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DOE OSTI2025

Impact of gasoline composition on the effects of nitric oxide on autoignition and knock in a DISI engine

Modern spark-ignition engines use exhaust gas recirculation (EGR) to dilute the charge and suppress knock, enabling the use of higher compression ratios and/or more optimum combustion phasing for higher efficiency. The effectiveness of EGR is affected by the composition of the fuel and its chemical-kinetic interactions with combustion products. Among those, nitric oxide (NO) has been shown to strongly affect autoignition reactivity. However, the impact of fuel composition of the effect of NO on reactivity is not well-understood. Here, in this study, engine experiments were conducted to assess the impact of NO seeded to the intake on knock-limited operation of two gasoline fuels (high cycloalkane content, or HCA, and high olefin content, or HO). Results showed that compositionally-different fuels responded differently to NO. HCA, which was less knock-limited than HO for NO < 200 ppm, became more knock-limited for NO > 200 ppm. Moreover, it was found that differences in knock between fuels were caused by differences in autoignition chemistry and not in the sequential autoignition process of the end gas that occurs due to thermal stratification. Chemical kinetic simulations were performed to better understand the experimental results. For HCA, intermediate-temperature heat release had a greater impact on autoignition reactivity than low-temperature heat release, while the opposite was observed for HO. For both fuels, NO enhances the magnitude of low-temperature heat release via NO + HO 2 → NO 2 + OH. The effect of NO on reactivity was stronger for HCA because OH produced from NO helped to overcome the OH quenching effect of cyclopentane, a main species in HCA. In contrast, HO had relatively strong inherent low-temperature chemistry arising from iso-octane, which reduced the impact of NO on reactivity. For the range of NO mole fractions tested in this study, in-cylinder NO increased fuel’s knock propensity, especially for fuels with mild low-temperature chemistry.

Autoignition↗

DOE OSTI2026

Effects of Gasoline Composition and Operating Parameters on the Response of End-Gas Autoignition to Nitric Oxide in a Lean-Burn DI-SI Engine

Lean operation of spark-ignition engines can lead to engine thermal efficiency gains and lower NOx emissions due to reduced combustion temperatures. Yet, lean operation could still face challenges in end-gas autoignition and knock generation due to higher intake pressures and trapped NO in the residual gas. Here, this study evaluates the impact of NO on end-gas autoignition for two gasoline fuels with similar octane rating but different composition: high cycloalkane fuel (HCA) and high olefin fuel (HO). Experiments were performed at stoichiometric and lean (λ = 2) conditions and at two engine speeds of 1400 rpm and 2000 rpm. Accompanying chemical kinetics simulations in CHEMKIN revealed that the mechanisms controlling the effect of NO on autoignition are similar λ = 2 and λ = 1, with NO + HO 2 = NO 2 + OH being the main pathway for enhancing reactivity by promoting low-temperature heat release (LTHR). The compositionally different fuels reacted differently to NO seeding and engine speed, and differences were augmented at λ = 2 compared to λ = 1 as the end-gas autoignition shifted to the low temperature regime. HO, which has inherent low temperature chemistry, was strongly impacted by engine speed at low NO seeding levels, with no noticeable peak of LTHR detected at 2000 rpm. On the other hand, LTHR of HCA was marginally affected by shortened residence time at higher engine speed as NO + HO 2 reaction was not greatly affected by shorter time scales, since HO 2 production was sustained even at 2000 rpm to support OH generation from NO + HO 2 . Contrary to HO, HCA exhibited greater sensitivity to NO seeding, as the increased OH production at higher NO concentrations offset the OH-quenching effect of cyclopentane, which accounts for 28.6% of HCA’s composition. Consequently, a sensitivity analysis revealed that fuels with weak inherent low-temperature chemistry, like HCA, are likely to be more sensitive to variations in NO concentration and charge temperature, whereas fuels with strong low temperature chemistry are more sensitive to variations in end-gas λ and intake pressure.

