Karthik Reddy

Analysis of single nanoparticle detection by using 3-dimensionally confined optofluidic ring resonators.

Viral particles are responsible for the majority of human fatal diseases, including Ebola fever, influenza, HIV, SARS, dengue fever, and so on. Those small infectious agents with radius ranging from 1 nm to 800 nm spread and transmit extremely rapidly, and leave very limited time for treatment if humans are infected [1]. The prevention and early diagnosis of those diseases require fast and trace amount detection of virus in liquid and in air. Among many approaches employed, the optical ring resonator based biosensor is one of the most sensitive devices, capable of detecting a single virion or nanoparticle in a real-time and label-free manner [2–3]. In a ring resonator, light circulates and forms whispering-gallery modes (WGMs). When a virion or nanoparticle binds onto the resonator surface, its interaction with the WGM leads to a spectral shift or mode splitting [2–3]. To date, by measuring the wavelength shift, a single influenza particle (50 nm in radius) in liquid has been detected experimentally with a solid microsphere [2]. Recently, by measuring the mode splitting, the detection and sizing of a single nanoparticle (30 nm in radius) in air have also been demonstrated with a microtoroid [3]. However, despite their excellent sensing performance, both structures lack of an efficient fluidic system to rapidly deliver samples to the sensing head (i.e., the ring resonator), which may significantly lengthen the detection time, in particular, when detecting a single nanoparticle.

A quasi-droplet optofluidic ring resonator laser using a micro-bubble

Optofluidic ring resonator lasers based on micro-bubbles filled with liquid gain medium are demonstrated. Due to the sub-micron wall thickness of the micro-bubble, significant amount of the electric field resides inside the liquid. Consequently, micro-bubbles mimic the droplets in air that have 3-dimensional optical confinement, extremely high Q-factors, and versatility in handling liquids of different refractive index. Furthermore, they enable repetitive interrogation and easy directional laser emission out-coupling without evaporation or size/shape variations. The laser using Rhodamine 6G in methanol is achieved with a threshold of 300 nJ/mm2 and 5.3 μJ/mm2 for 1 mM and 10 μM in concentration, respectively.

Ultrasensitive optofluidic surface-enhanced Raman scattering detection with flow-through multihole capillaries.

3-Dimensional surface-enhanced Raman scattering (SERS) detection integrated with optofluidics offers many advantages over conventional SERS conducted under planar and static conditions. In this paper, we developed a novel optofluidic SERS platform based on nanoparticle-functionalized flow-through multihole capillaries for rapid, reliable, and ultrasensitive analyte detection. The unique configuration not only provides 3-dimensional geometry for significantly increased SERS-active area and inherent fluidic channels for rapid and efficient sample delivery, but also confines and transmits light along the capillary for large SERS signal accumulation. Using a capillary consisting of thousands of micrometer-sized holes adsorbed with gold nanoparticles, we investigated the proposed optofluidic SERS system using the transverse and longitudinal detection methods, where the SERS excitation and collection were perpendicular to and along the capillary, respectively. A detection limit better than 100 fM for rhodamine 6G was achieved with an enhancement factor exceeding 10(8).

Optofluidic Fabry–Pérot cavity biosensor with integrated flow-through micro-/nanochannels

An optofluidic Fabry–Perot cavity label-free biosensor with integrated flow-through micro-/nanochannels is proposed and demonstrated, which takes advantages of the large surface-to-volume ratio for analyte concentration and high detection sensitivity and built-in fluidic channels for rapid analyte delivery. The operating principle is first discussed, followed by assembly of a robust sensing system. Real-time measurements are performed to test its sensing feasibility and capability including bulk solvent change and removal/binding of molecules from/onto the internal surface of fluidic channels. The results show that this sensor provides a very promising platform for rapid, sensitive, and high-throughput biological and chemical sensing.

Tunable single mode lasing from an on-chip optofluidic ring resonator laser

Single mode lasing from the polydimethylsiloxane based on-chip coupled optofluidic ring resonator (OFRR) with the lasing threshold of a few μJ/mm2 is demonstrated using the Vernier effect. The single mode operation is highly stable even at high pump energy densities. The effect of the OFRR size and coupling strength on the single mode emission is investigated, showing that the excessive coupling results in incomplete side mode suppression. Tuning of the lasing wavelength is achieved by modifying the dye solution.

Optofluidic laser for dual-mode sensitive biomolecular detection with a large dynamic range

Enzyme-linked immunosorbent assay (ELISA) is a powerful method for biomolecular analysis. The traditional ELISA employing light intensity as the sensing signal often encounters large background arising from non-specific bindings, material autofluorescence and leakage of excitation light, which deteriorates its detection limit and dynamic range. Here we develop the optofluidic laser-based ELISA, where ELISA occurs inside a laser cavity. The laser onset time is used as the sensing signal, which is inversely proportional to the enzyme concentration and hence the analyte concentration inside the cavity. We first elucidate the principle of the optofluidic laser-based ELISA, and then characterize the optofluidic laser performance. Finally, we present the dual-mode detection of interleukin-6 using commercial ELISA kits, where the sensing signals are simultaneously obtained by the traditional and the optofluidic laser-based ELISA, showing a detection limit of 1 fg ml(-1) (38 aM) and a dynamic range of 6 orders of magnitude.

