Magnetic property changes of NdGa upon hydrogen absorption

Rare earth monogallide (REGa) Zintl phases are attractive for their properties in hydrogen storage and magnetic cooling. However, the magnetic effects upon hydrogen additions in REGa are not well understood. This study aims to explore the magnetic effects in <a:math xmlns:a="http://www.w3.org/1998/Math/MathML"><a:msub><a:mi>REGaH</a:mi><a:mi mathvariant="normal">x</a:mi></a:msub></a:math> using SQUID magnetometry and neutron powder diffraction. To avoid challenges due to absorption and high incoherent scattering in the neutron diffraction experiments, the compound <c:math xmlns:c="http://www.w3.org/1998/Math/MathML"><c:msub><c:mi>NdGaD</c:mi><c:mi>x</c:mi></c:msub></c:math> (<d:math xmlns:d="http://www.w3.org/1998/Math/MathML"><d:mi>x</d:mi></d:math> = 0, 0.9, or 1.6) was chosen for examination. It was found that NdGa exhibits two ferromagnetic structures below the Curie temperature of 42 K. Just below 42 K the magnetic moments are oriented along the crystallographic <e:math xmlns:e="http://www.w3.org/1998/Math/MathML"><e:mi>c</e:mi></e:math> axis, and at 20 K a spin reorientation occurs where the moments turn <f:math xmlns:f="http://www.w3.org/1998/Math/MathML"><f:mrow><f:mo>∼</f:mo><f:msup><f:mn>30</f:mn><f:mo>∘</f:mo></f:msup></f:mrow></f:math> toward the <g:math xmlns:g="http://www.w3.org/1998/Math/MathML"><g:mi>a</g:mi></g:math> axis. Upon partial deuteration (<h:math xmlns:h="http://www.w3.org/1998/Math/MathML"><h:mi>x</h:mi></h:math> = 0.9), the magnetization decreases and two magnetic phases are observed, one intermediate incommensurate phase, and one canted ferromagnetic phase with the net magnetization aligning along the <i:math xmlns:i="http://www.w3.org/1998/Math/MathML"><i:mi>b</i:mi></i:math> axis. For the full deuteride (<j:math xmlns:j="http://www.w3.org/1998/Math/MathML"><j:mi>x</j:mi></j:math> = 1.6) only one incommensurate magnetic phase is observed at low temperatures. Magnetometry also reveals that there are no isotope effects when absorbing H or D. The absorption of H or D changes the Nd-Nd distances as well as the electronic structure, which results in a drastic change in the magnetic properties as compared to NdGa. Published by the American Physical Society 2024