Laser-based Angle-resolved Photoemission Spectroscopy Research Articles

Evidence of Electron-Hole Imbalance in WTe2 from High-Resolution Angle-Resolved Photoemission Spectroscopy**Supported by the National Natural Science Foundation of China under Grant No 11574367, the National Basic Research Program of China under Grant Nos 2013CB921904 and 2015CB921300, the National Key Research and Development Program of China under Grant No 2016YFA0300600, the Strategic Priority Research Program (B) of the Chinese Academy of

WTe2 has attracted a great deal of attention because it exhibits extremely large and non-saturating magnetoresistance. The underlying origin of such a giant magnetoresistance is still under debate. Utilizing laser-based angle-resolved photoemission spectroscopy with high energy and momentum resolutions, we reveal the complete electronic structure of WTe2. This makes it possible to determine accurately the electron and hole concentrations and their temperature dependence. We find that, with increasing the temperature, the overall electron concentration increases while the total hole concentration decreases. It indicates that the electron-hole compensation, if it exists, can only occur in a narrow temperature range, and in most of the temperature range there is an electron-hole imbalance. Our results are not consistent with the perfect electron-hole compensation picture that is commonly considered to be the cause of the unusual magnetoresistance in WTe2. We identify a flat band near the Brillouin zone center that is close to the Fermi level and exhibits a pronounced temperature dependence. Such a flat band can play an important role in dictating the transport properties of WTe2. Our results provide new insight on understanding the origin of the unusual magnetoresistance in WTe2.

Development of laser-based scanning µ-ARPES system with ultimate energy and momentum resolutions

We have developed a laser-based scanning angle-resolved photoemission spectroscopy system (µ-ARPES) equipped with a high precision 6-axis control system, realizing not only high-resolution photoemission spectroscopy in energy and momentum, but also spatial resolution of a µm scale. This enables our µ-ARPES system to probe fine details of intrinsic electronic states near the Fermi level such as the superconducting gaps and lifetime broadening.

Three-dimensionality of the bulk electronic structure in WTe2

We use temperature- and field-dependent resistivity measurements [Shubnikov--de Haas (SdH) quantum oscillations] and ultrahigh resolution, tunable, vacuum ultraviolet (VUV) laser-based angle-resolved photoemission spectroscopy (ARPES) to study the three-dimensionality (3D) of the bulk electronic structure in WTe2, a type-II Weyl semimetal. The bulk Fermi surface (FS) consists of two pairs of electron pockets and two pairs of hole pockets along the X-Gamma-X direction as detected by using an incident photon energy of 6.7 eV, which is consistent with the previously reported data. However, if using an incident photon energy of 6.36 eV, another pair of tiny electron pockets is detected on both sides of the Gamma point, which is in agreement with the small quantum oscillation frequency peak observed in the magnetoresistance. Therefore, the bulk, 3D FS consists of three pairs of electron pockets and two pairs of hole pockets in total. With the ability of fine tuning the incident photon energy, we demonstrate the strong three-dimensionality of the bulk electronic structure in WTe2. The combination of resistivity and ARPES measurements reveal the complete, and consistent, picture of the bulk electronic structure of this material.

Unconventional Superconductivity in the BiS_{2}-Based Layered Superconductor NdO_{0.71}F_{0.29}BiS_{2}.

We investigate the superconducting-gap anisotropy in one of the recently discovered BiS_{2}-based superconductors, NdO_{0.71}F_{0.29}BiS_{2} (T_{c}∼5 K), using laser-based angle-resolved photoemission spectroscopy. Whereas the previously discovered high-T_{c} superconductors such as copper oxides and iron-based superconductors, which are believed to have unconventional superconducting mechanisms, have 3d electrons in their conduction bands, the conduction band of BiS_{2}-based superconductors mainly consists of Bi 6p electrons, and, hence, the conventional superconducting mechanism might be expected. Contrary to this expectation, we observe a strongly anisotropic superconducting gap. This result strongly suggests that the pairing mechanism for NdO_{0.71}F_{0.29}BiS_{2} is an unconventional one and we attribute the observed anisotropy to competitive or cooperative multiple paring interactions.

Shifts and Splittings of the Hole Bands in the Nematic Phase of FeSe

We report a high-resolution laser-based angle-resolved photoemission spectroscopy (laser-ARPES) study of single crystals of FeSe, focusing on the temperature-dependence of the hole-like bands around the ${\rm \Gamma}$ point. As the system cools through the tetragonal-orthorhombic "nematic" structural transition at 90~K, the splitting of the $d_{xz}$/$d_{yz}$ bands is observed to increase by a magnitude of 13 meV. Moreover, the onset of a $\sim$10 meV downward shift of the $d_{xy}$ band is also at 90~K. These measurements provide clarity on the nature, magnitude and temperature-dependence of the band shifts at the ${\rm \Gamma}$ point in the nematic phase of FeSe.

