Valence band electronic structure of the van der Waals ferromagnetic insulators: VI[Formula: see text] and CrI[Formula: see text].

Ferromagnetic van der Waals (vdW) insulators are of great scientific interest for their promising applications in spintronics. It has been indicated that in the two materials within this class, CrI[Formula: see text] and VI[Formula: see text], the magnetic ground state, the band gap, and the Fermi level could be manipulated by varying the layer thickness, strain or doping. To understand how these factors impact the properties, a detailed understanding of the electronic structure would be required. However, the experimental studies of the electronic structure of these materials are still very sparse. Here, we present the detailed electronic structure of CrI[Formula: see text] and VI[Formula: see text] measured by angle-resolved photoemission spectroscopy (ARPES). Our results show a band-gap of the order of 1 eV, sharply contrasting some theoretical predictions such as Dirac half-metallicity and metallic phases, indicating that the intra-atomic interaction parameter (U) and spin-orbit coupling (SOC) were not properly accounted for in the calculations. We also find significant differences in the electronic properties of these two materials, in spite of similarities in their crystal structure. In CrI[Formula: see text], the valence band maximum is dominated by the I 5p, whereas in VI[Formula: see text] it is dominated by the V 3d derived states. Our results represent valuable input for further improvements in the theoretical modeling of these systems.

Disappearance of superconductivity due to vanishing coupling in the overdoped Bi[Formula: see text]Sr[Formula: see text]CaCu[Formula: see text]O[Formula: see text].

In cuprate superconductors, superconductivity is accompanied by a plethora of orders and phenomena that complicate our understanding of superconductivity in these materials. Prominent in the underdoped regime, these orders weaken or vanish with overdoping. Here, we approach the superconducting phase from the more conventional overdoped side. We present angle-resolved photoemission spectroscopy studies of Bi[Formula: see text]Sr[Formula: see text]CaCu[Formula: see text]O[Formula: see text], cleaved and annealed in ozone to increase the doping all the way to the non-superconducting phase. We show that the mass renormalization in the antinodal region of the Fermi surface that possibly reflects the pairing, weakens with doping and completely disappears precisely where superconductivity disappears. This is the evidence that in the overdoped regime, superconductivity is determined primarily by the coupling strength. A doping dependence and an abrupt disappearance above the transition temperature eliminate phononic mechanism of the observed renormalization and identify the onset of spin-fluctuations as its likely origin.

Phase diagram of Bi2Sr2CaCu2O8+δ revisited.

In cuprate superconductors, the doping of carriers into the parent Mott insulator induces superconductivity and various other phases whose characteristic temperatures are typically plotted versus the doping level p. In most materials, p cannot be determined from the chemical composition, but it is derived from the superconducting transition temperature, Tc, using the assumption that the Tc dependence on doping is universal. Here, we present angle-resolved photoemission studies of Bi2Sr2CaCu2O8+δ, cleaved and annealed in vacuum or in ozone to reduce or increase the doping from the initial value corresponding to Tc = 91 K. We show that p can be determined from the underlying Fermi surfaces and that in-situ annealing allows mapping of a wide doping regime, covering the superconducting dome and the non-superconducting phase on the overdoped side. Our results show a surprisingly smooth dependence of the inferred Fermi surface with doping. In the highly overdoped regime, the superconducting gap approaches the value of 2Δ0 = (4 ± 1)kBTc.

Band Structure of the IV-VI Black Phosphorus Analog and Thermoelectric SnSe.

The success of black phosphorus in fast electronic and photonic devices is hindered by its rapid degradation in the presence of oxygen. Orthorhombic tin selenide is a representative of group IV-VI binary compounds that are robust and isoelectronic and share the same structure with black phosphorus. We measure the band structure of SnSe and find highly anisotropic valence bands that form several valleys having fast dispersion within the layers and negligible dispersion across. This is exactly the band structure desired for efficient thermoelectric generation where SnSe has shown great promise.

Sn-doped Bi1.1Sb0.9Te2S bulk crystal topological insulator with excellent properties.