Energy↗

DOE OSTI2025

Magnetic Properties and Large Second-Harmonic Generation Response of a Chiral Ternary Chalcogenide: Eu 2 SiSe 4

Eu(II)-containing chalcogenides are an emerging class of materials that are of great interest due to their high optical activity and intriguing magnetism. Here, we synthesized Eu 2 SiSe 4 as red-colored single crystals and characterized its structure with single-crystal X-ray diffraction, confirming the reported chiral monoclinic P2 1 symmetry at room temperature. The crystal structure of Eu 2 SiSe 4 comprises distorted SiSe 4 tetrahedral units and charge-balancing Eu(II) cations. Here, we develop a two-step solid-state synthesis method for Eu 2 SiSe 4 and compare it to the known boron chalcogenide method. We find the second-harmonic generation (SHG) activity of polycrystalline Eu 2 SiSe 4 to be ∼7 × AgGaS 2 , placing it among the highest-known SHG-active chalcogenides. No symmetry lowering is observed down to 100 K in single-crystal X-ray diffraction, although an anomalous expansion in the b-axis lattice parameter occurs and may be correlated to lattice modes of the SiSe 4 tetrahedra. We investigate the physical properties of Eu 2 SiSe 4 using magnetometry and heat capacity measurements and find a transition to an antiferromagnetic ground state at T N ≈ 5.5 K. The low-temperature transition releases less entropy than expected, which may be due to the complex crystal electric field effects of Eu(II).

36 MATERIALS SCIENCE↗

NASA NTRS1994

Noble gases in presolar diamonds II: Component abundances reflect thermal processing

Using the isotopic compositions derived in Huss and Lewis, 1994a, abundances of the P3, HL, and P6 noble-gas components were determined for 15 diamonds separates from primitive chondrites of 8 chondrite classes. Within a meteorite class, the relative abundances of these components correlate with the petrologic subtype of the host meteorite, indicating that metamorphism is primarily responsible for the variations. Relative abundances of P3, HL, and P6 among diamond samples can be understood in terms of thermal processing of a single mixture of diamonds like those now found in CI and CM2 chondrites. With relatively gentle heating, primitive diamonds first lose their low-temperature P3 gases and a 'labile' fraction of the HL component. Mass loss associated with release of these components produces an increase in the HL and P6 content of the remaining diamond relative to unprocessed diamond. Higher temperatures initiate destruction of the main HL carrier, while the HL content of the surviving diamonds remains essentially constant. At the same time, the P6 carrier begins to preferentially lose light noble gases. Meteorites that have experienced metamorphic temperatures greater than or = 650 C have lost essentially all of their presolar diamond through chemical reactions with surrounding minerals. The P3 abundance seems to be a function only of the maximum temperature experienced by the diamonds and thus is independent of the nature of the surrounding environment. If all classes inherited the same mixture of primitive diamonds, then P3 abundances would tie together the metamorphic scales in different meteorite classes. However, if the P3 abundance indicates a higher temperature than do other thermometers applicable to the host meteorite, then the P3 abundance may contain information about heating prior to accretion. Diamonds in the least metamorphosed EH, CV, and CO chondrites seem to carry a record of pre-accretionary thermal processing.

Huss, Gary R.↗

NASA NTRSDate not supplied

Asymptotic Analysis of Premixed N-alkane Cool Flame Propagation

A simplified chemical-kinetic cool-flame mechanism for n-alkanes developed recently is applied to premixed laminar cool-flame deflagrations. The present contribution derives the structure of the associated freely propagating cool premixed flame controlled by the low-temperature chemistry and develops formulas for calculating the corresponding laminar burning velocity. Application of activation-energy asymptotics reveals finite-rate chemistry without heat release occurring throughout the preheat zone and leakage of both fuel and oxygen through the thin heat-release zone, there being zones of consumption of an intermediate species on each side of the heat-release zone, thicker than that zone but still thin compared with the preheat-zone thickness. Predicted laminar burning velocities are compared with recently reported measurements for n-dodecane, performed in a newly deigned high-pressure ignition apparatus, resulting in reasonable agreement.

