Electronic structure of YMn₂O₅ studied by EELS and first-principles calculations

Abstract

The electronic structure of multiferroic YMn₂O₅ material has been studied by use of the generalized gradient approximation (GGA). The results demonstrate that the oxygen 2p and manganese 3d orbitals are strongly hybridized. Considering the on-site Coulomb interaction U, we performed the GGA+U calculations for 0<U≤8 eV, and it is found that the increase of U could enlarge the band gap and, on the other hand, weaken the Mn–O hybridization. The experimental measurements of the electron energy-loss spectrometry (EELS) exhibit a rich variety of structural features in both O–K edge and Mn–L edges. A theoretical and experimental analysis on the O–K edge suggests that the on-site Coulomb interaction (U) in YMn₂O₅ could be less than 4 eV. Certain electronic structural features of LaMn₂O₅ have been discussed in comparison with those of YMn₂O₅.

Keywords

YMn₂O₅ / multiferroics / electron energy-loss spectra / electronic structure / GGA+U

References

[1] W. Eerenstein, N. D. Mathur, and J. F. Scott, Nature, 2006, 442: 759

[2] G. Catalan and J. F. Scott, Adv. Mater. (Deerfield Beach Fla.), 2009, 21: 2463

[3] N. Hur, S. Park, P. A. Sharma, J. S. Ahn, S. Guha, and S. W. Cheong, Nature, 2004, 429: 392

[4] N. Hur, S. Park, P. A. Sharma, S. Guha, and S. W. Cheong, Phys. Rev. Lett., 2004, 93: 107207

[5] C. R. dela Cruz, F. Yen, B. Lorenz, M. Gospodinov, C. Chu, W. Ratcliff, J. Lynn, S. Park, and S. W. Cheong, Phys. Rev. B, 2006, 73: 100406

[6] P. G. Radaelli, L. C. Chapon, A. Daoud-Aladine, C. Vecchini, P. J. Brown, T. Chatterji, S. Park, and S. W. Cheong, Phys. Rev. Lett., 2008, 101: 067205

[7] A. Munoz, J. A. Alonso, M. T. Casais, M. J. Martinez-Lope, J. L. Martinez, and M. T. Fernandez-Diaz, Eur. J. Inorg.Chem., 2005, 2005: 685

[8] C. Vecchini, L. Chapon, P. Brown, T. Chatterji, S. Park, S. W. Cheong, and P. Radaelli, Phys. Rev. B, 2008, 77: 134434

[9] C. Wang, G. C. Guo, and L. He, Phys. Rev. Lett., 2007, 99: 177202

[10] C. Wang, G. C. Guo, and L. He, Phys. Rev. B, 2008, 77: 134113

[11] L. C. Chapon, P. G. Radaelli, G. R. Blake, S. Park, and S. W. Cheong, Phys. Rev. Lett., 2006, 96: 097601

[12] R. Egerton, Electron Energy-Loss Spectroscopy in the Electron Microscope, New York and London: Plenum Press, 1996

[13] S. L. Dudarev, G. A. Botton, S. Y. Savrasov, Z. Szotek, W. M. Temmerman, and A. P. Sutton, Phys. Status Solidi (a), 1998, 166(1): 429

[14] R. Xiao, H. Yang, L. Xu, H. Zhang, Y. Shi, and J. Li, Solid State Commun., 2005, 135(11-12): 687

[15] G. Radtke, A. Saúl, H. Dabkowska, B. Gaulin, and G. Botton, Phys. Rev. B, 2008, 77: 125130

[16] C. Delacalle, J. Alonso, M. Martinezlope, M. Garciahernandez, and G. Andre, Mater. Res. Bull., 2008, 43(2): 197

[17] P. Blaha, K. Schwarz, G. K. H. Madsen, D. Kvasnicka, and J. Luitz, Karlheinz Schwarz, Techn. University Wien, Austria, 2001

[18] Z. Wu and R. E. Cohen, Phys. Rev. B, 2006, 73: 235116

[19] V. I. Anisimov, I. V. Solovyev, M. A. Korotin, M. T. Czyzyk, and G. A. Sawatzky, Phys. Rev. B, 1993, 48: 16929

[20] M. Nelhiebel, P. H. Louf, P. Schattschneider, P. Blaha, K. Schwarz, and B. Jouffrey, Phys. Rev. B, 1999, 59: 12807

[21] J. Titantah, K. Jorissen, and D. Lamoen, Phys. Rev. B, 2004, 69: 125406

[22] A. Moskvin and R. Pisarev, Phys. Rev. B, 2008, 77: 060102

[23] B. Rafferty and L. M. Brown, Phys. Rev. B, 1998, 58: 10326

[24] B. Rafferty, S. J. Pennycook, and L. M. Brown, J. Electron Microsc. (Tokyo), 2000, 49(4): 517

[25] M. Stöger-Pollach, Micron, 2008, 39(8): 1092

[26] J. Heyd, J. E. Peralta, G. E. Scuseria, and R. L. Martin, J. Chem. Phys., 2005, 123: 174101

[27] P. G. Radaelli, C. Vecchini, L. C. Chapon, P. J. Brown, S. Park, and S. W. Cheong, Phys. Rev. B, 2009, 79: 020404

[28] J. Koo, C. Song, S. Ji, J. S. Lee, J. Park, T. H. Jang, C. H. Yang, J. H. Park, Y. H. Jeong, K. B. Lee, T. Y. Koo, Y. J. Park, J. Y. Kim, D. Wermeille, A. I. Goldman, G. Srajer, S. Park, and S. W. Cheong, Phys. Rev. Lett., 2007, 99: 197601

[29] A. D. Becke and E. R. Johnson, J. Chem. Phys., 2006, 124: 221101

[30] F. Tran and P. Blaha, Phys. Rev. Lett., 2009, 102: 226401

[31] D. J. Singh, Phys. Rev. B, 2010, 82: 205102

[32] P. Rez and D. A.Muller, Annu. Rev. Mater. Res., 2008, 38(1): 535

[33] J. B. Neaton, D. A. Muller, and N. W. Ashcroft, Phys. Rev. Lett., 2000, 85: 1298

[34] F. M. F. De Groot, M. Grioni, J. C. Fuggle, J. Ghijsen, G. A. Sawatzky, and H. Petersen, Phys. Rev. B, 1989, 40: 5715

[35] N. Mannella, A. Rosenhahn, M. Watanabe, B. Sell, A. Nambu, S. Ritchey, E. Arenholz, A. Young, Y. Tomioka, and C. S. Fadley, Phys. Rev. B, 2005, 71: 125117

[36] D. K. Shukla, S. Mollah, R. Kumar, P. Thakur, K. H. Chae, W. K. Choi, and A. Banerjee, J. Appl. Phys., 2008, 104: 033707

[37] G. Giovannetti and J. van den Brink, Phys. Rev. Lett., 2008, 100: 227603

[38] F. Groot, Coord. Chem. Rev., 2005, 249(1-2): 31

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