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DOE OSTI2019

Plasmonic Lenses for Tunable Ultrafast Electron Emitters at the Nanoscale

Simultaneous spatio-temporal confinement of energetic electron pulses to femtosecond and nanometer scales is a topic of great interest in the scientific community, given the potential im- pact of such development on a wide spectrum of scientific and industrial applications. For example, in ultrafast electron scattering, nanoscale probes would enable accurate maps of structural dynamics in materials with nanoscale heterogeneity, thereby understanding the role of boundaries and defects on macroscopic properties. On the other hand, advances in this field are mostly limited by the electron source brightness and size. We present the design, fabrication, and optical characterization of bullseye plasmonic lenses for next-generation ultrafast electron sources. Using electromagnetic simulations, we examine how the interplay between light-plasmon coupling, plasmon propagation, dispersion, and resonance governs the properties of the photoemitted electron pulse. We also illus- trate how the pulse duration and strength can be tuned by geometric design, and predict sub-10 fs pulses with nanoscale diameter can be achieved. We then fabricated lenses in gold films and char- acterized their plasmonic properties with cathodoluminescence spectromicroscopy, demonstrating suitable plasmonic behavior for ultrafast, nanoscale photoemission.

43 PARTICLE ACCELERATORS↗

DOE OSTI2019

Superradiance in the Generalized (Non-Wiener) Dicke Model

It is shown that when nonresonant interactions between atoms and a vacuum electromagnetic field are included in analysis of emission of a localized ensemble of identical atoms, a delay must appear in the cooperative radiation pulse emitted by the atomic ensemble that is initially in a half-excited state. At the same time, the emission of cooperative radiation from a completely excited ensemble for certain parameters must begin without any delay. This contradicts the familiar facts of the conventional Dicke superradiance, in the theory of which nonresonant interactions are disregarded. The model taking into account nonresonant interactions along with other factors of the Dicke model is called the generalized Dicke model.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2023

Laser Ablation Plasmas and Spectroscopy for Nuclear Applications

The development of measurement methodologies to detect and monitor nuclear-relevant materials remains a consistent and significant interest across the nuclear energy, nonproliferation, safeguards, and forensics communities. Optical spectroscopy of laser-produced plasmas is becoming an increasingly popular diagnostic technique to measure radiological and nuclear materials in the field without sample preparation, where current capabilities encompass the standoff, isotopically resolved and phase-identifiable (e.g., UO and UO[Formula: see text]) detection of elements across the periodic table. These methods rely on the process of laser ablation (LA), where a high-powered pulsed laser is used to excite a sample (solid, liquid, or gas) into a luminous microplasma that rapidly undergoes de-excitation through the emission of electromagnetic radiation, which serves as a spectroscopic fingerprint for that sample. This review focuses on LA plasmas and spectroscopy for nuclear applications, covering topics from the wide-area environmental sampling and atmospheric sensing of radionuclides to recent implementations of multivariate machine learning methods that work to enable the real-time analysis of spectrochemical measurements with an emphasis on fundamental research and development activities over the past two decades. Background on the physical breakdown mechanisms and interactions of matter with nanosecond and ultrafast laser pulses that lead to the generation of laser-produced microplasmas is provided, followed by a description of the transient spatiotemporal plasma conditions that control the behavior of spectroscopic signatures recorded by analytical methods in atomic and molecular spectroscopy. High-temperature chemical and thermodynamic processes governing reactive LA plasmas are also examined alongside investigations into the condensation pathways of the plasma, which are believed to serve as chemical surrogates for fallout particles formed in nuclear fireballs. Laser-supported absorption waves and laser-induced shockwaves that accompany LA plasmas are also discussed, which could provide insights into atmospheric ionization phenomena from strong shocks following nuclear detonations. Furthermore, the standoff detection of trace radioactive aerosols and fission gases is reviewed in the context of monitoring atmospheric radiation plumes and off-gas streams of molten salt reactors. Finally, concluding remarks will present future outlooks on the role of LA plasma spectroscopy in the nuclear community.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Effect of self-generated magnetic fields on x-ray emission in Kr-filled targets at the National Ignition Facility

