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# Kinetics of phase separation in the driven lattice gas: Self-similar pattern growth under anisotropic nonequilibrium conditions

## I Introduction

Many alloys such as Al-Zn, which are homogeneous at high temperature, undergo phase separation after a sudden quench into the miscibility gap (for details, see the reviews rev1 -rev5 , for instance). One first observes nucleation in which small localized regions (grains) form. This is followed by “spinodal decomposition”. That is, some grains grow at the expense of smaller ones, and eventually coarsen, while their composition evolves with time. In addition to theoretically challenging, the details are of great practical importance. For example, hardness and conductivities are determined by the spatial pattern finally resulting in the alloy, and this depends on how phase separation competes with the progress of solidification from the melt.

A complete kinetic description of these highly non-linear processes is lacking.rev5  Nevertheless, the essential physics for some special situations is now quite well understood. This is the case when nothing prevents the system from reaching the equilibrium state, namely, coexistence of two thermodynamic phases. The simplest example of this is the (standard) lattice gas evolving from a fully disordered state to segregation into liquid (particle-rich phase) and gas (particle-poor phase). (Alternatively, using the language of the isomorphic lattice binary alloy, ma  the segregation is into, say Al-rich and Zn-rich phases.) As first demonstrated by means of computer simulations,prl00 ; rev1 ; rev2  this segregation, as well as similar processes in actual mixtures exhibit time self-similarity. This property is better defined at sufficiently low temperature, when the thermal correlation length is small. The system then exhibits a single relevant length, the size $`\mathrm{}\left(t\right)`$ of typical grains growing algebraically with time. Consequently, any of the system properties (including the spatial pattern) look alike, except for a change of scale, at different times.

This interesting property is revealed, for example, by the sphericalized structure factor $`S(k,t)`$ as observed in scattering experiments. After a relatively short transient time, one observes that $`S(k,t)J\left(t\right)F\left[k\mathrm{}\left(t\right)\right].`$ Taking this as a hypothesis, one may interpret $`J`$ and $`\mathrm{}`$ as phenomenological parameters to scale along the $`S`$ and $`k`$ axes, respectively. The hypothesis is then widely confirmed, and it follows that $`J\left(t\right)\mathrm{}\left(t\right)^d`$ where $`d`$ is the system dimension. It also follows that $`F(\varkappa )=\mathrm{\Phi }(\varkappa )\mathrm{\Psi }\left(\sigma \varkappa \right)`$ where $`\mathrm{\Phi }`$ and $`\mathrm{\Psi }`$ are universal functions. In fact, $`\mathrm{\Phi }`$ describes the diffraction by a single grain, $`\mathrm{\Psi }`$ is a grain interference function, and $`\sigma `$ characterizes the point in the (density$``$temperature) phase diagram where the sample is quenched. It then ensues that $`\mathrm{\Psi }1`$ except at small values of $`k`$, so that, for large $`\varkappa `$, $`F(\varkappa )`$ becomes almost independent of density and temperature, and even the substance investigated.prl00 ; zahra ; rev5

The grain distribution may also be directly monitored. A detailed study of grains in both microscopy experiments and computer simulations confirms time scale invariance. More specifically, one observes that the relevant length grows according to a simple power law, $`\mathrm{}\left(t\right)t^a,`$ and one typically measures $`a=1/3`$ at late times. This is understood as a consequence of diffusion of monomers that, in order to minimize surface tension, evaporate from small grains of high curvature and condensate onto larger ones (Ostwald ripening). In fact, Lifshitz and Slyozov, and Wagner independently predicted $`\mathrm{}t^{1/3},`$LSW  which is often observed, even outside the domain of validity of the involved approximations.LSWbis  In some circumstances, one should expect other, non-dominant mechanisms inducing corrections to the Lifshitz-Slyozov-Wagner one.rev1 ; rev3 ; rev5  For instance, effective diffusion of grains (Smoluchowski coagulation) leads to $`a=1/6,`$ which may occur at early times;toral  interfacial conduction leads to $`a=1/4;`$huse ; puri0  and, depending on density and viscosity, a fluid capable of hydrodynamic interactions may exhibit crossover with time to viscous ($`a=1`$) and then inertial ($`a=2/3`$) regimes.rev4

Extending the above interesting picture to more realistic situations is an open question. The assumption that the system asymptotically tends to the coexistence of two thermodynamic (equilibrium) phases is often unjustified in nature. This is the case, for example, for mixtures under a shear flow, whose study has attracted considerable attention, e.g.critic -corberi . The problem is that sheared flows asymptotically evolve towards a nonequilibrium steady state and that this is highly anisotropic. Studying the consequences of anisotropy in the behavior of complex systems is in fact an important challenge (see, for instance, mandel -md ). Another important example is that of binary granular mixtures under horizontal shaking. The periodic forcing causes in this case phase separation and highly anisotropic clustering.Mullin

In this paper, we study in detail the kinetics of the driven lattice gas (DLG) katz  following a deep quench. Our motivation is twofold. On one hand, the DLG is recognized to be an excellent microscopic model for nonequilibrium anisotropic phenomena.md  On the other, the DLG is not affected by hydrodynamic interactions, which makes physics simpler. Our goal is timely given that the asymptotic state of the DLG is now rather well understood, and previous studies of kinetics altogether reveal an intriguing situation.md -albano  Following this pioneering effort, we here present a new theoretical description of the essential physics during anisotropic, nonequilibrium pattern growth. This is compared with new extensive computer simulations. A brief and preliminary account of some of our results was presented elsewhere.new

## II Model and simulation details

The DLG consists of a $`d`$dimensional, e.g., simple-cubic lattice with configurations $`𝐧=\{n_i;i=1,\mathrm{},N\}`$. The variable at each lattice site has two possible states, $`n_i=1`$ (particle) or $`0`$ (hole). As for the standard lattice gas, dynamics is a stochastic process at temperature $`T`$ consisting of nearest-neighbor (NN) particle/hole exchanges. This conserves the particle density, $`\rho =N^1_in_i,`$ and depends on $`𝐧.`$

A distinguishing feature of the DLG is that exchanges are favored in one of the principal lattice directions, say $`\stackrel{}{x}.`$ Therefore, assuming periodic (toroidal) boundary conditions, a net current of particles is expected to set in along $`\stackrel{}{x}.`$ This is accomplished in practice by defining a biased transition rate. We shall refer here to the energy function $`H=4J_{NN}n_in_j,`$ which describes attractive interactions between particles at NN sites, and to the transition rate (per unit time):md

$$\omega (𝐧𝐧^{})=\mathrm{min}\{1,\mathrm{e}^{\left(\mathrm{\Delta }H+E\delta \right)/T}\}.$$
(1)
$`𝐧^{}`$ stands for configuration $`𝐧`$ after jumping of a particle to a NN hole; $`\mathrm{\Delta }H=H\left(𝐧^{}\right)H\left(𝐧\right)`$ is the energy change brought about by the jump; and units are such that both the coupling strength $`J`$ and the Boltzmann constant are set to unity. One further defines $`\delta =(1,0)`$ for NN jumps along $`\pm \stackrel{}{x}`$ or along any of the transverse directions, say $`\stackrel{}{y},`$ respectively. Consistent with this, $`\stackrel{}{E}=E\stackrel{}{x}`$ may be interpreted as a field driving particles, e.g., an electric field if one assumes that particles are charged. (One may adopt other interpretations, e.g., the binary alloy one.ma  Dynamics then consists of interchanges between particles of different species, one of them favored along $`\stackrel{}{x}.`$)

The DLG was described as modelling surface growth, fast ionic conduction and traffic flow, among a number of actual situations of practical interest.md  A common feature in these situations is anisotropy, and that steady states are out of equilibrium. Both are essential features of the DLG induced by the rate (1). The only trivial case is for $`E=0,`$ which reduces (1) to the Metropolis algorithm. In this case, detailed balance holds, and one simply has the familiar lattice gas with a unique (equilibrium) steady state. For any, even small $`E,`$ qualitatively new behavior emerges. In fact, detailed balance breaks down for $`E>0`$ and, consequently, the steady state depends on $`\omega (𝐧𝐧^{}).`$ Increasing $`E,`$ one eventually reaches saturation. That is, particles cannot jump backwards, i.e., $`\stackrel{}{x},`$ which formally corresponds to an infinite field $`(E=\mathrm{}).`$

The way in which the microscopic anisotropy (1) conveys into macroscopic behavior is amazing.md  Consider, for simplicity, $`d=2,`$ $`\rho =\frac{1}{2}`$ and $`E=\mathrm{}.`$ The system then exhibits a critical point at $`T=T_C^{\mathrm{}}1.4T_C\left(E=0\right)`$, where $`T_c(E=0)2.2691`$, with novel critical behavior.prl01 ; albano  Furthermore, the asymptotic, steady states below $`T_C^{\mathrm{}}`$ do not comprise equilibrium phases. Instead, one observes a particle current and fully anisotropic phases; both are nonequilibrium features. The intensity of the current increases with $`T,`$ and suddenly changes slope at $`T_C^{\mathrm{}}`$ (in fact, this property may serve to accurately locate the critical point). The stable ordered configurations consist of one stripe, to be interpreted as a liquid (rich-particle) phase of density $`\rho _L\left(T\right).`$ The gas (poor-particle) phase of density $`\rho _G\left(T\right)`$ fills the remainder of the system. Except for some microscopic roughness, the interface is linear and rather flat, in general.interfases

