Dipolophoresis and Travelling-Wave Dipolophoresis of Metal Microparticles

We study theoretically and numerically the electrokinetic behavior of metal microparticles immersed in aqueous electrolytes. We consider small particles subjected to non-homogeneous ac electric fields and we describe their motion as arising from the combination of electrical forces (dielectrophoresis) and the electroosmotic flows on the particle surface (induced-charge electrophoresis). The net particle motion is known as dipolophoresis. We also study the particle motion induced by travelling electric fields. We find analytical expressions for the dielectrophoresis and induced-charge electrophoresis of metal spheres and we compare them with numerical solutions. This validates our numerical method, which we also use to study the dipolophoresis of metal cylinders.Spanish Research Agency MCI under contract PGC2018-099217-B-I00

Precision manipulation of organic and inorganic nanoentities for enhanced optical biodetection at deterministic positions

In the last decade, considerable research interests are focused on applying semiconductor quantum dots (QDs) for bioimaging, sensing, and therapeutic delivery. Compared to traditional organic dyes, semiconductor QDs exhibit higher fluorescent brightness, better resistance to photo-bleaching, tunable sizes/colors, wider absorption peak and larger stokes shifts. However, the applications of QDs as biosensors are still largely conducted in bulk colloidal suspensions, which present considerable difficulties in sensing a minute amount of bioanalyte. It is highly desirable if the QDs can be registered at designated locations for position-predicable optical analysis and sensing. Raman scattering spectroscopy has been utilized to unambiguously identify molecules based on their intrinsic vibrational "fingerprint" states. However, due to the relatively small Raman scattering cross-section, the intensity of Raman signal is usually 1/10⁶ of that of Rayleigh scattering. The recent discovery of Surface enhanced Raman scattering (SERS) dramatically improves the Raman signal and rejuvenates this field. An enhancement factor (EF) as high as 10¹² have been reported, which can readily detect various single molecules, essential for early-stage disease detection, warfare agent detection, environmental pollutant detection, and biomolecule detection. However, SERS substrates with such high EF usually suffer from reproducibility and uniformity issues. Moreover, SERS detection is still largely conducted in a seek-and-find manner which substantially limits the detection efficiency. Most SERS detections are carried out by drying analyte solutions on SERS substrates to force molecules to attach to hotspots before the detection. The employed drying methods can be different among individual research groups. Quantitative comparison of these results should be conducted carefully. It is highly desirable to directly detect molecules in suspension to accurately evaluate the performances of different SERS substrates. However, when directly measuring SERS signals of molecules in suspension, due to the inefficient diffusion based binding process, much less molecules can closely interact with hot spots compared to those on dried SERS samples. As a result, direct SERS detection from suspension can often be less sensitive by a few orders of magnitudes compares to those in dried condition. It is of great interest to investigate new mechanisms to detect analyte molecules directly from analyte solutions with high sensitivity. In this research, I rationally designed and synthesized various types of nanostructures, including ZnO, Si, and Au nanowires, ZnO nanosuperstructures, and hybrid nanocapsules. Such materials have unique optical/plasmonic properties and could be used in various applications, particularly in biochemical sensing. Two types of optical nanobiosensors have been designed, fabricated, characterized, and investigated. They are fluorescence-based QD-on-nanowire assemblies and SERS-photonic-crystal hybrid nanosensors. The QD-on-nanowire florescent nanosensors operated uniquely by focusing analyte molecules to the assembled QDs on tips of nanowires before detection via specific biochemical conjugation. Molecules, such as biotin, can be revealed unambiguously in a location deterministic manner with substantially enhanced sensitivity. In the development of SERS-photonic-crystal hybrid nanosensors, two enhancement mechanisms, including guided-mode resonance (GMR) and electrokinetic effect, were studied and applied in improving the sensitivity and efficiency of molecule detection, respectively. Such a hybrid device has been proposed and studied for the first time, which can readily improve the detection sensitivity by a robust 4-5 times in addition to the 10⁹-10¹⁰ SERS enhancement. This dissertation work, exploring innovative materials design, synthesis, and manipulation, has made an important forward step in the next-generation biochemical detection platform.Materials Science and Engineerin

Advances in colloidal manipulation and transport via hydrodynamic interactions

In this review article, we highlight many recent advances in the field of micromanipulation of colloidal particles using hydrodynamic interactions (HIs), namely solvent mediated long-range interactions. At the micrsocale, the hydrodynamic laws are time reversible and the flow becomes laminar, features that allow precise manipulation and control of colloidal matter. We focus on different strategies where externally operated microstructures generate local flow fields that induce the advection and motion of the surrounding components. In addition, we review cases where the induced flow gives rise to hydrodynamic bound states that may synchronize during the process, a phenomenon essential in different systems such as those that exhibit self-assembly and swarming

