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Time-resolved angle-resolved photoemission spectroscopy (Tr-APRES) gives direct insight into electron dynamics by providing temporal-, energy-, and momentum-resolved information in one experiment. A major obstacle to using high harmonic generation (HHG) probe pulses for photoemission spectroscopy is the low conversion efficiency, that is, the low flux of probe photons. We use a Yb-KGW based duo-laser source with an oscillator to pump two separate amplifiers and generate two synchronized pulsed laser sources with average energies of 7.5 and 6 W. By using the multiplate continuum method and chirped mirrors, the resulting flux of HHG photons at 33–70 eV can be increased 50-fold (up to 1011 photons/s) by using post-compressed 30 fs pulses compared with the photon flux generated by the fundamental 190 fs pulses. Moreover, pulses from the 6 W amplifier are used to pump an optical parametric amplifier that can vary the wavelengths for photoexcitation. The system performance is demonstrated by applying Tr-ARPES to single-crystal graphite. The front tilt broadening is significantly suppressed by the off-plane mounted conical grating, leading to a 184 fs temporal resolution that is mainly limited by the pump pulse. The energy resolution is 176 meV.

Ferroelectricity in two-dimensional (2D) van der Waals (vdW) layers has revolutionized our understanding of the vdW layered coupling, and has been introduced in the domains of moiré superlattice patterns generated by interlayer twisting or sliding. In the smallest limit of thickness, untwisted and epitaxial vdW stacking layers exhibiting ferroelectricity would clearly serve as building blocks for realizing 2D devices with nonvolatile and reconfigurable functionalities. In this study, we grew ferroelectric hexagonal boron nitride (h-BN) films on single-crystal graphene synthesized on a SiC (0001) substrate using nitrogen plasma-assisted molecular beam epitaxy (PA-MBE). Systematic angle-resolved photoemission spectroscopy (ARPES) studies and first-principles calculations revealed that the epitaxial mono-, bi-, and tri-layer h-BN films exhibit layer-number-dependent µ-band dispersions due to an AB stacking sequence on a Bernal-stacked graphene substrate. Furthermore, our piezoelectric force microscopy (PFM) confirmed the coexistence of robust moiré and sliding ferroelectricity at the well-aligned h-BN/graphene heterojunction and in multilayered h-BN films, respectively. In principle, as-developed epitaxially ferroelectric h-BN is limited only by the size of the crystalline graphene substrate, thereby providing a versatile and scalable 2D ferroelectric platform with promising exotic physics and vdW device applications down to a few atomic layers.

Effect of passive Q-switched solid-state laser for different absorption behaviours of absorbers.

Combination of low-dimensionality and electron correlation is vital for exotic quantum phenomena such as the Mott-insulating phase and high-temperature superconductivity. Transition-metal dichalcogenide (TMD) 1T-TaS2 has evoked great interest owing to its unique nonmagnetic Mott-insulator nature coupled with a charge-density-wave (CDW). To functionalize such a complex phase, it is essential to enhance the CDW-Mott transition temperature TCDW-Mott, whereas this was difficult for bulk TMDs with TCDW-Mott 2. Furthermore, the electron correlation derived lower Hubbard band survives under external perturbations such as carrier doping and photoexcitation, in contrast to the bulk counterpart. The enhanced Mott-Hubbard and CDW gaps for monolayer TaSe2 compared to NbSe2, originating in the lattice distortion assisted by strengthened correlations and disappearance of interlayer hopping, suggest stabilization of a likely nonmagnetic CDW-Mott insulator phase well above the room temperature. The present result lays the foundation for realizing monolayer CDW-Mott insulator based devices operating at room temperature.

Understanding characteristic energy scales is a fundamentally important issue in the study of strongly correlated systems. In multiband systems, an energy scale is affected not only by the effective Coulomb interaction but also by the Hund’s coupling. Direct observation of such energy scale has been elusive so far in spite of extensive studies. Here, we report the observation of a kink structure in the low energy dispersion of NiS2−xSex and its characteristic evolution with x, by using angle resolved photoemission spectroscopy. Dynamical mean field theory calculation combined with density functional theory confirms that this kink originates from Hund’s coupling. We find that the abrupt deviation from the Fermi liquid behavior in the electron self-energy results in the kink feature at low energy scale and that the kink is directly related to the coherence-incoherence crossover temperature scale. Our results mark the direct observation of the evolution of the characteristic temperature scale via kink features in the spectral function, which is the hallmark of Hund’s physics in the multiorbital system.

