Angle-resolved Photoemission Measurements Research Articles

Optical manipulation of the topological phase in ZrTe5 revealed by time- and angle-resolved photoemission

High-resolution time- and angle-resolved photoemission measurements were conducted on the topological insulator ZrTe5. With strong femtosecond photoexcitation, a possible ultrafast phase transition from a weak to a strong topological insulating phase was experimentally realized by recovering the energy gap inversion in a time scale that was shorter than 0.15 ps. This photoinduced transient strong topological phase can last longer than 2 ps at the highest excitation fluence studied, and it cannot be attributed to the photoinduced heating of electrons or modification of the conduction band filling. Additionally, the measured unoccupied electronic states are consistent with the first-principles calculation based on experimental crystal lattice constants, which favor a strong topological insulating phase. These findings provide new insights into the longstanding controversy about the strong and weak topological properties in ZrTe5, and they suggest that many-body effects including electron–electron interactions must be taken into account to understand the equilibrium weak topological insulating phase in ZrTe5.

Enhanced vacuum ultraviolet photoemission from graphene nanoribbons

Photon-energy dependence of photoemission from seven-atoms-wide armchair graphene nanoribbons (GNRs) is studied experimentally and theoretically up to eV. A strong photon energy dependence of the normal emission from the valence band maximum (VB1) is observed, sharply peaked at eV. The detailed analysis of the light-polarization dependence of the photoemission from VB1 unambiguously characterizes the symmetry of the state. The experimental observations are analyzed based on ab initio one-step theory of photoemission. Off-normal emission is studied in detail and its relation to the standing-wave character of the valence band states is discussed. Excellent agreement with the earlier experiment (Senkovskiy et al 2018 2D Mater. 5 035007) is obtained. Rapid variations of the intensity with the ribbon-transverse photoelectron momentum are predicted from the ab initio theory, which are at variance with the prediction of the tight-binding rigid-wall model. These findings can help interpret angle-resolved photoemission measurements of similar systems. Moreover, the strong enhancement of the photoyield could trigger the GNR application as narrow-band photodetectors and contribute to the design of novel photocathodes for vacuum ultraviolet photodetection.

A unique van Hove singularity in kagome superconductor CsV3-xTaxSb5 with enhanced superconductivity

Van Hove singularity (VHS) has been considered as a driving source for unconventional superconductivity. A VHS in two-dimensional (2D) materials consists of a saddle point connecting electron-like and hole-like bands. In a rare case, when a VHS appears at Fermi level, both electron-like and hole-like conduction can coexist, giving rise to an enhanced density of states as well as an attractive component of Coulomb interaction for unconventional electronic pairing. However, this van Hove scenario is often destroyed by an incorrect chemical potential or competing instabilities. Here, by using angle-resolved photoemission measurements, we report the observation of a VHS perfectly aligned with the Fermi level in a kagome superconductor CsV3-xTaxSb5 (x ~ 0.4), in which a record-high superconducting transition temperature is achieved among all the current variants of AV3Sb5 (A = Cs, Rb, K) at ambient pressure. Doping dependent measurements reveal the important role of van Hove scenario in boosting superconductivity, and spectroscopic-imaging scanning tunneling microscopy measurements indicate a distinct superconducting state in this system.

Observation of spin-polarized surface states in the nodal-line semimetal SnTaS2

The superconductor ${\mathrm{SnTaS}}_{2}$ is theoretically predicted to be an intriguing topological nodal line semimetal without consideration of spin-orbit coupling. By carrying out angle-resolved photoemission (ARPES) and spin-resolved ARPES measurements combined with band structure calculations, we have provided a complete picture of the electronic structure and spin polarization property for the prominent surface states of ${\mathrm{SnTaS}}_{2}$. The low-energy electronic states are dominated by surface states; two of them are from the S-terminated surface, while four of them are from the Sn-terminated surface. These give rise to interesting Fermi surface topology of ${\mathrm{SnTaS}}_{2}$: three pockets located at $\overline{\mathrm{\ensuremath{\Gamma}}}, \overline{M}$ and $\overline{K}$ for the S-terminated surface and two pockets surrounding $\overline{\mathrm{\ensuremath{\Gamma}}}$ and $\overline{K}$ for the Sn-terminated surface. We further reveal that two surface states that cross the Fermi level are spin-polarized. Since ${\mathrm{SnTaS}}_{2}$ is also a superconductor, our observations indicate that it may provide a new platform to explore topological superconductivity and other exotic properties.

