Quantification of the ionization probability during desorption/ionization of oligopeptides induced by neutral cluster impact

Lee, B.-J.; Baur, Markus; Gebhardt, Christoph; Dürr, Michael

doi:10.1002/rcm.6550

Cited by 20 publications

(18 citation statements)

References 32 publications

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“…Although we have shown that the ionization probability of a given analyte molecule is not strongly influenced by the presence of co-adsorbates or co-constituents in mixed samples 17,24 , the ionization probability may vary from substance to substance 13 . Thus, it is even more important to work under clean conditions as contaminants, depending on their ionization probability, may contribute to the signal much stronger than the analyte.…”

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confidence: 78%

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Analysis of Complex Molecules and Their Reactions on Surfaces by Means of Cluster-Induced Desorption/Ionization Mass Spectrometry

Bomhardt

Schneider

Portz

et al. 2020

JoVE

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Desorption/Ionization Induced by Neutral SO 2 Clusters (DINeC) is employed as a very soft and efficient desorption/ionization technique for mass spectrometry (MS) of complex molecules and their reactions on surfaces. DINeC is based on a beam of SO 2 clusters impacting on the sample surface at low cluster energy. During cluster-surface impact, some of the surface molecules are desorbed and ionized via dissolvation in the impacting cluster; as a result of this dissolvation-mediated desorption mechanism, low cluster energy is sufficient and the desorption process is extremely soft. Both surface adsorbates and molecules of which the surface is composed of can be analyzed. Clear and fragmentationfree spectra from complex molecules such as peptides and proteins are obtained. DINeC does not require any special sample preparation, in particular no matrix has to be applied. The method yields quantitative information on the composition of the samples; molecules at a surface coverage as low as 0.1 % of a monolayer can be detected. Surface reactions such as H/D exchange or thermal decomposition can be observed in real-time and the kinetics of the reactions can be deduced. Using a pulsed nozzle for cluster beam generation, DINeC can be efficiently combined with ion trap mass spectrometry. The matrix-free and soft nature of the DINeC process in combination with the MS n capabilities of the ion trap allows for very detailed and unambiguous analysis of the chemical composition of complex organic samples and organic adsorbates on surfaces. Video Link The video component of this article can be found at https://www.jove.com/video/60487/ 11,12,13,14,15,16,17. DINeC is based on a beam of molecular clusters which consist of 10 3 to 10 4 SO 2 molecules (Figure 1). When the clusters impact on the sample, they interact in various ways with the molecules on and in the surface: first, a part of the cluster's kinetic energy is redistributed and activates desorption. Similarly

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confidence: 78%

“…. The latter can act as an efficient proton source which further promotes the ionization process in case of ionization via proton uptake (positive ion mode) 13,18 .…”

mentioning

confidence: 99%

Analysis of Complex Molecules and Their Reactions on Surfaces by Means of Cluster-Induced Desorption/Ionization Mass Spectrometry

Bomhardt

Schneider

Portz

et al. 2020

JoVE

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“…Thus, the proposed formation of H 2 SO 3 from SO 2 in the cluster and H 2 O in the film seems to be plausible and the resulting increase in H 3 O + concentration might explain the predominance of the cations as well as the observed ionization efficiency. [9,11] Further experiments are necessary to clarify the desorption/ionization mechanism in more detail.…”

Section: Discussionmentioning

confidence: 99%

“…[5][6][7][8] In contrast to the techniques using charged (non-reactive) primary particles, we have recently shown that a beam of neutral SO 2 clusters can also be employed for very soft and matrix-free desorption and ionization of oligopeptides. [9][10][11] With the high dipole moment of the SO 2 molecules (1.6 debye), the impacting SO 2 clusters do not only provide the energy necessary for the desorption, but also serve as a transient matrix in which the desorbing molecule is dissolved during the desorption process; as a consequence desorption takes place at comparably low cluster energies (<1 eV/molecule). Shattering of the cluster during and after surface impact then leads to a rapid redistribution of the system's energy thus avoiding heating and fragmentation of the desorbing molecules.…”

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confidence: 99%

Desorption/ionization induced by neutral cluster impact as a soft and efficient ionization source for ion trap mass spectrometry of biomolecules

Baur

Gebhardt

Dürr

2013

Rapid Comm Mass Spectrometry

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Desorption and ionization induced by neutral clusters can efficiently be combined with ion trap mass spectrometry since the pulse width and repetition rate of a typical pulsed cluster beam correspond well to the discontinuous accumulation time as well as the spectral rate of the ion trap. Clear mass spectra were obtained with such a setup for a variety of biosamples demonstrating the wider applicability of the DINeC process.

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“…27 This is approximately 2 orders of magnitude greater than our numbers when our UY values are corrected for an estimated 10% overall efficiency of transmission and detection in our instrument. It would be good to determine useful yield values for massresolved ion species in the Gebhardt approach.…”

Section: Analytical Chemistrymentioning

confidence: 93%

Mass Spectra and Yields of Intact Charged Biomolecules Ejected by Massive Cluster Impact for Bioimaging in a Time-of-Flight Secondary Ion Microscope

et al. 2015

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Impacts of massive, highly charged glycerol clusters (≳10(6) Da, ≳ ± 100 charges) have been used to eject intact charged molecules of peptides, lipids, and small proteins from pure solid samples, enabling imaging using these ion species in a time-of-flight secondary ion microscope with few-micrometer spatial resolution. Here, we report mass spectra and useful ion yields (ratio of intact charged molecules detected to molecules sputtered) for several molecular species-two peptides, bradykinin and angiotensin II; two lipids, phosphatidylcholine and sphingomyelin; Irganox 1010 (a detergent); insulin; and rhodamine B-and show that useful ion yields are high enough to enable bioimaging of peptides and lipids in biological samples with few-micrometer resolution and acceptable signals. For example, several hundred molecular ion counts should be detectable from a 3 × 3 μm(2) area of a pure lipid bilayer given appropriate instrumentation or tens of counts from a minor constituent of such a layer.

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Quantification of the ionization probability during desorption/ionization of oligopeptides induced by neutral cluster impact

Cited by 20 publications

References 32 publications

Analysis of Complex Molecules and Their Reactions on Surfaces by Means of Cluster-Induced Desorption/Ionization Mass Spectrometry

Analysis of Complex Molecules and Their Reactions on Surfaces by Means of Cluster-Induced Desorption/Ionization Mass Spectrometry

Desorption/ionization induced by neutral cluster impact as a soft and efficient ionization source for ion trap mass spectrometry of biomolecules

Mass Spectra and Yields of Intact Charged Biomolecules Ejected by Massive Cluster Impact for Bioimaging in a Time-of-Flight Secondary Ion Microscope

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