Microscopic organic analysis using two-step laser mass spectrometry:  application to meteoritic acid residues

Kovalenko, L. J.; Maechling, C. R.; Clemett, S. J.; Philippoz, J. M.; Zare, Richard N.; Alexander, Conel M. O'd.

doi:10.1021/ac00030a021

Cited by 96 publications

(57 citation statements)

References 33 publications

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“…The development of this device has also benefited greatly from the contributions of several postdoctoral research associates including F. Engelke, J.-M. Phillipoz, L. J. Kovalenko, and X. D. F. Chillier. The detailed applications of this instrument to the study of meteoritic samples may be found elsewhere Zenobi et al 1989Zenobi et al , 1992Kovalenko et al 1991Kovalenko et al , 1992Zenobi h Zare, 1991;Clemett et al 1993;Thomas et al 1995a;Maechling et al 1995;McKay et al 1996). In what follows we emphasize the capabilities of this analytic tool and its present limitations.…”

mentioning

confidence: 91%

Microprobe two-step laser mass spectrometry as an analytical tool for meteoritic samples

Clemett

Zare

1997

Symp. - Int. Astron. Union

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Abstract. Microprobe two-step laser mass spectrometry (/iL 2 MS) is a new mass spectrometric method in which the two essential steps of any mass spectrometric analysis, vaporization and ionization, are carried out using two independent laser sources. In the first step, the output of a pulsed infrared laser is focused on the sample to cause rapid heating in the spot area illuminated, which is typically 40 /zm by 40 /im. In the second step, the output of a pulsed ultraviolet laser causes (1+1) resonance-enhanced multiphoton ionization (REMPI) of those desorbed neutral molecules that (1) are able to absorb this UV wavelength and (2) whose ionization potential is less than the energy of two photons of this UV wavelength. The resulting ions are then mass analyzed in a reflectron time-of-flight apparatus. Under suitable conditions fragmentation can be avoided in both the vaporization and ionization steps so that μΙι 2 Μ8 can be applied to the analysis of a mixture of molecules. Applications of ^L 2 MS to meteorite samples are presented as a means of detecting trace amounts of certain organic molecules present in complex materials without prior sample preparation, extraction, purification, and separation steps. Moreover, this analysis can be carried out with micrometer spatial resolution so that in favorable cases the presence or absence of certain molecules can be correlated to mineralogical features of the sample.

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confidence: 91%

Microprobe two-step laser mass spectrometry as an analytical tool for meteoritic samples

Clemett

Zare

1997

Symp. - Int. Astron. Union

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“…In one research project, two such particles exhibited broad PAH envelopes (29), as well as other signatures (28,30,31), which confirmed their identification as IDPs. PAHs were found to cluster in three mass envelopes (with peaks at 60, 250, and 370 amu) and exhibited more extensive alkylation and nitrogen addition (i.e., -NH 2 , -CN, or -NC) than those observed in carbonaceous chondrites (14,19,20). Relative to carbonaceous chondrites, a strikingly low abundance of PAHs Ͻ192 amu was found.…”

Section: Interplanetary Dust Particles (Idps)mentioning

confidence: 93%

“…The degree of PAH alkylation [PAH-(CH 2 ) n ], in particular, was characterized in carbonaceous chondrites (15,19,20) and Antarctic micrometeorites (AMMs) (21), which represent a range of thermal and aqueous alteration histories. Increasing PAH alkylation was found to associate with increasing aqueous exposure of carbonaceous chondrite parent bodies (19).…”

Section: Review Of L 2 Ms For the Study Of Extraterrestrial Materialsmentioning

confidence: 99%

Laser mass spectrometric detection of extraterrestrial aromatic molecules: Mini-review and examination of pulsed heating effects

Spencer

Hammond

Zare

2008

Proc. Natl. Acad. Sci. U.S.A.

