Pressure-induced magnetic collapse and metallization of $\mathrm{TlF}{\mathrm{e}}_{1.6}\mathrm{S}{\mathrm{e}}_{2}$

Pressure-induced magnetic collapse and metallization of $TlF e_{1.6} S e_{2}$

P. G. Naumov, K. Filsinger, S. I. Shylin, O. I. Barkalov, V. Ksenofontov, Y. Qi, T. Palasyuk, W. Schnelle, S. A. Medvedev, M. Greenblatt, and C. Felser

Phys. Rev. B 96, 064109 – Published 16 August 2017

Abstract

The crystal structure, magnetic ordering, and electrical resistivity of $TlF e_{1.6} S e_{2}$ were studied at high pressures. Below $\sim 7 GPa$ , $TlF e_{1.6} S e_{2}$ is an antiferromagnetically ordered semiconductor with a $ThC r_{2} S i_{2}$ -type structure. The insulator-to-metal transformation observed at a pressure of $\sim 7 GPa$ is accompanied by a loss of magnetic ordering and an isostructural phase transition. In the pressure range $\sim 7.5 – 11 GPa$ a remarkable downturn in resistivity, which resembles a superconducting transition, is observed below 15 K. We discuss this feature as the possible onset of superconductivity originating from a phase separation in a small fraction of the sample in the vicinity of the magnetic transition.

Received 18 May 2017

DOI:https://doi.org/10.1103/PhysRevB.96.064109

Physics Subject Headings (PhySH)

Solid-solid transformations

Chalcogenides Unconventional superconductors

Mössbauer spectroscopy Pressure techniques

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

P. G. Naumov^1,2, K. Filsinger¹, S. I. Shylin^3,4, O. I. Barkalov^1,5, V. Ksenofontov^3,*, Y. Qi¹, T. Palasyuk⁶, W. Schnelle¹, S. A. Medvedev¹, M. Greenblatt⁷, and C. Felser¹

¹Max Planck Institute for Chemical Physics of Solids, Nöthnitzer Straße 40, 01187 Dresden, Germany
²Shubnikov Institute for Crystallography of Federal Scientific Research Centre “Crystallography and Photonics” of Russian Academy of Sciences, Leninskii prospekt 59, Moscow, 119333, Russia
³Institute for Inorganic and Analytical Chemistry, Johannes Gutenberg University Mainz, 55128 Mainz, Germany
⁴Department of Chemistry, Taras Shevchenko National University of Kyiv, 01601 Kyiv, Ukraine
⁵Institute for Solid State Physics, Russian Academy of Sciences, Academician Ossipyan Street 2, Chernogolovka, Moscow District, 142432, Russia
⁶Institute for Physical Chemistry, Polish Academy of Sciences, PL-01224 Warsaw, Poland
⁷Department of Chemistry and Chemical Biology, Rutgers University, Piscataway, NJ 08854, USA

^*Corresponding author: v.ksenofontov@uni-mainz.de

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Vol. 96, Iss. 6 — 1 August 2017

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Figure 1
(a) Magnetization of $TlF e_{1.6} S e_{2}$ measured in a magnetic field of 0.1 T applied in the $a b$ plane (red) and along the $c$ axis (black). Extrapolations of the fitted curves intersect at 460 K and thus show the approximate Néel temperature. $T_{1}$ and $T_{2}$ mark the temperatures at which spin canting occurs. (b) Electrical resistivity of $TlF e_{1.6} S e_{2}$ as a function of temperature.
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Figure 2
Mössbauer spectra of ${}^{57}{Fe}$ -enriched $TlF e_{1.6} S e_{2}$ acquired at 293 K from (a) a mosaic-crystalline sample with the $c$ axis parallel to the direction of the $γ$ rays and (b) the sample in the DAC at an initial pressure of 0.5 GPa. The coexistence of two sextets is observed when mosaic-crystalline $TlF e_{1.6} S e_{2}$ is cooled to 105 K (c) due to partial spin canting between the temperatures $T_{1}$ and $T_{2}$ indicated in Fig. 1. Below $T_{2}$ , only the one Fe site with parameters close to those above $T_{1}$ is observed (d).
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Figure 3
Temperature dependence of the resistivity of $TlF e_{1.6} S e_{2}$ at pressures below (a) and above (b) 7 GPa. The inset in (a) shows the Arrhenius plots at different pressures. The inset in (b) shows the dependence of low-temperature resistivity measured with different probe currents at 7.5 GPa. The red curve at 0.2 GPa in (a) shows the resistance curve recorded after pressure release from the highest value used in this experiment (25 GPa).
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Figure 4
(a) Pressure evolution of the powder x-ray diffraction patterns of $TlF e_{1.6} S e_{2}$ during pressure increase. The single-phase diffraction pattern at 10.4 GPa is indexed with the $ThC r_{2} S i_{2}$ -type structure. The blue curve shows the diffraction pattern recorded at 1.0 GPa after pressure release from the highest pressure 21.0 GPa. (b) Powder-diffraction patterns in the vicinity of the structural phase transition indicated by the splitting of the (110) reflection. (c) Decrease of the lattice parameters of $TlF e_{1.6} S e_{2}$ under pressure showing the collapse of its crystal structure around 8 GPa.
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Figure 5
Pressure-dependent Mössbauer spectra of ${}^{57}{Fe}$ -enriched $TlF e_{1.6} S e_{2}$ at room- and low temperature showing collapse of the antiferromagnetic state. Coexistence of the magnetic and paramagnetic states in approximately equal amounts is observed at 7.8 GPa. Application of the magnetic field of 6 T to the sample at 25.6 GPa magnetically splits the Mössbauer spectrum. Fitting of the in-field spectrum with an effective hyperfine magnetic field of 6.0(2) T indicates no localized magnetic moments at the Fe atoms in the metallic phase of $TlF e_{1.6} S e_{2}$ .
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Physical Review B

covering condensed matter and materials physics

Pressure-induced magnetic collapse and metallization of $TlF e_{1.6} S e_{2}$

P. G. Naumov, K. Filsinger, S. I. Shylin, O. I. Barkalov, V. Ksenofontov, Y. Qi, T. Palasyuk, W. Schnelle, S. A. Medvedev, M. Greenblatt, and C. Felser

Phys. Rev. B 96, 064109 – Published 16 August 2017

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Physical Review B

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Pressure-induced magnetic collapse and metallization of TlFe1.6Se2

P. G. Naumov, K. Filsinger, S. I. Shylin, O. I. Barkalov, V. Ksenofontov, Y. Qi, T. Palasyuk, W. Schnelle, S. A. Medvedev, M. Greenblatt, and C. Felser

Phys. Rev. B 96, 064109 – Published 16 August 2017

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Pressure-induced magnetic collapse and metallization of $TlF e_{1.6} S e_{2}$