Pressure dependence of upper critical fields in FeSe single crystals

We investigate the pressure dependence of the upper critical fields ({\mu}$_0$$H$$_{c2}$) for FeSe single crystals with pressure up to 2.57 GPa. The superconducting (SC) properties show a disparate behavior across a critical pressure where the pressure-induced antiferromagnetic phase coexists with superconductivity. The magnetoresistance for $H//ab$ and $H//c$ is very different: for $H//c$, magnetic field induces and enhances a hump in the resistivity close to the $T_c$ for pressures higher than 1.2 GPa, while it is absent for $H//ab$. Since the measured {\mu}$_0$$H$$_{c2}$ for FeSe samples is smaller than the orbital limited upper critical field ($H$$^{orb}$$_{c2}$) estimated by the Werthamer Helfand and Hohenberg (WHH) model, the Maki parameter ({\alpha}) related to Pauli spin-paramagnetic effects is additionally considered to describe the temperature dependence of {\mu}$_0$$H$$_{c2}$($T$). Interestingly, the {\alpha} value is hardly affected by pressure for $H//ab$, while it strongly increases with pressure for $H//c$. The pressure evolution of the {\mu}$_0$$H$$_{c2}$(0)s for the FeSe single crystals is found to be almost similar to that of $T_c$($P$), suggesting that the pressure-induced magnetic order adversely affects the upper critical fields as well as the SC transition temperature.Comment: 23 pages, 6 figures, 1 tabl

Enhanced critical current density in the pressure-induced magnetic state of the high-temperature superconductor FeSe

We investigate the relation of the critical current density (Jc) and the remarkably increased superconducting transition temperature (Tc) for the FeSe single crystals under pressures up to 2.43 GPa, where the Tc is increased by ~8 K/GPa. The critical current density corresponding to the free flux flow is monotonically enhanced by pressure which is due to the increase in Tc, whereas the depinning critical current density at which the vortex starts to move is more influenced by the pressure-induced magnetic state compared to the increase of Tc. Unlike other high-Tc superconductors, FeSe is not magnetic, but superconducting at ambient pressure. Above a critical pressure where magnetic state is induced and coexists with superconductivity, the depinning Jc abruptly increases even though the increase of the zero-resistivity Tc is negligible, directly indicating that the flux pinning property compared to the Tc enhancement is a more crucial factor for an achievement of a large Jc. In addition, the sharp increase in Jc in the coexisting superconducting phase of FeSe demonstrates that vortices can be effectively trapped by the competing antiferromagnetic order, even though its antagonistic nature against superconductivity is well documented. These results provide new guidance toward technological applications of high-temperature superconductors.Comment: 24pages, 8 figure

Growth of Transition-Metal Dichalcogenides by Solvent Evaporation Technique

Due to their physical properties and potential applications in energy conversion and storage, transition-metal dichalcogenides (TMDs) have garnered substantial interest in recent years. Among this class of materials, TMDs based on molybdenum, tungsten, sulfur, and selenium are particularly attractive due to their semiconducting properties and the availability of bottom-up synthesis techniques. Here we report a method which yields high-quality crystals of transition-metal diselenide and ditelluride compounds (PtTe2, PdTe2, NiTe2, TaTe2, TiTe2, RuTe2, PtSe2, PdSe2, NbSe2, TiSe2, VSe2, ReSe2) from their solid solutions, via vapor deposition from a metal-saturated chalcogen melt. Additionally, we show the synthesis of rare-earth-metal polychalcogenides and NbS2 crystals using the aforementioned process. Most of the crystals obtained have a layered CdI2 structure. We have investigated the physical properties of selected crystals and compared them to state of the art findings reported in the literature. Remarkably, the charge density wave transition in 1T-TiSe2 and 2H-NbSe2 crystals is well-defined at TCDW ≈ 200 and 33 K, respectively. Angle-resolved photoelectron spectroscopy and electron diffraction are used to directly access the electronic and crystal structures of PtTe2 single crystals and yield state of the art measurements. © 2020 American Chemical Society.M.A.-H. acknowledges support from the VR starting grant 2018-05339 and KL1824/6. The crystal growth experiments were supported by the Russian Science Foundation, Project 19-12-00414. The work has been supported by the program 211 of the Russian Federation Government agreements 02.A03.21.0006 and 02.A03.21.0011, by the Russian Government Program of Competitive Growth of Kazan Federal University. We acknowledge MAX IV Laboratory for time on Beamline Bloch under Proposal 20190335. Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under contract 2018-07152 the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496. We acknowledge ARPES experiment support from Craig Polley (MAX IV), Maciej Dendzik (KTH) Antonija Grubisic-Cabo (KTH) and Oscar Tjernberg (KTH). H.R., D.P. and G.J.M. acknowledge the Swedish Research Council (2018-06465, 2018-04330) and the Swedish Energy Agency (P43549-1) for financial support

