A Comparison of the Optical Emission Spectra of Insulating Gases During Pulsed Discharge
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Physics - Plasma physics↗
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High-resolution spectroscopy of neutral Yb atoms in a solid Ne matrix
Here, we present an experimental and theoretical study of the absorption and emission spectra of Yb atoms in a solid Ne matrix at a resolution of 0.025 nm. Five absorption bands were identified as due to transitions from the 4 f 14 5 d 0 6 s 2 1 S 0 ground-state configuration to 4 f 14 5 d 0 6 s 6 p and 4 f 13 5 d 1 6 s 2 configurations. The two lowest-energy bands were assigned to outer-shell transitions to 6 s 6 p 3 P 1 and 1 P 1 atomic states and displayed the structure of a broad doublet and an asymmetric triplet, respectively. The remaining three higher-frequency bands were assigned to inner-shell transitions to distinct J = 1 states arising from the 4 f 13 5 d 1 6 s 2 configuration and were highly structured with narrow linewidths. A classical simulation was performed to identify the stability and symmetry of possible trapping sites in the Ne crystal. It showed that the overarching 1 + 2 structure of the high-frequency bands could be predominantly ascribed to crystal-field splitting in the axial field of a 10-atom vacancy of C 4 v symmetry. Their prominent substructures were shown to be manifestations of phonon sidebands associated with the zero-phonon lines on each crystal-field state. Unprecedented for a metal–rare-gas system, resolution of individual phonon states on an allowed electronic transition was possible under excitation spectroscopy which reflects the semiquantum nature of solid Ne. In contrast to the absorption spectra, emission spectra produced by steady-state excitation into the 1 P 1 absorption band consisted of simple, unstructured fluorescence bands.
74 ATOMIC AND MOLECULAR PHYSICS↗
Thermal emission from particulate surfaces: A comparison of scattering models with measured spectra
Emissivity spectra of particulate mineral samples are highly dependent on particle size when that size is comparable to the wavelength of light emitted (5-50 micrometers for the midinfrared). Proper geologic interpretation of data from planetary infrared spectrometers will require that these particle size effects be well understood. To address this issue, samples of quartz powders were produced with narrow, well-characterized particle size distributions. Mean particle diameters in these samples ranged from 15 to 227 micrometers. Emission spectra of these powders allow the first detailed comparison of the complex spectral variations with particle size observed in laboratory data with the predictions of radiative transfer models. Four such models are considered here. Hapke's relectance theory (converted to emissivity via Kirchoff's law) is the first model tested. Hapke's more recently published emission theory is also employed. The third model, the 'Mie/Conel' model, uses Mie single scattering with a two-stream approximation for multiple scattering. This model, like the first, is a converted reflec- tance model. Mie scattering assumes particles are both spherical and well separated, which is not true for the quartz powders, but includes diffraction effects. The fourth model uses the Mie solution for single scattering by spheres and inputs those results into the multiple scattering formalism of Hapke's emission theory. The results of the four models are considered in relation to the values of the optical constants n and k. We have grouped these as class 1 (k large), class 2 (k moderate, n is approximately 2), class 3 (k small, n is approximately 2), and class 4 (k small, n is approximately 1). In general, the Mie/Hapke hybrid model does best at predicting variations with grain size. In particular, it predicts changes of the correct pattern, although incorrect magnitude, for class 1 bands, where large increases in emissivity with decreasing grain size are observed. This model also does an excellent job on moderate (class 2) and very weak and intraband (class 3) regions, and correctly predicts the emission maximum and its invariance with grain size near the Christiansen frequency (class 4). The Mie/Hapke hybrid model also has the fewest free parameters of the four models examined, while maintaining the most physical treatment of the radiative transfer. The Mie/Conel model performs as well as the Mie/Hapke hybrid model in strong bands (class 1) but does not accurately model the behavior of moderate (class 2) and very weak (class 3) bands.
Moersch, J. E.↗
Peculiarities of spectra of induced emission of polymethine dye solutions at low temperatures
Results from studying the induced emission spectra with monochromatic excitation (superluminescent regime) within a temperature range of 300 K - 5.2 K are presented. The significant feature of such operations is the appearance of quasi-lines whose minimum width is realized at 4.2 K. The frequency distribution of the quasi-lines unambiguously characterizes the dye investigated. When interpreting these results, the idea of an inhomogeneous broadening of the polymethine dye spectra in the solution being studied experimentally was used for the first time. The quasi-lines observed are interpreted as a manifestation of the electron vibration structure of singlet states of a complex molecule.
