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Anisotropic orbital occupation and Jahn-Teller distortion of orthorhombic YMnO3epitaxial films: A combined experimental and theoretical study on polarization-dependent x-ray absorption spectroscopy
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Anisotropic orbital occupation and Jahn-Teller distortion of orthorhombic YMnO3epitaxial films: A combined experimental and theoretical study on polarization-dependent x-ray absorption spectroscopy

S. C. Haw, J. M. Lee, S. A. Chen, K. T. Lu, P. A. Lin, C. H. Lee, M. T. Lee, T.W. Pi, Z. HuJ. M. Chen
The Journal of Chemical Physics The Journal of Chemical Physics, 卷.140(15), 頁碼.1-4
2014

摘要

Anisotropic orbital occupation;Jahn-Teller distortion;orthorhombic YMnO3;polarization-dependent x-ray absorption spectroscopy
The b-axis oriented orthorhombic YMnO3 (o-YMnO3) epitaxial films on a YAlO3 (010) substrate were fabricated with pulsed-laser deposition. The anisotropic orbital occupation and Jahn-Teller (JT) distortion of an o-YMnO3 film were investigated with polarization-dependent x-ray absorption spectra and configuration-interaction multiplet-cluster calculations. A significant energy difference, ∼3.8 eV, for the main white line along E//b and E//a in polarization-dependent Mn K-edge spectra of o-YMnO3 indicates an extraordinary JT distortion and significant anisotropic Mn–O bonding within the ab plane in the o-YMnO3 film. Most importantly, although the orbital occupation of 3d electrons in o-YMnO3 films is almost the same as that in single crystalline o-DyMnO3, the JT distortion of o-YMnO3 films is larger than that of single crystalline o-DyMnO3, deduced from the multiplet calculations. We speculate that this JT distortion predominantly contributes to the origin of the cycloidal spin deformation in bulk o-YMnO3, because of a suppressed nearest-neighbor superexchange interaction and an enhanced next-nearest-neighbor superexchange interaction. These complementary results provide insight into the origin of the E-type magnetic configuration of o-YMnO3.

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