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At least 487 records · Page 27

Unraveling shock-induced chemistry using ultrafast lasers

The exquisite time synchronicity between shock and diagnostics needed to unravel chemical events occurring in picoseconds has been achieved using a shaped ultrafast laser pulse to both drive the shocks and interrogate the sample via a multiplicity of optical diagnostics. The shaped laser drive pulse can produce well-controlled shock states of sub-ns duration with sub-10 ps risetimes, sufficient for investigation offast reactions or phase transformations in a thin layer with picosecond time resolution. The shock state is characterized using ultrafast dynamic ellipsometry (UDE) in either planar or Gaussian spatial geometries, the latter allowing measurements of the equation of state of materials at a range of stresses in a single laser pulse. Time-resolved processes in materials are being interrogated using UDE, ultrafast infrared absorption, ultrafast UV/visible absorption, and femtosecond stimulated Raman spectroscopy. Using these tools we showed that chemistry in an energetic thin film starts only after an induction time of a few tens of ps, an observation that allows differentiation between proposed shock-induced reaction mechanisms. These tools are presently being applied to a variety of energetic and reactive sample systems, from nitromethane and carbon disulfide, to microengineered interfaces in tunable energetic mixtures. Recent results will be presented, and future trends outlined.

47 OTHER INSTRUMENTATION↗

Activatino of Erbium Films for Hydrogen Storage

Hydriding of metals can be routinely performed at high temperature in a rich hydrogen atmosphere. Prior to the hydrogen loading process, a thermal activation procedure is required to promote facile hydrogen sorption into the metal. Despite the wide spread utilization of this activation procedure, little is known about the chemical and electronic changes that occur during activation and how this thermal pretreatment leads to increased rates of hydrogen uptake. This study utilized variable kinetic energy X-ray photoelectron spectroscopy to interrogate the changes during in situ thermal annealing of erbium films, with results confirmed by time-of-flight secondary ion mass spectrometry and low energy ion scattering. Activation can be identified by a large increase in photoemission between the valence band edge and the Fermi level and appears to occur over a two stage process. The first stage involves desorption of contaminants and recrystallization of the oxide, initially impeding hydrogen loading. Further heating overcomes the first stage and leads to degradation of the passive surface oxide leading to a bulk film more accessible for hydrogen loading.

08 HYDROGEN↗

Comparing modern measurements of the {sup 11}B(d,n{gamma}{sub 15.1}){sup 12}C excitation function with previous values

A possible means of active interrogation of special nuclear materials is detection of signature emissions following induced photofission. This method requires a probe gamma-ray beam to induce the photofission. The {sup 11}B(d,n{gamma}{sub 15.1}){sup 12}C reaction is a candidate for the source of this probe beam. The reaction is prolific and the produced 15.1 MeV gamma-ray is close to a photofission cross-section peak for {sup 235,238}U and {sup 238,239}Pu. In order to model an active interrogation system using the {sup 11}B(d,n{gamma}{sub 15.1}){sup 12}C reaction as a source probe an accurate value for its differential crosssection must be included in data libraries. Measurements of the differential cross-section for the {sup 11}B(d,n{gamma}{sub 15.1}){sup 12}C reaction have been carried out with a BGO detector and found to differ from previous measurements reported by Kavanagh (1958) and Kuan (1964). The discrepancy in the measurements may be explained by examining the detector response function used by Kavanagh and presumably Kuan to that modeled with MCNP5. A comparison of the MCNP5 and Kavanagh detector response functions normalized to the 15.1 MeV gamma-ray peak pulse height shows a factor of approximately 1.7 difference in integrated counts. Applying this correction to the differential cross-section previously reported by Kuan brings the values into agreement, within uncertainties, to the more recent measurements. The evaluation of the detector response function for the 15.1 MeV gamma-ray signal in the NaI detector reported by Kavanagh to that modeled by MCNP5 is shown. This result is applied to the comparison of recent measurements on the {sup 11}B(d,n{gamma}{sub 15.1}){sup 12}C reaction differential cross-section to those previously reported.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Fiber optic probe of free electron evanescent fields in the optical frequency range

We introduce an optical fiber platform which can be used to interrogate proximity interactions between free-electron evanescent fields and photonic nanostructures at optical frequencies in a manner similar to that in which optical evanescent fields are sampled using nanoscale aperture probes in scanning near-field microscopy. Conically profiled optical fiber tips functionalized with nano-gratings are employed to couple electron evanescent fields to light via the Smith-Purcell effect. We demonstrate the interrogation of medium energy (30–50 keV) electron fields with a lateral resolution of a few micrometers via the generation and detection of visible/UV radiation in the 700–300 nm (free-space) wavelength range.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Ultrafast photo-induced nuclear relaxation of a conformationally disordered conjugated polymer probed with transient absorption and femtosecond stimulated Raman spectroscopies

