Resolved Photoemission Spectra Research Articles

Carrier Relaxation and Multiplication in Bi Doped Graphene (Small 18/2023)

Bi Doped Graphene In article number 2206218, Xianyang Lu, Thomas Frauenheim, Yongbing Xu, and co-workers investigate femtosecond laser excitation induced electronic dynamic in Bi doped graphene, using time resolved and angular resolved photoemission spectrum. The Fermi surface in Dirac cone and carrier concentration is modulated by adatoms' content. This effectively tailors the competition between auger combination and impact excitation, tuning the carrier multiplication in graphene.

Single crystal growth of topological semimetals and magnetic topological materials

Topological materials have attracted much attention due to their novel physical properties. These materials can not only serve as a platform for studying the fundamental physics, but also demonstrate a significant potential application in electronics, and they are studied usually in two ways. One is to constantly explore new experimental phenomena and physical problems in existing topological materials, and the other is to predict and discover new topological material systems and carry out synthesis for further studies. In a word, high-quality crystals are very important for studying quantum oscillations, angle resolved photoemission spectra or scanning tunneling microscopy. In this work, the classifications and developments of topological materials, including topological insulators, topological semimetals, and magnetic topological materials, are introduced. As usually employed growth methods in growing topological materials, flux and vapour transport methods are introduced in detail. Other growth methods, such as Bridgman, float-zone, vapour deposition and molecular beam epitaxy methods, are also briefly mentioned. Then the details about the crystal growth of some typical topological materials, including topological insulators/semimetals, high Chern number chiral topological semimetals and magnetic topological materials, are elaborated. Meanwhile, the identification of crystal quality is also briefly introduced, including the analysis of crystal composition and structure, which are greatly important.

Single crystal growth of topological semimetals and magnetic topological materials

Topological materials have attracted much attention due to their novel physical properties. These materials can not only serve as a platform for studying the fundamental physics, but also demonstrate a significant potential application in electronics, and they are studied usually in two ways. One is to constantly explore new experimental phenomena and physical problems in existing topological materials, and the other is to predict and discover new topological material systems and carry out synthesis. In a word, high-quality crystals are very important for studying quantum oscillations, angle resolved photoemission spectra or scanning tunneling microscopy. In this work, the classifications and developments of topological materials, including topological insulators, topological semimetals, and magnetic topological materials, are introduced. As usually employed growth methods in growing topological materials, flux and vapour transport methods are introduced in detail. Other growth methods, such as Bridgman, float-zone, vapour deposition and molecular beam epitaxy methods, are also briefly mentioned. Then the details about the crystal growth of some typical topological materials, including topological insulators/semimetals, high Chern number chiral topological semimetals and magnetic topological materials, are elaborated. Meanwhile, the identification of crystal quality is also briefly introduced, including the analysis of crystal composition and structure, which are greatly important.

Fourier-based methods for removing mesh anomalies from angle resolved photoemission spectra

Recent improvements to spatial resolution in angle-resolved photo-emission spectroscopy (ARPES) have made it common to perform measurements with a very brief dwell time, for the purpose of mapping the spectral function over large surface regions. However, rapid measurement modalities can suffer a grid-like intensity modulation due to a wire mesh that is typically placed in front of the ARPES detector to block stray electrons. Here, we explore Fourier-based methods that can effectively remove this artifact, and improve the quality of ARPES images obtained in rapid scanning modes. An open source software package is provided containing implementations of demonstrated algorithms.

