Separation of cells is a critical process for studying cell properties, disease diagnostics, and therapeutics. Cell sorting by acoustic waves offers a means to separate cells on the basis of their size and physical properties in a label-free, contactless, and biocompatible manner. The separation sensitivity and efficiency of currently available acousticbased approaches, however, are limited, thereby restricting their widespread application in research and health diagnostics. In this work, we introduce a unique configuration of tilted-angle standing surface acoustic waves (taSSAW), which are oriented at an optimally designed inclination to the flow direction in the microfluidic channel. We demonstrate that this design significantly improves the efficiency and sensitivity of acoustic separation techniques. To optimize our device design, we carried out systematic simulations of cell trajectories, matching closely with experimental results. Using numerically optimized design of taSSAW, we successfully separated 2-and 10-μm-diameter polystyrene beads with a separation efficiency of ∼99%, and separated 7.3-and 9.9-μm-polystyrene beads with an efficiency of ∼97%. We illustrate that taSSAW is capable of effectively separating particles-cells of approximately the same size and density but different compressibility. Finally, we demonstrate the effectiveness of the present technique for biological-biomedical applications by sorting MCF-7 human breast cancer cells from nonmalignant leukocytes, while preserving the integrity of the separated cells. The method introduced here thus offers a unique route for separating circulating tumor cells, and for label-free cell separation with potential applications in biological research, disease diagnostics, and clinical practice.particle separation | microfluidics | cancer cell separation | acoustofluidics | tilt-angle optimization
induced scission measurements, imaging with AFM and TEM, and analysis of data. A.J.L. performed FRET measurements and analysis of the data. X.Z., T.C.-T., and Y.C. performed solution X-ray scattering, and analysis of the data. A.J.L. and Y.C. conceptualized nanoribbon thread processing and Y.C. and M.G. prepared nanoribbon threads. M.G. performed tensile testing of nanoribbon threads and analysis of the data. T.C.-T. and Y.C. performed X-ray scattering of solid-state nanoribbon threads and analysis of the data. J.
The ability to measure the bulk dynamic behavior of soft materials with combined time-and frequency-resolution is instrumental for improving our fundamental understanding of connections between the microstructural dynamics and the macroscopic mechanical response. Current state-ofthe-art techniques are often limited by a compromise between resolution in the time and frequency domain, mainly due to the use of elementary input signals that have not been designed for fast time-evolving systems such as materials undergoing gelation, curing or self-healing. In this work, we develop an optimized and robust excitation signal for time-resolved mechanical spectroscopy through the introduction of joint frequency-and amplitude-modulated exponential chirps. Inspired by the biosonar signals of bats and dolphins, we optimize the signal profile to maximize the signal-to-noise ratio while minimizing spectral leakage with a carefully-designed modulation of the envelope of the chirp, obtained using a cosine tapered window function. A combined experimental and numerical investigation reveals that there exists an optimal range of window profiles (around 10% of the total signal length) that minimizes the error with respect to standard single frequency sweep techniques. The minimum error is set by the noise floor of the instrument, suggesting that the accuracy of an optimally windowed chirp (OWCh) sequence is directly comparable to that achievable with a standard frequency sweep, while the acquisition time can be reduced by up to two orders of magnitude, for comparable spectral content. Finally, we demonstrate the ability of this optimized signal to provide time-and frequency-resolved rheometric data by studying the fast gelation process of an acid-induced protein gel using repeated OWCh pulse sequences. The use of optimally windowed chirps enables a robust time-resolved rheological characterization of a wide range of soft materials undergoing rapid mutation and has the potential to become an invaluable tool for researchers across different disciplines.
