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DOE OSTI2025

Second harmonic Bessel-Gauss beam shaping with elliptic axicon aberrations

The second harmonic (SH) of an axicon generated Bessel-Gauss beam is created through the nonlinear interaction of photons with a crystal, resulting in the energy doubling of the output photons. In this work, we show experimentally that in addition to frequency doubling, the SH of Bessel-Gauss beams under asymmetric aberrations from an elliptic axicon exhibit intriguing beam formation. Particularly, the central region of the SH beam profile is composed of two central spots of various geometries surrounded by nested ellipses; one of which is the configuration of two central gamma dots with similar radius knotted by nested ellipses for a zeroth-order Bessel-Gauss pump. These SH beams consistently maintain their spatial profile throughout propagation, reminiscing the behavior of screw dislocations in wave patterns. Our numerical simulations produce beam dynamics consistent with that of experiments and further implicate the remarkable interweaving of bright spots with dark vortices. This is especially noticeable when the beams dynamically oscillate along the optical axis, resulting in the genesis of spatially polarized beams with a knotted framework. The insights gained from our study establish a novel paradigm for exploring interactions of Bessel-like beams with vortex dynamics. This, in turn, has the potential to spark innovations in optical applications, fostering new methodologies to harness and manipulate complex light structures. Our experimental findings could spur new methods of generating logical states of light and new opportunities for material processing control. Published by the American Physical Society 2025

Wang, Tianhong (ORCID:0000000169104201)↗

DOE OSTI2025

Valence Electron Distributions from Sub-Angstrom Convergent Beam Electron Diffraction

Modern aberration-corrected scanning transmission electron microscopes can acquire four-dimensional data sets (“4D STEM”) by recording convergent beam electron diffraction (CBED) patterns, using precisely positioned, sub-angstrom probes. Here, we demonstrate that these patterns can probe the site symmetry, atomic displacements, and valence electron distributions at individual atomic columns. To this end, 4D STEM CBED patterns were acquired from SrTiO 3 single crystals and compared with patterns calculated using scattering potentials derived from density functional theory. Here, we show that an aspherical valence electron charge build-up at the oxygen sites causes intensity asymmetries in the low-angle scattering portion of the patterns. Using strained SrTiO 3 films containing subtle polar displacements within nanometer-sized domains, it is shown that the high-angle scattering portion in each pattern is sensitive to atomic displacements.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Rapid Demonstration of Bremsstrahlung Diode Optimization

Optimization of the radiation pattern from a Bremsstrahlung target for a given application is possible by controlling the electron beam that impacts the high-atomic-number target. In this work, the electron beam is generated by a 13MV vacuum diode that terminates a coaxial magnetically insulted transmission line (MITL) on the HERMES-III machine at Sandia National Labs. Work by Sanford introduced a geometry for vacuum diodes that can control the flow within bounds. The "indented anode", as coined by Sanford, can straighten out the electron beam in a high-current diode that would otherwise be prone to beam pinching. A straighter beam will produce a more forwardly directed radiation pattern while a pinching electron beam will yield a focal point or hot spot on axis and a more diffuse radiation pattern. Either one of these may be desirable depending on the application. This work serves as a first attempt to optimize the radiation pattern in the former sense of collimating the radiation pattern given a limited parameter space. The optimization is attempted first using electromagnetic particle-in-cell simulations in the EMPIRE code suite. The setup of the models used in EMPIRE is discussed along with some basic theory behind some of the models used in the simulations such as anode heating and secondary ions. Theoretical work performed by Allen Garner and his students at Purdue is included here, which concerns the impact of collisions in these vacuum diodes. The EMPIRE simulations consider both an aggressive and a conservative design. The aggressive design is inherently riskier while the conservative design is chosen as something that, while still a risk, is more likely to perform as expected. The ultimate goal of this work was to validate the EMPIRE code results with experimental data. While the experiment that tested the diode designs proposed by the simulation results fell outside of the fiscal boundaries of this project (and for that reason the results of which are not included in this report), the hardware for the experiment was designed and drafted within those same fiscal boundaries, and is thus included in this report. However, there was yet another experiment performed in this project that tested a key feature of the diode: the hemispherical cathode. Those results are documented here as well, which show that the cathode tip is an important aspect to controlling the diode flow. A short series of simulations on this diode were also performed after the experiment in order to gain a better understanding of the effect of ions. on the flow pattern and faceplate dose profile.

