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We describe a compact and stable setup for detecting the optical second harmonics, in which the incident plane rotates with respect to the sample. The setup is composed of rotating Fresnel-rhomb optics and a femtosecond ytterbium-doped fiber-laser source operating at the repetition frequency of 10 MHz. The setup including the laser source occupies an area of 1 m2 and is stable so that the intensity fluctuation of the laser harmonics can be less than 0.2 % for 4 h. We present the isotropic harmonic signal of a gold mirror of 0.5 pW and demonstrate the integrity and sensitivity of the setup. We also show the polarization-dependent six-fold pattern of the harmonics of a few-layer WSe2, from which we infer the degree of local-field effects. Finally, we describe the extendibility of the setup to investigate the samples in various conditions such as cryogenic, strained, ultrafast non-equilibrium, and high magnetic fields.

The protected surface conduction of topological insulators is in high demand for the next generation of electronic devices. What is needed to move forward are robust settings where topological surface currents can be controlled by simple means, ideally by the application of external stimuli. Surprisingly, this direction is only little explored. In this work we demonstrate that we can boost the surface conduction of a topological insulator by both light and electric field. This happens in a fully controlled way, and the additional Dirac carriers exhibit ultra-long lifetimes. We provide a comprehensive understanding, namely that carriers are injected from the bulk to the surface states across an intrinsic Schottky barrier. We expect this mechanism to be at play in a broad range of materials and experimental settings.

Electron emission can be utilised to measure the work function of the surface. However, the number of significant digits in the values obtained through thermionic-, field- and photo-emission techniques is typically just two or three. Here, we show that the number can go up to five when angle-resolved photoemission spectroscopy (ARPES) is applied. This owes to the capability of ARPES to detect the slowest photoelectrons that are directed only along the surface normal. By using a laser-based source, we optimised our setup for the slow photoelectrons and resolved the slowest-end cutoff of Au(111) with the sharpness not deteriorated by the bandwidth of light nor by Fermi-Dirac distribution. The work function was leveled within $\pm$0.4 meV at least from 30 to 90 K and the surface aging was discerned as a meV shift of the work function. Our study opens the investigations into the fifth significant digit of the work function., Comment: For an associated blog-type posting, see https://devicematerialscommunity.nature.com/posts/measuring-the-work-function-precisely-by-using-laser-arpes

We investigate how the direction of polarized light can affect the dichroism pattern seen in angle-resolved photoemission spectroscopy. To this end, we prepared a sample composed of highly-oriented Bi(111) micro-crystals that macroscopically has infinite rotational and mirror symmetry of the point group $\rm{C}_{\infty\rm{v}}$ and examined whether the dichroism pattern retains the $\rm{C}_{\infty\rm{v}}$ symmetry under the stationary configuration of the light and sample. The direction of the light was imprinted in the pattern. Thereby, we apply group theory and classify the pattern with the configuration of light taken into account. We complete the classification by discussing the cases when the out-of-plane component of the polarization can be neglected, when the incidence angle is either 0$^{\circ}$ or 90$^{\circ}$, when the polarization is either elliptic or linear, and also when the sample is a crystal.

The electronic nematic phase is an unconventional state of matter that spontaneously breaks the rotational symmetry of electrons. In iron-pnictides/chalcogenides and cuprates, the nematic ordering and fluctuations have been suggested to have as-yet-unconfirmed roles in superconductivity. However, most studies have been conducted in thermal equilibrium, where the dynamical property and excitation can be masked by the coupling with the lattice. Here we use femtosecond optical pulse to perturb the electronic nematic order in FeSe. Through time-, energy-, momentum- and orbital-resolved photo-emission spectroscopy, we detect the ultrafast dynamics of electronic nematicity. In the strong-excitation regime, through the observation of Fermi surface anisotropy, we find a quick disappearance of the nematicity followed by a heavily-damped oscillation. This short-life nematicity oscillation is seemingly related to the imbalance of Fe 3dxz and dyz orbitals. These phenomena show critical behavior as a function of pump fluence. Our real-time observations reveal the nature of the electronic nematic excitation instantly decoupled from the underlying lattice.

