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Title: Long coherence times in nuclear spin-free vanadyl qubits [Long coherence times in surface-compatible nuclear spin-free vanadium qubits]

Abstract

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, (Ph 4P) 2[VO(C 8S 8) 2] (1), (Ph 4P) 2[VO(β-C 3S 5) 2] (2), (Ph 4P) 2[VO(α-C 3S 5) 2] (3), and (Ph 4P) 2[VO(C 3S 4O) 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 SO 2, a uniquely polar nuclear spinfree solvent, reveal T2 values of up tomore » 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 12, 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.« less

Authors:
 [1];  [1];  [1];  [2];  [1];  [1];  [2];  [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1351310
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 44; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 97 MATHEMATICS AND COMPUTING; pulsed EPR; quantum computing; quantum information processing; qubits; relaxation

Citation Formats

Yu, Chung -Jui, Graham, Michael J., Zadrozny, Joseph M., Niklas, Jens, Krzyaniak, Matthew D., Wasielewski, Michael R., Poluektov, Oleg G., and Freedman, Danna E. Long coherence times in nuclear spin-free vanadyl qubits [Long coherence times in surface-compatible nuclear spin-free vanadium qubits]. United States: N. p., 2016. Web. doi:10.1021/jacs.6b08467.
Yu, Chung -Jui, Graham, Michael J., Zadrozny, Joseph M., Niklas, Jens, Krzyaniak, Matthew D., Wasielewski, Michael R., Poluektov, Oleg G., & Freedman, Danna E. Long coherence times in nuclear spin-free vanadyl qubits [Long coherence times in surface-compatible nuclear spin-free vanadium qubits]. United States. doi:10.1021/jacs.6b08467.
Yu, Chung -Jui, Graham, Michael J., Zadrozny, Joseph M., Niklas, Jens, Krzyaniak, Matthew D., Wasielewski, Michael R., Poluektov, Oleg G., and Freedman, Danna E. Mon . "Long coherence times in nuclear spin-free vanadyl qubits [Long coherence times in surface-compatible nuclear spin-free vanadium qubits]". United States. doi:10.1021/jacs.6b08467. https://www.osti.gov/servlets/purl/1351310.
@article{osti_1351310,
title = {Long coherence times in nuclear spin-free vanadyl qubits [Long coherence times in surface-compatible nuclear spin-free vanadium qubits]},
author = {Yu, Chung -Jui and Graham, Michael J. and Zadrozny, Joseph M. and Niklas, Jens and Krzyaniak, Matthew D. and Wasielewski, Michael R. and Poluektov, Oleg G. and Freedman, Danna E.},
abstractNote = {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 12, 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.},
doi = {10.1021/jacs.6b08467},
journal = {Journal of the American Chemical Society},
number = 44,
volume = 138,
place = {United States},
year = {2016},
month = {10}
}

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