Long coherence times in nuclear spin-free vanadyl qubits

Yu, Chung -Jui; Graham, Michael J.; Zadrozny, Joseph M.; Niklas, Jens; Krzyaniak, Matthew D.; Wasielewski, Michael R.; Poluektov, Oleg G.; Freedman, Danna E.

doi:10.1021/jacs.6b08467

Title: Long coherence times in nuclear spin-free vanadyl qubits

Journal Article · Mon Oct 31 00:00:00 EDT 2016 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.6b08467· OSTI ID:1351310

Yu, Chung -Jui ^[1]; Graham, Michael J. ^[1]; Zadrozny, Joseph M. ^[1]; Niklas, Jens ^[2]; Krzyaniak, Matthew D. ^[1]; Wasielewski, Michael R. ^[1]; Poluektov, Oleg G. ^[2]; Freedman, Danna E. ^[1]

Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Quantum information processing (QIP) offers the potential to create new frontiers in fields ranging from quantum biology to cryptography. Two key figures of merit for electronic spin qubits, the smallest units of QIP, are the coherence time (T₂), the lifetime of the qubit, and the spin–lattice relaxation time (T₁), the thermally defined upper limit of T₂. To achieve QIP, processable qubits with long coherence times are required. Recent studies on (Ph₄P-d₂₀)₂[V(C₈S₈)₃], a vanadium-based qubit, demonstrate that millisecond T₂ times are achievable in transition metal complexes with nuclear spinfree environments. Applying these principles to vanadyl complexes offers a route to combine the previously established surface compatibility of the flatter vanadyl structures with a long T₂. Toward those ends, we investigated a series of four qubits, (Ph₄P)₂[VO(C₈S₈)₂] (1), (Ph₄P)₂[VO(β-C₃S₅)₂] (2), (Ph₄P)₂[VO(α-C₃S₅)₂] (3), and (Ph₄P)₂[VO(C₃S₄O)₂] (4), by pulsed electron paramagnetic resonance (EPR) spectroscopy and compared the performance of these species with our recently reported set of vanadium tris(dithiolene) complexes. Crucially we demonstrate that solutions of 1–4 in SO₂, a uniquely polar nuclear spinfree solvent, reveal T₂ values of up to 152(6) μs, comparable to the best molecular qubit candidates. Upon transitioning to vanadyl species from the tris(dithiolene) analogues, we observe a remarkable order of magnitude increase in T₂, attributed to stronger solute–solvent interactions with the polar vanadium-oxo moiety. Simultaneously, we detect a small decrease in T₂ for the vanadyl analogues relative to the tris(dithiolene) complexes. We attribute this decrease to the absence of one nuclear spinfree ligand, which served to shield the vanadium centers against solvent nuclear spins. Lastly, our results highlight new design principles for long T₁ and T₂ times by demonstrating the efficacy of ligand-based tuning of solute–solvent interactions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1351310

Journal Information:: Journal of the American Chemical Society, Vol. 138, Issue 44; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 92 works

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