Magnetically coupled charge-transport crossover and giant negative magnetoresistance in iodine-incorporated Cr2Se3
Abstract
We report the synthesis and comprehensive investigation of iodine-incorporated Cr2Se3, a non-van der Waals quasi-two-dimensional magnetic material, using structural, magnetic, transport, spectroscopic, and first-principles methods. Magnetization and electron spin resonance measurements reveal an antiferromagnetically ordered state below TN ≈ 52 K. At higher temperatures, a second, broader anomaly emerges near T* ≈ 150 K, coinciding with a shallow minimum in the temperature-dependent resistivity that resembles a metal-to-insulator-like crossover. Hall measurements indicate predominantly hole-like conduction at high temperatures (≥ 150 K), while the nonlinear Hall response below T*, together with an anomaly in the third-harmonic electrical signal, suggests the emergence of mobility-dependent multichannel and spatially inhomogeneous transport. A large, non-saturating negative magnetoresistance reaching approximately -78\% at 25 K and 12 T further demonstrates strong coupling between charge transport and the magnetic state. Temperature-dependent Raman spectroscopy reveals no symmetry-changing structural transition near T*, whereas angle resolved photoemission spectroscopy (ARPES) measurements show no major reconstruction of the electronic structure occupied across the crossover. Taken together, these results identify the high-temperature anomaly as a broad magnetically coupled transport crossover arising from the interplay of short-range magnetic correlations, chemical disorder, and redistribution among competing conduction channels. These findings demonstrate that anion incorporation provides an effective route to tuning the coupled electronic and magnetic properties of non-layered Cr2Se3, establishing this system as a promising platform for investigating correlated transport and emergent spintronic functionalities in transition-metal chalcogenides.
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BibTeX
@misc{das2026magnetically,
title = {{Magnetically coupled charge-transport crossover and giant negative magnetoresistance in iodine-incorporated Cr$_2$Se$_3$}},
author = {Bikash Das and Shibnath Mandal and Kapildeb Dolui and Oleksi Laguta and Sambit Choudhury and Suvadip Masanta and Tanima Kundu and Jorge Andres Navarro Giraldo and Alexey Barinov and Shibabrata Nandi and Kai Rossnagel and Sanjoy Kr Mahatha and Rajib Mondal and Petr Neugebauer and Subhadeep Datta},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.17945},
eprint = {2609.17945},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.17945},
}
RIS
TY - UNPB
TI - Magnetically coupled charge-transport crossover and giant negative magnetoresistance in iodine-incorporated Cr_2Se_3
AU - Bikash Das
AU - Shibnath Mandal
AU - Kapildeb Dolui
AU - Oleksi Laguta
AU - Sambit Choudhury
AU - Suvadip Masanta
AU - Tanima Kundu
AU - Jorge Andres Navarro Giraldo
AU - Alexey Barinov
AU - Shibabrata Nandi
AU - Kai Rossnagel
AU - Sanjoy Kr Mahatha
AU - Rajib Mondal
AU - Petr Neugebauer
AU - Subhadeep Datta
PY - 2026
DA - 2026/09/16
PB - arXiv
DO - 10.48550/arxiv.2609.17945
UR - https://arxiv.org/abs/2609.17945
AB - We report the synthesis and comprehensive investigation of iodine-incorporated Cr_2Se_3, a non-van der Waals quasi-two-dimensional magnetic material, using structural, magnetic, transport, spectroscopic, and first-principles methods. Magnetization and electron spin resonance measurements reveal an antiferromagnetically ordered state below T_N ≈ 52 K. At higher temperatures, a second, broader anomaly emerges near T^* ≈ 150 K, coinciding with a shallow minimum in the temperature-dependent resistivity that resembles a metal-to-insulator-like crossover. Hall measurements indicate predominantly hole-like conduction at high temperatures (≥ 150 K), while the nonlinear Hall response below T*, together with an anomaly in the third-harmonic electrical signal, suggests the emergence of mobility-dependent multichannel and spatially inhomogeneous transport. A large, non-saturating negative magnetoresistance reaching approximately -78\% at 25 K and 12 T further demonstrates strong coupling between charge transport and the magnetic state. Temperature-dependent Raman spectroscopy reveals no symmetry-changing structural transition near T*, whereas angle resolved photoemission spectroscopy (ARPES) measurements show no major reconstruction of the electronic structure occupied across the crossover. Taken together, these results identify the high-temperature anomaly as a broad magnetically coupled transport crossover arising from the interplay of short-range magnetic correlations, chemical disorder, and redistribution among competing conduction channels. These findings demonstrate that anion incorporation provides an effective route to tuning the coupled electronic and magnetic properties of non-layered Cr_2Se_3, establishing this system as a promising platform for investigating correlated transport and emergent spintronic functionalities in transition-metal chalcogenides.
ER -