Competition between orbital effects, Pauli limiting, and Fulde-Ferrell-Larkin-Ovchinnikov states in 2D transition metal dichalcogenide superconductors

We compare the upper critical field of bulk single-crystalline samples of the two intrinsic transition metal dichalcogenide superconductors, 2H-NbSe2 and 2H-NbS2, in high magnetic fields where their layer structure is aligned strictly parallel and perpendicular to the field, using magnetic torque experiments and a high-precision piezo-rotary positioner. While both superconductors show that orbital effects still have a significant impact when the layer structure is aligned parallel to the field, the upper critical field of NbS2 rises above the Pauli limiting field and forms a Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state, while orbital effects suppress superconductivity in NbSe2 just below the Pauli limit, which excludes the formation of the FFLO state. From the out-of-plane anisotropies, the coherence length perpendicular to the layers of 31 angstrom in NbSe2 is much larger than the interlayer distance, leading to a significant orbital effect suppressing superconductivity before the Pauli limit is reached, in contrast to the more 2D NbS2

The State of Trace Elements (In, Cu, Ag) in Sphalerite Studied by X-Ray Absorption Spectroscopy of Synthetic Minerals

The oxidation state and local atomic environment of admixtures of In, Cu, and Ag in synthetic sphalerite crystals were determined by X-ray absorption spectroscopy (XAS). The sphalerite crystals doped with In, Cu, Ag, In–Cu, and In–Ag were synthesized utilizing gas transport, salt flux, and dry synthesis techniques. Oxidation states of dopants were determined using X-ray absorption near edge structure (XANES) technique. The local atomic structure was studied by X-ray absorption fine structure spectroscopy (EXAFS). The spectra were recorded at Zn, In, Ag, and Cu K-edges. In all studied samples, In was in the 3+ oxidation state and replaced Zn in the structure of sphalerite, which occurs with the expansion of the nearest coordination shells due to the large In ionic radius. In the presence of In, the oxidation state of Cu and Ag is 1+, and both metals can form an isomorphous solid solution where they substitute for Zn according to the coupled substitution scheme 2Zn2+ ↔ Me+ + In3+. Moreover, Ag K-edges EXAFS spectra fitting, combined with the results obtained for In- and Au-bearing sphalerite shows that the Me-S distances in the first coordination shell in the solid solution state are correlated with the ionic radii and increase in the order of Cu < Ag < Au. The distortion of the atomic structure increases in the same order. The distant (second and third) coordination shells of Cu and Ag in sphalerite are split into two subshells, and the splitting is more pronounced for Ag. Analysis of the EXAFS spectra, coupled with the results of DFT (Density Function Theory) simulations, showed that the In–In and Me+–In3+ clustering is absent when the metals are present in the sphalerite solid solution. Therefore, all studied admixtures (In, Cu, Ag), as well as Au, are randomly distributed in the matrix of sphalerite, where the concentration of the elements in the “invisible” form can reach a few tens wt.%

Evidence for the Fulde-Ferrell-Larkin-Ovchinnikov state in bulk NbS2

We present measurements of the magnetic torque, specific heat and thermal expansion of the bulk transition metal dichalcogenide (TMD) superconductor NbS2 in high magnetic fields, with its layer structure aligned strictly parallel to the field using a piezo rotary positioner. The upper critical field of superconducting TMDs in the 2D form is known to be dramatically enhanced by a special form of Ising spin orbit coupling. This Ising superconductivity is very robust to the Pauli paramagnetic effect and can therefore exist beyond the Pauli limit for superconductivity. We find that superconductivity beyond the Pauli limit still exists in bulk single crystals of NbS2 for a precisely parallel field alignment. However, the comparison of our upper critical field transition line with numerical simulations rather points to the development of a Fulde-Ferrell-Larkin-Ovchinnikov state above the Pauli limit as a cause. This is also consistent with the observation of a magnetic field driven phase transition in the thermodynamic quantities within the superconducting state near the Pauli limit. Superconductivity is often destroyed under magnetic field larger than a critical value called Pauli limit. Here, the authors report superconductivity beyond the Pauli limit in bulk single crystals of NbS2, suggesting the development of a Fulde-Ferrell-Larkin-Ovchinnikov state