Storage and Retrieval of Electronic Spin Coherence Using Nuclear Spins in a Vanadyl Paddlewheel
Abstract
Electronic and nuclear spins are complementary carriers of quantum information: whereas nuclear spins exhibit long coherence times suitable for information storage, electronic spins ensure rapid addressing and readout. A key challenge is harvesting the benefits of both spin degrees of freedom by transferring coherence between them. In this work, we achieved this goal by working on a molecular architecture that affords precise control over the hyperfine multiplets, spin dispersion, and molecular orientation within a crystalline host. As a model system, we used heterobimetallic paddlewheel complex [VOPt(SOCPh) 4 ] diluted in [TiOPt(SOCPh) 4 ]•2THF diamagnetic crystalline host matrix (nominal concentrations of 1 and 10%). In [VOPt(SOCPh) 4 ], vanadyl electronic spin S = 1/2 is hyperfinely coupled to the nuclear spin I = 7/2 of 51 V. These electronic and nuclear spins were simultaneously manipulated using sequences of radiofrequency (RF) and microwave (MW) pulses generated by a multifrequency on-chip setup operating at a cryogenic temperature. First, Electron-Nuclear DOuble Resonance (ENDOR) experiments were performed to show the readout of the 51 V nuclear spin transitions through the electronic spin echo. Further experiments with a dedicated RF-MW pulse sequence demonstrated that electronic phase coherence can be stored in the nuclear spins and retrieved (Storage and Retrieval, SR) after a total free precession time that greatly exceeds the electronic phase memory time. This result demonstrates the possibility of simultaneous manipulation of electronic and nuclear spins and establishes a route for encoding quantum information on both degrees of freedom of a chemically tunable platform.
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BibTeX
@article{lanza2026storage,
title = {{Storage and Retrieval of Electronic Spin Coherence Using Nuclear Spins in a Vanadyl Paddlewheel}},
author = {Matteo Lanza and Olga Mironova and Claudio Bonizzoni and Giacomo Bellini and Alessio Nicolini and Alberto Ghirri and Rodolphe Clérac and Mathieu Rouzières and Andrea Cornia and Marco Affronte},
journal = {Journal of the American Chemical Society},
year = {2026},
month = oct,
doi = {10.1021/jacs.6c10524},
url = {https://hal.science/hal-05785763v1},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Storage and Retrieval of Electronic Spin Coherence Using Nuclear Spins in a Vanadyl Paddlewheel
AU - Matteo Lanza
AU - Olga Mironova
AU - Claudio Bonizzoni
AU - Giacomo Bellini
AU - Alessio Nicolini
AU - Alberto Ghirri
AU - Rodolphe Clérac
AU - Mathieu Rouzières
AU - Andrea Cornia
AU - Marco Affronte
PY - 2026
DA - 2026/10/08
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c10524
UR - https://hal.science/hal-05785763v1
AB - Electronic and nuclear spins are complementary carriers of quantum information: whereas nuclear spins exhibit long coherence times suitable for information storage, electronic spins ensure rapid addressing and readout. A key challenge is harvesting the benefits of both spin degrees of freedom by transferring coherence between them. In this work, we achieved this goal by working on a molecular architecture that affords precise control over the hyperfine multiplets, spin dispersion, and molecular orientation within a crystalline host. As a model system, we used heterobimetallic paddlewheel complex [VOPt(SOCPh) 4 ] diluted in [TiOPt(SOCPh) 4 ]•2THF diamagnetic crystalline host matrix (nominal concentrations of 1 and 10%). In [VOPt(SOCPh) 4 ], vanadyl electronic spin S = 1/2 is hyperfinely coupled to the nuclear spin I = 7/2 of 51 V. These electronic and nuclear spins were simultaneously manipulated using sequences of radiofrequency (RF) and microwave (MW) pulses generated by a multifrequency on-chip setup operating at a cryogenic temperature. First, Electron-Nuclear DOuble Resonance (ENDOR) experiments were performed to show the readout of the 51 V nuclear spin transitions through the electronic spin echo. Further experiments with a dedicated RF-MW pulse sequence demonstrated that electronic phase coherence can be stored in the nuclear spins and retrieved (Storage and Retrieval, SR) after a total free precession time that greatly exceeds the electronic phase memory time. This result demonstrates the possibility of simultaneous manipulation of electronic and nuclear spins and establishes a route for encoding quantum information on both degrees of freedom of a chemically tunable platform.
SN - 0002-7863
SN - 1520-5126
ER -