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At least 361 records · Page 20

Mid-infrared Pulsed Upconversion Imaging in a Rotating Detonation Combustor

To meet the challenges associated with performing mid-InfraRed (IR) imaging in Rotating Detonation Combustors (RDCs), a novel pulsed mid-IR UpConversion Imaging (UCI) diagnostic has been implemented. UCI is an alternative to direct mid-IR detection that uses nonlinear optical frequency mixing to shift mid-IR wavelengths carrying a target image to shorter wavelengths that can be imaged with high-performance silicon-based CCD/CMOS cameras. This approach offers several favorable properties including high spectral selectivity, high temporal resolution, and superior low-light detectivity. A hydrogen-air research RDC was operated with carbon dioxide addition to allow pulsed UCI imaging of mid-IR luminosity within the combustion channel from spontaneous thermal emissions. The resulting measurements demonstrate high spatiotemporal resolution capable of imaging small structures near the supersonically propagating detonation wave front. The results show how this technique can be used to observe sharp gradients and millimeter-scale structures in the high-temperature, high-pressure zones RDC flow fields.

White, Logan W.↗

Reducing Methane Emissions with an Engine Fuel Reformer

Southwest Research Institute (SwRI) designed and demonstrated a compact, plasma-based fuel reformer designed to reduce methane leaks from natural-gas engines used in pipeline compression and industrial power applications. The system uses pulsed electrical discharges to convert a small portion of methane (CH4) into hydrogen (H2) and light hydrocarbons, promoting more complete combustion and reducing unburned methane in the exhaust. The reformer was evaluated through bench-scale testing, high-flow facility testing, and engine-integration testing on representative low-speed and high-speed natural-gas engines. Measured methane-leak reductions ranged from 1 to 27 percent, depending on engine type and operating condition, while reformer energy consumption remained below one percent of total engine output. Design refinements addressed thermal and electrical challenges, resulting in reliable operation with minimal impact on engine control systems. The project achieved all performance objectives within budget and schedule, produced a patentable pulsed-power system design, and established a scalable, energy-efficient pathway for mitigating methane leaks from existing natural-gas engine infrastructure.

03 NATURAL GAS↗

Pulse Radiolysis Investigation of Radicals Derived from Water-Soluble Cyanine Dyes: Implications for Super-resolution Microscopy

Light-induced blinking, an inherent feature of many forms of super-resolution microscopy, has been linked to transient reduction of the fluorescent cyanine dye used as an imaging agent. There is, however, only scant literature information related to one-electron reduced cyanine dyes, especially in an aqueous environment. Here, we examine a small series of cyanine dyes, possessing disparate π-conjugation lengths, under selective reducing or oxidizing conditions. The experiment allows recording of both differential absorption spectra and decay kinetics of the resultant one-electron reduced or oxidized transient species in water. Relative to the ground state, absorption transitions for the various radicals are weak and somewhat broadened but do allow correlation with the π-conjugation length. In all cases, absorption maxima lie to the blue of the main ground-state transition. Under anaerobic conditions, the transient species decay on the microsecond to millisecond time scale, with the mean lifetime depending on molecular structure, radiation dose, and dye concentration. The experimental absorption spectra recorded for the one-electron reduced radicals and the presumed dimer cation radical compare well to spectra obtained from time-dependent density functional theory calculations. Furthermore, the results allow conclusions to be drawn regarding the plausibility of the reduced species being responsible for light-induced blinking in direct stochastic optical reconstruction microscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Megahertz pulse trains enable multi-hit serial femtosecond crystallography experiments at X-ray free electron lasers

The European X-ray Free Electron Laser (XFEL) and Linac Coherent Light Source (LCLS) II are extremely intense sources of X-rays capable of generating Serial Femtosecond Crystallography (SFX) data at megahertz (MHz) repetition rates. Previous work has shown that it is possible to use consecutive X-ray pulses to collect diffraction patterns from individual crystals. Here, we exploit the MHz pulse structure of the European XFEL to obtain two complete datasets from the same lysozyme crystal, first hit and the second hit, before it exits the beam. The two datasets, separated by <1 µs, yield up to 2.1 Å resolution structures. Comparisons between the two structures reveal no indications of radiation damage or significant changes within the active site, consistent with the calculated dose estimates. This demonstrates MHz SFX can be used as a tool for tracking sub-microsecond structural changes in individual single crystals, a technique we refer to as multi-hit SFX.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Pulse Energy and Pulse Duration Effects in the Ionization and Fragmentation of Iodomethane by Ultraintense Hard X Rays

