Influence of local fullerene orientation on the electronic properties of A3C60 compounds

We have investigated sodium containing fullerene superconductors Na2AC60, A = Cs, Rb, and K, by Na-23 nuclear magnetic resonance (NMR) spectroscopy at 7.5 T in the temperature range of 10 to 400 K. Despite the structural differences from the Rb3C60 class of fullerene superconductors, in these compounds the NMR line of the tetrahedrally coordinated alkali nuclei also splits into two lines (T and T') at low temperature. In Na2CsC60 the splitting occurs at 170 K; in the quenched cubic phase of Na2RbC60 and Na2KC60 we observe split lines at 80 K. Detailed investigations of the spectrum, spin-spin and spin-lattice relaxation as well as spin-echo double resonance (SEDOR) in Na2CsC60 we show that these two different tetrahedral sites are mixed on a microscopic scale. The T and T' sites differ in the orientation of first-neighbor C60 molecules. We present evidence that the orientations of neighboring molecules are uncorrelated. Thermally activated molecular reorientations cause an exchange between the T and T' sites and motional narrowing at high temperature. We infer the same activation energy, 3300 K, in the temperature range 125 to 300 K. The spin lattice relaxation rate is the same for T and T' down to 125 K but different below. Both the spin-lattice relaxation rate and Knight shift are strongly temperature dependent in the whole range investigated. We interpret this temperature variation by the effect of phonon excitations involving the rigid librational motion of the C60 molecules. By extending the understanding of the structure and molecular dynamics of C60 superconductors, these results may help in clarifying the effects of the structure on the superconducting properties.Comment: 13 pages, 10 figures, submitted to PR

Charge Order Driven spin-Peierls Transition in NaV2O5

We conclude from 23Na and 51V NMR measurements in NaxV2O5(x=0.996) a charge ordering transition starting at T=37 K and preceding the lattice distortion and the formation of a spin gap Delta=106 K at Tc=34.7 K. Above Tc, only a single Na site is observed in agreement with the Pmmn space group of this first 1/4-filled ladder system. Below Tc=34.7 K, this line evolves into eight distinct 23Na quadrupolar split lines, which evidences a lattice distortion with, at least, a doubling of the unit cell in the (a,b) plane. A model for this unique transition implying both charge density wave and spin-Peierls order is discussed.Comment: 4 pages, 3 figures, submitted to Phys. Rev. Let

Entanglement in a Solid State Spin Ensemble

Entanglement is the quintessential quantum phenomenon and a necessary ingredient in most emerging quantum technologies, including quantum repeaters, quantum information processing (QIP) and the strongest forms of quantum cryptography. Spin ensembles, such as those in liquid state nuclear magnetic resonance, have been powerful in the development of quantum control methods, however, these demonstrations contained no entanglement and ultimately constitute classical simulations of quantum algorithms. Here we report the on-demand generation of entanglement between an ensemble of electron and nuclear spins in isotopically engineered phosphorus-doped silicon. We combined high field/low temperature electron spin resonance (3.4 T, 2.9 K) with hyperpolarisation of the 31P nuclear spin to obtain an initial state of sufficient purity to create a non-classical, inseparable state. The state was verified using density matrix tomography based on geometric phase gates, and had a fidelity of 98% compared with the ideal state at this field and temperature. The entanglement operation was performed simultaneously, with high fidelity, to 10^10 spin pairs, and represents an essential requirement of a silicon-based quantum information processor.Comment: 4 pages, 3 figures plus supporting information of 4 pages, 1 figure v2: Updated reference

An all silicon quantum computer

A solid-state implementation of a quantum computer composed entirely of silicon is proposed. Qubits are Si-29 nuclear spins arranged as chains in a Si-28 (spin-0) matrix with Larmor frequencies separated by a large magnetic field gradient. No impurity dopants or electrical contacts are needed. Initialization is accomplished by optical pumping, algorithmic cooling, and pseudo-pure state techniques. Magnetic resonance force microscopy is used for readout. This proposal takes advantage of many of the successful aspects of solution NMR quantum computation, including ensemble measurement, RF control, and long decoherence times, but it allows for more qubits and improved initialization.Comment: ReVTeX 4, 5 pages, 2 figure

Spin coherence lifetime extension in Tm3+^{3+}:YAG through dynamical decoupling

We report on spin coherence lifetime extension on Tm$^{3+}$:YAG obtained through dynamically decoupling the thulium spins from their magnetic environment. The coherence lifetime reached with a Carr-Purcell-Meiboom-Gill sequence revealed a 450-fold extension [$\sim$$(230 \pm 30)$ ms] with respect to previously measured values. Comparison to a simple theoretical model allowed us to estimate the correlation time of the fluctuations of the ground level transition frequency to $(172 \pm 30)$ $\mu$s at 1.7 K. For attaining efficient decoupling sequences, we developed a strategy inspired by the \emph{zero-first-order Zeeman} effect to minimize the large inhomogeneous broadening of the ground level spin transition.Comment: 10 pages, 7 figure

