Gigantic surface lifetime of an intrinsic topological insulator.

The interaction between light and novel two-dimensional electronic states holds promise to realize new fundamental physics and optical devices. Here, we use pump-probe photoemission spectroscopy to study the optically excited Dirac surface states in the bulk-insulating topological insulator Bi_{2}Te_{2}Se and reveal optical properties that are in sharp contrast to those of bulk-metallic topological insulators. We observe a gigantic optical lifetime exceeding 4 µs (1 µs=10^{-6} s) for the surface states in Bi_{2}Te_{2}Se, whereas the lifetime in most topological insulators, such as Bi_{2}Se_{3}, has been limited to a few picoseconds (1 ps=10^{-12} s). Moreover, we discover a surface photovoltage, a shift of the chemical potential of the Dirac surface states, as large as 100 mV. Our results demonstrate a rare platform to study charge excitation and relaxation in energy and momentum space in a two-dimensional system.

Imaging the three-dimensional Fermi-surface pairing near the hidden-order transition in URu2Si2 using angle-resolved photoemission spectroscopy.

We report angle-resolved photoemission spectroscopy experiments probing deep into the hidden-order state of URu(2)Si(2), utilizing tunable photon energies with sufficient energy and momentum resolution to detect the near Fermi-surface (FS) behavior. Our results reveal (i) the full itinerancy of the 5f electrons, (ii) the crucial three-dimensional k-space nature of the FS and its critical nesting vectors, in good comparison with density-functional theory calculations, and (iii) the existence of hot-spot lines and pairing of states at the FS, leading to FS gapping in the hidden-order phase.

Effect of spin-orbit coupling on the actinide dioxides AnO2 (An=Th, Pa, U, Np, Pu, and Am): a screened hybrid density functional study.

We present a systematic comparison of the lattice structures, electronic density of states, and band gaps of actinide dioxides, AnO(2) (An=Th, Pa, U, Np, Pu, and Am) predicted by the Heyd-Scuseria-Ernzerhof screened hybrid density functional (HSE) with the self-consistent inclusion of spin-orbit coupling (SOC). The computed HSE lattice constants and band gaps of AnO(2) are in consistently good agreement with the available experimental data across the series, and differ little from earlier HSE results without SOC. ThO(2) is a simple band insulator (f(0)), while PaO(2), UO(2), and NpO(2) are predicted to be Mott insulators. The remainders (PuO(2) and AmO(2)) show considerable O2p/An5f mixing and are classified as charge-transfer insulators. We also compare our results for UO(2), NpO(2), and PuO(2) with the PBE+U, self interaction correction (SIC), and dynamic mean-field theory (DMFT) many-body approximations.

Ultrafast hopping dynamics of 5f electrons in the Mott insulator UO2 studied by femtosecond pump-probe spectroscopy.

We describe a femtosecond pump-probe study of ultrafast hopping dynamics of 5f electrons in the Mott insulator UO2 following Mott-gap excitation at temperatures of 5-300 K. Hopping-induced response of the lattice and electrons is probed by transient reflectivity at mid- and above-gap photon energies, respectively. These measurements show an instantaneous hop, subsequent picosecond lattice deformation, followed by acoustic phonon emission and microsecond relaxation. Temperature-dependent studies indicate that the slow relaxation results from Hubbard excitons formed by U³âº-U5⁺ pairs.

Observation of Dirac state in half-Heusler material YPtBi.

The prediction of non-trivial topological electronic states in half-Heusler compounds makes these materials good candidates for discovering new physics and devices as half-Heusler phases harbour a variety of electronic ground states, including superconductivity, antiferromagnetism, and heavy-fermion behaviour. Here, we report a systematic studies of electronic properties of a superconducting half-Heusler compound YPtBi, in its normal state, investigated using angle-resolved photoemission spectroscopy. Our data reveal the presence of a Dirac state at the [Formula: see text] point of the Brillouin zone at 500 meV below the Fermi level. We observe the presence of multiple Fermi surface pockets, including two concentric hexagonal and six half-oval shaped pockets at the [Formula: see text] and K points of the Brillouin zone, respectively. Furthermore, our measurements show Rashba-split bands and multiple surface states crossing the Fermi level, this is also supported by the first-principles calculations. Our findings of a Dirac state in YPtBi contribute to the establishing of half-Heusler compounds as a potential platform for novel topological phases.

Dispersion in the Mott insulator UO2: A comparison of photoemission spectroscopy and screened hybrid density functional theory.