43 PARTICLE ACCELERATORS↗

DOE OSTI2023

Direct LiF imaging diagnostics on refractive X-ray focusing at the EuXFEL High Energy Density instrument

The application of fluorescent crystal media in wide-range X-ray detectors provides an opportunity to directly image the spatial distribution of ultra intense X-ray beams including investigation of the focal spot of free-electron lasers. Here the capabilities of the micro- and nano-focusing X-ray refractive optics available at the High Energy Density instrument of the European XFEL are reported, as measured in situ by means of a LiF fluorescent detector placed into and around the beam caustic. The intensity distribution of the beam focused down to several hundred nanometers was imaged at 9 keV photon energy. A deviation from the parabolic surface in a stack of nanofocusing Be compound refractive lenses (CRLs) was found to affect the resulting intensity distribution within the beam. Comparison of experimental patterns in the far field with patterns calculated for different CRL lens imperfections allowed the overall inhomogeneity in the CRL stack to be estimated. The precise determination of the focal spot size and shape on a sub-micrometer level is essential for a number of high energy density studies requiring either a pin-size backlighting spot or extreme intensities for X-ray heating.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

THz Radar Observations of Hydrometeors in a Spray Chamber

Abstract A THz radar, with its wide bandwidth, is capable of high‐resolution imaging down to the centimeter scale. In this study, a THz radar is applied to detect hydrometeors generated in a spray chamber. The observed backscattering signals show fluctuations at centimeter scales, indicating various hydrometeor distribution patterns along the radar beam. A co‐located High‐Speed Imaging (HSI) sensor is used to measure the Drop Size Distributions (DSD) in the spray chamber. The radar sampling beam is well aligned with the HSI probes, allowing an objective comparison between the remote sensing and in situ observations. In this study, the observed radar power is compared with the power estimated from the HSI measurements. Results show great consistency, with power difference smaller than 0.5 dB. This study demonstrates the feasibility and great potential of using a THz radar for ultra‐high‐resolution observations of clouds in a laboratory facility, and in the real atmosphere.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Development of a Beam Sweeping System for the Fermilab Antiproton Source Target

Intensity of the incident 120-GeV proton beam on the antiproton production target is scheduled to increase to 5x10 12 protons per pulse. To prevent damage to the target, we plan to spread the hot spot on target with a beam sweeping system, Now under development are rotating-field magnets for installation upstream and downstream of the target. These magnets will deflect the beam in a circular pattern on the target. Peak current of 7 kA and peak voltage drop of 6 kV are expected. The power supply, which is separated from the magnet by a distance of about 10 m, utilizes magnetic pulse compression by saturating inductors to drive the magnets through the long transmission lines.

43 PARTICLE ACCELERATORS↗

DOE OSTI2022

Laser pulse shaping for additive manufacturing

The present disclosure relates to an apparatus for additively manufacturing a product in a layer-by-layer sequence, wherein the product is formed using powder particles deposited on an interface layer of a substrate. A laser generates first and second beam components. The second beam component has a higher power level and a shorter duration than the first beam component. A mask creates a 2D optical pattern in which only select portions of the second beam components can irradiate the powder particles. The first beam component heats the powder particles close to a melting point, where the particles experience surface tension forces relative to the interface layer. While the particles are heated, the second beam component further heats the particles and also melts the interface layer before the surface tension forces can act on and distort the particles, enabling the particles and the interface layer are able to bond together.

