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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 1,117 records · Page 62
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Quantum interference between the optical Stark effect and resonant harmonic generation in WS 2

An applied field can modulate optical signals by resonance shifting via the Stark effect. The optical Stark effect uses ultrafast light in the transparency region of a material to shift resonances with speeds limited by the pulse duration or system coherence. In this Rapid Communication, we investigate the optical Stark effect in resonant optical harmonic generation using the A exciton transition of WS 2 . Multidimensional pump-harmonic-probe measurements, in which the probe is second- or third-harmonic emission, reveal not only large Stark shifts that are commensurate with the large optical susceptibilities common to WS 2 excitons, but also behaviors more complex than simple optical Stark effect treatments predict. We show how another manifestation of the Stark effect, brought forth by coherent photon exchange between the pump and harmonic generation fundamental fields, can strongly enhance or suppress harmonic generation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

A Pockels cell enabled heterodyne phase contrast imaging diagnostic for detection of ion cyclotron emission

This work describes a novel optical heterodyne detection scheme that significantly extends the frequency response of the phase contrast imaging method to detect electron density fluctuations in tens of megahertz frequency range. The system employs a variable frequency electro-optic modulator to allow operation at any frequency in the range 10–40 MHz without the need to realign the system. The frequency coverage of the system makes it suitable to measure the radial structure of the electron density component of ion cyclotron emission on devices having confining magnetic field of a few tesla, thus extending the purely temporal measurements provided so far by magnetic probes.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Pulse-by-pulse transient thermal deformation in crystal optics under high-repetition-rate FEL

Time-domain modeling of the thermal deformation of crystal optics can help define acceptable operational ranges across the pulse-energy repetition-rate phase space. In this paper, we have studied the transient thermal deformation of a water-cooled diamond crystal for a cavity-based X-ray free-electron laser (CBXFEL), either an X-ray free-electron laser oscillator (XFELO) or a regenerative amplifier X-ray free-electron laser (RAFEL), by numerical simulations including finite-element analysis and advanced data processing. Pulse-by-pulse transient thermal deformation of a 50 µm-thick diamond crystal has been performed with X-ray pulse repetition rates between 50 kHz and 1 MHz. Results for temperature and thermal deformation have been compared with the results of transient analysis using a continuous wave (CW) power loading. Temperature and thermal deformation results from pulse-by-pulse transient analysis vary with time about the results for the CW case for the same average power. The variation amplitude increases with pulse energy and decreases with repetition rate. When the repetition rate increases to infinity, both temperature and thermal deformation converge to the results for the CW case. Two critical time scales for the operation of crystal optics in a CBXFEL are (1) first-turn time, i.e. the time for the XFEL pulse to complete the first turn around the cavity so that the crystal sees the recirculated XFEL pulse, and (2) period-end time, i.e. the time that the next electron bunch arrives for the amplification, so that the crystal outcouples the amplified FEL power. For the same average power, simulation results show that the crystal thermal deformation seen by the XFEL beam decreases with repetition rate at the first-turn time of a 300 m-long cavity and increases with repetition rate at the period-end time. For the wavefront preservation requirement of the crystal optics, a pulse-energy versus repetition-rate phase space has been established. The upper bounds of the pulse energy at both first-turn and period-end times decreases with repetition rate, especially at the period-end time. The upper bound of the thermal deformation of the crystal at the period-end time for any repetition frequency can be estimated from the CW case. For a water-cooled diamond crystal of dimension 5 mm × 5 mm × 0.05 mm, the time to reach a quasi steady-state is about 50 ms for temperature and 50 µs for thermal deformation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Data driven drift correction for complex optical systems

To exploit the thousand-fold increase in spectral brightness of modern light sources, increasingly intricate experiments are being conducted that demand extremely precise beam trajectory. Maintaining the optimal trajectory over several hours of an experiment with the needed precision necessitates active drift control. Here, we outline time varying Bayesian optimization (TVBO) as a data driven approach for robust drift correction, and illustrate its application for a split and delay optical system composed of six crystals and twelve input dimensions. Using numerical simulations, we exhibit the application of TVBO for linear drift, non-smooth temporal drift as well as constrained TVBO for multi-objective control settings, representing real-life operating conditions. This approach can be easily adapted to other X-ray beam conditioning and guidance systems, including multi-crystal monochromators and grazing-incidence mirrors, to maintain sub-micrometer and nanoradian beam stability over the course of an experiment spanning several hours.