Light modulation of electric field driven semiconductor micromotors

The future micro/nanorobots require high degrees of freedom in motion control to perform complex tasks by individuals or by a swarm. It remains a great challenge to control the motions of an individual nanomachine amidst many, to switch the operation modes facilely, and it is even more difficult to actuate several components of a nanomachine coordinately for purposed actions. This high degree of versatility is essential for the future micro/nanorobots and requires investigation of innovative actuation mechanisms. In this dissertation, we report our recent finding about a new approach combining two types of stimulation to achieve such goal. The micromotors being studied are made of semiconductor silicon nanowires. Mechanical motion of the motors is driven by several types of AC electric field. Meanwhile, the electrical property of the nanowires can be locally and instantaneously modulated by visible light illumination in a reversible manner. We demonstrate that visible light is able to change the electric polarization of semiconductor nanowires under AC electric field, and reflected by the dramatic change of mechanical motions with very rich configurations. Under a rotating electric field, the rotation speed of semiconductor Si nanowires in electric fields can instantly increase, decrease, and even reverse the orientation by light illumination in the visible to infrared regime at various AC E-field frequencies. Under a linear AC electric field, instantaneous change of alignment direction and speed of semiconductor nanowires is observed under visible-light exposure. With theoretical analysis and simulation, the working principle can be attributed to the optically tuned imaginary-part (out-phase) and real-part (in-phase) electrical polarization of a semiconductor nanowire in aqueous suspension. Based on the understanding of this system, we further propose a new approach to control the semiconductor micromotor via light tunable dielectrophoresis. Localized control of collective behavior in a highly density silicon nanowire suspension is also investigated. Finally, we demonstrated how to utilize the mechanical motion at microscale for practical application of biosensing.Materials Science and Engineerin

PROBING AND CONTROLLING FLUID RHEOLOGY AT MICROSCALE WITH MAGNETIC NANORODS

This Dissertation is focused on the development of new methods for characterization and control of fluid rheology using magnetic nanorods. This Dissertation consists of five chapters. In the first chapter, we review current microrheologial methods and develop a Magnetic Rotational Spectroscopy (MRS) model describing nanorod response to a rotating magnetic field. Using numerical modeling, we analyze the effects of materials parameters of nanorods and fluids on the MRS characteristic features. The model is designed for a specific experimental protocol. We introduce and examine physical parameters which can be measured experimentally. The model allows identification of MRS features enabling the calculation of fluid viscosity. The MRS of Non-Newtonian fluids with exponentially increasing viscosity is discussed for the first time. In the second chapter, we review the techniques for magnetic nanorods synthesis. We describe a setup and experimental protocol to synthesize nickel nanorods with the desired geometrical properties, in particular, with the controlled length to diameter ratio. We review magnetic systems used for manipulation of magnetic nanoparticles. A multifunctional magnetic rotator is introduced and described in detail in this chapter. We believe that this multifunctional magnetic system will be useful not only for micro and nanorheological studies, but will find much broader applications requiring remotely controlled manipulation of micro and nanoobjects. In the third chapter, we describe the MRS experiments and use the model developed in the first chapter for characterization of magnetic properties of synthesized nickel nanorods. The same setup is used to measure viscosity of microdroplets. We show that the diffraction pattern from the suspension of nickel nanorods aligned in a magnetic field can be rotated by a spinning magnetic field. This effect opens up an opportunity for the MRS using much smaller nanorods. Another practical application of the controlled diffraction patterns is discussed: the use of this pattern in medical optofluidic devices producing stationary illuminating spots, for example, in endoscopes. In the fourth chapter, we report on a new MRS method which can be used for the in-situ (or in-vivo) rheological measurements of fluids and polymer systems when the fluid viscosity increases exponentially with time. We use this method to measure the exponential change of the viscosity of HEMA (2-hydroxyethyl-methacrylate) undergoing photopolymerization. Remarkably, an exponential increase of viscosity can be traced beyond the point when the polymer system undergoes transition to a gel and the gel domains start to appear. We expect that this method will open up new horizons in the quantitative rheological analysis of fluids inside living cells, microorganisms, and aerosol droplets with thickeners. In the fifth chapter, we describe a physical principle of self-assembly of magnetic nanorods into droplets of different sizes. These droplets can be formed on demand using magneto-static interactions between magnetic nanorods and a magnetic field gradient. We theoretically and experimentally confirmed that the cluster of nanorods at the top of the droplet is acting as a cone-shape solid body deforming the top part of the droplet when moving towards the magnet. The developed model allows one to selectively concentrate a finite amount of magnetic nanorods at the free surface and print multiple microdroplets on demand

