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At least 19 records

Evanescent Mode Photoemission

Photoemission of electrons from solid surfaces into vacuum is routinely used in two configurations: reflection mode, in which light is incident on the emitting surface, and transmission mode, in which light illuminates the photoemissive material from behind. Here, using silicon nitride waveguides integrated beneath a high quantum efficiency cesium antimonide thin film, we demonstrate a new photoemission regime─the evanescent mode photoemission─in which light travels parallel to the surface in the waveguide while evanescently coupling into the thin film to excite and emit photoelectrons. Furthermore, our experiments show that this configuration enables direct visualization of guided optical modes over an unprecedented range (∼100 nm to 1 mm) and allows electron beam shaping at the source with transverse features well below ∼600 nm, establishing evanescent mode photoemission as a new platform for nanoscale optical field mapping and precise generation of electron beams.

Electron Sources

Photoemission of Single Dust Grains for Heliospheric Conditions

Initial results of an experiment to measure the photoemission of single dust grains as a function of far ultraviolet wavelengths are presented. Coulombic forces dominate the interaction of the dust grains in the heliosphere. Knowledge of the charge state of dust grains, whether in a dusty plasma (Debye length < intergrain distance) or in the diffuse interplanetary region, is key to understanding their interaction with the solar wind and other solar system constituents. The charge state of heliospheric grains is primarily determined by primary electron and ion collisions, secondary electron emission and photoemission due to ultraviolet sunlight. We have established a unique experimental technique to measure the photoemission of individual micron-sized dust grains in vacuum. This technique resolves difficulties associated with statistical measurements of dust grain ensembles and non-static dust beams. The photoemission yield of Aluminum Oxide 3-micron grains For wavelengths from 120-300 nm with a spectral resolution of 1 nm FWHM is reported. Results are compared to interplanetary conditions.

Spann, James F., Jr.

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

Cavity-enhanced high-order harmonic generation for high-performance time-resolved photoemission experiments

Recent breakthroughs in high repetition-rate extreme ultraviolet (XUV) light sources and photoelectron analyzers have led to dramatic advances in the performance of time-resolved photoemission experiments. In this perspective article, we discuss the application of cavity-enhanced high-order harmonic generation, with repetition rates exceeding 10 MHz, to photoemission experiments using advanced endstations incorporating time-of-flight photoelectron analyzers. We discuss recent results, perspective on future areas for further technological improvement, and the wide array of science enabled by ultrafast XUV photoemission experiments, now in a qualitatively new regime.

Allison, Thomas K. (ORCID:0000000302898830)

Reexamining circular dichroism in photoemission from a topological insulator

The orbital angular momentum (OAM) of electron states is an essential ingredient for topological and quantum geometric quantities in solids. For example, Dirac surface states with helical spin- and orbital-angular momenta are a hallmark of a 3D topological insulator. Angle-resolved photoemission spectroscopy (ARPES) with variable circular light polarization, known as circular dichroism (CD), has been assumed to be a direct probe of OAM and, by proxy, of the Berry curvature of electronic bands in energy- and momentum-space. Indeed, topological surface states have been shown to exhibit angle-dependent CD (CDAD), and more broadly, CD is often interpreted as evidence of spin-orbit coupling. Meanwhile, it is well-established that CD originates from the photoemission matrix elements, which can have extrinsic contributions related to the experimental geometry and the inherently broken inversion symmetry at the sample surface. Therefore, it is important to broadly examine CD-ARPES to determine the scenarios in which it provides a robust probe of intrinsic material physics. We performed CD-ARPES on the canonical topological insulator Bi 2 ⁢Se 3 over a wide range of incident photon energies. Not only do we observe angle-dependent CD in the surface states, as expected, but we also find CD of a similar magnitude in virtually all bulk bands. Since OAM is forbidden by inversion symmetry in the bulk, we conclude this originates from symmetry-breaking in the photoemission process. Comparison with theoretical calculations supports this view and suggests that “hidden” OAM—localized to atomic sites within each unit cell—contributes significantly. Additional effects, including inter-atomic interference and final-state resonances, are responsible for the rapid variation of the CDAD signal with photon energy.

