# Mechanisms of Granular Spontaneous Stratification and Segregation in Two-Dimensional Silos

## I Introduction

Segregation is a prominent example of the peculiar properties of granular matter . For example, shaking a container filled with two types of grains of different sizes leads not to mixing—as in liquids—but to segregation, with the large grains on the top of the container and the small grains on the bottom. This striking behavior and the importance of mixing problems from a technological point of view have led to a broad interest in granular materials in the physics community.

Several types of segregation have been investigated, namely, segregation by vibrating a container (the “Brazil nut effect”) , and segregation in rotating cylinders, where the segregation occurs through surface flow .

Segregation can also been obtained in the absence of any periodic oscillation by simply pouring a mixture of grains of different sizes onto a pile. One experimental set-up, which has attracted much recent attention, consists of a quasi-two dimensional cell or vertical Hele-Shaw cell where a mixture of grains is constantly poured next to one end of the cell \[Fig. 1(a)\]. When a mixture of small and large grains is poured into the cell, a pile builds up and the small grains are observed to segregate near the top of the pile and the large ones near the bottom of the pile . This segregation is due to the different grain sizes, because large grains roll down more easily on top of small grains than small grains on top of large grains.

It has been recently observed  that if the shapes of the species are sufficiently different, a novel type of segregation can take place: when such a mixture of small rounded grains and large rough grains is poured between two vertical slabs, a spontaneous stratification of the mixture in alternating layers of small and large grains parallel to the pile surface is observed. Additionally, there is an overall tendency for the large and small grains to segregate into different regions of the cell. Spontaneous stratification is also found for more than two species . The layers are then ordered forming a sequence parallel to the surface pile (from bottom to top, small-medium-large, small-medium-large for 3 species).

This phenomenon could possibly be relevant in different fields, such as geomorphology . For example, stones coming from sand dune solidification (sandstone) present successive alternation of layers of different types of grains. This regularity cannot be explained by periodic sedimentation. But one could imagine that the sand dune was built with sand brought by the wind and flowing down the slip-face of the dune , where stratification could appear as in the experiments of . This phenomenon may also have important consequences in industry where processing and transport of initially mixed grains could lead to stratification.

Spontaneous stratification has been observed in  after a transient regime and only when the large grains are rougher than the small grains. When the large grains are the smoothest stratification does not occur but only the segregation of the mixture in different regions of the cell occurs, with the large and rounded being at the bottom of the cell, and the small and rough at the top. These phenomena can be qualitatively understood as the growth of an instability due to the competition of two opposite effects. (i) On the one hand, if the grains have the same shape (spherical for example) or, more precisely, the same repose angle, then the large grains will roll more easily on the top of the small ones than the reverse. This will lead to segregation, with the small grains at the top of the pile and the large at the bottom. (ii) On the other hand, if the grains have the same size but different shape, the rougher grains will have a larger friction coefficient than the other grains, and we expect segregation with the rougher grains at the top of the sandpile. In the case of large grains rougher than small grains, those two effects will compete, giving rise to an instability, and then to spontaneous stratification. However, in the case where the smaller grains are rougher than the large grains, the two effects will contribute in the same way, and the segregation pattern will be stable, without the occurrence of stratification .

In this paper, we study granular flow in the spirit of , where one assumes a sharp distinction between the rolling or fluid phase composed of the layer of grains flowing down and the static phase or bulk composed of grains forming the sandpile. The essential feature to understand sandpile formation is then to describe how the rolling grains are flowing down and how they interact with the static grains. In this context, it is important to distinguish two different regimes, the thin flow regime and the thick flow regime, where the interaction between rolling grains and static grains are very different. Moreover, experiments have been done in both regimes, so that both regimes are important to study.

Here we propose a mechanism to understand spontaneous stratification and segregation in two-dimensional silos. We adopt two different approaches. First we introduce a cellular automaton model to give insight into the proposed mechanism. This model displays stratification as soon as the large grains are rougher than the small ones, in agreement with experiments . The dynamics are also very close to the experiments , where the layers are built through a “kink” going uphill where the rolling grains are stopped.

Second, we study a continuum model which is built on a phenomenological formalism describing granular flow on sandpiles. This formalism was introduced by Bouchaud et al.  for the case of a single species, and recently generalized by Boutreux and de Gennes (BdG)  to the case of a mixture of two species. The essential feature to understand sandpile formation is to describe the interaction between the rolling or fluid phase and the bulk, as well as any segregation which may occur in the rolling phase itself. In contrast to the cellular automaton model, this formalism includes amplification processes, i.e., the conversion of static grains at the surface of the sandpile into rolling grains by the flow (this feature is essential to understand avalanching when one tilts a sandpile above the maximum angle of repose, or to understand avalanche dynamics in rotating drums).

In the large flux regime, the rolling grains form a thick phase and the grains are kinematically segregated in the rolling phase, an effect called kinematic sieving, free surface segregation, or percolation \[Fig. 1(b)\] . Due to this phenomenon the large grains in the rolling phase are found to rise to the top of the rolling phase while the small grains sink downward through the gaps left by the motion of larger grains in the rolling phase. Thus, small rolling grains form a sub-layer underneath the sub-layer of large rolling grains. Then only the lower grains of this layer interact with the sandpile. Thus, a segregation effect that we refer to as percolation takes place inside the rolling phase where the large grains are convected along the flow to the top of the layer. Thus, if small rolling grains are present, they will preferentially be on the bottom of the layer, preventing the large grains from interacting with the sandpile.

We will develop a continuum formalism that includes the percolation effect, and show that stratification arises in a similar way as in the experiments. When the large grains are rougher, stratification is made of layers spreading all along the sandpile; the layers of the two types of grains being of the same size for an equal volume mixture of grains. When the small grains are rougher than the large grains, we observe the complete segregation of the mixture but not stratification, with the small and roughest grains being found at the top of the pile in agreement with the experiments. A thick rolling phase is a condition for the percolation effect to take place. However a large difference in size is also necessary to observe the percolation effect: we expect $`d_2/d_1\stackrel{>}{}1.5`$, where $`d_1`$ and $`d_2`$ are the typical size of the small and large grains, respectively.

In the small flow regime each rolling grain is always in contact with the sandpile and so interacts with it. In this case a thin rolling phase is expected— of the order $`d_2`$— and percolation effects are expected to be irrelevant. However strong segregation effects are expected, as in the case of percolation, since we will consider the case of large size difference between the grains. The large grains are not being captured on top of static small grains (although they interact with them) because of the large difference in size, while the small grains are easily captured on top of the large static grains. Using the theoretical formalism adapted to this case, we will show that stratification is observed when the large grains are rougher than the small grains, in agreement with the experiments.

Cross-amplification processes—whose influence was greatly reduced in the case of thick flows due to percolation effects—now plays an important role since all grains are interacting with the pile and cross-interactions of the type small/large grains are expected to occur at the fluid-bulk interface. Due to cross-amplification, the transition from stratification to segregation does not occur sharply when the small grains become the roughest. We find a regime where the small grains are slightly rougher than the large grains, which also gives rise to stratification. When the small grains are more rounded than the large grains, then we find the segregation of the grains in agreement with experiments.