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Laser mass spectrometry is a powerful tool for the sensitive, selective, and spatially resolved analysis of organic compounds in extraterrestrial materials. Using microprobe two-step laser mass spectrometry ( L 2 MS), we have explored the organic composition of many different exogenous materials, including meteorites, interplanetary dust particles, and interstellar ice analogs, gaining significant insight into the nature of extraterrestrial materials. Recently, we applied L 2 MS to analyze the effect of heating caused by hypervelocity particle capture in aerogel, which was used on the NASA Stardust Mission to capture comet particles. We show that this material exhibits complex organic molecules upon sudden heating. Similar pulsed heating of carbonaceous materials is shown to produce an artifactual fullerene signal. We review the use of L 2 MS to investigate extraterrestrial materials, and we discuss its recent application to characterize the effect of pulsed heating on samples of interest. (not from Earth), including meteorites, interplanetary dust particles (IDPs), and cometary coma dust, is a fascinating endeavor, and its pursuit can significantly increase our knowledge of planetary formation and interstellar chemistry. Several factors make this task challenging, including sample acquisition in a manner that does not alter compounds and analysis of micrometer-scale samples. Mass spectrometry (MS) offers one means of meeting these criteria. In the past, MS instruments have flown on missions to outer space and the surrounding planets. Notably, the NASA Viking Landers, which touched down on Mars in 1976, used gas chromatography followed by MS to gain the first analysis of the Martian atmosphere (1). MS investigations in space have enabled the understanding that planets exchange material and, in particular, that Earth has received meteorites from the moon and Mars. Much information about our surroundings has been gained by the MS analysis of extraterrestrial materials.Laser MS techniques have particular utility when analyzing low concentrations of organic compounds on complex surfaces and particulates, which are often encountered with extraterrestrial materials. In general, these techniques are able to perform spatially resolved, micrometer-scale surface analyses and have achieved sensitivities in the subattomole regime (2). Most commercial laser MS instrumentation uses one laser pulse, to both thermally desorb surface material and ionize resulting gaseous compounds. A matrix is often added to the sample to facilitate desorption, such as in matrix-assisted laser desorption/ionization (MALDI) (3, 4). Less widespread, because of an increased complexity and specificity, are laser MS techniques that use two lasers, one for sample desorption and one for ionization (2). This two-step laser MS can be used to selectively detect specific organic compound classes with high sensitivity and does not require matrix addition. Only femtograms of surface material are removed during desorption, minimally altering the sample and pe...

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“…Of course, PAHs have also been analyzed in carbonaceous chondrites (Pering and Ponnamperuma, 1971;Clemett et al, 1992;Kovalenko et al, 1992). However, the rapid contamination of newly fallen meteorite material (e.g., the Allende fall in 1968) by terrestrial organic compounds (Han et al, 1969) suggests caution in interpreting results, and requires rigorous background control and blank analyses.…”

Section: Nonbiomarkersmentioning

confidence: 99%

Molecular indicators (biomarkers) of past life

Simoneit

2002

Anat. Rec.

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Biomarkers in geological samples on Earth are products derived from biochemical precursors (i.e., natural products) by reductive and oxidative alteration processes (e.g., cholestanes from cholesterol). Generally, lipids, pigments, and some biomembranes are preserved best over longer geological times, and labile compounds such as amino acids, sugars, etc. are useful biomarkers for recent times. Thus, the detailed characterization of biomarker composition permits the assessment of the major contributing species of extinct and/or extant life. Nonbiomarkers and abiogenic organic compounds are also discussed. In the case of the early Earth, work has progressed to elucidate biomarker structures and carbon isotopic signals preserved in ancient sedimentary rocks. In addition, the combination of bacterial biochemistry with the organic geochemistry of contemporary and ancient hydrothermal ecosystems permits the modeling of the nature, behavior, and preservation potential of primitive microbial communities. This approach entails combined molecular and isotopic analyses to characterize lipids and biopolymers produced by cultured bacteria (representative of ancient strains) and to test a variety of culture conditions that affect their biosynthesis processes. In regards to Mars, the biomarkers from lipids and biopolymers would be expected to be preserved best if life flourished there during its early history (3.5-4 ϫ 10 9 years ago). Both oxidized and reduced products would be expected. This is based on the inference that hydrothermal activity occurred during that time, with the concomitant preservation of biochemically-derived carbonaceous matter. Known biomarkers (i.e., as elucidated for early terrestrial samples and for primitive terrestrial microbiota) as well as novel, potentially unknown compounds, should be characterized. Anat

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Microscopic organic analysis using two-step laser mass spectrometry: application to meteoritic acid residues

Cited by 96 publications

References 33 publications

Microprobe two-step laser mass spectrometry as an analytical tool for meteoritic samples

Microprobe two-step laser mass spectrometry as an analytical tool for meteoritic samples

Laser mass spectrometric detection of extraterrestrial aromatic molecules: Mini-review and examination of pulsed heating effects

Molecular indicators (biomarkers) of past life

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