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 CrSiTe3 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 CrSiTe3 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.
This technique will be particularly useful for studying anisotropic or geometrically frustrated magnetic systems, which tend to display interesting short-range spin correlations. It will also be useful for uncovering magnetic ordering mechanisms in monolayer or few layer ferromagnetic and antiferromagnetic nanoscale flakes and devices26,27,28,29, which are often unclear because of their inaccessibility by neutron diffraction. We anticipate that access to this type of information may offer new strategies to control magnetism based on manipulating SRO induced distortions through chemical synthesis, static perturbations or even out-of-equilibrium excitations30.
Read the full paper A. Ron, E. Zoghlin, L. Balents, S.D. Wilson, D. Hsieh (2019) Dimensional crossover in a layered ferromagnet detected by spin correlation driven distortions. Nature Communications, 10 . Art. No. 1654.
See Figure 4. Hyper-polarizable bond model and dimensional crossover. Plots show hyper-polarizable bond model calculations of the change in each of the eight allowed SHG susceptibility tensor elements relative to their undistorted values