In general, we find that the thick flow regime and the thin flow regime show similar results regarding the stratification and segregation of the species. This is valid provided that the grains differ appreciably in size (in term of the size ratio we expect $`d_2/d_1\stackrel{>}{}1.5`$ ). Then we study analytically a mechanism for stratification and segregation valid for both regimes. We study the “kink” mechanism, and we obtain predictions for the wavelength of the layers as a function of the different parameters of the system. In particular we find that the wavelength of the layers is proportional to the flux of adding grains (i.e., proportional to the thickness of the rolling phase), and we also find a crossover behavior at the thin-thick flow transition. Finally we discuss our results in regard to previous approaches to segregation  and stratification  and to the experiments . A short report of some of the results presented here has been published in .

## II Cellular Automaton Model

### A Motivation and Definitions

We first introduce a simplified discrete model to understand the mechanism leading to stratification. Discrete models have been used before for modeling the complex behavior of granular materials. The role played by the angle of repose has been used to understand the complex dynamics of granular flows of mixtures . The concept of angle of repose normally involves a macroscopic definition—i.e., the angle of repose is the angle of the pile surface after the grains are poured onto a heap. Here, we will define a microscopic angle of repose as the maximum angle at which a rolling grain is trapped at the surface of the pile. This definition must be understood in terms of a coarse grained distance along the surface of the pile—of the order of a few grain sizes—over which all the quantities involved in the model are averaged.

In the case of a single-species sandpile, as sand is added to the sandpile we consider a critical angle of repose $`\theta _r`$. When the local angle of the pile is smaller than $`\theta _r`$ the rolling grain is stable and there is no flow. When the local angle of the pile is larger than $`\theta _r`$ the rolling grain is unstable and flow occurs.

We develop a simple discrete model, based on the idea that grains flow when the local angle of the sandpile is larger than the angle of repose. We consider that the angle of repose depends on the type of rolling grains and also on the composition of the surface. Thus, in the case of granular mixtures of two different species, we consider the existence of four different generalized angles of repose.

The sandpile is built on a lattice, where the grains have the same horizontal and vertical size as the lattice spacing. The two species will be distinguished according to different generalized angles of repose. In general, we will call species type $`1`$ to the small grains, and species type $`2`$ to the large grains. The species can also have rough or smooth surface properties, which, together with the different size, will define the different angles of repose of the species. Following , we regard each grain as belonging to one of two phases:

* Static phase: if the grain is part of the sandpile,
* Rolling phase: if the grain is not part of the sandpile and rolls downward with a constant drift velocity.

We consider the local slope

$$s_ih_ih_{i+1}$$
(1)   
of the static grains as the variable controlling the dynamics of the rolling grains. Here, $`h_i`$ denotes the height of the sandpile at coordinate $`i`$, and we assume the pouring point at $`i=1`$.

At each time step a set of $`N_1`$ small grains and $`N_2`$ large grains is deposited at the top of column $`1`$ of the pile \[see Fig. 2(a)\]. These grains are considered to belong to the rolling phase. In the case of thin flow we assume that the rolling phase is homogeneous and both types of species are mixed in the fluid phase and interact with the surface. Then one rolling grain of each species interacts with the surface at each time step, and can be converted from the rolling phase to the static phase. In the thick flow regime, the percolation effect is expected to take place, and the small grains screen the interaction of the large rolling grains with the pile surface. Thus in the thick flow regime, we consider that the large grains interact with the pile surface only when the number of small rolling grains at a given position falls below a given threshold $`ϵN_2`$.

The remaining rolling grains which do not interact with the pile surface are convected “downward” with unit “drift velocity”—i.e., they move to the next column at each time step.

The dynamics of each rolling grain interacting with the sandpile surface is governed by its local angle of repose. We consider that the repose angle depends on the local composition on the surface, so we define $`\theta _{\alpha \beta }`$ as the generalized repose angle of a rolling grain of type $`\alpha `$ on a surface with local grains of type $`\beta `$. We propose that

$$\theta _{21}<\theta _{12}$$
(2)   
to take into account the fact that large rolling grains roll more easily on top of small static grains than small grains roll on top of large static grains \[since the surface “looks” smoother for large grains rolling on top of small grains, see Fig. 2(b)\]. The repose angles of pure species $`\theta _{\alpha \alpha }`$ lie between $`\theta _{21}`$ and $`\theta _{12}`$.

Since a large grain roll easier than a small rolling grains on top of a layer of small static grains, we have

$$\theta _{21}<\theta _{11}.$$
(3)   
Conversely, a large grain roll easier than a small grain on top of a layer of large static grains, so that

$$\theta _{22}<\theta _{12}.$$
(4)   
The stratification experiments  use a mixture smaller less faceted grains and larger more faceted grains. Thus, the last inequality between the angles of repose is provided by the fact that the grains differ in shape of friction properties. Since the small species are the most rounded, then the repose angle of the smaller pure species is smaller than the repose angle of the large pure species—i.e.,

$$\theta _{11}<\theta _{22}.$$
(5)   
Therefore, to mimic the experimental conditions for stratification , we propose

$$\theta _{21}<\theta _{11}<\theta _{22}<\theta _{12}.$$
(6)   
We notice that the conditions (2)-(4) are a consequence of the different size of the species, while the condition $`\theta _{11}\theta _{22}`$ is achieved for mixtures of grains with different shapes, and does not depend on the size of the grains. Thus the model incorporates the size segregation and shape segregation in the definition of the angles of repose. In general the grains with the larger angle of repose will tend to be captured first. Thus the small grains will tend to be captured at the top of the pile, and the smoothest grains at the bottom of the pile. The percolation effects tend to segregate the small grains at the top of the pile, thus, it acts in the same way as the size segregation due to different angles of repose Eqs. (2)-(4).

At each time step, the rolling grain interacting with the sandpile surface at coordinate $`i`$ either will stop (by being converted into a static grain) if the local slope of the surface

$$h_ih_{i+1}s_{\alpha \beta }\mathrm{tan}\theta _{\alpha \beta },$$
(7)   
where $`s_{\alpha \beta }`$ is the local slope, or will continue to roll (together with the remaining rolling grains) to column $`i+1`$ if

$$h_ih_{i+1}>s_{\alpha \beta }.$$
(8)   
We iterate this algorithm to form a large sandpile of typically $`10^5`$ grains. We assume that the substrate is made of a layer of large grains.

The discrete model in the thick flow and thin flow regime gives rise to very similar results. Then in the following we will concentrate only on the thick flow regime where most of the experiments are done, and where the grains are segregated in the rolling phase. Indeed, we will see that the differences between the thin flow regime and the thick flow regime arise only when cross-amplification processes are taken into account. Since the discrete model neglects these type of processes, then it gives rise to similar results for both flow regimes.

### B Kink Mechanism

Figure 3a shows the resulting morphology predicted by the discrete model when the large grains are rougher than the small grains. This fact is quantified by taking into account that the angle of repose of the pure large species is larger than the angle of repose of the pure small species, $`\theta _{22}>\theta _{11}`$. The stratification is qualitatively the same as that found experimentally , both in regard to the statics of the sandpile \[seen in Fig. 3(a)\], and also in regard to the dynamics (seen in Fig. 4).

