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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 127 records · Page 7

Ultracold Electrons via Near-Threshold Photoemission from Single-Crystal Cu(100)

Achieving a low mean transverse energy or temperature of electrons emitted from the photocathode-based electron sources is critical to the development of next-generation and compact x-ray free electron lasers and ultrafast electron diffraction, spectroscopy, and microscopy experiments. In this Letter, we demonstrate a record low mean transverse energy of 5 meV from the cryo-cooled (100) surface of copper using near-threshold photoemission. Further, we also show that the electron energy spread obtained from such a surface is less than 11.5 meV, making it the smallest energy spread electron source known to date: more than an order of magnitude smaller than any existing photoemission, field emission, or thermionic emission based electron source. Overall, our measurements also shed light on the physics of electron emission and show how the energy spread at few meV scale energies is limited by both the temperature and the vacuum density of states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Optimisation of NSLS-II Blade X-ray Beam Position Monitors: from Photoemission type to Diamond Detector

Optimisation of blade type x-ray beam position monitors (XBPM) was performed for NSLS-II undulator IVU20. Blade material, con and #64257;guration and operation principle was analysed in order to improve XBPM performance. Optimisation is based on calculation of the XBPM signal spatial distribution. Along with standard photoemission type XBPM a Diamond Detector Blades (DDB) were analysed as blades for XBPMs. DDB XBPMs can help to overcome drawbacks of the photoemission blade XBPMs.

43 PARTICLE ACCELERATORS↗

Enhancement of Photoemission on p-Type GaAs Using Surface Acoustic Waves

We demonstrate that photoemission properties of p-type GaAs can be altered by surface acoustic waves (SAWs) generated on the GaAs surface due to dynamical piezoelectric fields of SAWs. Multiphysics simulations indicate that charge-carrier recombination is greatly reduced, and electron effective lifetime in p-doped GaAs may increase by a factor of 10× to 20×. It implies a significant increase, by a factor of 2× to 3×, of quantum efficiency (QE) for GaAs photoemission applications, like GaAs photocathodes. Conditions of different SAW wavelengths, swept SAW intensities, and varied incident photon energies were investigated. Essential steps in SAW device fabrication on a GaAs substrate are demonstrated, including deposition of an additional layer of ZnO for piezoelectric effect enhancement, measurements of current–voltage (I–V) characteristics of the SAW device, and ability to survive high-temperature annealing. Results obtained and reported in this study provide the potential and basis for future studies on building SAW-enhanced photocathodes, as well as other GaAs photoelectric applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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↗

Photoemission Electron Microscopy of a Plasmonic Silver Nanoparticle Trimer

We present a combined experimental and theoretical study to investigate the spatial distribution of photoelectrons emitted from core-shell silver (Ag) nanoparticles. We use two-photon photoemission microscopy (2P-PEEM) to spatially resolve electron emission from a trimeric core-shell aggregate of triangular symmetry. Finite difference time domain (FDTD) simulations are performed to model the intensity distributions of the electromagnetic near-fields resulting from femtosecond (fs) laser excitation of localized surface plasmon oscillations in the triangular core-shell structure. We demonstrate that the predicted FDTD near-field intensity distribution reproduces the 2P-PEEM photoemission pattern.

Environmental Molecular Sciences Laboratory↗

Hartmann characterization of the PEEM-3 aberration-corrected X-ray photoemission electron microscope

Aberration correction by an electron mirror dramatically improves the spatial resolution and transmission of photoemission electron microscopes. We will review the performance of the recently installed aberration corrector of the X-ray Photoemission Electron Microscope PEEM-3 and show a large improvement in the efficiency of the electron optics. Hartmann testing is introduced as a quantitative method to measure the geometrical aberrations of a cathode lens electron microscope. Here, we find that aberration correction leads to an order of magnitude reduction of the spherical aberrations, suggesting that a spatial resolution of below 100 nm is possible at 100% transmission of the optics when using x-rays. We demonstrate this improved performance by imaging test patterns employing element and magnetic contrast.

36 MATERIALS SCIENCE↗

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↗

Observation of possible topological in-gap surface states in the Kondo insulator SmB 6 by photoemission

SmB 6 , a well-known Kondo insulator, exhibits a transport anomaly at low temperature. This anomaly is usually attributed to states within the hybridization gap. Recent theoretical work and transport measurements suggest that these in-gap states could be ascribed to topological surface states, which would make SmB6 the first realization of topological Kondo insulator. Here by performing angle-resolved photoemission spectroscopy experiments, we directly observe several dispersive states within the hybridization gap of SmB 6 . These states show negligible k z dependence, which indicates their surface origin. Furthermore, we perform photoemission circular dichroism experiments, which suggest that the in-gap states possess chirality of the orbital angular momentum. These states vanish simultaneously with the hybridization gap at around 150 K. Together, these observations suggest the possible topological origin of the in-gap states.

