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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Multiplexing of frequency-modulation spectroscopy by spread-spectrum codes, demonstrated in continuous-wave LIDAR

Frequency-modulation spectroscopy (FMS) is generally suited to code-division multiplexing, and we demonstrate that capacity in a form of continuous-wave LIDAR, utilizing a sharp CO 2 absorption transition at 1.6 µm in simple ranging setups. The approach retains the advantages of FMS, including coherent detection and good rejection of broad absorption backgrounds. Extensions of this multiplexed approach to the continuous, simultaneous detection of several transitions would come by transmitting an encoded combination of frequency-modulated carriers, each tuned to detect a unique absorption transition. Signal analysis at the receiver involves a simple process of de-multiplexing that, in a general application, reveals targets at various distances and the absorption-related FMS signals in between.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

One-colour (~220 nm) resonance-enhanced (S 1 –S 0 ) multi-photon dissociation of acetylene: probe of the C 2 A 1 Π u – X 1 Σ + g band by frequency-modulation spectroscopy

In a recent paper, we demonstrated that one-colour (~220 nm), resonance-enhanced (S 1 –S 0 ), photodissociation of acetylene generates strong $C_2$ Swan band ($d^3Π_g–a^3Π_u$) and $C_2$ Deslandres-d'Azambuja band ($C^1Π_g–A^1Π_u$) fluorescence, and long-lived (>3 µs) fluorescence from an electronically-excited $C_2$H * species. It was not known whether the $C_2A^1Π_u$ and $X^1Σ^+_g$ states are also directly populated in this process. In this paper, multiple vibration-rotation transitions between the $C_2A$-state v = 2 and the X-state v = 0 level are examined by time-resolved frequency-modulation (FM) spectroscopy. The photolysis laser wavelength is tuned into resonance at the one-photon level with S 1 –S 0 transitions that populate individual rotational levels of the S 1 $_{trans}$-conformer $3^2,3^3,$ and $3^4$ vibrational states. By comparing the phase of the FM signals from the $C_2A–X$ transitions with that from the Rb D 1 -line absorption transition, we determine that, for all of the probed A–X transitions, the X-state level is more populated than the A-state level. We propose that the acetylene S 1 level is excited by the second photon to an acetylene dissociation precursor state, which undergoes sequential C-H bond-breaking to produce the $C_2X$ state. The dissociation precursor is assigned as the $1^1B_g(trans-bent)/1^1B_1(cis-bent)$ valence state, which correlates to a doubly-excited configuration, $(1π_u)^2(1π_g)^2$, at linear geometry. Based on the rotational distributions of the $C_2X$-state fragments, we believe that at least one of the transition states involved in the photolysis via S 1 $3^4$ has a larger CC-H bend-angle for the departing H-atom than that involved in the S 1 $3^2$ and $3^3$ photolysis.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Near-MHz temperature and H 2 O measurements in post-detonation fireballs of 25 g hemispherical explosives using scanned-wavelength-modulation spectroscopy

A laser absorption spectroscopy diagnostic integrated within a hardened optical probe was used to measure temperature and water mole fraction at 500 kHz in post-detonation fireballs of explosives. In the experiments, an exploding-bridgewire detonator initiated a 25 g hemisphere of explosive (N5 or PETN). This produced a hemispherical fireball that traveled radially towards a hardened measurement probe. The probe contained a pressure transducer and optical equipment to pitch fiber-coupled laser light across a 12.6 cm gap onto a detector. Tunable diode lasers emitting near 7185.6 and 6806 c m − <#comment/> 1 were used to measure the absorbance spectrum of H 2 O utilizing peak-picking scanned-wavelength-modulation spectroscopy with a scan frequency of 500 kHz and modulation frequencies of 35 and 45.5 MHz, respectively. This enabled measurements of temperature and X H 2 O in the shock-heated air and trailing fireball at 500 kHz. Time histories of pressure, temperature, and H 2 O mole fraction were acquired at different standoff distances to quantify how the fireball evolved in space and time as well as to compare measured quantities between PETN and N5 fireballs. The standard deviation of temperature and X H 2 O during one representative test were found to be 17 K (1.3%) and 0.011 (5%), respectively. These measurements demonstrate this diagnostic’s ability to provide rapid and reliable measurements in harsh, highly transient post-detonation environments produced by solid explosives.

