Closed-loop pulse shaping with <1ps resolution over >2ns records using STILETTO combined with Three Phase Spectral Interferometry (3PSI)
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Physics - Plasma physics↗
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Closed-loop pulse shaping with <1ps resolution over >2ns records using STILETTO combined with Three Phase Spectral Interferometry (3PSI)
Explore the source record for details and available documents.
Energy, Lasers, Optics and optical instruments↗
Nanostructure‐Derived Antireflectivity in Leafhopper Brochosomes
Understanding how insect‐derived biomaterials interact with light has led to new advances and interdisciplinary insights in entomology and physics. Leafhoppers are insects that coat themselves with highly ordered biological nanostructures known as brochosomes. Brochosomes are thought to provide a range of protective properties to leafhoppers, such as hydrophobicity and antireflectivity, which has inspired the development of synthetic brochosomes that mimic their structures. Despite recent progress, the high antireflective properties of brochosome structures are not fully understood. Herein, a combination of experiments and computational modeling is used to understand the structure‐, material‐, and polarization‐dependent optical properties of brochosomes modeled on the geometries found in three leafhopper species. The results qualitatively represent that light interference interaction with nanostructures naturally occurring in brochosomes is responsible for the spectral tuning and the asymmetric line shape of the reflectance spectra. Whereas prior work has focused on the computational modeling of idealized pitted particles, this work shows that light–matter interactions with brochosome structures can be tuned by varying the geometry of their cage‐like nanoscale features and by changing the arrangement of multiparticle assemblies. Broadly, this work establishes principles for the guided design of new optically active materials inspired by these unique insect nanostructures.
Banerjee, Progna↗
Diagnosing up-scattered deuterium–tritium fusion neutrons produced in burning plasmas at the National Ignition Facility (invited)
In the push to higher performance fusion plasmas, two critical quantities to diagnose are α-heat deposition that can improve and impurities mixed into the plasma that can limit performance. In high-density, highly collisional inertial confinement fusion burning plasmas, there is a significant probability that deuterium–tritium (DT) fusion products, 14.1 MeV neutrons and 3.5 MeV α-particles, will collide with and deposit energy onto (“up-scatter”) surrounding deuterium and tritium fuel ions. These up-scattered D and T ions can then undergo fusion while in-flight and produce an up-scattered neutron (15–30 MeV). These reaction-in-flight (RIF) neutrons can then be uniquely identified in the measured neutron energy spectrum. Further, the magnitude, shape, and relative size of this spectral feature can inform models of stopping-power in the DT plasma and hence is directly proportional to α-heat deposition. In addition, the RIF spectrum can be related to mix into the burning fuel, particularly relevant for high-Z shell and other emerging National Ignition Facility platforms. The neutron time-of-flight diagnostic upgrades needed to obtain this small signal, ~10 –5 times the primary DT neutron peak, will be discussed. Results from several gain > 1 implosions will be shown and compared to previous RIF spectra. Finally, comparisons of experimental data to a simplified computational model will be made.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
High-resolution 3D-printed plastic scintillators with tertiary dye
Additive manufacturing offers efficient production of plastic scintillators with nontrivial geometries using vat polymerization, allowing fabrication of geometries which would be difficult or even impossible to produce using conventional subtractive manufacturing. This work presents a novel photocurable scintillator formula that includes coumarin 450 as a tertiary dye to enable high-resolution 3D printing via the manipulation of the 405 nm cure light. Bulk photocured and 3D printed (with and without tertiary dye) samples were compared through observational assessment and spectral response. All samples showed pulse shape discrimination between neutron and gamma events. Inclusion of the tertiary dye has minimal impact on emission spectrum and light output, but significant impact on print resolution as shown by comparison of printed high-complexity geometries and feature resolution test objects. With the use of a cure-limiting dye, unsupported features — such as freestanding pillars — were resolvable down to 0.7 mm. Even finer resolution at or below 0.1 mm was achieved in fully supported, integrated structures printed with off-the-shelf 405 nm desktop 3D printer. Scintillators demonstrated a light output up to 50% of EJ-200 with a PSD figure of merit up to 1.35 at 0.9–1.1 MeVee.
