Alain Brunelle

Alain Brunelle
French National Centre for Scientific Research | CNRS · Laboratoire d'Archéologie Moléculaire et Structurale LAMS UMR 8220 CNRS Sorbonne University

PhD, HDR

About

217
Publications
39,285
Reads
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7,115
Citations
Citations since 2017
40 Research Items
2595 Citations
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20172018201920202021202220230100200300400
20172018201920202021202220230100200300400
Introduction
From 1988 to 2002, my main research subject was the study of the interactions of energetic particles (ions, clusters, molecules, photons) with matter. From 2002 to 2018 at the ICSN in Gif-sur-Yvette, in charge of a project of biological imaging by mass spectrometry by cluster-TOF-SIMS and MALDI-TOF. From 2010 to 2018, Head of Mass Spectrometry Group at ICSN-CNRS. Since 2019, new project at the Laboratoire d'Archéologie Moléculaire et Structurale (LAMS UMR8220, CNRS, Sorbonne Université, Paris) to study cultural heritage samples like old paintings, by submicrometric and 3D TOF-SIMS
Additional affiliations
September 2002 - present
French National Centre for Scientific Research
Position
  • Research Director
September 1988 - August 2002
French National Centre for Scientific Research
Position
  • Research Associate

Publications

Publications (217)
Article
Time-of-flight secondary ion mass spectrometry (TOF-SIMS) imaging is a surface analysis technique that identifies and spatially resolves the chemical composition of a sample with a lateral resolution of less than 1 μm. Depth analyses can also be performed over thicknesses of several microns. In the case of a painting cross section, for example, TOF...
Chapter
Over the past couple of years, imaging mass spectrometry (IMS) has arisen as a powerful tool to answer research questions in the biomedical field. Imaging mass spectrometry allows for label-free chemical imaging by providing full molecular information. The IMS technique best positioned for cell and tissue analysis is time-of-flight secondary ion ma...
Article
The material evidence for the wax finish on ancient marble statues, known as ganosis, is scarce and controversial, although Greek and Latin sources describe the recipes and cultural value of this treatment. The surface treatment of a colossal Roman head from the Roman theatre of Dougga (Tunisia), dated to the end of the second century CE, is studie...
Article
The two paintings Infant Bacchanals (Museo Nazionale d'Arte Antica, Palazzo Barberini, Rome, Italy) executed by Nicolas Poussin (Les Andelys, 1594-Rome, 1665) in around 1626 are thought to have been painted "a guazzo", which means either with a glue or with an egg binding medium. To date, this has never been confirmed through analysis. Dual-beam ti...
Article
Full-text available
Molecular imaging has the potential to unearth important spatial and temporal relationships in biological systems, including intercellular signaling as well as environmentally-cued morphological changes. Various chemical imaging techniques show functional groups, molecular weights, etc., but no individual technique to date has the ability to simult...
Article
Ion signal detection at the true (unperturbed) cyclotron frequency instead of the conventional reduced cyclotron frequency has remained a formidable challenge since the inception of Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). Recently, routine FT-ICR MS at the true cyclotron frequency has become a reality with the imple...
Article
Resolving Internal Structures and Composition of Biominerals: The Case of Calcitic Prisms of Mollusk Shells - Yannicke Dauphin, Jean-Pierre Cuif, Alain Brunelle, Kadda Medjoubi, Murielle Salomé, Andrea Somogyi
Article
Full-text available
Pulmonary arterial hypertension (PAH) is a rare and deadly disease affecting roughly 15-60 people per million in Europe with a poorly understood pathology. There are currently no diagnostic tools for early detection nor does a curative treatment exist. The lipid composition of arteries in lung tissue samples from human PAH and control patients were...
Article
Full-text available
Lipid disorders have been associated with glomerulopathies, a distinct type of renal pathologies, such as nephrotic syndrome. Global analyses targeting kidney lipids in this pathophysiologic context have been extensively performed, but most often regardless of the architectural and functional complexity of the kidney. The new developments in mass s...
Article
Full-text available
Molecular analysis by parallel tandem mass spectrometry (MS/MS) imaging contributes to the in situ characterization of biosynthetic intermediates which is crucial for deciphering the metabolic pathways in living organisms. We report the first use of TOF-SIMS MS/MS imaging for the cellular localization and characterization of biosynthetic intermedia...
