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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 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Above-threshold multiphoton photoemission from noble metal surfaces

Exciting solids with intense femtosecond laser pulses prompts electrons of the interrogated material to respond in a highly nonlinear manner, as is evident in the emission of high-order harmonic radiation and photoelectrons with kinetic energies well above that of the driving photons. Such high-field interactions can be resolved, for example, in above-threshold multiphoton photoemission (ATP) spectroscopy. In this work, we interrogate the nonlinear photoelectric responses of the pristine copper, silver, and gold noble metal surfaces in (111) and (100) crystal orientations in the perturbative regime. Using multiphoton photoemission spectroscopy (mPP) excited by finely tuned optical fields, we characterize enhancement of the mPP and ATP yields from (111) surfaces in selected k||-momentum ranges when the occupied Shockley surface (SS) states are (near-)resonantly coupled by multiphoton transitions to image potential (IP) intermediate states in the excitation process. The ATP signal from the IP states of (111) surfaces is largely defined by their formation through polarization of SS electrons; this observation is contrasted with ATP experiments from the Ag(100) surface, for which the SS becomes an unoccupied resonance and the IP states can only be excited from bands with significantly more bulk character. In addition, based on the optical power and nonlinear order-dependent mPP spectra, we provide evidence for ATP being a one-step, rather than a sequential process, as previously postulated.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Photoemission and dynamical mean field theory study of electronic correlations in a t 2 g 5 metal SrRhO 3 thin film

Perovskite rhodates are characterized by intermediate strengths of both electronic correlation as well as spin-orbit coupling (SOC) and usually behave as moderately correlated metals. A recent publication on epitaxial SrRhO 3 thin films reported a bad-metallic behavior and suggested the occurrence of antiferromagnetism below 100 K. In this work, we have further studied this SrRhO 3 thin film by hard x-ray photoemission spectroscopy and found a very small density of states (DOS) at the Fermi level $(E_F)$, which is consistent with the previously reported bad-metallic behavior. However, the absence of DOS persists up to room temperature, which contradicts the explanation of antiferromagnetic transition at ~100 K. We also employed electronic structure calculations within the framework of density functional theory and dynamical mean-field theory. In contrast to the photoemission results, our calculations indicate metallic behaviors of both bulk SrRhO 3 and the SrRhO 3 thin film, and a stronger correlation effect was observed in the thin film than that in the bulk. The calculated uniform magnetic susceptibility is substantially larger in the thin film than that in the bulk. We also investigated the role of SOC and found only a moderate modulation of the band structure. Hence SOC is not expected to significantly affect the electronic correlation in SrRhO 3 . Extrinsic effects of finite-thickness effects beyond our calculations and localization effects may play important roles to induce the negligible spectral weight at $(E_F)$.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Glide-resolved photoemission spectroscopy: Measuring topological invariants in nonsymmorphic space groups

The two classes of 3D, time-reversal-invariant insulators are known to subdivide into four classes in the presence of glide symmetry. Here, we extend this classification of insulators to include glide-symmetric Weyl metals and find a finer $\mathbb{Z}_4 ⊕\mathbb {Z}$ classification. We further elucidate the smoking-gun experimental signature of each class in the photoemission spectroscopy of surface states. Measuring the $\mathbb{Z}_4$ topological invariant by photoemission relies on identifying the glide representation of the initial Bloch state before photoexcitation—we show how this is accomplished with relativistic selection rules, combined with standard spectroscopic techniques to resolve both momentum and spin. In this work, our method relies on a spin-momentum locking that is characteristic of all glide-symmetric solids (inclusive of insulators and metals in trivial and topological categories). As an orthogonal application, given a glide-symmetric solid with an ideally symmetric surface, we may utilize this spin-momentum locking to generate a source of fully spin-polarized photoelectrons, which have diverse applications in solid-state spectroscopy. Our ab initio calculations predict Ba 2 Pb, stressed Na 3 Bi, and KHgSb to realize all three, nontrivial insulating phases in the $\mathbb{Z}_4$ classification.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2011

Electronic structure of elemental curium studied by photoemission.