High p doped and robust band structure in Mg-doped hexagonal boron nitride.

In two dimensional materials, substitutional doping during growth can be used to alter the electronic properties. Here, we report on the stable growth of p-type hexagonal boron nitride (h-BN) using Mg-atoms as substitutional impurities in the h-BN honeycomb lattice. We use micro-Raman spectroscopy, angle-resolved photoemission measurements (nano-ARPES) and Kelvin probe force microscopy (KPFM) to study the electronic properties of Mg-doped h-BN grown by solidification from a ternary Mg-B-N system. Besides the observation of a new Raman line at ∼1347 cm-1 in Mg-doped h-BN, nano-ARPES reveals p-type carrier concentration. Our nano-ARPES experiments demonstrate that the Mg dopants can significantly alter the electronic properties of h-BN by shifting the valence band maximum about 150 meV toward higher binding energies with respect to pristine h-BN. We further show that, Mg doped h-BN exhibits a robust, almost unaltered, band structure compared to pristine h-BN, with no significant deformation. Kelvin probe force microscopy (KPFM) confirms the p-type doping, with a reduced Fermi level difference between pristine and Mg-doped h-BN crystals. Our findings demonstrate that conventional semiconductor doping by Mg as substitutional impurities is a promising route to high-quality p-type doped h-BN films. Such stable p-type doping of large band h-BN is a key feature for 2D materials applications in deep ultra-violet light emitting diodes or wide bandgap optoelectronic devices.

Surface doping of rubrene single crystals by molecular electron donors and acceptors.

The surface molecular doping of organic semiconductors can play an important role in the development of organic electronic or optoelectronic devices. Single-crystal rubrene remains a leading molecular candidate for applications in electronics due to its high hole mobility. In parallel, intensive research into the fabrication of flexible organic electronics requires the careful design of functional interfaces to enable optimal device characteristics. To this end, the present work seeks to understand the effect of surface molecular doping on the electronic band structure of rubrene single crystals. Our angle-resolved photoemission measurements reveal that the Fermi level moves in the band gap of rubrene depending on the direction of surface electron-transfer reactions with the molecular dopants, yet the valence band dispersion remains essentially unperturbed. This indicates that surface electron-transfer doping of a molecular single crystal can effectively modify the near-surface charge density, while retaining good charge-carrier mobility.

Structure and electronic properties of stable facets in the 2D material hexagonal boron nitride (hBN) on curved platinum

<h2>Abstract</h2> A hexagonal boron nitride (hBN) monolayer was grown on a curved crystal c-Pt(331) substrate including all vicinal surfaces between Pt(111) and Pt(110) faces. The surface structure has been studied by a combination of low-energy electron diffraction (LEED) and scanning tunnelling microscopy (STM). We observed that the hBN monolayer covers the entire curved crystal, but induces a faceting subsequent to the growth. We encountered (111), (221), (441), (991), and (110) as stable facets. We assign this faceting to two factors i) a better lattice coincidence and ii) the existence of local covalent bonds and non-local Van der Waals interactions. The electronic structure was characterized by near-edge x-ray absorption fine structure (NEXAFS), X-ray photoemission spectroscopy and angle-resolved photoemission spectroscopy (ARPES). The hBN/Pt(111) has the weakest interacting overlayer system, while the hBN on vicinal surfaces is more strongly bound to the Pt substrate. Additionally, we determined using angle-resolved photoemission measurements (ARPES) that the π band shifts downward when going away from the hBN/Pt(111) surface towards hBN/Pt(110). In the latter case, the π band shift is the largest.

Fine details of sixfold Dirac fermions in pyrite-structured PdSb2

We report detailed angle-resolved photoemission measurements on the electronic structure of an unconventional multifold Dirac fermionic semimetal ${\mathrm{PdSb}}_{2}$ with a pyrite structure. By exploiting the photon energy and polarization dependence of the matrix element in photoemission intensity and by comparing photoemission data with ab initio band calculations, we experimentally identify the exact electronic structure, including the orbital characters of the electron pockets at the $R$ point in the Brillouin zone of ${\mathrm{PdSb}}_{2}$. Each electron pocket and hole-pocket-like structure consists of three doubly degenerate parabolic bands, respectively, which cross one another at the $R$ point, forming a sixfold Dirac fermion. The overall electronic structure is consistent with the band calculations, but the gap size between two sextuple points is very sensitive to the Wyckoff position of Sb atoms, which is a result of the competition between the band energies and crystal symmetries.

