Our paper on “Storage and Retrieval of Electronic Spin Coherence using Nuclear Spins in a Vanadyl Paddlewheel” is finally online on Journal of the American Chemical Society (J.A.C.S.): https://doi.org/10.1021/jacs.6c10524

Storage and Retrieval of Spin Coherence. a) molecular structure of the Vanadyl Paddlewheel and of its diamagnetic analogue (top). Planar microwave resonator with the radiofrequency coil on it (bottom). b) Storage and Retireval protocol implemented in this work. Red wiggling line shown the location of the coherence along the sequence. Double arrows correspond to supeimposition of states. c) Refence Hahn echo sequence used to obtain the reference signals (spin components Sx and Sy) for assessing the Storage and Retrieval protocol. d) Spin component extracted after encoding the full protocol in (b). The case T=10μsT = 10 \mu s is shown but similar results are obtained also for longer delays values (up to T=50μsT = 50 \mu s).

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 51V. 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 51V 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.

NEW PAPER!! Storage and Retrieval of Electronic Spin Coherence using Nuclear Spins in a Vanadyl Paddlewheel