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DOE OSTI2014

Opto-mechano-fluidic viscometer

The recent development of opto-mechano-fluidic resonators has provided—by harnessing photon radiation pressure—a microfluidics platform for the optical sensing of fluid density and bulk modulus. Here, we show that fluid viscosity can also be determined through optomechanical measurement of the vibrational noise spectrum of the resonator mechanical modes. A linear relationship between the spectral linewidth and root-viscosity is predicted and experimentally verified in the low viscosity regime. Our result is a step towards multi-frequency measurement of viscoelasticity of arbitrary fluids, without sample contamination, using highly sensitive optomechanics techniques.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

Dynamics of a spherical particle in an acoustic field: A multiscale approach

A rigid spherical particle in an acoustic wave field oscillates at the wave period but has also a mean motion on a longer time scale. The dynamics of this mean motion is crucial for numerous applications of acoustic microfluidics, including particle manipulation and flow visualisation. It is controlled by four physical effects: acoustic (radiation) pressure, streaming, inertia, and viscous drag. In this paper, we carry out a systematic multiscale analysis of the problem in order to assess the relative importance of these effects depending on the parameters of the system that include wave amplitude, wavelength, sound speed, sphere radius, and viscosity. We identify two distinguished regimes characterised by a balance among three of the four effects, and we derive the equations that govern the mean particle motion in each regime. This recovers and organises classical results by King [“On the acoustic radiation pressure on spheres,” Proc. R. Soc. A 147, 212–240 (1934)], Gor'kov [“On the forces acting on a small particle in an acoustical field in an ideal fluid,” Sov. Phys. 6, 773–775 (1962)], and Doinikov [“Acoustic radiation pressure on a rigid sphere in a viscous fluid,” Proc. R. Soc. London A 447, 447–466 (1994)], clarifies the range of validity of these results, and reveals a new nonlinear dynamical regime. In this regime, the mean motion of the particle remains intimately coupled to that of the surrounding fluid, and while viscosity affects the fluid motion, it plays no part in the acoustic pressure. Simplified equations, valid when only two physical effects control the particle motion, are also derived. They are used to obtain sufficient conditions for the particle to behave as a passive tracer of the Lagrangian-mean fluid motion.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Multi-focus parallel detection of fluorescent molecules at picomolar concentration with photonic nanojets arrays

Fluorescence sensing and fluorescence correlation spectroscopy (FCS) are powerful methods to detect and characterize single molecules; yet, their use has been restricted by expensive and complex optical apparatus. Here, we present a simple integrated design using a self-assembled bi-dimensional array of microspheres to realize multi-focus parallel detection scheme for FCS. We simultaneously illuminate and collect the fluorescence from several tens of microspheres, which all generate their own photonic nanojet to efficiently excite the molecules and collect the fluorescence emission. Each photonic nanojet contributes to the global detection volume, reaching FCS detection volumes of several tens of femtoliters while preserving the fluorescence excitation and collection efficiencies. The microspheres photonic nanojets array enables FCS experiments at low picomolar concentrations with a drastic reduction in apparatus cost and alignment constraints, ideal for microfluidic chip integration.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Inertial migration of deformable droplets in a microchannel

The microfluidic inertial effect is an effective way of focusing and sorting droplets suspended in a carrier fluid in microchannels. To understand the flow dynamics of microscale droplet migration, we conduct numerical simulations on the droplet motion and deformation in a straight microchannel. The results are compared with preliminary experiments and theoretical analysis. In contrast to most existing literature, the present simulations are three-dimensional and full length in the streamwise direction and consider the confinement effects for a rectangular cross section. To thoroughly examine the effect of the velocity distribution, the release positions of single droplets are varied in a quarter of the channel cross section based on the geometrical symmetries. The migration dynamics and equilibrium positions of the droplets are obtained for different fluid velocities and droplet sizes. Droplets with diameters larger than half of the channel height migrate to the centerline in the height direction and two equilibrium positions are observed between the centerline and the wall in the width direction. In addition to the well-known Segré-Silberberg equilibrium positions, new equilibrium positions closer to the centerline are observed. This finding is validated by preliminary experiments that are designed to introduce droplets at different initial lateral positions. Small droplets also migrate to two equilibrium positions in the quarter of the channel cross section, but the coordinates in the width direction are between the centerline and the wall. The equilibrium positions move toward the centerlines with increasing Reynolds number due to increasing deformations of the droplets. The distributions of the lift forces, angular velocities, and the deformation parameters of droplets along the two confinement direction are investigated in detail. Comparisons are made with theoretical predictions to determine the fundamentals of droplet migration in microchannels. In addition, existence of the inner equilibrium position is linked to the quartic velocity distribution in the width direction through a simple model for the slip angular velocities of droplets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Role of the potential landscape on the single-file diffusion through channels

