First principles simulations of energy and polarization dependent angle-resolved photoemission spectra of Bi2212

We discuss first-principles simulations of angle-resolved photoemission (ARPES) intensity in Bi2212 where the photoexcitation process is modeled realistically by taking into account the full crystal wavefunctions of the initial and final states in the presence of the surface. Some recent results aimed at understanding the effects of the energy and polarization dependencies of the ARPES matrix element are presented. The nature of the Fermi surface (FS) maps obtained via ARPES by holding the initial state energy fixed at the Fermi energy (E_F) is clarified. The theoretically predicted FS map at 21 eV photon energy displays a remarkable level of agreement with the corresponding ARPES spectrum taken over a large area of the (k_x,k_y) plane. Our analysis shows how the ARPES matrix element can help disentangle closely spaced energy levels and FS sheets and highlight different aspects of the electronic spectrum in complex materials under various experimental conditions.     

Direct photoemission spectroscopy and electronic properties of in situ grown,strained high-Tc and related oxide films

We have optimized laser ablation thin film deposition and transfer procedures within synchrotron vault, specifically to perform angle-integrated and angle-resolved photoemission spectroscopy (ARPES) on high-T_c and related films without cleaving the samples. However, the chain-containing phases like YBCO-123 easily loose surface oxygen and do not exhibit stable Fermi edge, hence are not suitable for ARPES studies. Direct in situ ARPES studies on strained LSCO-214 films show striking strain effects on the electronic structure. The Fermi surface (FS) of LSCO evolves with doping, yet changes even more significantly with strain. The strain changes the FS topology from hole-like to electron-like, and causes band dispersion along k_x and the Fermi level crossing before the Brillouin zone boundary, in sharp contrast to the ‘usual’ flat band remaining ≈30 meV below E_F measured on unstrained samples. The associated reduction of the density of states does not diminish the superconductivity; T_c is enhanced in all our strained samples. Implications for the evolving high-T_c theory and studies of nano-engineered film heterostructures are briefly discussed.     

Bulk vs. surface effects in ARPES experiment from La2/3Sr1/3MnO3 thin films

Experiments directly probing the electronic states using angle-resolved photoemission (ARPES) were carried out on La_2/3Sr_1/3MnO₃ in order to elucidate its electronic properties. ARPES is a surface sensitive technique where bulk and surface states are usually both present. We present high-resolution ARPES studies in the (1 0 0) and (1 1 0) mirror planes and compare them with simulated ARPES based on GGA + U band structure calculations. In the (1 1 0) mirror plane we identify surface umklapps accounted by surface reconstruction which couple to bulk electronic states. As predicted by the simulated spectra there is additional spectral intensity at the Fermi level detected in ARPES data due to k_⊥-broadening effects in the photoemission final states. We demonstrate that this additional spectral intensity is a convenient spectral marker for determination of the k_F Fermi momenta.     

Polarization dependence of angle-resolved photoemission spectroscopy of graphite

We have used variable polarization synchrotron radiation to map the valence band electronic structure of graphite by angle-resolved photoemission spectroscopy (ARPES). The experimental results with two orthogonal linear polarization of light signifies the contribution of either even or odd symmetry with respect to the crystal mirror plane towards the photoemission intensity. The σ₁ and σ₂ valence bands show odd reflection symmetry while the π valence band shows even symmetry with respect to the mirror plane. The measured ARPES spectrum using left and right circular polarized lights shows asymmetry in intensity around M point of the Brillouin zone, which ultimately mimicking different partial wave character of σ₁ and σ₃ bands.     

Bridging charge-orbital ordering and Fermi surface instabilities in half-doped single-layered manganite La(0.5)Sr(1.5)MnO₄

The single-layered half-doped manganite La(0.5)Sr(1.5)MnO? (LSMO), was studied by means of the angle-resolved photoemission spectroscopy (ARPES), scanning tunneling microscopy (STM), and resistivity measurements. STM revealed a smooth reconstruction-free surface; the density of states, extracted from photoemission and tunneling spectroscopy, is in agreement with transport measurements. The derived from ARPES Fermi surface (FS) nesting properties correspond to the known pattern of the charge-orbital ordering (COO), which implies that FS instability is related to the propensity to form a COO state in LSMO.     