Fermi surface of LaSb2 and direct observation of a CDW transition

We have studied the temperature-dependent electronic structure of the light rare-earth antimonide LaSb2 by combining angle-resolved photoemission (ARPES) measurements and density functional theory (DFT) calculations. ARPES measurements show the appearance of band replicas in the low-temperature Fermi surface with q = 0.25 ± 0.02 A−1 and a band folding of the same periodicity with a considerable spectral weight in the folded band. From our calculations we elucidate that the folded band exhibiting the new periodicity is associated with the La-Sb layer. We propose that an in-plane distortion, probably affecting the whole unit cell, is the structural modification related to the electronic changes. All these results converge to support that a charge density wave is stabilized in LaSb2 at low temperature.

Uniaxial ferromagnetism in the kagome metal TbV6Sn6

The synthesis and characterization of the vanadium-based kagome metal TbV${_6}$Sn${_6}$ is presented. X-ray measurements confirm this material forms with the same crystal structure type as the recently investigated kagome metals GdV$_6$Sn$_6$ and YV$_6$Sn$_6$, with space group symmetry P6/mmm. A signature of a phase transition at 4.1K is observed in heat capacity, resistivity, and magnetic susceptibility measurements, and both resistivity and magnetization measurements exhibit hysteresis in magnetic field. Furthermore, a strikingly large anisotropy in the magnetic susceptibility was observed, with the c-axis susceptibility nearly 100 times the ab plane susceptibility at 2K. This is highly suggestive of uniaxial ferromagnetism, and the large size of 9.4$\mu_b$/f.u. indicates the Tb$^{3+}$ $4f$ electronic moments cooperatively align perpendicular to the V kagome lattice plane. The entropy at the phase transition is nearly Rln(2), indicating that the CEF ground state of the Tb$^{3+}$ ion is a doublet, and therefore the sublattice of $4f$ electrons in this material can be shown to map at low temperatures to the Ising model in a D$_{6h}$ symmetry environment. Hall measurements at temperatures from 300K to 1.7K can be described by two-band carrier transport at temperatures below around 150K, with a large increase in both hole and electron mobilities, similar to YV$_6$Sn$_6$, and an anomalous Hall effect is seen below the ordering temperature. Angle-resolved photoemission measurements above the magnetic ordering temperature reveal typical kagome dispersions. Our study presents TbV${_6}$Sn${_6}$ as an ideal system to study the interplay between Ising ferromagnetism and non-trivial electronic states emerging from a kagome lattice.

Giant and reversible electronic structure evolution in a magnetic topological material EuCd2As2

The electronic structure and the physical properties of quantum materials can be significantly altered by charge carrier doping and magnetic state transition. Here we report a discovery of a giant and reversible electronic structure evolution with doping in a magnetic topological material. By performing high-resolution angle-resolved photoemission measurements on EuCd2As2,we found that a huge amount of hole doping can be introduced into the sample surface due to surface absorption. The electronic structure exhibits a dramatic change with the hole doping which can not be described by a rigid band shift. Prominent band splitting is observed at high doping which corresponds to a doping-induced magnetic transition at low temperature (below -15 K) from an antiferromagnetic state to a ferromagnetic state. These results have established a detailed electronic phase diagram of EuCd2As2 where the electronic structure and the magnetic structure change systematically and dramatically with the doping level. They further suggest that the transport, magnetic and topological properties of EuCd2As2 can be greatly modified by doping. These work will stimulate further investigations to explore for new phenomena and properties in doping this magnetic topological material.

