Observation of robust spin-phonon coupling and indication of hidden structural transition in the spin-driven ferroelectrics Mn4B_2O_9 (B= Nb, Ta)

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Main Authors: Jana, Rajesh, Garg, Alka, Rao, Rekha, Meier, Thomas
Format: Preprint
Published: 2026
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author Jana, Rajesh
Garg, Alka
Rao, Rekha
Meier, Thomas
author_facet Jana, Rajesh
Garg, Alka
Rao, Rekha
Meier, Thomas
contents We report detailed Raman spectroscopic and magnetic susceptibility studies on the spin-driven ferroelectric compounds Mn4Nb2O9 (MNO) and Mn4Ta2O9 (MTO). Both systems exhibit strong spin-phonon coupling below the short-range magnetic ordering temperature (T(sro)=223 K), followed by further renormalization of several Raman modes at the long-range magnetic ordering temperatures (TN = 120 K for MNO and 110 K for MTO). Pronounced anomalies in Raman mode frequencies and linewidths, along with the emergence of octahedral modes between Tsro and TN, indicate a possible low-symmetry structural transition, more evident in MNO and closely linked to magnetic ordering in MTO. Distinct low-temperature evolutions of Raman mode shift, linewidth, and integrated intensity in MNO and MTO highlight the role of the nonmagnetic B-site cation in tuning spin-lattice coupling, driven by differences in spin-orbit coupling and orbital hybridization between Nb5+ (4d) and Ta5+ (5d). By combining Raman spectroscopy with nuclear magnetic resonance, and diffuse reflectance spectroscopy, we further show that Mn-based systems possess a more distorted local structure than their Co analogues, while their electronic structures differ despite comparable band gaps. These results provide a comprehensive understanding of spin-lattice coupling in Mn- and Co-based A4B2O9 magnetoelectric systems.
format Preprint
id arxiv_https___arxiv_org_abs_2602_06311
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Observation of robust spin-phonon coupling and indication of hidden structural transition in the spin-driven ferroelectrics Mn4B_2O_9 (B= Nb, Ta)
Jana, Rajesh
Garg, Alka
Rao, Rekha
Meier, Thomas
Materials Science
We report detailed Raman spectroscopic and magnetic susceptibility studies on the spin-driven ferroelectric compounds Mn4Nb2O9 (MNO) and Mn4Ta2O9 (MTO). Both systems exhibit strong spin-phonon coupling below the short-range magnetic ordering temperature (T(sro)=223 K), followed by further renormalization of several Raman modes at the long-range magnetic ordering temperatures (TN = 120 K for MNO and 110 K for MTO). Pronounced anomalies in Raman mode frequencies and linewidths, along with the emergence of octahedral modes between Tsro and TN, indicate a possible low-symmetry structural transition, more evident in MNO and closely linked to magnetic ordering in MTO. Distinct low-temperature evolutions of Raman mode shift, linewidth, and integrated intensity in MNO and MTO highlight the role of the nonmagnetic B-site cation in tuning spin-lattice coupling, driven by differences in spin-orbit coupling and orbital hybridization between Nb5+ (4d) and Ta5+ (5d). By combining Raman spectroscopy with nuclear magnetic resonance, and diffuse reflectance spectroscopy, we further show that Mn-based systems possess a more distorted local structure than their Co analogues, while their electronic structures differ despite comparable band gaps. These results provide a comprehensive understanding of spin-lattice coupling in Mn- and Co-based A4B2O9 magnetoelectric systems.
title Observation of robust spin-phonon coupling and indication of hidden structural transition in the spin-driven ferroelectrics Mn4B_2O_9 (B= Nb, Ta)
topic Materials Science
url https://arxiv.org/abs/2602.06311