Spins in molecules are particularly attractive targets for next-generation quantum technologies, enabling chemically programmable qubits and potential for scale-up via self-assembly. Here we report the observation of one of the largest hyperfine interactions for a molecular system, A = 3,467 ± 50 MHz, as well as a very large associated clock transition. This is achieved through chemical control of the degree of s-orbital mixing into the spin-bearing d orbital associated with a series of spin-½ La(II) and Lu(II) complexes.
View Article and Find Full Text PDFThe utility of the bulky aryloxide ligands 2,6-Ad-4-Me-CHO (ArO) and 2,6-Ad-4--Bu-CHO (ArO; Ad = 1-adamantyl) for stabilizing the Y(II) ion is reported and compared with the results with 2,6--Bu-4-Me-CHO (Ar'O). In contrast to the reduction product obtained from reducing Y(OAr') with potassium graphite, which is only stable in solution for 60 s at room temperature, KC reduction of Y(OAr) in THF in the presence of 2.2.
View Article and Find Full Text PDFThe possibility that the relative reactivity of complexes of actinide metals in the +2 and +3 oxidation states could be investigated by examining reactions between An and An species of Th and U with rare-earth metal reagents that provide EPR confirmation of electron transfer reactivity has been explored. Neither Cp'' Th nor Cp'' U will reduce Cp'' La or Cp' Y (Cp'=C H SiMe , Cp''=C H (SiMe ) ). However, both [K(2.
View Article and Find Full Text PDFThe suitability of aryloxide ligands for stabilizing +2 oxidation states of Sc and Y has been examined and EPR evidence indicating the first O-donor complexes of Sc and Y has been obtained, as well as an X-ray crystal structure of a Sc aryloxide complex. The trivalent rare-earth metal aryloxide precursors, Ln(OAr') , 1-Ln (Ln=Sc, Y, Gd, Dy, Ho, Er; OAr'=OC H tBu -2,6-Me-4), were synthesized from the corresponding rare-earth metal trichlorides and LiOAr'⋅OEt . Reduction of THF solutions of 1-Ln with potassium graphite in the presence of 2.
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