Schwartz, Charles J.↗
DOE OSTI2023

THz Plasmonics and Topological Optics of Weyl Semimetals

THz magneto-optical properties of 3D topological Weyl semimetals were investigated with both THz spectroscopy and THz pump-probe measurements. The unique THz effects predicted in these materials may have important applications in THz technology. The electronic band structure was characterized spectroscopically through THz zero-field reflectance and/or cyclotron resonance measurements. The studies included the dynamic chiral pumping and the study of the predicted novel magneto-electric effects arising from the underlying Berry curvature and magneto plasmonic-like effects in the absence of an applied magnetic field. Chiral pumping in the extreme quantum limit was studied on Weyl semimetals to directly probe the chiral N=0 Landau level. Non-linear pump-probe measurements were used to measure the chiral pumping lifetime. Solids with topologically robust electronic states exhibit unusual electronic and optical transport properties that do not exist in other materials. A particularly interesting example is chiral charge pumping, the so-called chiral anomaly, in recently discovered topological Weyl and Dirac semimetals, where simultaneous application of parallel DC electric and magnetic fields creates an imbalance in the number of carriers of opposite topological charge (chirality). In an earlier study we investigated the Weyl metals Na 3 Bi and Cd 3 As 2 . In this grant we followed up with magneto-optical studies of TaAs, another Weyl semimetal. More recently, we have also characterized other Weyl and Dirac systems that have come on line. The Physics community is still looking for the “hydrogen atom” of the Weyl semimetal. CoSi is one promising new system which features Weyl node spacing comparable to the Brillouin zone size. This system may be suitable for study of the predicted chiral plasmons that arise from the Berry curvature in Weyl materials. In other experiments gates can be applied to the samples in order to study the Fermi arc surface states by modulation reflectance spectroscopy at THz frequencies.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Watching Polarons Move in the Energy and Frequency Domains Using Color Impedance Spectroscopy

The hybrid electronic–ionic transport property of π-conjugated polymers enables new (opto)electrochemical device constructs for energy conversion and storage and biosensing applications. One major challenge is separating the energy and frequency dependence of Faradaic events–those involving charge transfer and the redox processes of the conjugated backbone–from the non-Faradaic components, such as ionic motion. Herein, we combine optical spectroscopy with electrochemical impedance spectroscopy (EIS) to resolve the frequency response of ionic–electronic coupling as a function of electrochemical doping potential. First, using EIS, we identify two different frequency regimes resulting in potential-dependent capacitive elements on the order of ~10 μF/cm 2 in a high-frequency regime and ~50–150 μF/cm 2 in a low-frequency regime. Given the larger magnitude and greater potential dependence, we posit that polaronic motion is more likely to occur at low frequencies (<1 kHz) and overlaps with ionic motion. The use of color impedance spectroscopy (CIS) enables observation of polaronic motion with frequency modulation. We observe that higher doping potentials show a greater motion of polarons above the DC-bias baseline concentration for onset in electrochemical doping, but all potentials considered demonstrate a critical frequency at which the polaronic motion is “frozen” (~40 Hz). Furthermore, this critical information obtained from CIS in highly dielectric environments offers a unique figure of merit for future studies on electronic–ionic coupling by which to compare across polymer/electrolyte interfaces, including the role of a charge-supporting electrolyte, a solvent, and alternative Faradaic processes (e.g., electrocatalysis).

