text:
# Competing tunneling trajectories in a 2D potential with variable topology as a model for quantum bifurcations.

## I Introduction

Molecules possessing more than one stable or metastable configurations (so-called non-rigid molecules be1 , be2 ) are interesting as many of their properties differ considerably from those of rigid molecules. In addition, such molecules have practical applications as building blocks of present and future display and sensor technologies. Theoretical modelling of non-rigid molecules is often hampered by a lack of detailed knowledge concerning their eigenstates and eigenfunctions. As a rule, vibrational spectra of the non-rigid molecules are characterized by local oscillations around the minima and tunneling splittings due to transitions between these quasi-local states. When only one ”coordinate” (the reaction path) is related to a large amplitude motion while all other degrees of freedom can be approximated as small amplitude oscillations be3 , be4 , the behavior of the system is determined completely by a single minimum action trajectory. The dynamics becomes more complex when more than one coupled large amplitude motions (i.e. more than one strongly fluctuating variables) are present. In this case, several minimum energy paths connect minima of the potential energy surface (PES). Phenomena like instabilities or bifurcations can appear in certain regions of parameters describing the PES, and the analysis of such a situation is the main issue of the present paper.

In the general case of a PES with n minima, states of the system can be described using $`n`$ sets of eigenfunctions, quasi-localized near each minimum, while tunneling between different states is related to the overlap between these functions. The characteristic energy scale for tunneling, usually much smaller than the thermal energy, is determined by the chemical nature of the non-rigid molecule, or, in other words, by the quantum chemistry of the system. Depending on the parameters describing the PES of a non-rigid molecule, one may expect different types of behavior, which can be treated in terms of quantum instabilities also called quantum phase transitions.

Quantum phase transitions (that occur in a quantum mechanical system at zero temperature as a function of some non-thermal control parameter) and related phenomena, like quantum bifurcations and instabilities have been a subject of great theoretical interest in recent years (see e.g. monograph SA99  and references herein). Unlike ordinary phase transitions, quantum transitions occur between ground states and involve negligible changes in entropy. Examples include transitions in Quantum Hall systems, localization phenomena, and the superconductor - insulator transition in two-dimensional systems SA99 , SG97 . Usually these phenomena take place in many particle systems driven by competing interactions (a well known example is the superconductor - normal metal quantum phase transition at $`T=0`$ arising from electron - electron correlation competing with electron - phonon interaction MA62 ). As a result of the competition, a quantum bifurcation may occur at a critical value of the coupling constant, leading to singularities of some properties. The most robust features of quantum bifurcations are divergences or singularities in certain characteristics of the system at the critical value of the coupling constant and drastic changes of the behavior below and above. Both classical and quantum critical points are governed by a divergent correlation length, although quantum systems possess additional properties that do not have classical counterparts. The fact that the ground state wavefunction undergoes a qualitative change at a quantum instability is one of these and is the subject of this paper.

Remarkably, similar features may arise in few-body systems. A well-known example is the so-called level crossing phenomenon LL65  when an excited level becomes the ground state at a critical value of the interaction parameter. In this paper we analyze another type of quantum instability taking place for a 2D PES changing its topology as a function of a continuous parameter $`\alpha `$ and illustrate the results by numerical investigations. The model PES has two equivalent minima separated by one or two saddle points. The change from one to two saddle points takes place for a certain critical value of $`\alpha =\alpha _c`$. In addition, the PES may be symmetric or asymmetric with respect to the second coordinate, perpendicular to the one relating the two minima. For the symmetric case (two equivalent saddle points) there are two regions (I and II) of the phase diagram, where tunneling is realized either along one minimum action trajectory essential for the semiclassical description of the motion (region I), or along two equivalent paths (region II). Zero point fluctuations smear out a sharp second order transition between the two regions and lead to a certain crossover behavior. For the asymmetric case, one can have also a first order phase transition related to the fact that one of the two trajectories becomes unstable.

The competition between trajectories in this model plays the role of competing interactions in many body systems with quantum bifurcations. Divergences in thermodynamic quantities are mapped onto a certain singular behavior in our model (critical fluctuations at finite-temperatures have their equivalent in the zero-point quantum delocalization) and, in fact, reflect more fundamental phenomena. Loosely speaking, any continuous quantum bifurcation is related to specific conditions (or specific values of parameters) when the lowest excitations become gapless and a qualitative change in the nature of the frequency spectrum occurs.

In the literature KS00 , SK01 , several analogies have been proposed to describe the ground state stability of a small system (such as an atom or a molecule) in terms of phase transitions, mapping a $`d`$-dimensional quantum systems onto a $`d+1`$-dimensional classical system. This formal equivalence (first proposed long ago jo1 , jo2 ) is based on the observation that the quantum action includes not only an integration over the space variables but includes also one imaginary time dimension, which, for $`T=0`$, is of infinite extent. The quantum - classical mapping is a very general fact. One can always reinterpret the imaginary time functional integral of a $`d`$-dimensional quantum theory as a finite temperature Gibbs distribution function of a $`d+1`$-dimensional classical theory.

Naively, this seems to imply that quantum bifurcations are not very interesting. However, as elsewhere in science, the devil is in the details of this mapping. For example it turns out SA99  that there is no guarantee that the Gibbs weights, found by such a mapping, are positive (they can even be complex valued). This implies that one may not use the mapping blindly, i.e. for any arbitrary system. Thus a direct and explicit treatment of the quantum models is required.

Instead of the divergence of the correlation length (which is the cornerstone of traditional descriptions of criticality in determining the scaling behavior of all other quantities) any quantity that changes its scaling behavior at $`\alpha =\alpha _c`$ can be used. Thus, it is not necessary to restrict analogies of phase transition to the search for the points where the correlation length diverges. As shown below, in the present model the wave functions itself manifest a characteristic critical behavior.

The remainder of this paper is organized as follows. In Section II we investigate a model 2D potential having two equivalent minima, and two saddle points. The shape and the topology of the potential depend on one continuous parameter, $`\alpha `$, playing the role of a controlling parameter in a phase transition terminology. At the critical value $`\alpha =\alpha _c`$, two saddle points (and the maximum of the potential in between) merge into one saddle point. In this Section we also present a qualitative picture of the quantum bifurcation. Section III is devoted to the numerical verification of the qualitative scenario. Minimum energy and extremal tunneling trajectories of the potential are determined. In the Section IV the results presented in the Section III are generalized to an anisotropically deformed PES, with the aim to relate predictions of the theoretical results to possible experimental verifications such as the effect of partial deuteration. Some specific examples of non-rigid molecules are also discussed in this section. Finally, in Section V we conclude.

## II Instanton approach to a model 2D potential.

In order to investigate the scenario of quantum bifurcations described above, one should solve the Schrödinger equation for a 2D PES of variable shape and topology. No standard method of solution is known for a 2D PES of general shape. In the semiclassical approximation (the concern of this paper), the commonly used WKB method LL65 , HE62 , is reduced to matching wave functions between classically allowed and forbidden regions. This matching is easily achieved in the 1D case with only one strongly fluctuating variable. Technically, already for two dimensions with one strongly and one weakly fluctuating variable the procedure becomes tedious and computationally demanding. However for higher dimensional PES and for more than coupled large amplitude motions, fundamental difficulties are encountered of how to match many-valued semiclassical wave functions at a non-trivial set of boundaries between allowed and forbidden regions in multidimensional phase space. To the best of our knowledge this problem has not been investigated previously in any general form.

However, there is an alternative to the universal WKB semiclassical formalism, the so-called extreme tunneling trajectory or instanton method, which is not only very efficient for calculating globally uniform wave functions of the ground state (as initially formulated PO77 , CO ) but which can also be adapted for the description of low-energy excited states BM , BV99 , BV00  (and which can even be extended with reasonable accuracy to highly excited states BK02 ). The instanton method eliminates much of the tedious WKB calculations because there are no classically allowed regions in the formalism (and as a consequence there are no singularities of semiclassical wave functions). Within the instanton method, bifurcations or instabilities are simply related to the existence of multiple-valued solutions of the equations of motion, i.e. appearance of two (or more) solutions with similar values of their action. Unlike WKB wave functions, which have singularities at the boundaries between classically allowed and forbidden regions, the variations over the space of instanton wave functions can be followed continuously. The price to pay for this advantage is related to the nonexistence of classically allowed regions and the absence of natural Bohr - Sommerfeld quantization rules. In the instanton approach, these rules must be established by different methods. In addition, the instanton equations contain second order turning points whereas the WKB equations have only linear, first order, turning points.

The main steps of the instanton method, used to determine semiclassical solutions to the Schrödinger equation in the potential $`V(X,Y)`$, are:

* i) The so-called Wick rotation in phase space, corresponding to the transformation to imaginary time ($`tit`$), is made.
* ii) Solutions of the Schrödinger equation are represented in the form

$`\mathrm{\Psi }=A(X,Y)\mathrm{exp}(\gamma W(X,Y)),`$ (1)
$`\gamma 1`$ is a large semiclassical parameter, $`\gamma m\mathrm{\Omega }_0a_0^2/\mathrm{}`$, where $`m`$ is a mass of a particle, $`a_0`$ is a ”microscopic” characteristic length of the problem, e.g. the tunneling distance, $`\mathrm{\Omega }_0`$ is a characteristic frequency, e.g. the oscillation frequency around the potential minimum, $`\mathrm{}`$ is set equal to 1, measuring energies in frequency units, and $`W`$ has a meaning of action.
* iii) The terms in the Schrödinger equation, first and second order in $`\gamma ^1`$, become identically zero, if the wave function in the form of Eq. (1) satisfies the time independent Hamilton-Jacobi equation for $`W`$ and the so-called transport equation for $`W`$ and $`A`$ (see below and also BM , BV99 , BV00  for details).

