“…Lanthanide (Ln) molecular materials have attracted strong interest and have been intensively studied in a wide range of areas such as catalysis, [1][2][3][4][5] bioinorganic chemistry, 6,7 Magnetic Resonance Imaging, [8][9][10] luminescent materials, [11][12][13][14] multimodal imaging probes, [15][16][17] Single-Molecule Magnets (SMMs) [18][19][20][21] and Quantum Information Processing (QIP). [22][23][24][25][26][27][28][29][30][31][32][33][34] Many of the interesting properties of Ln complexes originate from their special electronic structure, where the 4f subshell is shielded from the environment by the 5s and 5p orbitals. 35 For example, this results in a large unquenched orbital-angular momentum which has been essential to build SMMs [36][37][38] with record blocking temperatures, [39][40][41] and leads to sharp absorption and emission bands, due to the lower inuence of vibrations on the f-f transitions.…”