Two-dimensional (2D) topological insulators (TIs) have attracted a lot of attention owing to their striking optical nonlinearity. However, the ultra-low saturable intensity (SI) of TIs resulting from the bulk conduction band limits their applications, such as in mode-locking solid-state lasers. In this work, through fabricating a graphene/Bi2Te3 heterojunction which combines monolayer graphene and a Bi2Te3 nanoplate, the optical nonlinearities are analyzed. Moreover, the thickness-dependent characteristics are also investigated by varying the thickness of the Bi2Te3 when synthesizing the heterojunctions. Furthermore, with the aid of the estimated junction electron escape time, a model of the photo-excited carrier-transfer mechanism is proposed and used to describe the phenomena of depression of ultra-low saturable absorption (SA) from the Bi2Te3 bulk band. The increased modulation depth of the graphene/Bi2Te3 heterojunction can accordingly be realized in more detail. In addition, a Q-switched solid-state laser operating at 1064 nm with heterojunction saturable absorbers is built up and characterized for validating the proposed model. The laser performance with varied Bi2Te3 thickness, such as pulse duration and repetition rate, agrees quite well with our proposed model. Our work demonstrates the functionality of optical nonlinear engineering by tuning the thickness of the graphene/Bi2Te3 heterojunction and demonstrates its potential for applications.

Molybdenum disulfide (MoS2) is one of the two-dimensional layered semiconductor transition metal dichalcogenides (TMDCs) with great potential in electronics, optoelectronics, and spintronic devices. Sulfur vacancies in MoS2 are the most prevalent defects. However, the effect of sulfur vacancies on the electronic structure of MoS2 is still in dispute. Here we experimentally and theoretically investigated the effect of sulfur vacancies in MoS2. The vacancies were intentionally introduced by thermal annealing of MoS2 crystals in a vacuum environment. Angle-resolved photoemission spectroscopy (ARPES) was used directly to observe the electronic structure of the MoS2 single crystals. The experimental result distinctly revealed the appearance of an occupied defect state just above the valence band maximum (VBM) and an upward shift of the VBM after creating sulfur vacancies. In addition, density functional theory (DFT) calculations also confirmed the existence of the occupied defect state close to the VBM as well as two deep unoccupied states induced by the sulfur vacancies. Our results provide evidence to contradict that sulfur vacancies indicate the origin of n-type behaviour in MoS2. This work provides a rational strategy for tuning the electronic structures of MoS2.

Antimonene is a promising two-dimensional (2D) material that is calculated to have a significant fundamental bandgap usable for advanced applications such as field-effect transistors, photoelectric devices, and the quantum-spin Hall (QSH) state. Herein, we demonstrate a phenomenon termed topological proximity effect, which occurs between a 2D material and a three-dimensional (3D) topological insulator (TI). We provide strong evidence derived from hydrogen etching on Sb2Te3 that large-area and well-ordered antimonene presents a 2D topological state. Delicate analysis with a scanning tunneling microscope of the evolutionary intermediates reveals that hydrogen etching on Sb2Te3 resulted in the formation of a large area of antimonene with a buckled structure. A topological state formed in the antimonene/Sb2Te3 heterostructure was confirmed with angle-resolved photoemission spectra and density-functional theory calculations; in particular, the Dirac point was located almost at the Fermi level. The results reveal that Dirac fermions are indeed realized at the interface of a 2D normal insulator (NI) and a 3D TI as a result of strong hybridization between antimonene and Sb2Te3. Our work demonstrates that the position of the Dirac point and the shape of the Dirac surface state can be tuned by varying the energy position of the NI valence band, which modifies the direction of the spin texture of Sb-BL/Sb2Te3via varying the Fermi level. This topological phase in 2D-material engineering has generated a paradigm in that the topological proximity effect at the NI/TI interface has been realized, which demonstrates a way to create QSH systems in 2D-material TI heterostructures.