We present a comparison between the screened hybrid density functional theory of Heyd, Scuseria, and Enzerhof (HSE06) and high-resolution photoemission (PES) measurement on a single crystal of UO(2). Angle-resolved photoemission data show a slight dispersion in the f-orbital derived bands in good agreement with the HSE band structure. The effect of spin-orbit coupling on the HSE band gap has also been calculated and found to be negligible.

Discovery of topological nodal-line fermionic phase in a magnetic material GdSbTe.

Topological Dirac semimetals with accidental band touching between conduction and valence bands protected by time reversal and inversion symmetry are at the frontier of modern condensed matter research. A majority of discovered topological semimetals are nonmagnetic and conserve time reversal symmetry. Here we report the experimental discovery of an antiferromagnetic topological nodal-line semimetallic state in GdSbTe using angle-resolved photoemission spectroscopy. Our systematic study reveals the detailed electronic structure of the paramagnetic state of antiferromagnetic GdSbTe. We observe the presence of multiple Fermi surface pockets including a diamond-shape, and small circular pockets around the zone center and high symmetry X points of the Brillouin zone (BZ), respectively. Furthermore, we observe the presence of a Dirac-like state at the X point of the BZ and the effect of magnetism along the nodal-line direction. Interestingly, our experimental data show a robust  Dirac-like state both below and above the magnetic transition temperature (TN = 13 K). Having a relatively high transition temperature, GdSbTe provides an archetypical platform to study the interaction between magnetism and topological states of matter.

Distinct multiple fermionic states in a single topological metal.

Among the quantum materials that have recently gained interest are the topological insulators, wherein symmetry-protected surface states cross in reciprocal space, and the Dirac nodal-line semimetals, where bulk bands touch along a line in k-space. However, the existence of multiple fermion phases in a single material has not been verified yet. Using angle-resolved photoemission spectroscopy (ARPES) and first-principles electronic structure calculations, we systematically study the metallic material Hf2Te2P and discover properties, which are unique in a single topological quantum material. We experimentally observe weak topological insulator surface states and our calculations suggest additional strong topological insulator surface states. Our first-principles calculations reveal a one-dimensional Dirac crossing-the surface Dirac-node arc-along a high-symmetry direction which is confirmed by our ARPES measurements. This novel state originates from the surface bands of a weak topological insulator and is therefore distinct from the well-known Fermi arcs in semimetals.

Electronic structure and relaxation dynamics in a superconducting topological material.

Topological superconductors host new states of quantum matter which show a pairing gap in the bulk and gapless surface states providing a platform to realize Majorana fermions. Recently, alkaline-earth metal Sr intercalated Bi2Se3 has been reported to show superconductivity with a Tc ~ 3 K and a large shielding fraction. Here we report systematic normal state electronic structure studies of Sr0.06Bi2Se3 (Tc ~ 2.5 K) by performing photoemission spectroscopy. Using angle-resolved photoemission spectroscopy (ARPES), we observe a quantum well confined two-dimensional (2D) state coexisting with a topological surface state in Sr0.06Bi2Se3. Furthermore, our time-resolved ARPES reveals the relaxation dynamics showing different decay mechanism between the excited topological surface states and the two-dimensional states. Our experimental observation is understood by considering the intra-band scattering for topological surface states and an additional electron phonon scattering for the 2D states, which is responsible for the superconductivity. Our first-principles calculations agree with the more effective scattering and a shorter lifetime of the 2D states. Our results will be helpful in understanding low temperature superconducting states of these topological materials.

Observation of the spin-polarized surface state in a noncentrosymmetric superconductor BiPd.

Recently, noncentrosymmetric superconductor BiPd has attracted considerable research interest due to the possibility of hosting topological superconductivity. Here we report a systematic high-resolution angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES study of the normal state electronic and spin properties of BiPd. Our experimental results show the presence of a surface state at higher-binding energy with the location of Dirac point at around 700 meV below the Fermi level. The detailed photon energy, temperature-dependent and spin-resolved ARPES measurements complemented by our first-principles calculations demonstrate the existence of the spin-polarized surface states at high-binding energy. The absence of such spin-polarized surface states near the Fermi level negates the possibility of a topological superconducting behaviour on the surface. Our direct experimental observation of spin-polarized surface states in BiPd provides critical information that will guide the future search for topological superconductivity in noncentrosymmetric materials.

Quasiparticle dynamics across the full Brillouin zone of Bi2Sr2CaCu2O8+δ traced with ultrafast time and angle-resolved photoemission spectroscopy.