36 MATERIALS SCIENCE↗
DOE OSTI2024

Integrated frequency-modulated optical parametric oscillator

Optical frequency combs have revolutionized precision measurement, time-keeping, and molecular spectroscopy. A substantial effort has developed around "microcombs": integrating comb-generating technologies into compact, reliable photonic platforms. Current approaches for generating these microcombs involve either the electro-optic (EO) or Kerr mechanisms. Despite rapid progress, maintaining high efficiency and wide bandwidth remains challenging. Here, we introduce a new class of microcomb -- an integrated optical frequency comb generator that combines electro-optics and parametric amplification to yield a frequency-modulated optical parametric oscillator (FM-OPO). In stark contrast to EO and Kerr combs, the FM-OPO microcomb does not form pulses but maintains operational simplicity and highly efficient pump power utilization with an output resembling a frequency-modulated laser. We outline the working principles of FM-OPO and demonstrate them by fabricating the complete optical system in thin-film lithium niobate (LNOI). We measure pump to comb internal conversion efficiency exceeding 93% (34% out-coupled) over a nearly flat-top spectral distribution spanning approximately 1,000 modes (approximately 6 THz). Compared to an EO comb, the cavity dispersion rather than loss determines the FM-OPO bandwidth, enabling broadband combs with a smaller RF modulation power. The FM-OPO microcomb, with its robust operational dynamics, high efficiency, and large bandwidth, contributes a new approach to the field of microcombs and promises to herald an era of miniaturized precision measurement, and spectroscopy tools to accelerate advancements in metrology, spectroscopy, telecommunications, sensing, and computing.

42 ENGINEERING↗
DOE OSTI2023

Implementing an electronic sideband offset lock for isotope shift spectroscopy in radium

We demonstrate laser frequency stabilization with at least 6 GHz of offset tunability using an in-phase/quadrature (IQ) modulator to generate electronic sidebands (ESB) on a titanium sapphire laser at 714 nm and we apply this technique to perform isotope shift spectroscopy of 226 Ra and 225 Ra. By locking the laser to a single resonance of a high finesse optical cavity and adjusting the lock offset, we determine the frequency difference between the magneto-optical trap (MOT) transitions in the two isotopes to be 2630.0 ± 0.3 MHz, a factor of 29 more precise than the previously available data. Using the known value of the hyperfine splitting of the 3 P 1 level, we calculate the isotope shift for the 1 S 0 to 3 P 1 transition to be 2267.0 ± 2.2 MHz, a factor of 8 more precise than the best available value. Our technique could be applied to countless other atomic systems to provide unprecedented precision in isotope shift spectroscopy and other relative frequency comparisons.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Semi-Transparent Perovskite Solar Cells in a Stacked Tandem Module: Cooperative Research and Development Final Report, CRADA Number CRD-19-00810

This project seeks to develop device design, materials composition, and processing tools and parameters to fabricate semi-transparent perovskite solar cells and modules for application in stand-alone products or added to other solar cells in a mechanically stacked tandem configuration. This technology presents significant advanced manufacturing challenges and opportunities in getting to scale, including development of perovskite inks, scalable perovskite and heterojunction deposition and annealing processes, heterojunction composition, transparent electrode composition and deposition process, anti-reflection layer composition and deposition process, and cell to module integration processes. Modification 5: The proposed project seeks to develop device design, materials composition, and processing tools and parameters to fabricate semi-transparent perovskite solar cells and modules for application in stand-alone products or added to other solar cells in a mechanically-stacked tandem configuration. This technology presents significant advanced manufacturing challenges and opportunities in getting to scale, including development of perovskite inks, scalable perovskite and heterojunction deposition and annealing processes, heterojunction composition, transparent electrode composition and deposition process, passivation layers including in module scribes, anti-reflection layer composition and deposition process, and cell to module integration processes. Advanced metrology and characterization will be performed on perovskite films, cells and module. Furthermore, we will examine module or materials recycling for circular economy considerations. Modifcation 6: Gigahertz frequency microwave pump-probe spectroscopies are highly sensitive to thin film semiconductor photoconductivity of individual and stacks of layers that comprise perovskite solar cells. As such, these techniques will be used to qualify reproducibility and quality correlations during the manufacturing process. Modification 7: Mechanical adhesion of top contacts within perovskite modules significantly impacts the durability of the module when exposed to accelerated degradation testing. The adhesion between the perovskite/transport layer interface and the transport layer/top contact interface are both very sensitive small changes in processing. ALD processing conditions of the transport layer will be tuned to optimize the mechanical adhesion within the perovskite module stack.

