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arXiv · 2412.07913

Spin-Orbital-Lattice Coupling and the Phonon Zeeman Effect in the Dirac Honeycomb Magnet CoTiO$_3$

Abstract

The entanglement of electronic spin and orbital degrees of freedom is often the precursor to emergent behaviors in condensed matter systems. With considerable spin-orbit coupling strength, the cobalt atom on a honeycomb lattice offers a platform that can make accessible the study of novel magnetic ground states. Using temperature-dependent Raman spectroscopy and high-magnetic field Raman and infrared (IR) spectroscopy, we studied the lattice and spin-orbital excitations in CoTiO$_3$, an antiferromagnetic material that exhibits topologically protected magnon Dirac crossings in the Brillouin zone. Under the application of an external magnetic field up to 22 T along the crystal's $c$-axis, we observed the splitting of both the spin-orbital excitations and a phonon nearby in energy. Using density functional theory (DFT), we identify a number of new modes that below the antiferromagnetic (AFM) transition become Raman-active due to the zone-folding of the Brillouin zone caused by the doubling of the magnetic unit cell. We use a model that includes both the spin and orbital degrees of freedom of the Co$^{2+}$ ions to explain the spin-orbital excitation energies and their behavior in an applied field. Our experimental observations along with several deviations from the model behavior point to significant coupling between the spin-orbital and the lattice excitations.

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Thuc T. Mai, Yufei Li, K. F. Garrity, D. Shaw, T. DeLazzer, R. L. Dally, T. Adel, M. F. Muñoz, 1 A. Giovannone, C. Lyon, A. Pawbake, C. Faugeras, F. Le Mardele, M. Orlita, J. R. Simpson, K. Ross, R. Valdés Aguilar, A. R. Hight Walker. 2024-12-10. Spin-Orbital-Lattice Coupling and the Phonon Zeeman Effect in the Dirac Honeycomb Magnet CoTiO$_3$. https://arxiv.org/abs/2412.07913

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