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Spatiotemporal measurement of surfactant distribution on gravity–capillary waves

Published online by Cambridge University Press:  20 July 2015

Stephen L. Strickland*
Affiliation:
Department of Physics, North Carolina State University, Raleigh, NC 27695, USA
Michael Shearer
Affiliation:
Department of Mathematics, North Carolina State University, Raleigh, NC 27695, USA
Karen E. Daniels
Affiliation:
Department of Physics, North Carolina State University, Raleigh, NC 27695, USA
*
†Email address for correspondence: slstric2@ncsu.edu

Abstract

Materials adsorbed onto the surface of a fluid – for instance, crude oil, biogenic slicks or industrial/medical surfactants – will move in response to surface waves. Owing to the difficulty of non-invasive measurement of the spatial distribution of a molecular monolayer, little is known about the dynamics that couple the surface waves and the evolving density field. Here, we report measurements of the spatiotemporal dynamics of the density field of an insoluble surfactant driven by gravity–capillary waves in a shallow cylindrical container. Standing Faraday waves and travelling waves generated by the meniscus are superimposed to create a non-trivial surfactant density field. We measure both the height field of the surface using moiré imaging, and the density field of the surfactant via the fluorescence of NBD-tagged phosphatidylcholine, a lipid. Through phase averaging stroboscopically acquired images of the density field, we determine that the surfactant accumulates on the leading edge of the travelling meniscus waves and in the troughs of the standing Faraday waves. We fit the spatiotemporal variations in the two fields using an ansatz consisting of a superposition of Bessel functions, and report measurements of the wavenumbers and energy damping factors associated with the meniscus and Faraday waves, as well as the spatial and temporal phase shifts between them. While these measurements are largely consistent for both types of waves and both fields, it is notable that the damping factors for height and surfactant in the meniscus waves do not agree. This raises the possibility that there is a contribution from longitudinal waves in addition to the gravity–capillary waves.

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Papers
Copyright
© 2015 Cambridge University Press 
Figure 0

Figure 1.Experimental apparatus. The container (black) is connected by low-friction air bushings to an electromagnetic shaker, and filled with a thin layer of water onto which a monolayer of NBD-PC surfactant is deposited. The shaker vibrates the container vertically with acceleration $a(t)=a_{0}\sin {\it\omega}t$, generating meniscus and Faraday waves. The fluorescence imaging system involves a ring of blue LEDs around the outer edge that excites the fluorophore on the lipids; digital images of the fluorescence emission are collected through an optical notch filter. A silicon wafer sits flush with the bottom surface of the container, and reflects the excess light from the LEDs away from the camera. The moiré imaging system consists of a patterned light source shining downwards on the fluid surface, and the camera that records the distorted reflection of the pattern.

Figure 1

Figure 2.Stroboscopic imaging allows for the collection and phase-averaging of low-intensity fluorescence images over many cycles. During each second of the experiment, the container oscillates 20 times with an acceleration $a(t)$ (black curve). During that second, the camera is triggered at four different phases of the oscillation (eight different phases of the Faraday wave oscillation). The eight distinct phases (represented as $i=1$ to $i=8$) each have an exposure time of $1/8$th of the Faraday wave period, represented by the width of the grey bars. The time from the end of one exposure to the beginning of the next exposure is one whole Faraday wave period (100 ms), so that we sequentially sample each of the eight phases cyclically. The same stroboscopic pattern was used for both experiments, and both the FI and MI data.

Figure 2

Figure 3.Calibration of surfactant fluorescence intensity as a function of surfactant density. The stroboscopic exposure data were obtained with the same exposure time, number of images and gain settings as used for the FI technique. The long-exposure data were obtained with a single 2 s exposure and no gain, to confirm the trend. The markers show the mean intensity of the pixels within the field of view, while the error bars illustrate the standard error of the pixels for the stroboscopic exposure data. The linear fit, shown as a dashed line, is used in the range ${\it\Gamma}>0.1~{\rm\mu}\text{g}~\text{cm}^{-2}$ of the experiments.