Article
Full-text available
Full-text access to a view-only version : https://rdcu.be/bbLU7 Abiotic hydrocarbons and carboxylic acids are known to be formed on Earth, notably during the hydrothermal alteration of mantle rocks. Although the abiotic formation of amino acids has been predicted both from experimental studies and thermodynamic calculations, its occurrence has n...
Article
The emission/ionization process under massive argon cluster bombardment was investigated by measuring the internal energy distributions of a series of benzylpyridinium ions. Argon clusters with kinetic energies between 10 and 20 keV and cluster sizes ranging from 500 to 10,000 were used to establish the influence of their size, energy, and velocity...
Article
Full-text available
The prismatic layer of Pinna (Mollusca) is one of the most studied models for the understanding of the biomineralization mechanisms, but our knowledge of the organic components of this layer is limited to the proteins of the soluble organic matrices. The interplay of the mineral and organic matrices is studied using scanning electron and atomic for...
Article
Wood extractives in the xylem of European larch Larix decidua were mapped by time-of-flight secondary ion mass spectrometry (TOF-SIMS) imaging, which allows the radial distribution of both mineral and lipophilic extractives in the xylem to be scrutinized with high spatial resolution for the first time. Results show that all the components are inhom...
Article
Driven by a necessity for confident molecular identification at high spatial resolution, a new time-of-flight secondary ion mass spectrometry (TOF-SIMS) tandem mass spectrometry (tandem MS) imaging instrument has been recently developed. In this report, the superior MS/MS spectrometry and imaging capability of this new tool is shown for natural pro...
Article
Imaging mass spectrometry (IMS) has become a powerful tool to characterise the spatial distribution of biomolecules in thin tissue sections. In the case of matrix-assisted laser desorption ionisation (MALDI) IMS, homogeneous matrix deposition is critical to produce high quality ion images and sublimation in particular has shown to be an excellent m...
Article
Full-text available
An integrative approach combining traditional natural products chemistry, molecular networking, and mass spectrometry imaging has been undertaken to decipher the molecular dialogue between the fungus Paraconiothyrium variabile and the bacterium Bacillus subtilis, which were isolated as endophytes from the conifer Cephalotaxus harringtonia and are c...
Article
Full-text available
Rationale: Mass spectrometry imaging (MSI) is a powerful tool for mapping the surface of a sample. Time-of-flight secondary ion mass spectrometry (TOF-SIMS) and atmospheric pressure matrix-assisted laser desorption/ionization (AP-MALDI) offer complementary capabilities. Here, we present a workflow to apply both techniques to a single tissue sectio...
Article
Full-text available
A supercritical fluid chromatography-based targeted purification procedure using tandem mass spectrometry and molecular networking was developed to analyze, annotate, and isolate secondary metabolites from complex plant extract mixture. This approach was applied for the targeted isolation of new antiviral diterpene esters from Euphorbia semiperfoli...
Article
Full-text available
Natural oils are commonly used in topical pharmaceutical formulations as emulsifiers, stabilizers or solubility enhancers. They are presented as safe and inert components, mainly used for formulation purposes. It is confirmed that natural oils can affect the skin penetration of various substances. Fatty acids are mainly responsible for this effect....
Article
Using a time-of-flight secondary ion mass spectrometer equipped with an argon cluster ion for sputtering and a bismuth liquid metal ion source for analysis, both surfaces of leaves and fruits of Macaranga vedeliana, an endemic New Caledonian species have been for the first time analyzed by a dual beam depth profiling. To prevent in-vacuum evaporati...
Article
Introduction: Acetogenins are plant polyketides known to be cytotoxic and proposed as antitumor candidates. They are also suspected to be alimentary neurotoxins. Their occurrence as complex mixtures renders their dereplication and structural identification difficult using liquid chromatography coupled to tandem mass spectrometry and efforts are re...
Article
Full-text available
Nonalcoholic steatohepatitis (NASH) is a condition which can progress to cirrhosis and hepatocellular carcinoma. Markers for NASH diagnosis are still lacking. We performed a comprehensive lipidomic analysis on human liver biopsies including normal liver, nonalcoholic fatty liver and NASH. Random forests-based machine learning approach allowed chara...
Poster
Full-text available
This is a poster representing continuous collaborative work. We have showed the TOF-SIMS applicability for human skin penetration studies of dihydroquercetin incorporated into nano structured carriers.
