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At least 109 records · Page 6

Nematic transitions in iron pnictide superconductors imaged with a quantum gas

The Scanning Quantum Cryogenic Atom Microscope (SQCRAMscope) uses an atomic Bose–Einstein condensate to measure magnetic fields emanating from solid-state samples. The quantum sensor does so with unprecedented d.c. sensitivity at micrometre resolution, from room to cryogenic temperatures. An additional advantage of the SQCRAMscope is the preservation of optical access to the sample so that magnetometry imaging of, for example, electron transport may be performed in concert with other imaging techniques. Here, we apply this multimodal imaging capability to the study of nematicity in iron pnictide high-temperature superconductors, where the relationship between electronic and structural symmetry breaking resulting in a nematic phase is under debate. We combine the SQCRAMscope with an in situ microscope that measures optical birefringence near the surface. This enables simultaneous and spatially resolved detection of both bulk and near-surface manifestations of nematicity via transport and structural deformation channels, respectively. By performing local measurements of emergent resistivity anisotropy in iron pnictides, we observe sharp, nearly concurrent transport and structural transitions. More broadly, these measurements demonstrate the SQCRAMscope’s ability to reveal important insights into the physics of complex quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Hybrid microstructure of smectite clay gels revealed using neutron and synchrotron X-ray scattering

Aqueous suspensions of swelling clays display a nematic sol-gel transition at very low solid concentrations. The underlying microstructure of the gel has remained a point of contention since the time of Irving Langmuir and has been a major obstacle to fully realizing the potential of clays for practical applications. Here, we comprehensively probe the microstructure of a smectite clay suspension using ultra-small angle neutron/X-ray scattering and find that the nematic gel is structurally ordered and contains entities that are at least an order of magnitude larger than the individual particles. Complementary cryo-electron microscopy shows the presence of domains having particle-particle ordering responsible for nematic texture and regions of particle-particle aggregation responsible for gel-like behavior. We find that the smectic clay gels have a hybrid microstructure with co-existing repulsive nematic domains and attractive disordered domains.

36 MATERIALS SCIENCE↗

Cascade of vestigial orders in two-component superconductors: Nematic, ferromagnetic, s -wave charge- 4 e , and d -wave charge- 4 e states

Electronically ordered states that break multiple symmetries can melt in multiple stages, similarly to liquid crystals. In a partially melted phase, known as vestigial phase, a bilinear made out of combinations of the multiple components of the primary order parameter condenses. Multicomponent superconductors are thus natural candidates for vestigial order since they break both the U⁡(1)-gauge and also time-reversal or lattice symmetries. Here, we use group theory to classify all possible real-valued and complex-valued bilinears of a generic two-component superconductor on a tetragonal or hexagonal lattice. While the more widely investigated real-valued bilinears correspond to vestigial nematic or ferromagnetic order, the little explored complex-valued bilinears correspond to a vestigial charge-4e condensate, which itself can have an underlying s-wave, d x 2 –y 2 -wave, or d xy -wave symmetry. To properly describe the fluctuating regime of the superconducting Ginzburg-Landau action and thus access these competing vestigial phases, we employ both a large-N and a variational method. We show that while vestigial order can be understood as a weak-coupling effect in the large-N approach, it is akin to a moderate-coupling effect in the variational method. Despite these distinctions, both methods yield similar results in wide regions of the parameter space spanned by the quartic Landau coefficients. Specifically, we find that the nematic and ferromagnetic phases are the leading vestigial instabilities, whereas the various types of charge-4⁢e order are attractive albeit subleading vestigial channels. The only exception is for the hexagonal case, in which the nematic and s-wave charge-4e vestigial states are degenerate. Finally, we discuss the limitations of our approach, as well as the implications of our results for the realization of exotic charge-4⁢e states in material candidates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Spin and orbital metallic magnetism in rhombohedral trilayer graphene

