# Spontaneous Stratification in Granular Mixtures

## Abstract

Granular materials  size segregate when exposed to external periodic perturbations such as vibrations . Moreover, mixtures of grains of different sizes spontaneously segregate in the absence of external perturbations: when a mixture is simply poured onto a pile, the large grains are more likely to be found near the base, while the small grains are more likely to be near the top . Here, we report a novel spontaneous phenomenon arising when we pour a mixture between two vertical plates: the mixture spontaneously stratifies into alternating layers of small and large grains whenever the large grains have larger angle of repose than the small grains. In contrast, we find only spontaneous segregation when the large grains have smaller angle of repose than the small grains. The stratification is related to the occurrence of avalanches; during each avalanche the grains comprising the avalanche spontaneously stratify into a pair of layers, with the small grains forming a sublayer underneath the layer of large grains.

Our experimental system consists of a vertical “quasi-two-dimensional” cell with a gap of 5 mm separating two transparent plates (made of plexiglass, or of glass) measuring 300 mm $`\times `$ 200 mm (see Fig. 1a). We choose this quasi-two-dimensional geometry since, by using this setup, the internal features of the avalanche process can be easily visualized, both statically and dynamically. To avoid the effects of electrostatic interaction with the wall, the wall is cleaned with an antistatic cleaner.

In a first series of experiments, we close the left edge of the cell leaving the right edge free, and we pour, near the left edge, an equal-volume mixture of white glass beads (mean size 0.27 mm, spherical shape, and repose angle $`26^o`$), and red sugar crystals (typical size 0.8 mm, cubic shape, and repose angle $`39^o`$). Figure 1a shows the result of the first series of experiments. We note two features:

* Spontaneous Stratification. We see the formation of alternating layers consisting of small and large grains—with a “wavelength” of about 1.2 cm.
* Spontaneous Segregation. We find that the smaller grains segregate near the left edge and the larger grains segregate furthest from it and near the base .

In a second series of experiments, we confirmed the results of these initial experiments by testing for stratification and segregation using a mixture of grains of same density, consisting of fine sand (typical size 0.4 mm) and coarse sand (typical size 1 mm), suggesting that the density of the grains may not play an important role in stratification.

In all the above experiments we used mixtures composed of two types of grain with different shape, and therefore with different angles of repose. In particular we obtain stratification (plus segregation) when we use larger cubic grains and smaller spherical grains: the angle of repose of the large species is then larger than the angle of repose of the small species. Otherwise we obtain only segregation and not stratification when the large grains are less faceted than the small grains, i.e., the large grains have smaller angle of repose than the small grains.

To confirm this, we performed a series of experiments using mixtures of irregular shaped sand grains (repose angle $`35^o`$, and mean size 0.3 mm), and spherical glass beads (repose angle $`26^o`$ smaller than the repose angle of the sand grains). We find that stratification (plus segregation) occurs for two different experiments using spherical beads of size 0.07 mm and 0.11 mm (so that the larger grains have larger repose angle). In contrast, we obtain only segregation but not stratification for two experiments using spherical beads of size 0.55 mm and 0.77 mm (so that the larger grains have smaller repose angle). In all cases the segregation of grains occurs with the smaller grains being found near the left edge of the cell and the larger grains near the base of the cell. These results suggest that the phenomenon of segregation is always expected when pouring a granular mixture of grains of different sizes, no matter the values of the angles of repose of the species. However, the phenomenon of stratification is only expected when the large species have larger angle of repose than the small species.

Additionally, we performed a series of experiments in which we find similar stratification by using different mixtures of differing size ratio between large and small grains (1.66, 2.1, 2.25, 3.25, and 6.66), suggesting that the phenomenon occurs for a broad regime of grain size ratios. We find a similar stratification when we double the gap between the vertical plates of the cell and simultaneously double the flow rate of grains.

