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arXiv · 2601.16927

Strong Spin-Lattice Interaction in Layered Antiferromagnetic CrCl$_\textrm{3}$

Łucja Kipczak·Tomasz Woźniak·Chinmay K. Mohanty·Igor Antoniazzi·Jakub Iwański·Przemysław Oliwa·Jan Pawłowski·Meganathan Kalaiarasan·Zdeněk Sofer·Andrzej Wysmołek·Adam Babiński·Maciej Koperski·Maciej R. Molas
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Abstract

Understanding the coupling between lattice vibrations and magnetic order is crucial for controlling properties of two-dimensional magnetic materials. Here, we investigate the vibrational properties of bulk and thick-flake CrCl$_\textrm{3}$ using polarization-resolved Raman spectroscopy, complemented by photoluminescence, photoluminescence excitation, and optical absorption measurements. Symmetry analysis, supported by first-principles phonon calculations, enables the unambiguous assignment of all eight Raman-active modes, four $\textrm{A}_\textrm{g}$ and four $\textrm{E}_\textrm{g}$, previously predicted only theoretically. Excitation-energy-dependent measurements reveal that the strong enhancement of selected phonon modes originates primarily from interference effects rather than resonant Raman scattering. Temperature-dependent Raman spectroscopy further reveals pronounced signatures of spin-phonon coupling across the transition from a fully antiferromagnetic phase, through an intermediate regime with local, domain-like ferromagnetic order, to the paramagnetic phase, accompanied by a clear rhombohedral-to-monoclinic structural transition. Together, these results demonstrate how lattice, electronic, and magnetic degrees of freedom collectively govern the Raman response of CrCl$_\textrm{3}$.

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Łucja Kipczak, Tomasz Woźniak, Chinmay K. Mohanty, Igor Antoniazzi, Jakub Iwański, Przemysław Oliwa, Jan Pawłowski, Meganathan Kalaiarasan, Zdeněk Sofer, Andrzej Wysmołek, Adam Babiński, Maciej Koperski, Maciej R. Molas. 2026-01-23. Strong Spin-Lattice Interaction in Layered Antiferromagnetic CrCl$_\textrm{3}$. https://arxiv.org/abs/2601.16927

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