Giving Gold Wings: Ultrabright and Fragmentation Free Mass Spectrometry Reporters for Barcoding, Bioconjugation Monitoring, and Data Storage

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...

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Bibliographic Details
Published inAngewandte Chemie Vol. 135; no. 21
Main Authors Dominique, Nathaniel L., Jensen, Isabel M., Kaur, Gurkiran, Kotseos, Chandler Q., Boggess, William C., Jenkins, David M., Camden, Jon P.
Format Journal Article
LanguageEnglish
Published Weinheim Wiley Subscription Services, Inc 15.05.2023
Subjects
Bright plating
Chemistry
Contrast agents
Contrast media
Data storage
Fragmentation
Gold
Ionization
Laser applications
Ligands
Mass Spectrometry
Mass spectroscopy
Monitoring
Multiplexed Imaging
Multiplexing
N-Heterocyclic Carbenes
Nanoparticles
Small Molecule Data Storage
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Summary: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. N‐Heterocyclic Carbene (NHC) functionalized gold nanoparticles (AuNPs) are highly tunable and bright mass spectrometry reporters. NHC ligands fragment less and achieve higher ion yield than conventional thiol systems, which enables bioconjugation monitoring, mass spectrometry imaging, and data storage applications.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202219182