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Using state‐of‐the‐art, aberration‐corrected scanning transmission electron microscopy and electron energy loss spectroscopy  with atomic‐scale spatial resolution, experimental evidence for an intrinsic electronic reconstruction at the LAO/STO interface is shown. Simultaneous measurements of interfacial electron density and system polarization are crucial for establishing the highly debated origin of the 2D electron gas.

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Electron Transfer and Ionic Displacements at the Origin of the 2D Electron Gas at the LAO/STO Interface: Direct Measurements with Atomic‐Column Spatial Resolution