Raman Scattering Evidence for Fluctuating Kagome-Plane Moments in B ∥ [111] in Pr2Zr2O7 pyrochlore
Abstract
The exotic magnetic properties of the pyrochlore Pr2Zr2O7 are determined by the coupling of spin, orbital, and lattice degrees of freedom. Magnetism in this material originates from the non-Kramers Pr3+ ion, and the exotic behavior has been discussed both in the framework of dipole-quadrupole properties of magnetic moments and disorder splitting the non-Kramers doublet. We use magneto-Raman spectroscopy to probe the crystal electric field (CEF) excitations of Pr3+ in magnetic fields up to 14 T applied along the [100] and [111] crystallographic directions at 2 K. For B∥[100], the field evolution of the Raman active crystal field modes is quantitatively described by conventional Zeeman splitting of the Pr3+ ground state doublet, including the thermally populated upper Zeeman branch at elevated temperature. For B∥[111], the spectra separate into responses from the triangular and kagome sublattices, and the CEF excitations of Pr3+ on the triangular lattice exhibit the expected Zeeman shift consistent with full moments polarization. In contrast, the CEF excitations of Pr3+ on the kagome lattice do not split as expected and instead broaden strongly with increasing field. This behavior is inconsistent with a static polarized configuration and is captured phenomenologically by a motional-narrowing description in which the kagome plane moments fluctuate between Zeeman-split levels on a meV timescale. This result offers a natural explanation for the reduced magnetization observed in B∥[111] and provides further evidence of the dipole-quadrupole properties of magnetic moments. It highlights Raman scattering as a sensitive probe of exotic spin-orbital dynamics in frustrated magnets.
Related
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BibTeX
@misc{xu2026raman,
title = {{Raman Scattering Evidence for Fluctuating Kagome-Plane Moments in $\mathrmB \parallel [111]$ in Pr$_2$Zr$_2$O$_7$ pyrochlore}},
author = {Yuanyuan Xu and Huiyuan Man and Nan Tang and Li Xiang and Sami Muhammad and Komalavalli Thirunavukkuarasu and Dmitry Smirnov and Satoru Nakatsuji and Natalia Drichko},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.24696},
eprint = {2609.24696},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.24696},
}
RIS
TY - UNPB
TI - Raman Scattering Evidence for Fluctuating Kagome-Plane Moments in B ∥ [111] in Pr_2Zr_2O_7 pyrochlore
AU - Yuanyuan Xu
AU - Huiyuan Man
AU - Nan Tang
AU - Li Xiang
AU - Sami Muhammad
AU - Komalavalli Thirunavukkuarasu
AU - Dmitry Smirnov
AU - Satoru Nakatsuji
AU - Natalia Drichko
PY - 2026
DA - 2026/09/21
PB - arXiv
DO - 10.48550/arxiv.2609.24696
UR - https://arxiv.org/abs/2609.24696
AB - The exotic magnetic properties of the pyrochlore Pr_2Zr_2O_7 are determined by the coupling of spin, orbital, and lattice degrees of freedom. Magnetism in this material originates from the non-Kramers Pr^3+ ion, and the exotic behavior has been discussed both in the framework of dipole-quadrupole properties of magnetic moments and disorder splitting the non-Kramers doublet. We use magneto-Raman spectroscopy to probe the crystal electric field (CEF) excitations of Pr^3+ in magnetic fields up to 14 T applied along the [100] and [111] crystallographic directions at 2 K. For B∥[100], the field evolution of the Raman active crystal field modes is quantitatively described by conventional Zeeman splitting of the Pr^3+ ground state doublet, including the thermally populated upper Zeeman branch at elevated temperature. For B∥[111], the spectra separate into responses from the triangular and kagome sublattices, and the CEF excitations of Pr^3+ on the triangular lattice exhibit the expected Zeeman shift consistent with full moments polarization. In contrast, the CEF excitations of Pr^3+ on the kagome lattice do not split as expected and instead broaden strongly with increasing field. This behavior is inconsistent with a static polarized configuration and is captured phenomenologically by a motional-narrowing description in which the kagome plane moments fluctuate between Zeeman-split levels on a meV timescale. This result offers a natural explanation for the reduced magnetization observed in B∥[111] and provides further evidence of the dipole-quadrupole properties of magnetic moments. It highlights Raman scattering as a sensitive probe of exotic spin-orbital dynamics in frustrated magnets.
ER -