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Full-Text Articles in Physical Sciences and Mathematics

Improved Detection By Ensemble-Decision Aliquot Ranking Of Circulating Tumor Cells With Low Numbers Of A Targeted Surface Antigen, Eleanor S. Johnson, Robbyn K. Anand, Daniel T. Chiu Aug 2015

Improved Detection By Ensemble-Decision Aliquot Ranking Of Circulating Tumor Cells With Low Numbers Of A Targeted Surface Antigen, Eleanor S. Johnson, Robbyn K. Anand, Daniel T. Chiu

Robbyn Anand

Circulating tumor cells (CTCs) are shed from a solid tumor into the bloodstream and can seed new metastases. CTCs hold promise for cancer diagnosis and prognosis and to increase our understanding of the metastatic process. However, their low numbers in blood and varied phenotypic characteristics make their detection and isolation difficult. One source of heterogeneity among CTCs is molecular: When they leave the primary tumor, these cells must undergo a molecular transition, which increases their mobility and chance of survival in the blood. During this molecular transition, the cells lose some of their epithelial character, which is manifested by the …

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Synthetic Strategies For Tailoring The Physicochemical And Magnetic Properties Of Hydrophobic Magnetic Ionic Liquids, Omprakash Nacham, Kevin D. Clark, Honglian Yu, Jared L. Anderson Jan 2015

Synthetic Strategies For Tailoring The Physicochemical And Magnetic Properties Of Hydrophobic Magnetic Ionic Liquids, Omprakash Nacham, Kevin D. Clark, Honglian Yu, Jared L. Anderson

Jared L. Anderson

Magnetic ionic liquids (MILs) are a subclass of ionic liquids (ILs) containing paramagnetic components and are readily manipulated by an external magnetic field. Due to their hydrophilic nature, very few applications of MILs in aqueous systems have been reported. In this study, three general classes of hydrophobic MILs including monocationic, symmetrical/unsymmetrical dicationic, and symmetrical/unsymmetrical tricationic MILs were synthesized and characterized. By tuning the structure of the MIL, various physicochemical properties including water solubility, magnetic susceptibility, and melting point were regulated. MILs synthesized with the benzimidazolium cation were shown to exhibit lower water solubility (0.1% (w/v)) when compared to those containing …

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Extraction Of Dna By Magnetic Ionic Liquids: Tunable Solvents For Rapid And Selective Dna Analysis, Kevin D. Clark, Omprakash Nacham, Honglian Yu, Tianhao Li, Melissa M. Yamsek, Donald R. Ronning, Jared L. Anderson Jan 2015

Extraction Of Dna By Magnetic Ionic Liquids: Tunable Solvents For Rapid And Selective Dna Analysis, Kevin D. Clark, Omprakash Nacham, Honglian Yu, Tianhao Li, Melissa M. Yamsek, Donald R. Ronning, Jared L. Anderson

Jared L. Anderson

DNA extraction represents a significant bottleneck in nucleic acid analysis. In this study, hydrophobic magnetic ionic liquids (MILs) were synthesized and employed as solvents for the rapid and efficient extraction of DNA from aqueous solution. The DNA-enriched microdroplets were manipulated by application of a magnetic field. The three MILs examined in this study exhibited unique DNA extraction capabilities when applied toward a variety of DNA samples and matrices. High extraction efficiencies were obtained for smaller single-stranded and double-stranded DNA using the benzyltrioctylammonium bromotrichloroferrate(III) ([(C8)3BnN+][FeCl3Br–]) MIL, while the dicationic 1,12-di(3-hexadecylbenzimidazolium)dodecane bis[(trifluoromethyl)sulfonyl]imide bromotrichloroferrate(III) ([(C16BnIM)2C122+][NTf2–, FeCl3Br–]) MIL produced higher extraction efficiencies for larger …

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Large Interdomain Rearrangement Triggered By Suppression Of Micro- To Millisecond Dynamics In Bacterial ​Enzyme I, Vincenzo Venditti, Vitali Tugarinov, Charles D. Schwieters, Alexander Grishaev, G. Marius Clore Jan 2015

Large Interdomain Rearrangement Triggered By Suppression Of Micro- To Millisecond Dynamics In Bacterial ​Enzyme I, Vincenzo Venditti, Vitali Tugarinov, Charles D. Schwieters, Alexander Grishaev, G. Marius Clore

