Meissner transition $`T_c`$ becomes the transition $`T_\mathrm{\Phi }`$ within the vortex line liquid phase, and we expect the exact same scaling as in Eq. (8) above, when applied to the quantity $`b_{s\mu }`$ defined in Eq. (6). Taking the limit of $`q0`$ in Eq. (8), and applying to systems with fixed aspect ratio $`L_z=gL_{}`$, we expect the scaling,

$$(\underset{s}{}b_{s\mu })^2/L_{}^3L_{}^1f(tL_{}^{1/\nu }),$$
(10)
where $`tTT_\mathrm{\Phi }`$ and $`f(x)=F(x,0,1)`$.

For the directions $`\widehat{\mu }=\widehat{x}`$ or $`\widehat{y}`$,

$$\underset{s}{}b_{s\mu }=\underset{s}{}n_{s\mu }^{\mathrm{lines}}W_\mu L_{}$$
(11)
is the net vorticity of the magnetic field induced vortex lines in the transverse direction $`\widehat{\mu }`$. The two dimensional vector $`𝐖=(W_x,W_y)`$ defined above is the integer valued “winding number” that counts the net number of times the field induced vortex lines wind around the system in the transverse directions $`\widehat{x}`$ and $`\widehat{y}`$. If $`\{\alpha \}`$ is the set of vortex line paths that define the field induced vortex lines $`n_{s\mu }^{\mathrm{lines}}`$, and $`𝐑_\alpha `$ is the net displacement along path $`\alpha `$ as defined earlier, then $`_\alpha 𝐑_\alpha =𝐖L_{}`$, where $`𝐑_{}(R_x,R_y)`$. We thus expect from Eq. (10) the finite size scaling,

$$W^2f(tL_{}^{1/\nu }).$$
(12)
Note, the neutrality condition of Eq. (3) implies that the total transverse vorticity in the system must always vanish. For $`𝐖0`$, it is therefore necessary that any such winding of the field induced lines is exactly canceled out by an equal and opposite transverse winding of the loops. In the thermodynamic limit, $`L_{}\mathrm{}`$, Eq. (9) implies that $`W^2=0`$ for $`T<T_\mathrm{\Phi }`$, and $`W^2`$ increases continuously from zero as one increases $`T>T_\mathrm{\Phi }`$. The proposed transition at $`T_\mathrm{\Phi }`$ is thus associated with the appearance of infinite transverse loops (see following Section IV).

Another interpretation of the $`T_\mathrm{\Phi }`$ transition follows from the “two dimensional (2D) boson” modelR14  of interacting vortex lines, in which the field induced vortex lines are viewed as the world lines of two dimensional bosons traveling down the imaginary time axis. For $`T<T_\mathrm{\Phi }`$ where $`W^2=0`$, the field induced vortex lines behave like charged two dimensional bosons,R2 ; R12.2  with a long range retarded Coulomb interaction. In the vortex line liquid, $`T_m<T<T_\mathrm{\Phi }`$, where phase coherence is lost parallel to the applied magnetic field, the analog 2D bosons are in a charged superfluid state. For $`T>T_\mathrm{\Phi }`$, where $`W^20`$, screening by the infinitely large loops $`n_{s\mu }^{\mathrm{loops}}`$ results in an effective short ranged interaction between the field induced lines. In this case the winding number squared $`W^2`$ is proportional to the superfluid density of what is now an uncharged superfluid. Thus $`T_\mathrm{\Phi }`$ corresponds to a transition between a charged superfluid and an uncharged superfluid in the analog 2D boson theory. Equivalently, if one considers the quanta that mediate the interaction between the analog 2D bosons, the transition is from massless quanta for $`T<T_\mathrm{\Phi }`$ to massive quanta for $`T>T_\mathrm{\Phi }`$.

To arrive at Eq. (12), we considered the transverse components of Eq. (10). However, we can also consider the parallel, $`\widehat{\mu }=\widehat{z}`$ component. Now,

$$\underset{s}{}b_{sz}=\underset{s}{}n_{sz}^{\mathrm{lines}}fL_{}^2L_zW_zL_z,$$
(13)
and so we expect the scaling

$$W_z^2f_z(tL_{}^{1/\nu }).$$
(14)
If $`\{\alpha \}`$ is the set of vortex line paths that define the field induced vortex lines $`n_{s\mu }^{\mathrm{lines}}`$, and $`𝐑_\alpha `$ is the net displacement along path $`\alpha `$ as defined earlier, then $`_\alpha R_{\alpha z}=(fL_{}^2+W_z)L_z`$. Thus $`W_z`$ gives the number of “lines” in excess of the average value $`fL_{}^2`$ set by the applied magnetic field. The neutrality condition of Eq. (3) requires that when $`W_z>0`$, there must be an equal and opposite parallel winding of the loops $`n_{s\mu }^{\mathrm{loops}}`$. As $`L\mathrm{}`$, we have $`W_z=0`$ for $`T<T_\mathrm{\Phi }`$, and $`W_z>0`$ for $`T>T_\mathrm{\Phi }`$. Thus a transition at $`T_\mathrm{\Phi }`$ should be characterized by fluctuations in the number of field induced lines and by the appearance of infinite parallel loops directed opposite to the direction of the applied magnetic field.

### III.2 Numerical Results

To test the above predictions, we have simulated the 3D uniformly frustrated XY model of Eq. (1) using a vortex density $`f=1/20`$, anisotropy $`J_z/J_{}=0.02`$, and aspect ratio $`L_z/L_{}=1`$, for $`L_{}=10,`$ $`20`$, $`30`$, $`40`$ and $`60`$. For these parameters, the vortex lattice melting temperature is $`T_m0.24J_{}`$, and the zero field critical temperature is $`T_{c0}1.14J_{}`$. We compute the transverse winding $`𝐖`$ of the field induced lines, defined by Eq. (11), using both method (i) and method (ii) to decompose each configuration into “lines” and “loops”. According to the scaling equation (12), we expect that plots of $`W^2`$ vs. $`T`$ for different sizes $`L_{}`$ should all intersect at the common point $`t=0`$, or $`T=T_\mathrm{\Phi }`$.

In Fig. 1 we show a semilog plot of $`W^2`$ vs. $`T/J_{}`$ using method (i) (random reconnections at intersections) for $`L_{}=10`$, $`20`$, and $`30`$. We see that there is clearly no common intersection point of the curves. As $`L_{}`$ increases, $`W^2`$ decreases uniformly over the entire temperature range. This is in qualitative agreement with earlier computations of $`W^2`$ by one of us (see Fig. 15 of Ref.R3.1, ). For $`L_{}=60`$, we have found no net transverse winding of the field induced lines at all, i.e. for the length of our simulation we had $`𝐖=0`$, for the temperature range $`1.36T/J_{}1.44`$.

Next, in Fig. 2, we show the same quantities but now using method (ii) (search first for maximal transverse loops), for $`L_{}=10,`$ $`20`$, $`30`$, $`40`$ and $`60`$. We see that as $`L_{}`$ increases, the curves do seem to approach a common intersection point, giving a $`T_\mathrm{\Phi }1.4J_{}`$. Note that this $`T_\mathrm{\Phi }`$ is above the zero field critical temperature $`T_{c0}1.14J_{}`$.

From Eq. (12), we expect that the slopes of these curves at $`T_\mathrm{\Phi }`$ should scale with system size as, $`dW^2/dTL_{}^{1/\nu }`$. Fitting each of the curves of $`W^2`$ to a cubic polynomial in $`T`$, we compute their derivatives at the intersection point $`T=1.4J_{}`$, and plot the results vs. $`L_{}`$ in Fig. 3. We see that the slopes, to an excellent approximation, scale linearly with $`L_{}`$, thus suggesting a critical exponent $`\nu 1`$. On closer inspection, the data in Fig. 3 show a small systematic downwards curvature about the linear fit; however this curvature can be removed by assuming a slightly higher critical temperature of $`T=1.403J_{}`$. Note that this value of $`\nu 1`$ is larger than the predicted value of $`2/3`$.

As an alternative method to compute the critical behavior, we can take the scaling equation (12), expand the scaling function $`f(x)`$ as a polynomial for small $`x`$, and do a nonlinear fitting to the data to determine the unknown polynomial coefficients, $`T_\mathrm{\Phi }`$, and $`\nu `$. To obtain the best fit we use a 4th order polynomial and fit only the data from the two largest sizes, $`L_{}=40`$ and $`60`$. The results give $`T_\mathrm{\Phi }1.403J_{}`$ and $`\nu 0.96`$, in agreement with the earlier estimates. In Fig. 4 we show the scaling collapse that results from this polynomial fit. There are systematic deviations from the fitted curve on the $`T>T_\mathrm{\Phi }`$ side, though these appear to decrease as $`L_{}`$ increases.