DeMuth, James A.↗

DOE OSTI2023

Laser pulse shaping for additive manufacturing

DeMuth, James A.↗

DOE OSTI2021

Heat treatment to anneal residual stresses during additive manufacturing

The present disclosure relates to a method of producing a product through additive manufacturing with heat treatment. The method involves using a fusing beam to melt powder particles disposed on a substrate, where the fusing beam is impressed with a two dimensional pattern containing image information from a first layer to be printed. The fused powder particles are then heat treated with a beam impressed with an additional two dimensional pattern. The additional two dimensional pattern has image information from the first layer to achieve heat treatment of the product. The heat treatment is completed prior to laying down additional new layers of material. The heat treatment is an annealing operation. The method may further involve providing a new layer of powdered material on top of the layer of fused powder particles subsequent to the heat treatment, and repeating the melting and heat treating operations in a layer-by-layer fashion using the two dimensional pattern and the additional two dimensional pattern, until the part is completed.

DeMuth, James A.↗

DOE OSTI2026

Unsupervised anomaly detection in MeV ultrafast electron diffraction

MeV ultrafast electron diffraction (MUED) is a pump-probe technique used to study the dynamic structural evolution of materials. An ultrashort laser pulse triggers structural changes, which are then probed by an ultrashort relativistic electron beam. To overcome low signal-to-noise ratios, diffraction patterns are averaged over thousands of shots. However, shot-to-shot instabilities in the electron beam can distort individual patterns, introducing uncertainty. Improving MUED accuracy requires detecting and removing these anomalous patterns from large datasets. In this work, we developed a fully unsupervised methodology for the detection of anomalous diffraction patterns. Using a convolutional autoencoder, we calculate the reconstruction mean squared error of the diffraction patterns. Based on the statistical analysis of this error, we provide the user an estimation of the probability that the pattern is normal, which also allows a posterior visual inspection of the images that are difficult to classify. This method has been trained with only 100 diffraction patterns and tested on 1521 patterns, resulting in a false positive rate between 0.2% and 0.4%, with a training time of 10 s per image and a test time of about 1 s per image. Here, the proposed methodology can also be applied to other diffraction techniques in which large datasets are collected that include faulty images due to instrumental instabilities.

43 PARTICLE ACCELERATORS↗

DOE OSTI2024

Selected Area Manipulation of MoS 2 via Focused Electron Beam-Induced Etching for Nanoscale Device Editing

Here we demonstrate direct-write patterning of single and multilayer MoS 2 via a focused electron beam-induced etching (FEBIE) process mediated with the XeF 2 precursor. MoS 2 etching is performed at various currents, areal doses, on different substrates, and characterized using scanning electron and atomic force microscopies as well as Raman and photoluminescence spectroscopies. Scanning transmission electron microscopy reveals a sub-40 nm etching resolution and the progression of point defects and lateral etching of the consequent unsaturated bonds. The results confirm that the electron beam-induced etching process is minimally invasive to the underlying material in comparison to ion beam techniques, which damage the subsurface material. Single-layer MoS 2 field-effect transistors are fabricated, and device characteristics are compared for channels that are edited via the selected area etching process. The source–drain current at constant gate and source–drain voltage scale linearly with the edited channel width. Moreover, the mobility of the narrowest channel width decreases, suggesting that backscattered and secondary electrons collaterally affect the periphery of the removed area. Focused electron beam doses on single-layer transistors below the etching threshold were also explored as a means to modify/thin the channel layer. The FEBIE exposures showed demonstrative effects via the transistor transfer characteristics, photoluminescence spectroscopy, and Raman spectroscopy. While strategies to minimize backscattered and secondary electron interactions outside of the scanned regions require further investigation, here, we show that FEBIE is a viable approach for selective nanoscale editing of MoS 2 devices.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Statistical Study of the Nonthermal Continuum Radiation Beaming Angle Measured by the High Frequency Receiver on Van Allen Probes-A

