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# Preprint MPI-PhT/2000-38 Adiabatic Inversion in the SQUID, Macroscopic Coherence and Decoherence

## I Introduction

One of the first and certainly probably the most discussed systems in which one tries to demonstrate coherence between apparently macroscopically different states is the SQUID .

In the last decade a number of beautiful experiments at low temperature  have seen effects connected with the quantized energy levels  expected in the SQUID, showing that it does in fact in many ways resemble a “macroscopic atom”. A fast sweeping method  has also seen the effects of these quantized levels even at relatively high temperature.

If we could further show in some way that the quantum phase between two fluxoid states of the SQUID, where a great number of electrons go around a ring in one direction or the other, is physically meaningful and observable it would certainly provide even more impressive evidence for the applicability of quantum mechanics on large scales and help put to sleep any ideas about the existence of some mysterious scale where quantum mechanics stops working.

At this meeting, results using microwave spectroscopy have indeed been reported showing the repulsion of energy levels expected from the quantum mechanical mixing of different fluxoid states . These results indicate by implication that two opposite fluxoid states can exist in meaningful linear combinations and so that their relative phase is significant.

Here we would like to propose another method for demonstrating the coherence between opposite fluxoid states and the meaningfulness of the phase between them. Furthermore the method to be described allows a measurement of the “decoherence time”, the time in which the definite phase or the coherence between the two states is lost. This is interesting of itself since it never has been done and is also relevant to the “quantum computer” where decoherence is the main obstacle to be overcome.

Our basic idea is to use the process of adiabatic inversion or level crossing where a slowly varying field is used to reverse the states of a quantum system. In its most straightforward realization, our proposal consists of starting with the SQUID in its lowest state, making a fast but adiabatic sweep, and reading out to see if the final state is the same or the opposite fluxoid state. If the state has switched to the other fluxoid, the system has behaved quantum mechanically, with phase coherence between the two states. If it stays in the original fluxoid state, the phase coherence between the states was lost and the system behaved classically (see Figs. 3 and 4).

In order for these effects to be unambiguously observable, relaxation towards thermal equilibrium must be small on the time scales involved in the experiment. As is discussed in section IV, this seems to be obtainable at low temperature with suitably chosen sweep times.

A very interesting aspect of the present proposal, as we shall discuss below, is the possiblity of passing between these two regimes, quantum and classical, by simply varying the sweep speed. This allows us to obtain, for adiabatic conditions, the decoherence time as the longest sweep time for which the inversion is successful.

## II Adiabatic Inversion in the rf Squid

Most workers in this field are probably accustomed to discussing level crossing problems such as ours in a Landau-Zener picture where one exhibits the spacing of the two crossing energy levels as some external parameter or field is varied. This is of course a perfectly good and useful picture for many applications. However I would like to urge consideration of another perhaps more intuitive visualization, one which is particularly well suited to time dependent problems as we have here, and which also has the advantage that it gives a complete representation of the state of the system at a given time and not just the level splitting.

This picture utilizes the fact that any two-state system may viewed as constituting the two components of a “spin”. Looking at this “spin” and its motions then provides an easy visualization, one which has been used in many contexts . That is, if we have two states $`|L>`$ and $`|R>`$, which for us will be the two lowest opposing fluxoid states, then the general state

$$\alpha |L>+\beta |R$$
(1)
has the interpretation of a spin pointing in some direction. Even the relative phase is represented: the numbers $`\alpha `$ and $`\beta `$ are complex numbers and the spin points in different directions when we change their relative phase. Thus the spin visualizastion gives a complete picture of the state (up to an irrelevant overall phase).

To identify $`|L>`$ and $`|R>`$ here, consider (Fig. 1) the familiar double well potential  for the rf SQUID biased with an external flux $`\mathrm{\Phi }_x`$

$$U=U_0[1/2(\mathrm{\Phi }\mathrm{\Phi }_x)^2+\beta _Lcos\mathrm{\Phi }].$$
(2)
The horizontal axis, the “position” coordinate of the present problem, is $`\mathrm{\Phi }`$ the flux in the SQUID ring. Depending on whether the system is in the left or right well, the flux through the ring has a different sign and the current goes around in opposite directions. The potential can be varied by altering the external $`\mathrm{\Phi }_x`$, becoming symmetric for $`\mathrm{\Phi }_x=0`$. We identify the lowest level in each well with $`|L>`$ and $`|R>`$. Quantum mechanical linear combinations of them result from tunneling through the barrier. In the adiabatic inversion procedure to be discussed, the external $`\mathrm{\Phi }_x`$ is swept from a maximum to an minimum value, passing through zero, such that the initially asymmetric left and right wells exchange roles, the originally higher well becoming the lower one and vice versa. The asymmetry of the configurations, however, is kept small so that we effectively have only a two-state system, composed of the lowest state in each well.

Various influences such as the tunneling energy or the external flux may affect the orientation of the spin. Pursuing the analogy, these influences may be thought of as creating a kind of pseudo-magnetic field $`𝐕`$ which causes the spin to precess. Representing the spin by a “polarization” $`𝐏`$ we get the picture of Fig. 2. The equation governing the motion of $`𝐏`$ is

$$\dot{𝐏}=𝐕\times 𝐏D𝐏_{tr},$$
(3)
where $`𝐕`$ can be time dependent. The quantity $`D`$ is the decoherence parameter, which we neglect for the moment and will deal with below. Note that in the absence of $`D`$, according to Eq , $`𝐏`$ cannot change its length, so the density matrix, which $`𝐏`$ parameterizes, retains its degree of purity. In using Eq  one assumes the temperature low enough so that relaxation processes like barrier hoping or jumps between prinicpal levels may be neglected, thus there is damping of only the transverse components, $`𝐏_{tr}`$ (see below).

Now it is a familiar fact under adiabatic conditions, where $`𝐕`$ varies slowly, that the “spin” $`𝐏`$ will tend to “follow” a moving magnetic field $`𝐕(t)`$. This is a completely familiar procedure when rotating the spin of say an atom or a neutron by a magnetic field. If we wish, we can completely invert the state by having $`𝐕`$ swing from “up” to “down”.

In the present problem, we can create a moving $`𝐕`$ by sweeping $`\mathrm{\Phi }_x`$. This is because the vertical component of $`𝐕`$, $`V_{vert}`$ corresponds to the difference in the two lowest energy levels. Hence we can induce a level crossing and reverse the potential wells (see Figs. 3 and 4) by reversing $`\mathrm{\Phi }_x`$ and so the direction of $`V_{vert}`$. For small asymmetry of the wells the splitting is linear in $`\mathrm{\Phi }_x`$. Thus if $`ϵ`$ is the initial level splitting, obtained when $`\mathrm{\Phi }_x=\mathrm{\Phi }_x^{max}`$, we can write $`V_{vert}(t)=ϵ(\mathrm{\Phi }_x(t)/\mathrm{\Phi }_x^{max})`$. As $`\mathrm{\Phi }_x`$ sweeps from its positive maximum value to its negative minimum value, $`V_{vert}`$ reverses direction.

In doing so, $`V_{vert}`$ passes through zero where $`𝐕`$ is horizontal with only a transverse component $`𝐕_{\mathrm{𝐭𝐫}}`$. $`𝐕_{tr}`$ corresponds to the tunneling energy between the two quasi-degenerate states, $`V_{tr}=\omega _{tunnel}`$. As $`V_{vert}`$ passes through zero at $`\mathrm{\Phi }_x=0`$, the $`|L>`$ and $`|R>`$ states are strongly mixed and the splitting of the resulting energy eigenstates is determined by $`V_{tr}`$ alone, as is also familiar in the Landau-Zener picture. The magnitude of $`V(t)`$ at a given time, $`|𝐕|=\sqrt{V_{vert}^2+V_{tr}^2}`$ gives the instantaneous splitting of the two levels. This varies from approximately $`ϵ`$ in the vertical position of $`𝐕`$ to $`\omega _{tunnel}`$ in the horizontal position.

