Coherent Manipulation of a Molecular Ln-Based Nuclear Qudit Coupled to an Electron Qubit

Hussain, Riaz; Allodi, G.; Chiesa, Alessandro; Garlatti, Elena; Mitcov, Dmitri; Konstantatos, Andreas; Pedersen, Kasper S.; Renzi, R. De; Piligkos, Stergios; Carretta, S.

doi:10.1021/jacs.8b05934

Cited by 104 publications

(153 citation statements)

References 62 publications

(123 reference statements)

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“…Both nuclear spins [5] and electron spins, [6] as well as electron-nuclear hybrid systems, [7,8] can be exploited for this purpose. Electron spins interact more strongly with the environment, compared to the nuclear ones, and thus they are easier to read out.…”

Section: Introductionmentioning

confidence: 99%

First-Principles Investigation of Spin–Phonon Coupling in Vanadium-Based Molecular Spin Quantum Bits

Albino¹,

Benci²,

Tesi³

et al. 2019

Inorg. Chem.

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Paramagnetic molecules can show long spin-coherence times, which make them good candidates as quantum bits. Reducing the efficiency of the spin-phonon interaction is the primary challenge towards achieving long coherence times over a wide temperature range in soft molecular lattices. The lack of a microscopic understanding about the role of vibrations in spin relaxation strongly undermines the possibility to chemically design better performing molecular qubits. Here we report a first-principles characterization of the main mechanism contributing to the spin-phonon coupling for a class of vanadium(IV) molecular qubits. Post Hartree Fock and Density Functional Theory are used to determine the effect of both reticular and intra-molecular vibrations on the modulation of the Zeeman energy for four molecules showing different coordination geometries and ligands. This comparative study provides the first insight into the role played by coordination geometry and ligand field strength in determining the spinlattice relaxation time of molecular qubits, opening the avenue to a rational design of new compounds.

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Section: Introductionmentioning

confidence: 99%

First-Principles Investigation of Spin–Phonon Coupling in Vanadium-Based Molecular Spin Quantum Bits

Albino¹,

Benci²,

Tesi³

et al. 2019

Inorg. Chem.

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“…he two main pillars of the current research in molecular magnetism are the possibilities of exploiting molecules as classical bits for high-density magnetic memories [1][2][3][4][5] or as quantum bits (qubits) for quantum information processing [6][7][8][9][10][11][12] . The use of molecular nanomagnets (MNMs) as classical bits relies on their slow relaxation of the magnetisation, which is undermined by spin-phonon interactions 13 .…”

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confidence: 99%

Unveiling phonons in a molecular qubit with four-dimensional inelastic neutron scattering and density functional theory

et al. 2020

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Phonons are the main source of relaxation in molecular nanomagnets, and different mechanisms have been proposed in order to explain the wealth of experimental findings. However, very limited experimental investigations on phonons in these systems have been performed so far, yielding no information about their dispersions. Here we exploit state-ofthe-art single-crystal inelastic neutron scattering to directly measure for the first time phonon dispersions in a prototypical molecular qubit. Both acoustic and optical branches are detected in crystals of [VO(acac) 2 ] along different directions in the reciprocal space. Using energies and polarisation vectors calculated with state-of-the-art Density Functional Theory, we reproduce important qualitative features of [VO(acac) 2 ] phonon modes, such as the presence of low-lying optical branches. Moreover, we evidence phonon anti-crossings involving acoustic and optical branches, yielding significant transfers of the spin-phonon coupling strength between the different modes.

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“…The aim was to produce molecules with three qubits capable to realize more complex qugates, such as quantum error correction protocols. [38][39] We thus turned our attention to the ligand H2LA (Fig 1), which had been synthesized by us as the precursor of another multidentate ligand. [40] H2LA exhibits an additional β-diketone (O,O) unit as compared with H3L, thus having the ability to chelate a third Ln, while featuring still only two different environments and thus two-metal selectivity.…”

mentioning

confidence: 99%

“…We explored this eventuality through reactions in pyridine of H2LA with Ce(NO3)3/Ln(NO3) mixtures in the 1:2 molar ratio, Ln being Ho III , Er III or Yb III , thus with a marked smaller ionic radius than Ce III . The choice of metals is justified by our future interest in studying these compounds as qugates to perform quantum error correction protocols [38] or other three qubit qugates. The Ce and Er metals are interesting for their low content of nuclear spin (I = 0 for Ce and only 23% of I = 7/2 for Er), reducing the sources of decoherence.…”

mentioning

confidence: 99%

Controlled Heterometallic Composition in Linear Trinuclear [LnCeLn] Lanthanide Molecular Assemblies

Velasco

Barrios

Schütze

et al. 2019

Chemistry A European J

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The combination of two different β-diketone ligands facilitates the size-controlled assembly of pure heterometallic [LnLn'Ln] linear compounds thanks to two different coordination sites present in the molecular scaffold.[HoCeHo], [ErCeEr] and [YbCeYb] analogues are presented here and are characterized both in the solid state and solution, demonstrating the selectivity of thi s unique method to produce heterometallic 4f molecular entities.

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Coherent Manipulation of a Molecular Ln-Based Nuclear Qudit Coupled to an Electron Qubit

Cited by 104 publications

References 62 publications

First-Principles Investigation of Spin–Phonon Coupling in Vanadium-Based Molecular Spin Quantum Bits

First-Principles Investigation of Spin–Phonon Coupling in Vanadium-Based Molecular Spin Quantum Bits

Unveiling phonons in a molecular qubit with four-dimensional inelastic neutron scattering and density functional theory

Controlled Heterometallic Composition in Linear Trinuclear [LnCeLn] Lanthanide Molecular Assemblies

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