Cu(tn)Cl2 belongs to family of molecular magnets
with
low-dimensional magnetism mediated by hydrogen bonds. Here, the X-ray
diffraction, electron paramagnetic resonance, specific heat measurements,
and ab initio calculations performed within the framework of density
functional theory have been employed to investigate the structural
phase transition in Cu(tn)Cl2. Satellite reflections in
the X-ray diffraction pattern from single crystals, visible anomaly
in the specific heat measured in a zero magnetic field, rapid growth
of the EPR resonance line width, along with the increase of the g-factors
in the vicinity of 160 K are indicative of the structural phase transition
in Cu(tn)Cl2. Our results reveal that this system undergoes
transition from a disordered structure of the Pnma symmetry to a modulated structure with the Pnma(0β0)s00 superspace group. The transition
is reversible and driven by the reorientation of the diaminopropane
ligands. The density functional theory studies support results of
our specific heat measurements.