The distribution of photoelectrons acquired in angle-resolved photoemission spectroscopy can be mapped onto energy-momentum space of the Bloch electrons in the crystal. The explicit forms of the mapping function $f$ depend on the configuration of the apparatus as well as on the type of the photoelectron analyzer. We show that the existence of the analytic forms of $f^{\text{-}1}$ is guaranteed in a variety of setups. The variety includes the case when the analyzer is equipped with a photoelectron deflector. Thereby, we provide a demonstrative mapping program implemented by an algorithm that utilizes both $f$ and $f^{\text{-}1}$. The mapping methodology is also usable in other spectroscopic methods such as momentum-resolved electron-energy loss spectroscopy., Comment: Mapping program is open accessed from publisher's site

The paper describes a time- and angle-resolved photoemission apparatus consisting of a hemispherical analyzer and a pulsed laser source. We demonstrate 1.48-eV pump and 5.90-eV probe measurements at the >10.5-meV and >240-fs resolutions by use of fairly monochromatic 170-fs pulses delivered from a regeneratively amplified Ti:sapphire laser system operating typically at 250 kHz. The apparatus is capable to resolve the optically filled superconducting peak in the unoccupied states of a cuprate superconductor, Bi2Sr2CaCu2O8+d. A dataset recorded on Bi(111) surface is also presented. Technical descriptions include the followings: A simple procedure to fine-tune the spatio-temporal overlap of the pump-and-probe beams and their diameters; achieving a long-term stability of the system that enables a normalization-free dataset acquisition; changing the repetition rate by utilizing acoustic optical modulator and frequency-division circuit.

The paper describes a time-resolved photoemission (TRPES) apparatus equipped with a Yb-doped fiber laser system delivering 1.2-eV pump and 5.9-eV probe pulses at the repetition rate of 95 MHz. Time and energy resolutions are 11.3 meV and ~310 fs, respectively; the latter is estimated by performing TRPES on a highly oriented pyrolytic graphite (HOPG). The high repetition rate is suited for achieving high signal-to-noise ratio in TRPES spectra, thereby facilitating investigations of ultrafast electronic dynamics in the low pump fluence (p) region. TRPES of polycrystalline bismuth (Bi) at p as low as 30 nJ/mm2 is demonstrated. The laser source is compact and is docked to an existing TRPES apparatus based on a 250-kHz Ti:sapphire laser system. The 95-MHz system is less prone to space-charge broadening effects compared to the 250-kHz system, which we explicitly show in a systematic probe-power dependency of the Fermi cutoff of polycrystalline gold. We also describe that the TRPES response of an oriented Bi(111)/HOPG sample is useful for fine-tuning the spatial overlap of the pump and probe beams even when p is as low as 30 nJ/mm2.

We discover a pair of spin-polarized surface bands on the (111) face of grey arsenic by using angle-resolved photoemission spectroscopy (ARPES). In the occupied side, the pair resembles typical nearly-free-electron Shockley states observed on noble-metal surfaces. However, pump-probe ARPES reveals that the spin-polarized pair traverses the bulk band gap and that the crossing of the pair at $\bar\Gamma$ is topologically unavoidable. First-principles calculations well reproduce the bands and their non-trivial topology; the calculations also support that the surface states are of Shockley type because they arise from a band inversion caused by crystal field. The results provide compelling evidence that topological Shockley states are realized on As(111)., Comment: 5 pages, 4 figures

Interference of spin-up and spin-down eigenstates depicts spin rotation of electrons, which is a fundamental concept of quantum mechanics and accepts technological challenges for the electrical spin manipulation. Here, we visualize this coherent spin physics through laser spin- and angle-resolved photoemission spectroscopy on a spin-orbital entangled surface-state of a topological insulator. It is unambiguously revealed that the linearly polarized laser can simultaneously excite spin-up and spin-down states and these quantum spin-basis are coherently superposed in photoelectron states. The superposition and the resulting spin rotation is arbitrary manipulated by the direction of the laser field. Moreover, the full observation of the spin rotation displays the phase of the quantum states. This presents a new facet of laser-photoemission technique for investigation of quantum spin physics opening new possibilities in the field of quantum spintronic applications.

There is still no general consensus on how one can describe the out-of-equilibrium phenomena in matter induced by an ultrashort light pulse. We investigate the pulse-induced dynamics in a layered Dirac semimetal SrMnBi2 by pump-and-probe photoemission spectroscopy. At ~<1 ps, the electronic recovery slowed upon increasing the pump power. Such a bottleneck-type slowing is expected in a two-temperature model (TTM) scheme, although opposite trends have been observed to date in graphite and in cuprates. Subsequently, an unconventional power-law cooling took place at ~100 ps, indicating that spatial heat diffusion is still ill defined at ~100 ps. We identify that the successive dynamics before the emergence of heat diffusion is a canonical realization of a TTM scheme. Criteria for the applicability of the scheme is also provided.

