Xianming Dai

Ultrasensitive surface-enhanced Raman scattering detection in common fluids

Significance Many analytes in real-life samples, such as body fluids, soil contaminants, and explosives, are dispersed in liquid, solid, or air phases. However, it remains a challenge to create a platform to detect these analytes in all of these phases with high sensitivity and specificity. Here, we demonstrate a universal platform termed slippery liquid-infused porous surface-enhanced Raman scattering (SLIPSERS) that enables the enrichment and delivery of analytes originating from various phases into surface-enhanced Raman scattering (SERS)-sensitive sites and their subsequent detection down to the subfemtomolar level (<10−15 mol⋅L−1). Based on SLIPSERS, we have demonstrated detection of various chemicals, biological molecules, and environmental contaminants with high sensitivity and specificity. Our platform may lead to ultrasensitive molecular detection for applications related to analytical chemistry, diagnostics, environmental monitoring, and national security. Detecting target analytes with high specificity and sensitivity in any fluid is of fundamental importance to analytical science and technology. Surface-enhanced Raman scattering (SERS) has proven to be capable of detecting single molecules with high specificity, but achieving single-molecule sensitivity in any highly diluted solutions remains a challenge. Here we demonstrate a universal platform that allows for the enrichment and delivery of analytes into the SERS-sensitive sites in both aqueous and nonaqueous fluids, and its subsequent quantitative detection of Rhodamine 6G (R6G) down to ∼75 fM level (10−15 mol⋅L−1). Our platform, termed slippery liquid-infused porous surface-enhanced Raman scattering (SLIPSERS), is based on a slippery, omniphobic substrate that enables the complete concentration of analytes and SERS substrates (e.g., Au nanoparticles) within an evaporating liquid droplet. Combining our SLIPSERS platform with a SERS mapping technique, we have systematically quantified the probability, p(c), of detecting R6G molecules at concentrations c ranging from 750 fM (p > 90%) down to 75 aM (10−18 mol⋅L−1) levels (p ≤ 1.4%). The ability to detect analytes down to attomolar level is the lowest limit of detection for any SERS-based detection reported thus far. We have shown that analytes present in liquid, solid, or air phases can be extracted using a suitable liquid solvent and subsequently detected through SLIPSERS. Based on this platform, we have further demonstrated ultrasensitive detection of chemical and biological molecules as well as environmental contaminants within a broad range of common fluids for potential applications related to analytical chemistry, molecular diagnostics, environmental monitoring, and national security.

Slippery Wenzel State

Enhancing the mobility of liquid droplets on rough surfaces is of great interest in industry, with applications ranging from condensation heat transfer to water harvesting to the prevention of icing and frosting. The mobility of a liquid droplet on a rough solid surface has long been associated with its wetting state. When liquid drops are sitting on the top of the solid textures and air is trapped underneath, they are in the Cassie state. When the drops impregnate the solid textures, they are in the Wenzel state. While the Cassie state has long been associated with high droplet mobility and the Wenzel state with droplet pinning, our work challenges this existing convention by showing that both Cassie and Wenzel state droplets can be highly mobile on nanotexture-enabled slippery rough surfaces. Our surfaces were developed by engineering hierachical nano- and microscale textures and infusing liquid lubricant into the nanotextures alone to create a highly slippery rough surface. We have shown that droplet mobility can be maintained even after the Cassie-to-Wenzel transition. Moreover, the discovery of the slippery Wenzel state allows us to assess the fundamental limits of the classical and recent Wenzel models at the highest experimental precision to date, which could not be achieved by any other conventional rough surface. Our results show that the classical Wenzel eq (1936) cannot predict the wetting behaviors of highly wetting liquids in the Wenzel state.

Enhanced Nucleate Boiling on Horizontal Hydrophobic-Hydrophilic Carbon Nanotube Coatings

Ideal hydrophobic-hydrophilic composite cavities are highly desired to enhance nucleate boiling. However, it is challenging and costly to fabricate these types of cavities by conventional micro/nano fabrication techniques. In this study, a type of hydrophobic-hydrophilic composite interfaces were synthesized from functionalized multiwall carbon nanotubes by introducing hydrophilic functional groups on the pristine multiwall carbon nanotubes. This type of carbon nanotube enabled hydrophobic-hydrophilic composite interfaces were systematically characterized. Ideal cavities created by the interfaces were experimentally demonstrated to be the primary reason to substantially enhance nucleate boiling.

Can multiple flow boiling regimes be reduced into a single one in microchannels

We report that multiple and transitional flow boiling regimes in microchannels can be reduced into a single annular flow from the onset of nucleate boiling to the critical heat flux condition. Hydrophilic silicon nanowires directly grown on inner walls of microchannels were tailored to create boiling surfaces with optimal submicron pores surrounded by nanogaps through controlling the height and density of silicon nanowires using the nanocarpet effect. A single two-phase regime can be realized by controlling the flow structure in two aspects: reducing bubble size and transforming the dominant surface tension force from the cross-sectional plane to the inner-wall plane.

