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J Am Chem Soc. 2018 Jan 24;140(3):1123-1130. doi: 10.1021/jacs.7b12170. Epub 2018 Jan 10.

Endohedral Metallofullerene as Molecular High Spin Qubit: Diverse Rabi Cycles in Gd2@C79N.

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National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, Beijing Key Laboratory for Magnetoelectric Materials and Devices, College of Chemistry and Molecular Engineering, Peking University , Beijing 100871, People's Republic of China.
CAESR, The Clarendon Laboratory, Department of Physics, University of Oxford , Oxford OX1 3PU, U.K.


An anisotropic high-spin qubit with long coherence time could scale the quantum system up. It has been proposed that Grover's algorithm can be implemented in such systems. Dimetallic aza[80]fullerenes M2@C79N (M = Y or Gd) possess an unpaired electron located between two metal ions, offering an opportunity to manipulate spin(s) protected in the cage for quantum information processing. Herein, we report the crystallographic determination of Gd2@C79N for the first time. This molecular magnet with a collective high-spin ground state (S = 15/2) generated by strong magnetic coupling (JGd-Rad = 350 ± 20 cm-1) has been unambiguously validated by magnetic susceptibility experiments. Gd2@C79N has quantum coherence and diverse Rabi cycles, allowing arbitrary superposition state manipulation between each adjacent level. The phase memory time reaches 5 μs at 5 K by dynamic decoupling. This molecule fulfills the requirements of Grover's searching algorithm proposed by Leuenberger and Loss.


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