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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Compositionally Complex Alloys: Some Insights from Photoemission Spectroscopy

Photoemission spectroscopy (PES) is an underrepresented part of current and past studies of compositionally complex alloys (CCA) such as high-entropy alloys (HEA) and their derivatives. PES studies are very important for understanding the electronic structure of materials, and are therefore essential in some cases for a correct description of the intrinsic properties of CCAs. Here, we present several examples showing the importance of PES. First, we show how the difference between the split-band structure and the common-band structure of the valence band (VB), observed by PES, can explain a range of properties of CCAs and alloys in general. A simple description of the band crossing in CCAs composed from the early and late transition metals showing a split band is discussed. We also demonstrate how a high-accuracy PES study can determine the variation in the density of states at the Fermi level as a function of Cu content in Ti-Zr-Nb-Ni-Cu metallic glasses. Finally, the first results of an attempt to single out the contributions of particular constituents in Cantor-type alloys to their VBs are presented. The basic principles of PES, the techniques employed in studies presented, and some issues associated with PES measurements are also described.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Development of deflector mode for spin-resolved time-of-flight photoemission spectroscopy

Spin- and angle-resolved photoemission spectroscopy (“spin-ARPES”) is a powerful technique for probing the spin degree-of-freedom in materials with nontrivial topology, magnetism, and strong correlations. Spin-ARPES faces severe experimental challenges compared to conventional ARPES attributed to the dramatically lower efficiency of its detection mechanism, making it crucial for instrumentation developments that improve the overall performance of the technique. Here in this paper, we demonstrate the functionality of our spin-ARPES setup based on time-of-flight spectroscopy and introduce our recent development of an electrostatic deflector mode to map out spin-resolved band structures without sample rotation. We demonstrate the functionality by presenting the spin-resolved spectra of the topological insulator Bi2Te3 and describe in detail the spectrum calibrations based on numerical simulations. By implementing the deflector mode, we minimize the need for sample rotation during measurements, hence improving the overall efficiency of experiments on small or inhomogeneous samples.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Tuning time and energy resolution in time-resolved photoemission spectroscopy with nonlinear crystals

Time- and angle-resolved photoemission spectroscopy is a powerful probe of electronic band structures out of equilibrium. Tuning time and energy resolution to suit a particular scientific question has become an increasingly important experimental consideration. Many instruments use cascaded frequency doubling in nonlinear crystals to generate the required ultraviolet probe pulses. In this work, we demonstrate how calculations clarify the relationship between laser bandwidth and nonlinear crystal thickness contributing to experimental resolutions and place intrinsic limits on the achievable time-bandwidth product. Experimentally, we tune time and energy resolution by varying the thickness of nonlinear β-BaB 2 O 4 crystals for frequency upconversion, providing a flexible experiment design. We achieve time resolutions of 58–103 fs and corresponding energy resolutions of 55–27 meV. We propose a method to select crystal thickness based on desired experimental resolutions.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Measuring the Debye energy in superconductors via two-electron photoemission spectroscopy

In this work, we demonstrate theoretically that double angle resolved photoemission spectroscopy (2eARPES) can directly probe the existence of Cooper pairs away from the Fermi surface, and can thus provide insight into the characteristic energy scale around the Fermi surface, the Debye energy, in which electrons are bound into Cooper pairs. To this end, we compute the photoelectron counting rate 𝑃 (2) in two different types of unconventional superconductors, a 𝑑 𝑥 2 −𝑦 2 -wave superconductor, and a topological superconductor with a broken time-reversal symmetry. We show that 𝑃 (2) provides insight into the relative strength of intra- and interband pairing in multiband systems, as well as into the spin polarization of the bands.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Ultraviolet Photoemission Spectroscopy and Kelvin Probe Measurements on Metal Halide Perovskites: Advantages and Pitfalls

In this essay, a case study is presented on the electronic structure of several metal halide perovskites (MHP) using Kelvin probe (KP)-based surface photovoltage (SPV) measurements and ultraviolet photoemission spectroscopy (UPS) to demonstrate the advantages, but also the pitfalls, of using these techniques to characterize the surfaces of these materials. The first part addresses the loss of halide species from perovskite surfaces upon supragap illumination in vacuum. This has the potential to cause both a long-term alteration of the sample work function and a modification of the KP tip during SPV measurements. If undetected, this leads to a misinterpretation of the MHP surface potential. The second part illustrates the difficulties in determining the valence band maximum (VBM) of MHP surfaces with UPS and stresses the importance of taking into account the low density of states at the VBM edge. Given this circumstance, specific care must be taken to eliminate measurement artifacts in order to ascertain the presence or absence of low densities of electronic gap states above the VBM. This essay also highlights issues such as film degradation, nonequilibrium situations (e.g., SPV), and satellite emissions, which occur during photoemission spectroscopy.