Below, the instanton approach is used to determine semiclassical solutions of the Schrödinger equation in the following model 2D PES:

$`V(X,Y)={\displaystyle \frac{1}{2}}(1X^2)^2+{\displaystyle \frac{\omega ^2}{1\alpha }}\left[{\displaystyle \frac{1}{2}}(X^2\alpha )Y^2+{\displaystyle \frac{1}{4}}Y^4\right].`$ (2)
The PES given by Eq. (2) is dimensionless: coordinates $`X`$ and $`Y`$ are measured in units of the distance, $`a_0`$, between two minima along $`X`$, the energy is measured in units of the oscillation frequency, $`\mathrm{\Omega }_0`$, in one of the wells. The prefactor of the second term of Eq. (2) is chosen such that the oscillation frequency along $`Y`$ (at $`X=\pm 1`$) is independent of $`\alpha `$, and equals the parameter $`\omega `$. The potential, Eq. (2), is bound for $`\alpha <1`$ and has in this case the following stationary points: $`\{X=\pm 1,Y=0\}`$ are two equivalent minima; $`\{X=0,Y=0\}`$ is a saddle point for $`\alpha <0`$ and becomes a maximum at $`0<\alpha <1`$; $`\{X=0,Y=\pm \sqrt{\alpha }\}`$ are two saddle points at $`0<\alpha <2/(2+\omega ^2)`$, becoming minima when $`\alpha >2/(2+\omega ^2)`$ with the appearance of four additional saddle points. In the following, the discussion is restricted to the region of $`0<\alpha <2/(2+\omega ^2)`$, where additional stationary points, having no ”critical” behavior, are absent. The bifurcation phase diagram in the plane of the parameters $`\alpha ,\omega ^2`$ is shown in Fig. 1. For a classical system, one would have a continuous bifurcation at the line $`\alpha =0`$ from a behavior governed by one minimum energy trajectory (region I in the Fig. 1) to dynamics with two minimum energy paths passing through the two saddle points (region II). Representative equipotential maps of PES corresponding to the two regions are shown in Fig. 2. As discussed in the next Section, quantum zero point fluctuations shift and deform the transition line and smear out the bifurcation line. Finally there is a certain crossover behavior between regions (I and II).

A simple physical realization of a PES such as given by Eq. (2) would be a molecule with two equivalent coupled wide amplitude coordinates $`x`$ and $`y`$ describing, for example, proton tunneling (in monograph BM  many such examples are discussed). When the coupling between the tunneling particles is neglected, the dimensionless PES is represented as a sum of two strongly fluctuating motions:

$`V_0(x,y)={\displaystyle \frac{1}{2}}(1x^2)^2+{\displaystyle \frac{1}{2}}(1y^2)^2.`$ (3)
Taking into account symmetric coupling, a term:

$`V_1(x,y)=c(x^2y^2)^2,`$ (4)
must be added to Eq. (3). After a transformation to coordinates $`X=(x+y)/2`$ and $`Y=(xy)/2\sqrt{3}`$, one obtains the PES given by Eq. (2), provided that the parameters $`\omega `$ and $`\alpha `$ are related as follows:

$$\omega =3\sqrt{2(1\alpha )}.$$

To explore the behavior of the system with respect to variations of parameters $`\omega `$ and $`\alpha `$, controlling the shape and the topology of the model PES, Eq. (2), the minimum energy and extreme tunneling trajectories should be fully analyzed. Dealing with quantum transitions between different states of the system, one must distinguish between adiabatic and non-adiabatic transitions. Adiabatic transitions take place at $`\omega 1`$ along the minimum (maximum) energy paths (MEP), defined by the condition that the PES should have an extremum orthogonal to the MEP:

$`{\displaystyle \frac{dY}{dX}}={\displaystyle \frac{V/Y}{V/X}}={\displaystyle \frac{2(1X^2)(1\alpha )+\omega ^2Y^2}{(X^2\alpha )Y^2}}{\displaystyle \frac{X}{\omega ^2Y}}.`$ (5)
From the symmetry of Eq. (5) is clear that $`Y^2`$ is a function of $`1X^2`$, and $`dY/dX=0`$ on the surface $`X=0`$. In the region II of Fig. 1, there exist therefore two types of paths satisfying Eq. (5):

(i) two equivalent paths I via the saddle points;

(ii) a shorter path II, $`Y=0`$ passing through the maximum.

The extreme tunneling (i.e. instanton) zero energy trajectories are described by the equation of motions (”Newton laws”) in imaginary time and for the inverted PES (i.e. for $`VV`$)

$`\ddot{X}={\displaystyle \frac{V}{X}},\ddot{Y}={\displaystyle \frac{V}{Y}}.`$ (6)
At $`\alpha >0`$, the trajectories satisfying Eq. (6) lie between the paths I and II due to a non-adiabaticity of the transitions caused by the finite frequency of the transverse oscillations. The instanton action increases when $`\alpha `$ decreases, since the absolute value of the potential at the saddle points increases as:

$`V^{}V(0,\pm \sqrt{\alpha })={\displaystyle \frac{1}{2}}{\displaystyle \frac{\omega ^2\alpha ^2}{4(1\alpha )}}.`$ (7)
## III Quantum bifurcation.

In this section, the results of the previous section are used to illustrate numerically the appearance of quantum bifurcations (already qualitatively discussed in the introduction). Standard applications of the instanton method reduce to minimizing the non-local action along a one dimensional trajectory. Such an approach supposes that there is a single path connecting initial and final states. This is evidently not the case for our model. As a first step, the equations of motion, Eq. (6), are solved and the resulting minimum energy and extreme tunneling (instanton) trajectories are shown in Fig. 2 for two values of the controlling parameter $`\alpha `$. As the instanton trajectories deviate from the minimum energy paths, the collapse of the two instanton trajectories, when $`\alpha `$ decreases, occurs at a certain finite value of $`\alpha ^{}>0`$ which does not coincide with the point $`\alpha =0`$ where the PES changes its topology. The dashed line in Fig. 1 defines region $`II^{}`$ within region II, where two minimum action trajectories exist, in the remainder of region II the minimum action trajectory is the 1D trajectory $`Y=0`$. Thus, the potential Eq. (2), admits two types of instantons: a 1D instanton ( $`Y=0`$ and $`\dot{Y}=0`$); and 2D instantons where the transverse displacements have a maximum at the plane $`X=0`$, separating initial and final states, while the transverse velocities achieve extrema at intermediate points where the trajectories deviate from the 1D instanton. The contribution of any trajectory to the transition rate is a result of the tradeoff between the length of the path and the barrier height along this path. Naively, exploiting such idea, we come to the bifurcation criterion, which determines the critical value of the controlling parameter $`\alpha `$ as the value at which the actions along the both competing trajectories become equal. We designate the value by $`\alpha ^{}`$. However, by definition of instanton actions, the point $`\alpha ^{}`$ corresponds to the harmonic approximation of the potential, and therefore this criterion is too crude for our anharmonic model potential, Eq. (2). In Fig. 3, the minimum action as a function of $`\alpha `$ is plotted for $`\omega =1`$. In the same figure the action along the minimum energy paths is also represented.

A more rigorous approach is based on the observation that at the bifurcation point a new type of the trajectory (2D) appears, and the initial 1D trajectory becomes unstable. To study the stability of the trajectory it is sufficient to restrict oneself to a Gaussian (harmonic) approximation for the transverse motion, and the instanton approach is therefore adequate. The one dimensional instanton solution becomes unstable when the lowest eigenvalue of the second functional derivative of the action over the trajectory variations becomes zero

$$\frac{\delta ^2W}{\delta X^2}=0.$$

This lowest eigenvalue is traditionally called the stability parameter $`\lambda `$. When the value of $`\lambda `$ becomes zero (the corresponding value of $`\alpha `$ will be called the critical value and denoted $`\alpha _c`$) the tunneling channel centred around an extreme 1D path becomes infinitely wide (and the transverse fluctuations are no longer Gaussian) and new types of the trajectories (2D), possessing a smaller action, appear. We believe that this criterium is physical, and it will be shown below that just around the value $`\alpha _c`$ the critical behavior of the tunneling splitting takes place (more precisely the crossover due to quantum zero point fluctuations).

The next step is to determine the wave functions. The ground state instanton wave functions can be represented in the form of Eq. (1) as

$`\mathrm{\Psi }_0(X,Y)=A_0(X,Y)\mathrm{exp}(\gamma W(X,Y)),`$ (8)
where the functions $`A_0(X,Y)`$ and $`W(X,Y)`$ should satisfy the Hamilton-Jacobi and transport equations BM , BV99  , BV00

$`{\displaystyle \frac{1}{2}}\left({\displaystyle \frac{W}{X}}\right)^2+{\displaystyle \frac{1}{2}}\left({\displaystyle \frac{W}{Y}}\right)^2=V(X,Y),`$ (9)
and

$`{\displaystyle \frac{W}{X}}{\displaystyle \frac{A_0}{X}}+{\displaystyle \frac{W}{Y}}{\displaystyle \frac{A_0}{Y}}+{\displaystyle \frac{1}{2}}\left({\displaystyle \frac{^2W}{X^2}}+{\displaystyle \frac{^2W}{Y^2}}2E_0\right)A_0=0,`$ (10)
$`E_0`$ is the ground state energy.

