Angular Resolved Photoemission Research Articles

Closing in on possible scenarios for infinite-layer nickelates: Comparison of dynamical mean-field theory with angular-resolved photoemission spectroscopy

Conflicting theoretical scenarios for infinite-layer nickelate superconductors have been hotly debated, particularly regarding whether only a single Ni-3dx2−y2 band is relevant at low energies besides electron pockets or whether multiorbital physics including Ni-3dz2 is instead essential. The first scenario has emerged from density-functional theory plus dynamical mean-field theory (DFT + DMFT) calculations. Comparing the previous DFT + DMFT spectra to recent angular-resolved photoemission spectroscopy (ARPES) experiments, we find excellent agreement for both the Fermi surface and the strongly renormalized quasiparticle bands, supporting the first scenario. Our key findings further suggest that the “waterfalls” observed in ARPES might emerge from the quasiparticle-to-Hubbard-band crossover, and that additional spectral weight close to the A pocket likely originates from the Ni-3dxy orbital. Published by the American Physical Society 2024

Direct observation of altermagnetic band splitting in CrSb thin films

Altermagnetism represents an emergent collinear magnetic phase with compensated order and an unconventional alternating even-parity wave spin order in the non-relativistic band structure. We investigate directly this unconventional band splitting near the Fermi energy through spin-integrated soft X-ray angular resolved photoemission spectroscopy. The experimentally obtained angle-dependent photoemission intensity, acquired from epitaxial thin films of the predicted altermagnet CrSb, demonstrates robust agreement with the corresponding band structure calculations. In particular, we observe the distinctive splitting of an electronic band on a low-symmetry path in the Brilliouin zone that connects two points featuring symmetry-induced degeneracy. The measured large magnitude of the spin splitting of approximately 0.6 eV and the position of the band just below the Fermi energy underscores the significance of altermagnets for spintronics based on robust broken time reversal symmetry responses arising from exchange energy scales, akin to ferromagnets, while remaining insensitive to external magnetic fields and possessing THz dynamics, akin to antiferromagnets.

Finite-Temperature Hole-Magnon Dynamics in an Antiferromagnet.

Employing the numerically accurate multiple Davydov Ansatz in combination with the thermo-field dynamics approach, we delve into the interplay of the finite-temperature dynamics of holes and magnons in an antiferromagnet, which allows for scrutinizing previous predictions from the self-consistent Born approximation while offering, for the first time, accurate finite-temperature computation of detailed magnon dynamics as a response and a facilitator to the hole motion. The study also uncovers a pronounced temperature dependence of the magnon and hole populations, pointing to the feasibility of potential thermal manipulation and control of hole dynamics. Our methodology can be applied not only to the calculation of steady-state angular-resolved photoemission spectra but also to the simulation of femtosecond terahertz pump-probe and other nonlinear signals for the characterization of antiferromagnetic materials.

Temperature dependent ARPES of the metallic-like bands in Si(553)-Au

We conducted a thorough investigation into the temperature dependence of the metallic-like bands of Si(553)-Au using angular-resolved photoemission spectroscopy (ARPES). Our study addresses the challenges posed by the short-term stability of the surface and photo-voltage effects, which we overcame to extract changes in the band-filling and Fermi-velocity. Our findings shed light on the low-temperature phase of the step edge in Si(553)-Au, which has been a topic of ongoing debate regarding its structural or electronic nature. Through comparison with theoretical predictions of a structural-related low-temperature to high-temperature phase transition, we discovered that the band-filling and Fermi-velocity do not change accordingly, thereby ruling out this scenario. Our study contributes to a better understanding of this material system and provides an important reference for future research.

Spectrum of the Hole Excitation in Spin-Orbit Mott Insulator Na2IrO3

We study the motion of a hole with internal degrees of freedom, introduced to the zigzag magnetic ground state of Na2IrO3, by using the self-consistent Born approximation. We find that the low-, intermediate-, and high-energy spectra are primarily attributed to the singlet, triplet, and quintet hole contributions, respectively. The spectral functions exhibit distinct features such as the electron-like dispersion of low-energy states near the Γ point, the maximum M-point intensity of mid-energy states, and the hole-like dispersion of high-energy states. These features are robust and almost insensitive to the exchange model and Hund’s coupling, and are in qualitative agreement with the angular-resolved photoemission spectra observed in Na2IrO3. Our results reveal that the interference between internal degrees of freedom in different sublattices plays an important role in inducing the complex dispersions.