A combination of transient absorption (TAS) and femtosecond stimulated Raman (FSRS) spectroscopies were used to interrogate the photo-induced nuclear relaxation dynamics of poly(3-cyclohexyl,4-methylthiophene) (PCMT). The large difference in inter-ring dihedral angles of ground and excited-state PCMT make it an ideal candidate for studying large-amplitude vibrational relaxation associated with exciton trapping. Spectral shifting in the S{sub 1} TA spectra on sub-ps timescales (110 ± 20 and 800 ± 100 fs) is similar to spectroscopic signatures of excited-state relaxation observed with related photoexcited conjugated polymers and which have been attributed to exciton localization and a combination of resonant energy transfer and torsional relaxation, respectively. Measurements made with both techniques reveal fast PCMT S{sub 1} decay and triplet formation (τ{sub S1} = 25–32 ps), which is similar to the excited-state dynamics of short oligothiophenes and highly twisted polyconjugated molecules. On ultrafast timescales FSRS of S{sub 1} PCMT offers a new perspective on the nuclear dynamics that underlie localization of excitons in photoexcited conjugated polymers: Spectral dynamics in the C=C stretching region (1400–1600 cm{sup −1}) include a red-shift of the in-phase C=C stretching frequency, as well as a change in the relative intensity of in-phase and out-of-phase stretch intensities on a timescale of ∼100 fs. Both changes indicate an ultrafast vibrational distortion that increases the conjugation length in the region of the localized excitation and are consistent with exciton self-localization or trapping. Wavelength-dependent excited-state FSRS measurements further demonstrate that the C=C stretching frequency provides a useful spectroscopic handle for interrogating the degree of delocalization in excited conjugated polymers given the selectivity achieved via resonance enhancement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Single Hit Energy-resolved Laue Diffraction

In situ white light Laue diffraction has been successfully used to interrogate the structure of single crystal materials undergoing rapid (nanosecond) dynamic compression up to megabar pressures. However, information on strain state accessible via this technique is limited, reducing its applicability for a range of applications. Here, we present an extension to the existing Laue diffraction platform in which we record the photon energy of a subset of diffraction peaks. This allows for a measurement of the longitudinal and transverse strains in situ during compression. Consequently, we demonstrate measurement of volumetric compression of the unit cell, in addition to the limited aspect ratio information accessible in conventional white light Laue. We present preliminary results for silicon, where only an elastic strain is observed. VISAR measurements show the presence of a two wave structure and measurements show that material downstream of the second wave does not contribute to the observed diffraction peaks, supporting the idea that this material may be highly disordered, or has undergone large scale rotation.

47 OTHER INSTRUMENTATION↗

Simulations of in situ x-ray diffraction from uniaxially compressed highly textured polycrystalline targets

A growing number of shock compression experiments, especially those involving laser compression, are taking advantage of in situ x-ray diffraction as a tool to interrogate structure and microstructure evolution. Although these experiments are becoming increasingly sophisticated, there has been little work on exploiting the textured nature of polycrystalline targets to gain information on sample response. Here, we describe how to generate simulated x-ray diffraction patterns from materials with an arbitrary texture function subject to a general deformation gradient. We will present simulations of Debye-Scherrer x-ray diffraction from highly textured polycrystalline targets that have been subjected to uniaxial compression, as may occur under planar shock conditions. In particular, we study samples with a fibre texture, and find that the azimuthal dependence of the diffraction patterns contains information that, in principle, affords discrimination between a number of similar shock-deformation mechanisms. For certain cases, we compare our method with results obtained by taking the Fourier transform of the atomic positions calculated by classical molecular dynamics simulations. Illustrative results are presented for the shock-induced α–ϵ phase transition in iron, the α–ω transition in titanium and deformation due to twinning in tantalum that is initially preferentially textured along [001] and [011]. The simulations are relevant to experiments that can now be performed using 4th generation light sources, where single-shot x-ray diffraction patterns from crystals compressed via laser-ablation can be obtained on timescales shorter than a phonon period.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Efficient power combiner for THz radiation