In Fig. 4, the ground state wave function at the surface $`X=0`$ is shown for different values of the parameter $`\alpha `$. Far away from the critical region, the wave functions are localized at the saddle points while the probability distribution is smeared out over the whole region between the potential minima in the critical region. The tunneling splitting is given by the expression:

$`\mathrm{\Delta }_0={\displaystyle _{\mathrm{}}^+\mathrm{}}\mathrm{\Psi }(0,Y)\left({\displaystyle \frac{\mathrm{\Psi }}{Y}}\right)_{X=0}𝑑Y.`$ (11)
The value of this splitting given by the probability flow integrated over the dividing plane $`X=0`$ depends on the exponential factor, $`\mathrm{exp}(\gamma W^{})`$, where $`W^{}`$ is Euclidean action between the minima. Appart from this leading term, $`\mathrm{\Delta }`$ depends on prefactors characterizing both type trajectories. In order to eliminate the leading term contribution and visualize the critical behavior of $`\mathrm{\Delta }`$, $`\mathrm{\Delta }_0\mathrm{exp}(\gamma W^{})`$ is plotted as a function of $`\alpha `$ in Fig. 5. The width of the maximum around the critical value, $`\alpha =\alpha _c`$, is determined by quantum (zero point) fluctuations.

Tunneling leads to an energy splitting (tunneling splitting, $`\mathrm{\Delta }_0`$) between two otherwise degenerate states and the eigenstates are symmetric and antisymmetric combination of these states. This tunneling splitting between the two lowest eigenstates of the Hamiltonian is therefore the quantity of interest. Alternatively, the rate of oscillation between the two classically degenerate states can be measured after the system has been prepared in one of these states.

At small values of $`\alpha `$ some new phenomenon could occur due to these quantum fluctuations. In this region, at the surface $`X=0`$, the depth of the wells becomes so small that wave functions are effectively delocalized due to quantum fluctuations. The natural (though qualitative) criterion of the delocalization should compare amplitude of zero point oscillations along $`Y`$ in one well with the distance between wells. The same criterion as given above, could be formulated as the condition that there are no discrete energy levels in a shallow well. Both criteria compare the energy difference between the maximum and the saddle point of the PES, Eq. (2), $`V(0,0)V(0,\sqrt{\alpha })`$, with the energy of zero-point oscillations in one-well, $`\stackrel{~}{\omega }/\gamma `$, where $`\stackrel{~}{\omega }`$ is the frequency of oscillations around $`\pm \sqrt{\alpha }`$ in the potential $`V(0,Y)`$, renormalized by anharmonic corrections. Taking into account all numerical factors we obtain:

$`{\displaystyle \frac{\alpha _c^2\omega ^2}{4(1\alpha _c)}}(1+\sqrt{2}){\displaystyle \frac{\omega }{\gamma }}\sqrt{{\displaystyle \frac{2\alpha _c}{1\alpha _c}}},`$ (12)
Eq. (12) is fulfilled for $`\alpha _c=0.56`$ (at $`\omega =1`$) as found in our numerical computations shown in Fig. 5.

The square root divergence of the localization length at $`\alpha _c`$ corresponds to the critical behavior of the correlation length in standard classical second order phase transitions. The tunneling splitting $`\mathrm{\Delta }_0`$, calculated above, is our main result. $`\mathrm{\Delta }_0`$ is the product of an exponential and pre-exponential factor, and only the pre-factor demonstrates the critical behavior (more precisely - the crossover behavior) shown in the Fig. 5. It may, of course, not be easy (if possible at all) to measure directly the contribution of a small pre-factor with a singular behavior as a function of $`\alpha `$ when $`\mathrm{\Delta }_0`$ is dominated by the large exponential factor with a regular behavior. Given that a measurement of a non-linear susceptibility of the system is equivalent to the measurement of the corresponding derivative of $`\mathrm{\Delta }_0`$ over the controlling parameter $`\alpha `$ offers one possibility. For example, when a local dipole moment is associated with the tunneling particles in a system with inversion symmetry, an applied external electric field will make the two 2D paths inequivalent, while the single 1D path would be unaffected. Let us emphasize that the symmetry breaking phenomenon takes place due to tunneling processes only and is thus by its nature a dynamic phenomenon. We will discuss this issue in the next section.

The second possibility to observe this kind of critical (crossover) behavior is based on the general Herring-Lifshits formula (see Eq. (11) and LL65 ), which shows that the splitting $`\mathrm{\Delta }_0`$ is determined by the integral over the $`Y`$ coordinate at the dividing surface $`X=0`$, and is thus proportional to the total width of the tunneling channels. Therefore, the effect we got, might be considerably enhanced in 3D systems due to increase of the phase volume of tunneling channels. A 3D model PES, of which our 2D model PES, Eq. (2), is a plane section, is given by $`V(X,\rho )`$, where ($`\rho =(Y^2+Z^2)^{1/2}`$.

## IV Anisotropy.

The PES, investigated in the previous sections, is symmetric with respect to the reflection $`YY`$. Both tunneling particles are therefore identical as are the two tunneling paths.

As mentioned above, breaking this symmetry may be useful, in order to expose more clearly the singular behavior of the pre-factor. Indeed, the response should to expose a qualitatively different behavior with respect to any factor breaking the symmetry near the critical region (i.e. close to the bifurcation point) or far from it. This idea, the so-called fluctuation - dissipation theorem relating correlation and response functions, is well known for conventional thermodynamic phase transitions. Two mechanisms of breaking this mirror symmetry, which are easily realized, will be analyzed below. First, partial deuteration will make the tunneling particles different. Second, as mentioned above, an external electric field may render inequivalent the tunneling channels for the two particles. Both mechanisms can be described in a phenomenological way by adding the following anisotropic perturbation to the bare symmetric PES, Eq. (2):

$`V_a(X,Y)=\beta (1X^2)Y,`$ (13)
The parameter $`\beta `$ describes the strength of the anisotropy. In the potential (13) higher order anisotropic terms, $`Y^3(1X^2)`$, and so on, were neglected for the sake of simplicity. Even though, strictly speaking, this assumption is not justified, since $`Y`$ is a strongly fluctuating degree of freedom, this approximation correctly identifies the characteristic scales in the problem and all qualitative features of its behavior. For hydrogen - deuterium substitution of one of the two tunneling atoms, for example, the resulting anisotropy parameter is easily evaluated as:

$`\beta ={\displaystyle \frac{1}{4}}\left(\sqrt{{\displaystyle \frac{m_1}{m_0}}}1\right),`$ (14)
where $`m_0`$ and $`m_1`$ are masses of the $`H`$ and $`D`$ isotopes. In an applied electric field, the anisotropy parameter $`\beta `$ will be proportional to the field strength. The precise choice of the anisotropic PES, Eq. (13), is delicate, and depends on the detailed structure of the system under consideration. Aiming at a qualitative description, we have chosen the simplest form of breaking the $`YY`$ symmetry while the symmetry $`XX`$ is preserved, so that the two potential well are still equivalent.

The analysis of this modified PES is analogous the one presented in the section II for the symmetric PES. In the $`\alpha ,\beta `$ parameter phase plane, we should first find all minimum energy and extreme tunneling trajectories. There are 4 different regions on this plane as shown in Fig. 6. In the region II one maximum and two saddle points exist, in region I there is only one saddle point. The behavior is more subtle in region III, where the saddle point that is more distant from the maximum is transformed into the minimum (i.e. the $`X`$ -”oscillation” frequency changes its sign). By the dashed lines we depicted also the sub-region $`II^{}`$, where there are two extreme tunneling trajectories. In the remaining part of the region II, corresponding to relatively small values of $`\alpha `$, the extreme tunneling trajectory close to the maximum becomes unstable.

In Fig. 7 we show the minimum energy and extreme tunneling (instanton) trajectories for a small value of the anisotropy parameter ($`\beta =0.05`$) and for different values of $`\alpha `$. It illustrates that even a small anisotropy lifts the degeneracy of two instanton trajectories. In addition, the straight line path II, passing through the maximum $`\{X=0,Y=0\}`$, for the symmetric PES, Eq. (2), becomes curvilinear and deviates from $`Y=0`$. Hence for the anisotropic PES ($`\beta 0`$) all regions in the phase diagram with different types of the trajectories have the same symmetry, and therefore only first order bifurcations between the regions are allowed. Finally, in Fig. 8, the actions along the instanton and the minimum energy paths are plotted. The figure shows again that the anisotropy, Eq. (13), removes the degeneracy, and that two instanton trajectories appear when $`\alpha `$ exceeds a certain threshold value. This disappearance of one instanton trajectory is a specific feature of discontinuous first order bifurcations. Concluding this section, we emphasize that it is this sensitivity to anisotropy, which can lead to a drastic change of behavior.

## V Experimental consequences

Bifurcations of minimum energy paths (due to the presence of more than one saddle point separating stable configurations of the PES) are rather common in molecules with several strongly fluctuating coordinates. In non-rigid molecules, dynamically strongly fluctuating coordinates of this sort of are typically different combinations of hydrogen transfer, hindered rotation of $`XH_n`$ groups, or inversions. Molecular systems with two hydrogen transfers (synchronous or stepwise) attract special attention, as these processes are thought to be relevant for many biological processes, including so-called tautomeric reactions be1 , be2 , be3 , BM .