Transport of colloid particles through narrow channels is ubiquitous in cell biology as well as becoming increasingly important for microfluidic applications or targeted drug delivery. Membrane channels in cells are useful models for artificial designs because of their high efficiency, selectivity, and robustness to external fluctuations. Here, we model the passive channels that let cargo simply diffuse through them, affected by a potential profile along the way. Passive transporters achieve high levels of efficiency and specificity from binding interactions with the cargo inside the channel. This however leads to a paradox: why should channels which are so narrow that they are blocked by their cargo evolve to have binding regions for their cargo if that will effectively block them? Using Brownian dynamics simulations, we show that different potentials, notably symmetric, increase the flux through narrow passive channels – and investigate how shape and depth of potentials influence the flux. We find that there exist optimal depths for certain potential shapes and that it is most efficient to apply a small force over an extended region of the channel. On the other hand, having several spatially discrete binding pockets will not alter the flux significantly. We also explore the role of many-particle effects arising from pairwise particle interactions with their neighbours and demonstrate that the relative changes in flux can be accounted for by the kinetics of the absorption reaction at the end of the channel.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Nanoliter-sized overheated reactor

We report on a microfluidic system formed by 200 nl water droplets, encapsulated by a 600 nl mineral oil placed on a hydrophobically coated glass microscope cover slip. The micromachined heater underneath the glass was able to heat up the sample at a heating rate of 650 °C/s, heating the water sample up to 200 °C in less than 2 s. The sample/glass and the sample/oil interface did not have nucleation centers, showing that the sample reached a superheated stage without the necessity of being pressurized to suppress boiling. This method can be utilized for various applications currently being conducted in autoclaves.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Electronic desalting for controlling the ionic environment in droplet-based biosensing platforms

The ability to control the ionic environment in saline waters and aqueous electrolytes is useful for desalination as well as electronic biosensing. We demonstrate a method of electronic desalting at micro-scale through on-chip micro electrodes. We show that, while desalting is limited in bulk solutions with unlimited availability of salts, significant desalting of ≥1 mM solutions can be achieved in sub-nanoliter volume droplets with diameters of ∼250 μm. Within these droplets, by using platinum-black microelectrodes and electrochemical surface treatments, we can enhance the electrode surface area to achieve >99% and 41% salt removal in 1 mM and 10 mM salt concentrations, respectively. Through self-consistent simulations and experimental measurements, we demonstrate that conventional double-layer theory over-predicts the desalting capacity and, hence, cannot be used to model systems that are mass limited or undergoing significant salt removal from the bulk. Our results will provide a better understanding of capacitive desalination, as well as a method for salt manipulation in high-throughput droplet-based microfluidic sensing platforms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Three-dimensional micro-printing of temperature sensors based on up-conversion luminescence

The pronounced temperature dependence of up-conversion luminescence from nanoparticles doped with rare-earth elements enables local temperature measurements. By mixing these nanoparticles into a commercially available photoresist containing the low-fluorescence photo-initiator Irgacure 369, and by using three-dimensional direct laser writing, we show that micrometer sized local temperature sensors can be positioned lithographically as desired. Positioning is possible in pre-structured environments, e.g., within buried microfluidic channels or on optical or electronic chips. We use the latter as an example and demonstrate the measurement for both free space and waveguide-coupled excitation and detection. For the free space setting, we achieve a temperature standard deviation of 0.5 K at a time resolution of 1 s.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

A review on the processing accuracy of two-photon polymerization

Two-photon polymerization (TPP) is a powerful and potential technology to fabricate true three-dimensional (3D) micro/nanostructures of various materials with subdiffraction-limit resolution. And it has been applied to microoptics, electronics, communications, biomedicine, microfluidic devices, MEMS and metamaterials. These applications, such as microoptics and photon crystals, put forward rigorous requirements on the processing accuracy of TPP, including the dimensional accuracy, shape accuracy and surface roughness and the processing accuracy influences their performance, even invalidate them. In order to fabricate precise 3D micro/nanostructures, the factors influencing the processing accuracy need to be considered comprehensively and systematically. In this paper, we review the basis of TPP micro/nanofabrication, including mechanism of TPP, experimental set-up for TPP and scaling laws of resolution of TPP. Then, we discuss the factors influencing the processing accuracy. Finally, we summarize the methods reported lately to improve the processing accuracy from improving the resolution and changing spatial arrangement of voxels.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Electrically and magnetically dual-driven Janus particles for handwriting-enabled electronic paper

