Simultaneous electrostatic trapping of merged cation & anion beams.

Simultaneous trapping of merged cation and anion beams in the hybrid electrostatic ion beam trap (HEIBT) opens new opportunities for the study of the interactions of isolated atomic molecular or cluster ions with oppositely charged ionic species. Application of the trapped merged beams requires a detailed understanding of the trapping dynamics and the effect of the Coulombic attractive and repulsive forces between the ions on their motion in the trap. The simultaneous trapping regime is explored experimentally for SF anion and SF cation beams and compared to realistic ion trajectory simulations.

Single-photon Coulomb explosion of methanol using broad bandwidth ultrafast EUV pulses.

Single-photon Coulomb explosion of methanol is instigated using the broad bandwidth pulse achieved through high-order harmonics generation. Using 3D coincidence fragment imaging of one molecule at a time, the kinetic energy release (KER) and angular distributions of the products are measured in different Coulomb explosion (CE) channels. Two-body CE channels breaking either the C-O or the C-H bonds are described as well as a proton migration channel forming HO, which is shown to exhibit higher KER.

Nonresonant Raman Effects on Femtosecond Pump-Probe with Chirped White Light: Challenges and Opportunities.

Impulsive Raman excitation in neat organic liquids far from resonance is followed using chirped broad-band supercontinuum probe pulses. Spectral modulations due to impulsively induced coherent vibrations vary in intensity 10-fold as a function of the probe's linear chirp. Simulations clarify why the vibrational signature is maximized for a group delay dispersion (GDD) in reduced units of ν = 0.

Rewriting the Story of Excimer Formation in Liquid Benzene.

Formation of benzene excimer following UV excitation of the neat liquid is monitored with femtosecond spectroscopy. A prompt rise component in excimer transient absorption, which contradicts the classical scenario of gradual reorientation and pairing of the excited monomers, is observed. Three-pulse experiments in which the population of evolving excimers is depleted by a secondary dump pulse demonstrate that the excimer absorption band is polarized along the interfragment axis.

Self-assembly of luminescent Ag nanocluster-functionalized nanowires.

Two different methods to self-assemble red- or yellow-luminescent nucleic acids-stabilized Ag nanoclusters (NCs) nanowires are presented. By one method, the autonomous hybridization-polymerization process between two nucleic acids leads to polymer chains consisting of sequence-specific loops for the stabilization of the red- or yellow-emitting Ag NCs. By the other method, the nucleic acid-triggered hybridization chain reaction (HCR) involving the cross-opening of two functional hairpins leads to sequence-specific DNA loops and a nucleic acid scaffold that stabilize the respective red- or yellow-emitting Ag NCs.

DNA computing circuits using libraries of DNAzyme subunits.

Biological systems that are capable of performing computational operations could be of use in bioengineering and nanomedicine, and DNA and other biomolecules have already been used as active components in biocomputational circuits. There have also been demonstrations of DNA/RNA-enzyme-based automatons, logic control of gene expression, and RNA systems for processing of intracellular information. However, for biocomputational circuits to be useful for applications it will be necessary to develop a library of computing elements, to demonstrate the modular coupling of these elements, and to demonstrate that this approach is scalable.

Logic gates and antisense DNA devices operating on a translator nucleic Acid scaffold.

A series of logic gates, "AND", "OR", and "XOR", are designed using a DNA scaffold that includes four "footholds" on which the logic operations are activated. Two of the footholds represent input-recognition strands, and these are blocked by complementary nucleic acids, whereas the other two footholds are blocked by nucleic acids that include the horseradish peroxidase (HRP)-mimicking DNAzyme sequence. The logic gates are activated by either nucleic acid inputs that hybridize to the respective "footholds", or by low-molecular-weight inputs (adenosine monophosphate or cocaine) that yield the respective aptamer-substrate complexes.

Ultrasensitive surface plasmon resonance detection of trinitrotoluene by a bis-aniline-cross-linked Au nanoparticles composite.

A bis-aniline-cross-linked Au nanoparticles (NPs) composite is electropolymerized on Au surfaces. The association of trinitrotoluene, TNT, to the bis-aniline bridging units via pi-donor-acceptor interactions allows the amplified detection of TNT by following the surface plasmon resonance (SPR) reflectance changes as a result of the coupling between the localized plasmon of the AuNPs and the surface plasmon wave associated with the gold surface. The detection limit for analyzing TNT by this method is approximately 10 pM.

