# Magnetic history dependence of metastable states in systems with dipolar interactions.

## I Introduction

The magnetic and transport properties of thin films and nanostructured materials have been the subject of intense research during at least the last two past decades because of their interest for magnetic recording and technological applications . Among the interesting phenomena observed in this kind of materials there are the reorientation transitions of the magnetization with increasing temperature  or film thickness , the giant magnetoresistance effect , and the wide variety of magnetic patterns that can be stabilized depending on the interplay between the perpendicular induced surface anisotropy, the exchange interaction and the long-range dipolar forces between the microscopic entities.

The development of different microscopy techniques like MFM, AFM, LEM or SEMPA  have helped experimentalists to understand the interplay between the transport properties and the magnetic structure of the materials. Moreover, these techniques have shown that the magnetic structures formed in thin films are strongly influenced by the magnetic history of the sample. Thus, the observed patterns may display either out-of-plane ordering with labyrinthian striped domains  or bubble-like patterns  as well as in-plane vortex-like structures .

Most of the experimental samples being studied at present are epitaxial magnetic thin films of thickness ranging from $`10`$ to $`500`$ nm  or granular alloy films from $`200`$ nm to $`1\mu `$m thickness . Current experimental techniques allow to control the ferromagnetic content of granular alloys deposited on nonmagnetic metallic matrices  and therefore vary the range of dipolar and exchange interactions between the grains. It seems clear that these experimental systems should be efficiently modeled by a two-dimensional lattice of spins coupled by exchange interaction and shape anisotropy perpendicular to the plane of the sample and that the consideration of long-range forces between the spins, mainly of dipolar origin, is essential to understand the magnetic properties of these systems. The finite thickness of the samples can be taken into account by decreasing the value of the effective local anisotropy constant.

From the theoretical point of view the current understanding of dipolar spin systems can be summarized as follows. It is well established that the ground state of a pure planar dipolar system (no anisotropy and no exchange interaction) is a continuously degenerate manifold of antiferromagnetic (AF) states  (checkerboard phase). The introduction of exchange interactions ($`J>0`$) between the spins establishes a competition between the short-range ferromagnetic (FM) order and the long-range dipolar interaction that favours AF order . Contrary to what one would expect, increasing $`J`$ does not serve to stabilize a FM ground state but instead results in the appearance of striped phases of increasing width that do not disappear at high $`J`$. A finite perpendicular anisotropy $`K`$ favours the formation of out-of-plane configurations against the in-plane configurations induced by the dipolar interaction. Monte Carlo simulations  as well as theoretical analysis  have shown that there is a reorientation transition from out to in-plane order or from in to out-of-plane order depending on the ratio of $`K`$ to $`J`$ as the temperature is increased . In the above mentioned works main attention was put on the determination of phase diagrams but apparently an accurate description of the detailed structure of the ground state has not been reported.

In this work we present the results of extensive Monte Carlo simulations of a model of a thin film with the aim to explain the variety of magnetic behaviours of the above mentioned experimental observations. We start by the description of the model Hamiltonian Sec. II, in Sec. III the phase diagram and ground state configurations of the model are presented demonstrating that it qualitatively reproduces the patterns observed in experiments. In Sec. IV we present the results of two simulations that show the effect of two different magnetic histories on the magnetic order of the system. We conclude with the conclusions in Sec. V

## II Numerical Model and Hamiltonian

Our general model of a thin film consists of a two-dimensional square lattice (lattice spacing $`a`$ and linear size $`N`$) of continuous spins Heisenberg $`𝐒_i`$ with magnetic moment $`\mu `$ and uniaxial anisotropy $`K`$ perpendicular to the lattice plane described by the Hamiltonian

$$=\overline{J}_{exch}\overline{K}_{anis}+_{dip}$$
(1)   
where $`\overline{J}`$, $`\overline{K}`$, and $``$ are given in units of

$$g\frac{\mu ^2}{a^3}$$
(2)   
with $`a`$ the lattice spacing. The spin $`𝐒_i`$ may represent either an atomic spin or the total spin of a grain.

