Field-induced multipolar character in the dipolar ground state of the honeycomb rare-earth chalcohalide NdOF

Abstract

Field-tunable reconstruction of crystalline electric field (CEF) doublets offers a promising avenue for inducing multipolar character, while its observation in real materials has been little explored so far. Here we establish the honeycomb rare-earth chalcohalide NdOF as such a platform. Raman spectroscopy identifies four CEF excitations at 1.7, 15.6, 19.2, and 80.9~meV, and a Zeeman--CEF analysis reproduces their nonlinear field splitting into seven branches. Magnetization and susceptibility over 0.1--9~T are well described by a CEF model for the total angular momentum $J=9/2$ manifold, confirming the robustness of the extracted CEF scheme. These results demonstrate a field-driven continuous evolution of the ground-state doublet from dipolar to dipolar-multipolar character, with pressure providing a complementary tuning knob, establishing NdOF as a model system for exploring the controlled induction of multipolar components in rare-earth magnets.

7 pages, 4 figures

References in corpus (17)

• Implementation strategies in phonopy and phono3py
• Crystalline Electric Field Randomness in the Triangular Lattice Spin-Liquid YbMgGaO${}_4$
• Kitaev materials beyond iridates: order by quantum disorder and Weyl magnons in rare-earth double perovskites
• Structural and Magnetic Investigations of Single-Crystals of the Neodymium Zirconate Pyrochlore, Nd2Zr2O7
• Hidden multipolar orders of dipole-octupole doublets on a triangular lattice
• Distinguishing dipolar and octupolar quantum spin ices using contrasting magnetostriction signatures
• Rare-earth chalcohalides: A family of van der Waals layered Kitaev spin liquid candidates
• Anisotropic exchange coupling and ground state phase diagram of Kitaev compound YbOCl
• Uncovering footprints of dipolar-octupolar quantum spin ice from neutron scattering signatures
• Field-induced Kitaev multipolar liquid in spin-orbit coupled $d^2$ honeycomb Mott insulators
• Ground State Magnetic Structure and Magnetic Field Effects in the Layered Honeycomb Antiferromagnet YbOCl
• Crystalline electric field excitations and their nonlinear splitting under magnetic fields in YbOCl
• Multipolar spin liquid in an exactly solvable model for $j_{\mathrm{eff}}=\frac{3}{2}$ moments
• Magnetic Field Response of Dipolar-Octupolar Quantum Spin Ice
• Gapless spinon excitations emerging from a multipolar transverse field in the triangular-lattice Ising antiferromagnet NaTmSe2
• Anomalous enhancement of magnetism by nonmagnetic doping in the honeycomb-lattice antiferromagnet ErOCl
• Emergent Dispersive Multipolar Excitations in NaErSe${}_2$