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Title: Spin–lattice and electron–phonon coupling in 3d/5d hybrid Sr3NiIrO6

Abstract

While 3d-containing materials display strong electron correlations, narrow band widths, and robust magnetism, 5d systems are recognized for strong spin–orbit coupling, increased hybridization, and more diffuse orbitals. Combining these properties leads to novel behavior. Sr3NiIrO6, for example, displays complex magnetism and ultra-high coercive fields—up to an incredible 55 T. Here, we combine infrared and optical spectroscopies with high-field magnetization and first-principles calculations to explore the fundamental excitations of the lattice and related coupling processes including spin–lattice and electron–phonon mechanisms. Magneto-infrared spectroscopy reveals spin–lattice coupling of three phonons that modulate the Ir environment to reduce the energy required to modify the spin arrangement. While these modes primarily affect exchange within the chains, analysis also uncovers important inter-chain motion. This provides a mechanism by which inter-chain interactions can occur in the developing model for ultra-high coercivity. At the same time, analysis of the on-site Ir4+ excitations reveals vibronic coupling and extremely large crystal field parameters that lead to a t2g-derived low-spin state for Ir. These findings highlight the spin–charge–lattice entanglement in Sr3NiIrO6 and suggest that similar interactions may take place in other 3d/5d hybrids.

Authors:
ORCiD logo; ; ; ; ; ; ; ORCiD logo; ; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC). Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1619757
Alternate Identifier(s):
OSTI ID: 1558967
Report Number(s):
LA-UR-18-31654
Journal ID: ISSN 2397-4648; 48; PII: 184
Grant/Contract Number:  
FG02-01ER45885; 89233218CNA000001
Resource Type:
Published Article
Journal Name:
npj Quantum Materials
Additional Journal Information:
Journal Name: npj Quantum Materials Journal Volume: 4 Journal Issue: 1; Journal ID: ISSN 2397-4648
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
36 MATERIALS SCIENCE; High Magnetic Field Science

Citation Formats

O’Neal, Kenneth R., Paul, Arpita, al-Wahish, Amal, Hughey, Kendall D., Blockmon, Avery L., Luo, Xuan, Cheong, Sang-Wook, Zapf, Vivien S., Topping, Craig V., Singleton, John, Ozerov, Mykhalo, Birol, Turan, and Musfeldt, Janice L. Spin–lattice and electron–phonon coupling in 3d/5d hybrid Sr3NiIrO6. United Kingdom: N. p., 2019. Web. https://doi.org/10.1038/s41535-019-0184-x.
O’Neal, Kenneth R., Paul, Arpita, al-Wahish, Amal, Hughey, Kendall D., Blockmon, Avery L., Luo, Xuan, Cheong, Sang-Wook, Zapf, Vivien S., Topping, Craig V., Singleton, John, Ozerov, Mykhalo, Birol, Turan, & Musfeldt, Janice L. Spin–lattice and electron–phonon coupling in 3d/5d hybrid Sr3NiIrO6. United Kingdom. https://doi.org/10.1038/s41535-019-0184-x
O’Neal, Kenneth R., Paul, Arpita, al-Wahish, Amal, Hughey, Kendall D., Blockmon, Avery L., Luo, Xuan, Cheong, Sang-Wook, Zapf, Vivien S., Topping, Craig V., Singleton, John, Ozerov, Mykhalo, Birol, Turan, and Musfeldt, Janice L. Wed . "Spin–lattice and electron–phonon coupling in 3d/5d hybrid Sr3NiIrO6". United Kingdom. https://doi.org/10.1038/s41535-019-0184-x.
@article{osti_1619757,
title = {Spin–lattice and electron–phonon coupling in 3d/5d hybrid Sr3NiIrO6},
author = {O’Neal, Kenneth R. and Paul, Arpita and al-Wahish, Amal and Hughey, Kendall D. and Blockmon, Avery L. and Luo, Xuan and Cheong, Sang-Wook and Zapf, Vivien S. and Topping, Craig V. and Singleton, John and Ozerov, Mykhalo and Birol, Turan and Musfeldt, Janice L.},
abstractNote = {While 3d-containing materials display strong electron correlations, narrow band widths, and robust magnetism, 5d systems are recognized for strong spin–orbit coupling, increased hybridization, and more diffuse orbitals. Combining these properties leads to novel behavior. Sr3NiIrO6, for example, displays complex magnetism and ultra-high coercive fields—up to an incredible 55 T. Here, we combine infrared and optical spectroscopies with high-field magnetization and first-principles calculations to explore the fundamental excitations of the lattice and related coupling processes including spin–lattice and electron–phonon mechanisms. Magneto-infrared spectroscopy reveals spin–lattice coupling of three phonons that modulate the Ir environment to reduce the energy required to modify the spin arrangement. While these modes primarily affect exchange within the chains, analysis also uncovers important inter-chain motion. This provides a mechanism by which inter-chain interactions can occur in the developing model for ultra-high coercivity. At the same time, analysis of the on-site Ir4+ excitations reveals vibronic coupling and extremely large crystal field parameters that lead to a t2g-derived low-spin state for Ir. These findings highlight the spin–charge–lattice entanglement in Sr3NiIrO6 and suggest that similar interactions may take place in other 3d/5d hybrids.},
doi = {10.1038/s41535-019-0184-x},
journal = {npj Quantum Materials},
number = 1,
volume = 4,
place = {United Kingdom},
year = {2019},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
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https://doi.org/10.1038/s41535-019-0184-x

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