Integration of Nanostructures into Microsensor Devices on Whole Wafers

Chemical sensors are used in a wide variety of applications, such as environmental monitoring, fire detection, emission monitoring, and health monitoring. The fabrication of chemical sensors involving nanostructured materials holds the potential for the development of sensor systems with unique properties and improved performance. However, the fabrication and processing of nanostructures for sensor applications currently are limited in the ability to control their location on the sensor, which in turn hinders the progress for batch fabrication. This report discusses the advantages of using nanomaterials in sensor designs, some of the challenges encountered with the integration of nanostructures into microsensor / devices, and then briefly describes different methods attempted by other groups to address this issue. Finally, this report will describe how our approach for the controlled alignment of nanostructures onto a sensor platform was applied to demonstrate an approach for the mass production of sensors with nanostructures

Assembly of multicellular constructs and microarrays of cells using magnetic nanowires

An approach is described for controlling the spatial organization of mammalian cells using ferromagnetic nanowires in conjunction with patterned micromagnet arrays. The nanowires are fabricated by electrodeposition in nanoporous templates, which allows for precise control of their size and magnetic properties. The high aspect ratio and large remanent magnetization of the nanowires enable suspensions of cells bound to Ni nanowires to be controlled with low magnetic fields. This was used to produce one- and two-dimensional field-tuned patterning of suspended 3T3 mouse fibroblasts. Self-assembled one-dimensional chains of cells were obtained through manipulation of the wires\u27 dipolar interactions. Ordered patterns of individual cells in two dimensions were formed through trapping onto magnetic microarrays of ellipsoidal permalloy micromagnets. Cell chains were formed on the arrays by varying the spacing between the micromagnets or the strength of fluid flow over the arrays. The positioning of cells on the array was further controlled by varying the direction of an external magnetic field. These results demonstrate the possibility of using magnetic nanowires to organize cells

High-performance artificial micro/nanomachines and their bioapplications

Artificial micro/nanomachines are micrometer or nanometer scale mechanical devices that convert diverse energy sources into controlled mechanical motions. The development and applications of these micro/nanomachines are among the most pressing challenges in the research field of nanoscience and nanotechnology. In this dissertation, we report innovative designs and operations of artificial micro/nanomachines for bioapplications in biochemical sensing, biomolecule capture, drug delivery and release. Based on the electric tweezers, innovative rotary nanomotors are bottom-up assembled with high efficiency from nanoscale building blocks, which are massively fabricated and less than 1 μm in all dimensions. After assembling, the rotary nanomotors achieve an ultrafast speed up to 18,000 rpm, an ultradurable operation lifetime of 80 hours, and over 1.1 million rotation cycles. To explore diverse alternative energy inputs for nanomotors, we also applied electric tweezers in the guided manipulation of chemical nanomotors: the motions of chemical nanomotors are aligned along the direction of AC electric fields and their speeds are modulated by the DC electric fields. The prowess of the manipulation of chemical nanomotors by the electric tweezers is demonstrated for applications in cargo delivery to designated microdocks and assembling of chemical nanomotors for powering rotary nanoelectromechanical system (NEMS) devices. To integrate the function of Raman sensing on the micro/nanomachines, plasmonic nanomotors and bio-photonic-plasmonic micromotors with silver (Ag) nanoparticle coating are designed and fabricated, which provide ultrasensitive detection of biochemicals by Surface-enhanced Raman spectroscopy (SERS). The plasmonic nanomotors are designed with nanoporous superstructures, providing high capacities of drug loading and large numbers of hotspots. The plasmonic nanomotors also actively manipulate molecules and tune the release rate in electric fields due to the induced electrokinetic effect. The bio-photonic-plasmonic micromotors based on biosilica diatom frustules are applied in the capture and detection of DNA molecules, which are significantly accelerated during the rotation of the micromotors. The fundamental mechanism is investigated and attributed to the reduction of Nernst diffusion layer caused by the rotation. The innovations of artificial micro/nanomachines including concept, design, fabrication, manipulation, and bioapplications in this dissertation, are expected to inspire various research areas including NEMS, nanorobotics, microfluidics, biochemical delivery, and diagnostic sensingMaterials Science and Engineerin