The results of magnetic measurements, electron spin resonance, heat capacity, resistivity, and magnetocaloric effect as well as density functional theory (DFT), are presented for the compound NdRh2 (MgCu2-type structure). This compound was synthesized at a pressure of 8 GPa and a temperature of 1700 K. The magnetic properties of the material are shown to be determined by the high-temperature (over 400 K) spin polarization of the 4d Rh electrons and by the ferrimagnetic (FiM) interaction of Rh and Nd magnetic subsystems. Concurrently, the spontaneous magnetization of the spin polarization of 4d Rh electrons is ≈0.01μB/Rh, while the Nd magnetic moment is ≈1.7μB/Nd. This leads to complicated magnetic behavior with long range FiM order at TC≲7 K at zero field and with wide temperature range of spin fluctuations TC<T≲50 K. Specific heat and resistivity data provide corroboration of the spin fluctuation regime with the spin fluctuation temperature Θsf≈28.5 K. The optimal critical parameters were identified as β=1.18±0.02, γ=0.85±0.02, and TC≈40 K from modified Arrott plotting, which are distinct from any conventional universality class. The maximum magnetocaloric effect, when the magnetic field changes from 0 to 9 T, ΔH=9 T occurs at T≈11 K and the magnetic entropy change reaches −ΔSm=7.0 J (kg K)−1. In our DFT calculations, the FiM arrangement was obtained, with values of magnetic moments of Nd and Rh. Additionally, the Fermi surface was constructed.
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