14 SOLAR ENERGY↗
DOE OSTI2023

Dispersive Charge Transfer State Electroluminescence in Organic Solar Cells

Abstract The notion of quasi‐equilibrium is central to most solar cells; however, it has been questioned in organic photovoltaics (OPVs) owing to strong energetic disorder that frustrates efficient relaxation of electrons and holes within their respective density of states (DOS). Here, modulation electroluminescence (EL) spectroscopy is applied to OPVs and it is found that the frequency response of charge transfer (CT) state EL on the high energy side of the spectrum differs from that of the low energy side. This observation confirms that static disorder contributes substantially to the linewidth of the steady‐state EL spectrum and is unambiguous proof that the distribution of CT states formed by electrical injection in the dark is not in quasi‐equilibrium. These results emphasize the need for caution when analyzing OPV cells on the basis of reciprocity models that assume quasi‐equilibrium holds, and highlight a new method to study this unusual aspect of OPV operation.

14 SOLAR ENERGY↗
DOE OSTI2021

SILIA: software implementation of a multi-channel, multi-frequency lock-in amplifier for spectroscopy and imaging applications

In this work, we describe a software implementation of a multi-channel, multi-frequency Lock-in Amplifier (SILIA) to extract modulated signals from noisy data distributed over multiple channels of arbitrary number and size. This software implementation emulates the functionality of a multi-channel, multi-frequency lock-in amplifier in a post-processing step following data acquisition. Unlike most traditional lock-in amplifiers, SILIA can work with any number of input channels and is especially useful to analyze data distributed over many channels. We demonstrate the versatility and performance for extracting weak signals in spectroscopy and fluorescence microscopy. We also discuss more general applications and exhibit a method to automatically estimate error from a lock-in result.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Identity of the JET M-mode and the ASDEX Upgrade I-phase phenomena

An H-mode plasma state free of edge-localized mode (ELM), close to the L-H transition with clear density and temperature pedestal has been observed both at the Joint European Torus (JET) and at the ASDEX Upgrade (AUG) tokamaks usually identified by a low frequency (LFO, 1–2 kHz), m = 1, n = 0 oscillation of the magnetics and the modulation of pedestal profiles. The regime at JET is referred to as M-mode while at AUG as intermediate phase or I-phase. This contribution aims at a comparative analysis of these phenomena in terms of the density and temperature pedestal properties, the magnetic oscillations and symmetries. Lithium beam emission spectroscopy (Li-BES) and reflectometer measurements at JET and AUG show that the M-mode and the I-phase modulates the plasma edge density. A high frequency oscillation of the magnetics and the density at the pedestal is also associated with both the M-mode and the I-phase, and its power is modulated with the LFO frequency. The power modulation happens simultaneously in every Mirnov coil signal where it can be detected. The bursts of the magnetic signals and the density at the pedestal region are followed by the flattening of the density profile, and by a radially outward propagating density pulse in the scrape-off layer (SOL). The analysis of the helium line ratio spectroscopy (He-BES) signals at AUG revealed that the electron temperature is modulated in phase with the density, thus the I-phase modulates the pressure profile gradient. Overall, this analysis gave opportunity to compare Li-BES and He-BES density profiles at different locations suggesting a toroidal and poloidal symmetry of the density modulation. The presented results indicate that the regimes, the AUG I-phase and the JET M-mode, exhibit similar characteristics, which leads to the conclusion that the regimes are likely the same.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Near-field imaging and spectroscopy of terahertz resonators and metasurfaces [Invited]

