text:
# Anatomy of nuclear shape transition in the relativistic mean field theory

## I Introduction

Interaction between nucleons in a nucleus may give rise to preferred orientations of the single-particle orbitals leading to deformed intrinsic shapes of the nuclei. With thermal excitations, they undergo a phase transition to spherical shapes. This has been studied in the experiments on the shapes of giant dipole resonances (GDR) built on excited states . The understanding of the mean field shape evolution with temperature has been attempted in a macroscopic approach  generally referred to as the Landau theory of phase transitions. They have also been studied in microscopic framework like finite-temperature non-relativistic Hartree-Fock  and Hartree-Fock-Bogoliubov (HFB) approaches  with the pairing-plus-quadrupole (P$`+`$Q) interaction. The shape transition temperature is found to be in the domain of $`1.0`$ to $`1.8`$ MeV for the rare-earth nuclei. Here the model Hamiltonian is simplistic, the model space is small, an inert core is assumed and moreover, the role of the Coulomb field is taken into consideration in an effective manner. Recently, we have studied  this same phenomenon in the framework of relativistic mean field theory (RMF). Here the model space is sufficiently large, all the nucleons are treated on equal footing and the Coulomb interaction is properly accounted for. It is then found that the shape transition temperature is noticeably higher. Except for some calculations in the s-d shell nuclei , nearly all the calculations have been done for nuclei in the rare-earth region; it is found that the deformation undergoes a sudden collapse at the shape transition temperature. Grossly, one understands the dissolution of the deformation with temperature in these nuclei from the following: shell structure leads to the population of the deformation-driving states, the so-called intruder states producing the static ground state deformation; their depopulation with gradual heating restores the spherical symmetry.

The aim of the present paper is to analyse in more microscopic details the collapse of the deformation with temperature. In doing so, we also explore whether the sudden collapse observed in the rare-earth nuclei is universal or system-specific. The stability towards the deformed ground state for the axially symmetric nuclei that we consider is given by the arrangement of the single-particle orbitals of good projection quantum number; the evolution of the energies of these single-particle orbitals with temperature, particularly those near the Fermi surface and also their occupancy evolution lead to a self-consistent rearrangement of the orbitals and thus can reveal in detail why the deformed nuclei undergo a shape transition.

The non-linear $`\sigma `$coupling term in the effective Lagrangian has been introduced  to reproduce properly the finite size effect, particularly the surface properties of nuclei. Since the spin-orbit coupling term is sensitive to the fall of the density at the nuclear surface, the structure of the Fermi surface is expected to depend on the non-linear term and thus might affect the ground state deformation and its thermal evolution. These aspects are also investigated using a parameter set (HS) where the non-linear $`\sigma `$-coupling term is absent.

A brief discussion of the theoretical framework we employ is given in section II. The results and discussions are presented in section III. The concluding remarks are given in section IV.

## II Formalism

The details of the formalism are given in Ref.. For the sake of completeness, however, we write down the effective Lagrangian density describing the nucleon-meson many body system followed by a very brief discussion. The Lagrangian density is given by

$``$ $`=`$ $`\overline{\mathrm{\Psi }}_i\left(i\gamma ^\mu _\mu M\right)\mathrm{\Psi }_i+{\displaystyle \frac{1}{2}}^\mu \sigma _\mu \sigma U(\sigma )g_\sigma \overline{\mathrm{\Psi }}_i\sigma \mathrm{\Psi }_i`$ (3)
$`{\displaystyle \frac{1}{4}}\mathrm{\Omega }^{\mu \nu }\mathrm{\Omega }_{\mu \nu }+{\displaystyle \frac{1}{2}}m_\omega ^2\omega ^\mu \omega _\mu g_\omega \overline{\mathrm{\Psi }}_i\gamma ^\mu \omega _\mu \mathrm{\Psi }_i{\displaystyle \frac{1}{4}}\stackrel{}{R}^{\mu \nu }\stackrel{}{R}_{\mu \nu }+{\displaystyle \frac{1}{2}}m_\rho ^2\stackrel{}{\rho }^\mu \stackrel{}{\rho }_\mu `$
$`g_\rho \overline{\mathrm{\Psi }}_i\gamma ^\mu \stackrel{}{\rho }_\mu \stackrel{}{\tau }\mathrm{\Psi }_i{\displaystyle \frac{1}{4}}F^{\mu \nu }F_{\mu \nu }e\overline{\mathrm{\Psi }}_i\gamma ^\mu {\displaystyle \frac{(1\tau _3)}{2}}A_\mu \mathrm{\Psi }_i.`$
The mesons included in the description are scalar-isoscalar $`\sigma `$, vector-isoscalar $`\omega `$ and vector-isovector $`\rho `$ mesons. The arrows in Eq.(3) indicate isovector quantities. The scalar self-interaction term $`U(\sigma )`$ of the $`\sigma `$ meson is taken to be non-linear

$$U(\sigma )=\frac{1}{2}m_\sigma ^2\sigma ^2+\frac{1}{3}g_2\sigma ^3+\frac{1}{4}g_3\sigma ^4.$$
(4)
The nucleon mass is $`M`$; $`m_\sigma `$, $`m_\omega `$ and $`m_\rho `$ are the meson masses, $`g_\sigma `$, $`g_\omega `$ and $`g_\rho `$ are the coupling constants for the mesons and $`e^2/4\pi =1/137`$ is the fine structure constant. The field tensors for $`\omega `$ and $`\rho `$ are given by $`\mathrm{\Omega }^{\mu \nu }`$ and $`\stackrel{}{R}_{\mu \nu }`$; for the electromagnetic field, it is $`F^{\mu \nu }`$. Recourse to the variational principle followed by the mean field approximation treating the field as $`c`$numbers results in the Dirac equation for the nucleon and Klein-Gordon type equations for the mesons and the photon. For the static case, along with the time-reversal invariance and charge conservation, the equations get simplified. The resulting equations, known as the relativistic Hartree equations or RMF equations alongwith the BCS approximation for inclusion of pairing are solved to yield the fields and the single-particle energies.

The self-consistent solutions are obtained using the basis expansion method ; this yields the quadrupole deformation $`\beta _2`$ and also the single-particle states as a function of temperature.

## III Results and Discussions

For the values of the coupling constants and the masses of the mesons and the nucleons occuring in the Lagrangian density given by Eq. (3), we choose the NL3 parameter set. This parameter set reproduces the ground state properties of finite nuclei very well; it yields also the compressional properties satisfactorily . The single-particle states are calculated using spherical oscillator basis with twelve shells. The values of the chemical potential and the pairing gap at a given temperature are determined using all the single-particle states upto $`2\mathrm{}\omega _0`$ above the Fermi surface without assuming any core. In order to check the convergence of the calculation, we have enlarged the basis space from twelve to twenty shells and have extended the model space to include single-particle states upto $`3\mathrm{}\omega _0`$ above the Fermi surface. For this extended model space, the pairing strength is adjusted to reproduce the ground state pairing gap. The change in the values of the observables are found to be insignificant due to this extension of the basis and the model space even at the highest temperature we consider. Continuum corrections are neglected as their effects are found to be negligible  in the temperature domain of relevance (less than $`3.0`$ MeV); the shape transition temperatures for the systems considered are within this range.

In the rare-earth region, we have studied the thermal evolution of the shapes of even-even isotopes of $`Sm`$, $`Gd`$ and $`Dy`$; for neutron number 86 and 88, their quadrupole deformation $`\beta _2`$ as a function of temperature is presented in Fig. 1. The following aspects are apparent from the figure: (i) for the isotopes differing by two neutrons, the difference in the ground state deformation $`\beta _2^0`$ is significant, (ii) addition of two protons does not increase $`\beta _2^0`$ significantly (compare $`\beta _2^0`$ for $`{}_{}{}^{148}Sm`$ and $`{}_{}{}^{150}Gd`$), (iii) there is a close correlation between $`\beta _2^0`$ and the critical tempeature $`T_c`$  and that (iv) $`\beta _2`$ remains nearly constant with temperature and then there is a sudden collapse of the deformation near $`T_c`$ in a temperature window of $`0.2`$ MeV. To elucidate these phenomena more clearly in microscopic terms, we present results for the thermal evolution of the single-particle levels and their occupancies in the next couple of figures for $`{}_{}{}^{148}Sm`$ and $`{}_{}{}^{150}Sm`$. These representative cases guide one to draw inference about the shape evolution of the other nuclei. In Figs. 2-5, the single particle levels near the Fermi surface for the protons and the neutrons in $`{}_{}{}^{148}Sm`$ and $`{}_{}{}^{150}Sm`$ are displayed as a function of temperature. The Fermi energies are shown by the dashed lines; in the range of the temperature concerned, they are nearly constant. The ground state is axially symmetric and the levels are degenerate in $`\pm K`$, $`K`$ being the projection quantum number. The level structures remain practically unaltered upto $`T0.75`$ MeV for $`{}_{}{}^{148}Sm`$ and upto $`1.0`$ MeV for $`{}_{}{}^{150}Sm`$ beyond which the different $`K`$levels pertaining to a definite ($`nlj`$)-orbit start to converge. At the temperature $`T_c`$ (1.15 MeV for $`{}_{}{}^{148}Sm`$ and 1.6 MeV for $`{}_{}{}^{150}Sm`$ ) they become degenerate signifying transition to spherical symmetry. It may be mentioned that in the simplistic (P+Q) model, the phase transition to a spherical shape occurs relatively earlier; in a recent HFB calculation in an extended model space with the realistic Gogny force , it has however been found that the transition temperature is in keeping with that found in our calculations in the RMF framework .

