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Title: Metal-assisted polyatomic SIMS and laser desorption/ionization for enhanced small molecule imaging of bacterial biofilms

Journal Article · · Biointerphases
DOI:https://doi.org/10.1116/1.4942884· OSTI ID:1371711
 [1];  [1];  [1];  [1];  [2];  [3];  [3];  [2];  [4]
  1. Univ. of Illinois, Urbana-Champaign, IL (United States). Dept. of Chemistry and Beckman Inst. for Advanced Science and Technology
  2. Univ. of Notre Dame, IN (United States). Dept. of Chemistry and Biochemistry, Dept. of Chemical and Biomolecular Engineering
  3. Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Sciences, Dept. of Biological Sciences, Eck Inst. for Global Health
  4. Univ. of Illinois, Urbana-Champaign, IL (United States). Dept. of Chemistry, Beckman Inst. for Advanced Science and Technology

Mass spectrometry imaging (MSI) has become an important analytical tool for many sectors of science and medicine. As the application of MSI expands into new areas of inquiry, existing methodologies must be adapted and improved to meet emerging challenges. In particular salient is the need for small molecule imaging methods that are compatible with complex multicomponent systems, a challenge that is amplified by the effects of analyte migration and matrix interference. Furthermore, with a focus on microbial biofilms from the opportunistic pathogen Pseudomonas aeruginosa, the relative advantages of two established microprobe-based MSI techniques—polyatomic secondary ion mass spectrometry (SIMS) and laser desorption/ionization—are compared, with emphasis on exploring the effect of surface metallization on small molecule imaging. A combination of qualitative image comparison and multivariate statistical analysis demonstrates that sputtering microbial biofilms with a 2.5 nm layer of gold selectively enhances C60-SIMS ionization for several molecular classes including rhamnolipids and 2-alkyl-quinolones. Metallization also leads to the reduction of in-source fragmentation and subsequent ionization of media-specific background polymers, which improves spectral purity and image quality. Our findings show that the influence of metallization upon ionization is strongly dependent on both the surface architecture and the analyte class, and further demonstrate that metal-assisted C60-SIMS is a viable method for small molecule imaging of intact molecular ions in complex biological systems. VC 2016 American Vacuum Society.

Research Organization:
University of Notre Dame, IN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
SC0006642; DBI-9871103; R01AI113219; T32 GM70421; DE SC-0006642
OSTI ID:
1371711
Alternate ID(s):
OSTI ID: 1421229
Journal Information:
Biointerphases, Vol. 11, Issue 2; ISSN 1934-8630
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 19 works
Citation information provided by
Web of Science

References (55)

