An Orbitrap/Time-of-Flight Mass Spectrometer for Photofragment Ion Imaging and High-Resolution Mass Analysis of Native Macromolecular Assemblies

Anjusha Mathew, Frans Giskes, Alexandros Lekkas, Jean-François Greisch, Gert B Eijkel, Ian G M Anthony, Kyle Fort, Albert J R Heck, Dimitris Papanastasiou, Alexander A Makarov, Shane R Ellis*, Ron M A Heeren*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

We discuss the design, development, and evaluation of an Orbitrap/time-of-flight (TOF) mass spectrometry (MS)-based instrument with integrated UV photodissociation (UVPD) and time/mass-to-charge ratio ( m/ z)-resolved imaging for the comprehensive study of the higher-order molecular structure of macromolecular assemblies (MMAs). A bespoke TOF analyzer has been coupled to the higher-energy collisional dissociation cell of an ultrahigh mass range hybrid quadrupole-Orbitrap MS. A 193 nm excimer laser was employed to photofragment MMA ions. A combination of microchannel plates (MCPs)-Timepix (TPX) quad and MCPs-phosphor screen-TPX3CAM assemblies have been used as axial and orthogonal imaging detectors, respectively. The instrument can operate in four different modes, where the UVPD-generated fragment ions from the native MMA ions can be measured with high-mass resolution or imaged in a mass-resolved manner to reveal the relative positions of the UVPD fragments postdissociation. This information is intended to be utilized for retrieving higher-order molecular structural details that include the conformation, subunit stoichiometry, and molecular interactions as well as to understand the dissociation dynamics of the MMAs in the gas phase.

Original languageEnglish
Pages (from-to)1359-1371
Number of pages13
JournalJournal of the American Society for Mass Spectrometry
Volume34
Issue number7
Early online date15 Jun 2023
DOIs
Publication statusPublished - 5 Jul 2023

Keywords

  • Orbitrap mass spectrometry
  • Timepix detector
  • UV photodissociation
  • macromolecular assemblies
  • orthogonal time-of-flight mass spectrometry
  • photofragment ion imaging

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