Examination of the single-particle spectra is helpful in understanding why the two neutron addition to $`{}_{}{}^{148}Sm`$ increases the ground state deformation whereas the two proton addition does not alter it significantly. Because of pairing, the occupancies of the states near the Fermi surface is partial for a nucleus in its ground state. From Figs. 3 and 5 one sees that the two neutron addition increases maximally the population of the $`{}_{}{}^{1/2}f_{7/2}^{}`$ state (for the orbitals, we have used the notation $`{}_{}{}^{K}l_{j}^{}`$); the populations of the states $`{}_{}{}^{1/2}h_{9/2}^{}`$ and $`{}_{}{}^{3/2}h_{9/2}^{}`$ are also significantly enhanced. All these orbitals are intrinsically highly prolate which explains the increase in the ground state deformation of $`{}_{}{}^{150}Sm`$. (Because of axially symmetry in the even-even nuclei we study, the projection $`K`$ is a good quantum number and is degenerate with ($`K`$) because of time reversal invariance. The states $`{}_{}{}^{K}l_{j}^{}`$ just mentioned are the ones that have the largest amplitude for the orbital with projection $`K`$). From Figs. 2 and 4 we also note that the deep lying $`{}_{}{}^{7/2}g_{7/2}^{}`$ proton orbital in $`{}_{}{}^{148}Sm`$ which is intrinsically oblate moves up closer to the Fermi surface in $`{}_{}{}^{150}Sm`$ and thus is less populated. This also contributes to the increase in the prolate deformation for $`{}_{}{}^{150}Sm`$. Examination of the single-particle spectra for $`{}_{}{}^{148}Sm`$ and $`{}_{}{}^{150}Gd`$ (not shown here) shows that the addition of two protons does not practially affect the neutron occupancies near the Fermi surface; For protons only the $`{}_{}{}^{3/2}h_{11/2}^{}`$ orbitals get noticeably more populated thus slightly enhancing the deformation in the ground state for the $`{}_{}{}^{150}Gd`$ nucleus compared to $`{}_{}{}^{148}Sm`$ as shown in Fig. 1. The ground state deformation properties of $`Dy`$ isotopes can be explained in a similar fashion.

The suddenness of the transition from a prolate to the spherical shape at the temperature $`T_c`$ can be understood as follows: as the temperature rises, the states above the Fermi surface get increasingly more populated at the expense of the states below. This causes a self-consistent reorganization of the single-particle field because of which the single-particle states evolve with temperature as depicted in Figs. 2-5. With increase in temperature for $`T`$ above $``$ 0.5 MeV, one finds from Fig.6 for the proton orbitals in $`{}_{}{}^{148}Sm`$ a tendency for equalisation of the single-particle occupancies for different $`K`$states emanating from the same $`j`$orbital. Around $`T_c`$, one could readily see the sharp drop in the occupancies of the prolate orbitals with an accompanied enhancement of the same for the oblate orbitals resulting in the rapid collapse of the deformation. The neutron orbitals (not shown here) have also the similar features. All these arguments apply also for the other rare-earth nuclei considered.

To examine whether the sudden collapse of the deformation as observed in the rare-earth nuclei is a generic feature or system-specific, one needs to consider the shape evolution of some other nuclei in a different mass region. For this purpose, we study two isotopes of zinc nuclei, namely $`{}_{}{}^{64}Zn`$ and $`{}_{}{}^{66}Zn`$. As all the features related to shape evolution in these isotopes are found to be very similar, we discuss only the nucleus $`{}_{}{}^{64}Zn`$. In Fig. 7, we display the thermal evolution of the deformation $`\beta _2`$ for this nucleus. To draw a comparison of the shape evolution with the rare-earth systems, we also display in the same figure the temperature dependent deformation for the nucleus $`{}_{}{}^{150}Sm`$. It is seen that the fall-off of the deformation with temperature of $`{}_{}{}^{64}Zn`$ is somewhat slower. This is magnified in Fig.8 where the heat capacity per particle for the two systems $`{}_{}{}^{150}Sm`$ and $`{}_{}{}^{64}Zn`$ are displayed. For each curve, the twin peaks at lower temperature correspond to the neutron and proton pairing transitions. For the ligher nucleus, this transition is relatively more prominent and is at a little higher temperature as expected. The peaks at higher temperatures ($`1.6`$ MeV for $`Sm`$ and $`2.0`$ MeV for $`Zn`$) refer to the shape transition; whereas it is very prominent for the rare-earth system, it is rather weak and looks more like a plateau for the $`{}_{}{}^{64}Zn`$ nucleus signalling a relatively smoother shape transition to the spherical configuration. It is further that though the ground state deformations of these two nuclei are nearly the same, the transition temperature for $`{}_{}{}^{64}Zn`$ is significantly higher. Comparison of the thermal evolution of the level structures of $`{}_{}{}^{64}Zn`$ (shown in Fig.9) with those of $`{}_{}{}^{150}Sm`$ displayed in Figs.4 and 5 may help in understanding the delayed shape transition in $`{}_{}{}^{64}Zn`$. For $`{}_{}{}^{150}Sm`$, in the vicinity of the transition temperature, the single-particle orbitals of opposite intrinsic deformations cross each other near the Fermi surface hastening ite approach towards a spherical configuration. The higher $`T_c`$ in $`{}_{}{}^{64}Zn`$ may be partially attributed to the absence of these level crossings.

It has been mentioned that the non-linear $`\sigma `$coupling term is necessary to explain the surface properties of finite nuclei . Though in the absence of this term, the nuclear matter binding energy and the saturation density are reproduced, the binding energies of finite nuclei can not be obtained properly . The fall-off of the nucleon density profile at the surface is found to be stiffer without the non-linear term. Since the spin-orbit splitting is proportional to the density gradient, this splitting is then likely to be larger without the non-linear $`\sigma `$term. This may affect the single-particle level structure to which the shape evolution is expected to be sensitive. In order to study this effect on the ground state deformation and the thermal shape evolution of nuclei, calculations have been performed with a parameter set that does not contain the non-linear $`\sigma `$coupling term. The HS parameter set  is chosen for this purpose. In Fig. 10, the results for the temperature evolution of deformation $`\beta _2`$ are shown for two representative cases, namely, $`{}_{}{}^{148}Sm`$ and $`{}_{}{}^{150}Sm`$. For comparison, $`\beta _2`$ with the NL3 parameter set for $`{}_{}{}^{150}Sm`$ is also displayed in this figure. It is observed that with the HS set the ground state deformation is larger, the transition temperature smaller and that the collapse of the deformation is somewhat faster. The sharper deformation collapse is corroborated in the thermal evolution of the specific heat with and without the non-linear $`\sigma `$term in the representative case of $`{}_{}{}^{150}Sm`$ as shown in Fig. 11 (upper panel). This is amplified further in the case of $`{}_{}{}^{64}Zn`$ as shown in the bottom panel of the figure. The change in the ground state deformation obtained with the HS parameter set can be understood from the examination of the single-particle spectra near the Fermi surface. For example, as shown in Fig. 12 for the proton single-particle spectra for $`{}_{}{}^{150}Sm`$, the strong prolate deformation-producing $`{}_{}{}^{1/2}h_{11/2}^{}`$ and $`{}_{}{}^{3/2}h_{11/2}^{}`$ orbitals are significantly deeper down the Fermi surface as compared to those displayed in Fig. 4 for the NL3 parameter set. This is mostly responsible for the larger ground state deformation for $`{}_{}{}^{150}Sm`$. The somewhat sharper dissolution of the deformation with the HS parameter set is again traced back to the self-consistent occupancy evolution with temperature leading to the spherical configuration. Comparison of Fig. 12 with Fig. 4 shows that the spin-orbit splitting is significantly larger (typically $`40\%`$) in case of HS parameter set as envisaged earlier.