Figure 3

Figure 4.Sample FI composite image. (a) Image showing ${\rm\Delta}{\it\Gamma}$ from the $i=2$ stroboscopic phase of experiment 1, smoothed by a Gaussian filter of ${\it\sigma}=0.04~\text{cm}$. (b) The corresponding ${\rm\Delta}{\it\Gamma}_{T}$, the best fit to (2.2). (c) The meniscus wave (harmonic) component and (e) the Faraday wave (subharmonic) component of the same ${\rm\Delta}{\it\Gamma}$ as shown in (a). These components are isolated by adding and subtracting (and dividing by 2) the FI composite images from the $i=2$ and $i=6$ stroboscopic phases. (d) The meniscus wave (harmonic) component and (f) the Faraday wave (subharmonic) component of the same ${\rm\Delta}{\it\Gamma}_{T}$ as shown in (b). (g) This image is generated by subtracting (d) from (c). The resulting pattern (smoothed with a Gaussian filter of ${\it\sigma}=0.09~\text{cm}$) is a higher-order mode, which is not accounted for in the ansatz (2.2). This mode has 24-fold symmetry and oscillates harmonically with peak-to-mean variation of $0.03~{\it\Gamma}_{c}$.

Figure 4

Figure 5.Sample MI images. (a) Contrast-enhanced image and (b) binarization of the target pattern reflected off a flat fluid surface. (c) Contrast-enhanced moiré image and (d) binarization of the target pattern reflected off the fluid surface at phase $i=2$ for experiment 1. (e) Ray-traced pseudo-image and (f) binarization of the best-fitting $h(\boldsymbol{r})$ for image (c) using parameters given in table 1.

Figure 5

Table 1.Summary of experimental parameters and best-fitting parameters (2.1) and (2.2) for the two experiments. The uncertainty of all parameter values is in the last reported digit. The centre of the Faraday wave (axis of pattern rotation) is within $\pm 3.5~\text{mm}$ of the container axis.

Figure 6

Figure 6.Visualization of ${\rm\Delta}h_{T}$ and ${\rm\Delta}{\it\Gamma}$ for experiment 1, within the annular field of view. The best fit using the $h$ ansatz (2.1) (mesh surface) and the FI composite data (colouration) for the $i=2$ stroboscopic phase. The peak-to-mean variations in ${\rm\Delta}h_{T}$ and ${\rm\Delta}{\it\Gamma}_{T}$ are $\pm 60~{\rm\mu}\text{m}$ and $\pm 0.15~{\it\Gamma}_{c}$, respectively. The ${\rm\Delta}{\it\Gamma}$ field is smoothed by a Gaussian filter of ${\it\sigma}=0.04~\text{cm}$ to reduce noise. In figures 7 and 8, these same data are decomposed into meniscus and Faraday wave components. A video version of this plot is available in the online supplementary movie.

Figure 7

Figure 7.Meniscus wave component of ${\rm\Delta}h_{T}$ and ${\rm\Delta}{\it\Gamma}$ for experiment 1. (a) The best-fitting ${\rm\Delta}h_{MT}$ ansatz from (2.1) (mesh surface) and the harmonic component of ${\rm\Delta}{\it\Gamma}$ (colouration) for the $i=2$ stroboscopic phase. (b) Radial slice of both fields along ${\it\theta}=2.83~\text{rad}$, the orange strip shown in (a), at phase $i=2$. The solid line is the best-fitting height field ${\rm\Delta}h_{MT}(r)$, and the surfactant density field is shown both as the data ${\rm\Delta}{\it\Gamma}_{M}$ (orange points) and as the ansatz ${\rm\Delta}{\it\Gamma}_{MT}$ (dashed line). The lines are the Bessel modes given in (2.1) and (2.2). (c) The temporal dynamics of ${\rm\Delta}h_{MT}$ (solid line) and ${\rm\Delta}{\it\Gamma}_{MT}$ (dashed line) at the location $r=4.79~\text{cm}$ and ${\it\theta}=2.83~\text{rad}$, marked by the magenta dot in (a). The lines are the sinusoids given in (2.1) and (2.2). In all cases, the ${\rm\Delta}{\it\Gamma}$ fields are smoothed by a Gaussian filter of ${\it\sigma}=0.04~\text{cm}$ to reduce noise. A video version of this plot is available in the online supplementary movie.