36 MATERIALS SCIENCE↗
DOE OSTI2023

magnetoARPES: Angle Resolved Photoemission Spectroscopy with magnetic field control

Angle-Resolved Photoemission Spectroscopy (ARPES) is a premier technique for understanding the electronic excitations in conductive, crystalline matter, in which the induced photocurrent is collected and dispersed in energy and angle of emission to reveal the energy- and momentum-dependent single particle spectral function A (k,ω). So far, ARPES in a magnetic field has been precluded due to the need to preserve the electron paths between the sample and detector. Here, in this paper we report progress towards “magnetoARPES”, a variant of ARPES that can be conducted in a magnetic field. It is achieved by applying a microscopic probe beam (≲10 μm) to a thinned sample mounted upon a special sample holder that generates magnetic field confined to a thin layer near the sample surface. In this geometry we could produce ARPES in magnetic fields up to around ±100 mT. The magnetic fields can be varied from purely in-plane to nearly purely out-of-plane, by scanning the probe beam across different parts of the device. We present experimental and simulated data for graphene to explore the aberrations induced by the magnetic field. These results demonstrate the viability of the magnetoARPES technique for exploring symmetry breaking effects in weak magnetic fields.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Electronic structure of non-centrosymmetric PtBi2 studied by angle-resolved photoemission spectroscopy

Using high-resolution angle-resolved photoemission spectroscopy (ARPES), we have systematically studied the electronic structure of non-centrosymmetric PtBi2 with a layered structure. Through photon energy dependent measurements, the surface state and the bulk state were identified. Consistent with the non-centrosymmetric structure, different surface states were observed on opposite PtBi2(001) surfaces. Experimental bulk bands agree nicely with first-principle calculations. By combining ARPES and calculations, energy bands that contribute to triply degenerate point fermion were all detected. We also suggest that there are “canted” tube-like Fermi surfaces that might cause strong anisotropy in electronic transportation in non-centrosymmetric PtBi2.

Jiang, Wenxiang (ORCID:000000020524259X)↗
DOE OSTI2022

Growth of PdCoO 2 films with controlled termination by molecular-beam epitaxy and determination of their electronic structure by angle-resolved photoemission spectroscopy

Utilizing the powerful combination of molecular-beam epitaxy (MBE) and angle-resolved photoemission spectroscopy (ARPES), we produce and study the effect of different terminating layers on the electronic structure of the metallic delafossite PdCoO 2 . Attempts to introduce unpaired electrons and synthesize new antiferromagnetic metals akin to the isostructural compound PdCrO 2 have been made by replacing cobalt with iron in PdCoO 2 films grown by MBE. Using ARPES, we observe similar bulk bands in these PdCoO 2 films with Pd-, CoO 2 -, and FeO 2 -termination. Nevertheless, Pd- and CoO 2 -terminated films show a reduced intensity of surface states. Additionally, we are able to epitaxially stabilize PdFe x Co 1– x O 2 films that show an anomaly in the derivative of the electrical resistance with respect to temperature at 20 K, but do not display pronounced magnetic order.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Unveiling the orbital texture of 1T-TiTe 2 using intrinsic linear dichroism in multidimensional photoemission spectroscopy

The momentum-dependent orbital character in crystalline solids, referred to as orbital texture, is of capital importance in the emergence of symmetry-broken collective phases, such as charge density waves as well as superconducting and topological states of matter. By performing extreme ultraviolet multidimensional angle-resolved photoemission spectroscopy for two different crystal orientations linked to each other by mirror symmetry, we isolate and identify the role of orbital texture in photoemission from the transition metal dichalcogenide 1T-TiTe 2 . By comparing our experimental results with theoretical calculations based on both a quantitative one-step model of photoemission and an intuitive tight-binding model, we unambiguously demonstrate the link between the momentum-dependent orbital orientation and the emergence of strong intrinsic linear dichroism in the photoelectron angular distributions. Our results represent an important step towards going beyond band structure (eigenvalues) mapping and learning about electronic wavefunction and orbital texture of solids by exploiting matrix element effects in photoemission spectroscopy.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Topography of Fermi arcs in 𝑡−PtBi 2 using high-resolution angle-resolved photoemission spectroscopy

Here, we use high-resolution angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) to investigate the electronic structure of trigonal phase PtBi 2 (𝑡 −PtBi 2 ), a proposed Weyl semimetal that is expected to exhibit topological Fermi arcs. Our ARPES data elucidates the topography of these objects and confirms their Fermi arc character. The arcs are formed by surface bands that have fairly flat bottoms located very close to the chemical potential ∼ 6–8 meV, before they merge with bulk bands at higher binding energy. Comparison of the ARPES data with DFT calculations shows good agreement about their location and topography. Data acquired at low temperatures does not show any signatures of superconductivity down to 3 K in terms of expected changes in dispersion due to formation of Bogoliubov quasiparticles or superconducting gap in the form of reliable shifts of peaks in energy distribution curves.