In a conventional framework, superconductivity is lost at a critical temperature (T_c) because, at higher temperatures, gluing bosons can no longer bind two electrons into a Cooper pair. In high-T_c cuprates, it is still unknown how superconductivity vanishes at T_c. We provide evidence that the so-called <~70-meV kink bosons that dress the quasi-particle excitations are playing a key role in the loss of superconductivity in a cuprate. We irradiated a 170-fs laser pulse on Bi2Sr2CaCu2O8+\delta and monitored the responses of the superconducting gap and dressed quasi-particles by time- and angle-resolved photoemission spectroscopy. We observe an ultrafast loss of superconducting gap near the d-wave node, or light-induced Fermi arcs, which is accompanied by spectral broadenings and weight redistributions occurring within the kink binding energy. We discuss that the underlying mechanism of the spectral broadening that induce the Fermi arc is the undressing of quasi-particles from the kink bosons. The loss mechanism is beyond the conventional framework, and can accept the unconventional phenomena such as the signatures of Cooper pairs remaining at temperatures above T_c.

Strong spin-orbit coupling fosters exotic electronic states such as topological insulators and superconductors, but the combination of strong spin-orbit and strong electron-electron interactions is just beginning to be understood. Central to this emerging area are the 5d transition metal iridium oxides. Here, in the pyrochlore iridate Pr2Ir2O7, we identify a nontrivial state with a single point Fermi node protected by cubic and time-reversal symmetries, using a combination of angle-resolved photoemission spectroscopy and first principles calculations. Owing to its quadratic dispersion, the unique coincidence of four degenerate states at the Fermi energy, and strong Coulomb interactions, non-Fermi liquid behavior is predicted, for which we observe some evidence. Our discovery implies that Pr2Ir2O7 is a parent state that can be manipulated to produce other strongly correlated topological phases, such as topological Mott insulator, Weyl semi-metal, and quantum spin and anomalous Hall states.

Recent studies suggest that an exemplary Kondo insulator SmB6 belongs to a new class of topological insulators (TIs), in which non-trivial spin-polarized metallic states emerge on surface upon the formation of Kondo hybridization gap in the bulk. Remarkably, the bulk resistivity reaches more than 20 Ohm cm at 4 K, making SmB6 a candidate for a so-called bulk-insulating TI. We here investigate optical-pulse responses of SmB6 by pump-and-probe photoemission spectroscopy. Surface photovoltage effect is observed below ~90 K. This indicates that an optically-active band bending region develops beneath the novel metallic surface upon the bulk-gap evolution. The photovoltaic effect persists for >200 microsec, which is long enough to be detected by electronics devices, and could be utilized for optical gating of the novel metallic surface.

In contrast to a complex feature of antinodal state, suffering from competing order(s), the "pure" pairing gap of cuprates is obtained in the nodal region, which therefore holds the key to the superconducting mechanism. One of the biggest question is whether the point nodal state as a hallmark of d-wave pairing collapses at Tc like the BCS-type superconductors, or it instead survives above Tc turning into the preformed pair state. A difficulty in this issue comes from the small magnitude of the nodal gap, which has been preventing experimentalists from solving it. Here we use a laser ARPES capable of ultrahigh energy resolution, and detect the point nodes surviving far beyond Tc in Bi2212. By tracking the temperature evolution of spectra, we reveal that the superconductivity occurs when the pair breaking rate is suppressed smaller than the single particle scattering rate on cooling, which governs the value of Tc in cuprates.

We have studied the electronic structure of bulk single crystals and epitaxial films of magnetite Fe$_3$O$_4$. Fe $2p$ core-level spectra show clear differences between hard x-ray (HAX-) and soft x-ray (SX-) photoemission spectroscopy (PES), indicative of surface effects. The bulk-sensitive spectra exhibit temperature ($T$)-dependent charge excitations across the Verwey transition at $T_V$=122 K, which is missing in the surface-sensitive spectra. An extended impurity Anderson model full-multiplet analysis reveals roles of the three distinct Fe-species (A-Fe$^{3+}$, B-Fe$^{2+}$, B-Fe$^{3+}$) below $T_V$ for the Fe $2p$ spectra, and its $T-$dependent evolution. The Fe $2p$ HAXPES spectra show a clear magnetic circular dichroism (MCD) in the metallic phase of magnetized 100-nm-thick films. The model calculations also reproduce the MCD and identify the magnetically distinct sites associated with the charge excitations. Valence band HAXPES shows finite density of states at $E_F$ for the polaronic metal with remnant order above $T_V$, and a clear gap formation below $T_V$. The results indicate that the Verwey transition is driven by changes in the strongly correlated and magnetically active B-Fe$^{2+}$ and B-Fe$^{3+}$ electronic states, consistent with resistivity and bulk-sensitive optical spectra., Comment: 5 pages, 4 figures Accepted in Physical Review Letters

