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# Speckle visibility spectroscopy and variable granular fluidization

## Abstract

We introduce a dynamic light scattering technique capable of resolving motion that changes systematically, and rapidly, with time. It is based on the visibility of a speckle pattern for a given exposure duration. Applying this to a vibrated layer of glass beads, we measure the granular temperature and its variation with phase in the oscillation cycle. We observe several transitions involving jammed states, where the grains are at rest during some portion of the cycle. We also observe a two-step decay of the temperature on approach to jamming.

A wealth of spectacular phenomena occur when granular materials are subjected to periodic vertical vibration Jaeger et al. (1996); Duran (2000). For example, shallow layers exhibit period doubling and pattern formation; deep layers exhibit heaping, convection, and logarithmically-slow compaction. It is relevant to ask: What grain-scale physics gives rise to all this intriguing macroscopic behavior? Since the driving is generally at high-amplitude but low-frequency, the dynamics vary dramatically during the oscillation cycle. At first, the grains are jammed Cates et al. (1998); Liu and Nagel (1998), completely at rest in some random packing configuration. When the downward acceleration exceeds $`g`$, the grains are launched upward from the plate. The layer expands as the grains collide and move about randomly. Soon they crash back into the bottom plate, and pick up energy from this impact. Finally, they come to rest after rattling away energy by inelastic collisions. This approach to jamming can be accompanied by clustering and “inelastic collapse”, a finite time singularity where the collision rate diverges and the collision length vanishes Goldhirsch and Zanetti (1993); Du et al. (1995). This regime is especially significant because granular hydrodynamics Jenkins and Savage (1983); Garzo and Dufty (1999); Bocquet et al. (2002) and statistical mechanics, extended to an athermal system, both break down.

Unfortunately, the above sequence of dynamics has not been experimentally accessible. Because of multiple light scattering, video imaging is restricted to dilute granular gasses or surface behavior Rouyer and Menon (2000). Even then, the spatial resolution is much larger than the collision length as the grains come to rest. This limitation holds for other imaging techniques as well, like MRI Ehrichs et al. (1995); Yang et al. (2002), x-ray microtomography Seidler and et al. (2000), and positron emission particle tracking Wildman and Parker (2002). Furthermore, none is fast enough to capture the high collision rates when the grains are barely fluidized. By contrast, diffusing-wave spectroscopy (DWS) Weitz and Pine (1993) is a dynamic light scattering (DLS) Berne and Pecora (1976) method that applies to bulk granular media. It has superior spatial and temporal resolution, and can be extended to unsteady dynamics Lemieux and Durian (2000). However, it is based on temporal correlation functions, which implicitly assume that all times are statistically equivalent; therefore, it is not appropriate for periodic or aging systems. Altogether, the leading probe of dynamics in vibrated 3D granular systems currently is an NMR technique Yang et al. (2002). It allows tracking of individual grains throughout a highly-fluidized sample to within about 150 $`\mu `$m and 1.4 ms.

In this paper, we introduce a new DLS technique and use it to study the bulk grain dynamics throughout the oscillation cycle. Here the resolution is limited by the wavelength of light and by the speed of a fast CCD camera. Taking advantage of multiple light scattering, we achieve a resolution of $``$1 nm and $``$20 $`\mu `$s. With this advance, we have unlocked regimes where the grains barely move. In particular, we observe three dynamic transitions: the onset of fluidization, where the acceleration amplitude just exceeds $`g`$; a jamming transition, where the grains crash into the plate and then come to rest; and a transition to continuous fluidization, where the grains do not jam up at any point during the cycle. In contrast, the NMR study of Ref. Yang et al. (2002) was conducted far above this point, where granular hydrodynamics is applicable in the bulk. Our three transitions all involve a jammed state, and therefore cannot be captured by granular hydrodynamics. Since our observations quantify the microscopics that underlie a host of intriguing phenomena, they present a theoretical challenge.

Our granular system consists of $`780\pm 35\mu `$m diameter glass beads, approximately twelve layers deep in a $`10\times 10`$ cm2 box with a flat transparent bottom, vertical walls, and open top. This is mounted on a shake table, which in turn is leveled on an optical bench. Two three-axis accelerometers monitor the quality and peak amplitude, $`a_{}\mathrm{\Gamma }g`$, of the vertical sinusoidal oscillations. All data are taken at frequency $`f=10`$ Hz. We define the phase to be $`\varphi =0`$ when the plate is at height $`z=0`$ and moving upward. Properly leveled, we observe no discernable heaping, pattern formation, or convection across the range of amplitudes studied, $`0<\mathrm{\Gamma }<2.2`$.

