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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
NASA NTRS2018

Polarization-Controlled Directional Multiphoton Photoemission from Hot Spots on Single Au Nanoshells

Directional photoemission from single Au nanoshells is demonstrated in the low-intensity, multiphoton regime. Thisdirectionality is shown to be due to the plasmonic excitation of highly photoemissive, nanometer scale surface regions, which are characterized by correlated momentum mapping, scanning electron microscopy (SEM), and laser polarization-dependence studies. Furthermore, the photoelectron flux from a single nanoshell can be systematically rotated by over 90° in momentum space simply by polarization-controlled coupling to different hot spots. Photoelectrondistributions are directly characterized in momentum space via velocity map imaging (VMI) of the two-dimensional transverse (px, py) momentum components for single nanoshells. For the majority of nanoshells studied, the photoemission is directionally orthogonal to the laser polarization, which implicates nanoscale crevice-shaped "hotspots" clearly observed in the correlated SEM/VMI studies, with the near-field plasmonic nature of these crevices clarified further via finite-element simulations. These results rationalize the large photoemission enhancements observed in previous Au nanoshell studies, but more importantly provide a novel experimental access to directionally tunable electron emission from nanoscale sources. The ability to control photoemission/photocurrent angular distributions at the nanoscale with only modest optical fields indicates a new parameter for optimizing nanoplasmonic system performance and suggests new plasmonic applications such as ultrafast, polarization-controlled photoelectric/photovoltaic switches.

Pettine, Jacob↗
DOE OSTI2019

Orbital Character Effects in the Photon Energy and Polarization Dependence of Pure C 60 Photoemission

We report that recent direct experimental observation of multiple highly dispersive C 60 valence bands has allowed for a detailed analysis of the unusual photoemission traits of these features through photon energy- and polarization-dependent measurements. Previously obscured dispersions and strong photoemission traits are now revealed by specific light polarizations. The observed intensity effects prove the locking in place of the C 60 molecules at low temperatures and the existence of an orientational order imposed by the substrate chosen. Most importantly, photon energy- and polarization-dependent effects are shown to be intimately linked with the orbital character of the C 60 band manifolds which allow for a more precise determination of the orbital character within the third highest occupied molecular orbital (HOMO-2). In conclusion, our observations and analysis provide important considerations for the connection between molecular and crystalline C 60 electronic structure, past and future band structure studies, and for increasingly popular C 60 electronic device applications, especially those making use of heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2018

The S-matrix for surface boundary states: An application to photoemission for Weyl semimetals

We present a new theory of photoemission for Weyl semimetals. We derive this theory using a model with a boundary surface at z=0. Due to the boundary, the self adjoint condition needs to be verified in order to ensure physical solutions. The solutions are given by two chiral zero modes which propagate on the boundary. Due to the Coulomb interaction, the chiral boundary model is in the same universality class as interacting graphene. The interactions cause a temperature dependence of the velocity and life time. Using the principle of minimal coupling, we identify the electron–photon Hamiltonian. The photoemission intensity is computed using the S-matrix formalism. The S-matrix is derived using the initial photon state, the final state of a photoelectron and a hole in the valence band. The photoemission reveals the final valence band dispersion ħv(±k{sub y}−k{sub 0})+ħΩ after absorbing a photon of frequency Ω (k{sub 0} represents the shift in the momentum due to the crystal potential). The momentum in the z direction is not conserved, and is integrated out. As a result, the scattering matrix is a function of the parallel momentum . We observe two dimensional contours, representing the “Fermi arcs”, which for opposite spin polarization have opposite curvature. This theory is in agreement with previous experimental observations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Nonmetal to Metal Transition and Ultrafast Charge Carrier Dynamics of Zn Clusters on p-Si(100) by fs-XUV Photoemission Spectroscopy

Understanding the electronic structure and charge carrier dynamics of supported clusters is important due to their many potential applications in photochemistry and catalysis. In this investigation, photoemission spectroscopy, in conjunction with femtosecond extreme ultraviolet (XUV) laser pulses, is used to investigate the electronic structure and ultrafast charge carrier dynamics at a Si(100) surface decorated with Zn clusters. Static photoemission spectroscopy is used to investigate the changes in the electronic structure as the dimensionality of the Zn is increased from small clusters composed of a very few atoms to metallic Zn particles. Furthermore, femtosecond optical-pump XUV-probe photoemission spectroscopy is employed to induce a charge transfer from the p-Si(100) substrate to the Zn clusters and to measure in real time the charge trapping at the Zn cluster as well as the subsequent charge relaxation. The ultrafast charge carrier dynamics are also investigated for small clusters and metallic Zn particles. Significant transient charging of the Zn clusters after excitation of the Si(100) substrate by 800 nm light is observed for Zn coverages greater than 0.12 ML Zn, which coincides with the formation of a Schottky barrier at the interface between the Zn particle and the p-Si(100) substrate. The transient signals show that the charge trapping time at the Zn cluster varies with the cluster size, which is rationalized based on the electronic structure of the cluster as well as the band energy alignment at the Zn cluster-Si(100) junction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2011

