A First-Principles Study of Structure-Property Correlation and the Origin of Ferrimagnetism in Gallium Ferrite

Amritendu Roy, Ashish Garg, Rajendra Prasad, Sushil Auluck

Department of Materials Science and Engineering.
Department of Physics Indian Institute of Technology Kanpur Kanpur, India – 208016.
National Physical Laboratory Dr. K. S. Krishnan Marg, New Delhi, India-110012.

DOI: 10.4236/ampc.2012.24B001                

Abstract

A first-principles study of structure property correlation and the origin of ferrimagnetism is presented based on LSDA+U method. In particular, the results for the ground state structure, electronic band structure, density of states, Born effective charges, spontaneous polarization and cationic disorder are discussed. The calculations were done using Vienna ab-initio simulation package (VASP) with projector augmented wave method. We find that the ground state structure is orthorhombic and insulating having A-type antiferromagnetic spin configuration. The cationic disorder is found to play an important role. Although the cationic site disorder is not spontaneous in the ground state, interchange of octahedrally coordinated Ga2 and Fe2 sites is most favored. We find that ferrimagnetism  in gallium ferrite is primarily due to this exchange between Ga-Fe sites  such that Fe spins at Ga1 and Ga2 sites are antiferromagnetically aligned  while maintaining ferromagnetic coupling between Fe spins at Ga1 and Fe1  sites as well as between Fe spins at Ga2 and Fe2 sites. Further, the partial density of states shows noticeable hybridization of Fe 3d, Ga 4s,  Ga 4p and O 2p states indicating some covalent character of Ga/Fe-O bonds.  However, the charge density and electron localization functions show largely the ionic character of these bonds. Our calculation predicts spontaneous polarization of ~59 μC/cm² along b-axis.

Keywords

Gallium Ferrite; LSDA+U; Spontaneous Polarization; Ferrimagnetism; Cation Site Disorder

Conflicts of Interest

The authors declare no conflicts of interest.

References

[1]	T. Arima, D. Higashiyama, Y. Kaneko, J. P. He, T. Goto, S. Miyasaka, T. Kimura, K. Oikawa, T. Kamiyama, R. Kumai, and Y. Tokura, Physical Review B 70 (6), 064426 (2004).
[2]	J. P. Remeika, Journal of Applied Physics 31 (5), S263 (1960).
[3]	C. H. Nowlin and R. V. Jones, Journal of Applied Physics 34 (4), 1262 (1963).
[4]	M. B. Mohamed, A. Senyshyn, H. Ehrenberg, and H. Fuess, Journal of Alloys and Compounds 492 (1-2), L20.
[5]	W. Kim, J. H. We, S. J. Kim, and C. S. Kim, Journal of Applied Physics 101 (9), 09M515 (2007).
[6]	Y. Kaneko, T. Arima, J. P. He, R. Kumai, and Y. Tokura, Journal of Magnetism and Magnetic Materials 272-276 (Part 1), 555 (2004).
[7]	S. Mukherjee, A. Garg, and R. Gupta, Journal of Physics: Condensed Matter 23 (44), 445403 (2011).
[8]	R. B. Frankel, N. A. Blum, S. Foner, A. J. Freeman, and M. Schieber, Physical Review Letters 15 (25), 958 (1965).
[9]	D. L. White, Bull. Am. Phys. Soc. 5, 189 (1960).
[10]	S. C. Abrahams and J. M. Reddy, Physical Review Letters 13 (23), 688 (1964).
[11]	G. Kresse and D. Joubert, Physical Review B 59 (3), 1758 (1999).
[12]	P. E. Blochl, Physical Review B 50 (24), 17953 (1994).
[13]	W. Kohn and L. J. Sham, Physical Review 140 (4A), A1133 (1965).
[14]	V. I. Anisimov, F. Aryasetiawan, and A. I. Lichtenstein, Journal of Physics: Condensed Matter 9 (4), 767 (1997).
[15]	H. J. Monkhorst and J. D. Pack, Physical Review B 13 (12), 5188 (1976).
[16]	R. D. King-Smith and D. Vanderbilt, Physical Review B 47 (3), 1651 (1993).
[17]	M. J. Han, T. Ozaki, and J. Yu, Physical Review B 75 (6), 060404 (2007).
[18]	S. C. Abrahams, J. M. Reddy, and J. L. Bernstein, The Journal of Chemical Physics 42 (11), 3957 (1965).
[19]	J. B. Goodenough, Physical Review 100 (2), 564 (1955).
[20]	Z. H. Sun, S. Dai, Y. L. Zhou, L. Z. Cao, and Z. H. Chen, Thin Solid Films 516 (21), 7433 (2008).
[21]	A. Roy and et al., Journal of Physics: Condensed Matter 22 (16), 165902 (2010).
[22]	S. Chen, X. G. Gong, A. Walsh, and S.-H. Wei, Applied Physics Letters 94 (4), 041903 (2009).
[23]	A. Savin, R. Nesper, S. Wengert, and T. F. Fassler, Angewandte Chemie International Edition in English 36 (17), 1808 (1997).
[24]	A. Roy, S. Mukherjee, R. Gupta, S. Auluck, R. Prasad, and A. Garg, Journal of Physics: Condensed Matter 23 (32), 325902 (2011).
[25]	A. Roy, R. Prasad, S. Auluck, and A. Garg, Journal of Applied Physics 111 (4), 043915 (2012).
[26]	R. E. Cohen, in Piezoelectricity (Springer Berlin Heidelberg, 2008), Vol. 114, pp. 471.