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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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11 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

A straightforward method for Vacuum-Ultraviolet flux measurements: The case of the hydrogen discharge lamp and implications for solid-phase actinometry

Vacuum-Ultraviolet (VUV) radiation is responsible for the photo-processing of simple and complex molecules in several terrestrial and extraterrestrial environments. In the laboratory such radiation is commonly simulated by inexpensive and easy-to-use microwave-powered hydrogen discharge lamps. However, VUV flux measurements are not trivial and the methods/devices typically used for this purpose, mainly actinometry and calibrated VUV silicon photodiodes, are not very accurate or expensive and lack of general suitability to experimental setups. Here, we present a straightforward method for measuring the VUV photon flux based on the photoelectric effect and using a gold photodetector. This method is easily applicable to most experimental setups, bypasses the major problems of the other methods, and provides reliable flux measurements. As a case study, the method is applied to a microwave-powered hydrogen discharge lamp. In addition, the comparison of these flux measurements to those obtained by O{sub 2} actinometry experiments allow us to estimate the quantum yield (QY) values QY{sub 122} = 0.44 ± 0.16 and QY{sub 160} = 0.87 ± 0.30 for solid-phase O{sub 2} actinometry.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Energy resolved actinometry for simultaneous measurement of atomic oxygen densities and local mean electron energies in radio-frequency driven plasmas

A diagnostic method for the simultaneous determination of atomic oxygen densities and mean electron energies is demonstrated for an atmospheric pressure radio-frequency plasma jet. The proposed method is based on phase resolved optical emission measurements of the direct and dissociative electron-impact excitation dynamics of three distinct emission lines, namely, Ar 750.4 nm, O 777.4 nm, and O 844.6 nm. The energy dependence of these lines serves as basis for analysis by taking into account two line ratios. In this frame, the method is highly adaptable with regard to pressure and gas composition. Results are benchmarked against independent numerical simulations and two-photon absorption laser-induced fluorescence experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Optical emission spectroscopic studies and comparisons of CH{sub 3}F/CO{sub 2} and CH{sub 3}F/O{sub 2} inductively coupled plasmas

A CH{sub 3}F/CO{sub 2} inductively coupled plasma (ICP), sustained in a compact plasma reactor, was investigated as a function of power (5–400 W) and feed gas composition, at a pressure of 10 mTorr, using optical emission spectroscopy and rare gas actinometry. Number densities of H, F, and O increased rapidly between 74% and 80% CO{sub 2}, ascribed to the transition from polymer-covered to polymer-free reactor walls, similar to that found previously in CH{sub 3}F/O{sub 2} ICPs at 48% O{sub 2}. Below 40% O{sub 2} or CO{sub 2}, relative emission intensity ratios were almost identical for most key species in CH{sub 3}F/O{sub 2} and CH{sub 3}F/CO{sub 2} ICPs except for higher OH/Xe (a qualitative measure of OH and H{sub 2}O densities) over the full range of CH{sub 3}F/O{sub 2} composition. The number density of H, F, and O increased with power in CH{sub 3}F/CO{sub 2} (20%/80%) plasmas (polymer-free walls), reaching 4.0, 0.34, and 1.6 × 10{sup 13}/cm{sup 3}, respectively, at 300 W. The CO number density increased with power and was estimated, based on self-actinometry, to be 8.8 × 10{sup 13}/cm{sup 3} at 300 W. The CO{sub 2} number density was independent of power below 40 W (where very little decomposition occurred), and then decreased rapidly with increasing power, reaching 2.8 × 10{sup 13}/cm{sup 3} at 300 W, corresponding to 83% dissociation. Films deposited on p-Si, 10 cm from the open, downstream end of the plasma reactor, were analyzed by x-ray photoelectron spectroscopy. Between 10% and 40% CO{sub 2} or O{sub 2} addition to CH{sub 3}F, film deposition rates fell and O content in the films increased. Faster deposition rates in CH{sub 3}F/CO{sub 2} plasmas were ascribed mainly to a larger thermodynamic driving force to form solid carbon, compared with CH{sub 3}F/O{sub 2} plasmas. Oxygen content in the films increased with increasing CO{sub 2} or O{sub 2} addition, but for the same deposition rate, no substantial differences were observed in the composition of the films.

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

Kinetic studies of excited singlet oxygen atom O( 1 D) reactions with ethanol

In this work, themultichannel reaction of excited singlet oxygen atom with ethanol, O( 1 D) + C 2 H 5 OH (1), was studied in a photolysis flow reactor coupled with mid-infrared Faraday rotation spectroscopy (FRS) and UV-IR direct absorption spectroscopy (DAS) at 297 K with reactor pressures of 60, 120, and 150 Torr (bath He). The excited singlet oxygen atom was generated through the photolysis of O 3 at 266 nm. The photon flux and O( 1 D) concentrations were determined by in situ actinometry based on O 3 depletion. Temporal profiles of OH and H 2 O were monitored via DAS signals at ca. 3568.62 and 3568.29 cm –1 , while temporal profiles of HO 2 were measured via FRS signals at ca. 1396.90 cm –1 . The branching ratios of the target reaction (1) were determined by fitting temporal profiles to simulations from an in-house reaction mechanism. Two major reaction channels were identified as CH 3 CHOH + OH and CH 3 O + CH 2 OH, and their branching ratios were determined as 0.46 ± 0.12 and 0.42 ± 0.11, respectively. A specific HO 2 + RO 2 reaction between HO 2 and O 2 CH 2 CH 2 OH (β-RO 2 ) at the low-temperature range is estimated in this work as HO 2 + O 2 CH 2 CH 2 OH → products with a rate constant of 7 × 10 –12 cm 3 molecule –1 s –1 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Spectroscopic analysis of H{sub 2}/CH{sub 4} microwave plasma and fast growth rate of diamond single crystal

