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

doi:10.1021/jasms.3c00053

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 journal › Article › Academic › peer-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 language	English
Pages (from-to)	1359-1371
Number of pages	13
Journal	Journal of the American Society for Mass Spectrometry
Volume	34
Issue number	7
Early online date	15 Jun 2023
DOIs	https://doi.org/10.1021/jasms.3c00053
Publication status	Published - 5 Jul 2023

Bibliographical note

Funding Information:
This research is part of the M4i research program supported by the Dutch Province of Limburg through the LINK program and funded through The Netherlands Organization for Scientific Research (NWO) TTW project 15575 (Structural analysis and position-resolved imaging of macromolecular structures using novel mass spectrometry-based approaches). We would like to thank the Instrument Development Engineering & Evaluation (IDEE) department of Maastricht University for the technical support and Pascal Huysmans (Research Engineering (IDEE)) for the mechanical schematic of the Orbitrap/TOF instrument. S.R.E. acknowledges support from the Australian Research Council Future Fellowship scheme (FT 190100082).

Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.

Funding

This research is part of the M4i research program supported by the Dutch Province of Limburg through the LINK program and funded through The Netherlands Organization for Scientific Research (NWO) TTW project 15575 (Structural analysis and position-resolved imaging of macromolecular structures using novel mass spectrometry-based approaches). We would like to thank the Instrument Development Engineering & Evaluation (IDEE) department of Maastricht University for the technical support and Pascal Huysmans (Research Engineering (IDEE)) for the mechanical schematic of the Orbitrap/TOF instrument. S.R.E. acknowledges support from the Australian Research Council Future Fellowship scheme (FT 190100082).

Funders	Funder number
Dutch Province of Limburg
Australian Research Council	FT 190100082
Nederlandse Organisatie voor Wetenschappelijk Onderzoek	15575

Keywords

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

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10.1021/jasms.3c00053Licence: CC BY

jasms.3c00053Final published version, 5.53 MBLicence: CC BY

Cite this

Mathew, A., Giskes, F., Lekkas, A., Greisch, J.-F., Eijkel, G. B., Anthony, I. G. M., Fort, K., Heck, A. J. R., Papanastasiou, D., Makarov, A. A., Ellis, S. R., & Heeren, R. M. A. (2023). An Orbitrap/Time-of-Flight Mass Spectrometer for Photofragment Ion Imaging and High-Resolution Mass Analysis of Native Macromolecular Assemblies. Journal of the American Society for Mass Spectrometry, 34(7), 1359-1371. https://doi.org/10.1021/jasms.3c00053

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

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. ",

keywords = "Orbitrap mass spectrometry, Timepix detector, UV photodissociation, macromolecular assemblies, orthogonal time-of-flight mass spectrometry, photofragment ion imaging",

author = "Anjusha Mathew and Frans Giskes and Alexandros Lekkas and Jean-Fran{\c c}ois Greisch and Eijkel, {Gert B} and Anthony, {Ian G M} and Kyle Fort and Heck, {Albert J R} and Dimitris Papanastasiou and Makarov, {Alexander A} and Ellis, {Shane R} and Heeren, {Ron M A}",

note = "Funding Information: This research is part of the M4i research program supported by the Dutch Province of Limburg through the LINK program and funded through The Netherlands Organization for Scientific Research (NWO) TTW project 15575 (Structural analysis and position-resolved imaging of macromolecular structures using novel mass spectrometry-based approaches). We would like to thank the Instrument Development Engineering & Evaluation (IDEE) department of Maastricht University for the technical support and Pascal Huysmans (Research Engineering (IDEE)) for the mechanical schematic of the Orbitrap/TOF instrument. S.R.E. acknowledges support from the Australian Research Council Future Fellowship scheme (FT 190100082). Publisher Copyright: {\textcopyright} 2023 The Authors. Published by American Chemical Society.",

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Mathew, A, Giskes, F, Lekkas, A, Greisch, J-F, Eijkel, GB, Anthony, IGM, Fort, K , Heck, AJR, Papanastasiou, D, Makarov, AA, Ellis, SR & Heeren, RMA 2023, 'An Orbitrap/Time-of-Flight Mass Spectrometer for Photofragment Ion Imaging and High-Resolution Mass Analysis of Native Macromolecular Assemblies', Journal of the American Society for Mass Spectrometry, vol. 34, no. 7, pp. 1359-1371. https://doi.org/10.1021/jasms.3c00053

An Orbitrap/Time-of-Flight Mass Spectrometer for Photofragment Ion Imaging and High-Resolution Mass Analysis of Native Macromolecular Assemblies. / Mathew, Anjusha; Giskes, Frans; Lekkas, Alexandros et al.
In: Journal of the American Society for Mass Spectrometry, Vol. 34, No. 7, 05.07.2023, p. 1359-1371.

Research output: Contribution to journal › Article › Academic › peer-review

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AU - Papanastasiou, Dimitris

AU - Makarov, Alexander A

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KW - macromolecular assemblies

KW - orthogonal time-of-flight mass spectrometry

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

Abstract

Bibliographical note

Funding

Keywords

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