Terahertz (THz) metasurfaces have become a key platform for engineering light-matter interaction at THz frequencies. They have evolved from simple metallic resonator arrays into tunable and programmable devices, displaying ultrafast modulation rates and incorporating emerging quantum materials. The electrodynamics which govern metasurface operation can only be directly revealed at the scale of subwavelength individual metasurface elements, through sampling their evanescent fields. It requires near-field spectroscopy and imaging techniques to overcome the diffraction limit and provide spatial resolution down to the nanoscale. Through a series of case studies, this review provides an in-depth overview of recently developed THz near-field microscopy capabilities for research on metamaterials.

Hale, Lucy L. (ORCID:0000000176544272)↗
DOE OSTI2021

Evidence of E × B staircase in HL-2A L-mode tokamak discharges

Theory and simulation suggest the existence of an E ×B staircase in the plasma core consisting of a series of nested m/n = 0/0 E×B shear layers that regulate turbulent transport across the layers together with mesoscale transport events occurring between them. Here, we show evidence for these phenomena in HL-2A L-mode discharges. Both high resolution electron cyclotron emission Te profiles and frequency modulated continuous wave reflectometer ne profiles show multiple gradient corrugations. The analysis of simultaneous poloidally and radially separated beam emission spectroscopy turbulent density fluctuation measurements over most of the minor radius of the plasma provides the evidence of eddy tilting and propagation direction reversals largely coincident with the profile corrugations, with long-range transport events occurring between these locations. The results provide significant additional evidence for the existence of an E × B staircase that influences particle and heat transport in L-mode discharges.

Liu, Wenbin (ORCID:0000000310424117)↗
DOE OSTI2024

Efficient Optical Control of Magnon Dynamics in van der Waals Ferromagnets

Optical control of magnons in two-dimensional (2D) materials promises new functionalities for spintronics and magnonics in atomically thin devices. Here, we report control of magnon dynamics, using laser polarization, in a ferromagnetic van der Waals (vdW) material, Fe 3.6 Co 1.4 GeTe 2 . The magnon amplitude, frequency, and lifetime are controlled and monitored by time-resolved pump-probe spectroscopy. We show substantial (over 25%) and continuous modulation of magnon dynamics as a function of incident laser polarization. Our results suggest that the modification of the effective demagnetization field and magnetic anisotropy by the pump laser pulses with different polarizations is due to anisotropic optical absorption. This implies that pump laser pulses modify the local spin environment, which enables the launch of magnons with tunable dynamics. Our first-principles calculations confirm the anisotropic optical absorption of different crystal orientations. Our findings suggest a new route for the development of opto-spintronic or opto-magnonic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Cosolvent-tuned interactions in ionic liquids: A vibrational and quantum-chemical study of ethylene glycol ratio effects

Ionic liquids (ILs) are attractive media for CO 2 capture but remain limited by viscosity and cost. Blending ILs with ethylene glycol (EG) is a practical route to mitigate these constraints, yet the molecular origins of cosolvent effects and their dependence on composition are not well resolved. We combine Fourier-transform infrared (FT-IR) spectroscopy with quantum-chemical (DFT) analysis to elucidate how the IL:EG molar ratio modulates intermolecular interactions and electronic structure. Computed vibrational frequencies enable mode assignment and deconvolution of overlapping bands, revealing systematic, ratio-dependent shifts and broadenings in (i) EG O–H stretching, (ii) cation and EG C–H stretchings (imidazolium C2–H, C4–H, C5–H, methyl and ethyl groups, -CH2 of EG), (iii) anion signature modes (e.g., CN motifs), and (iv) EG C–O and C–C stretchings, consistent with the redistribution of hydrogen-bonding networks. Molecular electrostatic potential (MESP) maps quantify attenuation of extreme potential regions with increasing EG, indicating progressive screening of cation–anion electrostatic interactions. Quantum Theory of Atoms in Molecules (QTAIM) identifies emergent bond critical points between EG and the IL ions, while Reduced Density Gradient–Noncovalent Interaction (RDG–NCI) analysis differentiates strong directional hydrogen bonds from dispersive contacts across compositions. Together, these results show that EG fraction controls a switch from predominantly ion–ion to mixed ion–EG coordination, altering local polarity and polarizability that underlie the observed FT-IR trends. The framework provides composition–structure–spectrum relationships that can guide rational selection of IL:EG ratios to balance favorable molecular interactions with practical performance targets in scalable CO 2 capture systems.