The electronic structure of curium metal has been investigated by valence-band and 4f core-level photoemission spectroscopy using a high-purity 248Cm sample. The experimental spectra are dominated by poorly screened features and indicate full localization of the 5f electrons, in strong contrast to the lighter actinides, including Pu and Am. The results obtained are in good agreement with the Cm photoemission obtained by atomic multielectronic calculations for a 5f 7 configuration and with the total 5f density of states calculated ab initio within a correlated band theory model based on the self-consistent, local-density-matrix approximation to the dynamical mean-field theory.

Gouder, T↗
DOE OSTI2016

Laser angle-resolved photoemission as a probe of initial state k z dispersion, final-state band gaps, and spin texture of Dirac states in the Bi 2 Te 3 topological insulator

Here, we have obtained angle-resolved photoemission (ARPES) spectra from single crystals of the topological insulator material Bi 2 Te 3 using tunable laser spectrometer. The spectra were collected for eleven different photon energies ranging from 5.57 to 6.70 eV for incident light polarized linearly along two different in-plane directions. Parallel first-principles, fully relativistic computations of photo-intensities were carried out using the experimental geometry within the framework of the one-step model of photoemission. Good overall accord between theory and experiment is used to gain insight into how properties of the initial and final state band structures as well as those of the topological surface states and their spin-textures are reflected in the laser-ARPES spectra. In conclusion, our analysis reveals that laser-ARPES is sensitive to both the initial state k z dispersion and the presence of delicate gaps in the final state electronic spectrum.

36 MATERIALS SCIENCE↗
DOE OSTI2017

One-step model of photoemission from single-crystal surfaces

In our paper, we present a three-dimensional one-step photoemission model that can be used to calculate the quantum efficiency and momentum distributions of electrons photoemitted from ordered single-crystal surfaces close to the photoemission threshold. Using Ag(111) as an example, we also show that the model can not only calculate the quantum efficiency from the surface state accurately without using any ad hoc parameters, but also provides a theoretical quantitative explanation of the vectorial photoelectric effect. This model in conjunction with other band structure and wave function calculation techniques can be effectively used to screen single-crystal photoemitters for use as electron sources for particle accelerator and ultrafast electron diffraction applications.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Amplitude mode oscillations in pump-probe photoemission spectra from a d -wave superconductor

Recent developments in the techniques of ultrafast pump-probe photoemission have made possible the search for collective modes in strongly correlated systems out of equilibrium. Including inelastic scattering processes and a retarded interaction, we simulate time- and angle-resolved photoemission spectroscopy (trARPES) to study the amplitude mode of a d-wave superconductor, a collective mode excited through the nonlinear light-matter coupling to the pump pulse. We find that the amplitude mode oscillations of the d-wave order parameter occur in phase at a single frequency that is twice the quasi-steady-state maximum gap size after pumping. As a result, we comment on the necessary conditions for detecting the amplitude mode in trARPES experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Revisiting the origin of satellites in core-level photoemission of transparent conducting oxides: The case of $\mathcal{n}$-doped SnO 2

In this work, the longstanding problem of interpretation of satellite structures in core-level photoemission spectra of metallic systems with a low density of conduction electrons is addressed using the specific example of Sb-doped SnO 2 . Comparison of ab initio many-body calculations with experimental hard x-ray photoemission spectra of the Sn 4d states shows that strong satellites are produced by coupling of the Sn core hole to the plasma oscillations of the free electrons introduced by doping. Within the same theoretical framework, spectral changes of the valence band spectra are also related to dynamical screening effects. These results demonstrate that, for the interpretation of electron correlation features in the core-level photoelectron spectra of such narrow-band materials, going beyond the homogeneous electron gas electron-plasmon coupling model is essential.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Atomic-layer-resolved composition and electronic structure of the cuprate B i 2 S r 2 CaC u 2 O 8 + δ from soft x-ray standing-wave photoemission