Ultrasensitive vapor detection with surface-enhanced Raman scattering-active gold nanoparticle immobilized flow-through multihole capillaries.

We developed novel flow-through surface-enhanced Raman scattering (SERS) platforms using gold nanoparticle (Au-NP) immobilized multihole capillaries for rapid and sensitive vapor detection. The multihole capillaries consisting of thousands of micrometer-sized flow-through channels provide many unique characteristics for vapor detection. Most importantly, its three-dimensional SERS-active micro-/nanostructures make available multilayered assembly of Au-NPs, which greatly increase SERS-active surface area within a focal volume of excitation and collection, thus improving the detection sensitivity. In addition, the multihole capillarys inherent longitudinal channels offer rapid and convenient vapor delivery, yet its micrometer-sized holes increase the interaction between vapor molecules and SERS-active substrate. Experimentally, rapid pyridine vapor detection (within 1 s of exposure) and ultrasensitive 4-nitrophenol vapor detection (at a sub-ppb level) were successfully achieved in open air at room temperature. Such an ultrasensitive SERS platform enabled, for the first time, the investigation of both pyridine and 4-nitrophenol vapor adsorption isotherms at very low concentrations. Type I and type V behaviors of the International Union of Pure and Applied Chemistry isotherm were well observed, respectively.

Adaptive Two-Dimensional Microgas Chromatography

We proposed and investigated a novel adaptive two-dimensional (2-D) microgas chromatography system, which consists of one 1st-dimensional column, multiple parallel 2nd-dimensional columns, and a decision-making module. The decision-making module, installed between the 1st- and 2nd-dimensional columns, normally comprises an on-column nondestructive vapor detector, a flow routing system, and a computer that monitors the detection signal from the detector and sends out the trigger signal to the flow routing system. During the operation, effluents from the 1st-dimensional column are first detected by the detector and, then, depending on the signal generated by the detector, routed to one of the 2nd-dimensional columns sequentially for further separation. As compared to conventional 2-D GC systems, the proposed adaptive GC scheme has a number of unique and advantageous features. First and foremost, the multiple parallel columns are independent of each other. Therefore, their length, stationary phase, flow rate, and temperature can be optimized for best separation and maximal versatility. In addition, the adaptive GC significantly lowers the thermal modulator modulation frequency and hence power consumption. Finally, it greatly simplifies the postdata analysis process required to reconstruct the 2-D chromatogram. In this paper, the underlying working principle and data analysis of the adaptive GC was first discussed. Then, separation of a mixture of 20 analytes with various volatilities and polarities was demonstrated using an adaptive GC system with a single 2nd-dimensional column. Finally, an adaptive GC system with dual 2nd-dimensional columns was employed, in conjunction with temperature ramping, in a practical application to separate a mixture of plant emitted volatile organic compounds with significantly shortened analysis time.

Self-referenced composite Fabry-Pérot cavity vapor sensors

We develop a versatile, self-referenced composite Fabry-Pérot (FP) sensor and the corresponding detection scheme for rapid and precise measurement of vapors. The composite FP vapor sensor is formed by etching two juxtaposed micron-deep wells, with a precisely controlled offset in depth, on a silicon wafer. The wells are then coated with a vapor sensitive polymer and the reflected light from each well is detected by a CMOS imager. Due to its self-referenced nature, the composite FP sensor is able to extract the change in thickness and refractive index of the polymer layer upon exposure to analyte vapors, thus allowing for accurate vapor quantitation regardless of the polymer thickness, refractive index, and light incident angle and wavelength. Theoretical analysis is first performed to elucidate the underlying detection principle, followed by experimental demonstration at two different incident angles showing rapid and consistent measurement of the polymer changes when the polymer is exposed to three different analytes at various concentrations. The vapor detection limit is found to be on the order of a few pico-grams (~100 ppb).

Electrical Probing and Tuning of Molecular Physisorption on Graphene

The ability to tune the molecular interaction electronically can have profound impact on wide-ranging scientific frontiers in catalysis, chemical and biological sensor development, and the understanding of key biological processes. Despite that electrochemistry is routinely used to probe redox reactions involving loss or gain of electrons, electrical probing and tuning of the weaker noncovalent interactions, such as molecular physisorption, have been challenging, primarily due to the inability to change the work function of conventional metal electrodes. To this end, we report electrical probing and tuning of the noncovalent physisorption of polar molecules on graphene surface by using graphene nanoelectronic heterodyne sensors. Temperature-dependent molecular desorptions for six different polar molecules were measured in real-time to study the desorption kinetics and extract the binding affinities. More importantly, we demonstrate electrical tuning of molecule-graphene binding kinetics through electrostatic gating of graphene; the molecular desorption can be slowed down nearly three times within a gate voltage range of 15 V. Our results provide insight into small molecule-nanomaterial interaction dynamics and signify the ability to electrically tailor interactions, which can lead to rational designs of complex chemical processes for catalysis and drug discovery.