Most dangerous explosive materials, both toxic and radioactive, contain nitrogen salts with resonant absorption lines in the frequency range 0.3-10 THz. Therefore, there has been growing interest in remotely detecting such materials by observing the spectrum of reflected signals when the suspicious material is interrogated by THz radiation. Practical portable THz sources available today generate only 20–40 mW output power. This power level is too low to interrogate suspicious material from a safe distance, especially if the material is concealed. Hence, there is a need for sources that can provide greater power in the THz spectrum. Generating and extracting high output power from THz sources is complicated and inefficient. The efficiency of vacuum electronic microwave sources is very low when scaled to the THz range and THz sources based on scaling down semiconductor laser sources have low efficiency as well, resulting in the well known “THz gap.” The reason for such low efficiencies for both source types is material losses in the THz band. In this article an efficient power combiner is described that is based on scaling to higher frequencies a microwave combiner that increases the output power in the THz range of interest in simulation studies. The proposed power combiner not only combines the THz power output from several sources, but can also form a Gaussian wavebeam output. A minimum conversion efficiency of 89% with cophased inputs in a lossy copper power combiner and maximum efficiency of 100% in a Perfect Electric Conductor (PEC)-made power combiner were achieved in simulations. Also, it is shown that the TE{sub 01} output mode is a reasonable option for THz applications due to the fact that conductive loss decreases for this mode as frequency increases.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Harnessing quantum light for microscopic biomechanical imaging of cells and tissues

The biomechanical properties of cells and tissues play an important role in our fundamental understanding of the structures and functions of biological systems at both the cellular and subcellular levels. Recently, Brillouin microscopy, which offers a label-free spectroscopic means of assessing viscoelastic properties in vivo, has emerged as a powerful way to interrogate those properties on a microscopic level in living tissues. However, susceptibility to photodamage and photobleaching, particularly when high-intensity laser beams are used to induce Brillouin scattering, poses a significant challenge. This article introduces a transformative approach designed to mitigate photodamage in biological and biomedical studies, enabling nondestructive, label-free assessments of mechanical properties in live biological samples. By leveraging quantum-light-enhanced stimulated Brillouin scattering (SBS) imaging contrast, the signal-to-noise ratio is significantly elevated, thereby increasing sample viability and extending interrogation times without compromising the integrity of living samples. The tangible impact of this methodology is evidenced by a notable three-fold increase in sample viability observed after subjecting the samples to three hours of continuous squeezed-light illumination, surpassing the traditional coherent light-based approaches. The quantum-enhanced SBS imaging holds promise across diverse fields, such as cancer biology and neuroscience where preserving sample vitality is of paramount significance. By mitigating concerns regarding photodamage and photobleaching associated with high-intensity lasers, this technological breakthrough expands our horizons for exploring the mechanical properties of live biological systems, paving the way for an era of research and clinical applications.

Li, Tian↗

Measurement of Photoneutrons from Depleted Uranium and Comparison Study Using MCNPX-PoliMi

High-energy photon interrogation is a nondestructive technique that is used to detect special nuclear materials and characterize nuclear waste. The development of such systems is complex and requires Monte Carlo simulations to optimize system performance. Monte Carlo simulations rely on various scattering, absorption, and photonuclear cross-section data. While the scattering and absorption cross-section data have been extensively studied and validated with experiments, the results obtained from photonuclear simulations are often found to underpredict measured results, indicating uncertainties in the photonuclear cross sections themselves. Thus, there is a need for new measured results that can be used to quantify underpredictions in simulations using photonuclear cross-section data. In the present work, we interrogated depleted uranium with a 9-MV electron linac and detected photoneutrons with trans-stilbene organic scintillators. The measurement of photoneutrons with organic scintillators is challenging due to the presence of the intense photon flux, which causes issues such as pulse pile-up, detector saturation, and poor signal-to-background ratio. To mitigate these challenges, we used iron and polyethylene shielding of varying thicknesses around the depleted uranium target and a neural network–based digital pulse processing algorithm to recover neutron and photon information from piled-up events. Our goal was to compare the measured photoneutron count rate with the simulated rate obtained using the MCNPX-PoliMi transport code. For a light output window of 0.28 to 2.67 MeVee (1.66- to 6.85-MeV proton recoil energy), we found that the simulated count rate obtained using the ENDF/B-VII photonuclear cross-section library underpredicts the measured rate by 32.8% 3.2%. Additionally, we compared the simulated and measured photoneutron light output distributions. For the least thicknesses of shielding, the simulation was found to underpredict measurements in the 0.70- to 2.67-MeVee light output window. For the greatest thicknesses of shielding, the simulation was found to underpredict the measurement across the entire light output window of 0.28 to 2.67 MeVee.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Time-resolved particle image velocimetry