The interaction of intense femtosecond x-ray pulses with molecules sensitively depends on the interplay between multiple photoabsorptions, Auger decay, charge rearrangement, and nuclear motion. Here, we report on a combined experimental and theoretical study of the ionization and fragmentation of iodomethane (CH 3 I) by ultraintense (~10 19 W/cm 2 ) x-ray pulses at 8.3 keV, demonstrating how these dynamics depend on the x-ray pulse energy and duration. We show that the timing of multiple ionization steps leading to a particular reaction product and, thus, the product’s final kinetic energy, is determined by the pulse duration rather than the pulse energy or intensity. While the overall degree of ionization is mainly defined by the pulse energy, our measurement reveals that the yield of the fragments with the highest charge states is enhanced for short pulse durations, in contrast to earlier observations for atoms and small molecules in the soft x-ray domain. Finally, we attribute this effect to a decreased charge transfer efficiency at larger internuclear separations, which are reached during longer pulses.

36 MATERIALS SCIENCE↗

Enhanced quantum radiation with flying-focus laser pulses

The emission of a photon by an electron in an intense laser field is one of the most fundamental processes in electrodynamics and underlies the many applications that utilize high-energy photon beams. This process is typically studied for electrons colliding head-on with a stationary-focus laser pulse. Here, we show that the energy lost by electrons in the quantum regime and the yield of emitted photons can be substantially increased by replacing a stationary-focus pulse with an equal-energy flying-focus pulse whose focus co-propagates with the electrons. Furthermore, these advantages of the flying focus result from the energy loss and the photon yield scaling more favorably with the interaction time than the laser intensity in the quantum regime, with the latter also holding in the classical regime. Monte Carlo simulations of electrons colliding with equal-energy stationary and flying-focus laser pulses demonstrate these advantages.

Compton scattering↗

Calibration of a compact ASIC-based data acquisition system for neutron/$γ$ discrimination and spectroscopy with organic scintillators

Segmented neutron detectors that use silicon photomultipliers (SiPMs) are receiving significant attention in nuclear security applications. Some of these detectors employ hundreds of channels and would therefore benefit from the use of high-channel-density and low-cost-per-channel data acquisition (DAQ) systems. Candidate DAQ systems that meet these requirements exist, but few perform full waveform digitization, which permits neutron and gamma-ray interaction discrimination via pulse shape. In this work, we study the performance of the TOFPET2 (PETsys Electronics), an ASIC-based DAQ designed for positron emission tomography, which has been adapted to provide sensitivity to pulse shape by the use of variable-period charge integration. We use a light-emitting diode to calibrate a combination of an ON Semiconductor (SensL) 60035-64P J-Series SiPM and TOPFET2 DAQ and evaluate the linearity of their response and dynamic range. Here, the calibration curve was obtained by comparing the DAQ response to that measured with a photodiode interfaced with a traditional waveform digitizer. This calibration process was used for rudimentary spectroscopy of various neutron and sources.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Intrinsic 1${T}^{{\prime} }$ phase induced in atomically thin 2 H -MoTe 2 by a single terahertz pulse

The polymorphic transition from 2H to 1${T}^{{\prime} }$-MoTe 2 , which was thought to be induced by high-energy photon irradiation among many other means, has been intensely studied for its technological relevance in nanoscale transistors due to the remarkable improvement in electrical performance. However, it remains controversial whether a crystalline 1${T}^{{\prime} }$ phase is produced because optical signatures of this putative transition are found to be associated with the formation of tellurium clusters instead. Here we demonstrate the creation of an intrinsic 1${T}^{{\prime} }$ lattice after irradiating a mono- or few-layer 2H-MoTe 2 with a single field-enhanced terahertz pulse. Unlike optical pulses, the low terahertz photon energy limits possible structural damages. We further develop a single-shot terahertz-pump-second-harmonic-probe technique and reveal a transition out of the 2H-phase within 10 ns after photoexcitation. Our results not only provide important insights to resolve the long-standing debate over the light-induced polymorphic transition in MoTe 2 but also highlight the unique capability of strong-field terahertz pulses in manipulating quantum materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Self-absorption and Phonon Pulse Shape Discrimination in Scintillating Bolometers

In this work, we show that self-absorption of photons in scintillating bolometers can differentiate phonon pulse shapes between α (or nuclear recoil) and β/γ signals. This enables phonon pulse shape discrimination for particle identification. We establish a detector signal model that includes self-absorption and compare the simulated phonon pulse shapes with previously reported experimental results. The model predicts increase in pulse shape difference at higher self-absorption. Based on this result, we propose a new design of scintillating bolometers using 4π light reflectors for maximized self-absorption and only a single phonon readout, instead of light detectors that are typically employed for particle discrimination in scintillating bolometers.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Enhanced Neutron and γ-Ray Detection via 6 Li Substitution in Undoped and Tl-Doped Zero-Dimensional Perovskite Cs 3 Cu 2 I 5 Scintillators

