Dimensional crossover in a layered ferromagnet detected by spin correlation driven distortions

Abstract

Magneto-elastic distortions are commonly detected across magnetic long-range ordering (LRO) transitions. In principle, they are also induced by the magnetic short-range ordering (SRO) that precedes a LRO transition, which contains information about short-range correlations and energetics that are essential for understanding how LRO is established. However these distortions are difficult to resolve because the associated atomic displacements are exceedingly small and do not break symmetry. Here we demonstrate high-multipole nonlinear optical polarimetry as a sensitive and mode selective probe of SRO induced distortions using CrSiTe${}_3$ as a testbed. This compound is composed of weakly bonded sheets of nearly isotropic ferromagnetically interacting spins that, in the Heisenberg limit, would individually be impeded from LRO by the Mermin-Wagner theorem. Our results show that CrSiTe${}_3$ evades this law via a two-step crossover from two- to three-dimensional magnetic SRO, manifested through two successive and previously undetected totally symmetric distortions above its Curie temperature.

arXiv comment17 pages main text, 4 figures, 12 pages supplementary information

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Cited by in corpus (18)

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• Direct imaging of antiferromagnetic domains and anomalous layer-dependent mirror symmetry breaking in atomically thin MnPS${}_3$
• Direct observation of the energy gain underpinning ferromagnetic superexchange in the electronic structure of CrGeTe${}_3$
• Anomalous mirror symmetry breaking in a model insulating cuprate Sr${}_2$CuO${}_2$Cl${}_2$
• Ultrafast enhancement of ferromagnetic spin exchange induced by ligand-to-metal charge transfer
• Selection rules in symmetry-broken systems by symmetries in synthetic dimensions
• Electric quadrupole second harmonic generation revealing dual magnetic orders in a magnetic Weyl semimetal
• Spin-phonon scattering-induced low thermal conductivity in a van der Waals layered ferromagnet Cr${}_2$Si${}_2$Te${}_6$
• Observation of enhanced spin-spin correlations at triple point in 2D ferromagnetic Cr2X2Te6 (X=Si, Ge)
• Two-Step Electronic Response to Magnetic Ordering in a van der Waals Ferromagnet
• Evidence for an extended critical fluctuation region above the polar ordering transition in LiOsO${}_3$
• Pressure tuning of intrinsic and extrinsic sources to the anomalous Hall effect in CrGeTe${}_3$
• Spontaneously formed phonon frequency combs in van der Waals solid CrXTe${}_3$ (X=Ge,Si)
• In-plane anisotropy of charge density wave fluctuations in 1$T$-TiSe${}_2$
• Evidence for distortion-induced local electric polarization in $\alpha$-RuCl${}_3$
• Wideband covariance magnetometry below the diffraction limit
• Probing of magnetic dimensional crossover in CrSiTe${}_3$ through picosecond strain pulses
• Triplet resonating valence bond theory and transition metal chalcogenides