Magnetic field-temperature phase diagram of multiferroic (NH4)2FeCl5·H2O

Amanda J. Clune; Jisoo Nam; Minseong Lee; Kendall D. Hughey; Wei Tian; Jaime A. Fernandez-Baca; Randy S. Fishman; John Singleton; Jun Hee Lee; Janice L. Musfeldt

doi:10.1038/s41535-019-0180-1

Magnetic field-temperature phase diagram of multiferroic (NH₄)₂FeCl₅·H₂O

Amanda J. Clune, Jisoo Nam, Minseong Lee, Kendall D. Hughey, Wei Tian, Jaime A. Fernandez-Baca, Randy S. Fishman, John Singleton, Jun Hee Lee, Janice L. Musfeldt

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

13 Scopus citations

Abstract

Owing to their overall low energy scales, flexible molecular architectures, and ease of chemical substitution, molecule-based multiferroics are extraordinarily responsive to external stimuli and exhibit remarkably rich phase diagrams. Even so, the stability and microscopic properties of various magnetic states in close proximity to quantum critical points are highly under-explored in these materials. Inspired by these opportunities, we combined pulsed-field magnetization, first-principles calculations, and numerical simulations to reveal the magnetic field–temperature (B–T) phase diagram of multiferroic (NH₄)₂FeCl₅⋅H₂O. In this system, a network of intermolecular hydrogen and halogen bonds creates a competing set of exchange interactions that generates additional structure in the phase diagram—both in the vicinity of the spin flop and near the 30 T transition to the fully saturated state. Consequently, the phase diagrams of (NH₄)₂FeCl₅⋅H₂O and its deuterated analog are much more complex than those of other molecule-based multiferroics. The entire series of coupled electric and magnetic transitions can be accessed with a powered magnet, opening the door to exploration and control of properties in this and related materials.

Original language	English
Article number	44
Journal	npj Quantum Materials
Volume	4
Issue number	1
DOIs	https://doi.org/10.1038/s41535-019-0180-1
State	Published - Dec 1 2019

Funding

Research at Tennessee is supported by the National Science Foundation (DMR-1707846) and the Materials Research Fund at the University of Tennessee. A portion of this work was performed at the National High Magnetic Field Laboratory, which is supported by the National Science Foundation through DMR-1644779 and the States of Florida and New Mexico. J.S. appreciates funding from Basic Energy Sciences, U.S. Department of Energy FWP “Science in 100T program”. Research at Oak Ridge National Laboratory is sponsored by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering, and Scientific User Facilities Division. J.H.L. at UNIST is supported by Basic Research Laboratory (NRF2017R1A4A1015323), Creative Materials Discovery Program (2017M3D1A1040828) of NRF, the MOTIE (Ministry of Trade, Industry Energy) (No. 10080657), and KRSC (Korea Semiconductor Research Consortium) support program. We appreciate useful conversations with Brian J. Donahoe.

Funders	Funder number
Korea Semiconductor Research Consortium
Materials Sciences and Engineering, and Scientific User Facilities Division
National Science Foundation	DMR-1644779, 1707846, DMR-1707846
U.S. Department of Energy
Office of Science
Basic Energy Sciences
University of Tennessee
Basic Research Laboratory	NRF2017R1A4A1015323, 2017M3D1A1040828
Ulsan National Institute of Science and Technology
Ministry of Trade, Industry and Energy	10080657
National Research Foundation of Korea	2017R1A4A1015323

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title = "Magnetic field-temperature phase diagram of multiferroic (NH4)2FeCl5·H2O",

abstract = "Owing to their overall low energy scales, flexible molecular architectures, and ease of chemical substitution, molecule-based multiferroics are extraordinarily responsive to external stimuli and exhibit remarkably rich phase diagrams. Even so, the stability and microscopic properties of various magnetic states in close proximity to quantum critical points are highly under-explored in these materials. Inspired by these opportunities, we combined pulsed-field magnetization, first-principles calculations, and numerical simulations to reveal the magnetic field–temperature (B–T) phase diagram of multiferroic (NH4)2FeCl5⋅H2O. In this system, a network of intermolecular hydrogen and halogen bonds creates a competing set of exchange interactions that generates additional structure in the phase diagram—both in the vicinity of the spin flop and near the 30 T transition to the fully saturated state. Consequently, the phase diagrams of (NH4)2FeCl5⋅H2O and its deuterated analog are much more complex than those of other molecule-based multiferroics. The entire series of coupled electric and magnetic transitions can be accessed with a powered magnet, opening the door to exploration and control of properties in this and related materials.",

author = "Clune, {Amanda J.} and Jisoo Nam and Minseong Lee and Hughey, {Kendall D.} and Wei Tian and Fernandez-Baca, {Jaime A.} and Fishman, {Randy S.} and John Singleton and Lee, {Jun Hee} and Musfeldt, {Janice L.}",

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AU - Tian, Wei

AU - Fernandez-Baca, Jaime A.

AU - Fishman, Randy S.

AU - Singleton, John

AU - Lee, Jun Hee

AU - Musfeldt, Janice L.

PY - 2019/12/1

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N2 - Owing to their overall low energy scales, flexible molecular architectures, and ease of chemical substitution, molecule-based multiferroics are extraordinarily responsive to external stimuli and exhibit remarkably rich phase diagrams. Even so, the stability and microscopic properties of various magnetic states in close proximity to quantum critical points are highly under-explored in these materials. Inspired by these opportunities, we combined pulsed-field magnetization, first-principles calculations, and numerical simulations to reveal the magnetic field–temperature (B–T) phase diagram of multiferroic (NH4)2FeCl5⋅H2O. In this system, a network of intermolecular hydrogen and halogen bonds creates a competing set of exchange interactions that generates additional structure in the phase diagram—both in the vicinity of the spin flop and near the 30 T transition to the fully saturated state. Consequently, the phase diagrams of (NH4)2FeCl5⋅H2O and its deuterated analog are much more complex than those of other molecule-based multiferroics. The entire series of coupled electric and magnetic transitions can be accessed with a powered magnet, opening the door to exploration and control of properties in this and related materials.

AB - Owing to their overall low energy scales, flexible molecular architectures, and ease of chemical substitution, molecule-based multiferroics are extraordinarily responsive to external stimuli and exhibit remarkably rich phase diagrams. Even so, the stability and microscopic properties of various magnetic states in close proximity to quantum critical points are highly under-explored in these materials. Inspired by these opportunities, we combined pulsed-field magnetization, first-principles calculations, and numerical simulations to reveal the magnetic field–temperature (B–T) phase diagram of multiferroic (NH4)2FeCl5⋅H2O. In this system, a network of intermolecular hydrogen and halogen bonds creates a competing set of exchange interactions that generates additional structure in the phase diagram—both in the vicinity of the spin flop and near the 30 T transition to the fully saturated state. Consequently, the phase diagrams of (NH4)2FeCl5⋅H2O and its deuterated analog are much more complex than those of other molecule-based multiferroics. The entire series of coupled electric and magnetic transitions can be accessed with a powered magnet, opening the door to exploration and control of properties in this and related materials.

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Magnetic field-temperature phase diagram of multiferroic (NH₄)₂FeCl₅·H₂O

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