Melishchuk, M. V.↗
Picosecond flash spectroscopic studies on ultraviolet stabilizers and stabilized polymers
Spectroscopic and excited state decay kinetics are reported for monomeric and polymeric forms of ultraviolet stabilizers in the 2-(2'-hydroxyphenyl)-benzotriazole and 2-hydroxybenzophenone classes. For some of these molecules in various solvents at room temperature, (1) ground state absorption spectra, (2) emission spectra, (3) picosecond time-resolved transient absorption spectra, (4) ground state absorption recovery kinetics, (5) emission kinetics, and (6) transient absorption kinetics are reported. In the solid state at low temperatures, emission spectra and their temperature dependent kinetics up to approximately 200K as well as, in one case, the 12K excitation spectra of the observed dual emission are also reported.
Scott, G. W.↗
Observations of silicate reststrahlen bands in lunar infrared spectra
Thermal emission spectra of three lunar sites (Apollo 11, Descartes Formation, and Tycho central peak) are measured in the 8-14 micron spectral range. Transmission and instrument effects are accounted for by forming ratios of the Descartes and Tycho spectra to the Apollo 11 spectrum. The ratio spectra are compared with ratios of published laboratory spectra of returned lunar samples and also with ratio spectra calculated using the Aronson-Emslie (1975) model. The comparisons show pyroxene bands in the Descartes ratio spectrum and plagioclase bands in the Tycho ratio spectrum. The Tycho spectrum is found to be consistent with the existence of fine plagioclase dust (approximately 1 micron) at the rock surface and a higher-than-usual sodium content of the plagioclase.
Potter, A. E., Jr.↗
Probing and Tuning Strain‐Localized Exciton Emission in 2D Material Bubbles at Room Temperature
In monolayer transition metal dichalcogenides bubbles-nanoscale deformations typically exhibiting a dome-like shape-Excitons are confined by the strain effect, which exhibits extraordinary emission properties, such as single photon generation, enhanced light emission, and spectrally tunable excitonic states. While the strain profiles of these bubbles are extensively studied, this work provides an approach 1) to directly visualize the associated exciton properties in bubbles formed in WSe2 monolayer, revealing an intrinsic emission wavelength shift of ≈40 nm, and 2) actively modify local strain, enabling further exciton emission tuning over a range of 50 nm. These are achieved by emission mapping and nanoindentation using a dielectric near-field probe, which enables the detection of local emission spectra and emission lifetimes within individual bubbles. Statistical analysis of 67 bubbles uncovers an emission wavelength distribution centered around 780 nm. Furthermore, saturation behavior in the power-dependent studies and the associated lifetime change reveal the localized nature of the strain-induced states. These findings provide direct insights into the strain-localized emission dynamics in bubbles and establish a robust framework for non-destructive, reversible, and predictable nanoscale emission control, presenting a potential avenue for developing next-generation tunable quantum optical sources.
2D materials bubbles↗
Covert MOF-Based Photoluminescent Tags via Tunable Linker Energetics
We report that the optical anticounterfeiting tags utilize the photoluminescent properties of materials to encode unique patterns, enabling identification and validation of important items and assets. These tags must combine optical complexity with ease of production and authentication to both prevent counterfeiting and to remain practical for widespread use. Metal–organic frameworks (MOFs) based on polynuclear, rare earth clusters are ideal materials platforms for this purpose, combining fine control over structure and composition, with tunable, complex energy transfer mechanisms via both linker and metal components. Here we report the design and synthesis of a set of heterometallic MOFs based on combinations of Eu, Nd, and Yb with the tetratopic linker 1,3,6,8-tetrakis(4-carboxyphenyl)pyrene. The energetics of this linker facilitate the intentional concealment of the visible emissions from Eu while retaining the infrared emissions of Nd and Yb, creating an optical tag with multiple covert elements. Unique to the materials system reported herein, we document the occurrence of a previously not observed 11-metal cluster correlated with the presence of Yb in the MOFs, coexisting with a commonly encountered 9-metal cluster. We demonstrate the utility of these materials as intricate optical tags with both rapid and in-depth screening techniques, utilizing orthogonal identifiers across composition, emission spectra, and emission decay dynamics. This work highlights the important effect of linker selection in controlling the resulting photoluminescent properties in MOFs and opens an avenue for the targeted design of highly complex, multifunctional optical tags.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Two micron laser development for atmospheric remote sensing at NASA Langley Research Center
The topics addressed are: (1) eye safety revision of infrared MPE; (2) Tm:Ho dynamics characterization, which includes spectroscopy, laser experiments, and modeling; and (3) Q.M. model calculation, which includes energy levels, electric and magnetic dipole transition probabilities, lifetimes, branching ratios, absorption spectra, and emission spectra; (3) Q.M. model calculation; and (4) heat propagation in a laser rod.