Next we consider the excess parallel winding of the field induced lines $`W_z`$. As discussed earlier, Tešanović’s theory predicts a scaling of $`W_z^2`$ as in Eq. (14). To determine $`W_z`$ we count the winding of vortex line paths $`\{\alpha \}`$ that wind negatively in the $`z`$ direction, i.e. have a net displacement of $`R_{\alpha z}=m_\alpha L_z`$, with $`m_\alpha `$ a positive integer ($`𝐑_{}`$ may have any value for such paths). Since such negative parallel windings must be compensated for by excess field “lines”, we have $`W_z=_\alpha m_\alpha `$.

However, when we have used either of our tracing methods (i) or (ii), we have never found any such negative parallel windings up to the highest temperature we have simulated, $`T=1.6J_{}`$. This has motivated us to define a third tracing scheme: (iii) we first search through all possible connections to find any paths with $`R_{\alpha z}<0`$.

In Fig. 5 we show results, using tracing scheme (iii), for $`W_z^2`$ vs. $`T/J_{}`$ for the same system parameters and sizes as used in Fig. 2 for $`W^2`$. Note that the values of $`W_z^2`$ where the curves for different $`L_{}`$ intersect are exceedingly small. The intersection points appear to decrease in $`T`$ as $`L_{}`$ increases, however we do not have the accuracy to make any firm conclusions.

In an attempt to improve the analysis of $`W_z^2`$ we have repeated the calculation, but using a new system aspect ratio of $`L_z=L_{}/5`$. This has the effect of increasing the value where the curves of $`W_z^2`$ intersect, and so hopefully improving our accuracy. We have explicitly checked that changing the aspect ratio does not shift the transition temperature $`T_\mathrm{\Phi }`$ that is observed in $`W^2`$ (see also Section IV.B). In Fig. 6 we show results for $`W_z^2`$ vs. $`T/J_{}`$ for this new aspect ratio. Again we find no common intersection point for the sizes considered. As $`L_{}`$ increases, the intersection point continues to decrease. Whether this is a failure of the scaling hypothesis of Eq. (14), or whether we have simply failed to reach the scaling limit of sufficiently large $`L_z`$ ($`L_z=24`$ is the largest value in Fig. 6), we cannot be certain. Note that in both Figs. 5 and 6, $`W_z^2`$ appears to be vanishing at a temperature noticeably above the $`T_\mathrm{\Phi }1.4J_{}`$ where the curves of the transverse winding, $`W^2`$, intersect.

We have also tried to fit the data of Fig. 6 to the scaling form, $`W_z^2L^xf_z(tL_{}^{1/\nu })`$, assuming a non trivial anomalous scaling dimension $`x`$ (although we have no specific theoretical reason to propose this form). When we do so, we obtain $`T_c=1.44`$, $`\nu =0.76`$, and $`x=1.185`$, however our data in the vicinity of this $`T_c`$ is too scattered for us to place much significance on this fit.

Having used tracing method (iii) to first eliminate all possible lines percolating in the negative $`\widehat{z}`$ direction, we can then go and search for all possible transversely percolating lines and compute the resulting transverse winding $`W^2`$. When we do this, we find our results for $`W^2`$ virtually unchanged from tracing method (ii) in the vicinity of $`T_\mathrm{\Phi }1.4J_{}`$. The extremely low number of negative $`\widehat{z}`$ percolating lines at this temperature produces no noticeable effect on the transverse tracing.

## IV Percolating Loops

### IV.1 Summary of Sudbø’s Method

As discussed in the preceding Section III.A, a transition at $`T_\mathrm{\Phi }`$ would mark the appearance of infinite transverse loops, as $`T`$ is increased. The idea to explicitly look for transverse paths that percolate across the system was first put forth by Jagla and Balseiro.R16  Later, Sudbø and co-workersR6 ; R7 ; R8  refined this idea. They defined a quantity which they denoted $`O_L`$, which is the probability that a vortex path exists which travels completely across the system in a direction transverse to the applied magnetic field, without ever traveling completely across the system in the direction parallel to the field. If such a path exists in a given configuration, that configuration counts as unity in the average for $`O_L`$; if not, that configuration counts as zero.

Since having $`W^2>0`$ in a given configuration necessarily implies that there is a percolating transverse loop in that configuration, there is a close connection between the quantities $`W^2`$ and $`O_L`$. They differ in that (i) for a configuration with $`W^2>1`$, and hence with more than one percolating transverse loop, the contribution to $`O_L`$ remains unity, rather than increasing with the number of percolating transverse loops; and (ii) in a configuration with two percolating but oppositely oriented transverse loops, the contribution to $`O_L`$ will be unity, but these loops cancel each other in their contribution to $`W^2`$, which might therefore be zero.

Since $`O_L`$ is a pure number one might expect it to be a scale invariant quantity, and hence, similar to $`W^2`$, plots of $`O_L`$ vs. $`T`$ for different system sizes $`L_{}`$ should have a common intersection point at $`T_\mathrm{\Phi }`$.

Sudbø and co-workers’ method of searching for such percolating transverse paths is similar to our method (ii) except for one crucial difference.R17  They do not require that the transverse path closes upon itself; they only require that the path start at one end of the system, say at $`x=0`$, and continue until reaching the opposite end, $`x=L_{}`$, while keeping the distance traveled along $`\widehat{z}`$ less than $`L_z`$, that is the displacement traveled along the path $`\alpha `$ satisfies $`R_{x\alpha }=L_{}`$ and $`R_{z\alpha }<L_z`$. Since, by the periodic boundary conditions, all paths must eventually close upon themselves, there are two possibilities for the transverse percolating paths that Sudbø and co-workers find. We illustrate these in Fig. 7: (1) the path $`\alpha `$ eventually closes upon itself without ever traveling the length $`L_z`$, in which case $`R_{z\alpha }=0`$; or (2) the path $`\alpha `$, when followed until it closes upon itself, does wind up traveling the length $`L_z`$, with a displacement $`R_{z\alpha }=L_z`$; in this case, our method (ii) would consider this path as part of the field induced vortex lines $`n_{s\mu }^{\mathrm{lines}}`$, contributing to the winding $`𝐖`$, rather than as a transverse loop that contributes to $`n_{s\mu }^{\mathrm{loops}}`$. We will call Sudbø’s path tracing method (ii) to distinguish it from our method (ii). The probability for a percolating path using method (ii) we will denote by $`O_L^{}`$; using method (ii) we will denote it by $`O_L`$. Paths of type (2) will contribute to $`O_L^{}`$, but not to $`O_L`$. We will see that there are very dramatic differences between these two methods, and that only $`O_L`$ gives self-consistent results.

### IV.2 Numerical Results

First, we note that if we use method (i) (random connections) to search for percolating transverse paths, the result is essentially the same as found for $`W^2`$ in section III.B. As $`L_{}`$ increases, the probability to find a percolating transverse loop steadily decreases for the entire temperature range, becoming immeasurably small for our biggest system size. Hence we will focus here on methods (ii) and (ii).

We now consider the computation of $`O_L^{}`$ using method (ii), the one used by Sudbø and co-workers, which never checks to see how the percolating transverse path closes upon itself. We first use parameters $`J_z=0.02J_{}`$ and $`L_z=L_{}`$, the same as in section III.B, but a more dilute density of vortex lines $`f=1/90`$. For these parameters, the vortex lattice melting temperature is $`T_m0.49J_{}`$, and the zero field critical temperature, as before, is $`T_{c0}1.14J_{}`$. These parameters are very close to the parameters of one of the cases studied by Sudbø and co-workers in Refs. R7,  and R8,  (they used $`f=1/90`$, $`J_z=(1/49)J_{}`$ and $`L_zL_{}`$). Our results for $`O_L^{}`$ vs $`T/J_{}`$, for three system sizes, $`L_{}=30`$, $`60`$ and $`90`$, are shown as the solid symbols on the left hand side of Fig. 8. These results agree quite closely with those of Sudbø and co-workers (see Fig. 8 of Ref. R7, ), and seem to show what might be a common intersection of the three curves near $`T0.7J_{}`$. However, we now consider the same parameters and sizes $`L_{}`$, only using a different system aspect ratio, $`L_z=L_{}/6`$. The results are shown as the open symbols on the right hand side of Fig. 8. We see that there no longer appears to be a common intersection point, but more importantly, the curves have all shifted dramatically to higher temperatures. Thus, any value of $`T_\mathrm{\Phi }`$ that one might try to extract from $`O_L^{}`$ depends sensitively on the system aspect ratio. We have also considered other values of the aspect ratio $`L_z/L_{}`$, not shown here. The clear trend is that the sharp rise in $`O_L^{}`$ shifts to increasing temperatures as $`L_z/L_{}`$ decreases. But if $`T_\mathrm{\Phi }`$ represents a true phase transition, it must be independent of aspect ratio. We therefore conclude that $`O_L^{}`$ and method (ii) do not give any self-consistent evidence of the proposed vortex loop blowout transition.

The problems with $`O_L^{}`$ are even clearer if we consider the parameters $`f=1/20`$ and $`J_z=0.02J_{}`$, the same ones used for our computation of $`W^2`$ in section III.B. In Fig. 9 we show our results for $`L_{}=10`$, $`20`$, and $`40`$, for the two aspect ratios $`L_z=L_{}`$ and $`L_z=L_{}/2`$. In both cases, there is no common intersection point of the three curves for the three sizes, and the curves for the smaller aspect ratio are shifted to higher temperatures. Note also that, for both aspect ratios, the temperatures at which $`O_L^{}`$ rises to unity lie quite significantly below the value of $`T_\mathrm{\Phi }1.4J_{}`$ found from our analysis of $`W^2`$.

