Magnetic Hysteresis at 31 K in a Four-Coordinate Dysprosium(III) Amide Complex

<p dir="ltr">Supporting data for: 10.1021/jacs.5c13255.</p><p dir="ltr">Contains raw files for: ATR-IR, Luminescence, NMR, PXRD, SQUID magnetometry, UV-Vis-NIR data, and processed SC-XRD data.</p><p dir="ltr">Manuscript abstract:</p><p dir="ltr">The state-of-the-art in single-molecule magnet (SMM) design is dominated by charged dysprosium sandwich complexes with mono- or dianionic π-ligands and which exhibit some of the highest open-loop magnetic hysteresis temperatures (<i>T</i>_H), the highest 100 s blocking temperatures (<i>T</i>_B100) and some of the largest barriers to magnetic reversal (<i>U</i>_eff).

Architectures that leverage more charge-dense ligands, such as amides or alkoxides, with axial coordination and weak equatorial interactions can generate larger crystal fields (CFs), and hence larger <i>U</i>_eff values; however, this is often not accompanied by correspondingly high <i>T</i>_H or <i>T</i>_B100 values. Here we report a four-coordinate dysprosium(III) single-molecule magnet, [Dy{Me₂Si(NSi<i>i</i>Pr₃)₂}₂{K(toluene)₂}]_n (<b>1Dy</b>), with charge-dense amide donors, but a coordination environment that is between axial and tetrahedral in structure.