Persistence of correlation-driven surface states in SmB6 under pressure

The proposed topological Kondo insulator SmB$_{6}$ hosts a bulk Kondo hybridization gap that stems from strong electronic correlations and a metallic surface state whose effective mass remains disputed. Thermopower and scanning tunneling spectroscopy measurements argue for heavy surface states that also stem from strong correlations, whereas quantum oscillation and angle-resolved photoemission measurements reveal light effective masses that would be consistent with a Kondo breakdown scenario at the surface. Here we investigate the evolution of the surface state via electrical and thermoelectric transport measurements under hydrostatic pressure, a clean symmetry-preserving tuning parameter that suppresses the Kondo gap and increases the valence of Sm from 2.6+ towards a 3+ magnetic metallic state. Electrical resistivity measurements reveal that the surface carrier density increases with increasing pressure, whereas thermopower measurements show an unchanged Fermi energy under pressure. As a result, the effective mass of the surface state charge carriers linearly increases with pressure as the Sm valence approaches 3+. Our results are consistent with the presence of correlation-driven surface states in SmB$_{6}$ and suggest that the surface Kondo effect persists under pressure to 2 GPa.

Anomalous Contribution to the Nematic Electronic States from the Structural Transition in FeSe Revealed by Time- and Angle-Resolved Photoemission Spectroscopy.

High-resolution time- and angle-resolved photoemission measurements were made on FeSe superconductors. With ultrafast photoexcitation, two critical excitation fluences that correspond to two ultrafast electronic phase transitions were found only in the d_{yz}-orbit-derived band near the Brillouin-zone center within our time and energy resolution. Upon comparison to the detailed temperature dependent measurements, we conclude that there are two equilibrium electronic phase transitions (at approximately 90 and 120K) above the superconducting transition temperature, and an anomalous contribution on the scale of 10meV to the nematic states from the structural transition is experimentally determined. Our observations strongly suggest that the electronic phase transition at 120K must be taken into account in the energy band development of FeSe, and, furthermore, the contribution of the structural transition plays an important role in the nematic phase of iron-based high-temperature superconductors.

Conservation of the particle–hole symmetry in the pseudogap state in optimally-doped Bi2Sr2CuO6+δ superconductor

The pseudogap state is one of the most enigmatic characteristics in the anomalous normal state properties of the high temperature cuprate superconductors. A central issue is to reveal whether there is a symmetry breaking and which symmetries are broken across the pseudogap transition. By performing high resolution laser-based angle-resolved photoemission measurements on the optimally-doped Bi2Sr1.6La0.4CuO6+δ superconductor, we report the observations of the particle–hole symmetry conservation in both the superconducting state and the pseudogap state along the entire Fermi surface. These results provide key insights in understanding the nature of the pseudogap and its relation with high temperature superconductivity.

A new class of bilayer kagome lattice compounds with Dirac nodal lines and pressure-induced superconductivity

Kagome lattice composed of transition-metal ions provides a great opportunity to explore the intertwining between geometry, electronic orders and band topology. The discovery of multiple competing orders that connect intimately with the underlying topological band structure in nonmagnetic kagome metals AV3Sb5 (A = K, Rb, Cs) further pushes this topic to the quantum frontier. Here we report a new class of vanadium-based compounds with kagome bilayers, namely AV6Sb6 (A = K, Rb, Cs) and V6Sb4, which, together with AV3Sb5, compose a series of kagome compounds with a generic chemical formula (Am-1Sb2m)(V3Sb)n (m = 1, 2; n = 1, 2). Theoretical calculations combined with angle-resolved photoemission measurements reveal that these compounds feature Dirac nodal lines in close vicinity to the Fermi level. Pressure-induced superconductivity in AV6Sb6 further suggests promising emergent phenomena in these materials. The establishment of a new family of layered kagome materials paves the way for designer of fascinating kagome systems with diverse topological nontrivialities and collective ground states.

Spectroscopic evidence for Dirac nodal surfaces and nodal rings in the superconductor NaAlSi

The discovery of the topological states has become a key topic in condensed matter physics with the focus evolving from the Dirac or Weyl points to high-dimension topological states of the nodal lines and nodal surfaces. For a topological material to manifest its quantum properties and become useful in applications, the topological states need to be genuine and clean so that they lie close to the Fermi level without other trivial bands existing at the Fermi level. While a number of high-dimension topological materials are predicted, only a few of them have been synthesized and confirmed and the genuine and clean ones are especially scarce. Here we report the realization of the genuine clean multiple high-dimension topological states in NaAlSi. By performing high-resolution angle-resolved photoemission measurements and band structure calculations, we have observed two sets of nodal surfaces and the formation of two homocentric nodal ring states in NaAlSi. The observed nodal rings are distinct in that the inner one is a type-{\uppercase\expandafter{\romannumeral1}} nodal ring while the outer one is a type-{\uppercase\expandafter{\romannumeral1}} nodal ring embedded with four type-{\uppercase\expandafter{\romannumeral3}} nodal points. All the bands involved in the nodal rings lie very close to the Fermi level with no other trivial bands coexisting at the Fermi level. These observations make NaAlSi a desirable topological material to explore for novel quantum states and exotic properties.