Having identified the components of $`𝐕`$, our next task is to ascertain the meaning of “adiabatic” or “slow” for the motion of $`𝐕`$. Adiabatic conditions obtain when the time variation in question does not contain significant frequencies or fourier components corresponding to the energy splitting between levels. Expressed in terms of time, the rate of variation of $`𝐕`$ should be slow on the time scale corresponding to the tunneling time between the two states. Thus we have the requirement on $`𝐕`$ that its relative rate of variation $`\dot{V}/V`$ always be small compared to $`V`$ itself. Since the varying component of $`𝐕`$ is $`V_{vertical}`$ (neglecting the indirect effect of $`\mathrm{\Phi }_x`$ on $`\omega _{tunnel}`$) we require $`\dot{V}_{vertical}/V<<V`$. Thus taking the near degenerate configuration where $`V\omega _{tunnel}`$ we find

$$ϵ\frac{\dot{\mathrm{\Phi }}_x(t)}{\mathrm{\Phi }_x^{max}}ϵ\omega _{sweep}<<\omega _{tunnel}^2$$
(4)
as the condition for adiabaticity.

If the adiabatic condition is violated then $`𝐏`$ cannot follow $`𝐕`$ (See Fig. 6 below) . We stress that for adiabatic inversion there must be a well-defined quantum phase between the two states, and that when this phase is lost the inversion is suppressed.

In Figs. 3 and 4 we give a schematic representation of the whole procedure. In Fig. 3 a succesful inversion takes place. Starting (upper sketch) with the system in the lowest state since we are at low temperature, a sweep is performed. After the level crossing has been performed (lower sketch ), the system has reversed flux, remaining in the lowest energy state. In the visualization of Fig. 2, $`P_{vert}`$ has reversed direction. This is the behavior to be expected of a quantum mechanical system with well-defined phase relations.

In Fig. 4 we have the same starting situation but the inversion is unsuccessful. The system ends up in the same fluxoid state, $`P_{vert}`$ does not reverse. This is the behavior to be expected classically, when decoherence is significant and there is no well- defined quantum phase between the two states.

More detailed information, as well as intermediate cases will be discussed in terms of the behavior of $`𝐏`$, as shown in Fig. 5 and Fig. 6 below. For this a discussion of the role of damping or decoherence is necessary. This is the topic of the next section.

## III Damping

We now turn to a quantitative discusssion of dissipative or damping effects, those effects tending to destroy the quantum coherence of the system; that is we consider the role of the $`D`$ term in Eq . While the vertical component of $`𝐏`$ characterizes the relative amounts of the two states which are present in a probablistic sense, the quantity $`𝐏_{tr}`$ measures the degree of phase coherence between the two states. $`D`$ gives the rate of loss of this phase coherence.

One could also have included a damping parameter for the vertical component of $`𝐏`$. Instead of the loss of phase coherence, this would represent direct transitions from one well to the other. Such relaxation processes, like jumping the potential barrier due to thermal effects, or “radiative transitions” from one well to another with emission or absorption of some energy can be minimized by low temperatures and fast sweep times, as discussed in the next section.

In the present problem we are in particular interested in the effect of $`D`$ on the inversion process. With an increasing loss of phase coherence, we expect the situation to become more and more “classical” and finally when the $`D`$ is large, for the inversion to be inhibited. Indeed, in solving Eq in the limit of large $`D`$ one finds the inversion is strongly blocked and that one arrives in the “Turing-Watched Pot-Zeno” regime where $`𝐏_{vert}`$ is essentially “frozen” . (See the lower right panels of Figs. 5 and 6).

These general expectations are confirmed by a numerical study  of Eq  with a moving $`𝐕(𝐭)`$. Figs. 5 and 6 show results of the numerical study. The horizontal axis represents the time, running from the beginning to the end of the sweep. The two curves in each picture represent $`𝐏_{vert}`$ (labeled $`P_3`$) and $`𝐏_{trans}`$. $`𝐏_{trans}`$ is represented in absolute value, while $`𝐏_{vert}`$ can change sign. In Fig. 5 an adiabatic sweep is performed. In the first panel, where $`D=0`$, one sees the succesful inversion of $`𝐏_{vert}`$ as it moves from +1 to -1. $`𝐏_{trans}`$ passes through 1 as $`𝐏`$ passes through the horizontal position. In the next panel, where $`D`$ is increased somewhat, to $`0.01`$, the picture is essentially unchanged. In the third panel where $`D=0.2`$, decoherence takes effect since the decoherence time, given by $`1/D`$, is on the order of the sweep time. $`𝐏`$ shrinks to zero during the sweep, showing the loss of phase coherence. Finally, with very large $`D`$, $`𝐏_{vert}`$ evolves hardly at all during the sweep and $`𝐏_{trans}`$ stays at zero. This final case is the “Turing-Watched Pot-Zeno” behavior.

We see three regimes for the result of the sweep: A) the system stays in the original state (classical case), B) goes to the opposite state (quantum case), or C) ends sometimes in one state and sometimes in the other (intermediate case). These correspond to $`P_{vert}`$ starting as +1 and ending as +1, -1, or 0, respectively. Or in terms of Fig. 5, A) corresponds to the last panel (lower right), B) to the first two panels, and C) to the middle panel (lower left).

We stress that all this arises simply from solving Eq  and that no further notions or assumptions are necessary.

In Fig. 6 we show the effects of non-adiabaticity, using a sweep a factor of ten faster than in Fig. 5. Even with $`D=0`$ the inversion is incomplete, with $`𝐏`$ keeping unit length, but ending up rotating roughly in the horizontal plane. As $`D`$ is turned on, $`𝐏`$ shrinks and finally for very large $`D`$ the “Turing- Watched Pot-Zeno” behavior sets in.

Given adiabatic conditions, the important relation is that between the sweep speed and the decoherence time $`1/D`$. As one sees from Fig. 5, there is no effective decoherence until $`1/D`$ is on the order of the sweep time. This relation determines if the system has time to “decohere” during the sweep. Roughly speaking, one enters the classical regime when $`P_{tr}`$, characterizing the phase coherence, has time to shrink during the inversion. This is very interesting for us, since it means, if the experimental situation is favorable, that we can pass from the quantum regime to the classical regime simply by varying the sweep speed.

