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Register a new userRobust block magnetism in the spin ladder compound BaFe$_2$Se$_3$ under hydrostatic pressure
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The majority of the iron-based superconductors (FeSCs) exhibit a two-dimensional square lattice structure. Recent reports of pressure-induced superconductivity in the spin-ladder system, BaFe$_2$X$_3$ (X =S,Se), introduce a quasi-one-dimensional prototype and an insulating parent compound to the FeSCs. Here we report X-ray, neutron diffraction and muon spin relaxation experiments on BaFe$_2$Se$_3$ under hydrostatic pressure to investigate its magnetic and structural properties across the pressure-temperature phase diagram. A structural phase transition was identified at a pressure of 3.7(3) GPa. Neutron diffraction measurements at 6.8(3) GPa and 120 K show that the block magnetism persists even at these high pressures. A steady increase and then fast drop of the magnetic transition temperature $Trm_N$ and greatly reduced moment above the pressure $P_s$ indicate potentially rich and competing phases close to the superconducting phase in this ladder system.
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The electronic structure of BaFe$_2X_3$ ($X$ = S and Se) and CsFe$_2$Se$_3$ in which two-leg ladders are formed by the Fe sites are studied by means of x-ray absorption and resonant inelastic x-ray scattering spectroscopy. The x-ray absorption spectra at the Fe L edges for BaFe$_2X_3$ exhibit two components, indicating that itinerant and localized Fe 3$d$ sites coexist. Substantial x-ray linear dichroism (XLD) is observed in polarization dependent spectra, indicating the existence of orbital order or fluctuation in the Fe-ladder even above the N{e}el temperature $T_N$. Direct exchange interaction along the legs of the Fe-ladder stabilizes the orbital and antiferromagnetic orders in BaFe$_2$S$_3$, while the ferromagnetic molecular orbitals are realized between the rungs in CsFe$_2$Se$_3$.
We report pressure-dependent neutron diffraction and muon spin relaxation/rotation measurements combined with first-principles calculations to investigate the structural, magnetic, and electronic properties of BaFe$_2$S$_3$ under pressure. The experimental results reveal a gradual enhancement of the stripe-type ordering temperature with increasing pressure up to 2.6 GPa and no observable change in the size of the ordered moment. The ab initio calculations suggest that the magnetism is highly sensitive to the Fe-S bond lengths and angles, clarifying discrepancies with previously published results. In contrast to our experimental observations, the calculations predict a monotonic reduction of the ordered moment with pressure. We suggest that the robustness of the stripe-type antiferromagnetism is due to strong electron correlations not fully considered in the calculations.
We report a comprehensive study of the spin ladder compound BaFe$_2$S$_{2.5}$Se$_{0.5}$ using neutron diffraction, inelastic neutron scattering, high pressure synchrotron diffraction, and high pressure transport techniques. We find that BaFe$_2$S$_{2.5}$Se$_{0.5}$ possesses the same $Cmcm$ structure and stripe antiferromagnetic order as does BaFe$_2$S$_3$, but with a reduced N{{e}}el temperature of $T_N=98$ K compared to 120 K for the undoped system, and a slightly increased ordered moment of 1.40$mu_B$ per iron. The low-energy spin excitations in BaFe$_2$S$_{2.5}$Se$_{0.5}$ are likewise similar to those observed in BaFe$_2$S$_{3}$. However, unlike the reports of superconductivity in BaFe$_2$S$_3$ below $T_c sim 14$~K under pressures of 10~GPa or more, we observe no superconductivity in BaFe$_2$S$_{2.5}$Se$_{0.5}$ at any pressure up to 19.7~GPa. In contrast, the resistivity exhibits an upturn at low temperature under pressure. Furthermore, we show that additional high-quality samples of BaFe$_2$S$_3$ synthesized for this study likewise fail to become superconducting under pressure, instead displaying a similar upturn in resistivity at low temperature. These results demonstrate that microscopic, sample-specific details play an important role in determining the ultimate electronic ground state in this spin ladder system. We suggest that the upturn in resistivity at low temperature in both BaFe$_2$S$_3$ and BaFe$_2$S$_{2.5}$Se$_{0.5}$ may result from Anderson localization induced by S vacancies and random Se substitutions, enhanced by the quasi-one-dimensional ladder structure.
We report on the effects of hydrostatic pressure (HP) on the charge density wave observed in underdoped cuprates. We studied YBa$_2$Cu$_3$O$_{6.6}$ ($T_c$=61 K) using high-resolution inelastic x-ray scattering (IXS), and reveal an extreme sensitivity of the phonon anomalies related to the charge density wave (CDW) order to HP. The amplitudes of the normal state broadening and superconductivity induced phonon softening at Q$_{CDW}$ rapidly decrease as HP is applied, resulting in the complete suppression of signatures of the CDW below $sim$1 GPa. Additional IXS measurements on YBa$_2$Cu$_3$O$_{6.75}$ demonstrate that this very rapid effect cannot be explained by pressure-induced modification of the doping level and highlight the different role of external pressure and doping in tuning the phase diagram of the cuprates. Our results provide new insights into the mechanisms underlying the CDW formation and its interplay with superconductivity.
We report experimental studies of a series of BaFe$_2$S$_{3-x}$Se$_x$ ($0leq xleq3$) single crystals and powder specimens using x-ray diffraction, neutron diffraction, muon spin relaxation, and electrical transport measurements. A structural transformation from Cmcm (BaFe$_2$S$_3$) to Pnma (BaFe$_2$Se$_3$) was identified around $x = 0.7sim 1$. Neutron diffraction measurements on the samples with $x$ = 0.2, 0.4, and 0.7 reveal that the N${e}$el temperature of the stripe antiferromagnetic order is gradually suppressed from $sim$120 to 85 K, while the magnitude of the ordered Fe$^{2+}$ moments shows very little variation. Similarly, the block antiferromagnetic order in BaFe$_2$Se$_3$ remains robust for $1.5leq xleq3$ with negligible variation in the ordered moment and a slight decrease of the N${e}$el temperature from 250 K ($x=3$) to 225 K ($x=1.5$). The sample with $x=1$ near the Cmcm and Pnma border shows coexisting, two-dimensional, short-range stripe- and block-type antiferromagnetic correlations. The system remains insulating for all $x$, but the thermal activation gap shows an abrupt increase when traversing the boundary from the Cmcm stripe phase to the Pnma block phase. The results demonstrate that the crystal structure, magnetic order, and electronic properties are strongly coupled in the BaFe$_2$S$_{3-x}$Se$_x$ system.
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