Role of “Dumbbell” Pairs of Fe in Spin Alignments and Negative Thermal Expansion of Lu2Fe17-Based Intermetallic Compounds

Knowledge of negative thermal expansion (NTE) is an interesting issue in the field of materials science and engineering. It has been proposed that the unique dumbbell pairs of Fe (dumbbells) are highly entangled in the NTE behaviors of R2Fe17 (R = rare earth) compounds but still remain controversial. Here, a facile method is employed to explore the role of dumbbells in spin alignments and NTE by the nonstoichiometric design of Lu2–x Fe17 compounds. The powder synchrotron X-ray diffraction, magnetometry, and neutron powder diffraction investigations indicate that a decrease of the Lu content can enhance the dumbbell concentration and motivate an incommensurate magnetic structure simultaneously. However, increasing the dumbbell concentration makes little difference in the amplitude of the ordered magnetic moments of Fe sublattices, which reveals an equivalent NTE behavior for Lu2–x Fe17 compounds. This work gives insight into the role that dumbbells played in spin alignments and NTE for Lu2Fe17-based compounds, correcting the previously proposed conjecture and probably conducive to adjusting the related magnetic performances of R2Fe17 compounds in the future.