Fermi surface↗
DOE OSTI2021

Prospects for the expansion of standing wave ambient pressure photoemission spectroscopy to reactions at elevated temperatures

Standing wave ambient pressure photoemission spectroscopy (SWAPPS) is a promising method to investigate chemical and potential gradients across solid-vapor and solid-liquid interfaces under close-to-realistic environmental conditions, far away from high vacuum. Until now, these investigations have been performed only near room temperature, but for a wide range of interfacial processes, chief among them being heterogeneous catalysis, measurements at elevated temperatures are required. One concern in these investigations is the temperature stability of the multilayer mirrors, which generate the standing wave field. At elevated temperatures, degradation of the multilayer mirror due to, for example, interdiffusion between the adjacent layers, decreases the modulation of the standing wave field, thus rendering SWAPPS experiments much harder to perform. Here, we show that multilayer mirrors consisting of alternate B4C and W layers are stable at temperatures exceeding 600 °C and are, thus, promising candidates for future studies of surface and subsurface species in heterogeneous catalytic reactions using SWAPPS.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Paramagnetic electronic structure of CrSBr: Comparison between ab initio G W theory and angle-resolved photoemission spectroscopy

Here, we explore the electronic structure of paramagnetic CrSBr by comparative first-principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent GW theory, without and with the inclusion of excitonic vertex corrections to the screened Coulomb interaction (QS GW and QS $G\widehat{W}$, respectively). Comparing the quasiparticle band-structure calculations to angle-resolved photoemission data collected at 200 K results in excellent agreement. This allows us to qualitatively explain the significant broadening of some bands as arising from the broken magnetic long-range order and/or electronic dispersion perpendicular to the quasi-two-dimensional layers of the crystal structure. The experimental band gap at 200 K is found to be at least 1.51 eV at 200 K. At lower temperature, no photoemission data can be collected as a result of charging effects, pointing towards a significantly larger gap, which is consistent with the calculated band gap of approximately 2.1 eV.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Hourglass-type bulk Ni 3 d band and Ce 4 f Kondo resonance states in the potential topological Kondo semimetal CeNiSn via angle-resolved photoemission spectroscopy

The electronic structure of CeNiSn, which is a potential topological Kondo insulator and a Dirac nodal-loop semimetal, has been investigated by employing temperature (T) dependent angle-resolved photoemission spectroscopy (ARPES). The Fermi surfaces (FSs) and the band structures of CeNiSn for three orthogonal crystallographic planes are measured, in which both the very dispersive bands and the flat bands are observed, having mainly the Ni 3d character and the Ce 4f character, respectively. The measured FSs and ARPES bands agree reasonably well with the density functional theory (DFT) calculations. The Fermi-edge (E F ) photon energy (hν) map along k b (=k (010) ) shows that the metallic E F -crossing states on the (010) surface have the three-dimensional character, suggesting that the observed E F -crossing metallic states do not correspond to the topological surface states of the two-dimensional character. On the other hand, albeit weak, the features of the hourglass-type bulk band crossings are observed along SXS, with the energies and the slopes being similar to those predicted by the DFT calculations, supporting the Dirac semimetallic nature of CeNiSn. In T-dependent ARPES, the Ce 4f Kondo resonance states are clearly revealed at low T, which become much suppressed above ~80 K. This feature is consistent with the Kondo temperature of CeNiSn, estimated from its ρ(T) data. This work demonstrates the importance of the coherent Kondo states in determining the topological properties of CeNiSn.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Electronic structure of superconducting nickelates probed by resonant photoemission spectroscopy

We report the discovery of infinite-layer nickelate superconductors has spurred enormous interest. While the Ni 1+ cations possess nominally the same 3d 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 with density functional theory + U (on-site Coulomb repulsion energy) calculations, we estimate U ~5 eV, smaller than the charge transfer energy Δ ~8 eV, confirming the Mott-Hubbard electronic structure in contrast to charge-transfer cuprates. Near the Fermi level (E F ), we observe a signature of occupied rare-earth states in the parent compound, which is consistent with a self-doping picture. Our results demonstrate a correlation between the superconducting transition temperature and the oxygen 2p hybridization near E F when comparing hole-doped nickelates and cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Hybridization of Bogoliubov Quasiparticles between Adjacent CuO 2 Layers in the Triple-Layer Cuprate Bi 2 Sr 2 Ca 2 Cu 3 O 10 + δ Studied by Angle-Resolved Photoemission Spectroscopy