Capillary evaporation on micromembrane-enhanced microchannel wicks with atomic layer deposited silica

Due to the difficulty in depositing conformal coatings on high aspect ratio surfaces, capillary evaporation on superhydrophilic porous structures have not been well studied. In this work, superhydrophilic hybrid wick was fabricated by coating micromembrane-enhanced microchannels with 20 nm-thick silica (SiO2) using the atomic layer deposited (ALD) technique. Rapid ALD SiO2 coatings improve thin film evaporation of water on hybrid wicks by up to 56%. An appreciable enhancement of critical heat flux was not obtained in this study because of a compromise between the increased capillary pressure and viscous drag resulting from superhydrophilic ALD SiO2 coatings.

High frequency microbubble-switched oscillations modulated by microfluidic transistors

Creating high frequency two-phase oscillations (HF-TPOs) remains an important goal in advancing microscale fluidic logic devices, micro-mixers, micro-actuators, and flow controls. However, thermally driven TPO frequency has been hindered by confinements of compressible vapor bubbles and low thermal diffusivity in microfluidic systems. In this study, a mechanism creating high frequency microbubbles growth/collapse cycle has been developed to achieve HF-TPOs. A “microfluidic transistor” was conceptualized and fabricated to passively sustain and modulate HF-TPOs. Three orders of magnitude higher TPO frequency has been achieved compared to TPOs reported in literatures under similar working conditions.

Hydrophilic directional slippery rough surfaces for water harvesting

A hydrophilic directional slippery rough surface outperforms conventional liquid-repellent surfaces in water harvesting. Multifunctional surfaces that are favorable for both droplet nucleation and removal are highly desirable for water harvesting applications but are rare. Inspired by the unique functions of pitcher plants and rice leaves, we present a hydrophilic directional slippery rough surface (SRS) that is capable of rapidly nucleating and removing water droplets. Our surfaces consist of nanotextured directional microgrooves in which the nanotextures alone are infused with hydrophilic liquid lubricant. We have shown through molecular dynamics simulations that the physical origin of the efficient droplet nucleation is attributed to the hydrophilic surface functional groups, whereas the rapid droplet removal is due to the significantly reduced droplet pinning of the directional surface structures and slippery interface. We have further demonstrated that the SRS, owing to its large surface area, hydrophilic slippery interface, and directional liquid repellency, outperforms conventional liquid-repellent surfaces in water harvesting applications.

Biphilic Nanoporous Surfaces Enabled Exceptional Drag Reduction and Capillary Evaporation Enhancement

Simultaneously achieving drag reduction and capillary evaporation enhancement is highly desired but challenging because of the trade-off between two distinct hydrophobic and hydrophilic wettabilities. Here, we report a strategy to synthesize nanoscale biphilic surfaces to endow exceptional drag reduction through creating a unique slip boundary condition and fast capillary wetting by inducing nanoscopic hydrophilic areas. The biphilic nanoporous surfaces are synthesized by decorating hydrophilic functional groups on hydrophobic pristine multiwalled carbon nanotubes. We demonstrate that the carbon nanotube-enabled biphilic nanoporous surfaces lead to a 63.1% reduction of the friction coefficient, a 61.7% wetting speed improvement, and up to 158.6% enhancement of capillary evaporation heat transfer coefficient. A peak evaporation heat transfer coefficient of 21.2 W/(cm2·K) is achieved on the biphilic surfaces in a vertical direction.

Characterization of Hybrid-Wicked Copper Heat Pipe

Thermal management of high power electronics is becoming a critical issue as the power density of semiconductors increasing. The flat heat pipe (FHP) is widely used in the electronic cooling because it is possible to interface with flat electronics packages without additional conductive and interface resistances. The heat flux of the next generation electronics may exceed 100 W/cm2 , which is significantly beyond the cooling capabilities of commercially available FHP today. A novel micro scale hybrid wick was developed in this study to improve the effective thermal conductivity and working heat flux of FHP. The hybrid wick consists of multilayer of sintered copper woven meshes to promote the capillary pressure and microchannels underneath to reduce the flow resistance. The analysis indicates that the effective thermal conductivity and the capillary limit of flat heat pipe (FHPs) with this novel micro scale hybrid wicking structure can be significantly enhanced as compared to the reported FHPs. In this paper, the design of this innovative micro scale hybrid wick is illustrated. The fabrication and charging processes are also outlined. The preliminary experimental results show that the effective thermal conductivity can approach 12,270 W/(m·K), which is more than 30 times better than pure copper at approximate 91.3 W input heat.Copyright

Decoupling the influence of surface structure and intrinsic wettability on boiling heat transfer

Surface structure and intrinsic wettability are both important for boiling heat transfer. While superhydrophilic micro, nano, and hierarchical surfaces are widely used for boiling enhancement, in which the surface structure and intrinsic wettability usually couple together. This study aims to decouple their influences on boiling heat transfer. Copper meshes are utilized as the microporous structures, and conformal superhydrophilic films of TiO2 are deposited by atomic layer deposition (ALD). Although ALD coatings for boiling have been done on flat surfaces, this study separates the influence of surface structure from that of intrinsic wettability on a three-dimensional microporous surface. By comparing two and four layer meshes, we show that the surface structure has no obvious influence on the critical heat flux (CHF), but can significantly enhance the heat transfer coefficient (HTC). The intrinsic superhydrophilicity dramatically increases the CHF due to the fast rewetting of dryout regions. Our conclus...