The three terms in the Hamiltonian correspond to short-range nearest neighbour exchange interaction (direct between atomic spins or indirect through the matrix), uniaxial anisotropy energy perpendicular to the lattice plane, and long-range dipolar interaction

$`_{exch}={\displaystyle \underset{n.n.}{}}(𝐒_i𝐒_j)`$ (3)   
$`_{anis}={\displaystyle \underset{n=1}{\overset{N^2}{}}}(S_n^z)^2`$ (4)   
$`_{dip}={\displaystyle \underset{nm}{\overset{N^2}{}}}{\displaystyle \underset{\alpha ,\beta =1}{\overset{3}{}}}S_n^\alpha W_{nm}^{(\alpha \beta )}S_m^\beta .`$ (5)   
In the last term we have defined the following set of dipolar interaction matrices

$$W_{nm}^{(\alpha \beta )}=\frac{1}{r_{nm}^3}\left(\delta _{\alpha \beta }\frac{3\delta _{\alpha \gamma }\delta _{\beta \eta }r_{nm}^\gamma r_{nm}^\eta }{r_{nm}^2}\right),$$
(6)   
$`r_{nm}`$ a vector connecting spins at sites $`n`$ and $`m`$. The matrices $`W_{nm}^{(\alpha \beta )}`$ depend only on the lattice geometry and boundary conditions and not on the particular spin configuration. In this expression the first term favours antiferromagnetic long-range order while the second one introduces an effective easy-plane anisotropy.

Thus, the properties of the model depend only on two parameters. $`\overline{J}`$, which accounts for the competition between the ferromagnetic ($`J>0`$) interaction and the antiferromagnetic order induced by $`g`$, and $`\overline{K}`$, which accounts for the competition between the out-of-plane alignment favoured by $`K`$ and the in-plane order induced by $`g`$.

This model reduces to the Ising model in the limit $`K=+\mathrm{}`$ when the out-of-plane components are restricted to $`S_i^z=\pm 1`$, and to the planar model when $`K=\mathrm{}`$ and the spins are forced to lie in the lattice plane. Both cases depend only on one parameter $`J/g`$, the ratio of exchange to dipolar energies and are described by the same formal Hamiltonian $`=\overline{J}_{exch}+_{dip}`$. All the simulations have been performed on a system of size $`50\times 50`$ with periodic boundary conditions.

## III Ground State properties

We start by studying the properties of the ground state of the model. For this purpose we have followed the simulated thermal annealing method: starting at a high temperature with a configuration with spins randomly oriented, the temperature is slowly decreased by a constant factor $`\mathrm{\Delta }T`$ (we started with a temperature of 10 and we used a reduction factor of $`0.9`$), at every temperature step the system is allowed to evolve during a number $`t`$ of MC steps long enough (usually between 200 and 250 MCS per spin in our system) so as to reach thermal equilibrium at every temperature, the process is continued until the number of accepted trial jumps is less than a small percentage. In this way we have obtained the ground state energies and configurations of the system.

### A Phase diagram

In Fig. 1 we present the results of the simulations for the ground state energies of the finite $`K`$ model as a function of the reduced exchange parameter $`\overline{J}`$ and for different values of the anisotropy constant (open symbols). In filled circles the energy of the corresponding Ising model ($`K=+\mathrm{}`$) is also given for comparison, the dashed lines correspond to the same curve with the corrections for the different finite anisotropy values added. The continuous line corresponds to the same calculation for the planar (XY) model.