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.

Importance of accurately measuring LDOS maps using scanning tunneling spectroscopy in materials presenting atom-dependent charge order: The case of the correlated Pb/Si(111) single atomic layer

We address here general issues and show how to properly extract the local charge order in two-dimensional systems from scanning tunneling microscopy/spectroscopy (STM/STS) measurements. When the charge order presents spatial variations at the atomic scale inside the unit cell and is energy dependent, particular care should be taken. We show that the widely used lock-in technique performed while acquiring an STM topography in a closed feedback loop cannot be used to extract this local charge order from STS $dI/dV$ differential conductance maps. In such situations, the use of the lock-in technique leads to systematically incorrect $dI/dV$ measurements, giving a false local charge order. We show that a correct method is either to perform a constant height measurement or to perform a full grid of $dI/dV(V)$ spectroscopies, using a set point for the bias voltage outside the bandwidth of the correlated material where the local density of states (LDOS) is expected to be spatially homogeneous. We take as a paradigmatic example of two-dimensional material the 1/3 single-layer Pb/Si(111) phase. As large areas of this phase cannot be grown, charge ordering in this system is not accessible to angular resolved photoemission or grazing x-ray diffraction. Two previous investigations by STM/STS supplemented by ab initio density functional theory (DFT) calculations concluded that this material undergoes a phase transition to a low-temperature $3\ifmmode\times\else\texttimes\fi{}3$ reconstruction where one Pb atom moves up, the two remaining Pb atoms shifting down. A third STM/STS study by Adler et al. [F. Adler, S. Rachel, M. Laubach, J. Maklar, A. Fleszar, J. Sch\"afer, and R. Claessen, Phys. Rev. Lett. 123, 086401 (2019)] came to the opposite conclusion, i.e., that two Pb atoms move up, while one Pb atom shifts down. We show that this latter erroneous conclusion comes from an artifact induced by the lock-in technique. In contrast, using a full grid of $dI/dV$($V$) spectroscopy measurements, our results show that the energy-dependent LDOS maps agree very well with state-of-the-art DFT calculations, confirming the one-up two-down charge ordering. We show that this structural and charge reordering inside the $3\ifmmode\times\else\texttimes\fi{}3$ unit cell is equally driven by electron-electron interactions and the coupling to the substrate.

Influence of Orbital Character on the Ground State Electronic Properties in the van Der Waals Transition Metal Iodides VI3 and CrI3.

Two-dimensional van der Waals magnetic semiconductors display emergent chemical and physical properties and hold promise for novel optical, electronic and magnetic “few-layers” functionalities. Transition-metal iodides such as CrI3 and VI3 are relevant for future electronic and spintronic applications; however, detailed experimental information on their ground state electronic properties is lacking often due to their challenging chemical environment. By combining X-ray electron spectroscopies and first-principles calculations, we report a complete determination of CrI3 and VI3 electronic ground states. We show that the transition metal-induced orbital filling drives the stabilization of distinct electronic phases: a wide bandgap in CrI3 and a Mott insulating state in VI3. Comparison of surface-sensitive (angular-resolved photoemission spectroscopy) and bulk-sensitive (X-ray absorption spectroscopy) measurements in VI3 reveals a surface-only V2+ oxidation state, suggesting that ground state electronic properties are strongly influenced by dimensionality effects. Our results have direct implications in band engineering and layer-dependent properties of two-dimensional systems.

