Matrix-assisted ultraviolet laser desorption of non-volatile compounds

doi:10.1016/0168-1176(87)87041-6

International Journal of Mass Spectrometry and Ion Processes

Volume 78, 24 September 1987, Pages 53-68

International Journa...

https://doi.org/10.1016/0168-1176(87)87041-6 Get rights and content

Abstract

The use of a matrix for pulsed ultraviolet laser desorption mass spectrometry is shown to extend its applicability into the range of larger, thermally labile biomolecules. The matrix compounds tested show strong resonance absorption at the laser wavelength of 266 nm and can be either solid or liquid. Characteristic features of the matrix-assisted LD mass spectra are high quasimolecular ion yield with little or no fragmentation and only a few signals in the low mass range. The matrix effect is discussed in the light of three possible mechanisms: an effective and controllable energy transfer of the laser energy to the condensed phase by predominantly one-photon absorption, the creation of a uniform and soft disintegration of the condensed phase at moderate irradiances independent of the analyte's individual properties, and an enhancement of ionization yield by protonation via excited state molecules.

References (29)

G.J.Q. Van der Peyl et al.
Int. J. Mass Spectrom. Ion Phys.
(1982)
C.L. Wilkins et al.
Int. J. Mass Spectrom. Ion Processes
(1986)
P. Feigl et al.
Int. J. Mass Spectrom. Ion Phys.
(1983)
T.M. Barlak et al.
Int. J. Mass Spectrom. Ion Phys.
(1983)
I. Katakuse et al.
Int. J. Mass Spectrom. Ion Processes
(1984)
J.F. Ireland et al.
M. Barber et al.
Anal. Chem.
(1982)
J.L. Gower
Biomed. Mass Spectrom.
(1985)
A. Benninghoven et al.
Anal. Chem.
(1978)
J.-C. Tabet et al.
Anal. Chem.
(1984)

R.B. van Breemen et al.

Biomed. Mass Spectrom.

(1984)

R. Stoll et al.

Z. Naturforsch. Teil A

(1982)

D.M. Hercules et al.

Anal. Chem.

(1982)

E.D. Hardin et al.

Anal. Chem.

(1983)

Cited by (1760)