A characteristic feature of the finite $`\overline{K}`$ model is that it behaves in a bimodal way. For small $`\overline{J}`$ ($`\overline{J}<\overline{J}^{}`$) it is completely equivalent to the corresponding Ising model, displaying out-of-plane order while for $`\overline{J}>\overline{J}^{}`$ it behaves like the planar model and it orders in-plane. The value of $`\overline{J}^{}`$ at which the crossover occurs is simply the one for which the ground state energy of the planar model (thick solid line) equals the energy of the corresponding Ising model with the finite anisotropy correction corresponding to a given value of $`K`$ (dashed lines). Therefore, the phase diagram for the finite $`K`$ model can be directly obtained from the results for the planar model by shifting the energy of the Ising model with the corresponding value of $`K`$. Consequently, the Heisenberg model for finite $`K`$ is the combination of the simpler Ising and planar models and its behaviour is dominated by the one having the lowest ground state energy.

The region of parameters of interest to us is precisely those values of $`\overline{J}`$ around the crossover points $`\overline{J}^{}`$ since in this region the out and in-plane configurations are quasi-degenerated in energy and the system displays metastability, that is to say, different kinds of ordering may be induced depending on how the system is driven to the quasi-equilibrium state as we will show in the next sections.

### B Configurations

Before proceeding further let us analyze the ground state configurations in more detail. On the one hand, for $`\overline{J}<\overline{J}^{}`$ (Ising regime) all the curves show three characteristic regions corresponding to different kinds of-out-of plane order. For small values of $`\overline{J}`$ the dipolar energy dominates over the exchange energy and the system orders antiferromagnetically (AF) in a checkerboarded phase of increasing energy as $`\overline{J}`$ increases (two left columns in Fig. 2). At intermediate $`\overline{J}`$ values the system enters a constant energy region in which a phase of AF stripes of width $`h=1`$ is stabilized by the exchange interaction (third column from the left in Fig. 2). Out from this plateau the FM ordering increases resulting in a widening of the stripes and an almost linear decrease of the energy with $`\overline{J}`$ (forth and fifth columns for $`\overline{K}=5.0,10.0`$ in the same figure).

In the metastable region ($`\overline{J}\overline{J}^{}`$) the system starts to turn to the planar regime first displaying configurations with a regular array of vortices with remanent out of plane internal order. This fact can be observed for the case $`\overline{K}=3.3,\overline{J}=1,1.33`$ in Fig. 2 and Fig. 3 where the in-plane projections of the spins are displayed with arrows. The diameter of the vortices progressively increases with increasing $`\overline{J}`$ until the FM order induced by the exchange energy stabilizes the in-plane FM configuration.

Moreover, at small values of $`\overline{K}`$, the system can change to the planar phase without entering some or any of the above mentioned Ising regions. On the contrary, at high enough $`\overline{K}`$ the system never crosses to the planar phase, behaving as the Ising model for any value of $`\overline{J}`$.

## IV Magnetic history dependence simulations

In this section we will show simulations that mimic some of the experimental processes found in recent experiments on thin films. In all of them the measuring protocol consists in taking the sample out of its equilibrium state by the application of an external perturbation that is subsequently removed. Usually this external perturbation is a magnetic field applied perpendicular to or in the thin film plane. The final state induced by this procedure may be very different from the initial one, magnetic domains may be erased or created depending on the magnetic history to which the sample has been submitted.

### A Relaxation after perpendicular saturation

In the first simulation experiment we have considered a system with $`\overline{K}=3.3`$ and $`\overline{J}=1.0`$ which is just at the crossover between the Ising and planar regimes and has a ground state configuration with in-plane vortices. We simulate the application of a saturating field perpendicular to the film plane by starting with a configuration with all the spins pointing along the positive easy-axis direction $`S_i^z=+1`$ and we let the system relax to equilibrium in zero applied field during a long sequence of Monte Carlo steps during which we record the intermediate system configurations. One example of temporal evolution is shown in Fig. 4 where we can see a sequence of snapshots of the system taken at different stages of the relaxation. In the first stages of the evolution the system forms striped out-of-plane structures that evolve very slowly towards the equilibrium configuration of in-plane vortices. Similar results are obtained for other values of $`\overline{J}`$ close to the intersection point of the Ising and planar regimes. For values of $`\overline{J}`$ smaller than $`\overline{J}^{}`$ the system reaches the same state as after an annealing process.

