Zheng Tengfei,
Wang Chaohui,
Niu Dong,
Jiang Weitao,
Shi Yongsheng,
Yin Lei,
Chen Bangdao,
Liu Hongzhong* and
Ding Yucheng
State Key Laboratory for Manufacturing Systems Engineering, Xi'an Jiaotong University, Xi'an 710049, People's Republic of China. E-mail: hzliu@mail.xjtu.edu.cn
First published on 4th September 2014
Ultrafast particle assembly plays an important role in subsequent analytical procedures and the development of miniaturized biological and chemical sensors. In this paper, standing surface acoustic wave (SSAW) devices are employed to drive nanoparticles in microlitre droplets with different concentrations of sodium chloride by exciting a MHz-order acoustic wave. Different patterns formed by particles are strongly dependent on the concentrations of sodium chloride. Two forces, i.e., the dielectrophoresis (DEP) force generated by the alternating voltage, and the fluid viscous drag force generated by the acoustic streaming, should dominate the particles' assembling process, and induce various assembling patterns. The intricate and interesting interplay between the fluid viscous drag force and the dielectrophoresis (DEP) force on the particles is investigated in this study. We consider electric dipolar interaction to study behaviors of particles in droplets with different sodium chloride concentrations caused by SSAWs. Theoretical analysis and experiments reveal that nanoparticles would form a regular pattern only when the dielectrophoresis (DEP) decreased via increasing the conductivity of the droplet.
Surface acoustic waves (SAWs) have proven to be a promising method for particle assembling and micro/nanostructure alignment. There has been much progress in controlling alignment of cells and microscale particles in droplets by SSAWs,7–9 as mentioned previously. The behaviors of particles in droplets are complex because of existence of the acoustic streaming. Priscilla et al.,10 for the first time, demonstrates the existence of a frequency-dependent crossover particle size that can be used for effective particles partitioning. Li et al.11 observes spatiotemporal patterns formed by colloids along the free surface of a drop beneath which SSAWs are applied.
Considering the particles in droplets driven by SSAWs, almost all the previous studies focus on the indirect drag force arising from acoustic streaming and the acoustic radiation force acting on the suspended particles.12,13 Priscilla et al.10 reveals that for a SSAW device with a certain frequency, there exists a critical size range, under which the particles are dominated by the drag force. In our paper, the size of the particles is smaller than the critical size range, so the particles are dominated by drag force. However, as the results of the piezoelectric effect and the inverse piezoelectric effect, a transient inhomogeneous electric field would be generated on the surface, while the SSAWs propagate along the free surface. The particles and the colloids, widely existing in chemical, biological and biomedical fields, will be acted by an electric field force14,15 in a high-frequency electric field, besides the drag force arising from acoustic streaming. In earlier studies, acoustic radiation forces caused by pressure fluctuations in the liquid played a major role in the manipulation of microscale objects. Recently, a piezoelectric field induced by the SSAWs is used to align and pattern metallic nanowires by dielectrophoresis (DEP) in microchannels.16–18 SSAWs induce an alternating electric field and create virtual electrodes19 on a piezoelectric substrate. Chen et al.18 manipulates nanowires in real time by controlling the distribution of the SSAW field.
In this paper, the role of the DEP force in the process of particles movement in a microlitre droplet is investigated. We demonstrate the complicated movement of particles in the droplet when SSAWs propagate into it. The experimental results indicate that, a force (namely DEP force), caused by the electric field when SSAWs propagating, also contributes to the particle concentration. By decreasing DEP forces, particle lines are obtained. Further experiments and simulations are carried out to prove the effects of DEP force. This paper reveals the novel coupling of the DEP force and the drag force (arising from acoustic streaming) acting on a particle suspension to drive size-dependent spatial assembling and partitioning in a sessile droplet atop the substrate of a SAW device.
A SSAW device has been fabricated to investigate the electric field force generated by the inverse piezoelectric effect. The device consists of a lithium niobate substrate and two dual layer interdigital transducers (IDTs). The dual layer (Al/Cr) IDTs comprise straight finger pairs (typically 20) and are actuated at its characteristic resonant frequency (at 2.8 MHz). A voltage (25 V) is supplied to the SAW device (the voltage is generated by a signal generator (AFG3022, USA) and amplified by an amplifier (TREK MODEL 2100HF)), and measured by a digital oscilloscope (Tektronix TDS3014B, USA). The silica particles are synthesized by the classical Stober method. The hydrolysis of tetraethyl orthosilicate in the chemical reaction induces the adsorption of hydroxyl on the particle/liquid interface, resulting in an increase in the surface conductance to approximate 0.18 S m−1. The silica particles were then suspended in aqueous solution at individual concentration on the order of 106 particles per mL. The assembling behaviors of the particles in the microlitre droplet are observed by a microscope (Nikon eclipse LV100, Japan).