Cool flames↗

NASA NTRSDate not supplied

Asymptotic Analysis of Premixed N-alkane Cool Flame Propagation

cool flames↗

DOE OSTI2026

Refined Sensitivity Estimates for Single-Molecule Magnet Dark Matter Detectors

We revisit the sensitivity of Single Molecule Magnet (SMM) crystals as detectors for low-mass dark matter. In previous work, we established the concept of the ``magnetic bubble chamber'', where energy deposited by dark matter triggers a magnetic avalanche in a metastable crystal. The original sensitivity estimates relied on a conservative criterion requiring the spin relaxation time to be strictly shorter than the thermal diffusion time. Here, we demonstrate that this criterion effectively ignores the stochastic nature of spin relaxation. We derive a refined analytic estimate which accounts for the fraction of spins that relax even when diffusion is fast. We show that the Zeeman energy released by this fraction contributes to local heating, significantly lowering the energy threshold for avalanche formation. We present simulation results confirming this effect and report on experimental verification of the assumed low-temperature thermal properties of two representative SMM crystals, Mn$_{12}$-acetate and Mn$_{32}$. Together, these efforts extend this pathfinder program toward the realization of SMM-based detectors with controlled material properties and enhanced dark matter sensitivity.

Eberhardt, Andrew [Tokyo U., IPMU]↗

NASA NTRS1992

Solar-type xenon - Isotopic abundances in Pesyanoe

Elemental and isotopic abundances of Ar and Xe were measured in three grain-size separates in the dark phase of the enstatite achondrite Pesyanoe by stepwise heating, using a combination of pyrolysis and combustion steps. The data reveal a low-temperature gas fraction with Ar/Xe ratios close to the solar ratio and isotopically similar to solar-type Ar and Xe observed in lunar samples. The gas released at intermediate temperature steps shows that Ar and Xe are isotopically fractionated, compared to the low-temperature components. Pesyanoe does not have excess Ar-40 and fission Xe, which means its parent body was too small for ion reimplantation. It is concluded that solar-type Xe isotopic abundances can be inferred from the low-temperature component. A comparison of Pesyanoe and lunar data shows that isotopic signatures of solar-wind Xe, as sampled at two different points in solar system space and time, are identical within experimental error.

Kim, J. S.↗

NASA NTRS2006

NASA Tech Briefs, November 2006

Topics include: Simulator for Testing Spacecraft Separation Devices; Apparatus for Hot Impact Testing of Material Specimens; Instrument for Aircraft-Icing and Cloud-Physics Measurements; Advances in Measurement of Skin Friction in Airflow; Improved Apparatus for Testing Monoball Bearings; High-Speed Laser Scanner Maps a Surface in Three Dimensions; Electro-Optical Imaging Fourier-Transform Spectrometer; Infrared Instrument for Detecting Hydrogen Fires; Modified Coaxial Probe Feeds for Layered Antennas; Detecting Negative Obstacles by Use of Radar; Cryogenic Pound Circuits for Cryogenic Sapphire Oscillators; PixelLearn; New Software for Predicting Charging of Spacecraft; Conversion Between Osculating and Mean Orbital Elements; Generating a 2D Representation of a Complex Data Structure; Making Activated Carbon by Wet Pressurized Pyrolysis; Composite Solid Electrolyte Containing Li+- Conducting Fibers; Electrically Conductive Anodized Aluminum Surfaces; Rapid-Chill Cryogenic Coaxial Direct-Acting Solenoid Valve; Variable-Tension-Cord Suspension/Vibration- Isolation System; Techniques for Connecting Superconducting Thin Films; Versatile Friction Stir Welding/Friction Plug Welding System; Thermal Spore Exposure Vessels; Enumerating Spore-Forming Bacteria Airborne with Particles; Miniature Oxidizer Ionizer for a Fuel Cell; Miniature Ion-Array Spectrometer; Promoted-Combustion Chamber with Induction Heating Coil; Miniature Ion-Mobility Spectrometer; Mixed-Salt/Ester Electrolytes for Low-Temperature Li+ Cells; Miniature Free-Space Electrostatic Ion Thrusters; Miniature Bipolar Electrostatic Ion Thruster; Holographic Plossl Retroreflectors; Miniature Electrostatic Ion Thruster With Magnet; Using Apex To Construct CPM-GOMS Models; Sequence Detection for PPM Optical Communication With ISI; Algorithm for Rapid Searching Among Star-Catalog Entries; Expectation-Based Control of Noise and Chaos; Radio Heating of Lunar Soil to Release Gases; Using Electrostriction to Manipulate Ullage in Microgravity; Equations for Scoring Rules When Data Are Missing; Insulating Material for Next-Generation Spacecraft; and Pseudorandom Switching for Adding Radar to the AFF Sensor.