The computer evolutions reported here always begin with a completely disordered state to simulate the system at infinite temperature. We then model a sudden quench and the subsequent time evolution. With this aim, one proceeds with rate (1) that involves the temperature $`T`$ at which the system is quenched. The run is followed until one stripe is obtained (eventually, in order to save computer time, the run was sometimes stopped before reaching the final stationary state). The code involves a list of $`\eta \left(t\right)`$ particle-hole NN pairs from where the next move is drawn. Time is then increased by $`\mathrm{\Delta }t=\eta \left(t\right)^1,`$ so that its unit or MC step involves a visit to all sites on the average.deltat

The lattice is rectangular, $`L_{}\times L_{},`$ with sides ranging from 64 to 256 and, in a few cases, 512. Results concern an average over around thousand independent runs. Due to the great computational effort which is consequently involved, this paper describes simulations concerning a single point of the two-dimensional DLG phase diagram. That is, most of our evolutions are for $`\rho =\frac{1}{2}`$ and $`E=\mathrm{},`$ and simulate a quench at $`T=0.8T_C\left(E=0\right)0.6T_C^{\mathrm{}}.`$ This choice is motivated by the fact that clustering is then reasonably compact, which helps to obtain good statistics, while it proceeds fast enough, so that one can observe full relaxation to the steady state. In spite of this restriction, brief investigation of other points, together with some of our observations below, led us to believe that the validity of our results extends to a large domain around the center of the miscibility gap; in fact, such generality of behavior has been reported for $`E=0.`$rev2 ; prl00 ; toral ; rev5

## III Growth of order

The DLG exhibits different time regimes during phase separation. Though they parallel the ones for $`E=0,`$ the peculiarities induced by the anisotropic condition are essential.

Starting from complete disorder, there is a very short initial regime in which small grains form. The novelty is that typical grains are now fully anisotropic, stretched along $`\stackrel{}{x}.`$ The grains then rapidly coarsen to form macroscopic strings, as illustrated in fig.1. Sheared fluids (an experimentally accessible situation that also involves both nonequilibrium physics and anisotropy) seem to exhibit similar initial regimes.onuki ; corberi  That is, during a short time interval, they show larger growth rate along the flow than in the other directions, which is assumed to correspond to the initial formation of anisotropic regions. Afterwards, sheared fluids develop string-like macroscopic domains similar to the ones in the DLG.

Fig.1 includes a comparison with the zero-field case, i.e., the standard, isotropic lattice gas (LG). This clearly illustrates the strong anisotropy of nucleation and early phase separation for the DLG. Close inspection of these and similar graphs also seems to indicate relatively small but significant differences in the degree of segregation between the two cases at a given time. That is, at small distances, there is a more homogeneous distribution of particles, both longitudinally and transversely, in the DLG than in the LG. The latter shows up more segregated at the same time, which is already rather evident by direct inspection of graphs for $`1<t100`$ in fig.1. We believe this reveals the different role played by surface tension as the degree of anisotropy is varied: Typical DLG grains are rather linear except at their longitudinal ends, where curvature may be even stronger than for the spherical clusters in the LG at comparable times. This seems to be at the origin of a smother transverse distribution of particles in the DLG at early times. On the other hand, the field also tends to smooth things longitudinally.

In order to quantify the aforementioned observation, we evaluated the number of broken bonds in the direction of (perpendicular to) the field, $`n_{}(t)`$ ($`n_{}(t)`$) as a function of time during the early evolution stage. Then $`A(t)[n_{}(t)+n_{}(t)]/2N`$ is the density of broken bonds. The higher the degree of segregation at time $`t`$, the smaller is $`A(t)`$. For instance, we observe in a large $`256\times 256`$ lattice that $`A(t=10)=0.295`$ and $`A(t=10)=0.38`$ for the LG and DLG respectively, confirming the above observation. On the other hand, let $`B(t)[n_{}(t)n_{}(t)]/2N`$. One would expect $`B(t)0`$ (up to fluctuations) only for the isotropic system. In fact, we measured $`B(t)0`$ for the LG, while $`B(t)`$ rapidly converges to a nonzero value $`B(t)0.05`$ for the DLG at early times (again for a large $`256\times 256`$ lattice). We take this number, $`B(t)=0.05`$, as characterizing the anisotropic shape of DLG clusters at early times.

The difference of segregation between the DLG and the LG at early times merits further study. This will need to take into account the anisotropy of surface tension. In any case, this concerns a regime very near the initial, melt state that only bears minor practical importance, given that it extends extremely shortly on the macroscopic time scale. We are interested in the rest of this paper on the subsequent evolution, to be described on the assumption of a simple flat interface, which holds in fig. 1 for $`t>100.`$

The DLG strings coarsen with time until well defined, relatively-narrow longitudinal (i.e., directed along $`\stackrel{}{x})`$ stripes are formed. (For periodic boundary conditions, the case of our simulations, each stripe forms a ring.) This results into a multi-stripe state, as illustrated in figs. 1 and 2. The ordering time in the DLG, defined as the time the system needs to form the stripes, scales with the system size in the direction of the field, $`L_{}`$, since in this case ordered clusters (stripes) percolate along the field direction (see below).mukamel  This is not the case for the equilibrium LG, where the ordering time depends exclusively on system intensive parameters such as temperature and density.

The multi-stripe states are not stable, however. They are only partially segregated and, in fact, a definite tendency towards a fully segregated state with a single stripe is generally observed in computer simulations. One may also develop simple arguments indicating that, in general, a multi-stripe state will monotonically evolve until forming a single stripe.25bis ; md  It is true that, in practice, the complete relaxation may take a very long time. More specifically, a macroscopic system may take to decay into the true stable state a long, macroscopic time interval, namely, a time that may show up as mathematically infinite in some time scales. In fact, the complete relaxation time is observed to increase with system size, as first demonstrated in mukamel . It should also be remarked that this property is not a nonequilibrium feature but occurs already in the equilibrium ($`E=0`$) case; see, for instance, rev2 ; rev4  and references therein. Slow relaxation is a consequence of the conservation of particle density $`\rho `$ implied by the particle-hole exchange dynamics; this induces scale invariance, namely, slow (power-law) evolution of correlations so that, once enough order sets in, all but very small pattern modifications during a single MC step are precluded. Consequently, certain individual runs sometimes block for a long time in a state with several stripes; however, this does not correspond to the average behavior. As illustrated by fig.2, which shows a typical evolution, and demonstrated below by our averages corresponding to thousand evolutions, the number of stripes monotonically decreases with time (see also §V), and the whole relaxation can easily be observed in computer simulations if one waits long enough.

We next attempt a theoretical description of the relaxation process. Our interest is on the anisotropic spinodal decomposition by which the earliest state with many well-defined stripes decays into a single stripe.We shall assume that relaxation is a consequence of monomer events causing effective diffusion of liquid stripes. (Note that assuming gas stripes here would be completely equivalent.) That is, due to single particle processes, liquid stripes move transversely as a whole, and may collide and eventually coalesce with one of the neighboring stripes; see the late evolution depicted in fig.2. We notice that coalescence implies evaporation of the gas stripe between the two involved liquid stripes. Therefore, given the particle/hole symmetry, our assumption is in a sense equivalent to assuming that growth is due to evaporation of stripes;mukamel  however, the view adopted here allows for a more detailed description below.

In order to evaluate the implications of stripe effective diffusion via monomer events, lets assume that stripes are well defined, compact and exhibit a (linear) interface which is rather flat. This is perfectly justified at sufficiently low temperature (the case analyzed in detail here),md  and it might hold more generally, in a wide region including the center of the miscibility gap but excluding the critical region. Under this assumption, consider a stripe of mean width $`\mathrm{}\left(t\right)`$ that consists of $`M`$ particles whose coordinates along the transverse (vertical) direction are $`y_j\left(t\right);`$ $`j=1,\mathrm{},M.`$ We characterize the stripe position by its center of masses, $`Y_{\text{cm}}\left(t\right)M^1_jy_j\left(t\right).`$

Let us evaluate the mobility coefficient $`𝒟_{\mathrm{}}N_{\text{me}}(\mathrm{\Delta }Y_{\text{cm}})^2`$ which depends on the stripe width $`\mathrm{}(t).`$ Here $`N_{\text{me}}`$ is the number of monomer events per unit time, and $`(\mathrm{\Delta }Y_{\text{cm}})^2`$ is the mean squared displacement of the stripe associated to one of the monomer events. We think of two possible types of events, each giving a different contribution to $`𝒟_{\mathrm{}}:`$