Concealed d-wave pairs in the s± condensate of iron-based superconductors

A central question in iron-based superconductivity is the mechanism by which the paired electrons minimize their strong mutual Coulomb repulsion. In most unconventional superconductors, Coulomb repulsion is minimized through the formation of higher angular momentum Cooper pairs, with Fermi surface nodes in the pair wavefunction. The apparent absence of such nodes in the iron-based superconductors has led to a belief they form an s-wave ([Formula: see text]) singlet state, which changes sign between the electron and hole pockets. However, the multiorbital nature of these systems opens an alternative possibility. Here, we propose a new class of [Formula: see text] state containing a condensate of d-wave Cooper pairs, concealed by their entanglement with the iron orbitals. By combining the d-wave ([Formula: see text]) motion of the pairs with the internal angular momenta [Formula: see text] of the iron orbitals to make a singlet ([Formula: see text]), an [Formula: see text] superconductor with a nontrivial topology is formed. This scenario allows us to understand the development of octet nodes in potassium-doped Ba1-x KXFe2As2 as a reconfiguration of the orbital and internal angular momentum into a high spin ([Formula: see text]) state; the reverse transition under pressure into a fully gapped state can then be interpreted as a return to the low-spin singlet. The formation of orbitally entangled pairs is predicted to give rise to a shift in the orbital content at the Fermi surface, which can be tested via laser-based angle-resolved photoemission spectroscopy.

Momentum dependence of the superconducting gap and in-gap states inMgB2multiband superconductor

We use tunable laser-based angle-resolved photoemission spectroscopy to study the electronic structure of the multiband superconductor ${\mathrm{MgB}}_{2}$. These results form the baseline for detailed studies of superconductivity in multiband systems. We find that the magnitude of the superconducting gap on both $\ensuremath{\sigma}$ bands follows a BCS-like variation with temperature with ${\mathrm{\ensuremath{\Delta}}}_{0}\ensuremath{\sim}7\phantom{\rule{0.28em}{0ex}}\mathrm{meV}$. The value of the gap is isotropic within experimental uncertainty and in agreement with a pure $s$-wave pairing symmetry. We also observe in-gap states confined to ${k}_{F}$ of the $\ensuremath{\sigma}$ band that occur at some locations of the sample surface. The energy of this excitation, $\ensuremath{\sim}3$ meV, is somewhat larger than the previously reported gap on $\ensuremath{\pi}$ Fermi sheet and therefore we cannot exclude the possibility of interband scattering as its origin.

Weak Electron-Phonon Coupling and Unusual Electron Scattering of Topological Surface States in Sb(111) by Laser-Based Angle-Resolved Photoemission Spectroscopy

High-resolution laser-based angle-resolved photoemission (ARPES) measurements are carried out on Sb(111) single crystal. Two kinds of Fermi surface sheets are observed, which are derived from the topological surface states: one small hexagonal electron-like Fermi pocket around Γ point and the other six elongated lobes of hole-like Fermi pockets around the electron pocket. Clear Rashba-type band splitting due to the strong spin-orbit coupling is observed to be anisotropic in the momentum space. Our super-high-resolution ARPES measurements reveal no obvious kink in the surface band dispersions, indicating a weak electron-phonon interaction in the surface states. In particular, the electron scattering rate for these topological surface states is nearly a constant over a large energy window near the Fermi level that is unusual in terms of the conventional picture.

Evidence for excluding the possibility ofd-wave superconducting-gap symmetry in Ba-doped KFe2As2

We have investigated the superconducting (SC)-gap anisotropy for several Ba-doped KFe${}_{2}$As${}_{2}$ samples using laser-based angle-resolved photoemission spectroscopy. We show that the SC-gap anisotropy and node positions drastically change with a small amount of Ba doping. Our results totally exclude a possibility of $d$-wave symmetry and strongly suggest that both spin and orbital fluctuations are important for the pairing interaction in the Ba-doped K122.