## IV Conclusions

In this paper, we have attempted to understand in microscopic detail the shape evolutions of deformed nuclei with temperature in the RMF framework. For the rare-earth nuclei we have studied, namely, $`Sm`$, $`Gd`$ and $`Dy`$ with 86 and 88 neutrons, it is seen that the ground state deformation increases with addition of neutrons appreciably whereas it is not that sensitive to proton addition. Similar inference on the sensitivity of the shape transition temperature can be drawn to neutron and proton addition. It has been found that these transition temperatures are noticeably larger compared to those obtained in the schematic model with pairing-plus-quadrupole interaction but agree reasonably well with those calculated  using a realistic force like the Gogny force. From microscopic viewpoint the ground state deformation can be understood in terms of the single-particle level structure near the Fermi surface. The sudden drop of the deformation can also be understood from the temperature-driven fast equalisation of the occupancies of different $`K`$states originating from the same $`j`$orbital near the Fermi surface close to the transition temperature.

We have also investigated the role of the non-linear self-coupling of the $`\sigma `$ mesons on the shape evolution of the nuclei. In absence of the non-linear term, the spin-orbit splitting is enhanced which affects the single-particle level structure near the Fermi surface leading to a sharper shape transition at a lower temperature.

Figure Captions:

* The temperature evolution of the deformation ($`\beta _2`$) for a few rare-earth nuclei with the NL3 parameter set.
* The proton single-particle level spectrum near the Fermi surface for $`{}_{}{}^{148}Sm`$ as a function of temperature with the NL3 parameter set. The dashed line corresponds to the Fermi surface.
* The neutron single-particle level spectrum near the Fermi surface for $`{}_{}{}^{148}Sm`$ as a function of temperature with the NL3 parameter set. The dashed line corresponds to the Fermi surface.
* Same as Fig. 2 for $`{}_{}{}^{150}Sm`$.
* Same as Fig. 3 for $`{}_{}{}^{150}Sm`$.
* The thermal evolution of single-particle occupancy for protons in $`{}_{}{}^{148}Sm`$ for a few levels with good projection quantum number $`K`$ (as indicated) near the Fermi surface. The degeneracy of $`\pm K`$ has been taken into account in the occupancy.
* Comparison of the thermal evolution of deformation $`\beta _2`$ for $`{}_{}{}^{64}Zn`$ (solid line) with $`{}_{}{}^{150}Sm`$ (dotted line).
* The specific heat per particle as a function of temperature for the systems $`{}_{}{}^{150}Sm`$ and $`{}_{}{}^{64}Zn`$.
* The proton (top panel) and neutron (bottom panel) single-particle spectra for $`{}_{}{}^{64}Zn`$ near the Fermi surface as a function of temperature.
* The thermal evolution of deformation for $`{}_{}{}^{148}Sm`$ and $`{}_{}{}^{150}Sm`$ with the HS parameter set. For the sake of comparison, the same for $`{}_{}{}^{150}Sm`$ with the NL3 parameter set is also shown.
* The specific heat per particle as a function of temperature for $`{}_{}{}^{150}Sm`$ with the HS (solid line) and the NL3 (dotted line) parameter sets (top panel). In the bottom panel, the same is shown for $`{}_{}{}^{64}Zn`$.
* The proton single-particle level spectrum near the Fermi surface with the HS parameter set for $`{}_{}{}^{150}Sm`$ as a function of temperature.


format: text

text:
# Fluctuation Magnetoconductance in MgB2

## Abstract

We report fluctuation magnetoconductance in a MgB2 superconductor prepared under a high pressure of 3 GPa. This excess magnetoconductance, $`\mathrm{\Delta }\sigma (H)`$, follows the three-dimensional scaling function for the critical fluctuations proposed by Ullah and Dorsey. This feature is inferred to originate from the isotropic nature of the MgB2 compound.

The recent discovery of superconductivity at about 40 K in MgB2  brought about an avalanche of research. While the type of carrier was found to be hole-like , other properties have been reminiscent of conventional BCS superconductivity, and are significantly different from those found in the cuprate superconductors. These properties include a notable shift in the $`T_c`$ due to the boron isotope, , a stable metallic behavior with a higher carrier density , and prominent bulk pinning.

It is well-known that high-$`T_c`$ superconductors have a two-dimensional layered structure and a very short out-of-plane coherence length, which is quite different from conventional superconductors. Thus, a strong superconducting fluctuation effect around $`T_c`$ is evident for thermodynamic and transport quantities. In the MgB2 system, various superconducting properties, including the electrical conductivity, are believed to be isotropic even though the boron planes are thought to act like the CuO2 planes in the cuprate superoconductors . Thus, it could be very interesting to investigate the conductivity fluctuation effect in this compound.

In this paper, we present the magnetoconductance fluctuation in a MgB2 polycrystal. The scaling functions for the critical fluctuations were employed to analyze the excess conductance of our sample. We found that the conductivity in the critical region scales with the three dimensional scaling functions.

A 12-mm cubic multi-anvil press was used for the high-pressure sintering. The pellet, which was made of a commercially available powder of MgB2, was sintered at about $`900^{}`$C after being subjected to pressures of up to $`3`$ GPa. The zero-field resistivity transition temperature, $`T_c^R(0)`$, is 38.3 K. A transmission electron microscope (TEM) study  showed that all grains were compactly connected and that no discernable empty space or impurities at the boundaries. The weak link behavior is expected to be less than that observed in to the high-Tc superconductors. The details of the sample preparation and the properties of sample can be found elsewhere.

The voltage noise was successfully reduced to a lower level by preparing a very thin and optically clean specimen polished from a strong, dense bulk pellet. The dimensions of the specimen were about $`2.4\times 4.0\times 0.1`$ mm3. The standard photolithography technique was used to make electrical leads on the specimen. To obtain good ohmic contacts between the Au pads and the sample, we cleaned the surface using an ion beam before depositing Au-contact pads. The magnetic field was applied perpendicular to the sample surface and the current direction. The resistivity measurements were carried out in a cryostat with a superconducting magnet by using the standard 4-probe technique. A dc current source (model Keithley 220), two channel nanovoltmeters (model HP 34420A), and dc preamplifier (model EM electronics N11) with $`J=4050`$ A/cm2 were used.

Figure 1 shows the temperature dependence of the resistance for applied magnetic fields of 0 T $`H`$ 5 T. The gradual change in the resistance near the transition temperature is similar to the case of typical metallic superconductors. The resistance just above $`T_c`$ did not change with the applied field. It is clearly seen that the resistivity curves shift toward lower temperature as the field increases. The rate of decrease of $`T_c(H)`$ with respect to the field is significantly larger than that of the cuprates. The transition temperature $`T_c(H)`$ was estimated from the 90% drop of the normal-state resistivity, and the slope $`(dH_{c2}/dT)|_{T_c}`$ was found to be about -0.54 T/K. This value of the slope is much smaller than the $`dH_{c2}/dT`$ of $`2`$ T/K observed in high-temperature superconductors such as YBa2Cu3O7 and Bi2Sr2CaCu2O8. Using this slope, the estimated $`H_{c2}(0)`$ was found to be 13.9 T through the relationship $`H_{c2}(0)0.7T_c(dH_{c2}/dT)_{T_c}`$ this value is about ten times smaller than the value for cuprate superconductors. The coherence length $`\xi (0)=[\varphi _0/2\pi H_{c2}(0)]^{1/2}`$ was calculated to be 48.6 Å, where $`\varphi _0`$ is the flux quantum.