42 ENGINEERING↗

Layer-resolved many-electron interactions in delafossite PdCoO2 from standing-wave photoemission spectroscopy

Abstract When a three-dimensional material is constructed by stacking different two-dimensional layers into an ordered structure, new and unique physical properties can emerge. An example is the delafossite PdCoO 2 , which consists of alternating layers of metallic Pd and Mott-insulating CoO 2 sheets. To understand the nature of the electronic coupling between the layers that gives rise to the unique properties of PdCoO 2 , we revealed its layer-resolved electronic structure combining standing-wave X-ray photoemission spectroscopy and ab initio many-body calculations. Experimentally, we have decomposed the measured VB spectrum into contributions from Pd and CoO 2 layers. Computationally, we find that many-body interactions in Pd and CoO 2 layers are highly different. Holes in the CoO 2 layer interact strongly with charge-transfer excitons in the same layer, whereas holes in the Pd layer couple to plasmons in the Pd layer. Interestingly, we find that holes in states hybridized across both layers couple to both types of excitations (charge-transfer excitons or plasmons), with the intensity of photoemission satellites being proportional to the projection of the state onto a given layer. This establishes satellites as a sensitive probe for inter-layer hybridization. These findings pave the way towards a better understanding of complex many-electron interactions in layered quantum materials.

36 MATERIALS SCIENCE↗

Angle-resolved Photoemission Spectroscopy Study on the Surface States of the Correlated Topological Insulator YbB 6

YbB 6 is recently predicted to be a moderately correlated topological insulator, which provides a playground to explore the interplay between correlation and topological properties. With angle-resolved photoemission spectroscopy, we directly observed almost linearly dispersive bands around the time-reversal invariant momenta $\bar{Γ}$ and $\bar{X}$ with negligible k z dependence, consistent with odd number of surface states crossing the Fermi level in a Z 2 topological insulator. Circular dichroism photoemission spectra suggest that these in-gap states possess chirality of orbital angular momentum, which is related to the chiral spin texture, further indicative of their topological nature. The observed insulating gap of YbB 6 is about 100 meV, larger than that found by theoretical calculations. Our results present strong evidence that YbB 6 is a correlated topological insulator and provide a foundation for further studies of this promising material.

36 MATERIALS SCIENCE↗

Electronic structure investigation of atomic layer deposition ruthenium(oxide) thin films using photoemission spectroscopy

Analyzing and manipulating the electronic band line-up of interfaces in novel micro- and nanoelectronic devices is important to achieve further advancement in this field. Such band alignment modifications can be achieved by introducing thin conformal interfacial dipole layers. Atomic layer deposition (ALD), enabling angstrom-precise control over thin film thickness, is an ideal technique for this challenge. Ruthenium (Ru{sup 0}) and its oxide (RuO{sub 2}) have gained interest in the past decade as interfacial dipole layers because of their favorable properties like metal-equivalent work functions, conductivity, etc. In this study, initial results of the electronic structure investigation of ALD Ru{sup 0} and RuO{sub 2} films via photoemission spectroscopy are presented. These experiments give insight into the band alignment, growth behavior, surface structure termination, and dipole formation. The experiments were performed in an integrated vacuum system attached to a home-built, stop-flow type ALD reactor without exposing the samples to the ambient in between deposition and analysis. Bis(ethylcyclopentadienyl)ruthenium(II) was used as precursor and oxygen as reactant. The analysis chamber was outfitted with X-ray photoemission spectroscopy (LIXPS, XPS). The determined growth modes are consistent with a strong growth inhibition situation with a maximum average growth rate of 0.21 Å/cycle for RuO{sub 2} and 0.04 Å/cycle for Ru.{sup 0} An interface dipole of up to −0.93 eV was observed, supporting the assumption of a strongly physisorbed interface. A separate experiment where the surface of a RuO film was sputtered suggests that the surface is terminated by an intermediate, stable, non-stoichiometric RuO{sub 2}/OH compound whose surface is saturated with hydroxyl groups.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Angle-resolved photoemission with circularly polarized light in the nodal mirror plane of underdoped Bi 2 Sr 2 CaCu 2 O 8+ δ superconductor

Unraveling the nature of pseudogap phase in high-temperature superconductors holds the key to understanding their superconducting mechanisms and potentially broadening their applications via enhancement of their superconducting transition temperatures. Angle-resolved photoemission spectroscopy (ARPES) experiments using circularly polarized light have been proposed to detect possible symmetry breaking state in the pseudogap phase of cuprates. Here, the presence (absence) of an electronic order which breaks mirror symmetry of the crystal would in principle induce a finite (zero) circular dichroism in photoemission. Different orders breaking reflection symmetries about different mirror planes can also be distinguished by the momentum dependence of the measured circular dichroism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A cryogenically cooled high voltage DC photoemission electron source

Linear electron accelerators and their applications such as ultrafast electron diffraction require compact high-brightness electron sources with high voltage and electric field at the photocathode to maximize the electron density and minimize space-charge induced emittance growth. Achieving high brightness from a compact source is a challenging task because it involves an often-conflicting interplay between various requirements imposed by photoemission, acceleration, and beam dynamics. Here we present a new design for a compact high voltage DC electron gun with a novel cryogenic photocathode system and report on its construction and commissioning process. This photoemission gun can operate at ~200 kV at both room temperature and cryogenic temperature with a corresponding electric field of 10 MV/m, necessary for achieving high quality electron beams without requiring the complexity of guns, e.g., based on RF superconductivity. Furthermore, it hosts a compact photocathode plug compatible with that used in several other laboratories opening the possibility of generating and characterizing electron beam from photocathodes developed at other institutions.