36 MATERIALS SCIENCE↗
Anharmonic phonons, thermal expansion, and nuclear quantum effects in Zn
The anharmonic behavior of phonons and thermal expansion of hexagonal zinc were studied from 15 to 690 K by inelastic neutron scattering (INS) and ab initio simulations. Phonon spectra were measured for Q-points covering the full Brillouin zone, giving the phonon density of states (DOS) and dispersions along high-symmetry directions. The dispersions were sharp at 15 K, but diffuse intensity was observed at energies above them. The dispersions broadened with temperature T and the diffuse intensity became stronger. This diffuse intensity appeared in all INS measurements and simulations, except for classical molecular dynamics at 15 K. The temperature-dependent effective potential (TDEP) method, which included the nuclear quantum effect from zero-point vibrational dynamics, was used to calculate the free energy and thermal expansion. For T < 100 K nuclear quantum effects were important for obtaining the correct negative thermal expansion, and path integral molecular dynamics (PIMD) was particularly effective for obtaining the negative thermal expansion in the basal plane. A Heisenberg-Langevin model for interacting phonons coupled to a thermal bath was able to reproduce the shape and intensity of the diffuse spectral features.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Measuring scale-dependent shape anisotropy by coarse-graining: Application to inhomogeneous Rayleigh-Taylor turbulence
Here, we generalize the “filtering spectrum” to probe scales along different directions by spatial coarse-graining. This multidimensional filtering spectrum quantifies the spectral content of flows that are not necessarily homogeneous. From multidimensional spectral information, we propose a simple metric for shape anisotropy at various scales. The method is applied to simulations of two-dimensional (2D) and 3D Rayleigh-Taylor (RT) turbulence, which is inhomogeneous and anisotropic. We show that 3D RT has clear shape anisotropy at large scales with approximately 4:3 vertical to horizontal aspect ratio but tends toward isotropy at small scales as expected. In sharp contrast, we find that RT in 2D simulations, which are still the main modeling framework for many applications, is isotropic at large scales and its shape anisotropy increases at smaller scales where structures tend to be horizontally elongated. While this may be surprising, it is consistent with recent results that large-scale isotropy in 2D RT is due to the generation of a large-scale overturning circulation via an upscale cascade, while small-scale anisotropy is due to the stable stratification resultant from such overturning and the inefficient mixing in 2D.
42 ENGINEERING↗
Spectrally reconfigurable quantum emitters enabled by optimized fast modulation
The ability to shape photon emission facilitates strong photon-mediated interactions between disparate physical systems, thereby enabling applications in quantum information processing, simulation and communication. Spectral control in solid state platforms such as color centers, rare earth ions, and quantum dots is particularly attractive for realizing such applications on-chip. Here we propose the use of frequency-modulated optical transitions for spectral engineering of single photon emission. Using a scattering-matrix formalism, we find that a two-level system, when modulated faster than its optical lifetime, can be treated as a single-photon source with a widely reconfigurable photon spectrum that is amenable to standard numerical optimization techniques. To enable the experimental demonstration of this spectral control scheme, we investigate the Stark tuning properties of the silicon vacancy in silicon carbide, a color center with promise for optical quantum information processing technologies. We find that the silicon vacancy possesses excellent spectral stability and tuning characteristics, allowing us to probe its fast modulation regime, observe the theoretically-predicted two-photon correlations, and demonstrate spectral engineering. Our results suggest that frequency modulation is a powerful technique for the generation of new light states with unprecedented control over the spectral and temporal properties of single photons.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
A comparison of strategies for state-selective coherent Raman excitation
Here we report on the theoretical and experimental evaluation of state-selective bond activation for coherent Raman spectroscopy and control of chemical reactivity. We compare six different strategies for state-selective activation using shaped broadband femtosecond laser pulses. Results for a pair of long pulses with different wavelengths are also considered. For each of these approaches, we report on their theoretical and experimental ability to excite a desired vibrational mode while minimizing excitation of other modes including harmonics. We find that the double parabola spectral phase function gives the most intense Raman excitation with 10 cm -1 selectivity with the lowest background. The sinusoidal phase function produces intense Raman excitation with high selectivity but gives a series of harmonic excitations which could hinder selectivity. Implications of this study on several fields ranging from sensing, to controlling chemical reactions, and selective excited state excitation by X-ray pulses are discussed.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Development and Characterization of Electrodes for Surface-Specific Attenuated Total Reflection Two-Dimensional Infrared Spectroelectrochemistry