To measure grain motion, we introduce a method that we call “speckle visibility spectroscopy” (SVS). As shown in Fig. 1a, we illuminate the grains from above with a $``$1 cm diameter beam of a 100 mW frequency-doubled Nd-YAG laser ($`\lambda =532`$ nm). Photons perform a random walk with transport mean free path of $``$4 grains. Since the sample is 12 layers deep, about $`\frac{1}{3}`$ of the photons reach the bottom plate, and the rest are backscattered after a few scattering events. The backscattered light forms a speckle pattern in the far field, which we detect using a digital linescan CCD camera (Basler-160: 1024 pixels, 8 bits deep), and no intervening optics except a 532 nm filter. The sample-CCD distance is $``$20 cm, such that the speckle size is comparable to the pixel size ($`10\mu `$m). Therefore, as the grains move and the speckle pattern changes, large intensity fluctuations occur at each pixel. For the speckle pattern to be visible, however, the exposure time of the CCD must be short compared to the time scale for speckle fluctuations. If the exposure time is longer, then the speckle blurs out and the same average intensity is recorded at each pixel. This is the essence of SVS. It is illustrated qualitatively in Fig. 1b by the space-time plot of speckle vs phase during the cycle. When the grains are at rest on the plate, the speckle is clearly visible. When the grains are fluidized, the speckle is blurry. The speckle is least visible just after impact, where rapid grain motion is excited by the sudden injection of energy. This is reminiscent of “laser speckle photography”, where the absence of speckle in a laser-illuminated scene indicates motion Fercher and Briers (1981); Aizu and Asakura (1991).

The key measurable quantity in SVS is the variance of intensity across the pixels. For an exposure duration $`T`$, each of the $`N`$ pixels reports a time-integrated intensity, $`S_i=_0^TI_i(t)𝑑t/T`$. The ensemble-averaged intensity and intensity-squared are computed as $`I_T=_{i=1}^NS_i/N`$ and $`I^2_T=_{i=1}^NS_{i}^{}{}_{}{}^{2}/N`$, respectively. If there are enough speckles, then the former is independent of $`T`$ and the subscript may be dropped. By contrast, $`I^2_T`$ depends on $`T`$ and indicates the visibility of the speckles to the extent that it exceeds $`I^2`$. To quantify visibility on a scale of $`01`$, we define a normalized variance:

$$V_2(T)\left[I^2_T/I^21\right]/\beta .$$
(1)
The factor $`1/\beta `$ is roughly the number of speckles per pixel, and is determined experimentally by measuring the system at rest. Fig. 1c shows an example of $`V_2(T)`$ vs phase during the cycle, for a fixed exposure of $`T=100\mu `$s. It is closer to 0 when the grains are moving rapidly, and closer to 1 when the grains are coming to rest.

To relate the variance to grain motion, note that Eq. (1) involves ensemble averages, rather than time averages. Therefore, the Siegert relation Berne and Pecora (1976) holds, giving $`I^2_T_0^T_0^TI_i(t^{})I_i(t^{\prime \prime })dt^{}dt^{\prime \prime }/T^2_i=I^2_0^T_0^T[1+\beta |g_1(t^{}t^{\prime \prime })|^2dt^{}dt^{\prime \prime }/T^2`$. Here, $`\beta `$ is the same as above, and $`g_1(t)`$ is the normalized electric field autocorrelation. Since $`g_1(t)`$ is even, the double integral simplifies and we arrive at the fundamental equation of SVS:

$$V_2(T)=2_0^T(1t/T)|g_1(t)|^2𝑑t/T.$$
(2)
The variance is thus a weighted average of $`|g_1(t)|^2`$ over the exposure time $`T`$. Both functions are 1 at short times, and 0 at long times. Given $`g_1(t)`$ from SVS measurements, the scattering site motion may then be deduced by standard DLS practice. For random ballistic motion of average speed $`\delta v`$, the theory of DWS for backscattered light gives $`g_1(t)=\mathrm{exp}(\gamma t)`$ with $`\gamma =4\pi \delta v/\lambda `$ Weitz and Pine (1993). The corresponding variance is

$$V_2(T)=2[\mathrm{exp}(2\gamma T)(12\gamma T)]/(2\gamma T)^2.$$
(3)
At short times, the initial decay is linear: $`V_2(T)1\frac{2}{3}\gamma T`$; at long times, it is a power-law: $`V_2(T)1/(\gamma T)`$. The heavy weighting in Eq. (2) near $`t=0`$ slows the decay, aiding in the measurement of fast processes.

We now return to Fig. 1, where the grains are vibrated at $`f=10`$ Hz and $`\mathrm{\Gamma }=1.25`$, and exploit our SVS method. Three representative phases in the cycle are marked by triangles in the $`V_2(100\mu \mathrm{s})`$ data in Fig. 1c: where the grain motion is most rapid both in mid-flight and after impact, and where the grain motion ceases. For each of these three events, we show $`V_2(T)`$ vs $`T`$ in Fig. 2a. All data tend toward 1 (0) at short (long) times, as expected, where the speckle is most (least) visible. The actual dynamic range of our data is limited by two effects that are specific to our experiment (not the SVS method). First, for exposures faster than $`50\mu `$s, our 100 mW laser produces a signal that is a small fraction of the 0-255 range of the CCD. Therefore, the distribution of intensities is binned coarsely, which systematically distorts the variance. This limitation could be reduced by a brighter laser. Second, the macroscopic motion of the system contributes to the variance, becoming significant for $`T\mathrm{}`$ and/or $`V_21`$. In particular, even if the grains are at rest, the speckles form a static pattern that washes as a whole across the CCD pixels. This “speckle-wash” can be seen as a swirling in the space-time plot of Fig. 1b.

