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Birgeneau, Robert J.

Publications and source records attributed to Birgeneau, Robert J..

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Tailoring physical properties of crystals through synthetic temperature control: A case study for new polymorphic NbFeT e 2 phases

Growth parameters play a significant role in the crystal quality and physical properties of layered materials. Here we present a case study on a van der Waals magnetic NbFeTe 2 material. Two different types of polymorphic NbFeTe 2 phases, synthesized at different temperatures, display significantly different behaviors in crystal symmetry, electronic structure, electrical transport, and magnetism. While the phase synthesized at low temperature showing behavior consistent with previous reports, the new phase synthesized at high temperature, has completely different physical properties, such as metallic resistivity, long-range ferromagnetic order, anomalous Hall effect, negative magnetoresistance, and distinct electronic structures. Neutron diffraction reveals out-of-plane ferromagnetism below 70 K, consistent with the electrical transport and magnetic susceptibility studies. Finally, our work suggests that simply tuning synthetic parameters in a controlled manner could be an effective route to alter the physical properties of existing materials potentially unlocking new states of matter, or even discovering new materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Thermal evolution of spin excitations in honeycomb Ising antiferromagnetic FePSe 3

We use elastic and inelastic neutron scattering (INS) to study the antiferromagnetic (AF) phase transitions and spin excitations in the two-dimensional (2D) zig-zag antiferromagnet FePSe 3 . By determining the magnetic order parameter across the AF phase transition, we conclude that the AF phase transition in FePSe 3 is first-order in nature. In addition, our INS measurements reveal that the spin waves in the AF ordered state have a large easy-axis magnetic anisotropy gap, consistent with an Ising Hamiltonian, and possible biquadratic magnetic exchange interactions. On warming across T N , we find that dispersive spin excitations associated with three-fold rotational symmetric AF fluctuations change into FM spin fluctuations above T N . These results suggest that the first-order AF phase transition in FePSe 3 may arise from the competition between C 3 symmetric AF and C 1 symmetric FM spin fluctuations around T N , in place of a conventional second-order AF phase transition.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Antiferromagnetic order in the layered magnetic topological insulator MnBi 2 ⁢Se 4 probed by resonant soft x-ray scattering

The quasi-two-dimensional magnetic topological insulator MnBi 2 Se 4 , stabilized via nonequilibrium molecular beam epitaxy, is investigated by resonant soft x-ray scattering. Kiessig fringes are observed, confirming a high sample quality and a thin film thickness of 10 septuple layers (∼13 nm). An antiferromagnetic Bragg peak is observed at the structurally forbidden reflection, whose magnetic nature is validated by studying its temperature, energy, and polarization dependence. Through a detailed analysis, an A-type antiferromagetic order with in-plane moments is implied. This alternative spin structure in MnBi 2 Se 4 , in contrast to the Ising antiferromagnetic states in other magnetic topological insulators, might be relevant for hosting new topological states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Spectral evidence for local-moment ferromagnetism in the van der Waals metals $\mathrm{Fe_3GaTe_2}$ and $\mathrm{Fe_3GeTe_2}$

Magnetism in two-dimensional (2D) materials has attracted considerable attention recently for both fundamental understanding of magnetism and its tunability towards device applications. The isostructural Fe 3 GeTe 2 and Fe 3 GaTe 2 are two members of the Fe-based van der Waals (vdW) ferromagnet family, but exhibit very different Curie temperatures (T C ) of 210 and 360 K, respectively. In this report by using angle-resolved photoemission spectroscopy and density functional theory, we systematically compare the electronic structures of the two compounds. Qualitative similarities in the Fermi surface can be found between the two compounds, with expanded hole pockets in Fe 3 GaTe 2 suggesting additional hole carriers compared to Fe 3 GeTe 2 . Interestingly, we observe almost no band shift in Fe 3 GaTe 2 across its T C of 360 K, compared to a small shift in Fe 3 GeTe 2 across its T C of 210 K. The weak temperature-dependent evolution strongly deviates from the expectations of an itinerant Stoner mechanism. Our results suggest that itinerant electrons have minimal contributions to the enhancement of T C in Fe 3 GaTe 2 compared to Fe 3 GeTe 2 , and that the nature of ferromagnetism in these Fe-based vdW ferromagnets must be understood with considerations of the electron correlations.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Two-step electronic response to magnetic ordering in a van der Waals ferromagnet