A detailed low-energy electronic structure of a Kondo insulator YbB$_{12}$ was revealed by a synergetic combination of ultrahigh-resolution laser photoemission spectroscopy (PES) and time-resolved PES. The former confirmed a 25-meV pseudogap corresponding to the Kondo temperature of this material, and more importantly, it revealed that a 15-meV gap and a Kondo-peak feature developed below a crossover temperature $T^\ast \sim 110$ K. In harmony with this, the latter discovered a very long recombination time exceeding 100 ps below $\sim$$T^\ast$. This is a clear manifestation of photoexcited carriers due to the bottleneck in the recovery dynamics, which is interpreted as a developing hybridization gap of a hard gap., Comment: 6 pages, 4 figures, revised version accepted for publication in PRB Rapid Communications

In contrast to a complex feature of antinodal state, suffering from competing order(s), the "pure" pairing gap of cuprates is detected in the nodal region, which therefore holds the key to the superconducting mechanism. The pairing gap has been viewed to be rather conventional, closing at the superconducting transition temperature (Tc). However, the density of states contributed from the nodal region was claimed to have a gap-like structure even above Tc. Here we present a missing evidence for a single-particle gap near the node signifying the realization of a phase incoherent d-wave superconductivity above Tc in the optimally doped Bi2Sr2CaCu2O8+d. We find that the pair formation is formulated by momentum-independent temperature evolutions of three parameters: a BCS-type energy gap (Delta), a single particle scattering rate (Gamma_single) and a pair breaking rate (Gamma_pair). The superconductivity occurs when the Gamma_pair value is suppressed smaller than Gamma_single on cooling, and the magnitude of Tc in cuprates is governed by a condition of Gamma_single(Tc)=Gamma_pair(Tc).

We performed a Laser angle-resolved photoemission spectroscopy (ARPES) study on a wide doping range of Ba1-xKxFe2As2 (BaK) iron-based superconductor. We observed a robust low-binding energy (BE) kink structure in the dispersion which is doping dependent where its energy peaks at the optimally-doped (OP) level (x~0.4) and decreases towards the underdoped (UD) and overdoped (OD) sides. It is also temperature-dependent and survives up to ~90K. We attribute this kink to electron-mode coupling in good agreement with the inelastic neutron scattering (INS) and scanning tunneling microscopy (STM) results on the same compound which observed a similar bosonic mode associated with spin excitations. The relation between the mode energy ({\Omega}) and the SC transition temperature (Tc) deduced from our Laser ARPES data follow the universal relation deduced from INS and STM. In addition, we could resolve another kink at higher BE showing less doping and temperature dependence and may thus be of different origin., Comment: 5 pages, 3 figures

Quasiparticle dynamics on the topological surface state of Bi2Se3, Bi2Te3, and superconducting CuxBi2Se3 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, which leads to an exceptionally large coupling constant 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 Bi2Se3, 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 CuxBi2Se3., Comment: 5 pages, 4 figures

The nodal band-dispersion in (Bi,Pb)2(Sr,La)2CuO6+d (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 Bi2Sr2CaCu2O8+d (Bi2212), also occurs in Bi2201, but at a binding energy around half that in Bi2212, implying its scaling to Tc. Surprisingly the coupling-energy dramatically increases with a decrease of carrier concentration, showing a sharp enhancement across the optimal doping. This strongly contrasts to other mode-couplings at higher binding-energies (~20, ~40, and ~70 meV) with almost no doping variation in energy scale. These nontrivial properties of the low-energy kink (material- and doping-dependence of the coupling-energy) demonstrate the significant correlation among the mode-coupling, the Tc, and the strong electron correlation.

We performed a Laser angle-resolved photoemission spectroscopy (ARPES) study on a wide doping range of Ba1-xKxFe2As2 (BaK) and precisely determined the doping evolution of the superconducting (SC) gaps in this compound. The gap size of the outer hole Fermi surface (FS) sheet around the Brillioun zone (BZ) center shows an abrupt drop with overdoping (for x > 0.6) while the inner and middle FS gaps roughly scale with Tc. This is accompanied by the simultaneous disappearance of the electron FS sheet with similar orbital character at the BZ corner. These results browse the different contributions of X2-Y2 and XZ/YZ orbitals to superconductivity in BaK and can be hardly completely reproduced by the available theories on iron-based superconductors.