(A) Evaporation-condensation of particles and holes in the stripe surface. Here particles (holes) at the stripe interface evaporate to the hole (particle) gas, and condensate later at the same interface. The evolution of the evaporated particle (hole) in the bulk can be seen as a one dimensional random walk with two absorbing walls, the left and right interfaces, respectively. According to standard random walk theory,gambler  the evaporated particle (hole) will go again with unit probability to one of the (two) possible interfaces, Moreover, the random walker will stick again to its original interface with high probability, so trapping a particle (hole) from the opposite interface is unlikely. Consequently, in this case (A), $`N_{\text{me}}`$ is simply the evaporation rate. That is, $`N_{\text{me,A}}=\nu _j^{}\mathrm{exp}(2T^1\mathrm{\Delta }_j),`$ where $`\nu `$ is the a priori frequency, the sum is over the surface particles and $`\mathrm{\Delta }_j`$ is the number of resulting broken bonds. For a flat linear interface, particles can only jump transversely away the surface, $`\nu `$ equals the inverse of the lattice coordination number, $`q,`$ and one may write $`N_{\text{me,A}}4q^1L_{}\mathrm{exp}(2\overline{\mathrm{\Delta }}/T)`$ where $`\overline{\mathrm{\Delta }}`$ is the mean number of broken bonds per evaporation event. We multiplied here by 2 to take into account evaporation of surface holes that travel within the stripe to reach the (same) surface again. On the other hand, evaporation processes induce changes $`\mathrm{\Delta }Y_{\text{cm}}=M^1\delta y,`$ where $`\delta y`$ is the net particle (transverse) displacement, and $`ML_{}\times \mathrm{}(t)`$ for compact stripes. Therefore,

$$𝒟_{\mathrm{}}^{(\text{A})}4q^1\delta y^2\mathrm{e}^{2\overline{\mathrm{\Delta }}/T}L_{}^1\mathrm{}^2.$$
(2)
(B) A hole jumps one lattice spacing away within the stripe interior. This induces $`\mathrm{\Delta }Y_{\text{cm}}=1/M`$ or 0, depending on the jump direction. One may write $`N_{\text{me,B}}=2\nu \rho _h\left(T\right)L_{}\mathrm{}p_h\left(T\right),`$ where $`\rho _h`$ is the density of holes, $`L_{}\mathrm{}`$ is the volume or total number of sites within the liquid stripe, and $`p_h`$ is the jumping probability per unit time. The factor 2 here comes from the fact that a hole modifies $`Y_{\text{cm}}`$ when jumping to any of the two directions $`\pm \stackrel{}{y}.`$ At low $`T,`$ $`\rho _h`$ is small; holes are then rather isolated from each other, so that jumps do not modify the number of broken bonds, and $`p_h1.`$ It ensues

$$𝒟_{\mathrm{}}^{(\text{B})}2q^1\rho _hL_{}^1\mathrm{}^1.$$
(3)
Note that a different dependence of (2) and (3) on $`\mathrm{}`$ is a consequence of the fact that the rates $`N_{\text{me,A}}`$ and $`N_{\text{me,B}}`$ involve processes consisting of evaporation on the line and difussion on the bulk, respectively.

For $`\rho =\frac{1}{2},`$ one has on the average stripes of width $`\mathrm{}`$ that are separated a distance $`\mathrm{}`$ from each other. Therefore, a given stripe takes a mean time $`\tau _{\mathrm{}}=\mathrm{}^2/𝒟_{\mathrm{}}`$ to find (and thus to coalesce with) another one, and this causes its width to increase by $`\mathrm{\Delta }\mathrm{}=\mathrm{}.`$ Consequently, $`\mathrm{d}\mathrm{}/\mathrm{d}t\mathrm{\Delta }\mathrm{}\tau _{\mathrm{}}^1=𝒟_{\mathrm{}}\mathrm{}^1.`$ Together with (2) and (3), respectively, this implies that mechanism A is characterized by a power law $`\mathrm{}t^{1/4},`$ and that mechanism B is to be associated with $`\mathrm{}t^{1/3}.`$ Furthermore, assuming that pattern growth in the DLG is the result of competition between the two mechanisms, and that they are independent of each other, $`𝒟_{\mathrm{}}=𝒟_{\mathrm{}}^{(\text{A})}+𝒟_{\mathrm{}}^{(\text{B})},`$ it follows that

$$\frac{\mathrm{d}\mathrm{}}{\mathrm{d}t}\frac{1}{L_{}}\left(\frac{\alpha _\text{A}}{\mathrm{}^3}+\frac{\alpha _\text{B}}{\mathrm{}^2}\right),$$
(4)
where $`\alpha _\text{A}=4\nu \delta y^2\mathrm{e}^{2\overline{\mathrm{\Delta }}/T}`$and $`\alpha _\text{B}=2\nu \rho _h.`$ This is our general result for the DLG as far as the field $`E`$ is large, e.g., infinite, and the temperature $`T`$ is low enough so that the interfaces, and mechanisms A and B, are sufficiently simple as assumed. This is to be compared with the Lifshitz-Slyozov-Wagner behavior $`\mathrm{d}\mathrm{}/\mathrm{d}t\mathrm{}^2`$ which assumes spatial isotropy and diffusion directly governed by surface tension. Formally, (4) is similar to an equation obtained before by assuming isotropic conditions; see §1.huse

The consequences of (2)–(4) are as follows. Both (2) and (3) imply independently that

$$\mathrm{}\left(\phi \theta \right)^{1/\phi }\left(t/L_{}\right)^{1/\phi }.$$
(5)
The difference is that $`\theta =\alpha _A`$ and $`\phi =4`$ from (2) while one obtains $`\theta =\alpha _B`$ and $`\phi =3`$ from (3). On the other hand, for sufficiently late times, $`\mathrm{}`$ becomes large and equation (4) simply solves into

$$\mathrm{}(t)\alpha t^{1/3}+\zeta ,$$
(6)
where $`\alpha ^3=3\alpha _\text{B}L_{}^1`$ and $`\zeta =\alpha _\text{A}/2\alpha _\text{B}.`$ That is, the prediction is that hole diffusion within the stripe (mechanism B) will be dominant at late times. A different hypothesis, based on the stripe evaporation picture, was shown in mukamel  to imply $`\mathrm{}\left(t/L_{}\right)^{1/3}`$. This coincidence is not surprising since, as argued above, the coalescence of two particles stripes implies the evaporation of the intermediate hole stripe and due to the particle/hole simmetry in our system, both mechanisms (stripe diffusion/coalescence and stripe evaporation) correspond to the same physical process yielding the same behavior. In order to uncover the close analogy between the two pictures, one may notice that, to evaporate a particle stripe, many of its particles must cross the surrounding hole stripes and stick on the neighboring particle stripes (this is so since the particle density in the gas phase remains almost constant). This particle migration process through the surrounding hole stripes is in fact what we have called ’hole diffusion within the stripe’ in the presence of particle/hole simmetry. Hence the fundamental mechanism involved in a stripe evaporation is the diffusion of its constituents through the neighboring stripes. This observation is a key one to understand the relation between stripe’s evaporation and hole (particle) diffusion.

The effect of mechanism A —surface evaporation and subsequent condensation— on growth is more subtle. In fact, our theory predicts a crossover from the $`t^{1/4}`$ regime to the $`t^{1/3}`$ regime as time is increased. That is, the two mechanisms will have a comparable influence at $`t\tau _{\text{cross}}`$ with

$$\tau _{\text{cross}}=\frac{\left(4\alpha _\text{A}\right)^3}{\left(3\alpha _\text{B}\right)^4}L_{}.$$
(7)
For times $`t<\tau _{\text{cross}}`$, mechanism A is dominant and the $`t^{1/4}`$ behavior is expected, while mechanism B is dominant for $`t>\tau _{\text{cross}}`$ and the asymptotic $`t^{1/3}`$ growth law is then observed. The crossover time $`\tau _{\text{cross}}`$ is a macroscopic, observable time. Further, we may define the time $`\tau _{\text{ss}}`$ at which a single stripe is reached by the condition that $`\mathrm{}\left(t\right)\frac{1}{2}L_{}.`$ One obtains

$`\tau _{\text{ss}}`$ $`=`$ $`{\displaystyle \frac{L_{}}{\alpha _\text{B}}}\{{\displaystyle \frac{L_{}^3}{24}}{\displaystyle \frac{\zeta L_{}^2}{4}}+2\zeta ^2L_{}`$ (8)
$`8\zeta ^3[\mathrm{ln}{\displaystyle \frac{\alpha _\text{B}(2\zeta +\frac{1}{2}L_{})}{L_{}}}\mathrm{ln}{\displaystyle \frac{2\zeta \alpha _\text{B}}{L_{}}}]\}`$
Hence our system is characterized by two different time scales, namely, $`\tau _{\text{cross}}`$ and $`\tau _{\text{ss}}`$. They depend on system size in a different way. For large systems one generally obtains $`\tau _{\text{ss}}\tau _{\text{cross}}`$, so that the system converges, after a short, perhaps unobservable transient time, to the relevant $`t^{1/3}`$ behavior. However, there are small systems for which $`\tau _{\text{ss}}<\tau _{\text{cross}}`$. These systems will reach the stationary state (a single stripe) before having time to enter into the asymptotic $`t^{1/3}`$ regime. For these small systems, the only relevant behavior is the $`t^{1/4}`$ one. Therefore, there is a size crossover between $`t^{1/4}`$ asymptotic behavior for small systems and $`t^{1/3}`$ asymptotic behavior for large ones. The condition $`\tau _{\text{cross}}(T,L_{})=\tau _{\text{ss}}(T,L_{},L_{})`$ defines the crossover size.

Consider now the parameter $`\gamma \tau _{\text{cross}}(T,L_{})/\tau _{\text{ss}}(T,L_{},L_{}).`$ It follows that the $`t^{1/3}`$ behavior is dominant for $`\gamma 1.`$ However, one also has that $`\gamma (T,L_{},L_{})0`$ for finite $`T`$ in the thermodynamic limit ($`L_{},L_{}\mathrm{},L_{}/L_{}=\mathrm{const}.).`$ Consequently, the $`t^{1/3}`$ growth law is the general one, namely, the only one we should expect to observe in a macroscopic system. Corrections to this should only occur at early times in small systems. This is fully confirmed below.

