Role of 4f-Orbitals on the Magnetodielectric Properties and Spin-Phonon Coupling in Orthorhombic Sm0.50M0.50MnO3 (M = Ho and Eu)

Mohit Chandra; Satish Yadav; Vaidehi Deshmukh; Rajeev Rawat; V. G. Sathe; R. J. Choudhary; Kiran Singh

doi:10.1021/acsaelm.5c00397

Role of 4f-Orbitals on the Magnetodielectric Properties and Spin-Phonon Coupling in Orthorhombic Sm_0.50M_0.50MnO₃ (M = Ho and Eu)

Mohit Chandra
, Satish Yadav
, Vaidehi Deshmukh
, Rajeev Rawat
, V. G. Sathe
, R. J. Choudhary
, Kiran Singh

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

1 Scopus citations

Abstract

The polycrystalline samples of SmMnO₃ (SMO), Sm_0.50Ho_0.50MnO₃ (SHMO), and Sm_0.50Eu_0.50MnO₃ (SEMO) have been synthesized to understand the effect of Ho and Eu substitution on the structural and physical properties. Detailed crystal structure, magnetic, dielectric, magnetodielectric (MD), and Raman spectroscopy measurements have been performed to investigate the role of 4f-orbital on the magnetic, MD, and spin-phonon coupling in these materials. The pristine SMO exhibits an antiferromagnetic (AFM) transition around 58 K due to the canted A-type AFM ordering of Mn³⁺ moments. The Mn-O-Mn bond angle, unit cell volume, and the AFM transition temperature decrease with the partial substitution of Ho and Eu. All the studied samples exhibit anomalies in the dielectric measurement corresponding to the magnetic ordering. The temperature-dependent dielectric results of SHMO illustrate a sharp peak at 22 K, which shifted toward the lower temperature side with increasing magnetic field. These results are similar to orthorhombic RMnO₃. The temperature-dependent Raman measurements of all the studied samples reveal an anomaly at the magnetic ordering temperature, which suggests the spin-phonon coupling. The sign of MD is different for SEMO and SHMO samples. Our results demonstrated the enhancement of the MD value in SHMO and SEMO as compared to SMO. The SHMO exhibits both positive and negative MD in the magnetically ordered state. These findings highlight the strong magnetoelectric coupling in SHMO and SEMO as compared to pristine SMO.

Original language	English
Pages (from-to)	4231-4241
Number of pages	11
Journal	ACS Applied Electronic Materials
Volume	7
Issue number	9
DOIs	https://doi.org/10.1021/acsaelm.5c00397
State	Published - May 13 2025
Externally published	Yes

Funding

The authors would like to thank Dr. Velaga Srihari, High Pressure, and Synchrotron Radiation Physics Division, BARC, Mumbai, India, for room-temperature synchrotron X-ray diffraction measurements. The authors are also thankful to Dr. Dileep Kumar and Mr. Sharanjit Singh, UGC-DAE CSR, Indore, for SEM and EDX measurements. K.S. would like to thank the UGC-DAE Consortium for Scientific Research for the Collaborative Research Scheme CSR-IC-ISUM-26/CRS-309 and the Anusandhan National Research Foundation (ANRF), Department of Science and Technology, New Delhi, for financial support under Core Research Grant Project No. CRG/2021/007075.

Keywords

crystal structure
electric polarization
magnetization
magnetodielectric
magnetoelectric
multiferroics
spin-phonon coupling

Access to Document

10.1021/acsaelm.5c00397

Cite this

@article{7f79637fa44742879c648ba18399b39c,

title = "Role of 4f-Orbitals on the Magnetodielectric Properties and Spin-Phonon Coupling in Orthorhombic Sm0.50M0.50MnO3 (M = Ho and Eu)",

abstract = "The polycrystalline samples of SmMnO3 (SMO), Sm0.50Ho0.50MnO3 (SHMO), and Sm0.50Eu0.50MnO3 (SEMO) have been synthesized to understand the effect of Ho and Eu substitution on the structural and physical properties. Detailed crystal structure, magnetic, dielectric, magnetodielectric (MD), and Raman spectroscopy measurements have been performed to investigate the role of 4f-orbital on the magnetic, MD, and spin-phonon coupling in these materials. The pristine SMO exhibits an antiferromagnetic (AFM) transition around 58 K due to the canted A-type AFM ordering of Mn3+ moments. The Mn-O-Mn bond angle, unit cell volume, and the AFM transition temperature decrease with the partial substitution of Ho and Eu. All the studied samples exhibit anomalies in the dielectric measurement corresponding to the magnetic ordering. The temperature-dependent dielectric results of SHMO illustrate a sharp peak at 22 K, which shifted toward the lower temperature side with increasing magnetic field. These results are similar to orthorhombic RMnO3. The temperature-dependent Raman measurements of all the studied samples reveal an anomaly at the magnetic ordering temperature, which suggests the spin-phonon coupling. The sign of MD is different for SEMO and SHMO samples. Our results demonstrated the enhancement of the MD value in SHMO and SEMO as compared to SMO. The SHMO exhibits both positive and negative MD in the magnetically ordered state. These findings highlight the strong magnetoelectric coupling in SHMO and SEMO as compared to pristine SMO.",

