Giving Gold Wings: Ultrabright and Fragmentation Free Mass Spectrometry Reporters for Barcoding, Bioconjugation Monitoring, and Data Storage
Nathaniel L. Dominique
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN, 46556 USA
Contribution: Conceptualization (supporting), Data curation (lead), Formal analysis (lead), Investigation (lead), Methodology (lead)
Search for more papers by this authorIsabel M. Jensen
Department of Chemistry, University of Tennessee, Knoxville, Knoxville, TN, 37996 USA
Contribution: Investigation (supporting), Methodology (supporting)
Search for more papers by this authorGurkiran Kaur
Department of Chemistry, University of Tennessee, Knoxville, Knoxville, TN, 37996 USA
Contribution: Investigation (supporting), Methodology (supporting)
Search for more papers by this authorChandler Q. Kotseos
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN, 46556 USA
Contribution: Investigation (supporting), Methodology (supporting)
Search for more papers by this authorDr. William C. Boggess
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN, 46556 USA
Contribution: Investigation (supporting), Methodology (supporting)
Search for more papers by this authorCorresponding Author
Prof. David M. Jenkins
Department of Chemistry, University of Tennessee, Knoxville, Knoxville, TN, 37996 USA
Contribution: Conceptualization (supporting), Funding acquisition (equal), Project administration (equal), Supervision (supporting), Writing - original draft (supporting), Writing - review & editing (supporting)
Search for more papers by this authorCorresponding Author
Prof. Jon P. Camden
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN, 46556 USA
Contribution: Conceptualization (lead), Funding acquisition (equal), Project administration (equal), Supervision (lead), Writing - original draft (lead), Writing - review & editing (lead)
Search for more papers by this authorNathaniel L. Dominique
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN, 46556 USA
Contribution: Conceptualization (supporting), Data curation (lead), Formal analysis (lead), Investigation (lead), Methodology (lead)
Search for more papers by this authorIsabel M. Jensen
Department of Chemistry, University of Tennessee, Knoxville, Knoxville, TN, 37996 USA
Contribution: Investigation (supporting), Methodology (supporting)
Search for more papers by this authorGurkiran Kaur
Department of Chemistry, University of Tennessee, Knoxville, Knoxville, TN, 37996 USA
Contribution: Investigation (supporting), Methodology (supporting)
Search for more papers by this authorChandler Q. Kotseos
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN, 46556 USA
Contribution: Investigation (supporting), Methodology (supporting)
Search for more papers by this authorDr. William C. Boggess
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN, 46556 USA
Contribution: Investigation (supporting), Methodology (supporting)
Search for more papers by this authorCorresponding Author
Prof. David M. Jenkins
Department of Chemistry, University of Tennessee, Knoxville, Knoxville, TN, 37996 USA
Contribution: Conceptualization (supporting), Funding acquisition (equal), Project administration (equal), Supervision (supporting), Writing - original draft (supporting), Writing - review & editing (supporting)
Search for more papers by this authorCorresponding Author
Prof. Jon P. Camden
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN, 46556 USA
Contribution: Conceptualization (lead), Funding acquisition (equal), Project administration (equal), Supervision (lead), Writing - original draft (lead), Writing - review & editing (lead)
Search for more papers by this authorAbstract
The widespread application of laser desorption/ionization mass spectrometry (LDI-MS) highlights the need for a bright and multiplexable labeling platform. While ligand-capped Au nanoparticles (AuNPs) have emerged as a promising LDI-MS contrast agent, the predominant thiol ligands suffer from low ion yields and extensive fragmentation. In this work, we develop a N-heterocyclic carbene (NHC) ligand platform that enhances AuNP LDI-MS performance. NHC scaffolds are tuned to generate barcoded AuNPs which, when benchmarked against thiol-AuNPs, are bright mass tags and form unfragmented ions in high yield. To illustrate the transformative potential of NHC ligands, the mass tags were employed in three orthogonal applications: monitoring a bioconjugation reaction, performing multiplexed imaging, and storing and reading encoded information. These results demonstrate that NHC-nanoparticle systems are an ideal platform for LDI-MS and greatly broaden the scope of nanoparticle contrast agents.
Conflict of interest
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
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