A rotating unidirectional magnetic field generated by a motor-mounted permanent magnet was used to dynamically aggregate paramagnetic particles from suspension to form chains. Video microscopy and image processing were used to analyze the data. Good synchronicity was observed between the chains and the field up to 8 Hz frequency. Chain growth is facilitated at very low rotational frequencies initially after starting from static conditions, after which the mean chain length decreases in response to increasing viscous drag forces. As the frequency is increased from low values, the mean chain length decreases initially rapidly and later more slowly at higher frequencies, thus resulting in two regimes: the fast and the slow decrease regimes. Typical structures such as linear chains and S-shaped chains are observed as well as unusual U-shaped structures. The formation of dynamic S-shaped structures can be predicted based on the flexibility of the chains and the principle of conservation of angular momentum. Formation of single-chain aggregates is observed in microwells that are up to 50 µm wide, whereas in larger microwells multichain formation was noticed. The motor-mounted permanent magnet arrangement has applications in the development of portable microchip biosensors. The arrangement proved sufficient and reliable in forming chains, which display behavior similar to that observed under more elaborate and controlled conditions.
Paramagnetic particles, when subjected to external unidirectional rotating magnetic fields, form chains which rotate along with the magnetic field. In this paper three simulation methods, particle dynamics (PD), Stokesian dynamics (SD) and lattice Boltzmann (LB) methods, are used to study the dynamics of these rotating chains. SD simulations with two different levels of approximations-additivity of forces (AF) and additivity of velocities (AV)-for hydrodynamic interactions have been carried out. The effect of hydrodynamic interactions between paramagnetic particles under the effect of a rotating magnetic field is analyzed by comparing the LB and SD simulations, both of which include hydrodynamic interactions, with PD simulations in which hydrodynamic interactions are neglected. It was determined that for macroscopically observable properties like average chain length as a function of Mason number, reasonable agreement is found between all the three methods. For microscopic properties like the force distribution on each particle along the chain, inclusion of hydrodynamic interaction becomes important to understand the underlying physics of chain formation.
Mixing in microscale flows with rotating chains of paramagnetic particles can be enhanced by adjusting the ratio of viscous to magnetic forces so that chains dynamically break and reform. Lattice Boltzmann (LB) simulations were used to calculate the interaction between the fluid and suspended paramagnetic particles under the influence of a rotating magnetic field. Fluid velocities obtained from the LB simulations are used to solve the advection diffusion equation for massless tracer particles. At relatively high Mason numbers, small chains result in low edge velocities, and hence mixing is slower than at other Mason numbers. At low Mason numbers, long, stable chains form and produce little mixing toward the center of the chains. A peak in mixing rate is observed when chains break and reform. The uniformity of mixing is greater at higher Mason numbers because more small chains result in a larger number of small mixing areas.
Hormones are important bioactive compounds in blood and tissue that vary in concentration in response to stress and certain disease states. Establishing the changes in physiological hormone concentrations over time can lead to more effective diagnoses and perhaps a better understanding of the evolution of stress and disease. To monitor concentration over time, the sampling must be rapid and noninvasive; specimens such as saliva that require little effort to collect are preferred. However, more sensitive assay techniques are needed when compared to blood analysis since free hormone concentration in saliva is only a small fraction of the concentration in circulating blood. In this work, magnetic field-induced structures of paramagnetic particles are used as a solid substrate to demonstrate improved detection limits for a separation-free assay of cortisol. Once formed, the structures are subjected to a rotating magnetic field and this leads to two important features. First is the ability to utilize frequency and phase filtering (lock-in amplification) for the signal generated from surface-bound labeled species. Second is the improved mass transport of the antigen to the surface of the rotating structures. These two unique capabilities result in a quantifiable signal at a relatively low target antigen concentration. This method has been demonstrated with the detection of fluorescein isothiocyanate-labeled cortisol (FITC-cortisol) at a concentration of 300 pM.
Paramagnetic particle suspensions placed in a rotating unidirectional magnetic field form magnetic chains that rotate with the same frequency as the field. The motion of the fluid and particles surrounding the chain differs in phase and frequency from the chain rotation, a phenomenon that forms the basis of a sensitive detection scheme. Fluorescent particles that bind to the paramagnetic particles through their surface chemistry are used to demonstrate the concept. Epifluorescence video microscopy is used to capture images of the rotating chains. View windows placed over sequential images of rotating chains allows for measurement of the fluorescence brightness in the window, which is composed of periodic signal from the steady rotation of the chain plus the background. A lock-in reference synchronized to the chain rotation is used to enhance the fluorescence signal from chain and improve signal to noise. Two different modes of chain rotation and signal collection are demonstrated. This technique can be used to develop a fast and sensitive, homogenous microdevice based solid-phase immunoassay.