The two-dimensional material Cr 2 ⁢Ge 2 ⁢Te 6 is a member of the class of insulating van der Waals (vdW) magnets. Here, using high resolution angle-resolved photoemission spectroscopy in a detailed temperature dependence study, we identify a clear response of the electronic structure to a dimensional crossover in the form of two distinct temperature scales marking onsets of modifications in the electronic structure. Specifically, we observe Te 𝑝-orbital-dominated bands to undergo changes at the Curie transition temperature 𝑇 𝐶 while the Cr 𝑑-orbital-dominated bands begin evolving at a higher temperature scale. Combined with neutron scattering, density functional theory calculations, and Monte Carlo simulations, we find that the electronic system can be consistently understood to respond sequentially to the distinct temperatures at which in-plane and out-of-plane spin correlations exceed a characteristic length scale. Finally, our findings reveal the sensitivity of the orbital-selective electronic structure for probing the dynamical evolution of local moment correlations in vdW insulating magnets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Room-Temperature, Current-Induced Magnetization Self-Switching in A Van Der Waals Ferromagnet

2D layered materials with broken inversion symmetry are being extensively pursued as spin source layers to realize high-efficiency magnetic switching. Such low-symmetry layered systems are, however, scarce. In addition, most layered magnets with perpendicular magnetic anisotropy show a low Curie temperature. Here, in this study, the experimental observation of spin–orbit torque magnetization self-switching at room temperature in a layered polar ferromagnetic metal, Fe 2.5 Co 2.5 GeTe 2 is reported. The spin–orbit torque is generated from the broken inversion symmetry along the c-axis of the crystal. These results provide a direct pathway toward applicable 2D spintronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Ideal weak topological insulator and protected helical saddle points

Here we report the design and observation of an ideal weak topological insulator in a quasi-one-dimensional bismuth halide, Bi 4 I 1.2 Br 2.8 . Via angle-resolved photoemission spectroscopy, we identify that Bi 4 I 1.2 Br 2.8 hosts topological surface states on the (100)′ side surface in the form of two anisotropic π-offset Dirac cones while topologically dark on the (001) top surface. The results fully determine a unique side-surface Hamiltonian and thereby identify two pairs of nondegenerate helical saddle points. The fact that both the surface Dirac and helical saddle points are in the global bulk band gap of 195 meV suggests the potential of this system to be a fertile ground for topological many-body physics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Discovery of Charge Order in the Transition Metal Dichalcogenide Fe x NbS 2

The Fe intercalated transition metal dichalcogenide (TMD), Fe 1/3 NbS 2 , exhibits remarkable resistance switching properties and highly tunable spin ordering phases due to magnetic defects. We conduct synchrotron x-ray scattering measurements on both underintercalated ( x = 0.32 ) and overintercalated ( x = 0.35 ) samples. We discover a new charge order phase in the overintercalated sample, where the excess Fe atoms lead to a zigzag antiferromagnetic order. The agreement between the charge and magnetic ordering temperatures, as well as their intensity relationship, suggests a strong magnetoelastic coupling as the mechanism for the charge ordering. In conclusion, our results reveal the first example of a charge order phase among the intercalated TMD family and demonstrate the ability to stabilize charge modulation by introducing electronic correlations, where the charge order is absent in bulk 2H - NbS 2 compared to other pristine TMDs.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Charge order induced Dirac pockets in the nonsymmorphic crystal TaTe 4