We examine the effects of self-generated magnetic fields in a Kr gas pipe x-ray source platform. X-ray emission from Kr plasma is dependent on the plasma conditions, as the ionization state is largely a function of temperature. Magnetic fields are known to limit heat conduction, which increases temperature. We show that the emission in simulations of the gas pipe x-ray source is dependent on how self-generated magnetic fields are modeled. The inclusion of self-generated magnetic fields in simulations more accurately captures the emission of lower energy x-ray emission (L-shell), bringing results closer to experiments. The modeled x-ray emission and self-generated magnetic fields are shown to be particularly sensitive to the inclusion of the Nernst effect in simulations. Severely limiting the Nernst effect leads to a hotter Kr plasma, which can account for the discrepancy seen in earlier studies. By modifying the Nernst effect multiplier, we can achieve better experimental agreement in x-ray emission from gas pipes; the value of the multiplier that leads to the best agreement is dependent on the laser power of the drive. Currently, the suppression factor of the Nernst effect needed for high power drives (PL>200 TW) is more restrictive than what is currently put forward by non-local models.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Towards isolated attosecond electron bunches using ultrashort-pulse laser-solid interactions

We investigate MeV-level attosecond electron bunches from ultrashort-pulse laser-solid interactions through similarities between experimental and simulated electron energy spectra. We show measurements of the bunch duration and temporal structure from particle-in-cell simulations. The experimental observation of such bunches favors specular reflection direction when focusing the laser pulse onto a subwavelength boundary of thick overdense plasmas at grazing incidence. Particle-in-cell simulation further reveals that the attosecond duration is a result of ultra-thin (~tenth of a micron) gaps of zero electromagnetic energy density in the modulated reflected radiation, while the bunching (locally peaked electron concentration) comes from the highly-directional electron angular distribution acquired by the electrons in a grazing incidence setup. To isolate a single electron bunch, we perform simulations using 1-cycle laser pulses and analyze the effect of carrier-envelop phase with particle tracking. The duration of the electron bunch can be further decreased by increasing the laser intensity and the focal spot size, while its direction can be changed by tuning the preplasma density gradient.

High-harmonic generation↗

DOE OSTI2020

Nanoparticle-Enhanced Plasma Discharge Using Nanosecond High-Voltage Pulses

By discharging nanosecond high-voltage (5 kV) pulses across an insulating substrate containing Au, Pt, or Cu nanoparticles, a 3 order of magnitude (1000×) enhancement in the generation of plasma can be achieved through local field enhancement on the surface of the nanoparticles. The low-temperature nature of this transient plasma is crucial to maintaining the structural integrity of these delicate nanoparticles. These nanoparticles provide up to a 1000-fold enhancement in the generation of the plasma, which is localized to the surface of the nanoparticles where it is potentially useful (e.g., for catalysis). Additionally, we performed both time-domain and frequency-domain calculations of the electromagnetic response of the nanoparticles based on high-resolution transmission electron microscope (HRTEM) images, which show local field enhancement of the nanosecond high-voltage pulse on the order of 3×. Since the plasma initiation depends exponentially on the peak electric field strength, this 3-fold increase in the local electric field can result in a several orders of magnitude increases in the generation of plasma at a given applied external field strength. In order to rule out plasmon-resonance enhancement, which is often associated with small metal nanoparticles, we performed finite difference time domain (FDTD) simulations in the optical frequency domain, which show that the effect of plasmon resonance is negligible for Pt nanoparticles. We therefore attribute the nanoparticle-based enhancement to the generation of plasma (an electrostatic effect) rather than enhanced coupling of light from the near field to the far field via the plasmon resonance phenomenon (an optical effect).

36 MATERIALS SCIENCE↗

DOE OSTI2018

Metasurface-based multi-harmonic free-electron light source

Metasurfaces are subwavelength spatial variations in geometry and material where the structures are of negligible thickness compared to the wavelength of light and are optimized for far-field applications, such as controlling the wavefronts of electromagnetic waves. Here, we investigate the potential of the metasurface near-field profile, generated by an incident few-cycle pulse laser, to facilitate the generation of high-frequency light from free electrons. In particular, the metasurface near-field contains higher-order spatial harmonics that can be leveraged to generate multiple higher-harmonic X-ray frequency peaks. We show that the X-ray spectral profile can be arbitrarily shaped by controlling the metasurface geometry, the electron energy, and the incidence angle of the laser input. Using ab initio simulations, we predict bright and monoenergetic X-rays, achieving energies of 30 keV (with harmonics spaced by 3 keV) from 5-MeV electrons using 3.4-eV plasmon polaritons on a metasurface with a period of 85 nm. As an example, we present the design of a four-color X-ray source, a potential candidate for tabletop multicolor hard X-ray spectroscopy. Our developments could help pave the way for compact multi-harmonic sources of high-energy photons, which have potential applications in industry, medicine, and the fundamental sciences.