Vibrationally resolved photoemissions of N2 (C3Πu → B3Πg) and CO (b3Σ+ → a3Π) by low-energy electron impacts

Vibrationally resolved photoemission spectra of the electronic-state transitions C3Πu → B3Πg of N2 and b3Σ+ → a3Π of CO following low-energy electron impacts are measured with a crossed-beam experimental arrangement. The absolute cross sections of C3Πu (ν') → B3Πg (ν″) of N2 are presented for the vibrational state-to-state transitions (ν',ν″) = (0,0), (0,1), (1,0), (1,2), and (2,1). The excitation cross sections of the metastable state C3Πu of N2 show the maxima at the electron-impact energies 14.10 (ν' = 0) eV and 14.50 (ν' = 1) eV, which are potentially related to the core-excited vibrational Feshbach resonant state 2Σu + of N2 - formed by electron attachment. The absolute cross sections of b3Σ+ (ν' = 0) → a3Π (ν″ = 0, 1, 2, 3, 4) of CO are given by the calibrations with those of N2 measured in this work. Besides the maximum excitation cross section 5.85 × 10-18 cm2 at 10.74 eV of the CO b3Σ+ (ν' = 0) state, some fine structures on the excitation function profile are attributed to different shapes and Feshbach resonant states of CO- formed by electron attachment, while the others arise from the direct electron-impact excitation. Some discrepancies, particularly for N2, between the present data and the results available in the literature studies arise from different experimental techniques and data-processing procedures. Furthermore, contributions of physical processes such as wave-packet evolution and non-Franck-Condon dynamics are highlighted here.

Prominent Cooper pairing away from the Fermi level and its spectroscopic signature in twisted bilayer graphene

We investigate phonon-mediated Cooper pairing in flat electronic band systems by solving the full-bandwidth multiband Eliashberg equations for superconductivity in magic angle twisted bilayer graphene using a realistic tight-binding model. We find that Cooper pairing away from the Fermi level contributes decisively to superconductivity by enhancing the critical temperature and ensures a robust finite superfluid density. We show that this pairing yields particle-hole asymmetric superconducting domes in the temperature-gating phase diagram and gives rise to distinct spectroscopic signatures in the superconducting state. We predict several such features in tunneling and angle resolved photoemission spectra for future experiments.

Coherent excitonic quantum beats in time-resolved photoemission measurements

Coherent excitation of materials via ultrafast laser pulses can have interesting, observable dynamics in time-resolved photoemission measurements. The broad spectral width of ultrafast pump pulses can coherently excite multiple exciton energy levels. When such coherently excited states are probed by means of photoemission spectroscopy, interference between the polarization of different exciton levels can lead to observable coherent exciton beats. Here, we present the theoretical formalism for evaluating the Time- and Angle- Resolved Photoemission Spectra (tr-ARPES) arising from the coherently excited exciton states. We subsequently apply our formalism to a simple model example of hydrogenic exciton energy levels to identify the dependencies that control the quantum beats. Our findings indicate that the most pronounced effect of coherent quantum excitonic beats is seen midway between the excited exciton energy levels and the central energy of the pump pulse provides tunability of this effect.

Influence of the multiplet structure on the photoemission spectra of spin-orbit driven Mott insulators: Application to Sr2IrO4

Most of the low-energy effective descriptions of spin-orbit driven Mott insulators consider spin orbit coupling (SOC) as a second order perturbation to electron-electron interactions. However, when SOC is comparable to anisotropic Hund's coupling, such as in Ir, validity of this formally weak-SOC approach is not a priori known. Depending on the relative strength of SOC and anisotropic Hund's coupling, different descriptions of the multiplet structure should be employed in the weak and strong SOC limits, \textit{viz.} \textit{LS} and \textit{jj} coupling schemes, respectively. We investigate the implications of both the coupling schemes on the low-energy effective $t-J$ model and calculate the angle resolved photoemission (ARPES) spectra using self-consistent Born approximation. In particular, we obtain the ARPES spectra of quasi-two-dimensional square-lattice iridate ${\rm Sr_2IrO_4}$ in both weak and strong SOC limits. The differences in the limiting cases are understood in terms of the composition and relative energy splittings of the multiplet structure. Our results indicate that the LS coupling scheme yields better agreement with the experiment, thus providing an indirect evidence for the validity of LS coupling scheme for iridates. We also discuss the implications for other metal ions with strong SOC.

Epitaxial Growth of Honeycomb Monolayer CuSe with Dirac Nodal Line Fermions.