Electrochemical interfaces still have remaining mysteries surrounding the interfacial region of the electrical double layer, despite being prevalent throughout the energy and water remediation industries. The electrical double layer is where many important dynamic processes such as catalysis and electron transfer occur. The goal of this work is to study the electrical double layer with two-dimensional infrared (2D IR) spectroscopy to experimentally access the details of the structural dynamics of this complex environment. However, there are several experimental challenges to applying 2D IR spectroscopy to this application, such as assuring the surface specificity of the spectrum, optimizing the signal strength while minimizing spectral distortions from dispersion and Fano line shapes, and selecting electrode materials that are both sufficiently IR compatible and conductive. Here we will discuss various considerations when designing 2D IR experiments of electrode interfaces utilizing several substrates and experimental configurations and demonstrate a robust method for 2D IR experiments of electrode interfaces under applied potential that combines nonconducting Si ATR wafers with conductive ITO and thin nanostructured films of plasmonically active Au functionalized with 3-mercapto-2-butanone (MCB). We show that layered electrodes on thin Si ATR wafers with MCB are sensitive to applied potential and that the distortions in the linear and 2D IR spectra are heavily dependent on the morphology of the Au surface.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Investigating the electronic structure of high explosives with X-ray Raman spectroscopy
Abstract We investigate the sensitivity and potential of a synergistic experiment-theory X-ray Raman spectroscopy (XRS) methodology on revealing and following the static and dynamic electronic structure of high explosive molecular materials. We show that advanced ab-initio theoretical calculations accounting for the core-hole effect based on the Bethe-Salpeter Equation (BSE) approximation are critical for accurately predicting the shape and the energy position of the spectral features of C and N core-level spectra. Moreover, the incident X-ray dose typical XRS experiments require can induce, in certain unstable structures, a prominent radiation damage at room temperature. Upon developing a compatible cryostat module for enabling cryogenic temperatures ( $$\approx$$ ≈ 10 K) we suppress the radiation damage and enable the acquisition of reliable experimental spectra in excellent agreement with the theory. Overall, we demonstrate the high sensitivity of the recently available state-of-the-art X-ray Raman spectroscopy capabilities in characterizing the electronic structure of high explosives. At the same time, the high accuracy of the theoretical approach may enable reliable identification of intermediate structures upon rapid chemical decomposition during detonation. Considering the increasing availability of X-ray free-electron lasers, such a combined experiment-theory approach paves the way for time-resolved dynamic studies of high explosives under detonation conditions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
X-ray spectroscopic identification of strain and structure-based resonances in a series of saturated carbon-cage molecules: Adamantane, twistane, octahedrane, and cubane
Novel nanocarbons such as fullerenes, nanotubes, graphene, and nanodiamond reside at the cutting edge of nanoscience and technology. Along with chemical functionalization, geometric constraints (such as extreme curvature in nanotubes or defects within or at the surfaces of diamond nanoparticles) significantly alter the electronic states of the nanocarbon material. Understanding the effects of steric strain on the electronic structure is critical to developing nanoelectronic applications based on these materials. This paper presents a fundamental study of how strain affects the electronic structure in a benchmark series of some fundamental saturated carbon cage compounds. Adamantane, C10H16, the smallest diamondoid and arguably the smallest nanodiamond crystallite, has carbon atoms essentially commensurate with diamond lattice positions and possesses by far the least molecular strain of this series. Twistane also is a C10H16 isomer but the fixed cyclohexane twist conformation of the central ring introduces additional strain into the cage. Octahedrane [(CH)12] and cubane [(CH)8] are considerably more strained, culminating in cubane where carbon–carbon bonds lie either parallel or orthogonal to one another. Using gas-phase near-edge x-ray absorption fine structure spectroscopy to probe the unoccupied electronic states, we observe two major progressions across this series. First, a broad C–C σ* resonance in the absorption splits into two more narrow and intense resonances with increasing strain. Second, the first manifold of states previously associated with tertiary C–H σ* in the diamondoid series appears to broaden and shift to lower energy. This feature is more than twice as intense in cubane than in octahedrane, even though these two molecules have only tertiary carbons, with the chemical formula (CH)x. The spectral differences are entirely due to the shape of the molecules; in particular, in cubane, the features arise from a high degree of p-p interaction between parallel C–C bonds. In contrast to the conventional wisdom that near-edge x-ray absorption is primarily an atomically localized spectroscopy, molecular shape and associated strain lead to the dominant features in spectra acquired from this fundamental series of carbon cage structures.