Article
Full-text available
Linoleic, oleic, palmitoleic, palmitic, and stearic fatty acids (FAs) are commonly used in dermatological formulations. They differ by their structure, presence in the skin, and mode of application in pharmaceuticals and cosmetics compounding. These FAs are also known as chemical penetration enhancers, but their mechanisms of penetration enhancemen...
Preprint
Full-text available
A supercritical fluid chromatography-based targeted purification workflow using tandem mass spectrometry and molecular networking was developed to analyze, annotate and isolate secondary metabolites from complex mixture. This approach was applied for targeted isolation of new antiviral diterpene esters from Euphorbia semiperfoliata whole plant extr...
Article
The painting Rebecca and Eliezer at the Well, which hangs in the Fitzwilliam Museum, Cambridge, UK, is possibly one of the last figure painting executed by Nicolas Poussin at the very end of his life and is usually dated to the early 1660s. In this perspective special feature, Philippe Walter, Alain Brunelle and colleagues give new insights on the...
Article
Time-of-flight secondary ion mass spectrometry (TOF-SIMS) imaging using cluster primary ion beams is used for the identification of the pigments in the painting of Rebecca and Eliezer at the Well by Nicolas Poussin. The combination of the high mass resolution of the technique with a sub-micrometer spatial resolution offered by a delayed extraction...
Article
The preparation of tropical wood surface sections for time-of-flight secondary ion mass spectrometry imaging is described, and the use of delayed extraction of secondary ions and its interest for the analysis of vegetal surface are shown. The method has been applied to the study by time-of-flight secondary ion mass spectrometry imaging with a resol...
Article
Full-text available
Annonaceous acetogenins (AAGs) are environmental neurotoxins from the fruit pulp of several Annonaceae species, whose consumption was linked to the occurrence of sporadic atypical Parkinsonism with dementia. The quantification of the prototypical AAG annonacin in Rat brain homogenates was performed by UPLC-MS/MS in selected reaction monitoring (SRM...
Article
The Annonaceous acetogenin annonacin is an environmental neurotoxin identified in the pulp of several fruits of the Annonaceae family, whose consumption was linked to the occurrence of sporadic atypical Parkinsonism with dementia. A method for its quantification in Rat brain homogenates by UPLC-MS/MS in selected reaction monitoring (SRM) mode was d...
Conference Paper
Full-text available
The topical use of natural oils has been increasing each year and their effects on human health are being debated as controversial. Changes in skin barrier permeability profiles after application of fatty acids found in natural oils have been demonstrated. Current study is a continuum of previous research, when the effect of fatty acids to enhance...
Article
Annonacin is an environmental neurotoxin identified in the pulp of several fruits of the Annonaceae family (for example in Annona muricata, Asimina triloba), whose consumption was linked with the occurrence of sporadic atypical Parkinsonism with dementia. Pharmacokinetic parameters of this molecule are unknown. A method for its quantification in Ra...
Article
Since several decades, secondary ion mass spectrometry (SIMS) coupled to time of flight (TOF) is used for atomic or small inorganic/organic fragments imaging on different materials. With the advent of polyatomic ion sources leading to a significant increase of sensitivity in combination with a reasonable spatial resolution (1-10 μm), TOF-SIMS is be...
Conference Paper
Full-text available
The increasing topical use of natural oils can be related to controversial effects on human health. Skin penetration enhancing effects of fatty acids from natural oils have been demonstrated. This study continues previous research, when the effect of fatty acids to enhance tolnaftate dermal penetration has been evaluated, and a biological imaging T...
Article
Full-text available
RationaleIn Time-of-Flight Secondary Ion Mass Spectrometry (TOF-SIMS), pulsed and focused primary ion beams enable mass spectrometry imaging, a method which is particularly useful to map various small molecules such as lipids at the surface of biological samples. When using TOF-SIMS instruments, the focusing modes of the primary ion beam delivered...
Article
For the most effective analytical strategies, development and validation include optimization of such analytical variables as resolution, detectability, sensitivity, simplicity, cost effectiveness, flexibility, and speed. However, other aspects concerning operator safety and environmental impact are not considered at the same level. The result has...