Growth of Xene, referred to as the analog of graphene made of atoms other than carbon, with higher lattice quality and more intrinsic electronic structures, is an important challenge to the development of two-dimensional (2D) materials. We report an approach using Pb-atom deposition to striped-phase (SP) germanene grown on Ag(111) to trigger it to a quasifreestanding phase (QP). Using low-energy electron diffraction (LEED) and scanning tunneling microscopy (STM), we demonstrate that the 2D monatomic Pb layer, instead of being on top, grows side-by-side with QP germanene, not only driving the SP-to-QP transition but further enhancing the lattice order of QP as revealed by the dramatic evolution of LEED-spot shape and uniform STM-imaged array of moir\'e patterns. Originally oriented at 30\ifmmode^\circ\else\textdegree\fi{} to Ag(111), the QP germanene transits first to a narrow distribution of rotations then to two sharp domains at \ifmmode\pm\else\textpm\fi{}3\ifmmode^\circ\else\textdegree\fi{} from 30\ifmmode^\circ\else\textdegree\fi{}, while the monoatomic Pb domains twist from \ifmmode\pm\else\textpm\fi{}4.3\ifmmode^\circ\else\textdegree\fi{} to \ifmmode\pm\else\textpm\fi{}9.5\ifmmode^\circ\else\textdegree\fi{} with respect to Ag(111). The analysis of higher-order coincidence for both layers on Ag(111) is in complete agreement with LEED results and reveals a picture of two insoluble monatomic layers driving each other to a more optimal configuration. Moreover, the corresponding density of states measured by scanning tunneling spectroscopy for quality-enhanced QP germanene exhibits a clear V-shape distribution at the energy \ensuremath{\sim}0.4 eV above Fermi level, indicating the Fermi-Dirac cone, which agrees with our density functional theory calculation.

Two-dimensional (2D) topological insulators (TIs) have attracted a lot of attention owing to their striking optical nonlinearity. However, the ultra-low saturable intensity (SI) of TIs resulting from the bulk conduction band limits their applications, such as in mode-locking solid-state lasers. In this work, through fabricating a graphene/Bi

Understanding characteristic energy scales is a fundamentally important issue in the study of strongly correlated systems. In multiband systems, an energy scale is affected not only by the effective Coulomb interaction but also by the Hund’s coupling. Direct observation of such energy scale has been elusive so far in spite of extensive studies. Here, we report the observation of a kink structure in the low energy dispersion of NiS2−xSex and its characteristic evolution with x, by using angle resolved photoemission spectroscopy. Dynamical mean field theory calculation combined with density functional theory confirms that this kink originates from Hund’s coupling. We find that the abrupt deviation from the Fermi liquid behavior in the electron self-energy results in the kink feature at low energy scale and that the kink is directly related to the coherence-incoherence crossover temperature scale. Our results mark the direct observation of the evolution of the characteristic temperature scale via kink features in the spectral function, which is the hallmark of Hund’s physics in the multiorbital system., A decisive spectroscopic evidence of the Hund’s coupling energy scale in multi-orbital correlated systems has been lacking. Here, the authors identify a kink feature due to Hund´s coupling in the spectral function of NiS2xSex as they track its evolution across the Mott-insulator transition.

The electronic transport and photoconduction properties of the molybdenum diselenide (MoSe2 ) nanosheets were investigated. The transfer length method analysis suggests the electric current following an anomalously two-dimensional (2D) flow rather than the general 3D mode. The 2D current implies a higher electron concentration and downward band bending at the surface. A broad spectral photoresponse from ultraviolet to near-infrared wavelengths was also observed for the MoSe 2 nanosheets. The optimal responsivity and photoconductive gain respectively at 58 A/W and 179 under the wavelengths at 405 nm were achieved. A surface-controlled photoconduction mechanism based on the surface band bending and electron accumulation is proposed to explain the long carrier lifetime and its dependence of light intensity and environment in MoSe 2 nanostructures .