DAC↗
DOE OSTI2024

Broadband rapid-scanning phase-modulated Fourier transform electronic spectroscopy

We present a phase-modulated approach for ultrabroadband Fourier transform electronic spectroscopy. To overcome the bandwidth limitations and spatial chirp introduced by acousto-optic modulators (AOMs), pulses from a 1 µm laser are modulated using AOMs prior to continuum generation. This phase modulation is transferred to the continuum generated in a yttrium aluminum garnet crystal. Separately generated phase-modulated continua in two arms of a Mach-Zehnder interferometer interfere with the difference of their modulation frequencies, enabling physical under-sampling of the signal and the suppression of low-frequency noise. By interferometrically tracking the relative time delay of the continua, we perform continuous, rapid-scanning Fourier transform electronic spectroscopy with a high signal-to-noise ratio and spectral resolution. As proof of principle, we measure the linear absorption and fluorescence excitation spectra of a laser dye and various biological samples.

Javed, Ariba↗
DOE OSTI2022

Remote surface optical phonon scattering in ferroelectric Ba 0.6 Sr 0.4 TiO 3 gated graphene

We report the effect of remote surface optical (RSO) phonon scattering on carrier mobility in monolayer graphene gated by ferroelectric oxide. We fabricate monolayer graphene transistors back-gated by epitaxial (001) Ba 0.6 Sr 0.4 TiO 3 films, with field effect mobility up to 23 000 cm 2 V –1 s –1 achieved. Switching ferroelectric polarization induces nonvolatile modulation of resistance and quantum Hall effect in graphene at low temperatures. Ellipsometry spectroscopy studies reveal four pairs of optical phonon modes in Ba 0.6 Sr 0.4 TiO 3 , from which we extract RSO phonon frequencies. The temperature dependence of resistivity in graphene can be well accounted for by considering the scattering from the intrinsic longitudinal acoustic phonon and the RSO phonon, with the latter dominated by the mode at 35.8 meV. Furthermore, our study reveals the room temperature mobility limit of ferroelectric-gated graphene transistors imposed by RSO phonon scattering.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Frequency combs in optically injected terahertz ring quantum cascade lasers

Quantum cascade lasers (QCLs) have emerged as promising candidates for generating chip-scale frequency combs in mid-infrared and terahertz wavelengths. In this work, we demonstrate frequency comb formation in ring terahertz QCLs using the injection of light from a distributed feedback (DFB) laser. The DFB design frequency is chosen to match the modes of the ring cavity (near 3.3 THz), and light from the DFB is injected into the ring QCL via a bus waveguide. By controlling the power and frequency of the optical injection, we show that combs can be selectively formed and controlled in the ring cavity. Numerical modeling suggests that this comb is primarily frequency-modulated in character, with the injection serving to trigger comb formation. We also show that the ring can be used as a filter to control the output of the DFB QCL, potentially being of interest in terahertz photonic integrated circuits. Our work demonstrates that waveguide couplers are a compelling approach for injecting and extracting radiation from ring terahertz combs and offer exciting possibilities for the generation of new comb states in terahertz, such as frequency-modulated waves, solitons, and more.

47 OTHER INSTRUMENTATION↗