The mechanism for spontaneous stratification involves the formation of a kink at which the grains are stopped during an avalanche. After a pair of static layers is formed with a layer of large grains on top of a layer of small grains, the angle of the sandpile is close to $`\theta _{22}`$ \[Fig. 4(a)\]. Since the surface of the sandpile is made of large grains and $`\theta _{22}<\theta _{12}`$, a thin layer of small grains is trapped on top of the layer of large grains as more grains are poured onto the cell. These small grains smooth the surface without changing significantly the sandpile angle, and allow rolling small grains to go further down (since $`\theta _{11}<\theta _{22}`$) \[Fig. 4(b)\]. The large grains are rolling down on this thin layer of small grains without being captured ($`\theta _{21}<\theta _{22}`$), and are the first to reach the bottom of the sandpile, giving rise to segregation \[Fig. 4(b)\]. When the flow reaches the base of the pile, the grains develop a profile which displays a kink where the grains are stopped: the small grains are stopped first at the kink since $`\theta _{21}<\theta _{11}`$, and a pair of layers begins to form, with the small grains underneath the large grains \[Fig. 4(c)\]. The kink moves upward (in the opposite direction to the flow of grains) until it reaches the top of the pile and a complete pair of layers has been formed \[Fig. 4(d)\].

If, on the other hand, we consider $`\theta _{22}<\theta _{11}`$ in the model—corresponding to a mixture of smaller “more faceted” grains, and larger “less faceted” grains—we find the complete segregation of the mixture but no stratification \[Fig. 3(b)\]. In this case, the small and faceted grains are to be found near the top of the pile, while the large and rounded grains are found near the bottom of the pile. Thus, the control parameter for spontaneous stratification appears to be the difference in the repose angle of the pure species, which quantifies the difference in shape of the grains.

As seen in Fig. 3(a), before the layers appear there is an initial regime where only segregation is found. At the onset of the instability leading to stratification, a few large grains are captured on top of the region of small grains near the center of the pile where the angle of the pile is $`\theta \theta _{11}`$. The repose angle for large rolling grains is now $`\theta _{22}`$. Thus, if $`\theta \theta _{11}<\theta _{22}`$, more large grains can be trapped (since the angle of the surface is smaller than the repose angle), leading to the first sub-layer of large grains and then to stratification. On the other hand, if $`\theta \theta _{11}>\theta _{22}`$, no more large grains can get captured, the fluctuation disappears, and the segregation profile remains stable. Thus this picture suggests that, in agreement with , the segregation profile observed in the initial regime is “stable” so long as $`\theta _{22}<\theta _{11}`$, and unstable (evolving to stratification for large enough systems) when $`\theta _{11}<\theta _{22}`$. This explains qualitatively why the control parameter for the stratification-segregation transition is the angle of repose of the pure species.

## III Continuum Theory for granular flow

A theoretical approach to segregation in granular flow is not a simple task. On one hand, extensive numerical simulations (such as molecular dynamics , or lattice gas models ) have been able to reproduce several segregation phenomena observed experimentally. On the other hand, an analytical approach of segregation, considering granular medium as continuum, would be instructive, since it would allow to reduce the problem to a small set of parameters that control the system, and then to get a clear phenomenological understanding of the problem. However, an important question is whether the grains can be treated as a continuum medium. A continuum approach means that we will be able to replace the grains belonging to a same region of space by some average quantities, for example the density, or the averaged speed. But specific grains can play a peculiar role, i.e., in the case of arching effects, where an arrangement of several grains in a special way (an arch) supports the above grains, prevents the flow by gravity, and creates large discontinuities for the local density or the force .

In this section, we study spontaneous stratification using a continuum formalism. We will show that the results obtained are very close to the experiment, and then we extract the important parameters of the problem. Our results shows that a continuum formalism is able to reproduce a complex phenomenon in granular matter such as spontaneous stratification.

The continuum theory of granular flow for a single-species sandpile was proposed by Mehta et al.  and Bouchaud et al. . Bouchaud et al. recognized the necessity of treating differently the rolling grains (rolling on the surface of the surface), and the static grains that form the sandpile. The rolling grains are in a “liquid” state, flowing down by gravity and interacting with the static grains in the “solid” state. The dynamics of the sandpile is then given by how the rolling grains move on the surface and how they interact with the sandpile. The equations for those two quantities for the case of single-species sandpiles are

$`{\displaystyle \frac{d}{dt}}R[x(t)]`$ $`=`$ $`\mathrm{\Gamma }(R,h),`$ (10)   
$`{\displaystyle \frac{h(x,t)}{t}}`$ $`=`$ $`\mathrm{\Gamma }(R,h).`$ (11)   
Here $`R[x(t)]`$ is the height of the layer of rolling grains in the Lagrange representation (following the rolling grains), and $`h(x,t)`$ the height of the sandpile \[Fig. 1(a)\]. The rolling grains interact with the sandpile through $`\mathrm{\Gamma }(R,h)`$, which represents the height of rolling grains becoming part of the sandpile. Equations (III) conserve the number of grains.

We need to define how the rolling grains move on the surface, and how they interact with the sandpile. Two forces are acting on the rolling grain: (i) gravity and (ii) friction coming from the collisions of the rolling grain with the grains of the sandpile. The number of collisions at the scale of interest for continuum equations (several times the size of a grain) is large enough to say that at this scale, the speed is always at its limit value where the two forces balance exactly, and the motion of a grain is overdamped. Equations (10) and (11) can be rewritten in Euler representation (looking at the height of grains at a given position $`x`$)

$`{\displaystyle \frac{R(x,t)}{t}}`$ $`=`$ $`v{\displaystyle \frac{R(x,t)}{x}}+\mathrm{\Gamma }(R,h),`$ (13)   
$`{\displaystyle \frac{h(x,t)}{t}}`$ $`=`$ $`\mathrm{\Gamma }(R,h).`$ (14)   
Here $`R(x,t)`$ is now a function of the time and the position $`x`$, and we assume the pouring point at $`x=0`$. The rolling grains are moving down at a speed $`v(x,t)`$ in the positive $`x`$ direction, where $`v(x,t)`$ could depend on the local slope of the sandpile. However, in the spirit of capturing only the essential physical mechanisms to recover the observed phenomena, we will consider the speed $`v`$ to be constant all over the sandpile.

Bouchaud et al.  proposed a form for $`\mathrm{\Gamma }(R,h)`$ in the general case, that has been simplified by de Gennes  for the simpler case of a continuous flow of rolling grains. In this case, there is no discrete avalanching and only the repose angle must be included in the formalism . The interaction term $`\mathrm{\Gamma }(R,h)`$ is

$$\mathrm{\Gamma }(R,h)=\gamma [\theta (x,t)\theta _r]R,$$
(15)   
where

$$\theta (x,t)\frac{h(x,t)}{x}$$
(16)   
is the local angle of the surface (we will make no distinction between the angle of the surface and the tangent of the angle).

