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

Abstract

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-SIMSmore » is a viable method for small molecule imaging of intact molecular ions in complex biological systems. VC 2016 American Vacuum Society.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [3];  [2];  [4]
+ Show Author Affiliations
  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
Publication Date:
Research Org.:
University of Notre Dame, IN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1371711
Alternate Identifier(s):
OSTI ID: 1421229
Grant/Contract Number:  
SC0006642; DBI-9871103; R01AI113219; T32 GM70421; DE SC-0006642
Resource Type:
Accepted Manuscript
Journal Name:
Biointerphases
Additional Journal Information:
Journal Volume: 11; Journal Issue: 2; Journal ID: ISSN 1934-8630
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
60 APPLIED LIFE SCIENCES; 59 BASIC BIOLOGICAL SCIENCES

Citation Formats

Dunham, Sage J. B., Comi, Troy J., Ko, Kyungwon, Li, Bin, Baig, Nameera F., Morales-Soto, Nydia, Shrout, Joshua D., Bohn, Paul W., and Sweedler, Jonathan V. Metal-assisted polyatomic SIMS and laser desorption/ionization for enhanced small molecule imaging of bacterial biofilms. United States: N. p., 2016. Web. doi:10.1116/1.4942884.
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Dunham, Sage J. B., Comi, Troy J., Ko, Kyungwon, Li, Bin, Baig, Nameera F., Morales-Soto, Nydia, Shrout, Joshua D., Bohn, Paul W., & Sweedler, Jonathan V. Metal-assisted polyatomic SIMS and laser desorption/ionization for enhanced small molecule imaging of bacterial biofilms. United States. https://doi.org/10.1116/1.4942884
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Dunham, Sage J. B., Comi, Troy J., Ko, Kyungwon, Li, Bin, Baig, Nameera F., Morales-Soto, Nydia, Shrout, Joshua D., Bohn, Paul W., and Sweedler, Jonathan V. Fri . "Metal-assisted polyatomic SIMS and laser desorption/ionization for enhanced small molecule imaging of bacterial biofilms". United States. https://doi.org/10.1116/1.4942884. https://www.osti.gov/servlets/purl/1371711.
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@article{osti_1371711,
title = {Metal-assisted polyatomic SIMS and laser desorption/ionization for enhanced small molecule imaging of bacterial biofilms},
author = {Dunham, Sage J. B. and Comi, Troy J. and Ko, Kyungwon and Li, Bin and Baig, Nameera F. and Morales-Soto, Nydia and Shrout, Joshua D. and Bohn, Paul W. and Sweedler, Jonathan V.},
abstractNote = {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.},
doi = {10.1116/1.4942884},
journal = {Biointerphases},
number = 2,
volume = 11,
place = {United States},
year = {Fri Mar 04 00:00:00 EST 2016},
month = {Fri Mar 04 00:00:00 EST 2016}
}
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Works referenced in this record:

Biofilms: the matrix revisited
journal, January 2005

The biofilm matrix
journal, August 2010

  • Flemming, Hans-Curt; Wingender, Jost
  • Nature Reviews Microbiology, Vol. 8, Issue 9
  • DOI: 10.1038/nrmicro2415

Introducing npj Biofilms and Microbiomes
journal, March 2015

Subsurface Biomolecular Imaging of Streptomyces coelicolor Using Secondary Ion Mass Spectrometry
journal, February 2008

  • Vaidyanathan, Seetharaman; Fletcher, John S.; Goodacre, Roy
  • Analytical Chemistry, Vol. 80, Issue 6
  • DOI: 10.1021/ac701921e

Multimodal chemical imaging of molecular messengers in emerging Pseudomonas aeruginosa bacterial communities
journal, January 2015

  • Baig, Nameera F.; Dunham, Sage J. B.; Morales-Soto, Nydia
  • The Analyst, Vol. 140, Issue 19
  • DOI: 10.1039/C5AN01149C

Mass spectrometric metabolomic imaging of biofilms on corroding steel surfaces using laser ablation and solvent capture by aspiration
journal, March 2015