36 MATERIALS SCIENCE↗
Establishing robust correction schemes for improved and reliable ARM-AOS aerosol optical data products
Aerosol light absorption and scattering of solar radiation play an important role in the earth’s atmosphere in terms of direct and semi-direct radiative forcing. Optical parameters of importance to the US Department of Energy (DOE) climate models include absorption and scattering coefficients, single scattering albedo (SSA), absorption Angstrom exponents (AAE), and the asymmetry parameter (g). These parameters depend on aerosol size, shape and composition (refractive index), and are spectrally sensitive in the shortwave region. Additionally, these parameters have a complex dependency on the emission source, especially for carbonaceous aerosols. The DOE Atmospheric Radiation Measurement (ARM) user facility has deployed aerosol observing systems (AOS) containing several filter-based instruments to measure and constrain aerosol optical properties and related parameters at multiple sites worldwide. For measurement of aerosol light absorption, the AOS includes filter-based instruments (particle soot absorption photometer and tricolor absorption photometer) that infer particle-phase aerosol absorption coefficients at nominal red, green, and blue wavelength bands from the attenuation (ATN) of light passing through a particulate filter on which aerosols are deposited. Measurement of aerosol scattering is done in situ using nephelometers. By combining inferred absorption coefficients from filter-based ATN measurements and in situ scattering coefficients, value-added products (VAPs) such as SSA, AAE, and g are derived.
54 ENVIRONMENTAL SCIENCES↗
FRAM Version 7.1’s Bias
The Fixed-Energy Response-Function Analysis with Multiple Efficiency (FRAM) code was developed at Los Alamos National Laboratory to measure the gamma-ray spectrometry of the isotopic composition of plutonium, uranium, and other actinides. For FRAM versions 4 and earlier, the reported uncertainties of the results come from the propagation of the statistics in the peak areas only. No systematic error components are included in the reported uncertainties. For FRAM versions 5 and 6, we examined the FRAM analytical results of both the archival plutonium data and the data specifically acquired for the isotopic uncertainty analysis project and found the relationship between the bias and other parameters. We worked out the equations representing the biases of the measured isotopes from each measurement using internal spectral parameters, such as peak resolution and shape, region of analysis, and burnup (for plutonium) or enrichment (for uranium). The resulting biases were included in the reported uncertainties of FRAM v.5 and v.6.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Automated Gold Nanorod Spectral Morphology Analysis Pipeline
The development of a colloidal synthesis procedure to produce nanomaterials with high shape and size purity is often a time-consuming, iterative process. This is often due to quantitative uncertainties in the required reaction conditions and the time, resources, and expertise intensive characterization methods required for quantitative determination of nanomaterial size and shape. Absorption spectroscopy is often the easiest method for colloidal nanomaterial characterization. However, due to the lack of a reliable method to extract nanoparticle shapes from absorption spectroscopy, it is generally treated as a more qualitative measure for metal nanoparticles. This work demonstrates a gold nanorod (AuNR) spectral morphology analysis tool, called AuNR-SMA, which is a fast and accurate method to extract quantitative structural information from colloidal AuNR absorption spectra. To demonstrate the practical utility of this model, we apply it to three distinct applications. First, we demonstrate this model's utility as an automated analysis tool in a high-throughput AuNR synthesis procedure by generating quantitative size information from optical spectra. Second, we use the predictions generated by this model to train a machine learning model to predict the resulting AuNR size distributions under specified reaction conditions. Third, we apply this model to spectra extracted from the literature where no size distributions are reported and impute unreported quantitative information on AuNR synthesis. This approach can potentially be extended to any other nanocrystal system where absorption spectra are size dependent, and accurate numerical simulation of absorption spectra is possible. In addition, this pipeline could be integrated into automated synthesis apparatuses to provide interpretable data from simple measurements, help explore the synthesis science of nanoparticles in a rational manner, or facilitate closed-loop workflows.