In this work, we describe the synthesis of novel electrically and magnetically dual-driven Janus particles for a handwriting-enabled twisting ball display via the microfluidic technique. One hemisphere of the Janus particles contains a charge control agent, which allows the display color to be controlled by applying a voltage and superparamagnetic nanoparticles, allows handwriting by applying a magnetic field to the display. We fabricated a twisting ball display utilizing these Janus particles and tested the electric color control and handwriting using a magnet. As a result, the display was capable of permitting handwriting with a small magnet in addition to conventional color control using an applied voltage (80 V). Handwriting performance was improved by increasing the concentration of superparamagnetic nanoparticles and was determined to be possible even when 80 V was applied across the electrodes for 4 wt. % superparamagnetic nanoparticles in one hemisphere. This improvement was impossible when the concentration was reduced to 2 wt. % superparamagnetic nanoparticles. The technology presented in our work can be applied to low-cost, lightweight, highly visible, and energy-saving electronic message boards and large whiteboards because the large-size display can be fabricated easily due to its simple structure.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Lattice Boltzmann simulation of immiscible fluid displacement in porous media: Homogeneous versus heterogeneous pore network

Injection of anthropogenic carbon dioxide (CO{sub 2}) into geological formations is a promising approach to reduce greenhouse gas emissions into the atmosphere. Predicting the amount of CO{sub 2} that can be captured and its long-term storage stability in subsurface requires a fundamental understanding of multiphase displacement phenomena at the pore scale. In this paper, the lattice Boltzmann method is employed to simulate the immiscible displacement of a wetting fluid by a non-wetting one in two microfluidic flow cells, one with a homogeneous pore network and the other with a randomly heterogeneous pore network. We have identified three different displacement patterns, namely, stable displacement, capillary fingering, and viscous fingering, all of which are strongly dependent upon the capillary number (Ca), viscosity ratio (M), and the media heterogeneity. The non-wetting fluid saturation (S{sub nw}) is found to increase nearly linearly with logCa for each constant M. Increasing M (viscosity ratio of non-wetting fluid to wetting fluid) or decreasing the media heterogeneity can enhance the stability of the displacement process, resulting in an increase in S{sub nw}. In either pore networks, the specific interfacial length is linearly proportional to S{sub nw} during drainage with equal proportionality constant for all cases excluding those revealing considerable viscous fingering. Our numerical results confirm the previous experimental finding that the steady state specific interfacial length exhibits a linear dependence on S{sub nw} for either favorable (M ≥ 1) or unfavorable (M < 1) displacement, and the slope is slightly higher for the unfavorable displacement.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

The interaction between hexagonal boron nitride and water from first principles

The use of hexagonal boron nitride (h-BN) in microfluidic and nanofluidic applications requires a fundamental understanding of the interaction between water and the h-BN surface. A crucial component of the interaction is the binding energy, which is sensitive to the treatment of electron correlation. In this work, we use state of the art quantum Monte Carlo and quantum chemistry techniques to compute the binding energy. Compared to high-level many-body theory, we found that the second-order Møller-Plesset perturbation theory captures the interaction accurately and can thus be used to develop force field parameters between h-BN and water for use in atomic scale simulations. On the contrary, density functional theory with standard dispersion corrections tends to overestimate the binding energy by approximately 75%.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Note: A single-chamber tool for plasma activation and surface functionalization in microfabrication

We present a simple apparatus for improved surface modification of polydimethylsiloxane (PDMS) microfluidic devices. A single treatment chamber for plasma activation and chemical/physical vapor deposition steps minimizes the time-dependent degradation of surface activation that is inherent in multi-chamber techniques. Contamination and deposition irregularities are also minimized by conducting plasma activation and treatment phases in the same vacuum environment. An inductively coupled plasma driver allows for interchangeable treatment chambers. Atomic force microscopy confirms that silane deposition on PDMS gives much better surface quality than standard deposition methods, which yield a higher local roughness and pronounced irregularities in the surface.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Dynamic microscale temperature gradient in a gold nanorod solution measured by diffraction-limited nanothermometry

