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Probing Vibrational Symmetry Effects and Nuclear Spin Economy Principles in Molecular Spin Qubits.

ABSTRACT: The selection of molecular spin qubits with a long coherence time, T_m, is a central task for implementing molecule-based quantum technologies. Even if a sufficiently long T_m can be achieved through an efficient synthetic strategy and ad hoc experimental measurement procedures, many factors contributing to the loss of coherence still need to be thoroughly investigated and understood. Vibrational properties and nuclear spins of hydrogens are two of them. The former plays a paramount role, but a detailed theoretical investigation aimed at studying their effects on the spin dynamics of molecular complexes such as the benchmark phthalocyanine (Pc) is still missing, whereas the effect of the latter deserves to be examined in detail for such a class of compounds. In this work, we adopted a combined theoretical and experimental approach to investigate the relaxation properties of classical [Cu(Pc)] and a Cu^II complex based on the ligand tetrakis(thiadiazole)porphyrazine (H₂TTDPz), characterized by a hydrogen-free molecular structure. Systematic calculations of molecular vibrations exemplify the effect of normal modes on the spin-lattice relaxation process, unveiling a different contribution to T₁ depending on the symmetry of normal modes. Moreover, we observed that an appreciable T_m enhancement could be achieved by removing hydrogens from the ligand.

SUBMITTER: Santanni F

PROVIDER: S-EPMC7872321 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature

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Probing Vibrational Symmetry Effects and Nuclear Spin Economy Principles in Molecular Spin Qubits.

Santanni Fabio F Albino Andrea A Atzori Matteo M Ranieri Davide D Salvadori Enrico E Chiesa Mario M Lunghi Alessandro A Bencini Andrea A Sorace Lorenzo L Totti Federico F Sessoli Roberta R

Inorganic chemistry 20201211 1

The selection of molecular spin qubits with a long coherence time, Tm, is a central task for implementing molecule-based quantum technologies. Even if a sufficiently long Tm can be achieved through an efficient synthetic strategy and ad hoc experimental measurement procedures, many factors contributing to the loss of coherence still need to be thoroughly investigated and understood. Vibrational properties and nuclear spins of hydrogens are two of them. ...[more]

PMID: 33305944

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Project description:Molecular spin qubits are chemical nanoobjects with promising applications that are so far hampered by the rapid loss of quantum information, a process known as decoherence. A strategy to improve this situation involves employing so-called Clock Transitions (CTs), which arise at anticrossings between spin energy levels. At CTs, the spin states are protected from magnetic noise and present an enhanced quantum coherence. Unfortunately, these optimal points are intrinsically hard to control since their transition energy cannot be tuned by an external magnetic field; moreover, their resilience towards geometric distortions has not yet been analyzed. Here we employ a python-based computational tool for the systematic theoretical analysis and chemical optimization of CTs. We compare three relevant case studies with increasingly complex ground states. First, we start with vanadium(iv)-based spin qubits, where the avoided crossings are controlled by hyperfine interaction and find that these S = 1/2 systems are very promising, in particular in the case of vanadyl complexes in an L-band pulsed EPR setup. Second, we proceed with a study of the effect of symmetry distortions in a holmium polyoxotungstate of formula [Ho(W5O18)2]9- where CTs had already been experimentally demonstrated. Here we determine the relative importance of the different structural distortions that causes the anticrossings. Third, we study the most complicated case, a polyoxopalladate cube [HoPd12(AsPh)8O32]5- which presents an unusually rich ground spin multiplet. This system allows us to find uniquely favorable CTs that could nevertheless be accessible with standard pulsed EPR equipment (X-band or Q-band) after a suitable chemical distortion to break the perfect cubic symmetry. Since anticrossings and CTs constitute a rich source of physical phenomena in very different kinds of quantum systems, the generalization of this study is expected to have impact not only in molecular spin science but also in other related fields such as molecular photophysics and photochemistry.

Dataset Information

Probing Vibrational Symmetry Effects and Nuclear Spin Economy Principles in Molecular Spin Qubits.

Publications

Probing Vibrational Symmetry Effects and Nuclear Spin Economy Principles in Molecular Spin Qubits.

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