Orbital ordering and ultrafast carrier dynamics anisotropies in orientation-engineered orthorhombic YMnO3 films

材料科学 正交晶系 凝聚态物理 各向异性 结晶学 离子半径 线性二色性 晶体结构 离子 光学 化学 物理 圆二色性 有机化学
作者
My Ngoc Duong,Yu-Xun Chen,Wen‐Yen Tzeng,Tahta Amrillah,Song Yang,Cheng‐En Liu,Dimitre Dimitrov,Shu‐Chih Haw,Chia‐Hung Hsu,Jin‐Ming Chen,J.‐Y. Lin,Kaung‐Hsiung Wu,Chih‐Wei Luo,Chien‐Te Chen,Chang‐Yang Kuo,Jenh‐Yih Juang
出处
期刊:APL Materials [American Institute of Physics]
卷期号:12 (2)
标识
DOI:10.1063/5.0188612
摘要

The rich physical properties unveiled in a plethora of transition and rare-earth metal oxides have been attributed to the intricate interplays between the orbital, charge, and spin degrees of freedom. Among them, rare-earth manganites (RMnO3) have been attracting tremendous attention owing to the ionic size-induced lattice distortion dictated by the Goldschmidt tolerance factor and the substantial Jahn–Teller distortion unique to Mn3+ ions, which evidently have resulted in a variety of emergent characteristics in electronic, magnetic, and orbital ordering. In this work, we deliberately engineered the orientation of a series of orthorhombic YMnO3 (o-YMO) films grown on SrTiO3(100) [STO(100)] and SrTiO3(110) [STO(110)] substrates by means of pulsed laser deposition. The x-ray diffraction (XRD) and reciprocal space mapping revealed that o-YMO/STO(100) is c-axis-oriented and o-YMO/STO(110) is a-axis-oriented, respectively. The XRD ϕ-scans further indicate that both films have excellent in-plane crystallinity, allowing the exploration of anisotropies along the respective crystallographic orientations. Indeed, the x-ray absorption linear dichroism spectroscopy taken along the respective crystallographic orientations evidently exhibited substantial anisotropy. Theoretical fitting with configuration interaction cluster calculations suggests that the d3z2−r2 orbitals are parallel to YMO[001]/(100), leading to stronger electron scattering along the c-axis. Independent polarization-dependent Δ R/R spectra obtained using the femtosecond pump–probe method exhibited substantial anisotropic behaviors in carrier relaxation dynamics when probing along different crystallographic orientations, presumably due to orbital ordering anisotropies.

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