Equation (15) states that the rate of the interaction is proportional to the number of grains interacting with the sandpile. Rolling grains will become part of the sandpile if the angle of the surface $`\theta (x,t)`$ is smaller than the repose angle $`\theta _r`$ (“capture”), while static grains will become rolling grains if $`\theta (x,t)`$ is larger than $`\theta _r`$ (“amplification”). The constant $`\gamma `$ is the inverse of the time on which this interaction is effective because the distance on which a rolling grain is stopped when $`\theta (x,t)`$ is smaller than $`\theta _r`$ is $`v/\gamma `$. This distance must scale with the size of the grain $`d`$. Thus 

$$v/\gamma d.$$
(17)   
The linear dependence of $`\mathrm{\Gamma }(R,h)`$ on the quantity $`[\theta (x,t)\theta _r]`$ can be understood as a first order development of a more complicated function of $`\theta (x,t)`$. As soon as the angle of the sandpile is far from the repose angle, non-linear terms must be added (avoiding the non-physical divergences that could be found with the linear development). Finally the proportionality of $`\mathrm{\Gamma }(R,h)`$ to $`R(x,t)`$ is meaningful in the case where all the grains interact at each time with the surface (thin-flow limit). This imposes the height of the rolling layer to be of the order of the grain size $`R(x,t)d.`$ However we will argue that this approximation might be still valid in the case of thick flows as well, since the interaction might be proportional to the pressure exerted by the fluid phase, which in turn is proportional to $`R(x,t)`$ for a fluid .

To treat the problem of segregation in granular flow composed of binary mixtures, Boutreux and de Gennes (BdG)  have extended this formalism to the case of flows made of two types of grains, identifying three variables: the two heights of rolling grains $`R_\alpha (x,t)`$ (i.e. the total thickness of the rolling phase multiplied by the local volume fraction of the $`\alpha `$ grains in the rolling phase at position $`x`$), and the height of the sandpile $`h(x,t)`$. BdG generalized Eqs. (III) to

$`{\displaystyle \frac{R_\alpha }{t}}`$ $`=`$ $`v_\alpha {\displaystyle \frac{R_\alpha }{x}}+\mathrm{\Gamma }_\alpha ,\text{ }\alpha =1,2`$ (19)   
$`{\displaystyle \frac{h}{t}}`$ $`=`$ $`\mathrm{\Gamma }_1\mathrm{\Gamma }_2,`$ (20)   
where the interaction term $`\mathrm{\Gamma }_\alpha `$ takes into account the conversion of the rolling grains into static grains, and is defined through the collision matrix $`M_{\alpha \beta }`$

$$\mathrm{\Gamma }_\alpha \underset{\beta =1}{\overset{2}{}}M_{\alpha \beta }R_\beta .$$
(21)   
The collision matrix, governing capture and amplification, depends on the local angle of the pile $`\theta (x,t)`$ and on the local composition of the surface of the sandpile $`\varphi _\alpha (x,h)`$, which is a function of $`x`$ and $`h`$. However, writing an equation of evolution for $`\varphi _\alpha (x,h)`$ is not easy. When both rolling species are captured, the height of the sandpile increases, and $`\varphi _\alpha (x,h)`$ is given by

$$\varphi _\alpha (x,h)=\frac{\mathrm{\Gamma }_\alpha }{h/t},$$
(22)   
and

$$\varphi _1+\varphi _2=1.$$
(23)   
As soon as amplification dominates for one or both species, Eq. (22) is no longer valid. When $`\mathrm{\Gamma }_\alpha >0`$ for both species, the height of the sandpile decreases, and $`\varphi _\alpha (x,h)`$ does not have to be updated. Finally, when grains of type $`\alpha `$ are captured and grains of type $`\beta `$ are amplified, the composition will be $`\varphi _\alpha (x,h)=1`$.

The general form of the collision matrix is defined by taking into account a set of binary collisions between a rolling and a static grains 

$$\widehat{\text{M}}\left(\begin{array}{cc}a_1(\theta )\varphi _1b_1(\theta )\hfill & \hfill x_2(\theta )\varphi _1\\ x_1(\theta )\varphi _2\hfill & \hfill a_2(\theta )\varphi _2b_2(\theta )\end{array}\right).$$
(24)   
This definition involves a set of a priori unknown collision functions contributing to the rate processes: $`a_\alpha (\theta )`$ is the contribution due to an amplification process (when a static grain of type $`\alpha `$ is converted into a rolling grain due to a collision by a rolling grain of type $`\alpha `$), $`b_\alpha (\theta )`$ is the contribution due to capture of a rolling grain of type $`\alpha `$ (when a rolling grain of type $`\alpha `$ is converted into a static grain), and $`x_\alpha (\theta )`$ is the contribution due to a cross-amplification process, (the amplification of a static grain of type $`\beta `$ due to a collision by a rolling grain of type $`\alpha `$).

BdG  proposed an analytically tractable form for the collision matrix which includes capture and amplification, in the case where the two species have the same size but differ in respect to their repose angle. BdG found the steady state solution in the geometry of the silo, in the case where the repose angle does not depend on the composition of the surface. The BdG model explains the segregation of the two type of grains in different regions of the sandpile, but not the phenomenon of spontaneous stratification. A generalization of the model to include also the different sizes of the grains  shows a smooth segregation of the species with the concentrations of static grains behaving as a power law of the position along the surface pile; results valid only when the species do not differ too much (a fact that allows to perform linear approximations of the collision functions around the angles of repose ). In the following we propose a form of the collision functions valid when there is a large difference in size and shape between the species and we treat the thin and thick flow regimes, in order to understand stratification and segregation as seen in the experiments.

## IV Continuum Model for Stratification of Granular Mixtures

### A The collision matrix and the generalized angle of repose

We present the collision matrix $`M_{\alpha \beta }`$ that includes the effects of capture and amplification, and the dependence of the repose angle on the composition of the surface as discussed in . Considering one type of rolling grain $`\alpha `$, we define capture and amplification as follows: if the local angle of the surface $`\theta (x,t)=h(x,t)/x`$ is smaller than the generalized angle of repose of the rolling specie $`\alpha `$ $`\theta _\alpha `$, the $`\alpha `$ rolling grains will be captured. In the reverse case $`\theta (x,t)>\theta _\alpha `$, the static grains at position $`x`$ will be amplified. Amplification will cause locally a small hole, i.e., the two types of static grains will be amplified the same way according to their local concentration $`\varphi _\alpha `$.

