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<p>X-ray linear dichroism has been pivotal for probing electronic anisotropies, but its inherent limited spatial resolution precludes the atomic-scale investigations of orbital polarization. Here we introduce a versatile electron linear dichroism methodology in scanning transmission electron microscopy that overcomes these constraints. Using electron energy loss spectroscopy with an atomic-sized probe and selecting momentum transfers along two orthogonal directions, we directly visualize orbital occupation at individual atomic columns in real space. Using strained La<sub>0.7</sub>Sr<sub>0.3</sub>MnO<sub>3</sub> thin films as a model system, we resolve the Mn3<i>d</i> e<sub>g</sub> orbital polarization with sub-ångström precision. We show that compressive strain stabilizes 3<i>z</i><sup>2</sup>–<i>r</i><sup>2</sup> occupation whereas tensile strain favours <i>x</i><sup>2</sup>–<i>y</i><sup>2</sup>. These results validate our approach against established X-ray measurements, achieving the ultimate single-atomic-column sensitivity. We further demonstrate two optimized signal extraction protocols that adapt to experimental constraints without compromising sensitivity. This generalizable platform opens unique opportunities to study symmetry-breaking phenomena at individual defects, interfaces and in quantum materials where atomic-scale electronic anisotropy governs emergent functionality.</p>

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Detecting linear dichroism with atomic resolution

  • 期刊论文

  • 发表日期：

    2026年5月12日

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  • Roger Guzman,
  • Ján Rusz,
  • Ang Li,
  • Juan Carlos Idrobo,
  • Wu Zhou,
  • Jaume Gazquez

摘要

X-ray linear dichroism has been pivotal for probing electronic anisotropies, but its inherent limited spatial resolution precludes the atomic-scale investigations of orbital polarization. Here we introduce a versatile electron linear dichroism methodology in scanning transmission electron microscopy that overcomes these constraints. Using electron energy loss spectroscopy with an atomic-sized probe and selecting momentum transfers along two orthogonal directions, we directly visualize orbital occupation at individual atomic columns in real space. Using strained La0.7Sr0.3MnO3 thin films as a model system, we resolve the Mn3d eg orbital polarization with sub-ångström precision. We show that compressive strain stabilizes 3z2–r2 occupation whereas tensile strain favours x2–y2. These results validate our approach against established X-ray measurements, achieving the ultimate single-atomic-column sensitivity. We further demonstrate two optimized signal extraction protocols that adapt to experimental constraints without compromising sensitivity. This generalizable platform opens unique opportunities to study symmetry-breaking phenomena at individual defects, interfaces and in quantum materials where atomic-scale electronic anisotropy governs emergent functionality.