Colloidal gels result from the aggregation of Brownian particles suspended in a solvent. Gelation is induced by attractive interactions between individual particles that drive the formation of clusters, which in turn aggregate to form a space-spanning structure. We study this process in aluminosilicate colloidal gels through time-resolved structural and mechanical spectroscopy. Using the time–connectivity superposition principle a series of rapidly acquired linear viscoelastic spectra, measured throughout the gelation process by applying an exponential chirp protocol, are rescaled onto a universal master curve that spans over eight orders of magnitude in reduced frequency. This analysis reveals that the underlying relaxation time spectrum of the colloidal gel is symmetric in time with power-law tails characterized by a single exponent that is set at the gel point. The microstructural mechanical network has a dual character; at short length scales and fast times it appears glassy, whereas at longer times and larger scales it is gel-like. These results can be captured by a simple three-parameter constitutive model and demonstrate that the microstructure of a mature colloidal gel bears the residual skeleton of the original sample-spanning network that is created at the gel point. Our conclusions are confirmed by applying the same technique to another well-known colloidal gel system composed of attractive silica nanoparticles. The results illustrate the power of the time–connectivity superposition principle for this class of soft glassy materials and provide a compact description for the dichotomous viscoelastic nature of weak colloidal gels.
We present the results of a combined experimental and theoretical study of drop coalescence in the presence of an initial temperature difference T 0 between a drop and a bath of the same liquid. We characterize experimentally the dependence of the residence time before coalescence on T 0 for silicone oils with different viscosities. Delayed coalescence arises above a critical temperature difference T c that depends on the fluid viscosity: for T 0 > T c , the delay time increases as T 2/3 0 for all liquids examined. This observed dependence is rationalized theoretically through consideration of the thermocapillary flows generated within the drop, the bath and the intervening air layer.
We use molecular dynamics simulations of a model three-dimensional particulate gel, to investigate the linear viscoelastic response. The numerical simulations are combined with a novel test protocol (the optimallywindowed chirp or OWCh), in which a continuous exponentially-varying frequency sweep windowed by a tapered cosine function is applied. The mechanical response of the gel is then analyzed in the Fourier domain. We show that i) OWCh leads to an accurate computation of the full frequency spectrum at a rate significantly faster than with the traditional discrete frequency sweeps, and with a reasonably high signal-tonoise ratio, and ii) the bulk viscoelastic response of the microscopic model can be described in terms of a simple mesoscopic constitutive model. The simulated gel response is in fact well described by a mechanical model corresponding to a fractional Kelvin-Voigt model with a single Scott-Blair (or springpot) element and a spring in parallel. By varying the viscous damping and the particle mass used in the microscopic simulations over a wide range of values, we demonstrate the existence of a single master curve for the frequency dependence of the viscoelastic response of the gel that is fully predicted by the constitutive model. By developing a fast and robust protocol for evaluating the linear viscoelastic spectrum of these soft solids, we open the path towards novel multiscale insight into the rheological response for such complex materials. arXiv:1805.07987v1 [cond-mat.soft]
An experimental protocol is developed to directly measure the new material functions revealed by medium amplitude parallel superposition (MAPS) rheology. This experimental protocol measures the medium amplitude response of a material to a simple shear deformation composed of three sine waves at different frequencies. Imposing this deformation and measuring the mechanical response reveals a rich data set consisting of up to 19 measurements of the third order complex modulus at distinct three-frequency coordinates. We discuss how the choice of the input frequencies influences the features of the MAPS domain studied by the experiment. A polynomial interpolation method for reducing the bias of measured values from spectral leakage and variance due to noise is discussed, including a derivation of the optimal range of amplitudes for the input signal. This leads to the conclusion that conducting the experiment in a stress-controlled fashion possesses a distinct advantage to the strain-controlled mode. The experimental protocol is demonstrated through measurements of the MAPS response of a model complex fluid: a surfactant solution of wormlike micelles. The resulting data set is indeed large and feature-rich, while still being acquired in a time comparable to similar medium amplitude oscillatory shear (MAOS) experiments. We demonstrate that the data represents measurements of an intrinsic material function by studying its internal consistency, its compatibility with low-frequency predictions for Coleman-Noll simple fluids, and its agreement with data obtained via MAOS amplitude sweeps. Finally, the data is compared to predictions from the corotational Maxwell model to demonstrate the power of MAPS rheology in determining whether a constitutive model is consistent with a material's time-dependent response.
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