4.8 Article

Influence of Electronic Spin and Spin-Orbit Coupling on Decoherence in Mononuclear Transition Metal Complexes

期刊

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 136, 期 21, 页码 7623-7626

出版社

AMER CHEMICAL SOC
DOI: 10.1021/ja5037397

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资金

  1. Northwestern University
  2. Institute for Sustainability and Energy at Northwestern University (ISEN) [10031846]
  3. NSF [DMR-1309463, DMR-0654118]
  4. United States Air Force (AOARD) [134031]
  5. MRSEC program of the NSF at Northwestern University [DMR-1121262]
  6. International Institute for Nanotechnology
  7. State of Illinois DCEO Award [10-203031]
  8. Division Of Materials Research
  9. Direct For Mathematical & Physical Scien [1309463] Funding Source: National Science Foundation

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Enabling the rational synthesis of molecular candidates for quantum information processing requires design principles that minimize electron spin decoherence. Here we report a systematic investigation of decoherence via the synthesis of two series of paramagnetic coordination complexes. These complexes, [M(C2O4)(3)](3-) (M = Ru, Cr, Fe) and [M(CN)(6)](3-) (M = Fe, Ru, Os), were prepared and interrogated by pulsed electron paramagnetic resonance (EPR) spectroscopy to assess quantitatively the influence of the magnitude of spin (S = 1/2, 3/2, 5/2) and spin orbit coupling (zeta = 464, 880, 3100 cm(-1)) on quantum decoherence. Coherence times (T-2) were collected via Hahn echo experiments and revealed a small dependence on the two variables studied, demonstrating that the magnitudes of spin and spin-orbit coupling are not the primary drivers of electron spin decoherence. On the basis of these conclusions, a proof-of-concept molecule, [Ru(C2O4)(3)](3-), was selected for further study. The two parameters establishing the viability of a qubit are a long coherence time, T-2, and the presence of Rabi oscillations. The complex [Ru(C2O4)(3)](3-) exhibits both a coherence time of T-2 = 3.4 mu s and the rarely observed Rabi oscillations. These two features establish [Ru(C2O4)(3)](3-) as a molecular qubit candidate and mark the viability of coordination complexes as qubit platforms. Our results illustrate that the design of qubit candidates can be achieved with a wide range of paramagnetic ions and spin states while preserving a long-lived coherence.

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