We investigated the nonequilibrium electronic structure of 2H-NbSe$_2$ by time- and angle-resolved photoemission spectroscopy. We find that the band structure is distinctively modulated by strong photo-excitation, as indicated by the unusual increase in the photoelectron intensities around E$_F$. In order to gain insight into the observed photo-induced electronic state, we performed DFT calculations with modulated lattice structures, and found that the variation of the Se height from the Nb layer results in a significant change in the effective mass and band gap energy. We further study the momentum-dependent carrier dynamics. The results suggest that the relaxation is faster at the K-centered Fermi surface than at the $Γ$-centered Fermi surface, which can be attributed to the stronger electron-lattice coupling at the K-centered Fermi surface. Our demonstration of band structure engineering suggests a new role for light as a tool for controlling the functionalities of solid-state materials.
We present the first observation of dynamically modulated quantum phase transition (QPT) between two distinct charge density wave (CDW) phases in 2-dimensional 2H-NbSe$_2$. There is recent spectroscopic evidence for the presence of these two quantum phases, but its evidence in bulk measurements remained elusive. We studied suspended, ultra-thin \nbse devices fabricated on piezoelectric substrates - with tunable flakes thickness, disorder level and strain. We find a surprising evolution of the conductance fluctuation spectra across the CDW temperature: the conductance fluctuates between two pre…
We revisit charge density wave (CDW) behavior in the archetypal quasi-one-dimensional (quasi-1D) material NbSe$_3$ by high-resolution angle-resolved photoemission spectroscopy measurements utilizing a microfocused laser with a photon energy of 6.3 eV. We present a detailed view of the electronic structure of this complex multiband system and unambiguously resolve CDW gaps at the Fermi level ($E_F$). By employing a tight-binding model, we argue that these gaps are the result of interband coupling between electronic states that reside predominantly on distinct 1D chains within the material. Two …
We have probed the crystalline electric-field ground states of pure $|J = 7/2, J_z = \pm 5/2\rangle$ as well as the anisotropic $c$-$f$ hybridization in both valence fluctuating systems $α$- and $β$-YbAlB$_4$ by linear polarization dependence of angle-resolved core level photoemission spectroscopy. Interestingly, the small but distinct difference between \abyb was found in the polar angle dependence of linear dichroism, indicating the difference in the anisotropy of $c$-$f$ hybridization which may be essential to a heavy Fermi liquid state in $α$-YbAlB$_4$ and a quantum critical state in $β$-Y…
Hybridization between surface flat bands and bulk bands in the topological nodal-line semimetal Sn$_{0.15}$NbSe$_{1.75}$ probed via soft-point-contact spectroscopy
We show that a small number of intentionally introduced defects can be used as a spectroscopic tool to amplify quasiparticle interference in 2H-NbSe$_{2}$, that we measure by scanning tunneling spectroscopic imaging. We show from the momentum and energy dependence of the quasiparticle interference that Fermi surface nesting is inconsequential to charge density wave formation in 2H-NbSe$_{2}$. We demonstrate that by combining quasiparticle interference data with additional knowledge of the quasiparticle band structure from angle resolved photoemission measurements, one can extract the wavevecto…
A combined experimental and theoretical study of very-low-energy electron diffraction at the (0001) surface of 2H-NbSe2 is presented. Electron transmission spectra have been measured for energies up to 50 eV above the Fermi level with k|| varying along the GammaK line of the Brillouin zone. Ab initio calculations of the spectra have been performed with the extended linear augmented plane wave k-p method. The experimental spectra are interpreted in terms of three-dimensional one-electron band structure. Special attention is paid to the quasi-particle lifetimes: by comparing the broadening of th…
We have studied disorder-induced in-gap states and effect of light illumination in the insulating phase of spinel-type CuIr$_2$S$_4$ using ultra-violet photoemission spectroscopy (UPS). The Ir$^{3+}$/Ir$^{4+}$ charge-ordered gap appears below the metal-insulator transition temperature. However, in the insulating phase, in-gap spectral features with $softgap$ are observed in UPS just below the Fermi level ($E_F$), corresponding to the variable range hopping transport observed in resistivity. The spectral weight at $E_F$ is not increased by light illumination, indicating that the Ir$^{4+}$-Ir$^{…
We have successfully observed linear dichroism in angle-resolved Yb3+ 3d5/2 core-level photoemission spectra for YbB12 in cubic symmetry. Its anisotropic 4f charge distribution due to the crystal-field splitting is responsible for the linear dichroism, which has been verified by spectral simulations using ionic calculations with the full multiplet theory for a single-site Yb3+ ion in cubic symmetry. The observed linear dichroism as well as the polarization-dependent spectra in two different photoelectron directions for YbB12 are quantitatively reproduced by theoretical analysis for the Gamma_8…
High-resolution photoemission has been used to study the electronic structure of the charge density wave (CDW) and superconducting (SC) dichalcogenide, 2H- NbSe2. From the extracted self-energies, important components of the quasiparticle (QP) interactions have been identified. In contrast to previously studied TaSe2, the CDW transition does not affect the electronic properties significantly. The electron-phonon coupling is identified as a dominant contribution to the QP self-energy and is shown to be very anisotropic (k-dependent) and much stronger than in TaSe2.