Biofilms: the matrix revisited journal January 2005
The biofilm matrix journal August 2010
Introducing npj Biofilms and Microbiomes journal March 2015
Subsurface Biomolecular Imaging of Streptomyces coelicolor Using Secondary Ion Mass Spectrometry journal February 2008
Multimodal chemical imaging of molecular messengers in emerging Pseudomonas aeruginosa bacterial communities journal January 2015
Mass spectrometric metabolomic imaging of biofilms on corroding steel surfaces using laser ablation and solvent capture by aspiration journal March 2015
Spatial Profiling with MALDI MS:  Distribution of Neuropeptides within Single Neurons journal September 2003
Secondary Ion Mass Spectrometry Imaging of Molecular Distributions in Cultured Neurons and Their Processes: Comparative Analysis of Sample Preparation journal August 2012
Vitamin E Imaging and Localization in the Neuronal Membrane journal September 2005
Imaging and 3D Elemental Characterization of Intact Bacterial Spores by High-Resolution Secondary Ion Mass Spectrometry journal August 2008
A concise review of mass spectrometry imaging journal June 2010
Imaging mass spectrometry in microbiology journal August 2011
A novel strategy for MALDI-TOF MS analysis of small molecules journal January 2010
Optimization and Comparison of Multiple MALDI Matrix Application Methods for Small Molecule Mass Spectrometric Imaging journal October 2014
Comprehensive bioimaging with fluorinated nanoparticles using breathable liquids journal January 2015
MALDI-guided SIMS: Multiscale Imaging of Metabolites in Bacterial Biofilms journal August 2014
LDI-MS Assisted by Chemical-Free Gold Nanoparticles: Enhanced Sensitivity and Reduced Background in the Low-Mass Region journal November 2013
Metal condensates for low-molecular-weight matrix-free laser desorption/ionization journal April 2012
Nanostructure-initiator mass spectrometry: a protocol for preparing and applying NIMS surfaces for high-sensitivity mass analysis journal July 2008
Desorption–ionization mass spectrometry on porous silicon journal May 1999
Matrix-free methods for laser desorption/ionization mass spectrometry journal January 2006
journal December 2023
SIMS—A precursor and partner to contemporary mass spectrometry journal February 2015
Fluid Flow and Effusive Desorption: Dominant Mechanisms of Energy Dissipation after Energetic Cluster Bombardment of Molecular Solids journal July 2011
Characterisation of biological material with ToF-SIMS: a review journal March 2014
Improved Molecular Imaging in Rodent Brain with Time-of-Flight-Secondary Ion Mass Spectrometry Using Gas Cluster Ion Beams and Reactive Vapor Exposure journal April 2015
Biomolecular Imaging with a C60-SIMS/MALDI Dual Ion Source Hybrid Mass Spectrometer: Instrumentation, Matrix Enhancement, and Single Cell Analysis journal September 2014
Matrix-enhanced cluster-SIMS journal July 2006
Gold-Enhanced Biomolecular Surface Imaging of Cells and Tissue by SIMS and MALDI Mass Spectrometry journal February 2006
Gold and silver nanoparticle-assisted laser desorption ionization mass spectrometry compatible with secondary ion mass spectrometry for lipid analysis journal July 2014
Silver deposition on freeze-dried cells allows subcellular localization of cholesterol with imaging TOF-SIMS journal August 2004
Higher sensitivity secondary ion mass spectrometry of biological molecules for high resolution, chemically specific imaging journal September 2006
Insights into the yield enhancement and ion emission process in metal-assisted SIMS journal June 2012
Investigation of methods to enhance the secondary ion yields in TOF-SIMS of organic samples journal January 2008
Mechanisms of metal-assisted secondary ion mass spectrometry: a mixed theoretical and experimental study journal February 2010
Investigations of secondary ion yield-enhancing methods in combination journal June 2010
Metal-Assisted Secondary Ion Mass Spectrometry Using Atomic (Ga + , In + ) and Fullerene Projectiles journal May 2007
Organic Secondary Ion Mass Spectrometry:  Sensitivity Enhancement by Gold Deposition journal October 2002
Effects of Metal Nanoparticles on the Secondary Ion Yields of a Model Alkane Molecule upon Atomic and Polyatomic Projectiles in Secondary Ion Mass Spectrometry journal July 2008
Reduction of matrix effects in TOF-SIMS analysis by metal-assisted SIMS (MetA-SIMS) journal January 2005
Metal-Assisted Secondary Ion Mass Spectrometry:  Influence of Ag and Au Deposition on Molecular Ion Yields journal October 2004
Enhancement of the static SIMS secondary ion yields of lipid moieties by ultrathin gold coating of aged oil paint surfaces journal January 2004
Correlation between molecular secondary ion yield and cluster ion sputtering for samples with different stopping powers journal July 2012
The Matrix Reloaded: How Sensing the Extracellular Matrix Synchronizes Bacterial Communities journal March 2015
Preparation, Imaging, and Quantification of Bacterial Surface Motility Assays journal January 2015
A cross-platform toolkit for mass spectrometry and proteomics journal October 2012
Inclusive sharing of mass spectrometry imaging data requires a converter for all journal August 2012
MSiReader: An Open-Source Interface to View and Analyze High Resolving Power MS Imaging Files on Matlab Platform journal March 2013
4-Quinolones: Smart Phones of the Microbial World journal January 2011
Rhamnolipids: diversity of structures, microbial origins and roles journal March 2010
Quinolones: from antibiotics to autoinducers journal March 2011
Electrospray/mass spectrometric identification and analysis of 4-hydroxy-2-alkylquinolines (HAQs) produced by Pseudomonas aeruginosa journal June 2004
Deposition of Ni and Ag on Benzene Multilayers Adsorbed on W(110) journal January 1996
Computer simulations of cluster impacts: effects of the atomic masses of the projectile and target journal January 2013
Interaction of energetic clusters (Au3, Au400 and C60) with organic material and adsorbed gold nanoparticles
  • Restrepo, Oscar A.; Prabhakaran, Aneesh; Delcorte, Arnaud
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 269, Issue 14 https://doi.org/10.1016/j.nimb.2010.11.014
journal July 2011

Cited By (3)

Solid Sampling with a Diode Laser for Portable Ambient Mass Spectrometry journal July 2017
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A concise tutorial review of TOF-SIMS based molecular and cellular imaging journal January 2019