In the strong-field region, since the quasi-particles are mainly confined to their lowest Landau level,  an effective reduction of the dimensionality occurs, hence the fluctuation-induced conductance exhibits a critical behavior. Critical phenomena and scaling properties of the thermodynamic quantities near the transition temperature in a mixed state have been studied by a number of groups.  Ullah and Dorsey proposed scaling functions for various thermodynamic and transport quantities within the Hartree approximation. The quartic term $`|\psi |^4`$ in the Ginzburg-Landau free energy was included which was in contrast to the free fluctuation theory where the quartic term is neglected. The scaling functions for the excess conductance are given by

$$\mathrm{\Delta }\sigma (H)_{2D}=\left[\frac{T}{H}\right]^{1/2}F_{2D}\left[A\frac{TT_c(H)}{(TH)^{1/2}}\right]\text{for 2D,}$$
(1)
$$\mathrm{\Delta }\sigma (H)_{3D}=\left[\frac{T^2}{H}\right]^{1/3}F_{3D}\left[B\frac{TT_c(H)}{(TH)^{2/3}}\right]\text{for 3D,}$$
(2)
where $`F_{2D}`$ and $`F_{3D}`$ are unspecified scaling functions, and $`A`$ and $`B`$ are field and temperature-independent coefficients. In these equations, the Aslamazov-Larkin(AL) term  of the fluctuation conductance was taken into account.

To obtain the excess conductance $`\mathrm{\Delta }\sigma (H)`$, we substracted the extrapolated normal conductance from the total conductance by using a normal fit at temperatures far above $`T_c(H)`$ for each magnetic field. The correct determination of the $`T_c(H)`$ is critical for obtaining the best scaling behavior. For $`T_c(H)`$, we used the refined temperature around the 10% resistive superconducting transition point for each field. The excess conductance scaled excellently with the 3D form. Figure 2(a) shows $`\mathrm{\Delta }(1/R)/(T^2/H)^{1/3}`$ versus the scaling parameter $`(TT_c(H))/(TH)^{2/3}`$. All the data for the various fields collapse into a single curve while the 2D scaling plot gives a poor result, as shown in Fig. 2(b), for whatever value of $`T_c(H)`$. The values of $`T_c(H)`$ for the best fits were 34.9, 32.8, 31.0, 28.8, and 27.2 K for H = 1, 2, 3, 4, and 5 T, respectively, which slightly deviated from linearity in H but agreed with the generalized prediction by Maki.

It is quite surprising to find 3D scaling behavior in a polycrystalline sample. A compactly connected morphology with no discernable empty space was observed using a TEM, thus, the weakly linked grain boundary effect is negligible. The high degree of iosotropy is another feature for this 3D scaling behavior. The spreadout of the scaled conductance at low temperatures, indicated by the arrow in Fig. 2(a), is not unusual for the scaling behavior in the fluctuation conductivity. Several results obtained from high-$`T_c`$ superconductors , as well as $`R`$Ni2B2C materials  have commonly given the same broadening due to the vortex motion at the tail of the transition line .

In summary, we observed magnetoconductance fluctuations in MgB2. With critical fluctuations includede, the scaling behavior of MgB2 was better explained by the 3D theory rather than by the 2D theory. Even though the grains in the sample are randomly oriented, the excess conductance follows the 3D scaling function for critical fluctuations. This feature may indicate that MgB2 is nearly isotropic. However, more rigorous studies of the suggested 3D nature of MgB2 require at least a grain-aligned sample such as a $`c`$-axis oriented film or a single crystal.

This work is supported by the Ministry of Science and Technology of Korea through the Creative Research Initiative Program.


text:
# Fractal Geometry of Normal Phase Clusters and Magnetic Flux Trapping in High-Tc Superconductors

## Abstract

The effect of geometry and morphology of superconducting structure on magnetic flux trapping is considered. It is found that the clusters of normal phase, which act as pinning centers, have significant fractal properties. The fractal dimension of the boundary of these clusters is estimated using a simple area-perimeter relation. A superconductor is treated as a percolation system. It is revealed that the fractality intensifies the magnetic flux trapping and thereby enhances the critical current value.

One of the important properties of the clusters of a normal phase in superconductors consists in their capability to act as pinning centers of high efficiency -. When these clusters are out of contact with one another they can validly trap a magnetic flux, so that the vortices are held from moving under the action of the Lorentz force. It is the geometric and morphological properties of such clusters as well as their effect on the magnetic flux dynamics that will interest us. Let us consider a superconductor containing inclusions of a normal phase of columnar shape. When such a superconducting structure is cooled below the critical temperature in the magnetic field along the direction of the longest size of those inclusions, the distribution of the trapped magnetic flux will be two-dimensional. As an example we can consider the superconducting films where the normal phase inclusions were created during the growth process at the sites of defects on the boundary with the substrate -. Let us suppose that the film surface fraction covered by the normal phase is below the percolation threshold for the transfer of magnetic flux (50% in the case of 2D-percolation ). At the same time, the relative portion of superconducting phase exceeds the percolation threshold, so that the transport current can flow through the superconducting percolation cluster. Such a structure provides for effective pinning and thereby raises the critical current, because the magnetic flux is trapped in the finite normal phase clusters. When the transport current is rising, the trapped magnetic flux will be changed, for the vortices will break away from the clusters of pinning force weaker than the Lorentz force created by the current. Since the infinite superconducting cluster is formed in the film, the vortices must cross a region occupied by the superconducting phase when they are coming out from the pinning centers.

In the subsequent examination it must be taken into account that high-Tc superconductors (HTSC) are characterized by an extremely short coherence length, so weak links form readily in these materials. Various structural defects as grain boundaries, crystallites, and especially twins, which would simply cause some additional scattering at long coherence length, give rise to the weak links over a wide range of scales in HTSC , , . Moreover, the presence of a magnetic field is favorable to the formation of weak links, because its action further reduces a coherence length . Thus around each normal phase cluster there are always weak links through which the vortices may pass under the action of the Lorentz force. The larger the cluster size, the more such weak sites are along its border with the surrounding superconducting space, and therefore, the smaller is the critical current at which the magnetic flux breaks away from a given pinning center. It appears that each normal phase cluster has its own value of the critical current, which make the contribution to the total statistical distribution. On the basis of these geometric arguments, let us suppose that this critical current $`I`$ is inversely proportional to the perimeter $`P`$ of the normal phase cluster: $`I1/P`$ , because the larger the perimeter is, the higher is the probability to get a weak link there. At this point we shall assume that the weak links concentration per unit perimeter length is constant for all clusters and that all the clusters of equal area have the same pinning force.

On the other hand, when a transport current is slowly increased, magnetic flux will break away first from the clusters of small pinning force, of small critical current, and therefore, of large size. Thus the decrease in the trapped magnetic flux $`\mathrm{\Delta }\mathrm{\Phi }`$ caused by a transport current is proportional to the number of all the normal phase clusters of critical currents less than a preset value. Taking into account that the magnetic flux trapped into a single cluster is proportional to its area $`A`$, the relative decrease in the total trapped flux can be expressed with the accumulated probability function $`F=F(A)`$ for the distribution of the areas of the normal phase clusters, which is a measure of the number of the clusters of area smaller than a given value of $`A`$:

$$\frac{\mathrm{\Delta }\mathrm{\Phi }}{\mathrm{\Phi }}=1F(A)\text{ ,         where }F(A)=𝖯\{A_j<A\}$$
(1)
Here $`𝖯`$ is the probability that any $`j`$th cluster has the area $`A_j`$ less than a given value $`A`$.

Thus, in order to clear up how the transport current acts on the trapped magnetic flux, it is necessary to find out the relationship between the perimeter of the normal phase clusters and the distribution of their areas. To analyze the geometric probability characteristics of normal phase clusters an electron photomicrograph of YBCO film, which was similar to that published earlier in Ref. , has been studied. The region of a total area of 200 $`\mu `$m2 containing 528 clusters has been scanned. The areas and perimeters of the clusters have been measured by covering their digitized pictures with a rectangular grid of resolution cell $`60\times 60`$nm2. The results of the statistical treatment of those data are presented in the Table I. The normal phase occupies 20% of the total area only, so the percolation superconducting cluster is dense enough. A high skewness (1.76) as well as the statistically insignificant (5%) difference between the sample mean and the standard deviation allow us to conclude that there is an exponential distribution for areas of the normal phase clusters which has such an accumulated probability function

$$F(A)=1\mathrm{exp}\left(\frac{A}{\overline{A}}\right)$$
(2)
where $`\overline{A}`$ is the mean area of the cluster.