We next consider the the computation of $`O_L`$ using method (ii) (percolating transverse path must close upon itself keeping $`R_{z\alpha }=0`$). In Fig. 10 we show results using the same parameters as were used to compute $`O_L^{}`$in Fig. 8, i.e. $`f=1/90`$, $`J_z=0.02J_{}`$, and $`L_{}=30`$, $`60`$ and $`90`$, for the same two aspect ratios $`L_z=L_{}`$ and $`L_z=L_{}/6`$. We see now that for both aspect ratios, curves for the three different sizes appear to approach a common intersection point, $`T_\mathrm{\Phi }1.17J_{}>T_{c0}1.14J_{}`$, and that this intersection point is independent of aspect ratio (note: for $`L_z=L_{}/6`$, the thinness of the system $`L_z=5`$, for $`L_{}=30`$, presumably makes it too small to be in the scaling region, hence it intersects the other two curves at somewhat lower temperatures).

In Fig. 11 we show similar results using the same parameters as were used in our computation of $`W^2`$ in section III.B, i.e. $`f=1/20`$, $`J_z=0.02J_{}`$ and $`L_z=L_{}`$. We see that the curves of $`O_L`$ vs. $`T/J_{}`$ for the different system sizes, $`L_{}=10`$, $`20`$, $`30`$ and $`40`$, all intersect at a common point, $`T_\mathrm{\Phi }1.4J_{}`$. This is exactly the same value as found in our analysis of $`W^2`$ (see Fig. 2).

We therefore conclude that $`O_L`$ gives a self-consistent determination of $`T_\mathrm{\Phi }`$, and that this value is considerably larger than estimates one would get from consideration of $`O_L^{}`$. In fact, estimates of a $`T_\mathrm{\Phi }`$ from $`O_L^{}`$ all lie below the zero field critical temperature $`T_{c0}`$ and decrease as $`f`$ increases, while the values determined from $`O_L`$ all lie above $`T_{c0}`$, and increase as $`f`$ increases.

If $`O_L`$ is indeed a scale invariant quantity, we can postulate that it should obey a scaling relation similar to $`W^2`$, i.e.,

$$O_L(T,L_{})=\stackrel{~}{f}(tL^{1/\nu })$$
(15)
Based on our analysis of $`W^2`$ in section III.B, we may expect $`\nu 1`$. In Fig. 12 we therefore show a scaling collapse of the data for $`f=1/90`$ from Fig. 10, plotting $`O_L`$ vs. $`[(TT_\mathrm{\Phi })/J_{}]L_{}`$, where $`T_\mathrm{\Phi }`$ is determined by a best fit of the data to the scaling form. We find a reasonably good collapse for all sizes, for both aspect ratios, using a single value of $`T_\mathrm{\Phi }1.168J_{}`$.

In Fig. 13 we show a similar scaling collapse of the data for $`f=1/20`$ from Fig. 11. Fitting the data for $`O_L`$ to a 4th order polynomial expansion of the scaling function, we find an excellent collapse, for all system sizes, using the parameters $`T_\mathrm{\Phi }1.399J_{}`$ and $`\nu =1.006`$. These results agree very well with the values obtained from the scaling analysis of $`W^2`$, given in section III.B. The quality of the collapse is very much better here than it was for $`W^2`$ in Fig. 4.

Finally, in analogy with the winding $`W_z^2`$, we have also considered the probability $`O_{Lz}`$ to find a vortex path percolating through the system in the negative $`\widehat{z}`$ direction, opposite to the applied magnetic field. We expect $`O_{Lz}`$ to obey a scaling relation similar to that of Eq. (15). To compute $`O_{Lz}`$ we have used tracing method (iii) in which we explicitly search through all possible connections to find any such paths. We show our results for $`O_{Lz}`$ vs. $`T/J_{}`$ for vortex density $`f=1/20`$ and anisotropy $`J_z=0.02J_{}`$ in Figs. 14 and 15, for system aspect ratios $`L_z=L_{}`$ and $`L_z=L_{}/5`$ respectively. As with $`W_z^2`$ shown in Figs. 5 and 6, the intersection points of the curves for different sizes appear to decrease in temperature as $`L_{}`$ increases. Again, we cannot say if this is a failure of our scaling hypothesis, or a failure to reach sufficiently large $`L_z`$. Also, analogous to our findings for the windings $`W^2`$ and $`W_z^2`$, $`O_{Lz}`$ appears to be vanishing at a temperature above the $`T_\mathrm{\Phi }=1.4J_{}`$ where the curves of $`O_L`$ intersect.

## V Specific Heat

If $`T_\mathrm{\Phi }`$, as determined by $`W^2`$ or $`O_L`$, does indeed represent a true thermodynamic transition, we would expect to see some signature of this transition in more conventional thermodynamic quantities. In the recent experiments of Ref.R9, , a step like anomaly in the specific heat $`C`$ was observed in the vortex line liquid region, reminiscent of an inverted mean field transition. In their numerical simulations,R7 ; R8  Nguyen and Sudbø claimed to see an anomalous glitch in the specific heat at the temperature they identified as $`T_\mathrm{\Phi }`$ from their calculation of $`O_L^{}`$. However, this glitch corresponded to only a single data point very slightly displaced above an otherwise smooth background; and in the previous section we have demonstrated that $`O_L^{}`$ significantly underestimates $`T_\mathrm{\Phi }`$, hence there is no reason to expect any anomaly in $`C`$ at that temperature.

In this section we report on high precision measurements of the specific heat $`C`$, for the same parameters we have studied in the earlier sections. If the $`T_\mathrm{\Phi }`$, as found using the vortex path tracing method (ii), is indeed a true thermodynamic phase transition with critical exponent $`\nu 1`$ (as our scaling analyses found), then hyperscaling would suggest a specific heat exponent of $`\alpha =2d\nu 1`$. We thus do not expect to see a diverging $`C`$, however some feature should be present.

In Fig. 16 we plot $`C`$ vs. $`T/J_{}`$, in the near vicinity of $`T_\mathrm{\Phi }1.4J_{}`$, for the same parameters $`f=1/20`$, $`J_z=0.02J_{}`$, and $`L_z=L_{}`$ as used in Figs. 2, 11 and 13. We show results for $`L_{}=10`$, $`20`$, $`30`$ and $`40`$, using from $`310\times 10^7`$ Monte Carlo passes through the lattice, depending on the system size. We find no noticeable finite size dependence, and no hint of any feature at all, near the previously determined $`T_\mathrm{\Phi }1.4J_{}`$.

In Fig. 17 we plot $`C`$ vs. $`T/J_{}`$, over a broad temperature range, for the same parameters $`f=1/90`$ and $`J_z=0.02J_{}`$ as used in Figs. 10 and 12, but for a single large system size $`L_{}=30`$ and $`L_z=90`$. Again we see no hint of any anomaly near the previously determined $`T_\mathrm{\Phi }1.168J_{}`$.

## VI Conclusions

We have carried out detailed Monte Carlo investigations of the 3D uniformly frustrated XY model in order to search for a proposed “vortex loop blowout” transition within the vortex line liquid phase of a pure extreme type-II superconductor. Such a transition had been predicted from general theoretical arguments by Tešanović.R5  Evidence for such a transition was claimed in numerical simulations by Sudbø and co-workers,R6 ; R7 ; R8  and in specific heat measurements on high purity YBCO single crystals.R9  We have made explicit measurements of the vortex line windings $`W^2`$ and $`W_z^2`$, which are the key quantities in Tešanović’s theory. We have re-examined Sudbø’s calculation of the percolation probability $`O_L`$.

Our results raise several questions concerning Tešanović’s theory. We have found that the values of $`W^2`$ and $`W_z^2`$ depend sensitively on the precise scheme one uses to trace out vortex line paths. For the natural choice of random connectivity at vortex line intersections, both $`W^2`$ and $`W_z^2`$ appear to vanish at all temperatures as $`L\mathrm{}`$. Only when we specifically search first for percolating paths, when computing the windings, do we find that the windings converge to non zero values above a certain temperature. In this case, we find that the transverse winding $`W^2`$ obeys the finite size scaling form expected from Tešanović’s theory, however the critical exponent we find is $`\nu 1`$, rather than the predicted $`\nu _{XY}2/3`$ of the inverted 3D XY transition. For the longitudinal winding $`W_z^2`$ we have been unable to find the expected scaling form. Whether this is because $`W_z^2`$ does not scale, or because our systems are all too small to be in the scaling limit, we cannot be certain. It does appear that, upon cooling, $`W_z^2`$ vanishes at a temperature above that where $`W^2`$ vanishes. This would be contrary to Tešanović’s theory. However, since we have not succeeded to find scaling for $`W_z^2`$, we cannot be certain of knowing exactly where it vanishes as $`L\mathrm{}`$.