Ce 基重费米子材料的电子态研究与维度调控

重费米子材料作为一类典型的强关联电子体系,蕴含着非常规超导、奇异金属、量子临界、 磁有序、重电子态、关联拓扑态等新奇的量子态,而4f 电子在其中扮演着重要的作用。随着高分 辨角分辨光电子能谱和薄膜生长技术的发展,精确探测重费米子材料中4f 电子在能量/动量空间 的色散和谱权重成为了可能,这为从微观上理解这类材料中的电子关联效应和新奇量子现象提供 了重要的基础。本论文总结了几个典型的重费米子单晶和薄膜体系的电子态研究,包括Ce-115 体 系、CeCu2Si2、CeRh6Ge4 以及单晶 Ce 膜等。这些结果为理解重费米子体系中重电子态的形成 和温度演化、近藤杂化的能带/动量依赖、重电子能带与超导的关系、近藤效应与磁性和其它量子 态的竞争、4f 电子的维度调控等重要物理问题提供了谱学证据。     

Electronic structure and anomalous photoemission line-shape of quasi-2D oxide η-Mo4O11

The η-Mo₄O₁₁ compound is a layered two-dimensional (2D) metallic system whose reduced dimensionality originates non-linear properties as charge density wave (CDW) instabilities. We report on synchrotron radiation angle resolved photoemission spectroscopy (ARPES) measurements in order to obtain a detailed picture of the electronic structure of this material. The symmetry of the states near the Fermi level (E_F) has been discussed in relation to the photoemission symmetry selections rules. Our results are in excellent agreement with previous tight-binding calculations and support the hidden nesting concept proposed to explain the CDW instabilities exhibited by this family of compounds. In addition, a very peculiar photoemission line-shape has been found with the presence of localized non-dispersive states. Some possible explanations are discussed.     

Valence band photoemission on metallic Ce systems

The valence band photoemission spectroscopy of metallic Ce systems is inspected with regard to the different models employed for the interpretation of the data. It is concluded, that contrary to general believe, in most systems higher lyingf-excitations within the 4f manifold are observed, and the observation of the Kondo resonance is difficult.     

Direct observation of dispersive Kondo resonance peaks in a heavy-fermion system

Ce 4d-4f resonant angle-resolved photoemission spectroscopy was carried out to study the electronic structure of strongly correlated Ce 4f electrons in a quasi-two-dimensional nonmagnetic heavy-fermion system CeCoGe1.2Si0.8. For the first time, dispersive coherent peaks of an f state crossing the Fermi level, the so-called Kondo resonance, are directly observed together with the hybridized conduction band. Moreover, the experimental band dispersion is quantitatively in good agreement with a simple hybridization-band picture based on the periodic Anderson model. The obtained physical quantities, i.e., coherent temperature, Kondo temperature, and mass enhancement, are comparable to the results of thermodynamic measurements. These results manifest an itinerant nature of Ce 4f electrons in heavy-fermion systems and clarify their microscopic hybridization mechanism.     

Photoemission from Cerium systems

The analysis of the valence band photoemission spectra of Ce compounds is inspected. It is found that the data and the models agree in that they give a 4f hole state at a binding energy of 2 eV and a 4f band near (within 100 meV) the Fermi energy. The implications of photoemission data for the electronic structures of heavy fermion systems is discussed.     