Furthermore, it might be natural to believe that the perimeter-area relation for the normal phase clusters obeys the well known geometric formula: $`P\sqrt{A}`$. However, it would be a very rough approximation only, because this relationship holds for Euclidean geometric objects but on no account for the fractals. It is just the fractal nature of the normal phase clusters that is of fundamental importance here. For fractal geometric objects perimeter-area relation must be re-written in a different way :

$$PA^{\frac{D}{2}}$$
(3)
where $`D`$ is the fractal dimension of the perimeter. This is consistent with the generalized Euclid theorem , which states that, for similar geometric objects, the ratios of corresponding measures are equal when reduced to the same dimension. Hence it follows that $`P^{1/D}A^{1/2}`$, which is applicable both to fractal ($`D>1`$) and Euclidean ($`D=1`$) figures.

The perimeter-area relation for the normal phase clusters is shown in Fig. 1. Although all 528 points mentioned above are plotted on the graph, certain of them coincide for the finite resolution of the picture digitization. This feature is noticeable, primarily, for small clusters: some points at the lower left of Fig. 1 are arranged discretely with the spacing equal to the limit of resolution (60 nm). Fig. 1 demonstrates such an important peculiarity: perimeter-area relation obeys the scaling law of Eq. (3). There are no apparent crossovers or breaks on this graph over the range of more than two orders of magnitude in area. These data apply to the clusters of different shape, nevertheless all the points fall on a straight line in logarithmic scale. Thus, the fractal dimension $`D`$ of the cluster boundary can be found from the slope of the regression line of the form of Eq. (3); a least squares treatment of the perimeter-area data gives the estimate of $`D=1.44\pm 0.02`$ with correlation coefficient 0.93. The scaling perimeter-area behavior implies an absence of any characteristic length scale between 0.1 $`\mu `$m and 10 $`\mu `$m in the linear size of the normal phase cluster. Hence these clusters have all the properties of stochastic fractals .

The problem on the fractal cluster perimeter is quite similar to the one on the fractal boundary of clouds in atmosphere , . The main distinction is that instead of the projection of a cloud on the Earth’s surface we are considering the cross-section of the extended columnar object by the plane carrying a transport current. Therefore, though a normal phase cluster, as well as a cloud, represents a self-affine fractal , it is possible to consider its geometric probability properties in the planar section only, where the boundary of the cluster is statistically self-similar.

Next, using relation of Eq. (3) between the fractal perimeter and the area of the cluster, for critical current we get: $`I=\alpha A^{D/2}`$, where $`\alpha `$ is the form factor. In accordance with starting formula (1), the exponential distribution of cluster area of Eq. (2) gives rise to an exponential-hyperbolic distribution of critical currents:

$$\frac{\mathrm{\Delta }\mathrm{\Phi }}{\mathrm{\Phi }}=\mathrm{exp}\left[\left(\frac{2+D}{2}\right)^{\frac{2}{D}+1}i^{\frac{2}{D}}\right]$$
(4)
where $`iI/I_c`$ , and $`I_c=\left(2/\left(2+D\right)\right)^{\left(2+D\right)/2}\alpha \left(\overline{A}\right)^{D/2}`$ is the critical current of the resistive transition.

Thus, the entire distribution of critical currents determined by the geometric probability properties of the normal phase clusters can be found with the aid of Eq. (4) from the changes in the trapped magnetic flux caused by transport currents of different amplitude. The effect of the transport current on the trapped flux is illustrated in Fig. 2. The critical current distribution of Eq. (4) for fractal dimension $`D=1.44`$ is drawn there by the line (a).

In order to get the relationship between the dynamics of the trapped magnetic flux and the geometric morphological properties of the superconducting structure the empirical distribution function $`F^{}=F^{}\left(A\right)`$ for the sampling of the areas of normal phase clusters has been computed (step line in Fig. 2). This function gives a statistical estimate of the accumulated probability function $`F=F\left(A\right)`$. The value $`F^{}\left(A\right)`$ was calculated for each order statistic as the relative number of clusters of area smaller than a given value $`A`$. A co-ordinate transformation of the form

$`\left\{F^{}1F^{}\text{ , }A\left({\displaystyle \frac{2+D}{2}}\right)^{\frac{2+D}{2}}\left({\displaystyle \frac{\overline{A}}{A}}\right)^{\frac{D}{2}}\right\}`$

allows us to get an empirical function of distribution of the normal phase clusters in their critical currents, which is a statistical analog of the distribution function of Eq. (4). This distribution reflects the morphological properties of the superconducting structure of the specimen, and as it is seen from the Fig. 2, both distributions coincide well (the thick line (a) and the step one on the main chart).

Furthermore, Fig. 2 shows that currents of amplitude less than $`i_{\mathrm{min}}=0.77`$ have no action upon the trapped flux because there are no pinning centers of such small critical currents in the specimen. Since the pinning force is smaller for larger clusters, the constancy of the trapped flux in this range of currents is attributed to the absence of such normal phase clusters that have the perimeter greater than a certain threshold value. The magnitude of the corresponding critical current can be obtained from the formula

$`i_{\mathrm{min}}=\left({\displaystyle \frac{2+D}{2}}\right)^{\frac{2+D}{2}}\left({\displaystyle \frac{\overline{A}}{A_{\mathrm{max}}}}\right)^{\frac{D}{2}}`$

where $`A_{\mathrm{max}}`$ is the area of the largest cluster in the sampling (see “Max value” in the Table I).

It is important to note that the specimen may remain superconducting under the action of pulsed current of amplitude even greater than the critical current of resistive transition ($`i=1`$), because the thermo-magnetic instability, which would be inevitable when a constant current of the same amplitude flowed through the specimen, does not manage to develop during a short-lived disturbance.

The inset on Fig. 2 shows how the fractal dimension affects the trapping of the magnetic flux. The curve of $`D=1`$ (line (b)) relates to usual Euclidean clusters; the curve of $`D=2`$ (line (c)) applies to the case of the greatest possible fractal dimension for curves in a plane (as an example, the plane-filling Hilbert curve of infinite order has such a fractal dimension). Whatever the geometric morphological properties of the normal phase clusters may be, the graph for their transport current dependence of the trapped magnetic flux will fall within the region bounded by those two limiting curves (like line (a)). The practically important conclusion follows from Fig. 2: fractality of the normal phase clusters strengthens the trapping of the flux, thus hindering the vortices to break away from the pinning centers, thereby the current-carrying capability of superconductor with such fractal clusters is enhanced. Actually, the transport current of a magnitude $`i=2`$ causes the 43% of the total trapped flux to break away from the usual Euclidean clusters ($`D=1`$ , line (b)), whereas this value is equal only to 13% for the normal phase clusters of a maximal fractality ($`D=2`$ , line (c)) what is equivalent that the pinning is three times greater in the latter case.

Thus, in the present work the fractal nature of the normal phase clusters is found and its effect on the magnetic flux trapping in superconductors is revealed. The fractal dimension of the cluster perimeter is estimated. It is shown that the fractality contributes to the trapping of the magnetic flux that can cause the critical current to increase.


text:
# Non-exponential decays and nonextensivity

## Abstract

We demonstrate that non-exponential decays of unstable systems can be understood as yet another example of nonextensivity encountered in many physical systems and as such can be characterized by the nonextensivity parameter $`q`$.

PACS numbers: 05.40.Fb 24.60.-k 05.10.Gg
Keywords: Nonextensive statistics, Lévy distributions, Thermal models

It is known that for the unstable system, for which the probability $`\gamma `$ to decay in a unit of time is constant, its survival time probability is given by simple exponential law

$$P(t)=\mathrm{exp}(\gamma t).$$
(1)
This means that our system is not really aging but with passing time shows its persistency to decay. On the other hand, it is also widely known  that spontaneous decays of quantum-mechanical unstable systems cannot be described by the pure exponential law (neither for short nor for long times), i.e., one observes that for them $`P(t)>\mathrm{exp}(\gamma t)`$ and, in practice, $`P(t)`$ exhibits the power-like behaviour of the type 111The ability to observe such nonexponential decays  and interest in quantum version of the Zeno paradox  resulted in the increase of interest in the problem of unstable quantum systems.

$$P(t)t^\delta .$$
(2)
We would like to concentrate in this letter on the observation that there is enormous variety of different physical phenomena which do exhibit a power-like behaviour instead of naively expected exponential one. They can be described in a most economical and adequate way in terms of Tsallis nonextensive statistics  by introducing only one new parameter $`q`$, known as the nonextensivity parameter. The common feature of these phenomena is that they are characterized either by long-range interactions and/or long-range microscopic memories or by space-time (and/or phase-space) (multi)fractal structure of the underlying physical process , or by intrinsic fluctuations of some parameters present in the system under consideration 222This last point, which we shall explore here, is receiving growing attention recently .. In this approach one parameter power-like formula replaces the usual exponential (Boltzmann-Gibbs) one333We would like to stress at this point the fact that eq. (3) is the exact solution of a simple nonlinear ordinary differential equation of the type: $`\frac{dy}{dt}=\frac{y^q}{\tau }`$ with $`y(t)=\frac{L(t)}{L(0)}`$, as discussed in detail in cf. .:

$$L_q(t)=\frac{2q}{\tau }\left[\mathrm{\hspace{0.17em}1}(1q)\frac{t}{\tau }\right]^{\frac{1}{1q}}\stackrel{q1}{}L_{q=1}(t)=\frac{1}{\tau }\mathrm{exp}\left[\frac{t}{\tau }\right].$$
(3)
The question we would like to address is whether non-exponentiality of decays mentioned above can be expressed in the same approach, by deviation of the suitably defined parametr $`q`$ from unity.