36 MATERIALS SCIENCE↗

DOE OSTI2017

SIMULATION STUDIES OF A PROTOTYPE STRIPLINE KICKER FOR THE APS-MBA UPGRADE

A prototype dual-blade stripline kicker for the APS multi-bend achromat (MBA) upgrade has been designed and developed. It was optimized with 3D CST Microwave Studio. The high voltage (HV) feedthrough and air-side connector were designed and optimized. Electromagnetic fields along the beam path, the deflecting angle, the high electric fields and their locations were calculated with 15kV differential pulse voltage applied to the kicker blades through the feedthroughs. Beam impedance and the power dissipation on different parts of the kicker and external loads were studied for a 48-bunch fill pattern. Our results show that the prototype kicker with its HV feedthroughs meets the specified requirements. The results of TDR (time-domain reflectometer) test, high voltage pulse test and beam test of the prototype kicker assembly agreed with the simulations.

APS MBA UPGRADE↗

DOE OSTI2021

Characterization of the Redesigned Extended MITL for HERMES III

Modeling and simulation of the legacy HERMES III Magnetically Insulated Transmission Line (MITL) has been performed using EMPHASIS, an unstructured time-domain electromagnetic (UTDEM) particle-in-cell (PIC) simulation software. This design when used lost roughly half of its current before the pulse reached the load. The cause of the current loss in the MITL was found to be the vacuum impedance changes along the MITL. The MITL was then redesigned to maintain constant impedance and simulated in EMPHASIS once again. Following predicting simulation results, the new MITL was then built, installed, and tested, showing minimal current loss and good agreement with simulation and theoretical results, all of which are reported here. Additionally, an analysis of experimental voltage calculation techniques using cathode and anode currents is performed and compared to simulation results.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2019

An inverse free electron laser acceleration-driven Compton scattering X-ray source

Abstract The generation of X-rays and γ-rays based on synchrotron radiation from free electrons, emitted in magnet arrays such as undulators, forms the basis of much of modern X-ray science. This approach has the drawback of requiring very high energy, up to the multi-GeV-scale, electron beams, to obtain the required photon energy. Due to the limit in accelerating gradients in conventional particle accelerators, reaching high energy typically demands use of instruments exceeding 100’s of meters in length. Compact, less costly, monochromatic X-ray sources based on very high field acceleration and very short period undulators, however, may enable diverse, paradigm-changing X-ray applications ranging from novel X-ray therapy techniques to active interrogation of sensitive materials, by making them accessible in energy reach, cost and size. Such compactness and enhanced energy reach may be obtained by an all-optical approach, which employs a laser-driven high gradient accelerator based on inverse free electron laser (IFEL), followed by a collision point for inverse Compton scattering (ICS), a scheme where a laser is used to provide undulator fields. We present an experimental proof-of-principle of this approach, where a TW-class CO 2 laser pulse is split in two, with half used to accelerate a high quality electron beam up to 84 MeV through the IFEL interaction, and the other half acts as an electromagnetic undulator to generate up to 13 keV X-rays via ICS. These results demonstrate the feasibility of this scheme, which can be joined with other techniques such as laser recirculation to yield very compact photon sources, with both high peak and average brilliance, and with energies extending from the keV to MeV scale. Further, use of the IFEL acceleration with the ICS interaction produces a train of high intensity X-ray pulses, thus enabling a unique tool synchronized with a laser pulse for ultra-fast strobe, pump-probe experimental scenarios.