Ultrafast Spin‐Charge Conversion at SnBi2Te4/Co Topological Insulator Interfaces Probed by Terahertz Emission Spectroscopy

AbstractSpin‐to‐charge conversion (SCC) involving topological surface states (TSS) is one of the most promising routes for highly efficient spintronic devices for terahertz (THz) emission. Here, the THz generation generally occurs mainly via SCC consisting in efficient dynamical spin injection into spin‐locked TSS. In this work, sizable THz emission from a nanometric thick topological insulator (TI)/ferromagnetic junction—SnBi2Te4/Co—specifically designed to avoid bulk band crossing with the TSS at the Fermi level, unlike its parent material Bi2Te3 is demonstrated. THz emission time domain spectroscopy (TDS) is used to indicate the TSS contribution to the SCC by investigating the TI thickness and angular dependence of the THz emission. This work illustrates THz emission TDS as a powerful tool alongside angular resolved photoemission spectroscopy (ARPES) methods to investigate the interfacial spintronic properties of TI/ferromagnet bilayers.

Time-resolved photoemission spectroscopy on correlated electrons: Insights from dynamical mean-field theory

Time- and angular-resolved photoemission spectroscopy (trARPES) can directly probe the electronic structure of quantum materials out of equilibrium. This can shed light on the interaction of the electrons with spin, lattice, and orbital degrees of freedom, and help to unravel pathways towards novel out-of-equilibrium phases. Dynamical mean-field theory (DMFT) and its extensions provide a versatile toolbox to interpret such experiments through a theoretical simulation of the underlying microscopic processes. The approach can be applied both to Mott insulators and correlated metals, and it is formulated in terms of non-equilibrium Green's functions, which directly relate to the photoemission spectrum. This article reviews the theoretical description of trARPES within DMFT and related diagrammatic non-equilibrium Green's function techniques. Several applications are discussed, including the photo-induced melting of excitonic order, femtosecond relaxation processes in Mott insulators, and the manipulation of the electronic structure of Mott and charge transfer insulators using photo-doping and strong THz fields.

Transport properties of the parent LaNiO$$_2$$

Here, we study the transport properties of a nickelate compound, namely LaNiO $$_2$$ using density functional theory (DFT) in conjunction with dynamical mean field theory (DMFT). An interacting multi-orbital spin-resolved scenario for LaNiO $$_2$$ yields a metallic ground state with ferromagnetic correlations. The latter contrasts an antiferromagnetic order reported earlier. The metallic behaviour persists even at large values of the interaction energies. Further support of the metallic state is provided by the angular resolved photoemission spectroscopy (ARPES) data.

Massive Dirac fermions and strong Shubnikov–de Haas oscillations in single crystals of the topological insulator Bi2Se3 doped with Sm and Fe

Topological insulators (TIs) are emergent materials with unique band structure, which allow the study of quantum effect in solids, as well as contribute to high-performance quantum devices. To achieve the better performance of TIs, here, we present a codoping strategy using synergistic rare-earth (RE) Sm and transition-metal Fe dopants in ${\mathrm{Bi}}_{2}{\mathrm{Se}}_{3}$ single crystals, which combine the advantages of both a transition-metal-doped TI [high ferromagnetic ordering temperature and observed quantum anomalous Hall effect (QAHE)], and a RE doped TI (large magnetic moments and significant spin-orbit coupling). In the as-grown single crystals, clear evidences of ferromagnetic ordering were observed. The angle-resolve photoemission spectroscopy indicates the ferromagnetism opens a \ensuremath{\sim}44 meV band gap at the surface Dirac point. Moreover, the mobility of the carriers at 3 K is $\ensuremath{\sim}7400\phantom{\rule{0.16em}{0ex}}\mathrm{c}{\mathrm{m}}^{2}/\mathrm{Vs}$, and we thus observed an ultra-strong Shubnikov--de Haas oscillation in the longitudinal resistivity, as well as the Hall steps in transverse resistivity 14 T. Our transport and angular-resolved photoemission spectroscopy results suggest that the RE and transition metal codoping in the ${\mathrm{Bi}}_{2}{\mathrm{Se}}_{3}$ system is a promising avenue to implement the QAHE, as well as harnessing the massive Dirac fermion in electrical devices.