Two proton exchange in pairs of $`OH\mathrm{}O`$ fragments of various carbonic acid dimers is an example of synchronous tunneling. In our model, this transfer corresponds to a one dimensional trajectory in region II, and the longitudinal $`X`$ and transverse $`Y`$ coordinates are symmetric and antisymmetric combinations of proton displacements $`d_1`$, $`d_2`$:

$`X={\displaystyle \frac{1}{2}}(d_1+d_2);Y={\displaystyle \frac{1}{2\sqrt{3}}}(d_1d_2).`$ (15)
The coefficients are chosen such that Eq. (2) is the sum of Eqs. (3) and (4), and the results of Sections II and III can therefore be used. For the 1D path $`Y=0`$, with one saddle point $`\{X=0,Y=0\}`$, the displacements of the both tunneling protons are always (i.e. at any point of the trajectory) equal to each other ($`d_1=d_2`$). In the pure classical limit, the width of the tunneling channel is determined by the corresponding potential curvature:

$$\mathrm{\Delta }_{}=\left(\frac{^2V}{Y^2}\right)_{0,0}^{1/2},$$

Within the harmonic approximation, there is a mean field ($`\alpha ^{1/2}`$) divergency. In the plane $`X=0`$, the anharmonic $`Y^4`$ contribution provides a cutting-off of this divergency.

Quantum, zero point transverse fluctuations spread out this singularity, and the width of the tunneling channel depends on $`\alpha `$ even in region II of Fig. 1. The characteristic potential barrier height, $`V^{}`$, for the synchronic two proton transfer in the carbonic acid dimers is $`V^{}(1015)`$ Kcal/mol (5000 - 7000 K), while the energy $`E_{st}`$ corresponding to a step wise transfer (that is paths $`d_1=0,d_2=1`$ or $`d_1=1,d_2=0`$) is two or even three times larger BM88 , LK97 . On the other hand, within the frame of our model PES, the ratio $`E_{st}/V^{}`$ depends on the controlling parameter $`\alpha `$ as follows:

$`{\displaystyle \frac{E_{st}}{V^{}}}=1{\displaystyle \frac{3}{2}}\alpha ,\alpha <0.`$ (16)
Inserting the numerical values of the characteristic energies given above into Eq. (16), one can see that even in the systems where the strongly fluctuating motions are believed to be strongly correlated, the controlling parameter $`\alpha `$ is close to -0.5, and quantum fluctuations must be taken into account to describe correctly the tunneling dynamics.

Many examples of intermediate (between synchronic and step wise) dynamics exist also, one example being the so-called free base porphyrin compounds BM88 , SM89 . In these compounds with molecular symmetry $`D_{4h}`$, four nitrogen atoms (numbered clockwise: $`A`$, $`B`$, $`C`$, $`D`$) form a square and two mobile protons $`a`$ and $`b`$ occupy positions such that configurations ($`aA`$, $`bC`$) and ($`aB`$, $`bD`$) are equivalent minima, while configurations ($`aA`$, $`bD`$) and ($`aB`$, $`bC`$) are equivalent saddle points (taking into account clockwise motions only). Our model PES, Eq. (2), can be adapted to this case with . According to experimental data and quantum chemistry calculations BM88 , SM89  the energy of the saddle points is of the order of 0.3 -0.5 of the energy at the maximum ($`X=0,Y=0`$). Thus from Eq. (7) we come to the estimation $`\alpha 0.30.4`$. For these intermediate values of $`\alpha `$, the quantum (minimum action) and the classical (minimum potential) trajectories are quiet different. Indeed, the classical and tunneling trajectories pass through the saddle points, and the maximum, respectively. The existence of saddle points lead to a considerable broadening of the tunneling channel as it is illustrated in the Fig. 3. Similar considerations are easily applied to the hydrazine molecule with two coupled inversion motions (see LK97  and references therein).

For the partially deuterated molecule, we can also evaluate the anisotropy parameter $`\beta `$ entering the PES, Eq. (12). According to Eq. (13) $`\beta 0.1`$, and the $`HD`$ isotopomer remains therefore in the same region I of the phase diagrams as protonated porphyrin. The main conclusion of this short analysis is that our simple model gives a fairly realistic representation of non-rigid molecules.

We have shown that effects due to competition of trajectories and quantum fluctuations are relevant in a broad range of the parameters entering our model. The examples discussed above lead to the conclusion that the widely accepted classification of synchronic and step wise motions must be used with care, since in typical cases both types of motions are involved. This implies also that the traditional CO  Gaussian approximation (small fluctuations around one extreme tunneling trajectory) in not valid in the case of strong coupling between both tunneling particles, and one must take into account both competing tunneling channels. Similar phenomena might play a role in pairing of isolated nucleic-acid bases in the absence of the DNA backbone. In Ref. NK00  spectroscopic characteristics of the hydrogen bonding in isolated guanine-cytosine ($`GC`$) and guanine-guanine ($`GG`$) base pairs have been investigated. The results show that the gas phase $`GC`$ base pair adopts a single configuration, whereas $`GG`$ exists in two different configurations. We already mentioned in the section II that the effect, obtained here, may be considerably enhanced in 3D systems due to the increase of the phase volume of the tunneling channels (our 2D model PES can be considered as a section of the corresponding 3D space). Among systems, where a 3D generalization of our model could be applicable, are cubic alkali halide crystals doped with a light atomic or molecular ions as substitutional impurity. Due to mismatch in size, these impurities frequently occupy off-centre positions in the lattice. There is a small number of equivalent off-centre positions, so that the impurity ground state is degenerate, and tunneling transitions between these positions are observed. However, the vibrational frequencies of off-centre impurities are usually much smaller than characteristic host lattice phonon frequencies, and therefore the coupling to the lattice vibrations is relatively small. As a first approximation, one can visualize the system as one particle in a potential where the tunneling transitions between the initial and the final state can proceed in several alternative ways. In the trajectory language it signifies the possibility of competition (and bifurcation) between extremal paths of different types. Since transitions between different off-centre positions are associated to a charge displacement, the corresponding PES changes upon application of external electric field or mechanical stress. We anticipate that the bifurcations described above by our model could be observable for off-centre impurities as well, and that understanding this mechanism will be essential to predict and to describe the behavior. A more specific study of 3D systems undergoing this kind of the quantum bifurcations, might become appropriate as suitable experimental results become available.

A completely different system might also be a physical realization of our model. The tunneling of magnetic spins has recently received much attention (see e.g. GB95 ) in view of its promise as one of the few realistic candidates for quantum computing. Conventional magnetic materials used in the experiments contain many domains, each possessing its own set of parameters. Besides the spins interact with the crystal matrix and complicates the physical picture with respect to our model. However, quantum tunneling of spin is also possible in a spinor condensate trapped in double - well potential GB95 ) and this system possesses several decisive advantages compared with more conventional solid state materials and is more suitable for a description in the frame work of our model (the system is characterized by a few simple parameters amenable to experimental control).

## VI Conclusion.

We have presented here a path-integral approach to treat a 2D model of quantum bifurcations. A PES, the shape of which is determined by a continuous parameter, offers a natural way to examine quantum instability phenomena. Candidates that realize our model for quantum bifurcations are non-rigid molecules, spin condensates, and some other systems. In any system exhibiting some kind of quantum phase transitions it is important to understand how its genuine quantum aspects evolve throughout the transition. We investigated the behavior of the ground state wavefunction undergoing qualitative changes at a quantum instability, but other indicators of the phase transition could be examined in the same way (in a very recent publication, for example, the authors studied wave function entanglement phenomena OA02 ).

A second order bifurcation takes place for a 2D model PES with mirror symmetry, which changes its topology at a certain critical value $`\alpha _c`$ of the continuous parameter $`\alpha `$. At $`|\alpha \alpha _c|\alpha _c`$ only one minimum action trajectory is essential for semiclassical description of the particle motion, while in the ”critical” region at $`|\alpha \alpha _c|\alpha _c`$ the behavior is governed by two different trajectories almost degenerate with respect to the magnitude of the action. In our model, the competition between trajectories plays the role of competing interactions in many body systems experiencing quantum phase transitions. The divergence in correlation length is mapped onto a singular behavior of the localization length. Due to zero point quantum fluctuations, the system manifests a smoothed crossover behavior only instead of a sharp bifurcation. When the PES becomes asymmetric, a first order phase transition is associated with the disappearance (in a certain region of the potential parameters) of one minimum action trajectory. We illustrate the results by numerically investigating this behavior. The approach is general and has potential applicability for large (many particle) systems. Furthermore, it is possible to fabricate structures which are small enough (mesoscopic) for the electronic transport to be largely coherent, so that the wave (quantum) properties of electrons dominate. Note also that the usefulness of our results can be substantially enhanced by the advent of semiconductor heterostructures in which the potential for the electrons can be tuned and varied in space with great precision.

One more an interesting line of thought for future work would be to analyze, in analogy with the approach presented here, a phase stability with respect to small fluctuations for conventional phase transitions. It is known for Landau-Ginzburg type models stat , that the corresponding Landau-Khalatnikov equations have a form analogous to the Schrödinger equation (where a coordinate plays the role of an imaginary time) AF91 .