Electronic properties of V$_2$OPO$_4$ have been investigated by means of hard x-ray photoemission spectroscopy (HAXPES) and subsequent theoretical calculations. The V 1$s$ and 2$p$ HAXPES spectra are consistent with the charge ordering of V$^{2+}$ and V$^{3+}$. The binding energy difference between the V$^{2+}$ and V$^{3+}$ components is unexpectedly large indicating large bonding-antibonding splitting between them in the final states of core level photoemission. The V 1$s$ HAXPES spectrum exhibits a charge transfer satellite which can be analyzed by configuration interaction calculations on a…
Recently, $α$-$\textrm{RuCl}_3$ has attracted much attention as a possible material realization of the honeycomb Kitaev model, which may stabilize a quantum-spin-liquid state. Compared to extensive studies on its magnetic properties, there is still a lack of understanding on its electronic structure, which is strongly related with its Kitaev physics. Here, the electronic structure of $α$-$\textrm{RuCl}_3$ is investigated by photoemission (PE) and inverse photoemission (IPE) spectroscopies. The band gap, directly measured from PE/IPE spectra, is found to be 1.9 eV, much larger than previous est…
Using angle-resolved photoemission spectroscopy (ARPES), we report on the direct observation of the energy gap in 2H-NbSe2 caused by the charge-density waves (CDW). The gap opens in the regions of the momentum space connected by the CDW vectors, which implies a nesting mechanism of CDW formation. In remarkable analogy with the pseudogap in cuprates, the detected energy gap also exists in the normal state (T>T0) where it breaks the Fermi surface into 'arcs', it is non-monotonic as a function of temperature with a local minimum at the CDW transition temperature (T0) and it forestalls the superco…
We have studied the electronic structure of RuP and related Ru pnictides using photoemission spectroscopy. Ru 3d core-level and valence-band spectra of RuP show that the Ru valence is +3 with t_{2g}^5 configuration. The photoemisson spectral weight near the Fermi level is moderately suppressed in the pseudogap phase of RuP, consistent with the pseudogap opening of 2Δ/k_BT_c ~ 3 (gap size Δ~ 50 meV and transition temperature T_c ~ 330 K). The Ru 3d peak remains sharp in the pseudogap phase and the insulating phase of RuP, suggesting that the electronic orderings responsible for the phase transi…
Here we apply high resolution angle-resolved photoemission spectroscopy (ARPES) using a wide excitation energy range to probe the electronic structure and the Fermi surface topology of the Ba1-xKxFe2As2 (Tc = 32 K) superconductor. We find significant deviations in the low energy band structure from that predicted in calculations. A set of Fermi surface sheets with unexpected topology is detected at the Brillouin zone boundary. At the X-symmetry point the Fermi surface is formed by a shallow electron-like pocket surrounded by four hole-like pockets elongated in G-X and G-Y directions.
