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The complex [NiL 2 (NCS) 2 ] ( 1 ), L =  N , N -dimethyl-l,3-propanediamine, exhibits thennochromic solid state phase transition (temperature range 383 K–397.5 K) producing a high temperature isomer [NiL 2 (NCS) 2 ] ( 2 ). The crystal structure of ( 2 ) has been solved by the X-ray powder as well as single crystal data sets and the precision of the structure determined with the X-ray single crystal diffraction data is higher than that obtained from the powder diffraction data. The triclinic unit cell of ( 2 ) having a volume approximately double to that of ( 1 ) consists of two symmetrically independent octahedral [NiL 2 (NCS) 2 ] complexes with the metal atoms lying at (0 0 0) and (0 1/2 1/2), respectively. The equatorial planes around the two metal centers in isomer ( 2 ) are inclined to each other by 155.8(2)°. With the decrease of the specific volume per molecule of [NiL 2 (NCS) 2 ] on isomerization ( 1  →  2 ) and significant changes in the molecular packing of the two isomers ( 1 ) and ( 2 ), the possible way of phase transition ( 1  →  2 ) is through a break up of the crystal body of isomer ( 1 ) and recrystallization into isomer ( 2 ).

Structure and isomerization in N , N -dimethyl-l,3-propanediamine nickel(II) thiocyanate