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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 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Realization of a wide steering end-fire facet optical phased array using silicon rich silicon nitride

The design, fabrication, and characterization of a 16-element optical phased array (OPA) using a high index (n = 3.1) silicon-rich silicon nitride (SRN) is demonstrated. Here, we present one-dimensional beam steering with end-fire facet antennas over a wide steering range of >115° at a fixed wavelength of 1525 nm. A beam width of 6.3° has been measured at boresight, consistent with theory. We demonstrate SRN as a viable material choice for chip-scale OPA applications due to its high thermo-optic coefficient, high optical power handling capacity [negligible two-photon absorption (TPA)], wide transparency window, and CMOS compatibility.

Nejadriahi, Hani↗
DOE OSTI2021

Double photoionization of atomic oxygen: Feshbach resonances in the two-electron continuum

In this work, we describe a joint experimental and theoretical investigation on oxygen double photoionization—the emission of two electrons from atomic oxygen following single photon absorption. High-resolution experimental measurements were performed at the Advanced Light Source, revealing sharp resonance structure superimposed on the more familiar Wannier-like, nearly-linear background. These resonance features are attributed to ionization-plus-excitation Feshbach resonances embedded in the double ionization continuum, doubly-excited states that lie above the double-ionization threshold. Such features are absent in the double photoionization cross section of He, or other quasi-two-electron systems, for which the doubly-ionized atomic core remains inert. For a corresponding theoretical analysis, the R-matrix with pseudostates (RMPS) method was invoked by calculating final-state, two-electron resonances-plus-continua wavefunctions and corresponding single-photon absorption cross sections. Overall agreement is found in the direct, background double photoionization cross section. However, the RMPS method, using a small basis due to practical computational limitations, was unable to reproduce quantitatively the smooth background or the sharper resonance features observed in the measurements, showing instead large-scale oscillations about the experimental background, and characteristic pseudoresonance jitter, associated with an insufficient convergence of the pseudostate representation to the true two-electron infinite series of Feshbach resonances embedded in the two-electron continuum. The prominent resonance structure observed highlights the need to consider multiple excitation processes in atoms more complex than He or quasi-two-electron systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Dark matter absorption via electronic excitations

We revisit the calculation of bosonic dark matter absorption via electronic excitations. Working in an effective field theory framework and consistently taking into account in-medium effects, we clarify the relation between dark matter and photon absorption. As is well-known, for vector (dark photon) and pseudoscalar (axion-like particle) dark matter, the absorption rates can be simply related to the target material’s optical properties. However, this is not the case for scalar dark matter, where the dominant contribution comes from a different operator than the one contributing to photon absorption, which is formally next-to-leading-order and does not suffer from in-medium screening. It is therefore imperative to have reliable first-principles numerical calculations and/or semi-analytic modeling in order to predict the detection rate. We present updated sensitivity projections for semiconductor crystal and superconductor targets for ongoing and proposed direct detection experiments.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Attosecond delays in X-ray molecular ionization

The photoelectric effect is not truly instantaneous, but exhibits attosecond delays that can reveal complex molecular dynamics. Sub-femtosecond duration light pulses provide the requisite tools to resolve the dynamics of photoionization. Accordingly, the past decade has produced a large volume of work on photoionization delays following single photon absorption of an extreme ultraviolet (XUV) photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required x-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. We have now measured the x-ray photoemission delay of core-level electrons, and here report unexpectedly large delays, ranging up to 700 attoseconds in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft x-ray pulses from a free-electron laser (XFEL) to scan across the entire region near the K-shell threshold. Furthermore, we find the delay spectrum is richly modulated, suggesting several contributions including transient trapping of the photoelectron due to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule, and multi-electron scattering effects. Finally, the results demonstrate how x-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Nonlinear X-ray Optics