The three-dimensional Fermi surface structure of hole-doped metallic layered nickelate Eu2-xSrxNiO4 (x=1.1), an important counterpart to the isostructural superconducting cuprate La2-xSrxCuO4, is investigated by energy-dependent soft-x-ray angle-resolved photoemission spectroscopy. In addition to a large cylindrical hole Fermi surface analogous to the cuprates, we observe a Gamma-centered 3z2-r2-derived small electron pocket. This finding demonstrates that in the layered nickelate the 3z2-r2 band resides close to the x2-y2 one in energy. The resultant multi-band feature with varying orbital ch…
High-resolution angle-resolved photoemission spectroscopy (ARPES) data reveal evidence of a crossover from one-dimensional (1D) to three-dimensional (3D) behavior in the prototypical charge density wave (CDW) material NbSe3. In the low-temperature 3D regime, gaps in the electronic structure are observed due to two incommensurate CDWs, in agreement with x-ray diffraction and electronic-structure calculations. At higher temperatures we observe a spectral weight depletion that approaches the power-law behavior expected in 1D. From the warping of the quasi-1D Fermi surface at low temperatures, we …
A set of LaAlO3/SrTiO3 (LAO-STO) interfaces has been probed by X-ray photoemission spectroscopy in order to contrast and compare the effects of LAO overlayer thickness and of the growth conditions on the electronic properties of these heterostructures. These effects are tracked by considering the band-offset and the density of Ti3+ states, respectively. It is shown that the dominant effects on the local electronic properties are determined by the O2 partial pressure during the growth. In particular, a low P(O2) yields Ti3+ states with higher density and lower binding energy as compared to the …
Eu2Ir2O7, a candidate Weyl semimetal, shows an insulator-to-metal transition as a function of Bi substitution at the Eu site. In this work, we investigate the (Eu_1-xBi_x)2Ir2O7 series via Hard X-ray Photoemission Spectroscopy (HAXPES), where substitution of larger Bi3+ for Eu3+ is reported to result in an anomalous lattice contraction (20 %) for low Bi doping (3.5 %). Using HAXPES, we confirm that all the cations retain their nominal valence state throughout the series. The asymmetric nature of Bi core-level spectra for compositions in the metallic region indicates that Bi contributes to the …
The discovery of infinite-layer nickelate superconductors has spurred enormous interest. While the Ni$^{1+}$ cations possess nominally the same 3$d^9$ configuration as Cu$^{2+}$ in cuprates, the electronic structure variances remain elusive. Here, we present a soft x-ray photoemission spectroscopy study on parent and doped infinite-layer Pr-nickelate thin films with a doped perovskite reference. By identifying the Ni character with resonant photoemission and comparison to density functional theory + U (on-site Coulomb repulsion energy) calculations, we estimate U ~5 eV, smaller than the charge…
The electronic properties of the Mn:GaSe interface, produced by evaporating Mn at room temperature on an epsilon-GaSe(0001) single crystal surface, have been studied by soft X-ray spectroscopies. Substitutional effects of Mn replacing Ga cations and Mn-Se hybridization effects are found both in core level and valence band photoemission spectra. The Mn cation valence state is probed by XAS measurements at the Mn L-edge, which indicate that Mn diffuses into the lattice as a Mn2+ cation with negligible crystal field effects. The Mn spectral weight in the valence band is probed by resonant photoem…
Recent renewed interest in the mixed valent insulator SmB6 comes from topological theory predictions and surface transport measurements of possible in-gap surface states whose existence is most directly probed by angle-resolved photoemission spectroscopy (ARPES). Early photoemission leading up to a recent flurry of ARPES studies of in-gap states is reviewed. Conflicting interpretations about the nature of the Sm 4f-5d hybridization gap and observed X-point bands between the f-states and the Fermi level are critically assessed using the important tools of photon polarization and spatial depende…