One may also define a longitudinal length,prl01 ; mukamel  say $`\mathrm{}_{}t^a_{},`$ where one expects $`a_{}>1/3`$ (given that the growth is more rapid longitudinally than transversely). This length is only relevant during the initial regime, until stripes become well-defined, all of them extending the whole length $`L_{}`$. This condition may be taken as defining the onset of the multi-stripe state, which may be characterized by $`\mathrm{}_{}\left(\tau _{\text{ms}}\right)=L_{},`$ from where it follows that $`\tau _{\text{ms}}L_{}^{1/a_{}}.`$ Interesting enough, this is on the macroscopic time scale, as for both $`\tau _{\text{cross}}`$ and $`\tau _{\text{ss}}`$ (more precisely, $`\tau _{\text{cross}}L_{}`$ and $`\tau _{\text{ss}}L_{}L_{}^3).`$ The fact that all these relevant times are on the macroscopic, observable time scale confirms that, as argued above, the single-stripe (and not the multi-stripe) state is the only stable one in general. It is also to be remarked that, once the multi-stripe state sets in, the only relevant length is the transverse one, $`\mathrm{}.`$ Of course, this is compatible with the possible existence of two correlation lengths describing thermal fluctuations at criticality.

In order to test our predictions, several measures of the relevant length in computer simulations were monitored, namely:

* the maximum width of the stripe, $`\mathrm{}_{\text{max}},`$ averaged over all stripes in the configuration. This maximun width is defined as the distance in the direction perpendicular to the field between the leftmost and the rightmost particles within the stripe;
* $`\mathrm{}_MM/L_{},`$ where $`M=M\left(t\right)`$ is the mass, or number of particles belonging to the stripe, averaged over all stripes in the configuration. This mass width is defined as the width of a perfectly dense stripe with $`M`$ particles.
* $`\mathrm{}_sL_{}/2N_s,`$ where $`N_s`$ is the number of stripes in the configuration.

After averaging over many independent evolutions, all these quantities happen to behave similarly with time. Further measures of the relevant length that we define in the next section behave in the same way. We shall refer to this common behavior, which is illustrated in fig.3, as $`\mathrm{}\left(t\right).`$ (It is noticeable that, before showing a common behavior, Fig.3 reveals some significant differences between our measures of $`\mathrm{}\left(t\right)`$ at early times. This confirms the more difficult description —not attempted here— which is required by the initial regime.)

In fig.4 we illustrate our analysis and main results concerning the (late) time evolution of $`\mathrm{}\left(t\right).`$ The predictions above are confirmed and, in particular, “small” lattices —fig.4(a)— happen to behave differently than “large” lattices —fig.4(b). In both cases we plotted $`\mathrm{}\left(t\right)`$ versus $`t^a_{}`$ for varying $`a_{},`$ looking for the best linear fit $`\mathrm{}(t)=\alpha t^a_{}+\zeta ,`$ excluding the initial time regime. The upper insets in the figures show the chi square function associated to each fit, namely,

$$\chi ^2\left(a_{}\right)=\underset{i=1}{\overset{\eta }{}}\frac{\left[\mathrm{}(t_i)\left(\alpha t_i^a_{}+\zeta \right)\right]^2}{\alpha t_i^a_{}+\zeta },$$
(9)
for a least-squares fit to $`\eta `$ data points using parameters $`a_{},`$ $`\alpha `$ and $`\zeta `$. The main graphs confirm the existence of a common behavior for all the monitored measures of $`\mathrm{}\left(t\right)`$ (indicated by different symbols). These graphs also demonstrate that $`\mathrm{}(t)=\alpha t^a_{}+\zeta ,`$ with small $`\zeta ,`$ during the whole time regime of consideration. On the other hand, the upper insets indicate that $`a_{}`$ is very close to $`\frac{1}{4}`$ for “small” systems (in fact, for $`L_{}128`$) while $`a_{}\frac{1}{3}`$ as the system becomes larger, say $`L_{}256`$ that corresponds to a “large” lattice according to familiar MC standards. As an alternative method to analyze $`\mathrm{}\left(t\right),`$ one may evaluate

$$\overline{a}\left(t\right)\frac{\mathrm{d}\mathrm{log}_n\mathrm{}\left(t\right)}{\mathrm{d}\mathrm{log}_nt}.$$
(10)
Our prediction is that $`\overline{a}\left(t\right)=a_{}\zeta a_{}/\mathrm{}\left(t\right),`$ i.e., this should provide the exponent $`a_{}`$ by extrapolating to large $`\mathrm{}\left(t\right)`$ (late time). The insets at the bottom of each fig.4 show the results for $`n=2.`$ They are in agreement with the other method, and again confirm our predictions.

As indicated above, the size crossover between the $`t^{1/4}`$ and $`t^{1/3}`$ asymptotic regimes is expected for a system size $`(L_{},L_{})`$ such that $`\tau _{\text{cross}}(T,L_{})=\tau _{\text{ss}}(T,L_{},L_{}).`$ In order to make this condition explicit, we need to estimate the amplitudes $`\alpha _\text{A}`$and $`\alpha _\text{B}`$ in (4); see equations (7) and (8). These amplitudes, which state the relative importance of surface evaporation/condensation versus bulk hole-diffusion, are given respectively by $`\alpha _\text{A}=4q^1\delta y^2\mathrm{e}^{2\overline{\mathrm{\Delta }}/T}`$and $`\alpha _\text{B}=2q^1\rho _h.`$ We note that, for a sufficiently flat interface (i.e., one that involves microscopic –but not macroscopic– roughness), $`\delta y^2𝒪\left(1\right)`$ and $`\overline{\mathrm{\Delta }}5.`$ On the other hand, the excess energy associated with an isolated hole is 16, so that $`\rho _h\mathrm{exp}\left(16/T\right)`$ is a rough estimate of the hole density. As depicted in fig.5, it follows numerically, in full agreement with our observations, that $`a_{}=\frac{1}{4}`$ is to be observed only at early times, earlier for larger systems; to be more specific, the crossover for $`L_{}=64,`$ for instance, is predicted for $`L_{}140,`$ which confirms the above; see also figures 4.

This behavior may be understood on simple grounds. The surface/volume ratio is large initially and, consequently, mechanism A (based on surface events) is then dominant. This is more dramatic the smaller the system is. That is, the surface is negligible for macroscopic systems, in general, and, as illustrated in fig.2, even if the surface is relevant at very early times, its ratio to the volume will monotonically decrease with time. This causes hole diffusion in the bulk (mechanism B) to become dominant, more rapidly for larger systems, as the liquid phase is trying to exhibit only two surfaces. On the other hand, ref. mukamel  studies the stripe coarsening process in the infinitely driven lattice gas. Pure $`t^{1/3}`$ behavior is reported assuming the stripe evaporation mechanism. This result is perfectly compatible with our results, given that the systems in ref. mukamel  correspond to very large values of $`L_{}`$ ($`800`$ and $`960`$) and small values of $`L_{}`$ ($`8`$, $`16`$ and $`32`$). For these shapes our theory also predicts the (simple) $`t^{1/3}`$ asymptotic behavior.

## IV Correlations and the structure factor

Consider now the Fourier transform of the pair correlation function $`C(x,y;t)=n_{0,0}\left(t\right)n_{x,y}\left(t\right),`$ where $`n_{x,y}`$ stands for the occupation variable at lattice site $`\stackrel{}{r}=(x,y).`$ This is the so-called structure factor, $`S(\stackrel{}{k},t),`$ where $`\stackrel{}{k}=(k_{},k_{}).`$ Given that the $`k_{}`$ dependence is only relevant at early times, before the multi-stripe state sets in, i.e., for $`t<\tau _{\text{ms}}`$, we shall set $`k_{}=0`$ in the following. That is, our interest here is on

$$S(k_{};t)=\frac{1}{L_{}L_{}}\left|\underset{x,y}{}n_{x,y}\left(t\right)\mathrm{exp}\left[\text{i}k_{}y\right]\right|^2.$$
(11)
As illustrated in fig.6, this function develops a peak at $`k_{}=k_{\text{max}}\left(t\right)`$ immediately after quenching. The peak then monotonically shifts towards smaller wave numbers with increasing $`t;`$ in fact, one expects $`k_{}0`$ as $`t\mathrm{}`$ in a macroscopic system. The wave length $`\mathrm{}_S2\pi /k_{\text{max}}`$ turns out to be an excellent characterization of the relevant order, namely, it measures both the stripe width and the stripe separation during phase segregation. In particular, we confirm that $`\mathrm{}_S\left(t\right)`$ has the common behavior discussed above for length $`\mathrm{}\left(t\right);`$ see figs. 3 and 4.

