Site-Selective Electronic Structure and Dynamical Softness in the Metallic Antiferromagnet Mn3CuN
Abstract
Electronic structure, local bonding, and magnetic order are intimately coupled in correlated antiperovskites, making it challenging to distinguish the contributions of individual crystallographic sites to their collective properties. Here, we combine element-specific X-ray spectroscopy, temperature-dependent X-ray absorption spectroscopy, X-ray magnetic circular dichroism, electrical transport measurements, and first-principles calculations to investigate the site-selective electronic structure of epitaxial metallic antiferromagnetic Mn3CuN thin films. We reveal an anomalous charge distribution characterized by effective low-valent Mn and subvalent Cu states stabilized by covalent Mn–N–Cu interactions. While the Mn sublattice forms a robust noncollinear antiferromagnetic framework below ∼120 K, the electronically distinct Cu sites remain magnetically inactive yet exhibit pronounced temperature-dependent local structural evolution. Despite the onset of magnetic ordering, Mn3CuN retains metallic transport with a near-zero temperature coefficient of resistivity (NZ-TCR), indicating minimal coupling between magnetic ordering and charge transport. These findings demonstrate that site-selective electronic structure enables chemically differentiated lattice dynamics while preserving a robust magnetic framework, establishing Mn3CuN antiperovskite in which electronic, structural, and magnetic responses can be selectively decoupled. This work provides a materials design principle for engineering multifunctional metallic antiperovskites through site-selective electronic structure and local chemical bonding.
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BibTeX
@article{keshri2026siteselective,
title = {{Site-Selective Electronic Structure and Dynamical Softness in the Metallic Antiferromagnet Mn3CuN}},
author = {Aryan Keshri and Sourav Chowdhury and Pushpendra Gupta and Naveen Goyal and Anju Ahlawat and Garima Kaura and Ram Janay Choudhury and Moritz Hoesch and N. Ravishankar and Manuel Bibes and A. Garcia-Castro and Sujit Das},
journal = {Journal of the American Chemical Society},
year = {2026},
month = oct,
doi = {10.1021/jacs.6c16429},
url = {https://hal.science/hal-05853149v1},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - JOUR
TI - Site-Selective Electronic Structure and Dynamical Softness in the Metallic Antiferromagnet Mn3CuN
AU - Aryan Keshri
AU - Sourav Chowdhury
AU - Pushpendra Gupta
AU - Naveen Goyal
AU - Anju Ahlawat
AU - Garima Kaura
AU - Ram Janay Choudhury
AU - Moritz Hoesch
AU - N. Ravishankar
AU - Manuel Bibes
AU - A. Garcia-Castro
AU - Sujit Das
PY - 2026
DA - 2026/10/01
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c16429
UR - https://hal.science/hal-05853149v1
AB - Electronic structure, local bonding, and magnetic order are intimately coupled in correlated antiperovskites, making it challenging to distinguish the contributions of individual crystallographic sites to their collective properties. Here, we combine element-specific X-ray spectroscopy, temperature-dependent X-ray absorption spectroscopy, X-ray magnetic circular dichroism, electrical transport measurements, and first-principles calculations to investigate the site-selective electronic structure of epitaxial metallic antiferromagnetic Mn3CuN thin films. We reveal an anomalous charge distribution characterized by effective low-valent Mn and subvalent Cu states stabilized by covalent Mn–N–Cu interactions. While the Mn sublattice forms a robust noncollinear antiferromagnetic framework below ∼120 K, the electronically distinct Cu sites remain magnetically inactive yet exhibit pronounced temperature-dependent local structural evolution. Despite the onset of magnetic ordering, Mn3CuN retains metallic transport with a near-zero temperature coefficient of resistivity (NZ-TCR), indicating minimal coupling between magnetic ordering and charge transport. These findings demonstrate that site-selective electronic structure enables chemically differentiated lattice dynamics while preserving a robust magnetic framework, establishing Mn3CuN antiperovskite in which electronic, structural, and magnetic responses can be selectively decoupled. This work provides a materials design principle for engineering multifunctional metallic antiperovskites through site-selective electronic structure and local chemical bonding.
SN - 0002-7863
SN - 1520-5126
ER -