We provide a theoretical interpretation of the metallic broken spin-valley (flavor) symmetry states recently discovered in hole-doped rhombohedral trilayer (ABC) graphene in large electric displacement fields. Our conclusions about the phase diagram and phase transitions combine insights from ABC graphene electronic structure models and mean-field theory, and are guided by the precise magneto-oscillation Fermi-surface-area measurements of recent experiments. We find that the principle of momentum-space condensation plays a key role in determining Fermi-surface reconstructions enabled by broken flavor symmetries when the single-particle bands imply thin annular Fermi seas. The reconstructed Fermi sea consists of one large outer Fermi-surface-enclosed majority-flavor states in reciprocal-space area A maj and one or more small inner holelike Fermi-surface-enclosed minority-flavor states in A min that are primarily responsible for nematic order. The competing ground states (valley-Ising, valley-XY, and spin-polarized state) have different A maj /A min and exchange energy maximizes this ratio and selects valley-XY nematic metal as the lowest-energy state. Here, we discuss how the nematic pockets explain the observed fractionalization of quantum oscillation frequencies, and propose anisotropic transport and the nonlinear Hall effect as additional observables.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Kondo enabled transmutation between spinons and superconducting vortices: Origin of magnetic memory in 4 H b − TaS 2

Recent experiments [Persky , ] demonstrate a magnetic memory effect in 4 H b − TaS 2 above its superconducting transition temperature, where Abriokosov vortices are spontaneously generated by lowering the temperature at zero magnetic field after field training the normal state. Motivated by the experiment, we propose the chiral quantum spin liquid (QSL) stabilized in the constituent layers of 4 H b − TaS 2 as a mechanism. We model 4 H b − TaS 2 as coupled layers of the chiral QSL and the superconductor. Through the Kondo coupling between the localized moments and conduction electrons, there is mutual transmutation between spinons and vortices during the thermal-cycling process, which yields the magnetic memory effect observed in experiments. We also propose a mechanism to stabilize chiral and nematic superconductivity in 4 H b − TaS 2 through the Kondo coupling of conduction electrons to the chiral QSL. Our picture suggests 4 H b − TaS 2 as an exciting platform to explore the interplay between QSL and superconductivity through the Kondo effect. Published by the American Physical Society 2024

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Magnetism and charge density wave order in kagome FeGe

Electron correlations often lead to emergent orders in quantum materials, and one example is the kagome lattice materials where topological states exist in the presence of strong correlations between electrons. This arises from the features of the electronic band structure that are associated with the kagome lattice geometry: flat bands induced by destructive interference of the electronic wavefunctions, topological Dirac crossings, and a pair of van Hove singularities. Various correlated electronic phases have been discovered in kagome lattice materials, including magnetism, charge density waves, nematicity, and superconductivity. Recently, a charge-density wave was discovered in the magnetic kagome FeGe, providing a platform for understanding the interplay between charge order and magnetism in kagome materials. Here, we observe all three electronic signatures of the kagome lattice in FeGe using angle-resolved photoemission spectroscopy. The presence of van Hove singularities near the Fermi level is driven by the underlying magnetic exchange splitting. Furthermore, we show spectral evidence for the charge-density wave as gaps near the Fermi level. Furthermore, our observations point to the magnetic interaction-driven band modification resulting in the formation of the charge-density wave, and indicate an intertwined connection between the emergent magnetism and charge order in this moderately-correlated kagome metal.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Final Technical Report for DE-FG02-86ER45268

