Abstract
AbstractFrom low‐temperature Synchrotron X‐ray diffraction, a precise thermal characterization of octahedral distortions in single‐phase Ruddlesden‐Popper Ca3Mn2O7 is performed. Highly sensitive close‐steps temperature dependences of Mn‐O‐Mn bond angles connecting MnO6 octahedra clearly reveal the signature of spin ordering in the system. Spin‐lattice coupling is thus revealed via the structural distortions, responsible for the evolution of the magnetic state. Further, benchmark temperature anomalies observed in the unit cell volume and its polarization‐measure highlight the interplay between spin, lattice, and charge degrees of freedom. Strong spin‐lattice coupling is supported by the Raman spectroscopy results across the magnetic ordering. Dielectric study on Ca3Mn2O7 features relaxor‐like segmented dynamics below the antiferromagnetic ordering. Dipolar relaxations of different origins are spectrally resolved, exhibiting distinct H‐field alterations which identify their allegiance to different magnetic subphases. Dipole‐relaxation characteristics examined under applied magnetic field and the ensuing magneto‐dielectricity consistently correlate with the concurrent magnetic, structural, and vibrational features.
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