Vincenzo Venditti

Enzyme I (EI), the first component of the bacterial phosphotransfer signal transduction system, undergoes one of the largest substrate-induced interdomain rearrangements documented to date. Here we characterize the perturbations generated by two small molecules, the natural substrate phosphoenolpyruvate and the inhibitor a-ketoglutarate, on the structure and dynamics of EI using NMR, small-angle X-ray scattering and biochemical techniques. The results indicate unambiguously that the open-to-closed conformational switch of EI is triggered by complete suppression of micro- to millisecond dynamics within the C-terminal domain of EI. Indeed, we show that a ligand-induced transition from a dynamic to a more rigid conformational state …

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Negative Dielectrophoretic Capture And Repulsion Of Single Cells At A Bipolar Electrode: The Impact Of Faradaic Ion Enrichment And Depletion, Robbyn K. Anand, Eleanor S. Johnson, Daniel T. Chiu Jan 2015

Negative Dielectrophoretic Capture And Repulsion Of Single Cells At A Bipolar Electrode: The Impact Of Faradaic Ion Enrichment And Depletion, Robbyn K. Anand, Eleanor S. Johnson, Daniel T. Chiu

Robbyn Anand

This paper describes the dielectrophoretic (DEP) forces generated by a bipolar electrode (BPE) in a microfluidic device and elucidates the impact of faradaic ion enrichment and depletion (FIE and FID) on electric field gradients. DEP technologies for manipulating biological cells provide several distinct advantages over other cell-handling techniques including label-free selectivity, inexpensive device components, and amenability to single-cell and array-based applications. However, extension to the array format is nontrivial, and DEP forces are notoriously short-range, limiting device dimensions and throughput. BPEs present an attractive option for DEP because of the ease with which they can be arrayed. Here, we present …

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Influence Of Environment On The Measurement Of Rates Of Charge Transport Across Agts/Sam//Ga2o3/Egain Junctions, Jabulani R. Barber, Hyo Jae Yoon, Carleen M. Bowers, Martin M. Thuo, Benjamin Breiten, Diana M. Gooding, George M. Whitesides Jun 2014

Influence Of Environment On The Measurement Of Rates Of Charge Transport Across Agts/Sam//Ga2o3/Egain Junctions, Jabulani R. Barber, Hyo Jae Yoon, Carleen M. Bowers, Martin M. Thuo, Benjamin Breiten, Diana M. Gooding, George M. Whitesides

Martin M. Thuo

This paper investigates the influence of the atmosphere used in the fabrication of top electrodes from the liquid eutectic of gallium and indium (EGaIn) (the so-called “EGaIn” electrodes), and in measurements of current density, J(V) (A/cm2), across self-assembled monolayers (SAMs) incorporated into Ag/SR//Ga2O3/EGaIn junctions, on values of J(V) obtained using these electrodes. A gas-tight measurement chamber was used to control the atmosphere in which the electrodes were formed, and also to control the environment in which the electrodes were used to measure current densities across SAM-based junctions. Seven different atmospheres—air, oxygen, nitrogen, argon, and ammonia, as well as air containing …

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Fabrication Of Low-Cost Paper-Based Microfluidic Devices By Embossing Or Cut-And-Stack Methods, Martin M. Thuo, Ramses V. Martinez, Wen-Jie Lan, Xinyu Liu, Jabulani Barber, Manza B. Atkinson, Dineth Bandarage, Jean-Francis Bloch, George M. Whitesides Jun 2014

Fabrication Of Low-Cost Paper-Based Microfluidic Devices By Embossing Or Cut-And-Stack Methods, Martin M. Thuo, Ramses V. Martinez, Wen-Jie Lan, Xinyu Liu, Jabulani Barber, Manza B. Atkinson, Dineth Bandarage, Jean-Francis Bloch, George M. Whitesides

Martin M. Thuo

This article describes the use of embossing and “cut-and-stack” methods of assembly, to generate microfluidic devices from omniphobic paper and demonstrates that fluid flowing through these devices behaves similarly to fluid in an open-channel microfluidic device. The porosity of the paper to gases allows processes not possible in devices made using PDMS or other nonporous materials. Droplet generators and phase separators, for example, could be made by embossing “T”-shaped channels on paper. Vertical stacking of embossed or cut layers of omniphobic paper generated three-dimensional systems of microchannels. The gas permeability of the paper allowed fluid in the microchannel to contact …

