Influence of electronic spin and spin-orbit coupling on decoherence in mononuclear transition metal complexes

Michael J. Graham, Joseph M. Zadrozny, Muhandis Shiddiq, John S. Anderson, Majed S. Fataftah, Stephen Hill*, Danna E Freedman

*Corresponding author for this work

Research output: Contribution to journalArticle

62 Scopus citations

Abstract

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 (ζ = 464, 880, 3100 cm-1) on quantum decoherence. Coherence times (T2) 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, T2, and the presence of Rabi oscillations. The complex [Ru(C2O4) 3]3- exhibits both a coherence time of T2 = 3.4 μs 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.

Original languageEnglish (US)
Pages (from-to)7623-7626
Number of pages4
JournalJournal of the American Chemical Society
Volume136
Issue number21
DOIs
StatePublished - May 28 2014

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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