Studying the heterogeneity of the CrxTi1-xCh2 (Ch = S, Se) single crystals using X-ray scanning photoemission microscopy

The morphology of the heterogeneous CrxTi1-xSe2 and CrxTi1-xS2 single crystals has been studied using X-ray scanning photoemission microscopy (SPEM) and angular resolved photoemission spectroscopy (ARPES). A direct method of SPEM provided us the insight into the origin of the blurred ARPES images for Cr0.78Ti0.36Se2 single crystal. Using SPEM, we confirmed the formation of the CrSe2-based structural fragments inside the CrxTi1-xSe2 single crystals with x ≥ 0.75. The chemical composition of the forming structural fragments depends on the chalcogen (S, Se) forming the crystal lattice.

Pump-probe photoemission simulated in real time: Revealing many-particle signatures

We simulate the photoemission from an electronically excited system by computing the escape of electron density in real space using time-dependent density functional theory in real time. We show that for a one-electron system, the angular resolved photoemission after an initial excitation can be interpreted as the mapping of a previously unoccupied orbital. For the molecule perylene-3,4,9,10-tetracarboxylic dianhydride, the angular resolved photoemission (ARPES) calculated after a preceding pump pulse reveals signatures of the many-particle character of the first electronic excitation: The photoemission results from more than one time-dependent orbital, and comparing the ARPES pattern to a particle-hole analysis of the first electronic excitation confirms that the excitation does not just correspond to one electron having been moved into a previously empty orbital, but is a superposition of several single-particle excitations.

Measuring spin-polarized electronic states of quantum materials: 2H−NbSe2

Probing the energy and spin electron properties of materials by means of photoemission spectroscopy gives insights into the low-energy phenomena of matter driven by spin orbit coupling or exchange interaction. The information that can be derived from complete photoelectron spectroscopy experiments, beyond $E$(k), is contained in the photoemission transition matrix elements that determine peak intensities. We present here a complete photoemission study of the spin-polarized bands of $2H\text{\ensuremath{-}}{\mathrm{NbSe}}_{2}$, a material that presents a surface spin-texture. Circular dichroism in angular-resolved photoemission spectroscopy (CD-ARPES) data are compared with spin-polarized angular-resolved spectra (SARPES) as measured with linearly polarized radiation in a well-characterized experimental chirality, at selected photon energy values. CD-ARPES is due to a matrix element effect that depends strongly on photon energy and experimental geometry: we show that it cannot be used to infer intrinsic spin properties in $2H\text{\ensuremath{-}}{\mathrm{NbSe}}_{2}$. On the other hand, SARPES data provide reliable direct information on the spin properties of the electron states. The results on $2H\text{\ensuremath{-}}{\mathrm{NbSe}}_{2}$ are discussed, and general methodological conclusions are drawn on the best experimental approach to the determination of the spin texture of quantum materials.

Cascade of replica bands in flat-band systems: Predictions for twisted bilayer graphene

We investigate the effect of electron-phonon interactions (EPI) in systems exhibiting one or more flat electron bands close to the Fermi level and a comparatively large phonon energy scale. After solving the self-consistent full-bandwidth Eliashberg equations, we compute Angular Resolved Photo Emission Spectroscopy and Scanning Tunneling Spectroscopy/Microscopy spectra. We obtain a sequence of quasiparticle replica bands in both the normal and superconducting states that originate from frequency dependent features of the electron mass renormalization function. We show that these replica bands can be used to extract the relevant phonon energy scale from experiments. Focusing in particular on twisted bilayer graphene, we predict replica-band formation which, when observed, will shed light on the role of EPI in this archetypal flat-band system.

Spatial locality of electronic correlations in LiFeAs

We address the question of the degree of spatial non-locality of the self energy in the iron-based superconductors, a subject which is receiving considerable attention. Using LiFeAs as a prototypical example, we extract the self energy from angular-resolved photoemission spectroscopy (ARPES) data. We use two distinct electronic structure references: density functional theory in the local density approximation and linearized quasiparticle self consistent GW (LQSGW). We find that with the LQSGW reference, spatially local dynamical correlations provide a consistent description of the experimental data, and account for some surprising aspects of the data such as the substantial out of plan dispersion of the electron Fermi surface having dominant xz/yz character. Hence, correlations effects can be separated into static non-local contributions well described by LQSGW and dynamical local contributions. Hall effect and resistivity data are shown to be consistent with this description.

