Single-walled carbon nanotubes (SWNT) are particularly attractive for biomedical applications, because they exhibit a fluorescent signal in a spectral region where there is minimal interference from biological media. Although SWNT have been used as highly-sensitive detectors for various molecules, their use as in vivo biosensors requires the simultaneous optimization of various parameters, including biocompatibility, molecular recognition, high fluorescence quantum efficiency and signal transduction. Here we demonstrate that a polyethylene glycol ligated copolymer stabilizes near infrared fluorescent SWNT sensors in solution, enabling intravenous injection into mice and the selective detection of local nitric oxide (NO) concentration with a detection limit of 1 μM. The half-life for liver retention is 4 hours, with sensors clearing the lungs within 2 hours after injection, thus avoiding a dominant route of in vivo nanotoxicology. After localization within the liver, it is possible to follow the transient inflammation using NO as a marker and signalling molecule. To this end, we also report a spatial-spectral imaging algorithm to deconvolute fluorescence intensity and spatial information from measurements. Finally, we show that alginate encapsulated SWNT can function as an implantable inflammation sensor for in vivo NO detection, with no intrinsic immune reactivity or other adverse response, for more than 400 days. These results open new avenues for the use of such nanosensors in vivo for biomedical applications.

Implantable, near infrared (nIR) fluorescent nanosensors are advantageous for in vivo monitoring of biological analytes since they can be rendered selective for particular target molecule while utilizing their unique optical properties and the nIR tissue transparency window for information transfer without an internal power source or telemetry. However, basic questions remain regarding the optimal encapsulation platform, geometrical properties, and concentration ranges required for effective signal to noise ratio through biological tissue. In this work, we systematically explore these variables quantitatively to optimize the performance of such optical nanosensors for biomedical applications. We investigate both alginate and polyethylene glycol (PEG) as model hydrogel systems, encapsulating d(GT)15 ssDNA-wrapped single walled carbon nanotubes (SWNT) as model fluorescent nanoparticle sensors, responsive to riboflavin. Hydrogel sensors implanted 0.5 mm into thick tissue samples cause 50% reduction of initial fluorescence intensity, allowing an optical detection limit of 5.4 mm and 5.1 mm depth in tissue for alginate and PEG gels, respectively, at a SWNT concentration of 10 mg L−1, and 785 nm laser excitation of 80 mW and 30 s exposure. These findings are supported with in vivo nIR fluorescent imaging of SWNT hydrogels implanted subcutaneously in mice. For the case of SWNT, we find that the alginate system is preferable in terms of emission intensity, sensor response, rheological properties, and shelf life.

Capillary assisted passively pumped thermal management devices have gained importance due to their simple design and reduction in energy consumption. The performance of these devices is strongly dependent on the shape of the curved interface between the liquid and vapor phases. We developed a transient laser interferometry technique to investigate the evolution of the shape of the liquid-vapor interface in micropillar arrays during evaporation heat transfer. Controlled cylindrical micropillar arrays were fabricated on the front side of a silicon wafer, while thin-film heaters were deposited on the reverse side to emulate a heat source. The shape of the meniscus was determined using the fringe patterns resulting from interference of a monochromatic beam incident on the thin liquid layer. We studied the evolution of the shape of the meniscus on these surfaces under various operating conditions including varying the micropillar geometry and the applied heating power. By monitoring the transient behavior of the evaporating liquid-vapor interface, we accurately measured the absolute location and shape of the meniscus and calculated the contact angle and the maximum capillary pressure. We demonstrated that the receding contact angle which determines the capillary pumping limit is independent of the microstructure geometry and the rate of evaporation (i.e., the applied heating power). The results of this study provide fundamental insights into the dynamic behavior of the liquid-vapor interface in wick structures during phase-change heat transfer.

We captured interesting static and dynamic behavior of the liquid-vapor interface in well-defined silicon micropillar arrays during thermally driven evaporation of water from the microstructured surface. The 3-D shape of the meniscus was characterized via laser interferometry where bright and dark fringes result from the interference of incident and reflected monochromatic light due to a variable thickness thin liquid film (FIG. 1). During steady state evaporation experiments, water was supplied to the sample with a syringe pump at 10 μL/min. FIG. 2a and 2b show a SEM image of a typical fabricated micropillar array and a schematic of the experimental setup, respectively. When water wicks through the micropillar array, the meniscus in a unit cell (four pillars in FIG. 1) assumes an equilibrium shape depending on the location from the liquid source/reservoir and the ambient conditions (ambient evaporation at Qin = 0 W). At this point, the meniscus is pinned at the top of the pillars. As the evaporation rate increases due the applied heat flux, the meniscus increases in curvature, thus increasing the capillary pressure to sustain the higher evaporation rate. This is evidenced by the increasing number of fringes in the unit cell when Qin is increased (0 W, 0.11 W, 0.44 W, and 0.99 W, FIG. 1a-1d respectively). Beyond a maximum curvature, the meniscus de-pins from the pillar top surface and recedes within the unit cell. This occurs when the capillary pressure generated at this curvature, cannot balance the viscous loss resulting from flow through the micropillar array. We observed that this receding shape was independent of the applied heat, and only depended on the micropillar array geometry and the intrinsic wettability of the material. Representative meniscus profiles along the diagonal direction of the unit cell obtained from image analysis of FIG. 1 at various Qin are shown in FIG. 2c.

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