Novel X-ray free-electron lasers (XFELs) are capable of producing radiation with unprecedented properties. Specifically, their ultrashort coherent X-ray pulses can generate extreme peak intensities where ordinary rules of light-matter interaction may no longer apply, and nonlinear processes start to become important. XFELs have made it possible to observe some of the most important coherent non-sequential nonlinearities, including X-ray-optical sum frequency generation (SFG), X-ray second harmonic generation (XSHG), two-photon absorption (TPA) and nonlinear two-photon Compton scattering (2PCS). In particular, the 2PCS experiment has led to unexpected results, namely the observation of a substantial anomalous red shift in the energy of photons generated by nonlinear two-photon X-ray Compton scattering in beryllium. The energy shift is in addition to the predicted nonlinear Compton shift and was neither expected from extrapolations from linear X-ray interactions nor from nonlinear effects at optical wavelengths. Our results suggest a novel nonlinear scattering mechanism that can only be observed at high fields at X-ray wavelengths, where the photon energy is a significant fraction of the electron rest mass (and thus a significant momentum transfer to the electron occurs during the scattering) and where the interaction is not dominated by the quiver motion of the electron in the field (ponderomotive potential) as is usually the case at longer (optical) wavelengths. The goal of this research project was the investigation of fundamental nonlinear X-ray-matter interactions. As these processes are typically weak, part of this research is the exploration of more efficient nonlinear X-ray processes by studying novel mechanisms including solid-state effects, the assistance of optical radiation and novel phase-matching techniques. These experiments require extremely large X-ray field strengths, such as produced by XFELs. Nonlinear X-ray effects can lead to important applications in many research fields. For example, it could lead to instantaneous plasma diagnostics for materials in extreme conditions, as a method for combining atomic-scale structural sensitivity with chemical specificity, or as a probe of electron dynamics in solids on the attosecond (1 as = 10 -18 s) time- and Ångstrom (10 -10 m) length scales. In addition, a detailed understanding of nonlinear X-ray matter interactions is crucial for understanding and extending the limits of structural determination at high intensity such as in serial femto-crystallography. The results could have a profound impact on advanced XFEL light sources such as the LCLS-II.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Symmetry Protected Two-Photon Coherence Time

We report the observation of symmetry protected two-photon coherence time of biphotons generated from backward spontaneous four-wave mixing in laser-cooled 87 Rb atoms. When biphotons are nondegenerate, nonsymmetric photonic absorption loss results in exponential decay of the temporal waveform of the two-photon joint probability amplitude, leading to shortened coherence time. In contrast, in the case of degenerate biphotons, when both paired photons propagate with the same group velocity and absorption coefficient, the two-photon coherence time, protected by space-time symmetry, remains unaffected by medium absorptive losses. Furthermore, our experimental results validate these theoretical predictions. This outcome highlights the pivotal role of symmetry in manipulating and controlling photonic quantum states.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Nonlinear optical properties of lanthanum titanate glasses prepared by levitation melting

Lanthanum titanate glasses (17 La 2 O 3 -83 TiO 2 ) are fabricated via aerodynamic levitation melting. Here, nonlinear refraction and absorption were measured with the Z scan technique using ps optical pulses at 532 nm wavelength with peak intensities in the range of 0.25–2.5 GW/cm 2 . The two-photon absorption coefficient (β) and the effective nonlinear refraction coefficient (⁠$n^{eff}_{2}$) are found to be, respectively, 2.19 cm/GW and 152 × 10 -16 cm 2 /W (85 × 10 -13 esu). The Raman gain is measured to be 106 × 10 -11 cm/W. The nonlinearity strength is found to be nearly 60 times larger in lanthanum titanate glasses relative to silica.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Photon-recoil and laser-focusing limits to Rydberg gate fidelity

Limits to Rydberg gate fidelity that arise from the entanglement of internal states of neutral atoms with the motional degrees of freedom due to the momentum kick from photon absorption and re-emission is quantified. This occurs when the atom is in a superposition of internal states but only one of these states is manipulated by visible or UV photons. The Schrödinger equation that describes this situation is presented and two cases are explored. In the first case, the entanglement arises because the spatial wave function shifts due to the separation in time between excitation and stimulated emission. For neutral atoms in a harmonic trap, the decoherence can be expressed within a sudden approximation when the duration of the laser pulses are shorter than the harmonic oscillator period. In this limit, the decoherence is given by simple analytic formulas that account for the momentum of the photon, the temperature of the atoms, the harmonic oscillator frequency, and atomic mass. In the second case, there is a reduction in gate fidelity because the photons causing absorption and stimulated emission are in focused beam modes. This leads to a dependence of the optically induced changes in the internal states on the center of mass atomic position. In the limit where the time between pulses is short, the decoherence can be expressed as a simple analytic formula involving the laser waist, temperature of the atoms, the trap frequency, and the atomic mass. These limits on gate fidelity are studied for the standard π-2π-π Rydberg gate and a protocol based on a single adiabatic pulse with a Gaussian envelope.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Observation and origin of multi-THz quantum beats in superfluorescent emission from argon