47 OTHER INSTRUMENTATION↗

Ultrafast extreme ultraviolet photoemission without space charge

Time- and Angle-resolved photoelectron spectroscopy from surfaces can be used to record the dynamics of electrons and holes in condensed matter on ultrafast time scales. However, ultrafast photoemission experiments using extreme-ultraviolet (XUV) light have previously been limited by either space-charge effects, low photon flux, or limited tuning range. In this article, we describe XUV photoelectron spectroscopy experiments with up to 5 nA of average sample current using a tunable cavity-enhanced high-harmonic source operating at 88 MHz repetition rate. The source delivers >1011 photons/s in isolated harmonics to the sample over a broad photon energy range from 18 to 37 eV with a spot size of 58 × 100 μm2. From photoelectron spectroscopy data, we place conservative upper limits on the XUV pulse duration and photon energy bandwidth of 93 fs and 65 meV, respectively. The high photocurrent, lack of strong space charge distortions of the photoelectron spectra, and excellent isolation of individual harmonic orders allow us to observe laser-induced modifications of the photoelectron spectra at the 10−4 level, enabling time-resolved XUV photoemission experiments in a qualitatively new regime.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Sub-threshold ultrafast one-photon photoemission from a Cu(111) photocathode

Single-photon photoemission of electrons for incident photon energies below the surface work function is reported for a single-crystal Cu(111) photocathode. Spectral characterization of the quantum efficiency and mean transverse energy of the emitted electrons is shown to be consistent with emission from a thermalized hot electron distribution photoexcited on sub-picosecond time scales into an upper conduction band at the L-point of the Brillouin zone of copper. To our knowledge, this is the first time that such excited-state thermionic emission has been observed from a planar metal photocathode, and then from a commonly used photocathode material. The results, therefore, indicate the potential importance of such band structure dependent sub-threshold photoemission mechanisms on the performance of photocathodes employed for the generation of short electron pulses using sub-picosecond laser pulses. Consequently, the combined experimental and theoretical work presented in this paper contributes to solid-state photocathode-based research aimed at our understanding and selection (or discovery) of high brightness photo-electron sources required for many electron-based diffraction, imaging, and accelerator applications.

43 PARTICLE ACCELERATORS↗

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↗

Unraveling intrinsic correlation effects with angle-resolved photoemission spectroscopy

Interaction effects can change materials properties in intriguing ways, and they have, in general, a huge impact on electronic spectra. In particular, satellites in photoemission spectra are pure many-body effects, and their study is of increasing interest in both experiment and theory. However, the intrinsic spectral function is only a part of a measured spectrum, and it is notoriously difficult to extract this information, even for simple metals. Our joint experimental and theoretical study of the prototypical simple metal aluminum demonstrates how intrinsic satellite spectra can be extracted from measured data using angular resolution in photoemission. A nondispersing satellite is detected and explained by electron–electron interactions and the thermal motion of the atoms. Additional nondispersing intensity comes from the inelastic scattering of the outgoing photoelectron. The ideal intrinsic spectral function, instead, has satellites that disperse both in energy and in shape. Theory and the information extracted from experiment describe these features with very good agreement.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Tracking surface photovoltage dipole geometry in Bi 2 Se 3 with time-resolved photoemission

Topological insulators have been shown to exhibit strong and long-lived surface photovoltages when excited by an infrared pump. The ability to generate long-lived potentials on these surfaces provides opportunities to manipulate the spin-momentum locked topological surface states. Moreover, the photo-induced nature of this effect allows for localized excitation of arbitrary geometries. Knowing precisely how these potentials form and evolve is critical in understanding how to manage the effect in applications. The uniqueness of the photoemission experimental geometry, in which the photoelectron must traverse the induced surface field in vacuum, provides an interesting probe of the electric dipole shape generated by the surface photovoltage. In this study, we are able to match the observed decay of the geometric effect on the photoelectron to an essential electrodynamics model of the light-induced dipole thereby tracking the fluence-dependent evolution of the dipole geometry. Finally, by utilizing a standard time-resolved angle-resolved photoemission experiment, we are able to determine real-space information of the dipole while simultaneously recovering time-resolved band structure.

42 ENGINEERING↗