43 PARTICLE ACCELERATORS↗

DOE OSTI2023

Photodissociation of H 2 on Ag and Au Nanoparticles: Effect of Size and Plasmon versus Interband Transitions on Threshold Intensities for Dissociation

This Article provides new insights concerning the simulation of plasmon-driven chemical reactions using real-time TDDFT based on the tight-binding electronic structure code DFTB+, with applications to the dissociation of H 2 on octahedral silver and gold nanoparticles with 19–489 atoms. A new component of these calculations involves sampling a 300 K canonical ensemble to determine the distribution of possible outcomes of the calculations, and with this approach we are able to determine the threshold for dissociation as a function of laser intensity, wavelength, and nanocluster size. We show that the threshold intensity varies as an inverse power of nanocluster size, which makes it possible to extrapolate the results to sizes that are more typical of experimental studies. The intensities obtained from this extrapolation are around a factor of 100 above powers used in the pulsed experiments. This is a closer comparison of theory and experiment than has been obtained in previous real-time simulations, and the remaining discrepancy can be understood in terms of electromagnetic hot spots that are associated with cluster formation. Here, we also compare the influence of plasmon excitation versus interband excitation on reaction thresholds, revealing that for silver clusters plasmon excitation leads to lower thresholds, but for gold clusters interband excitation is more effective. Our study also includes an analysis of charge transfer to and from the H 2 molecule, and a determination of orbital populations during and after the pulse, showing the correlation between metal excitations and the location of the antibonding level of H 2 .

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2020

Direct electron acceleration in multi-kilojoule, multi-picosecond laser pulses

The physics mechanism behind the acceleration of electrons to energies much higher than the laser ponderomotive potential is reported. While electrons with these energies have been observed for the last twenty years at the one percent level, it is only with the recent advent of high power lasers with extended pulse durations, large focal spots, and high intensities that significant numbers (>10%) of the so-called “superponderomotive” electrons have been observed. Evidence is provided that the dominant acceleration mechanism of superponderomotive electrons is direct acceleration by the electromagnetic (EM) wave of the laser as they co-propagate in an under-dense plasma; one-dimensional particle-in-cell simulations yield electron spectra with typically ten times the ponderomotive temperature. Direct acceleration requires tens of plasma wavelengths of under-dense plasma, as well as pulse durations of tens of plasma periods, conditions that can be found in large focal spot multi-picosecond laser pulses. It is shown that the plasma simply provides the source of accelerated electrons and a variety of methods to inject a significant population of electrons into the EM waves at relativistic energy.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

A study of space charge induced non-linearity in the Single Line Of Sight camera

We report a new generation of gated x-ray detectors at the National Ignition Facility has brought faster, enhanced imaging capabilities. Their performance is currently limited by the amount of signal they can be operated with before space charge effects in their electron tube start to compromise their temporal and spatial response. We present a technique to characterize this phenomenon and apply it to a prototype of such systems, the Single Line Of Sight camera. Results of this characterization are used to benchmark Particle In Cell simulations of the electrons drifting inside the detector, which are found to well reproduce experimental data. These simulations are then employed to predict the optimum photon flux to the camera, with the goal to increase the quality of the images obtained on an experimental campaign while preventing the appearance of deleterious effects. They also offer some insight into some of the improvements that can be brought to the new pulse-dilation systems being built at Lawrence Livermore National Laboratory

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Deuterated polyethylene nanowire arrays for high-energy density physics

Abstract The interaction of intense, ultrashort laser pulses with ordered nanostructure arrays offers a path to the efficient creation of ultra-high-energy density (UHED) matter and the generation of high-energy particles with compact lasers. Irradiation of deuterated nanowires arrays results in a near-solid density environment with extremely high temperatures and large electromagnetic fields in which deuterons are accelerated to multi-megaelectronvolt energies, resulting in deuterium–deuterium (D–D) fusion. Here we focus on the method of fabrication and the characteristics of ordered arrays of deuterated polyethylene nanowires. The irradiation of these array targets with femtosecond pulses of relativistic intensity and joule-level energy creates a micro-scale fusion environment that produced $2\times {10}^6$ neutrons per joule, an increase of about 500 times with respect to flat solid CD 2 targets irradiated with the same laser pulses. Irradiation with 8 J laser pulses was measured to generate up to 1.2 × 10 7 D–D fusion neutrons per shot.