In  we have demonstrated that parameter $`q`$ (and power-like distribution it characterizes) occurs whenever parameter $`1/\tau `$ of the original exponential distribution fluctuates according to gamma distribution. In this case $`q`$ is given by the relative variance of such fluctuations. We shall demonstrate now, using random matrix approach  that, indeed, the non-exponential decays can emerge in a natural way from the possible fluctuations of parameter $`\gamma =1/\tau `$ in exponential distribution (1). To this end let us start with discussion of some consequences of quantum chaos, which emerge from applying random matrix hamiltonians, elements of which follow some random probability distribution . Namely, let us consider situation where we have $`N`$ intercoupled states with couplings between them described by hamiltonian given in terms of $`N\times N`$ hermitian (and rotatiotionally and time reversal invariant) matrix (with real matrix elements): $`H=\left[H_{ij}\right]_{N\times N}`$, $`(H_{ij}=H_{ji})`$. Suppose that one is interested in ensemble of such random matrices with $`P(H)`$ being a probability of a given matrix $`H`$. There is a number of propositions how to define $`P(H)`$ correspoding to different models of randomness of matrix elements used . However, in the limit of large matrices (large $`N`$) which are hermitian and real, all of them lead to results analogous to those obtained by assuming gaussian ensemble444The gaussian ensembles were first discussed by E.P.Wigner . For analysis of the gaussian ensemble considered here see .. This can be seen as follows. Let $`P(H)`$ be such that: $`(i)`$ \- elements $`H_{ij}`$ are uncorrelated, i.e.,

$$P(H)=\underset{i=1}{\overset{N}{}}\underset{j1}{\overset{N}{}}P(H_{ij}),$$
(4)
$`(ii)`$ \- distribution (4) is invariant in respect to arbitrary unitary transformation of the basic states (because initial basic states $`|i>`$ used to define $`H_{ij}`$ have been chosen in arbitrary way). Let us now look for distribution $`P(C_i)`$ of the amplitudes $`C_i`$ for eigenvectors of $`H`$ assuming that our hermitean ensemble is invariant in respect to the orthogonal change of the basic vectors. Such ensemble is distributed in the probability space with some density $`P(C_1,\mathrm{},C_N)`$ with $`C_1^2+C_2^2+C_3^2+\mathrm{}+C_N^2=\mathrm{\hspace{0.17em}1}`$ and joint distribution function for $`N`$ amplitudes has the form

$$P(C_1,\mathrm{},C_N)=\frac{2}{\mathrm{\Omega }_N}\delta \left(1\underset{i=1}{\overset{N}{}}C_i^2\right)$$
(5)
(where normalization constant $`\mathrm{\Omega }_N`$ is equal to the volume of $`N`$-dimensional sphere of unit radius and factor $`2`$ originates from the fact that both positive and negative $`C_i`$ enter $`P(C_1,\mathrm{},C_N)`$). Integrating (5) over all but one coordinates $`C_i`$ gives the following distribution $`P(C_i)`$ of amplitude $`C_i`$

$$P(C_i)=\frac{\mathrm{\Omega }_{N1}}{\mathrm{\Omega }_N}\left(1C_i^2\right)^{\frac{N3}{2}}=\frac{\mathrm{\Gamma }\left(\frac{N+2}{2}\right)}{\sqrt{\pi }\mathrm{\Gamma }\left(\frac{N+1}{2}\right)}\left(1C_i^2\right)^{\frac{N3}{2}},$$
(6)
which in the limit of large $`N`$ has the following form 555By using Stirling formula for ($`N>>1`$) leading to $`\mathrm{ln}P(C_i)\frac{1}{2}\mathrm{ln}\frac{N}{2\pi }+\frac{N}{2}\mathrm{ln}\left(1C_i^2\right)`$, and noticing that for large $`N`$ we have $`C_i^2<<1`$.

$$P(C_i)=\sqrt{\frac{N}{2\pi }}\mathrm{exp}\left(\frac{N}{2}C_i^2\right)=\frac{1}{\sqrt{2\pi C_i^2}}\mathrm{exp}\left(\frac{C_i^2}{2C_i^2}\right),$$
(7)
where

$$C_i^2=\frac{1}{N}\mathrm{and}\frac{\left(C_i^2\right)^2C_i^2^2}{C_i^2^2}=\mathrm{\hspace{0.17em}2}.$$
(8)
However, for our purpose we are really interested in decay width $`\gamma _i`$, which is proportional to the probability $`C_i^2`$ of finding single component $`|i>`$ in the composite state. Its distribution is given by

$$P(\gamma _i)d\gamma _i=\mathrm{\hspace{0.17em}2}P(C_i)|dC_i|,$$
(9)
where factor $`2`$ reflects the fact that both positive and negative values of $`C_i`$ contribute to the same value of $`\gamma _i`$. Because $`|dC_i|=\left|\frac{dC_i}{d\gamma _i}\right|d\gamma _i`$ one gets following distribution of such widths:

$$P(\gamma _i)d\gamma _i=\mathrm{\hspace{0.17em}2}P(C_i)\left|\frac{d\gamma _i}{d\gamma _i/dC_i}\right|=\frac{1}{\sqrt{2\pi \gamma _i<\gamma _i>}}\mathrm{exp}\left(\frac{\gamma _i}{2<\gamma _i>}\right)d\gamma _i$$
(10)
characteristic function of which is $`\varphi (z)=(1i\mathrm{\hspace{0.17em}2}<\gamma _i>z)^{1/2}`$. In the case where contribution to the width $`\gamma `$ comes from many channels, distribution we are looking for is obtained by summing all contributions from the particular channels of widths $`\gamma _i`$. For $`\nu `$ different independent channels with the same mean values $`\gamma _0=<\gamma _i>`$ the corresponding characteristic function will be $`\varphi _\nu (z)=(1i\mathrm{\hspace{0.17em}2}\gamma _0z)^{\nu /2}`$ (with $`<\gamma >=\nu \gamma _0`$), i.e., the corresponding distribution function will be gamma function of the form

$$P_\nu (\gamma )d\gamma =\frac{1}{\mathrm{\Gamma }\left(\frac{\nu }{2}\right)}\left(\frac{\nu }{2<\gamma >}\right)\left(\frac{\nu \gamma }{2<\gamma >}\right)^{\frac{\nu }{2}1}\mathrm{exp}\left(\frac{\nu \gamma }{2<\gamma >}\right).$$
(11)
This completes our proof that, as a results of composition of contributions from the $`\nu `$ channels, we obtain distribution of the widths of the decays $`P_\nu (\gamma )`$ in the form of gamma distribution, fluctuations of which are characterized by the relative variance of the form

$$\frac{(\gamma <\gamma >)^2}{<\gamma >^2}=\frac{2}{\nu }$$
(12)
and they decrease with growing $`\nu `$ 666The (11) is for the integer values of $`\nu `$ encoutered here identical to the $`\chi ^2`$ distribution obtained in ..

We have therefore demonstrated that, indeed (at least in the above example), the fluctuations of the life times $`\tau =1/\gamma `$ around mean value $`\tau _0=1/<\gamma >`$ are described by gamma distribution of the form (11) of the variable $`1/\tau `$. According to our philosophy such fluctuations of parameter $`\gamma `$ in the exponential distribution (1) lead therefore directly to the Lévy distribution of the form

$$L_q(t,\tau _0)=_0^{\mathrm{}}d\left(\frac{t}{\tau }\right)P_\nu \left(\frac{t}{\tau }\right)\mathrm{exp}\left(\frac{t}{\tau }\right)=\frac{2q}{\tau _0}\left[1(1q)\frac{t}{\tau _0}\right]^{\frac{1}{1q}}$$
(13)
with nonextensivity parameter $`q`$ equal to $`q=1+\frac{2}{\nu }`$.