Our results can in principle be tested also by investigations of low temperature properties of disordered materials, containing certain point defects that undergo atomic tunneling ES98 . Recently KF99 , WU02  the low temperature dielectric properties of certain multi-component glasses were tentatively assigned to the existence of coupled two-level tunneling systems. This means that several tunneling paths between potential minima exist, as in the model presented here.

It is important to notice that the investigation of our paper refers to a singular behavior in the ground state of the system, as, strictly speaking, quantum phase transitions occur only at $`T=0`$. Because all experiments are necessarily done at some nonzero temperature, care must be taken when comparing our theoretical results to experiment, and we have to keep in mind the consequences of the $`T=0`$, and $`\alpha =\alpha _c`$ singularity on physical properties at $`T>0`$. Technically, finite temperature effects also can be incorporated into the instanton method. To do this, one should take into account the finite period ($`1/T`$) of instanton trajectories (an analogous approach was developed for the WKB method WL85 , GO87 ). When these contributions become comparable to zero point quantum oscillations, the quantum phase transition is smeared out.

###### Acknowledgements.

The research described in this publication was made possible in part by RFFR Grants. We thank A. Hüller and P. Nozières and J.Lajzerowicz for thought-provoking discussions. One of us (E.K.) is indebted to INTAS Grant (under No. 01-0105) for partial support.

Figure Captions.

Fig. 1

$`\omega ^2\alpha `$ phase diagram. In the region II the PES has two minima and two saddle points, only in the region $`II^{}`$ two minimum action paths coexist with 1d trajectory $`Y=0`$, in the region I the PES has two minima and one saddle point and in the region III more than two minima.

Fig. 2

Equipotential map for 2D PES Eq. (2); dashed lines designate minimum energy trajectories, and the solid lines show the minimum action (tunneling) trajectories. (a) $`\omega =1,\alpha =0.55`$ , (b) $`\omega =1,\alpha =0.20`$ .

Fig. 3

The action $`W^{}`$ as a function of the parameter $`\alpha `$ at $`\omega =1`$ for: (1) the minimum action tunneling trajectory , (2) the 1d path, $`Y=0`$ , and (3) the minimum energy trajectory.

Fig. 4

Ground state wave functions ($`n=0`$) at $`X=0`$ for $`\omega =1`$ and $`\gamma =20`$: (1) $`\alpha =0.625`$ ; (2) $`\alpha =0.55`$ ; (3) $`\alpha =0.3`$.

Fig. 5

Tunneling splitting as a function of $`\alpha `$ for $`\omega =1`$, and $`\gamma =20`$ in the critical region (the dashed line is a continuation to the stability region).

Fig. 6

The phase diagram for the anisotropic PES, Eq. (13), in the $`\alpha \beta `$-plane with $`\omega =1`$. In the region II the the PES has one maximum and two saddle points and in the region I only one saddle point. In the region III one of the saddle points from region II (more distant from the maximum) is transformed into the minimum. In the region $`II^{}`$ there are two minimum action trajectories.

Fig. 7

Equipotential map for the anisotropic PES. Instanton (solid lines) and minimum energy (dashed lines) trajectories. $`\omega =1`$, $`\beta =0.05`$: (a) $`\alpha =0.58`$; (b) $`\alpha =0.45`$; (c) $`\alpha =0.20`$.

Fig. 8 The action $`W^{}`$ as a function of $`\alpha `$ along the instanton (solid lines) and minimum energy (dashed lines) paths. $`\omega =1`$, and $`\beta =0.05`$. The curves 1 and $`1^{}`$ correspond to the trajectories more distant from the maximum, whereas lines 2 and $`2^{}`$ correspond to the trajectories close to the maximum.


format: text

text:
# Magnetic flux jumps in textured Bi2Sr2CaCu2O8+δ

## I INTRODUCTION

Magnetic flux jumps are one of the peculiar phenomena of interest in both conventional, hard type II superconductors and in high temperature superconductors (HTSs). Studies of flux instabilities in superconducting materials are of interest both from a basic point of view and also in light of their potential applications. In addition, the investigation of flux jumps in HTSs are relevant to the understanding the complexity of the vortex matter in the mixed phase of these materials. It is known that under appropriate conditions, the critical state of a superconductor may become unstable, leading to an avalanche-like process, initiated by a small fluctuation of the temperature or external magnetic field. This process is associated with the sudden puncture of magnetic flux into the volume of the superconductor with a corresponding increase in the material’s temperature. During this process, the screening current is appreciably reduced, perhaps even to zero. From the point of view of the applications, magnetic flux jumps are problematic as they may drive superconductor into a normal or resistive state. Flux jumps cause also abrupt changes to the sample dimensions, which may be observed via magnetostriction measurements nab97 . Flux jumps phenomenon have been studied primarily by magnetization measurements, screening experiments and torque magnetometry (see reference wip92  for review).

The basic theory appropriate to magnetic flux jumping was developed in late 1960s by Swartz, Bean and Wipf wip65 ; wip67 ; swa68 . Theoretical analysis usually assumes the fulfillment of the local adiabatic conditions for the sample, which in turn depends upon the relation between the thermal (Dt) and the magnetic (Dm) diffusivity of the material. If Dt$``$Dm, the local adiabatic conditions for the occurrence of the flux jump process are assumed to be satisfied. Flux jumps are associated with the diffusion of magnetic flux into the superconductor. The diffusion time $`\tau `$m of magnetic flux, is inversely proportional to magnetic diffusivity, i.e. $`\tau `$m$``$1/Dm. Similarly, the thermal diffusion time $`\tau `$t is inversely proportional to thermal diffusivity, $`\tau `$t$``$1/Dt. If the thermal diffusion time is significantly longer than the characteristic time for the process, the conditions of this process are considered to be locally adiabatic. In the case of magnetic flux jumps, these conditions are satisfied when $`\tau `$t$``$$`\tau `$m or Dt$``$Dm.

The stability criteria of the critical state of hard type II superconductors may be obtained by analysis of a loop of several interconnected processes, as was discussed for example by Wipf wip92  (see also Fig.2 in reference wip92, ). A small thermal fluctuation, $`\mathrm{\Delta }`$T1, causes an appropriate decrease in the critical current density. This in turn decreases the screening current of the superconductor, allowing some additional magnetic flux to enter the volume of the sample. The additional flux causes heat dissipation, which generates an additional increase of the temperature of the superconductor by amount of $`\mathrm{\Delta }`$T2. If $`\mathrm{\Delta }`$T2$`>`$$`\mathrm{\Delta }`$T1 an avalanche-like process in form of a flux jump is induced. The range of temperature and magnetic field for which flux jumps occur is determined by two parameters. The first one is the instability field Bfj. In the adiabatic approximation, and for an infinite slab geometry sample, the instability field for the first flux jump (after cooling the sample in zero magnetic field) is given by the formula:

$`B_{fj1}`$ $`=`$ $`\sqrt{{\displaystyle \frac{2\mu _0cJ_c}{dJ_c/dT}}}`$ (1)
where c is specific heat, Jc is critical current density and, $`\mu `$0 and T are the magnetic permeability of vacuum and temperature, respectively. This theory assumes that Jc is independent on the magnetic field, and Bfj1 are measured after cooling the sample in zero magnetic field.

At sufficiently low temperatures, both the specific heat of the superconductor and the instability field for the first flux jump Bfj1 increase with temperature. At some higher temperature, the Bfj1(T) curve reaches a maximum and then drops to zero at the critical temperature of the superconductor (Tc), because at this temperature the critical current of the superconductor vanishes. At 4.2 K typical values of Bfj1 predicted by eq. (1) are of the order of 0.1 T. Thus, flux jumping is expected to be an important problem from the point of view of applications of type II superconductors, as it limits the performance of these materials in a low temperature regime.

The second parameter affecting the appearance of flux jumps is the critical dimension of the superconductor, i.e. the minimum sample dimension for which flux jumps occur. The critical dimension of the sample depends on the sample’s shape, its orientation relative to the external magnetic field and on the relation between Bfj1 and the value of the field of full penetration (B) of the superconductor. For the case of infinite slab geometry sample, or for an infinitely long cylindrical sample with an external magnetic field aligned parallel to its surface (slab sample) or axis (cylindrical sample), the role of the critical dimension is played by the sample diameter. The parameter B depends on the sample shape, the sample’s orientation in the magnetic field and the field dependence of the critical current density. To the good approximation B is proportional to the critical current density (Jc) and sample dimensions.

