arXiv subjects

Richard E. P. Winpenny

Publications and source records attributed to Richard E. P. Winpenny.

7 recordsLinked to original sources

arXiv2026

Beyond Pure Dephasing: Quantum Error Correction in Single Molecules Requires Multiple Spins

We propose multi-spin molecules as a viable architecture for fault-tolerant quantum computing. To this aim, we introduce a correction protocol handling both diagonal and off-diagonal errors, typically associated with dephasing and relaxation. The scheme is based on a hybrid encoding which combines dephasing-tolerant units suppressing the leading pure dephasing error into a multi-spin molecule implementing a multi-qubit code for residual off-diagonal errors. Our proposal leverages peculiar properties of molecular spins, i.e. the strong hierarchy between different errors and the possibility to engineer multi-spin molecules at the synthetic level. Moreover, it addresses the important issue of the loss of coherences in anharmonic systems subject to off-diagonal errors, which hampers their correction at the single spin level. Thanks to the huge suppression of dephasing by the first-level code, we numerically demonstrate the potential performance of this strategy even with a limited number of spins per logical unit.

cond-mat.mes-hall↗

arXiv2025

Enhancing Coherence with a Clock Transition and Dynamical Decoupling in the Cr$_7$Mn Molecular Nanomagnet

Molecular magnets are attractive as spin qubits due to their chemical tunability, addressability through electron-spin resonance techniques, and long coherence times. Clock transitions (CTs), for which the system is immune to the effect of magnetic-field fluctuations to first order, provide a method to enhance the coherence time $T_2$, and to reveal mechanisms of decoherence that are not due to such fluctuations. Here we investigate two variants of Cr$_7$Mn, a spin-1 molecular nanomagnet, at fields near a zero-field CT. We find that at temperatures $\le$2 K, $T_2\sim1$ $μ$s at the CT using a Hahn-echo pulse sequence. Away from the CT, electron-spin-echo envelope modulation (ESEEM) oscillations due to coupling to nuclear spins are observed and have a $T_2$ as high as $1.35$ $μ$s, indicating a distinct mechanism of coherence preservation. Dynamical decoupling with the CPMG pulse sequence yields $T_2\sim\!2.8$ $μ$s at the CT and up to $\sim\!3.6$ $μ$s in the ESEEM regime along with a demodulation of the oscillatory behavior. The experimental values of $T_2$ are largely independent of the degree of dilution of the molecules in solvent or whether the solvent is deuterated, indicating that much of the decoherence and ESEEM arises from sources within the molecules themselves. To account for decoherence, we develop a model that includes not only field fluctuations but also fluctuations in the CT transition frequency itself. Our results can be well explained by treating the environment as a combination of noise at the nuclear Larmor precession frequency and $1/f$ noise in the transverse anisotropy parameter $E$. Such information about the microscopic origins of decoherence can aid the rational design of molecular-based spin qubits.

cond-mat.mes-hall↗

arXiv2018

Electric field control of spins in molecular magnets

Coherent control of individual molecular spins in nano-devices is a pivotal prerequisite for fulfilling the potential promised by molecular spintronics. By applying electric field pulses during time-resolved electron spin resonance measurements, we measure the sensitivity of the spin in several antiferromagnetic molecular nanomagnets to external electric fields. We find a linear electric field dependence of the spin states in Cr$_7$Mn, an antiferromagnetic ring with a ground-state spin of $S=1$, and in a frustrated Cu$_3$ triangle, both with coefficients of about $2~\mathrm{rad}\, \mathrm{s}^{-1} / \mathrm{V} \mathrm{m}^{-1}$. Conversely, the antiferromagnetic ring Cr$_7$Ni, isomorphic with Cr$_7$Mn but with $S=1/2$, does not exhibit a detectable effect. We propose that the spin-electric field coupling may be used for selectively controlling individual molecules embedded in nanodevices.

cond-mat.str-el↗

arXiv2018

A Clock Transition in the Cr$_7$Mn Molecular Nanomagnet

A viable qubit must have a long coherence time $T_2$. In molecular nanomagnets $T_2$ is often limited at low temperatures by the presence of dipole and hyperfine interactions, which are often mitigated through sample dilution, chemical engineering and isotope substitution in synthesis. Atomic-clock transitions offer another route to reducing decoherence from environmental fields by reducing the effective susceptibility of the working transition to field fluctuations. The Cr$_7$Mn molecular nanomagnet, a heterometallic ring, features a clock transition at zero field. Both continuous-wave and spin-echo electron-spin resonance experiments on Cr$_7$Mn samples diluted via co-crystallization, show evidence of the effects of the clock transition with a maximum $T_2\sim350$ ns at 1.8 K. We discuss improvements to the experiment that may increase $T_2$ further.

cond-mat.mes-hall↗

arXiv2015

Engineering coherent interactions in molecular nanomagnet dimers

Proposals for systems embodying condensed matter spin qubits cover a very wide range of length scales, from atomic defects in semiconductors all the way to micron-sized lithographically-defined structures. Intermediate scale molecular components exhibit advantages of both limits: like atomic defects, large numbers of identical components can be fabricated; as for lithographically defined structures, each component can be tailored to optimize properties such as quantum coherence. Here, we demonstrate what is perhaps the most potent advantage of molecular spin qubits, the scalability of quantum information processing structures using bottom-up chemical self-assembly. Using Cr7Ni spin qubit building blocks, we have constructed several families of two-qubit molecular structures with a range of linking strategies. For each family, long coherence times are preserved, and we demonstrate control over the inter-qubit quantum interactions that can be used to mediate two-qubit quantum gates.

cond-mat.mtrl-sci↗

arXiv2014

Quantum spin coherence in halogen-modified Cr$_7$Ni molecular nanomagnets

Among the factors determining the quantum coherence of the spin in molecular magnets is the presence and the nature of nuclear spins in the molecule. We have explored modifying the nuclear spin environment in Cr$_7$Ni-based molecular nanomagnets by replacing hydrogen atoms with deuterium or the halogen atoms, fluorine or chlorine. We find that the spin coherence, studied at low temperatures by pulsed electron spin resonance, is modified by a range of factors, including nuclear spin and magnetic moment, changes in dynamics owing to nuclear mass, and molecular morphology changes.

cond-mat.mtrl-sci↗

arXiv2004

Spin frustration effects in an odd-member antiferromagnetic ring and the magnetic Moebius strip

The magnetic properties of the first odd-member antiferromagnetic ring comprising eight chromium(III) ions, S=3/2 spins, and one nickel(II) ion, S=1 spin, are investigated. The ring possesses an even number of unpaired electrons and a S=0 ground state but, due to competing AF interactions, the first excited spin states are close in energy. The spin frustrated ring is visualized by a Moebius strip. The ?knot? of the strip represents the region of the ring where the AF interactions are more frustrated. In the particular case of this bimetallic ring electron paramagnetic resonance (EPR) has unambiguously shown that the frustration is delocalized on the chromium chain, while the antiparallel alignment is more rigid at the nickel site.

cond-mat.mes-hall↗