Radiation detectors are crucial in a wide variety of research and commercial applications, such as oil and gas exploration, medical imaging, nuclear nonproliferation, and homeland security. Neutron and gamma-ray detectors are fundamental components in portal monitors at ports and border crossings, bolstering national security against radiological threats. This study presents a dual-mode scintillator, undoped and Tl-doped 6 Li-Cs 3 Cu 2 I 5 , and demonstrates its potential as a promising material for simultaneous thermal neutron and gamma-ray detection. We explore the Bridgman growth of both undoped and thallium doped Li → Cu and Li → Cs substitutional systems with various Li doping levels and assess their impact on scintillation properties. Under 662 keV gamma-ray excitation, the undoped crystals had light yields up to 35,900 ph/MeV, with energy resolutions down to 4.5%. The Tl-doped crystals performed better than the undoped crystals with light yields peaking at 65,900 ph/MeV and energy resolutions as low as 3.5%. When exposed to a moderated 252 Cf excitation source, our crystals had light yields between 102,900 and 167,200 photons per thermal neutron capture, with a full energy thermal neutron peak reaching 3 MeV in gamma equivalent energy. Pulse shape discrimination studies reveal well-separated gamma and neutron events, resulting in Figure-Of-Merit (FOM) as high as 3.7. Furthermore, these findings highlight the potential of Li-doped Cs 3 Cu 2 I 5 as a viable candidate for next-generation dual-mode scintillators.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Deciphering Photoinduced Catalytic Reaction Mechanisms in Natural and Artificial Photosynthetic Systems on Multiple Temporal and Spatial Scales Using X-ray Probes

Utilization of renewable energies for catalytically generating value-added chemicals is highly desirable in this era of rising energy demands and climate change impacts. Artificial photosynthetic systems or photocatalysts utilize light to convert abundant CO 2 , H 2 O, and O 2 to fuels, such as carbohydrates and hydrogen, thus converting light energy to storable chemical resources. Here, the emergence of intense X-ray pulses from synchrotrons, ultrafast X-ray pulses from X-ray free electron lasers, and table-top laser-driven sources over the past decades opens new frontiers in deciphering photoinduced catalytic reaction mechanisms on the multiple temporal and spatial scales. Operando X-ray spectroscopic methods offer a new set of electronic transitions in probing the oxidation states, coordinating geometry, and spin states of the metal catalytic center and photosensitizers with unprecedented energy and time resolution. Operando X-ray scattering methods enable previously elusive reaction steps to be characterized on different length scales and time scales. The methodological progress and their application examples collected in this review will offer a glimpse into the accomplishments and current state in deciphering reaction mechanisms for both natural and synthetic systems. Looking forward, there are still many challenges and opportunities at the frontier of catalytic research that will require further advancement of the characterization techniques.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Selective Detection in Impulsive Low-Frequency Raman Imaging Using Shaped Probe Pulses

Impulsive stimulated Raman scattering (ISRS) using a single short femtosecond pump pulse to excite molecular vibrations offers an elegant pump-probe approach to perform vibrational imaging below 200 cm –1 . One shortcoming of ISRS is its inability to offer vibrational selectivity as all the vibrational bonds whose frequencies lie within the short pump-pulse bandwidth are excited. To date, several coherent control techniques have been explored to address this issue and selectively excite a specific molecular vibration by shaping the pump pulse. There has not been any systematic work that reports an analogous shaping of the probe pulse to implement preferential detection. In this work, we focus on vibrational imaging and report vibrational selective detection by shaping the probe pulse in time. Here, we demonstrate numerically and experimentally two pulse-shaping strategies with one functioning as a vibrational notch filter and the other functioning as a vibrational low-pass filter. This enables fast (25 μs/pixel) and selective hyperspectral imaging in the low-frequency regime (< 200 cm –1 ).

74 ATOMIC AND MOLECULAR PHYSICS↗

Dephasingless Laser Wakefield Acceleration

Laser wakefield accelerators (LWFAs) produce significantly high gradients enabling compact accelerators and radiation sources, but face design limitations, such as dephasing, occurring when trapped electrons outrun the accelerating phase of the wakefield. In this report we combine spherical aberration with a novel cylindrically symmetric echelon optic to spatiotemporally structure an ultra-short, high-intensity laser pulse that can overcome dephasing by propagating at any velocity over any distance. The ponderomotive force of the spatiotemporally shaped pulse can drive a wakefield with a phase velocity equal to the speed of light in vacuum, preventing trapped electrons from outrunning the wake. Simulations in the linear regime and scaling laws in the bubble regime illustrate that this dephasingless LWFA can accelerate electrons to high energies in much shorter distances than a traditional LWFA—a single 4.5 m stage can accelerate electrons to TeV energies without the need for guiding structures.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Nonuniform Flow Dynamics Probed by Nanosecond X-Ray Speckle Visibility Spectroscopy

