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Noncentrosymmetric triangular magnets offer a unique platform for realizing strong quantum fluctuations. However, designing these quantum materials remains an open challenge attributable to a knowledge gap in the tunability of competing exchange interactions at the atomic level. Here, a new noncentrosymmetric triangularS = 3/2 magnet CaMnTeO₆is created based on careful chemical and physical considerations. The model material displays competing magnetic interactions and features nonlinear optical responses with the capability of generating coherent photons. The incommensurate magnetic ground state of CaMnTeO₆with an unusually large spin rotation angle of 127°(1) indicates that the anisotropic interlayer exchange is strong and competing with the isotropic interlayer Heisenberg interaction. The moment of 1.39(1) µB, extracted from low‐temperature heat capacity and neutron diffraction measurements, is only 46% of the expected value of the static moment 3 µB. This reduction indicates the presence of strong quantum fluctuations in the half‐integer spinS = 3/2 CaMnTeO₆magnet, which is rare. By comparing the spin‐polarized band structure, chemical bonding, and physical properties of AMnTeO₆(A = Ca, Sr, Pb), how quantum‐chemical interpretation can illuminate insights into the fundamentals of magnetic exchange interactions, providing a powerful tool for modulating spin dynamics with atomically precise control is demonstrated.

We use neutron scattering to show that ferromagnetism and antiferromagnetism coexist in the low T state of the pyrochlore quantum magnet${\text{Yb}}_2{\text{Ti}}_2{\mathrm{O}}_7$. While magnetic Bragg peaks evidence long-range static ferromagnetic order, inelastic scattering shows that short-range correlated antiferromagnetism is also present. Small-angle neutron scattering provides direct evidence for mesoscale magnetic structure that we associate with metastable antiferromagnetism. Classical Monte Carlo simulations based on exchange interactions inferred from$⟨111⟩$-oriented high-field spin wave measurements confirm that antiferromagnetism is metastable within the otherwise ferromagnetic ground state. The apparent lack of coherent spin wave excitations and strong sensitivity to quenched disorder characterizing${\text{Yb}}_2{\text{Ti}}_2{\mathrm{O}}_7$is a consequence of this multiphase magnetism.

CrSBr is an air‐stable two‐dimensional (2D) van der Waals semiconducting magnet with great technological promise, but its atomic‐scale magnetic interactions—crucial information for high‐frequency switching—are poorly understood. An experimental study is presented to determine the CrSBr magnetic exchange Hamiltonian and bulk magnon spectrum. TheA‐type antiferromagnetic order using single crystal neutron diffraction is confirmed here. The magnon dispersions are also measured using inelastic neutron scattering and rigorously fit the excitation modes to a spin wave model. The magnon spectrum is well described by an intra‐plane ferromagnetic Heisenberg exchange model with seven nearest in‐plane exchanges. This fitted exchange Hamiltonian enables theoretical predictions of CrSBr behavior: as one example, the fitted Hamiltonian is used to predict the presence of chiral magnon edge modes with a spin‐orbit enhanced CrSBr heterostructure.