Time-resolved particle image velocimetry (TR-PIV) has become widespread in fluid dynamics. Essentially a velocity field movie, the dynamic content provides temporal as well as spatial information, in contrast to conventional PIV offering only statistical ensembles of flow quantities. From these time series arise further analyses such as accelerometry, space-time correlations, frequency spectra of turbulence including spatial variability, and derivation of pressure fields and forces. The historical development of TR-PIV is chronicled, culminating in an assessment of the current state of technology in high-repetition-rate lasers and high-speed cameras. Commercialization of pulse-burst lasers has expanded TR-PIV into more flows, including the compressible regime, and has achieved MHz rates. Particle response times and peak locking during image interrogation require attention but generally are not impediments to success. Accuracy considerations are discussed, including the risks of noise and aliasing in spectral content. Oversampled TR-PIV measurements allow use of multi-frame image interrogation methods, which improve the precision of the correlation and raise the velocity dynamic range of PIV. In combination with volumetric methods and data assimilation, a full four-dimensional description of a flow is not only achievable but becoming standardized. Lastly, a survey of exemplary applications is followed by a few predictions concerning the future of TR-PIV.

47 OTHER INSTRUMENTATION↗

Clock Precision beyond the Standard Quantum Limit at 10 −18 Level

Optical atomic clocks with unrivaled precision and accuracy have advanced the frontier of precision measurement science and opened new avenues for exploring fundamental physics. A fundamental limitation on clock precision is the standard quantum limit (SQL), which stems from the uncorrelated projection noise of each atom. State-of-the-art optical lattice clocks interrogate large ensembles to minimize the SQL, but density-dependent frequency shifts pose challenges to scaling the atom number. The SQL can be surpassed, however, by leveraging entanglement, though it remains an open problem to achieve quantum advantage from spin squeezing at state-of-the-art stability levels. Here, we demonstrate clock performance beyond the SQL, achieving a fractional frequency precision of 1.1 × 10 −18 for a single spin-squeezed clock. With cavity-based quantum nondemolition measurements, we prepare two spin-squeezed ensembles of ∼30 000 strontium atoms confined in a two-dimensional optical lattice. A synchronous clock comparison with an interrogation time of 61 ms achieves a metrological improvement of 2.0(2) dB beyond the SQL, after correcting for state preparation and measurement errors. These results establish the most precise entanglement-enhanced clock to date and offer a powerful platform for exploring the interplay of gravity and quantum entanglement.

cavity quantum electrodynamics↗

Above-threshold multiphoton photoemission from noble metal surfaces

Exciting solids with intense femtosecond laser pulses prompts electrons of the interrogated material to respond in a highly nonlinear manner, as is evident in the emission of high-order harmonic radiation and photoelectrons with kinetic energies well above that of the driving photons. Such high-field interactions can be resolved, for example, in above-threshold multiphoton photoemission (ATP) spectroscopy. In this work, we interrogate the nonlinear photoelectric responses of the pristine copper, silver, and gold noble metal surfaces in (111) and (100) crystal orientations in the perturbative regime. Using multiphoton photoemission spectroscopy (mPP) excited by finely tuned optical fields, we characterize enhancement of the mPP and ATP yields from (111) surfaces in selected k||-momentum ranges when the occupied Shockley surface (SS) states are (near-)resonantly coupled by multiphoton transitions to image potential (IP) intermediate states in the excitation process. The ATP signal from the IP states of (111) surfaces is largely defined by their formation through polarization of SS electrons; this observation is contrasted with ATP experiments from the Ag(100) surface, for which the SS becomes an unoccupied resonance and the IP states can only be excited from bands with significantly more bulk character. In addition, based on the optical power and nonlinear order-dependent mPP spectra, we provide evidence for ATP being a one-step, rather than a sequential process, as previously postulated.

74 ATOMIC AND MOLECULAR PHYSICS↗

Floquet Prethermalization with Lifetime Exceeding 90 s in a Bulk Hyperpolarized Solid

Here, we report the observation of long-lived Floquet prethermal states in a bulk solid composed of dipolar-coupled 13 C nuclei in diamond at room temperature. For precessing nuclear spins prepared in an initial transverse state, we demonstrate pulsed spin-lock Floquet control that prevents their decay over multiple-minute-long periods. We observe Floquet prethermal lifetimes $T^{'}_{2}$≈90.9 s, extended >60 000-fold over the nuclear free induction decay times. The spins themselves are continuously interrogated for ~10 min, corresponding to the application of ≈5.8×10 6 control pulses. The 13 C nuclei are optically hyperpolarized by lattice nitrogen vacancy centers; the combination of hyperpolarization and continuous spin readout yields significant signal-to-noise ratio in the measurements. This allows probing the Floquet thermalization dynamics with unprecedented clarity. We identify four characteristic regimes of the thermalization process, discerning short-time transient processes leading to the prethermal plateau and long-time system heating toward infinite temperature. This Letter points to new opportunities possible via Floquet control in networks of dilute, randomly distributed, low-sensitivity nuclei. In particular, the combination of minutes-long prethermal lifetimes and continuous spin interrogation opens avenues for quantum sensors constructed from hyperpolarized Floquet prethermal nuclei.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Status of the nuclear measurement stations for the process control of spent fuel reprocessing at AREVA NC/La Hague

