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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 OSTI2024

Wehnelt photoemission in an ultrafast electron microscope: Stability and usability

We tested and compared the stability and usability of three different cathode materials and configurations in a thermionic-based ultrafast electron microscope: (1) on-axis thermionic and photoemission from a custom 100 μm diameter LaB 6 source with a graphite guard ring, (2) off-axis photoemission from the Ni aperture surface of the Wehnelt electrode, and (3) on-axis thermionic and photoemission from a custom 200 μm diameter polycrystalline Ta source. For each cathode type and configuration, including the Ni Wehnelt aperture, we illustrate how the photoelectron beam-current stability is deleteriously impacted by simultaneous cooling of the source following thermionic heating. Furthermore, we demonstrate usability via collection of parallel- and convergent-beam electron diffraction patterns and by formation of the optimum probe size. We find that usability of the off-axis Ni Wehnelt-aperture photoemission is at least comparable to on-axis LaB 6 thermionic emission, as well as to on-axis photoemission [the heretofore conventional approach to ultrafast electron microscopy (UEM) in thermionic-based instruments]. However, the stability and achievable beam currents for off-axis photoemission from the Wehnelt aperture were superior to that of the other cathode types and configurations, regardless of the electron-emission mechanism. Beam-current stability for this configuration was found to be ±1% (one standard deviation from the mean) for 70 min (longest duration tested), and steady-state beam current was reached within the sampling-time resolution used here (~1 s) for 15 pA beam currents (i.e., 460 electrons per packet for a 200 kHz repetition rate). Repeatability and robustness of the steady-state condition were also found to be within ±1% of the mean. We discuss the implications of these findings for UEM imaging and diffraction experiments, for pulsed-beam damage measurements, and for practical switching between optimum conventional TEM and UEM operation within the same instrument.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

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↗
DOE OSTI2025

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)↗
DOE OSTI2025

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 (↗
DOE OSTI2025

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↗
DOE OSTI2025

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↗
DOE OSTI2026

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↗
DOE OSTI2025

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↗
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)↗
DOE OSTI2025

Quasiparticle description of angle-resolved photoemission spectroscopy for SrCuO 2

SrCuO 2 has long been considered a near-archetypal realization of a quasi-one-dimensional (1D) system of interacting electrons with short-range interactions. Within this framework, experimental observations - interpreted through the lens of the 1D Hubbard model - suggest that electron and hole excitations decay into two types of (unphysical) collective bosonic modes: "spinons", which carry the spin degree of freedom, and "holons", which carry the charge degree of freedom. This model, known as spin-charge separation, is most directly evidenced by angle-resolved photoemission spectroscopy (ARPES), where a photo-induced hole decays into a continuum of these excitations. Here we present an alternative perspective grounded in first-principles, self-consistent, and parameter-free many-body perturbation theory. In this revised quasiparticle framework, ARPES can be understood as a one-body effect arising from mild disorder in a long-range antiferromagnetic ground state. the emergence of the so-called spinon branch arises naturally from spin disorder, the anomalous linewidths are accurately captured, and we provide a compelling explanation for the spectral weight observed at the non-magnetic zone boundary. This reinterpretation provides a unified explanation for key experimental signatures previously attributed to spin-charge separation, including features observed in optical conductivity. Additionally, we show that SrCuO 2 exhibits a nontrivial interchain coupling that significantly influences both its one-particle and two-particle spectral functions. By comparing the spectral features of SrCuO 2 with those of La 2 CuO 4 , we argue that SrCuO 2 shares notable similarities with the two-dimensional cuprates-both being rooted in a common CuO 4 plaquette-based molecular orbital framework.

1D cuprates↗
DOE OSTI2025

Detecting thermodynamic phase transition via explainable machine learning of photoemission spectroscopy

Identifying thermodynamic signatures of electronic phases, such as superconductivity, is challenging in low-dimensional materials due to strong fluctuations and low probing volume. Spectroscopic methods are often used to identify new bulk phases, but their main measurable quantity—electronic energy gaps—is no longer an effective order parameter in low-dimensional and fluctuating systems. Combining angle-resolved photoemission with a domain-adversarial neural network, we report a data-driven method to identify thermodynamic phase transitions solely based on single-particle spectra. We demonstrate 97.6% accuracy in cuprate superconductor Bi 2 Sr 2 CaCu 2 O 8+δ with strong superconducting fluctuations. This model notably compensates for the scarcity of experimental data by leveraging virtually inexhaustible simulated data. Further, its explainability reveals the crucial role of in-gap spectral weight in detecting phase fluctuations and thermodynamic transitions. Our work pinpoints the spectroscopic signatures of fluctuating orders and enables using spectroscopy for machine-learning-assisted material discovery for low-dimensional and strong coupling systems.

