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In particular, 2DEGs in KTaO<jats:sub>3<\/jats:sub> (KTO) with 5d <jats:italic>t<\/jats:italic><jats:sub>2g<\/jats:sub> orbitals exhibit larger atomic spin\u2010orbit coupling and crystal\u2010facet\u2010dependent superconductivity absent for 3d 2DEGs in SrTiO<jats:sub>3<\/jats:sub> (STO). Herein, by tracing the interfacial chemistry, weak anti\u2010localization magneto\u2010transport behavior, and electronic structures of (001), (110), and (111) KTO 2DEGs, unambiguously cation exchange across KTO interfaces is discovered. Therefore, the origin of the 2DEGs at KTO\u2010based interfaces is dramatically different from the electronic\u00a0reconstruction observed at STO interfaces. More importantly, as the interface polarization grows with the higher order planes in the KTO case, the Rashba spin splitting becomes maximal for the superconducting (111) interfaces approximately twice that of the (001) interface. The larger Rashba spin splitting couples strongly to the asymmetric chiral texture of the orbital angular moment, and results mainly from the enhanced inter\u2010orbital hopping of the <jats:italic>t<\/jats:italic><jats:sub>2g<\/jats:sub> bands and more localized wave functions. This finding has profound implications for the search for topological superconductors, as well as the realization of efficient spin\u2010charge interconversion for low\u2010power spin\u2010orbitronics based on (110) and (111) KTO interfaces.<\/jats:p>","DOI":"10.1002\/adma.202313297","type":"journal-article","created":{"date-parts":[[2024,3,13]],"date-time":"2024-03-13T02:08:56Z","timestamp":1710295736000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":31,"title":["Giant Tunability of Rashba Splitting at Cation\u2010Exchanged Polar Oxide Interfaces by Selective Orbital Hybridization"],"prefix":"10.1002","volume":"36","author":[{"given":"Hao","family":"Xu","sequence":"first","affiliation":[{"name":"Beijing National Laboratory of Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences  Beijing 100190 China"},{"name":"School of Physical Sciences University of Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hang","family":"Li","sequence":"additional","affiliation":[{"name":"Photon Science Division Paul Scherrer Institute  Villigen 5232 Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nicolas","family":"Gauquelin","sequence":"additional","affiliation":[{"name":"Electron Microscopy for Materials Science (EMAT) University of Antwerp  4Groenenborgerlaan 171 Antwerp 2020 Belgium"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuejiao","family":"Chen","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Magnetic Materials and Devices and Zhejiang Province Key Laboratory of Magnetic Materials and Application Technology Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences  Ningbo 315201 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wen\u2010Feng","family":"Wu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Materials Physics Institute of Solid State Physics HFIPS Chinese Academy of Sciences  Hefei 230031 P. 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