Independent of Tešanović’s theory, it is natural to think that, as temperature and hence vorticity increases, the vortex lines may form percolating paths (note however that the directedness of the vortex line segments, and the condition of divergenceless paths, means that this is no ordinary percolation problem!). We have therefore, following Sudbø and co-workers, searched explicitly for such percolating paths in the direction transverse to the applied magnetic field, as well as in the direction parallel but opposite to the applied magnetic field. Defining transverse percolation as the existence of a vortex line path that extends entirely across the system in the direction transverse to the applied magnetic field without simultaneously extending entirely across the system in the parallel direction, we have shown that Sudbø’s procedure, which ignores the transverse periodic boundary conditions and does not require the percolating path to close upon itself, leads to inconsistent predictions for the transition temperature as one varies the system aspect ratio. Only by requiring that the transverse percolating path close upon itself, without ever winding in the parallel direction, do we find a consistent transition temperature independent of aspect ratio. The percolation transition found this way agrees both in critical temperature $`T_\mathrm{\Phi }`$ and exponent $`\nu `$ with the results from our analysis of the transverse winding $`W^2`$. We have also computed the probability to find a percolating path in the direction parallel but opposite to the applied magnetic field. Here, analogous to our results for $`W_z^2`$, this negative $`\widehat{z}`$ percolation appears to occur at a temperature higher than that of the transverse percolation, however we have not succeeded to find a clear scaling of this parallel percolation probability.

Note that the transverse percolation transition temperature $`T_\mathrm{\Phi }(f)`$ that we find increases above the zero field transition temperature $`T_{c0}`$ as the magnetic flux density $`f`$ increases. This is in striking contrast to the conclusion of Sudbø and co-workers who proposed $`T_\mathrm{\Phi }(f)`$ to decrease below $`T_{c0}`$ as $`f`$ increases.

While our results do seem consistent with a well defined transverse percolation transition, one can ask if this is a purely geometrical feature of the vortex line paths, or whether it also corresponds to a true thermodynamic phase transition, i.e. something one could detect in a suitable thermodynamic derivative of the free energy. To investigate this question we have carried out high precision Monte Carlo measurements of the specific heat $`C`$. Our results for $`C`$ show no feature whatsoever near the percolation transition $`T_\mathrm{\Phi }`$, nor do we find any finite size effect. In particular we see no evidence for a step like feature as was observed experimentally in YBCO.

To conclude, we have found evidence for a well defined transverse percolation temperature within the vortex line liquid phase of a model type-II superconductor. The connection between this transition and Tešanović’s theory of a vortex loop “blowout” transition remains unclear. It also remains unclear whether or not this percolation transition has any observable thermodynamic manifestation.

## Acknowledgements

We would like to thank Prof. Z. Tešanović and Prof. A. Sudbø for many helpful conversations. This work was supported by the Engineering Research Program of the Office of Basic Energy Sciences at the Department of Energy grant DE-FG02-89ER14017, the Swedish Natural Science Research Council Contract No. E 5106-1643/1999, and by the resources of the Swedish High Performance Computing Center North (HPC2N). Travel between Rochester and Umeå was supported by grants NSF INT-9901379 and STINT 99/976(00).


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# Hard X-ray and radio observations of Abell 754

## 1 Introduction

Shocks and turbulence associated with a major cluster merger event could provide the ingredients necessary to the formation of extended radio regions detected so far in a limited number of clusters, namely a diffuse magnetic field amplification and particle reacceleration (Tribble 1993; Roettiger, Burns, & Stone 1999; Roettiger, Stone, & Burns 1999; Brunetti et al. 2001). The existence of Mpc-scale radio halos or relics combined with the relatively short radiative lifetimes suggests an in-situ electron reacceleration induced by a very recent or current merger event. This hypothesis is supported by observational evidence (Feretti 1999). The existence of large radio regions could be at the origin of the nonthermal hard X-ray (HXR) emission detected in the Coma cluster (Fusco-Femiano et al. 1999; Rephaeli, Gruber, & Blanco 1999) and Abell 2256 (Fusco-Femiano et al. 2000) both showing extended radio emission. A considerable fraction of the input energy during a merger process can be released in particle acceleration and re-emitted in various energy bands. In particular, the same accelerated electrons responsible for the diffuse radio synchrotron emission can scatter the Cosmic Microwave Background (CMB) photons to produce nonthermal inverse Compton (IC) X-ray emission. Alternative relativistic particles to primary re-accelerated electrons emitting in radio halos or relics and responsible for IC nonthermal HXR emission could be secondary electrons produced in the interactions of cosmic rays in the ICM (Dennison 1980; Blasi & Colafrancesco 1999).

X-ray and optical observations report a violent merger event in the galaxy cluster Abell 754 (Henry & Briel 1995; Zabludoff & Zaritsky 1995; Henriksen & Markevitch 1996; Bliton et al. 1998; Markevitch et al. 1998; De Grandi & Molendi 2001) and a numerical hydro/N-body model of this cluster (Roettiger, Stone, & Mushotzky 1998) has shown that many of its observed morphological properties can be explained by a very recent merger ($`<`$ 0.3 Gyr), slightly off-axis, between two clusters having a total mass-ratio less than 2.5:1. Therefore, the intracluster medium (ICM) of A754 appears to be a suitable place for the formation of radio halos or relics. As a consequence, radio and HXR observations of this cluster are relevant to establish robust evidence of the suggested link between the presence of nonthermal phenomena and merger activity in clusters of galaxies and to obtain information on the processes that can inject relativistic electrons. The cluster has been recently imaged at 74 and 330 MHz with the NRAO VLA observatory (Kassim et al. 2001) suggesting the existence of a radio halo and at least one radio relic. Observations at higher resolution and sensitivity are required to confirm the obtained results. A754 was observed in hard X-rays with RXTE in order to search for a nonthermal component (Valinia et al. 1999). The fit to the PCA and HEXTE data set an upper limit of $``$ 1.4$`\times `$ 10$`{}_{}{}^{12}\mathrm{erg}\mathrm{cm}^2\mathrm{s}^1`$ in the 10-40 keV band to the nonthermal emission.

In this paper we present the results of a high sensitivity VLA radio observation at 1.4 GHz and of a long BeppoSAX observation, exploiting the unique capabilities of the PDS (Frontera et al. 1997) to search for HXR emission. We discuss the new radio data and the origin of the excess detected at energies above $``$ 45 keV with respect to the thermal emission.

Throughout this paper, we assume a Hubble constant of $`\mathrm{H}_0=50\mathrm{km}\mathrm{s}^1\mathrm{Mpc}^1h_{50}`$ and $`q_0`$ = 1/2, so that an angular distance of $`1^{}`$ corresponds to 86 kpc ($`z_{A754}`$ = 0.054; Bird 1994). Quoted confidence intervals are at a 90% level, if not otherwise specified.

## 2 Hard X-ray data

### 2.1 PDS and MECS data reduction

The pointing coordinates of BeppoSAX are at J2000 $`\alpha `$ = 9h 9m 21.0s, $`\delta `$ = -9 41 24.0". The total effective exposure time for the PDS was $``$ 84250 sec in the two observations of 2000 May 6th and May 17th. The observed count rate was 0.333 $`\pm `$ 0.021 counts s-1 in the 15-100 keV energy range, at a confidence level of $``$16$`\sigma `$.

Since the source is rather faint in the PDS band (approximately 2 mcrab in the 15-100 keV), a careful check of the background subtraction must be performed. PDS spectra were extracted using the XAS v2.0 (Chiappetti & Dal Fiume 1997). The background sampling was performed using the default rocking law of the two PDS collimators that samples ON,+OFF, ON,-OFF fields for each collimator with a dwell time of 96 s (Frontera et al. 1997). When one collimator is pointing ON source, the other collimator is pointing toward one of the two OFF positions. We used the standard procedure to obtain PDS spectra (Dal Fiume et al. 1997); this procedure consists of extracting one accumulated background spectra in the two different +/-OFF sky direction. The comparison between the two accumulated backgrounds (\[+OFF\]vs.\[-OFF\]) shows a difference in the pointings for the first of the two observations. In particular, the background in the position +OFF was much greater than that in position -OFF. So, for the analysis, we have considered only the background in the -OFF position. In the second observation we do not find differences between the spectra extracted from the two offset positions. The background level of the PDS is the lowest and most stable obtained so far with the high-energy instruments on board satellites thanks to its equatorial orbit. No modelling of the time variation of the background is required. The correctness of the PDS background subtraction has been checked by verifying that the counts fluctuate at about zero flux as the signal falls below detectability. This happens at energies greater than $``$ 75 keV.

The total exposure time for the MECS was $``$ 1.85$`\times `$105 sec with a count rate of 0.748 $`\pm `$ 0.002 counts s-1. MECS data preparation and linearization were performed using the SAXDAS package under an FTOOLS environment. We have extracted an MECS spectrum from a circular region of $``$ 20 radius (corresponding to about 1.7 Mpc). From the ROSAT PSPC radial profile, we estimate that about 95% of the total cluster emission falls within this radius. The background subtraction has been performed using spectra extracted from blank sky event files in the same region of the detector as the source. For more details see De Grandi & Molendi (2001) that used the same MECS data to determine the temperature profile of A754.