A long-standing issue in topological insulator research has been to find a bulk single crystal material that provides a high-quality platform for characterizing topological surface states without interference from bulk electronic states. This material would ideally be a bulk insulator, have a surface state Dirac point energy well isolated from the bulk valence and conduction bands, display quantum oscillations from the surface state electrons and be growable as large, high-quality bulk single crystals. Here we show that this material obstacle is overcome by bulk crystals of lightly Sn-doped Bi1.1Sb0.9Te2S grown by the vertical Bridgman method. We characterize Sn-BSTS via angle-resolved photoemission spectroscopy, scanning tunnelling microscopy, transport studies, X-ray diffraction and Raman scattering. We present this material as a high-quality topological insulator that can be reliably grown as bulk single crystals and thus studied by many researchers interested in topological surface states.

Gapped Surface States in a Strong-Topological-Insulator Material.

A three-dimensional strong-topological insulator or semimetal hosts topological surface states which are often said to be gapless so long as time-reversal symmetry is preserved. This narrative can be mistaken when surface state degeneracies occur away from time-reversal-invariant momenta. The mirror invariance of the system then becomes essential in protecting the existence of a surface Fermi surface. Here we show that such a case exists in the strong-topological-semimetal Bi(4)Se(3). Angle-resolved photoemission spectroscopy and ab initio calculations reveal partial gapping of surface bands on the Bi(2)Se(3) termination of Bi(4)Se(3)(111), where an 85 meV gap along Γ̅K̅ closes to zero toward the mirror-invariant Γ̅M̅ azimuth. The gap opening is attributed to an interband spin-orbit interaction that mixes states of opposite spin helicity.

Spin-orbit interactions and the nematicity observed in the fe-based superconductors.

High-resolution angle-resolved photoelectron spectroscopy is used to examine the electronic band structure of FeTe_{0.5}Se_{0.5} near the Brillouin zone center. A consistent separation of the α_{1} and α_{2} bands is observed with little k_{z} dependence of the α_{1} band. First-principles calculations for bulk and thin films demonstrate that the antiferromagnetic coupling between the Fe atoms and hybridization-induced spin-orbit effects lifts the degeneracy of the Fe d_{xz} and d_{yz} orbitals at the zone center leading to orbital ordering. These experimental and computational results provide a natural microscopic basis for the nematicity observed in the Fe-based superconductors.

Quasiparticle interference, quasiparticle interactions, and the origin of the charge density wave in 2H-NbSe2.

We show that a small number of intentionally introduced defects can be used as a spectroscopic tool to amplify quasiparticle interference in 2H-NbSe2 that we measure by scanning tunneling spectroscopic imaging. We show, from the momentum and energy dependence of the quasiparticle interference, that Fermi surface nesting is inconsequential to charge density wave formation in 2H-NbSe2. We demonstrate that, by combining quasiparticle interference data with additional knowledge of the quasiparticle band structure from angle resolved photoemission measurements, one can extract the wave vector and energy dependence of the important electronic scattering processes thereby obtaining direct information both about the fermiology and the interactions. In 2H-NbSe2, we use this combination to confirm that the important near-Fermi-surface electronic physics is dominated by the coupling of the quasiparticles to soft mode phonons at a wave vector different from the charge density wave ordering wave vector.

Surface Collective Modes in the Topological Insulators Bi_{2}Se_{3} and Bi_{0.5}Sb_{1.5}Te_{3-x}Se_{x}.

We used low-energy, momentum-resolved inelastic electron scattering to study surface collective modes of the three-dimensional topological insulators Bi_{2}Se_{3} and Bi_{0.5}Sb_{1.5}Te_{3-x}Se_{x}. Our goal was to identify the "spin plasmon" predicted by Raghu and co-workers [Phys. Rev. Lett. 104, 116401 (2010)]. Instead, we found that the primary collective mode is a surface plasmon arising from the bulk, free carriers in these materials. This excitation dominates the spectral weight in the bosonic function of the surface χ^{"}(q,ω) at THz energy scales, and is the most likely origin of a quasiparticle dispersion kink observed in previous photoemission experiments. Our study suggests that the spin plasmon may mix with this other surface mode, calling for a more nuanced understanding of optical experiments in which the spin plasmon is reported to play a role.

Electronic structure basis for the extraordinary magnetoresistance in WTe2.

The electronic structure basis of the extremely large magnetoresistance in layered nonmagnetic tungsten ditelluride has been investigated by angle-resolved photoelectron spectroscopy. Hole and electron pockets of approximately the same size were found at low temperatures, suggesting that carrier compensation should be considered the primary source of the effect. The material exhibits a highly anisotropic Fermi surface from which the pronounced anisotropy of the magnetoresistance follows. A change in the Fermi surface with temperature was found and a high-density-of-states band that may take over conduction at higher temperatures and cause the observed turn-on behavior of the magnetoresistance in WTe2 was identified.

