Davies electron-nuclear double resonance revisited: Enhanced sensitivity and nuclear spin relaxation
Journal of Chemical Physics 124:23 (2006)
Abstract:
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 T1n, and can be severely reduced for long T1n. 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 T1n can be exploited to measure nuclear relaxation, as we demonstrate for phosphorous donors in silicon and for endohedral fullerenes N@ C60 in C S2. © 2006 American Institute of Physics.Synthesis and reactivity of N@C60 O
Physical Chemistry Chemical Physics 8:17 (2006) 2083-2088
Abstract:
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°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. © the Owner Societies 2006.Coherence of spin qubits in silicon
Journal of Physics Condensed Matter 18:21 (2006)
Abstract:
Given the effectiveness of semiconductor devices for classical computation one is naturally led to consider semiconductor systems for solid state quantum information processing. Semiconductors are particularly suitable where local control of electric fields and charge transport are required. Conventional semiconductor electronics is built upon these capabilities and has demonstrated scaling to large complicated arrays of interconnected devices. However, the requirements for a quantum computer are very different from those for classical computation, and it is not immediately obvious how best to build one in a semiconductor. One possible approach is to use spins as qubits: of nuclei, of electrons, or both in combination. Long qubit coherence times are a prerequisite for quantum computing, and in this paper we will discuss measurements of spin coherence in silicon. The results are encouraging - both electrons bound to donors and the donor nuclei exhibit low decoherence under the right circumstances. Doped silicon thus appears to pass the first test on the road to a quantum computer. © IOP 2006 Publishing Ltd.Towards a fullerene-based quantum computer
Journal of Physics Condensed Matter 18:21 (2006)
Abstract:
Molecular structures appear to be natural candidates for a quantum technology: individual atoms can support quantum superpositions for long periods, and such atoms can in principle be embedded in a permanent molecular scaffolding to form an array. This would be true nanotechnology, with dimensions of order of a nanometre. However, the challenges of realizing such a vision are immense. One must identify a suitable elementary unit and demonstrate its merits for qubit storage and manipulation, including input/output. These units must then be formed into large arrays corresponding to an functional quantum architecture, including a mechanism for gate operations. Here we report our efforts, both experimental and theoretical, to create such a technology based on endohedral fullerenes or 'buckyballs'. We describe our successes with respect to these criteria, along with the obstacles we are currently facing and the questions that remain to be addressed. © 2006 IOP Publishing Ltd.Synthesis and reactivity of N@C60O.
Phys Chem Chem Phys 8:17 (2006) 2083-2088