A numerical relative normalization factor among the two instruments has been included in the fitting procedure (see next section) to account for (1) the fact that the MECS spectrum included emission out to $``$ 1.7 Mpc from the X-ray peak, while the PDS field of view (FWHM = 1.3) covers the entire emission from the cluster; (2) the slight mismatch in the absolute calibration of the MECS and PDS response matrices employed; and (3) the vignetting in the PDS instrument (the MECS vignetting is included in the response matrix). The estimated normalization factor is $``$ 0.8. In the fitting procedure, we allow this factor to vary within 15% from the above value to account for the uncertainty in this parameter.

## 3 Radio data

A radio observation at 1.365 GHz was obtained with the Very Large Array (VLA) in D configuration on September 25, 2000, for a total integration time of about 2.5 h. Data were calibrated and reduced with the Astronomical Image Processing System (AIPS), following the standard procedure (Fourier inversion, Clean and Restore, Self-calibration).

The radio image obtained with angular resolution of 70″ is presented in Fig.1, overimposed onto the optical image. The rms noise is of 0.1 mJy/beam, i.e. about 5 times better than the NRAO VLA Sky Survey (NVSS) image (published by Giovannini et al. 1999). The diffuse emission detected here is complex and it is much more extended than in any previous image at any frequency.

The cluster halo is easily visible around the brightest optical cD galaxy. This emission is not detected in the NVSS, but is detected at 330 MHz and 74 MHz by Kassim et al. (2001). As pointed out by these authors, several discrete sources are embedded within the radio halo. In addition, we detect in the present image an extended diffuse emission to the east of the halo. Although a connection of this emission to the radio halo cannot be excluded, we tentatively classify this feature as a peripheral cluster relic. The cluster radio relic is detected by Kassim et al. (2001) at 74 MHz and not at 330 MHz. At 74 MHz it is much less extended than the feature detected here at 1.4 GHz, and it is located at the eastern boundary of our relic image. The possible connection relic-halo present in the 1.4 GHz image does not appear in the 74 MHz image.

The total flux density of the radio halo at 1.4 GHz, after subtraction of the discrete sources, is 86 $`\pm `$ 2 mJy. Comparison to the total flux at 330 MHz given by Kassim et al. (2001) leads to a spectral index $`\alpha _{330}^{1400}`$ $``$ 1.5. The halo spectrum appears to be steeper than that estimated by the previous observations in the 74-330 MHz frequency band ($`\alpha _{74}^{330}`$ $``$ 1.1), indicating the presence of a spectral cutoff. The total flux density of the relic is 69 $`\pm `$ 2 mJy. Since the relic source in the map of Kassim et al. (2001) at 74 MHz is significantly less extended than in the present map at 1.4 GHz, we obtain a lower limit $``$ 1 for the spectral index in the range 74-1400 MHz. An upper limit of $``$ 1.7 in the range 330-1400 MHz is derived from the lack of detection in the 330 MHz image of Kassim et al. (2001).

### 3.1 Hard X-ray results

The temperature profile derived from the MECS data analysis of this BeppoSAX observation confirms that A754 is an extremely disturbed and substructured cluster, as reported in previous X-ray and optical observations. The MECS spectrum is extracted from a circular region of radius $`20^{}`$ that gives a mean temperature of 9.42$`{}_{0.17}{}^{}{}_{}{}^{+0.16}`$ keV consistent with the value of $``$ 9 keV determined from other X-ray instruments (ASCA GIS, Ginga LAC, RXTE PCA) within their respective errors bars. The iron abundance results to be 0.25$`{}_{0.03}{}^{}{}_{}{}^{+0.04}`$. These results are reported in De Grandi & Molendi 2001.

To search for a nonthermal component in the spectrum of A754, we have performed a simultaneous fit (see Fig. 2) to the MECS and PDS data with a MEKAL model that reports an average gas temperature of $``$9.4 keV ($`\chi ^2`$=194.4 for 158 d.o.f.). A systematic error of 1% was added in quadrature to the statistical uncertainties of the spectral data of the PDS, on the basis of the results obtained from routinely performed Crab Nebula observations. The normalization factor for the two data sets is $``$ 0.72. At energies above $``$ 45 keV there is a conspicuous excess with respect to thermal emission at a confidence level of $`3.2\sigma `$. This long BeppoSAX observation is composed of two observations with a time interval of few days and the separate data analysis does not evidence significative variability. We infer a robust indication for the nonthermal nature of the detected excess by fitting the MECS/PDS data with a 2-T model and with a T plus a power law model. In the first model one of the temperatures has the value of $``$ 9.4 keV, while the second temperature assumes unrealistic values greater than 50-60 keV that strongly support a nonthermal mechanism for the second component. In the second model the fit, with a $`\chi ^2`$ value of 177.4 for 156 d.o.f., is not able to determine the spectral index, but the improvement of the $`\chi ^2`$ value with respect to a single thermal component (MEKAL model) is significant at more than 99.92% confidence level, according to the F-test. In the 10 - 40 keV energy range the fit gives a nonthermal flux of $`1.6\times 10^{12}\mathrm{erg}\mathrm{cm}^2\mathrm{s}^1`$ consistent with the upper limit reported by the RXTE observation (Valinia et al. 1999).

In the next session we discuss the origin for the detected nonthermal excess considering the presence of the radio halo in the ICM of the cluster and that of the radio galaxy 26W20, which displays BL Lacertae characteristics (Silverman, Harris, & Junor 1998), in the field of view of the PDS at a distance of about 27 from the BeppoSAX pointing.

## 4 Discussion

Nonthermal X-ray emission has been detected in the Coma cluster and Abell 2256 by the PDS onboard BeppoSAX , while a flux upper limit has been reported for Abell 3667 (Fusco-Femiano et al. 2001). The deviation of these ”hard tails” from the the thermal bremsstrahlung spectra appears to start at energies above 20-25 keV. A likely origin for the detected nonthermal HXR radiation is IC emission by scattering of CMB photons by the radio synchrotron electrons responsible for extended radio regions present in the center (radio halo) or in the periphery (radio relic) of the cluster. Alternative mechanisms to the IC model have been proposed (Blasi & Colafracesco 1999; Sarazin & Kempner 2000; Dogiel 2000; Blasi 2000; Liang, Dogiel, & Birkinshaw 2002), some of these motivated by the discrepancy between the value for the intracluster magnetic field derived by the BeppoSAX observation of the Coma cluster ($`B_X0.16\mu G`$; Fusco-Femiano et al. 1999) and the value derived from the Faraday rotation ($`B_{FR}6\mu G`$; Feretti et al. 1995) of polarized radiation of sources through the ICM. Recently, Newman, Newman, & Rephaeli (2002) have pointed out that many and large uncertainties are associated to the determination of $`B_{FR}`$ (see also Govoni et al. 2002). However, this discrepancy can be attenuated considering models that include the effects of more realistic electron spectra, spatial profiles of the magnetic fields and anisotropies in the pitch angle distribution of the electrons (Goldshmidt & Rephaeli 1993; Brunetti et al. 2001; Petrosian 2001). Another possibility is that the detected excesses are due to the presence of very obscured sources like Circinus (Matt et al. 1999) in the field of view of the PDS (1.3). In the case of Coma and A2256 the analysis of the MECS images excludes the presence of this kind of sources in the central region ($``$ 30 in radius) of the cluster unless the obscured source is within 2 of the central bright cores. We have re-observed A2256 after about two years from the first observation and the two spectra are consistent (Fusco-Femiano et al. 2002). Besides, both observations comprise two exposures with a time interval of $``$ 1 year and $``$ 1 month, respectively and all these observations do not show significant flux variations. These results and the fact that the two clusters, Coma and A2256, with a detected HXR excess both have extended radio regions strongly supports the idea that a diffuse nonthermal mechanism involving the ICM is responsible for the observed excesses. Support to this interpretation is given by a second recent RXTE observation of the Coma cluster (Rephaeli & Gruber 2002) that confirms the previous observation (Rephaeli, Gruber, & Blanco 1999) of a likely presence of a nonthermal component in the spectrum of the cluster.

