Multi-mass velocity-map imaging studies of photoinduced and electron-induced chemistry

Vallance, Claire

doi:10.1039/c9cc02426c

Cited by 11 publications

(11 citation statements)

References 115 publications

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“…This work supports previous studies highlighting the utility of the TPX detector, and other similar detectors such as pixel imaging mass spectrometry (PImMS) camera for simultaneously imaging of ions with different arrival times and for studying ion optical processes. , Active pixel detectors are demonstrated to offer significant advantages over traditional charge-coupled-device-based approaches that are widely used in ion imaging applications such as velocity map imaging. , …”

Section: Discussionsupporting

confidence: 85%

Ion Imaging of Native Protein Complexes Using Orthogonal Time-of-Flight Mass Spectrometry and a Timepix Detector

Mathew

Buijs

Eijkel

et al. 2021

J. Am. Soc. Mass Spectrom.

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Native mass spectrometry (native MS) has emerged as a powerful technique to study the structure and stoichiometry of large protein complexes. Traditionally, native MS has been performed on modified time-of-flight (TOF) systems combined with detectors that do not provide information on the arrival coordinates of each ion at the detector. In this study, we describe the implementation of a Timepix (TPX) pixelated detector on a modified orthogonal TOF (O-TOF) mass spectrometer for the analysis and imaging of native protein complexes. In this unique experimental setup, we have used the impact positions of the ions at the detector to visualize the effects of various ion optical parameters on the flight path of ions. We also demonstrate the ability to unambiguously detect and image individual ion events, providing the first report of single-ion imaging of protein complexes in native MS. Furthermore, the simultaneous space-and time-sensitive nature of the TPX detector was critical in the identification of the origin of an unexpected TOF signal. A signal that could easily be mistaken as a fragment of the protein complex was explicitly identified as a secondary electron signal arising from ion-surface collisions inside the TOF housing. This work significantly extends the mass range previously detected with the TPX and exemplifies the value of simultaneous space-and timeresolved detection in the study of ion optical processes and ion trajectories in TOF mass spectrometers.

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Section: Discussionsupporting

confidence: 85%

Ion Imaging of Native Protein Complexes Using Orthogonal Time-of-Flight Mass Spectrometry and a Timepix Detector

Mathew

Buijs

Eijkel

et al. 2021

J. Am. Soc. Mass Spectrom.

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Section: Three-dimensional Recoil-frame Covariance Mappingmentioning

confidence: 79%

“…It is also possible to generate three-dimensional covariance maps from a pair of three-dimensional velocity-map images recorded using slice imaging. 3D covariances of this type have been demonstrated recently by Vallance and coworkers , for various Coulomb explosion products of multiply charged CF 3 I ions. An example is shown in Figure , which shows 3D recoil-frame covariances for various subsets of the two-body dissociation products CF 3 + and I + .…”

Section: Covariance Mappingmentioning

confidence: 79%

“…These concerns proved to be unfounded, and there have since been many studies in which the photoproducts of significantly larger molecules have yielded highly structured, and therefore information-rich, images (see refs − for a few examples). In parallel with experimental developments such as multimass velocity-map imaging, dramatic increases in available computational power have made it possible to calculate at least reduced-dimensionality potential energy surfaces for much larger molecules than had been accessible previously. Taken together, these advances have made it possible to perform detailed gas-phase chemical physics studies on chemical systems of real-world interest to a broad audience of chemists.…”

Section: Introductionmentioning

confidence: 99%

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Covariance-Map Imaging: A Powerful Tool for Chemical Dynamics Studies

2021

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Over the past decade or so, the state-of-the-art in the eld of chemical reaction dynamics has progressed from studies of few-atom systems to wide-ranging investigations into a variety of photoinduced and collision-induced processes in much larger molecules. Many of these studies are of direct relevance to a wide audience of chemists, spanning elds such as atmospheric chemistry, astrochemistry, synthetic chemistry, and chemical biology. Key to this work has been the technique of velocity-map imaging, which allows complete product scattering distributions to be recorded for the process of interest. Recent advances in

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“…Recently-developed multi-mass velocity-map imaging approaches [10][11][12] have extended the technique to larger chemical systems by enabling detection of all products on each experimental cycle, an advance over earlier approaches in which only one species could be detected in a given experiment. In addition to substantial gains in data acquisition speed, multi-mass imaging also enables correlations to be uncovered between the scattering distributions of different reaction products, providing even more detailed information on the reaction mechanism.…”

mentioning

confidence: 99%

Three-dimensional covariance-map imaging of molecular structure and dynamics on the ultrafast timescale

et al. 2020

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Ultrafast laser pump-probe methods allow chemical reactions to be followed in real time, and have provided unprecedented insight into fundamental aspects of chemical reactivity. While evolution of the electronic structure of the system under study is evident from changes in the observed spectral signatures, information on rearrangement of the nuclear framework is generally obtained indirectly. Disentangling contributions to the signal arising from competing photochemical pathways can also be challenging. Here we introduce the new technique of three-dimensional covariance-map Coulomb explosion imaging, which has the potential to provide complete three-dimensional information on molecular structure and dynamics as they evolve in real time during a gas-phase chemical reaction. We present first proof-of-concept data from recent measurements on CF3I. Our approach allows the contributions from competing fragmentation pathways to be isolated and characterised unambiguously, and is a promising route to enabling the recording of ‘molecular movies’ for a wide variety of gas-phase chemical processes.

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Multi-mass velocity-map imaging studies of photoinduced and electron-induced chemistry

Abstract: Multimass velocity-map imaging promises new mechanistic insights into chemistry relevant to fields ranging from atmospheric chemistry and astrochemistry through to synthetic organic photochemistry and biology.

Cited by 11 publications

References 115 publications

Ion Imaging of Native Protein Complexes Using Orthogonal Time-of-Flight Mass Spectrometry and a Timepix Detector

Ion Imaging of Native Protein Complexes Using Orthogonal Time-of-Flight Mass Spectrometry and a Timepix Detector

Covariance-Map Imaging: A Powerful Tool for Chemical Dynamics Studies

Three-dimensional covariance-map imaging of molecular structure and dynamics on the ultrafast timescale

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