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<p>The direct experimental probing and detailed imaging of octahedral tilt, along with the control of magnetic ground state and spin-orbit occupancies in an artificially engineered heterointerface through the strain manipulation via interface engineering, is the long-standing challenging issue addressed here. We introduce an innovative methodology to measure the projected O-O-O angles (O-O-O<sub>proj</sub>) between the neighboring in-plane BO<sub>6</sub> octahedra of perovskite oxide (ABO<sub>3</sub>), demonstrating a precise quantification of strain-manipulated octahedral tilt in atomically engineered LaCoO<sub>3</sub> (LCO)/La<sub>0.7</sub>Sr<sub>0.3</sub>MnO<sub>3</sub> (LSMO) bilayer interfaces. The pronounced octahedral tilt on SrTiO<sub>3</sub> (STO) substrate (tensile strain) compared to LaAlO<sub>3</sub> (LAO) substrate (compressive strain) correlates to the magnetism especially within the framework of bond angle geometry and spin-charge-orbital reconstructions, contrasting with individual single-phase films. Interfacial orbital reconstruction, Co/Mn antiferromagnetic coupling and their strain manipulation are quantified through X-ray linear dichroism (XLD) and X-ray magnetic circular dichroism (XMCD) measurements, further confirmed by both molecular orbital theory and Goodenough-Kanamori-Anderson rules. First principles calculations unveil a higher (lower) magnetic moment of individual magnetic atoms with tensile (compressive) strain, including unusual interfacial antiferromagnetism arising <i>d</i>-orbital occupations, and bond angle geometry. This endeavor paves a potential method to manipulate the octahedral tilt to tailor emergent phenomena at heterointerfaces via atomically precise strain-interface engineering.</p>

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An unconventional pathway to correlate the octahedral tilt coupling and spin-orbit reconstruction at oxide interfaces

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月15日

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  • Jayjit Kumar Dey,
  • Koushik Jagadish,
  • Arka Bandyopadhyay,
  • Sourav Chowdhury,
  • Moritz Hoesch,
  • Manuel Valvidares,
  • Anju Ahlawat,
  • Feras Afaneh,
  • Aryan Keshri,
  • Basanta Roul,
  • Saluru Baba Krupanidhi,
  • Mukul Gupta,
  • Ram Janay Choudhary,
  • Thirumalai Venkatesan,
  • Awadhesh Narayan,
  • N. Ravishankar,
  • Sujit Das

摘要

The direct experimental probing and detailed imaging of octahedral tilt, along with the control of magnetic ground state and spin-orbit occupancies in an artificially engineered heterointerface through the strain manipulation via interface engineering, is the long-standing challenging issue addressed here. We introduce an innovative methodology to measure the projected O-O-O angles (O-O-Oproj) between the neighboring in-plane BO6 octahedra of perovskite oxide (ABO3), demonstrating a precise quantification of strain-manipulated octahedral tilt in atomically engineered LaCoO3 (LCO)/La0.7Sr0.3MnO3 (LSMO) bilayer interfaces. The pronounced octahedral tilt on SrTiO3 (STO) substrate (tensile strain) compared to LaAlO3 (LAO) substrate (compressive strain) correlates to the magnetism especially within the framework of bond angle geometry and spin-charge-orbital reconstructions, contrasting with individual single-phase films. Interfacial orbital reconstruction, Co/Mn antiferromagnetic coupling and their strain manipulation are quantified through X-ray linear dichroism (XLD) and X-ray magnetic circular dichroism (XMCD) measurements, further confirmed by both molecular orbital theory and Goodenough-Kanamori-Anderson rules. First principles calculations unveil a higher (lower) magnetic moment of individual magnetic atoms with tensile (compressive) strain, including unusual interfacial antiferromagnetism arising d-orbital occupations, and bond angle geometry. This endeavor paves a potential method to manipulate the octahedral tilt to tailor emergent phenomena at heterointerfaces via atomically precise strain-interface engineering.