Sidilkover, Ittai [Tel Aviv University, Tel Aviv (

Reexamining Circular Dichroism in Photoemission From a Topological Insulator

The orbital angular momentum (OAM) of electron states is an essential ingredient for topological and quantum geometric quantities in solids. For example, Dirac surface states with helical spin- and orbital-angular momenta are a hallmark of a 3D topological insulator. Angle-resolved photoemission spectroscopy (ARPES) with variable circular light polarization, known as circular dichroism (CD), has been assumed to be a direct probe of OAM and, by proxy, of the Berry curvature of electronic bands in energy- and momentum-space. Indeed, topological surface states have been shown to exhibit angle-dependent CD (CDAD), and more broadly, CD is often interpreted as evidence of spin-orbit coupling. Meanwhile, it is well-established that CD originates from the photoemission matrix elements, which can have extrinsic contributions related to the experimental geometry and the inherently broken inversion symmetry at the sample surface. Therefore, it is important to broadly examine CD-ARPES to determine the scenarios in which it provides a robust probe of intrinsic material physics. We performed CD-ARPES on the canonical topological insulator $\mathrm{Bi}_2\mathrm{Se}_3$ over a wide range of incident photon energies. Not only do we observe angle-dependent CD in the surface states, as expected, but we also find CD of a similar magnitude in virtually all bulk bands. Since OAM is forbidden by inversion symmetry in the bulk, we conclude this originates from symmetry-breaking in the photoemission process. Comparison with theoretical calculations supports this view and suggests that $\textit{hidden}$ OAM - localized to atomic sites within each unit cell - contributes significantly. Additional effects, including inter-atomic interference and final-state resonances, are responsible for the rapid variation of the CDAD signal with photon energy.

FOS: Physical sciences

Photoemission from CsI - Experiment.

Considerable attention in the investigation was given to the resolution maximization of details in the spectra. Very thin films were used in the measurements, which were conducted at 300 and 77 C with the aid of an improved photoemission apparatus. It was found that the principal features of the photoemission spectra from CsI cannot be explained on the basis of simple transitions from localized ionic states because such a model would predict a doublet instead of the triplet observed in the photoemission data.

Distefano, T. H.

Two-photon photoemission from metals induced by picosecond laser pulses

We have measured the two-photon photoemission current density from tungsten, tantalum, and molybdenum when irradiated by 532-nm wavelength radiation. This wavelength was produced by the second-harmonic radiation of single picosecond laser pulses from a mode-locked neodymium-doped yttrium-aluminum-garnet laser. The results are interpreted in terms of both a simple temperature-independent two-photon photoemission effect and a generalization of the Fowler-DuBridge theory of photoemission. The laser polarization dependence of the emitted current is also reported.

Bechtel, J. H.

Photoemission Experiments for Charge Characteristics of Individual Dust Grains

Photoemission experiments with UV radiation have been performed to investigate the microphysics and charge characteristics of individual isolated dust grains of various compositions and sizes by using the electrodynamic balance facility at NASA Marshall Space Flight Center. Dust particles of 2-10 gm diameter are levitated in a vacuum chamber at pressures approximately 10(exp-5) torr and exposed to a collimated beam of UV radiation in the 120-200 nm spectral range from a deuterium lamp source with a MgF2 window. A monochromator is used to select the UV wavelength with a spectral resolution of 8 nm. The electrodynamic facility permits measurements of the charge and diameters of particles of known composition, and monitoring of photoemission rates with the incident UV radiation. Experiments have been conducted on test particles of silica and polystyrene to determine the photoelectric yields and surface equilibrium potentials when exposed to UV radiation. A brief description of an experimental procedure for photoemission studies is given and some preliminary laboratory measurements of the photoelectric yields of individual dust particles are presented.

Abbas, M. M.

Photoemission Experiments for Charge Characteristics of Individual Dust Grains

Photoemission experiments with UV radiation have been performed to investigate the microphysics and charge characteristics of individual isolated dust grains of various compositions and sizes by using the electrodynamic balance facility at NASA Marshall Space Flight Center. Dust particles of 1 - 100 micrometer diameter are levitated in a vacuum chamber at pressures approx. 10(exp -5) torr and exposed to a collimated beam of UV radiation in the 120-300 nanometers spectral range from a deuterium lamp source with a MgF2 window. A monochromator is used to select the UV radiation wavelength with a spectral resolution of 8 nanometers. The electrodynamic facility permits measurements of the charge and diameters of particles of known composition, and monitoring of photoemission rates with the incident UV radiation. Experiments have been conducted on Al2O3 and silicate particles, and in particular on JSC-1 Mars regolith simulants, to determine the photoelectron yields and surface equilibrium potentials of dust particles when exposed to UV radiation in the 120-250 micrometers spectral range. A brief discussion of the experimental procedure, the results of photoemission experiments, and comparisons with theoretical models will be presented.

Abbas, M. M.