We report observations of nanosecond nonuniform colloidal dynamics in a free flowing liquid jet using ultrafast x-ray speckle visibility spectroscopy. Utilizing a nanosecond double-bunch mode, the Linac Coherent Light Source free electron laser produced pairs of femtosecond coherent hard x-ray pulses. By exploring anisotropy in the visibility of summed speckle patterns which relates to the correlation functions, we evaluate not only the average particle flow rate in a colloidal nanoparticle jet, but also the nonuniform flow field within. The methodology presented here establishes the foundation for the study of nano- and atomic-scale inhomogeneous fluctuations in complex matter using x-ray free electron laser sources.

47 OTHER INSTRUMENTATION↗

Sources of Primary Electrons in Nanosecond Pulsed Breakdown in Water (Final Technical Report)

Electrical breakdown of liquid dielectrics under ns or sub-ns pulsed electric field has been studied extensively in the last decade. Summarized in [7], this relatively young research area makes significant contributions to the theories of liquid breakdown by introducing a new mechanism (electrostrictive cavitation) that is unique at the ns timescale. It is also fundamentally important to plasma sources for biomedical applications and insulation of pulsed power equipment. For water in particular, the understanding of the mechanisms and processes of ns/sub-ns breakdown also sheds new light on cavitation studies, one of the most exciting areas of modern fluid mechanics. The objective of this collaborative research with PCRF was to construct a complete picture of the physical mechanisms and processes at the initial phase of electrical breakdown in liquid dielectrics under nanosecond (ns) pulsed inhomogeneous fields. The research funded by the initial award DE‐ SC0021182 aimed to address the sources of primary electrons in ns breakdown in water, which led to one journal publication and multiple conference presentations. The PI also gave presentations to the PPPL/PCRF audience twice, one in October 2020 and the other during the 2021 PCRF Annual Meeting

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Ionization-Based Optical Structures for the Control of Short-Pulse Lasers (Full LDRD Report)

High-power lasers require enormous beam sizes to avoid optics damage; without plasma control of light, future higher-power systems will have prohibitive costs. The laser-induced formation of ionization patterns in gases provides an opportunity to manipulate the spatial and temporal properties of femtosecond to picosecond beams with precise control at high intensity, providing a path towards compact multi-petawatt lasers. In this project, we proposed new concepts of diffractive optics elements relying on ionization-based structures, including a holographic lens and a compression grating. The theoretical characterization of these optical elements was supported by particle-in-cell simulations. Experiments have been carried out to achieve reflective elements (i.e., plasma-based gratings) that demonstrated high robustness and efficiencies on the order of 50%, which validates the feasibility of our new concepts and paves the way for future plasma-based high-power laser systems.

47 OTHER INSTRUMENTATION↗

Vector measurements using a pulsed, optically pumped atomic magnetometer

An atomic magnetometer, and a method for using same is disclosed. The method for measuring an ambient magnetic field uses an atomic magnetometer that has a probe light beam with a probe axis that probes a polarization vector of an atomic population confined within a vapor cell. The method employs one or more measurement cycles. In each measurement cycle, the polarization vector is prepared in an initial state via an optical pumping pulse. The vapor cell is then subjected to the ambient magnetic field, which results in rotation of the polarization vector by Larmor precession. Within the measurement cycle, at a point in time after the polarization vector has been prepared in the initial state, the ambient magnetic field rotates the direction of the polarization vector, and at least one measurement is made of a projection of the Larmor-rotated polarization vector onto the probe axis during or after application of a magnetic waveform.

Schwindt, Peter↗

Metastable‐State Photoacids with Fast Reverse Reactions

Metastable-state photoacid (mPAH) has become a common tool for controlling and driving chemical processes with light. mPAHs with fast reverse reactions are desirable for precise temporal control or generating quick pulses of proton concentration. Here, in this work, different approaches towards fast reversing mPAHs are studied. Experimental and computational results showed that stabilizing the charge–transfer intermediate is an effective way to increase the rate. A novel mPAH with a reverse reaction ≈500 times faster than the most used mPAH in methanol is developed. Another water-soluble mPAH showed a reverse reaction with a rate constant of 7.8 s −1 , which is the fastest ever reported. The half-life of the acidic state is calculated to be 89 ms, which allowed to demonstrate sub-second switching using this mPAH.

Abbood, Rana [Florida Institute of Technology, Mel↗