Charge-density-wave partial gap opening in quasi-2D KMo6O17 purple bronze studied by angle resolved photoemission spectroscopy

Low dimensional (LD) metallic oxides have been a subject of continuous interest in the last two decades, mainly due to the electronic instabilities that they present at low temperatures. In particular, charge density waves (CDW) instabilities associated with a strong electron-phonon interaction have been found in Molybdenum metallic oxides such as KMo₆O₁₇ purple bronze. We report an angle resolved photoemission (ARPES) study from room temperature (RT) to T ∼40 K well below the Peierls transition temperature for this material, with CDW transition temperature T_CDW ∼120 K. We have focused on photoemission spectra along ΓM high symmetry direction as well as photoemission measurements were taken as a function of temperature at one representative k_F point in the Brillouin zone in order to look for the characteristic gap opening after the phase transition. We found out a pseudogap opening and a decrease in the density of states near the Fermi energy, E_F, consistent with the partial removal of the nested portions of the Fermi surface (FS) at temperature below the CDW transition. In order to elucidate possible Fermi liquid (FL) or non-Fermi liquid (NFL) behaviour we have compared the ARPES data with that one reported on quasi-1D K_0.3MoO₃ blue bronze.     

Electronic structure of La (0001) thin films on W (110) studied by photoemission spectroscopy and first principle calculations

Surface states that have a dz2 symmetry around the center of the surface Brillouin zone(BZ)have been regarded common in closely-packed surfaces of rare-earth metals.In this work,we report the electronic structure of dhcp La(0001)thin films by ultrahigh energy resolution angle-resolved photoemission spectroscopy(ARPES)and first principle calculations.Our first principle analysis is based on the many-body approach,therefore,density function theory(DFT)combined with dynamic mean-field theory(DMFT).The experimentally observed Fermi surface topology and band structure close to the Fermi energy qualitatively agree with first principle calculations when using a renormalization factor of between 2 and 3 for the DFT bands.Photon energy dependent ARPES measurements revealed clear kZ dependence for the hole-like band around the BZ center,previously regarded as a surface state.The obtained ARPES results and theoretical calculations suggest that the major bands of dhcp La(0001)near the Fermi level originate from the bulk La 5d orbits as opposed to originating from the surface states.     

Tuning the dispersion of 4f bands in the heavy-fermion material YbRh2Si2

Localized Yb 4f and itinerant Rh 4d states are subject to substantial hybridization effects in the heavy-fermion material YbRh₂Si₂. The proximity to the Fermi level and the high anisotropy in k space naturally raise questions regarding the role of these hybridization effects for the observed, unusual physical properties. Using angle-resolved photoemission spectroscopy (ARPES) we found that the non-dispersive behavior of the localized Yb f states is broken around the Γ point due to interaction with approaching Rh 4d bands. The intriguing point here is that the hybridization strength turns out to be systematically tunable by electron doping of the material. Gradual deposition of silver atoms onto the atomically clean, silicon terminated surface of YbRh₂Si₂ leads to transfer of Ag 5s charge into the Rh 4d bands. This substantially changes the energy overlap, and thus the hybridization strength, between the interacting Yb 4f and Rh 4d bands in the surface and subsurface region. The shown possibility to control the variation of the f-d hybridization at the surface of heavy-fermion materials may also be helpful for other ARPES studies on the diverse phenomena in electron-correlated materials.     

Angle-resolved photoemission spectroscopy study of Fe(1 1 0) single crystal: Many-body interactions between quasi-particles at the Fermi level

A high-resolution angle-resolved photoemission spectroscopy (ARPES) study of Fe(1 1 0) single crystal was conducted to elucidate many-body interactions between quasi-particles at the Fermi level at low-temperature. Two kink structures were observed in the energy-band dispersion at the binding energies of ∼40 meV and ∼270 meV for the bulk-derived band on the majority-spin Fermi surface around the Γ point. Based on analyses of the experimentally obtained real parts of the self-energy, these kink structures are derived from electron-phonon and electron-magnon interactions.     