The interplay between charge order (CO) and nontrivial band topology has spurred tremendous interest in understanding topological excitations beyond the single-particle description. In a quasi-one-dimensional nonsymmorphic crystal TaTe 4 , the (2a×2b×3c) charge ordered ground state drives the system into a space group where the symmetry indicator features the emergence of Dirac fermions and unconventional double Dirac fermions. In this study, using angle-resolved photoemission spectroscopy and first-principles calculations, we provide evidence of the CO induced Dirac fermion-related bands near the Fermi level. Furthermore, the band folding at the Fermi level is compatible with the new periodicity dictated by the CO, indicating that the electrons near the Fermi level follow the crystalline symmetries needed to host double Dirac fermions in this system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Spectral evidence for unidirectional charge density wave in detwinned BaNi 2 As 2

In the iron-based superconductors, unconventional superconductivity emerges in proximity to intertwined electronic orders consisting of an electronic nematic order and a spin density wave (SDW). Recently, BaNi 2 As 2 , like its well-known iron-based analog BaFe 2 As 2 , has been discovered to host a symmetry-breaking structural transition but coupled to a unidirectional charge density wave (CDW) instead of SDW, providing a novel platform to study intertwined orders. Here, in this work, through a systematic angle-resolved photoemission spectroscopy study combined with a detwinning B 1 g uniaxial strain, we identify distinct spectral evidence of band evolution due to the structural transition as well as CDW-induced band folding. In contrast to the nematicity and spin density wave in BaFe 2 As 2 , the structural and CDW order parameters in BaNi 2 As 2 are observed to be strongly coupled and do not separate in the presence of uniaxial strain. Furthermore, no nematic band splitting is resolved above the structural transition. Our measurements point to a likely lattice origin of the CDW order in BaNi 2 As 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Kramers nodal lines and Weyl fermions in SmAlSi

Kramers nodal lines (KNLs) have recently been proposed theoretically as a special type of Weyl line degeneracy connecting time-reversal invariant momenta. KNLs are robust to spin orbit coupling and are inherent to all non-centrosymmetric achiral crystal structures, leading to unusual spin, magneto-electric, and optical properties. However, their existence in in real quantum materials has not been experimentally established. Here we gather the experimental evidence pointing at the presence of KNLs in SmAlSi, a non-centrosymmetric metal that develops incommensurate spin density wave order at low temperature. Using angle-resolved photoemission spectroscopy, density functional theory calculations, and magneto-transport methods, we provide evidence suggesting the presence of KNLs, together with observing Weyl fermions under the broken inversion symmetry in the paramagnetic phase of SmAlSi. We discuss the nesting possibilities regarding the emergent magnetic orders in SmAlSi. Our results provide a solid basis of experimental observations for exploring correlated topology in SmAlSi.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Thermal cycling induced alteration of the stacking order and spin-flip in the room temperature van der Waals magnet Fe 5 GeTe 2

The magnetic properties of the quasi-two-dimensional van der Waals magnet Fe 5–δ GeTe 2 (F5GT), which has a high ferromagnetic ordering temperature T C ~315 K, remain to be better understood. It has been demonstrated that the magnetization of F5GT is sensitive to both the Fe deficiency δ and the thermal-cycling history. Here, we investigate the structural and magnetic properties of F5GT single crystals with a minimal Fe deficiency (|δ |≤ 0.1), utilizing combined x-ray and neutron scattering techniques. Herein our study reveals that the quenched F5GT single crystals experience an irreversible, first-order transition at T S ~110 K upon first cooling, where the stacking order partly or entirely converts from ABC-stacking order to AA-stacking order. Importantly, the magnetic properties, including the magnetic moment direction and the enhanced T C after the thermal cycling, are intimately related to the alteration of the stacking order. Our work highlights the significant influence of the lattice symmetry to the magnetism in F5GT.

