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Main Authors: Bhartiya, V. K., Goswami, Anirban, Ng, Nicholas, Tian, Wei, Tucker, Matthew G., Aryal, Niraj, Wu, Lijun, Yin, Weiguo, Zhu, Yimei, Abeykoon, Milinda, Yakubu, Emmanuel, Guchhait, Samaresh, Tranquada, J. M.
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2512.06262
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author Bhartiya, V. K.
Goswami, Anirban
Ng, Nicholas
Tian, Wei
Tucker, Matthew G.
Aryal, Niraj
Wu, Lijun
Yin, Weiguo
Zhu, Yimei
Abeykoon, Milinda
Yakubu, Emmanuel
Guchhait, Samaresh
Tranquada, J. M.
author_facet Bhartiya, V. K.
Goswami, Anirban
Ng, Nicholas
Tian, Wei
Tucker, Matthew G.
Aryal, Niraj
Wu, Lijun
Yin, Weiguo
Zhu, Yimei
Abeykoon, Milinda
Yakubu, Emmanuel
Guchhait, Samaresh
Tranquada, J. M.
contents Cr$_{1+x}$Te$_2$ is a self-intercalated vdW system that is of current interest for its room-temperature FM phases and tunable topological properties. Early NPD measurements on the monoclinic phase Cr$_3$Te$_4$ ($x=0.5$) presented evidence for competing FM and AFM phases. Here we apply neutron diffraction to a single crystal of Cr$_{3+δ}$Te$_4$ with $δ=-0.10$ and discover that it consists of two distinct monoclinic phases, one with FM order below $T_{\rm C} \approx 321$ K and another that develops AFM order below $T_{\rm N} \approx 86$ K. In contrast, we find that a crystal with $δ=-0.26$ exhibits only FM order. The single-crystal analysis is complemented by results obtained with NPD, XPD, and TEM measurements on the $δ=-0.10$ composition. From observations of spontaneous magnetostriction of opposite sign at $T_{\rm C}$ and $T_{\rm N}$, along with the TEM evidence for both monoclinic phases in a single thin ($\approx$ 100 nm) grain, we conclude that the two phases must have a fine-grained ($\lesssim$ 100 nm) intergrowth character, as might occur from high-temperature spinodal decomposition during the growth process. Calculations of the relaxed lattice structures for the FM and AFM phases with DFT provide a rationalization of the observed spontaneous magnetostrictions. Correlations between the magnitude and orientation of the magnetic moments with lattice parameter variation demonstrate that the magnetic orders are sensitive to strain, thus explaining why magnetic ordering temperatures and anisotropies can be different between bulk and thin-film samples, when the latter are subject to epitaxial strain. Our results point to the need to investigate the supposed coexistence FM and AFM phases reported elsewhere in the Cr$_{1+x}$Te$_2$ system, such as in the Cr$_5$Te$_8$ phase ($x=0.25$).
format Preprint
id arxiv_https___arxiv_org_abs_2512_06262
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Competing magnetic phases in Cr$_{3+δ}$Te$_4$ are spatially segregated
Bhartiya, V. K.
Goswami, Anirban
Ng, Nicholas
Tian, Wei
Tucker, Matthew G.
Aryal, Niraj
Wu, Lijun
Yin, Weiguo
Zhu, Yimei
Abeykoon, Milinda
Yakubu, Emmanuel
Guchhait, Samaresh
Tranquada, J. M.
Strongly Correlated Electrons
Cr$_{1+x}$Te$_2$ is a self-intercalated vdW system that is of current interest for its room-temperature FM phases and tunable topological properties. Early NPD measurements on the monoclinic phase Cr$_3$Te$_4$ ($x=0.5$) presented evidence for competing FM and AFM phases. Here we apply neutron diffraction to a single crystal of Cr$_{3+δ}$Te$_4$ with $δ=-0.10$ and discover that it consists of two distinct monoclinic phases, one with FM order below $T_{\rm C} \approx 321$ K and another that develops AFM order below $T_{\rm N} \approx 86$ K. In contrast, we find that a crystal with $δ=-0.26$ exhibits only FM order. The single-crystal analysis is complemented by results obtained with NPD, XPD, and TEM measurements on the $δ=-0.10$ composition. From observations of spontaneous magnetostriction of opposite sign at $T_{\rm C}$ and $T_{\rm N}$, along with the TEM evidence for both monoclinic phases in a single thin ($\approx$ 100 nm) grain, we conclude that the two phases must have a fine-grained ($\lesssim$ 100 nm) intergrowth character, as might occur from high-temperature spinodal decomposition during the growth process. Calculations of the relaxed lattice structures for the FM and AFM phases with DFT provide a rationalization of the observed spontaneous magnetostrictions. Correlations between the magnitude and orientation of the magnetic moments with lattice parameter variation demonstrate that the magnetic orders are sensitive to strain, thus explaining why magnetic ordering temperatures and anisotropies can be different between bulk and thin-film samples, when the latter are subject to epitaxial strain. Our results point to the need to investigate the supposed coexistence FM and AFM phases reported elsewhere in the Cr$_{1+x}$Te$_2$ system, such as in the Cr$_5$Te$_8$ phase ($x=0.25$).
title Competing magnetic phases in Cr$_{3+δ}$Te$_4$ are spatially segregated
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2512.06262