Ultrahigh-resolution laser photoemission study of URu2Si2 across the hidden-order transition

We have studied the electronic structures of URu₂Si₂ employing ultrahigh-resolution laser angle-resolved photoemission spectroscopy. The change of photoemission spectra is investigated across the hidden-order transition, and the emergence of a narrow band is clearly observed near the Fermi level for both (π,0) and (π,π) directions. In addition, it is shown that tuning of light's polarization allows the signal of a hole-like dispersive feature to enhance. These observations prove that laser angle-resolved photoemission spectroscopy is an effective tool for studying the evolution of electronic structures across the hidden-order transition in URu₂Si₂.     

Impact of Ultrathin Pb Films on the Topological Surface and Quantum-Well States of Bi<Subscript>2</Subscript>Se<Subscript>3</Subscript> and Sb<Subscript>2</Subscript>Te<Subscript>3</Subscript> Topological Insulators

The effect of an ultrathin Pb film deposited on the surface of Bi₂Se₃ and Sb₂Te₃ compounds on the electronic state structure of topological insulators is studied experimentally by the angle-resolved photoemission spectroscopy (ARPES) technique. The following features are revealed: formation of two-dimensional quantum-well states in the near-surface region, an increase in the binding energy of the Dirac cone and the core levels, and a simultaneous electronic states intensity redistribution in the system in photoemission spectra. The results obtained show that topological states may coexist at the interface between studied materials and a superconductor, which seems to be promising for application in quantum computers.     

The formation of heavy-fermion states in non-Fermi-liquid impurity systems

A mechanism for the occurrence of heavy-fermion states in non-Fermi-liquid (NFL) metals with f-shell impurities is proposed. The impurity with an unstable valence is suggested to have an energy spectrum consisting of a deep f-level and quasicontinuum states (narrow band) in resonance with the Fermi energy. Depending on the impurity concentration, the single-site NFL states are generated by the two-channel Kondo scattering for the low concentration (the Kondo regime) or by the screening interaction for a relatively high concentration (the X-ray-edge regime). It is shown that the NFL states are unstable against the scattering of the NFL excitations by electron states of the narrow band. This scattering generates additional narrow Fermi-liquid (FL) resonances at/near the Fermi level in the Kondo regime and in the X-ray-edge regime. The mixed-valence states are shown to be induced by new FL resonances. The mixed valence mechanism is local and is related to the instability of single-site NFL states. The FL resonances lead to the existence of additional energy scales and of pseudogaps near the Fermi level in the mixed-valence states. They also considerably narrow the region with a nearly integer valence.     

Missing xy-band Fermi surface in 4d transition-metal oxide Sr2RhO4: effect of the octahedra rotation on the electronic structure

Electronic structures of the 4d transition-metal oxide compound Sr2RhO4 are investigated by angle-resolved photoemission spectroscopy and density-functional electronic structure calculations. In the measured Fermi surfaces (FS) of Sr2RhO4, the xy-band FS sheet expected from the well-established results of the FS of Sr2RuO4 is missing, the volume of which should be different only by one additional electron for Sr2RhO4. The apparent contradiction is resolved by a careful analysis of the band structure where the rotation of octahedra results in the hybridization of e(g) and t(2g) states and thus plays a key role in the determination of the electronic structure near EF. The modification of the FS structure due to the distorted lattice is related to the charge transfer among the orbital states and suggested to be relevant to the metal-insulator transition in Ca(2-x)Sr(x)RuO4.     

Quasiparticle lifetime in graphite studied by ultrahigh-resolution ARPES

We have performed ultrahigh-resolution angle-resolved photoemission spectroscopy (ARPES) to elucidate the nature of quasiparticle dynamics in graphite. We found fairly sharp quasiparticle peak of π band around K(H) point in the vicinity of the Fermi level, together with the strong mass renormalization of the band (kink). The imaginary part of electron self-energy (ImΣ) shows a sudden drop below 0.18 eV, indicative of a strong electron-phonon coupling. The linear energy dependence of ImΣ at higher binding energies provides an evidence for the deviation from the conventional Fermi liquid theory.