We propose a physical mechanism responsible for the observed stratification that is related to the fact that not one but rather a pair of layers is formed in the course of each avalanche. When the flow of grains reaches the base of the pile, we find that the grains develop a profile characterized by a well-defined “kink”, at which the grains are stopped (see Fig. 1b); but we find that the small grains stop first, so a pair of layers forms with the small grains underneath the large grains. As more grains are added, the kink appears to move upward in the direction opposite to the flow of grains. Once the kink reaches the top, the pair of layers is complete and the cycle is then repeated: a new avalanche occurs, the kink develops, and a new pair of layers forms.

The “wavelength” of a pair of layers $`\lambda `$ can be determined by the mean value of the downward velocity $`v`$ of the rolling grains during an avalanche, the upward velocity $`v^{}`$ of the kink, and the thickness of the layer of rolling grains $`R_0`$ during the avalanche. If the volume of grains in an avalanche scales approximately as the volume of grains in a well-formed kink, we predict $`\lambda R_0(v+v^{})/v^{}`$, and we confirm this relation experimentally.

To test this physical mechanism by computer simulation we consider a mixture comprising small grains of width one pixel and of height $`H_1`$, and large grains, also of width one pixel but of height $`H_2>H_1`$. To generate an equal-volume mixture, we randomly drop a small grain with probability $`pH_2/(H_1+H_2)`$, and drop a large grain with probability $`1p`$ (see Fig. 2).

In critical phenomena, it is often useful to first develop a “mean field” type model (in which, for example, spin orientation is determined by a macroscopic variable, the net magnetization), before devising models in which spin orientation is determined by the microscopic quantities such as the orientations of the other spins comprising the system. In this spirit, we focus first not on the “microscopic” grain motions, but rather on the “macroscopic” angle of the sandpile, whose value alternates in time between the maximum angle of stability $`\theta _m`$ which defines the onset of an avalanche, and the angle of repose $`\theta _r`$ which defines the end of the avalanche . Using this model (described in the legend of Fig. 2), we find a morphology that displays both segregation and stratification.

In addition to the simplest “mean field” approach, we develop a model  in which we treat the individual grain motion in accord with microscopic rules that depend not on the macroscopic angle of the sandpile, but rather on the local angles formed between each grain and its neighbors. Specifically, the dynamics of the small and large rolling grains are governed by the critical angles of repose corresponding to the interactions between the rolling grain and the static grains of the sandpile surface. This model incorporates the experimental fact that grains segregate because large grains roll down more easily on top of small grains than small grains on top of large grains (for rolling large grains on top of a surface of small grains the surface appears smoother than for rolling small grains rolling on top of a surface of large grains). Thus the model correctly predicts that the small grains form a sublayer beneath the large grains. We find stratification, as in the simplest “mean field” model, and also find that the profile of the sandpile displays a kink at which rolling grains are stopped—just as in the experiment.

Next we test the above principles by generalizing from two grain sizes to three. The experiment results in stratification with three layers, with the finest grains on the bottommost of each triplet of layers and the coarsest grains on the topmost layer (see Fig. 1c where the same experimental setup of Fig. 1a is used to obtain an alternation of three layers of grains of three different sizes: 0.15 mm, 0.4 mm, and 0.8 mm). Experiments using a continuum size distribution are ongoing, since geological rock formations (which also display stratification) generally occur in the presence of a continuum distribution of grain size.

As another test of the proposed physical mechanism, we note that the case of spherical grains should not lead to stratification because the angles of repose of the large and small grains are the same. We confirm this prediction experimentally. The case of spherical grains was also studied by Williams ; his results (showing segregation plus a hint of stratification) differ from our results (showing only segregation), presumably because his grains were not quite spherical— i.e., the repose angle of the large and small “spheres” were slightly unequal.

Finally, we note that Boutreux and de Gennes have recently made considerable progress  in developing a general theoretical framework  to treat the case of granular flows of two different grains. Their conclusions  are consistent with the experiments presented here.

ACKNOWLEDGEMENTS. We thank T. Boutreux, G. Davies, P.-G. de Gennes, H. J. Herrmann, and S. Tomassone for stimulating discussions, and P. Cizeau for collaboration in stages of this work.