keywords = "crystal structure, electric polarization, magnetization, magnetodielectric, magnetoelectric, multiferroics, spin-phonon coupling",

author = "Mohit Chandra and Satish Yadav and Vaidehi Deshmukh and Rajeev Rawat and Sathe, \{V. G.\} and Choudhary, \{R. J.\} and Kiran Singh",

note = "Publisher Copyright: {\textcopyright} 2025 American Chemical Society.",

year = "2025",

month = may,

day = "13",

doi = "10.1021/acsaelm.5c00397",

language = "English",

volume = "7",

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journal = "ACS Applied Electronic Materials",

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TY - JOUR

T1 - Role of 4f-Orbitals on the Magnetodielectric Properties and Spin-Phonon Coupling in Orthorhombic Sm0.50M0.50MnO3 (M = Ho and Eu)

AU - Chandra, Mohit

AU - Yadav, Satish

AU - Deshmukh, Vaidehi

AU - Rawat, Rajeev

AU - Sathe, V. G.

AU - Choudhary, R. J.

AU - Singh, Kiran

PY - 2025/5/13

Y1 - 2025/5/13

N2 - The polycrystalline samples of SmMnO3 (SMO), Sm0.50Ho0.50MnO3 (SHMO), and Sm0.50Eu0.50MnO3 (SEMO) have been synthesized to understand the effect of Ho and Eu substitution on the structural and physical properties. Detailed crystal structure, magnetic, dielectric, magnetodielectric (MD), and Raman spectroscopy measurements have been performed to investigate the role of 4f-orbital on the magnetic, MD, and spin-phonon coupling in these materials. The pristine SMO exhibits an antiferromagnetic (AFM) transition around 58 K due to the canted A-type AFM ordering of Mn3+ moments. The Mn-O-Mn bond angle, unit cell volume, and the AFM transition temperature decrease with the partial substitution of Ho and Eu. All the studied samples exhibit anomalies in the dielectric measurement corresponding to the magnetic ordering. The temperature-dependent dielectric results of SHMO illustrate a sharp peak at 22 K, which shifted toward the lower temperature side with increasing magnetic field. These results are similar to orthorhombic RMnO3. The temperature-dependent Raman measurements of all the studied samples reveal an anomaly at the magnetic ordering temperature, which suggests the spin-phonon coupling. The sign of MD is different for SEMO and SHMO samples. Our results demonstrated the enhancement of the MD value in SHMO and SEMO as compared to SMO. The SHMO exhibits both positive and negative MD in the magnetically ordered state. These findings highlight the strong magnetoelectric coupling in SHMO and SEMO as compared to pristine SMO.

AB - The polycrystalline samples of SmMnO3 (SMO), Sm0.50Ho0.50MnO3 (SHMO), and Sm0.50Eu0.50MnO3 (SEMO) have been synthesized to understand the effect of Ho and Eu substitution on the structural and physical properties. Detailed crystal structure, magnetic, dielectric, magnetodielectric (MD), and Raman spectroscopy measurements have been performed to investigate the role of 4f-orbital on the magnetic, MD, and spin-phonon coupling in these materials. The pristine SMO exhibits an antiferromagnetic (AFM) transition around 58 K due to the canted A-type AFM ordering of Mn3+ moments. The Mn-O-Mn bond angle, unit cell volume, and the AFM transition temperature decrease with the partial substitution of Ho and Eu. All the studied samples exhibit anomalies in the dielectric measurement corresponding to the magnetic ordering. The temperature-dependent dielectric results of SHMO illustrate a sharp peak at 22 K, which shifted toward the lower temperature side with increasing magnetic field. These results are similar to orthorhombic RMnO3. The temperature-dependent Raman measurements of all the studied samples reveal an anomaly at the magnetic ordering temperature, which suggests the spin-phonon coupling. The sign of MD is different for SEMO and SHMO samples. Our results demonstrated the enhancement of the MD value in SHMO and SEMO as compared to SMO. The SHMO exhibits both positive and negative MD in the magnetically ordered state. These findings highlight the strong magnetoelectric coupling in SHMO and SEMO as compared to pristine SMO.

KW - crystal structure

KW - electric polarization

KW - magnetization

KW - magnetodielectric

KW - magnetoelectric

KW - multiferroics

KW - spin-phonon coupling

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DO - 10.1021/acsaelm.5c00397

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