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...