Biomedical subjects
Publications and source records attributed to Arzhang Ardavan.
We have produced the fullerene dimers C(120), C(120)O, and C(120)O(2) by a high-speed vibration milling technique. The thermal stability of C(120), C(120)O, and C(120)O(2) has been studied in the temperature range 150-350 degrees C for up to 4 h under vacuum. The bridging oxygen atoms were found to substantially increase the stability of the fullerene dimer molecules.
Over the past 50 years, electron-nuclear double resonance (ENDOR) has become a fairly ubiquitous spectroscopic technique, allowing the study of spin transitions for nuclei which are coupled to electron spins. However, the low spin number sensitivity of the technique continues to pose serious limitations. Here we demonstrate that signal intensity in a pulsed Davies ENDOR experiment depends strongly on the nuclear relaxation time T(1n), and can be severely reduced for long T(1n). We suggest a development of the original Davies ENDOR sequence that overcomes this limitation, thus offering dramatically enhanced signal intensity and spectral resolution. Finally, we observe that the sensitivity of the original Davies method to T(1n) can be exploited to measure nuclear relaxation, as we demonstrate for phosphorous donors in silicon and for endohedral fullerenes N@C(60) in CS(2).
We have introduced defects into clean samples of the organic superconductor kappa-(BEDT-TTF)(2)Cu(SCN)(2) in order to determine their effect on the temperature dependence of the interlayer conductivity and the critical temperature T(c). We find a violation of Matthiessen's rule that can be explained by a model of involving a defect-assisted interlayer channel which acts in parallel with the bandlike conductivity. We observe an unusual dependence of T(c) on residual resistivity, inconsistent with the generalized Abrikosov-Gor'kov theory for an order parameter with a single component, providing an important constraint on models of the superconductivity in this material.
The endohedral fullerene epoxide N@C60O was synthesised, isolated by High Performance Liquid Chromatography (HPLC), and characterised by Electron Spin Resonance (ESR). This nitrogen radical displays predominantly axial symmetry characteristics as expected for a monoadduct, evidenced by a zero-field splitting D parameter of 6.6 MHz and an E parameter of 0.5 MHz in powder at 77 K. Photo- and thermally-activated silencing of the nitrogen radical were observed, the latter showing the evolution of a new spin signal during heating at 100 degrees C. We suggest that loss of nitrogen spin is due to coupling with a radical formed by opening of the epoxide ring. This implies that the reaction of C60O with C60 in the solid state proceeds via a radical, rather than ionic, intermediate.
We examine the temperature dependence of the electron spin relaxation times of the molecules N@C60 and N@C70 (which comprise atomic nitrogen trapped within a carbon cage) in liquid CS2 solution. The results are inconsistent with the fluctuating zero-field splitting (ZFS) mechanism, which is commonly invoked to explain electron spin relaxation for S> or =1 spins in liquid solution, and is the mechanism postulated in the literature for these systems. Instead, we find an Arrhenius temperature dependence for N@C60 , indicating the spin relaxation is driven primarily by an Orbach process. For the asymmetric N@C70 molecule, which has a permanent ZFS, we resolve an additional relaxation mechanism caused by the rapid reorientation of its ZFS. We also report the longest coherence time (T2) ever observed for a molecular electron spin, being 0.25 ms at 170 K.
Systematic errors in spin rotation operations using simple rf pulses place severe limitations on the usefulness of the pulsed magnetic resonance methods in quantum computing applications. In particular, the fidelity of quantum logic operations performed on electron spin qubits falls well below the threshold for the application of quantum algorithms. Using three independent techniques, we demonstrate the use of composite pulses to improve this fidelity by several orders of magnitude. The observed high-fidelity operations are limited by pulse phase errors, but nevertheless fall within the limits required for the application of quantum error correction.
Electron spin echo envelope modulation (ESEEM) has been observed for the first time from a coupled heterospin pair of electron and nucleus in liquid solution. Previously, modulation effects in spin-echo experiments have only been described in liquid solutions for a coupled pair of homonuclear spins in nuclear magnetic resonance or a pair of resonant electron spins in electron paramagnetic resonance. We observe low-frequency ESEEM (26 and 52 kHz) due to a new mechanism present for any electron spin with S > 12 that is hyperfine coupled to a nuclear spin. In our case these are electron spin (S = 32) and nuclear spin (I = 1) in the endohedral fullerene N@C(60). The modulation is shown to arise from second-order effects in the isotropic hyperfine coupling of an electron and (14)N nucleus.
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We report the application of SWNTs as templates for forming covalent polymeric chains from C(60)O reacting inside SWNTs; the resulting peapod polymer topology is different from the bulk polymer in that it is linear and unbranched.
We have assembled molecular arrays of C60 inside double-walled carbon nanotubes (DWNTs) with internal diameters of 11-26 A and directly observed the existence of different crystalline phases of C60 previously predicted theoretically. The structure of the encapsulated C60 crystal is defined by the internal diameter of the DWNT, as the molecules adjust their packing arrangement in order to maximize van der Waals interactions. We have also shown that fullerenes in C(60)@DWNT interact with the outer layer of DWNTs, as demonstrated by the efficient filling of DWNTs with internal diameters of less than 12 A.
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We present a theoretical study of the emission from a superluminal polarization current whose distribution pattern rotates (with an angular frequency omega) and oscillates (with a frequency Omega) at the same time and that comprises both poloidal and toroidal components. This type of polarization current is found in recent practical machines designed to investigate superluminal emission. We find that the superluminal motion of the distribution pattern of the emitting current generates localized electromagnetic waves that do not decay spherically, i.e., that do not have an intensity diminishing as RP(-2) with the distance RP from their source. The nonspherical decay of the focused wave packets that are emitted by the polarization currents does not contravene conservation of energy: The constructive interference of the constituent waves of such propagating caustics takes place within different solid angles on spheres of different radii (RP) centered on the source. For a polarization current whose longitudinal distribution (over an azimuthal interval of length 2pi) consists of m cycles of a sinusoidal wave train, the nonspherically decaying part of the emitted radiation contains the frequencies Omega +/- momega; i.e., it contains only the frequencies involved in the creation and implementation of the source. This is in contrast to recent studies of the spherically decaying emission, which was shown to contain much higher frequencies. The polarization of the emitted radiation is found to be linear for most configurations of the source.
Exohedrally functionalised fullerenes have been inserted in single-walled carbon nanotubes (SWNTs) with the aid of supercritical carbon dioxide to form peapods; C(61)(COOEt)(2) are encapsulated in SWNTs in high yield, whereas C(61)(COOH)(2) aggregate via hydrogen bonding to form a supramolecular complex, which sterically hinders encapsulation and causes it to adhere to the exterior surface of the SWNTs.
We investigate the spectral features of the emission from a superluminal polarization current whose distribution pattern rotates (with an angular frequency omega) and oscillates (with a frequency omega > omega differing from an integral multiple of omega) at the same time. This type of polarization current is found in recent practical machines designed to investigate superluminal emission. Although all of the processes involved are linear, we find that the broadband emission contains frequencies that are higher than omega by a factor of the order of (omega/omega)2. This generation of frequencies not required for the creation of the source stems from mathematically rigorous consequences of the familiar classical expression for the retarded potential. The results suggest practical applications for superluminal polarization currents as broadband radio-frequency and infrared sources.