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Tuning The Selectivity Of Ionic Liquid Stationary Phases For Enhanced Separation Of Nonpolar Analytes In Kerosene Using Multidimensional Gas Chromatography, Leandro W. Hantao, Ali Najafi, Cheng Zhang, Fabio Augusto, Jared L. Anderson Mar 2014

Tuning The Selectivity Of Ionic Liquid Stationary Phases For Enhanced Separation Of Nonpolar Analytes In Kerosene Using Multidimensional Gas Chromatography, Leandro W. Hantao, Ali Najafi, Cheng Zhang, Fabio Augusto, Jared L. Anderson

Jared L. Anderson

In this study, a series of ionic liquids (ILs) are evaluated as stationary phases in comprehensive two-dimensional gas chromatography (GC × GC) for the separation of aliphatic hydrocarbons from kerosene. IL-based stationary phases were carefully designed to evaluate the role of cavity formation/dispersive interaction on the chromatographic retention of nonpolar analytes by GC × GC. The maximum allowable operating temperature (MAOT) of the IL-based columns was compared to that of commercial IL-based columns. Evaluation of the solvation characteristics of GC columns guided the selection of the best performing IL-based stationary phases for the resolution of aliphatic hydrocarbons, namely, trihexyl(tetradecyl)phosphonium tetrachloroferrate …

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A Nmr Experiment For Simultaneous Correlations Of Valine And Leucine/Isoleucine Methyls With Carbonyl Chemical Shifts In Proteins, Vitali Tugarinov, Vincenzo Venditti, G. Marius Clore Jan 2014

A Nmr Experiment For Simultaneous Correlations Of Valine And Leucine/Isoleucine Methyls With Carbonyl Chemical Shifts In Proteins, Vitali Tugarinov, Vincenzo Venditti, G. Marius Clore

Vincenzo Venditti

A methyl-detected ‘out-and-back’ NMR experiment for obtaining simultaneous correlations of methyl resonances of valine and isoleucine/leucine residues with backbone carbonyl chemical shifts, SIM-HMCM(CGCBCA)CO, is described. The developed pulse-scheme serves the purpose of convenience in recording a single data set for all Ileδ1, Leuδ and Valγ (ILV) methyl positions instead of acquiring two separate spectra selective for valine or leucine/isoleucine residues. The SIM-HMCM(CGCBCA)CO experiment can be used for ILV methyl assignments in moderately sized protein systems (up to ~100 kDa) where the backbone chemical shifts of 13Cα, 13Cβ and 13CO are known from prior NMR studies and where some losses in …

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Interplay Of Hydrogen Bonds And N→Π* Interactions In Proteins, Gail J. Bartlett, Robert W. Newberry, Brett Vanveller, Ronald T. Raines, Derek N. Woolfson Nov 2013

Interplay Of Hydrogen Bonds And N→Π* Interactions In Proteins, Gail J. Bartlett, Robert W. Newberry, Brett Vanveller, Ronald T. Raines, Derek N. Woolfson

Brett VanVeller

Protein structures are stabilized by multiple weak interactions, including the hydrophobic effect, hydrogen bonds, electrostatic effects, and van der Waals interactions. Among these interactions, the hydrogen bond is distinct in having its origins in electron delocalization. Recently, another type of electron delocalization, the n→π* interaction between carbonyl groups, has been shown to play a role in stabilizing protein structure. Here we examine the interplay between hydrogen bonding and n→π* interactions. To address this issue, we used data available from high-resolution protein crystal structures to interrogate asparagine side-chain oxygen atoms that are both acceptors of a hydrogen bond and donors of …

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Ionic Liquids In Analytical Chemistry: Fundamentals, Advances, And Perspectives, Tien D. Ho, Cheng Zhang, Leandro W. Hantao, Jared L. Anderson Nov 2013

Ionic Liquids In Analytical Chemistry: Fundamentals, Advances, And Perspectives, Tien D. Ho, Cheng Zhang, Leandro W. Hantao, Jared L. Anderson

Jared L. Anderson

Since their initial discovery in 1914, ionic liquids (ILs) have been widely studied in multiple chemistry disciplines. Applications of ILs in analytical chemistry have enjoyed much success and contributed to the rapid evolution of the ionic liquid field. ILs are collectively known as organic salts which possess melting points at or below 100 °C. In most cases, ILs are composed of an organic cation and an organic or inorganic anion. It has been estimated there can be up to 1018 possible combinations of ILs, due to the ability to interchange their corresponding cationic/anionic moieties.

