TY - JOUR
T1 - Metal-ligand covalency enables room temperature molecular qubit candidates
AU - Fataftah, Majed S.
AU - Krzyaniak, Matthew D.
AU - Vlaisavljevich, Bess
AU - Wasielewski, Michael R.
AU - Zadrozny, Joseph M.
AU - Freedman, Danna E.
N1 - Funding Information:
We thank S. C. Coste, K. A. Collins, and D. W. Laorenza for helpful discussions and experimental assistance. This work was supported by Northwestern University, the State of Illinois, the Institute for Sustainability and Energy at Northwestern University, and the National Science Foundation CAREER Award No. CHE-1455017. (M. S. F., J. M. Z, and D. E. F.) and Award No. CHE-1565925 (M. R. W.). All synthetic work on qubit design was supported by CHE-1455017. X-ray crystallography was performed at the IMSERC at Northwestern University, which has received support from the So and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNC).
Publisher Copyright:
© The Royal Society of Chemistry 2019.
PY - 2019
Y1 - 2019
N2 - 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).
AB - 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).
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U2 - 10.1039/c9sc00074g
DO - 10.1039/c9sc00074g
M3 - Article
AN - SCOPUS:85068862103
SN - 2041-6520
VL - 10
SP - 6707
EP - 6714
JO - Chemical Science
JF - Chemical Science
IS - 27
ER -