Impact of work function induced electric fields on laser-based angle-resolved photoemission spectroscopy

We examine the effects of the electric fields caused by the difference in work function between a sample and its surroundings in laser-based angle-resolved photoemission spectroscopy (laser ARPES) experiments. To simulate these effects we created several samples and surrounding puck geometries using SimIon 8.0 modeling software, and found that in most cases the system can be approximated by a circular sample mounted on an infinite conducting plane. Experimental measurements of the cuprate superconductor Bi2Sr2CaCu2O8+δ mounted on copper, aluminum, and graphite pucks confirmed the model's accuracy. Both the model and experimental data showed that work-function-induced fields have a significant effect on the outgoing trajectories of electrons for kinetic energies up to six times the work function difference between the sample and the puck. However, with the exception of effects very close to the sample edge, all electric field effects can be taken into account using linear corrections.

Doping Evolution of Nodal Band Renormalization in Bi2Sr2CuO6+δ Superconductor Revealed by Laser-Based Angle-Resolved Photoemission Spectroscopy

High resolution laser-based angle-resolved photoemission measurements are carried out on Bi2Sr2CuO6+δ superconductor covering a wide doping range from heavily underdoped to heavily overdoped samples. Two obvious energy scales are identified in the nodal dispersions: one is the well-known 50–80 meV high energy kink and the other is <10 meV low energy kink. The high energy kink increases monotonously in its energy scale with increasing doping and shows weak temperature dependence, while the low energy kink exhibits a non-monotonic doping dependence with its coupling strength enhanced sharply below Tc. These systematic investigations on the doping and temperature dependence of these two energy scales favor electron-phonon interactions as their origin. They point to the importance in involving the electron-phonon coupling in understanding the physical properties and the superconductivity mechanism of high temperature cuprate superconductors.

Anomalous Doping Variation of the Nodal Low-Energy Feature of Superconducting(Bi,Pb)2(Sr,La)2CuO6+δCrystals Revealed by Laser-Based Angle-Resolved Photoemission Spectroscopy

The nodal band dispersion in (Bi,Pb)(2)(Sr,La)(2)CuO(6+δ) (Bi2201) is investigated over a wide range of doping by using 7-eV laser-based angle-resolved photoemission spectroscopy. We find that the low-energy band renormalization ("kink"), recently discovered in Bi(2)Sr(2)CaCu(2)O(8+δ) (Bi2212), also occurs in Bi2201, but at a binding energy around half that in Bi2212. Surprisingly, the coupling energy dramatically increases with a decrease of carrier concentration, showing a sharp enhancement across the optimal doping. These properties (material and doping dependence of the coupling energy) demonstrate the significant correlation among the mode coupling, the energy gap close to the node, and the strong electron correlation. Our results suggest forward scattering arising from the interplay between the electrons and in-plane polarized acoustic phonon branch as the origin of the low-energy renormalization.

Anomalous Dressing of Dirac Fermions in the Topological Surface State ofBi2Se3,Bi2Te3, and Cu-DopedBi2Se3

Quasiparticle dynamics on the topological surface state of Bi(2(3), Bi(2)Te(3), and superconducting Cu(x)Bi(2)Se(3) are studied by 7 eV laser-based angle resolved photoemission spectroscopy. We find strong mode couplings in the Dirac-cone surface states at energies of ~3 and ~15-20 meV associated with an exceptionally large coupling constant λ of ~3, which is one of the strongest ever reported for any material. This result is compatible with the recent observation of a strong Kohn anomaly in the surface phonon dispersion of Bi(2)Se(3), but it appears that the theoretically proposed "spin-plasmon" excitations realized in helical metals are also playing an important role. Intriguingly, the ~3 meV mode coupling is found to be enhanced in the superconducting state of Cu(x)Bi(2)Se(3).

Direct observation of superconducting gaps in iron-based superconductors by laser ARPES

We have developed a new apparatus for carrying out ultra-high energy resolution laser-based angle-resolved photoemission spectroscopy (laser ARPES). From the spectra of the evaporated gold and superconducting (SC) gap of Sn (Tc=3.7K) sample, we conclude that the best energy resolution is ∼70μeV and the lowest sample temperature is ∼1.0K. We have used this laser-ARPES apparatus, to directly observe the SC gap of various iron-based superconductors. The spectra of FeTe0.6Se0.4 below Tc show a very clear temperature-dependent superconducting coherence peak, and the SC-gap nodes of KFe2As2 are found in the middle Fermi surface (FS) around the FS angle φ=±5.0°.