Enzyme cascades activated on topologically programmed DNA scaffolds.

The ability of DNA to self-assemble into one-, two- and three-dimensional nanostructures, combined with the precision that is now possible when positioning nanoparticles or proteins on DNA scaffolds, provide a promising approach for the self-organization of composite nanostructures. Predicting and controlling the functions that emerge in self-organized biomolecular nanostructures is a major challenge in systems biology, and although a number of innovative examples have been reported, the emergent properties of systems in which enzymes are coupled together have not been fully explored. Here, we report the self-assembly of a DNA scaffold made of DNA strips that include 'hinges' to which biomolecules can be tethered.

Characterization of nanostructured surfaces generated by reconstitution of the porin MspA from Mycobacterium smegmatis.

Nanostructures with long-term stability at the surface of gold electrodes are generated by reconstituting the porin MspA from Mycobacterium smegmatis into a specially designed monolayer of long-chain lipid surfactant on gold. Tailored surface coverage of gold electrodes with long-chain surfactants is achieved by electrochemically assisted deposition of organic thiosulfates (Bunte salts). The subsequent reconstitution of the octameric-pore MspA is guided by its extraordinary self-assembling properties.

Concatenated logic gates using four coupled biocatalysts operating in series.

The assembly of three concatenated enzyme-based logic gates consisting of OR, AND, XOR is described. Four biocatalysts, acetylcholine esterase, choline oxidase, microperoxidase-11, and the NAD+-dependent glucose dehydrogenase, are used to assemble the gates. Four inputs that include acetylcholine, butyrylcholine, O2, and glucose are used to drive the concatenated-gates system.

Logic gates and elementary computing by enzymes.

Different selected enzymes, glucose oxidase (GOx), catalase (Cat), glucose dehydrogenase (GDH), horseradish peroxidase (HRP), and formaldehyde dehydrogenase (FDH), are used alone or coupled to construct eight different logic gates. The added substrates for the respective enzymes, glucose and H(2)O(2), act as the gate inputs, while the biocatalytically generated gluconic acid or NADH are the output signals that follow the operation of the gates. Different enzyme-based gates are XOR, INHIBIT A, INHIBIT B, AND, OR, NOR, Identity and Inverter gates.

An electrochemical/photochemical information processing system using a monolayer-functionalized electrode.

An electroactive and photoisomerizable monolayer associated with a Au electrode acts as a Write-Read-Erase information processing system and as a flip-flop Set/Reset memory element.

Two coupled enzymes perform in parallel the 'AND' and 'InhibAND' logic gate operations.

The coupled activation of two enzymes: glucose dehydrogenase (GDH) and horseradish peroxidase (HRP), is used to construct the parallel-operating AND and InhibAND logic gates. The added substrates for the respective enzymes, glucose and H(2)O(2), act as the gate inputs, while the biocatalytically generated NADH and gluconic acid provide the output signals that follow the operations of the gates. The two gates are generated in the same vial, thus allowing the logic operations to take place in parallel, and the simultaneous readout of the functions of the gates.

Magneto-switchable single-electron charging of Au-nanoparticles using hydrophobic magnetic nanoparticles.

Reversible magneto-switchable quantum charging of a Au nanoparticle array associated with a Au electrode is observed in the presence of hydrophobic magnetic nanoparticles attracted to the functionalized electrode surface.

Endonuclease-based logic gates and sensors using magnetic force-amplified readout of DNA scission on cantilevers.

The endonuclease scission of magnetic particles functionalized with sequence-specific DNAs, which are associated on cantilevers, is followed by the magnetic force-amplified readout of the reactions by the nano-mechanical deflection/retraction of the cantilevers. The systems are employed to develop AND or OR logic gates and to detect single base mismatch specificity of the endonucleases. The two endonucleases EcoRI (E(A)) and AscI (E(B)) are used as inputs.

Magnetomechanical detection of the specific activities of endonucleases by cantilevers.

Thiolated nucleic acids 1 or 2 are immobilized on Au-coated cantilevers and hybridized with the complementary nucleic acids 1a or 2a associated with magnetic particles. The duplexes 1/1a or 2/2a include specific sequences for the scission by Apa I or Mse I, respectively. The cantilevers positioned in a flow cell are subjected to an external magnetic field, leading to the deflection of the cantilevers.

Magnetic field effects on bioelectrocatalytic reactions of surface-confined enzyme systems: enhanced performance of biofuel cells.