Modifications in the charge trap landscape in Hf 0.5 Zr 0.5 O 2 as a function of oxygen vacancy concentration observed with photoemission electron microscopy

Oxygen vacancies in Hf x Zr (1-x) O 2 (HZO) both contribute to stabilization of the ferroelectric orthorhombic phase and promote leakage pathways that limit the endurance of devices based on the material. Here, for this reason, the defect states of oxygen vacancies were investigated using photoemission electron microscopy (PEEM) and photoluminescence spectroscopy (PL), as their concentration was varied via ex situ laser exposure. Following a controlled oxygen vacancy reduction via visible (2.54 eV) laser dosing of HZO, deep-ultraviolet (DUV, 5.82 eV) PEEM was used to spatially probe the resulting mid-gap defect states and work function. Work function was found to increase monotonically with the laser-induced reduction in oxygen vacancy concentration culminating in a total increase near 70 meV. The change implies a Fermi level shift toward the valence band as the total available electron-filled charge states are reduced with the removal of oxygen vacancies. A reduction in charge states is corroborated by the observed lessening of both photoemission and photoluminescence intensities after laser dosing. The deduced position of the Fermi level is within a band of near-conduction band defect states produced by oxygen vacancies that are linked to endurance limiting leakage currents. Together, these results directly identify the primary role of oxygen vacancies on the defect states in HZO while demonstrating that laser exposure can be used for their modification.

42 ENGINEERING

Si 1-X Ge X /Si Heterojunction Internal Photoemission Long Wavelength Infrared Detector

Long wavelength Si 1-X Ge X /Si heterojunction internal photoemission (HIP) infrared detectors have been successfully demonstrated utilizing the growth of degenerately boron doped Si 1-X Ge X layers on Si. Recently, Si 0.7 GE 0.3 /SI HIP detectors with either a Si 1-X Ge X single layer or a Si 1-X Ge X /Si multilayer have been demonstrated with cutoff wavelengths out to 23 µm. Near-ideal thermionic emission dark current characteristics were measured and the electrical potential barriers were determined by the Richardson plot. A photoresponse model, similar to the modified Fowler Equation has been developed for the Si 1-X Ge X /Si heterojunction internal photoemission infrared detector at wavelengths corresponding to photon energies less than the Fermi energy. The optical potential barriers, the corresponding cutoff wavelengths, and the emission coefficients, C 1 , for the HIP detectors have been determined from the measured spectral responses using the photoresponse model. Similar optical and thermal potential barriers were obtained.

infrared

Optimized Photoemission from Organic Molecules in 2D Layered Halide Perovskites

In recent years, hybrid organic−inorganic metal halides have been at the forefront of materials research. Typically, the functional (e.g., optoelectronic) properties of hybrid halides are derived from the inorganic structural part, whereas the organic structural units can add extra advantages in terms of stability, rigidity, and processability. Here, we report the design, synthesis, and characterization of two new hybrid materials in which the outstanding photophysical properties originate from the organic structural part. The new compounds, (C 15 H 16 N) 2 CdCl 4 and ((Br)C 15 H 15 N) 2 CdCl 4 , have 2D layered Ruddlesden−Poppertype perovskite structures. These hybrids are blue-white light emitters just like their corresponding pure organic salts, but with much improved emission efficiencies. Optical spectroscopy and density functional theory (DFT) studies confirm that photoemission comes from the trans-stilbene organic cations. The photoluminescence quantum yield (PLQY) values of these new materials are among the highest known, 50.83% and 26.60% for (C 15 H 16 N) 2 CdCl 4 and ((Br)C 15 H 15 N) 2 CdCl 4 , respectively. This is up to a 5-fold increase as compared to the light emission efficiency of the precursor salt C 15 H 16 NCl (PLQY of 10.33%). Alongside their outstanding optical properties, their environmental and thermal stability allow their consideration for potential practical applications such as radiation detection. This work shows that hybrid metal halides can be compositionally and structurally engineered to have highly efficient photoemission originating from the organic components for fast scintillation applications.

Halogens

Analysis methodology of coherent oscillations in time- and angle-resolved photoemission spectroscopy

Oscillatory signals from coherently excited phonons are regularly observed in ultrafast pump–probe experiments on condensed matter samples. Electron–phonon coupling implies that coherent phonons also modulate the electronic band structure. These oscillations can be probed with energy and momentum resolution using time- and angle-resolved photoemission spectroscopy (trARPES), which reveals the orbital dependence of the electron–phonon coupling for a specific phonon mode. However, a comprehensive analysis remains challenging when multiple coherent phonon modes couple to multiple electronic bands. Complex spectral line shapes due to strong correlations in quantum materials add to this challenge. In this work, we examine how the frequency domain representation of trARPES data facilitates a quantitative analysis of coherent oscillations of the electronic bands. Here, we investigate the frequency domain representation of the photoemission intensity and the first moment of the energy distribution curves. Both quantities provide complementary information and are able to distinguish oscillations of binding energy, linewidth, and intensity. We analyze a representative trARPES dataset of the transition metal dichalcogenide WTe 2 and construct composite spectra, which intuitively illustrate how much each electronic band is affected by a specific phonon mode. We also show how a linearly chirped probe pulse can generate extrinsic artifacts that are distinct from the intrinsic coherent phonon signal.

47 OTHER INSTRUMENTATION

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

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)

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.

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.

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