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Robert J. Birgeneau

Publications and source records attributed to Robert J. Birgeneau.

At least 73 records · Page 4Linked to original sources

Non-superconducting electronic ground state in pressurized BaFe$_2$S$_3$ and BaFe$_2$S$_{2.5}$Se$_{0.5}$

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{é}el temperature of $T_N=98$ K compared to 120 K for the undoped system, and a slightly increased ordered moment of 1.40$μ_B$ 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.

cond-mat.supr-con↗

The Nematic Energy Scale and the Missing Electron Pocket in FeSe

Superconductivity emerges in proximity to a nematic phase in most iron-based superconductors. It is therefore important to understand the impact of nematicity on the electronic structure. Orbital assignment and tracking across the nematic phase transition prove to be challenging due to the multiband nature of iron-based superconductors and twinning effects. Here, we report a detailed study of the electronic structure of fully detwinned FeSe across the nematic phase transition using angle-resolved photoemission spectroscopy. We clearly observe a nematicity-driven band reconstruction involving dxz, dyz, and dxy orbitals. The nematic energy scale between dxz and dyz bands reaches a maximum of 50 meV at the Brillouin zone corner. We are also able to track the dxz electron pocket across the nematic transition and explain its absence in the nematic state. Our comprehensive data of the electronic structure provide an accurate basis for theoretical models of the superconducting pairing in FeSe.

cond-mat.supr-con↗

Strain-induced spin-nematic state and nematic susceptibility arising from $2\times2$ Fe clusters in KFe$_{0.8}$Ag$_{1.2}$Te$_2$

Spin nematics break spin-rotational symmetry while maintaining time-reversal symmetry, analogous to liquid crystal nematics that break spatial rotational symmetry while maintaining translational symmetry. Although several candidate spin nematics have been proposed, the identification and characterization of such a state remain challenging because the spin-nematic order parameter does not couple directly to experimental probes. KFe$_{0.8}$Ag$_{1.2}$Te$_2$ (K$_5$Fe$_4$Ag$_6$Te$_{10}$, KFAT) is a local-moment magnet consisting of well-separated 2$\times$2 Fe clusters, and in its ground state the clusters order magnetically, breaking both spin-rotational and time-reversal symmetries. Using uniform magnetic susceptibility and neutron scattering measurements we find a small strain induces sizable spin anisotropy in the paramagnetic state of KFAT, manifestly breaking spin-rotational symmetry while retaining time-reversal symmetry, resulting in a strain-induced spin-nematic state in which the $2\times2$ clusters act as the spin analogue of molecules in a liquid crystal nematic. The strain-induced spin anisotropy in KFAT allows us to probe its nematic susceptibility, revealing a divergent-like increase upon cooling, indicating the ordered ground state is driven by a spin-orbital entangled nematic order parameter.

cond-mat.str-el↗

Observation of a C-type short range antiferromagnetic order in expanded FeS

We report neutron diffraction studies of FeS single crystals obtained from Rb$_x$Fe$_{2-y}$S$_2$ single crystals via a hydrothermal method. While no $\sqrt {5}\times \sqrt {5}$ iron vacancy order or block antiferromagnetic order typical of Rb$_x$Fe$_{2-y}$S$_2$ is found in our samples, we observe $C$-type short range antiferromagnetic order with moments pointed along the $c$-axis hosted by a new phase of FeS with an expanded inter-layer spacing. The Néel temperature for this magnetic order is determined to be 165 K. Our finding of a variant FeS structure hosting this $C$-type antiferromagnetic order demonstrates that the known FeS phase synthesized in this method is in the vicinity of a magnetically ordered ground state, providing insights into understanding a variety of phenomena observed in FeS and the related FeSe$_{1-x}$S$_x$ iron chalcogenide system.

cond-mat.supr-con↗

Robust block magnetism in the spin ladder compound BaFe$_2$Se$_3$ under hydrostatic pressure

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 $T\rm_N$ and greatly reduced moment above the pressure $P_s$ indicate potentially rich and competing phases close to the superconducting phase in this ladder system.

cond-mat.supr-con↗

Quantitative characterization of short-range orthorhombic fluctuations in FeSe through pair distribution function analysis