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Defining The Value Of Injection Current And Effective Electrical Contact Area For Egain-Based Molecular Tunneling Junctions, Felice C. Simeone, Hyo Jae Yoon, Martin M. Thuo, Jabulani R. Barber, Barbara Smith, George M. Whitesides Nov 2013

Defining The Value Of Injection Current And Effective Electrical Contact Area For Egain-Based Molecular Tunneling Junctions, Felice C. Simeone, Hyo Jae Yoon, Martin M. Thuo, Jabulani R. Barber, Barbara Smith, George M. Whitesides

Martin M. Thuo

Analysis of rates of tunneling across self-assembled monolayers (SAMs) of n-alkanethiolates SCn (with n = number of carbon atoms) incorporated in junctions having structure AgTS-SAM//Ga2O3/EGaIn leads to a value for the injection tunnel current density J0 (i.e., the current flowing through an ideal junction with n = 0) of 103.6±0.3 A·cm–2 (V = +0.5 V). This estimation of J0 does not involve an extrapolation in length, because it was possible to measure current densities across SAMs over the range of lengths n = 1–18. This value of J0 is estimated under the assumption that values of the geometrical contact area …

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A Microfluidic Paper-Based Electrochemical Biosensor Array For Multiplexed Detection Of Metabolic Biomarkers, Chen Zhao, Martin M. Thuo, Xinyu Liu Oct 2013

A Microfluidic Paper-Based Electrochemical Biosensor Array For Multiplexed Detection Of Metabolic Biomarkers, Chen Zhao, Martin M. Thuo, Xinyu Liu

Martin M. Thuo

Paper-based microfluidic devices have emerged as simple yet powerful platforms for performing low-cost analytical tests. This paper reports a microfluidic paper-based electrochemical biosensor array for multiplexed detection of physiologically relevant metabolic biomarkers. Different from existing paper-based electrochemical devices, our device includes an array of eight electrochemical sensors and utilizes a handheld custom-made electrochemical reader (potentiostat) for signal readout. The biosensor array can detect several analytes in a sample solution and produce multiple measurements for each analyte from a single run. Using the device, we demonstrate simultaneous detection of glucose, lactate and uric acid in urine, with analytical performance comparable to …

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Detection Of Boronic Acids Through Excited-State Intramolecular Proton-Transfer Fluorescence, Matthew R. Aronoff, Brett Vanveller, Ronald T. Raines Oct 2013

Detection Of Boronic Acids Through Excited-State Intramolecular Proton-Transfer Fluorescence, Matthew R. Aronoff, Brett Vanveller, Ronald T. Raines

Brett VanVeller

Boronic acids are versatile reagents for the chemical synthesis of organic molecules. They and other boron-containing compounds can be detected readily by the interruption of the excited-state intramolecular proton transfer (ESIPT) of 10-hydroxybenzo[h]quinolone. This method is highly sensitive and selective, and useful for monitoring synthetic reactions and detecting boron-containing compounds on a solid support.

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A Divalent Protecting Group For Benzoxaboroles, Brett Vanveller, Matthew R. Aronoff, Ronald T. Raines Sep 2013

A Divalent Protecting Group For Benzoxaboroles, Brett Vanveller, Matthew R. Aronoff, Ronald T. Raines

Brett VanVeller

1-Dimethylamino-8-methylaminonaphthalene is put forth as a protecting group for benzoxaboroles. The ensuing complex is fluorescent, charge-neutral, highly stable under basic conditions, stable to anhydrous acid, and readily cleavable in aqueous acid to return the free benzoxaborole.