## IV Parameter Values

We now discuss some some typical parameters of our system. In particular since we envision working at time scales shorter than have been common in this field, it may be useful to give a qualitative discussion of the various time scales involved. The highest frequency or shortest time present is the ordinary harmonic frequency $`\omega _0`$ (Fig. 1) giving the approximate level spacing in the well. For typical conditions this spacing may be on the order of several Kelvin ($`K`$), or some hundred $`GHZ`$. Since we suppose working in the Kelvin to milliKelvin range, this implies that for the equilibrium system at the start of the sweep only the lowest level is populated. The next parameter is the tunneling frequency through the barrier. This is a sensitive function of the SQUID parameters, with sample values \[$`\beta _L=1.19,C=0.1pF,L=400pH,R=5M\mathrm{\Omega }`$\] we have $`\omega _{tunnel}600MHZ`$. This corresponds to $`\omega _{tunnel}/\omega _010^2`$, the tunneling introduces small energy shifts on the scale of the principal level splitting

The next two parameters concern the extent and speed of the sweep. The initial asymmetry $`ϵ`$ (Fig. 1) should be small compared to $`\omega _0`$ in order to retain the approximate two-state character of the system, but large compared to $`\omega _{tunnel}`$ to avoid initial mixing of the two states, say $`ϵ/\omega _010^110^2`$. The speed of the sweep, $`\omega _{sweep}`$ will be the easiest experimental parameter to control, and the behavior of the results as $`\omega _{sweep}`$ is varied will be an important check on the theory. It must not be so fast as to lose adiabaticity, but not so slow as to allow relaxation processes to mask the results. We may suppose it to be in the range $`10^3\omega _010^4\omega _0=10100MHZ`$. With these numbers it seems possible to satisfy the adiabatic condition Eq on the one hand and to sweep fast relative to the relaxation time (see below) on the other.

We now come to the dissipative parameters: $`D`$, and $`\omega _{relax}`$, the relaxation rate for transitions among the SQUID levels. The calculation of dissipative effects in the SQUID is usually approached in terms of the Caldeira- Leggett model , where a coupling to a pseudoboson field, related to the resistance of the device, represents the dissipative effects. The distinction between relaxation and decoherence in the SQUID is principally a question of energy scale. For the former, influences (e.g. the pseudobosons), involving jumps between levels, energies on the order of the level splitting or more are involved. For the latter, where there is only a “dephasing”, low energies, those below the level splitting, are important. In general, of course, both processes are present, but at low enough temperture relaxation should become small. For this reason the damping term in Eq  is taken to only affect the transverse components of $`𝐏`$.

Weiss and Grabert , have given a calculation of the effects of dissipation on coherence, and we may identify their “decay rate” at weak dissipation with $`D`$. This gives the estimate $`D=T/Re^2`$ (their $`\mathrm{\Gamma }`$). For $`R=5M\mathrm{\Omega }`$, we find $`D=0.08mk=9.6MHZ`$ at $`T=100mk`$, and $`D=0.008mk=960kHZ`$ for $`T=10mK`$. (Units: $`1K=8meV=120GHZ`$, $`1/e^2=4k\mathrm{\Omega }`$). With these estimates, say 1-10 MHZ, we are in an interesting range since as mentioned, this offers the interesting possiblity of being able to choose sweep speeds either slow or fast with respect to the decoherence time, while still retaining the adiabatic condition. The resulting switches between classical and quantum behavior would provide persuasive evidence for the correctness of our general picture, and allow the measurement of $`D`$ and its temperature dependence.

Our last parameter is the relaxation rate $`\omega _{relax}`$, characterizing, as said, the rate of conventional kinetic relaxation processes. We wish this to be small for two reasons. One is that relaxation should not take place during the sweep, which would obviously obscure our effects. Secondly, relaxation should also be small during the readout time, otherwise for example, the final configuration of Fig. 4 might turn into that of Fig. 3 before it could be detected.

Here we may use calculations which have been made in connection with the tunneling to the voltage state . The rate one finds depends on the separation of the states in question. If we call $`\omega _{relax}`$ the value with the level seperation at the beginning or end of the sweep we obtain in our example$`20kHZ`$. This characterizes the time in which the readout must occur.

During the sweep itself the level spacing is changing. Taking this into account we obtain the curve of Fig. 7, which shows the probability of an inter-level jump as a function of $`\omega _{sweep}`$. It appears that for sweeps shorter than a microsecond relaxation is indeed negligible.

To indicate the general relationship of the various time scales, the frequencies $`\omega _{relax},\omega _{dec}=1/D`$ and $`\omega _{tunnel}`$ are marked for the horizontal axis. As may be seen, we may indeed be able to obtain the favorable situation of being able to sweep slow or fast relative to the decoherence time, while retaining small relaxation.

Concerning the readout, we have examined a scheme involving a switchable flux linkage to a DC SQUID, which would be sufficiently fast for the above estimates . Here one profits from the fact that observation of the system is only necessary after the procedure is completed.

## V Nonadiabatic Procedures

In general, we need not necessarily limit ourselves to slow, adiabatic processes. There is, say, the opposite case of the “sudden approximation” where $`𝐕`$ is changed very quickly and $`𝐏`$ tends to stays put, as was beginning to happen in Fig. 6. This could be of interest for example, if we find experimentally that we always get an inversion (Fig. 3), and never a failed inversion (Fig. 4) for the range of parameters available to us operationally. There could be two reasons for this behavior. It could be a true result in the sense that the decoherence is very small; we are always in the quantum situation and the adiabatic inversion always works.

But we might worry that instead we have a rapid relaxation from the upper state to the lower one after or during the sweep. That is, perhaps we really had no inversion and Fig. 4 applies. The relaxation rate is greater than we think and the system just falls back to the lowest energy state with the emission of some energy before we can read out.

A way to clarify the situation would be to start our adiabatic inversion procedure from the upper state. Then a succesful inversion means we end in the upper state. If relaxation was not the problem, we should then detect the upper state. On the other hand if relaxation is significant, we should always end in the lower state, regardless of where we start.

Since at low temperature everything is in the lowest state, in order perform this check we need a method of getting the system into the upper state at the start of the sweep. We can accomplish this by a sudden, nonadiabatic, reversal of $`V_{vertical}`$, that is, of the applied flux. Since the wavefunction or $`𝐏`$ will (approximately) not change, we will have the system in the upper state to start with. We now proceed with the adiabatic sweep as before and we can check if the results were due to relaxation or true quantum coherence.

Other interesting configurations and procedures can undoubtedly be arrived at by combining various operations in this way.

## VI qbits and the quantum computer

The two-state system under discussion here suggests itself as a physical embodiment of the “quantum computer”. The “qbit” itself is naturally represented by L and R playing the role of 0 and 1. A linear combination of L and R may be created by adiabatically rotating $`𝐏`$ from some starting position. Adiabatic inversion is evidently an embodiment of NOT since it will turn one linear combination into another one with the weights of L and R interchanged. As for CNOT, the other basic operation, a NOT is performed or not performed on a “target bit” according to the state of a second, “control bit”, which itself does not change its state. One straightforward realization of this would be to perform the NOT operation as just described in the presence of an additional linking flux supplied by a second SQUID nearby. The magnitude and direction of this linking flux would be so arranged that the inversion of the first SQUID is or is not successful depending on the state of the second SQUID. This and many other interesting combinations of junctions and flux linkages, not to mention other devices , may be contemplated and are under study .

SQUID systems like these would seem to be particularly well suited for the embodiment of the quantum computer, where we wish to generate a series of unitary transformations for the various steps of computation. This may be done by creating a “moving landscape” of potential maxima and minima, as in our simplest one-dimensional example of the adiabatic inversion. This imaginary landscape can be produced and manipulated by controlling various external parameters (as with our sweeping flux), performing the various operations in one physical device. Naturally, practicality will depend very much on the relation between the speed of these operations and the decoherence/ relaxation times which we hope to determine by the present methods.

Although our interest here has been the SQUID, it will be evident that the principle of determining decoherence times through the inhibition of adiabatic inversion could be applied to many other types of systems as well.


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# Diffusion-Reorganized Aggregates: Attractors in Diffusion Processes?