Tuning the Fermi level (EF) in Bi2Te3 topological-insulator (TI) films is demonstrated on controlling the temperature of growth with molecular-beam epitaxy (MBE). Angle-resolved photoemission spectra (ARPES) reveal that EF of Bi2Te3 thin films shifts systematically with the growth temperature (Tg). The key role that a Bi-on-Te(1) (BiTe1) antisite defect plays in the electronic structure is identified through extended X-ray-absorption fine-structure (EXAFS) spectra at the Bi L3-edge. Calculations of electronic structure support the results of fitting the EXAFS, indicating that the variation of EF is due to the formation and suppression of BiTe1 that is tunable with the growth temperature. Our findings provide not only insight into the correlation between the defect structure and electronic properties but also a simple route to control the intrinsic topological surface states, which could be useful for applications in TI-based advanced electronic and spintronic devices.

Highly ordered Ag films grown on cleaved mica with a two-step procedure were characterized in detail with several techniques for surface analysis, including low-energy electron diffraction, X-ray photoemission spectra, a scanning tunneling microscope and angle-resolved photoemission spectra. Silver films of a thickness ≥ 100 nm were deposited on mica substrates at 300 K and stored under ambient conditions. The Ag/mica films became atomically flat and free of contamination when they were transferred into ultra-high vacuum and prepared with sputtering and annealing. The experimental results indicate that the surfaces of the cleaned Ag/mica films have structural and electronic properties resembling those of a Ag(111) single crystal with ordered domains aligned over a macroscopic region, but the surfaces of the Ag/mica films became rough on annealing above 623 K. On the rough surfaces, the surface steps tended to bunch together, yielding flat terraces bound with steps of large heights. With the decreased thermal stability in mind, the Ag/mica film is adoptable as a cheap platform alternative to a Ag(111) single crystal for the growth of highly ordered overlayers.

Ultrathin bilayers (BLs) of bismuth have been predicated to be a two-dimensional (2D) topological insulator. Here we report on a new route to manufacture the high-quality Bi bilayers from a 3D topological insulator, a top-down approach to prepare large-area and well-ordered Bi(111) BL with deliberate hydrogen etching on epitaxial Bi2Se3 films. With scanning tunneling microscopy (STM) and X-ray photoelectron spectra (XPS) in situ, we confirm that the removal of Se from the top of a quintuple layer (QL) is the key factor, leading to a uniform formation of Bi(111) BL in the van der Waals gap between the first and second QL of Bi2Se3. The angle resolved photoemission spectroscopy (ARPES) in situ and complementary density functional theory (DFT) calculations show a giant Rashba splitting with a coupling constant of 4.5 eV A in the Bi(111) BL on Bi2Se3. Moreover, the thickness of Bi BLs can be tuned by the amount of hydrogen exposure. Our ARPES and DFT study indicated that the Bi hole-like bands increase with i...

Ultrathin Pb and Ge films deposited on Ag(111) surfaces have been investigated and compared. We found that at 1/3 ML, both films formed surface alloys, ${\mathrm{Ag}}_{2}\mathrm{Pb}$ and ${\mathrm{Ag}}_{2}\mathrm{Ge}$, with $\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{3}R{30}^{\ensuremath{\circ}}$ and $\frac{19}{20}\sqrt{3}\ifmmode\times\else\texttimes\fi{}\frac{19}{20}\sqrt{3}R{30}^{\ensuremath{\circ}}$ structures on Ag(111) but the surface electronic structures exhibit a most evident difference at the Ag(111) surface zone boundary ${\overline{M}}_{\mathrm{Ag}(111)}$, where the single band and the splitting ones were observed, respectively. Up to 1 ML, ${\mathrm{Ag}}_{2}\mathrm{Ge}$ subsequently develops into germanene with a striped phase and then a quasifreestanding phase, as previously reported [Lin et al., Phys. Rev. Mater. 2, 024003 (2018)], while ${\mathrm{Ag}}_{2}\mathrm{Pb}$ evolves to a dense Pb(111) phase that also reveals splitting bands at ${\overline{M}}_{\mathrm{Ag}(111)}$. We discover that the larger (smaller) atomic size of a Pb (Ge) atom with respect to an Ag atom causes the commensurate (incommensurate) interfaces and further demonstrate that the splitting bands of ${\mathrm{Ag}}_{2}\mathrm{Ge}$ surface alloy and 1-ML Pb film originated from the commonly incommensurate interface with Ag(111), which mediates umklapp scattering by inducing the mirror image of the pristine ${\mathrm{Ag}}_{2}\mathrm{Ge}$ and Pb(111) bands relative to ${\overline{M}}_{\mathrm{Ag}(111)}.$