For the case of an infinite slab or cylinder and under the assumption that Jc(B)=constant (the so-called Bean model bean62 ), the field of full penetration can be calculated using relation B=$`\mu _0`$Jcd, where d is a half of the diameter of the infinite slab or the cylinder. At sufficiently low temperatures Bfj1 increases with increasing temperature, whereas B decreases. At some temperature (T1), B(T1)$`=`$Bfj1(T1) and at higher temperatures B$`<`$Bfj1. Assuming that Jc(B)=constant, the critical diameter of the slab or cylinder sample for which $`\mathrm{\Phi }_{crit}`$=2dcrit, may be determined from the equation B(T1)=$`\mu _0`$Jc(T1)dcrit. For a slab (or cylinder) with diameter smaller than the critical one, no flux jumps occur at any temperature for any external magnetic field, independent of whether the measurements are made during the virgin magnetization curve (taken after cooling the sample in zero external magnetic field) or for other parts of magnetization hysteresis loop. However, when the critical current density depends on magnetic field, the situation becomes more complex. In this case, even if there are no jumps in the virgin magnetization curve, some jumps (so-called ”solitary jumps” mll94 ) may appear after reversal of external magnetic field direction. When the critical current density is a non-monotonic function of the magnetic field (the so-called ”fish tail” or ”butterfly” effect), then under appropriate conditions so-called ”island jumps” may also be found cha98 . All these phenomena result from the changes in magnetic field profile in a superconducting sample caused by the field dependence of the critical current density as well as by magnetic history. In all cases, however, some critical dimension of the sample exists and for samples with dimensions smaller than the critical one, no jumps occur at any temperature or magnetic field. Thus, by reducing the diameter of the superconductor it is possible to avoid flux jumping. This approach is commonly used in producing multifilament superconducting wires. Flux jumping in conventional superconductors, including the extension of the basic flux jumping theory to non-adiabatic conditions, has been thoroughly reviewed in reference min81 .

Magnetic flux jumps have also been observed in high temperature superconductors wip92 . Because of the existence of a critical dimension, flux jumping in HTSs was observed only in relatively large single crystals or well-textured polycrystalline samples with high values of the critical current. No such effect has been observed in ceramics, because the critical dimension in these materials is limited by the grain size, which is typically very small, of the order of several microns. Most of the studies of flux jumps in HTSs that have been reported to date have been carried out on YBa2Cu3O6+δ wip92  or La2-xSrxCuO4 nab97 ; mch92 ; ger93  single crystals, or on highly textured polycrystalline materials. In contrast, there are only a few reports of magnetic flux jumping in the Bi2Sr2CaCu2O8+x system.

Early experiments by Guillot and co-workers gui89 , observed flux jumps in an assembly of preferentially oriented Bi2Sr2CaCu2O8+x single crystals. Unfortunately, no systematic studies of this phenomenon were reported. Magnetic flux jumps were also found in a large polycrystalline Bi2Sr2CaCu2O8+x flux tube bur94 . More systematic observations of flux jumping in BiSCCO system have been reported by Gerber and co-workers gerb93 . This work reports flux jumps in a Bi2Sr2CaCu2O8 sample consisting of a pile of c-oriented single-crystalline slabs, but only at relatively high magnetic field sweep rates, above 1 T/s gerb93 . Among HTS materials Bi2Sr2CaCu2O8+x is characterized by a strong anisotropy, much stronger than is the case in La2-xSrxCuO4 or YBa2Cu3O6+δ. Hence, flux jumps studies of Bi2Sr2CaCu2O8+x may be useful in understanding the development of the instability process in strongly anisotropic superconductors. A detailed understanding of the instability process in Bi2Sr2CaCu2O8+x is also important from the viewpoint of potential applications of Bi-based compounds in Ag/BiPbSrCaCuO composites.

Many aspects of magnetic flux instabilities in HTSs as well as in conventional superconductors require further investigation to both elucidate the intrinsic dynamics of magnetic flux in superconductors, and to enable future applications. The present paper deals with systematic studies of magnetic flux jumping phenomena in c-oriented, textured, Bi2Sr2CaCu2O8+δsamples at magnetic field sweep rates between 0.06-1.2 T/min. Specifically, we investigate the temperature dependence, magnetic field sweep rate dependence, as well as the presence of magnetic flux creep on the occurrence of flux jumping. The influence of demagnetizing effects on flux jumping is discussed in the framework of the Brand, Indenbom and Forkl model of the critical state of an infinitely long and thin superconducting strip in an external magnetic field perpendicular to its surface bra93 .

## II EXPERIMENTAL DETAILS

A Bi2Sr2CaCu2O8+δpolycrystalline boule sample with a circular cross-section of about 6 mm in diameter was grown by the floating zone technique in a four mirror optical furnace. The critical temperature of the as-grown material was about 92 K, very close to optimal for this HTS. From the as-grown boule, a sample of approximate dimensions 4.2x2.2x0.2 mm3 was detached by cleaving, such that the shortest edge of the detached sample was parallel to the c-axis.

X-ray diffraction studies of the cleaved sample show it to consist of a mosaic of several well-aligned single crystals. The rocking curve showed that the total misalignment of the c-axes of this mosaic of single crystals was about 5 degree. This sample was used for all further studies of magnetic flux jumps reported here. Magnetization measurements were carried out using a Quantum Design PPMS-9 system with the maximum external attainable field of 9 Tesla. The measurements were performed using the extraction magnetometer option. In this option the sample is moved between two pick-up coils with constant velocity, whereas the signal from the pick-up coils is integrated to calculate the magnetic moment of the sample under study. During experiment the sample was surrounded by a low pressure helium gas (around 0.5 Tr) thus, similar heat sinking conditions were maintained by crossing from 1.95 K to above 4.2 K. In all the magnetization measurements reported here, the temperature was varied between 1.95 K and Tc and the external magnetic field was changed in sweep mode. The temperature dependence of magnetization hysteresis loops was measured with constant sweep rate of 0.3 T/min. In addition, the magnetic field sweep rate dependence of the flux jumping was studied systematically at a single temperature of 4.2 K. The sweep rates were adjustable between the maximum and the minimum rates attainable in our system i.e. between 0.06 T/min and 1.2 T/min respectively.

## III RESULTS

Figure 1 shows magnetization hysteresis loops for our sample, with the external magnetic field parallel to its c-axis. This data was obtained for temperatures between 1.95 K and 6.5 K. All the measurements presented here were performed after cooling the sample in zero magnetic field. The external magnetic field was then swept from 0 T to 9 T, back to -9 T and again back to 0 T. The magnetic flux jumps are observed in the temperature range from 1.95 K up to 6 K and they are not evident at 6.5 K, as Figure 1 shows. Such magnetization hysteresis loops were also measured above 6.5 K, to temperatures up to Tc, but these measurements showed no magnetic flux jumping in the investigated sample. Similar measurements, carried out with magnetic field parallel to the sample surface i.e. perpendicular to the c-axis and at the same sweep rate of 0.3 T/min showed no magnetic flux jumps in the whole temperature range studied i.e between 1.95 K and Tc.

As can be seen in Figure 1, the number of observed jumps decreases with increasing temperature. Increasing the temperature increases both the value of the field at the first flux jump, Bfj1 (see also Fig. 4), as well as an increase in the field spacing between subsequent jumps. At temperatures above 3 K, all of the observed jumps are complete, meaning that the magnetization of the sample during a jump drops to zero. Figure 1 shows also the influence of the magnetic history on flux jumping. This influence is most clearly seen in the hysteresis loop measured at relatively high temperatures such as 6 K. Here one can see that only a single jump occurs within the first quadrant of the M(H) plot i.e. while the external magnetic field increases from 0 T to 9 T. There are no jumps observed in the second quadrant of the M(H) curve, when the magnetic field is decreased from 9 T to 0 T. Subsequently there are two jumps present when the external magnetic field is changed from 0 T to -9 T (within the third quadrant).

The magnetic field sweep rate dependence on flux jumping has been studied at the temperature of 4.2 K and these results are shown in Figure 2. These measurements were carried out in the first quadrant of the M(H) hysteresis loop. With increasing sweep rate, and external magnetic field in the range from 0 T to 9 T, the number of observed flux jumps increases, whereas the value of Bfj1 decreases (see also Fig. 6). We emphasize that, at the lowest attainable sweep rate of 0.06 T/min and the same temperature of 4.2 K, no flux jumps occurred in our sample. Figure 2 shows all experimental points recorded. One can see that the observed jumps occur in a time interval shorter than that between the subsequent experimental points. The minimum time interval between experimental points is limited in our system to about 5 s.

In order to analyze the influence of flux creep on flux jumps we have measured the magnetic relaxation of our sample. The following procedure was adopted during the measurement. The sample was cooled in zero magnetic field to the temperature of 4.2 K, at which time the external magnetic field was increased from zero to 2 T at a rate of 0.3 T/min. This value of the field, 2 T, was chosen to prevent appearance of flux jumps, which first occur at this temperature at slightly higher magnetic fields i.e. at 2.38 T (see Figures 1,2,4,6). Measurements of magnetic moment were then performed over a period of one hour and these results are shown in Figure 3. The relaxation of the magnetic moment is approximately logarithmic in time. After one hour, about a 10% decrease from the initial value of magnetic moment is observed in the sample.

## IV ANALYSIS

The behavior of the magnetization jumps displayed by our Bi2Sr2CaCu2O8+δsample and shown in Figure 1, is typical for thermally activated flux jumps in type II superconductors nab97 ; wip92 ; wip65 ; wip67 ; swa68 ; mll94 ; cha98 ; min81 ; mch92 ; ger93 ; gui89 ; bur94 ; gerb93 . This data allows one to construct a relation between the field of the first flux jump, Bfj1 and temperature, as shown in Figure 4. The fact that Bfj1 increases with increasing temperature is consisitent with the adiabatic theory of flux jumping wip65 ; wip67 ; swa68 , discussed earlier.