This work addresses several key issues for understanding the unusual superconductivity in IBS, already shown to be technologically useful materials. 1a). Are reactive gasses like fluorine, chlorine, or water vapor behaving simply as electron donors to cause the superconductivity (at T conset =21 K) in undoped IBS like BaFe 2 As 2 ? 1b). Does exposure to fluorine increase T c in electron-doped IBS materials that are underdoped, e. g. Ba(Fe 0.96 Co 0.04 ) 2 As 2 ? 1c). Can fluorine as a reactive electron-donor, with its relatively greater ease of introduction into the lattice, be used as a rapid tool to search for superconductivity in new materials under investigation? Method of investigation: Using electron probe microanalysis, x-ray photoemission spectroscopy, and dynamical mean field theory calculations, we found that fluorine substitutes for As in the BaFe 2 As 2 lattice, and should therefore behave as an electron donor. We will F-dope Ba(Fe 0.96 Co 0.04 ) 2 As 2 and several new compounds under investigation for superconductivity upon doping to determine fluorine’s effect. Potential impact: If – like for fluorine - a brief exposure to hydrogen indeed causes superconductivity to a depth of 10 microns, this technique could be useful in creating long lengths of superconducting tape without the chemical aggressiveness of fluorine. Using the F ion, which substitutes for As - away from the Fe planes, in underdoped IBS like Ba(Fe 0.96 Co 0.04 ) 2 As 2 may form optimally doped IBS with less impurity scattering of the superconducting Fe 3d electrons resulting in improved superconducting properties. Another potential impact is the speed of checking for superconductivity in new materials under investigation for superconductivity upon doping. 2. What are the effects of Be substitution into IBS, beginning with FeSe and its derivatives (FeSe 1-x S x and FeSe 1-x Te x ) and BaFe 2-x Co x As 2 ? Method of investigation: We recently succeeded in adding Be to the FeSe lattice and found, surprisingly, a factor of four improvement of the low temperature residual resistivity ratio, consistent with improved electronic ordering. Using single crystal x-ray diffraction and x-ray dispersive spectroscopy, determine the concentration and location of the Be dopant. Using resistivity, determine if there is improvement in the residual resistivity achieved by Be doping in the FeSe derivatives (using AlCl 3 :KCl flux growth) and Co-doped BaFe 2 As 2 (using self-flux single crystal growth). Measuring resistivity under strain, determine the changes of the nematic susceptibility at the structural ordering transition causes by the increase in electronic order caused by Be doping in FeSe. Potential impact: Further understanding of IBS, including FeSe which - under physical pressure - has a T c increase to 40 K and -prepared as a monolayer - has a T c reported to be over 100 K. 3. In collaboration, prepare light atom compounds involving Be and look for high pressure-induced superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Local condensation of charge-4 ⁢e superconductivity at a nematic domain wall

In the fluctuation regime that precedes the onset of pairing in multi-component superconductors, such as nematic and chiral superconductors, the normal state is generally unstable towards the formation of charge-4e order – an exotic quantum state in which electrons form coherent quartets rather than Cooper pairs. However, charge-4e order is often suppressed by other competing composite orders, such as nematics. Importantly, the formation of nematic domains is unavoidable due to the long-range strains generated, leading to one-dimensional regions where the competing nematic order is suppressed. Here, we employ a real-space variational approach to demonstrate that, in such nematic domain walls, charge-4e order is locally condensed via a vestigial-order mechanism. Here, we explore the experimental manifestations of this effect and discuss materials in which it can be potentially observed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Charge-4e Superconductivity from Multicomponent Nematic Pairing: Application to Twisted Bilayer Graphene

We show that unconventional nematic superconductors with multicomponent order parameter in lattices with three- and sixfold rotational symmetries support a charge-4e vestigial superconducting phase above T c . The charge-4e state, which is a condensate of four-electron bound states that preserve the rotational symmetry of the lattice, is nearly degenerate with a competing vestigial nematic state, which is nonsuperconducting and breaks the rotational symmetry. This robust result is the consequence of a hidden discrete symmetry in the Ginzburg-Landau theory, which permutes quantities in the gauge sector and in the crystalline sector of the symmetry group. We argue that random strain generally favors the charge-4e state over the nematic phase, as it acts as a random mass to the former but as a random field to the latter. Furthermore, we propose that two-dimensional inhomogeneous systems displaying nematic superconductivity, such as twisted bilayer graphene, provide a promising platform to realize the elusive charge-4e superconducting phase.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Intrinsic nature of chiral charge order in the kagome superconductor Rb V 3 Sb 5

Superconductors with kagome lattices have been identified for over 40 years, with a superconducting transition temperature T c up to 7 K. Recently, certain kagome superconductors have been found to exhibit an exotic charge order, which intertwines with superconductivity and persists to a temperature being one order of magnitude higher than T c . Here, we use scanning tunneling microscopy to study the charge order in kagome superconductor Rb V 3 Sb 5 . We observe both a 2×2 chiral charge order and nematic surface superlattices (predominantly 1×4). We find that the 2×2 charge order exhibits intrinsic chirality with magnetic field tunability. Defects can scatter electrons to introduce standing waves, which couple with the charge order to cause extrinsic effects. While the chiral charge order resembles that discovered in KV 3 Sb 5 , it further interacts with the nematic surface superlattices that are absent in KV 3 Sb 5 but exist in CsV 3 Sb 5 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Orbital ordering in the layered perovskite material CsVF 4