Plasmonic Field Enhancement of Individual Nanoparticles by Correlated Scanning and Photoemission Electron Microscopy

We present results of a combined two-photon photoemission and scanning electron microscopy investigation to determine the electromagnetic enhancement factors of silver-coated spherical nanoparticles deposited on an atomically flat mica substrate. Femtosecond laser excitation, of the nanoparticles, produces intense photoemission, attributed to near-resonant excitation of localized surface plasmons. Enhancement factors are determined by comparing the respective two-photon photoemission yield measured for equal areas between single nanoparticles to that of the surrounding flat surface. For s-polarized, 400 nm (~ 3.1 eV) femtosecond radiation a distribution of enhancement factors are found with a large percentage (77%) of the nanoparticles falling within a median range. A correlated scanning electron microscopy analysis demonstrated that the nanoparticles typifying the median of the distribution were characterized by ideal spherical shapes and defect-free morphologies. The single largest enhancement factors were in contrast produced by a very small percentage (8%) of the total, for which evidence of silver defect anomalies were found that contributed to the overall structure of the nanoparticle. Comparisons are made between the experimentally measured enhancement factors and previously reported theoretical predictions of the localized surface plasmon near-field intensities for isolated nanometer-sized silver spheres.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2011

A single centre water splitting dye complex adsorbed on rutile TiO{sub 2}(110): Photoemission, x-ray absorption, and optical spectroscopy

A single centre water splitting dye complex (aqua(2,2'-bipyridyl-4,4'-dicarboxylic acid)-(2,2':6',6''-terpyridine)Ruthenium(II)), along with a related complex ((2,2'-bipyridyl-4,4'-dicarboxylic acid)-(2,2':6',6''-terpyridine)chloride Ruthenium(II)), has been investigated using photoemission and compared to molecules with similar structures. Dye molecules were deposited in situ using ultra-high vacuum electrospray deposition, which allows for the deposition of thermally labile molecules, such as these dye molecules. Adsorption of the dye molecules on the rutile TiO{sub 2}(110) surface has been studied using core-level and valence photoemission. Core-level photoemission spectra reveal that each complex bonds to the surface via deprotonation of its carboxylic acid groups. A consideration of the energy level alignments reveals that both complexes are capable of charge transfer from the adsorbed molecules to the conduction band of the rutile TiO{sub 2} substrate.

36 MATERIALS SCIENCE↗
DOE OSTI2012

A tunable low-energy photon source for high-resolution angle-resolved photoemission spectroscopy

We describe a tunable low-energy photon source consisting of a laser-driven xenon plasma lamp coupled to a Czerny-Turner monochromator. The combined tunability, brightness, and narrow spectral bandwidth make this light source useful in laboratory-based high-resolution photoemission spectroscopy experiments. The source supplies photons with energies up to {approx}7 eV, delivering under typical conditions >10{sup 12} ph/s within a 10 meV spectral bandwidth, which is comparable to helium plasma lamps and many synchrotron beamlines. We first describe the lamp and monochromator system and then characterize its output, with attention to those parameters which are of interest for photoemission experiments. Finally, we present angle-resolved photoemission spectroscopy data using the light source and compare its performance to a conventional helium plasma lamp.

43 PARTICLE ACCELERATORS↗
DOE OSTI2013

Integrated experimental setup for angle resolved photoemission spectroscopy of transuranic materials

We have developed the Angle Resolved Photoemission Spectroscopy (ARPES) system for transuranic materials. The ARPES transuranic system is an endstation upgrade to the Laser Plasma Light Source (LPLS) at Los Alamos National Laboratory. The LPLS is a tunable light source for photoemission with a photon energy range covering the vacuum ultraviolet (VUV) and soft x-ray regions (27–140 eV). The LPLS was designed and developed for transuranic materials. Transuranic photoemission is currently not permitted at the public synchrotrons worldwide in the VUV energy range due to sample encapsulation requirements. With the addition of the ARPES capability to the LPLS system there is an excellent opportunity to explore new details centered on the electronic structure of actinide and transuranic materials.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2014