Brockman, Philip↗
Spherulitic Growth of Hematite Under Hydrothermal Conditions: Insights into the Growth Mechanism of Hematite Spherules at Meridiani Planum Mars.
Hematite-rich spherules were discovered embedded in sulfate-rich outcrop rock and as lag deposits of whole and broken spherules by the Opportunity rover at Meridiani Planem [1-6]. The Mars Global Surveyor (MGS) Thermal Emission Spectrometer (TES), which has a wider spectral range compared to the Mars Exploration Rover Mini-TES, provided an important constraint that hematite-rich spherules are dominated by emission along the crystallographic c-axis [7-10]. We have previously synthesized hematite spherules whose mineralogic, chemical, and crystallographic properties are strikingly similar to those for the hematite-rich spherules at Meridiani Planum [11]. The spherules were synthesized in the laboratory along with hydronium jarosite and minor hydronium alunite from Fe-Al-Mg-S-Cl acid sulfate solutions under hydrothermal conditions. The reaction sequence was (1) precipitation of hydronium jarosite, (2) jarosite dissolution and precipitation of hematite spherules, and (3) precipitation of hydronium alunite upon depletion of hydronium jarosite. The spherules exhibit a radial growth texture with the crystallographic c-axis aligned along the radial direction, so that thermal emission spectra have no hematite emissivity minimum at approx.390/cm similar to the emission spectra returned by MGS TES. The objective of this paper is to expand on our initial studies [11] to examine the morphological evolution during growth of spherules starting from sub-micrometer crystals to spherules many orders of magnitude in size.
Ming, Douglas W.↗
TPSAS-NF1676L-10761-DND
The presentation summarizes the NASA CLARREO mission to observe decadal climate change using high accuracy SI traceable reflected solar spectra, infrared emission spectra, and radio occultation from the Earth.
Bruce A Wielicki↗
Theory of molecular emission power spectra. I. Macroscopic quantum electrodynamics formalism
In this work, we study the emission power spectrum of a molecular emitter with multiple vibrational modes in the framework of macroscopic quantum electrodynamics. The theory we present is general for a molecular spontaneous emission spectrum in the presence of arbitrary inhomogeneous, dispersive, and absorbing media. Moreover, the theory shows that the molecular emission power spectra can be decomposed into the electromagnetic environment factor and lineshape function. In order to demonstrate the validity of the theory, we investigate the lineshape function in two limits. In the incoherent limit (single molecules in a vacuum), the lineshape function exactly corresponds to the Franck–Condon principle. In the coherent limit (single molecules strongly coupled with single polaritons or photons) together with the condition of high vibrational frequency, the lineshape function exhibits a Rabi splitting, the spacing of which is exactly the same as the magnitude of exciton–photon coupling estimated by our previous theory [S. Wang et al., J. Chem. Phys. 151, 014105 (2019)]. Finally, we explore the influence of exciton–photon and electron–phonon interactions on the lineshape function of a single molecule in a cavity. The theory shows that the vibronic structure of the lineshape function does not always disappear as the exciton–photon coupling increases, and it is related to the loss of a dielectric environment.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Emission-line spectra of two active regions on the solar limb - 1175-1940 A
Skylab emission-line spectra (1175 to 1940 A) of two active regions on the solar limb are examined. Electron densities for the active regions are derived using the intensity ratios of selected intersystem and allowed lines. The intensity ratios in the active regions are compared with those observed previously in quiet-sun and coronal-hole regions. The behavior of coronal forbidden lines relative to transition-zone lines is discussed along with the solar continuum intensities near and above the limb. These continuum intensities are then compared with those at similar slit positions for the quiet sun and the previously studied coronal hole. The active-region data are found to be consistent with either (1) multithermal loops with the high-temperature plasma occupying the tops of the loops or (2) nearly isothermal loops with the hotter loops extending to higher altitudes.