Defects and imperfections in real thin films (commonly present in granular alloys) may act as pinning centers of these intermediate structures. This may be the explanation of the change observed in MFM images of granular films with low concentration of the FM content  that in the virgin state show no out-of-plane order but after the application of $`10kOe`$ perpendicular to the film plane display striped and bubble-like domains similar to the ones obtained in the simulation.

### B Demagnetizing filed cycling

The second kind of process consists in the application of a demagnetizing field cycling in the perpendicular direction. The parameters used for the simulation are in this case $`\overline{K}=5.0,\overline{J}=2.1`$, also in the metastable region. As in the previous case in the initial state the system is saturated in positive perpendicular direction with a field $`H_0`$ but now the field is cycled from the positive to negative direction and progressively reduced in magnitude with a period $`T`$ (see the drawing at the top of Fig. 5). In the simulation the initial field has been chosen as the minimum allowing the system to escape from the initial saturated state ($`H_0=10.4`$) and the period ($`T=40MCS`$) is such that the system has time to reverse its magnetization during the reversal of the field.

The results are displayed in the sequence of snapshots of Fig. 5. At the first stages of the process (not shown in the figure) the spins reverse following at each reversal of the field. As the time elapses and the field decreases some reversed groups of spins start to nucleate (black spots in the two first rows). They continue to grow forming out-of-plane labyrinthian configurations separated by in-plane ordered zones (grey areas) arranged in vortices. As in the preceding experiment we find that a system with an in-plane ordered ground state may be driven to a very different ordering state by the magnetic history. What is more remarkable in this case is that the state attained after the cycling process it is not lost with time. Far from relaxing to the in-plane ordered ground state, when the system is allowed to relax in zero field, the incipient structure formed during the demagnetizing cycle is stabilized. The narrow adjacent stripes coalesce one with another to form wider stripes separated by narrower regions of in-plane spins.

## V Conclusions

We have shown that a model of two dimensional Heisenberg spins with anisotropy perependicular to the plane and interacting via exchange and long-range dipolar forces is able to reproduce the different magnetic patterns observed in experiments, from out-of-plane labyrinthian and striped domains to in-plane FM and vortex structures. The long-range character of the dipolar interaction play an essential role to understand the ground state properties of this system, the results would have been very different if the dipolar field acting on the spins had been replaced by a mean-field demagnetizing field as is usually done in some works. An interesting characteristic of the model is that it behaves as the limiting Ising of planar models depending on the values of $`\overline{J}`$ for a given value of $`\overline{K}`$. However, for values of $`\overline{J}`$ around the itersection between the Ising and the planar ground state lines, in-plane and out-of-plane configurations are quasidegenerated in energy and metastable. In this range of parameters our simulations are able to reproduce a surprising experimental observation : if a magnetic field perpendicular to the film plane is applied to a virgin sample with in-plane FM domains, the out-of plane component of the magnetization increases by a factor of 10 and the magnetic pattern displays well contrasted domains. A similar situation happens after perpedicular demagnetizing cycles, now the domains elongate and become wider. The last case could be thought as dinamical phase transition from in to out-of-plane order induced by a driving time dependent magnetic field similar to that observed for Ising spins . Therefore, the application of an external perturbation that changes momentarily the energy landscape together with the existence of highly metastable states facilitates the driving of the system to a new stable configuration that nonetheless it is not the equilibrium one.

## Acknowledgements

We acknowledge CESCA and CEPBA under coordination of $`C^4`$ for the computer facilities. This work was supported by CICYT through project MAT97-0404 and CIRIT under project SR-119.