The generalized repose angle $`\theta _\alpha `$ of each type of rolling grain is now a continuous function of the composition of the surface $`\theta _\alpha =\theta _\alpha (\varphi _\beta )`$ (see Fig. 5)

$$\begin{array}{ccc}\hfill \theta _1(\varphi _2)& =& m\varphi _2+\theta _{11}\hfill \\ \hfill \theta _2(\varphi _2)& =& m\varphi _2+\theta _{21}=m\varphi _1+\theta _{22},\hfill \end{array}$$
(25)   
where $`m\theta _{12}\theta _{11}=\theta _{22}\theta _{21}`$. We have assumed the difference

$$\psi \theta _1(\varphi _2)\theta _2(\varphi _2)$$
(26)   
to be independent of the concentration $`\varphi _2`$. For simplicity, we choose a linear interpolation between the extreme values $`\theta _\alpha (\varphi _\beta =0)`$ and $`\theta _\alpha (\varphi _\beta =1)`$. If we label the small grains with $`\alpha =1`$ and the large grains with $`\alpha =2`$ and denote the extreme values of the repose angle by $`\theta _\alpha (\varphi _\beta =1)=\theta _{\alpha \beta }`$ as in Sec. II, the difference in size implies \[see Fig. 2(b)\]

$$\theta _{12}<\theta _{21}.$$
(27)   
If species 1 are the smallest then $`\theta _1(\varphi _2)>\theta _2(\varphi _2)`$ for any composition of the surface $`\varphi _2`$— i.e., the small grains are always the first to be captured. Thus, the angular difference $`\psi `$ is determined mainly by the difference in size between the species, and the value of $`\psi `$ determines the degree of segregation; the larger $`\psi `$, the stronger the segregation. The repose angles of the pure species $`\theta _{11}`$ and $`\theta _{22}`$ will be intermediate between $`\theta _{12}`$ and $`\theta _{22}`$, and their relative values will depend on the shape of the two species as discussed in Sec. II A.

For mixtures of grains with different shapes or friction coefficients we have $`\theta _{11}\theta _{22}`$, and $`\theta _{12}=\theta _{21}`$ if the species have the same size. If $`\theta _{11}`$ is the repose angle of the pure round species and $`\theta _{22}`$ is the repose angle of the pure rough species, then $`\theta _{11}<\theta _{22}`$. If the species have the same shape or friction coefficients then $`\theta _{11}=\theta _{22}`$.

When the size ratio is close to one ($`d_2/d_1\stackrel{<}{}1.5`$), the angle $`\psi `$ is expected to be small and then it is plausible to linearize the collision functions around the angles of repose as done in . When the is a larger difference in size ($`d_2/d_1\stackrel{>}{}1.5`$), we expect $`\psi `$ to be large, and we approximate the collision functions and define the following collision matrix:

$$M_{\alpha \beta }=\left(\begin{array}{cc}\gamma _{11}\delta \theta _1\mathrm{\Theta }_{\text{self}}[\delta \theta _1,\varphi _1]& \begin{array}{cc}\gamma _{12}\delta \theta _2\mathrm{\Theta }_{\text{cross}}[\delta \theta _2,\varphi _1]\hfill & \end{array}\\ & \\ \gamma _{21}\delta \theta _1\mathrm{\Theta }_{\text{cross}}[\delta \theta _1,\varphi _2]& \gamma _{22}\delta \theta _2\mathrm{\Theta }_{\text{self}}[\delta \theta _2,\varphi _2]\end{array}\right),$$
(28)   
where

$$\delta \theta _\alpha \theta (x,t)\theta _\alpha .$$
(29)   
Here, $`\gamma _{\alpha \alpha }>0`$ has dimension of inverse time, and $`v/\gamma _{\alpha \alpha }`$ represents the length scale at which a rolling grain will interact significantly with a surface at an angle above or below the angle of repose.

The functions $`\mathrm{\Theta }(\delta \theta _\alpha ,\varphi _\alpha )`$ distinguish capture from amplification. $`\mathrm{\Theta }_{\text{self}}`$ treats the case of self amplification, i.e., amplification of static grains $`\alpha `$ by rolling grains $`\alpha `$, and $`\mathrm{\Theta }_{\text{cross}}`$ the case of cross-amplification, i.e., amplification of static grains $`\alpha `$ by rolling grains $`\beta `$. More specifically, we consider

$$\mathrm{\Theta }_{\text{self}}(\theta \theta _\alpha ,\varphi _\alpha )=\{\begin{array}{cc}1\hfill & \text{ if }\theta \theta _\alpha <0\hfill \\ \varphi _\alpha \hfill & \text{ if }\theta \theta _\alpha >0\hfill \end{array}.$$
(30)   
These equations mean that in the case of capture, the amount of rolling grains of type $`\alpha `$ converted to static grains is proportional to the number of grains interacting with the surface, i.e., $`R_\alpha `$; in the case of amplification, the amount of static grains converted to rolling grains is proportional to $`R_\alpha `$ again and to the number of static grains $`\alpha `$ on the surface, i.e., $`\varphi _\alpha `$. Accordingly, we obtain

$$\mathrm{\Theta }_{\text{cross}}(\theta \theta _\alpha ,\varphi _\beta )=\{\begin{array}{cc}0\hfill & \text{ if }\theta \theta _\alpha <0\hfill \\ \varphi _\beta \hfill & \text{ if }\theta \theta _\alpha >0\hfill \end{array}.$$
(31)   
In terms of the collision functions defined in (24) we have

$$\begin{array}{cccc}a_\alpha (\theta )\hfill & \hfill & \gamma _{\alpha \alpha }& \mathrm{\Pi }[\theta (x,t)\theta _\alpha (\varphi _\beta )],\hfill \\ b_\alpha (\theta )\hfill & \hfill & \gamma _{\alpha \alpha }& \mathrm{\Pi }[\theta _\alpha (\varphi _\beta )\theta (x,t)],\hfill \\ x_\beta (\theta )\hfill & \hfill & \gamma _{\beta \alpha }& \mathrm{\Pi }[\theta (x,t)\theta _\beta (\varphi _\beta )],\hfill \end{array}$$
(33)   
where

$$\mathrm{\Pi }[x]\{\begin{array}{cc}0& \hfill \text{if }x<0\\ x& \hfill \text{if }x0\end{array}.$$
(34)   
This form for the matrix $`M_{\alpha \beta }`$ supposes that amplification (respectively capture) occurs only when the local angle is larger (respectively smaller) than the repose angle. Thus, for a given angle only capture or amplification can occur at a given time; an assumption which is expected to be valid when the grains differ appreciable ($`\psi `$ large). This fact gives rise to strong segregation effects with exponential behavior of the concentrations as we will corroborate when calculating the steady state solution of the problem in Sec. V A. In contrast, the form of the collision functions proposed in  assumes that amplification and capture are linear functions of the local angle. For a given angle both amplification and capture act simultaneously, and the repose angle corresponds to the angle where amplification and capture are equal. This linear approximation is valid when the species do not differ much (for small $`\psi `$), and gives rise to a weaker segregation of the species— with a power law behavior of the concentrations as a function of the position along the pile surface— than the segregation found in this study which is valid when the species differ appreciable in size and shape.

We focus here on the dependence of the repose angles on the composition of the surface. We will consider that the other parameters—i.e., $`\gamma _{\alpha \alpha }`$ and $`v_\alpha `$—do not depend on the composition of the surface and on the species considered

$$\gamma _{11}=\gamma _{22}=\gamma ,v_1=v_2=v.$$
(35)   
In the conditions of the experiment , where an equal volume of the two species is poured at the left side of the cell, the boundary conditions are

$$R_\alpha (0,t)=R_\alpha ^0=\frac{R^0}{2}.$$
(36)   
These equations are meaningful if all the rolling grains interact each time with the surface, and do not interact directly with each other. Then, when there is percolation in the rolling phase, the interaction terms have to be modified accordingly. In the next section we will show how to introduce the percolation effect characteristic of the thick flow regime. However, we will show that the above equations— although strictly valid in the thin-flow limit, i.e., $`R_\alpha d_\alpha `$— will be also needed to describe completely the thick flow regime.