## Abstract

A process based on particle evaporation, diffusion and redeposition is applied iteratively to a two-dimensional object of arbitrary shape. The evolution spontaneously transforms the object morphology, converging to branched structures. Independently of initial geometry, the structures found after long time present fractal geometry with a fractal dimension around 1.75. The final morphology, which constantly evolves in time, can be considered as the dynamic attractor of this evaporation-diffusion-redeposition operator. The ensemble of these fractal shapes can be considered to be the dynamical equilibrium geometry of a diffusion controlled self-transformation process.

This letter reports the discovery of a diffusion mediated process which spontaneously builds a dynamic fractal equilibrium structure, in contrast with fractal morphologies linked to far-from-equilibrium processes . The process is a surface to surface evaporation-diffusion-condensation process which conserves the total mass of the system. During the time evolution, one observes a progressive transformation of the surface through bulk diffusion. After a long relaxation period, the system reaches a dynamical fractal structure. This structure appears as the final equilibrium state towards which any initial morphology of $`M`$ particles will converge after sufficient evaporation-diffusion-condensation iterations. It can then be considered as a general statistical attractor for that specific dynamic process.

The underlying ideas that have suggested this study come from our knowledge of the basic mathematical objects which govern the exchange of Laplacian driven currents across irregular (or fractal) interfaces (as, for example, in the study of irregular or fractal electrodes). This problem can be mapped onto the study of the transfer of Brownian particles across irregular membranes with finite permeability . In this process, Brownian particles strike an irregular surface where they are absorbed with finite probability. When reflected, the particles undergo successive random paths, hitting and hitting again the static surface, until they are finally absorbed. Halsey first indicated that the response of such systems depends on the probability that a particle starting on the interface comes back to it . Generalizing these ideas, it has been recently shown that the Laplacian transfer across irregular interfaces is controlled by a single linear operator $`\stackrel{~}{Q}`$ which maps the static surface onto itself through effective ”Brownian bridges” . In this context, each surface has an operator $`\stackrel{~}{Q},`$ which is symmetric and positive.

The question arises naturally of the link between the Brownian bridges and a real diffusion process. This led us to study a dynamical process in which the notion of a $`\stackrel{~}{Q}`$ operator, which maps the surface onto itself through average diffusion, is transformed into a real operation which transforms the surface through discretized diffusion . The evolution mechanism then proceeds in the following steps (Fig. 1):

1. A particle is chosen at random on the surface of an initial structure and is dissolved, occupying an empty site next to its initial position.
2. The dissolved particle may jump back to its original site or start a Brownian random walk on a square lattice which represents the outer medium. The time step for each jump is $`\tau =1.`$ This motion is stopped when the particle hits the structure again as it sticks on first hit .
3. The process, which conserves the total mass, is then iterated. For practical reasons, the system is enclosed in a large square window: whenever a diffusing particle strikes the window boundary, this particle is reinitiated on another site of this external box, following a probability law that simulates the random walk in the infinite outer medium. As the probability to return to a starting site is equal to 1 in $`d=2`$, this does not modify the morphologies which are generated by the process. The existence of the external box only perturbs the time scale so that the number of computer steps is not proportional to a real time. For this reason, the number of steps will be called pseudo-time $`t`$.

The dissolution-recondensation process rapidly creates several branches. If particles of these branches were allowed to dissolve, it would lead to a progressive splitting of the structure into two, then many, disconnected parts. In order to avoid this progressive disconnection, one imposes the structure to remain connected throughout the process. The only particles allowed to evaporate are then the particles pertaining to the surface of the structure and that are not “red particles”: the red particles are defined as the particles which, if eliminated, would disconnect the structure in two or more distincts parts. The particles allowed to evaporate are therefore called “blue particles”. We also impose that an evaporated particle cannot stick on a site where it would disconnect the outer medium. In fact, one could release this last constraint since it does not modify the long term evolution of the structure. It simply avoids to create temporary “lakes” in which particles evaporating and redeposited would greatly reduce the speed of evolution of the structure. Particles on the internal surface of these lakes would spend most of the time to go back and forth until the lake opens spontaneously.

The results of the spontaneous evolution of structures obtained with different initial morphologies are shown in Fig. 2. The left column shows the initial shape and the corresponding final morphologies are shown on the right. In case (a), the initial morphology is a compact dense structure described by a dimensionality equal to 2. In case (b), the starting shape is a line with dimensionality 1. Finally, in case (c), the initial morphology is an ordinary Diffusion-Limited Aggregate (DLA), first introduced by Witten and Sander .

In all three cases (a), (b) and (c), the final morphologies present branched structures, like DLA but less open. The complete statistical study of the morphologies is difficult because the process is very time consuming in the computer. For instance, the time necessary to reach the morphology shown in Fig. 2(a) is of the order of several weeks of CPU time on a Hewlett-Packard C160 workstation. The similarity in the final shapes, independent of initial geometry, suggests that this class of morphologies is an attractor for such self-reorganization processes. We call these structures “Diffusion-Reorganized Aggregates” (or “DRA”).

The fact that morphologies are “attracted” by the fractal final form is also indicated in Fig. 3. The figure gives the determination of the fractal dimension of the final morphologies starting respectively with initial dimension $`D_f=2`$, $`D_f=1`$, and $`D_f=1.65`$ (Fig. 2 (a), (b) and (c)). Although the initial dimension are very different, the final plots are within reasonable uncertainty concentrated and compatible with $`D_f=1.740\pm 0.02`$, a value which is significantly different from the fractal dimension of lattice animals  and compatible with that of the branched structures which are the results of a far-from-equilibrium process .

The dynamics of the restructuration process has several specific properties. To follow the dynamics, one can compute two memory functions. First, a density-density memory function. For this purpose, the structure is characterized by a number $`s_i`$ on each site $`i`$ of the lattice, with $`s_i=1`$ if the site is occupied by the structure and $`0`$ if not. Calling $`M`$ the mass of the initial structure, which is equal to the number of occupied sites, this memory function can be defined as:

$$C(t)=\frac{1}{M}\underset{\mathrm{lattice}\mathrm{sites}i}{}s_i(0)s_i(t)$$
(1)
This first function does not discriminate between particles as $`s_i(0)s_i(t)`$ is equal to 1 if a lattice site $`i`$ is occupied both at pseudo-times $`0`$ and $`t`$ (by any particle) and 0 otherwise. The pseudo-time evolution of $`C(t)`$ is shown in Fig. 4. One observes a memory loss which does not go to zero. There can be two reasons for incomplete decorrelation. First, it could happen that a part of the object is not restructured. Second, it could be that the density-density memory does not vanish due to an average statistical overlap, even if the structure has completely forgotten its initial geometry. To clarify this point, one can compute a particle-particle memory function which characterizes the speed at which the particles of a given structure finally move from their initial positions. This second function is

$$P(t)=\frac{1}{M}\underset{particlesj}{}\delta (\stackrel{}{r_j}(0)\stackrel{}{r_j}(t))$$
(2)
where $`\stackrel{}{r_j}(t)`$ is the position of the particle $`j`$ at time $`t`$.

The evolution of $`P(t)`$ is also given in Fig. 4. One observes that the particle-particle memory is lost to zero very rapidly. When it has reached very small values, one can say that the structure has completely lost the memory of its microscopic configuration. Apart from these two rapid processes, one observes in Fig. 4 the very slow global evolution. Note that the DRA geometry loses constantly its memory whereas the DLA growth keeps the total memory of its previous structure.

A more detailed characterization of the rapid regimes is displayed in Fig. 5, where the decorrelations are found to be exponential, a non-usual time behavior in this context.