Absence of a proximity effect for a thin-films of a Bi2Se3 topological insulator grown on top of a Bi2Sr2CaCu2O(8+δ) cuprate superconductor.

Proximity-induced superconductivity in a 3D topological insulator represents a new avenue for observing zero-energy Majorana fermions inside vortex cores. Relatively small gaps and low transition temperatures of conventional s-wave superconductors put hard constraints on these experiments. Significantly larger gaps and higher transition temperatures in cuprate superconductors might be an attractive alternative to considerably relax these constraints, but it is not clear whether the proximity effect would be effective in heterostructures involving cuprates and topological insulators. Here, we present angle-resolved photoemission studies of thin Bi(2)Se(3) films grown in situ on optimally doped Bi(2)Sr(2)CaCu(2)O(8+δ) substrates that show the absence of proximity-induced gaps on the surfaces of Bi(2)Se(3) films as thin as a 1.5 quintuple layer. These results suggest that the superconducting proximity effect between a cuprate superconductor and a topological insulator is strongly suppressed, likely due to a very short coherence length along the c axis, incompatible crystal and pairing symmetries at the interface, small size of the topological surface state's Fermi surface, and adverse effects of a strong spin-orbit coupling in the topological material.

Inducing a Lifshitz transition by extrinsic doping of surface bands in the topological crystalline insulator Pb1-xSnxSe.

The narrow gap semiconductor Pb1-xSnxSe was investigated for topologically protected surface states in its rocksalt structural phase for x=0.45, 0.23, 0.15, and 0. Angle-resolved photoelectron spectroscopy of intrinsically p-doped samples showed a clear indication of two Dirac cones, eccentric about the time-reversal invariant point X¯ of the surface Brillouin zone for all but the x=0 sample. Adsorption of alkalies gradually filled the surface bands with electrons, driving the x>0 topological crystalline insulator systems through Lifshitz transitions, and from a holelike to electronlike Fermi surface. The electron-doped bands in x>0 samples exhibited the full configuration of the Dirac cones, also confirming electron-hole symmetry of the surface bands.

The mechanism of caesium intercalation of graphene.

Properties of many layered materials, including copper- and iron-based superconductors, topological insulators, graphite and epitaxial graphene, can be manipulated by the inclusion of different atomic and molecular species between the layers via a process known as intercalation. For example, intercalation in graphite can lead to superconductivity and is crucial in the working cycle of modern batteries and supercapacitors. Intercalation involves complex diffusion processes along and across the layers; however, the microscopic mechanisms and dynamics of these processes are not well understood. Here we report on a novel mechanism for intercalation and entrapment of alkali atoms under epitaxial graphene. We find that the intercalation is adjusted by the van der Waals interaction, with the dynamics governed by defects anchored to graphene wrinkles. Our findings are relevant for the future design and application of graphene-based nano-structures. Similar mechanisms can also have a role for intercalation of layered materials.

Measurement of an exceptionally weak electron-phonon coupling on the surface of the topological insulator Bi2Se3 using angle-resolved photoemission spectroscopy.

Gapless surface states on topological insulators are protected from elastic scattering on nonmagnetic impurities which makes them promising candidates for low-power electronic applications. However, for widespread applications, these states should have to remain coherent at ambient temperatures. Here, we studied temperature dependence of the electronic structure and the scattering rates on the surface of a model topological insulator, Bi2Se3, by high-resolution angle-resolved photoemission spectroscopy. We found an extremely weak broadening of the topological surface state with temperature and no anomalies in the state's dispersion, indicating exceptionally weak electron-phonon coupling. Our results demonstrate that the topological surface state is protected not only from elastic scattering on impurities, but also from scattering on low-energy phonons, suggesting that topological insulators could serve as a basis for room-temperature electronic devices.

Photoemission spectroscopy of magnetic and nonmagnetic impurities on the surface of the Bi2Se3 topological insulator.