Source record↗

NASA NTRS2013

A Mars Sample Return Sample Handling System

We present a sample handling system, a subsystem of the proposed Dragon landed Mars Sample Return (MSR) mission [1], that can return to Earth orbit a significant mass of frozen Mars samples potentially consisting of: rock cores, subsurface drilled rock and ice cuttings, pebble sized rocks, and soil scoops. The sample collection, storage, retrieval and packaging assumptions and concepts in this study are applicable for the NASA's MPPG MSR mission architecture options [2]. Our study assumes a predecessor rover mission collects samples for return to Earth to address questions on: past life, climate change, water history, age dating, understanding Mars interior evolution [3], and, human safety and in-situ resource utilization. Hence the rover will have "integrated priorities for rock sampling" [3] that cover collection of subaqueous or hydrothermal sediments, low-temperature fluidaltered rocks, unaltered igneous rocks, regolith and atmosphere samples. Samples could include: drilled rock cores, alluvial and fluvial deposits, subsurface ice and soils, clays, sulfates, salts including perchlorates, aeolian deposits, and concretions. Thus samples will have a broad range of bulk densities, and require for Earth based analysis where practical: in-situ characterization, management of degradation such as perchlorate deliquescence and volatile release, and contamination management. We propose to adopt a sample container with a set of cups each with a sample from a specific location. We considered two sample cups sizes: (1) a small cup sized for samples matching those submitted to in-situ characterization instruments, and, (2) a larger cup for 100 mm rock cores [4] and pebble sized rocks, thus providing diverse samples and optimizing the MSR sample mass payload fraction for a given payload volume. We minimize sample degradation by keeping them frozen in the MSR payload sample canister using Peltier chip cooling. The cups are sealed by interference fitted heat activated memory alloy caps [5] if the heating does not affect the sample, or by crimping caps similar to bottle capping. We prefer cap sealing surfaces be external to the cup rim to prevent sample dust inside the cups interfering with sealing, or, contamination of the sample by Teflon seal elements (if adopted). Finally the sample collection rover, or a Fetch rover, selects cups with best choice samples and loads them into a sample tray, before delivering it to the Earth Return Vehicle (ERV) in the MSR Dragon capsule as described in [1] (Fig 1). This ensures best use of the MSR payload mass allowance. A 3 meter long jointed robot arm is extended from the Dragon capsule's crew hatch, retrieves the sample tray and inserts it into the sample canister payload located on the ERV stage. The robot arm has capacity to obtain grab samples in the event of a rover failure. The sample canister has a robot arm capture casting to enable capture by crewed or robot spacecraft when it returns to Earth orbit

Wilson, David↗

DOE OSTI2025

Non-Equilibrium in a Dust-Forming Low-Temperature Plasma: A CARS Study

Dust-forming low-temperature plasmas are versatile systems for the production of nanoparticles with tunable functionalities. While attractive from a materials processing point of view, these systems are inherently complex, with several plasma-induced phenomena determining the properties of the produced materials. Here, we characterize a carbon nanoparticle-forming plasma using coherent anti-Stokes Raman spectroscopy (CARS), with the primary goal of measuring gas temperature. While gas temperature is typically assumed to be at or slightly above room temperature in these reactors, we measure gas temperatures exceeding 1000 K under typical process conditions. We find a correlation between the gas temperature and the nanoparticle yield, suggesting that the particle nucleation and growth process releases energy within the reaction volume, leading to significant gas heating. In addition, we find that the relaxation of vibrationally excited species at the particle surfaces is a major contributor to their heating. In conclusion, these results underscore the complexity of these systems and the need for their more in-depth characterization using advanced techniques such as CARS.

Basic Plasma Phenomena and Gas Discharges↗

DOE OSTI2025

Experimental and modeling study of the autoignition behavior of a saturated heterocycle: Pyrrolidine