The fact that the DLG shows a unique time-dependent relevant length, $`\mathrm{}_{}=\mathrm{}\left(t\right),`$ has some important consequences. For example, extrapolating from the equilibrium case (see §1),prl00  one should probably expect dynamical scaling, i.e.

$$S(k_{};t)\mathrm{}\left(t\right)F\left[k_{}\mathrm{}\left(t\right)\right]$$
(12)
for the anisotropic DLG in two dimensions. This is indeed observed to hold during most of the relaxation and, in particular, during all the segregation process after formation of well-defined stripes. This is illustrated in fig.7 depicting the scaling function $`F.`$ A time-dependent mean-field model of a binary mixture in shear flow has recently been demonstrated to exhibit a similar property, though involving two lengths both behaving differently from $`\mathrm{}\left(t\right)`$ above.corberi

The structure factor may be obtained by scattering, which makes it an important tool in many studies. Analyzing further the details of functions $`S(k_{};t)`$ and $`F\left(\varkappa \right)`$ or, alternatively, the universal function $`\mathrm{\Phi }\left(\varkappa \right)S/\mathrm{}L`$, as observed in computer simulations is therefore of great interest (the extra $`L`$ factor in the definition of $`\mathrm{\Phi }\left(\varkappa \right)`$ is our finite size scaling ansatz). Experimental studies often refer to the mean ‘radius of gyration’ of the grains as the slope of the straight portion in a plot of $`\mathrm{ln}\left[S(k,t)\right]`$ versus $`k^2.`$guin  We checked the validity under anisotropic conditions of this concept, which is in fact quite useful in equilibrium even outside the domain of validity of its approximations.prl00  We confirm that $`S(k_{};t)`$ exhibits the Guinier Gaussian peak, namely,

$$\mathrm{\Phi }\left(\varkappa \right)\mathrm{exp}\left[\text{const.}\left(\varkappa \varkappa _{\text{max}}\right)^2\right]$$
(13)
around the maximum $`\varkappa _{\text{max}}.`$ More intriguing is the behavior of $`\mathrm{\Phi }\left(\varkappa \right)`$ before the peak, $`\varkappa <\varkappa _{\text{max}}.`$ Fig.7 indicates that scaling does not hold in this region even at the end of our (otherwise long enough) simulations. This is so because $`\mathrm{\Phi }\left(\varkappa \right)`$ goes as $`\rho ^2L/\mathrm{}\left(t\right)`$ at $`k_{}=0`$, and thus depends on time for very small values of $`\kappa `$, breaking the scaling observed for larger values of $`\kappa `$. However, a detailed study of data reveals that the scaling function near the origin tends with time towards a common envelope $`\mathrm{\Phi }\left(\varkappa \right)\varkappa ^{1+1/3}`$ for $`\varkappa _0<\varkappa <\varkappa _{\text{max}};`$ we do not have a simple explanation of this. In any case, this behavior breaks down close to the origin, $`\varkappa \varkappa _0,`$ where $`\mathrm{\Phi }\left(\varkappa \right)0`$ as $`\varkappa 0`$ and $`t\mathrm{}`$ for the infinite system.

The behavior after the peak, $`\varkappa >\varkappa _{\text{max}},`$ may be predicted on simple grounds. The (sphericalized) structure factor for (equilibrium) isotropic binary mixtures is known to satisfy the Porod’s law, $`Sk^{(d+1)}`$ at large enough $`k,`$ where $`d`$ is the system dimension,prl00  i.e., $`Sk^3`$ in two dimensions. The main contribution to the large-$`k`$ tail comes from the short-distance behavior of $`C(x,y;t).`$ That is, the Porod’s region for the DLG may be taken to correspond to $`\lambda _{}k_{}^1\mathrm{}\left(t\right),`$ where $`\lambda _{}`$ stands for a (transverse) thermal length that characterizes the smallest, thermal fluctuations. Let two points, $`\stackrel{}{r}_0`$ and $`\stackrel{}{r}_0+\stackrel{}{r},`$ $`\stackrel{}{r}=(x,y).`$ For any $`x`$ such that $`\lambda _{}x\mathrm{}(t),`$ one roughly has that the product $`n_{\stackrel{}{r}_0}\left(t\right)n_\stackrel{}{r}\left(t\right)`$ equals $`+1`$ if the two points are on the stripe, and $`0`$ otherwise, i.e., if either an interface exists between them or else the two points belong to the gas between stripes. Since $`x\mathrm{}(t)`$, the probability that $`\stackrel{}{r}`$ crosses more than one interface is negligible. For a half-filled system, the probability that $`\stackrel{}{r}_0`$ lies at a particle stripe is $`\frac{1}{2},`$ and the probability that both $`\stackrel{}{r}_0`$ and $`\stackrel{}{r}_0+\stackrel{}{r}`$ belong to the same stripe is roughly $`\frac{1}{2}\left(\mathrm{}\left(t\right)x\right)/\mathrm{}\left(t\right).`$ Hence,

$$C(x,y;t)\frac{1}{2}\left(1\frac{x}{\mathrm{}\left(t\right)}\right),x\mathrm{}\left(t\right).$$
(14)
By power counting, this implies the anisotropic Porod law (in two dimensions):

$$S(k_{};t)\frac{1}{\mathrm{}\left(t\right)k_{}^2},\lambda _{}k_{}^1\mathrm{}\left(t\right).$$
(15)
Therefore, $`\mathrm{\Phi }\left(\varkappa \right)\varkappa ^2L^1,`$ which is confirmed in fig.7. This is in contrast with the (isotropic) Porod’s result. The difference is a consequence of the fact that the DLG clusters are stripes that percolate in the direction of the field, instead of the isotropic clusters of the LG. The short-distance pair correlation function for the latter is $`C(\stackrel{}{r};t)\frac{1}{2}\left(1|r|/\mathrm{}\left(t\right)\right)`$, from which one has that $`\mathrm{\Phi }\left(\varkappa \right)\varkappa ^3.`$ It follows that anisotropy may easily be detected by looking at the tail of the structure factor.

The detailed analysis of $`S(k_{};t)`$ also reveals that, as $`L_{}`$ is increased in computer simulations, the anisotropic behavior $`\mathrm{\Phi }\varkappa ^2`$ crosses over to $`\mathrm{\Phi }\varkappa ^3`$ for larger $`\varkappa `$; see fig.7. We believe this reflects the existence of standard thermal fluctuations. That is, very small clusters of particles occur in the gas in the asymptotic regime whose typical size in the direction perpendicular to the field is of order $`\lambda _{}`$. These very-small asymptotic clusters are rather isotropic, namely, they do not differ essentially from the corresponding ones in equilibrium binary mixtures. More specifically, for $`x\lambda _{},`$ one may approximate $`C(\stackrel{}{r};t)1|r|/\lambda _{}(t),`$ which implies the $`\varkappa ^3`$ power-law tail for large $`\varkappa .`$ On the other hand, according to (5), the mean stripe width grows as $`\mathrm{}(t)(t/L_{})^a`$ with $`a=1/4`$ or $`a=1/3,`$ depending on the value of $`L_{}`$. Therefore, the number of stripes at time $`t`$ is proportional to $`L_{}L_{}^a/t^a`$ and, for a given time, the number of stripes increases with $`L_{}`$ as $`L_{}^a`$. We also know that, at a given time, the number of small, fluctuating clusters is proportional to $`L_{}`$. Hence the relative importance of small clusters due to thermal fluctuations as compared to stripes is proportional to $`L_{}.`$ In fact, the $`\varkappa ^3`$ tail is observed for large enough values of $`L_{}`$ but not for small lattices.

## V A continuum description

The rigorous derivation of a general continuum analog of the driven lattice gas is an open problem.md  Recent studies led to the following proposal for a coarse-grained density, $`\varphi (𝐫,t):`$Rbien

$$_t\varphi (𝐫,t)=\tau _{}_{}^2\varphi _{}^4\varphi +\frac{\lambda }{6}_{}^2\varphi ^3+\tau _{}_{}^2\varphi +_{}\xi (𝐫,t).$$
(16)
Here, the last term stands for a conserved Gaussian noise representing the fast degrees of freedom, and $`\tau _{}`$, $`\tau _{}`$ and $`\lambda `$ are model parameters. Compared to previous proposals,Rmal ; zia  this Langevin type of equation amounts to neglect a nonlinear current term, $`\alpha _{}\varphi ^2,`$ that was believed to be essential (relevant) at criticality. However, one may show that, at least in the limit $`E\mathrm{},`$ the coefficient $`\alpha `$ cancels out (due in this case to a subtle saturation effect).Rbien  In fact, recent scaling analysis has unambiguously confirmed that a particle current is not relevant and that equation (16) captures the correct critical behavior of the DLG.prl01 ; albano  Consequently, an important question is now whether (16) reproduces also the kinetic behavior of the DLG as described in previous sections. We present in this paper a first confirmation that, as compared with other approaches,zia  (16) is indeed a proper continuum description of the DLG kinetic relaxation. A more complete study of the kinetic consequences of this equation will be presented elsewhere.

In order to numerically integrate (16), let us introduce the indexes $`i,j=1,\mathrm{},N`$ to represent, respectively, the two components of $`𝐫(x_{},x_{}).`$ One thus makes a trivial discretization of the space, and then of the time by Cauchy-Euler method.CEmethod  The result is a set of $`N^21`$ coupled nonlinear equations, namely,

$`\varphi (i,j;t+\mathrm{\Delta }t)`$ $`=`$ $`\varphi (i,j,t)+\mathrm{\Delta }t[\tau _{}\stackrel{~}{}_{}^2\varphi \stackrel{~}{}_{}^4\varphi +{\displaystyle \frac{\lambda }{6}}\stackrel{~}{}_{}^2\varphi ^3`$ (17)
$`+\tau _{}\stackrel{~}{}_{}^2\varphi ]+\sqrt{\mathrm{\Delta }t}\stackrel{~}{}_{}\xi (i,j;t).`$
This equation is to be solved by the computer. With this aim, we may write $`\stackrel{~}{}_{}\xi (i,j;t)=\left[\xi (i+1,j;t)\xi (i1,j;t)\right]/2\mathrm{\Delta }x_{}`$ and $`\varphi (i,j;t)\varphi (i\mathrm{\Delta }x_{},j\mathrm{\Delta }x_{};t)`$ where $`\mathrm{\Delta }x_{}=L_{}/N`$ and $`\mathrm{\Delta }x_{}=L_{}/N.`$ The maximum value of $`\mathrm{\Delta }x_{}`$ is thus limited by the interface width. For fig.8, which concerns a $`256\times 256`$ lattice $`(N=256)`$ we —rather arbitrarily— used $`\mathrm{\Delta }x_{}=\mathrm{\Delta }x_{}=1.7,`$ and $`\mathrm{\Delta }t=0.05,`$ which produce a locally stable solution. The parameters $`\tau _{}`$, $`\tau _{}`$ and $`\lambda `$, are fixed on the basis of its physical meaning. The mass terms $`\tau _{}`$ and $`\tau _{}`$ represent temperatures along the longitudinal and transverse directions, respectively, relative to the critical temperature, i.e., $`\tau _{}(T_{}T_C^{\mathrm{}}).`$ Given the anisotropy of phase segregation, with longitudinal interfaces only, $`\tau _{}<0`$ and $`\tau _{}>0.`$ On the other hand, $`\left|\tau _{}\right|`$ should be small enough to allow for a relatively fast evolution. Our choices for fig.8 are $`\tau _{}=0.25`$, $`\tau _{}=0.5`$ and $`\lambda =1`$.