The nonthermal continuum (NTC) radiation beaming angle is computed over the entire Van Allen Probes-A mission when the spacecraft was in the dawn sector. The conditions in the dawn sector are favorable for the wave vector to lie near/in the spacecraft's spin plane allowing a favorable estimate of the beaming angle, and the dawn sector is also advantageous in that previous studies show NTC occurrence to peak in this sector. We found that scatter plots, over the entire mission, of beaming angle versus magnetic latitude form a distinct inverted-V pattern, with the apex at/near the magnetic equator. This pattern was sharpest for frequencies ( f ) ≲ 100 kHz. Using the NTC beaming formula from the linear mode conversion theory (LMCT), we show that such an inverted-V pattern is expected due to the large variation in the plasmapause location over the entire mission. The theoretical derived pattern qualitatively reproduces the observed pattern but not quantitatively. The lack of quantitative agreement is discussed and is attributed to several factors, one factor is off-centered emissions from the radio window. The qualitative agreement strongly supports LMCT as being the dominant mechanism generating NTC for f ≲ 100 kHz. For f ≳ 100 kHz, the inverted-V pattern becomes less distinct, and strong near-equatorial beaming is observed. Finally, after considering contamination of our selections by left-handed polarized AKR, our study suggests that besides LMCT another unidentified NTC generation mechanism becomes important for f ≳ 100 kHz.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

Large-Angle Rocking Beam Electron Diffraction of Large Unit Cell Crystals Using Direct Electron Detector

We report a large-angle rocking beam electron diffraction (LARBED) technique for electron diffraction analysis. Diffraction patterns are recorded in a scanning transmission electron microscope (STEM) using a direct electron detector with large dynamical range and fast readout. We use a nanobeam for diffraction and perform the beam double rocking by synchronizing the detector with the STEM scan coils for the recording. Using this approach, large-angle convergent beam electron diffraction (LACBED) patterns of different reflections are obtained simultaneously. By using a nanobeam, instead of a focused beam, the LARBED technique can be applied to beam-sensitive crystals as well as crystals with large unit cells. Here, this paper describes the implementation of LARBED and evaluates the performance using silicon and gadolinium gallium garnet crystals as test samples. We demonstrate that our method provides an effective and robust way for recording LARBED patterns and paves the way for quantitative electron diffraction of large unit cell and beam-sensitive crystals.

4DSTEM↗

DOE OSTI2021

Revealing the Three-Dimensional Orientation and Interplay between Plasmons and Interband Transitions for Single Gold Bipyramids by Photoluminescence Excitation Pattern Imaging

Gold bipyramids (AuBPs) attract significant attention due to the large enhancement of the electric field around their sharp tips and well-defined tunability of their plasmon resonances. Excitation patterns of single AuBPs are recorded using raster-scanning confocal microscopy combined with radially and azimuthally polarized laser beams. Photoluminescence spectra (PL) and excitation patterns of the same AuBP are acquired with three different excitation wavelengths. Here, the isotropic excitation patterns suggest that the AuBPs are mainly excited by interband transitions with 488/530 nm radiation, while excitation patterns created with a 633 nm laser exhibit a double lobed shape that indicates a single dipole excitation process associated with the longitudinal plasmon resonance mode. We are able to determine the three-dimensional orientation of single AuBPs nonperturbatively by comparing experimental patterns with theoretical simulations. The asymmetric patterns show that the AuBPs are lying on the substrate with an out-of-plane tilt angle of around 10° to 15°.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

FEgen (v.1): Field Emission Distribution Generator Freeware Based on Fowler–Nordheim Equation

