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Thickness-Dependent Photoelectrochemical Water Splitting on Ultrathin LaFeO3 Films Grown on Nb:SrTiO3. - The journal of physical chemistry letters
The performance of photoelectrodes can be modified by changing the material chemistry, geometry, and interface engineering. Specifically, nanoscale active layers can facilitate the collection of charge carriers. In heterostructure devices, the multiple material interfaces are particularly important, which at present are not well understood for oxides. Here, we report a detailed study of ultrathin (2-25 nm) LaFeO3 films grown epitaxially on Nb-doped SrTiO3. The films exhibit thickness-dependence with sensitivity to less than 10 nm in both the through-plane charge transfer conductivity and in the potential-dependent photoresponse. Supplementing photoelectrochemical measurements with X-ray photoelectron spectroscopy, spectroscopic ellipsometry, and electrochemical impedance spectroscopy, we construct a band model that accounts for this thickness dependence via a shifting valence-band offset at the film-substrate interface and the potential-dependent overlap of the depletion regions present at both the film-substrate and film-electrolyte interfaces. These results illustrate the utility of using active layer thickness and film-substrate interactions to tune the performance of photoelectrodes, providing insight for the design of efficient heterostructure oxide photoelectrochemical devices.
Piezotransistive transduction of femtoscale displacement for photoacoustic spectroscopy. - Nature communications
Measurement of femtoscale displacements in the ultrasonic frequency range is attractive for advanced material characterization and sensing, yet major challenges remain in their reliable transduction using non-optical modalities, which can dramatically reduce the size and complexity of the transducer assembly. Here we demonstrate femtoscale displacement transduction using an AlGaN/GaN heterojunction field effect transistor-integrated GaN microcantilever that utilizes piezoelectric polarization-induced changes in two-dimensional electron gas to transduce displacement with very high sensitivity. The piezotransistor demonstrated an ultra-high gauge factor of 8,700 while consuming an extremely low power of 1.36â€‰nW, and transduced external excitation with a superior noise-limited resolution of 12.43â€‰fmâ€‰Hz(-1/2) and an outstanding responsivity of 170â€‰nVâ€‰fm(-1), which is comparable to the optical transduction limits. These extraordinary characteristics, which enabled unique detection of nanogram quantity of analytes using photoacoustic spectroscopy, can be readily exploited in realizing a multitude of novel sensing paradigms.
Electronic Nose for Recognition of Volatile Vapor Mixtures Using a Nanopore-Enhanced Opto-Calorimetric Spectroscopy. - Analytical chemistry
An electronic nose (e-nose) for identification and quantification of volatile organic compounds (VOCs) vapor mixtures was developed using nanopore-enhanced opto-calorimetric spectroscopy. Opto-calorimetric spectroscopy based on specific molecular vibrational transitions in the mid infrared (IR) "molecular fingerprint" regime allows highly selective detection of VOCs vapor mixtures. Nanoporous anodic aluminum oxide (AAO) microcantilevers, fabricated using a two-step anodization and simple photolithography process, were utilized as highly sensitive thermomechanical sensors for opto-calorimetric signal transduction. The AAO microcantilevers were optimized by fine-tuning AAO nanopore diameter in order to enhance their thermomechanical sensitivity as well as their surface area. The thermomechanical sensitivity of a bilayer AAO microcantilever with a 60 nm pore diameter was approximately 1 Î¼m/K, which is far superior to that of a bilayer plain silicon (Si) microcantilever. The adsorbed molecules of VOCs mixtures on the AAO microcantilever were fully recognized and quantified by variations of peak positions and amplitudes in the opto-calorimetric IR spectra as well as by shifts in the resonance frequency of the AAO microcantilever with the adsorbed molecules. Furthermore, identification of complex organic compounds with a real industrial sample was demonstrated by this e-nose system.
Rapid discrimination of DNA strands using an opto-calorimetric microcantilever sensor. - Lab on a chip
A rapid technique for quantitative detection and discrimination of DNA strands without using immobilized probe molecules is demonstrated using an opto-calorimetric, self-powered sensor based on a Pb(Zr(0.52)Ti(0.48))O3 (PZT) microcantilever. Microcalorimetric infrared (IR) spectroscopy provides excellent chemical selectivity based on the unique molecular vibrational characteristics of each nucleotide in the mid IR region. The piezoelectric and pyroelectric properties of the PZT microcantilever were exploited in the quantitative detection and discrimination of adsorbed DNA strands with their spectral characteristics. We report the unique spectral characteristics of different DNA nucleotides that are monitored by wavelength-dependent temperature variations for different relative molar ratio of each nucleotide. This approach offers a fast, label-free technique which is highly sensitive and selective for the detection of single nucleotide differences in DNA strands and has the potential to be used as a rapid prescreening biosensor for various biomolecules.
Direct detection and speciation of trace explosives using a nanoporous multifunctional microcantilever. - Analytical chemistry
We have developed a highly selective and sensitive nanomechanical infrared (IR) calorimetric spectrometer for use in the direct detection of ultralow concentrations of explosive vapors using a nanoporous TiO2 cantilever. These cantilevers were fabricated using a two-step anodization and photolithography process. By patterning nanoscale wells onto a cantilever, its surface area is increased by 2 orders of magnitude and the surface is converted into a preconcentrator. Resonant excitation of adsorbed molecules using IR radiation causes the cantilever to bend due to temperature changes originating from the nonradiative decay process. The porous structure of the cantilever increases its thermomechanical sensitivity as well as the number of adsorbed molecules. The system performance was demonstrated by detecting binary explosive mixtures under ambient conditions. The TiO2 sensor surface also allows regeneration through the photocatalytic decomposition of adsorbates under UV irradiation.
