In the development of two-qubit quantum gates, precise control over the intramolecular spin-spin interaction between molecular spin units plays a pivotal role. A weak but measurable exchange coupling is especially important for achieving selective spin addressability that allows controlled manipulation of the computational basis states |00⟩ |01⟩ |10⟩ |11⟩ by microwave pulses. Here, we report the synthesis and Electron Paramagnetic Resonance (EPR) study of a heterometallic meso-meso (m-m) singly-linked VIV O-CuII porphyrin dimer. X-band continuous wave EPR measurements in frozen solutions suggest a ferromagnetic exchange coupling of ca. 8 ⋅ 10-3  cm-1 . This estimation is supported by Density Functional Theory calculations, which also allow disentangling the ferro- and antiferromagnetic contributions to the exchange. Pulsed EPR experiments show that the dimer maintains relaxation times similar to the monometallic CuII porphyrins. The addressability of the two individual spins is made possible by the different g-tensors of VIV and CuII -ions, in contrast to homometallic dimers where tilting of the porphyrin planes plays a key role. Therefore, single-spin addressability in the heterometallic dimer can be maintained even with small tilting angles, as expected when deposited on surface, unlocking the full potential of molecular quantum gates for practical applications.

A Heterometallic Porphyrin Dimer as a Potential Quantum Gate: Magneto-Structural Correlations and Spin Coherence Properties / Ranieri, Davide; Privitera, Alberto; Santanni, Fabio; Urbanska, Karolina; Strachan, Grant J; Twamley, Brendan; Salvadori, Enrico; Liao, Yu-Kai; Chiesa, Mario; Senge, Mathias O; Totti, Federico; Sorace, Lorenzo; Sessoli, Roberta. - In: ANGEWANDTE CHEMIE. INTERNATIONAL EDITION. - ISSN 1433-7851. - ELETTRONICO. - (2023), pp. e202312936-e202312936. [10.1002/anie.202312936]

A Heterometallic Porphyrin Dimer as a Potential Quantum Gate: Magneto-Structural Correlations and Spin Coherence Properties

Ranieri, Davide;Privitera, Alberto;Santanni, Fabio;Totti, Federico;Sorace, Lorenzo
;
Sessoli, Roberta
2023

Abstract

In the development of two-qubit quantum gates, precise control over the intramolecular spin-spin interaction between molecular spin units plays a pivotal role. A weak but measurable exchange coupling is especially important for achieving selective spin addressability that allows controlled manipulation of the computational basis states |00⟩ |01⟩ |10⟩ |11⟩ by microwave pulses. Here, we report the synthesis and Electron Paramagnetic Resonance (EPR) study of a heterometallic meso-meso (m-m) singly-linked VIV O-CuII porphyrin dimer. X-band continuous wave EPR measurements in frozen solutions suggest a ferromagnetic exchange coupling of ca. 8 ⋅ 10-3  cm-1 . This estimation is supported by Density Functional Theory calculations, which also allow disentangling the ferro- and antiferromagnetic contributions to the exchange. Pulsed EPR experiments show that the dimer maintains relaxation times similar to the monometallic CuII porphyrins. The addressability of the two individual spins is made possible by the different g-tensors of VIV and CuII -ions, in contrast to homometallic dimers where tilting of the porphyrin planes plays a key role. Therefore, single-spin addressability in the heterometallic dimer can be maintained even with small tilting angles, as expected when deposited on surface, unlocking the full potential of molecular quantum gates for practical applications.
2023
e202312936
e202312936
Goal 9: Industry, Innovation, and Infrastructure
Ranieri, Davide; Privitera, Alberto; Santanni, Fabio; Urbanska, Karolina; Strachan, Grant J; Twamley, Brendan; Salvadori, Enrico; Liao, Yu-Kai; Chiesa, Mario; Senge, Mathias O; Totti, Federico; Sorace, Lorenzo; Sessoli, Roberta
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Utilizza questo identificatore per citare o creare un link a questa risorsa: https://hdl.handle.net/2158/1345646
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