Tapping mode Atomic Force Microscopy (TmAFM) has been used to study the fungal polysaccharide scleroglucan deposited from aqueous solution and dimethyl sulfoxide (DMSO) onto a mica surface. The solutions from which the microscope samples were produced were prepared by first dissolving the solid scleroglucan in 0.1M NaOH, then neutralizing the solution with HCl, followed by dilution to the required concentration in either water or DMSO. It was found that from the aqueous solution described above, scleroglucan forms networks. Based on a comparison of the denatured‐renatured and aqueous solution samples, network formation is due to the imperfect registration between the chains forming the triple helices. The relatively large stiffness of the scleroglucan triple helix is also assumed to contribute to the formation of the extended networks. The triple helix diameter was measured to be 0.92 ± 0.27 nm, which is in the same range as that obtained by other researchers using similar techniques. Denatured scleroglucan, deposited from DMSO onto mica, forms a web‐like layer on top of which there are sphere‐like structures. These morphologies are believed to be due to triple helix denaturation yielding highly flexible single chains in DMSO, which results in coiling and web‐like dense packing of scleroglucan upon deposition onto mica. Most interestingly after addition of water to the samples deposited from DMSO, some of the chains can be renatured into short, stiff rod‐like structures which are similar to the structures observed by other researchers. The imaging data for aqueous solution deposition can be analyzed by plotting maximum end‐to‐end distance versus the perimeter of the networks deposited onto mica. This yields a Flory‐like exponent of 0.67, which is almost similar in value to that obtained by other researchers for linear structures of scleroglucan but less than that expected for a polymer chain following a self‐avoiding walk (v = 0.75) model on a two‐dimensional surface. The fractal dimension that can be used to characterize the networks was determined graphically to be 1.22 ± 0.06. © 1997 John Wiley & Sons, Inc. Biopoly 42: 89–100, 1997
Novel biochemical sensors consisting of rotating chains of microscale paramagnetic particles have been proposed that would enable convenient, sensitive analyte detection. Predicting the dynamics of these particles is required to optimise their design. The results of lattice Boltzmann (LB) and particle dynamics (PD) simulations are reported, where the LB approach provides a verified solution of the complete Navier-Stokes equations, including the hydrodynamic interactions among the particles. On the other hand, the simpler PD approach neglects hydrodynamic interactions, and does not compute the fluid motion. It is shown that macroscopic properties, like the number of aggregated particles, depend only on the drag force and not on the total hydrodynamic force, making PD simulations yield reasonably accurate predictions. Relatively good agreement between the LB and PD simulations, and qualitative agreement with experimental data, are found for the number of aggregated particles as a function of the Mason number. The drag force on a rotating cylinder is significantly different from that on particle chains calculated from both simulations, demonstrating the different dynamics between the two cases. For microscopic quantities like the detailed force distributions on each particle, the complete Navier-Stokes solution, here represented by the LB simulation, is required.
The microflow and stirring around paramagnetic particle microchains, referred to as microrotors, are modeled as a circular cylinder rotating about its radial axis at very low Reynolds number. Time scales for momentum transfer under these conditions are determined to be much smaller than those for boundary movement, hence a quasi-steady approximation can be used. The flow is derived at every instant from the case of a steady motion of a horizontally translating cylinder, with the rotation approximated to a series of differential incremental translations. A numerical simulation is used to determine the pathlines and material lines of virtual point fluid elements, which were analyzed to understand the behavior of the flow around the microrotor. The results indicate the flow to be unsteady, with chaotic advection observed in the system. The fluid motion is primarily two-dimensional, parallel to the rotational plane, with mixing limited to the immediate area around the rotating cylinder. Fluid layers, up to many cylinder diameters, in the axial direction experience the disturbance. Elliptic and star shaped pathlines, including periodic orbits, are observed depending on the fluid element's initial location. The trajectories and phase angles compare well with the experimental results, as well as with data from particle dynamics simulations. Material lines and streaklines display stretching and folding, which are indicative of the chaotic behavior and stirring characteristics of the system. The material lines have similar lengths for the same amount of rotation at different speeds, and the effect of rotational speeds appears to be primarily to change the time of mixing. The results are expected to help in the design of a particle microrotor based sensing technique.
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