Direct Analysis of Ion-Induced Peptide Fragmentation in Secondary-Ion Mass Spectrometry

Schneider, Pascal; Verloh, Felix; Portz, André; Aoyagi, Satoka; Rohnke, Marcus; Dürr, Michael

doi:10.1021/acs.analchem.0c03765

Cited by 8 publications

(12 citation statements)

References 47 publications

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“…With the employment of large noble gas cluster primary ions for much softer sputtering, depth-profiling of polymers has been achieved without signal loss during the measurement . Due to the high sputter yield of cluster ions in combination with the localization of primary-ion induced damage at the surface, the material altered by one cluster impact is removed by the next cluster impact at a given site, thus significant damage accumulation and cross-linking does not occur . However, primary ion induced fragmentation is still observed, different from desorption/ionization induced by neutral, low-energy SO 2 clusters as employed in our study.…”

Section: Resultsmentioning

confidence: 99%

“…As the detailed molecular properties of the polymer molecules determine the electrical and optical properties of these devices, sample characterization is a crucial step for both research and production purposes, thus making a powerful analytical tool mandatory. Secondary-ion mass spectrometry (SIMS) is a widespread method for the characterization of solid samples of polymers and organic materials in general; however, it typically comes with significant fragmentation induced by the primary ions. − While this can be an advantage, e.g., for identification of larger molecules or for depth profiling of polymer samples, − characterization of sample properties like the mass distribution of the smaller molecules will benefit from a nondestructive approach.…”

Section: Introductionmentioning

confidence: 99%

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Cluster-Induced Desorption/Ionization of Polystyrene: Desorption Mechanism and Effect of Polymer Chain Length on Desorption Probability

Schneider

Verloh

Dürr

2022

J. Am. Soc. Mass Spectrom.

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Soft cluster-induced desorption/ionization of polystyrene oligomers was investigated with respect to application in mass spectrometry. Clear peak progressions corresponding to intact polystyrene molecules were observed in the mass spectra, and no fragmentation was detected; efficient desorption was deduced from quartz crystal microbalance measurements. Molecular dynamics (MD) simulations of the process revealed that even in the case of the nonpolar polystyrene molecules cluster-induced desorption proceeds via dissolvation in the polar clusters. Experimentally, a significantly lower desorption efficiency was observed for polystyrene molecules with larger chain length. Taking into account MD simulations and further experiments with mixed samples consisting of long- and short-chain polystyrene oligomers, the reduced desorption efficiency for longer chain polystyrene molecules was attributed to a stronger entanglement of the larger polystyrene molecules.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Cluster-Induced Desorption/Ionization of Polystyrene: Desorption Mechanism and Effect of Polymer Chain Length on Desorption Probability

Schneider

Verloh

Dürr

2022

J. Am. Soc. Mass Spectrom.

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“…The impurity levels were measured in advance with a magnetic‐sector‐type dynamic‐SIMS using the raster change method 11,12 . The concentrations of carbon, oxygen, hydrogen, and nitrogen were 2 × 10, 15 3 × 10, 15 less than 6 × 10, 15 and less than 2 × 10 14 atoms/cm 3 , respectively. Depth profiling done using dynamic‐SIMS confirmed that the depth‐wise distribution of these elements was uniform and that aggregation had not occurred.…”

Section: Methodsmentioning

confidence: 99%

“…Related to dynamic‐SIMS, time‐of‐flight (TOF)‐SIMS has been employed as a unique analytical technique for chemical as well as elemental characterization at the sample surface. Furthermore, combining sputtering ion beams, such as Ar + , O 2 + , and Cs + , and gas cluster ion beams (GCIB) has enabled depth profiling, and these methods have been used for both inorganic and organic materials 13–16 . TOF‐SIMS has the advantage of qualitative analysis with a higher lateral resolution than dynamic‐SIMS.…”

Section: Introductionmentioning

confidence: 99%

Behavior and process of background signal formation of hydrogen, carbon, nitrogen, and oxygen in silicon wafers during depth profiling using dual‐beam TOF‐SIMS