  • Brauer, Jonathan I.; Makama, Zakari; Bonifay, Vincent
  • Biointerphases, Vol. 10, Issue 1
  • DOI: 10.1116/1.4906744

Spatial Profiling with MALDI MS:  Distribution of Neuropeptides within Single Neurons
journal, September 2003

  • Rubakhin, Stanislav S.; Greenough, William T.; Sweedler, Jonathan V.
  • Analytical Chemistry, Vol. 75, Issue 20
  • DOI: 10.1021/ac034498+

Secondary Ion Mass Spectrometry Imaging of Molecular Distributions in Cultured Neurons and Their Processes: Comparative Analysis of Sample Preparation
journal, August 2012

  • Tucker, Kevin R.; Li, Zhen; Rubakhin, Stanislav S.
  • Journal of the American Society for Mass Spectrometry, Vol. 23, Issue 11
  • DOI: 10.1007/s13361-012-0472-1

Vitamin E Imaging and Localization in the Neuronal Membrane
journal, September 2005

  • Monroe, Eric B.; Jurchen, John C.; Lee, Jinju
  • Journal of the American Chemical Society, Vol. 127, Issue 35
  • DOI: 10.1021/ja051223y

Imaging and 3D Elemental Characterization of Intact Bacterial Spores by High-Resolution Secondary Ion Mass Spectrometry
journal, August 2008

  • Ghosal, Sutapa; Fallon, Stewart J.; Leighton, Terrance J.
  • Analytical Chemistry, Vol. 80, Issue 15
  • DOI: 10.1021/ac8006279

A concise review of mass spectrometry imaging
journal, June 2010

  • Amstalden van Hove, Erika R.; Smith, Donald F.; Heeren, Ron M. A.
  • Journal of Chromatography A, Vol. 1217, Issue 25
  • DOI: 10.1016/j.chroma.2010.01.033

Imaging mass spectrometry in microbiology
journal, August 2011

  • Watrous, Jeramie D.; Dorrestein, Pieter C.
  • Nature Reviews Microbiology, Vol. 9, Issue 9
  • DOI: 10.1038/nrmicro2634

A novel strategy for MALDI-TOF MS analysis of small molecules
journal, January 2010

  • Zhang, Shu; Liu, Jian’an; Chen, Yi
  • Journal of the American Society for Mass Spectrometry, Vol. 21, Issue 1
  • DOI: 10.1016/j.jasms.2009.09.024

Optimization and Comparison of Multiple MALDI Matrix Application Methods for Small Molecule Mass Spectrometric Imaging
journal, October 2014

  • Gemperline, Erin; Rawson, Stephanie; Li, Lingjun
  • Analytical Chemistry, Vol. 86, Issue 20
  • DOI: 10.1021/ac5028534

Comprehensive bioimaging with fluorinated nanoparticles using breathable liquids
journal, January 2015

  • Kurczy, Michael E.; Zhu, Zheng-Jiang; Ivanisevic, Julijana
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms6998

MALDI-guided SIMS: Multiscale Imaging of Metabolites in Bacterial Biofilms
journal, August 2014

  • Lanni, Eric J.; Masyuko, Rachel N.; Driscoll, Callan M.
  • Analytical Chemistry, Vol. 86, Issue 18
  • DOI: 10.1021/ac5020222

LDI-MS Assisted by Chemical-Free Gold Nanoparticles: Enhanced Sensitivity and Reduced Background in the Low-Mass Region
journal, November 2013

  • Amendola, Vincenzo; Litti, Lucio; Meneghetti, Moreno
  • Analytical Chemistry, Vol. 85, Issue 24
  • DOI: 10.1021/ac401662r

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

  • Woo, Hin-Koon; Northen, Trent R.; Yanes, Oscar
  • Nature Protocols, Vol. 3, Issue 8
  • DOI: 10.1038/nprot.2008.110