A major remaining challenge in the superconducting cuprates is the unambiguous differentiation of the composition and electronic structure of the CuO 2 layers and those of the intermediate layers. The large c axis for these materials permits employing soft x-ray (930.3 eV) standing wave (SW) excitation in photoemission that yields atomic layer-by-layer depth resolution of these properties. Applying SW photoemission to Bi 2 Sr 2 CaCu 2 O 8+δ yields the depth distribution of atomic composition and the layer-resolved densities of states. We detect significant Ca presence in the SrO layers and oxygen bonding to three different cations. The layer-resolved valence electronic structure is found to be strongly influenced by the atomic supermodulation structure, as determined by comparison to density functional theory calculations, by Ca-Sr intermixing, and by correlation effects associated with the Cu 3 d -3 d Coulomb interaction, further clarifying the complex interactions in this prototypical cuprate. Here, measurements of this type for other quasi-two-dimensional materials with large c represent a promising future direction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Efficient prediction of time- and angle-resolved photoemission spectroscopy measurements on a nonequilibrium BCS superconductor

We study how time- and angle-resolved photoemission (tr-ARPES) reveals the dynamics of BCS-type, s -wave superconducting systems with time-varying order parameters. Approximate methods are discussed, based on previous approaches to either optical conductivity or quantum dot transport, to enable computationally efficient prediction of photoemission spectra. One use of such predictions is to enable extraction of the underlying order parameter dynamics from experimental data, which is topical given the rapidly growing use of tr-ARPES in studying unconventional superconductivity. The methods considered model the two-time lesser Green's functions with an approximated lesser self-energy that describes relaxation by coupling of the system to two types of baths. The approach primarily used here also takes into consideration the relaxation of the excited states into equilibrium by explicitly including the level-broadening of the retarded and advanced Green's functions. Here, we present equilibrium and nonequilibrium calculations of tr-ARPES spectrum from our model and discuss the signatures of different types of superconducting dynamics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Doping dependence of the magnitude of fluctuating spin moments in the normal state of the pnictide superconductor Sr ( F e 1 - x C o x ) 2 A s 2 inferred from photoemission spectroscopy

We report systematic temperature- and doping-dependent measurements of the Fe3s core-level photoemission spectra in the normal state of superconducting Sr(Fe 1- x Co x ) 2 As 2 . The analysis of the Fe3s spectrum provides an element-specific determination of the mean value of the magnitude of the Fe spin moment measured on the fast (10 -16 -10 -15 s) timescale of the photoemission process. The data reveal the ubiquitous presence in the normal state of Fe spin moments with magnitude fluctuating on short timescales. The data reveal a significant reduction of the magnitude of the effective Fe spin moment on going from the parent to the optimal doped compound. The doping dependence of the magnitude of the spin moment at higher doping level is less clear, being either constant, or even nonmonotonic, depending on temperature. This phenomenology indicates the importance of the interaction between spin and itinerant degrees of freedom in shaping the properties of the normal state. These findings reaffirm the complexity of the normal state of 122 Fe-pnictides, which are typically viewed as the least correlated of the high-temperature unconventional superconductors.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Correlation-driven attosecond photoemission delay in the plasmonic excitation of C60 fullerene

Extreme light confinement in plasmonic nanosystems enables novel applications in photonics, sensor technology, energy harvesting, biology, and quantum information processing. Fullerenes represent an extreme case for nanoplasmonics: they are sub-nanometer carbon- based molecules showing high-energy and ultrabroad plasmon resonances, however the fundamental mechanisms driving the plasmonic response and the corresponding collective electron dynamics are still elusive. Here, we uncover the dominant role of electron correlations in the dynamics of the giant plasmon resonance (GPR) of the sub-nanometer system C60 by employing attosecond photoemission chronoscopy. We find a characteristic photoemission delay of up to about 300 attoseconds that is purely induced by coherent large-scale electron correlations in the plasmonic potential. These results provide novel insights into the nature of the plasmon resonances in sub-nanometer systems and open new perspectives for advancing nanoplasmonic applications.

