Will spin-relaxation times in molecular magnets permit quantum information processing?

Using X-band pulsed electron spin resonance, we report the intrinsic spin-lattice ($T_1$) and phase coherence ($T_2$) relaxation times in molecular nanomagnets for the first time. In Cr$_7M$ heterometallic wheels, with $M$ = Ni and Mn, phase coherence relaxation is dominated by the coupling of the electron spin to protons within the molecule. In deuterated samples $T_2$ reaches 3 $\mu$s at low temperatures, which is several orders of magnitude longer than the duration of spin manipulations, satisfying a prerequisite for the deployment of molecular nanomagnets in quantum information applications.Comment: 4 pages, 3 figures, in press at Physical Review Letter

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

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

Electrochemical Conversion of the Lignin Model Veratryl Alcohol to Veratryl Aldehyde Using Manganese(III)-Schiff Base Homogeneous Catalysts

Lignin and other colored structures need to be bleached after the Kraft process in the pulp industry. Development of environmentally-safe bleaching catalysts or electrocatalysts constitutes an attractive strategy for selective removal of lignin. Seven manganese(III)-complexes with Schiff base ligands 1–7 were synthetized and characterized by different analytical and spectroscopic techniques. The tetragonally elongated octahedral geometry for the manganese coordination sphere and the global µ-aquo dimeric structure were revealed by X-ray diffraction (XRD) studies for 1, Mn2L12(H2O)2(N(CN)2)2 (N(CN)2 = dicyanamide). Complexes 1–4 behave as more efficient peroxidase mimics as compared to 5–7. Electrochemical oxidation of the lignin model veratrylalcohol (VA) to veratrylaldehyde (VAH) is efficiently catalyzed by a type of dimanganese(III) complexes in a chlorine-free medium. The electrocatalytic reaction proceeds through the oxidation of chloride into hypochlorite at alkaline pH along with the formation of hydrogen from water as a subproductThis research was funded by Xunta de Galicia (GRC GI-1584-ED431C2018/13 Suprabioin Research Group, and MetalBIO Network ED431D 2017/01)S

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

Contactless photoconductivity-detected electron spin resonance of P donors in isotopically purified Si

Coherence times of electron spins bound to phosphorus donors have been measured, using a standard Hahn echo technique, to be up to 20 ms in isotopically pure silicon with [P]$= 10^{14}$ cm$^{-3}$ and at temperatures $\leq 4$K. Although such times are exceptionally long for electron spins in the solid state, they are nevertheless limited by donor electron spin-spin interactions. Suppressing such interactions requires even lower donor concentrations, which lie below the detection limit for typical electron spin resonance (ESR) spectrometers. Here we describe an alternative method for phosphorus donor ESR detection, exploiting the spin-to-charge conversion provided by the optical donor bound exciton transition. We characterise the method and its dependence on laser power and use it to measure a coherence time of $T_2 = 130$ms for one of the purest silicon samples grown to-date ([P]$= 5\times 10^{11}$cm$^{-3}$). We then benchmark this result using an alternative application of the donor bound exciton transition: optically polarising the donor spins before using conventional ESR detection at 1.7~K for a sample with [P]$= 4\times10^{12}$cm$^{-3}$, and measuring in this case a $T_2$ of 350 ms

A new mechanism for electron spin echo envelope modulation

Electron spin echo envelope modulation (ESEEM) has been observed for the first time from a coupled hetero-spin 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 NMR or a pair of resonant electron spins in EPR. We observe low-frequency ESEEM (26 and 52 kHz) due to a new mechanism present for any electron spin with S>1/2 that is hyperfine coupled to a nuclear spin. In our case these are electron spin (S=3/2) and nuclear spin (I=1) in the endohedral fullerene N@C60. The modulation is shown to arise from second order effects in the isotropic hyperfine coupling of an electron and 14N nucleus.Comment: 15 pages, 4 figure