Interplay of Orbital Degeneracy and Vacancies in Stabilizing Collinear Magnetic Order in Cr$_{1+δ}$Te$_2$

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Main Authors: Chowdhury, Prasanta, Sau, Jyotirmoy, Numan, Mohamad, Sannigrahi, Jhuma, Gutmann, Matthias, Das, Gangadhar, Adroja, D. T., Giri, Saurav, Kumar, Manoranjan, Majumdar, Subham
Format: Preprint
Published: 2025
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author Chowdhury, Prasanta
Sau, Jyotirmoy
Numan, Mohamad
Sannigrahi, Jhuma
Gutmann, Matthias
Das, Gangadhar
Adroja, D. T.
Giri, Saurav
Kumar, Manoranjan
Majumdar, Subham
author_facet Chowdhury, Prasanta
Sau, Jyotirmoy
Numan, Mohamad
Sannigrahi, Jhuma
Gutmann, Matthias
Das, Gangadhar
Adroja, D. T.
Giri, Saurav
Kumar, Manoranjan
Majumdar, Subham
contents Cr$_{1+δ}$Te$_2$, a two-dimensional van der Waals ferromagnet, displays a contested magnetic structure, poised between collinear and non-collinear spin configurations. In this work, we investigate the magnetic structure of Cr$_{1.33}$Te$_2$ at the microscopic level by combining single-crystal neutron diffraction, X-ray absorption spectroscopy, and first-principles calculations. Neutron diffraction measurements reveal a distinct collinear spin alignment, whereas spectroscopic analyses reveal inherent structural vacancies at both Cr and Te sites. These vacancies lead to local symmetry breaking that elevates the orbital degeneracy of the Cr 3$d$ states, as demonstrated by our first-principles analysis. The resulting modification of magnetocrystalline anisotropy emerges as the key mechanism stabilising the collinear magnetic ground state over the non-collinear one in the presence of vacancies. Our findings uncover a vacancy-driven route to control spin anisotropy and magnetic ordering in layered ferromagnets, offering new insights into the design of tunable 2D magnetic materials.
format Preprint
id arxiv_https___arxiv_org_abs_2512_05563
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Interplay of Orbital Degeneracy and Vacancies in Stabilizing Collinear Magnetic Order in Cr$_{1+δ}$Te$_2$
Chowdhury, Prasanta
Sau, Jyotirmoy
Numan, Mohamad
Sannigrahi, Jhuma
Gutmann, Matthias
Das, Gangadhar
Adroja, D. T.
Giri, Saurav
Kumar, Manoranjan
Majumdar, Subham
Strongly Correlated Electrons
Materials Science
Cr$_{1+δ}$Te$_2$, a two-dimensional van der Waals ferromagnet, displays a contested magnetic structure, poised between collinear and non-collinear spin configurations. In this work, we investigate the magnetic structure of Cr$_{1.33}$Te$_2$ at the microscopic level by combining single-crystal neutron diffraction, X-ray absorption spectroscopy, and first-principles calculations. Neutron diffraction measurements reveal a distinct collinear spin alignment, whereas spectroscopic analyses reveal inherent structural vacancies at both Cr and Te sites. These vacancies lead to local symmetry breaking that elevates the orbital degeneracy of the Cr 3$d$ states, as demonstrated by our first-principles analysis. The resulting modification of magnetocrystalline anisotropy emerges as the key mechanism stabilising the collinear magnetic ground state over the non-collinear one in the presence of vacancies. Our findings uncover a vacancy-driven route to control spin anisotropy and magnetic ordering in layered ferromagnets, offering new insights into the design of tunable 2D magnetic materials.
title Interplay of Orbital Degeneracy and Vacancies in Stabilizing Collinear Magnetic Order in Cr$_{1+δ}$Te$_2$
topic Strongly Correlated Electrons
Materials Science
url https://arxiv.org/abs/2512.05563