### B Thick flow regime and the percolation effect

An important consideration of the model proposed above is that the two types of rolling grains do not interact significantly each other when the flow of grains is small, i.e., $`R_\alpha (x,t)<ϵ`$, where $`ϵ`$ is a cut-off of the order of the grain size $`d_\alpha `$. This hypothesis may not be valid in experiments where the input flux is large, where the layer of rolling grains could be larger than one grain size.

In the case of a thick layer of rolling grains, the phenomenon of percolation occurs; during the flow of grains down an inclined plane, the small rolling grains percolate downward through the gaps left by the motion of larger rolling grains  \[Fig. 1(b)\]. Therefore, as they are convected down, the rolling grains segregate, the concentration of small grains being large at the bottom of the rolling layer, and the concentration of large grains large at the top of the rolling layer. As only the lowest grains of the rolling layer interact with the sandpile, the above effect imposes that small grains will preferentially interact with the static grains. We include the percolation effect in the continuum model and see how the results related to spontaneous stratification are affected.

To model this effect, we consider the extreme situation where the segregation is present as soon as the grains start to roll, i.e., up to the top of the sandpile, and that only the small grains will interact with the sandpile as soon as $`R_1(x,t)>ϵ`$, with $`ϵR^0`$. $`ϵ`$ is thus the height of small grains below which the percolation stops to be effective, and for which the large rolling grains start to interact with the surface. The interaction terms discussed in Sec. IV A have to be modified accordingly.

This model implies that except for a small region where $`R_1<ϵ`$, the surface of the sandpile is always divided in two regions. The upper region corresponds to the part of the surface where small rolling grains are present. As they are the only one to interact with the sandpile, the sandpile will be made only of small grains. In the lower part, only large grains are present (except for the $`ϵ`$ part of small grains). The division point between the two regions is able to move with time.

For the upper part of the sandpile, defined by $`R_1(x,t)>ϵ`$, only small grains are captured, with $`R_2(x,t)=R_2^0=R^0/2`$ and $`\varphi _1(x,t)=1`$. The equations become

$`{\displaystyle \frac{R_1}{t}}`$ $`=`$ $`v{\displaystyle \frac{R_1}{x}}+\gamma (\theta \theta _{11})(R_1+R_2)`$ (38)   
$`{\displaystyle \frac{h}{t}}`$ $`=`$ $`\gamma (\theta \theta _{11})(R_1+R_2)`$ (39)   
When $`R_1(x,t)<ϵ`$, the percolation effect disappears and the equations of evolution of $`R_\alpha `$ and $`h`$ can be considered to be the same as the one defined by the collision matrix (28) valid for the thin flow limit.

The effectiveness of the interaction (given by $`\gamma `$ before) must be multiplied now by the vertical pressure acting on the lowest rolling grain interacting with the surface, i.e., the weight of the column of rolling grains above the interacting grain . This explains the presence of the $`R_2(x,t)`$ terms in the interaction term $`\mathrm{\Gamma }_1`$ in Eq. (IV B).

We numerically solve Eqs. (III) with the interaction terms given by (28) when $`R_1(x,t)<ϵ`$ and by (IV B) when $`R_1(x,t)>ϵ`$ as discussed above. We find qualitatively the same results as in the experiments , with stratification appearing when the large grains are rougher than the small grains \[$`\theta _{22}>\theta _{11}`$, Fig. 6(a)\]. The dynamics of stratification show also the formation of the kink as observed in the experiments and in the discrete model shown in Fig. 4. When the small grains are rougher than the large grains ($`\theta _{11}>\theta _{22}`$), then we obtain the strong segregation of the mixture with the small rough grains found at the top of the heap (Fig. 6(b)) and a small region of mixing in the center of the pile .

### C Thin flow regime

In the absence of the percolation effect, Eq. (28) remains valid along all the pile since in the small flow limit a thin rolling phase is expected with $`R_\alpha (x,t)<ϵ`$. However, we assume a large difference in size, so that strong segregation effects are expected anyway, and the collision functions are expected to behave as in (28). We then solve Eqs. (III)–(28) numerically. Defining the “control parameter” 

$$\delta \theta _{22}\theta _{11},$$
(40)   
we obtain stratification when $`\delta >0`$, i.e., when the large grains are rougher than the small grains as in the experiments and in the thick flow regime above. However, we find that the transition to segregation does not occur sharply at $`\delta =0`$ but occurs at a small negative value $`\delta _c<0`$, which depends on the value of the cross-amplification rates $`\gamma _{\alpha \beta }`$. When the cross-rates are zero, then the transition occurs at $`\delta =0`$ as we found for the thick flow regime above. For smaller values of $`\delta <\delta _c<0`$ we find the complete segregation pattern found in the experiments. Thus, the presence of cross-amplification processes—which appear only in the low flux limit—shifts the transition from stratification to segregation to a value $`\delta _c`$ different from zero . However, the stratification we find for $`\delta _c<\delta <0`$ is less pronounced than in the case $`\delta >0`$: the layers do not go to the top of the sandpile, and the layer of small grains is very thin. Similar results at the neighborhood of the stratification-segregation transition have been found with a microscopic model of grains dynamics . We also find a kink, corresponding to the growth of the new pair of static layers, with a well-defined steady-state profile and upward velocity for $`\delta >0`$.

This model, valid for thin flows, is qualitatively close the preceding one valid for thick flows, where we also found a regime of complete segregation separating the surface of the sandpile in two regions. This can be understood noting that the dependence of the repose angle on the composition of the surface in the thin flow model is comparable to the effect of percolation in the rolling layer in the thick flow regime. Since for a given composition $`\varphi _\beta `$, the repose angle of the small grains is always larger than the repose angle of the large grains (Fig. 5), the small grains are also the first to be trapped before the large ones. The composition of small grains on the surface increases, amplifying the effect, up to the point where the surface is made of only small grains.

## V Analytical results

The thick flow and the thin flow regime show similar results as long as there is a large difference in size between the grains. We will now show analytical results valid for both regimes.

### A Steady state solution

We next study the stationary solution of Eqs. (III) and then we study how a perturbation to this solution can be amplified giving rise to stratification. For simplicity, we consider the geometry of a silo of lateral size $`L`$, i.e., all the rolling grains are stopped when they reach a wall at position $`x=L`$ \[Fig. 1(a)\]. Moreover, we assume the difference

$$\psi \theta _2(\varphi _2)\theta _1(\varphi _2)$$
(41)   
to be independent of the concentration $`\varphi _2`$. We seek for a solution where the profiles of the sandpile and of the rolling grains are conserved in time. Thus, stratification that corresponds to periodic variations in time of the different variables of interest cannot be observed for this solution. The conservation of the grains gives 

$$\frac{h}{t}=\frac{vR^0}{L},$$
(42)   
and we impose

$$\frac{R_\alpha }{t}(x)=0.$$
(43)   
We assume that, as in the experiment, an equal volume mixture is used, so

$$R_1^0=R_2^0=R^0/2,$$
(44)   
and the boundary conditions are

$$\begin{array}{c}R_\alpha (L)=0,\hfill \\ R_\alpha (0)=R^0/2.\hfill \end{array}$$
(45)   
The steady-state solution of (III)-(28) shows total segregation: except in a region of size of $`v/\gamma `$ at the center of the sandpile where the grains are mixed, the sandpile is exclusively made of small grains in the upper part of the pile, and of large grains in the lower part of the pile. The details of the calculations can be found in . Here we present a simplified results for the case of $`v/\gamma L`$, since we expect (17).