Feldman, U.↗
Outer atmospheres of cool stars. XII - A survey of IUE ultraviolet emission line spectra of cool dwarf stars
Quantitative information is obtained on the chromospheres and transition regions of M dwarf stars, in order to determine how the outer atmospheres of dMe stars differ from dM stars and how they compare with the outer atmospheres of quiet and active G and K type dwarfs. IUE spectra of six dMe and four dM stars, together with ground-based photometry and spectroscopy of the Balmer and Ca II H and K lines, show no evidence of flares. It is concluded, regarding the quiescent behavior of these stars, that emission-line spectra resemble that of the sun and contain emission lines formed in regions with 4000-20,000 K temperatures that are presumably analogous to the solar chromosphere, as well as regions with temperatures of 20,000-200,000 K that are presumably analogous to the solar transition region. Emission-line surface fluxes are proportional to the emission measure over the range of temperatures at which the lines are formed.
Linsky, J. L.↗
Single photon infrared emission spectroscopy: a study of IR emission from UV laser excited PAHs between 3 and 15 micrometers
Single-photon infrared emission spectroscopy (SPIRES) has been used to measure emission spectra from polycyclic aromatic hydrocarbons (PAHs). A supersonic free-jet expansion has been used to provide emission spectra of rotationally cold and vibrationally excited naphthalene and benzene. Under these conditions, the observed width of the 3.3-micrometers (C-H stretch) band resembles the bandwidths observed in experiments in which emission is observed from naphthalene with higher rotational energy. To obtain complete coverage of IR wavelengths relevant to the unidentified infrared bands (UIRs), UV laser-induced desorption was used to generate gas-phase highly excited PAHs. Lorentzian band shapes were convoluted with the monochromator-slit function in order to determine the widths of PAH emission bands under astrophysically relevant conditions. Bandwidths were also extracted from bands consisting of multiple normal modes blended together. These parameters are grouped according to the functional groups mostly involved in the vibration, and mean bandwidths are obtained. These bandwidths are larger than the widths of the corresponding UIR bands. However, when the comparison is limited to the largest PAHs studied, the bandwidths are slightly smaller than the corresponding UIR bands. These parameters can be used to model emission spectra from PAH cations and cations of larger PAHs, which are better candidate carriers of the UIRs.
Non-NASA Center↗
Design of Hypervelocity Flow Generator (HFG) and Its Diagnostics
Ground facilities for hypersonic research are a key element for successful development of aerodynamically proven hypervelocity vehicles. Design concepts and diagnostics of a hypervelocity flow generator (HFG) were made as a test platform for hypersonic/hypervelocity spacecraft models at the NASA Langley Research Center. The HFG is a hypersonic flow field generator using optically heated gas which is blown into an 80 cu m vacuum chamber. The vacuum chamber is kept at a stable vacuum pressure with a combination of three large vacuum pumps, while the HFG is in the test mode. The HFG provides a relatively small test section with approximately a 20 cm window. This facility was designed to generate 2.45 km/sec of flow speed, and potentially generate a continuous flow with the nozzle and vacuum system. The window in test section provides a direct view of the shock wave around a model in order to measure temperature, pressure, and density profile within the shock layer. One of the key test goals under this project is to understand why the emission spectra from the standing shockwave plasma predicted by Lora-Loran codes are significantly different from the measured emission spectra from the Flight Investigation Reentry Environment (FIRE II) Flight. The correct estimate of the thermal loading on the leading edge of hypersonic vehicles greatly affects the aerodynamic design, the material selection for the vehicle, and the cooling requirement and can be obtained by the precise modeling of emission spectra from shockwave plasma. However, the estimation of thermal loading is not an easy task due to complex non-equilibrium radiative process within high temperature shock layers that still falls into a category of cold plasma. Direct flight experiments are the most desirable, but not a cost-effective approach. Analysis by computational fluid dynamics (CFD) offers many test flexibilities. However, the CFD codes must be fully tested and validated with experimental data before the codes are effectively