Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}

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Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${Fe}_{2} ({Mo O}_{4})_{3}$

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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$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (1)$

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$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (2)$

Abstract

${Fe}_{2} ({Mo O}_{4})_{3}$ is a well-established L-type ferrimagnetic (L-FIM) material with field-induced magnetic ordering ( $T_{N 2}$ ) and multiferroic properties below $T_{N 1}$ (around 12K). In this study, we investigate the magnetic properties of ${Fe}_{2} ({Mo O}_{4})_{3}$ through temperature- and field-dependent ac and dc magnetic susceptibility $χ (T)$ measurements. Isothermal magnetization data reveal an additional metamagnetic transition ( $H_{C 2}$ ) beyond the existing boundary between L-FIM and multiferroic phases ( $H_{C 1}$ ). Frequency-dependent ac magnetic susceptibility data demonstrate reentrant-spin-glass-like behavior below $T_{N 1}$ , with a critical temperature ( $T_{g 0}$ ) of 6.2K. Notably, a nonlinear magnetodielectric response and concurrent anomalies in M(H) at the two metamagnetic transitions ( $H_{C 1}$ and $H_{C 2}$ ) allude to a profoundly intertwined magnetoelectric (ME) nature. A finite nonlinear ME effect ( $α_{ME}$ ) of about 0.56ps/m is comparable to that of ME materials such as ${Nd Cr Ti O}_{5}$ and ${Mn Ga}_{2} O_{4}$ . The temperature-dependent adiabatic temperature change (Δ $T_{m}$ ) 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 $T_{ME}$ ) owing to magnetoelectric coupling is quite large (5.2K under a 7T magnetic field) near $T_{N 2}$ . The tunability of $T_{N 2}$ 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.

$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (3)$
$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (4)$
$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (5)$
$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (6)$
$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (7)$

Received 30 November 2023
Revised 7 February 2024
Accepted 22 April 2024

DOI:https://doi.org/10.1103/PhysRevApplied.21.054025

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. Lin^3,4, Nidhi Puri³, C.W. Wang⁵, C. H. Prashanth¹, C. Dhanasekhar¹, C.L. Huang⁶, H.D. Yang^2,7,*, Krishnamurthy Jyothinagaram^1,†, and D. Chandrasekhar Kakarla^2,‡

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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Vol. 21, Iss. 5 — May 2024

Subject Areas

Condensed Matter Physics
Energy Research
Materials Science

$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (8)$

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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)$

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$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (12)$
Figure 1
(a) Isothermal dM/dH vs H curves at different temperatures for T < T_N1. The inset displays isothermal M(H) data at 2K, featuring two critical fields (H_C1 and H_C2), (b) The H-T phase diagram for ${Fe}_{2} ({Mo O}_{4})_{3}$ . Data points are derived from metamagnetic transitions (H_C1 and H_C2), and metadielectric transitions ( $H_{ε^{'} C 1}$ and $H_{ε^{'} C 2}$ ) as shown in (a) and Fig.3. Additionally, T_N1 (χ), T_N2 (C_P), T_N2(χ), T_N2(ε′), and T_N2 (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.
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$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (13)$
Figure 2
(a) T-dependent coercive field (H_co) (left panel) and remanent magnetization (M_r) (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 χ_phase at different frequencies. The inset of Fig.2 shows the fit of the spin-glass temperature (T_g) to the power law (solid line) of Eq.(1).
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$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (14)$
Figure 3
Isothermal (a) dM/dH vs H curve and (b) MD (%) vs H curve at 2K. The inflection points H_C1 and H_C2 in the dM/dH vs H curve represent the two corresponding metamagnetic transitions. The metadielectric transitions are denoted as $H_{ε^{'} C 1}$ and $H_{ε^{'} C 2}$ , respectively. (c) T-dependent magnetoelectric coefficient (α_ME) for different H values.
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$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (15)$
Figure 4
(a) The T-dependent heat capacity (C_p) under 0T and the solid line in the main panel are derived from the fitted lattice term (C_phonon) described in the text and magnetic specific heat C_m (obtained by subtracting C_phonon from C_p). Inset to (a) is the T- dependent C_p in the vicinity of magnetic transition for various H values. (b) The T-dependent magnetic entropy (S_m) and C_m/T [inset to (b)] for different H.
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$Hidden magnetism, nonlinear magnetodielectric coupling, and large multicaloric effect in multiferroic L-type ${\mathrm{Fe}}_{2}({\mathrm{Mo}\mathrm{O}}_{4}{)}_{3}$ (16)$
Figure 5
(a) Magnetically induced adiabatic temperature change ΔT_m vs T, (b) adiabatic temperature change due to magnetoelectric coupling ΔT_ME vs T, and (c) the total adiabatic temperature change ΔT_total vs T for different H values in various temperature regimes (green, PM state; pink, L-FIM regime; and yellow, multiferroic regime).
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