36 MATERIALS SCIENCE↗
An improved synthetic signal injection routine for the Haloscope At Yale Sensitive To Axion Cold dark matter (HAYSTAC)
Microwave cavity haloscopes are among the most sensitive direct detection experiments searching for dark matter axions via their coupling to photons. When the power of the expected microwave signal due to axion–photon conversion is on the order of 10 −24 W, having the ability to validate the detector response and analysis procedure by injecting realistic synthetic axion signals becomes helpful. Here, we present a method based on frequency hopping spread spectrum for synthesizing axion signals in a microwave cavity haloscope experiment. It allows us to generate a narrow and asymmetric shape in frequency space that mimics an axion’s spectral distribution, which is derived from a Maxwell–Boltzmann distribution. In addition, we show that the synthetic axion’s power can be calibrated with reference to the system noise. Further, compared to the synthetic axion injection in the Haloscope At Yale Sensitive to Axion Cold dark matter (HAYSTAC) Phase I, we demonstrated synthetic signal injection with a more realistic line shape and calibrated power.
47 OTHER INSTRUMENTATION↗
Hyperfine structure and isotope shifts of xenon measured for near-infrared transitions with Doppler-free saturated absorption spectroscopy
Hyperfine structure and isotope shifts of Xe were investigated with Doppler-free saturated absorption spectroscopy for all transitions in the 820-841 nm spectral interval. The Xe samples were commercial gases of natural isotopic abundances. The measurements were performed by employing a widely tunable narrow line Ti:sapphire laser. The hyperfine structures for 129 Xe and 131 Xe were well resolved. For the transitions with the wavelengths in vacuum near 820.860 nm and 841.150 nm also isotope shifts of the even isotopes were clearly observed. The modeling of the shapes of the observed absorption lines qualitatively reproduces experimental spectral profiles. The measured absorption peaks of the hyperfine structure and isotope shifts of Xe isotopes present characteristic spectral fingerprints for their identification. Eventually, quantitative spectral analysis will provide isotopic abundances of natural, as well as radioactive Xe gas samples.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Fluctuation-driven excess noise near superconducting phase transition
We discuss intrinsic mechanisms of nonequilibrium excess noise in superconducting devices and transition edge sensors. In particular, we present an overview of fluctuation-driven contributions to the current noise in the vicinity of the superconducting transition. We argue that sufficiently close to the critical temperature fluctuations of conductivity may become correlated provided that the rate of quasiparticle relaxation is slow as compared to dynamics of superconducting fluctuations. In this regime, fluctuations of conductivity adiabatically follow the fluctuations of the electron distribution. This leads to a substantial enhancement of current noise. Here, the corresponding spectral power density of noise has a Lorentzian shape in the frequency domain while its magnitude scales proportionally to the inelastic relaxation time. It also sensitively depends on the dephasing and Ginzburg–Landau timescales. Further estimates suggest that this mechanism dominates over the conventional temperature fluctuations in the same range of parameters. To describe these effects microscopically, we use the nonequilibrium Keldysh technique in the semiclassical approximation of superconductivity with Boltzmann–Langevin random forces to account for correlations of fluctuations.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