For A754 we discuss two possible origins for the detected excess at the level of $`3.2\sigma `$, lower than that measured in Coma and A2256 ($`4.5\sigma `$). As reported in the Introduction, the ICM of A754 appears to be a suitable place to host relativistic electrons considering that X-ray and optical observations indicate that the cluster is undergoing a violent merger process, and that Hydro/N-body simulations show that the merger must be very recent. The time elapsed from the start of the merger in A754 ($`<`$ 0.3 Gyr) is not greater than the radiative lifetime for electrons with $`\gamma 10^4`$. Shocks and turbulence associated with a recent or current major merger event can be able to provide energy for particle acceleration and magnetic field amplification to produce diffuse radio emission (Tribble 1993; Brunetti et al. 2001). This scenario seems to be confirmed by the presence of diffuse radio emission (Kassim et al. 2001) and now definitely confirmed by our deeper VLA observation at higher resolution at 1.4 GHz. The nonthermal HXR detected by the PDS could be IC emission by the same radio electrons scattering CMB photons. The lack of variability in the nonthermal flux detected by this long BeppoSAX observation is compatible with a diffuse mechanism of the observed excess. Assuming that the measured nonthermal flux of $`10^{11}\mathrm{erg}\mathrm{cm}^2\mathrm{s}^1`$ in the 40-100 keV energy range is due to IC emission, the volume-averaged intracluster magnetic field is $`0.1\mu G`$ obtained combining the radio halo and X-ray fluxes (see Fusco-Femiano et al. 1999, eq.1) and using our measured value of 1.5 for the radio halo index. A similar value of $`B_X`$ is obtained for the radio relic assuming a radio spectral index of 1.7. The equipartition value of the magnetic field, computed with standard assumptions, is in the range $`0.30.6\mu G`$.

The presence of diffuse radio radiation in A754, considered the prototype of a merging cluster, is a further evidence of the link between Mpc-scale radio emission and very recent or current merger processes (Feretti 1999). Radio observations and the detection of nonthermal HXR emission are of great importance for the understanding of the origin of the electron population responsible for nonthermal phenomena in clusters of galaxies. In the Coma cluster, the prototype of halo clusters, the spectral cut-off (Deiss et al. 1997) represents a strong indication for the presence of a cut-off in the emitting electron spectrum. This cut-off and the HXR excess detected in the Coma cluster may be naturally accounted for in the context of re-acceleration models (Brunetti et al. 2001) in which relativistic electrons with $`\gamma `$ 100-300, produced by several sources in galaxy clusters and accumulated in the cluster volume over cosmological time, can be re-accelerated by various processes at the energies required to explain the radio halo in the Coma cluster. This cut-off is not naturally expected if the radio emission is produced by secondary electrons (Brunetti 2002) due to the decay of charged pions generated in cosmic ray collisions (Dennison 1980; Blasi & Colafrancesco 1999; Dolag & Ensslin 2000; Miniati et al. 2001). The radio and HXR observations of A754 seem to confirm the scenario described by the re-acceleration models in the Coma cluster. The detection of the hard excess in A754 determines, in the framework of the IC model, a volume-averaged intracluster magnetic field of the same order ($`B_X0.1\mu G`$) of that determined in the Coma cluster (Fusco-Femiano et al. 1999). This value of $`B_X`$ implies relativistic electrons at energies $`\gamma 10^4`$ to explain the observed diffuse synchrotron emission. At these energies IC losses may determine a cut-off in the electron spectrum in agreement with the spectral cut-off observed in A754. So, the radio and HXR results obtained by our observations of A754 support the scenario that primary and not secondary electrons are responsible for nonthermal emission in clusters of galaxies.

However, we cannot ignore the presence of the radio galaxy 26W20 in the field of view of the PDS, located at a distance of about 27 from the BeppoSAX pointing, that could be responsible for the hard excess in A754. This source, discovered in the Westerbork radio survey by Harris et al. (1980), shows a X-ray bright core similar to that of a BL Lac object but with weak emission lines and this makes 26W20 different from a typical BL Lac object. The source is preferred to be classified as tailed radio galaxy for the presence of a single jet or tail and being member of a small group of galaxies. The radio galaxy has had several X-ray observations due to its close proximity to A754. It was first observed with Einstein (Harris, Costain & Dewdney 1984) and the IPC spectrum could be equally well fit by a power law (energy index 0.8$`\pm `$0.4) or with a thermal model (kT $``$ 3 keV). In the following the nonthermal nature of the X-ray emission was clarified by a ROSAT observation. In particular, the fit to an on-axis PSPC observation gives a core emission described by a nonthermal model with energy index 1.32$`\pm `$0.17 and log $`N_H=20.90\pm 0.04`$. The X-ray luminosity is $`3\times 10^{43}\mathrm{erg}\mathrm{s}^1`$ in the 0.5 - 3 KeV energy range (Silverman, Harris, & Junor 1998). The source shows variability. An 18% increase in the luminosity has been determined by two PSPC observations within 5 days in 1992.

The spectral energy distributions (SED) of BL Lac sources are characterized by two main peaks. The peak at low energy is commonly explained as synchrotron emission by relativistic electrons while that at higher energies as IC emission of the same electrons scattering the synchrotron photons (e.g. Dermer et al. 1997; Ghisellini et al. 1998).

In Figure 3 we show the SED for 26W20 where the highest energy points refer to the PDS observation assuming that this source is responsible for the detected excess. The fit with a Synchrotron Self-Compton (SSC) model is consistent with the SED of a BL Lac object (Perry 2001; Padovani, Perlman, & Landt 2002; Giommi et al. 2002), but a flat energy index of about 0.3 is required to extrapolate the flux detected by ROSAT in the PDS energy range, taking into account the angular response of the detector. The inclusion of the PDS points makes difficult to fit well all the points of the SED. However, due to the variability of this kind of sources only simultaneous observations can be used to fix the spectral properties in a large energy band. Unfortunately, the source does not appear in the field of view of the MECS because hidden by one of the calibration sources of the instrument.

## 5 Conclusions

Our VLA observation at 1.4 GHz definitely confirms diffuse radio emission in A754 composed by a radio halo and a relic, although a connection relic-halo cannot be excluded. The relic image at 1.4 GHz appears much more extended than that detected at 74 MHz by Kassim et al. (2001). Our observation determines with accuracy the slope of the radio halo spectrum in the 0.3-1.4 GHz frequency range that results to be steeper than that obtained in the band 74-330 MHz, indicating the presence of a radio spectral cutoff. A BeppoSAX observation of A754 shows a nonthermal HXR excess at energies above $``$ 45 keV with respect to the thermal emission, at a confidence level of $`3\sigma `$. One possible explanation is IC emission for the same relativistic electrons responsible for the diffuse radio emission. This interpretation has been invoked to explain the nonthermal emission detected in Coma and A2256 both showing extended radio regions. The lack of significative variability of the nonthermal flux detected in A754 is consistent with a diffuse mechanism for the observed excess. This detection, that needs to be confirmed by future observations, and the radio results seem indicate that primary re-accelerated electrons and not secondary electrons are at the origin of the observed nonthermal emission in clusters of galaxies. At present, it exists also the possibility that the radio galaxy 26W20, located in the field of view of the PDS, is responsible for the reported hard excess. The extrapolation of the ROSAT flux in the PDS energy range requires a flat index to explain the nonthermal HXR flux. However, considering the non simultaneity of the ROSAT and BeppoSAX observations the SED may have assumed a different shape at the moment of the BeppoSAX observation. To discriminate between these two interpretations a hard X-ray observation with imaging instruments is necessary.

###### Acknowledgements.

We thank G.Brunetti and P.Giommi for useful suggestions regarding the interpretation of the results. We are grateful to the referee for the stimulating comments.


text:
# A possible mechanism for cold denaturation of proteins at high pressure

## Abstract

We study cold denaturation of proteins at high pressures. Using multicanonical Monte Carlo simulations of a model protein in a water bath, we investigate the effect of water density fluctuations on protein stability. We find that above the pressure where water freezes to the dense ice phase ($`2`$ kbar), the mechanism for cold denaturation with decreasing temperature is the loss of local low-density water structure. We find our results in agreement with data of bovine pancreatic ribonuclease A.

Some proteins become thermodynamically unstable at low temperatures, a phenomenon called cold denaturation Pace ; Privalov ; Jonas . This phenomenon has been mainly observed at high pressures, ranging from approximately 200 MPa up to 700 MPa Kunugi . An explanation of the $`PT`$ phase diagram of a protein with cold denaturation has been proposed Hawley , but a microscopic understanding of the mechanisms leading to cold denaturation has yet to be developed, due in part to the complexity of protein-solvent interactions.

Existing theories of folding and unfolding of diluted proteins consider hydrophobicity as the driving force of protein stability Kauzmann ; Dill ; DillII ; Hummer98 ; Chandler . In the case of apolar macromolecules, hydrophobicity has been identified with the assembly and segregation of the macromolecule to minimize the disruption of hydrogen bonds among water molecules Kauzmann ; Chandler ; Stillinger . Water tends to be removed from the surface of apolar molecules, forming a cage composed of highly organized water molecules around the molecule, where the disruption of hydrogen bonds is minimized Frank . The simplest hydrophobic model features an effective attraction between hydrophobic molecules Vanderzande , but does not reproduce cold denaturation. In order to obtain cold denaturation with this model, new studies Dill89 ; Shimizu02  had to insert a temperature-dependent attraction derived from experimental observations at ambient pressure Nozaki71 . An explicit account of water around the hydrophobic molecules has also been considered in order to understand the cold denaturation process with temperature-independent interactions. Theoretical attempts modeled the effective water-protein interactions with the free energy cost of excluding the solvent around the nonpolar molecule Stillinger ; Pratt . Numerical simulations based on these attempts have been applied to study the pressure denaturation found in proteins Hummer98 .

