High Fidelity Single Qubit Operations using Pulsed EPR

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.Comment: 4 pages, 3 figures To appear in Phys. Rev. Let

Switchable ErSc2N rotor within a C80 fullerene cage: An EPR and photoluminescence excitation study

Systems exhibiting both spin and orbital degrees of freedom, of which Er3+ is one, can offer mechanisms for manipulating and measuring spin states via optical excitations. Motivated by the possibility of observing photoluminescence and electron paramagnetic resonance from the same species located within a fullerene molecule, we initiated an EPR study of Er3+ in ErSc2N@C80. Two orientations of the ErSc2N rotor within the C80 fullerene are observed in EPR, consistent with earlier studies using photoluminescence excitation (PLE) spectroscopy. For some crystal field orientations, electron spin relaxation is driven by an Orbach process via the first excited electronic state of the 4I_15/2 multiplet. We observe a change in the relative populations of the two ErSc2N configurations upon the application of 532 nm illuminations, and are thus able to switch the majority cage symmetry. This photoisomerisation, observable by both EPR and PLE, is metastable, lasting many hours at 20 K.Comment: 4 pages, 4 figure

Measuring errors in single qubit rotations by pulsed electron paramagnetic resonance

The ability to measure and reduce systematic errors in single-qubit logic gates is crucial when evaluating quantum computing implementations. We describe pulsed electron paramagnetic resonance (EPR) sequences that can be used to measure precisely even small systematic errors in rotations of electron-spin-based qubits. Using these sequences we obtain values for errors in rotation angle and axis for single-qubit rotations using a commercial EPR spectrometer. We conclude that errors in qubit operations by pulsed EPR are not limiting factors in the implementation of electron-spin based quantum computers

Environmental effects on electron spin relaxation in N@C60

We examine environmental effects of surrounding nuclear spins on the electron spin relaxation of the N@C60 molecule (which consists of a nitrogen atom at the centre of a fullerene cage). Using dilute solutions of N@C60 in regular and deuterated toluene, we observe and model the effect of translational diffusion of nuclear spins of the solvent molecules on the N@C60 electron spin relaxation times. We also study spin relaxation in frozen solutions of N@C60 in CS2, to which small quantities of a glassing agent, S2Cl2 are added. At low temperatures, spin relaxation is caused by spectral diffusion of surrounding nuclear 35Cl and 37Cl spins in the S2Cl2, but nevertheless, at 20 K, T2 times as long as 0.23 ms are observed.Comment: 7 pages, 6 figure

Immature HIV-1 assembles from Gag dimers leaving partial hexamers at lattice edges as potential substrates for proteolytic maturation

The CA (capsid) domain of immature HIV-1 Gag and the adjacent spacer peptide 1 (SP1) play a key role in viral assembly by forming a lattice of CA hexamers, which adapts to viral envelope curvature by incorporating small lattice defects and a large gap at the site of budding. This lattice is stabilized by intrahexameric and interhexameric CA-CA interactions, which are important in regulating viral assembly and maturation. We applied subtomogram averaging and classification to determine the oligomerization state of CA at lattice edges and found that CA forms partial hexamers. These structures reveal the network of interactions formed by CA-SP1 at the lattice edge. We also performed atomistic molecular dynamics simulations of CA-CA interactions stabilizing the immature lattice and partial CA-SP1 helical bundles. Free energy calculations reveal increased propensity for helix-to-coil transitions in partial hexamers compared to complete six-helix bundles. Taken together, these results suggest that the CA dimer is the basic unit of lattice assembly, partial hexamers exist at lattice edges, these are in a helix-coil dynamic equilibrium, and partial helical bundles are more likely to unfold, representing potential sites for HIV-1 maturation initiation

Electron spin coherence in metallofullerenes: Y, Sc and La@C82

Endohedral fullerenes encapsulating a spin-active atom or ion within a carbon cage offer a route to self-assembled arrays such as spin chains. In the case of metallofullerenes the charge transfer between the atom and the fullerene cage has been thought to limit the electron spin phase coherence time (T2) to the order of a few microseconds. We study electron spin relaxation in several species of metallofullerene as a function of temperature and solvent environment, yielding a maximum T2 in deuterated o-terphenyl greater than 200 microseconds for Y, Sc and La@C82. The mechanisms governing relaxation (T1, T2) arise from metal-cage vibrational modes, spin-orbit coupling and the nuclear spin environment. The T2 times are over 2 orders of magnitude longer than previously reported and consequently make metallofullerenes of interest in areas such as spin-labelling, spintronics and quantum computing.Comment: 5 pages, 4 figure

Towards a fullerene-based quantum computer

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 realising 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.Comment: 20 pages, 13 figs, single column forma

Electron spin relaxation of N@C60 in CS2

We examine the temperature dependence of the 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 > 1/2 spins in liquid solution, and is the mechanism postulated in the literature for these systems. Instead, we find a clear 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 non-zero 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 170K.Comment: 6 pages, 6 figures V2: Updated to published versio

Coherent state transfer between an electron- and nuclear spin in 15N@C60

Electron spin qubits in molecular systems offer high reproducibility and the ability to self assemble into larger architectures. However, interactions between neighbouring qubits are 'always-on' and although the electron spin coherence times can be several hundred microseconds, these are still much shorter than typical times for nuclear spins. Here we implement an electron-nuclear hybrid scheme which uses coherent transfer between electron and nuclear spin degrees of freedom in order to both controllably turn on/off dipolar interactions between neighbouring spins and benefit from the long nuclear spin decoherence times (T2n). We transfer qubit states between the electron and 15N nuclear spin in 15N@C60 with a two-way process fidelity of 88%, using a series of tuned microwave and radiofrequency pulses and measure a nuclear spin coherence lifetime of over 100 ms.Comment: 5 pages, 3 figures with supplementary material (8 pages