The present results show that all flux jumps we observe at temperatures higher than 3 K are complete. This indicates that the energy released during the jump is sufficient to drive the superconductor into the resistive state, which means that this energy is sufficient to increase the temperature of the sample to the value at which the critical current density of the superconductor vanishes. It is important to note that to reduce critical current density to zero in the case of HTSs, it is not necessary to heat the superconductor above Tc but just above the vortex melting temperature, where the vortices become virtually unpinned. At lower temperatures more energy is required to drive superconductor into the resistive state as compared to higher temperatures. The temperature increase during a jump depends on the quantity of energy released during the jump, and on the specific heat of the sample. At 1.95 K the magnetic field interval between the successive jumps is less than at higher temperatures. Thus the magnetic energy stored in the superconductor between two successive jumps at 1.95 K is smaller than it is at higher temperatures. It may be that this magnetic energy is insufficient to drive the superconductor into the resistive state. Therefore for a number of jumps observed at 1.95 K, the magnetization of the sample does not drop to zero, as one can see in Figure 1.

The magnetic history dependence on flux jumping, shown in Figure 1, can also be accounted for by the theory presented in references mll94 ; cha98 . In these references, the temperatures and magnetic field range for which flux jumps occur was studied in the framework of the adiabatic theory, assuming different dependences of the critical current density as a function of the magnetic field. It was found that, if the critical current density decreases with increasing magnetic field, flux jumps first appear in the third quadrant of the M(H) plot. Therefore, this quadrant of the M(H) plot is least stable from the point of view of appearance of flux jumping. Comparison of the magnetization hysteresis loops at different temperatures shows that as the temperature is lowered flux jumps appear in the first quadrant and also at the end in the second quadrant of the M(H) plot. Thus, the second quadrant of the M(H) plot is the most stable from the point of view of appearance of flux jumping. This behavior of the flux jumps has been also observed in our sample, as shown in Figure 1 (e.g. temperature 6 K).

In order to quantitatively compare the present experimental results with the predictions of the adiabatic theory, we have estimated the value of Bfj1 at 4.2 K. This requires an estimate of the specific heat as well as temperature dependence of the critical current density. Determination of the critical current densities on the basis of magnetization hysteresis loop measurements as well as the stability of the critical state depends strongly on the distribution of the screening currents in a superconducting sample. This problem is important in the case of polycrystalline HTSs, where the grain boundaries may act as the weak links, reducing the critical current density even by several orders of magnitude. However, the texture of the polycrystalline samples is of great importance for limiting the critical current. If the polycrystalline sample consists of a set of well aligned grains, a large current may be shunt by the substantial common areas between adjacent grains, bypassing the weak links. This phenomenon is described in terms of the so-called ”brick wall” model bula92  and it is commonly observed in superconducting thin films as well as in Ag/BiPbSrCaCuO tapes, which despite their polycrystalline structure are characterized by high critical current densities. Similar is applicable in the case of our sample, when an external magnetic field is parallel to the c-axes of the grains. In this case, screening currents flow within the ab-planes of the grains and they have very large areas with which to bypass the weak links. Hence, in our further analysis the whole sample will be treated as a single grain and the effect of the weak links will not be taken into account. It is also worth noting that after finishing our measurements the sample was cleaved again into several smaller pieces, each of which possessed almost the same surface area as the original sample. This suggests that the original sample had a sandwich-like structure of the weak links, which would not limit the screening currents in ab-planes, when the external magnetic field is parallel to the c-axes of the grains.

The temperature dependence of the critical current density in the direction parallel to the ab-plane is estimated based on the magnetization data and these results are shown in Figure 5. The widths of the magnetization hysteresis loops were measured at different temperatures at the zero external magnetic field, and subsequently, a value of the critical current density was estimated using a formula appropriate to a sample whose cross-section in the plane perpendicular to an external magnetic field is in shape of a rectangle, as discussed in reference gyo89 . As the flux jumps occur primarily at low temperatures, this procedure cannot be effectively used in this range, below 6 K. Thus, the temperature dependence of the critical current density was estimated only for temperatures above 6 K. Figure 5 shows this result between 6 K and 38 K.

As one can see in Figure 5 at zero external magnetic field and at 6 K critical current densities of the order of 106 A/cm2 were found. These values of the critical current density are close to the upper limit of the critical current densities usually observed in the Bi2Sr2CaCu2O8+δsystem. This fact is probably connected with the presence of a large number of structural defects acting as pinning centers. The temperature dependence of the critical current density at zero magnetic field is roughly exponential. However, it is difficult to fit a unique exponential formula to the whole range of experimental data (see Fig. 5a). An exponential temperature (as well as magnetic field) dependence of the critical current density in superconductors with weak pinning is expected from flux creep mchenry94 . A precise analysis of these dependencies must also reflect the scaling of fundamental pinning related parameters on temperature, as well as on magnetic field mchenry91 . To take into account the dependence of these parameters on temperature we have rescaled the temperature axis by a function g(T)=1-(T/Tc)2 (see Figure 5b). This function is consistent with Ginzburg-Landau theory and is discussed in references mchenry94 ; mchenry91 . In the case of HTSs the g(T) function is usually assumed in the form g(T)=1-(T/Tirr)2, where Tirr is the irreversibility temperature. At zero external magnetic field we have assumed Tirr=Tc. As one can see in Figure 5, after application of this procedure, very good fitting of the available experimental data is obtained by using exponential formula Jc(T)=Jc0\*exp(-T/T0) where: T=T/g(T), Jc0=3\*106 A/cm2 and T0=8.4 K.

The specific heat of Bi2Sr2CaCu2O8+δat 4.2 K was estimated using c(T)=$`\beta `$T3 with $`\beta `$=2 mJ/K4mol cas89 ; fis88 , from which we get c(4.2 K)=11x102 J/Km3. Using this value of specific heat, the above temperature dependence of the critical current density and formula (1), we estimate Bfj1(4.2 K)$``$0.15 T, a value roughly one order of magnitude lower than that observed in our experiment. Similar discrepancies between experimentally observed values of Bfj1 and those calculated within the framework of the adiabatic theory, have been reported for other HTS system nab97 ; wip92 ; mch92 ; ger93 ; gui89 ; gerb93 ; mll94 . In these studies, the experimentally observed values of Bfj1 at 4.2 K are of an order of 1 T or higher.

In order to account for why our sample appears more stable against flux jumping than would be expected from adiabatic theory, two phenomena need be considered. First, it is possible that adiabatic conditions may simply not be fulfilled in our experiment. Were this to be the case, we would expect the thermal anchoring of the sample to the cold finger of the cryostat to strongly influence flux jumping. The second possibility is flux creep. As was shown by McHenry and coworkers mch92 , flux creep stabilizes the critical state of the superconductor against the flux jumps. Both the possibilities may imply a dependence of the flux jumping on the sweep rate, as in fact is observed experimentally. This means that decreasing the sweep rate may stabilize the superconducting sample against flux jumping; thus the observed values of Bfj1 would be higher than those predicted by adiabatic theory.

Figure 6 shows the dependence of the field of the first flux jump, Bfj1 on the magnetic field sweep rate. As the sweep rate decreases the value of Bfj1 increases rapidly and at a sweep rate of 0.12 T/min it approaches a value of about 4.5 T (Fig.6). From Figure 6, one sees that Bfj1 tends to saturate at higher sweep rates. The exact value of the Bfj1 field at the saturation cannot be determined, as the maximum sweep rate attainable in our system is 1.2 T/min. However, we estimate it to be around 1 T, several times higher than the value predicted by adiabatic theory. Similar strong sweep rate dependence on Bfj1 was observed in other HTS systems mch92 ; ger93 ; gerb93 ; gui88 .

To check whether the adiabatic conditions are satisfied in our experiment we need to determine the relation between thermal (Dt) and magnetic (Dm) diffusivity. These parameters are estimated by applying standard procedure presented in reference mch92  from the formulas: Dt$``$$`\frac{\kappa }{c}`$ and Dm$``$$`\frac{\rho }{\mu _0}`$, where: $`\kappa `$ \- thermal conductivity, c - specific heat and $`\rho `$ \- resistivity. The estimation of these parameters in Bi2Sr2CaCu2O8+δis difficult for several reasons. Firstly, the transport properties of this system are extremely anisotropic. The value of the inplane thermal conductivity for Bi2Sr2CaCu2O8+δis estimated to be $`\kappa `$(4.2 K)$``$ 1 W/Km dam89 , which gives Dt(4.2 K)$``$9x10-4 m2/s. However, the value of the thermal conductivity along the c-axis of Bi2Sr2CaCu2O8+δis difficult to determine experimentally, although one expects this value, as well as that for the thermal diffusivity, to be significantly lower than in ab-plane, due to the planar nature of the material.