Pulsed laser ablation synthesis of fresh Te nanoparticles for matrix assisted laser desorption/ionization mass spectrometry (MALDI-MS) applications
2024, Talanta
This work aims to demonstrate the potential of pulsed laser ablation synthesis (PLA) of tellurium nanoparticles (Te NPs) for use in matrix assisted laser desorption/ionization mass spectrometry (MALDI-MS) applications. An experimental laboratory setup for PLA synthesis of fresh Te NPs was designed to prevent unwanted aggregation of uncoated Te NPs and avoid the need to use additional modifiers. Performing pulsed laser ablation synthesis in liquid (PLAL) using acetone was found to be the optimal way of preparing Te NPs. Another possibility is to use commercially available laser ablation devices for laser ablation – inductively coupled plasma mass spectrometry (LA-ICP-MS) to perform PLA in a helium atmosphere, but this approach is less efficient and results in the formation of unwanted larger particles.
The prepared Te NPs were studied using the transmission electron microscopy (TEM) and dynamic light scattering (DLS) methods. TEM images showed the formation of Te NP nanochains composed of many crystallized Te NPs with sizes ranging from 8 to 15 nm. The various size distributions of the synthesized Te NPs identified using the DLS method correspond to the size distributions of aggregations rather than individual Te NPs. The synthesized Te NPs were used for a pilot study of their possible use with the MALDI-MS technique. An important effect was observed when Te NPs were used to perform a MALDI-MS analysis of the α-cyclodextrin (α-CD) and cucurbit[7]uril (CB7) macrocycles, which consisted in a decline in the formation of matrix adducts. Furthermore, several changes in MALDI-MS mass spectra of intact cells and a positive effect of Te NPs on the crystallization of the MALDI-MS matrix were observed.
Strategies for MALDI-MS method development to investigate different pharmaceutical drug modalities
2023, International Journal of Mass Spectrometry
High-throughput screening (HTS) is an ultra-high throughput tool that allows the identification of diverse, pharmaceutically active compounds in the early stages of drug discovery, by enabling chemists to screen reactions at micromole/nanomole scales. To eliminate the bottleneck arising from analysis of large libraries, Matrix Assisted Laser Desorption Ionization Mass Spectrometry (MALDI-MS) can be utilized as a compatible, ultra-fast, label-free, analysis tool. Upon integrating this technique with suitable liquid handling robots that can accurately spot matrices and analytes on a MALDI plate, chemical reactions can be screened at a sampling rate of <1 s per sample. While earlier efforts to improve MALDI-HTS applications were geared towards the development of automation and data processing tools, a systematic method development study across different drug modalities was needed to understand the contribution of different parameters such as MALDI matrices, choice of matrices, additives, and solvent composition, on MALDI-MS signal intensities of analytes. The current study will demonstrate the importance of initial MALDI-MS method development on small molecules, peptides, antibodies, and antibody drug conjugates. This study is designed as a starting point for MALDI-MS signal optimization, which can eventually lead to the development of effective MALDI-HTS methods for various modalities, thus paving the way for a wide range of applications, including but not limited to conformational analysis.
Advances in mass spectrometry-based multi-scale metabolomic methodologies and their applications in biological and clinical investigations
2023, Science Bulletin
Metabolomics is a nascent field of inquiry that emerged in the late 20th century. It encompasses the comprehensive profiling of metabolites across a spectrum of organisms, ranging from bacteria and cells to tissues. The rapid evolution of analytical methods and data analysis has greatly accelerated progress in this dynamic discipline over recent decades. Sophisticated techniques such as liquid chromatograph mass spectrometry (MS), gas chromatograph MS, capillary electrophoresis MS, and nuclear magnetic resonance serve as the cornerstone of metabolomic analysis. Building upon these methods, a plethora of modifications and combinations have emerged to propel the advancement of metabolomics. Despite this progress, scrutinizing metabolism at the single-cell or single-organelle level remains an arduous task over the decades. Some of the most thrilling advancements, such as single-cell and single-organelle metabolic profiling techniques, offer profound insights into the intricate mechanisms within cells and organelles. This allows for a comprehensive study of metabolic heterogeneity and its pivotal role in multiple biological processes. The progress made in MS imaging has enabled high-resolution in situ metabolic profiling of tissue sections and even individual cells. Spatial reconstruction techniques enable the direct representation of metabolic distribution and alteration in three-dimensional space. The application of novel metabolomic techniques has led to significant breakthroughs in biological and clinical studies, including the discovery of novel metabolic pathways, determination of cell fate in differentiation, anti-aging intervention through modulating metabolism, metabolomics-based clinicopathologic analysis, and surgical decision-making based on on-site intraoperative metabolic analysis. This review presents a comprehensive overview of both conventional and innovative metabolomic techniques, highlighting their applications in groundbreaking biological and clinical studies.