Biswas, Shubhadeep [SLAC National Accelerator Labo↗
DOE OSTI2024

One-dimensional temperature measurement of supersonic jet flow by resonantly ionized photoemission thermometry of molecular nitrogen

As the field of fluid dynamics progresses, the demand for sophisticated diagnostic methods to accurately assess flow conditions rises. In this work, resonantly ionized photoemission thermometry (RIPT) has been used to directly target and ionize diatomic nitrogen (N 2 ) to measure one-dimensional (1D) temperature profiles in a supersonic jet flow. This technique can be considered non-intrusive as the premise uses resonantly enhanced multiphoton ionization (REMPI) to target molecular nitrogen. This resonance excites N 2 into absorption bands of the P, Q, and R rotational branches of N 2 ( b 1 Π u ). The ideal (3 + 1) REMPI scheme excites from the ground state and ionizes N 2 ( b 1 Π u ← X 1 Σ g + ) where de-excitation results in photoemission from the first negative band of ionized N 2 + ( B 2 Σ u + → X 2 Σ g + ) as nitrogen returns to the ground state. The resulting emission can be observed using an intensified camera, thus permitting inference of the rotational temperature of ground-state molecular nitrogen. A linearly regressive Boltzmann distribution is applied based on previous calibration data for this technique to quantify the temperature along the ionized line. This work applies this technique to a pure N 2 supersonic jet in cross-flow and counter-flow orientations to demonstrate N 2 RIPT’s applications in a supersonic flow. Temperature variations are observed at different locations downstream of the exit in cross-flow, and axisymmetric in counter-flow, to generate profiles characterizing the flow dynamics. Due to the collisional effects resulting from the number density of N 2 at higher pressures, a (3 + 2) REMPI scheme is observed throughout this text.

Clark, Aleksander (ORCID:0009000855600042)↗
NASA NTRS1972

Photoemission studies of wurtzite zinc oxide.

The electronic structure of wurtzite zinc oxide, investigated over the widest possible photon energy range by means of photoemission techniques, is described. Of particular interest among the results of the photoemission study are the location of the Zn 3rd core states, the width of the upper valence bands, and structure in the conduction-band and valence-band density of states.

Powell, R. A.↗
NASA NTRS1973

Study of photoemission and work function of large surface areas, phase 3, phase 4

The photoemission of materials which might be used in probe measurements of the exo-atmospheric electric field is considered by evaluating the wavelength dependence of their photoelectric yield for eleven elements over the range 800 to 3200 A. Yield data for zinc, copper beryllium, platinum, cadmium, graphite, carbon, gold, silver, tantalum, and tungsten show that copper-beryllium is a preferred material. Silver has one of the highest photoemissions when exposed to solar radiation.

Source record↗
NASA NTRS1975

Four-photon photoemission from tungsten

Four-photon photoemission is observed from tungsten using carefully controlled and calibrated single pulses produced by a passively mode-locked Nd:YAG laser system. The results are shown to be in quantitative agreement with a four-photon generalization of the Fowler and DuBridge theories of photoemission.

Bechtel, J. H.↗
NASA NTRS1983

Interface states and internal photoemission in p-type GaAs metal-oxide-semiconductor surfaces

An interface photodischarge study of p-type GaAs metal-oxide-semiconductor (MOS) structures revealed the presence of deep interface states and shallow donors and acceptors which were previously observed in n-type GaAs MOS through sub-band-gap photoionization transitions. For higher photon energies, internal photoemission was observed, i.e., injection of electrons to the conduction band of the oxide from either the metal (Au) or from the GaAs valence band; the threshold energies were found to be 3.25 and 3.7 + or - 0.1 eV, respectively. The measured photoemission current exhibited a thermal activation energy of about 0.06 eV, which is consistent with a hopping mechanism of electron transport in the oxide.

Kashkarov, P. K.↗
NASA NTRS1990

Layered Internal-Photoemission Sensor

High quantum efficiency achieved without multiple layer contacts. Proposed infrared sensor based on photoemission from multiple layers of metal silicide sandwiched between layers of silicon. Suitable for use in focal-plane arrays. Layered internal-photoemission sensor has positive/intrinsic/negative structure modified by inclusion of layers or islands of metal silicide. Holes photo-excited from silicide regions and swept to detection by reverse-bias electric field in intrinsic silicon. Easier to make because internal layers allowed to "float" electrically, contact being made with only two outer semiconductor layers.

Fathauer, Robert W.↗