Combining angle-resolved photoemission spectroscopy and magneto-transport measurements, we systematically investigated the possible origin of the extreme magnetoresistance in Pr/Sm mono-antimonides/bismuthides (PrSb, SmSb, PrBi, SmBi). Our photoemission measurements reveal that the bulk band inversion and surface states are absent (present) in Pr/Sm antimonides (bismuthides), implying that topological surface states are unlikely to play an important role for the observed extreme magnetoresistance. We found that the electron-hole compensation is well satisfied in all these compounds and the bulk band structure exhibits no obvious temperature dependence from 10 K up to 150 K. Simultaneous fittings of the magnetoresistance and Hall coefficient reveal that the carrier mobility is dramatically enhanced at low temperature, which naturally explains the suppression of extreme magnetoresistance at high temperatures. Our results therefore show that the extreme magnetoresistance in these compounds can be well accounted for by the two-band model with good electron-hole compensation. Finally, we found that both PrSb and SmSb exhibit highly linear bulk bands near the X point and lie close to the transition point between a topologically trivial and nontrivial phase, which might be relevant for the observed anomalous quantum oscillations., 6 figures

The Twenty-First NSRRC Users' Meeting was held at the Activity Center of the National Synchrotron Radiation Research Center (NSRRC) in Taiwan from September 9 to 10, 2015. At the same time, celebration of the first light of the Taiwan Photon Source (TPS), achieved at the end of 2014, highlighted the prospective scientific frontiers marked by the TPS storage ring. Jointly organized by the UEC Chair Ying-Hao Chu (National Chiao Tung Univ.) and Cheng-Maw Cheng (NSRRC), the meeting consisted of two plenary sessions and three featured workshops. Nearly 30 distinguished scholars, both domestic and international, were invited to present their research achievements. This highly anticipated event attracted an enthusiastic crowd of more than 370 synchrotron experts, users, and potential users.

An exfoliated Kish graphite sample on a heavily n-doped Si substrate covered with native oxide was prepared with a conventional micromechanical cleavage method. From angle-resolved photoemission spectra (ARPES), we measured the band structure of graphite over photon energies from 28 eV to 116 eV. The inner potential V0 = 17.25 eV is determined with a period from the band dispersion in the KH direction. A set of parameters in the tight-binding method and the SWMcC model for graphite is extracted from the fitted results. A comparison of constant-energy mapping results at large binding energy indicates the reliability of the tight-binding parameters extracted from the ARPES results.

Photoelectron spectra (PES) have played an important role since the beginning of research in surface and material science. When these techniques are applied for the analysis of a more complicated system such as: highly correlated, surface-interface, transition-metal-oxide, samples are maneuvered between UHV chambers for sputtering, deposition or cleavage with a multiple-degree-of-freedom manipulator that consists of an x-y-z translational stage as well as rotation about these three axis. After these processes, a sample surface must be annealed to re-crystallize or cooled to its critical temperature before studying; control of temperature over a wide range is thus also an essential capability of a manipulator system. To integrate all above functions, a sample manipulator was constructed featuring control of temperature over a wide range -- 20 K to 1000 K, six degrees of freedom for sample positioning, sample transfer with exchangeable sample-mounting modules to fulfill varied experimental needs. Another special feature of our design is a retractable welded bellows to replace the formed bellows that connects to the differentially pumped rotary platform (DPRP) that provide the rotational motion of the sample in polar angular directions. This modification prevents the long formed bellows connected to its pumping system from dangling around the analysis vacuum chamber and interfering with other instruments.