Desorption–ionization mass spectrometry on porous silicon
journal, May 1999

  • Wei, Jing; Buriak, Jillian M.; Siuzdak, Gary
  • Nature, Vol. 399, Issue 6733
  • DOI: 10.1038/20400

Matrix-free methods for laser desorption/ionization mass spectrometry
journal, January 2006

  • Peterson, Dominic S.
  • Mass Spectrometry Reviews, Vol. 26, Issue 1
  • DOI: 10.1002/mas.20104


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

  • Brenes, Daniel A.; Garrison, Barbara J.; Winograd, Nicholas
  • The Journal of Physical Chemistry Letters, Vol. 2, Issue 16
  • DOI: 10.1021/jz200708j

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

  • Angerer, Tina B.; Dowlatshahi Pour, Masoumeh; Malmberg, Per
  • Analytical Chemistry, Vol. 87, Issue 8
  • DOI: 10.1021/ac504774y

Biomolecular Imaging with a C60-SIMS/MALDI Dual Ion Source Hybrid Mass Spectrometer: Instrumentation, Matrix Enhancement, and Single Cell Analysis
journal, September 2014

  • Lanni, Eric J.; Dunham, Sage J. B.; Nemes, Peter
  • Journal of The American Society for Mass Spectrometry, Vol. 25, Issue 11
  • DOI: 10.1007/s13361-014-0978-9

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

  • Altelaar, A. F. Maarten; Klinkert, Ivo; Jalink, Kees
  • Analytical Chemistry, Vol. 78, Issue 3
  • DOI: 10.1021/ac0513111

Gold and silver nanoparticle-assisted laser desorption ionization mass spectrometry compatible with secondary ion mass spectrometry for lipid analysis
journal, July 2014

  • Mohammadi, Amir Saeid; Fletcher, John S.; Malmberg, Per
  • Surface and Interface Analysis, Vol. 46, Issue S1
  • DOI: 10.1002/sia.5609

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

  • McDonnell, Liam A.; Heeren, Ron M. A.; Lange, Robert P. J.
  • Journal of the American Society for Mass Spectrometry, Vol. 17, Issue 9
  • DOI: 10.1016/j.jasms.2006.05.003

Insights into the yield enhancement and ion emission process in metal-assisted SIMS
journal, June 2012

  • Nittler, L.; Delcorte, A.; Bertrand, P.
  • Surface and Interface Analysis, Vol. 45, Issue 1
  • DOI: 10.1002/sia.5045

Investigation of methods to enhance the secondary ion yields in TOF-SIMS of organic samples
journal, January 2008

  • Heile, A.; Lipinsky, D.; Wehbe, N.
  • Surface and Interface Analysis, Vol. 40, Issue 3-4
  • DOI: 10.1002/sia.2810

Mechanisms of metal-assisted secondary ion mass spectrometry: a mixed theoretical and experimental study
journal, February 2010

  • Restrepo, O.; Prabhakaran, A.; Hamraoui, K.
  • Surface and Interface Analysis, Vol. 42, Issue 6-7
  • DOI: 10.1002/sia.3203

Investigations of secondary ion yield-enhancing methods in combination
journal, June 2010

  • Heile, A.; Muhmann, C.; Lipinsky, D.
  • Surface and Interface Analysis, Vol. 43, Issue 1-2
  • DOI: 10.1002/sia.3556

Metal-Assisted Secondary Ion Mass Spectrometry Using Atomic (Ga + , In + ) and Fullerene Projectiles
journal, May 2007

  • Delcorte, A.; Yunus, S.; Wehbe, N.
  • Analytical Chemistry, Vol. 79, Issue 10
  • DOI: 10.1021/ac062406l

Organic Secondary Ion Mass Spectrometry:  Sensitivity Enhancement by Gold Deposition
journal, October 2002

  • Delcorte, A.; Médard, N.; Bertrand, P.
  • Analytical Chemistry, Vol. 74, Issue 19
  • DOI: 10.1021/ac020125h

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

  • Wehbe, Nimer; Heile, Andreas; Arlinghaus, Heinrich F.
  • Analytical Chemistry, Vol. 80, Issue 16
  • DOI: 10.1021/ac800568y