Unusual Band Splitting and Superconducting Gap Evolution with Sulfur Substitution in FeSe

High-resolution angle-resolved photoemission measurements were taken on FeSe1–x S x (x = 0, 0.04, and 0.08) superconductors. With an ultrahigh energy resolution of 0.4 meV, unusual two hole bands near the Brillouin-zone center, which was possibly a result of additional symmetry breaking, were identified in all the sulfur-substituted samples. In addition, in both of the hole bands highly anisotropic superconducting gaps with resolution limited nodes were evidenced. We find that the larger superconducting gap on the outer hole band is reduced linearly to the nematic transition temperature while the gap on the inner hole is nearly S-substitution independent. Our observations strongly suggest that the superconducting gap increases with enhanced nematicity although the superconducting transition temperature is not only governed by the pairing strength, demonstrating strong constraints on theories in the FeSe family.

Bulk and surface electronic structure of Bi4Te3 from GW calculations and photoemission experiments

We present a combined theoretical and experimental study of the electronic structure of stoichiometric Bi$_4$Te$_3$, a natural superlattice of alternating Bi$_2$Te$_3$ quintuple layers and Bi bilayers. In contrast to the related semiconducting compounds Bi$_2$Te$_3$ and Bi$_1$Te$_1$, density functional theory predicts Bi$_4$Te$_3$ to be a semimetal. In this work, we compute the quasiparticle electronic structure of Bi$_4$Te$_3$ in the framework of the $GW$ approximation within many-body perturbation theory. The quasiparticle corrections are found to modify the dispersion of the valence and conduction bands in the vicinity of the Fermi energy, leading to the opening of a small indirect band gap. Based on the analysis of the eigenstates, Bi$_4$Te$_3$ is classified as a dual topological insulator with bulk topological invariants $\mathbb{Z}_2$ (1;111) and magnetic mirror Chern number $n_M=1$. The bulk $GW$ results are used to build a Wannier-functions based tight-binding Hamiltonian that is further applied to study the electronic properties of the (111) surface. The comparison with our angle-resolved photoemission measurements shows excellent agreement between the computed and measured surface states and indicates the dual topological nature of Bi$_4$Te$_3$.

Electronic structure of 2D van der Waals crystals and heterostructures investigated by spatially- and angle-resolved photoemission

Angle-resolved photoemission is a direct probe of the momentum-resolved electronic structure and proved influential in the study of bulk crystals with novel electronic properties. Thanks to recent technical advances, this technique can now be applied for the first time for the study of van der Waals heterostructures built by stacking two-dimensional crystals. In this article we will present the current state of the art in angle-resolved photoemission measurements on two-dimensional materials and review this still young field. We will focus in particular on devices similar to those used in transport and optics experiments, including the latest developments on magic-angle twisted bilayer graphene and on the in-operando characterization of gate tunable devices.

A narrow bandwidth extreme ultra-violet light source for time- and angle-resolved photoemission spectroscopy.

Here, we present a high repetition rate, narrow bandwidth, extreme ultraviolet photon source for time- and angle-resolved photoemission spectroscopy. The narrow bandwidth pulses meV for photon energies eV are generated through high harmonic generation using ultra-violet drive pulses with relatively long pulse lengths (461 fs). The high harmonic generation setup employs an annular drive beam in tight focusing geometry at a repetition rate of 250 kHz. Photon energy selection is provided by a series of selectable multilayer bandpass mirrors and thin film filters, thus avoiding any time broadening introduced by single grating monochromators. A two stage optical-parametric amplifier provides < 100 fs tunable pump pulses from 0.65 μm to 9 μm. The narrow bandwidth performance of the light source is demonstrated through angle-resolved photoemission measurements on a series of quantum materials, including high-temperature superconductor Bi-2212, WSe2, and graphene.