used for practical design. Large discrepancies between experiments and codes appear in hypersonic/hypervelocity flow regimes at high altitudes of 60 km ~ 90 km. This HFG facility offers some important parameters for CFD code validation, such as collision cross-sections, relaxation times, reaction rate coefficients and transportation coefficients. The HFG test facility is based on the ejection flow of high temperature gas heated over to 3500 K through a nozzle. The tungsten gas chamber of the HFG is heated up to a desired temperature by a 60 kW optical power beam source. This system consists of an optical power source, a thermal chamber, an expansion nozzle, a test section, and an 80 cu m vacuum tank. 60 kW optical input power is obtained from the 150 kW Vortek arc lamp system (by Vortek Industries, Vancouver, Canada). This optical beam is focused to heat the gas chamber within which a flow media is heated. The maximum achievable temperature of the flow medium reached approximately 3500 K or even higher but is limited by the melting point of the chamber material used. The exhaust velocity through the nozzle was determined by the stagnation temperature and the molecular weight of the working medium at the test section. To provide design parameters, a NASA Chemical Equilibrium with Application (CEA) computer program is used for the simulation of aerothermal data. This CEA program can calculate chemical equilibrium and properties of complex mixtures using shock tube parameters. For nitrogen gas at 2666 K stagnation temperature, the maximum achievable velocity at the test section is approximately 2.45 km/sec which is within the range of the thermal velocity of 8000 K shock layer. Based on the calculation through the CEA program, the design parameters of a HFG were determined and implemented for the test section that includes an expansion nozzle. The installed test section of the experimental facility can sustain a condition of a re-entry vehicle from the Space at an altitude of 60-90 km. After installation of the HFG, the system was fully tested and its operational parameters were measured. An 80 cu m vacuum chamber of HFG was set at 1 torr level to keep a stable downstream condition. The pumping time to reach the minimum vacuum pressure (~ 1 torr) at the test chamber from atmospheric pressure was approximately an hour using Kinney (MBV-14000/MB -1600/KT-300) and Stokes (Model 1772 and 412) pumps. Such a setup condition allowed a continued stable operation of the HFG experiment with flowrates through 1-, 3-, or 5-mm diameters of nozzle throat. The flow characteristics of the HFG for various operating conditions were performed using a focused Schlieren method. At 0.8 torr chamber pressure, a barrel shock was observed at the test section. With a sphere obstacle of 12 mm diameter in the flow, a bow shock (~ 2-mm thickness) was observed by a focused Schlieren visualization method.
Hypervelocity flow↗
Design and use of a servo-controlled high pressure window bomb in spectroscopic studies of solid propellant combustion
The feasibility of using a high pressure window bomb as a laboratory scale model of actual motor conditions. The design and operation of a modified high pressure window bomb is discussed. An optical servocontrol mechanism has been designed to hold the burning surface of a propellant strand at a fixed position within the bomb chamber. This mechanism permits the recording of visible and infrared emission spectra from various propellants. Preliminary visible emission spectra of a nonmetalized and metalized propellant are compared with spectra recorded using the modified bomb.
Goetz, F.↗
Time resolved spectra in the infrared absorption and emission from shock heated hydrocarbons
The wavelength range of a previously constructed multichannel fast recording spectrometer was extended to the mid-infrared. With the initial configuration, light intensities were recorded simultaneously with a silicon-diode array simultaneously at 20 adjacent wavelengths, each with a 20-micron time resolution. For studies in the infrared, the silicon diodes were replaced by a 20-element PbSe array of similar dimensions, cooled by a three-stage thermoelectric device. It is proposed that infrared emissions could be due to shock-heated low molecular-weight hydrocarbons. The full Swan band system appeared in time-integrated emission spectra from shock-heated C2H2; no soot was generated. At low resolution, the profiles on the high-frequency side of the black body maximum show no distinctive features. These could be fitted to Planck curves, with temperatures that declined with time from an initial high that was intermediate between T5 (no conversion) and T5(eq).
Bauer, S. H.↗