2D transition metal chalcogenides have attracted tremendous attention due to their novel properties and potential applications. Although 2D transition metal dichalcogenides are easily fabricated due to their layer-stacked bulk phase, 2D transition metal monochalcogenides are difficult to obtain. Recently, a single atomic layer transition metal monochalcogenide (CuSe) with an intrinsic pattern of nanoscale triangular holes is fabricated on Cu(111). The first-principles calculations show that free-standing monolayer CuSe with holes is not stable, while hole-free CuSe is endowed with the Dirac nodal line fermion (DNLF), protected by mirror reflection symmetry. This very rare DNLF state is evidenced by topologically nontrivial edge states situated inside the spin-orbit coupling gaps. Motivated by the promising properties of hole-free honeycomb CuSe, monolayer CuSe is fabricated on Cu(111) surfaces by molecular beam epitaxy and confirmed success with high resolution scanning tunneling microscopy. The good agreement of angle resolved photoemission spectra with the calculated band structures of CuSe/Cu(111) demonstrates that the sample is monolayer CuSe with a honeycomb lattice. These results suggest that the honeycomb monolayer transition metal monochalcogenide can be a new platform to study 2D DNLFs.

Angle resolved Photoemission from Ag and Au single crystals: Final state lifetimes in the attosecond range

We present angle resolved photoemission spectra for Ag(111) and Au(111) single crystals in normal emission geometry, taken at closely spaced intervals for photon energies between 8eV and 160eV. The most dominant transitions observed are attributed to f-derived final states located about 16–17eV above EF for both materials. These transitions exhibit very distinct resonance phenomena and selection rules and are reminiscent of the angular momentum characteristics of the states involved. The excited electron lifetime is in the attosecond (as) range as determined from the energy width of the observed transitions. This serves as an alternate approach to the direct determination of excited electron lifetimes by as laser spectroscopy.

Spin galvanic effect at the conducting SrTiO3 surfaces

The (001) surface of SrTiO3 were transformed from insulating to conducting after Ar+ irradiation, producing a quasi two-dimensional electron gas (2DEG). This conducting surface layer can introduce Rashba spin orbital coupling due to the broken inversion symmetry normal to the plane. The spin splitting of such a surface has recently been demonstrated by magneto-resistance and angular resolved photoemission spectra measurements. Here, we present experiments evidencing a large spin-charge conversion at the conducting surface. We use spin pumping to inject a spin current from NiFe film into the surface, and measure the resulting charge current. The results indicate that the Rashba effect at the surface can be used for efficient charge-spin conversion. The conversion efficiency measured by the ratio of the spin flow density to the charge flow density is about 0.23 nm. This value is on the same order as the interfaces in metallic multilayers and 2DEG of LaAlO3/SrTiO3. In this point of view, the conducting SrTiO3 surface provides another solution for oxide spintronics.

Splitting of the Ti-3d bands of TiSe2 in the charge-density wave phase

Very high resolution angular resolved photoemission (ARPES) spectra on TiSe2 in two distinct polarization geometries (vertical and horizontal) at temperatures between 300K and 22K enabled the observation of details of bands near the Fermi level not reported so far. Calculations of the electronic band structure based on density functional theory (DFT) using B3LYP hybrid functional and MBJ potential (with and without spin-orbit coupling) were performed to obtain the orbital symmetry and dispersion. Two degenerate conduction bands (CB’s) were observed at the Γ-point, a weak CB- emission at the A-point, and two non degenerate CB’s (i.e. splitting of CB) at the M/L-point of the Brillouin Zone (BZ). The splitting was detected at L for both polarizations, while at M remarkably only for horizontal polarization. These results cannot be fully accounted for by current theories for the charge density wave (CDW) and point to a reduced symmetry of the electronic states, possibly due to the chiral CDW.

