Transition to collapsed tetragonal phase in CaFe2As2 single crystals as seen by 57Fe Mössbauer spectroscopy

Bud'ko, Sergey L.; Ma, Xiaoming; Tomić, Milan; Ran, Sheng; Valentí, Roser; Canfield, Paul C.

doi:10.1103/PhysRevB.93.024516

Transition to collapsed tetragonal phase in CaFe₂As₂ single crystals as seen by ⁵⁷Fe Mössbauer spectroscopy

Journal Article · Wed Jan 20 23:00:00 EST 2016 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.93.024516· OSTI ID:1239156

Bud'ko, Sergey L. ^[1]; Ma, Xiaoming ^[2]; Tomić, Milan ^[3]; Ran, Sheng ^[1]; Valentí, Roser ^[3]; Canfield, Paul C. ^[1]

Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States); Lanzhou Univ., Gansu Province (China)
Goethe-Univ. Frankfurt, Frankfurt am Main (Germany)

Temperature dependent measurements of ⁵⁷Fe Mössbauer spectra on CaFe₂As₂ single crystals in the tetragonal and collapsed tetragonal phases are reported. Clear features in the temperature dependencies of the isomer shift, relative spectra area, and quadrupole splitting are observed at the transition from the tetragonal to the collapsed tetragonal phase. From the temperature dependent isomer shift and spectral area data, an average stiffening of the phonon modes in the collapsed tetragonal phase is inferred. The quadrupole splitting increases by ~25% on cooling from room temperature to ~100 K in the tetragonal phase and is only weakly temperature dependent at low temperatures in the collapsed tetragonal phase, in agreement with the anisotropic thermal expansion in this material. In order to gain microscopic insight about these measurements, we perform ab initio density functional theory calculations of the electric field gradient and the electron density of CaFe₂As₂ in both phases. By comparing the experimental data with the calculations we are able to fully characterize the crystal structure of the samples in the collapsed-tetragonal phase through determination of the As z coordinate. Furthermore, based on the obtained temperature dependent structural data we are able to propose charge saturation of the Fe-As bond region as the mechanism behind the stabilization of the collapsed-tetragonal phase at ambient pressure.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1239156

Alternate ID(s):: OSTI ID: 1235760

Report Number(s):: IS-J--8883

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 2 Vol. 93; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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