We report observation of multi-THz quantum beats in the amplitude of superfluorescence in pure argon gas, using a time delayed 780-nm probe beam that interrogates the relevant population densities. The superfluorescence is induced by three-photon absorption of an ultrashort 260.5-nm laser pulse that creates coherent and coupled populations in multiple closely spaced 3⁢d and 5⁢s Ar levels. Argon pressure and pump laser focusing parameters are seen to modify the frequency of the quantum beats, which is attributed to the absorption of the self-generated, nonresonant third harmonic of the pump from Ar near the zero of the real part of the overlapping linear susceptibilities of the closely spaced 3⁢d and 5⁢s excited states. The self-absorption of the phase-matched THG photons creates a coherent population of atoms which acts like an atomic excited state (3⁢ω-induced state). Furthermore, we have also observed a new two-step superfluorescent cascade that results from the population redistribution enabled by the 780-nm probe pulse between the 3⁢d'[5/2] 3 and the 3⁢ω-induced state and gives rise to a previously unknown transition that emits on 1587 nm.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Measurement and control of optical nonlinearities in dispersive dielectric multilayers

Dispersive dielectric multilayer mirrors, high-dispersion chirped mirrors in particular, are widely used in modern ultrafast optics to manipulate spectral chirps of ultrashort laser pulses. Dispersive mirrors are routinely designed for dispersion compensation in ultrafast lasers and are assumed to be linear optical components. In this work, we report the experimental characterization of an unexpectedly strong nonlinear response in these chirped mirrors. At modest peak intensities <2 TW/cm 2 —well below the known laser-induced damage threshold of these dielectric structures—we observed a strong reflectivity decrease, local heating, transient spectral modifications, and time-dependent absorption of the incident pulse. Through computational analysis, we found that the incident laser field can be enhanced by an order of magnitude in the dielectric layers of the structure. The field enhancement leads to a wavelength-dependent nonlinear absorption, that shows no signs of cumulative damage before catastrophic failure. The nonlinear absorption is not a simply two-photon process but instead is likely mediated by defects that facilitate two-photon absorption. To mitigate this issue, we designed and fabricated a dispersive multilayer design that strategically suppresses the field enhancement in the high-index layers, shifting the high-field regions to the larger-bandgap, low-index layers. This strategy significantly increases the maximum peak intensity that the mirror can sustain. However, our finding of an onset of nonlinear absorption even at ‘modest’ fluence and peak intensity has significant implications for numerous past published experimental works employing dispersive mirrors. Additionally, our results will guide future ultrafast experimental work and ultrafast laser design.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Third-order photon correlations extract single-nanocrystal multiexciton properties in solution

Colloidal semiconductor nanocrystals are considered promising materials for high-flux optical applications, including lasing, light-emitting diodes, biological imaging, and quantum optics. In high-flux applications, multiexcitons can significantly contribute to emission, influencing its brightness, spectral purity, and kinetics. As a result, understanding and controlling multiexciton emission in colloidal nanocrystal materials is of the utmost importance. In the past, single-nanocrystal photon correlation methods have been applied to understand biexciton and triexciton efficiencies, lifetimes, and spectra. While powerful, such methods suffer from user selection bias and require stable emission from single nanocrystals. To compensate for this shortcoming, second-order correlation methods were developed to extract sample-averaged biexciton properties from a solution of nanocrystals. Until now, however, the analogous third-order solution photon correlation methods remained unexplored. In this work, we present a pair of third-order photon correlation techniques to obtain the sample-averaged single-nanocrystal triexciton quantum yield and lifetime in a solution-phase experiment. These techniques derive from the relationship between the Poisson probability of nanocrystal photon absorption and the intrinsic probability of nanocrystal photon emission. We validate the theoretical background of these techniques by creating a numerical model to simulate the diffusion and emission of many nanocrystals in solution. Our simulations confirm that the average triexciton quantum yield and triexciton lifetime can be extracted from a solution of nanocrystals. These techniques will enable researchers to gain a better understanding of the fundamental multiexciton properties of colloidal nanocrystals.