Bulk sensitive hard x-ray photoemission electron microscopy

Hard x-ray photoelectron spectroscopy (HAXPES) has now matured into a well-established technique as a bulk sensitive probe of the electronic structure due to the larger escape depth of the highly energetic electrons. In order to enable HAXPES studies with high lateral resolution, we have set up a dedicated energy-filtered hard x-ray photoemission electron microscope (HAXPEEM) working with electron kinetic energies up to 10 keV. It is based on the NanoESCA design and also preserves the performance of the instrument in the low and medium energy range. In this way, spectromicroscopy can be performed from threshold to hard x-ray photoemission. The high potential of the HAXPEEM approach for the investigation of buried layers and structures has been shown already on a layered and structured SrTiO{sub 3} sample. Here, we present results of experiments with test structures to elaborate the imaging and spectroscopic performance of the instrument and show the capabilities of the method to image bulk properties. Additionally, we introduce a method to determine the effective attenuation length of photoelectrons in a direct photoemission experiment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Photoemission electron microscopy of localized surface plasmons in silver nanostructures at telecommunication wavelengths

We image the field enhancement at Ag nanostructures using femtosecond laser pulses with a center wavelength of 1.55 μm. Imaging is based on non-linear photoemission observed in a photoemission electron microscope (PEEM). The images are directly compared to ultra violet PEEM and scanning electron microscopy (SEM) imaging of the same structures. Further, we have carried out atomic scale scanning tunneling microscopy on the same type of Ag nanostructures and on the Au substrate. Measuring the photoelectron spectrum from individual Ag particles shows a larger contribution from higher order photoemission processes above the work function threshold than would be predicted by a fully perturbative model, consistent with recent results using shorter wavelengths. Investigating a wide selection of both Ag nanoparticles and nanowires, field enhancement is observed from 30% of the Ag nanoparticles and from none of the nanowires. No laser-induced damage is observed of the nanostructures neither during the PEEM experiments nor in subsequent SEM analysis. By direct comparison of SEM and PEEM images of the same nanostructures, we can conclude that the field enhancement is independent of the average nanostructure size and shape. Instead, we propose that the variations in observed field enhancement could originate from the wedge interface between the substrate and particles electrically connected to the substrate.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Suppression of the vacuum space-charge effect in fs-photoemission by a retarding electrostatic front lens

The performance of time-resolved photoemission experiments at fs-pulsed photon sources is ultimately limited by the e–e Coulomb interaction, downgrading energy and momentum resolution. Here, we present an approach to effectively suppress space-charge artifacts in momentum microscopes and photoemission microscopes. A retarding electrostatic field generated by a special objective lens repels slow electrons, retaining the k-image of the fast photoelectrons. The suppression of space-charge effects scales with the ratio of the photoelectron velocities of fast and slow electrons. Fields in the range from -20 to 01100 V/mm for E kin = 100 eV to 4 keV direct secondaries and pump-induced slow electrons back to the sample surface. Ray tracing simulations reveal that this happens within the first 40 to 3 μm above the sample surface for E kin = 100 eV to 4 keV. An optimized front-lens design allows switching between the conventional accelerating and the new retarding mode. Time-resolved experiments at E kin = 107 eV using fs extreme ultraviolet probe pulses from the free-electron laser FLASH reveal that the width of the Fermi edge increases by just 30 meV at an incident pump fluence of 22 mJ/cm2 (retarding field -21 V/mm). For an accelerating field of +2 kV/mm and a pump fluence of only 5 mJ/cm 2 , it increases by 0.5 eV (pump wavelength 1030 nm). At the given conditions, the suppression mode permits increasing the slow-electron yield by three to four orders of magnitude. The feasibility of the method at high energies is demonstrated without a pump beam at E kin = 3830 eV using hard x rays from the storage ring PETRA III. The approach opens up a previously inaccessible regime of pump fluences for photoemission experiments.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Expanding the momentum field of view in angle-resolved photoemission systems with hemispherical analyzers

In photoelectron spectroscopy, the measured electron momentum range is intrinsically related to the excitation photon energy. Low photon energies <10 eV are commonly encountered in laser-based photoemission and lead to a momentum range that is smaller than the Brillouin zones of most materials. This can become a limiting factor when studying condensed matter with laser-based photoemission. An additional restriction is introduced by widely used hemispherical analyzers that record only electrons photoemitted in a solid angle set by the aperture size at the analyzer entrance. Here, we present an upgrade to increase the effective solid angle that is measured with a hemispherical analyzer. We achieve this by accelerating the photoelectrons toward the analyzer with an electric field that is generated by a bias voltage on the sample. Our experimental geometry is comparable to a parallel plate capacitor, and therefore, we approximate the electric field to be uniform along the photoelectron trajectory. With this assumption, we developed an analytic, parameter-free model that relates the measured angles to the electron momenta in the solid and verify its validity by comparing with experimental results on the charge density wave material TbTe3. By providing a larger field of view in momentum space, our approach using a bias potential considerably expands the flexibility of laser-based photoemission setups.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Role of matrix elements in the time-resolved photoemission signal