The reliable portion of the variance data in Fig. 2a compares well with Eq. (3), as shown by the curves. The form of the decay is therefore consistent with expectation: the grains appear to undergo random ballistic motion with some average fluctuation speed $`\delta v`$. For granular materials, the kinetic energy associated with $`\delta v`$ is called the granular temperature; it is directly proportional to the decay rate $`\gamma =4\pi \delta v/\lambda `$. Results for $`\gamma `$ are shown in Fig. 2b as a function of phase in the cycle. The grains “heat up” both in mid-flight and from impact. In both cases, they lose energy through inelastic collisions. About $`\frac{1}{5}`$ cycle ($`20`$ ms) after impact, the grains lose their energy and come to rest in a jammed state. Due to speckle wash, however, $`\gamma `$ doesn’t decay to zero but rather to a readily-identifiable baseline. To our knowledge, this is the first measurement of the bulk granular temperature during the collapse.

We now repeat the experiment versus $`\mathrm{\Gamma }`$, at constant $`f=10`$ Hz. A grayscale plot of $`\gamma `$ is shown in Fig. 3 vs both $`\mathrm{\Gamma }`$ and $`\varphi `$. Effectively, this is a phase diagram denoting the relative fluidization of the medium at different forcing rates and at different points in the cycle. Several transitions can be observed. First, below $`\mathrm{\Gamma }=1`$, there is no fluidization at all. Above $`\mathrm{\Gamma }=1`$, the grains become fluidized for some portion of the cycle. In particular, the grains are launched from the plate when the instantaneous acceleration is $`g`$, as denoted by a solid-white curve. The dotted-white curve denotes where the grains crash back down, assuming they undergo simple free-fall. Some time after the grains land, they lose their energy via collisions and jam. The onset of both jamming and unjamming depend on the driving amplitude. For $`\mathrm{\Gamma }>1.6`$, they merge together and the system undergoes a transition to continuous fluidization. Though the grains never come to rest, their dynamics still vary throughout the cycle. As expected, the motion is fastest (slowest) just after (before) impact.

Both the process of jamming, and the nature of the transition to continuous fluidization, may be studied in terms of the fluctuation speed, $`\delta v`$, vs the time following impact, $`\mathrm{\Delta }t`$. These data are extracted from Fig. 3 and displayed in Fig. 4. For amplitudes $`1<\mathrm{\Gamma }<1.6`$, $`\delta v`$ spikes at impact and then decays to a plateau after $``$2 ms; the initial decay rate appears to be independent of $`\mathrm{\Gamma }`$. Following the plateau, $`\delta v`$ decays to zero (within resolution set by speckle wash) as the grains jam up. This second decay is slower than the first. The temperature spike, the level of the plateau, and the duration of the plateau, all increase monotonically with $`\mathrm{\Gamma }`$. The impacts become progressively more violent, until suddenly at $`\mathrm{\Gamma }>1.6`$ the plateau extends across the entire cycle and the grains never come to rest. The impacts are no longer as violent; instead, the grains stay fluidized and $`\delta v`$ exhibits a smoother variation with time.

Conclusion The use of area detectors for “multispeckle” dynamic light scattering is on the rise Wong and Wiltzius (1993); Cipelletti and Weitz (1999); Lumma et al. (2000); Viasnoff et al. (2002). The general approach has been to autocorrelate each pixel, and then to average the results afterwards, all in software. Our new method, speckle variance spectroscopy (SVS), is dramatically different and offers advantages in terms of both simplicity and applicability. In effect we have created a “speckle ensemble correlator” in which all averages are explicitly-computed ensemble averages of a single exposure of the CCD camera; neither time averages, temporal autocorrelations, nor image storage are necessary. While the time resolution of prior methods is currently no better than $`2`$ ms, we achieve $`20\mu `$s. More significantly, we can follow dynamics that change on equally rapid time scales. This unprecedented resolution allows us to capture the transition to continuous fluidization in Fig. 3 and the two-step decay of the granular temperature in Fig. 4. With a brighter laser, and better control of speckle wash, we are poised to study these and other granular dynamics in greater detail. SVS also opens a new window for the study of bubble rearrangements in coarsening foams, motion and aging in glassy suspensions, gelation, phase-separation, and other phenomena that exhibit fast or quickly evolving nonstationary dynamics.

We gratefully acknowledge discussions with R. Ojha, P. Lemieux, and T. Usher, and the support of NSF-0070329.