Borohydride as Magnetic Superexchange Pathway in Late Lanthanide Borohydrides

The magnetic characteristics of a series of borohydride‐based systems, including binary α‐/β‐Ln(BH 4 ) 3 phases (Ln = Gd, Tb, Dy, Ho, Er, and Tm) with direct Ln–HBH–Ln bridges and selected mixed‐metal systems, LiYb(BH 4 ) 4 , NaYb(BH 4 ) 4 , KHo(BH 4 ) 4 , RbTm(BH 4 ) 4 , with isolated Ln 3+ ions embedded in [Ln(BH 4 ) 4 ] – anions are described for the first time using SQUID magnetometry and DFT+U calculations. Crystal field effects as well as...