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Paramagnetic Ionic Liquids For Measurements Of Density Using Magnetic Levitation, David K. Bwambok, Martin M. Thuo, Manza B.J. Atkinson, Katherine A. Mirica, Nathan D. Shapiro, George M. Whitesides Aug 2013

Paramagnetic Ionic Liquids For Measurements Of Density Using Magnetic Levitation, David K. Bwambok, Martin M. Thuo, Manza B.J. Atkinson, Katherine A. Mirica, Nathan D. Shapiro, George M. Whitesides

Martin M. Thuo

Paramagnetic ionic liquids (PILs) provide new capabilities to measurements of density using magnetic levitation (MagLev). In a typical measurement, a diamagnetic object of unknown density is placed in a container containing a PIL. The container is placed between two magnets (typically NdFeB, oriented with like poles facing). The density of the diamagnetic object can be determined by measuring its position in the magnetic field along the vertical axis (levitation height, h), either as an absolute value or relative to internal standards of known density. For density measurements by MagLev, PILs have three advantages over solutions of paramagnetic salts in aqueous …

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N→Π* Interactions Of Amides And Thioamides: Implications For Protein Stability, Robert W. Newberry, Brett Vanveller, Ilia A. Guzei, Ronald T. Raines May 2013

N→Π* Interactions Of Amides And Thioamides: Implications For Protein Stability, Robert W. Newberry, Brett Vanveller, Ilia A. Guzei, Ronald T. Raines

Brett VanVeller

Carbonyl–carbonyl interactions between adjacent backbone amides have been implicated in the conformational stability of proteins. By combining experimental and computational approaches, we show that relevant amidic carbonyl groups associate through an n→π* donor–acceptor interaction with an energy of at least 0.27 kcal/mol. The n→π* interaction between two thioamides is 3-fold stronger than between two oxoamides due to increased overlap and reduced energy difference between the donor and acceptor orbitals. This result suggests that backbone thioamide incorporation could stabilize protein structures. Finally, we demonstrate that intimate carbonyl interactions are described more completely as donor–acceptor orbital interactions rather than dipole–dipole interactions.

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Structural Basis For Enzyme I Inhibition By Α-Ketoglutarate, Vincenzo Venditti, Rodolfo Ghirlando, G. Marius Clore Jan 2013

Structural Basis For Enzyme I Inhibition By Α-Ketoglutarate, Vincenzo Venditti, Rodolfo Ghirlando, G. Marius Clore

Vincenzo Venditti

Creating new bacterial strains in which carbon and nitrogen metabolism are uncoupled is potentially very useful for optimizing yields of microbial produced chemicals from renewable carbon sources. However, the mechanisms that balance carbon and nitrogen consumption in bacteria are poorly understood. Recently, α-ketoglutarate (αKG), the carbon substrate for ammonia assimilation, has been observed to inhibit Escherichia coli enzyme I (EI), the first component of the bacterial phosphotransferase system (PTS), thereby providing a direct biochemical link between central carbon and nitrogen metabolism. Here we investigate the EI-αKG interaction by NMR and enzymatic assays. We show that αKG binds with a KD …

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Structure, Dynamics And Biophysics Of The Cytoplasmic Protein–Protein Complexes Of The Bacterial Phosphoenolpyruvate: Sugar Phosphotransferase System, Vincenzo Venditti Jan 2013

Structure, Dynamics And Biophysics Of The Cytoplasmic Protein–Protein Complexes Of The Bacterial Phosphoenolpyruvate: Sugar Phosphotransferase System, Vincenzo Venditti

Vincenzo Venditti

The bacterial phosphotransferase system (PTS) couples phosphoryl transfer, via a series of bimolecular protein–protein interactions, to sugar transport across the membrane. The multitude of complexes in the PTS provides a paradigm for studying protein interactions, and for understanding how the same binding surface can specifically recognize a diverse array of targets. Fifteen years of work aimed at solving the solution structures of all soluble protein–protein complexes of the PTS has served as a test bed for developing NMR and integrated hybrid approaches to study larger complexes in solution and to probe transient, spectroscopically invisible states, including encounter complexes. We review …

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Abraham Model Correlations For Predicting Gas-To-Liquid Partition Coefficients And Activity Coefficients Of Organic Solutes Dissolved In 1-(2-Methoxyethyl)-1- Methylpyrrolidinium Tris(Pentafluoroethyl)Trifluorophosphate, Rui Jiang, Jared L. Anderson, Timothy W. Stephens, William E. Acree Jr., Micael H. Abraham Jan 2013

Abraham Model Correlations For Predicting Gas-To-Liquid Partition Coefficients And Activity Coefficients Of Organic Solutes Dissolved In 1-(2-Methoxyethyl)-1- Methylpyrrolidinium Tris(Pentafluoroethyl)Trifluorophosphate, Rui Jiang, Jared L. Anderson, Timothy W. Stephens, William E. Acree Jr., Micael H. Abraham