Octet-Line Node Structure of Superconducting Order Parameter in KFe 2 As 2

In iron-pnictide superconductivity, the interband interaction between the hole and electron Fermi surfaces (FSs) is believed to play an important role. However, KFe(2)As(2) has three zone-centered hole FSs and no electron FS but still exhibits superconductivity. Our ultrahigh-resolution laser angle-resolved photoemission spectroscopy unveils that KFe(2)As(2) is a nodal s-wave superconductor with highly unusual FS-selective multi-gap structure: a nodeless gap on the inner FS, an unconventional gap with "octet-line nodes" on the middle FS, and an almost-zero gap on the outer FS. This gap structure may arise from the frustration between competing pairing interactions on the hole FSs causing the eightfold sign reversal. Our results suggest that the A(1g) superconducting symmetry is universal in iron-pnictides, in spite of the variety of gap functions.

Quantitative determination of Eliashberg function and evidence of strong electron coupling with multiple phonon modes in heavily overdoped (Bi,Pb)2Sr2CuO6+δ

Super-high resolution laser-based angle-resolved photoemission spectroscopy measurements have been carried out on a heavily overdoped (Bi,Pb)2Sr2CuO6 (Tc> 5 K) superconductor. Taking advantage of the high-precision data on the subtle change of the quasi-particle dispersion at different temperatures, we develop a general procedure to determine the bare band dispersion and extract the bosonic spectral function quantitatively. Our results show unambiguously that the 70 meV nodal kink is due to the electron coupling with the multiple phonon modes, with a large mass enhancement factor Lamda= 0.42 even in the heavily over-doped regime.

Universal intrinsic doping behavior of in-plane dc conductivity for hole-doped high-temperature cuprate superconductors

Understanding the normal state transport properties in hole-doped high-temperature cuprate superconductors (HTCSs) is a challenging task which has been widely believed to be one of the key steps toward revealing the pairing mechanism of high-temperature superconductivity. Here, we present a true intrinsic and universal doping dependence of in-plane dc conductivity for all underdoped HTCSs. The doping dependence of in-plane dc conductivity normalized to that at optimal doping can be represented by a simple exponential formula. The doping behavior of the square of the nodal Fermi velocity derived by the high-resolution laser-based angle-resolved photoemission spectroscopy in the superconducting state follows reasonably well the universal intrinsic doping behavior. Our findings suggest a commonality of the low-energy quasiparticles both in the normal and superconducting states that place a true universal and stringent constraint on the mechanism of high-temperature superconductivity for HTCSs.

Doping-Dependent Nodal Fermi Velocity of the High-Temperature SuperconductorBi2Sr2CaCu2O8+δRevealed Using High-Resolution Angle-Resolved Photoemission Spectroscopy

The improved resolution of laser-based angle-resolved photoemission spectroscopy (ARPES) allows reliable access to fine structures in the spectrum. We present a systematic, doping-dependent study of a recently discovered low-energy kink in the nodal dispersion of Bi2Sr2CaCu2O(8+δ) (Bi-2212), which demonstrates the ubiquity and robustness of this kink in underdoped Bi-2212. The renormalization of the nodal velocity due to this kink becomes stronger with underdoping, revealing that the nodal Fermi velocity is nonuniversal, in contrast with assumed phenomenology. This is used together with laser ARPES measurements of the gap velocity (v2) to resolve discrepancies with thermal conductivity measurements.

High Energy Dispersion Relations for the High TemperatureBi2Sr2CaCu2O8Superconductor from Laser-Based Angle-Resolved Photoemission Spectroscopy

Laser-based angle-resolved photoemission spectroscopy measurements have been carried out on the high energy electron dynamics in Bi2Sr2CaCu2O8 high temperature superconductor. Our superhigh resolution data, momentum-dependent measurements, and complete analysis provide important information to judge the nature of the high energy dispersion and kink. Our results rule out the possibility that the high energy dispersion from the momentum distribution curve (MDC) may represent the true bare band as believed in previous studies. We also rule out the possibility that the high energy kink represents electron coupling with some high energy modes as proposed before. Through detailed MDC and energy distribution curve analyses, we propose that the high energy MDC dispersion may not represent intrinsic band structure.

Experimental setup for low-energy laser-based angle resolved photoemission spectroscopy

A laser-based angle resolved photoemission (ARPES) system utilizing 6 eV photons from the fourth harmonic of a mode-locked Ti:sapphire oscillator is described. This light source greatly increases the momentum resolution and photoelectron count rate, while reducing extrinsic background and surface sensitivity relative to higher energy light sources. In this review, the optical system is described, and special experimental considerations for low-energy ARPES are discussed. The calibration of the hemispherical electron analyzer for good low-energy angle-mode performance is also described. Finally, data from the heavily studied high T(c) superconductor Bi(2)Sr(2)CaCu(2)O(8+delta) (Bi2212) is compared to the results from higher photon energies.