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Title: High-field/high-frequency electron spin resonances of Fe-doped β−Ga2O3 by terahertz generalized ellipsometry: Monoclinic symmetry effects
We demonstrate detection and measurement of electron paramagnetic spin resonances (EPR) of iron defects in β Ga 2 O 3 utilizing generalized ellipsometry at frequencies between 110 and 170 GHz. The experiments are performed on an Fe-doped single crystal in a free-beam configuration in reflection at 45 and magnetic fields between 3 and 7 T. In contrast with low-field, low-frequency EPR measurements, we observe all five transitions of the s = 5 / 2 high-spin state Fe 3 + simultaneously. We confirm that ferric Fe 3 + is predominantly found at octahedrally coordinated Ga sites. We obtain the full set of fourth-order monoclinic zero-field splitting parameters for both octahedrally and tetrahedrally coordinated sites by employing measurements at multiple sample azimuth rotations. The capability of high-field EPR allows us to demonstrate that simplified second-order orthorhombic spin Hamiltonians are insufficient, and fourth-order terms as well as consideration of the monoclinic symmetry are needed. These findings are supported by computational approaches based on density-functional theory for second-order and on ligand-field theory for fourth-order parameters of the spin Hamiltonian. Terahertz ellipsometry is a way to measure spin resonances in a cavity-free setup. Its possibility of varying the probe frequency arbitrarily without otherwise changing the experimental setup offers unique means of truly disentangling different components of highly anisotropic spin Hamiltonians. Published by the American Physical Society2024  more » « less
Award ID(s):
2044049
PAR ID:
10636519
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
Physical Review B
Date Published:
Journal Name:
Physical Review B
Volume:
109
Issue:
21
ISSN:
2469-9950
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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