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The emergence of Griffiths phase in CaCu3Ti(4−x)MnxO12 (CCTMO, x = 1, 2 and 3) geometrically frustrated antiferromagnetic complexes perovskite

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Abstract

In this work, we have reported the rare coexistence of a Griffiths phase (GP) in a complex perovskite oxide with geometrically frustrated antiferromagnetism. We have achieved this by substituting Manganese (Mn) in the titanium site of CaCu3Ti(4−x)MnxO12 (CCTMO, x = 1, 2 and 3). The occurrence of a Griffiths phase is observed when a strong contest between antiferromagnetic transition (TN) and paramagnetic (PM) occurs in the magnetic domain. As we increased the molar concentration of Manganese while substituting at titanium site in CaCu3Ti4O12, we observed the appearance of a step-like Griffiths phase. Manganese (Mn)-substituted materials exhibit paramagnetic (PM) to ferromagnetic (FM) phase transitions below CaCu3Ti3Mn1O12 (CCTM1O), CaCu3Ti2Mn2O12 (CCTM2O), and CaCu3Ti1Mn3O12 (CCTM3O), marked by a rapid step-like change in the magnetic moment due to spin ordering. The deviation of inverse magnetic susceptibility (χ−1) from Curie–Weiss behavior occurs in the temperature ranges of 75 to 190 K, 80 to 200 K, and 150 to 280 K, respectively. The emergence of the Griffiths phase before the actual PM–FM transition indicates that the inhomogeneous phase above the Curie temperature (TC), which can be defined as a Griffiths phase, is dominated by ferromagnetic interactions rather than antiferromagnetic ones. The presence of a Griffiths-like phase beyond its Curie temperature (TC) is indicated by low-field DC magnetization of the nanostructures, showing abnormal magnetic behavior. The presence of short-range magnetic correlations and ferromagnetic clusters in the system due to the size decrease is linked to this unexpected behaviour.

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Acknowledgements

Vinod Kumar thanks the Head, Department of Chemistry, IIT (BHU) Varanasi, India, for providing financial assistance as a Teaching Assistantship.The authors are grateful to the Incharge, CIFC, and IIT (BHU) Varanasi, for providing HR-SEM, and XPS facilities.

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Authors and Affiliations

  1. Department of Chemistry, Indian Institute of Technology (Banaras Hindu University), Varanasi, Uttar Pradesh, 221005, India

    Vinod Kumar, Anup Kumar, Shruti Singh, Manish Kumar Verma, Vishnu Shankar Rai, Dhanesh Tiwary & K. D. Mandal

  2. Department of Chemistry, Banaras Hindu University, Varanasi, Uttar Pradesh, 221005, India

    Krishna Kumar

  3. Department of Physics, Indian Institute of Technology (Banaras Hindu University), Varanasi, Uttar Pradesh, 221005, India

    Gurudeo Nirala & Shail Upadhyay

  4. Department of Physics, University of Allahabad, Prayagraj, 211002, India

    Navneet Yadav

  5. Department of Chemistry and Biochemistry and Computer Science and Electrical Engineering, University of Maryland, Baltimore County, 1000 Hilltop Circle, Baltimore, MD, 21250, USA

    N. B. Singh

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Kumar, V., Kumar, A., Singh, S. et al. The emergence of Griffiths phase in CaCu3Ti(4−x)MnxO12 (CCTMO, x = 1, 2 and 3) geometrically frustrated antiferromagnetic complexes perovskite. J Mater Sci: Mater Electron 35, 136 (2024). https://doi.org/10.1007/s10854-024-11930-z

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