Those results, together with the fractality evolution of Fig. 3, indicate that the final DRA morphologies behave as stable fixed points. The constantly changing DRA can then be viewed as a statistical equilibrium state. In that sense, it is analogous to the homogeneous state of an ideal gas, where the microscopic interactions between particles lead to a statistical macroscopic equilibrium, although it is constantly changing its microscopical structure.

One should also note that the transformation of the $`\stackrel{~}{Q}`$ operator, which maps the surface onto itself through average diffusion, into a real operation is analogous to the dielectric breakdown model of DLA . In the DBM model, the operator, that maps the source at infinity onto the growing morphology through average Brownian paths, is transformed into a real stochastic operation. In the model presented herein, the source is the object itself.

It is also interesting to return to the exact concept of the self-transport operator attached to a given morphology . Extending the notion of diffusive self-transport in this context, it might be that DRA shapes could be considered as ”eigenshapes” of these operators. By this, it is suggested here that the self-transport operators attached to these structures transform those structures into themselves, of course in a statistical sense.

All these results should be confirmed in the future through extensive numerical simulations and extension to diffusive self-transport in $`d=3`$. Some future extensions of this work can be envisaged. First, one should verify the universal character of this result. Second, if surface energy was included, it would be interesting to study how the equilibrium morphology would depend on its value. Last, one should study whether the self-transport operators $`\stackrel{~}{Q}`$ of these geometries possess some extremal properties.

In summary, it has been shown that diffusive self-transport statistically modifies an object morphology in an irreversible manner. This irreversible process leads to a class of branched structures, called DRA, with fractal dimension around 1.75. This class of structures plays the role of a statistical attractor. Moreover, its attraction basin seems to be the whole configuration space in the sense that, independent of the initial geometry of the system, the dissolution-redeposition process always tends to create the same category of geometries. The fractal DRA can be seen as a statistical equilibrium for this process, which would maximize a “geometrical entropy” still to be defined.

The authors wish to acknowledge useful discussions with B. Mandelbrot. The Laboratoire de Physique de la Matière Condensée is a “Unité Mixte de Recherches du Centre National de la Recherche Scientifique No. 7643”. This work has been partially supported from the European Network - Fractals, under contract no FMRX-CT98-0183.


text:
# Vortices in 𝑆𝑈(2) lattice gauge theory

## Abstract

We investigate some properties of thick vortices and thick monopoles in the $`SU(2)`$ lattice gauge theory by inserting operators that create these excitations. We measure the derivative of the free energy of the vortex with respect to the coupling and we find that it falls exponentially with the cross sectional area of the vortex. We also study the monopole-monopole potential energy of thick and thin monopoles. Our results suggest that vortices and monopoles of increasing thickness will play an important role in the large $`\beta `$ limit.

Vortices as a mechanism for quark confinement have attracted enormous interest in recent times. In non-abelian gauge theories, center vortices can be defined as multiple valued gauge transformations. Furthermore, it has been conjectured that center vortices can condense and produce quark confinement . Vortices can be introduced by applying twisted boundary conditions (in the spatial direction) . On the lattice, the twist translates to flipping the signs of a stack of plaquettes in a particular spatial direction, the same twist repeating at every time slice. Applying this twist corresponds to inserting a center vortex into the system. Recent work in  studied the free energy of a vortex, whereas the authors in  have constructed a vortex disorder operator and measured its expectation value. Vortices have also been studied in the center projection approach .

When one tries to define vortex like configurations on the lattice one is led to a distinction between thin and thick vortices . Thick vortices are configurations having $`sign(trU(p))=+1`$ everywhere but which nevertheless flip signs of Wilson loops linking them. Thin vortices, on the other hand, are configurations of co-closed sets of plaquettes with $`sign(trU(p))=1`$ and are defined at the scale of the lattice spacing. The two configurations are not only quite different, but also have different properties. It is a dynamical issue whether one is more important than the other. In this discussion we study some properties of thick vortices and thick monopoles by generalizing the idea of a twist.

We introduce a term in the partition function that creates a stress in the system and we study the effect of this stress on the system. More specifically, we add a term to the Wilson action

$$S^{}=\frac{\beta }{2}\underset{p}{}trU(p)\frac{\beta }{2}\underset{p^{}}{}trU(d).$$
(1)
The extra term is a Wilson loop variable defined over a square of side $`d`$ and it comes with a negative sign. This term is introduced at a point in the (say) $`(12)`$ plane, and it extends in the $`3`$ direction, and the term repeats itself in the $`4`$ direction. The effect of the extra term is to drive the system such that $`trU(d)`$ is negative, the effect of the usual Wilson action being to drive the system such that $`trU(p)`$ is positive. The stress that we are introducing into the system is nothing but a thick vortex of thickness $`d`$ piercing a region in the $`(12)`$ plane and wrapping around the lattice in $`3`$ direction. On the other hand, if the stress begins at a point, say $`z=z1`$, and terminates at, say $`z=z2`$, we are inserting a thick monopole-antimonopole pair joined together by a thick vortex line. We want to measure the system free energy cost for introducing these stresses. The case $`d=1`$ has been studied before , but we will be interested in the free energy cost as a function of $`d`$. Since direct free energy measurements are quite difficult we appeal to a simpler method to determine the effect of this stress ( the same idea is used in ). We first write

$$\mu _d=\frac{Z(\beta ^{})}{Z(\beta )}=\mathrm{exp}(F_dF_o).$$
(2)
$`Z(\beta ^{})`$ is the partition function of the system after applying the stress and $`Z(\beta )`$ is the partition function without the stress. $`F_dF_0`$ measures the free energy difference when an additional thick vortex (having a thickness $`d`$) is introduced into the original system (which may already contain thick vortices). Hence the effect of a large number of interacting vortices is already subsumed in this free energy difference. It is not difficult to see that $`\frac{\mathrm{log}\mu _d}{\beta }`$ is

$`{\displaystyle \frac{1}{\mu _d}}{\displaystyle \frac{\mu _d}{\beta }}=<{\displaystyle \frac{1}{2}}{\displaystyle \underset{p}{}}trU(p){\displaystyle \frac{1}{2}}{\displaystyle \underset{p^{}}{}}trU(d)>_1`$ (3)
$`<{\displaystyle \frac{1}{2}}{\displaystyle \underset{p}{}}trU(p)>_0.`$
The subscript $`1`$ indicates that the average is taken with respect to the stressed partition function, whereas the subscript $`0`$ indicates that the average is taken with respect to the unstressed partition function. This quantity directly measures the derivative of the free energy difference because

$$\frac{\mathrm{log}\mu _d}{\beta }=\frac{(F_dF_0)}{\beta }.$$
(4)
Fig. 1 shows $`\frac{log\mu _d}{\beta }`$ as a function of the area of the thickness of the vortex. There is an exponential fall-off with respect to the area of the vortex. A logarithm of the curve plotted vs the area of the vortex gives an approximately good straight line fit. The simulations were done on a lattice whose spatial extent was $`10X10`$ and the remaining size was $`6X6`$. Vortices of thickness ranging from $`1`$ to $`5`$ were studied, and in order to avoid finite size effects associated with these vortices the lattices were chosen to have a spatial extent of atleast twice the largest vortex size. The other parameters of the lattice were fixed by some limitations in the computer time. 300,000 data points were gathered at each point and the errors were estimated by binning.