Not until recently has cold denaturation been studied at the microscopic level. Simplified models Rios , based on a bimodal description of the energy of water in the shell around the hydrophobic molecule Muller , predicted cold denaturation. Similar results were obtained using a lattice model of a random hydrophobic-hydrophilic heteropolymer interacting with the solvent Trovato . Several models mimicking the interaction between water molecules and non-polar monomers have also been applied to the study of cold denaturation. Bakk . One possible reason for the inability of the previous models to capture both the molecular details of cold denaturation and the effect of pressure is the neglect of (i) correlations among water molecules near the freezing point, and (ii) the density anomaly due to the tetrahedral structure of the hydrogen bonded network. Here, we implement a two-dimensional lattice model of water that captures the above mentioned water properties FranzeseII . In the model, the possible orientations of water molecules are set by the allowed values of a $`q`$-state Potts variable $`\sigma _i`$. Only when two neighbor molecules $`i,j`$ are in the correct orientation ($`\sigma _i=\sigma _j`$) does a hydrogen bond (HB), that increases the volume of the system by $`\mathrm{\Delta }V`$, form. This interaction mimics the increment of volume due to the incipient formation of a tetrahedral structure. If the two neighbor molecules $`i,j`$ are not in the correct orientation, the interaction of the particles does not imply any increment in volume. The Hamiltonian for our model of water-water interaction may be written as FranzeseII

$$_{HB}=J\underset{i,j}{}\delta _{\sigma _i,\sigma _j},$$
(1)
were $`J>0`$ is the scale of the interaction between water molecules upon tetrahedral network formation. The total volume of the system is given by $`V=V_0+N_{HB}\mathrm{\Delta }V`$, where $`N_{HB}=_{i,j}\delta _{\sigma _i,\sigma _j}`$ is the total number of hydrogen bonds with $`\mathrm{\Delta }V>0`$ in the system. The sum $`_{i,j}`$ extends only to nearest neighbors, implying that two water molecules cannot form a hydrogen bond with $`\mathrm{\Delta }V>0`$ if they are separated by one residue of the protein. The enthalpy of the system ($`_{HB}+PV`$) is given by

$$_{HB}+PV=(JP\mathrm{\Delta }V)\underset{i,j}{}\delta _{\sigma _i,\sigma _j},$$
(2)
where $`P`$ is the pressure applied to the system.

Our model solvent features a limiting pressure $`P_c=J/\mathrm{\Delta }V`$. Above $`P_c`$, we find that $`N_{HB}`$ decreases as we decrease the temperature, and the water model undergoes a transition to a state where all hydrogen bonds with $`\mathrm{\Delta }V>0`$ are broken. Below $`P_c`$, we find that $`N_{HB}`$ increases as we decrease the temperature, and the water model undergoes a sharp transition, at $`T=T_c=(JP\mathrm{\Delta }V)/(\mathrm{ln}(1+\sqrt{q}))`$ FranzeseII , to a state where all hydrogen bonds with $`\mathrm{\Delta }V>0`$ are formed. Thus, our water model reproduces the freezing of water to low and high density ice, since for $`P<P_c`$ ($`P_c200`$MPa in real water) water freezes to the low density ice Ih, and for $`P>P_c`$, water freezes to the high density ice II Petrenko . A relation between these two phases of ice and protein folding has already been suggested from a thermodynamic point of view Wilse .

We model the protein as a self-avoiding random walk embedded in a water bath. For simplicity, we consider a non-polar homopolymer that interacts with water via the partial ordering of water molecules, forming hydrogen bonded structures around the protein. We mimic the interaction using the Hamiltonian,

$$_p=J_rn_{HB}(n_{max}\underset{i,j}{}n_in_j),$$
(3)
where the parameter $`J_r>0`$ is the strength of the repulsive interaction and $`n_{HB}N_{HB}/N_{water}`$ is the number density of hydrogen bonds with $`\mathrm{\Delta }V>0`$, $`N_{water}`$ is the number of water molecules. The water–protein repulsion increases as the water molecules tend to form the tetrahedral, low–density, hydrogen bonded network, where an unfolded apolar macromolecule is unlikely to be embedded. $`n_{max}`$ is the maximum number of residue–residue contacts and $`_{i,j}n_in_j`$ is the number of residue–residue contacts, where $`n_i=1`$ if the lattice position $`i`$ is occupied with a residue, and zero otherwise. Therefore, $`n_{max}_{i,j}n_in_j`$ is a measure of protein compactness, and equals zero when the protein is maximally compact. Thus, Eq. (3) states that the hydrophobic repulsion driving the protein to a compact state is equal to zero when the protein is maximally compact $`(_{i,j}n_in_jn_{max})`$ or when the water forms the high–density bond network ($`n_{HB}0`$).

We hypothesize that the inability of water molecules to arrange in the low density ice–like structures is the principal mechanism responsible for protein cold denaturation. At low pressures ($`P<P_c`$) and low temperatures, water molecules form a low density hydrogen bonded network, so the protein is forced to adopt a compact state. At high pressures ($`P>P_c`$), the water is not able to form the low density network and forms a more dense state. In this case the effective repulsion between the residues and the solvent decreases, and water molecules penetrate into the protein core, unfolding the compact state. Our hypothesis is supported by the experimental observations Kunugi  that cold denaturation exists mainly at high pressures (of the order of kbars), where water only freezes in the dense ice II phase other .

Next we demonstrate that our model of a protein embedded in a water network with an enthalpy given by

$$𝒲=_p+_{HB}+PV$$
(4)
gives rise to both cold and warm denaturation of the protein and agrees with experimentally-observed protein denaturation at high pressures. Since the energy landscape of the protein interacting with the water network is characterized by a multitude of local minima, we perform multicanonical Monte Carlo simulations to avoid transient trapping of our water-protein system in local energy minima at low temperatures. Specifically, we use the multiple-range random walk algorithm Wang  to calculate the density of states. We adopt the algorithm in order to embed the self-avoiding protein into the lattice, and to calculate the two-parameter density of states $`g(N_{HB},N_c)`$, where $`N_c_{i,j}n_in_j`$ is the number of residue-residue contacts. From the density of states we calculate the temperature and pressure dependence of the average number of residue-residue contacts

$$\overline{N}_c=\underset{N_{HB}}{}\underset{N_c}{}N_cg(N_{HB},N_c)\frac{e^{𝒲(N_{HB},N_c)/T}}{Z},$$
(5)
where $`Z`$ is the partition function. We perform Monte Carlo simulations of a system of $`383`$ water molecules and a protein consisting of $`17`$ non-polar residues with periodic boundary conditions. Fig. 1 shows the dependence of $`\overline{N}_c/n_{max}`$ on temperature for different values of the pressure both above and below $`P_c`$. The calculated density of states $`g(N_{HB},N_c)`$ converges to the true value with an accuracy of the order of $`10^5`$. The value of $`\overline{N}_c/n_{max}`$ ranges from one (maximally compact protein) to approximately $`0.71`$ (which is the average number of residue–residue contacts found at high temperatures). Only when $`P>P_c`$ do we observe the cold denaturation of the protein.

We also reconstruct the phase diagram of the water-protein system in the $`PT`$ plane (Fig. 2). We consider the protein to be in the collapsed state if $`96\%`$ of all possible contacts are formed, i.e., if $`\overline{N}_c/n_{max}>0.96`$. For each pressure value, the freezing lines of water shown in Fig. 2 are given by the temperature at which we observe a maximum in the specific heat of the water bath. We compare our findings to experimental observations Zhang  for bovine pancreatic ribonuclease A studied by 1H NMR spectroscopy. We find remarkable qualitative agreement between the experimental and numerical $`PT`$ phase diagrams. In both experimental and numerical $`PT`$ phase diagrams, we observe that cold denaturation occurs at high pressures and, as we lower the temperature, close to the water–ice II freezing line and in the region where water molecules are not capable of forming low density ice–like structures. In addition to the study of ribonuclease A Zhang , cold denaturation at very high pressures in the kbar range has also been observed in chymotrypsinogen Hawley , myoglobin Hawley , staphylococcal nuclease Panick99  and has been proposed as the principal mechanism for the observed pressure-inactivation of bacteria, such as Escherichia coli Ludwing96 .

Not all proteins behave equally as we decrease temperature at high pressure. In particular, there are some proteins that do not exhibit cold denaturation. We reproduce the variability of protein dynamics at high pressure and low temperature by varying the hydrophobic parameter $`J_r`$ to lower values, effectively impeding a stable compact state for pressures above the $`P=P_c`$ line. In Fig. 3 we present the phase diagrams obtained for different values of $`J_r`$, ranging from two to $`20`$. The shape of the phase diagram changes as we increase the value of the repulsive interaction $`J_r`$, allowing stabilization of the compact state and cold denaturation above the $`P=P_c`$ line.

Within the framework of our model, we reproduce the experimentally-observed thermodynamics of cold denaturation, but we cannot address the kinetics of this process. It could be also feasible to investigate in future work the dynamics with a more sophisticated model, where we consider not just the average number of hydrogen bonds with $`\mathrm{\Delta }V>0`$, but the actual numbers for each water molecule that is a neighbor to a residue.