An excitonic insulator phase is expected to arise from the spontaneous formation of electron-hole pairs (excitons) in semiconductors where the exciton binding energy exceeds the size of the electronic band gap. At low temperature, these ground state excitons stabilize a new phase by condensing at lower energy than the electrons at the valence band top, thereby widening the electronic band gap. The envisioned opportunity to explore many-boson phenomena in an excitonic insulator system is triggering a very active debate on how ground state excitons can be experimentally evidenced. Here, we emplo…
We report an in-depth Angle Resolved Photoemission Spectroscopy (ARPES) study on $2H$-TaS$_2$, a canonical incommensurate Charge Density Wave (CDW) system. This study demonstrates that just as in related incommensurate CDW systems, $2H$-TaSe$_2$ and $2H$-NbSe$_2$, the energy gap ($Δ_{\text{cdw}}\,$) of $2H$-TaS$_2$ is localized along the K-centered Fermi surface barrels and is particle-hole asymmetric. The persistence of $Δ_{\text{cdw}}\,$ even at temperatures higher than the CDW transition temperature $\it{T}_{\text{cdw}}\,$ in $2H$-TaS$_2$, reflects the similar pseudogap (PG) behavior observ…
We report photoemission studies of polycrystalline samples of Sr-doped GdTiO_{3+delta}, which undergoes a Mott-Hubbard-like metal-insulator transition at a Ti-concentration of about 20%. The Ti 3d-derived valence band near the Fermi level displays a two-peak structure consistent with a Hubbard-model-type interpretation as quasiparticle and lower Hubbard band. Contrary to the theoretical expectation the lower Hubbard band does not change its energy with doping. However, the analysis of the core level spectra and elemental mapping with a scanning electron microscope indicate a strongly inhomogen…
Electronic inhomogeneity in Cs- and Sb-terminated surfaces of CsV$_3$Sb$_5$ probed by scanning photoemission spectromicroscopy
Waseda University（早稻田大学）；Sincrotrone Trieste S.C.p.A.（的里雅斯特同步辐射中心）；Beijing Institute of Technology（北京理工大学）；Southern University of Science and Technology（南方科技大学）
We report the Fermi surfaces of the superconductor Sr2RuO4 and the non-superconductor Sr1.8Ca0.2RuO4 probed by bulk-sensitive high-energy angle-resolved photoemission. It is found that there is one square-shaped hole-like, one square-shaped electron-like and one circle-shaped electron-like Fermi surface in both compounds. These results provide direct evidence for nesting instability giving rise to magnetic fluctuations. Our study clarifies that the electron correlation effects are changed with composition depending on the individual band.
In order to determine the orbital characters on the various Fermi surface pockets of the Fe-based superconductors Ba$_{0.6}$K$_{0.4}$Fe$_{2}$As$_{2}$ and FeSe$_{0.45}$Te$_{0.55}$, we introduce a method to calculate photoemission matrix elements. We compare our simulations to experimental data obtained with various experimental configurations of beam orientation and light polarization. We show that the photoemission intensity patterns revealed from angle-resolved photoemission spectroscopy measurements of Fermi surface mappings and energy-momentum plots along high-symmetry lines exhibit asymmet…
We present angle-resolved photoelectron spectroscopy data probing the electronic structure of the Nd-substituted high-$T_c$ cuprate La$_{1.48}$Nd$_{0.4}$Sr$_{0.12}$CuO$_4$ (Nd-LSCO). Data have been acquired at low and high photon energies, $hν$ = 55 and 500 eV, respectively. Earlier comparable low-energy studies of La$_{1.4-x}$Nd$_{0.6}$Sr$_{x}$CuO$_4$ ($x = 0.10, 0.12, 0.15$) have shown strongly suppressed photoemission intensity, or absence thereof, in large parts of the Brillouin zone. Contrary to these findings we observe spectral weight at all points along the entire Fermi surface contour…
Development of ultrafast lasers and non-linear optical techniques over the last two decades provides tools to access real-time dynamics of low energy excitations in superconductors. For example, time-resolved THz spectroscopy and time- and angular-resolved photoemission spectroscopy provide access to the real-time dynamics of the superconducting gap amplitude. Such studies enable determination of microscopic parameters like quasi-particle recombination rates, pair-breaking rates and electron-boson coupling constants. Recently, intense THz pulses have been used to probe the non-linear dynamics,…
Clustering-Enhanced Time- and Angle-Resolved Photoemission Study of LaTe$_3$: Absence of a Photoinduced Secondary CDW in the Electronic Structure
