Anisotropic orbital occupation and Jahn-Teller distortion of orthorhombic YMnO{sub 3} epitaxial films: A combined experimental and theoretical study on polarization-dependent x-ray absorption spectroscopy

Journal Article · Mon Apr 21 00:00:00 EDT 2014 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4871114· OSTI ID:22254156

Haw, Shu-Chih; Chen, Shin-Ann ^[1]; Lee, Jenn-Min; Lu, Kueih-Tzu; Lee, Ming-Tao; Pi, Tun-Wen; Chen, Jin-Ming ^[2]; Lin, Pao-An ^[3]; Lee, Chih-Hao ^[1]; Hu, Zhiwei ^[4]

---

1. Department of Engineering and System Science, National Tsing Hua University, 30013 Hsinchu, Taiwan (China)
2. National Synchrotron Radiation Research Center (NSRRC), 101 HsinAnn Road, 30076 Hsinchu, Taiwan (China)
3. Department of Physics, National Tsing Hua University, 30013 Hsinchu, Taiwan (China)
4. Max Planck Institute for Chemical Physics of Solids, Nöthnitzer Straße 40, 01187 Dresden (Germany)

The b-axis oriented orthorhombic YMnO{sub 3} (o-YMnO{sub 3}) epitaxial films on a YAlO{sub 3} (010) substrate were fabricated with pulsed-laser deposition. The anisotropic orbital occupation and Jahn-Teller (JT) distortion of an o-YMnO{sub 3} 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-YMnO{sub 3} indicates an extraordinary JT distortion and significant anisotropic Mn–O bonding within the ab plane in the o-YMnO{sub 3} film. Most importantly, although the orbital occupation of 3d electrons in o-YMnO{sub 3} films is almost the same as that in single crystalline o-DyMnO{sub 3}, the JT distortion of o-YMnO{sub 3} films is larger than that of single crystalline o-DyMnO{sub 3}, deduced from the multiplet calculations. We speculate that this JT distortion predominantly contributes to the origin of the cycloidal spin deformation in bulk o-YMnO{sub 3}, 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-YMnO{sub 3}.

• OSTI ID: 22254156
• Journal Information: Journal of Chemical Physics, Vol. 140, Issue 15; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
ABSORPTION SPECTROSCOPY
ENERGY BEAM DEPOSITION
EPITAXY
FILMS
JAHN-TELLER EFFECT
LASER RADIATION
MONOCRYSTALS
ORTHORHOMBIC LATTICES
POLARIZATION
SUBSTRATES
X-RAY SPECTRA
X-RAY SPECTROSCOPY