“…Although [M(L) 2 (NO 3 )][2(NO 3 )], M 2:1, have likely been synthesized for M = Am in the past, 19,22 single crystals have never been isolated and characterized by X-ray diffraction until now. Similar compounds containing 2,6-[Ph 2 P(O)CH 2 ] 2 C 5 H 3 −NO, L, or analogous ligands with para alkyl groups, 29 trifluoromethyl groups, 26 tolyl groups, 28 benzyl groups, 28 ethyl groups, 28 cyclohexyl groups, 31 and more recently diethylcarbamoyl groups 1,30 have been structurally characterized when the metal center is a lanthanide. Here, we were able to consistently produce pure crystalline batches of M 2:1, for M = Eu, Eu 2:1; Nd, Nd 2:1; and Am, Am 2:1, (Figure 2) by reacting 2 or more equiv of L with 1 equiv of the f element precursor in a 1:1 CHCl 3 /EtOH solution, as confirmed by CHN elemental analysis for all except the Amcontaining species.…”