Hybridization of Bogoliubov quasiparticles (BQPs) between the CuO 2 layers in the triple-layer cuprate high-temperature superconductor Bi 2 Sr 2 Cu 2 Cu 3 O 10+δ is studied by angle-resolved photoemission spectroscopy (ARPES). In the superconducting state, an anticrossing gap opens between the outer- and inner-BQP bands, which we attribute primarily to interlayer single-particle hopping with possible contributions from interlayer Cooper pairing. We find that the d-wave superconducting gap of both BQP bands smoothly develops with momentum without an abrupt jump in contrast to a previous ARPES study. Hybridization between the BQPs also gradually increases in going from the off nodal to the antinodal region, which is explained by the momentum dependence of the interlayer single-particle hopping. As possible mechanisms for the enhancement of the superconducting transition temperature, the hybridization between the BQPs as well as the combination of phonon modes of the triple CuO 2 layers and spin fluctuations represented by a four-well model are discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Giant self-driven exciton-Floquet signatures in time-resolved photoemission spectroscopy of MoS 2 from time-dependent GW approach

Time-resolved, angle-resolved photoemission spectroscopy (TR-ARPES) is a one-particle spectroscopic technique that can probe excitons (two-particle excitations) in momentum space. We present an ab initio, time-domain GW approach to TR-ARPES and apply it to monolayer MoS 2 . We show that photoexcited excitons may be measured and quantified as satellite bands and lead to the renormalization of the quasiparticle bands. These features are explained in terms of an exciton-Floquet phenomenon induced by an exciton time–dependent bosonic field, which are orders of magnitude stronger than those of laser field–induced Floquet bands in low-dimensional semiconductors. Our findings imply a way to engineer Floquet matter through the coherent oscillation of excitons and open the new door for mechanisms for band structure engineering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Lattice and electronic structure of ScN observed by angle-resolved photoemission spectroscopy measurements

Scandium nitride (ScN) has recently attracted much attention for its potential applications in thermoelectric energy conversion, as a semiconductor in epitaxial metal/semiconductor superlattices, as a substrate for GaN growth, and alloying it with AlN for 5G technology. This study was undertaken to better understand its stoichiometry and electronic structure. ScN (100) single crystals 2 mm thick were grown on a single crystal tungsten (100) substrate by a physical vapor transport method over a temperature range of 1900–2000 °C and a pressure of 20 Torr. The core level spectra of Sc 2p 3/2,1/2 and N 1s were obtained by x-ray photoelectron spectroscopy (XPS). The XPS core levels were shifted by 1.1 eV toward higher values as the [Sc]:[N] ratio varied from 1.4 at 1900 °C to ~1.0 at 2000 °C due to the higher binding energies in stoichiometric ScN. Angle-resolved photoemission spectroscopy measurements confirmed that ScN has an indirect bandgap of ~1.2 eV.

42 ENGINEERING↗
DOE OSTI2022

Electronic Structure of InAs and InSb Surfaces: Density Functional Theory and Angle-Resolved Photoemission Spectroscopy

The electronic structure of surfaces plays a key role in the properties of quantum devices. However, surfaces are also the most challenging to simulate and engineer. Here, in this work, the electronic structure of InAs(001), InAs(111), and InSb(110) surfaces is studied using a combination of density functional theory (DFT) and angle-resolved photoemission spectroscopy (ARPES). Large-scale first principles simulations are enabled by using DFT calculations with a machine-learned Hubbard U correction [npj Comput. Mater. 6, 180 (2020)]. To facilitate direct comparison with ARPES results, a “bulk unfolding” scheme is implemented by projecting the calculated band structure of a supercell surface slab model onto the bulk primitive cell. For all three surfaces, a good agreement is found between DFT calculations and ARPES. For InAs(001), the simulations clarify the effect of the surface reconstruction. Different reconstructions are found to produce distinctive surface states, which may be detected by ARPES with low photon energies. For InAs(111) and InSb(110), the simulations help elucidate the effect of oxidation. Owing to larger charge transfer from As to O than from Sb to O, oxidation of InAs(111) leads to significant band bending and produces an electron pocket, whereas oxidation of InSb(110) does not. The combined theoretical and experimental results may inform the design of quantum devices based on InAs and InSb semiconductors, for example, topological qubits utilizing the Majorana zero modes.

42 ENGINEERING↗