We shall close with some remarks on chaotic systems and mixing of configurations. Notice first that distribution $`P_\nu (\gamma )d\gamma `$ is known for $`\nu =1`$ in the nuclear physics as the so called Porter-Thomas distribution  777Deviations from this distribution, which can be attributed to small $`N`$ involved, have been discussed recently in . and describes in a satisfactory way the widths of resonances observed experimentally . On the other hand the many channel case of $`\nu >2`$ corresponds, for example, to the case of total widths for gamma emision or for overbarrier fission. Model using random matrices corresponds to the extreme case of total mixing between allowed degrees of freedom. Such mixing of configurations is realized in the case of compound nucleus (where energy of excitation is divided among many degrees of freedom). It means that component representing one-particle motion in reference to the whole nucleus is decomposed into wave function of a large number of different resonance states. In the Fermi gas model the compound nucleus corresponds to a particularly strong mixing of different configurations, both corresponding to the stationary and to the resonance states. Such emergence of the mixing of configurations, which is leading to the compound nucleus, can be understood as effect of an increase of importance (paralel to the increase of the excitation energy of the system) of small perturbations in the one-particle motion. It happens because in this case the number of exciting particles increases (as increases the number of possible interactions) and excitation energy per single particle increases as well (the density of final states accessible in the collisions increases) 888In this respect there is a whole list of problems which could possibly be considered, for example, the problem of mixed states in the quantum physics, connection with the composite biochemical systems for which fluorescence time distributions are known to be non-exponential (and are usually described by a composition of a number of exponents)..

One should stress also that random matrix approach is applied in the chaotic quantum systems  and it seems to be the characteristic feature of such quantum systems, which in the classical limit show chaotic behaviour. It is connected with the fact that in such systems there is no symmetry, i.e., there is no degeneracy and no selection rules which would exclude interactions of some particular states 999For application of random matrices to description of chaos in quantum systems see .

We are grateful for fruitful discussions with Prof. C. Tsallis. The partial support of Polish Committee for Scientific Research (grants 2P03B 011 18 and 621/E-78/SPUB/CERN/P-03/DZ4/99) is acknowledged.


text:
# Magnetic Field Effects on the Far-Infrared Absorption in Mn12-acetate

## I Introduction

Molecular magnet materials have attracted a great deal of interest in recent years, exhibiting fascinating properties such as cooperative phenomena, magnetic memory, quantum tunneling, and unusual relaxation behavior that are most commonly associated with mesoscopic solids. One prototype single molecule magnet is \[Mn12O12(CH3COO)16(H2O)4\]$``$2CH3COOH$``$ 4H2O, denoted Mn12. It consists of eight Mn3+ ($`S=2`$) and four Mn4+ ($`S=3/2`$) ions, held together by oxygen atoms, acetate ligands, and waters of crystallization; the ferrimagnetic spin arrangement yields $`S`$=10 . Mn12 crystallizes in a tetragonal lattice, with weak exchange coupling and no long range magnetic ordering . Though a number of efforts have been made to understand the energetics of the Mn12 system, a quantitative theory is still lacking. Recent prospective Hamiltonians include anisotropy, Zeeman splitting, spin-phonon interaction, and transverse terms, as well as spin operators up to fourth order .

Mn12 initially attracted attention due to the striking steps and hysteresis loop in the magnetization, indicative of quantum tunneling. At present, these steps are thought to result from the double well potential that separates spin states; magnetization reorientation transitions have optimal probability when the “spin up” and “spin down” levels of the different magnetic quantum numbers align with applied magnetic field . High field EPR, neutron scattering, and sub-mm  techniques have been used to measure the excitation energies between levels in these magnetic clusters. The highest energy excitation (ms=10 $``$ ms=9) occurs in the very far infrared, near 10 cm-1 (300 GHz). That the magnetic dipole transition energies in the Mn12 system are irregular (especially near the top of the anisotropy barrier) clearly shows the presence of higher than second order terms in the spin Hamiltonian. Early heat capacity measurements revealed the irreversible/reversible effects between the two wells below/above the blocking temperature. The exact value of the blocking temperature, $`T_b`$ ($``$ 3 K), depends on the probe, due to the dynamic nature of the blocking process. Above 3 K, the magnetization relaxation is exponential in time and reversible; this is the thermally activated regime. Notable deviations from exponential relaxation are observed below 2 K .

Despite an explosion of interest in the low-energy quantum behavior, little is known about the vibrational characteristics of Mn12 and many other prototypical molecular magnet materials. Spin-phonon coupled modes have been investigated in other transition metal oxides such as EuO, LaMnO3, $`\alpha `$-NaV2O5, and CuO; the frequencies at which they appear correspond to vibrational modulation of the superexchange integral in the materials , rather than the aforementioned low-energy, phonon-assisted relaxation processes. In order to provide further information on the electrodynamic response of single molecule molecular magnets, we have measured the far-infrared spectra of Mn12 as a function of both temperature and applied magnetic field in the thermally activated regime. We use this data to assess spin-phonon coupling in this material.

## II Experimental

High quality single crystals of Mn12 were synthesized following the original procedure described by Lis. The single crystals of Mn12 were ground with paraffin at 77 K to prepare pellets of various concentrations suitable for transmittance measurements in the far infrared . A sample with $``$3.5% of Mn12 by mass proved to be optimal for most of the frequency range under investigation. A more concentrated pellet ($``$85%) was used for measurements between 30 and 110 cm-1.

Infrared transmission measurements were performed in our laboratory and at the National High Magnetic Field Laboratory (NHMFL) in Tallahassee, Florida, using a Bruker 113V Fourier transform infrared spectrometer. Spectra were taken using the 3.5, 12, 23, and 50 $`\mu `$m mylar beam splitters, covering a frequency range of 25–650 cm-1. Both absolute and relative transmittance spectra were measured as a function of temperature using a bolometer detector and a continuous flow helium cryostat. Small differences in the transmittance spectra were assessed at low temperature using absorption differences, calculated from the relative transmittance as $`\alpha (T)\alpha (T=5K)=\mathrm{ln}[𝒯(T)/𝒯(T=5K)]`$. The magnetic field dependence of the transmittance at 5 K was measured at the NHMFL using a 20 T superconducting magnet and a transmission probe equipped with a bolometer detector. Again, transmittance ratio spectra were used to investigate small deviations from unity due to the applied field. By taking the natural log of the transmittance ratio $`(\mathrm{ln}[𝒯(H)/𝒯(H=0)])`$, we obtain the absorption difference at each field: $`\alpha (H)\alpha (H=0)`$.

Upon examination of the absorption difference curves over the entire aforementioned frequency range, we identified three features that change with applied magnetic field. In order to distinguish signal from noise in a quantitative way, we calculated the standard deviation from the mean for each feature. In addition, the same analysis was performed on representative nearby frequency ranges containing no field-dependent features. We use these standard deviations from the mean to quantify the effects of the field and to characterize the intrinsic noise level in regimes away from the magneto-optic signatures . Field sweeps on an empty hole were also carried out for reference; as expected, no field dependence was observed.

## III Results and Discussion

### A Temperature Dependence of the Far Infrared Vibrational Spectra

Figure 1 displays the far infrared transmittance of Mn12 as a function of temperature. As expected for a molecular solid, intramolecular vibrational modes of the Mn12 molecule appear above 150 cm-1 . In agreement with previous authors , we also observe a weak low-energy structure centered near 35 cm-1 (Fig. 1, panel a). This magnetic-dipole allowed excitation has been cited as evidence for other excited state multiplets with $`S`$$``$10 existing in Mn12 . Within our sensitivity, we have found that the 35 cm-1 feature displays limited temperature dependence and no magnetic field dependence.

The far infrared spectra of Mn12 display a large number of intramolecular modes due to the relatively low symmetry of the molecule. They are grouped together in clusters and superimposed upon one another. These structures sharpen and harden with decreasing temperature (Fig. 1). Recent 20 K neutron diffraction studies by Langan $`etal.`$  assessed the low-temperature molecular distortion; compared to the 300 K structure, major characteristics include a gradual displacement of Mn(3) and carboxylate groups, and more extensive solvent interactions including a 4-center hydrogen bond. (Note that Mn(3) is part of the crown, according to the numbering scheme of Ref. , with connections/interactions to the bridges, ligands, and solvent.) These results motivated us to more carefully investigate the far infrared response in the low-temperature regime.