Bang-bang control of fullerene qubits using ultra-fast phase gates

Quantum mechanics permits an entity, such as an atom, to exist in a superposition of multiple states simultaneously. Quantum information processing (QIP) harnesses this profound phenomenon to manipulate information in radically new ways. A fundamental challenge in all QIP technologies is the corruption of superposition in a quantum bit (qubit) through interaction with its environment. Quantum bang-bang control provides a solution by repeatedly applying `kicks' to a qubit, thus disrupting an environmental interaction. However, the speed and precision required for the kick operations has presented an obstacle to experimental realization. Here we demonstrate a phase gate of unprecedented speed on a nuclear spin qubit in a fullerene molecule (N@C60), and use it to bang-bang decouple the qubit from a strong environmental interaction. We can thus trap the qubit in closed cycles on the Bloch sphere, or lock it in a given state for an arbitrary period. Our procedure uses operations on a second qubit, an electron spin, in order to generate an arbitrary phase on the nuclear qubit. We anticipate the approach will be vital for QIP technologies, especially at the molecular scale where other strategies, such as electrode switching, are unfeasible

Vortex State of Tl2_2Ba2_2CuO6+δ_{6+\delta} via 205^{205}Tl NMR at 2 Tesla

We report a $^{205}$Tl NMR study of vortex state for an aligned polycrystalline sample of an overdoped high-$T_c$ superconductor Tl$_2$Ba$_2$CuO$_{6+\delta}$ ($T_{c}\sim$85 K) with magnetic field 2 T along the c axis. We observed an imperfect vortex lattice, so-called Bragg glass at $T$=5 K, coexistence of vortex solid with liquid between 10 and 60 K, and vortex melting between 65 and 85 K. No evidence for local antiferromagnetic ordering at vortex cores was found for our sample.Comment: 4 pages with 5 figure

Electron Spin Density Distribution in the Polymer Phase of CsC 60 : Assignment of the NMR Spectrum

We present high resolution 133 Cs-13 C double resonance NMR data and 13 C-13 C NMR correlation spectra of 13 C enriched samples of the polymeric phase of CsC 60 . These data lead to a partial assignment of the lines in the 13 C NMR spectrum of CsC 60 to the carbon positions on the C 60 molecule. A plausible completion of the assignment can be made on the basis of an ab initio calculation. The data support the view that the conduction electron density is concentrated at the C 60 "equator," away from the interfullerene bonds. PACS numbers: 71.20.Tx, 76.70.Fz The electronic and magnetic properties of the alkali intercalated fullerides, A n C 60 , are still only partly understood. The case A Rb, Cs, n 1 has attracted particular interest The basic structural features of the polymer phase, such as the dimensions of the unit cell, C 60 center positions, and the 2 1 2 cycloaddition polymerization along the crystallographic a axis are widely supported through x-ray diffraction However the degree of deformation of the C 60 balls [25] and the rotational orientation of the polymer chains are less well characterized. Neutron diffraction NMR has proven a useful probe of structure and electronic properties both for the broader class of alkali intercalated fulleride materials In order to obtain sufficient sensitivity, samples of CsC 60 were synthesized using 13 C enriched fullerenes. These were prepared by packing and sintering 13 C enriched amorphous carbon into graphite tubes to create 13 C enriched carbon rods. The fullerenes were subsequently produced by arcing a 60 A, 25 V dc current between an ordinar

Spin-Gap Proximity Effect Mechanism of High Temperature Superconductivity

When holes are doped into an antiferromagnetic insulator they form a slowly fluctuating array of ``topological defects'' (metallic stripes) in which the motion of the holes exhibits a self-organized quasi one-dimensional electronic character. The accompanying lateral confinement of the intervening Mott-insulating regions induces a spin gap or pseudogap in the environment of the stripes. We present a theory of underdoped high temperature superconductors and show that there is a {\it local} separation of spin and charge, and that the mobile holes on an individual stripe acquire a spin gap via pair hopping between the stripe and its environment; i.e. via a magnetic analog of the usual superconducting proximity effect. In this way a high pairing scale without a large mass renormalization is established despite the strong Coulomb repulsion between the holes. Thus the {\it mechanism} of pairing is the generation of a spin gap in spatially-confined {\it Mott-insulating} regions of the material in the proximity of the metallic stripes. At non-vanishing stripe densities, Josephson coupling between stripes produces a dimensional crossover to a state with long-range superconducting phase coherence. This picture is established by obtaining exact and well-controlled approximate solutions of a model of a one-dimensional electron gas in an active environment. An extended discussion of the experimental evidence supporting the relevance of these results to the cuprate superconductors is given.Comment: 30 pages, 2 figure

Planar 17O NMR study of Pr_yY_{1-y}Ba_2Cu_3O_{6+x}

We report the planar ^{17}O NMR shift in Pr substituted YBa_{2}Cu_{3}O_{6+x}, which at x=1 exhibits a characteristic pseudogap temperature dependence, confirming that Pr reduces the concentration of mobile holes in the CuO_{2} planes. Our estimate of the rate of this counterdoping effect, obtained by comparison with the shift in pure samples with reduced oxygen content, is found insufficient to explain the observed reduction of T_c. From the temperature dependent magnetic broadening of the ^{17}O NMR we conclude that the Pr moment and the local magnetic defect induced in the CuO_2 planes produce a long range spin polarization in the planes, which is likely associated with the extra reduction of T_c. We find a qualitatively different behaviour in the oxygen depleted Pr_yY_{1-y}Ba_2Cu_3O_{6.6}, i.e. the suppression of T$_c$ is nearly the same, but the magnetic broadening of the ^{17}O NMR appears weaker. This difference may signal a weaker coupling of the Pr to the planes in the underdoped compound, which might be linked with the larger Pr to CuO_2 plane distance, and correspondingly weaker hybridization.Comment: 8 pages, 9 figures, accepted in Phys Rev