The coexistence of electrical and magnetic orders with intrinsic coupling, known as magnetoelectric coupling in multiferroics, has been extensively studied in oxide supplies however stays comparatively unexplored in van der Waals supplies. Amongst these, CuCrP2S6 (CCPS) is notable for its emergent antiferromagnetic (AFM) and antiferroelectric (AFE) traits. Nevertheless, investigations into magnetoelectric coupling in CCPS are restricted, and the consequences of dopants on its magnetic properties have but to be absolutely addressed. On this research, we synthesized CuCr1−xFexP2S6 (CCFPS) samples utilizing the chemical vapor transport (CVT) methodology to research the affect of iron doping on the magnetic and nonlinear optical properties of the CCFPS system. Our outcomes point out that the AFM state is preserved, whereas the Néel temperature (TN) varies with the doping focus. First-principles calculations had been employed to evaluate the trade interactions amongst magnetic atoms. Notably, for samples with doping concentrations x < 0.5, we noticed each magnetic-dielectric coupling and second harmonic technology (SHG) results. Nevertheless, these results had been absent at increased doping ranges. Moreover, our evaluation revealed a definite odd–even dependence of SHG, suggesting the presence of interlayer symmetry-breaking coupling. These findings advance our understanding of two-dimensional (2D) multiferroic supplies and lay the groundwork for designing and optimizing magnetoelectric coupling supplies with enhanced efficiency.