We wish to point out that though our result is for the derivative of the free energy of the vortex area as a function of the coupling, the free energy of the vortex will also fall-off exponentially with the area ( this is very easy to show in the strong coupling limit). This result has two immediate implications. It indicates that as we approach the weak coupling limit ($`\beta \mathrm{}`$), vortices of larger and larger area are more favourable than vortices of any fixed area. By spreading the core of the vortex over a large area, the energy of the vortex loops can be made arbitrarily (exponentially) small. It also means that in the region of the continuum limit we must be able to tackle a many body vortex problem in which vortices can have large overlaps with each other. This feature seems to make the study of such vortex gases quite difficult. However, from the point of view of the continuum limit, very large vortices are almost necessary; if lattice vortices are to survive as continuum excitations they must appear with a length scale which diverges in lattice units as the lattice spacing goes to zero. Only then can they yield a vortex corresponding to some physical thickness. Thick vortices indeed admit this possibility by appearing with arbitrarily large thicknesses.

We now turn to thick monopoles. As mentioned earlier, if the stress is taken to extend only between two points, say $`z=z1`$ and $`z=z2`$, it corresponds to an external thick monopole-monopole loop running along the $`4`$ direction at $`z=z1`$ and $`z=z2`$ and separated by a thick vortex sheet between $`z=z1`$ and $`z=z2`$.

Fig. 2 shows the potential energy of a monopole-monopole pair for monopoles of thickness $`d=1`$ at $`\beta =1.0`$ and $`\beta =2.4`$. The approximately linear rise at $`\beta =2.4`$ shows that their separation energy directly increases with the separation distance. By contrast, the curve for $`\beta =1.0`$ is quite flat. At $`\beta =2.4`$, the thin monopoles have become very rare and the screening mechanism between an external monopole-monopole pair is inoperative and their interaction energy is directly proportional to the length of vortex line joining them. On the other hand, at $`\beta =1.0`$, when the monopole density is quite large, the energy of the external pair does not increase linearly with their separation because of the screening effect of the large number of monopoles in the system. A similar measurement for thick monopoles shows very different behaviour. Fig. 3 shows the monopole-monopole potential energy for a thick monopole of thickness $`d=3`$. At $`\beta =2.4`$ the thick monopole-monopole potential energy curve is quite flat. This can again be understood from the presence of a large number of thick monopoles ($`d=3`$) in the system. At larger values of $`\beta `$, for example $`\beta =4.0`$, the thick monopoles also show a screening behaviour. The main difference between Fig. 2 and Fig. 3 is the signs of the slopes of the curves in the two plots. The slope of the curve is the negative of the derivative of the free energy of the monopole pair with respect to the coupling. While the first plot (with negative slope) shows a linear rise with the separation distance in the interaction energy of a thin monopole-monopole pair at $`\beta =2.4`$, the second plot ($`\beta =4.0`$) shows a decrease (with positive slope) in the interaction. This different behaviour of monopoles of finite thickness compared with monopoles of unit thickness again shows that the self- energy of thick monopoles has a more subtle behaviour than that of the thin monopoles. An appealing explanation of this difference is that thick monopoles tend to repel each other (like similarly charged particles) and lower their potential energy. This should be contrasted with the behaviour of thin monopoles which tend to be bound into monopole-monopole pairs as a result of the energy of the string joining them. The data in Fig. 2 and Fig. 3 were taken on a $`6^4`$ lattice after 50000 iterations.

It is also interesting, and important, to see how these thick objects scale as we decrease the lattice spacing. We expect that as the lattice spacing is reduced, objects that were thick on the larger lattice become thin on the smaller lattice. The time constant of the exponential in Figs. 1 should also scale in the large $`\beta `$ limit. These issues are being currently studied.

Acknowledgement: This work was supported in part by United States Department of Energy grant DE-FG 05-91 ER 40617.


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# Magnetic relaxation phenomena and cluster glass properties of La0.7-xYxCa0.3MnO3 manganites

## I Introduction

Extensive study of the doped perovskite manganites La1-yCayMnO3 revealed a very rich and complex phase diagram, which includes colossal magnetoresistance (CMR) behavior near the transition temperature of the metallic ferromagnetic compositions, 0.15$`<`$y$`<`$0.50. The ferromagnetic (FM) interaction appears as a consequence of the manganese mixed valence state. Substitution of La3+ by Ca2+ in antiferromagnetic LaMnO3 changes the Mn3+/Mn4+ ratio and produces holes in the eg orbitals. The simultaneous para-ferromagnetic and metal-insulator transitions are basically understood within the framework of the double-exchange theory , which considers the transfer of one eg electron between neighboring Mn3+ and Mn4+ ions through the path Mn-O-Mn.

For a given eg concentration the tolerance factor of the perovskite structure, proportional to the average ionic size of the A site, was shown to have a drastic influence on the physical properties of manganites. Compounds of the type (La0.7-xRx)Ca0.3MnO3 (R = Pr, Y, Dy, or Tb), where the Ca concentration is close to an optimum value in relation to the FM interaction, are particularly suited to investigate this effect: replacing La3+ with smaller rare-earth ions decreases the Mn-O-Mn bond angle, and thus affects the hopping of the eg electrons and weakens the double-exchange interaction, while the antiferromagnetic superexchange term is only marginally affected and therefore increase in importance. Consequently, both double exchange and superexchange interactions will compete more strongly depending on the structural distortion, giving rise to a magnetically disordered state. A magnetic and electronic phase diagram of several manganite systems plotted against the tolerance factor has been published on several investigations. Lowering the value of the average ionic size of the A site initially reduces the transition temperature TC, and below a critical value the low temperature phase changes to a spin-glass insulating state. Preliminary studies have additionally shown that the FM metallic phase of La0.7-xYxCa0.3MnO3 (x = 0.15) display signatures of a magnetic cluster glass state.

The purpose of the present work is to investigate the dynamic properties of this disordered phase by means of magnetic relaxation measurements. One characteristic feature of glassy systems is that the magnetization of a sample cooled in zero field to a certain temperature depends on how long it is held in zero field before the magnetic field is applied. This is the so called aging effect. Furthermore, if M(t) is differentiated with respect to lnt, the derivative S = $``$M/$``$(lnt) displays a maximum which shifts to higher t for longer values of the wait time, tw. These effects have been observed on a well characterized cluster glass compound, the cobaltite La0.5Sr0.5CoO3, where glassy behavior and intracluster ferromagnetism were shown to coexist. More recently, on Nd0.7Sr0.3MnO3, it was shown that disorder and frustration may occur in the ferromagnetic phase.

Within this context, this paper presents low temperature magnetic relaxation measurements on La0.7-xYxCa0.3MnO3, with 0 $``$ x $``$ 0.15. As yttrium is added in the compound, the results evidence for the first time the gradual appearance of glassy signatures within the ferromagnetic metallic phase, prior to the existence of the insulating spin glass phase which occurs with higher rare-earth doping at the La site. Relaxation measurements probe the out-of-equilibrium state of the system, where the clear observation of a peak in the magnetic relaxation as a function of temperature and the observation of aging effects further characterize the cluster glass properties of this system.

## II Experimental

The investigated compounds are polycrystalline samples of La0.7-xYxCa0.3MnO3, with x = 0, 0.07, 0.10 and 0.15, prepared by standard solid state reaction. X-ray analysis confirmed a single phase orthorhombic perovskite structure. Magnetic measurements were made with an extraction magnetometer (Quantum Design PPMS) when the applied field was greater then 5 mT. Low field data, H = 0.3 mT, was taken with a SQUID magnetometer (Quantum Design MPMS). Zero field cooled relaxation measurements were performed on all samples at different temperatures between 10K and 250 K, and for applied fields varying from 5mT to 0.5T. The samples were cooled from a reference temperature in the paramagnetic state with a constant cooling rate, and kept at a target temperature for a certain wait time tw. Thereafter, a dc field was applied and the magnetization was recorded vs. the elapsed time, t. The samples were additionally characterized by transport measurements, made by a conventional ac four-probe method. The results are shown on Fig. 1. All samples display a metal-insulator transition, below which a metallic-like electrical conductivity is observed. A similar behavior was previously reported for these compounds.