Neutron and x-ray total scattering measurements have been performed on powder samples of the iron chalcogenide superconductor FeSe. Using pair distribution function (PDF) analysis of the total scattering data to investigate short-range atomic correlations, we establish the existence of an instantaneous, local orthorhombic structural distortion attributable to nematic fluctuations that persists well into the high-temperature tetragonal phase, at least up to 300 K and likely to significantly higher temperatures. This short-range orthorhombic distortion is correlated over a length scale of about 1 nm at 300 K and grows to several nm as the temperature is lowered toward the long-range structural transition temperature. In the low-temperature nematic state, the local instantaneous structure exhibits an enhanced orthorhombic distortion relative to the average structure with a typical relaxation length of 3 nm. The quantitative characterization of these orthorhombic fluctuations sheds light on nematicity in this canonical iron-based superconductor.

cond-mat.supr-con↗

Intertwined magnetic and nematic orders in semiconducting KFe$_{0.8}$Ag$_{1.2}$Te$_2$

Superconductivity in the iron pnictides emerges from metallic parent compounds exhibiting intertwined stripe-type magnetic order and nematic order, with itinerant electrons suggested to be essential for both. Here we use X-ray and neutron scattering to show that a similar intertwined state is realized in semiconducting KFe$_{0.8}$Ag$_{1.2}$Te$_2$ (K$_5$Fe$_4$Ag$_6$Te$_{10}$) without itinerant electrons. We find Fe atoms in KFe$_{0.8}$Ag$_{1.2}$Te$_2$ form isolated $2\times2$ blocks, separated by nonmagnetic Ag atoms. Long-range magnetic order sets in below $T_{\rm N}\approx35$ K, with magnetic moments within the $2\times2$ Fe blocks ordering into the stripe-type configuration. A nematic order accompanies the magnetic transition, manifest as a structural distortion that breaks the fourfold rotational symmetry of the lattice. The nematic orders in KFe$_{0.8}$Ag$_{1.2}$Te$_2$ and iron pnictide parent compounds are similar in magnitude and how they relate to the magnetic order, indicating a common origin. Since KFe$_{0.8}$Ag$_{1.2}$Te$_2$ is a semiconductor without itinerant electrons, this indicates that local-moment magnetic interactions are integral to its magnetic and nematic orders, and such interactions may play a key role in iron-based superconductivity.

cond-mat.str-el↗

Widespread orthorhombic fluctuations in the (Sr,Na)Fe$_2$As$_2$ family of superconductors

We report comprehensive pair distribution function measurements of the hole-doped iron-based superconductor system Sr$_{1-x}$Na$_{x}$Fe$_2$As$_2$. Structural refinements performed as a function of temperature and length scale reveal orthorhombic distortions of the instantaneous local structure across a large region of the phase diagram possessing average tetragonal symmetry, indicative of fluctuating nematicity. These nematic fluctuations are present up to high doping levels ($x \gtrsim 0.48$, near optimal superconductivity) and high temperatures (above room temperature for $x = 0$, decreasing to 150 K for $x = 0.48$), with a typical length scale of 1-3 nm. This work highlights the ubiquity of nematic fluctuations in a representative iron-based superconductor and provides important details about the evolution of these fluctuations across the phase diagram.

cond-mat.supr-con↗

Gradual Enhancement of Stripe-Type Antiferromagnetism in Spin Ladder Material BaFe$_2$S$_3$ Under Pressure

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.

cond-mat.supr-con↗

Persistent low-energy phonon broadening near the charge order $q$-vector in bilayer cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$

We report a persistent low-energy phonon broadening around $q_{B} \sim 0.28$ r.l.u. along the Cu-O bond direction in the high-$T_c$ cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ (Bi-2212). We show that such broadening exists both inside and outside the conventional charge density wave (CDW) phase, via temperature dependent measurements in both underdoped and heavily overdoped samples. Combining inelastic hard x-ray scattering, diffuse scattering, angle-resolved photoemission spectroscopy, and resonant soft x-ray scattering at the Cu $L_3$-edge, we exclude the presence of a CDW in the heavily overdoped Bi-2212 similar to that observed in the underdoped systems. Finally, we discuss the origin of such anisotropic low-energy phonon broadening, and its potential precursory role to the CDW phase in the underdoped region.

cond-mat.str-el↗

Real-space investigation of short-range magnetic correlations in fluoride pyrochlores NaCaCo$_2$F$_7$ and NaSrCo$_2$F$_7$ with magnetic pair distribution function analysis

