Metal-ligand covalency enables room temperature molecular qubit candidates

Majed S. Fataftah, Matthew D. Krzyaniak, Bess Vlaisavljevich, Michael R Wasielewski, Joseph M. Zadrozny, Danna E. Freedman

Research output: Contribution to journalArticle

Abstract

Harnessing synthetic chemistry to design electronic spin-based qubits, the smallest unit of a quantum information system, enables us to probe fundamental questions regarding spin relaxation dynamics. We sought to probe the influence of metal-ligand covalency on spin-lattice relaxation, which comprises the upper limit of coherence time. Specifically, we studied the impact of the first coordination sphere on spin-lattice relaxation through a series of four molecules featuring V-S, V-Se, Cu-S, and Cu-Se bonds, the Ph4P+ salts of the complexes [V(C6H4S2)3]2- (1), [Cu(C6H4S2)2]2- (2), [V(C6H4Se2)3]2- (3), and [Cu(C6H4Se2)2]2- (4). The combined results of pulse electron paramagnetic resonance spectroscopy and ac magnetic susceptibility studies demonstrate the influence of greater M-L covalency, and consequently spin-delocalization onto the ligand, on elongating spin-lattice relaxation times. Notably, we observe the longest spin-lattice relaxation times in 2, and spin echos that survive until room temperature in both copper complexes (2 and 4).

Original languageEnglish
Pages (from-to)6707-6714
Number of pages8
JournalChemical Science
Volume10
Issue number27
DOIs
Publication statusPublished - Jan 1 2019

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Spin-lattice relaxation
Metals
Ligands
Relaxation time
Temperature
Magnetoelectronics
Magnetic susceptibility
Paramagnetic resonance
Copper
Information systems
Salts
Spectroscopy
Molecules

ASJC Scopus subject areas

  • Chemistry(all)

Cite this

Fataftah, M. S., Krzyaniak, M. D., Vlaisavljevich, B., Wasielewski, M. R., Zadrozny, J. M., & Freedman, D. E. (2019). Metal-ligand covalency enables room temperature molecular qubit candidates. Chemical Science, 10(27), 6707-6714. https://doi.org/10.1039/c9sc00074g

Metal-ligand covalency enables room temperature molecular qubit candidates. / Fataftah, Majed S.; Krzyaniak, Matthew D.; Vlaisavljevich, Bess; Wasielewski, Michael R; Zadrozny, Joseph M.; Freedman, Danna E.

In: Chemical Science, Vol. 10, No. 27, 01.01.2019, p. 6707-6714.

Research output: Contribution to journalArticle

Fataftah, MS, Krzyaniak, MD, Vlaisavljevich, B, Wasielewski, MR, Zadrozny, JM & Freedman, DE 2019, 'Metal-ligand covalency enables room temperature molecular qubit candidates', Chemical Science, vol. 10, no. 27, pp. 6707-6714. https://doi.org/10.1039/c9sc00074g
Fataftah MS, Krzyaniak MD, Vlaisavljevich B, Wasielewski MR, Zadrozny JM, Freedman DE. Metal-ligand covalency enables room temperature molecular qubit candidates. Chemical Science. 2019 Jan 1;10(27):6707-6714. https://doi.org/10.1039/c9sc00074g
Fataftah, Majed S. ; Krzyaniak, Matthew D. ; Vlaisavljevich, Bess ; Wasielewski, Michael R ; Zadrozny, Joseph M. ; Freedman, Danna E. / Metal-ligand covalency enables room temperature molecular qubit candidates. In: Chemical Science. 2019 ; Vol. 10, No. 27. pp. 6707-6714.
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