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Density functional theory (DFT) reveals that the frontier molecular orbitals of these complexes are predominantly localized on the [Te3]2\u2013 fragment, while the trivalent lanthanide ions stabilize the tellurium chain through weak but measurable metal\u2013ligand interactions. To experimentally resolve these interactions, we focus on complementary ligand- and metal-centered X-ray spectroscopic approaches. Ln L3-edge high-resolution XANES (HR-XANES) and valence-band resonant inelastic X-ray scattering (VB-RIXS) demonstrate that the Ln-Te\/C interaction has substantial Ln 5d orbital contributions, particularly for the Ln-Te bond, and remain largely constant across the three complexes. DFT-based bond analysis provides a mechanistic interpretation of these trends. The Ln\u2013C interaction exhibits increasing electron density at the bond critical point and a higher delocalization index (QTAIM analysis) from the lighter to the heavier lanthanides, reflecting enhanced Ln 4f participation within an energy-driven covalency regime. The Ln\u2013Te interaction is predominantly electrostatic, with meaningful orbital contributions arising mainly from Ln 5d participation within an orbital-overlap-driven covalency regime. These results demonstrate that the Ln\u2013C and Ln\u2013Te bonding in the present complexes follow fundamentally distinct covalency mechanisms, which together enable the stabilization and isolation of the small [Te3]2\u2013 fragment chain.<\/jats:p>","DOI":"10.1021\/jacs.6c06838","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T13:02:42Z","timestamp":1790773362000},"page":"42981-42995","source":"Crossref","is-referenced-by-count":0,"title":["Direct Evidence of\na La\u2013Te Bond and Bonding\nRegime Differences for Ln\u2013C and Ln\u2013Te in [K(18-Crown\n6)(Cp\u20332LnTe3)] (Ln = La, Ce, and Nd)"],"prefix":"10.1021","volume":"148","author":[{"given":"Cedric Y.","family":"Reitz","sequence":"first","affiliation":[{"name":"Karlsruhe Institute of Technology (KIT) , , Kaiserstra\u00dfe 12 , ,","place":["Karlsruhe, Germany, D-76131"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"David","family":"Frick","sequence":"additional","affiliation":[{"name":"Karlsruhe Institute of Technology (KIT) , , Kaiserstra\u00dfe 12 , ,","place":["Karlsruhe, Germany, D-76151"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Elena","family":"Pross","sequence":"additional","affiliation":[{"name":"Karlsruhe Institute of Technology (KIT) , , Kaiserstra\u00dfe 12 , ,","place":["Karlsruhe, Germany, D-76151"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3546-2622","authenticated-orcid":true,"given":"Emily M.","family":"Reynolds","sequence":"additional","affiliation":[{"name":"Karlsruhe Institute of Technology (KIT) , , Kaiserstra\u00dfe 12 , ,","place":["Karlsruhe, Germany, 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D-76131"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Julius","family":"Wolf","sequence":"additional","affiliation":[{"name":"Karlsruhe Institute of Technology (KIT) , , Kaiserstra\u00dfe 12 , ,","place":["Karlsruhe, Germany, D-76151"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9088-8944","authenticated-orcid":true,"given":"Dirk","family":"Hauschild","sequence":"additional","affiliation":[{"name":"Karlsruhe Institute of Technology (KIT) , , Kaiserstra\u00dfe 12 , ,","place":["Karlsruhe, Germany, D-76131"]},{"name":"University of Nevada, Las Vegas (UNLV) , , , ,","place":["Las Vegas, Nevada, United States of America, 89154-4003"]},{"name":"Karlsruhe Institute of Technology , , Kaiserstra\u00dfe 12 , ,","place":["Karlsruhe, Germany, D-76131"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jo\u0308rg","family":"Go\u0308ttlicher","sequence":"additional","affiliation":[{"name":"Karlsruhe Institute of 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