The estimate of the magnetic diffusivity in superconductors is also difficult. In nonsuperconducting materials the coefficient of the magnetic diffusivity is proportional to their resistivity. The normal state resistivity in Bi2Sr2CaCu2O8+δis extremely anisotropic mar88 . The in plane resistivity $`\rho _{ab}`$ varies linearly with temperature with d$`\rho _{ab}`$/dT=0.46 $`\mu `$$`\mathrm{\Omega }`$cm/K, whereas resistivity along the c-direction $`\rho _c`$ is about five orders of magnitude higher mar88 . In the configuration appropriate to our experiment, flux front moves in the direction parallel to ab plane. Hence, for the magnetic diffusivity, the estimation of $`\rho _{ab}`$ is the appropriate one. Assuming a linear temperture dependence to $`\rho _{ab}`$ below Tc, one obtains $`\rho _{ab}`$(4.2 K)$``$1.9x10-8 $`\mathrm{\Omega }`$m and therefore Dmab-normal(4.2 K)$``$1.5x10-2m2/s for the normal state diffusivity. This value of magnetic diffusivity is more than one order of magnitude higher than the in plane thermal diffusivity. However, since our sample is not in a normal state but in a superconducting mixed state, the flux flow resistivity ( $`\rho _f`$=$`\rho _n`$$`\frac{B}{B_{c2}}`$, where $`\rho _n`$ is the normal state resistivity, and $`B_{c2}`$ is the upper critical field of the superconductor) must be used to estimate the magnetic diffusivity. On the basis of our magnetization data and above expressions, we estimate $`\rho _f`$$``$$`\frac{1}{30}`$$`\rho _n`$ just before appearance of the first flux jump, which gives Dmab(4.2 K)$``$5x10-4 m2/s. This value of magnetic diffusivity is the same order of magnitude as the in plane thermal diffusivity. Therefore adiabatic conditions may be not fulfilled in our experiment at 4.2 K and this may be one reason for enhanced stability of our sample against flux jumping at this temperature. We may also expect an influence of the heat exchange conditions on flux jumping in our system as well. We should bear in mind, however, that our sample’s geometry is that of a relatively thin pellet with its flat surface parallel to the ab-planes. Such a geometry minimizes heat exchange by transport within the ab-plane, and heat transport along the c-axis is expected to be significantly lower than that in the ab-plane. On the other hand, the estimation of the magnetic diffusivity on the basis of flux flow resistivity alone, may be questionable. Recently, it was suggested by Mints dmints96  that the presence of flux creep may cause Dm$`<<`$Dt and as a result the local heat exchange conditions to be strongly non-adiabatic.

Flux creep is a phenomenon which may stabilize our sample against flux jumping, as well as imply a sweep rate dependence on flux jumps. Bi2Sr2CaCu2O8+δcrystals are characterized by relatively strong magnetic relaxation caused by flux creep biggs89 ; sved91 . At low temperatures and for a relatively small time window, this magnetic relaxation is logarithmic in time. Similar magnetic relaxation was found in our sample (see Fig.3). On the basis of our results we have estimated the effective pinning potential (Ueff) to be Ueff/k$``$210 K at T=4.2 K and H=2 T, where k is the Boltzman constant. This value of Ueff is typical for the given temperature and magnetic field range in Bi2Sr2CaCu2O8+δsystem.

Another system characterized by relatively strong flux creep and magnetic relaxation is La1-xSrxCuO4 mchenry91 . Similarly, a strong influence of the external magnetic field sweep rate on flux jumping was found in La1.86Sr0.14CuO4 crystals mch92 . The presence of flux creep changes the magnetic flux profile in a superconducting sample during a sweep of an external magnetic field. It was shown by McHenry and co-workers mch92  that in the presence of flux creep, heat generated in the superconducting sample by a fluctuation of an external magnetic field is relatively small compared to the case when flux creep is absent. This fact influences the stability conditions of the critical state. As a result we expect an increase of the value of Bfj1 relative to that predicted by the theory, in which flux creep phenomenon is not taken into account. Flux creep phenomenon can fully stabilize the superconducting sample against flux jumping as the rate of magnetic field changes decreases. Related behavior was indeed observed in our experiment (see Fig.2).

The influence of flux creep on flux jumping was also analyzed theoretically by Mints dmints96 . In this model a logarithmic dependence of the screening current density on the electric field (induced by external magnetic field changes) was assumed, whereas the thermal conditions were assumed to be extremely non-adiabatic. (i.e. $`\tau `$t$`<<`$$`\tau `$m or Dt$`>>`$Dm). As a result the predicted values of the Bfj1 depend strongly on the heat transfer coefficient. Assuming the Bean model bean62  (i.e. Jc(B)=const) this theory predicts Bfj1$``$(dHe/dt)-1/2, where dHe/dt is the external magnetic sweep rate. A fit of this formula to our experimental data is shown in Figure 6 by the dotted line. Comparison of the experimental and the fitt curve show that while the experimental curve tends to saturate at higher sweep rates around the value of Bfj1$``$1 T the formula predicts that it approaches zero. It was shown in reference dmints96  that taking into account a decrease of the critical current density with magnetic field slows down the decrease of Bfj1 with increasing dHe/dt. Nevertheless, the theoretical curve still approaches zero at sufficiently high sweep rates. For more accurate comparison of the theoretical formula (from reference dmints96 ) with experiment, investigations at higher sweep rates would be necessary. A quantitative comparison of this formula with our experimental results was impossible, because neither the electric-field dependence of the screening current nor the heat transfer coefficient in our experimental setup were known.

Finally, let us discuss the influence of demagnetizing effects on flux jumping. As our sample is in a form of a thin pellet and the external magnetic field is aligned perpendicular to its surface, one may expect a relatively strong influence of such effects on the flux instabilities. The easiest way to analyze the influence of demagnetizing effects on a magnetic material is to introduce a demagnetizing factor D. In the case of superconductors this factor is often estimated from the initial slope of the magnetization curve. Such procedure gives D$``$0.82 in our case. However, the application of the demagnetizing factor is not fully appropriate in the case of superconductors, due to the fact that the magnetization of superconductor is caused by macroscopic screening currents. The self-component of the magnetic field significantly alters the distribution of these currents in a superconducting sample. This fact was confirmed by a number of experiments performed on both conventional frank79  and high temperature superconductors theus92 ; tame93 . The experiments were performed by magneto-optic technique theus92  or by using scanning Hall-probes frank79 ; tame93  on thin conventional superconducting discs frank79 , HTS films theus92  or thin single crystals tame93 , in the external magnetic field perpendicular to their surfaces. Until now, many attempts have been undertaken to solve the problem of the magnetic field and screening current distribution in superconductors with non-zero demagnetizing factors sanch01 . In most cases this problem cannot be solved analytically and numerical calculations are necessary. However, the problem of the distribution of the screening currents and magnetic field was solved analytically for superconducting samples with large (close to 1) demagnetizing factors, i.e. for samples in shape of infinitely long and thin strips bra93  or infinitely thin disks dae89 .

Since the demagnetizing factor of our sample is large, let us discuss some features of the model presented in reference bra93  pertinent to the present studies of flux jumping. In the above mentioned model, the magnetization of an infinitely long and thin strip in an external magnetic field perpendicular to its surface as a function of this field (after cooling the sample in zero field) is given by:

$`M`$ $`=`$ $`{\displaystyle \frac{1}{2}}J_ca\mathrm{tanh}(\pi {\displaystyle \frac{\mu _0H_e}{B^{}}})`$ (2)
where: $`J_c`$ is the critical current density, a is half of the width of the strip, $`H_e`$ is the external magnetic field, B∗∗=$`\mu _0`$Jcd and d is the thickness of the strip. This model assumes that: d$``$a and Jc(B)=const.

On the basis of equation (2) one can conclude that the magnetization of the infinitely long and thin strip never saturates. The model implies that the center of the strip is fully screened even for extremely large external magnetic fields. Hence, one cannot use the concept of the field of full penetration the same way one would for the well-known case of a sample with zero demagnetizing factor (for example an infinitely long slab or cylinder). However, to some extent the role of the field of full penetration in the case of a strip is assumed by the B∗∗ parameter. It is important to note that in this case d is the thickness of the sample i.e. the dimension of the sample measured in the direction parallel to the external magnetic field. In the case of our sample, d$``$0.2 mm and it is significantly smaller than other sample dimensions. Using the critical current density we estimated earlier, we may estimate B∗∗(2K)$``$5 T and B∗∗(6K)$``$3.5 T. These values are indeed quite close to the maximum value of Bfj1 found in our experiment i.e. 4.86 T at 6 K (Fig. 1). Thus, one may conclude that in the case of very thin samples, such as single crystals or textured samples of the Bi2Sr2CaCu2O8+δsystem, with an external magnetic field perpendicular to their surfaces, the role of the critical dimension from the point of view of appearance of flux jumps, is played by the thickness of the sample.

## V SUMMARY

Flux jumps phenomena in a thin Bi2Sr2CaCu2O8+δtextured sample with an external magnetic field parallel to the c-axis have been systematically studied. The values of the experimentally observed instability fields depend strongly on the external magnetic field sweep rates. Both flux creep and the heat exchange conditions between the sample and its environment must be taken into account in a quantitative analysis of this phenomenon. For thin samples in an external magnetic field perpendicular to their surfaces, the role of the critical dimension from the point of view of appearance of flux jumps is played by their thickness.

We conclude that the necessary requirements for the avoiding flux jumping in Bi2Sr2CaCu2O8+δsingle crystals are following:

(i) The sample thickness has to be lower than its critical dimension, of the order of 0.1 mm, when Jc at the relevant field strengths and temperatures is of the order of 106 A/cm2.

(ii) The magnetic sweep rates have to be low enough to allow for the stabilizing influence of flux creep to operate effectively and to allow for the effective heat exchange between the sample and the experimental environment.

Most experiments performed so far on Bi2Sr2CaCu2O8+δsingle crystals reported in the literature have been carried out on SQUID systems with very low magnetic sweep rates and on very thin (of the order of 0.1 mm) samples. It is thus not surprising that flux jumps have not been reported in these experiments.

###### Acknowledgements.

We acknowledge financial support from the Natural Sciences and Engineering Research Council of Canada and Polish Government Agency KBN contract No. 8T11B03817. One of us (AN) would like to acknowledge a NATO Science Fellowship.