Experiments are conducted in both rapid compression machine (RCM) and shock tube (ST) to better quantify autoignition behavior (e.g., ignition delay, heat release) and understand heteroatomic effects in heterocyclic compounds, which are important reference components for the combustion of biomass-derived liquid fuels. These tests focus on the nitrogen-containing, five-membered saturated ring, pyrrolidine, at diluted conditions covering pressures of 20 and 50 bar, temperatures of 720–1450 K and a range of stoichiometries (ϕ = 0.5–2). A chemical kinetic model is developed and coupled to an existing combustion kinetics framework describing key nitrogen containing intermediates (e.g. pyrrole, ammonia and NOx). H-abstraction reactions by OH, H, CH 3 and HO 2 , are determined using ab-initio transition state theory methods, while analogies to cyclopentane are adopted for many other reactions, such as ring-opening. Here, the autoignition measurements reveal the lack of negative temperature coefficient (NTC) behavior and low-temperature chemistry for pyrrolidine, as opposed to its saturated hydrocarbon analogue, cyclopentane. Interestingly, at the lowest temperatures (T < 750 K), the reactivity of cyclopentane is greater than pyrrolidine, while at higher temperatures, pyrrolidine becomes more reactive. Agreement between the experimental measurements and the model is good, and it is found that H-abstraction reactions by HO 2 and ensuing chemistry play key roles in controlling the reactivity of this cyclic amine. Most of the fluxes, i.e., >70 %, are predicted to move through 1- or 2-pyrroline (C 4 H 7 N) and then the cyclic C 4 H 6 N radical, at both lower and higher temperatures, to form either CH 2 CHCHCHNH via ring-opening or pyrrole via β-scission. It appears that the ring opens more easily at lower temperature whereas the C–H β-scission dominates at higher temperature and lower pressure, such that the reaction of the fuel radical intermediate carrying an unpaired electron on the nitrogen atom with HO 2 is the next most notable in promoting oxidation. When comparing pyrrolidine and cyclopentane, which exhibits distinct pathways in different temperature regimes, the pyrrolidine pathways and sensitivity analysis align more closely to the high temperature case of cyclopentane where the important role of HO 2 radicals is seen to provide chain branching through HO 2 reaction with the fuel, accompanied by H 2 O 2 formation and decomposition to OH. The formation of 5-membered diene rings and ring opening reactions are also found to be highly relevant. Of particular note, it is found that there is little influence of small molecule nitrogen-chemistry, e.g., NH 2 , HCN, NO/NO 2 on the reactivity of the pyrrolidine mixtures investigated here where no recirculated combustion gases are included.

Autoignition↗

DOE OSTI2026

Flame stabilization in DME spray flames under engine-relevant conditions characterized by OH* chemiluminescence and formaldehyde laser-induced fluorescence

The transient and quasi-steady flame structures of Dimethyl Ether (DME) fuel sprays, produced by a single-hole injector (Spray D), were investigated using Planar Laser-Induced Fluorescence (PLIF) and chemiluminescence imaging in a constant-volume chamber under Engine Combustion Network (ECN) Spray A conditions (900 K ambient temperature, 60 bar ambient pressure, 1500 bar injection pressure, and 22.8 kg/m 3 ambient density). Low-temperature chemical reaction zones were visualized using formaldehyde (CH 2 O) PLIF with 355 nm excitation, while high-temperature flame regions were captured via chemiluminescence imaging of excited-state hydroxyl radicals (OH*). Both transient and quasi-steady flame structures clearly show the transition from CH 2 O to OH*, highlighting the progression from low- to high-temperature combustion, while the position of the flame is displaced for DME compared to reference hydrocarbon n-dodecane. Homogeneous reactor calculations with detailed chemistry and using adiabatic mixing for initial temperature show that CH 2 O peaks are significantly higher for DME at the same equivalence ratio, with a higher heat-release during the cool-flame regime with respect to the fuel heating value. Thus, the cool-flame dynamic as a precursor to high-temperature combustion and flame stabilization exhibit distinct behavior for DME relative to conventional hydrocarbons, and these phenomena are effectively resolved through the soot-free nature of DME and the high-speed, time-resolved diagnostics.

CH2O laser-induced fluorescence↗

NASA NTRS1979

Regolith layering processes based on studies of low-temperature volatile elements in Apollo core samples

The concentrations of Hg released at at the most 130 C increase with depth in near-surface samples from cores. This is in response to a daytime thermal gradient with temperatures of approximately 400 K at the surface decreasing to approximately 250 K at greater than 10 cm depth (Keihm and Langseth, 1973). The steepness of the slopes and the depths to which the concentration gradients extend appear to be determined by the color, density and possibly the grain size of the soils. Earlier surface layers can be identified and, in general, are in agreement with other indicators of such layers. Low temperature volatilized Br exhibits trends that parallel those of Hg in a number of cases. This is also true of Br and Hg fractions released in stepwise heating experiments at higher temperatures. The coherence, especially in higher temperature fractions, between these chemically dissimilar elements implies a common physical process of entrapment; possibly one related to the presence of vapor deposits on surfaces and to opening and closing of microcracks and pores.

