Lee E. Harrell

Effect of electron mediators on current generation and fermentation in a microbial fuel cell

Effects of select electron mediators [9,10-anthraquinone-2,6-disulfonic acid disodium salt (AQDS), safranine O, resazurin, methylene blue, and humic acids] on metabolic end-products and current production from cellulose digestion by Clostridium cellulolyticum in microbial fuel cells (MFCs) were studied using capillary electrophoresis and traditional electrochemical techniques. Addition of the mediator resazurin greatly enhanced current production but did not appear to alter the examined fermentation end-products compared to MFCs with no mediator. Assays for lactate, acetate, and ethanol indicate that the presence of safranine O, methylene blue, and humic acids alters metabolite production in the MFC: safranine O decreased the examined metabolites, methylene blue increased lactate formation, and humic acids increased the examined metabolites. Mediator standard redox potentials (E0) reported in the literature do not coincide with redox potentials in MFCs due presumably to the electrolytic complexity of media that supports bacterial survival and growth. Current production in MFCs: (1) can be effected by the mediator redox potential while in the media, which may be significantly shifted from E0, and (2) depended on the ability of the mediator to access the bacterial electron source, which may be cytoplasmic. In addition, some electron mediators had significant effects on metabolic end-products and therefore the metabolism of the organism itself.

Scanned-probe detection of electron spin resonance from a nitroxide spin probe

We report an approach that extends the applicability of ultrasensitive force-gradient detection of magnetic resonance to samples with spin-lattice relaxation times (T 1) as short as a single cantilever period. To demonstrate the generality of the approach, which relies on detecting either cantilever frequency or phase, we used it to detect electron spin resonance from a T 1 = 1 ms nitroxide spin probe in a thin film at 4.2 K and 0.6 T. By using a custom-fabricated cantilever with a 4 μm-diameter nickel tip, we achieve a magnetic resonance sensitivity of 400 Bohr magnetons in a 1 Hz bandwidth. A theory is presented that quantitatively predicts both the lineshape and the magnitude of the observed cantilever frequency shift as a function of field and cantilever-sample separation. Good agreement was found between nitroxide T 1 s measured mechanically and inductively, indicating that the cantilever magnet is not an appreciable source of spin-lattice relaxation here. We suggest that the new approach has a number of advantages that make it well suited to push magnetic resonance detection and imaging of nitroxide spin labels in an individual macromolecule to single-spin sensitivity.

170 nm nuclear magnetic resonance imaging using magnetic resonance force microscopy.

We demonstrate one-dimensional nuclear magnetic resonance imaging of the semiconductor GaAs with 170 nm slice separation and resolve two regions of reduced nuclear spin polarization density separated by only 500 nm. This was achieved by force detection of the magnetic resonance, magnetic resonance force microscopy (MRFM), in combination with optical pumping to increase the nuclear spin polarization. Optical pumping of the GaAs created spin polarization up to 12 times larger than the thermal nuclear spin polarization at 5K and 4T. The experiment was sensitive to sample volumes of 50 microm(3) containing approximately 4 x 10(11)71 Ga/Hz. These results demonstrate the ability of force-detected magnetic resonance to apply magnetic resonance imaging to semiconductor devices and other nanostructures.

Detailed description of a compact cryogenic magnetic resonance force microscope

We describe the design and operation of a cryogenic magnetic resonance force microscope for detecting nuclear magnetic resonance. Instrument-critical details are enumerated, including fabrication of a positionable radio-frequency coil, detection of angstrom-level microcantilever oscillations using an optical fiber interferometer, design of a compact fiber/cantilever alignment system, temperature compensation of the fiber/cantilever gap, control of sample temperature, and vibration isolation. Additionally, experimental protocols and sample specific considerations such as spin relaxation times are addressed. 19F nuclear magnetic resonance data obtained from a Nd-doped CaF2 sample are presented.

Spin polarization contrast observed in GaAs by force-detected nuclear magnetic resonance

We applied the technique of force-detected nuclear magnetic resonance to observe 71Ga, 69Ga, and 75As in GaAs. The nuclear spin-lattice relaxation time is 21±5 min for 69Ga at ∼5 K and 4.6 T. We have exploited this long relaxation time to first create and then observe spatially varying nuclear spin polarization within the sample, demonstrating a form of contrast for magnetic resonance force microscopy. Such nuclear spin contrast could be used to indirectly image electron spin polarization in GaAs-based spintronic devices.

