Defect Control via Cu Enrichment Enhances Multifunctional Properties in the Polar Semiconductor Cu1+xMn1-ySiTe3
Abstract
Polar materials have recently attracted significant interest due to their rich multifunctional properties. The chalcogenide polar semiconductor Cu1-xMn1+ySiTe3 (Cu-deficient) is an emerging multiferroic system in which electric polarization is coupled to magnetization. However, its macroscopic ferroelectric polarization is strongly suppressed due to the presence of a high density of stacking faults. In this work, we demonstrate that these crystal defects, likely originating from non-stoichiometry, can be substantially reduced by increasing the Cu content. Cu-enriched samples, Cu1+xMn1-ySiTe3, crystallize in a noncentrosymmetric monoclinic structure (space group Pm) as the Cu-deficient counterpart but show a nearly stacking-fault-free phase, which is attributed to the emergence of an interstitial site. Consequently, the Cu-enriched samples show a pronounced enhancement of the second-harmonic generation (SHG) response compared to Cu-deficient compositions. Magnetically, the Cu-enriched crystals retain long-range antiferromagnetic order with a Neel temperature of TN ~ 33 K without a glassy state but manifest a distinct spin-flop transition along the polar b-axis that is absent in the Cu-deficient compositions. Furthermore, the electronic ground state evolves from insulating to doped semiconducting behavior upon Cu enrichment. Together, these results establish this material system as a unique and versatile platform for elucidating the interplay among composition, crystal defects, and multifunctional properties, offering a route to design magnetic polar systems with tunable quantum functionalities.
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BibTeX
@misc{ghosh2026defect,
title = {{Defect Control via Cu Enrichment Enhances Multifunctional Properties in the Polar Semiconductor Cu1+xMn1-ySiTe3}},
author = {Subrata Ghosh and Yu Liu and Saugata Sarker and Boyang Zheng and Sreekant Anil and Soumi Mondal and Yuxi Zhang and Sai Venkata Gayathri Ayyagari and Mingyu Xu and Yingdong Guan and Tsung-Han Yang and Xiaoping Wang and Vincent H. Crespi and Nasim Alem and Weiwei Xie and Venkatraman Gopalan and Qiang Zhang and Zhiqiang Mao},
howpublished = {arXiv},
year = {2026},
month = may,
doi = {10.48550/arxiv.2605.18584},
eprint = {2605.18584},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2605.18584},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Defect Control via Cu Enrichment Enhances Multifunctional Properties in the Polar Semiconductor Cu1+xMn1-ySiTe3
AU - Subrata Ghosh
AU - Yu Liu
AU - Saugata Sarker
AU - Boyang Zheng
AU - Sreekant Anil
AU - Soumi Mondal
AU - Yuxi Zhang
AU - Sai Venkata Gayathri Ayyagari
AU - Mingyu Xu
AU - Yingdong Guan
AU - Tsung-Han Yang
AU - Xiaoping Wang
AU - Vincent H. Crespi
AU - Nasim Alem
AU - Weiwei Xie
AU - Venkatraman Gopalan
AU - Qiang Zhang
AU - Zhiqiang Mao
PY - 2026
DA - 2026/05/18
PB - arXiv
DO - 10.48550/arxiv.2605.18584
UR - https://arxiv.org/abs/2605.18584
AB - Polar materials have recently attracted significant interest due to their rich multifunctional properties. The chalcogenide polar semiconductor Cu1-xMn1+ySiTe3 (Cu-deficient) is an emerging multiferroic system in which electric polarization is coupled to magnetization. However, its macroscopic ferroelectric polarization is strongly suppressed due to the presence of a high density of stacking faults. In this work, we demonstrate that these crystal defects, likely originating from non-stoichiometry, can be substantially reduced by increasing the Cu content. Cu-enriched samples, Cu1+xMn1-ySiTe3, crystallize in a noncentrosymmetric monoclinic structure (space group Pm) as the Cu-deficient counterpart but show a nearly stacking-fault-free phase, which is attributed to the emergence of an interstitial site. Consequently, the Cu-enriched samples show a pronounced enhancement of the second-harmonic generation (SHG) response compared to Cu-deficient compositions. Magnetically, the Cu-enriched crystals retain long-range antiferromagnetic order with a Neel temperature of TN ~ 33 K without a glassy state but manifest a distinct spin-flop transition along the polar b-axis that is absent in the Cu-deficient compositions. Furthermore, the electronic ground state evolves from insulating to doped semiconducting behavior upon Cu enrichment. Together, these results establish this material system as a unique and versatile platform for elucidating the interplay among composition, crystal defects, and multifunctional properties, offering a route to design magnetic polar systems with tunable quantum functionalities.
ER -