We present time-of-flight neutron total scattering and polarized neutron scattering measurements of the magnetically frustrated compounds NaCaCo$_2$F$_7$ and NaSrCo$_2$F$_7$, which belong to a class of recently discovered pyrochlore compounds based on transition metals and fluorine. The magnetic pair distribution function (mPDF) technique is used to analyze and model the total scattering data in real space. We find that a previously-proposed model of short-range XY-like correlations with a length scale of 10-15 Å, combined with nearest-neighbor collinear antiferromagnetic correlations, accurately describes the mPDF data at low temperature, confirming the magnetic ground state in these materials. This model is further verified by the polarized neutron scattering data. From an analysis of the temperature dependence of the mPDF and polarized neutron scattering data, we find that short-range correlations persist on the nearest-neighbor length scale up to 200 K, approximately two orders of magnitude higher than the spin freezing temperatures of these compounds. These results highlight the opportunity presented by these new pyrochlore compounds to study the effects of geometric frustration at relatively high temperatures, while also advancing the mPDF technique and providing a novel opportunity to investigate a genuinely short-range-ordered magnetic ground state directly in real space.

cond-mat.str-el↗

Local orthorhombicity in the magnetic $C_4$ phase of the hole-doped iron-arsenide superconductor Sr$_{1-x}$Na$_{x}$Fe$_2$As$_2$

We report temperature-dependent pair distribution function measurements of Sr$_{1-x}$Na$_{x}$Fe$_2$As$_2$, an iron-based superconductor system that contains a magnetic phase with reentrant tetragonal symmetry, known as the magnetic $C_4$ phase. Quantitative refinements indicate that the instantaneous local structure in the $C_4$ phase is comprised of fluctuating orthorhombic regions with a length scale of $\sim$2 nm, despite the tetragonal symmetry of the average static structure. Additionally, local orthorhombic fluctuations exist on a similar length scale at temperatures well into the paramagnetic tetragonal phase. These results highlight the exceptionally large nematic susceptibility of iron-based superconductors and have significant implications for the magnetic $C_4$ phase and the neighboring $C_2$ and superconducting phases.

cond-mat.supr-con↗

Emergent phases in iron pnictides: Double-Q antiferromagnetism, charge order and enhanced nematic correlations

Electron correlations produce a rich phase diagram in the iron pnictides. Earlier theoretical studies on the correlation effect demonstrated how quantum fluctuations weaken and concurrently suppress a $C_2$-symmetric single-Q antiferromagnetic order and a nematic order. Here we examine the emergent phases near the quantum phase transition. For a $C_4$-symmetric collinear double-Q antiferromagnetic order, we show that it is accompanied by both a charge order and an enhanced nematic susceptibility. Our results provide understanding for several intriguing recent experiments in hole-doped iron arsenides, and bring out common physics that underlies the different magnetic phases of various iron-based superconductors.

cond-mat.supr-con↗

The influence of magnetic order on the magnetoresistance anisotropy of Fe$_{1+δ-x}$Cu$_{x}$Te

We performed resistance measurements on Fe$_{1+δ-x}$Cu$_{x}$Te with $x_{EDX}\leq 0.06$ in the presence of in-plane applied magnetic fields, revealing a resistance anisotropy that can be induced at a temperature far below the structural and magnetic zero-field transition temperatures. The observed resistance anisotropy strongly depends on the field orientation with respect to the crystallographic axes, as well as on the field-cooling history. Our results imply a correlation between the observed features and the low-temperature magnetic order. Hysteresis in the angle-dependence indicates a strong pinning of the magnetic order within a temperature range that varies with the Cu content. The resistance anisotropy vanishes at different temperatures depending on whether an external magnetic field or a remnant field is present: the closing temperature is higher in the presence of an external field. For $x_{EDX} = 0.06$ the resistance anisotropy closes above the structural transition, at the same temperature at which the zero-field short-range magnetic order disappears and the sample becomes paramagnetic. Thus we suggest that under an external magnetic field the resistance anisotropy mirrors the magnetic order parameter. We discuss similarities to nematic order observed in other iron pnictide materials.

cond-mat.str-el↗

Resonant x-ray scattering reveals possible disappearance of magnetic order under hydrostatic pressure in the Kitaev candidate $γ$-Li$_2$IrO$_3$