We quantify the dynamic microscale temperature gradient in a gold nanorod solution using quantum-dot-based microscopic fluorescence nanothermometry. By incorporating CdSe quantum dots into the solution as a nanothermometer, precise temperature mapping with diffraction-limited spatial resolution and sub-degree temperature resolution is achieved. The acquired data on heat generation and dissipation show an excellent agreement with theoretical simulations. This work reveals an effective approach for noninvasive temperature regulation with localized nanoheaters in microfluidic environment.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Quantification of protein interaction kinetics in a micro droplet

Characterization of protein interactions is essential to the discovery of disease biomarkers, the development of diagnostic assays, and the screening for therapeutic drugs. Conventional flow-through kinetic measurements need relative large amount of sample that is not feasible for precious protein samples. We report a novel method to measure protein interaction kinetics in a single droplet with sub microliter or less volume. A droplet in a humidity-controlled environmental chamber is replacing the microfluidic channels as the reactor for the protein interaction. The binding process is monitored by a surface plasmon resonance imaging (SPRi) system. Association curves are obtained from the average SPR image intensity in the center area of the droplet. The washing step required by conventional flow-through SPR method is eliminated in the droplet method. The association and dissociation rate constants and binding affinity of an antigen-antibody interaction are obtained by global fitting of association curves at different concentrations. The result obtained by this method is accurate as validated by conventional flow-through SPR system. This droplet-based method not only allows kinetic studies for proteins with limited supply but also opens the door for high-throughput protein interaction study in a droplet-based microarray format that enables measurement of many to many interactions on a single chip.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Manipulating bubbles with secondary Bjerknes forces

Gas bubbles in a sound field are submitted to a radiative force, known as the secondary Bjerknes force. We propose an original experimental setup that allows us to investigate in detail this force between two bubbles, as a function of the sonication frequency, as well as the bubbles radii and distance. We report the observation of both attractive and, more interestingly, repulsive Bjerknes force, when the two bubbles are driven in antiphase. Our experiments show the importance of taking multiple scatterings into account, which leads to a strong acoustic coupling of the bubbles when their radii are similar. Our setup demonstrates the accuracy of secondary Bjerknes forces for attracting or repealing a bubble, and could lead to new acoustic tools for noncontact manipulation in microfluidic devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

A self-adjustable four-point probing system using polymeric three dimensional coils and non-toxic liquid metal

This paper describes a self-adjustable four-point probe (S4PP) system with a square configuration. The S4PP system consists of 3D polymer coil springs for the independent operation of each tungsten (W) probe, microfluidic channels filled with a nontoxic liquid metal, and a LabView-based control system. The 3D coil springs made by PMMA are fabricated with a 3D printer and are positioned in a small container filled with the non-toxic liquid metal. This unique configuration allows independent self-adjustment of the probe heights for precise measurements of the electrical properties of both flexible and large-step-height microsamples. The feasibility of the fabricated S4PP system is evaluated by measuring the specific resistance of Cr and Au thin films deposited on silicon wafers. The system is then employed to evaluate the electrical properties of a Au thin film deposited onto a flexible and easily breakable silicon diaphragm (spring constant: ∼3.6 × 10{sup −5} N/m). The resistance of the Cr thin films (thickness: 450 nm) with step heights of 60 and 90 μm is also successfully characterized. These experimental results indicate that the proposed S4PP system can be applied to common metals and semiconductors as well as flexible and large-step-height samples.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Mutual capacitance of liquid conductors in deformable tactile sensing arrays

Advances in highly deformable electronics are needed in order to enable emerging categories of soft computing devices ranging from wearable electronics, to medical devices, and soft robotic components. The combination of highly elastic substrates with intrinsically stretchable conductors holds the promise of enabling electronic sensors that can conform to curved objects, reconfigurable displays, or soft biological tissues, including the skin. Here, we contribute sensing principles for tactile (mechanical image) sensors based on very low modulus polymer substrates with embedded liquid metal microfluidic arrays. The sensors are fabricated using a single-step casting method that utilizes fine nylon filaments to produce arrays of cylindrical channels on two layers. The liquid metal (gallium indium alloy) conductors that fill these channels readily adopt the shape of the embedding membrane, yielding levels of deformability greater than 400%, due to the use of soft polymer substrates. We modeled the sensor performance using electrostatic theory and continuum mechanics, yielding excellent agreement with experiments. Using a matrix-addressed capacitance measurement technique, we are able to resolve strain distributions with millimeter resolution over areas of several square centimeters.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