A hallmark in the cuprate family of high-temperature superconductors is the nodal-antinodal dichotomy. In this regard, angle-resolved photoemission spectroscopy (ARPES) has proven especially powerful, providing band structure information directly in energy-momentum space. Time-resolved ARPES (trARPES) holds great promise of adding ultrafast temporal information, in an attempt to identify different interaction channels in the time domain. Previous studies of the cuprates using trARPES were handicapped by the low probing energy, which significantly limits the accessible momentum space. Using 20.15 eV, 12 fs pulses, we show for the first time the evolution of quasiparticles in the antinodal region of Bi2Sr2CaCu2O8+δ and demonstrate that non-monotonic relaxation dynamics dominates above a certain fluence threshold. The dynamics is heavily influenced by transient modification of the electron-phonon interaction and phase space restrictions, in stark contrast to the monotonic relaxation in the nodal and off-nodal regions.

Possible Demonstration of a Polaronic Bose-Einstein(-Mott) Condensate in UO2(+x) by Ultrafast THz Spectroscopy and Microwave Dissipation.

Bose-Einstein condensates (BECs) composed of polarons would be an advance because they would combine coherently charge, spin, and a crystal lattice. Following our earlier report of unique structural and spectroscopic properties, we now identify potentially definitive evidence for polaronic BECs in photo- and chemically doped UO2(+x) on the basis of exceptional coherence in the ultrafast time dependent terahertz absorption and microwave spectroscopy results that show collective behavior including dissipation patterns whose precedents are condensate vortex and defect disorder and condensate excitations. That some of these signatures of coherence in an atom-based system extend to ambient temperature suggests a novel mechanism that could be a synchronized, dynamical, disproportionation excitation, possibly via the solid state analog of a Feshbach resonance that promotes the coherence. Such a mechanism would demonstrate that the use of ultra-low temperatures to establish the BEC energy distribution is a convenience rather than a necessity, with the actual requirement for the particles being in the same state that is not necessarily the ground state attainable by other means. A macroscopic quantum object created by chemical doping that can persist to ambient temperature and resides in a bulk solid would be revolutionary in a number of scientific and technological fields.

Integrated experimental setup for angle resolved photoemission spectroscopy of transuranic materials.

We have developed the Angle Resolved Photoemission Spectroscopy (ARPES) system for transuranic materials. The ARPES transuranic system is an endstation upgrade to the Laser Plasma Light Source (LPLS) at Los Alamos National Laboratory. The LPLS is a tunable light source for photoemission with a photon energy range covering the vacuum ultraviolet (VUV) and soft x-ray regions (27-140 eV). The LPLS was designed and developed for transuranic materials. Transuranic photoemission is currently not permitted at the public synchrotrons worldwide in the VUV energy range due to sample encapsulation requirements. With the addition of the ARPES capability to the LPLS system there is an excellent opportunity to explore new details centered on the electronic structure of actinide and transuranic materials.

Temperature dependence of hybridization gaps in metallic heavy-fermion systems.

There is evidence that a number of heavy-fermion/mixed-valence materials show hybridization gaps either at the Fermi energy or close to it. In the former case, a heavy-fermion semiconducting state ensues, and in the latter case, the system remains metallic at low temperatures. In either case, there are significant indications that the electronic structure is extremely temperature dependent. In particular, there is evidence from spectroscopic and transport properties that the gap closes at high temperatures and also that the heavy-quasiparticle bands disappear at high temperatures. The magnitudes of the gaps scale with the effective quasiparticle masses. We present a phenomenological model that exhibits a temperature dependence which is consistent with the above behavior. The model is based on a periodic array of Anderson impurities in which the electron correlations are represented by the coupling to bosons with Einstein spectra. The model can be approximately solved in a systematic manner. The solution consists of semi-analytic expressions which represent the temperature dependences of the coherent and incoherent structures in the electronic excitation spectra. We shall compare the hybridization gaps predicted by the theory for the metallic case and those inferred from photoemission experiments on UPd2Al3.

Temperature controller for thermal ionization mass spectrometry.

We describe the use of a simple voltage stabilizer that controls the filament temperature (T(f)) in the ion source of a thermal ionization mass spectrometer. The filament voltage (V(f)) is measured by means of a separate pair of wires connected inside of the ion source in parallel to the wires supplying power. It has been demonstrated that V(f) is directly proportional to T(f) in a wide range of filament temperature. The T(f) value is solely controlled by the reference voltage (V(r)) that can be manually selected from a voltage divider or by means of a computer. Digital signals from the computer in the form of a series of pulses are transmitted opto-electronically and subsequently converted to analog signals. The temperature controller described here was successfully applied for analysis of potassium concentration by the isotope dilution method.