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Crystals of the Fe-PNN-pincer complex [Fe(PNN- i Pr)Br 2 ]  1  (PNN- i Pr= N -(diisopropylphosphanyl)-6-[(isopropylamino)methyl]pyridin-2-amine) grown from a pentane/DCM mixture are made up of two independently diffracting domains with different stoichiometry,  viz.  1  [ P 2 1 / a ,  Z  = 4,  a  = 14.2995(10) Å,  b  = 11.8043(8) Å,  c  = 12.4229(8) Å,  β  = 93.618(4)°,  V  = 2092.8(2) Å 3 ] and its solvatomorph  1 ·DCM [ A 2/ a ,  Z  = 8,  a  = 14.2449(8) Å,  b  = 11.8208(8) Å,  c  = 30.091(2) Å,  β  = 111.501(4)°,  V  = 47142.3(5) Å 3 ] with a volume ratio of 64.30:35.70(9). Both domains belong to a family of merotypes (polysomes that feature one common layer). They contain equivalent  1  layers, which are intercalated in  1 ·DCM by solvent layers. The crystals are therefore an example of solvato-merotype-epitaxy. A crystal made up of only the solvate domain  1 ·DCM-d2 [ A 2/ a ,  Z  = 8,  a  = 14.2796(9) Å,  b  = 11.8868(7) Å,  c  = 29.9135(19) Å,  β  = 110.9847(8)°,  V  = 4740.7(5) Å 3 ] was grown from DCM-d2. An extension of the symmetry concepts of order-disorer (OD) theory to the more general case of merotypes or even polysomes is outlined.

[Fe(PNN- i Pr)Br 2 ]· x DCM: the first example of merotype-epitaxy of a molecular structure and its solvatomorph