Detection of extraterrestrial life is an ongoing goal in space exploration, and there is a need for advanced instruments and methods for the detection of signatures of life based on chemical and isotopic composition. Here, we present the first investigation of chemical composition of putative microfossils in natural samples using a miniature laser ablation/ionization time-of-flight mass spectrometer (LMS). The studies were conducted with high lateral (∼15 μm) and vertical (∼20–200 nm) resolution. The primary aim of the study was to investigate the instrument performance on micrometer-sized samples both in terms of isotope abundance and element composition. The following objectives had to be achieved: (1) Consider the detection and calculation of single stable isotope ratios in natural rock samples with techniques compatible with their employment of space instrumentation for biomarker detection in future planetary missions. (2) Achieve a highly accurate chemical compositional map of rock samples with embedded structures at the micrometer scale in which the rock matrix is easily distinguished from the micrometer structures. Our results indicate that chemical mapping of strongly heterogeneous rock samples can be obtained with a high accuracy, whereas the requirements for isotope ratios need to be improved to reach sufficiently large signal-to-noise ratio (SNR). Key Words: Biogenicity—Biomarkers—Biosignatures—Filaments—Fossilization. Astrobiology 15, 669–682.

High-speed detector systems with high dynamic range and pulse width characteristics in the sub-nanosecond regime are mandatory for high resolution and highly sensitive time-of-flight mass spectrometers. Typically, for a reasonable detector area, an impedance-matched anode design is necessary to transmit the registered signal fast and distortion-free from the anode to the signal acquisition system. In this report, a high-speed microstrip multi-anode multichannel plate detector is presented and discussed. The anode consists of four separate active concentric anode segments allowing a simultaneous readout of signal with a dynamic range of about eight orders of magnitude. The impedance matched anode segments show pulse width of about 250 ps, measured at full width at half maximum, and rise time of ∼170 ps, measured with an oscilloscope with a sampling rate of 20 GS/s and 4 GHz analogue bandwidth. The usage of multichannel plates as signal amplifier allowed the design of a lightweight, low power consuming, and compact detector system, suitable, e.g., for the integration into space instrumentation or portable systems where size, weight, and power consumption are limited parameters.

The last decade witnessed considerable progress in the development of laser ablation/ionisation time-of-flight mass spectrometry (LI-TOFMS). The improvement of both the laser ablation ion sources employing femtosecond lasers and the method of ion coupling with the mass analyser led to highly sensitive element and isotope measurements, minimisation of matrix effects, and reduction of various fractionation effects. This improvement of instrumental performance can be attributed to the progress in laser technology and accompanying commercialisation of fs-laser systems, as well as the availability of fast electronics and data acquisition systems. Application of femtosecond laser radiation to ablate the sample causes negligible thermal effects, which in turn allows for improved resolution of chemical surface imaging and depth profiling. Following in the footsteps of its predecessor ns-LIMS, fs-LIMS, which employs fs-laser ablation ion sources, has been developed in the last two decades as an important method of chemical analysis and will continue to improve its performance in subsequent decades. This review discusses the background of fs-laser ablation, overviews the most relevant instrumentation and emphasises their performance figures, and summarizes the studies on several applications, including geochemical, semiconductor, and bio-relevant materials. Improving the chemical analysis is expected by the implementation of laser pulse sequences or pulse shaping methods and shorter laser wavelengths providing current progress in mass resolution achieved in fs-LIMS. In parallel, advancing the methods of data analysis has the potential of making this technique very attractive for 3D chemical analysis with micrometre lateral and sub-micrometre vertical resolution.