Metal-ligand covalency enables room temperature molecular qubit candidates

Chemical Science
Majed S FataftahDanna E Freedman

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).

References

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Citations

Feb 15, 2020·Chemical Communications : Chem Comm·Ivana BorilovicGuillem Aromí
Jun 27, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Daniel Aravena, Eliseo Ruiz
Mar 27, 2020·Physical Chemistry Chemical Physics : PCCP·Ruben Mirzoyan, Ryan G Hadt
Dec 19, 2019·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Ivan V KurganskiiMatvey V Fedin
Jan 13, 2021·Physical Chemistry Chemical Physics : PCCP·Martín AmozaEliseo Ruiz
Dec 17, 2020·Chemical Reviews·Kade Head-MarsdenPrineha Narang
Apr 21, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Stephen Sproules
May 6, 2021·Chemical Society Reviews·Cassidy E JacksonJoseph M Zadrozny
Jun 4, 2021·ACS Central Science·Chung-Jui YuDanna E Freedman
Aug 13, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·David AguilàGuillem Aromí
Nov 20, 2020·Journal of the American Chemical Society·Majed S FataftahDanna E Freedman
Aug 14, 2020·Journal of the American Chemical Society·Michael K WojnarDanna E Freedman
Oct 8, 2021·Journal of the American Chemical Society·Nathanael P KazmierczakRyan G Hadt
Sep 29, 2021·Chemistry : a European Journal·Martín AmozaEliseo Ruiz
Nov 25, 2021·Journal of the American Chemical Society·Daniel W LaorenzaDanna E Freedman

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Methods Mentioned

BETA
electron paramagnetic resonance
saturation
saturation recovery

Software Mentioned

Easyspin

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