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Polymorphic Imidoylamidinato Platinum(II) Complex That Exhibits Inverse Symmetry Breaking Induced by Both Pressure
Shinnosuke Horiuchi1,2, Kenichiro Omoto3, Ryo Kishikawa1
1Division of Chemistry and Materials Science, Graduate School of Engineering, Nagasaki University, 1-14 Bunkyo-machi, Nagasaki 852-8521, Japan.
None:
The temperature and pressure dependence of the crystal structures and photophysical properties of three crystalline polymorphs of imidoylamidinato Pt(II) complexes exhibiting green luminescence (UG form, main phase), yellow luminescence (UY form), and orange luminescence (UO form) under ambient temperature and pressure were investigated. While the UG and UO forms did not show phase transitions in the temperature range of 300-90 K and below 6.5 GPa (UG) or 3.2 GPa (UO), the UY form exhibited inverse symmetry breaking induced by temperature and pressure. Based on observations of temperature- and pressure-induced phase transition processes using single-crystal X-ray diffraction and optical microscopy, these phase transitions were confirmed to proceed in a single-crystal to single-crystal manner via a twinning deformation process, in which multiple structural domains corresponding to different phases coexisted simultaneously within individual crystal particles during the transformation. It was revealed that, in the UY form, the strength of the interaction between BF4- ions and complex cations changes with temperature and pressure. This triggers a phase transition by inducing alterations in the arrangement of complex cations and counter-anions. In terms of contracting the crystal lattice, the effects of cooling and pressurization are similar. However, observing different luminescence behaviors in the UO and UY forms under temperature and pressure changes revealed that temperature and pressure do not necessarily have consistent effects on the stability of the excited state.
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