It is remarkable that, in spite of some apparent similarity, the problem here differs from the one in the study of (standard) spinodal decomposition by means of the isotropic ($`E=0`$) Cahn-Hilliard equation. In equilibrium,CHeq  one usually assumes that the influence of noise on growth, which is then assumed to be directly driven by surface tension, is negligible far from criticality. The noise term in (17) may be expected to be important in a more general context, however. That is, as described in §III, the DLG develops striped patterns in which surface tension smooths the interfaces but has no other dominant role on the basic kinetic events. Consequently, neglecting the noise in (17) would turn metastable any striped geometry after coarsening of strings, which is not acceptable (see §III).

Finally, it is interesting to notice that if a one-dimensional structure is assumed, and the gradient in the direction parallel to the field in Eq. 16 is eliminated, then this equation reduces to the one-dimensional time-dependent Ginzburg-Landau model in kawakatsu . There it was found a $`\mathrm{ln}(t)`$ growth at zero temperature and a crossover from $`\mathrm{ln}(t)`$ to $`t^{1/3}`$ at finite temperatures.

## VI Conclusion

This paper presents a theoretical description of spinodal decomposition in the DLG, and compares it with new data from a kinetic Monte Carlo study. This is also compared with the kinetic implications of a Langevin, continuum equation that had previously been shown to capture correctly the critical behavior of the DLG. The resulting picture from these three approaches, which is summarized below, should probably hold for a class of higly-anisotropic phase segregation phenomena. In fact, our results provide a method for analyzing experiments that could be checked against laboratory realizations of the DLG, i.e., the case of phase segregation under biased fields or other influences such as electric fields, gravity and elastic stresses.

Immediately after a deep quench, there is an early regime in which anisotropic grains develop. They tend to coarsen to form small strings that then combine into well-defined thin stripes. Such nucleation and early coarsening (fig.1) seem governed by surface tension at the string ends competing with other both surface and bulk processes. This complicated situation typically extends less than 10<sup>3</sup> MC steps in computer simulations, which corresponds to a very short macroscopic time, so that it would be hardly observable in experiments. As a matter of fact, most of the system relaxation proceeds by coarsening of stripes until full segregation (fig.2). Surprisingly enough, this regime, which has been studied for more than a decade now,aurora -mukamel  happens to be theoretically simpler than the corresponding one for the isotropic case.rev1 -toral

The evolution from many stripes to a single one mainly proceeds by competition of two mechanisms: (A) evaporation of a particle from one stripe surface and subsequent deposition at the same surface, and (B) diffusion of a hole within the bulk of the stripe. The first one dominates initially (and lasts more for smaller systems), when the surface/volume ratio is relatively large. Mechanism A implies that the relevant length (as defined in fig.3) increases with time according to $`\mathrm{}\left(t\right)t^{1/4}.`$ The surface/volume ratio decreases with time, however, and mechanism B soon becomes dominant. This implies $`\mathrm{}\left(t\right)t^{1/3}`$ which is the general prediction for a macroscopic system (cf. figures 4 and 5).voter  This was obtained before by assuming coarsening of two (liquid) stripes by evaporation of the gas stripe placed between them;mukamel  see also aurora  Note that the $`t^{1/3}`$ law is precisely the behavior which is acknowledged to be dominant under isotropy, but this has a different origin in the equilibrium case.rev4 ; rev5  Note also that surface tension determines evaporation rates but has no other influence on mechanisms A and B.

The $`t^{1/3}`$ growth law, (6), is perfectly confirmed by the DLG data (fig.4b). This indicates time-scale invariance. In fact, such invariance was demonstrated for the isotropic case, in which the situation is somewhat more involved (§1). The invariance property may be better analyzed by looking at the structure factor transversely to the drive, $`S(k_{},t)`$ (fig.6). This exhibits dynamic scaling, i.e., it remains self-similar during phase segregation.man  More specifically, $`\mathrm{\Phi }(\varkappa )S(k_{};t)/\mathrm{}L,`$ with $`\varkappa =k_{}\mathrm{}L^1`$, is universal, namely, the same at any (sufficiently late) time $`t`$ and for any square lattice of side $`L.`$ Furthermore, the function $`\mathrm{\Phi }(\varkappa )`$ has a well-defined shape. In particular, it exhibits the Guinier Gaussian peak, and this is followed by the anisotropic Porod decay, $`\mathrm{\Phi }\left(\varkappa \right)\varkappa ^2`$ and then by a thermal tail $`\mathrm{\Phi }\left(\varkappa \right)\varkappa ^3`$ (fig. 7). Also noticeable is the fact that the the parameter to scale along the $`S`$ axis is $`J(t)=\mathrm{}`$ and not $`\mathrm{}^2`$ as under isotropy.

Our results in this paper have two main restrictions, both due to the great computational effort required by this problem.md  Firstly, they follow from an extensive analysis of only one phase-diagram point, namely, $`\rho =\frac{1}{2},`$ $`E=\mathrm{},`$ and $`T=0.8T_C^0.`$ However, our own observations (including brief investigation of other points), together with an extrapolation of the many results known for the isotropic case, strongly suggest that the picture in this paper holds within a large domain around the center of the miscibility gap.fuera  In fact, the scaled structure factor for isotropic systems was shown to be almost independent of density and temperature, and even the substance investigated, in a wide region below the coexistence line.LSWbis  Our consideration of only a two-dimensional system does not seem a real restriction neither. That is, adding an extra (transverse) dimension should not essentially modify the picture here.LSWter

It would be interesting to look next in the laboratory for both time-scale invariance and $`t^{1/3}`$ growth under highly anisotropic conditions. In fact, there are some evidences of such behavior in sheared fluids (§1), and one may think of some more direct experimental realizations of the driven lattice gas. In particular, coarsening striped patterns very similar to those observed in our system are found in some intringuing experiments on granular binary mixtures under shaking.Mullin  We think that the mechanisms we propose in this paper should help the understanding of such experimental results. In general, we hope our observations will motivate both experiments and future more complete theories.

## Acknowledgments

We acknowledge very useful discussions with Raúl Toral and Miguel Ángel Muñoz, and support from MCYT, projects PB97-0842 and BFM2001-2841. We also acknowledge some useful comments by the referees.


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# Charge-ordered ferromagnetic phase in manganites

## Abstract

A mechanism for charge-ordered ferromagnetic phase in manganites is proposed. The mechanism is based on the double exchange in the presence of diagonal disorder. It is modeled by a combination of the Ising double-exchange and the Falicov-Kimball model. Within the dynamical mean-field theory the charge and spin correlation function are explicitely calculated. It is shown that the system exhibits two successive phase transitions. The first one is the ferromagnetic phase transition, and the second one is a charge ordering. As a result a charge-ordered ferromagnetic phase is stabilized at low temperature.

There has been much recent interest in the properties of doped manganese oxides R1-xAxMnO3 (R=rare earth, A=Ca,Sr). salamon ; dagotto  These materials present a very rich phase diagram involving phases with spin, charge and orbital order. The physically relevant electrons in manganites are those from the Mn $`3d`$ levels, which are split by the cubic crystal field into triply degenerate $`t_{2g}`$ levels and higher-energy doubly degenerate $`e_g`$ levels. Electrons from the $`e_g`$ levels are able to hop between Mn sites and form a conduction band. Electrons from the $`t_{2g}`$ levels are localized. The itinerant electrons and local spins are correlated by the double-exchange (DE) mechanism. zener ; anderson  The main feature of the DE is a cooperative effect where the motion of an itinerant electron favors the ferromagnetic (FM) ordering of local spins and, vice versa, the presence of the FM order facilitates the motion of the itinerant electron. The DE model qualitatively describes some of the magnetic properties of manganites, dagotto ; furukawa  and provides a well-established starting point toward comprehensive understanding of the phase diagram of manganites.