This work presents an open-source code, FEgen, that generates initial field emission distributions based on the time-dependent Fowler–Nordheim equation. Current in-demand and open-source beam tracking software—such as ASTRA, IMPACT-T, and GPT—do not contain native distribution generator functions suitable for field emitted electron tracking and phase space analysis. Furthermore, the intuitive graphical user interface of FEgen generates input files shown to be fully compatible with both ASTRA and GPT. Here, detailed application examples demonstrating a subset of FEgen’s capabilities are given by creating a customized emitter pattern with application to transverse beam shaping and longitudinal beam dynamic experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Multi-physics modeling of grain growth during solidification in electron beam additive manufacturing of Inconel 718

While experimental work has shown promising results regarding control of additive manufacturing metal grain structure, the effects of processing parameters on the grain structure is difficult to understand and predict from experiment alone. To this end, a modeling framework is developed which sequentially couples a macro-scale, semi-analytic thermal model, and a meso-scale, cellular automata-based microstructure model. This framework is applied to electron beam additive manufacturing of Inconel 718 using a complex spot scan pattern. The model shows that, with the same scan pattern, variations in the spot time and electron-beam current produce thermal histories with significant spatial and temporal differences, which then produce complex solidification conditions from the interplay between molten pools in the same layer and subsequent layers, resulting in vastly different grain structures. Additionally, it is noted that the framework can significantly reduce the computational expenses for coupled thermal-metallurgical problems, and has the potential to be used for component level problems.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Additive Lithography–Organic Monolayer Patterning Coupled with an Area-Selective Deposition

The combination of area-selective deposition (ASD) with a patternable organic monolayer provides a versatile additive lithography platform, enabling the generation of a variety of nanoscale feature geometries. Stearate hydroxamic acid self-assembled monolayers (SAMs) were patterned with extreme ultraviolet (λ = 13.5 nm) or electron beam irradiation and developed with ASD to achieve line space patterns as small as 50 nm. Density functional theory was employed to aid in the synthesis of hydroxamic acid derivatives with optimized packing density to enhance the imaging contrast and improve dose sensitivity. Near-edge X-ray absorption fine structure spectroscopy and infrared spectroscopy reveal that the imaging mechanism is based on improved deposition inhibition provided by the cross-linking of the SAM to produce a more effective barrier during a subsequent deposition step. With patterned substrates composed of coplanar copper lines and silicon spacers, hydroxamic acids selectively formed monolayers on the metal portions and could undergo a pattern-wise exposure followed by ASD in the first combination of a patternable monolayer with ASD. This material system presents an additional capability compared to traditional ASD approaches that generally reflect a starting patterned surface. Finally, this bottoms-up additive approach to lithography may be a viable alternative to subtractive nanoscale feature generation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

2D monochromatic x-ray imaging for beam monitoring of an x-ray free electron laser and a high-power femtosecond laser

Single-shot simultaneous beam monitoring of an x-ray free electron laser (XFEL) and a high-power femtosecond laser is demonstrated using 2D monochromatic Kα imaging. In a pump-probe experiment carried out at the Matter in Extreme Conditions end-station of the Linac Coherent Light Source, a thin solid titanium foil irradiated by a 25-TW relativistic intensity laser for fast electron isochoric heating was probed by a 7.0 keV XFEL beam for x-ray Thomson scattering measurements. Using a spherical crystal imager (SCI), the spatial overlap of the beams was examined by measuring 4.5 keV titanium Kα x rays produced by laseraccelerated fast electrons and the x-ray beam. Changes in XFEL-induced Kα emission patterns were observed down to a ~20×40 μm2 rectangular shape as the beam was focused. Laser-only and two-beam shots reveal that large spatial offsets of laser-induced Kα spots in a horizontal direction is attributed to imprecise target positioning rather than shot-to-shot laser pointing variations. As a consequence, successful beam overlapping was observed on ~58% of all two-beam shots for 10 μm thick samples. The Kα measurements also show a linear relationship between total Kα yields and integrated x-ray scattering signals. Monochromatic xray imaging with SCI could be used as an on-shot beam pointing diagnostic in XFEL-laser or multiple short-pulse laser experiments.

47 OTHER INSTRUMENTATION↗