The effect of a constant magnetic field on bioelectrocatalytic transformations of three different enzyme assemblies linked to electrodes is examined and correlated with a theoretical magnetohydrodynamic model. The systems consist of surface-reconstituted glucose oxidase (GOx), an integrated lactate dehydrogenase/nicotinamide/pyrroloquinoline quinone assembly (LDH/NAD+ -PQQ), and a cytochrome c/cytochrome oxidase system (Cyt c/COx) linked to the electrodes. Pronounced effects of a constant magnetic field applied parallel to the electrode surface are observed for the bioelectrocatalyzed oxidation of glucose and lactate by the GOx-electrode and LDH/NAD+ -PQQ-electrode, respectively.

Magnetic field effects on cytochrome c-mediated bioelectrocatalytic transformations.

Constant magnetic fields affect many biological transformations, but we lack mechanistic understanding of the processes. The magnetohydrodynamic effect may account for the enhancement of bioelectrocatalytic transformations at interfaces. This is exemplified by the bioelectrocatalyzed cytochrome c-mediated reduction of oxygen and oxidation of lactate in the presence of cytochrome oxidase and lactate dehydrogenase, respectively.

Enzyme-catalyzed bio-pumping of electrons into au-nanoparticles: a surface plasmon resonance and electrochemical study.

The enzyme glucose oxidase (GOx) is reconstituted on a flavin adenin dinucleotide (FAD, 1) cofactor-functionalized Au-nanoparticle (Au-NP), 1.4 nm, and the GOx/Au-NP hybrid is linked to a bulk Au-electrode by a short dithiol, 1,4-benzenedithiol (2), or a long dithiol, 1,9-nonanedithiol (3), monolayer. The reconstituted GOx/Au-NP hybrid system exhibits electrical communication between the enzyme redox cofactor and the Au-NP core.

Magneto-mechanical detection of nucleic acids and telomerase activity in cancer cells.

The ultra-sensitive magneto-mechanical detection of DNA, single-base-mismatches in nucleic acids, and the assay of telomerase activity are accomplished by monitoring the magnetically induced deflection of a cantilever functionalized with magnetic beads associated with the biosensing interface. The analyzed M13phi DNA hybridized with the nucleic acid-functionalized magnetic beads is replicated in the presence of dNTPs that include biotin-labeled dUTP. The resulting beads are attached to an avidin-coated cantilever, and the modified cantilever is deflected by an external magnetic field.

Au nanoparticle-enhanced surface plasmon resonance sensing of biocatalytic transformations.

N-(3-Aminopropyl)-N'-methyl-4,4'-bipyridinium is coupled to tiopronin-capped Au nanoparticles (diameter ca. 2 nm) to yield methyl(aminopropyl)viologen-functionalized Au nanoparticles (MPAV(2+)-Au nanoparticles). In situ electrochemical surface plasmon resonance (SPR) measurements are used to follow the electrochemical deposition of the bipyridinium radical cation modified Au nanoparticles on an Au-coated glass surface and the reoxidation and dissolution of the bipyridinium radical cation film.

Probing photoelectrochemical processes in Au-CdS nanoparticle arrays by surface plasmon resonance: application for the detection of acetylcholine esterase inhibitors.

The photoelectrochemical charging of Au-nanoparticles (NP) in a Au-nanoparticle/CdS-nanoparticle array assembled on a Au-coated glass surface is followed by means of surface plasmon resonance (SPR) spectroscopy upon continuous irradiation of the sample. The charging of the Au-NPs results in the enhanced coupling between the localized surface plasmon of the Au-NP and the surface plasmon of the bulk surface, leading to a shift in the plasmon angle. The charging effect of the Au-NPs is supported by concomitant electrochemical experiments in the dark.

Analysis of NAD(P)+/NAD(P)H cofactors by imprinted polymer membranes associated with ion-sensitive field-effect transistor devices and Au-quartz crystals.

Specific recognition sites for the NAD(P)+ and NAD(P)H cofactors are imprinted in a cross-linked acrylamide-acrylamidophenylboronic acid copolymer membrane. The imprinted membranes, associated with pH-sensitive field-effect transistors (ISFETs) or Au-quartz piezoelectric crystals, enable the potentiometric or microgravimetric analysis of the oxidized NAD(P)+ cofactors and the reduced NAD(P)H cofactors, respectively. The NAD+- and NADP+-imprinted membranes associated with the ISFET allow the analysis of NAD+ and NADP+ with sensitivities that correspond to 15.