Laser desorption/ionization-mass spectrometry for the analysis of interphases in lithium ion batteries
2023, iScience
Laser desorption/ionization-mass spectrometry (LDI-MS) is introduced as a complementary technique for the analysis of interphases formed at electrode|electrolyte interfaces in lithium ion batteries (LIBs). An understanding of these interphases is crucial for designing interphase-forming electrolyte formulations and increasing battery lifetime. Especially organic species are analyzed more effectively using LDI-MS than with established methodologies. The combination with trapped ion mobility spectrometry and tandem mass spectrometry yields additional structural information of interphase components. Furthermore, LDI-MS imaging reveals the lateral distribution of compounds on the electrode surface. Using the introduced methods, a deeper understanding of the mechanism of action of the established solid electrolyte interphase-forming electrolyte additive 3,4-dimethyloxazolidine-2,5-dione (Ala-N-CA) for silicon/graphite anodes is obtained, and active electrochemical transformation products are unambiguously identified. In the future, LDI-MS will help to provide a deeper understanding of interfacial processes in LIBs by using it in a multimodal approach with other surface analysis methods to obtain complementary information.
Ionization detection of neutral 2,5-dihydroxy benzoic acid molecules in the matrix-assisted laser desorption/ionization plume by ultraviolet laser post-ionization: Correlation between internal energy distribution and thermal decomposition rate
2023, International Journal of Mass Spectrometry
We probed neutral 2,5-dihydroxy benzoic acid (DHB) crystals in the matrix-assisted laser desorption/ionization (MALDI) plume using ultraviolet (UV) laser post-ionization at 266 nm to investigate the initial MALDI process involving fast phase transitions. Mainly three ion signals, DHB⁺, [DHB–H₂O]⁺ produced by the dissociative ionization of neutral DHB, and [DHB–CO₂]⁺ formed by pyrolysis in the dense plume, were detected using time-of-flight mass spectrometry. The [DHB–H₂O]⁺/DHB⁺ ratio was utilized as the fraction of highly excited neutral DHB molecules produced by photoexcitation and survived after phase explosion, and the [DHB–CO₂]⁺/DHB⁺ ratio indicated the extent of pyrolysis of neutral DHB molecules in the thermally heated condensed phase before phase explosion. The two indexes showed an inverse relationship with respect to the laser delay corresponding to the position in the plume, i.e., the [DHB–H₂O]⁺/DHB⁺ ratio revealed high values at the tip of the plume, whereas the [DHB–CO₂]⁺/DHB⁺ ratio increased in the rear part of the plume, reflecting the molecular dynamics of solid-to-gas phase transition involving the production of most MALDI analyte ions.
Gas chromatography-mass spectrometry and liquid chromatography-mass spectrometry metabolomics platforms: Tools for plant oligosaccharides analysis
2023, Carbohydrate Polymer Technologies and Applications
Oligosaccharides play a central role in plants and are involved in basal metabolism, and many other functions at cellular levels. Indeed, oligosaccharides analysis was stimulated by the development of analytical chemistry and computational biology and bioinformatics. The last decades have been marked by spectacular developments of metabolomics platforms, and gas or liquid chromatography coupled with mass spectrometer (GC-MS, LC-MS, UPLC-MS) or tandem mass spectrometer (GC-MS/MS, LC-MS/MS) became key technologies for the identification and quantification of oligosaccharides in plants. Oligosaccharides are mostly extracted using aqueous ethanol followed by successive hot water. GC is often used for quantification but it requires chemical derivatization prior to the analysis, making GC less attractive, compared to LC which is more efficient in the identification and quantification of oligosaccharides. Coupled with MS, these analytical techniques expanded further oligosaccharides analysis, and with the development of metabolomics raw data were transformed into decipherable ones, and further information on oligosaccharides and their anomeric forms were provided. However, these technologies showed some limits due to the huge amount of data generated and their processing. Thus, developing new methods, improvements in sample preparation and creation of chemical libraries will offer deeper insights into the spatio-temporal study of oligosaccharides in plants.

View all citing articles on Scopus

View full text

Matrix-assisted ultraviolet laser desorption of non-volatile compounds

Abstract

Int. J. Mass Spectrom. Ion Phys.

Int. J. Mass Spectrom. Ion Processes

Int. J. Mass Spectrom. Ion Phys.

Int. J. Mass Spectrom. Ion Phys.

Int. J. Mass Spectrom. Ion Processes

Anal. Chem.

Biomed. Mass Spectrom.

Anal. Chem.

Anal. Chem.

Biomed. Mass Spectrom.

Z. Naturforsch. Teil A

Anal. Chem.

Anal. Chem.