# Electrostatically-Driven Granular Media: Phase Transitions and Coarsening

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## Abstract

We report the experimental and theoretical study of electrostatically driven granular material. We show that the charged granular medium undergoes a hysteretic first order phase transition from the immobile condensed state (granular solid) to a fluidized dilated state (granular gas) with a changing applied electric field. In addition we observe a spontaneous precipitation of dense clusters from the gas phase and subsequent coarsening – coagulation of these clusters. Molecular dynamics simulations shows qualitative agreement with experimental results.

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Despite extensive study over the preceding decade, a fundamental understanding of the dynamics of granular materials still poses a challenge for physicists and engineers . Peculiar properties of granular materials can be attributed to strong contact interactions and inelastic collisions between grains . Fascinating collective behavior appears when small particles acquire an electric charge and respond to competing long-range electromagnetic and short range contact forces.

The electrostatic excitation of granular media offers unique new opportunities compared to traditional vibration techniques which have been developed to explore granular dynamics . It enables one to deal with extremely fine powders which are not easily controlled by mechanical methods. Fine particles are more sensitive to electrostatic forces which arise through particle friction or space charges in the particle environment. Their large surface to volume ratio amplifies the effect of water or other surfactants. These effects intervene in the dynamics causing agglomeration, charging, etc., making mechanical experiments uncontrollable. Electrostatic driving makes use of these bulk forces, and allows not only for removal of these ”side effects,” but also for control by long-range electric forces.

In this Letter we report experimental and theoretical study of electrostatically driven granular material. It is shown that the charged granular medium undergoes a first order phase transition from the immobile condensed state (granular solid) to a fluidized dilated state (granular gas) with a changing applied electric field. A spontaneous precipitation of dense clusters from the gas phase and subsequent coarsening – coagulation of these clusters is observed in a certain region of the electric field values. We find that the rate of coarsening is controlled by the amplitude and frequency of the applied electric field. We have also performed molecular dynamics simulations of electrostatically driven particles. These simulations show qualitative agreement with experiments.

The experimental cell is shown in Fig. 1. Conducting particles are placed between the plates of a large capacitor which is energized by a constant or alternating electric field. To provide optical access to the cell, the upper conducting plate is made transparent. We used $`4\times 6`$ cm capacitor plates with a spacing of 1.5 mm and 35 $`\mu `$m copper powder. The field amplitude varied from 0 to 10 kV/cm and the frequencies on the interval of 0 to 250 Hz. The number of particles in the cell was about $`10^7`$. The experiments were performed both in atmospheric pressure and in vacuum ( $`5\times 10^6`$ Torr).

When the conducting particles are in contact with the capacitor plate they acquire a surface charge. As the magnitude of the electric field in the capacitor exceeds the critical value $`E_1`$ the resulting (upward) electric force overcomes the gravitational force $`mg`$ ($`m`$ is the mass of the particle, $`g`$ is the acceleration due to gravity) and pushes the charged particles upward. When the grains hit the upper plate, they deposit their charge and fall back. Applying an alternating electric field $`E=E_0\mathrm{sin}(2\pi ft)`$, and adjusting its frequency $`f`$ one can control the particle elevation by effectively turning them back before they collide with the upper plate.

The phase diagram is shown in Fig. 2. We have found that at amplitudes of the electric field above a second threshold value, $`E_2>E_1`$, the granular medium forms a uniform gas-like phase (granular gas). This second field $`E_2`$ is 50-70% larger then $`E_1`$ in nearly the whole range of the parameters used. In the field interval $`E_1<E<E_2`$, a remarkable phenomenon analogous to coalescence dynamics in systems exhibiting first order phase transitions  was observed. Upon decreasing the field below $`E_2`$, the gas phase loses its stability and small clusters of immobile particles surrounded by the granular gas form. These clusters then evolve via coarsening dynamics: small clusters disappear and large clusters grow. Eventually the clusters assume almost perfect circular form (Figs 3a-c). In the process of coarsening the electric current also changes in time due to decrease of particles in the gas phase. A close-up image of one of the clusters is shown in Fig. 3a. Surprisingly, we can even see a larger particle near the center of the cluster which served as the nucleation point at the early stages of the aggregation. Due to its increased mass the large particle is the first to become immobile in the lower field. After a very large time ($`t30000`$ sec) a single cluster containing about $`10^6`$ grains survives. At the final stage a dynamic equilibrium between the granular solid and the surrounding gas persists – not all the particles join the last cluster.

For the cell under atmospheric pressure (open cell) we found that both fields $`E_1`$ and $`E_2`$ grow as a function of frequency for large $`f`$ and show non-monotonous behavior for $`f12`$Hz. This indicates a characteristic time of the order $`100`$ msec. We suggest that cohesion may be responsible for this relatively large time. Indeed, due to the humidity of the air a surface coating should exist, requiring a characteristic time $`\tau `$ for the grain to detach from the capacitor plate. In order to reduce the cohesion we evacuated the cell to $`5\times 10^6`$ Torr. As demonstrated from Fig. 2, the frequency dependence is indeed substantially reduced and becomes almost flat. Small oscillations in the dependence for low frequency are probably due to a residual coating on the particles which does not completely evaporate in vacuum.