Horowitz, Jonah R. [Massachusetts Institute of Tec↗
DOE OSTI2021

Photo-exfoliation of MoS 2 quantum dots from nanosheets: an in-situ transmission electron microscopy study

Fabrication of transition metal dichalcogenide (TMD) quantum dots (QDs) is complex and requires submerging of powders in binary solvents and the constant tuning of wavelength and pulsed frequency of light to achieve a desired reaction. Here,iInstead of liquid state photoexfoliation, we utilize infrared laser irradiation of free-standing MoS 2 flakes in transmission electron microscope (TEM) to achieve solid-state multi-level photoexfoliation of QDs. By investigating the steps involved in photochemical reaction between the surface of MoS 2 and the laser beam, we gain insight into each step of the photoexfoliation mechanism and observe high yield production of QDs, led by an inhomogeneous crystalline size distribution. Additionally, by using a laser with a lower energy than the indirect optical transition of bulk MoS 2 , we conclude that the underlying phenomena behind the photoexfoliation is from multi-photon absorption achieved at high optical outputs from the laser source. These findings provide an environmentally friendly synthesis method to fabricate QDs for potential applications in biomedicine, optoelectronics, and fluorescence sensing.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Photon management in silicon photovoltaic cells: A critical review

With the practical efficiency of the silicon photovoltaic (PV) cell approaching its theoretical limit, pushing conversion efficiencies even higher now relies on reducing every type of power loss that can occur within the device. Limiting optical losses is therefore critical and requires effective management of incident photons in terms of how they interact with the device. Ultimately, photon management within a PV cell means engineering the device and constituent materials to maximize photon absorption within the active semiconductor and therefore reduce the number of photons lost through other means, most notably reflection and parasitic absorption. There have been great advancements in the front and the rear side photon management techniques in recent years. This review aims to discuss these advancements and compare the various approaches, not only in terms of increases in photogenerated current, but also their compatibility with different PV cell architectures and potential trade-offs, like increased surface recombination or scalability for high-volume manufacturing. In this review, a comprehensive discussion of a wide variety of the front and the rear side photon management structures are presented with suggestions to improve the already achieved performance further. Here, this review is unique because it not only presents the recent development in photon management techniques, but also offers through analysis of these techniques and pathways to improve further.

14 SOLAR ENERGY↗
DOE OSTI2022

A diagnostic to measure neutral-atom density in fusion-research plasmas

For this study, a femtosecond two-photon-absorption laser-induced-fluorescence (TALIF) diagnostic was designed, installed, and operated on the Princeton-Field-Reversed Configuration-2 device to provide non-invasive measurements of the time and spatially resolved neutral-atom densities in its plasmas. Calibration of the H o density was accomplished by comparison with Kr TALIF. Measurements on plasmas formed of either H 2 or Kr fill gases allowed examination of nominally long and short ionization mean-free-path regimes. With multi-kW plasma heating and H 2 fill gas, a spatially uniform H o density of order 10 17 m –3 was measured with better than ±2 mm and 10 µs resolution. Under similar plasma conditions but with Kr fill gas, a 3-fold decrease in the in-plasma Kr density was observed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

O · , H · , and · OH radical etching probability of polystyrene obtained for a radio frequency driven atmospheric pressure plasma jet