Jovanovic, S.↗

NASA NTRS1980

Carbynes in meteorites - Detection, low-temperature origin, and implications for interstellar molecules

The presence, origin and implications of carbynes in meteorites are investigated. A sample of the Allende meteorite was pyrolyzed at temperatures from 25 to 750 C and examined by solid probe time-of-flight mass spectrometry and high-resolution mass spectrometry. Fragments released upon heating at 250 to 330 C are found to be composed of macromolecules containing triply bonded carbon units and cyanoacetylenes, as well as some methyl- and phenylacetylenes. Although carbynes are well known to form from the condensation of carbon vapors above 2600 K or by shock greater than 600 kbar, which would be unlikely in Allende, it is found that carbynes rather than graphite are formed metastably by the disproportionation of CO at low temperatures when chromite is present as a catalyst. Results imply that metastable formation mechanisms may be the principal source of interstellar polycyanoacetylenes and meteoritic and terrestrial carbynes.

Hayatsu, R.↗

NASA NTRS1989

Iron-rich clay minerals on Mars - Potential sources or sinks for hydrogen and indicators of hydrogen loss over time

Although direct evidence is lacking, indirect evidence suggests that iron-rich clay minerals or poorly-ordered chemical equivalents are widespread on the Martian surface. Such clays can act as sources or sinks for hydrogen ('hydrogen sponges'). Ferrous clays can lose hydrogen and ferric clays gain it by the coupled substitution Fe(3+)O(Fe(2+)OH)-1, equivalent to minus atomic H. This 'oxy-clay' substitution involves only proton and electron migration through the crystal structure, and therefore occurs nondestructively and reversibly, at relatively low temperatures. The reversible, low-temperature nature of this reaction contrasts with the irreversible nature of destructive dehydroxylation (H2O loss) suffered by clays heated to high temperatures. In theory, metastable ferric oxy-clays formed by dehydrogenation of ferrous clays over geologic time could, if exposed to water vapor, extract the hydrogen from it, releasing oxygen.