Fig. 2 illustrates the assembling process of nanoparticles in a deionized water droplet. As shown in Fig. 2(a), Particles distribute uniformly in a droplet before the SSAWs are applied. Fig. 2(b) shows that particles cluster to islands around the center of the droplet when SSAWs are applied, which is accompanied by low frequency sub-harmonic oscillations on the free surface of the droplet.11 Given that the SSAWs excitation power is kept constant and the drop is free to evaporate, by reducing the droplet volume, the amount and the positions of islands mutate subsequently. As a result, the concentration of the particles in the droplet is observed, as demonstrated in Fig. 2(c). After the drop volume decreased to a particular value, particles in the drop are collected to a double-pointed pattern, as showed in Fig. 2(d). The flow in the droplet, induced via acoustic streaming, attenuates along with the evaporation. And particles assemble in an island. Fig. 2(e) shows the assembling and partitioning of the particles in the drop.
Particles experience a complex motion when SSAWs are applied. The motion of particles in the droplet has been studied in previous works. However, the behaviors of the particles in ions solution have rarely been investigated. Fig. 3 illustrates the particle behaviors in the droplet of sodium chloride (0.144 g mL−1 in concentration). As shown in Fig. 3(a), particles distribute in a droplet uniformly before the SSAWs are applied. Fig. 3(b) shows the performance of the particles when the SSAWs are applied. Besides particles moving in cycles, most of the particles, dominated by the drag force, gather in chains located in the cycles. Then, the particles rings are broken up by the drag force and most particles are aligning along lines perpendicular to waves propagating direction (Fig. 3(c) and (d)). With further evaporation, the distance between the particles chains and the substrate surface diminishes, resulting in the FDEP increasing. Therefore, the particles chains rotate within the droplet. When the direction of the particle chains has an angle with the electric field lines, the chains are in an instant stable state balance of the drag force and the DEP force, as demonstrated in Fig. 3(d). Once the drop volume decreases to a certain value, the magnitude of the DEP exceed the drag force. The particle chains are dominated by the DEP force to align with the electric field (Fig. 3(f)). At first, particle chains are broken up and formed many particle islands distributing uniform within the drop. Then particle islands are moved to line up along the electric field lines and the wave propagation direction (Fig. 3(e) and (f)).
In our experiment, a similar phenomenon as that reported by Li et al.11 is observed at first. When deionized water is replaced by sodium chloride solution, however, particles begin to gather in lines perpendicular to the propagation direction of the SAW, and the behavior of gathering in lines is enhanced as the sodium chloride concentration increasing. The standing mechanical vibration induces an alternately charge distribution on the LiNbO3 substrate. The periodic distribution of electric charges, which is determined by SSAWs pressure antinodes, generates an AC electric field with electric field lines from positive charges to negative charges, and induces DEP force on the neutrally particles in the electric field. The DEP force has been used to align nanowires in the micro channel.16–18 The force on an induced dipole can be described as F ∝ (p·∇) E, where p is the dipole moment and E is the electric field.26 When deionized water was replaced by sodium chloride solution, the conductivity of the solution increased while the in-phase particle polarizability decreases.29,30 As a result, the DEP force decreases and the drag force dominates the movement of particles. Under the impact of the drag force, particles align in lines. To further study the functions of the DEP force and the drag force, an experiment about acoustic streaming and a simulation about DEP (Fig. 4) are employed.
In order to deeply understand the role of the drag force, further experiment is carried out by introducing a layer of coupling liquid (water) and an Au layer between the LiNbO3 substrate and the particle suspension droplet (Fig. 4(a)). The Au layer is designed to shield the particles from the electric field. As a result, the DEP force is significantly screened, whereas the SSAWs could still transmit into suspension. When a liquid droplet lies in the path of a SAW, the wave changes its mode to a leaky surface acoustic wave (LSAW) when it reaches the boundary between solid and liquid. The attenuation of the LSAW, due to viscous liquid loading, transfers a drag force into the droplet, resulting in a significant movement to the nodes in the droplet. Finally, particles assemble in lines perpendicular to the SAW wave line (Fig. 4(b)).
