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Title: Nonreciprocal directional dichroism of a chiral magnet in the visible range

Abstract

Nonreciprocal directional dichroism is an unusual light–matter interaction that gives rise to diode-like behavior in low-symmetry materials. The chiral varieties are particularly scarce due to the requirements for strong spin–orbit coupling, broken time-reversal symmetry, and a chiral axis. Here we bring together magneto-optical spectroscopy and first-principles calculations to reveal high-energy, broadband nonreciprocal directional dichroism in Ni3TeO6 with special focus on behavior in the metamagnetic phase above 52 T. In addition to demonstrating this effect in the magnetochiral configuration, we explore the transverse magnetochiral orientation in which applied field and light propagation are orthogonal to the chiral axis and, by so doing, uncover an additional configuration with a unique nonreciprocal response in the visible part of the spectrum. In a significant conceptual advance, we use first-principles methods to analyze how the Ni2+ d-to-d on-site excitations develop magneto-electric character and present a microscopic model that unlocks the door to theory-driven discovery of chiral magnets with nonreciprocal properties.

Authors:
 [1]; ORCiD logo [2];  [1];  [3];  [4];  [1];  [5];  [4]; ORCiD logo [3];  [6]; ORCiD logo [3]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Rutgers Univ., Piscataway, NJ (United States); Kangwon National Univ., Chuncheon (Korea, Republic of)
  3. Rutgers Univ., Piscataway, NJ (United States)
  4. Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab)
  5. Central Michigan Univ., Mount Pleasant, MI (United States)
  6. Rutgers Univ., Piscataway, NJ (United States); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE
OSTI Identifier:
1630856
Report Number(s):
LA-UR-19-28258
Journal ID: ISSN 2397-4648; TRN: US2200700
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
npj Quantum Materials
Additional Journal Information:
Journal Volume: 5; Journal Issue: 1; Journal ID: ISSN 2397-4648
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; High Magnetic Field Science

Citation Formats

Yokosuk, Michael O., Kim, Heung-Sik, Hughey, Kendall D., Kim, Jaewook, Stier, Andreas V., O’Neal, Kenneth R., Yang, Junjie, Crooker, Scott A., Haule, Kristjan, Cheong, Sang-Wook, Vanderbilt, David, and Musfeldt, Janice L. Nonreciprocal directional dichroism of a chiral magnet in the visible range. United States: N. p., 2020. Web. doi:10.1038/s41535-020-0224-6.
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Yokosuk, Michael O., Kim, Heung-Sik, Hughey, Kendall D., Kim, Jaewook, Stier, Andreas V., O’Neal, Kenneth R., Yang, Junjie, Crooker, Scott A., Haule, Kristjan, Cheong, Sang-Wook, Vanderbilt, David, & Musfeldt, Janice L. Nonreciprocal directional dichroism of a chiral magnet in the visible range. United States. https://doi.org/10.1038/s41535-020-0224-6
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Yokosuk, Michael O., Kim, Heung-Sik, Hughey, Kendall D., Kim, Jaewook, Stier, Andreas V., O’Neal, Kenneth R., Yang, Junjie, Crooker, Scott A., Haule, Kristjan, Cheong, Sang-Wook, Vanderbilt, David, and Musfeldt, Janice L. Fri . "Nonreciprocal directional dichroism of a chiral magnet in the visible range". United States. https://doi.org/10.1038/s41535-020-0224-6. https://www.osti.gov/servlets/purl/1630856.
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@article{osti_1630856,
title = {Nonreciprocal directional dichroism of a chiral magnet in the visible range},
author = {Yokosuk, Michael O. and Kim, Heung-Sik and Hughey, Kendall D. and Kim, Jaewook and Stier, Andreas V. and O’Neal, Kenneth R. and Yang, Junjie and Crooker, Scott A. and Haule, Kristjan and Cheong, Sang-Wook and Vanderbilt, David and Musfeldt, Janice L.},
abstractNote = {Nonreciprocal directional dichroism is an unusual light–matter interaction that gives rise to diode-like behavior in low-symmetry materials. The chiral varieties are particularly scarce due to the requirements for strong spin–orbit coupling, broken time-reversal symmetry, and a chiral axis. Here we bring together magneto-optical spectroscopy and first-principles calculations to reveal high-energy, broadband nonreciprocal directional dichroism in Ni3TeO6 with special focus on behavior in the metamagnetic phase above 52 T. In addition to demonstrating this effect in the magnetochiral configuration, we explore the transverse magnetochiral orientation in which applied field and light propagation are orthogonal to the chiral axis and, by so doing, uncover an additional configuration with a unique nonreciprocal response in the visible part of the spectrum. In a significant conceptual advance, we use first-principles methods to analyze how the Ni2+ d-to-d on-site excitations develop magneto-electric character and present a microscopic model that unlocks the door to theory-driven discovery of chiral magnets with nonreciprocal properties.},
doi = {10.1038/s41535-020-0224-6},
journal = {npj Quantum Materials},
number = 1,
volume = 5,
place = {United States},
year = {Fri Apr 03 00:00:00 EDT 2020},
month = {Fri Apr 03 00:00:00 EDT 2020}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41535-020-0224-6
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Cited by: 18 works
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Figures / Tables:

Fig. 1 Fig. 1: Phase diagram, optical properties, and measurement geometries of Ni3TeO6. a Comprehensive H–T phase diagram for H ∥ c. AFM, antiferromagnet; SF, spin flop, MM, metamagnetic. The phase diagram in the transverse configuration exhibits only gradual canting with increasing field. b Optical absorption spectrum of Ni3TeO6. The on-site Nimore » d-to-d excitations are labeled. c Schematic representation of magnetochiral dichroism. This measurement orientation requires a chiral axis in the material as well as light (±k) and magnetic field ±H aligned along the chiral direction in the Faraday geometry. The nonreciprocal effect will depend upon light propagation and field direction. The symmetry considerations are fully discussed in the Supplementary Information. d Image of the ab-plane sample under crossed linear polarizer and analyzer. The red circle indicates the position of the light spot, which is within a single chiral domain. e Optical rotation measurement using crossed polarizer and analyzer. The angle Θ corresponds to the angle between the analyzer and normal from the polarizer. The red symbols correspond to the lighter green portion of the crystal and the blue symbols correspond to the darker green portion in the corners. f The nonreciprocal effect also occurs in the transverse magnetochiral orientation. Here we maintain the Faraday geometry (with ±k and ±H) but the chiral (c) axis is in the plane of the polished crystal. The symmetry considerations of this unique geometry are discussed in the Supplementary Information. g Photographic image in which the c-axis is in the plane of the polished crystal under crossed linear polarizer and analyzer. The red circle indicates the measurement region, which is within a single chiral domain.« less
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