Bayesian optimization↗
DOE OSTI2023

The Influence of Nonlocal Metal–Dielectric Environments on Physical and Chemical Processes

Plasmonic nanolayers and laminar metallic/dielectric multilayers were originally developed for optical cloaking applications and lensing applications that could potentially image objects whose size was below the diffraction limit. These assemblies were initially formed from gold or silver nanorods grown within an alumina mesh. However, more recently, assemblies with similar properties have also been prepared by sequential thin-layer deposition of alternating layers of gold and magnesium fluoride (MgF 2 ). These metal/dielectric composite materials enable control of the dielectric constant in the directions perpendicular to the layers and balance the real and imaginary dielectric constants of the assembly such that the speed and the amplitude of the waves traveling through the assembly are not attenuated. In this Account, we will also focus on a few of the applications ranging from surface wetting to fluorescence quenching to enhancement of photochemical reactions. First, we will share an introduction to processes used to create these materials, which are combinations of low refractive index metals and transparent higher index materials arranged in a scalable repeating fashion. Two fabrication methods were employed: an electrochemical deposition of Ag nanorods into an anodized alumina matrix which produced materials with an anisotropic negative refractive index material within the plane of the film and lamellar metal/dielectric layers in which the negative index perpendicular to the growth direction. These alternating layers of plasmonic metals and dielectric materials were ultimately chosen to prepare films for further testing, because of their relative ease of fabrication. We will continue with a discussion of a few of the applications of both of these nonlocal dielectric composite materials including more specialized plasmonic, composite, and hyperbolic metamaterials including fluorescence quenching, photochemical reactions, and surface wetting. In each of these applications, the unique response caused by the enhancement of the electric field and the interface between hyperbolic materials and plasmonic materials as they interact photophysically with their near neighbors is presented. In each of the applications, the enhanced electric field extends from the composite substrate layer to interact with its near neighbors and beyond. Furthermore, the presence of this extended interaction can be observed in the form of decreased emission lifetime, enhancement of photochemical reaction rates, and changes in the surface energies measured by contact angle goniometry. In this Account, all of these situations will be addressed. Finally, we will conclude with a summary and vision for the future as well as a discussion of the unique challenges and opportunities available as research active faculty at an HBCU.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Probing time-resolved plasma-driven solution electrochemistry in a falling liquid film plasma reactor: Identification of HO$^−_2$ as a plasma-derived reducing agent

Many applications involving plasma–liquid interactions depend on the reactive processes occurring at the plasma–liquid interface. In this article, we report on a falling liquid film plasma reactor allowing for in situ optical absorption measurements of the time-dependence of the ferricyanide/ferrocyanide redox reactivity, complemented with ex situ measurement of the decomposition of formate. We found excellent agreement between the measured decomposition percentages and the diffusion-limited decomposition of formate by interfacial plasma-enabled reactions, except at high pH in thin liquid films, indicating the involvement of previously unexplored plasma-induced liquid phase chemistry enabled by long-lived reactive species. We also determined that high pH facilitates a reduction-favoring environment in ferricyanide/ferrocyanide redox solutions. In situ conversion measurements of a 1:1 ferricyanide/ferrocyanide redox mixture exceed the measured ex situ conversion and show that conversion of a 1:1 ferricyanide/ferrocyanide mixture is strongly dependent on film thickness. We identified three dominant processes: reduction faster than ms time scales for film thicknesses >100 µm, •OH-driven oxidation on time scales of <10 ms, and reduction on 15 ms time scales for film thickness <100 µm. We attribute the slow reduction and larger formate decomposition at high pH to HO$^−_2$ formed from plasma-produced H 2 O 2 enabled by the high pH at the plasma–liquid interface as confirmed experimentally and by computed reaction rates of HO$^−_2$ with ferricyanide. Overall, this work demonstrates the utility of liquid film reactors in enabling the discovery of new plasma-interfacial chemistry and the utility of atmospheric plasmas for electrodeless electrochemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Optical properties of cubic boron arsenide

