Unusual butterfly-shaped magnetization signals and spin-glass-like behaviour in highly oriented pyrolytic graphite

We report a novel investigation on the relationship between magnetic-ordering and graphitic-structure in highly-oriented-pyrolytic-graphite (HOPG). By employing orientation-dependent-X-ray-diffraction, Raman-spectroscopy and temperature-dependent-superconductive-quantum-interference-device (T-SQUID) we examined the presence of ferromagnetic- and superconductive-ordering in HOPG systems with 1) disordered (HOPG1, containing carbon-vacancy-rich weak-Bernal-stacking and Moiré-superlattices with θmisfit ∼ 0.5°) and 2) ordered (HOPG2, containing higher-degree of Bernal-stacking and Moiré-superlattices with θmisfit ∼ 0.5°, 0.8°, 11°) graphitic-layer-arrangement. A perfect-HOPG is expected to exhibit a diamagnetic-response to an applied-magnetic-field. Instead, additional 1) ferromagnetic-signals presenting a characteristic width-enhancement with the field increasing in HOPG1 and 2) complex butterfly-shaped ferromagnetic signals in HOPG2, are demonstrated. Temperature-dependent-magnetometry evidenced further the presence of randomly oriented ferromagnetic clusters originating from topological disorder in both HOPG1 and HOPG2. These magnetic signals were explained on the basis of the percolative-type model.