Optics↗

DOE OSTI2017

Sub-photospheric Shocks in Relativistic Explosions

This paper examines the mechanism of internal shocks in opaque relativistic outflows, in particular in cosmological gamma-ray bursts. The shocks produce neutrino emission and affect the observed photospheric radiation from the explosion. They develop from internal compressive waves and can be of different types depending on the composition of the outflow. (1) Shocks in “photon gas,” with negligible plasma inertia, have a unique structure determined by the force-free condition—zero radiation flux in the plasma rest frame. Radiation dominance over plasma inertia suppresses the formation of collisionless shocks mediated by collective electromagnetic fields. (2) If the outflow is sufficiently magnetized, a strong collisionless subshock develops, which is embedded in a thicker radiation-mediated structure. (3) Waves in outflows with a free neutron component lead to dissipation through nuclear collisions. At large optical depths, shocks have a thickness comparable to the neutron free path, with embedded radiation-mediated and collisionless subshocks. The paper also presents first-principles simulations of magnetized flows filled with photons, demonstrating the formation of shocks and their structure. Simple estimates show that magnetized sub-photospheric shocks are efficient producers of photons and have a great impact on the observed photospheric radiation. The shock structure changes as the outflow expands toward its photosphere. The dissipation is accompanied by strong e{sup ±} pair creation, and the e{sup ±}-dressed shock carries the photosphere with it up to two decades in radius, emitting a strong pulse of nonthermal radiation.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2019

The numerical investigation of colliding optical solitons as an all-optical-gate using the method of Lines

The bidirectional propagation and collision of counter-propagating optical solitons in a two-level resonant medium is analyzed. For sufficiently short duration of the pulses and sufficiently high power levels, self-induced transparency allows the pulses to propagate without losses at anomalously low velocities. Here, we use an extended semiclassical approach, called Maxwell–Bloch model. The quantization of the electromagnetic field is neglected, however, a full quantum mechanical formulation is used to describe the behavior of the matter. The numerical simulations are performed by using the method of lines. For improved accuracy, spline interpolation of the fields is introduced. Results are presented to demonstrate the use of soliton collision for all-optical switching, in particular, as OR- and XOR-gates.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2017

Laboratory reflectometer for the investigation of optical elements in a wavelength range of 5–50 nm: description and testing results

We describe a laboratory reflectometer developed at the IPM RAS for precision measurements of spectral and angular dependences of the reflection and transmission coefficients of optical elements in a wavelength range of 5–50 nm. The radiation is monochromatised using a high-resolution Czerny–Turner spectrometer with a plane diffraction grating and two spherical collimating mirrors. A toroidal mirror focuses the probe monochromatic beam on a sample. The X-ray source is a highly ionised plasma produced in the interaction of a high-power laser beam with a solid target at an intensity of 10{sup 11}–10{sup 12} W cm{sup –2}. To stabilise the emission characteristics, the target executes translatory and rotary motions in such a way that every pulse irradiates a new spot. The short-focus lens is protected from contamination by erosion products with the use of a specially designed electromagnetic system. The samples under study are mounted on a goniometer is accommodated in a dedicated chamber, which provides five degrees of freedom for samples up to 500 mm in diameter and two degrees of freedom for a detector. The sample mass may range up to 10 kg. The X-ray radiation is recorded with a detector composed of a CsI photocathode and two microchannel plates. A similar detector monitors the probe beam intensity. The spectral reflectometer resolution is equal to 0.030 nm with the use of ruled gratings with a density of 900 lines mm{sup –1} (spectral range: 5–20 nm) and to 0.067 nm for holographic gratings with a density of 400 lines mm{sup –1} (spectral range: 10–50 nm). We analyse the contribution of higher diffraction orders to the probe signal intensity and the ways of taking it into account in the measurements. Examples are given which serve to illustrate the reflectometer application to the study of multilayer mirrors and filters. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2019

WISE-CASING: Time Domain Reflectometry Data from Cymric Field, CA

The objective of this field test is to validate several technologies for non-invasive well integrity assessment using existing wells with a known completion. The tests were made at the Cymric oil field, which is a steam flood operation. The wells therefore undergo similar downhole conditions as geothermal wells. The Cymric field is mainly a cyclic steam operation where wells are 1000-15-00 ft in depth and the reservoir occupies the bottom 400ft. The maximum temperatures can exceed 500 degrees F and the well spacing is very close, often less than 50m. The field plan consisted of applying the Time Domain Reflectometry (TDR) method to the wells. The input voltages were set as 70 V shows the TDR responses at frequencies of 450 kHz, 2500 kHz, and 4500 kHz. There is a summary report will full information about the field tests.

15 GEOTHERMAL ENERGY↗