Burt, D. M.↗

NASA NTRS2001

Beagle 2: The Next Exobiology Mission to Mars

Beagle 2 is a 60 kg probe (with a 30 kg lander) developed in the United Kingdom for inclusion on the European Space Agency's 2003 Mars Express. Beagle 2 will deliver to the Martian surface a payload which consists of a high percentage of science instruments to landed spacecraft mass. Beagle 2 will be launched in June, 2003 with Mars Express on a Soyuz-Fregat rocket from the Baikonur Cosmodrome in Kazakhstan. Beagle 2 will land on Mars on December 26, 2003 in the Isidis Planitia basin (approximately 10 degrees N and 275 degrees W), a large sedimentary basin that overlies the boundary between ancient highlands and northern plains. Isidis Planitia, the third largest basin on Mars, which is possibly filled with sediment deposited at the bottom of long-standing lakes or seas, offers an ideal environment for preserving traces of life. Beagle 2 was developed to search for organic material and other volatiles on and below the surface of Mars in addition to the study of the inorganic chemistry and mineralogy. Beagle 2 will utilize a mechanical mole and grinder to obtain samples from below the surface, under rocks and inside rocks. A pair of stereo cameras will image the landing site along with a microscope for examination of surface and rock samples. Analyses will include both rock and soil samples at various wavelengths, X-ray spectrometer and Mossbauer spectrometer as well as a search for organics and other light element species (e.g. carbonates and water) and measurement of their isotopic compositions. Beagle 2 has as its focus the goal of establishing whether evidence for life existed in the past on Mars at the Isidis Planitia site or at least establishing if the conditions were ever suitable. Carbonates and organic components were first recognized as existing on Mars when they were found in the Martian meteorite Nakhla. Romanek et al showed the carbonates in ALH84001 were formed at low temperatures. McKay et al noted possible evidence of early life on Mars within the ALH84001 meteorite. Thomas-Keprta et al showed the magnetite biomarkers in ALH84001's carbonates are indistinguishable from those formed by magnetotactic bacteria found on Earth. Gibson et al showed there was significant evidence for liquid water and biogenic products present on Mars across a 3.9 billion year period. A mechanical arm (PAW) operates from the lander and is used for science operations along with sample acquisition. Instruments attached to the PAW include: stereo cameras, Mossbauer instrument, X-ray fluorescence instrument, microscope, environmental sensors, rock corer/grinder, a spoon, mirror, brushes, a mole attachment for acquisition of subsurface to depths of 1 to 2 meters and an illumination device. Each camera has 14 filters which have been optimized for mineralogy composition, dust and water vapor detection. The microscope's camera is designed for viewing the size and shape of dust particles, rock surfaces, microfossils, and characteristics of the samples prior to introduction into the gas analysis package (GAP). The camera has a resolution of 4 microns/pixel, features four color capability (red, green, blue and UV (ultraviolet) fluoresence), a depth of focus of 40 micrometers and translation stage of +3 millimeters. The heart of the Beagle 2's life detection package is the gas analysis package (GAP), which consists of a mass spectrometer with collectors at fixed masses for precise isotopic ratio measurements and voltage scanning for spectral analysis. Primary aim of the GAP is to search for the presence of bulk constituents, individual species, and isotopic fractionations for both extinct and extent life along with studying the low-temperature geochemistry of the hydrogen, carbon, nitrogen and oxygen components on Mars from both the surface and atmosphere. GAP is a magnetic sector mass spectrometer with the range of 1 to 140 amu which can be operated in both the static and dynamic modes. A triple Faraday collector array will be used for C, N and O ratios along with a double Faraday array for H/D. Pulse counting electron multiplier will be utilized for noble gases and selected organics. Anticipated detection limits are at the picomole level for operation in the static mode of operation and high precision isotopic measurements will be made in the dynamic mode. Sample processing and preparation system consists of reaction vessels along with references. Sample ovens capable of being heated are attached to the manifold for sample combustion. Surface, subsurface materials and interior rock specimens will be combusted in pure oxygen gas at various temperature intervals to release organic matter and volatiles. Combustion process will permit detection of all forms and all atoms of carbon present in the samples. A chemical processing system is capable of a variety of conversion reactions. Gases are manipulated either by cryogenic or chemical reactions and passed through the gas handling portion of the vacuum system. There are two modes of operation: quantitative analysis and precise isotopic measurements. Additional information is contained in the original extended abstract.

Gibson, Everett K., Jr.↗

NASA NTRS2001

Thermal Desorption/GCMS Analysis of Astrobiologically Relevant Organic Materials

Several macromolecular organic materials, both biologically-derived (type II kerogen and humic acid) and abiotic in origin (Murchison insoluble organic material, cyanide polymer, and Titan tholin) were subjected to thermal desorption using a Chromatoprobe attachment on a Varian Saturn 2000 GCMS system. Each sample was heated sequentially at 100, 200, and 300 C to release volatile components. The evolved compounds were then separated on a Supelco EC-1 dimethylsilica GC column and detected by the Saturn 2000 ion trap mass spectrometer. The various types of macromolecular organic material subjected to thermal desorption produced distinctly different GCMS chromatograms at each temperature, containing fractions of both low and high chromatographic mobility. The relative amounts of detectable volatiles released at each temperature also differed, with type II kerogen and cyanide polymer containing the highest percentage of low-temperature components. In all the samples, the highest yield of released compounds occurred at 300 C. Only cyanide polymer evolved a homologous hydrocarbon series, suggesting that it is the only material among those examined that contains a truly polymeric structure. Pyrolysis/gas chromatography/mass spectrometry has been used extensively for analysis of terrestrial organic macromolecular materials, and was also part of the instrument package on the Viking landers. Thorough analysis by pyrolysis usually employs temperatures of 500 C or higher, which for in situ analyses can be problematic given spacecraft power and materials constraints. This study demonstrates that heating of organic materials of astrobiological relevance to temperatures as low as 200-300 C for short periods releases volatile components that can be analyzed by gas chromatography and mass spectrometry. Even in the absence of full pyrolysis, useful chemical information on samples can be obtained, and materials from different biological and abiological sources can be distinguished. The research described in this paper was carried out at the Jet Propulsion Laboratory, California Institute of Technology, under a contract with the National Aeronautics and Space Administration.

McDonald, Gene D.↗