The ultrahigh thermal conductivity of cubic boron arsenide (BAs) makes it a promising material for next-generation electronics and optoelectronics. Here, we report measured optical properties of BAs crystals, including the complex dielectric function, refractive index, and absorption coefficient in the ultraviolet, visible, and near-infrared wavelength range. In this work, the data were collected at room temperature using spectroscopic ellipsometry and transmission and reflection spectroscopy. We further calculated the optical response using density functional theory and many-body perturbation theory, considering quasiparticle and excitonic corrections. The computed values for the direct and indirect bandgaps (4.25 eV and 2.07 eV) agree well with the measured results (4.12 eV and 2.02 eV). Our findings pave the way for using BAs in future electronic and optoelectronic applications that take advantage of its demonstrated ultrahigh thermal conductivity and predicted high ambipolar carrier mobility.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Precision measurement of lifetime and branching ratios of the 4⁢𝑓 13⁡ 5⁢𝑑⁢6⁢𝑠 1 ⁢[5/2] 5/2 state in Yb + ions

We report spectroscopic and time-resolved experimental observations to characterize the [Xe]⁢4⁢𝑓 13 ⁡( 2 𝐹$^𝑜_{5/2}$)⁢5⁢𝑑⁢6⁢𝑠⁡( 1 𝐷)⁢ 1 ⁢[5/2]$^𝑜_{5/2}$ state in 172 Yb + ions. We access this state from the metastable 4⁢𝑓 14 ⁡5⁢𝑑⁡( 2 𝐷 3/2,5/2 ) manifold and observe an unexpectedly long lifetime of 𝜏 = 37.9⁢(9) ⁢µ⁢s that allows visible Rabi oscillations and resolved-sideband spectroscopy. Using a combination of coherent population dynamics, high-fidelity detection and heralded state preparation, and optical pumping methods, we measure the branching ratios to the 2 𝐷 3/2 , 2 𝐷 5/2 , and 2 𝑆 1/2 states to be 0.359⁢(2), 0.639(2), and 0.0023⁢(16), respectively. The branching ratio to the 4⁢𝑓 13⁡ 6⁢𝑠 2 ⁡( 2 𝐹 7/2 ) is compatible with zero within our experimental resolution. We also report measurements of Landé 𝑔-factor of the 1 ⁢[5/2]$^𝑜_{5/2}$ state. Further, the branching ratio of the 2 𝐷 5/2 to 2 𝑆 1/2 decay in 172 Yb + was measured to be 0.188(3), improving its relative uncertainty by an order of magnitude. Our measurements provide experimental benchmarks for better understanding the atomic structure of Yb + ions, which still lacks accurate numerical descriptions, and the use of high-lying excited states for partial detection and qubit manipulation in the omg architecture.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

SDSS-IV MaNGA: the physical origin of off-galaxy H α blobs in the local Universe

ABSTRACT H α blobs are off-galaxy emission-line regions with weak or no optical counterparts. They are mostly visible in H α line, appearing as concentrated blobs. Such unusual objects have been rarely observed and studied, and their physical origin is still unclear. We have identified 13 H α blobs in the public data of MaNGA survey, by visually inspecting both the optical images and the spatially resolved maps of H α line for ∼4600 galaxy systems. Among the 13 H α blobs, 2 were reported in previously MaNGA-based studies and 11 are newly discovered. This sample, though still small in size, is by far the largest sample with both deep imaging and integral field spectroscopy. Therefore, for the first time we are able to perform statistical studies to investigate the physical origin of H α blobs. We examine the physical properties of these H α blobs and their associated galaxies, including their morphology, environments, gas-phase metallicities, kinematics of ionized gas, and ionizing sources. We find that the H α blobs in our sample can be broadly divided into two groups. One is associated with interacting/merging galaxy systems, of which the ionization is dominated by shocks or diffuse ionized gas. It is likely that these H α blobs used to be part of their nearby galaxies, but were stripped away at some point due to tidal interactions. The other group is found in gas-rich systems, appearing as low-metallicity star-forming regions that are visually detached from the main galaxy. These H α blobs could be associated with faint discs, spiral arms, or dwarf galaxies.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Magnetic‐Field‐Switchable Laser via Optical Pumping of Rubrene