Anomalous transport near the Lifshitz transition at theLaAlO3/SrTiO3interface

The two-dimensional electron liquid, at the (001) interface between band insulators {L}a{A}l{O}$_3$ and {S}r{T}i{O}$_3$, undergoes Lifshitz transition as the interface is doped with carriers. At a critical carrier density, two new orbitals populate at the Fermi level, with a concomitant change in the Fermi surface topology. Using dynamical mean-field theory, formulated within a realistic three-orbital model, we study the influence of the Lifshitz transition and local electron correlations on the transport properties. We look at the thermal conductivity, optical conductivity, Seebeck coefficient and angle resolved photoemission spectra and find that at a critical density, both the thermal and dc conductivities rise sharply to higher values while the Seebeck coefficient shows a cusp. The inter-orbital electron-electron interaction transfers spectral weight near the $\Gamma$ point towards lower energy, thereby reducing the critical density. In the presence of external magnetic field, the critical density further reduces due to exchange splitting. Beyond a sufficiently large field, multiple cusps appear in the Seebeck coefficient revealing multiple Lifshitz transitions.

Three-dimensional electronic structures and the metal-insulator transition in Ruddlesden-Popper iridates

In this study, we systematically investigate 3D momentum($\hbar k$)-resolved electronic structures of Ruddlesden-Popper-type iridium oxides Sr$_{n+1}$Ir$_n$O$_{3n+1}$ using soft-x-ray (SX) angle-resolved photoemission spectroscopy (ARPES). Our results provide direct evidence of an insulator-to-metal transition that occurs upon increasing the dimensionality of the IrO$_2$-plane structure. This transition occurs when the spin-orbit-coupled $j_{\rm eff}$=1/2 band changes its behavior in the dispersion relation and moves across the Fermi energy. In addition, an emerging band along the $\Gamma$(0,0,0)-R($\pi$,$\pi$,$\pi$) direction is found to play a crucial role in the metallic characteristics of SrIrO$_3$. By scanning the photon energy over 350 eV, we reveal the 3D Fermi surface in SrIrO$_3$ and $k_z$-dependent oscillations of photoelectron intensity in Sr$_3$Ir$_2$O$_7$. In contrast to previously reported results obtained using low-energy photons, folded bands derived from lattice distortions and/or magnetic ordering make significantly weak (but finite) contributions to the $k$-resolved photoemission spectrum. At the first glance, this leads to the ambiguous result that the observed $k$-space topology is consistent with the unfolded Brillouin zone (BZ) picture derived from a non-realistic simple square or cubic Ir lattice. Through careful analysis, we determine that a superposition of the folded and unfolded band structures has been observed in the ARPES spectra obtained using photons in both ultraviolet and SX regions. To corroborate the physics deduced using low-energy ARPES studies, we propose to utilize SX-ARPES as a powerful complementary technique, as this method surveys more than one whole BZ and provides a panoramic view of electronic structures.

Thermal and Chemical Stability of n-Hexadecanethiol Monolayers on Au(111) in O2 Environments

Understanding the mechanisms of degradation of self-assembled monolayers (SAM) is required for their use in molecular devices and in general in long term applications. In this context, we investigated the thermal and chemical stability of n-hexadecanethiolate (C16T) monolayers on Au(111) exposed to O2. The degradation of the monolayers was followed by electrochemical (EC) techniques, surface enhancement Raman spectroscopy (SERS) and high resolution photoemission spectra (HR-XPS). The C16T monolayers were heated both under N2 and O2 flux up to 480K for different times. The degradation of the SAM in the presence of O2 is characterized by the appearance of oxidized sulfur species and sulfur atoms on the surface. The formation time in the dipping solution also affects the thermal stability of the monolayer. Molecular dynamics (MD) simulations and density functional theory (DFT) calculations were performed to elucidate the possible degradation mechanisms. MD shows that O2 molecules easily penetrate the monolayer reaching the Au surface. The DFT calculations identified two oxidation mechanisms which involve the S atom and the alpha carbon of the alkylthiolate. Both mechanisms are very exothermic. The oxidation of the sulfur atom produces a sulfinate which does not alter the monolayer structure. On the contrary, the oxidation of the alpha carbon induces the breakage of the SC bond, the adsorption of atomic S and the desorption of the alkyl chain as an aldehyde.

