An exchange coupled <i>meso</i>–<i>meso</i> linked vanadyl porphyrin dimer for quantum information processing

Ranieri, Davide; Santanni, Fabio; Privitera, Alberto; Albino, Andrea; Salvadori, Enrico; Chiesa, Mario; Totti, Federico; Sorace, Lorenzo; Sessoli, Roberta

doi:10.1039/d2sc04969d

Cited by 30 publications

(81 citation statements)

References 70 publications

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“…Dipolar, D, and exchange, J, interactions cannot be distinguished experimentally here. The exchange coupling J is thus in the order of 1 GHz, which is stronger than in previously reported bis-vanadyl complexes with similar inter-spin distances, 50,66,67 but two orders of magnitude weaker than in the analogous Cu(II) porphyrin dimer. 44,45 ).…”

Section: Table 1 Epr Parameters For Vanadyl Porphyrinscontrasting

confidence: 53%

“…The exchange coupling J » 1 GHz deduced from magnetic susceptibility measurements (discussed below) suggests that syn-P2•VO THS and anti-P2•VO THS are in this strong-exchange regime, dominated by the J interaction. This places the conjugated vanadyl dimers in a regime that is different from previous non-conjugated molecular architectures, 50,66,67 which are paired quantum mechanically by dominant hyperfine and dipole-dipole interactions, rather than exchange coupling. Simulation of the spectra was achieved by considering that J is the dominant contribution and the hyperfine coupling values should be roughly half those of the monomer, with the Hamiltonian:…”

Section: Table 1 Epr Parameters For Vanadyl Porphyrinsmentioning

confidence: 62%

“…The singly-linked dimers sl-P2•VO are in an intermediate situation, being not weakly interacting doublets nor pure triplets, as recently reported for an analogous molecule. 50 The best simulation was achieved assuming the behavior as two weakly interacting doublets with the following set of parameters: gxy = 1.9612±0.0001 and gz = 1.9840±0.0002, Axy = 477±2 MHz and Az = 170±1 MHz, D = 84±1 MHz, and J = 272±1 MHz, with antiferromagnetic coupling. The values obtained in this way are in good agreement with those reported for a magnetically equivalent system.…”

Section: Resultsmentioning

confidence: 99%

“…To date, the influence of π-conjugation on the quantum coherence of vanadyl units in porphyrin arrays remains elusive, despite recent studies of edge-fused and singly-linked vanadyl dimers. 49,50 Meso-aryl substituents are commonly used to tune the solubility of porphyrin polymers. t-Busubstituted aryls are useful for growing crystals for X-ray diffraction analysis, whereas flexible side chains, such as Si(C6H13)3, confer higher solubility and prevent aggregation.…”

Section: Introductionmentioning

confidence: 99%

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Enhanced Coherence by Coupling Spins through a Delocalized π-System: Vanadyl Porphyrin Dimers

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Lombardi

et al. 2023

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Vanadium(IV) magnetic centers are prime candidates as molecular quantum units. One longstanding question is how to obtain a scaffold that connects multiple centers and allows two communication modalities: magnetic and electronic. We have synthesized and studied a selection of vanadyl porphyrin dimers, as models of the most synthetically accessible linear porphyrin arrays. We show that a strongly π-conjugated backbone places the magnetic system in the strong coupling regime and protects the quantum coherence against electron pair flip-flop processes at low temperatures (<10 K). This result is a fundamental step towards the design of molecular materials for single-molecule devices controlled by microwaves with electrical readout.

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Section: Table 1 Epr Parameters For Vanadyl Porphyrinscontrasting

confidence: 53%

Section: Table 1 Epr Parameters For Vanadyl Porphyrinsmentioning

confidence: 62%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Enhanced Coherence by Coupling Spins through a Delocalized π-System: Vanadyl Porphyrin Dimers

Pozo

Huang

Lombardi

et al. 2023

Preprint

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“…Here we choose the well-characterized and radiation-robust [VO(TPP)] complex (VO = vanadyl, TPP = tetraphenylporphyrinate) 27 as a benchmark to show the capabilities of a multi-technique approach with all these characteristics. [VO(TPP)] is also a very promising molecular qubit: It allows simultaneous coherent manipulation of both electronic and nuclear spins 20 , 28 and it forms dimeric species where the two electronic spins are distinguishable and exchange-coupled to implement quantum gates 29 . To fulfill point (i), we exploit Inelastic X-ray Scattering (IXS).…”

Section: Introductionmentioning

confidence: 99%

The critical role of ultra-low-energy vibrations in the relaxation dynamics of molecular qubits

et al. 2023

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Improving the performance of molecular qubits is a fundamental milestone towards unleashing the power of molecular magnetism in the second quantum revolution. Taming spin relaxation and decoherence due to vibrations is crucial to reach this milestone, but this is hindered by our lack of understanding on the nature of vibrations and their coupling to spins. Here we propose a synergistic approach to study a prototypical molecular qubit. It combines inelastic X-ray scattering to measure phonon dispersions along the main symmetry directions of the crystal and spin dynamics simulations based on DFT. We show that the canonical Debye picture of lattice dynamics breaks down and that intra-molecular vibrations with very-low energies of 1-2 meV are largely responsible for spin relaxation up to ambient temperature. We identify the origin of these modes, thus providing a rationale for improving spin coherence. The power and flexibility of our approach open new avenues for the investigation of magnetic molecules with the potential of removing roadblocks toward their use in quantum devices.

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Chirality‐Induced Spin Selectivity: An Enabling Technology for Quantum Applications

et al. 2023

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Molecular spins are promising building blocks of future quantum technologies thanks to the unparalleled flexibility provided by chemistry, which allows the design of complex structures targeted for specific applications. However, their weak interaction with external stimuli makes it difficult to access their state at the single‐molecule level, a fundamental tool for their use, for example, in quantum computing and sensing. Here, an innovative solution exploiting the interplay between chirality and magnetism using the chirality‐induced spin selectivity effect on electron transfer processes is foreseen. It is envisioned to use a spin‐to‐charge conversion mechanism that can be realized by connecting a molecular spin qubit to a dyad where an electron donor and an electron acceptor are linked by a chiral bridge. By numerical simulations based on realistic parameters, it is shown that the chirality‐induced spin selectivity effect could enable initialization, manipulation, and single‐spin readout of molecular qubits and qudits even at relatively high temperatures.

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An exchange coupled meso–meso linked vanadyl porphyrin dimer for quantum information processing

Abstract: We report here the synthesis of a new meso-meso (m-m) singly linked vanadyl-porphyrin dimer that crystallizes in two different pseudo-polymorphs. The single crystal continuous-wave Electron Paramagnetic Resonance investigation evidences a...

Cited by 30 publications

References 70 publications

Enhanced Coherence by Coupling Spins through a Delocalized π-System: Vanadyl Porphyrin Dimers

Enhanced Coherence by Coupling Spins through a Delocalized π-System: Vanadyl Porphyrin Dimers

The critical role of ultra-low-energy vibrations in the relaxation dynamics of molecular qubits

Chirality‐Induced Spin Selectivity: An Enabling Technology for Quantum Applications

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