Nuclear measurements are used at AREVA NC/La Hague for the monitoring of spent fuel reprocessing. The process control is based on gamma-ray spectroscopy, passive neutron counting and active neutron interrogation, and gamma transmission measurements. The main objectives are criticality and safety, online process monitoring, and the determination of the residual fissile mass and activities in the metallic waste remained after fuel shearing and dissolution (empty hulls, grids, end pieces), which are put in radioactive waste drums before compaction. The whole monitoring system is composed of eight measurement stations which will be described in this paper. The main measurement stations no. 1, 3 and 7 are needed for criticality control. Before fuel element shearing for dissolution, station no. 1 allows determining the burn-up of the irradiated fuel by gamma-ray spectroscopy with HP Ge (high purity germanium) detectors. The burn-up is correlated to the {sup 137}Cs and {sup 134}Cs gamma emission rates. The fuel maximal mass which can be loaded in one bucket of the dissolver is estimated from the lowest burn-up fraction of the fuel element. Station no. 3 is dedicated to the control of the correct fuel dissolution, which is performed with a {sup 137}Cs gamma ray measurement with a HP Ge detector. Station no. 7 allows estimating the residual fissile mass in the drums filled with the metallic residues, especially in the hulls, from passive neutron counting (spontaneous fission and alpha-n reactions) and active interrogation (fission prompt neutrons induced by a pulsed neutron generator) with proportional {sup 3}He detectors. The measurement stations have been validated for the reprocessing of Uranium Oxide (UOX) fuels with a burn-up rate up to 60 GWd/t. This paper presents a brief overview of the current status of the nuclear measurement stations. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Upgraded fiber-optic sensor system for dynamic strain measurement in Spallation Neutron Source

We describe an upgraded fiber-optic sensor system and its performance in measuring the dynamic strains in a mercury target of the Spallation Neutron Source (SNS). Strains result from dynamic pressure waves in the stainless-steel mercury target induced by short (~700 ns), intense (up to 23.3 kJ), high-energy (~1 GeV) proton pulses. In the upgraded sensor system, the output of each sensor head is interrogated with a compact, all-fiber based Faraday Michelson interferometer, which generates interference signals with a steady phase shift. Strain waveforms are recovered from the phase-shifted interference signals using a high-speed digital signal processing procedure developed in our previous work. We demonstrate successful measurements of dynamic strain pulses, e.g., 400με over 190μs , on a recently installed SNS target using the upgraded sensor system. The measured strain waveforms are analyzed for more than 20 sensor locations and/or orientations, and provide information regarding the temporal structure of strain profiles and dependence of the strain magnitude on the proton powers of 200 – 1400 kW. The new interrogator also measures the radiation-induced-attenuation (RIA) in the optical fiber, enabling experimental investigations of RIA profiles induced by a 700-ns radiation pulse. The radiation effects on the strain measurement performance are discussed over a radiation dose range of up to 4×10 8 Gy and an RIA compensation method is proposed. The measurements allow insight into the response of this unique piece of equipment and can be used for validation of simulations.

47 OTHER INSTRUMENTATION↗

Embedded Fiber Bragg Grating (FBG) Sensors Fabricated by Ultrasonic Additive Manufacturing for High-Frequency Dynamic Strain Measurements

This article demonstrates high-frequency dynamic strain measurements using fiber Bragg grating (FBG) sensors embedded in metal parts. Using an ultrasonic additive manufacturing (UAM) process, FBGs inscribed in polyimide coated optical fibers were embedded in aluminum parts. An electromagnetic shaker was used to exert dynamic events on the embedded FBG sensors with frequencies from 1 to 10 kHz. The high-speed interrogation of FBG sensors was accomplished using a tunable vertical-cavity surface-emitting laser (VCSEL) and a high-speed interrogation system sampling at 120 kHz. The strain response measured by the FBG sensors was compared with real-time measurements using a laser velocimeter. A finite-element analysis (FEA) was performed to simulate responses to both static strain and high-frequency dynamic strain. In conclusion, results show that strains as small as 2.5$με$ can be resolved at frequencies up to 10 kHz.

36 MATERIALS SCIENCE↗