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Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type
P. Athira, Ajay Tiwari, M.-J. Hsieh, J.-Y. Lin, Nidhi Puri, C.W. Wang, C. H. Prashanth, C. Dhanasekhar, C.L. Huang, H.D. Yang, Krishnamurthy Jyothinagaram, and D. Chandrasekhar Kakarla
Phys. Rev. Applied 21, 054025 – Published 13 May 2024
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Abstract
is a well-established L-type ferrimagnetic (L-FIM) material with field-induced magnetic ordering () and multiferroic properties below (around 12K). In this study, we investigate the magnetic properties of through temperature- and field-dependent ac and dc magnetic susceptibility measurements. Isothermal magnetization data reveal an additional metamagnetic transition () beyond the existing boundary between L-FIM and multiferroic phases (). Frequency-dependent ac magnetic susceptibility data demonstrate reentrant-spin-glass-like behavior below , with a critical temperature () of 6.2K. Notably, a nonlinear magnetodielectric response and concurrent anomalies in M(H) at the two metamagnetic transitions ( and ) allude to a profoundly intertwined magnetoelectric (ME) nature. A finite nonlinear ME effect () of about 0.56ps/m is comparable to that of ME materials such as and . The temperature-dependent adiabatic temperature change (Δ) due to the contribution of magnetic spin entropy exhibits a small value (approximately 0.8K) with an oscillatory-like magnetocaloric effect. Remarkably, the adiabatic temperature change (Δ) owing to magnetoelectric coupling is quite large (5.2K under a 7T magnetic field) near . The tunability of with temperature and magnetic field strength represents a unique multicaloric medium whose temperature and field parameters can be easily adjusted for potential cryogenic applications near liquid-helium temperatures.
- Received 30 November 2023
- Revised 7 February 2024
- Accepted 22 April 2024
DOI:https://doi.org/10.1103/PhysRevApplied.21.054025
© 2024 American Physical Society
Physics Subject Headings (PhySH)
- Research Areas
Magneto-dielectric effectMagnetocaloric effectMagnetoelectric effectMetamagnetism
- Physical Systems
FerrimagnetsMultiferroicsSolid-state refrigerationTransition metal oxides
Condensed Matter, Materials & Applied PhysicsEnergy Science & Technology
Authors & Affiliations
P. Athira1, Ajay Tiwari2, M.-J. Hsieh3, J.-Y. Lin3,4, Nidhi Puri3, C.W. Wang5, C. H. Prashanth1, C. Dhanasekhar1, C.L. Huang6, H.D. Yang2,7,*, Krishnamurthy Jyothinagaram1,†, and D. Chandrasekhar Kakarla2,‡
- 1Department of Physics, School of Sciences, National Institute of Technology, Tadepalligudem 534101, Andhra Pradesh, India
- 2Department of Physics, National Sun Yat-sen University, Kaohsiung, 80424, Taiwan
- 3Institute of Physics, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan
- 4Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan
- 5National Synchrotron Radiation Research Center, Hsinchu, 30076, Taiwan
- 6Department of Physics and Center for Quantum Frontiers of Research & Technology (QFort), National Cheng Kung University, 701 Tainan, Taiwan
- 7Center of Crystal Research, National Sun Yat-sen University, Kaohsiung, 80424, Taiwan
- *Corresponding author: yang@mail.nsysu.edu.tw
- †Corresponding author: krishnamurthy@nitandhra.ac.in
- ‡Corresponding author: chandu@mail.nsysu.edu.tw
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Issue
Vol. 21, Iss. 5 — May 2024
Subject Areas
- Condensed Matter Physics
- Energy Research
- Materials Science
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![Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (11) Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (11)](https://i0.wp.com/cdn.journals.aps.org/development/journals/images/author-services-placard.png)
Images
Figure 1
(a) Isothermal dM/dH vs H curves at different temperatures for T < TN1. The inset displays isothermal M(H) data at 2K, featuring two critical fields (HC1 and HC2), (b) The H-T phase diagram for . Data points are derived from metamagnetic transitions (HC1 and HC2), and metadielectric transitions ( and ) as shown in (a) and Fig.3. Additionally, TN1 (χ), TN2 (CP), TN2(χ), TN2(ε′), and TN2 (P) data points are extracted from Ref.[27]. In (b), white represents the paramagnetic (PM) state, yellow indicates the L-FIM regime, light blue denotes the multiferroic regime, and dark blue represents an unknown phase.
Figure 2
(a) T-dependent coercive field (Hco) (left panel) and remanent magnetization (Mr) (right panel) derived from the isothermal M(H) data. (b) T-dependent in-phase (χ′) (left panel) and out-of-phase (χ″) (right panel) components of ac susceptibility for a frequency of 11Hz. (c) T-dependent χphase at different frequencies. The inset of Fig.2 shows the fit of the spin-glass temperature (Tg) to the power law (solid line) of Eq.(1).
Figure 3
Isothermal (a) dM/dH vs H curve and (b) MD (%) vs H curve at 2K. The inflection points HC1 and HC2 in the dM/dH vs H curve represent the two corresponding metamagnetic transitions. The metadielectric transitions are denoted as and , respectively. (c) T-dependent magnetoelectric coefficient (αME) for different H values.
Figure 4
(a) The T-dependent heat capacity (Cp) under 0T and the solid line in the main panel are derived from the fitted lattice term (Cphonon) described in the text and magnetic specific heat Cm (obtained by subtracting Cphonon from Cp). Inset to (a) is the T- dependent Cp in the vicinity of magnetic transition for various H values. (b) The T-dependent magnetic entropy (Sm) and Cm/T [inset to (b)] for different H.
Figure 5
(a) Magnetically induced adiabatic temperature change ΔTm vs T, (b) adiabatic temperature change due to magnetoelectric coupling ΔTME vs T, and (c) the total adiabatic temperature change ΔTtotal vs T for different H values in various temperature regimes (green, PM state; pink, L-FIM regime; and yellow, multiferroic regime).