Dirac-like surface states on surfaces of topological insulators have a chiral spin structure that suppresses backscattering and protects the coherence of these states in the presence of nonmagnetic scatterers. In contrast, magnetic scatterers should open the backscattering channel via the spin-flip processes and degrade the state's coherence. We present angle-resolved photoemission spectroscopy studies of the electronic structure and the scattering rates upon the adsorption of various magnetic and nonmagnetic impurities on the surface of Bi2Se3, a model topological insulator. We reveal a remarkable insensitivity of the topological surface state to both nonmagnetic and magnetic impurities in the low impurity concentration regime. Scattering channels open up with the emergence of hexagonal warping in the high-doping regime, irrespective of the impurity's magnetic moment.

The electron spectro-microscopy beamline at National Synchrotron Light Source II: a wide photon energy range, micro-focusing beamline for photoelectron spectro-microscopies.

A comprehensive optical design for a high-resolution, high-flux, wide-energy range, micro-focused beamline working in the vacuum ultraviolet and soft x-ray photon energy range is proposed. The beamline is to provide monochromatic radiation to three photoelectron microscopes: a full-field x-ray photoelectron emission microscope and two scanning instruments, one dedicated to angle resolved photoemission spectroscopy (µ-ARPES) and one for ambient pressure x-ray photoelectron spectroscopy and scanning photoelectron microscopy (AP-XPS/SPEM). Microfocusing is achieved with state of the art elliptical cylinders, obtaining a spot size of 1 µm for ARPES and 0.5 µm for AP-XPS/SPEM. A detailed ray tracing analysis quantitatively evaluates the overall beamline performances.

Electronic structure of the topological insulator Bi2Se3 using angle-resolved photoemission spectroscopy: evidence for a nearly full surface spin polarization.

We performed high-resolution spin- and angle-resolved photoemission spectroscopy studies of the electronic structure and the spin texture on the surface of Bi2Se3, a model TI. By tuning the photon energy, we found that the topological surface state is well separated from the bulk states in the vicinity of kz = Z plane of the bulk Brillouin zone. The spin-resolved measurements in that region indicate a very high degree of spin polarization of the surface state, ~0.75, much higher than previously reported. Our results demonstrate that the topological surface state on Bi2Se3 is highly spin polarized and that the dominant factors limiting the polarization are mainly extrinsic.

Electronic structure of superconducting KC8 and nonsuperconducting LiC6 graphite intercalation compounds: evidence for a graphene-sheet-driven superconducting state.

We have performed photoemission studies of the electronic structure in LiC(6) and KC(8), a nonsuperconducting and a superconducting graphite intercalation compound, respectively. We have found that the charge transfer from the intercalant layers to graphene layers is larger in KC(8) than in LiC(6), opposite of what might be expected from their chemical composition. We have also measured the strength of the electron-phonon interaction on the graphene-derived Fermi surface to carbon derived phonons in both materials and found that it follows a universal trend where the coupling strength and superconductivity monotonically increase with the filling of graphene π(*) states. This correlation suggests that both graphene-derived electrons and graphene-derived phonons are crucial for superconductivity in graphite intercalation compounds.

Metal to insulator transition on the N=0 Landau level in graphene.

The magnetotransport in single layer graphene has been experimentally investigated in magnetic fields up to 18 T as a function of temperature. A pronounced T dependence is observed for T≲50 K, which is either metallic, or insulating, depending on the filling factor ν. The metal-insulator transition (MIT) occurs at |ν{c}|∼0.65 and in the regime of the dissipative transport, where the longitudinal resistance Rxx>1/2R{K}. The critical resistivity (Rxx per square) is ρ{xx}(ν{c})≈1/2R{K} and is correlated with the appearance of zero plateau in Hall conductivity σ{xy}(ν) and peaks in σ{xx}(ν). This leads us to construct a universal low-T (n, B) phase diagram of this quantum phase transition.

Anisotropic electron-phonon coupling and dynamical nesting on the graphene sheets in superconducting CaC6 using angle-resolved photoemission spectroscopy.

We present the first angle-resolved photoemission studies of electronic structure in CaC6, a superconducting graphite intercalation compound with T_{c}=11.6 K. We find that, contrary to theoretical models, the electron-phonon coupling on the graphene-derived Fermi sheets with high-frequency graphene-derived phonons is surprisingly strong and anisotropic. The shape of the Fermi surface is found to favor a dynamical intervalley nesting via exchange of high-frequency phonons. Our results suggest that graphene sheets play a crucial role in superconductivity in graphite intercalation compounds.