Jared L. Anderson

Chromatographic retention factors were measured for 45 different organic solutes of varying polarity and hydrogen-bonding capability on an anhydrous 1-(2-methoxyethyl)-1-methylpyrrolidinium tris(pentafluoroethyl)trifluorophosphate, ([MeoeMPyrr]+ [FAP]– ), stationary phase at both 323 K and 353 K. The experimental retention factor data were combined with recently published thermodynamic data for solutes dissolved in ([MeoeMPyrr]+ [FAP]– ) to give the corresponding gas-to-liquid partition coefficients (log K). The water-to-anhydrous ([MeoeMPyrr]+ [FAP]– ) partition coefficients (log P) were also calculated using published gas-to-water partition coefficient data for the solutes studied. The derived partition coefficients were analyzed in accordance with the Abraham model. The Abraham model expressions that …

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New Generation Of Ensemble-Decision Aliquot Ranking Based On Simplified Microfluidic Components For Large-Capacity Trapping Of Circulating Tumor Cells, Mengxia Zhao, Wyatt C. Nelson, Bingchuan Wei, Perry G. Schiro, Bejan M. Hakimi, Eleanor S. Johnson, Robbyn K. Anand, Grace S. Gyurkey, Lisa M. White, Samuel H. Whiting, Andrew L. Coveler, Daniel T. Chiu Jan 2013

New Generation Of Ensemble-Decision Aliquot Ranking Based On Simplified Microfluidic Components For Large-Capacity Trapping Of Circulating Tumor Cells, Mengxia Zhao, Wyatt C. Nelson, Bingchuan Wei, Perry G. Schiro, Bejan M. Hakimi, Eleanor S. Johnson, Robbyn K. Anand, Grace S. Gyurkey, Lisa M. White, Samuel H. Whiting, Andrew L. Coveler, Daniel T. Chiu

Robbyn Anand

Ensemble-decision aliquot ranking (eDAR) is a sensitive and high-throughput method to analyze circulating tumor cells (CTCs) from peripheral blood. Here, we report the next generation of eDAR, where we designed and optimized a new hydrodynamic switching scheme for the active sorting step in eDAR, which provided fast cell sorting with an improved reproducibility and stability. The microfluidic chip was also simplified by incorporating a functional area for subsequent purification using microslits fabricated by standard lithography method. Using the reported second generation of eDAR, we were able to analyze 1 mL of whole-blood samples in 12.5 min, with a 95% recovery …

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Ultraviolet Photoinitiated On-Fiber Copolymerization Of Ionic Liquid Sorbent Coatings For Headspace And Direct Immersion Solid-Phase Microextraction, Tien D. Ho, Honglian Yu, William T.S. Cole, Jared L. Anderson Sep 2012

Ultraviolet Photoinitiated On-Fiber Copolymerization Of Ionic Liquid Sorbent Coatings For Headspace And Direct Immersion Solid-Phase Microextraction, Tien D. Ho, Honglian Yu, William T.S. Cole, Jared L. Anderson

Jared L. Anderson

A high-throughput method for the production of solid-phase microextraction (SPME) sorbent coatings via ultraviolet (UV) photoinitiated copolymerization of ionic liquid (IL) monomers on a fused silica support is described. The copolymerization of monocationic and dicationic IL cross-linkers was performed “on-fiber” using UV initiated free radical polymerization. Mixtures composed of various amounts of the IL cross-linker, UV initiator (DAROCUR 1173), and IL monomer were dip-coated onto an etched and derivatized fused silica support and placed in a high-capacity UV reactor. The method requires no organic dispersive solvent and is much more rapid compared to traditional methods in which polymeric ionic liquid …

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A Simple Two-Dimensional Model System To Study Electrostatic-Self-Assembly, Rebecca Cademartiri Aug 2012

A Simple Two-Dimensional Model System To Study Electrostatic-Self-Assembly, Rebecca Cademartiri

Rebecca Cademartiri

This paper surveys the variables controlling the lattice structure and charge in macroscopic Coulombic crystals made from electrically charged, millimeter-sized polymer objects (spheres, cubes, and cylinders). Mechanical agitation of these objects inside planar, bounded containers caused them to charge electrically through contact electrification, and to self-assemble. The processes of electrification and self-assembly, and the characteristics of the assemblies, depended on the type of motion used for agitation, on the type of materials used for the objects and the dish, on the size and shape of the objects and the dish, and on the number of objects. Each of the three …

