Discovery of a layered multiferroic compound Cu1−xMn1+ySiTe3 with strong magnetoelectric coupling

Chandan De; Yu Liu; Sai Venkata Gayathri Ayyagari; Boyang Zheng; Kyle P. Kelley; Sankalpa Hazra; Jingyang He; Sylwia Pawledzio; Subin Mali; Samaresh Guchhait; Suguru Yoshida; Yingdong Guan; Seng Huat Lee; Milos Sretenovic; Xianglin Ke; Le Wang; Mark H. Engelhard; Yingge Du; Weiwei Xie; Xiaoping Wang; Vincent H. Crespi; Nasim Alem; Venkatraman Gopalan; Qiang Zhang; Zhiqiang Mao

doi:10.1126/sciadv.adp9379

Discovery of a layered multiferroic compound Cu_1−xMn_1+ySiTe₃ with strong magnetoelectric coupling

Chandan De, Yu Liu, Sai Venkata Gayathri Ayyagari, Boyang Zheng, Kyle P. Kelley, Sankalpa Hazra, Jingyang He, Sylwia Pawledzio, Subin Mali, Samaresh Guchhait, Suguru Yoshida, Yingdong Guan, Seng Huat Lee, Milos Sretenovic, Xianglin Ke, Le Wang, Mark H. Engelhard, Yingge Du, Weiwei Xie, Xiaoping WangVincent H. Crespi, Nasim Alem, Venkatraman Gopalan, Qiang Zhang, Zhiqiang Mao

Research output: Contribution to journal › Article › peer-review

Abstract

Multiferroic materials host both ferroelectricity and magnetism, offering potential for magnetic memory and spin transistor applications. Here, we report a multiferroic chalcogenide semiconductor Cu₁_−xMn₁_+ySiTe₃ (0.04 ≤ x ≤ 0.26; 0.03 ≤ y ≤ 0.15), which crystallizes in a polar monoclinic structure (Pm space group). It exhibits a canted antiferromagnetic state below 35 kelvin, with magnetic hysteresis and remanent magnetization under 15 kelvin. We demonstrate multiferroicity and strong magnetoelectric coupling through magnetodielectric and magnetocurrent measurements. At 10 kelvin, the magnetically induced electric polarization reaches ~0.8 microcoulombs per square centimeter, comparable to the highest value in oxide multiferroics. We also observe possible room-temperature ferroelectricity. Given that multiferroicity is very rare among transition metal chalcogenides, our finding sets up a unique materials platform for designing multiferroic chalcogenides.

Original language	English
Article number	eadp9379
Journal	Science Advances
Volume	11
Issue number	1
DOIs	https://doi.org/10.1126/sciadv.adp9379
State	Published - Jan 3 2025

Funding

The x-ray data were measured on the Rigaku XtaLab Synergy-R DW system housed in the SNS X-ray Diffraction Laboratory. This study is primarily based on research conducted at The Pennsylvania State University Two-Dimensional Crystal Consortium-Materials Innovation Platform (2DCC-MIP), which is supported by NSF Cooperative Agreement No. DMR-2039351. Z.M. also acknowledges the support from the NSF under grant no. DMR 2211327. S.V.G.A. acknowledges the support from the NSF through the Pennsylvania State University Materials Research Science and Engineering Center (MRSEC) DMR-2011839 (2020-2026). N.A., W.X. and S.V.G.A. acknowledge the support from the Experimental Condensed Matter Physics, Division of Materials Sciences and Engineering, Basic Energy Sciences, US DOE, grant no. DE-SC0024943 for the structure study using STEM and XRD. S.G. acknowledges the support from the National Science Foundation award no. DMR-2018579. X.K. acknowledges the support by the US DOE under award no. DE-SC0019259 for partial magnetic measurements. In-vacuum cleave and XPS measurements along with the corresponding analysis were supported by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences, Division of Materials Sciences and Engineering, Synthesis and Processing Science Program, under award no. 10122. S.H. and V.G. acknowledge the support from the DOE, Basic Energy Sciences grant no. DE-SC0012375 for the nonlinear optical characterization. J.H. and V.G. acknowledge the support from the NSF grant no. DMR-2210933 for linear optical characterization. Neutron diffraction research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.The piezoresponse force microscopy research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy Office of Science User Facility at Oak Ridge National Laboratory.

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De, C., Liu, Y., Ayyagari, S. V. G., Zheng, B., Kelley, K. P., Hazra, S., He, J., Pawledzio, S., Mali, S., Guchhait, S., Yoshida, S., Guan, Y., Lee, S. H., Sretenovic, M., Ke, X., Wang, L., Engelhard, M. H., Du, Y., Xie, W., ... Mao, Z. (2025). Discovery of a layered multiferroic compound Cu_1−xMn_1+ySiTe₃ with strong magnetoelectric coupling. Science Advances, 11(1), Article eadp9379. https://doi.org/10.1126/sciadv.adp9379