Abstract Volumetric optical imaging of magnetic fields is challenging with existing magneto‐optical materials, motivating the search for dyes with strong magnetic field interactions, distinct emission spectra, and an ability to withstand high photon flux and incorporation within samples. Here, the magnetic field effect on singlet‐exciton fission is exploited to demonstrate spatial imaging of magnetic fields in a thin film of rubrene. Doping rubrene with the high‐quantum yield dye dibenzotetraphenylperiflanthene (DBP) is shown to enable optically pumped, slab waveguide lasing. This laser is magnetic‐field‐switchable: when operated just below the lasing threshold, application of a 0.4 T magnetic field switches the device between nonlasing and lasing modes, accompanied by an intensity modulation of +360%. This is thought to be the first demonstration of a magnetically switchable laser, as well as the largest magnetically induced change in emission brightness in a singlet‐fission material to date. These results demonstrate that singlet‐fission materials are promising materials for magnetic sensing applications and could inspire a new class of magneto‐optical modulators.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Quantifying Temperature Dependence of Electronic Band Gaps and Optical Properties in SnO 2 and SnO via First-Principles Simulations

Tin metal oxides SnO x ( x = 1, 2) have gained interest as gas-sensing materials. For their applications as high-temperature sensors, however, a better understanding of their temperature dependence sensing responses is needed. Here, we comparatively quantify the temperature-dependent electronic band gaps and optical properties of SnO 2 and SnO using first-principles calculations. Without considering the temperature effect, SnO 2 and SnO are predicted to have direct and indirect band gaps of 2.18 and 1.66 eV, respectively, at the PBE + U -GGA level that we employed. The temperature effect on the electronic and optical properties is captured by taking account of the electron–phonon interaction. Band gap renormalization with temperature is calculated via the Allen–Heine–Cardona theory. For both oxides, we find a monotonic decrease in the electronic band gap such that renormalization at zero point (0 K) is ~–0.17 and ~–0.52 eV at 1000 K. These results are also analyzed by employing an analytical equation that helps characterize the band gap shift with temperature. In addition, the optical properties at finite temperatures are simulated using the frozen-phonon method that combines electron–phonon coupling with the momentum matrix. As temperature increases, the optical property spectra are smoothed because of the smearing effect, which diminishes optical constants at shorter wavelengths. Our results are of interest for high-temperature functional materials in applications of optical detection.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

First-Principles Study of Ferroelectric and Optical Properties in Derivatives of Thiourea

Organic ferroelectric materials in the form of molecular crystals are promising alternatives to well-known ferroelectric perovskite oxides due to their structural flexibility, tunability, and ease of processing. First-principles density functional theory calculations combined with group theory analyses are employed in this work to discuss polar nature of a class of derivatives of thiourea: CH 4 N 2 A where A = O, S, Se, and Te. Further, optical properties in the UV range along with thermodynamic and dynamic stability of such materials are also evaluated in the study. We find that CH 4 N 2 Te with bandgap energy of ~3.33 eV shows large spontaneous polarization of P = 10.92 μC/cm 2 . The electronic and optical properties become tunable under strain.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Reconfigurable plasma-dielectric hybrid photonic crystal as a platform for electromagnetic wave manipulation and computing

The introduction of 3D printing has enabled fabrication of photonic crystal devices with complex crystal structures that would be challenging to construct using other fabrication methods. In this paper, we construct and characterize a photonic crystal consisting of two 4 x 8 x 8 cubic lattices composed of spherical silicon nitride elements straddling a layer of 8 plasma discharge tubes, creating a 3D hybrid plasma photonic crystal device. Integrating under-dense gaseous plasma elements provides a unique coupling dynamic between the dielectric spheres and the cylindrical plasma discharges, creating a monolithic hybrid photonic crystal with solid state and reconfigurable elements. The device has resonant modes that have attenuation peaks that are either switchable, tunable in amplitude, or tunable in frequency with variations in plasma density. The response of these bands seen with varying plasma density is confirmed through simulations when effects due to the heating of the photonic crystal from the gaseous plasma elements are accounted for in the experiments. We discuss how this reconfigurable device may be used and expanded upon for applications in photonic artificial neural networks and optical computing systems.