The growth of Cu on Ag(1 1 1) under varied growth conditions was investigated with angle-resolved photoemission spectra. The evolution of Cu/Ag(1 1 1) during annealing was characterized on monitoring its surface states. The surface morphology of a Cu film on Ag(1 1 1) depends on the temperature and the Cu coverage. Islands or crystalline films develop when Cu is deposited at ∼300 K. Defects in the Cu films penetrate deeply into the Ag(1 1 1) substrate and expose the Ag(1 1 1) surface. The deposition of Cu at a low temperature results in disordered films. On annealing, the films become ordered with defects. Our results show the segregation of Ag on the Cu surface, which occurs at 300 K and becomes accelerated significantly at ∼380 K. After being annealed above 430 K, all islands and films of Cu are fully covered with Ag, showing a (9 × 9) reconstruction. Our results indicate also that the segregation of Ag on the Cu surface occurs only after the Ag(1 1 1) surface is exposed, indicating that Ag atoms migrate to the Cu(1 1 1) surface, not through bulk Cu, but along the walls of the islands and the defects in the films.

Compound semiconductors doped with magnetically active transition metals (TM) are actively pursued for semiconductor spintronics. Herein we report that delta doping (δ-doping) has been used to incorporate manganese (Mn) into the gallium nitride (GaN) matrix resulting in phase pure highly crystalline heteroepitaxial thin films of (Ga,Mn)N on c-plane sapphire (Al2O3) by plasma-assisted molecular beam epitaxy. Magnetotransport measurements reveal the anomalous Hall effect (AHE) while magnetic measurements show the existence of ferromagnetic ordering. Density functional theory calculations show that δ-doping of Mn atom enables exchange interactions between the Mn 3d states and N 2p states thereby resulting in spin polarized holes in the valence band giving rise to observed AHE and ferromagnetism. This work opens new avenues for incorporating spin polarized carriers in III-nitrides based semiconductors by creating magnetically active Mn layers in heterostructures for spintronics applications.

Here we report the evolution of bulk band structure and surface states in rare earth mono-bismuthides with partially filled f shell. Utilizing synchrotron-based photoemission spectroscopy, we determined the three-dimensional bulk band structure and identified the bulk band inversions near the X points, which, according to the topological theory, could give rise to nontrivial band topology with odd number of gapless topological surface states. Near the surface Gamma bar point, no clear evidence for predicted gapless topological surface state is observed due to its strong hybridization with the bulk bands. Near the M bar point, the two surface states, due to projections from two inequivalent bulk band inversions, interact and give rise to two peculiar sets of gapped surface states. The bulk band inversions and corresponding surface states can be tuned substantially by varying rare earth elements, in good agreement with density-functional theory calculations assuming local f electrons. Our study therefore establishes rare earth mono-bismuthides as an interesting class of materials possessing tunable electronic properties and magnetism, providing a promising platform to search for novel properties in potentially correlated topological materials., Comment: 7 figures

Two-dimensional (2D) honeycomb lattices beyond graphene promise new physical properties such as quantum spin Hall effect. While there have been claims of growth of such lattices (silicene, germanene, stanene), their existence needs further support and their preparation and characterization remain a difficult challenge. Our findings suggest that two distinct phases associated with germanene, the analog of graphene made of germanium (Ge) instead of carbon, can be grown on Ag(111) as observed by scanning tunneling microscopy, low-energy electron diffraction, and angle-resolved photoemission spectroscopy. One such germanene exhibits an atom-resolved alternatively buckled full honeycomb lattice, which is tensile strained and partially commensurate with the substrate to form a striped phase (SP). The other, a quasifreestanding phase (QP), is also consistent with a honeycomb lattice with a lattice constant incommensurate with the substrate but very close to the theoretical value for freestanding germanene. The SP, with a lower atomic density, can be driven into the QP and coexist with the QP by additional Ge deposition. Band mapping and first-principles calculations with proposed SP and QP models reveal an interface state exists only in the SP but the characteristic \ensuremath{\sigma} band of freestanding germanene emerges only in the QP---this leads to an important conclusion that adlayer-substrate commensurability plays a key role to affect the electronic structure of germanene. The evolution of the dual germanene phases manifests the competitive formation of Ge-Ge covalent and Ge-Ag interfacial bonds.