We have measured the number of clusters $`N`$ and the averaged radius of the clusters $`R`$ as a function of time $`t`$ (see Fig. 4) using images taken in time-lapse by a digital camera and then processed on a computer. The values of $`R`$ for both open and evacuated cells are consistent with a power law $`R\sqrt{t}`$. However, there is a substantial difference in the behavior of $`N`$. In open cells (no vacuum) we observed slow coarsening $`N1/\sqrt{t}`$; whereas the coarsening for the evacuated cell is much faster, $`N1/t`$. Remarkably, for the evacuated cell the exponents for $`N`$ and $`R`$ coincide with the exponents for two-dimensional bi-stable systems in the interface-controlled regime of Ostwald Ripening . We speculate that the slow-down in coarsening for open cells can be a result of cohesion between the particles and with the capacitor plate. This cohesion reduces the mobility of particles at the edges of the clusters, resulting in ”pinning” of the front between the granular solid and gas.

Let us compare the forces exerted on an isolated particle and on a particle which is held within a cluster at the same field. The force between an isolated sphere and the capacitor plate in contact can be found as a limit of the problem of two spheres when the radius of one sphere goes to infinity. This problem had been contemplated by several outstanding physicists including Kelvin, Poisson, Liouville and Kirchhoff . Building on the technique of Ref. , we arrive at the force $`F_e`$ in question:

$$F_e=ca^2E^2$$
(1)   
where $`a`$ is the radius of the sphere and $`E`$ is the field in the capacitor. The constant $`c=\zeta (3)+1/61.36`$ comes from summing of infinite series derived in . The electric force $`F_e`$ has to counterbalance the gravitational force $`G=4/3\pi \rho ga^3`$, where $`\rho `$ is the density of the material. Comparing $`F_e`$ and $`G`$ we find the first critical field $`E_1`$:

$$E_1=\sqrt{\frac{4\pi \rho ga}{31.36}}$$
(2)   
Our theory indicates no frequency dependence of $`E_1`$. For the parameters of our experiments we obtain $`E_1=2.05`$ kV/cm. The experimental critical field is $`E_12.4`$ kV/cm. This discrepancy seems reasonable since we did not take into account additional molecular and/or contact forces which will increase the critical field.

If the spheres are close to each other, the surface charge will redistribute: each sphere in the cluster acquires smaller charge than that of an individual sphere due to a screening of the field by its neighbors. The exact derivation of the force acting on the particle within the cluster is not available at present. The upper bound can be obtained by replacing the square lattice of spheres with radius $`a`$ by a lattice of squares with area $`4a^2`$. Since the charge density of the corresponding flat layer is $`\sigma =E/4\pi `$, the total electric force on the square is $`F_2=4a^2\sigma E/2`$. The ratio of the fields to lift individual particle $`E_1`$ and the particle in the square lattice $`E_2`$ is $`E_2/E_1=\sqrt{2\pi 1.36}=2.92`$. For closed-packed hexagonal lattice one obtains a slightly higher value $`E_2/E_13.14`$. As one sees, the ratio of the critical fields is independent of particle size and the density and the frequency $`f`$. This is consistent with the experimental findings, see Fig. 2, although it exceeds the experimental value by a factor of 2. A more accurate account for the surface shape will improve the ratio.

We have also performed molecular dynamics simulations of conducting spheres in applied electric field. Several simplifications have been implemented: the sphere polarization was neglected; the charge was assumed to be in the center of the sphere; all collisions were assumed to be inelastic. These simplifications are justified by the fact that the particle-particle collisions are rather rare in contrast to deep vibrated granular layers studied in Ref. . Interactions between the spheres are treated as being between point charges if the distance is smaller than the plate spacing. For larger distances we assumed no interaction due to screening of the far charge field by other particles (compare with Debye screening ).

In our molecular dynamics simulations we implemented explicitly that the charge acquired by each sphere from the conducting plate decreases gradually with the number of nearest neighbors: it is maximum for an isolated sphere and decreases by factor of two for the sphere inside the cluster. We simulated $`35`$ $`\mu `$m diameter 3000 copper spheres in the domain $`7\times 7`$ mm ($`200\times 200`$ particle diameters) with periodic boundary conditions. The capacitor spacing was $`1.5`$ mm, as it was in the experiment. Although the quantitative correspondence between the molecular dynamics simulations and the experiment was not planned (the number of particles and the size of the system are too small ), the simulations turns out to be in a qualitative agreement with the experiment. We have obtained a gas phase for high field levels and spontaneous formation of clusters and coarsening for lower filed level, see Fig. 5. However, detailed simulations with much large number of particles and more realistic account for sphere polarization effects are necessary to achieve quantitative agreement with experiment.

We have reported a hysteretic first-order phase transition accompanied by coarsening behavior in the electrostatically-driven conducting granular medium. The origin of coarsening dynamics and hysteresis is due to a screening of the electric field in dense particle clusters. Our results show surprisingly high sensitivity of the phase boundaries to surface coating of the grains due to humidity. Simplified molecular dynamics simulations with conducting particles demonstrate qualitative agreement with the experiment: existence of two critical fields and coarsening.

We thank Sid Nagel, Leo Kadanoff, Thomas Witten, Lorenz Kramer and Baruch Meerson for useful discussions. This research is supported by US DOE, grant W-31-109-ENG-38, and by NSF, STCS #DMR91-20000.