2D materials↗
DOE OSTI2025

Sub-tesla On-Chip Nanomagnetic Metamaterial Platform for Angle-Resolved Photoemission Spectroscopy

Magnetically controlled states in quantum materials are central to their unique electronic and magnetic properties. However, direct momentum-resolved visualization of these states via angle-resolved photoemission spectroscopy (ARPES) has been hindered by the disruptive effect of magnetic fields on photoelectron trajectories. Here, we introduce an in situ method that is, in principle, capable of applying magnetic fields up to 1 T. This method uses substrates composed of nanomagnetic metamaterial arrays with alternating polarity. Such substrates can generate strong, homogeneous, and spatially confined fields applicable to samples with thicknesses up to the micron scale, enabling ARPES measurements under magnetic fields with minimal photoelectron trajectory distortion. Here, we demonstrate this minimal distortion with ARPES data taken on monolayer graphene. Our method paves the way for probing magnetic field-dependent electronic structures and studying field-tunable quantum phases with state-of-the-art energy-momentum resolutions.

Magnetic properties↗
DOE OSTI2024

Polarization-dependent photoemission electron microscopy for domain imaging of inorganic and molecular materials

Polarization-dependent photoemission electron microscopy (PD-PEEM) exploits spatial variation in the optical selection rules of materials to image domain formation and material organization on the nanoscale. In this Perspective, we discuss the mechanism of PD-PEEM that results in the observed image contrast in experiments and provide examples of a wide range of material domain structures that PD-PEEM has been able to elucidate, including molecular and polymer domains, local electronic structure and defect symmetry, (anti)ferroelectricity, and ferromagnetism. As a result, we discuss challenges and new directions that are possible with this tool for probing domain structure in materials, including investigating the formation of transient ordered states, multiferroics, and the influence of molecular and polymer order and disorder on excited state dynamics and charge transport.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Model of photoemission and framework for relating quantum efficiency to stoichiometry

Simulating the quantum efficiency (QE) from photocathodes used in accelerators and photoinjectors requires accounting for the properties of the photoemissive material, the optical properties, scattering coefficients, and doping concentrations of which are dependent upon the stoichiometry. We present a rapid and flexible optical model that can be used to investigate the consequences of changes in the dielectric properties and their impact on the QE through such factors as reflectivity and laser penetration depth. Differences in materials can then be characterized by changes to parameters used to evaluate the dielectric function in a Lorentz–Drude–Resonant model. A method to characterize data is motivated by the example of copper and vetted by application to an exact analytical model. The effects of changes in parameters describing the resonant terms, which aggregate in the visible and UV regions of the spectrum, are shown.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Three-dimensional dispersion in the type-II Dirac semimetals PtTe 2 and PdTe 2 revealed through circular dichroism in angle-resolved photoemission spectroscopy

PtTe 2 and PdTe 2 are among the first transition metal dichalcogenides that were predicted to host type-II Dirac fermions, exotic particles prohibited in free space. These materials are layered and air stable, which makes them top candidates for technological applications that take advantage of their anisotropic magnetotransport properties. Here, in this work, we provide a detailed characterization of the electronic structure of PtTe 2 and PdTe 2 using angle-resolved photoemission spectroscopy (ARPES) and density functional theory calculations, offering an alternative interpretation for one of the Dirac-like dispersions in these materials. Through the use of circularly polarized light, we report a different behavior of such dispersion in PdTe 2 compared to PtTe 2 , that we relate to a symmetry analysis of the dipole matrix element. Such analysis reveals a link between the observed circular dichroism and the different momentum-dependent terms in the dispersion of these two compounds, despite their close similarity in crystal structure. Additionally, our data show a clear difference in the circular dichroic signal for the type-II Dirac cones characteristic of these materials, compared to their topologically protected surface states. Our paper provides a useful reference for the ARPES characterization of other transition metal dichalcogenides with topological properties and illustrates the use of circular dichroism as a guide to identify the topological character and attributes of two otherwise equivalent band dispersions.

angle-resolved photoemission spectroscopy↗
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 OSTI2025

Influence of Photoemission Geometry on Timing and Efficiency in 4D Ultrafast Electron Microscopy

Broader adoption of 4D ultrafast electron microscopy (UEM) for the study of chemical, materials, and quantum systems is being driven by development of new instruments as well as continuous improvement and characterization of existing technologies. Perhaps owing to the still-high barrier to entry, the full range of capabilities of laser-driven 4D UEM instruments has yet to be established, particularly when operated at extremely low beam currents (~fA). Accordingly, with an eye on beam stability, we have conducted particle tracing simulations of unconventional off-axis photoemission geometries in a UEM equipped with a thermionic-emission gun. Specifically, we have explored the impact of experimentally adjustable parameters on the time-of-flight (TOF), the collection efficiency (CE), and the temporal width of ultrashort photoelectron packets. The adjustable parameters include the Wehnelt aperture diameter (DW), the cathode set-back position (Ztip), and the position of the femtosecond laser on the Wehnelt aperture surface relative to the optic axis (Rphoto). Notable findings include significant sensitivity of TOF to DW and Ztip, as well as non-intuitive responses of CE and temporal width to varying Rphoto. As a means to improve accessibility, practical implications and recommendations are emphasized wherever possible.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