An electric field with frequency at MHz, which is generated on the surface while the SSAWs propagate on it, is exerted on the droplet. An alternating electric field hence exists in the liquid droplet, in which the field intensity attenuates with the increasing distance from the substrate surface. Since the conductivity of the particles is higher than its surroundings in the experimental conditions, they move closer to the chip substrate under the guidance of DEP force. Simultaneously, a near-field DEP attraction force would play its dominant role on particle chaining along the field lines once an appropriate particle concentration is applied.31 Therefore, the multiple activities of particles in the droplet are caused by the drag force and the DEP forces.
The periodic distribution of electric charges generates an electric field. To further study the forces exerted on nanoparticles, the electric field was simulated using COMSOL Multiphysics 4.3a software (Fig. 4(c)). The bottom part shows the vibration and potential of the lithium niobate. The up part shows the electric field in the droplet induced by the surface potential. The black arrows indicate that the field lines are parallel to the propagation direction of the SSAWs. When an electric field is imposed on suspension, the particles are polarized and a non-uniform induced free charge distribution accumulates at the particle surfaces. If further under the influence of a background field gradient, the DEP and the near-field DEP interaction force, acting on these interfacial dielectric gradients, would push nanoparticles in chain configuration with a parallel orientation to the local field lines. The simulation result shows that particles have the trend to line along the propagation direction of SAW (Fig. 4(d)).
The behavior of the particles is caused by the different orientations of the drag force and the DEP force acting on the particles (see Fig. 4(e)). As the SSAWs radiate into the droplet at the Rayleigh angle, the drag force, induced by the acoustic streaming, acts on the particles to drive them toward lines perpendicular to the SAW wave line, while the DEP force drives them toward the field lines. Under the combining effects of those two forces, most particles circulate within the droplet, except a few particles that locate in the crossing points of the field lines and the wave antinodes (see Fig. 2(b)). With the volume fraction of water decreasing in the evaporation process, the distance between the particles and the substrate reduces and the DEP force acting on particles increases. The intensive DEP force drives the particles to line up along the electric field line. As a result, particles form a baseball shape (see Fig. 2(c)). After the volume of the drop decreased to a certain value (see Fig. 2(d)), the area contained by the droplet is decreasing. The gradient of electric field diminishes and the DEP force decreases too, which leads to particles gathering in a double-pointed pattern (see Fig. 2(d)). Under the multiple effects of the acoustic fluid drag force and the DEP force, a double vortex flow pattern is produced in the droplet. To balance those forces, the vortexes locate at the line making angles with both the field lines and the wave antinodes. This arrangement is unstable not only for drag force but also for DEP force. Finally, the drag force disappears as the evaporation is continuous, particles around vortexes are broken up and gathering in an ellipse, aligning with the electric field line (see Fig. 2(e)).
When the deionized water is replaced by sodium chloride solution, the DEP force decreases due to the decreasing in-phase induced polarizability in high conductivity solution.29,30 The drag force dominates the movement of particles to form a regular pattern (see Fig. 3(b) and (c)). In the process of evaporation, the behaviors of particles are complicated. Since the distance between the particles chains and the substrate surface cuts down, the DEP force increases. Therefore, a trend can be clearly observed that particles try to align along the propagation direction of SSAWs (see Fig. 3(d)–(f)), which can be further proved by changing of the sodium chloride concentration. The experiment results are demonstrated as Fig. 5. In Fig. 5(a), only a few particles assemble in several islands, and those islands locate in circles formed by the combining effect of the drag force and the DEP force. With the decrease of DEP forces on account of higher conductivity, the length of particle chains increases and the new balance of the two forces makes the chains to align in lines having an angle with electric field line, as Fig. 5(b)–(d) show. When the concentration rises up to 0.144 g mL−1, most particles gather in lines perpendicular to the propagation direction of waves in Fig. 3(c). With the process of evaporation, the distance between the chains and the substrate surface diminishes. The DEP force FDEP, due to the Maxwell–Wagner interfacial charge relaxation, dominates the particles movement. Finally, particles gather in line along the electric field line. The length of the particle chains, perpendicular to the wave propagation direction, depends on the magnitude of the FDEP. Fig. 6 shows the FDEP dependence of the average length of particle chains, when the concentrations of the sodium chloride arise from 0.009 g mL−1 to 0.144 g mL−1.
The experimental results revel that, DEP force acting on particles exists when the SAW is applied in the fluid. The DEP force, induced by the inhomogeneous electric field arising from the inverse piezoelectric effect, enormously complicates the particles behaviors in the droplet. In order to manipulate nanoparticles in a droplet, more attention should be paid to the DEP force induced by SAW in the droplet.
Footnote |
| † Electronic supplementary information (ESI) available. See DOI: 10.1039/c4ra07090a |
| This journal is © The Royal Society of Chemistry 2014 |