Recent computer simulations studies Payne97  with all-atom models have studied the effect of pressure and average density on the hydrophobic effect. The authors performed simulations of two Lennard-Jones (LJ) particles in the TIP4P water model Mahoney00 . At constant temperature, they found that the aggregation of the two particles is favored with a moderate increase of pressure, or analogously, with a moderate increase of water density. However, this effect is reversed for pressures in the kbar range, so that aggregation becomes unstable with increasing water density. These studies support our results of a critical pressure above which an increase of pressure leads both to an increase of water density (because of the reduction of the number of hydrogen bonds with $`\mathrm{\Delta }V>0`$) and to destabilization of the model protein. Following these results and based on previous studies Chandler , Shimizu et al. Shimizu02  have shown that three-body interactions have a destabilization effect on the aggregation of three LJ particles. However, the inclusion of these interactions into a model of a more complex protein did not lead to significant changes. Finally, all-atom simulations recently addressed the pressure denaturation of proteins Paci02 , but they have not provided conclusive evidence.

We conclude that the effect of pressure on water density is key for understanding cold denaturation of proteins. The density anomaly of water arises from the low density hydrogen bonded structures responsible for the hydrophobic effect, driving the protein to a compact state Privalov ; DillII ; Chandler ; Frank . At extreme pressures above $`P_c`$, lowering the temperature implies an increasing free energy cost to form a hydrogen bond with $`\mathrm{\Delta }V>0`$, so the density anomaly disappears. In this scenario, the hydrophobic effect decreases and cold denaturation occurs. Our model supports this mechanism. Also, a specific arrangement of amino acids in the protein structure, determined by amino acid interactions, dictates the dynamics of proteins at low temperature and high pressure, thus making some proteins more stable than others at these $`PT`$ conditions.

We thank S. V. Buldyrev, D. Chandler, J. Hermans, G. Hummer, O. Mishima and F. Sciortino for helpful interactions, the NSF Chemistry Program Grant CHE0096892, the Spanish Ministry of Education and the Petroleum Research Fund for support.


text:
# References

PUTTING A SPIN ON THE

AHARONOV-BOHM OSCILLATIONS

Jeeva Anandan

Department of Physics and Astronomy

University of South Carolina

Columbia, SC 29208, USA

and

Clarendon Laboratory

University of Oxford

Parks Road

Oxford, UK

E-mail: jeeva@sc.edu

May 30,2002, revised June 8, 2002.

A slightly different version was published in Science, Vol. 297, 1656 (Sept. 6, 2002).

Of the many fascinating consequences of quantum mechanics, among the more mysterious ones is the Aharonov-Bohm effect. According to classical physics, a charged particle would be influenced by a magnetic field only if the particle goes through a region in which the magnetic field strength is nonzero. But according to quantum mechanics, if the quantum wave representing the state of a charged particle, such as an electron, is split into two waves that go around a solenoid and interfere, the resulting interference pattern is influenced by the magnetic flux enclosed by the waves, even though the particle is nowhere in the region of non vanishing field strength. This was predicted by Aharonov and Bohm in one of the most influential papers of physics in the latter part of the twentieth century . In addition to its charge, the electron has a magnetic moment proportional to its spin. So, if the magnetic field strength is non vanishing along the electron wave, then in addition to the above flux dependent effect, there are also spin dependent effects due to the interaction of the magnetic moment with the magnetic field. If in addition an electric field is present, there is the so the called spin-orbit interaction of the magnetic moment with the electric field , which further influences the interference pattern . All these effects are present in a recent beautiful experiment performed by Yau, De Poortere and Shayegan .

Figure 1. Electrons enter and leave the ring structure as indicated by the horizontal arrows. The quantum wave associated with each electron in the entrance region splits into two wave packets that go around the ring, as indicated by the curved arrows, and interfere in the exit region. Homogeneous magnetic field $`𝐁`$ and electric field $`𝐄`$ are applied normal to the plane of the ring. Whether the interference is constructive or destructive, and correspondingly whether the current is maximum or minimum, depends on the values of $`𝐁`$ and $`𝐄`$. Hence, varying these fields leads to oscillations of the current.

An interesting aspect of this experiment is that it is a miniaturized version of the original experiments that confirmed the Aharonov-Bohm effect . The apparatus consists of a ring structure (Fig. 1) with a diameter of only about one $`\mu `$m (micro-metre or one- thousandth of a millimetre) that is fabricated inside a GaAs/AlGaAs heterostructure. This is an example of the new field of mesoscopic physics that deals with structures that are intermediate between atomic and macroscopic scales. The linear dimensions of the tiny apparatus used in mesoscopic physics vary from about a $`\mu `$m to a nano-metre, which is only about ten times the size of an atom. If such a tiny apparatus made of metals or semi-conductors is made sufficiently cold (about $`30`$ milli-kelvin) then the conduction electron waves are coherent over the entire apparatus, because there is no randomization due to inelastic scattering. This leads to interesting quantum effects. In the present experiment, the conduction electrons are like a quantum gas that enters and exits the ring (Fig. 1), and therefore constitutes a current. Homogeneous magnetic and electric fields are applied normal to the plane of the ring structure. The electric field $`𝐄`$ is needed to confine the electrons to this plane.

It was predicted  that the electrical resistance of the current through a mesoscopic ring would vary as the magnetic flux $`\mathrm{\Phi }`$ through the ring is varied by changing the strength of the magnetic field $`𝐁`$. Moreover, this magneto-resistance is an oscillatory function of the magnetic flux with period $`h/e`$, where $`h`$ is Planck’s constant and $`e`$ is the charge of the electron. This is a consequence of the fact that the Aharonov-Bohm phase shift is $`\frac{2\pi e}{h}\mathrm{\Phi }`$, and the current is maximum when there is constructive interference and minimum when there is destructive interference, for a given externally applied potential. This has been well confirmed by experiments , including the present one (Fig. 2). This means that if one writes the magneto-resistance function $`R(\mathrm{\Phi })`$ as a sum of all possible (normalized) periodic functions of $`\mathrm{\Phi }`$, then the coefficients of this expansion that multiply the functions whose period $`\tau `$ is equal to or very close to $`h/e`$ are very large compared to the other coefficients. In other words, the Fourier transform of $`R`$ that is the function $`\stackrel{~}{R}(f)`$ of the frequency $`f=1/\tau `$ (whose values are the coefficients of the above expansion) would be highly peaked at $`f=e/h`$.

Figure 2. $`\mathrm{\Delta }R`$ is the resistance (in Ohms), after subtracting away a smooth background resistance, in the presence of an externally applied magnetic field $`B`$ (in Teslas). As $`B`$ is varied (with the externally applied electric field fixed), $`\mathrm{\Delta }R`$ oscillates. This is due to the oscillation of the current through the ring structure in Fig. 1 that is inversely proportional to the resistance, for a constant applied potential difference, according to Ohm’s law. (This graph is taken from ref. 4.)

In the experiment of Yau et al , this peak was observed. But in addition two other smaller peaks on either side of the main peak were also observed, suggesting a modulation of the Aharonov-Bohm oscillation of $`R`$. It is reasonable to regard these side peaks as being due to spin-dependent effects. These may be obtained by supposing that the electron interacts with an effective magnetic field  that is $`=𝐁\frac{1}{2}𝐯\times 𝐄`$, where $`𝐯`$ is the ‘velocity’ of the electron in the approximation that its wave is approximately a plane wave. The factor $`\frac{1}{2}`$ distinguishes the electron from the corresponding effective magnetic field experienced by a neutral dipole, such as the neutron, in the combined magnetic and electric fields. For an electron in an atom, this difference is traditionally attributed to the semi-classical Thomas precession . It should be noted that the $`𝐄`$ experienced by the electron is much larger than the applied electric field. This has been determined to be the case experimentally, and has been attributed to complex band effects in the semi-conductor .

The above combined effect of the electric and magnetic fields on the electrons may also be regarded as arising from Berry’s phase . This is a geometric phase acquired by the wave function when it evolves slowly (adiabatically) and returns to the original state. In the present case, because $``$ varies slowly during the motion of the electron along each semi-circular ring, the components of the spin state of each electron in the direction of $``$ remain pinned to this varying direction. However, owing to the rapid change in $`𝐯`$ at the point of entry, the initial directions of $``$ are different for the two states that go around the semi-circular rings from this point and interfere at the point of exit. Hence, only the non-cyclic Berry phase corresponding to a spin state going around a semi-circle, which is then completed to a closed curve by the longitude, may be defined for each semi- circular ring. Berry’s phase is half the solid angle subtended by the curve traced by $``$ on the sphere that represents all possible directions of the $``$ and completed into a closed curve by the geodesic joining the initial and final directions at the center of this sphere. For unpolarised electrons, as in the present experiment, the average of these Berry phase factors may be observed.

Acknowledgments

I thank Stephen L. Adler for discussions and support at the Institute for Advanced Study, Princeton, NJ 08540, where part of this work was done. This work was also supported by a Fulbright Distinguished Scholar award, an ONR and NSF grants.