Investigation of pH-induced protein conformation changes by nanomechanical deflection. - Langmuir : the ACS journal of surfaces and colloids
Broad-spectrum biosensing technologies examine sensor signals using biomarkers, such as proteins, DNA, antibodies, specific cells, and macromolecules, based on direct- or indirect-conformational changes. Here, we have investigated the pH-dependent conformational isomerization of human serum albumin (HSA) using microcantilevers as a sensing platform. Native and denatured proteins were immobilized on cantilever surfaces to understand the effect of pH on conformational changes of the protein with respect to the coupling ligand. Our results show that protonation and deprotonation of amino acid residues on proteins play a significant role in generating charge-induced cantilever deflection. Surface plasmon resonance (SPR) was employed as a complementary technique to validate the results.
Nanomechanical identification of liquid reagents in a microfluidic channel. - Lab on a chip
Integration of promising technologies that can enhance sensitivity, selectivity, and throughput into micro total analysis systems (Î¼TAS) are important in making them useful in precise screening of reaction byproducts in analytical chemistry, cellular biology and pharmaceutical industries. But unfortunately so far a method to precisely determine molecular signatures of reagents is missing in Î¼TAS. We have developed a technique whereby molecular signatures of 50 pL of liquid reagents confined within a bimetallic microchannel cantilever can be obtained. This is achieved using wavelength dependent mechanical bending of the cantilever under infrared (IR) radiation. This technique also allows simultaneous physical characterization of the liquid reagent using variations in resonance frequency. It is useful in lab-on-a-chip devices and has a myriad of applications in drug screening, bioreactor monitoring, and petrochemical analysis.
Photoacoustic spectroscopy of surface adsorbed molecules using a nanostructured coupled resonator array. - Nanotechnology
A rapid method of obtaining photoacoustic spectroscopic signals for trace amounts of surface adsorbed molecules using a nanostructured coupled resonator array is described. Explosive molecules adsorbed on a nanoporous anodic aluminum oxide cantilever, which has hexagonally ordered nanowells with diameters and well-to-well distances of 35 nm and 100 nm, respectively, are excited using pulsed infrared (IR) light with a frequency matching the common mode resonance frequency of the coupled resonator. The common mode resonance amplitudes of the coupled resonator as a function of illuminating IR wavelength present a photoacoustic IR absorption spectrum representing the chemical signatures of the adsorbed explosive molecules. In addition, the mass of the adsorbed molecules as an orthogonal signal for quantitative analysis is determined by measuring the variation of the localized, individual mode resonance frequency of a cantilever on the array. The limit of detection of the ternary mixture of explosive molecules (1:1:1 of trinitrotoluene (TNT), cyclotrimethylene trinitramine (RDX) and pentaerythritol tetranitrate (PETN)) is estimated to be ~ 100 ng cm(-2). These multi-modal signals enable us to perform quantitative and rapid chemical sensing and analysis in ambient conditions.
A negative dielectrophoresis and gravity-driven flow-based high-throughput and high-efficiency cell-sorting system. - Journal of laboratory automation
We present a negative dielectrophoresis (n-DEP)-based cell separation system for high-throughput and high-efficiency cell separation. To achieve a high throughput, the proposed system comprises macro-sized channel and cantilever-type electrode (CE) arrays (L Ã— W Ã—â€ƒH = 150 Âµm Ã— 500 Âµm Ã— 50 Âµm) to generate n-DEP force. For high efficiency, double separation modules, which have macro-sized channels and CE arrays in each separation module, are employed. In addition, flow regulators to precisely control the hydrodynamic force are allocated for each outlet. Because the hydrodynamic force and the n-DEP force acting on the target cell are the main determinants of the separation efficiency, we evaluate the theoretical amount of hydrodynamic force and n-DEP force acting on each target cell. Based on theoretical results, separation conditions are experimentally investigated. Finally, to demonstrate the separation performance, we performed the separation of target cells (live K562) from nontarget cells (dead K562) under conditions of low voltage (7Vp-p with 100 kHz) and a flow rate of 15 ÂµLâ€¢minâ»Â¹, 6 ÂµLâ€¢minâ»Â¹, and 8 ÂµLâ€¢minâ»Â¹ in outlets 1, 2, and 3, respectively. The system can separate target cells with 95% separation efficiency in the case of the ratio of 5:1 (live K562:dead K562).
In Situ Studies of the Temperature-Dependent Surface Structure and Chemistry of Single-Crystalline (001)-Oriented La0.8Sr0.2CoO3-Î´ Perovskite Thin Films. - The journal of physical chemistry letters
Perovskites are used to promote the kinetics of oxygen electrocatalysis in solid oxide fuel cells and oxygen permeation membranes. Little is known about the surface structure and chemistry of perovskites at high temperatures and partial oxygen pressures. Combining in situ X-ray reflectivity (XRR) and in situ ambient pressure X-ray photoelectron spectroscopy (APXPS), we report, for the first time, the evolution of the surface structure and chemistry of (001)-oriented perovskite La0.8Sr0.2CoO3-Î´ (LSC113) and (La0.5Sr0.5)2CoO4+Î´ (LSC214)-decorated LSC113 (LSC113/214) thin films as a function of temperature. Heating the (001)-oriented LSC113 surface leads to the formation of surface LSC214-like particles, which is further confirmed by ex situ Auger electron spectroscopy (AES). In contrast, the LSC113/214 surface, with activities much higher than that of LSC113, is stable upon heating. Combined in situ XRR and APXPS measurements support that Sr enrichment may occur at the LSC113 and LSC214 interface, which can be responsible for its markedly enhanced activities.
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57 Forest Gate Cir Oak Brook, IL 60523
1200 Harger Rd Suite 600
142 Saint Francis Circle
Provena St Joseph Hospital 77 N Airlite St
Elgin, IL 60523