Magnetic, structural and magnetocaloric properties of Y$_{0.9}$Gd$_{0.1}$Fe$_{2}$H$_{x}$ hydrides

Abstract

At 300 K, Y$_{0.9}$Gd$_{0.1}$Fe$_{2}$H$_{x}$ hydrides crystallize sequentially with increasing H concentration in various structures related to a lowering of the cubic MgCu$_{2}$ type structure of the parent alloy: cubic C1, monoclinic M1, cubic C2, monoclinic M2, cubic C3, orthorhombic O. Above 300 K, they undergo a first-order transition at a T$_{O-D}$ temperature driven by order-disorder of hydrogen atoms into interstitial sites. Their magnetic, structural and magnetocaloric properties have been investigated through magnetic measurements, and high-resolution synchrotron diffraction experiments. The magnetization at 5 K decreases slightly from 4 to 3.8 ${\mu}_{B}$ for x = 3 to 3.9 H f.u., then with a larger slope for higher H content. A discontinuous decrease of the magnetic transition temperature is observed: M1 and C2 hydrides are ferrimagnetic with T$_{C}$ near 300 K, M2 hydride displays a sharp ferromagnetic-antiferromagnetic transition at T$_{FM-AFM}$ =144 K, whereas C3 and O hydrides present only a sharp increase of the magnetization below 15 K and a weak magnetization up to RT. Negative magnetic entropy variations (${\Delta}$S$_{M}$) are measured near T$_{C}$ for the M1 and C2 phases, near T$_{FM-AFM}$ for the M2 phase, whereas positive ${\Delta}$S$_{M}$ peaks due to inverse MCE effect are found near T$_{O-D}$. A structural and magnetic phase diagram is proposed.