3D printing↗
DOE OSTI2020

Formation and optical properties of IR photoluminescence centres in bismuth-containing aluminophosphate glass

We have prepared aluminophosphate glass samples differing in bismuth oxide content and demonstrating broadband near-IR photoluminescence. Analysis of their photoluminescence spectra leads us to conclude that they contain two main types of emission centres, one of which seems to be a bismuth monocation and the other is a cluster ion. In addition to these luminescence centres, the aluminophosphate glasses contain a nonluminescent bismuth-containing centre responsible for the broad, strong optical absorption band peaking at 450 nm. (active media)

36 MATERIALS SCIENCE↗
DOE OSTI2025

Deconstructing Chirality: Probing Local and Nonlocal Effects in Azobenzene Derivatives with X-ray Circular Dichroism

Resolving molecular chirality on the atomic scale remains a critical challenge in chemistry. Conventional Optical Circular Dichroism spectroscopy often overlooks subtle and localized structural features. Here, we computationally investigate site-specific X-ray circular dichroism (XCD) across a series of trans-azobenzene derivatives to deconstruct and interpret chiroptical signals at the atomic level. Our modeling reveals that XCD is capable of distinguishing dichroic contributions arising from both a local chiral center and a global molecular twist, revealing their intricate interplay and potential for constructive or destructive interference. We show that sterically induced global distortions can dominate the XCD signal in some cases, even suppressing the response from the chiral center itself. This insight suggests a new molecular design principle for tuning the chiroptical activity, which we extend by proposing strategies to achieve unidirectional photoisomerization through steric gearing. Altogether, this work establishes a quantitative framework for engineering chiroptical responses, laying the foundation for the design of functional chiral systems utilizing principles of unidirectional molecular motor-like conformational dynamics.

X-ray spectroscopy↗
DOE OSTI2023

Finding Peas in the Early Universe with JWST

The Early Release Observations (EROs) of JWST beautifully demonstrate the promise of JWST in characterizing the universe at Cosmic Dawn. We analyze the Near Infrared Spectrograph ERO spectra of three z ~ 8 galaxies to determine their metallicities, gas temperatures, and ionization. These galaxies offer the first opportunity to understand the physical properties of Epoch-of-Reionization galaxies through detailed rest-optical emission-line spectroscopy. We show that these objects have metal abundances $12+\mathrm{log}[{\rm{O}}/{\rm{H}}]\,\approx$ 6.9–8.3, based on both the T e method and on a recent calibration of the R 23 metallicity indicator. Since the spectra are some of the earliest science data from JWST, we compare several line ratios with values expected from robust physics, to validate our measurement procedures. We compare the abundances and emission-line ratios to a nearby sample of Green Pea galaxies—a population of nearby emission-line galaxies whose UV properties resemble Epoch-of-Reionization galaxies, and which often have large Lyman continuum escape fractions. The JWST data show striking further similarities between these high-redshift galaxies and nearby Green Peas. The z ~ 8 galaxies span the metallicity range covered by Green Peas. They also show the compact morphology that is typical of emission-line-dominated galaxies at all redshifts. Based on these similarities with Green Peas, it is likely that these are the first rest-optical spectra of galaxies that are actively driving cosmological reionization.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Direct Optical Lithography of Colloidal Metal Oxide Nanomaterials for Diffractive Optical Elements with 2π Phase Control

Spatially patterned dielectric materials are ubiquitous in electronic, photonic, and optoelectronic devices. These patterns are typically made by subtractive or additive approaches utilizing vapor-phase reagents. On the other hand, recent advances in solution-phase synthesis of oxide nanomaterials have unlocked a materials library with greater compositional, microstructural, and interfacial tunability. However, methods to pattern and integrate these nanomaterials in real-world devices are less established. In this work, we directly optically pattern oxide nanoparticles (NPs) by mixing them with photosensitive diazo-2-naphthol-4-sulfonic acid and irradiating with widely available 405 nm light. We demonstrate the direct optical lithography of ZrO 2 , TiO 2 , HfO 2 , and ITO NPs and investigate the chemical and physical changes responsible for this photoinduced decrease in solubility. Micron-thick layers of amorphous ZrO 2 NPs were patterned with micron resolution and shown to allow 2 pi phase control of visible light. We also show multilayer patterning and use it to fabricate features with different thicknesses and distinct structural colors. Upon annealing at 400 degrees C, the deposited ZrO 2 structures have excellent optical transparency across a wide wavelength range (0.3-10 mu m), a high refractive index (n = 1.84 at 633 nm), and are optically smooth. We then fabricate diffractive optical elements, such as binary phase diffraction gratings, that show efficient diffractive behavior and good thermal stability. Different oxide NPs can also be mixed prior to patterning, providing a high level of material tunability. This work demonstrates a general patterning approach that harnesses the processability and diversity of colloidal oxide nanomaterials for use in photonic applications.

2𝜋 phase shift↗