## III Results and Discussion

To recall the characteristic magnetic behavior of La0.7-xYxCa0.3MnO3 compounds, Fig. 2 displays the zero field cooled (ZFC) and field cooled (FC) temperature dependence of the dc magnetization of the samples x = 0, 0.07, 0.10 and 0.15, measured at H =5 mT. The small hump visible at low temperatures in most of the FC data is due to a problem in the experimental apparatus. The results of Fig. 2 clearly show a standard FM transition for the x = 0 sample at TC = 252 K, as observed on numerous investigations. For the doped compounds (x $`>`$ 0) the ZFC curves evolve continuously, with higher yttrium concentration, to a cusp-like anomaly at a temperature Ta just below the Curie-like temperature TC, defined as the maximum inflection of the FC data. The TC values obtained are 143, 114, and 89 K, for x = 0.07, 0.10, and 0.15 respectively. An important point to be noted here is that the FC magnetization continues to increase strongly below the irreversibility temperature, Tr, at which ZFC and FC curves merge, a typical feature of various cluster glass systems. This effect is more pronounced on the x = 0.15 sample. On the other hand, in canonical spin glass systems the FC magnetization shows a nearly constant value below Tr. It worth noting that due to the fact that cluster glasses exhibit finite range ferromagnetic ordering below TC, this system may show some features similar to those found in reentrant spin glass systems (RSG), which undergo a PM-FM transition at TC and have a lower freezing temperature. Nevertheless, it may be noted that in several RSG systems, such as NiMn, AuFe, and FeZr, the irreversibility temperature Tr occurs at temperatures well below TC (when the measuring field is higher then the coercive field), whereas in a cluster glass the irreversibility arises just below TC, as observed in Fig. 2 for the yttrium doped samples.

On the other hand, magnetization curves measured as a function of field, M(H), do show signatures of a RSG behavior. The low field portion of a typical hysteresis loop measured after ZFC condition at 2.0 K, a temperature well below Tr, is shown in the inset of Fig. 3. The curve displays an S shape in the virgin branch, with a positive curvature at low fields, a typical characteristic of both canonical SG and RSG systems. In the same way, the variation of the coercive field HC with temperature, plotted in Fig. 3, is quite similar to those usually observed in RSG systems, where HC increases rapidly as the temperature is lowered below TC.  Such conflicting results evidence a more complex glassy behavior in these compounds.

Susceptibility measurements are a very efficient way to evidence glassy behavior. The temperature dependence of the ac susceptibility of La0.55Y0.15Ca0.3MnO3 is presented on Fig. 4. The variation with temperature of the in-phase susceptibility $`\chi `$’, shown on the inset of the figure, is comparable to that of the dc MZFC, with an onset around 120K related to the paramagnetic to ferromagnetic transition, followed by a maximum at T = 79 K, close to the MZFC cusp temperature Ta = 72 K. This maximum is not frequency dependent, which suggests that the FM state originates from intracluster ferromagnetism. Moreover, if the $`\chi `$’ maximum and Ta are related, the cusp on the MZFC curve is the dc signature of these FM interactions, rather than a consequence of cluster freezing. The out-of-phase susceptibility $`\chi `$” also shows a maximum at T = 87 K, which is frequency independent. It has been suggested that the temperature at which this maximum occurs is related to the irreversibility temperature, Tr = 88 K, obtained on the dc magnetization curves. Therefore the maximum in $`\chi `$” at higher temperatures is also related the intracluster FM interactions. However, an additional feature clearly visible in $`\chi `$” is the presence of a hump, at Tf $``$40K. This broad peak is frequency dependent and shifts towards higher temperatures with increasing frequency, a characteristic feature of the dynamics of spin glass systems. A similar behavior has previously been reported in other manganite samples. This double peak structure in $`\chi `$” is progressively less visible for lower Y doping, and it is not present in the Y=0 sample.

In order to gain further information on the underlying nature of this cluster glass system, we have measured the long time relaxation of the magnetization, with a time scale greater then 104 s. Figure 5a displays the normalized M(t)/M(0) data for all samples measured at a reduced temperature T/TC = 0.2, with H = 5 mT (this probing field is within the linear response regime). As Y is added in the compounds the data show a gradual increase of M(t)/M(0), at any given time. Quantitatively, after 104 seconds, the fractional change of the magnetization is 0.18, 0.93, 4.5, and 12% in the samples with x = 0, 0.07, 0.10, and 0.15 respectively. Relaxation data at different temperatures for La0.55Y0.15Ca0.3MnO3 are shown in Fig 5b. The slope of M(t)/M(0) increases below TC, reaches a maximum at T/TC $``$ 0.4, and decreases for lower temperatures. This evolution of the magnetization relaxation behavior with temperature is indicative of the development of the magnetic clusters as temperature is lowered. It is noteworthy that relaxation is observed not only below the freezing temperature Tf, but also up to the FM transition temperature TC, which indicates that the system is not in a true ferromagnetic state. This is reinforced with measurements of M(H) above and below TC (not shown), where Arrot plots M2 vs. H/M do not yield straight lines. Previous observations in RSG system also show that relaxation is present above the freezing temperature of the spin glass state.

Amongst the various functional forms that have been proposed to describe magnetization as a function of time, one of the most popular is a stretched exponential of the form :

$$M(t)=M_0M_r\mathrm{exp}\left[\left(\frac{t}{\tau _r}\right)^{1n}\right]$$
(1)
where M0 relates to an intrinsic FM component, and Mr to a glassy component mainly contributing to the relaxation effects observed. The time constant $`\tau _r`$ and the parameter n are related to the relaxation rate of the spin-glass like phase. The values of n are scattered between 0.48 and 0.6, in agreement with previous results. The variations of M0 and Mr with reduced temperature are shown on Fig. 6 for the samples with x = 0.10 and 0.15. As expected, M0 and Mr depend strongly upon temperature. The dependence of M0 with T/TC evidence the FM transition at T/TC $``$ 1. As observed on the temperature dependence of MZFC, the FM component first reaches a maximum at T/TC $``$ 0.8 that corresponds to Ta (MZFC cusp temperature) and decreases further with decreasing the temperature. The FM component M0 is larger for x = 0.10 compared to x = 0.15, in agreement with its stronger FM behavior. The variation of Mr with T/TC shows that for x = 0.15 the relaxing component first increases from T/TC $``$ 1 to T/TC $``$ 0.45, as a consequence either of an increase of the clusters number or of the growth of the clusters size, and decreases for T/TC $`<`$0.45. The resulting maximum in Mr coincides with the temperature of the frequency dependent lower maximum in the out-of-phase susceptibility, which supports the idea that it is related to the beginning of cluster freezing. A similar behavior is observed for x = 0.10, but at a lower temperature, with the maximum in Mr occurring around T/TC $``$ 0.20. The relaxing component Mr in x = 0.10 sample is also much lower than in x = 0.15, due to a less pronounced glassy behavior. The relaxation time $`\tau _r`$ is extremely sensitive to any noise in the data. However, our fitting (not shown) indicate that $`\tau _r`$ increases with decreasing temperature for both x = 0.15 and x = 0.10 , suggesting a regular stiffening of the spin relaxation, which is compatible with an increase of the clusters size and enhanced intercluster frustration.