Figure 2a displays the absorption difference spectra of Mn12 at low temperature . The gradual distortion of the cluster framework was previously assessed by neutron diffraction studies . From a magnetic properties point of view, the behavior of the Mn ions is most important; experiment indicates that Mn(3) on the crown displays the most significant low-temperature displacement . A number of vibrational features are modified in this temperature range and therefore likely contain a substantial Mn(3), carboxylate, and acetate ligand contribution. As will be discussed in the next Section, three modes (284, 306, and 409 cm-1) are of particular interest because of their dependence on magnetic field. The 284 cm-1 mode shows an intensity variation at low temperature and a small frequency shift at higher temperatures (Fig. 2b). The standard deviation from the mean in the vicinity of the 284 cm-1 feature (Fig. 2c) quantifies these changes, with an inflection point around 20 K. The maximum in the derivative of the fourth-order polynomial fit to this data better illustrates the position of this inflection point. The 306 cm-1 structure (not shown) is sensitive to this temperature regime as well. Although the feature centered at 409 cm-1 also exhibits changes in this temperature range, no peculiarities were observed around 20 K.

Preliminary molecular dynamics simulations  suggest that a majority of atoms in the Mn12 molecule are, in some way, involved in each vibration in this frequency range. The modes are many, both because of the low molecular symmetry and the large number of atoms. Using mode visualization and the spectra of several model compounds as a guide, particularly that of Mn(II)-Ac2 (Fig. 3), we propose the following general assignments. The low-energy motions below 300 cm-1 include a great deal of acetate (ligand) motion. Complex low energy motions of the core and crown begin around 180 cm-1. These motions include bending, rocking, shearing, twisting, and wagging. Asymmetric and symmetric stretching of the core and crown seem to begin slightly below 500 cm-1, thus providing a likely assignment for the complicated vibrational cluster observed in the spectrum centered near 540 cm-1. The simulations show that modes in this energy range contain sizable (core and crown) oxygen contributions. Comparison of the spectral data from the model compound Mn(II)-Ac2 and Mn12 confirm that the mode clusters centered near 360, 400, and 540 cm-1 in Mn12 are mainly motions of the magnetic center rather than the ligands. Related model compounds such as MnO, MnO2, and Mn2O3 also have characteristic vibrational features in the far infrared (below 600 cm-1). Although the structures are different and Mn valences unmixed compared to the title compound, the reference spectra of these model Mn-based solids  indicate that the far infrared response is rich and highly relevant to the Mn–O motion. Measurements on the Mn(II)-Ac2 model compound (Fig. 3) suggest that the structures centered at 590 and 635 cm-1 in the spectrum of Mn12 are acetate-related. The similar temperature dependence of these modes in the two samples supports this assignment.

In order to understand and model physical properties that contain important phonon contributions (for instance $`\rho `$DC or heat capacity) in the thermally activated regime, it is helpful to know realistic values of the most important low-energy infrared active phonons of Mn12. Our data suggests that use of a relatively small series of characteristic frequencies may be adequate. For instance, the three most intense structures are centered at 375, 410, and 540 cm-1. More complete models might take additional modes, the detailed mode clustering, and relative intensities into account.

### B Magnetic Field Dependence of the Far Infrared Vibrational Spectra

Figure 4 displays the magnetic field dependence of three features in the far infrared spectrum of Mn12. The center positions of these structures ($``$284, 306, and 409 cm-1) are indicated with arrows on the absolute transmittance spectra in Fig. 1. It is interesting that the 284 and 306 cm-1 features do not correspond to major modes in the absolute transmittance spectrum. As shown in the left-hand panels (Figs. 4a, 4c, and 4e), the field dependence as measured by the absorption difference spectra is well-defined for the mode near 284 cm-1, whereas it is more modest for the structures centered at 306 and 409 cm-1. The filled symbols and solid lines in the right-hand panels (Figs. 4b, 4d, and 4f) provide a quantitative view of the field dependent trends. The standard deviation from the mean for the three modes of interest shows a clear upward trend, in contrast to that of nearby spectral regions which shows no field dependence and provides an estimate of the intrinsic noise level .

The feature at 284 cm-1 is the most prominent of the three field dependent structures. The absorption decreases with applied field and shows a tendency toward saturation at 17 T, as indicated in Fig. 4b. The standard deviation from the mean in nearby spectral ranges (for instance, similarly sized regimes centered at $``$ 277 and 299 cm-1) shows no field dependence. The response of the 284 cm-1 feature is therefore well above the noise and characteristic of Mn12. Similar trends and a tendency towards saturation of the standard deviation from the mean are observed for the more complicated absorption difference structures centered near 306 and 409 cm-1, although the overall coupling of these modes to the applied field is weaker and the line shapes are different from that of the 284 cm-1 feature. The changes observed near 306 cm-1 are mainly caused by a 1 cm-1 softening, whereas the 409 cm-1 structure is due to both softening and broadening. The field dependence of these three features in the absorption difference spectra is confirmed by repeated measurements using different experimental parameters . Further, as seen in Fig. 4, the trend with applied field in both the difference spectra and the standard deviation from the mean near 306 and 409 cm-1 can be easily distinguished from that of the non-field-dependent intervals.

It is of interest to understand the microscopic character of the 284, 306, and 409 cm-1 modes and why they are affected by the magnetic field. Although there are a number of mechanisms that might explain this behavior, such as the effect of magnetic field on hybridization of ligand-metal bonds , we believe the most promising is that of spin-phonon coupling. Here, variations in the applied field modulate the magnetic system, thereby affecting the phonons coupled to it. Such an interaction has been thought to be important for describing the slow magnetization relaxation behavior of Mn12, making it an important term in the total Hamiltonian . That only three far-infrared features are observed to change with applied field up to 17 T suggests that these modes are related to motions that maximally change the low temperature spin interactions. One possible candidate for such motion might contain bending between the core and crown structures affecting the Mn-O-Mn angle, therefore modulating the superexchange between Mn ions. An alternate explanation involves the especially curious sensitivity of the 284 cm-1 mode to temperature variation (in the range 5-35 K) as well as to the applied magnetic field. This coincidence suggests that the magneto-elastic response at 284 cm-1 may be intimately related to the Mn(3) motion on the crown. Interestingly, the 306 cm-1 structure also displays some sensitivity to the displacement of the molecular framework. Further work is clearly needed to untangle these complex interactions.

The observed magnetic field dependencies at 284, 306, and 409 cm-1 suggest that $`_{sph}`$ can be augmented by including contributions from these three vibrational modes. Spin-lattice interactions in the far-infrared energy range have been observed in a number of other transition metal oxides in the past . However, the energy scale of the 284, 306, and 409 cm-1 features is larger than might be expected for relevant spin-phonon processes in Mn12, even in the thermally activated regime. Indeed, previous studies on the title compound have focused on acoustic phonons as the major contributors to $`_{sph}`$ . Thus, if these far-infrared phonons are connected with the Mn12 relaxation processes in any way, virtual states would likely be involved. The energy scale of the 284, 306, and 409 cm-1 phonons may be more relevant to high field transport or specific heat measurements.

## IV Conclusion

We have measured the far-infrared response of Mn12 as a function of temperature and magnetic field. The features in this region involve vibrations from all of the groups of atoms (core, crown, and ligands) in the molecule. Three structures related to intramolecular vibrations near 284, 306, and 409 cm-1 are observed to change in applied magnetic field, suggesting that they are coupled to the spin system. Of these three, the feature centered at 284 cm-1 displays the strongest coupling. Based on the similarity between the temperature and field dependent absorption difference data, we speculate that this mode involves Mn(3) motion on the crown. The data reported here may be helpful in understanding the role of vibrations in the theoretical models of magnetization relaxation in Mn12 and related systems.

Current address: Department of Chemistry, University of Tennessee, Knoxville, TN 37996.

## V Acknowledgements

Funding from the National Science Foundation (DMR-9623221) to support work at SUNY-Binghamton is gratefully acknowledged. The work at Florida State University was also partially funded by the NSF. A portion of the measurements were performed at the NHMFL, which is supported by NSF Cooperative Agreement No. DMR-9527035 and by the State of Florida. We thank Z.T. Zhu for technical assistance.