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Replacing −Ch2ch2– With −Conh– Does Not Significantly Change Rates Of Charge Transport Through Agts-Sam//Ga2o3/Egain Junctions, Martin M. Thuo, William F. Reus, Felice C. Simeone, Choongik Kim, Michael D. Schulz, Hyo Jae Yoon, George M. Whitesides Jun 2012

Replacing −Ch2ch2– With −Conh– Does Not Significantly Change Rates Of Charge Transport Through Agts-Sam//Ga2o3/Egain Junctions, Martin M. Thuo, William F. Reus, Felice C. Simeone, Choongik Kim, Michael D. Schulz, Hyo Jae Yoon, George M. Whitesides

Martin M. Thuo

This paper describes physical-organic studies of charge transport by tunneling through self-assembled monolayers (SAMs), based on systematic variations of the structure of the molecules constituting the SAM. Replacing a −CH2CH2– group with a −CONH– group changes the dipole moment and polarizability of a portion of the molecule and has, in principle, the potential to change the rate of charge transport through the SAM. In practice, this substitution produces no significant change in the rate of charge transport across junctions of the structure AgTS-S(CH2)mX(CH2)nH//Ga2O3/EGaIn (TS = template stripped, X = −CH2CH2– or −CONH–, and EGaIn = eutectic alloy of gallium and …

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The Sam, Not The Electrodes, Dominates Charge Transport In Metal-Monolayer//Ga2o3/Gallium–Indium Eutectic Junctions, William F. Reus, Martin M. Thuo, Nathan D. Shapiro, Christian A. Nijhuis, George M. Whitesides May 2012

The Sam, Not The Electrodes, Dominates Charge Transport In Metal-Monolayer//Ga2o3/Gallium–Indium Eutectic Junctions, William F. Reus, Martin M. Thuo, Nathan D. Shapiro, Christian A. Nijhuis, George M. Whitesides

Martin M. Thuo

The liquid–metal eutectic of gallium and indium (EGaIn) is a useful electrode for making soft electrical contacts to self-assembled monolayers (SAMs). This electrode has, however, one feature whose effect on charge transport has been incompletely understood: a thin (approximately 0.7 nm) film—consisting primarily of Ga2O3—that covers its surface when in contact with air. SAMs that rectify current have been measured using this electrode in AgTS-SAM//Ga2O3/EGaIn (where AgTS = template-stripped Ag surface) junctions. This paper organizes evidence, both published and unpublished, showing that the molecular structure of the SAM (specifically, the presence of an accessible molecular orbital asymmetrically located within the …

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Polycyclic Aromatic Triptycenes: Oxygen Substitution Cyclization Strategies, Brett Vanveller, Derek J. Schipper, Timothy M. Swager Apr 2012

Polycyclic Aromatic Triptycenes: Oxygen Substitution Cyclization Strategies, Brett Vanveller, Derek J. Schipper, Timothy M. Swager

Brett VanVeller

The cyclization and planarization of polycyclic aromatic hydrocarbons with concomitant oxygen substitution was achieved through acid catalyzed transetherification and oxygen-radical reactions. The triptycene scaffold enforces proximity of the alcohol and arene reacting partners and confers significant rigidity to the resulting π-system, expanding the tool set of iptycenes for materials applications.

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Measuring Markers Of Liver Function Using A Micropatterned Paper Device Designed For Blood From A Fingerstick, Sarah J. Vella, Patrick Beattie, Rebecca Cademartiri, Anna Laromaine, Andres W. Martinez, Scott T. Phillips, Katherine A. Mirica, George M. Whitesides Mar 2012

Measuring Markers Of Liver Function Using A Micropatterned Paper Device Designed For Blood From A Fingerstick, Sarah J. Vella, Patrick Beattie, Rebecca Cademartiri, Anna Laromaine, Andres W. Martinez, Scott T. Phillips, Katherine A. Mirica, George M. Whitesides