Band structure tuning of Heusler compounds: Spin- and momentum-resolved electronic structure analysis of compounds with different band filling

Half-metallic ferromagnetic Heusler compounds represent an important class of materials for spintronic applications. We experimentally observe the dispersion of electronic bands with spin resolution in three representative Heusler compounds (${\mathrm{Co}}_{2}\mathrm{MnGa}, {\mathrm{Co}}_{2}\mathrm{MnSi}$, and ${\mathrm{Co}}_{2}{\mathrm{Fe}}_{0.4}{\mathrm{Mn}}_{0.6}\mathrm{Si}$). Bulk-sensitive measurements at very low photon energy are complemented by spin-integrated hard x-ray angular resolved photoemission spectroscopy. The dispersion of majority and minority electrons allows us to link exchange splitting and band filling to the number of valence electrons ${N}_{v}$. Photoexcitation at $h\ensuremath{\nu}=6.05\phantom{\rule{0.16em}{0ex}}\mathrm{eV}$ gives access to the spin-polarization texture $\mathbit{P}({E}_{B},{k}_{x},{k}_{y})$ of the bulk bands covering a $({k}_{x},{k}_{y})$ range of 60% of the Brillouin zone. We find that ${\mathrm{Co}}_{2}\mathrm{MnSi}$ and ${\mathrm{Co}}_{2}{\mathrm{Fe}}_{0.4}{\mathrm{Mn}}_{0.6}\mathrm{Si}$ exhibit minority band gaps of 0.5 and 0.35 eV, i.e., decreasing band gap with increasing ${N}_{\mathrm{V}}$ in contrast to the rigid-band expectation. For ${\mathrm{Co}}_{2}\mathrm{MnGa}$, the minority valence state maximum lies at approx. 0.2 eV above ${E}_{\mathrm{F}}$.

Néel Vector Induced Manipulation of Valence States in the Collinear Antiferromagnet Mn2Au.

The coupling of real and momentum space is utilized to tailor electronic properties of the collinear metallic antiferromagnet Mn2Au by aligning the real space Néel vector indicating the direction of the staggered magnetization. Pulsed magnetic fields of 60 T were used to orient the sublattice magnetizations of capped epitaxial Mn2Au(001) thin films perpendicular to the applied field direction by a spin-flop transition. The electronic structure and its corresponding changes were investigated by angular-resolved photoemission spectroscopy with photon energies in the vacuum-ultraviolet, soft, and hard X-ray range. The results reveal an energetic rearrangement of conduction electrons propagating perpendicular to the Néel vector. They confirm previous predictions on the origin of the Néel spin-orbit torque and anisotropic magnetoresistance in Mn2Au and reflect the combined antiferromagnetic and spin-orbit interaction in this compound leading to inversion symmetry breaking.

Photoinduced metastable dd-exciton-driven metal-insulator transitions in quasi-one-dimensional transition metal oxides

Photoinduced phase transitions in matters have gained tremendous attention over the past few years. However, their ultrashort lifetime makes their study and possible control very challenging. Here, we report on highly anisotropic d-d excitonic excitations yielding photoinduced metal-insulator transitions (MITs) in quasi-one-dimensional metals Sr1-yNbOx using Mueller-Matrix spectroscopic ellipsometry, transient ultraviolet Raman spectroscopy, transient mid-infrared reflectivity and angular-resolved photoemission spectroscopy supported with density functional theory. Interestingly, the MITs are driven by photo-pumping of d-d excitons, causing the metallic a-axis to become insulating while the insulating b- and c-axis concomitantly become a correlated metal. We assign these effects to an interplay between the melting of charge and lattice orderings along the different anisotropic optical axes and Bose-Einstein-like condensation of the photoinduced excitons. The long lifetime in the order of several seconds of the metastable MITs gives greater flexibility to study and manipulate the transient excitonic state for potential applications in exciton-based optoelectronic devices.