Recently experiments have shown that beside the FM order a charge order can exist in the manganites. loudon ; uehara  The charge order exists in regions with no net magnetization and, surprisingly, can also occur in FM regions. loudon  Doping of A2+ ions creates Mn4+ holes in a Mn3+ background. The presence of two valence states Mn3+ and Mn4+ may lead the compounds to a charge-ordered (CO) state for appropriate doping. However, the DE model alone cannot explain the CO state which coexists in the FM phase. In principle, the nearest-neighbor Coulomb repulsion may stabilize a CO state. However, a large nearest-neighbor repulsion likely destabilizes the homogeneous FM state and may produce a checkerboard charge order in three directions. dagotto  Another possible mechanism for the CO phase stabilization is the coupling of itinerant electrons to the Jahn-Teller distortions. However, the electron Jahn-Teller phonon coupling can only stabilize a CO-FM state where the CO phase transition occurs before the FM transition. yunoki  At half filling experiments have only observed a charge order below the FM transition temperature. loudon ; dagotto  Therefore the Jahn-Teller coupling is unlikely responsible for the appearance of the CO-FM state at least at half filling. In this paper we present a possible alternative explanation for the CO-FM state in the manganites. The key idea is an interplay of the DE and randomness of the A-site substitution. The randomness is inevitably introduced by experiments. The importance of the randomness has been discussed both experimentally and theoretically. salamon ; dagotto  The randomness can substantially decrease the critical temperature of the FM transition. zhong ; letfulov ; kogan  Here we will incorporate the randomness of A-site substitution into the DE model. For simplicity, we adopt the randomness by A-site substitution as a random local potential of the itinerant electrons, although the randomness may cause other effects, for instance, randomness of the hoping or exchange integral. dogoto1  It is well known that the diagonal disorder with binary distribution can be modeled by the Falicov-Kimball (FK) model. falicov  Although the FK model is simple, it contains a rich variety of phases. In particular, it illustrates the disorder-order phase transition driven by electron interaction. kennedy ; brandt1  Incorporating the diagonal disorder of the FK type into the DE model, one may expect that a disorder-order phase transition could present. When the phase transition occurs, a CO-FM phase may be stabilized at low temperature. In order to detect the phase transition we study the charge and spin response of system by using the dynamical mean-field theory (DMFT). GKKR  The DMFT has extensively been used for investigating strongly correlated electron systems. GKKR  Within the DMFT we explicitely calculate the charge and spin correlation function. We find that the system stabilizes a CO-FM state at low temperature.

The system which we study is described by the following Hamiltonian

$`H`$ $`=`$ $`{\displaystyle \frac{t}{\sqrt{d}}}{\displaystyle \underset{<ij>,\sigma }{}}c_{i\sigma }^{}c_{j\sigma }\mu {\displaystyle \underset{i\sigma }{}}n_{i\sigma }2J_H{\displaystyle \underset{i}{}}S_i^zs_i^z+`$ (1)
$`E_w{\displaystyle \underset{i}{}}w_i+U{\displaystyle \underset{i\sigma }{}}n_{i\sigma }w_i,`$
where $`c_{i\sigma }^{}`$($`c_{i\sigma }`$) is the creation (annihilation) operator of an itinerant electron with spin $`\sigma `$ at lattice site $`i`$; $`t/\sqrt{d}`$ is the hoping parameter of the itinerant electrons. Here we have rescaled the hoping parameter with the dimension $`d`$ of the system. $`S_i^z`$ is the $`z`$ component of local spin at lattice site $`i`$, and for simplicity, it takes two values $`\pm 1`$. $`s_i^z=(n_in_i)/2`$, $`n_{i\sigma }=c_{i\sigma }^{}c_{i\sigma }`$, $`w_i`$ is a classical variable that assumes the value $`1`$($`0`$) if site $`i`$ is occupied (not occupied) by A ion. $`U`$ is the disorder strength and is mapped onto the difference in the local potential which splits energetically favor of Mn3+ and Mn4+ ions. The expectation value $`x=_iw_i/N`$, ($`N`$ is the number of lattice sites), corresponds to the concentration of unfavorable Mn4+ sites. The chemical potential $`\mu `$ controls the carrier doping, while $`E_w`$ controls the fraction of the sites having the additional local potential. We shall use the condition $`n+x=1`$, where $`n=_{i\sigma }n_{i\sigma }/N`$ is the electron doping. This condition determines $`E_w`$ for each doping $`n`$. The third term of Hamiltonian (1) is the Hund coupling of itinerant and local electrons. For simplicity we only take into account the Ising part of the Hund coupling. This simplification does not allow any spin-flip processes, which can be important at low temperature where spin-wave excitations may govern the thermodynamics of the system. However, in the DE processes the spin of itinerant electron ferromagnetically aligns with the local spin, hence, the Ising part of the Hund interaction plays a dominant role. The DMFT calculations for the DE model with classical local spins show that the simplification of the Hund coupling does not change the self energy of the single-particle Green function. furukawa  Moreover, within the DMFT the numerical results for quantum local spins do not show a significant difference from the ones for classical local spins. nagai  Thus, one expects that within the DMFT the simplification of the Hund interaction does not result in a serious backwardness. $`J_H`$ is the strength of the Hund coupling, and in the following we will take the limit $`J_H\mathrm{}`$. The first three terms of Hamiltonian (1) constitute a simplified DE model. This simplified model captures the most essential ingredient of the DE processes. The last two terms of Hamiltonian (1) describe a binary randomness of the A-site substitution. They together with the hoping term form the FK model. falicov  It is well known that within the FK model the $`U`$ term induces a disorder-order phase transition. kennedy ; brandt1  At low temperature a checkerboard ordering phase is stabilized. Hence, the model (1) may display an interplay of the FM and CO phase.

We solve model (1) by the DMFT. The DMFT is based on the infinite-dimension limit. In the infinite-dimension limit the self energy is pure local and has no momentum dependence. The Green function of itinerant electrons satisfies the Dyson equation

$$G_\sigma (𝐤,i\omega _n)=\frac{1}{i\omega _n\epsilon (𝐤)+\mu \mathrm{\Sigma }_\sigma (i\omega _n)},$$
(2)
where $`\omega _n=\pi T(2n+1)`$, $`\epsilon (𝐤)=2t_{j=1}^d\mathrm{cos}(k_j)`$, and $`\mathrm{\Sigma }_\sigma (i\omega _n)`$ is the self energy. In the infinite-dimension limit the bare density of states of itinerant electrons becomes $`\rho (\epsilon )=\mathrm{exp}(\epsilon ^2/t^2)/\sqrt{\pi }t`$ and we take $`t`$ as the unit of energy ($`t=1`$). The self energy is determined by solving an effective single-site problem. The effective action of this problem is

$`S_{\text{eff}}={\displaystyle \underset{\sigma }{}}{\displaystyle 𝑑\tau 𝑑\tau ^{}c_\sigma ^{}(\tau )\left(\frac{}{\tau }\delta (\tau \tau ^{})+\mathrm{\Lambda }_\sigma (\tau \tau ^{})\right)c_\sigma (\tau ^{})}`$
$`+{\displaystyle \underset{\sigma }{}}{\displaystyle 𝑑\tau c_\sigma ^{}(\tau )\left(\mu +UwJ_H\sigma S^z\right)c_\sigma (\tau )}+E_ww,`$
where $`\mathrm{\Lambda }_\sigma (\tau )`$ describes the effective medium. This effective single-site problem can exactly be solved. Indeed, the dynamics of the localized spin $`S^z`$ and impurity $`w`$ involved in the effective action are independent, hence, we could independently take the trace over $`S^z`$ and $`w`$ in calculating the partition function. This is similar to the DMFT solving of the FK model. brandt  We obtain the local Green function in the limit $`J_H\mathrm{}`$

$$G_\sigma (i\omega _n)=\frac{W_{0\sigma }}{Z_\sigma (i\omega _n)}+\frac{W_{1\sigma }}{Z_\sigma (i\omega _n)U},$$
(3)
where $`Z_\sigma (i\omega _n)=i\omega _n+\mu \mathrm{\Lambda }_\sigma (i\omega _n)`$, and

$`W_{\alpha \sigma }=\{{\displaystyle \underset{\alpha ^{}=0,1}{}}{\displaystyle \underset{\sigma ^{}}{}}\mathrm{exp}[\beta E_w(\alpha ^{}\alpha )+`$
$`{\displaystyle \underset{n}{}}\mathrm{ln}\left({\displaystyle \frac{Z_\sigma ^{}(i\omega _n)\alpha ^{}U}{Z_\sigma (i\omega _n)\alpha U}}\right)]\}^1`$
with $`\alpha =0,1`$. In taking the limit $`J_H\mathrm{}`$ in deriving Eq. (3) we must first renormalize the chemical potential $`\mu \mu +J_\text{H}`$. The self energy is determined by the Dyson equation for the effective single-site problem

$$\mathrm{\Sigma }_\sigma (i\omega _n)=Z_\sigma (i\omega _n)G_\sigma ^1(i\omega _n).$$
(4)
Within the DMFT, the local Green function must coincide with the single-site Green function of the original lattice, i.e.,

$$G_\sigma (i\omega _n)=\frac{1}{N}\underset{𝐤}{}G_\sigma (𝐤,i\omega _n).$$
(5)
Eqs. (2)-(5) form the complete set of equations, which self consistently determine the self energy and Green function.