Figure 8

Figure 8.Faraday wave component of ${\rm\Delta}h_{T}$ and ${\rm\Delta}{\it\Gamma}$ for experiment 1. (a) The best-fitting $h_{FT}$ ansatz from (2.1) (mesh surface) and the subharmonic component of ${\rm\Delta}{\it\Gamma}$ (colouration) for the $i=2$ stroboscopic phase. (b) Radial slice of both fields along ${\it\theta}_{c}=2.83$  rad, the orange strip shown in (a), at phase $i=2$. The solid line is the best-fitting height field ${\rm\Delta}h_{FT}(r,{\it\theta}_{c})$, and the surfactant density field is shown both as the data ${\rm\Delta}{\it\Gamma}_{F}$ (orange points) and as the ansatz ${\rm\Delta}{\it\Gamma}_{FT}$ (dashed line). The lines are the Bessel modes given in (2.1) and (2.2). (c) Azimuthal slice of both fields along $r_{c}=4.26~\text{cm}$, the cyan strip shown in (a), at phase $i=2$. Here, the surfactant density field data ${\rm\Delta}{\it\Gamma}_{F}$ are represented with cyan points. The lines are the sinusoids given in (2.1) and (2.2) and plotted within a restricted range of the azimuthal dimension $[-2{\rm\pi}/n,2{\rm\pi}/n]$ centred about ${\it\theta}_{c}$. (d) The temporal dynamics of ${\rm\Delta}h_{FT}$ (solid line) and ${\rm\Delta}{\it\Gamma}_{FT}$ (dashed line) at the location $r_{c}~\text{cm}$ and ${\it\theta}_{c}$ rad, marked by the magenta dot in (a). The lines are the sinusoids given in (2.1) and (2.2). The magenta circles in (d) plot the behaviour of ${\mathcal{T}}(t)$ given in (3.1), with error bars much smaller than the symbol size. The ${\rm\Delta}{\it\Gamma}$ fields in (a–c) are smoothed by a Gaussian filter of ${\it\sigma}=0.04~\text{cm}$ to reduce noise. A video version of this plot is available in the online supplementary movie.

Strickland et al. supplementary movie

The Movie1 videos show the spatiotemporal dynamics of the surface height (3-d mesh) and the surfactant density (coloration) fields for the combined Faraday and meniscus waves system. This video, collected at 80 frames per second, has been slowed by 53x. Details of this visualization method can be found in the caption to figure 6.

Download Strickland et al. supplementary movie(Video)
Video 7.4 MB

Strickland et al. supplementary movie

The Movie1 videos show the spatiotemporal dynamics of the surface height (3-d mesh) and the surfactant density (coloration) fields for the combined Faraday and meniscus waves system. This video, collected at 80 frames per second, has been slowed by 53x. Details of this visualization method can be found in the caption to figure 6.

Download Strickland et al. supplementary movie(Video)
Video 2.9 MB

Strickland et al. supplementary movie

The Movie2 videos show the spatiotemporal dynamics of the surface height (3-d mesh) and the surfactant density (coloration) fields for the meniscus wave component of the dynamics. This video, collected at 80 frames per second, has been slowed by 53x. Details of this visualization method can be found in the caption to figure 7.

Download Strickland et al. supplementary movie(Video)
Video 7 MB

Strickland et al. supplementary movie

The Movie2 videos show the spatiotemporal dynamics of the surface height (3-d mesh) and the surfactant density (coloration) fields for the meniscus wave component of the dynamics. This video, collected at 80 frames per second, has been slowed by 53x. Details of this visualization method can be found in the caption to figure 7.

Download Strickland et al. supplementary movie(Video)
Video 2.6 MB

Strickland et al. supplementary movie

The Movie3 videos show the spatiotemporal dynamics of the surface height (3-d mesh) and the surfactant density (coloration) fields for the Faraday wave component of the dynamics. This video, collected at 80 frames per second, has been slowed by 53x. Details of this visualization method can be found in the caption to figure 8.

Download Strickland et al. supplementary movie(Video)
Video 7.1 MB

Strickland et al. supplementary movie

The Movie3 videos show the spatiotemporal dynamics of the surface height (3-d mesh) and the surfactant density (coloration) fields for the Faraday wave component of the dynamics. This video, collected at 80 frames per second, has been slowed by 53x. Details of this visualization method can be found in the caption to figure 8.

Download Strickland et al. supplementary movie(Video)
Video 2.4 MB