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Although signatures of the orbital Edelstein effect have been reported, its microscopic mechanisms and quantitative validation remain underexplored. Here, by directly linking the atomic structure of (110) two\u2010dimensional electron gases to both their calculated and measured electronic band dispersions, we predict and provide experimental evidence for a significant orbital Edelstein contribution that governs the anisotropy of its harmonic transport response. Scanning transmission electron microscopy and electron energy\u2010loss spectroscopy resolve the interfacial atomic configuration, which is used as input for density\u2010functional calculations. Angle\u2010resolved photoemission spectroscopy then confirms the resulting band structure, which is fitted by a tight\u2010binding model enabling computation of the spin and orbital Edelstein responses. Harmonic magnetotransport measurements reveal an anisotropic response that cannot be accounted for within a purely spin Edelstein framework, and is quantitatively reproduced by including an orbital contribution of order 20%. Our results establish (110) as a model platform for orbitronics and demonstrate a pathway to generate and harness orbital polarization in quantum oxide systems while also offering new insights into pairing mechanisms in their superconducting\u00a0state.<\/jats:p>","DOI":"10.1002\/adma.73899","type":"journal-article","created":{"date-parts":[[2026,7,17]],"date-time":"2026-07-17T11:09:44Z","timestamp":1784286584000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Orbital and Spin Edelstein Effects in KTaO\n                    <sub>3<\/sub>\n                    (110) Two\u2010Dimensional Electron Gases"],"prefix":"10.1002","author":[{"given":"Hugo","family":"Witt","sequence":"first","affiliation":[{"name":"Laboratoire Albert Fert, CNRS Thales, Universit\u00e9 Paris\u2010Saclay Palaiseau France"},{"name":"Laboratoire de Physique et d'Etude des Mat\u00e9riaux, ESPCI Paris, CNRS Universit\u00e9 PSL Paris France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7643-2358","authenticated-orcid":false,"given":"Aravind","family":"Raji","sequence":"additional","affiliation":[{"name":"Laboratoire de Physique des Solides, CNRS Universit\u00e9 Paris\u2010Saclay Orsay France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Srijani","family":"Mallik","sequence":"additional","affiliation":[{"name":"Laboratoire Albert Fert, CNRS Thales, Universit\u00e9 Paris\u2010Saclay Palaiseau France"},{"name":"Saha Institute of Nuclear Physics, A CI of Homi Bhabha NationalInstitute  Kolkata India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"B\u00f6rge","family":"G\u00f6bel","sequence":"additional","affiliation":[{"name":"Institute of Physics Martin\u2010Luther\u2010Universit\u00e4t Halle\u2010Wittenberg  Halle (Saale) Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Luis M.","family":"Vicente\u2010Arche","sequence":"additional","affiliation":[{"name":"Laboratoire Albert Fert, CNRS Thales, Universit\u00e9 Paris\u2010Saclay Palaiseau France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sara","family":"Varotto","sequence":"additional","affiliation":[{"name":"Laboratoire Albert Fert, CNRS Thales, Universit\u00e9 Paris\u2010Saclay Palaiseau France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Julien","family":"Br\u00e9hin","sequence":"additional","affiliation":[{"name":"Laboratoire Albert Fert, CNRS Thales, Universit\u00e9 Paris\u2010Saclay Palaiseau France"},{"name":"SPINTEC Univ. 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