Time-resolved photoemission ofSr2IrO4

We investigate the temporal evolution of electronic states in strontium iridate Sr$_2$IrO$_4$. The time resolved photoemission spectra of intrinsic, electron doped and the hole doped samples are monitored in identical experimental conditions. Our data on intrinsic and electron doped samples, show that primary doublon-holon pairs relax near to the chemical potential on a timescale shorter than $70$ fs. The subsequent cooling of low energy excitations takes place in two step: a rapid dynamics of $\cong120$ fs is followed by a slower decay of $\cong 1$ ps. The reported timescales endorse the analogies between Sr$_2$IrO$_4$ and copper oxides.

Angle resolved photoemission from Cu single crystals: Known facts and a few surprises about the photoemission process

We present angle resolved photoemission spectra for Cu(100) and Cu(111) singly crystals in normal emission geometry, taken at tightly spaced intervals for photon energies between 8eV and 150eV. This systematic collection of spectra gives unprecedented insight into the influence of the final states to the photoemission process as well as the band structure and lifetimes of highly excited electrons in Cu.

Dot-bound and dispersive states in graphene quantum dot superlattices

We consider a square lattice configuration of circular gate-defined quantum dots in an unbiased graphene sheet and calculate the electronic, particularly spectral properties of finite albeit actual sample sized systems by means of a numerically exact kernel polynomial expansion technique. Analyzing the local density of states and the momentum resolved photoemission spectrum we find clear evidence for a series of quasi-bound states at the dots, which can be probed by optical measurements. We further analyze the interplay of the superlattice structure with dot localized modes on the electron energy dispersion. Effects of disordered dot lattices are discussed too.

Theory of extreme correlations using canonical Fermions and path integrals

The t–J model is studied using a novel and rigorous mapping of the Gutzwiller projected electrons, in terms of canonical electrons. The mapping has considerable similarity to the Dyson–Maleev transformation relating spin operators to canonical Bosons. This representation gives rise to a non Hermitian quantum theory, characterized by minimal redundancies. A path integral representation of the canonical theory is given. Using it, the salient results of the extremely correlated Fermi liquid (ECFL) theory, including the previously found Schwinger equations of motion, are easily rederived. Further, a transparent physical interpretation of the previously introduced auxiliary Greens function and the ‘caparison factor’, is obtained.The low energy electron spectral function in this theory, with a strong intrinsic asymmetry, is summarized in terms of a few expansion coefficients. These include an important emergent energy scale Δ0 that shrinks to zero on approaching the insulating state, thereby making it difficult to access the underlying very low energy Fermi liquid behavior. The scaled low frequency ECFL spectral function, related simply to the Fano line shape, has a peculiar energy dependence unlike that of a Lorentzian. The resulting energy dispersion obtained by maximization is a hybrid of a massive and a massless Dirac spectrum EQ∗∼γQ−Γ02+Q2, where the vanishing of Q, a momentum type variable, locates the kink minimum. Therefore the quasiparticle velocity interpolates between (γ∓1) over a width Γ0 on the two sides of Q=0, implying a kink there that strongly resembles a prominent low energy feature seen in angle resolved photoemission spectra (ARPES) of cuprate materials. We also propose novel ways of analyzing the ARPES data to isolate the predicted asymmetry between particle and hole excitations.

Hidden Quasiparticles and Incoherent Photoemission Spectra inNa2IrO3

We study two Kitaev-Heisenberg t-J-like models on a honeycomb lattice, focusing on the zigzag magnetic phase of Na(2)IrO(3), and investigate hole motion by exact diagonalization and variational methods. The spectral functions are quite distinct from those of cuprates and are dominated by large incoherent spectral weight at high energy, almost independent of the microscopic parameters-a universal and generic feature for zigzag magnetic correlations. We explain why quasiparticles at low energy are strongly suppressed in the photoemission spectra and determine an analog of a pseudogap. We point out that the qualitative features of the predominantly incoherent spectra obtained within the two different models for the zigzag phase are similar, and they have a remarkable similarity to recently reported angular resolved photoemission spectra for Na(2)IrO(3).