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Femtosecond Laser Desorption Postionization MS vs ToF-SIMS Imaging for Uncovering Biomarkers Buried in Geological Samples

Journal Article · · Analytical Chemistry
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  1. Univ. of Illinois, Chicago, IL (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
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The study of lipid molecular fossils by traditional biomarker analysis requires bulk sample crushing, followed by solvent extraction, and then the analysis of the extract by gas chromatography-mass spectrometry (GC–MS). This traditional analysis mixes all organic compounds in the sample regardless of their origins, with a loss of information on the spatial distribution of organic molecules within the sample. These shortcomings can be overcome using the chemical mapping of intact samples. Spectroscopic techniques such as UV fluorescence or Raman spectroscopy, laser ablation inductively coupled plasma mass spectrometry, and time-of-flight secondary ion mass spectrometry (ToF-SIMS) are among those elemental and molecular mapping techniques. This study employed femtosecond (fs) laser ablation combined with single-photon ionization, a method called fs-laser desorption postionization mass spectrometry (fs-LDPI-MS). In this work, a pulsed ~75 fs, 800 nm laser was used to ablate the geological sample, which was then photoionized after a few microseconds by a pulsed 7.9 eV vacuum ultraviolet laser. An organic carbon-rich geological sample was used for this study to map hydrocarbon biomarkers in sediments that were previously studied by GC–MS. The petrography of this sample was examined by optical and fluorescence microscopy. It is demonstrated here that fs-LDPI-MS combined with petrography for multimodal imaging can expose buried compounds within the sample via in situ layer removal. When used in conjunction with traditional organic geochemical analysis, this method has the potential to determine the spatial distribution of organic biomarkers in geological material. Finally, fs-LDPI-MS imaging data are compared with ToF-SIMS imaging that is commonly used for such studies.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Sponsoring Organization:
National Aeronautics and Space Administration (NASA); USDOE Office of Science (SC)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1883742
Journal Information:
Analytical Chemistry, Journal Name: Analytical Chemistry Journal Issue: 48 Vol. 93; ISSN 0003-2700
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (41)

Surface mass spectrometry of molecular species journal July 1999
New horizons in sputter depth profiling inorganics with giant gas cluster sources: Niobium oxide thin films journal July 2017
Removal of different-age biofilms using carbon dioxide aerosols journal June 2014
The sTOF, a Favorable Geometry for a Time-of-Flight Analyzer journal November 2016
Fluorescence of sedimentary organic matter in relation to its chemical composition journal January 1986
Molecular indicators for palaeoenvironmental change in a Messinian evaporitic sequence (Vena del Gesso, Italy): III. Stratigraphic changes in the molecular structure of kerogen in a single marl bed as revealed by flash pyrolysis journal June 1995
Diagenetic and catagenetic products of isorenieratene: Molecular indicators for photic zone anoxia journal November 1996
Fluorescence micro-spectrometry of synthetic and natural hydrocarbon fluid inclusions: crude oil chemistry, density and application to petroleum migration journal May 1997
In situ iron isotope ratio determination using UV-femtosecond laser ablation with application to hydrothermal ore formation processes journal July 2006
Okenane, a biomarker for purple sulfur bacteria (Chromatiaceae), and other new carotenoid derivatives from the 1640Ma Barney Creek Formation journal March 2008
Methods for full resolution data exploration and visualization for large 2D and 3D mass spectrometry imaging datasets journal April 2014
Removal of biofilms using carbon dioxide aerosols journal November 2010
Inclusive sharing of mass spectrometry imaging data requires a converter for all journal August 2012
First on-line analysis of petroleum from single inclusion using ultrafast laser ablation journal February 2010
Biomarker imaging of single diatom cells in a microbial mat using time-of-flight secondary ion mass spectrometry (ToF-SIMS) journal April 2013
UV Raman spectroscopy of hydrocarbon-bearing inclusions in rock salt from the Dongying sag, eastern China journal November 2016
Using petroleum inclusions to trace petroleum systems – A review journal March 2019
BIOMARKERS Occurence, Utility, and Detection journal August 1988
Laser Desorption Postionization Mass Spectrometry of Antibiotic-Treated Bacterial Biofilms Using Tunable Vacuum Ultraviolet Radiation journal September 2010
Feasibility of Depth Profiling of Animal Tissue by Ultrashort Pulse Laser Ablation journal April 2012
High Lateral Resolution vs Molecular Preservation in near-IR fs-Laser Desorption Postionization Mass Spectrometry journal December 2014
Light and Molecular Ions: The Emergence of Vacuum UV Single-Photon Ionization in MS journal June 2009
Laser Desorption Postionization Mass Spectrometry Imaging of Folic Acid Molecules in Tumor Tissue journal August 2017
An Experimental and Theoretical Study of Laser Postionization of Femtosecond-Laser-Desorbed Drug Molecules journal September 2020
Molecular Imaging and Depth Profiling of Biomaterials Interfaces by Femtosecond Laser Desorption Postionization Mass Spectrometry journal August 2013
Internal Energy of Thermometer Ions Formed by Femtosecond Laser Desorption: Implications for Mass Spectrometric Imaging journal June 2014
Biomarker evidence for green and purple sulphur bacteria in a stratified Palaeoproterozoic sea journal October 2005
Reassessing the first appearance of eukaryotes and cyanobacteria journal October 2008
Femtosecond laser ablation inductively coupled plasma source mass spectrometry for elemental and isotopic analysis: are ultrafast lasers worthwhile? journal January 2017
Photoionization mass spectrometer with a microscope laser desorption source journal June 1992
Depth profiling and imaging capabilities of an ultrashort pulse laser ablation time of flight mass spectrometer journal September 2012
SIMS analyses of the oldest known assemblage of microfossils document their taxon-correlated carbon isotope compositions journal December 2017
The Ladder of Life Detection journal November 2018
Analysis of hopanes and steranes in single oil-bearing fluid inclusions using time-of-flight secondary ion mass spectrometry (ToF-SIMS): Analysis of hopanes and steranes in single oil-bearing fluid inclusions journal January 2010
Ultrashort pulse laser ablation for depth profiling of bacterial biofilms
  • Milasinovic, Slobodan; Liu, Yaoming; Gasper, Gerald L.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 28, Issue 4 https://doi.org/10.1116/1.3397736
journal July 2010
Intermittent euxinia: Reconciliation of a Jurassic black shale with its biofacies journal January 2004
Isotopic biogeochemistry of the Oxford Clay Formation (Jurassic), UK journal January 1994
Laser Desorption Combined with Laser Postionization for Mass Spectrometry journal June 2019
Metabolic Imaging at the Single-Cell Scale: Recent Advances in Mass Spectrometry Imaging journal June 2019
Using Time-of-Flight Secondary Ion Mass Spectrometry to Study Biomarkers journal May 2011
Dynamic Modelling and Simulation of a Cryogenic Carbon Dioxide Cleaning Process journal November 2010

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