In strongly correlated electronic systems, several novel physical properties are induced by the orbital degree of freedom. In particular, orbital degeneracy near the Fermi level leads to spontaneous symmetry breaking, such as the nematic state in FeSe and the orbital ordering in several perovskite systems. Here, the novel layered perovskite material CsVF 4 , with a 3 d 2 electronic configuration, was systematically studied using density-functional theory and a multiorbital Hubbard model within the Hatree-Fock approximation. Furthermore, our results show that CsVF 4 should be magnetic, with a G-type antiferromagnetic arrangement in the a b plane and weak antiferromagnetic exchange along the c axis, in agreement with experimental results. Driven by the Jahn-Teller distortion in the VF 6 octahedra that shorten the c axis, the system displays an interesting electron occupancy d x y 1 ( d x z d y z ) 1 corresponding to the lower nondegenerate d x y orbital being half-filled and the other two degenerate d y z and d x z orbitals sharing one electron per site. We show that this degeneracy is broken and a novel d y z / d x z staggered orbital pattern is here predicted by both the first-principles and Hubbard model calculations. This orbital ordering is driven by the electronic instability associated with degeneracy removal to lower the energy.

36 MATERIALS SCIENCE↗

Impact of nematicity on the relationship between antiferromagnetic fluctuations and superconductivity in FeSe 0.91 S 0.09 under pressure

The sulfur-substituted FeSe system, FeSe 1 - x S x , provides a versatile platform for studying the relationship among nematicity, antiferromagnetism, and superconductivity. Herein, by nuclear magnetic resonance (NMR) and resistivity measurements up to 4.73 GPa on FeSe 0.91 S 0.09 , we established the pressure- ( p -) temperature ( T ) phase diagram in which the nematic state is suppressed with pressure showing a nematic quantum phase transition (QPT) around p = 0.5 GPa , two superconductivity (SC) regions separated by the QPT appear, and antiferromagnetic (AFM) phase emerges above ~ 3.3 GPa . From the NMR results up to 2.1 GPa, AFM fluctuations are revealed to be characterized by the stripe-type wave vector which remains the same for the two SC regions. Furthermore, the electronic state is discovered to change in character from non-Fermi liquid to Fermi liquid around the nematic QPT and persists up to ~ 2.1 GPa . In addition, although the AFM fluctuations correlate with T c in both SC states, demonstrating the importance of the AFM fluctuations for the appearance of SC in the system, we found that, when nematic order is absent, T c is strongly correlated with the AFM fluctuations whereas T c weakly depends on the AFM fluctuations when nematic order is present. Our findings on FeSe 0.91 S 0.09 were shown to be applied to the whole FeSe 1 - x S x system and offer an insight into the relationship between AFM fluctuations and SC in Fe-based superconductors.

36 MATERIALS SCIENCE↗

Nematic quantum criticality in an Fe-based superconductor revealed by strain-tuning

Quantum criticality may be essential to understanding a wide range of exotic electronic behavior; however, conclusive evidence of quantum critical fluctuations has been elusive in many materials of current interest. An expected characteristic feature of quantum criticality is power-law behavior of thermodynamic quantities as a function of a nonthermal tuning parameter close to the quantum critical point (QCP). Here, we observed power-law behavior of the critical temperature of the coupled nematic/structural phase transition as a function of uniaxial stress in a representative family of iron-based superconductors, providing direct evidence of quantum critical nematic fluctuations in this material. These quantum critical fluctuations are not confined within a narrow regime around the QCP but rather extend over a wide range of temperatures and compositions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Anomalous Nematic States in High Half-Filled Landau Levels

It is well established that the ground states of a two-dimensional electron gas with half-filled high ( N ≥ 2 ) Landau levels are compressible charge-ordered states, known as quantum Hall stripe (QHS) phases. The generic features of QHSs are a maximum (minimum) in a longitudinal resistance R x x ( R y y ) and a nonquantized Hall resistance R H . In this letter, we report on emergent minima (maxima) in R x x ( R y y ) and plateaulike features in R H in half-filled N ≥ 3 Landau levels. Remarkably, these unexpected features develop at temperatures considerably lower than the onset temperature of QHSs, suggestive of a new ground state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Aligned 2D carbon nanotube liquid crystals for wafer-scale electronics

