Impact of lattice dynamics on the phase stability of metamagnetic FeRh: Bulk and thin films

Wolloch, M.; Gruner, M. E.; Keune, W.; Mohn, P.; Redinger, J.; Hofer, F.; Suess, D.; Podloucky, R.; Landers, J.; Salamon, S.; Scheibel, F.; Spoddig, D.; Witte, R.; Roldan Cuenya, B.; Gutfleisch, O.; Hu, M. Y.; Zhao, J.; Toellner, T.; Alp, E. E.; Siewert, M.; Entel, P.; Pentcheva, R.; Wende, H.

doi:10.1103/PhysRevB.94.174435

Impact of lattice dynamics on the phase stability of metamagnetic FeRh: Bulk and thin films

Journal Article · Tue Nov 01 00:00:00 EDT 2016 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.94.174435· OSTI ID:1393459

Wolloch, M.; Gruner, M. E.; Keune, W.; Mohn, P.; Redinger, J.; Hofer, F.; Suess, D.; Podloucky, R.; Landers, J.; Salamon, S.; Scheibel, F.; Spoddig, D.; Witte, R.; Roldan Cuenya, B.; Gutfleisch, O.; Hu, M. Y.; Zhao, J.; Toellner, T.; Alp, E. E.; Siewert, M. more »

We present phonon dispersions, element-resolved vibrational density of states (VDOS) and corresponding thermodynamic properties obtained by a combination of density functional theory (DFT) and nuclear resonant inelastic x-ray scattering (NRIXS) across the metamagnetic transition of B2 FeRh in the bulk material and thin epitaxial films. We see distinct differences in the VDOS of the antiferromagnetic (AF) and ferromagnetic (FM) phases, which provide a microscopic proof of strong spin-phonon coupling in FeRh. The FM VDOS exhibits a particular sensitivity to the slight tetragonal distortions present in epitaxial films, which is not encountered in the AF phase. This results in a notable change in lattice entropy, which is important for the comparison between thin film and bulk results. Our calculations confirm the recently reported lattice instability in the AF phase. The imaginary frequencies at the X point depend critically on the Fe magnetic moment and atomic volume. Analyzing these nonvibrational modes leads to the discovery of a stable monoclinic ground-state structure, which is robustly predicted from DFT but not verified in our thin film experiments. Specific heat, entropy, and free energy calculated within the quasiharmonic approximation suggest that the new phase is possibly suppressed because of its relatively smaller lattice entropy. In the bulk phase, lattice vibrations contribute with the same sign and in similar magnitude to the isostructural AF-FM phase transition as excitations of the electronic and magnetic subsystems demonstrating that lattice degrees of freedom need to be included in thermodynamic modeling.

Research Organization:: Argonne National Laboratory (ANL)

Sponsoring Organization:: USDOE Office of Science; Deutsche Forschungsgemeinschaft (DFG)

DOE Contract Number:: AC02-06CH11357

OSTI ID:: 1393459

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 17 Vol. 94; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

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