Aarhus University（奥胡斯大学）；CNR, Consiglio Nazionale delle Ricerche, Istituto officina dei materiali（意大利国家研究委员会材料研究所）；Central Laser Facility, STFC Rutherford Appleton Laboratory（STFC鲁瑟福阿普尔顿实验室中央激光设施）；SUPA, School of Physics and Astronomy, University of St Andrews（圣安德鲁斯大学物理与天文学学院）；Stanford University（斯坦福大学）；Diamond Light Source Ltd（钻石光源有限公司）；Princeton University（普林斯顿大学）；Department of Physics, Indian Institute of Technology Guwahati（印度理工学院古瓦哈提分校物理系）
We use time- and angle-resolved photoemission spectroscopy to characterize the dynamics of the energy gap in superconducting Bi2Sr2CaCu2O8+delta (Bi2212). Photoexcitation drives the system into a nonequilibrium pseudogap state: Near the Brillouin zone diagonal (inside the normal-state Fermi arc), the gap completely closes for a pump fluence beyond F = 15 μJ/cm^2; toward the Brillouin zone face (outside the Fermi arc), it remains open to at least 24 μJ/cm^2. This strongly anisotropic gap response may indicate multiple competing ordering tendencies in Bi2212. Despite these contrasts, the gap rec…
We investigate the excited state electronic structure of the model phase transition system In/Si(111) using femtosecond time- and angle-resolved photoemission spectroscopy (trARPES) with an XUV laser source at 500 kHz . Excited state band mapping is used to characterize the normally unoccupied electronic structure above the Fermi level in both structural phases of indium nanowires on Si(111): the metallic (4x1) and the gapped (8x2) phases. The extracted band positions are compared with the band structure calculated using density functional theory (DFT) within both the LDA and GW approximations…
Electronic structure, electrical transport, dc and ac magnetization properties of the hole substituted (Sr2+) partially B-site disordered double perovskite Pr2-xSrxCoMnO6 system have been investigated. Electronic structure was probed by employing X-ray photoemission spectroscopy (XPS) measurements. The study suggested the presence of mixed valence states of the B-site ions (Co2+/Co3+ and Mn3+/Mn4+) with significant enhancement of the average oxidation states due to hole doping. The mere absence of electronic states near the Fermi level in the valence band (VB) spectra for both of the pure (x=0…
We used x-ray photoemission spectroscopy to investigate the electronic structure of the Mott insulator LaVO3 embedded in LaAlO3. By limiting the upper layer of LaAlO3 to 3 unit cells, the underlying LaVO3 could be probed. The V 2p core-level spectra had both V3+ and V4+ components, and above 2 unit cell thick LaVO3, the structures exhibited spectra similar to bulk samples. The atomically flat surfaces enabled study of the emission angle dependence, which indicates the V4+ is localized to the topmost layer. These results demonstrate the potential for probing interface electronic structure in ox…
The pursuit of a comprehensive understanding of the dynamical nature of intertwined orders in quantum matter has fueled the development of several new experimental techniques, including time- and angle-resolved photoemission spectroscopy (TR-ARPES). In this regard, the study of copper-oxide high-temperature superconductors, prototypical quantum materials, has furthered both the technical advancement of the experimental technique, as well as the understanding of their correlated dynamical properties. Here, we provide a brief historical overview of the TR-ARPES investigations of cuprates, and re…
We study the role of electron correlations in the presumed type II Weyl semimetallic candidate $γ$-MoTe$_2$ by employing density functional theory (DFT) where the on-site Coulomb repulsion (Hubbard U) for the Mo 4$d$ states is included within the DFT+U scheme. We show that pure DFT calculations fail to describe important features of the light-polarization dependence of the angular resolved photoemission intensity which can be accounted for by including the role of the Hubbard U. At the same time, while pure DFT calculations cannot explain the angular dependence of the Fermi surface as revealed…
Angle-resolved photoemission spectroscopy measurements on the recently discovered superconduc- tors in the KFe2Se2 family with critical temperatures up to - 33K suggest that no Fermi pockets of hole character centered on the Γ point of the Brillouin zone are present, in contrast to all other known ferropnictide and ferrochalcogenide superconductors. Using a fluctuation exchange approximation and a 5-orbital tight-binding description of the band structure, we calculate the effective pairing interaction. We find that the pairing state in this system is most likely to have d-wave symmetry due to …
