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Main Authors: Jaiswal, Arun Kumar, Wang, Di, Lim, Ji Soo, Roy, Shruti, Wilhelm, Fabrice, Wollersen, Vanessa, Rogalev, Andrei, Tacon, Matthieu Le, Fuchs, Dirk
Format: Preprint
Published: 2026
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Online Access:https://arxiv.org/abs/2603.25514
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author Jaiswal, Arun Kumar
Wang, Di
Lim, Ji Soo
Roy, Shruti
Wilhelm, Fabrice
Wollersen, Vanessa
Rogalev, Andrei
Tacon, Matthieu Le
Fuchs, Dirk
author_facet Jaiswal, Arun Kumar
Wang, Di
Lim, Ji Soo
Roy, Shruti
Wilhelm, Fabrice
Wollersen, Vanessa
Rogalev, Andrei
Tacon, Matthieu Le
Fuchs, Dirk
contents Interfacial charge transfer (ICT) provides a powerful route to engineer electronic phases in correlated oxide heterostructures, yet predictive design principles remain elusive. Here, we systematically investigate superlattices composed of the 5d spin-orbit coupled semimetal SrIrO3 and a series of correlated 3d perovskites (LaMnO3, LaFeO3, LaCoO3, and NdNiO3), thereby establishing a quantitative framework for ICT across 3d/5d interfaces. Combining element-specific x-ray absorption spectroscopy with spatially resolved electron energy loss spectroscopy, a homogeneous electron transfer from the 5d to the 3d layers is directly quantified, reaching up to 0.35 e per unit cell in the cobaltate superlattice. We show that the magnitude of ICT scales linearly with the difference in electronegativity between the transition-metal oxide layers, identifying electronegativity-driven band alignment as the dominant mechanism for ICT. Beyond interfacial doping, we find that strong 3d-5d hybridization induces a complete low-spin to high-spin conversion in the cobaltate layers, demonstrating interface-controlled spin-state engineering without chemical substitution. These results establish electronegativity mismatch as a predictive design parameter for correlated oxide interfaces and provide a materials platform for tailoring band filling, orbital hierarchy, and spin configurations in quantum oxide heterostructures, paving the way towards advanced oxide electronics and next-generation information technologies.
format Preprint
id arxiv_https___arxiv_org_abs_2603_25514
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Interfacial charge-transfer in 3d/5d complex oxide heterostructures
Jaiswal, Arun Kumar
Wang, Di
Lim, Ji Soo
Roy, Shruti
Wilhelm, Fabrice
Wollersen, Vanessa
Rogalev, Andrei
Tacon, Matthieu Le
Fuchs, Dirk
Materials Science
Interfacial charge transfer (ICT) provides a powerful route to engineer electronic phases in correlated oxide heterostructures, yet predictive design principles remain elusive. Here, we systematically investigate superlattices composed of the 5d spin-orbit coupled semimetal SrIrO3 and a series of correlated 3d perovskites (LaMnO3, LaFeO3, LaCoO3, and NdNiO3), thereby establishing a quantitative framework for ICT across 3d/5d interfaces. Combining element-specific x-ray absorption spectroscopy with spatially resolved electron energy loss spectroscopy, a homogeneous electron transfer from the 5d to the 3d layers is directly quantified, reaching up to 0.35 e per unit cell in the cobaltate superlattice. We show that the magnitude of ICT scales linearly with the difference in electronegativity between the transition-metal oxide layers, identifying electronegativity-driven band alignment as the dominant mechanism for ICT. Beyond interfacial doping, we find that strong 3d-5d hybridization induces a complete low-spin to high-spin conversion in the cobaltate layers, demonstrating interface-controlled spin-state engineering without chemical substitution. These results establish electronegativity mismatch as a predictive design parameter for correlated oxide interfaces and provide a materials platform for tailoring band filling, orbital hierarchy, and spin configurations in quantum oxide heterostructures, paving the way towards advanced oxide electronics and next-generation information technologies.
title Interfacial charge-transfer in 3d/5d complex oxide heterostructures
topic Materials Science
url https://arxiv.org/abs/2603.25514