Honeycomb iridates such as $γ$-Li$_2$IrO$_3$ are argued to realize Kitaev spin-anisotropic magnetic exchange, along with Heisenberg and possibly other couplings. While systems with pure Kitaev interactions are candidates to realize a quantum spin liquid ground state, in $γ$-Li$_2$IrO$_3$ it has been shown that the balance of magnetic interactions leads to the incommensurate spiral spin order at ambient pressure below 38 K. We study the fragility of this state in single crystals of $γ$-Li$_2$IrO$_3$ using resonant x-ray scattering (RXS) under applied hydrostatic pressures of up to 3.0 GPa. RXS is a direct probe of the underlying electronic order, and we observe the abrupt disappearance of the $q$=(0.57, 0, 0) spiral order at a critical pressure $P_c = 1.5\ $GPa with no accompanying change in the symmetry of the lattice. This dramatic disappearance is in stark contrast with recent studies of $β$-Li$_2$IrO$_3$ that show continuous suppression of the spiral order in magnetic field; under pressure, a new and possibly nonmagnetic ground state emerges.

cond-mat.mtrl-sci↗

Spin-Polarized Surface Resonances Accompanying Topological Surface State Formation

Topological insulators host spin-polarized surface states born out of the energetic inversion of bulk bands driven by the spin-orbit interaction. Here we discover previously unidentified consequences of band-inversion on the surface electronic structure of the topological insulator Bi$_2$Se$_3$. By performing simultaneous spin, time, and angle-resolved photoemission spectroscopy, we map the spin-polarized unoccupied electronic structure and identify a surface resonance which is distinct from the topological surface state, yet shares a similar spin- orbital texture with opposite orientation. Its momentum- dependence and spin texture imply an intimate connection with the topological surface state. Calculations show these two distinct states can emerge from trivial Rashba-like states that change topology through the spin-orbit-induced band inversion. This work thus provides a compelling view of the coevolution of surface states through a topological phase transition, enabled by the unique capability of directly measuring the spin-polarized unoccupied band structure.

cond-mat.mtrl-sci↗

Atomic-scale control of magnetic anisotropy via novel spin-orbit coupling effect in La2/3Sr1/3MnO3/SrIrO3 superlattices

Magnetic anisotropy (MA) is one of the most important material properties for modern spintronic devices. Conventional manipulation of the intrinsic MA, i.e. magnetocrystalline anisotropy (MCA), typically depends upon crystal symmetry. Extrinsic control over the MA is usually achieved by introducing shape anisotropy or exchange bias from another magnetically ordered material. Here we demonstrate a pathway to manipulate MA of 3d transition metal oxides (TMOs) by digitally inserting non-magnetic 5d TMOs with pronounced spin-orbit coupling (SOC). High quality superlattices comprised of ferromagnetic La2/3Sr1/3MnO3 (LSMO) and paramagnetic SrIrO3 (SIO) are synthesized with the precise control of thickness at atomic scale. Magnetic easy axis reorientation is observed by controlling the dimensionality of SIO, mediated through the emergence of a novel spin-orbit state within the nominally paramagnetic SIO.

cond-mat.str-el↗

Bandwidth and Electron Correlation-Tuned Superconductivity in Rb$_{0.8}$Fe$_{2}$(Se$_{1-z}$S$_z$)$_2$

We present a systematic angle-resolved photoemission spectroscopy study of the substitution-dependence of the electronic structure of Rb$_{0.8}$Fe$_{2}$(Se$_{1-z}$S$_z$)$_2$ (z = 0, 0.5, 1), where superconductivity is continuously suppressed into a metallic phase. Going from the non-superconducting Rb$_{0.8}$Fe$_{2}$(Se$_{1-z}$S$_z$)$_2$ to superconducting Rb$_{0.8}$Fe$_{2}$Se$_2$, we observe little change of the Fermi surface topology, but a reduction of the overall bandwidth by a factor of 2 as well as an increase of the orbital-dependent renormalization in the $d_{xy}$ orbital. Hence for these heavily electron-doped iron chalcogenides, we have identified electron correlation as explicitly manifested in the quasiparticle bandwidth to be the important tuning parameter for superconductivity, and that moderate correlation is essential to achieving high $T_C$.

cond-mat.supr-con↗