Ultrafast dynamics of graphite is investigated by time-resolved photoemission spectroscopy. We observe spectral features of direct photoexcitations, non-thermal electron distributions, and recovery dynamics occurring with two time scales having distinct pump-power dependences. Additionally, we find an anomalous increase of the spectral intensity around the Fermi level, and we attribute this to spectral broadenings due to coupled optical phonons in the transient. The fingerprints of the coupled optical phonons occur from the temporal region where the electronic temperature is still not definable. This implies that there is a mechanism of ultrafast-and-efficient phonon generations beyond a two-temperature model.

Circular dichroism in the angular distribution (CDAD) of photoelectrons from SrTiO3:Nb and CuxBi2Se3 is investigated by 7-eV laser ARPES. In addition to the well-known node that occurs in CDAD when the incidence plane matches the mirror plane of the crystal, we show that another type of node occurs when the mirror plane of the crystal is vertical to the incidence plane and the electronic state is two dimensional. The flower-shaped CDAD's occurring around the Fermi level of SrTiO3:Nb and around the Dirac point of CuxBi2Se3 are explained on equal footings. We point out that the penetration depth of the topological states of CuxBi2Se3 depends on momentum.

We have investigated charge dynamics and electronic structures for single crystals of metallic layered nickelates, R2-xSrxNiO4 (R=Nd, Eu), isostructural to La2-xSrxCuO4. Angle-resolved photoemission spectroscopy on the barely-metallic Eu0.9Sr1.1NiO4 (R=Eu, x=1.1) has revealed a large hole surface of x2-y2 character with a high-energy pseudogap of the same symmetry and comparable magnitude with those of underdoped (x<0.1) cuprates, although the antiferromagnetic interactions are one order of magnitude smaller. This finding strongly indicates that the momentum-dependent pseudogap feature in the layered nickelate arises from the real-space charge correlation., Comment: 4 pages, 4 figures. Accepted in Physical Review Letters

Time-resolved photoelectron spectroscopy (trPES) can directly detect transient electronic structure, thus bringing out its promising potential to clarify nonequilibrium processes arising in condensed matters. Here we report the result of core-level (CL) trPES on 1T-TaS2, realized by developing a high-intensity 60 eV laser obtained by high-order harmonic (HH) generation. Ta4f CL-trPES offers the transient amplitude of the charge-density-wave (CDW), via the site-selective and real-time observation of Ta electrons. The present result indicates an ultrafast photoinduced melting and recovery of CDW amplitude, followed by a peculiar long-life oscillation (i.e. collective amplitudon excitation) accompanying the transfer of 0.01 electrons among adjacent Ta atoms. CL-trPES offers a broad range of opportunities for investigating the ultrafast atom-specific electron dynamics in photo-related phenomena of interest.

We investigate the transport properties of LixCoO2 thin films whose resistivities are nearly an order of magnitude lower than those of the bulk polycrystals. A metal-nonmetal transition occurs at ~0.8 in a biphasic domain, and the Seebeck coefficient (S) is drastically increased at ~140 K (= T*) with increasing the Li concentration to show a peak of magnitude ~120 \muV/K in the S-T curve of x = 0.87. We show that T* corresponds to a crossover temperature in the conduction, most likely reflecting the correlation-induced temperature dependence in the low-energy excitations.

The magnetic properties of Zn$_{1-x}$Co$_x$O ($x=0.07$ and 0.10) thin films, which were homo-epitaxially grown on a ZnO(0001) substrates with varying relatively high oxygen pressure, have been investigated using x-ray magnetic circular dichroism (XMCD) at Co $2p$ core-level absorption edge. The line shapes of the absorption spectra are the same in all the films and indicate that the Co$^{2+}$ ions substitute for the Zn sites. The magnetic-field and temperature dependences of the XMCD intensity are consistent with the magnetization measurements, indicating that except for Co there are no additional sources for the magnetic moment, and demonstrate the coexistence of paramagnetic and ferromagnetic components in the homo-epitaxial Zn$_{1-x}$Co$_{x}$O thin films, in contrast to the ferromagnetism in the hetero-epitaxial Zn$_{1-x}$Co$_{x}$O films studied previously. The analysis of the XMCD intensities using the Curie-Weiss law reveals the presence of antiferromagnetic interaction between the paramagnetic Co ions. Missing XMCD intensities and magnetization signals indicate that most of Co ions are non-magnetic probably because they are strongly coupled antiferromagnetically with each other. Annealing in a high vacuum reduces both the paramagnetic and ferromagnetic signals. We attribute the reductions to thermal diffusion and aggregation of Co ions with antiferromagnetic nanoclusters in Zn$_{1-x}$Co$_{x}$O., Comment: 21 pages, 7 figures, accepted for Physical Review B