Higher-order Weyl nodes driven by helical magnetic order in EuAgAs
Agency for Science, Technology and Research (A*STAR)（科学技术研究局）；Centre for Quantum Technologies, National University of Singapore（新加坡国立大学量子科技中心）；Hunan Normal University（湖南师范大学）；University of Oxford（牛津大学）；Institut Laue-Langevin（朗之万研究所）；Diamond Light Source（钻石光源）；École Polytechnique Fédérale de Lausanne（洛桑联邦理工学院）；University of Macau（澳门大学）
Core-level signature of long-range density-wave order and short-range excitonic correlations probed by attosecond broadband spectroscopy
University of California at Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Center for Computational Sciences, University of Tsukuba（筑波大学计算科学中心）；Max Planck Institute for the Structure and Dynamics of Matter（马普物质结构与动力学研究所）；Tsung-Dao Lee Institute and Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong University（上海交通大学桐江书院与张江高等研究院）
Using angle-integrated photoemission spectroscopy we have probed the novel LaO$_{0.9}$F$_{0.1}$FeAs superconductor over a wide range of photon energies and temperatures. We have provided the first full characterization of the orbital character of the VB DOS and of the magnitude of the d-p hybridization energy. Finally, we have identified two characteristic temperatures: 90K where a pseudogap-like feature appears to close and 120K where a sudden change in the DOS near E$_F$ occurs. We associate these phenomena with the SDW magnetic ordering and the structural transition seen in the parent compo…
Using soft x-ray angle-resolved photoemission spectroscopy we probed the bulk electronic structure of Td MoTe2. We found that on-site Coulomb interaction leads to a Lifshitz transition, which is essential for a precise description of the electronic structure. A hybrid Weyl semimetal state with a pair of energy bands touching at both type-I and type-II Weyl nodes is indicated by comparing the experimental data with theoretical calculations. Unveiling the importance of Coulomb interaction opens up a new route to comprehend the unique properties of MoTe2, and is significant for understanding the …
A notable role in understanding of microscopic electronic properties of high temperature superconductors (HTSC) belongs to angle resolved photoemission spectroscopy (ARPES). This technique supplies a direct window into reciprocal space of solids: the momentum-energy space where quasiparticles (the electrons dressed in clouds of interactions) dwell. Any interaction in the electronic system, e.g. superconducting pairing, leads to modification of the quasi-particle spectrum--to redistribution of the spectral weight over the momentum-energy space probed by ARPES. A continued development of the tec…
Three dimensional topological insulator crystals consist of an insulating bulk enclosed by metallic surfaces, and detailed theoretical predictions about the surface state band topology and spin texture are available. While several topological insulator materials are currently known, the existence and topology of these metallic states have only ever been probed for one particular surface orientation of a given material. For most topological insulators, such as Bi$_{1-x}$Sb$_{x}$ and Bi$_2$Se$_3$, this surface is the closed-packed (111) surface and it supports one topologically guaranteed surfac…
We report an extensive study on the intrinsic bulk electronic structure of the high-temperature superconductor CeFeAsO0.89F0.11 and its parent compound CeFeAsO by soft and hard x-ray photoemission, x-ray absorption and soft-x-ray emission spectroscopies. The complementary surface/bulk probing depth, and the elemental and chemical sensitivity of these techniques allows resolving the intrinsic electronic structure of each element and correlating it with the local structure, which has been probed by extended-x-ray absorption fine structure spectroscopy. The measurements indicate a predominant 4f1…
Systematic angle-resolved photoemission spectroscopy (ARPES) experiments have been carried out to investigate the bulk and (100) surface electronic structures of a topological mixed-valence insulator candidate, YbB6. The bulk states of YbB6 were probed with bulk-sensitive soft X-ray ARPES, which show strong three-dimensionality as required by cubic symmetry. Surprisingly the measured Yb 4f states are located around 1 eV and 2.3 eV below the Fermi level (EF), instead of being near EF as indicated by first principle calculations. The dispersive bands near EF are B 2p states, which hybridize with…