@article{4c4e65e21d4a4da68346a01f676ee99f,

title = "Discovery of a layered multiferroic compound Cu1−xMn1+ySiTe3 with strong magnetoelectric coupling",

abstract = "Multiferroic materials host both ferroelectricity and magnetism, offering potential for magnetic memory and spin transistor applications. Here, we report a multiferroic chalcogenide semiconductor Cu1−xMn1+ySiTe3 (0.04 ≤ x ≤ 0.26; 0.03 ≤ y ≤ 0.15), which crystallizes in a polar monoclinic structure (Pm space group). It exhibits a canted antiferromagnetic state below 35 kelvin, with magnetic hysteresis and remanent magnetization under 15 kelvin. We demonstrate multiferroicity and strong magnetoelectric coupling through magnetodielectric and magnetocurrent measurements. At 10 kelvin, the magnetically induced electric polarization reaches ~0.8 microcoulombs per square centimeter, comparable to the highest value in oxide multiferroics. We also observe possible room-temperature ferroelectricity. Given that multiferroicity is very rare among transition metal chalcogenides, our finding sets up a unique materials platform for designing multiferroic chalcogenides.",

author = "Chandan De and Yu Liu and Ayyagari, {Sai Venkata Gayathri} and Boyang Zheng and Kelley, {Kyle P.} and Sankalpa Hazra and Jingyang He and Sylwia Pawledzio and Subin Mali and Samaresh Guchhait and Suguru Yoshida and Yingdong Guan and Lee, {Seng Huat} and Milos Sretenovic and Xianglin Ke and Le Wang and Engelhard, {Mark H.} and Yingge Du and Weiwei Xie and Xiaoping Wang and Crespi, {Vincent H.} and Nasim Alem and Venkatraman Gopalan and Qiang Zhang and Zhiqiang Mao",

note = "Publisher Copyright: Copyright {\textcopyright} 2025 The Authors, some rights reserved.",

year = "2025",

month = jan,

day = "3",

doi = "10.1126/sciadv.adp9379",

language = "English",

volume = "11",

journal = "Science Advances",

issn = "2375-2548",

publisher = "American Association for the Advancement of Science",

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De, C, Liu, Y, Ayyagari, SVG, Zheng, B, Kelley, KP, Hazra, S, He, J, Pawledzio, S, Mali, S, Guchhait, S, Yoshida, S, Guan, Y, Lee, SH, Sretenovic, M, Ke, X, Wang, L, Engelhard, MH, Du, Y, Xie, W, Wang, X, Crespi, VH, Alem, N, Gopalan, V, Zhang, Q & Mao, Z 2025, 'Discovery of a layered multiferroic compound Cu_1−xMn_1+ySiTe₃ with strong magnetoelectric coupling', Science Advances, vol. 11, no. 1, eadp9379. https://doi.org/10.1126/sciadv.adp9379

TY - JOUR

T1 - Discovery of a layered multiferroic compound Cu1−xMn1+ySiTe3 with strong magnetoelectric coupling

AU - De, Chandan

AU - Liu, Yu

AU - Ayyagari, Sai Venkata Gayathri

AU - Zheng, Boyang

AU - Kelley, Kyle P.

AU - Hazra, Sankalpa

AU - He, Jingyang

AU - Pawledzio, Sylwia

AU - Mali, Subin

AU - Guchhait, Samaresh

AU - Yoshida, Suguru

AU - Guan, Yingdong

AU - Lee, Seng Huat

AU - Sretenovic, Milos

AU - Ke, Xianglin

AU - Wang, Le

AU - Engelhard, Mark H.

AU - Du, Yingge

AU - Xie, Weiwei

AU - Wang, Xiaoping

AU - Crespi, Vincent H.

AU - Alem, Nasim

AU - Gopalan, Venkatraman

AU - Zhang, Qiang

AU - Mao, Zhiqiang

PY - 2025/1/3

Y1 - 2025/1/3

N2 - Multiferroic materials host both ferroelectricity and magnetism, offering potential for magnetic memory and spin transistor applications. Here, we report a multiferroic chalcogenide semiconductor Cu1−xMn1+ySiTe3 (0.04 ≤ x ≤ 0.26; 0.03 ≤ y ≤ 0.15), which crystallizes in a polar monoclinic structure (Pm space group). It exhibits a canted antiferromagnetic state below 35 kelvin, with magnetic hysteresis and remanent magnetization under 15 kelvin. We demonstrate multiferroicity and strong magnetoelectric coupling through magnetodielectric and magnetocurrent measurements. At 10 kelvin, the magnetically induced electric polarization reaches ~0.8 microcoulombs per square centimeter, comparable to the highest value in oxide multiferroics. We also observe possible room-temperature ferroelectricity. Given that multiferroicity is very rare among transition metal chalcogenides, our finding sets up a unique materials platform for designing multiferroic chalcogenides.

AB - Multiferroic materials host both ferroelectricity and magnetism, offering potential for magnetic memory and spin transistor applications. Here, we report a multiferroic chalcogenide semiconductor Cu1−xMn1+ySiTe3 (0.04 ≤ x ≤ 0.26; 0.03 ≤ y ≤ 0.15), which crystallizes in a polar monoclinic structure (Pm space group). It exhibits a canted antiferromagnetic state below 35 kelvin, with magnetic hysteresis and remanent magnetization under 15 kelvin. We demonstrate multiferroicity and strong magnetoelectric coupling through magnetodielectric and magnetocurrent measurements. At 10 kelvin, the magnetically induced electric polarization reaches ~0.8 microcoulombs per square centimeter, comparable to the highest value in oxide multiferroics. We also observe possible room-temperature ferroelectricity. Given that multiferroicity is very rare among transition metal chalcogenides, our finding sets up a unique materials platform for designing multiferroic chalcogenides.

UR - http://www.scopus.com/inward/record.url?scp=85214340782&partnerID=8YFLogxK

U2 - 10.1126/sciadv.adp9379

DO - 10.1126/sciadv.adp9379

M3 - Article

C2 - 39742500

AN - SCOPUS:85214340782

SN - 2375-2548

VL - 11

JO - Science Advances

JF - Science Advances

IS - 1

M1 - eadp9379

ER -

Discovery of a layered multiferroic compound Cu_1−xMn_1+ySiTe₃ with strong magnetoelectric coupling

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