At the upper part of the pile, for $`0xx_m`$, with $`x_mL/2v/(\gamma \psi )`$, only small grains are present ($`\varphi _1(x)=1`$, and $`\varphi _2(x)=0`$), and the profiles are

$`R_1(x)`$ $`=`$ $`R^0\left({\displaystyle \frac{1}{2}}{\displaystyle \frac{x}{L}}\right),`$ (47)   
$`R_2(x)`$ $`=`$ $`R^0/2,`$ (48)   
$`\theta (x)\theta _{11}`$ $`=`$ $`{\displaystyle \frac{v/\gamma +\psi \gamma _{21}L/(2\gamma )}{L(1+\gamma _{21}/\gamma )/2x}}.`$ (49)   
At the lower part of the pile ($`x_mxL`$), we find that after a small region of size of the order of $`v/(\gamma \psi )`$ (or equivalently, of the order of the size of the grain), mainly large grains are present. The profiles are

$`\varphi _1(x)`$ $`=`$ $`\mathrm{exp}\left[{\displaystyle \frac{\gamma \psi }{v}}(xx_m)\right],`$ (51)   
$`R_1(x)`$ $`=`$ $`{\displaystyle \frac{2v}{\gamma \psi L}}\varphi _1(x)R(x),`$ (52)   
$`\theta (x)\theta _{22}`$ $`=`$ $`m\varphi _1(x){\displaystyle \frac{v}{\gamma (Lx)}}.`$ (53)   
Here

$$R(x)R_1(x)+R_2(x)=R^0(1x/L),$$
(54)   
and $`m\theta _{22}\theta _{21}=\theta _{12}\theta _{11}`$.

When the system is in this stationary state, the angle of the upper part of the sandpile (where only small grains exist) is almost $`\theta _{11}`$; without cross-amplification ($`\gamma _{21}=0`$), the sandpile would be at its repose angle $`\theta _{11}`$, and because of cross-amplification, the angle is significantly reduced. The divergence around $`x=L/2`$ insures that all the small grains are captured despite cross amplification. Moreover the angle for the low part of the sandpile is almost $`\theta _{22}`$. If we now suppose a fluctuation in $`R_1`$ such that few small rolling grains enter the low part of the sandpile, capture will be of the order of $`\gamma (\theta _{22}\theta _1(\varphi _2))R_1`$, and amplification will be of the order of $`\gamma (\theta _{22}\theta _2(\varphi _2))R_2`$. As $`R_1R_2`$, amplification will dominate capture, and the small rolling grains will go downhill up to the point when capture starts to exceed amplification. As soon as this small layer of rolling grains exist, the large grains are convected down without being capture. This excess of large grain creates a kink at the bottom of the pile going uphill where large grains are now stopped; the first layers are formed and the same process starts again. This may explain why when cross-amplification terms are present the transition stratification-segregation is shifted from $`\delta =0`$ to $`\delta =\delta _c<0`$.

When percolation is present this shift disappears since cross-interactions are greatly reduced by the screening effect of the small rolling grains at the bottom of the rolling phase.

To analyze the stability of the steady-state solution for the different phenomenologic parameters, we impose the steady-state solution as the initial condition, and then we look numerically for the stability of the profile under perturbations (Fig. 7). For $`\theta _{11}>\theta _{22}`$, the steady state solution is stable, so that Eqs. (V A) and (V A) are the physical solution for this case. In this case, only segregation is observed, and the sandpile conserves in time the profiles (V A) and (V A). For $`\theta _{11}<\theta _{22}`$, the steady-state solution is unstable (evolving to stratification), just as in . The onset of the instability is clearly seen, where the kink first start at the center of the pile where some large grains are captured on top of small grains as seen in Fig. 7 for $`\theta _{22}>\theta _{11}`$.

Our model predicts the complete segregation of the species when $`\theta _{22}<\theta _{11}`$. The concentration of small grains drops very fast near the center of the pile in a characteristic region of the order of $`v/(\gamma \psi )`$cm according to experiments . As discussed in Sec. IV A this is a consequence of our assumption of large difference in properties of the species.

### B Analytical Shape of the Kink

We saw in a preceding section that the layers were constructed through a kink where all the grains are stopped. A precise analysis of this kink would allow us to understand the dynamic of the process and the characteristic size of the layers.

From the simulations we observe that the kink has a well define uphill speed and that its shape is preserved in time. To obtain an analytically tractable set of equations, we then look for a possible steady-state solution for the shape of the kink, and thus for $`R(x,t)`$ and $`h(x,t)`$. We also must make the assumptions that far below and above the kink, the sandpile has a constant angle $`\theta _0`$ and is only made of large grains. These assumptions are verified by comparing the obtained result for the shape of the kink with the numerical results.

The existence of a stationary solution for the kink implies that $`R_\alpha (x,t)`$ and $`f(x,t)h(x,t)+\theta _0x`$ are functions only of

$$ux+v_{}t,$$
(55)   
where $`v_{}`$ is the uphill speed of the kink. For the lowest layer of the kink composed of small grains (the upper part of the pile), as only small grains are captured ($`\varphi _1(u)=1`$, $`R_2(u)=R^0/2`$), Eqs. (III) reduce to equations for $`R_1(u)`$ and $`f(u)`$ (we assume $`\gamma _{21}=\gamma `$),

$$\begin{array}{ccc}\hfill (v_{}+v)\frac{R_1(u)}{u}& =\hfill & \gamma \left(\frac{f}{u}\delta _{11}\right)R_1+\hfill \\ & & \gamma \left(\frac{f}{u}\delta _{21}\right)R_2^0\hfill \\ \hfill v_{}\frac{f(u)}{u}& =\hfill & \gamma \left(\frac{f}{u}+\delta _{11}\right)R_1+\hfill \\ & & \gamma \left(\frac{f}{u}+\delta _{21}\right)R_2^0,\hfill \end{array}$$
(56)   
with

$$\delta _{11}\theta _{11}\theta _0,\delta _{21}\theta _{21}\theta _0$$
(57)   
We obtain the shape of the low part of the kink. For $`u0`$, $`f(u)=0`$ and for $`u>0`$, $`f(u)`$ and $`R_1(u)`$ obey the following equations:

$$\begin{array}{ccc}\frac{f}{u}& =& \frac{(\delta _{11}+\delta _{21})R^0/2w\delta _{11}f(u)}{v_{}/\gamma +wf(u)R^0},\hfill \\ R_1(u)& =& wf(u)+R^0/2\hfill \end{array}$$
(58)   
where $`wv_{}/(v+v_{})`$. Then the lower part of the kink is characterized by a linear dependence