2-dimensional systems↗
DOE OSTI2023

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↗
DOE OSTI2022

Single-crystal growth and superconductivity in RbNi 2 Se 2

Herein we report the synthesis and characterization of RbNi 2 Se 2 , an analog of the iron chalcogenide superconductor Rb x Fe 2 Se 2 , via transport, angle-resolved photoemission spectroscopy, and density functional theory calculations. A superconducting transition at T c =1.20 K is identified. In the normal state, RbNi 2 Se 2 shows paramagnetic and Fermi-liquid behaviors. A large Sommerfeld coefficient yields an effective electron mass of m* ≈ 6m e . In the superconducting state, zero-field electronic specific-heat data C es can be described by a two-gap BCS model, indicating that RbNi 2 Se 2 is a possible multigap superconductor. Our density functional theory calculations and angle-resolved photoemission spectroscopy measurements demonstrate that RbNi 2 Se 2 exhibits relatively weak correlations and multiband characteristics, consistent with the multigap superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Discovery of charge density wave in a kagome lattice antiferromagnet

A hallmark of strongly correlated quantum materials is the rich phase diagram resulting from competing and intertwined phases with nearly degenerate ground state energies. A well-known example is the copper oxides, where a charge density wave (CDW) is ordered well above and strongly coupled to the magnetic order to form spin-charge separated stripes that compete with superconductivity. Recently, such rich phase diagrams have also been revealed in correlated topological materials. In two-dimensional kagome lattice metals consisting of corner-sharing triangles, the geometry of the lattice can produce flat bands with localized electrons, non-trivial topology, chiral magnetic order, superconductivity and CDW order. While CDW has been found in weakly electron correlated nonmagnetic AV 3 Sb 5 (A = K, Rb, Cs), it has not yet been observed in correlated magnetic ordered kagome lattice metals. Here we report the discovery of CDW within the antiferromagnetic (AFM) ordered phase of kagome lattice FeGe. The CDW in FeGe occurs at wavevectors identical to that of AV 3 Sb 5 , enhances the AFM ordered moment, and induces an emergent anomalous Hall effect. Furthermore, our findings suggest that CDW in FeGe arises from the combination of electron correlations-driven AFM order and van Hove singularities-driven instability possibly associated with a chiral flux phase, in stark contrast to strongly correlated copper oxides and nickelates, where the CDW precedes or accompanies the magnetic order.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Antiferromagnetic order in Co-doped Fe 5 GeTe 2 probed by resonant magnetic x-ray scattering

The quasi-two-dimensional van der Waals magnet Fe 5-δ GeTe 2 has emerged as a promising platform for electronic and spintronic functionalities at room temperature, owing to its large ferromagnetic ordering temperature T C ≈ 315 K. Interestingly, by cobalt (Co) substitution of iron in F5GT, i.e., (Fe 1-x Co x ) 5-δ GeTe 2 (Co-F5GT), not only can its magnetic transition temperature be further enhanced, but the magnetic and structural ground states can also be tuned. Specifically, an antiferromagnetic (AFM) order is induced beyond the Co doping level x ≥ 0.4. Here, in this work, we investigate the magnetic properties of a Co-F5GT single crystal at x = 0.45(1), by utilizing the element-specific, resonant magnetic x-ray scattering technique. Our study reveals an A-type, Ising-like AFM ground state, with a transition temperature T N ≈ 340 K. In addition, our work unveils an important contribution from Co magnetic moments to the magnetic order. The application of the in-plane magnetic fields gradually polarizes the spin moments along the field direction, but without inducing incommensurate spin texture(s).

36 MATERIALS SCIENCE↗
DOE OSTI2022

Effect of iron vacancies on magnetic order and spin dynamics of the spin ladder BaFe 2-δ S 1.5 Se 1.5</sub

Quasi-one-dimensional iron chalcogenides possess various magnetic states depending on the lattice distortion, electronic correlations, and presence of defects. Here we present neutron diffraction and inelastic neutron scattering experiments on the spin ladder compound BaFe 2-δ S 1.5 Se 1.5 with ~6% iron vacancies. The data reveal that long-range magnetic order is absent, while the characteristic magnetic excitations that correspond to both the stripe- and block-type antiferromagnetic correlations are observed. First-principles calculations support the existence of both stripe- and block-type antiferromagnetic short-range orders in the experimental sample. The disappearance of long-range magnetic order may be due to the competition between these two magnetic orders, which is greatly enhanced for a certain concentration of iron vacancies, which we calculate to be about 6%, consistent with the measured iron vacancy concentration. Our results highlight how iron vacancies in the iron-based spin ladder system strongly influence the magnetic ground state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