We are interested in calculating the charge (c) and spin (s) correlation function

$$\chi ^{\text{c(s)}}(i,j)=(\delta n_i\pm \delta n_i)(\delta n_j\pm \delta n_j)$$
(6)
in the homogeneous paramagnetic (PM) phase ($`\delta n_{i\sigma }=n_{i\sigma }n_{i\sigma }`$). In order to calculate the charge and spin response of system one has to introduce an external field into the Hamiltonian. The charge and spin correlation function can be obtained by differentiating the Green function respected to the external field, and then taking the zero limit of the field. brandt  Following the standard techniques, brandt  one can express the correlation functions in the terms of charge (c) and spin (s) susceptibility $`\chi ^{\text{c(s)}}(𝐪,i\omega _n)`$ in momentum space

$$\chi ^{\text{c(s)}}(𝐪)=T^2\underset{n}{}\chi ^{\text{c(s)}}(𝐪,i\omega _n).$$
(7)
The charge and spin susceptibility can be obtained by differentiation of the Green function. brandt  We obtain

$$\chi ^{\text{c(s)}}(𝐪,i\omega _n)=\frac{2+\underset{\alpha =0,1}{}\left(\frac{\mathrm{\Sigma }(i\omega _n)}{W_\alpha }\right)_{G,W_{1\alpha }}\mathrm{\Gamma }_\alpha ^{\text{c(s)}}(𝐪)}{[\chi _0(𝐪,i\omega _n)]^1\left(\frac{\mathrm{\Sigma }(i\omega _n)}{G(i\omega _n)}\right)_W},$$
(8)
where $`\chi _0(𝐪,i\omega _n)=_𝐤G(𝐤+𝐪,i\omega _n)G(𝐤,i\omega _n)`$.

The matrix $`\widehat{\mathrm{\Gamma }}^{\text{c(s)}}(𝐪)`$ satisfies the following equation

$$\widehat{B}^{\text{c(s)}}(𝐪)\widehat{\mathrm{\Gamma }}^{\text{c(s)}}(𝐪)=\widehat{Q}^{\text{c(s)}}(𝐪),$$
(9)
where $`\widehat{B}^{\text{c(s)}}(𝐪)`$ and $`\widehat{Q}^{\text{c(s)}}(𝐪)`$ have the following elements

$`B_{\alpha \beta }^{\text{c(s)}}(𝐪)=\delta _{\alpha \beta }+`$
$`{\displaystyle \underset{n}{}}{\displaystyle \frac{A_\alpha ^{\text{c(s)}}(i\omega _n)\eta (𝐪,i\omega _n)G(i\omega _n)\left(\frac{\mathrm{\Sigma }(i\omega _n)}{W_\beta }\right)_{G,W_{1\beta }}}{1G^2(i\omega _n)\left(\frac{\mathrm{\Sigma }(i\omega _n)}{G(i\omega _n)}\right)_W+\eta (𝐪,i\omega _n)G(i\omega _n)}},`$ (10)
$`Q_\alpha ^{\text{c(s)}}(𝐪)=`$
$`{\displaystyle \underset{n}{}}{\displaystyle \frac{A_\alpha ^{\text{c(s)}}(i\omega _n)\left(G^2(i\omega _n)\left(\frac{\mathrm{\Sigma }(i\omega _n)}{G(i\omega _n)}\right)_W1\right)}{1G^2(i\omega _n)\left(\frac{\mathrm{\Sigma }(i\omega _n)}{G(i\omega _n)}\right)_W+\eta (𝐪,i\omega _n)G(i\omega _n)}}`$ (11)
with $`\alpha ,\beta =0,1`$. In deriving Eqs. (9)-(11) we have used the standard conversion brandt  $`[\chi _0(𝐪,i\omega _n)]^1=[G_\sigma (i\omega _n)]^2+\eta (𝐪,i\omega _n)[G_\sigma (i\omega _n)]^1,`$ and introduced quantity $`A_\alpha ^{\text{c(s)}}(i\omega _n)=\delta W_\alpha /\delta Z_{}(i\omega _n)\pm \delta W_\alpha /\delta Z_{}(i\omega _n).`$ In the infinite dimension limit all of the wave vector dependence of $`\chi _0(𝐪,i\omega _n)`$ and $`\eta (𝐪,i\omega _n)`$ include in the term $`X(𝐪)=_{j=1}^d\mathrm{cos}q_j/d`$. Hence, the spin and charge correlation function only depend on momentum via $`X(𝐪)`$. Each of the derivatives appearing in Eqs. (8)-(11) can directly be calculated from the DMFT solution of Eqs. (2)-(5). In such the way $`\widehat{B}^{\text{c(s)}}(𝐪)`$ and $`\widehat{Q}^{\text{c(s)}}(𝐪)`$ are calculable once the self-consistent equations of the DMFT are solved. Equation (9) reveals that $`\widehat{\mathrm{\Gamma }}^{\text{c(s)}}(𝐪)`$ will diverge at a temperature where the determinant of $`\widehat{B}^{\text{c(s)}}(𝐪)`$ vanishes, while $`\widehat{Q}^{\text{c(s)}}(𝐪)`$ remains finite. This results in an unphysical change of the sign of corresponding correlation function $`\chi ^{\text{c(s)}}(𝐪)`$ so that the assumption of the homogeneous PM phase fails for lower temperature. By a similar way one could also calculate the spin correlation function $`\chi _S(𝐪)`$ of local spins. After some calculations we obtain

$`\chi _S(𝐪)=\gamma _0(𝐪)+\gamma _1(𝐪),`$ (12)
$`{\displaystyle \underset{\beta =0,1}{}}B_{\alpha \beta }^\text{s}(𝐪)\gamma _\beta (𝐪)={\displaystyle \frac{2W_\alpha }{T}}.`$ (13)
From Eqs. (9), (12)-(13) one can see that the spin correlation function of itinerant electrons and local spins will diverge at the same temperature where the determinant of $`\widehat{B}^\text{s}(𝐪)`$ vanishes. This means that the spin of itinerant electrons parallel aligns with local spin, and thus is an important feature of the DE.

We calculate the charge and spin correlation function (7) by solving the DMFT set of self-consistent Eqs. (2)-(5). We are only interested in the FM and checkerboard CO phase stability. Hence, we only calculate the spin correlation function at $`X_𝐪=1`$ and the charge correlation function at $`X_𝐪=1`$. It is found that the spin correlation function $`\chi ^\text{s}(X_𝐪=1)`$ always diverges at a critical temperature. This is the signal of the FM phase transition. The charge correlation function $`\chi ^\text{c}(X_𝐪=1)`$ only diverges for $`U0`$. This means that without the disorder the system always is homogeneous. In Figs. 1 and 2 we present the critical temperature $`T_c`$ of the FM and CO phase transition as a function of doping and disorder strength. At half filling $`n=0.5`$ both critical temperatures reach their maximal value. The $`T_c`$ of the FM transition always decreases with increasing disorder strength. This means that the disorder substantially decrease $`T_c`$ of the FM transition. zhong ; letfulov ; kogan  At the same time, with increasing $`U`$, $`T_c`$ of the CO phase transition first increases, reaches its maximal value, and then decreases. The behavior of $`T_c`$ of the CO phase transition is similar to the one in the FK model. brandt  At very strong disorder ($`U1`$) the two critical temperatures approach to a same value . One also notices that $`T_c`$ of the CO phase transition always is smaller than the FM transition temperature. Thus, one may expect that the CO state is stabilized in the FM phase at low temperature. However, this CO phase stability is respected to the homogeneous PM phase, and for safety we also study an inhomogeneous phase. We divide the lattice into two penetrating sublattices $`A`$ and $`B`$. This lattice division allows us to study the checkerboard CO phase.

By using the standard technique GKKR  the matrix Green function can be written in the following form

$`\widehat{G}_\sigma ^1(𝐤,i\omega _n)=\left(\begin{array}{cc}i\omega _n+\mu \mathrm{\Sigma }_\sigma ^A(i\omega _n)& \epsilon (𝐤)\\ \epsilon (𝐤)& i\omega _n+\mu \mathrm{\Sigma }_\sigma ^B(i\omega _n)\end{array}\right),`$
where $`\mathrm{\Sigma }_\sigma ^{A(B)}(i\omega _n)`$ is the self energy of the Green function of sublattice $`A`$($`B`$). The self energies are determined by solving the effective problem of single site of the sublattices. GKKR  We find that at low temperature a checkerboard CO-FM state is stabilized. We plot the magnetization $`m_{A(B)}=2_{iA(B)}s_i^z/N`$ of sublattice $`A`$ ($`B`$) as a function of temperature in Fig. 3 (upper panel). In this figure we also plot the temperature dependence of the charge-order parameter $`\mathrm{\Delta }=(_{iA,\sigma }n_{i\sigma }_{jB,\sigma }n_{j\sigma })/N`$. It shows that below a critical temperature the magnetizations of both sublattices exist. They equal to each other until another critical temperature, where the charge-order parameter exists. At low temperature the system is in the checkerboard CO-FM state. In this phase the charge order coexists in the FM state, as experimentally observed. loudon  In the way the system exhibits two successive phase transitions. Initially the system goes to the homogeneous FM phase, and after that to the checkerboard CO phase, that the CO-FM phase is stabilized. We also calculate the free energy of the system. The free energy can only be expressed in terms of local quantities. GKKR  We plot the temperature dependence of the free energy $`F`$ in Fig 3 (lower panel). It shows that the CO-FM state has lowest free energy, hence the state must be stabilized at low temperature.

In conclusions, we have proposed a mechanism for the CO-FM phase which has recently been observed. The mechanism is based on a combination of diagonal disorder and a simple DE model with local Ising spins. Employing the DMFT we have calculated the charge and spin correlation function. It is found that the FM and CO state are stabilized at low temperature. As a result the checkerboard charge order can occur in the FM state. However, the manganites are too complicated a system to be completely described by this simple model. In particular, the phase with inhomogeneous percolation of FM and CO regions is beyond the scope of this paper.

This work was supported by the National Program of Basic Research on Natural Science of Vietnam, Project 4.1.2. The writing was completed at the National Chiao Tung University, and was supported by Project NSC 91-2811-M-009-006 of ROC.