$$f(u)\frac{(\delta _{11}+\delta _{21})/2}{v_{}/(\gamma R^0)1}u.$$
(59)   
Finally, this solution is valid up to the point where the large grains start to be captured, i.e., $`f/u=\delta _{21}`$. From Eqs. (58) and (59) we obtain the following inequalities:

$$\theta _0>\frac{\theta _{11}+\theta _{21}}{2},v_{}<\gamma R^0.$$
(60)   
The solution of the equations for the upper layer of the kink (the lowest part of the pile) where only large grains are present can be obtained in the same way and is

$$f(u)=\left(\frac{R^0}{w}\right)\mathrm{exp}\left(\frac{w\gamma \delta _{22}u}{v_{}}\right),$$
(61)   
where

$$\delta _{22}\theta _0\theta _{22}.$$
(62)   
We then find that the shape of the upper part of the kink is exponential, and that the stationary solution exists only for $`\delta _{22}<0`$.

Thus we see that the existence of the stationary solution for the kink implies that

$$\frac{\theta _{11}+\theta _{21}}{2}<\theta _{22},$$
(63)   
and that the sandpile is built on an intermediate angle $`\theta _0`$ between those two extreme values. We are now able to distinguish two types of stratification. When Eq. (63) is satisfied, a stationary solution exists for the kink and the layers are well formed. When Eq. (63) is not satisfied, the layers are very asymmetric, with thin layers of small grains.

### C Wavelength of the Layers

The layer thickness $`\lambda `$ is defined by the width of the kink, $`\lambda lim_u\mathrm{}f(u)`$. From Eq. (61), we obtain $`\lambda =R^0/w,`$ which is a consequence of the conservation law stating that all the rolling grains are stopped at the kink. This relation is obtained assuming that the density of the fluid phase is the same as the density of the bulk. However, in general we have $`\mu _{\text{fluid}}<\mu _{\text{bulk}}`$, where $`\mu _{\text{fluid}}`$ and $`\mu _{\text{bulk}}`$ are the number of rolling grains per unit volume of the fluid phase and bulk, respectively. Then we obtain

$$\lambda =\frac{\mu _{\text{fluid}}}{\mu _{\text{bulk}}}\frac{(v+v_{})}{v_{}}R^0.$$
(64)   
Furthermore, Eq. (59) implies that

$$v_{}=C_{}\gamma R^0,$$
(65)   
where $`C_{}`$ is a numerical constant that does not depend on $`v`$, $`\gamma `$, or $`R^0`$. Then we obtain

$$\lambda _{\text{thin}}=\frac{\mu _{\text{fluid}}}{\mu _{\text{bulk}}}\left(\frac{v}{C_{}\gamma }+R^0\right)\text{[thin flow regime].}$$
(66)   
This relation is relevant to the thin flow regime where $`v/\gamma d`$ and $`R^0d`$ are both of the order of the size of the grains, and the velocity of the rolling grains is constant since the rolling phase is homogeneous. However in the thick flow regime the mean value of the velocity of the grains scale with the thickness of the rolling phase as found recently experimentally 

$$v=C\gamma R^0,$$
(67)   
where $`C`$ is a numerical constant that does not depend on $`\gamma `$ or $`R^0`$, but may depend on the angles of repose and other features of the grains. In this case Eq. (64) becomes

$$\lambda _{\text{thick}}=\frac{\mu _{\text{fluid}}}{\mu _{\text{bulk}}}\left(1+\frac{C}{C_{}}\right)R^0\text{[thick flow regime].}$$
(68)   
Thus we see that we expect a linear dependence of the wavelength of the layers as a function of the thickness of the rolling phase, i.e. as a function of the flux of grains (if the plate separation is maintained constant ), but the proportionality constant is different in the thin flow regime and the thick flow regime. From (66) and (68) we can obtain an approximate estimation of the value of the cross-over from the thin flow regime to the thick flow regime $`R_c^0`$ assuming that $`\lambda _{\text{thin}}(R_c^0)\lambda _{\text{thick}}(R_c^0)`$, then $`R_c^0v_{\text{thin}}/(C\gamma ),`$ where $`v_{\text{thin}}`$ is the velocity of the rolling grains in the thin flow regime.

Typical experimental values of the phenomenological constants of the problem for a system of $`L=30`$ cm, $`d_1=0.27`$ mm, $`d_2=0.8`$ mm, are  $`v10`$ cm/sec, $`\gamma 20`$/sec, $`\mathrm{tan}\psi =\mathrm{tan}\theta _{11}\mathrm{tan}\theta _{21}0.2`$, $`\mu _{\text{fluid}}/\mu _{\text{bulk}}=0.85`$, and $`C/C_{}1`$. Therefore, $`v/(\gamma \mathrm{tan}\psi )2.5`$ cm. We also obtain $`R_c^00.5`$ cm as the value of the cross-over flux from the thin flow regime to the percolation regime. The above predictions regarding the dependence of the wavelength on the flux of grains have been confirmed in recent experiments .

## VI Discussion

In summary, we develop a mechanism to explain the spontaneous stratification observed in . This mechanism is related to the dependence of the local repose angle on the local surface composition. When we consider only capture (corresponding to the cellular automaton model), we find that spontaneous stratification occurs only when the repose angle of the large grains is larger than the repose angle of the small grains ($`\theta _{22}>\theta _{11}`$, corresponding to large grains rougher than small grains). This result is in agreement with the experiments. Stratification is also obtained when $`\theta _{22}`$ is slightly smaller than $`\theta _{11}`$ as soon as we include cross-amplification process, as we find in the thin flow regime with the continuum model. When $`\theta _{22}<\theta _{11}`$, the model predicts almost complete segregation, but not stratification. These results are in agreement with experiments .

It is interesting to compare those results with a previous study  where a continuum model was used neglecting cross-amplification (i.e., amplification of $`\alpha `$ static grains by $`\beta `$ rolling grains). In this case, it was shown that amplification never occurs during the formation of the sandpile, and stratification is obtained in the same conditions as in the experiments.

We discuss the possible importance of percolation effects in the rolling layer, that takes place when the input flux of grains is large. Although the continuum model must be deeply modified, the results are surprisingly close to the thin flow model.

The model describes well the static picture of the sandpile of  with alternating layers made of small and large grains, and also reproduces the dynamics, where the layers are built through a kink mechanism. The numerical simulations suggest that the motion of the kink is stationary. It allows us to make quantitative predictions for the dependence of the size of the layers on the different parameters of the problem.

From the theoretical point of view, it is the first time that this continuum formalism for granular flow is directly compared to experiments. The quality of the results suggest that this formalism includes the essential features of the physics of granular flow. Using this formalism, it may be possible to have theoretically access to 3D problems, such as periodic segregation in rotating cylinders , that are out of reach with present-day computer simulations.

#### Acknowledgments

We thank T. Boutreux, P. G. de Gennes, S. Havlin, H. J. Herrmann, P. R. King, and S. Tomassone for stimulating discussions, and NSF and BP for financial support.