To further investigate the dynamic magnetic behavior of these metallic glass compounds the wait time tw dependence of the long time relaxed magnetization, or aging effect, was studied. The results were obtained with a small dc field, H = 0.3 mT. Additional measurements (not shown) as a function of the applied field revealed that the magnitude of aging effect is reduced when the field increased, and totally disappears at H = 10 mT. Magnetization vs. time was measured with wait times tw = 100, 1000, and 10000 s, before application of the magnetic field. Results for the x = 0.10 sample, measured at T/TC = 0.2, are plotted in Fig. 7a. This temperature was chosen because it corresponds to the maximum in the relaxing component Mr. It is clear from the figure that the measured magnetization strongly depends on tw, which confirms the existence of aging processes. Macroscopically, aging means that the system becomes “stiffer” for larger wait time, i.e., the measured magnetization is lower for higher tw, as observed in the data. The corresponding time dependent relaxation rate, S(t) = $``$M/$``$(lnt), is plotted in Fig. 7b. The S(t) curves were obtained by taking the derivative of a polynomial fit of the magnetization data. It is readily observed that S(t) reaches a maximum, corresponding to an inflection point on the M(t)/M(0) curves, that shifts to longer observation times for longer values of tw. These results are similar to those reported for various glassy systems.  It may be pointed out that the maximum in S(t) is not centered on tw as expected. However, it is believed that this is related to the additional time required for stabilizing the temperature and the magnetic field applied.

For La0.55Y0.15Ca0.3MnO3, S(t) has been calculated at various temperatures, and the results are shown in Fig. 8. Aging effects are observed at T/TC = 0.2, 0.4 and 0.6. The wait time dependence of the peak in S(t) clearly increases with temperature. Aging effects are more pronounced at higher temperatures, i.e., when the FM state is stronger, as reported previously for La0.5Sr0.5CoO3 or for the two-dimensional ferromagnet Rb2Cu0.89Co0.11F4.  This may be explained by a more steady cluster growth in the FM phase. Larger clusters give rise to a slower response due to larger free-energy barriers and, correspondingly, a larger number of spins to be simultaneously flipped; the smaller the cluster, the more rapidly it will relax. At T/TC = 0.2 on the contrary, the relaxation is slow (Fig. 6b) and the aging effect small, because the regular cluster growth with decreasing temperature lead eventually to a blocking of the clusters at Tf and below. It may also be noted in the data that the maximum in S(t) occurs at higher observation times for lower temperatures. This effect is mostly experimental in origin at low tw (102 seconds), because tw is of the same order of the time it takes to reach the measuring temperature, which effectively increases the wait time at low temperatures. However, at high tw (104 seconds), the wait time is much higher than the time for temperature stabilization, and the shift in the maximum of S(t) with temperature may be associated with the slower response time of the clusters at low temperatures. It is worth mentioning that the measuring field of 0.3 mT may not be in the linear regime, which could affect these results. However, larger fields, outside the linear regime, mostly change the intensity but not the position of the maximum in S(t).

## IV Conclusions

The peak observed in the temperature dependence of the relaxing component of the magnetization, Mr, or equivalently a maximum in the slope of M(t)/M(0) at a given temperature (Fig. 5b), combined with the aging effects observed for La0.55Y0.15Ca0.3MnO3, and, to a lesser extend for La0.6Y0.10Ca0.3MnO3, evidence the importance of magnetic frustration in these samples and establish the existence of cluster glass properties over a broad temperature range. The enhanced lattice distortion resulting from the presence of cationic size mismatch on the perovskite A-site weakens the Mn3+-O-Mn4+ FM double-exchange interactions and favors frustration between the ferromagnetic and antiferromagnetic superexchange interactions. This competition is sufficient to suppress long range FM order, giving rise to the appearance of spatially confined ferromagnetic clusters, which in turn are responsible for the observed glassy behavior of the system due to frustrated interaction amongst their magnetic moments. It is important to stress out that the observed cluster glass behavior occurs within the metallic phase, as opposed to the standard spin glass phase of the manganites, which occurs in the insulating phase. From the behavior of Mr, it is inferred that clusters start to form just below the FM transition TC. As the temperature is lowered, the size and/or number of these magnetic clusters increase, leading to a maximum in the relaxing component of the magnetization. The slower (weaker) relaxation at lower temperatures can be attributed to the freezing of the clusters, similar to the blocking of the magnetic moments in a superparamagnet, due to an enhanced intercluster frustration resulting from oversized domains.

The overall relaxation results presented here demonstrate the existence of a magnetic glassy behavior within the metallic phase, which plays an important role in the physics of these compounds. An important issue which remains to be verified is whether the observed cluster glass properties in La0.7-xYxCa0.3MnO3 develop uniformly distributed due to disorder or enhanced canting within the FM phase, or possibly due to phase separated spin glass regions in a FM background. It is also worth noting that M vs. H measurements are similar to that obtained in RSG systems, indicating the existence of more complex frustration effects and disorder in this system. Within the phase segregation scenario, it is possible that the FM clusters and the FM background give rise to different glassy behavior.

## V Acknowledgments

We thank F. Wolff and P. Pureur for assistance with the SQUID measurements, and M.A. Gusmão for helpful discussions. This work was partially financed under the contract PRONEX/FINEP/CNPq no 41.96.0907.00. Additional support was given by FUJB. The sample preparation was funded by the UK-EPSRC.

* Corresponding author; e-mail: freitas@if.ufrj.br

Figure 1 - Temperature dependence of the resistivity of the studied compounds.

Figure 2 - Field-cooled (solid lines) and zero-field-cooled (dotted lines) dc magnetization of La0.7-xYxCa0.3MnO3, measured with 5 mT.

Figure 3 - Temperature dependence of the coercive field, HC, obtained from M(H) measurements after the application of H = 9 T. The inset shows the low field portion of the M(H) measurements taken at 2.0 K. The lines are only guide to the eyes.

Figure 4 - Out-of-phase susceptibility ($`\chi `$”) of La0.55Y0.15Ca0.3MnO3, measured with an ac field hac = 0.5 mT and frequencies f = 90 (circles), 250 (squares), 700 (triangles), and 2000 Hz ( diamonds). The position of a frequency dependent feature in the data is indicated by Tf. The inset shows the in-phase susceptibility ($`\chi `$’) of the same sample.

Figure 5 - (a) Normalized zero field cooled magnetization of La0.7-xYxCa0.3MnO3 measured as a function of time, with H = 5 mT at a reduced temperature T/TC = 0.2; (b) The same measurement for La0.55Y0.15Ca0.3MnO3, at T/TC = 0.1, 0.4, and 0.8.

Figure 6 - Evolution of the fitting parameters M0 and Mr (see text for details) as a function of a reduced temperature T/TC, for x = 0.10 and 0.15 samples.

Figure 7 - (a) Zero field cooled relaxation magnetization, and (b) the corresponding relaxation rate S(t) = $``$M/$``$lnt, of La0.60Y0.10Ca0.3MnO3, measured at T/TC = 0.2 with H = 0.3 mT, after different wait times tw = 102, 103, and 104 s.

Figure 8 -Relaxation rate S(t) = $``$M/$``$lnt of La0.55Y0.15Ca0.3MnO3 measured after different wait times tw = 102 (open circles) and 104 (solid circles) at T/TC = 0.2, 0.4, 0.6. The arrows indicate the peak position of each data curve.