Atmospheric pressure plasma jets have great potential for the surface modification of polymers. In this work, the authors report on polystyrene etching by a radio frequency driven atmospheric pressure plasma jet with a focus on the role of H · , O · , and · OH radicals in this process. The absolute flux of H · , O · , and · OH radicals reaching the surface of the polymer was determined by a COMSOL MULTIPHYSICS reacting fluid dynamics model incorporating detailed transport phenomena in the boundary layer near the substrate. The simulated results of H · and · OH densities in the jet effluent were experimentally verified by two-photon absorption laser induced fluorescence and laser induced fluorescence, respectively. The carbon atom removal flux from the polystyrene surface was taken from previously reported measurements using the same plasma source. The authors show that the boundary layer effects in the interfacial region above the substrate can have a significant impact on the calculated etching probabilities. The reaction probability (β) has a significant uncertainty although a variation of 2 orders of magnitude in β leads to uncertainties of approximately 1 order of magnitude variation in the determined etching probability. The etching probability of polystyrene by · OH radicals was confirmed to be at least an order of magnitude larger than the polystyrene etching probability by O · radicals. The authors also confirmed the weak polystyrene etching probability by H · radicals. The model suggests that the presence of a 30 ppm O 2 impurity can lead to the production of · OH radicals in the far effluent of the Ar + 1% H 2 plasma jet close to the substrate at sufficient densities to enable effective etching.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Measurement of atomic oxygen densities using TALIF on a dielectric barrier discharge: insights into the volume above a micro cavity plasma array

Dielectric barrier discharges, particularly micro cavity plasma arrays, offer significant potential for plasma-catalytic research due to their ability to ignite plasma in direct contact with a catalytic surface, enabling the observation of plasma-surface interactions. A key factor in their application is the generation of reactive species, such as atomic oxygen, within the cavities. These species can interact with both the surface (e.g. for activation or cleaning) and the gas being treated (e.g. for oxidation). Given the central role of oxygen atoms in plasma catalysis and their use as a model for more complex species, this work investigates the transport of these atoms out of the cavities. Two-photon absorption laser-induced fluorescence spectroscopy with picosecond laser excitation is performed in the volume above the cavities. The results are compared with a basic diffusion model. The reactor operates with a He/O 2 mixture at a flow rate of 1 slm and atmospheric pressure. Densities of up to 10 16 cm -3 are measured near the surface. Time-dependent measurements show that, at a distance of 350 µm from the surface, a density equilibrium is reached within less than 3 ms of reactor operation. Decay times due to ozone formation after the reactor is turned off are on a similar scale. Spatially resolved measurements show that the oxygen density decreases exponentially from the surface but remains detectable up to approximately 1 mm above the surface, indicating significant application potential. Variations in the O 2 admixture show a density maximum at 0.4%, confirming previous helium state enhanced actinometry measurements within the cavities.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Using Ultrafast Entangled Photon Correlations to Measure the Temporal Evolution of Optically Excited Molecular Entanglement (Final Technical Report)

The goal of this project is to build an ultrafast entangled photon spectrometer and use it to measure theoretical predictions that photoexcited states are enhanced by spin-photon interactions. Entanglement of two states describes a specific type of quantum superposition in which measuring one state gives information about a second state. While entanglement is well explored for quantum information and computing systems, its effects on photoexcited states are less understood, especially in the ultrafast domains of molecular vibronic coupling. The grant designs a frequency and temporally resolved entangled photon spectrometer and uses it to test theoretical predictions like enhanced two photon absorption, non-reciprocal Fourier relations, and coupling of photons to spin systems. The end goal of the project is an understanding of how, when, and where entanglement is useful for spectroscopy.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Decoupling absorption and radiative cooling in mid-wave infrared bolometric elements

We present a spectrally selective, passively cooled mid-wave infrared bolometric absorber engineered to spatially and spectrally decouple infrared absorption and thermal emission. The structure leverages an antenna-coupled metal–insulator–metal resonance for mid-wave infrared normal incidence photon absorption and a long-wave infrared optical phonon absorption feature, aligned closer to peak room temperature thermal emission. The phonon-mediated resonant absorption enables a strong long-wave infrared thermal emission feature limited to grazing angles, leaving the mid-wave infrared absorption feature undisturbed. The two independently controlled absorption/emission phenomena demonstrate decoupling of the photon detection mechanism from radiative cooling and offer a new design approach enabling ultra-thin, passively cooled mid-wave infrared bolometers.

Ware, Alexander (ORCID:0009000256937727)↗