Rebecca Cademartiri

This paper describes a paper-based microfluidic device that measures two enzymatic markers of liver function (alkaline phosphatase, ALP, and aspartate aminotransferase, AST) and total serum protein. A device consists of four components: (i) a top plastic sheet, (ii) a filter membrane, (iii) a patterned paper chip containing the reagents necessary for analysis, and (iv) a bottom plastic sheet. The device performs both the sample preparation (separating blood plasma from erythrocytes) and the assays; it also enables both qualitative and quantitative analysis of data. The data obtained from the paper-microfluidic devices show standard deviations in calibration runs and “spiked” standards that …

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Statistical Tools For Analyzing Measurements Of Charge Transport, William F. Reus, Christian A. Nijhuis, Jabulani R. Barber, Martin M. Thuo, Simon Tricard, George M. Whitesides Feb 2012

Statistical Tools For Analyzing Measurements Of Charge Transport, William F. Reus, Christian A. Nijhuis, Jabulani R. Barber, Martin M. Thuo, Simon Tricard, George M. Whitesides

Martin M. Thuo

This paper applies statistical methods to analyze the large, noisy data sets produced in measurements of tunneling current density (J) through self-assembled monolayers (SAMs) in large-area junctions. It describes and compares the accuracy and precision of procedures for summarizing data for individual SAMs, for comparing two or more SAMs, and for determining the parameters of the Simmons model (β and J0). For data that contain significant numbers of outliers (i.e., most measurements of charge transport), commonly used statistical techniques—e.g., summarizing data with arithmetic mean and standard deviation and fitting data using a linear, least-squares algorithm—are prone to large errors. The …

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Electrical Resistance Of Agts–S(Ch2)N−1ch3//Ga2o3/Egain Tunneling Junctions, Ludovico Cademartiri, Martin M. Thuo, Christian A. Nijhuis, William F. Reus, Simon Tricard, Jubulani R. Barber, Rana N.S. Sodhi, Peter Brodersen, Choongik Kim, Ryan C. Chiechi, George M. Whitesides Feb 2012

Electrical Resistance Of Agts–S(Ch2)N−1ch3//Ga2o3/Egain Tunneling Junctions, Ludovico Cademartiri, Martin M. Thuo, Christian A. Nijhuis, William F. Reus, Simon Tricard, Jubulani R. Barber, Rana N.S. Sodhi, Peter Brodersen, Choongik Kim, Ryan C. Chiechi, George M. Whitesides

Martin M. Thuo

Tunneling junctions having the structure AgTS–S(CH2)n−1CH3//Ga2O3/EGaIn allow physical–organic studies of charge transport across self-assembled monolayers (SAMs). In ambient conditions, the surface of the liquid metal electrode (EGaIn, 75.5 wt % Ga, 24.5 wt % In, mp 15.7 °C) oxidizes and adsorbs―like other high-energy surfaces―adventitious contaminants. The interface between the EGaIn and the SAM thus includes a film of metal oxide, and probably also organic material adsorbed on this film; this interface will influence the properties and operation of the junctions. A combination of structural, chemical, and electrical characterizations leads to four conclusions about AgTS–S(CH2)n−1CH3//Ga2O3/EGaIn junctions. (i) The oxide is ∼0.7 …

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Bacterial Isolation By Lectin-Modified Microengines, Susana Campuzano, Jahir Orozco, Daniel Kagan, Maria Guix, Wei Gao, Sirilak Sattayasamitsathit, Jonathan C. Claussen, Arben Merkoci, Joseph Wang Jan 2012

Bacterial Isolation By Lectin-Modified Microengines, Susana Campuzano, Jahir Orozco, Daniel Kagan, Maria Guix, Wei Gao, Sirilak Sattayasamitsathit, Jonathan C. Claussen, Arben Merkoci, Joseph Wang

Jonathan C. Claussen

New template-based self-propelled gold/nickel/polyaniline/platinum (Au/Ni/PANI/Pt) microtubular engines, functionalized with the Concanavalin A (ConA) lectin bioreceptor, are shown to be extremely useful for the rapid, real-time isolation of Escherichia coli (E. coli) bacteria from fuel-enhanced environmental, food, and clinical samples. These multifunctional microtube engines combine the selective capture of E. coli with the uptake of polymeric drug-carrier particles to provide an attractive motion-based theranostics strategy. Triggered release of the captured bacteria is demonstrated by movement through a low-pH glycine-based dissociation solution. The smaller size of the new polymer-metal microengines offers convenient, direct, and label-free optical visualization of the captured bacteria and …

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