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Register a new userOptimization of the Crystal Growth of the Superconductor CaKFe$_{4}$As$_{4}$ from Solution in the FeAs-CaFe$_{2}$As$_{2}$-KFe$_{2}$As$_{2}$ System
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Measurements of the anisotropic properties of single crystals play a crucial role in probing the physics of new materials. Determining a growth protocol that yields suitable high-quality single crystals can be particularly challenging for multi-component compounds. Here we present a case study of how we refined a procedure to grow single crystals of CaKFe$_{4}$As$_{4}$ from a high temperature, quaternary liquid solution rich in iron and arsenic (FeAs self-flux). Temperature dependent resistance and magnetization measurements are emphasized, in addition to the x-ray diffraction, to detect inter-grown CaKFe$_{4}$As$_{4}$, CaFe$_{2}$As$_{2}$ and KFe$_{2}$As$_{2}$ within, what appear to be, single crystals. Guided by the rules of phase equilibria and these data, we adjusted growth parameters to suppress formation of the impurity phases. The resulting optimized procedure yielded phase-pure single crystals of CaKFe$_{4}$As$_{4}$. This optimization process offers insight into the growth of quaternary compounds and a glimpse of the four-component phase diagram in the pseudo-ternary FeAs-CaFe$_{2}$As$_{2}$-KFe$_{2}$As$_{2}$ system.
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In a recent work, new two-dimensional materials, the monolayer MoSi$_{2}$N$_{4}$ and WSi$_{2}$N$_{4}$, have been successfully synthesized in experiment, and several other monolayer materials with the similar structure, such as MoSi$_{2}$As$_{4}$, have been predicted [{color{blue}Science 369, 670-674 (2020)}]. Here, based on first-principles calculations and theoretical analysis, we investigate the electronic and optical properties of monolayer MoSi$_{2}$N$_{4}$, WSi$_{2}$N$_{4}$ and MoSi$_{2}$As$_{4}$. We show that these materials are semiconductors, with a pair of Dirac-type valleys located at the corners of the hexagonal Brillouin zone. Due to the broken inversion symmetry and the effect of spin-orbit coupling, the valley fermions manifest spin-valley coupling, valley-contrasting Berry curvature, and valley-selective optical circular dichroism. We also construct the low-energy effective model for the valleys, calculate the spin Hall conductivity and the permittivity, and investigate the strain effect on the band structure. Our result reveals interesting valley physics in monolayer MoSi$_{2}$N$_{4}$, WSi$_{2}$N$_{4}$ and MoSi$_{2}$As$_{4}$, suggesting their great potential for valleytronics and spintronics applications.
We report high-resolution neutron scattering measurements of the low energy spin fluctuations of KFe$_{2}$As$_{2}$, the end member of the hole-doped Ba$_{1-x}$K$_x$Fe$_2$As$_2$ family with only hole pockets, above and below its superconducting transition temperature $T_c$ ($sim$ 3.5 K). Our data reveals clear spin fluctuations at the incommensurate wave vector ($0.5pmdelta$, 0, $L$), ($delta$ = 0.2)(1-Fe unit cell), which exhibit $L$-modulation peaking at $L=0.5$. Upon cooling to the superconducting state, the incommensurate spin fluctuations gradually open a spin-gap and form a sharp spin resonance mode. The incommensurability ($2delta$ = 0.4) of the resonance mode ($sim1.2$ meV) is considerably larger than the previously reported value ($2delta$ $approx0.32$) at higher energies ($gesim6$ meV). The determination of the momentum structure of spin fluctuation in the low energy limit allows a direct comparison with the realistic Fermi surface and superconducting gap structure. Our results point to an $s$-wave pairing with a reversed sign between the hole pockets near the zone center in KFe$_{2}$As$_{2}$.
The recent discovery and subsequent developments of FeAs-based superconductors have presented novel challenges and opportunities in the quest for superconducting mechanisms in correlated-electron systems. Central issues of ongoing studies include interplay between superconductivity and magnetism as well as the nature of the pairing symmetry reflected in the superconducting energy gap. In the cuprate and RE(O,F)FeAs (RE = rare earth) systems, the superconducting phase appears without being accompanied by static magnetic order, except for narrow phase-separated regions at the border of phase boundaries. By muon spin relaxation measurements on single crystal specimens, here we show that superconductivity in the AFe$_{2}$As$_{2}$ (A = Ca,Ba,Sr) systems, in both the cases of composition and pressure tunings, coexists with a strong static magnetic order in a partial volume fraction. The superfluid response from the remaining paramagnetic volume fraction of (Ba$_{0.5}$K$_{0.5}$)Fe$_{2}$As$_{2}$ exhibits a nearly linear variation in T at low temperatures, suggesting an anisotropic energy gap with line nodes and/or multi-gap effects.
The optical properties of KFe$_2$As$_2$ have been measured for light polarized in the a-b planes over a wide temperature and frequency range. Below $T^astsimeq 155$ K, where this material undergoes an incoherent-coherent crossover, we observe a new coherent response emerging in the optical conductivity. A spectral weight analysis suggests that this new feature arises out of high-energy bound states. Below about $T_{rm FL} simeq 75$ K the scattering rate for this new feature is quadratic in temperature, indicating a Fermi-liquid response. Theory calculations suggest this crossover is dominated by the $d_{xy}$ orbital. Our results advocate for Kondo-type screening as the mechanism for the orbital-selective incoherent-coherent crossover in hole-overdoped KFe$_2$As$_2$.
Fermi-surface topology governs the relationship between magnetism and superconductivity in iron-based materials. Using low-temperature transport, angle-resolved photoemission, and x-ray diffraction we show unambiguous evidence of large Fermi surface reconstruction in CaFe$_{2}$As$_{2}$ at magnetic spin-density-wave and nonmagnetic collapsed-tetragonal ($cT$) transitions. For the $cT$ transition, the change in the Fermi surface topology has a different character with no contribution from the hole part of the Fermi surface. In addition, the results suggest that the pressure effect in CaFe$_{2}$As$_{2}$ is mainly leading to a rigid-band-like change of the valence electronic structure. We discuss these results and their implications for magnetism and superconductivity in this material.
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