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

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Main Authors: Kipczak, Łucja, Woźniak, Tomasz, Mohanty, Chinmay K., Antoniazzi, Igor, Iwański, Jakub, Oliwa, Przemysław, Pawłowski, Jan, Kalaiarasan, Meganathan, Sofer, Zdeněk, Wysmołek, Andrzej, Babiński, Adam, Koperski, Maciej, Molas, Maciej R.
Format: Preprint
Published: 2026
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author Kipczak, Łucja
Woźniak, Tomasz
Mohanty, Chinmay K.
Antoniazzi, Igor
Iwański, Jakub
Oliwa, Przemysław
Pawłowski, Jan
Kalaiarasan, Meganathan
Sofer, Zdeněk
Wysmołek, Andrzej
Babiński, Adam
Koperski, Maciej
Molas, Maciej R.
author_facet Kipczak, Łucja
Woźniak, Tomasz
Mohanty, Chinmay K.
Antoniazzi, Igor
Iwański, Jakub
Oliwa, Przemysław
Pawłowski, Jan
Kalaiarasan, Meganathan
Sofer, Zdeněk
Wysmołek, Andrzej
Babiński, Adam
Koperski, Maciej
Molas, Maciej R.
contents 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$_\textrm{3}$.
format Preprint
id arxiv_https___arxiv_org_abs_2601_16927
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Strong Spin-Lattice Interaction in Layered Antiferromagnetic CrCl$_\textrm{3}$
Kipczak, Łucja
Woźniak, Tomasz
Mohanty, Chinmay K.
Antoniazzi, Igor
Iwański, Jakub
Oliwa, Przemysław
Pawłowski, Jan
Kalaiarasan, Meganathan
Sofer, Zdeněk
Wysmołek, Andrzej
Babiński, Adam
Koperski, Maciej
Molas, Maciej R.
Materials Science
Mesoscale and Nanoscale Physics
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$_\textrm{3}$.
title Strong Spin-Lattice Interaction in Layered Antiferromagnetic CrCl$_\textrm{3}$
topic Materials Science
Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2601.16927