Reduction of matrix effects in TOF-SIMS analysis by metal-assisted SIMS (MetA-SIMS)
journal, January 2005

  • Inoue, M.; Murase, A.
  • Surface and Interface Analysis, Vol. 37, Issue 12
  • DOI: 10.1002/sia.2121

Metal-Assisted Secondary Ion Mass Spectrometry:  Influence of Ag and Au Deposition on Molecular Ion Yields
journal, October 2004

  • Adriaensen, L.; Vangaever, F.; Gijbels, R.
  • Analytical Chemistry, Vol. 76, Issue 22
  • DOI: 10.1021/ac049108d

Enhancement of the static SIMS secondary ion yields of lipid moieties by ultrathin gold coating of aged oil paint surfaces
journal, January 2004

  • Keune, K.; Boon, J. J.
  • Surface and Interface Analysis, Vol. 36, Issue 13
  • DOI: 10.1002/sia.1996

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

  • Steinberg, Nitai; Kolodkin-Gal, Ilana
  • Journal of Bacteriology, Vol. 197, Issue 13
  • DOI: 10.1128/JB.02516-14

Preparation, Imaging, and Quantification of Bacterial Surface Motility Assays
journal, January 2015

  • Morales-Soto, Nydia; Anyan, Morgen E.; Mattingly, Anne E.
  • Journal of Visualized Experiments, Issue 98
  • DOI: 10.3791/52338

A cross-platform toolkit for mass spectrometry and proteomics
journal, October 2012

  • Chambers, Matthew C.; Maclean, Brendan; Burke, Robert
  • Nature Biotechnology, Vol. 30, Issue 10
  • DOI: 10.1038/nbt.2377

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

  • Robichaud, Guillaume; Garrard, Kenneth P.; Barry, Jeremy A.
  • Journal of The American Society for Mass Spectrometry, Vol. 24, Issue 5
  • DOI: 10.1007/s13361-013-0607-z

4-Quinolones: Smart Phones of the Microbial World
journal, January 2011

  • Huse, Holly; Whiteley, Marvin
  • Chemical Reviews, Vol. 111, Issue 1
  • DOI: 10.1021/cr100063u

Rhamnolipids: diversity of structures, microbial origins and roles
journal, March 2010

  • Abdel-Mawgoud, Ahmad Mohammad; Lépine, François; Déziel, Eric
  • Applied Microbiology and Biotechnology, Vol. 86, Issue 5
  • DOI: 10.1007/s00253-010-2498-2

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

  • Lépine, François; Milot, Sylvain; Déziel, Eric
  • Journal of the American Society for Mass Spectrometry, Vol. 15, Issue 6
  • DOI: 10.1016/j.jasms.2004.02.012

Deposition of Ni and Ag on Benzene Multilayers Adsorbed on W(110)
journal, January 1996

  • Whitten, J. E.; Gomer, R.
  • The Journal of Physical Chemistry, Vol. 100, Issue 6
  • DOI: 10.1021/jp952246+

Computer simulations of cluster impacts: effects of the atomic masses of the projectile and target
journal, January 2013

  • Restrepo, Oscar A.; Gonze, Xavier; Bertrand, Patrick
  • Physical Chemistry Chemical Physics, Vol. 15, Issue 20
  • DOI: 10.1039/c3cp50346a

Interaction of energetic clusters (Au3, Au400 and C60) with organic material and adsorbed gold nanoparticles
journal, July 2011

  • 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
  • DOI: 10.1016/j.nimb.2010.11.014
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    Solid Sampling with a Diode Laser for Portable Ambient Mass Spectrometry
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    Mass Spectrometry Imaging of Complex Microbial Communities
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    A concise tutorial review of TOF-SIMS based molecular and cellular imaging
    journal, January 2019

    • Massonnet, Philippe; Heeren, Ron M. A.
    • Journal of Analytical Atomic Spectrometry, Vol. 34, Issue 11
    • DOI: 10.1039/c9ja00164f
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