One of the best ways to increase the diamond growth rate is to couple high microwave power to the plasma. Indeed, increasing the power density leads to increase gas temperature the atomic hydrogen density in the plasma bulk, and to produce more hydrogen and methyl at the diamond surface. Experimental and numerical approaches were used to study the microwave plasma under high power densities conditions. Gas temperature was measured by optical emission spectroscopy and H-atom density using actinometry. CH{sub 3}-radical density was obtained using a 1D model that describes temperatures and plasma composition from the substrate to the top of the reactor. The results show that gas temperature in the plasma bulk, atomic hydrogen, and methyl densities at the diamond surface highly increase with the power density. As a consequence, measurements have shown that diamond growth rate also increases. At very high power density, we measured a growth rate of 40 μm/h with an H-atom density of 5 × 10{sup 17} cm{sup −3} which corresponds to a H{sub 2} dissociation rate higher than 50%. Finally, we have shown that the growth rate can be framed between a lower and an upper limit as a function depending only on the maximum of H-atom density measured or calculated in the plasma bulk. The results also demonstrated that increasing fresh CH{sub 4} by an appropriate injection into the boundary layer is a potential way to increase the diamond growth rates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Surface loss probability of atomic hydrogen for different electrode cover materials investigated in H₂-Ar low-pressure plasmas

In an inductively coupled H₂-Ar plasma at a total pressure of 1.5 Pa, the influence of the electrode cover material on selected line intensities of H, H₂, and Ar are determined by optical emission spectroscopy and actinometry for the electrode cover materials stainless steel, copper, tungsten, Macor{sup ®}, and aluminum. Hydrogen dissociation degrees for the considered conditions are determined experimentally from the measured emission intensity ratios. The surface loss probability β{sub H} of atomic hydrogen is correlated with the measured line intensities, and β{sub H} values are determined for the considered materials. Without the knowledge of the atomic hydrogen temperature, β{sub H} cannot be determined exactly. However, ratios of β{sub H} values for different surface materials are in first order approximation independent of the atomic hydrogen temperature. Our results show that β{sub H} of copper is equal to the value of stainless steel, β{sub H} of Macor{sup ®} and tungsten is about 2 times smaller and β{sub H} of aluminum about 5 times smaller compared with stainless steel. The latter ratio is in reasonable agreement with literature. The influence of the atomic hydrogen temperature T{sub H} on the absolute value is thoroughly discussed. For our assumption of T{sub H}=600 K, we determine a β{sub H} for stainless steel of 0.39±0.13.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Measurement of neutral gas temperature in a 13.56 MHz inductively coupled plasma

Measuring the temperature of neutrals in inductively coupled plasmas (ICP) is important as heating of neutral particles will influence plasma characteristics such as the spatial distributions of plasma density and electron temperature. Neutral gas temperatures were deduced using a non-invasive technique that combines gas actinometry, optical emission spectroscopy and simulation which is described here. Argon gas temperature in a 13.56 MHz ICP were found to fall within the range of 500 − 800 K for input power of 140 − 200 W and pressure of 0.05 − 0.2 mbar. Comparing spectrometers with 0.2 nm and 0.5 nm resolution, improved fitting sensitivity was observed for the 0.2 nm resolution.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
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 OSTI2015

Determination of the number density of excited and ground Zn atoms during rf magnetron sputtering of ZnO target

A combination of optical absorption spectroscopy (OAS) and optical emission spectroscopy measurements was used to monitor the number density of Zn atoms in excited 4s4p ({sup 3}P{sub 2} and {sup 3}P{sub 0}) metastable states as well as in ground 4s{sup 2} ({sup 1}S{sub 0}) state in a 5 mTorr Ar radio-frequency (RF) magnetron sputtering plasma used for the deposition of ZnO-based thin films. OAS measurements revealed an increase by about one order of magnitude of Zn {sup 3}P{sub 2} and {sup 3}P{sub 0} metastable atoms by varying the self-bias voltage on the ZnO target from −115 to −300 V. Over the whole range of experimental conditions investigated, the triplet-to-singlet metastable density ratio was 5 ± 1, which matches the statistical weight ratio of these states in Boltzmann equilibrium. Construction of a Boltzmann plot using all Zn I emission lines in the 200–500 nm revealed a constant excitation temperature of 0.33 ± 0.04 eV. In combination with measured populations of Zn {sup 3}P{sub 2} and {sup 3}P{sub 0} metastable atoms, this temperature was used to extrapolate the absolute number density of ground state Zn atoms. The results were found to be in excellent agreement with those obtained previously by actinometry on Zn atoms using Ar as the actinometer gas [L. Maaloul and L. Stafford, J. Vac. Sci. Technol., A 31, 061306 (2013)]. This set of data was then correlated to spectroscopic ellipsometry measurements of the deposition rate of Zn atoms on a Si substrate positioned at 12 cm away from the ZnO target. The deposition rate scaled linearly with the number density of Zn atoms. In sharp contrast with previous studies on RF magnetron sputtering of Cu targets, these findings indicate that metastable atoms play a negligible role on the plasma deposition dynamics of Zn-based coatings.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