Chemically Tuning Interlayer Coupling and Coherent Light Generation in AMTeO₆ Triangular Magnets

2-D triangular magnets with broken spatial inversion symmetry can uniquely offer the precision and tunability needed to meet the demands of spin–photon architectures for the second quantum revolution. While the intralayer coupling (<i>J</i>₁) within 2-D triangular spin lattice has been studied, a largely unexplored question is how the interlayer ionic/covalent bonding influences the electronic structure and interlayer interaction (<i>J</i>₂) of the low-dimensional magnets. To address this, we created a new material CaMnTeO₆ and surveyed AMTeO₆ systems (A = s⁰, s², and d⁰ cations; M = Mn, Cr) materials, in which the <i>S</i> = 3/2 transition-metal ion M site forms a 2-D triangular lattice and separated by the A site. CaMnTeO₆features an incommensurate magnetic ground state with AFM in the ab-plane and spiral FM along the c-axis. In addition, this new 2-D magnet exhibits nonlinear optical responses, a prerequisite for integrating spin–photon constructs. We supplemented the results of the structural and physical properties characterization with band structure and chemical bonding. In this talk, we will share our understanding of how the electronic structure of the A site affects the interlayer magnetic coupling of AMTeO₆ materials and their ability to generate coherent photons.