Time- and angle-resolved photoemission spectroscopy (TR-ARPES) provides access to the ultrafast evolution of electrons andmany-body interactions in solid-state systems. However, themomentum- and energy-resolved transient photoemission intensitymay not be unambiguously described by the intrinsic relaxation dynamics of photoexcited electrons alone.The interpretation of the time-dependent photoemission signal can be affected by the transient evolution of the electronic distribution, and both the one-electron removal spectral function aswell as the photoemissionmatrix elements. Here we investigate the topological insulator Bi 1.1 Sb 0.9 Te 2 S to demonstrate, bymeans of a detailed probe-polarization dependent study, the transient contribution ofmatrix elements toTR-ARPES.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Energy-resolved attosecond interferometric photoemission from Ag(111) and Au(111) surfaces

Photoelectron emission from solid surfaces induced by attosecond pulse trains into the electric field of delayed phase-coherent infrared (IR) pulses allows the surface-specific observation of energy-resolved electronic phase accumulations and photoemission delays. Here, we quantum-mechanically modeled interferometric photoemission spectra from the (111) surfaces of Au and Ag, including background contributions from secondary electrons and direct emission by the IR pulse, and adjusted parameters of our model to energy-resolved photoelectron spectra recently measured at a synchrotron light source by Roth et al. [J. Electron Spectrosc. 224, 84 (2018)]. Our calculated spectra and photoelectron phase shifts are in fair agreement with the experimental data of Locher et al. [Optica 2, 405 (2015)]. Our model's not reproducing the measured energy-dependent oscillations of the Ag(111) photoemission phases may be interpreted as evidence for subtle band-structure effects on the final-state photoelectron-surface interaction not accounted for in our simulation.

74 ATOMIC AND MOLECULAR PHYSICS↗
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

Angle-resolved pair photoemission theory for correlated electrons

Here in this paper we consider the possibility and conditions for pair photoemission whereby two incident photons emit pairs of electrons from a candidate material as a novel method to measure and visualize electronic correlations. As opposed to double photoemission - where a single photon precipitates the ejection of a pair electrons via a subsequent electron energy loss scattering process - we show that pair photoemission need not be limited to interference between initial photoelectrons and valence electrons, and moreover, can occur without the energy penalty of two work functions. This enables detection of pairs of electrons at high energy resolution that may be correlated in the same quantum many-body states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2011

Insulating state of ultrathin epitaxial LaNiO{sub 3} thin films detected by hard x-ray photoemission

In order to understand the influence of strain and film thickness on the electronic structure of thin films of strongly correlated oxides, we have applied hard x-ray photoemission (HXPS) at 6 keV, soft x-ray photoemission (XPS) at 1.5 keV, and transmission electron microscopy to epitaxial LaNiO{sub 3} films deposited on two substrates: LaAlO{sub 3} (compressive strain) and (LaAlO{sub 3}){sub 0.3}(Sr{sub 2}AlTaO{sub 6}){sub 0.7} (tensile strain). Using inelastic attenuation lengths in LaNiO{sub 3} determined from the HXPS data, we have decomposed valence-band spectra into layer-specific contributions. This decomposition is validated by comparing with the results of first-principles calculations using a hybrid functional. The resultant thin-film LaNiO{sub 3} densities of states exhibit significant differences in spectral weights for the thinnest LaNiO{sub 3} films. A gap opening consistent with a metal-to-insulator transition is observed for the thinnest 2.7 nm LaNiO{sub 3} film on an (LaAlO{sub 3}){sub 0.3}(Sr{sub 2}AlTaO{sub 6}){sub 0.7} substrate, with a similar gap opening also being observed in complementary soft x-ray photoemission at 1.5 keV for a thinner 1.4 nm film on an LaAlO{sub 3} substrate. A metal-to-insulator transition in very thin nm-scale films of LaNiO{sub 3} is thus suggested as a general phenomenon.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2010

Application of the Lucy–Richardson Deconvolution Procedure to High Resolution Photoemission Spectra

Angle-resolved photoemission has developed into one of the leading probes of the electronic structure and associated dynamics of condensed matter systems. As with any experimental technique the ability to resolve features in the spectra is ultimately limited by the resolution of the instrumentation used in the measurement. Previously developed for sharpening astronomical images, the Lucy-Richardson deconvolution technique proves to be a useful tool for improving the photoemission spectra obtained in modern hemispherical electron spectrometers where the photoelectron spectrum is displayed as a 2D image in energy and momentum space.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