We report on helicity-dependent terahertz emissions that originate from the helicity-dependent photocurrents in topological insulator $\mathrm{S}{\mathrm{b}}_{2}\mathrm{T}{\mathrm{e}}_{3}$ thin films due to ultrafast optical excitation. The polarity of the emitted terahertz radiation is controlled by both the incident angle and the helicity of optical pulses. Using an unprecedented decomposition-recombination procedure in the time domain, the signals of the Dirac fermions are fully separated from bulk contributions. These results provide insights into the optical coupling of topological surface states and open up opportunities for applying helicity-dependent terahertz emission spectroscopy in spintronics.

The determination of the band structure along k parallel to the chain direction demonstrates significant electronic delocalization. The small effective mass [m* = 0.106mo ] is consistent with the high measured mobility.

To explore the possibility of employing thermally generated H atoms to determine the chemical composition of a metallic surface, we investigated the adsorption and desorption of H atoms generated with a thermal cracker on surfaces Au(111) and Ag/Au(111). Angle-resolved photoemission spectra showed that the noble-metallic surfaces deteriorated upon exposure to a flux of H atoms at ~ 100 K. Upon subsequent annealing, the order of the surfaces was mostly recovered when H atoms on the surfaces desorbed, but the recovery was incomplete even with annealing at a temperature much higher than that at which H atoms desorb. X-ray photoemission spectra showed that O-containing contaminants existed on the surfaces after the H dosing. The evolution of O 1s during annealing indicated that the O-containing contaminants were H 2 O and its moieties generated during thermal cracking; the disturbances of the surfaces remaining above the desorption temperature of H atoms were likely caused by chemisorbed O. Our results show that it is possible to employ thermally generated H atoms to determine the chemical composition of a metallic surface, but a small proportion of H 2 O in a H 2 gas line might be unavoidable; precautions against possible O contamination are required when a thermal cracker is employed.

Alkali-metal adsorption on the surface of materials is widely used for in situ surface electron doping, particularly for observing unoccupied band structures by angle-resolved photoemission spectroscopy (ARPES). However, the effects of alkali-metal atoms on the resulting band structures have yet to be fully investigated, owing to difficulties in both experiments and calculations. Here, we combine ARPES measurements on cesium-adsorbed ultrathin bismuth films with first-principles calculations of the electronic charge densities and demonstrate a simple method to evaluate alkali-metal induced band deformation. We reveal that deformation of bismuth surface bands is directly correlated with vertical charge-density profiles at each electronic state of bismuth. In contrast, a change in the quantized bulk bands is well described by a conventional rigid-band-shift picture. We discuss these two aspects of the band deformation holistically, considering spatial distributions of the electronic states and cesium-bismuth hybridization, and provide a prescription for applying alkali-metal adsorption to a wide range of materials., Comment: 8 pages, 7 figures

A topological insulator (TI) is a quantum material in a new class with attractive properties for physical and technological applications. Here we derive the electronic structure of highly crystalline Sb2Te2Se single crystals studied with angle-resolved photoemission spectra. The result of band mapping reveals that the Sb2Te2Se compound behaves as a p-type semiconductor and has an isolated Dirac cone of a topological surface state, which is highly favored for spintronic and thermoelectric devices because of the dissipation-less surface state and the decreased scattering from bulk bands. More importantly, the topological surface state and doping level in Sb2Te2Se are difficult to alter for a cleaved surface exposed to air; the robustness of the topological surface state defined in our data indicates that this Sb2Te2Se compound has a great potential for future atmospheric applications.

Reference EPFL-ARTICLE-195580doi:10.1002/adom.201300221View record in Web of Science Record created on 2014-01-09, modified on 2017-05-12

We report on terahertz radiation from topological insulator (TI) Sb 2 Te 3 thin film under ultrafast optical excitation with different helicity. Polarity-reversals of the emitted THz radiation were observed as the helicity of optical pulses reversed. The observed phenomena are coincident with the characteristics of the helicity-dependent photocurrent on TIs. Our work demonstrates the potential applications of surface photocurrents on TIs for opto-spintronics devices.