Batch-fabrication of cantilevered magnets on attonewton-sensitivity mechanical oscillators for scanned-probe nanoscale magnetic resonance imaging.

We have batch-fabricated cantilevers with ∼100 nm diameter nickel nanorod tips and force sensitivities of a few attonewtons at 4.2 K. The magnetic nanorods were engineered to overhang the leading edge of the cantilever, and consequently the cantilevers experience what we believe is the lowest surface noise ever achieved in a scanned probe experiment. Cantilever magnetometry indicated that the tips were well magnetized, with a ≤ 20 nm dead layer; the composition of the dead layer was studied by electron microscopy and electron energy loss spectroscopy. In what we believe is the first demonstration of scanned probe detection of electron-spin resonance from a batch-fabricated tip, the cantilevers were used to observe electron-spin resonance from nitroxide spin labels in a film via force-gradient-induced shifts in cantilever resonance frequency. The magnetic field dependence of the magnetic resonance signal suggests a nonuniform tip magnetization at an applied field near 0.6 T.

Evading surface and detector frequency noise in harmonic oscillator measurements of force gradients

We introduce and demonstrate a method of measuring small force gradients acting on a harmonic oscillator in which the force-gradient signal of interest is used to parametrically up-convert a forced oscillation below resonance into an amplitude signal at the oscillators resonance frequency. The approach, which we demonstrate in a mechanically detected electron spin resonance experiment, allows the force-gradient signal to evade detector frequency noise by converting a slowly modulated frequency signal into an amplitude signal.

Temperature measurement at the end of a cantilever using oxygen paramagnetism in solid air

We demonstrate temperature measurement of a sample attached to the end of a cantilever using cantilever magnetometry of solid air “contamination” of the sample surface. In experiments like our magnetic resonance force microscopy (MRFM), the sample is mounted at the end of a thin cantilever with small thermal conductance. Thus, the sample can be at a significantly different temperature than the bulk of the instrument. Using cantilever magnetometry of the oxygen paramagnetism in solid air provides the temperature of the sample, without any modifications to our MRFM apparatus.

Practical recipes for the model order reduction, dynamical simulation and compressive sampling of large-scale open quantum systems

Practical recipes are presented for simulating high-temperature and nonequilibrium quantum spin systems that are continuously measured and controlled. The notion of a spin system is broadly conceived, in order to encompass macroscopic test masses as the limiting case of large-j spins. The simulation technique has three stages: first the deliberate introduction of noise into the simulation, then the conversion of that noise into an equivalent continuous measurement and control process, and finally, projection of the trajectory onto state-space manifolds having reduced dimensionality and possessing a K?hler potential of multilinear algebraic form. These state-spaces can be regarded as ruled algebraic varieties upon which a projective quantum model order reduction (MOR) is performed. The Riemannian sectional curvature of ruled K?hlerian varieties is analyzed, and proved to be non-positive upon all sections that contain a rule. These manifolds are shown to contain Slater determinants as a special case and their identity with Grassmannian varieties is demonstrated. The resulting simulation formalism is used to construct a positive P-representation for the thermal density matrix. Single-spin detection by magnetic resonance force microscopy (MRFM) is simulated, and the data statistics are shown to be those of a random telegraph signal with additive white noise. Larger-scale spin-dust models are simulated, having no spatial symmetry and no spatial ordering; the high-fidelity projection of numerically computed quantum trajectories onto low dimensionality K?hler state-space manifolds is demonstrated. The reconstruction of quantum trajectories from sparse random projections is demonstrated, the onset of Donoho?Stodden breakdown at the Cand?s?Tao sparsity limit is observed, a deterministic construction for sampling matrices is given and methods for quantum state optimization by Dantzig selection are given.

Wavefunction collapse through backaction of counting weakly interacting photons

We apply the formalism of quantum measurement theory to the idealized measurement of the position of a particle with an optical interferometer, finding that the backaction of counting entangled photons systematically collapses the particle’s wavefunction toward a narrow Gaussian wavepacket at the location xest determined by the measurement without appeal to environmental decoherence or other spontaneous collapse mechanism. Further, the variance in the particle’s position, as calculated from the post-measurement wavefunction, agrees precisely with shot-noise limited uncertainty of the measuredxest. Both the identification of the absolute square of the particle’s initial wavefunction as the probability density for xest and the de Broglie hypothesis emerge as consequences of interpreting the intensity of the optical field as proportional to the probability of detecting a photon. Linear momentum information that is encoded in the particle’s initial wavefunction survives the measurement, and the pre-measurement expectation values are preserved in the ensemble average.