1. Influence of hydrogenation on the vibrational density of states of magnetocaloric $\mathrm{LaFe}_\mathrm{11.4}\mathrm{Si}_\mathrm{1.6}\mathrm{H}_{1.6}$
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Terwey, Alexandra, Gruner, Markus E., Keune, Werner, Landers, Joachim, Salamon, Soma, Eggert, Benedikt, Ollefs, Katharina, Brabänder, Valentin, Radulov, Ilya, Skokov, Konstantin, Faske, Tom, Hu, Michael Y., Zhao, Jiyong, Alp, Esen E., Giacobbe, Carlotta, Gutfleisch, Oliver, and Wende, Heiko
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Condensed Matter - Materials Science - Abstract
We report on the impact of magnetoelastic coupling on the magnetocaloric properties of LaFe$_{11.4}$Si$_{1.6}$H$_{1.6}$ in terms of the vibrational density of states, which we determined with $^{57}$Fe nuclear resonant inelastic X-ray scattering measurements and with density-functional-theory based first-principles calculations in the ferromagnetic low-temperature and paramagnetic high-temperature phase. In experiments and calculations, we observe pronounced differences in the shape of the Fe-partial VDOS between non-hydrogenated and hydrogenated samples. This shows that hydrogen does not only shift the temperature of the first-order phase transition, but also affects the elastic response of the Fe-subsystem significantly. In turn, the anomalous redshift of the Fe VDOS, observed by going to the low-volume PM phase, survives hydrogenation. As a consequence, the change in the Fe specific vibrational entropy $\Delta S_\mathrm{lat}$ across the phase transition has the same sign as the magnetic and electronic contribution. DFT calculations show that the same mechanism, which is a consequence of the itinerant electron metamagnetism associated with the Fe subsystem, is effective in both the hydrogenated and he hydrogen-free compounds. Although reduced by 50 % as compared to the hydrogen-free system, the measured change $\Delta S_\mathrm{lat}$ of 3.2\pm1.9 J/kgK across the FM to PM transition contributes with 35 % significantly and cooperatively to the total isothermal entropy change $\Delta S_\mathrm{iso}$. Hydrogenation is observed to induce an overall blueshift of the Fe-VDOS with respect to the H-free compound; this effect, together with the enhanced Debye temperature observed, is a fingerprint of the hardening of the Fe sublattice by hydrogen incorporation. In addition, the mean Debye velocity of sound of LaFe$_{11.4}$Si$_{1.6}$H$_{1.6}$ was determined from the NRIXS and the DFT data., Comment: 13 pages 9 figures
- Published
- 2019
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