Sameshima

Numao

2021

Surface & Interface Analysis

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The behavior and mechanism of background signals during depth profiling of atmospheric elements using dual‐beam time‐of‐flight secondary ion mass spectrometry (TOF‐SIMS) have been experimentally investigated for silicon wafers. The background signals of atmospheric elements were found to be inversely proportional to the sputtering rate. Most of the background signals are largely attributable to the accumulation of components through adsorption and ion bombardment in the pre‐equilibrium state. On the other hand, the contribution of real‐time adsorption during the instant after the last sputtering in the equilibrium state is negligible under the present experimental conditions. H2O is dominant in the background formation process of hydrogen and oxygen, which is supported by the higher adsorption coefficients. The background levels of carbon and nitrogen are lower than those of hydrogen and oxygen. Furthermore, the background signal of carbon with respect to the sputtering rate shows a different trend than the other elements. This could be attributed to accumulation in the pre‐equilibrium state. These results indicate that the background levels can be lowered close to those of dynamic‐SIMS by using an extremely high sputtering rate in dual‐beam TOF‐SIMS.

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“…(ii) How are the internal energy and the conformation of the molecules influenced by the desorption conditions (cluster size, energy, incidence angle, etc. 12 )? (iii) Would much larger clusters or clusters with a different chemistry be more appropriate to transfer "cool" molecules (thereby preserving their initial conformation)?…”

Section: Introductionmentioning

confidence: 99%

A Microscopic View of Macromolecule Transfer in the Vacuum Using Gas and Bismuth Clusters

Delcorte

2022

J. Phys. Chem. C

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Transferring large nonvolatile molecules in the vacuum is key to both their characterization by mass spectrometry (ion mobility, etc.) and their use as nanofabrication building blocks in soft-landing-type experiments. Recently, our group performed the successful transfer and redeposition of intact and bioactive lysozyme (14 kDa) with large gas cluster ion beams, in the absence of a solvent or matrix, demonstrating that such beams could serve as tools for macromolecule manipulation. A number of fundamental questions arose in relation with this experimental proof-of-concept, concerning for instance the maximum molecular size for successful transfer, the effect of the cluster projectile incidence angle, the dependence of molecular dissociation on the projectile energy and size, the internal energy uptake ultimately leading to metastable decay reactions, or the influence of the surface interactions on desorption. To address these questions, a series of molecular dynamics simulations were conducted involving cluster impacts on an adsorbed globular polystyrene (PS) macromolecule of 60 kDa, with a mass and shape comparable to those of a protein such as bovine serum albumin. Conditions of intact desorption of this PS molecule by Ar clusters are identified, in terms of energy per atom and incidence angle, and the results are compared to 30 keV Bi5 impacts, commonly used for molecular analysis and 2D imaging in our time-of-flight secondary ion mass spectrometry experiments. When Ar cluster impact conditions are appropriate for intact desorption, the take-off angle of the macromolecule is larger than the projectile incidence. Bombardment by a massive methane projectile (6.6 × 104 methane molecules) does not induce qualitatively different results, and in general, the energy per atom or energy per unit mass remains the deciding factor concerning the survival or dissociation of the bombarded molecule. In contrast with large gas clusters, Bi5 projectiles largely fail at desorbing the intact macromolecules, because of the detrimental effect of the collision cascade and the insufficient momentum transferred by the crater expansion for molecular lift off. Additionally, 10 keV Ar5000 projectiles with 45–75° incidence with respect to the surface normal directly transfer momentum to the macromolecule via their backscattered Ar atoms and small clusters, inducing molecular desorption with center-of-mass velocities of the order of 1 km/s. The implications for future experiments are discussed.

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Direct Analysis of Ion-Induced Peptide Fragmentation in Secondary-Ion Mass Spectrometry

Cited by 8 publications

References 47 publications

Cluster-Induced Desorption/Ionization of Polystyrene: Desorption Mechanism and Effect of Polymer Chain Length on Desorption Probability

Cluster-Induced Desorption/Ionization of Polystyrene: Desorption Mechanism and Effect of Polymer Chain Length on Desorption Probability

Behavior and process of background signal formation of hydrogen, carbon, nitrogen, and oxygen in silicon wafers during depth profiling using dual‐beam TOF‐SIMS

A Microscopic View of Macromolecule Transfer in the Vacuum Using Gas and Bismuth Clusters

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