Semiconducting carbon nanotubes promise faster performance and lower power consumption than Si in field-effect transistors (FETs) if they can be aligned in dense arrays. Here, we demonstrate that nanotubes collected at a liquid/liquid interface self-organize to form two-dimensional (2D) nematic liquid crystals that globally align with flow. The 2D liquid crystals are transferred onto substrates in a continuous process generating dense arrays of nanotubes aligned within ±6°, ideal for electronics. Nanotube ordering improves with increasing concentration and decreasing temperature due to the underlying liquid crystal phenomena. The excellent alignment and uniformity of the transferred assemblies enable FETs with exceptional on-state current density averaging 520 μA μm -1 at only -0.6 V, and variation of only 19%. FETs with ion gel top gates demonstrate subthreshold swing as low as 60 mV decade -1 . Deposition across a 10-cm substrate is achieved, evidencing the promise of 2D nanotube liquid crystals for commercial semiconductor electronics.

42 ENGINEERING↗

Titanium doped kagome superconductor CsV 3–x Ti x Sb 5 and two distinct phases

The vanadium-based kagome superconductor CsV 3 Sb 5 has attracted tremendous attention due to its unexcepted anomalous Hall effect (AHE), charge density waves (CDWs), nematicity, and a pseudogap pair density wave (PDW) coexisting with unconventional strong-coupling superconductivity. The origins of CDWs, unconventional superconductivity, and their correlation with different electronic states in this kagome system are of great significance, but so far, are still under debate. Chemical doping in the kagome layer provides one of the most direct ways to reveal the intrinsic physics, but remains unexplored. Here, we report, for the first time, the synthesis of Ti-substituted CsV 3 Sb 5 single crystals and its rich phase diagram mapping the evolution of intertwining electronic states. The Ti atoms directly substitute for V in the kagome layers. CsV 3–x Ti x Sb 5 shows two distinct superconductivity phases upon substitution. The Ti slightly-substituted phase displays an unconventional V-shaped superconductivity gap, coexisting with weakening CDW, PDW, AHE, and nematicity. The Ti highly-substituted phase has a U-shaped superconductivity gap concomitant with a short-range rotation symmetry breaking CDW, while long-range CDW, twofold symmetry of in-plane resistivity, AHE, and PDW are absent. Furthermore, we also demonstrate the chemical substitution of V atoms with other elements such as Cr and Nb, showing a different modulation on the superconductivity phases and CDWs. These findings open up a way to synthesise a new family of doped CsV 3 Sb 5 materials, and further represent a new platform for tuning the different correlated electronic states and superconducting pairing in kagome superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Interplay of 𝑑- and 𝑝-states in RbTi3⁢Bi5 and CsTi3⁢Bi5 flat-band kagome metals

Shifting the Fermi level of the celebrated 𝐴⁢𝑀3⁢𝑋5 (135) compounds into proximity of flat bands strongly enhances electronic correlations and severely affects the formation of density waves and superconductivity. Our broadband infrared spectroscopy measurements of RbTi3⁢Bi5 and CsTi3⁢Bi5 combined with density-functional band-structure calculations reveal that the correlated Ti 𝑑-states are intricately coupled with the Bi 𝑝-states that form a tilted Dirac crossing. Electron-phonon coupling manifests itself in the strong damping of itinerant carriers and in the anomalous shape of the phonon line in RbTi3⁢Bi5. An anomaly in these spectral features around 150 K can be paralleled to the onset of nematicity detected by low-temperature probes. Our findings show that the materials with low band filling open unexplored directions in the physics of kagome metals and involve electronic states of different nature strongly coupled with lattice dynamics.

Wenzel, Matthew [ORNL]↗

Twisted bilayered graphenes at magic angles and Casimir interactions: correlation-driven effects

Twisted bilayered graphenes (TBGs) at magic angles are systems housing long ranged periodicity of moiré patterns together with short ranged periodicity associated with the individual graphenes. Such materials are a fertile ground for novel states largely driven by electronic correlations. Here we find that the ubiquitous Casimir force can serve as a platform for macroscopic manifestations of the quantum effects stemming from the magic angle bilayered graphenes properties and their phases determined by electronic correlations. In conclusion, by utilizing comprehensive calculations for the electronic and optical response, we find that Casimir torque can probe anisotropy from the Drude conductivities in nematic states, while repulsion in the Casimir force can help identify topologically nontrivial phases in magic angle TBGs.

36 MATERIALS SCIENCE↗