Article
Mass spectrometry imaging has become a popular tool for probing the chemical complexity of biological surfaces. This led to the development of a wide range of instrumentation and preparation protocols. It is thus desirable to evaluate and compare the data output from different methodologies and mass spectrometers. Here, we present an approach for t...
Article
Matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI MSI) enables the localization and the structural identification of a large set of molecules on a surface with 10-20 μm resolution. MALDI is often coupled to time-of-flight (TOF) tandem analyzers which remain a versatile instrument for the detection and the structural analy...
Article
Intensive fragmentations into b/y- and c-sequence ions have been reported for Substance P ionized under dopant-assisted atmospheric pressure photoionization (APPI) conditions. It was postulated that the fragmentation comes from the reaction of the doubly charged peptide with photoelectrons, released upon photoionization of the dopant, through an el...
Article
Recent developments in instrumentation, ion beams or analyzers, for cluster time-of-flight secondary ion mass spectrometry (TOF-SIMS) imaging are described here. The methods which are employed to increase the sensitivity or to perform three-dimensional analyses in the organic materials are also illustrated. This review shows the improvements made f...
Article
The development of ‘omics’ sciences offers new opportunities for the study of neurodegenerative diseases but increases at the same time the sample demand on brain banks that collect and store valuable human post-mortem tissue. Our study aims to evaluate in lipidomics the potential of formalin-fixed tissue compared with the cryopreservation method,...
Article
Monoterpenes are the main class of biogenic volatile organic compounds. They promptly react with oxygen and nitrogen species, leading to the formation of secondary aerosols. The determination of their physicochemical properties, such as their ionization energies (IEs), is crucial to understand better their reactivity. We previously introduced a mod...
Article
Epidemiological and toxicological studies suggested Annonaceaeous acetogenins to be environmental neurotoxins responsible for sporadic atypical parkinsonism / dementia in tropical areas. These compounds are present in the tropical genus Annona (Annonaceae), known for its fruits-yielding cultivated species such as A. cherimolia. This species is wide...
Article
Full-text available
Cytochromes P450 (CYPs) play critical roles in oxidative metabolism of many endogenous and exogenous compounds. Protein expression levels of CYPs in liver provide relevant information for a better understanding of the importance of CYPs in pharmacology and toxicology. This work aimed at establishing a simple method to quantify six CYPs (CYP3A4, CYP...
Article
Full-text available
A new approach to treating Duchenne muscular dystrophy was investigated by using the ester or amide covalent association of arginine [nitric oxide (NO) pathway] and butyrate [histone deacetylase (HDAC) inhibition] in mdx mice and patient myotubes. Two prodrugs were synthesized, and the beneficial effects on dystrophic phenotype were studied. Nerve...
Article
Full-text available
Despite advances in neonatal intensive care leading to an increased survival rate in preterm infants, brain lesions and subsequent neurological handicaps following preterm birth remain a critical issue. To prevent brain injury and/or enhance repair, one of the most promising therapies investigated in preclinical models is inhaled nitric oxide (iNO)...
Article
Imaging by secondary ion mass spectrometry coupled to time-of-flight mass analysis (TOF-SIMS) is a method of which the applications have greatly increased since 10 years. Taking advantage of the development of cluster ion sources, TOF-SIMS offers images of molecular ions at a micrometer lateral resolution or slightly below and does not require comp...
Article
Despite advances in neonatal intensive care leading to an increased survival rate in preterm infants, brain lesions and subsequent neurological handicaps following preterm birth remain a critical issue. To prevent brain injury and/or enhance repair, one of the most promising therapies investigated in preclinical models is inhaled nitric oxide (iNO)...
Article
Full-text available
Parkinson's disease (PD) is the second most common neurodegenerative disorder affecting ~1 % of the population older than 60 years. The administration of the proneurotoxin 1-methyl-4-phenyl-1,2,3,6-tetrahydropyridine (MPTP) in mice is one of the most widely used approach to elucidate the mechanisms of cell death involved in PD. Its toxicity is attr...
Article
Liposoluble vitamins are widely analyzed due to their significant antioxidant activity. Quantification by liquid or gas chromatography is often time consuming and requires sample treatments prior to the analysis. Supercritical fluid chromatography (SFC), especially with the developments of new commercial systems, is nowadays considered as a credibl...
Article
Full-text available
Fatty acids classified as chemical penetration enhancers (CPEs) might cause the fluidization and perturbation of stratum corneum (SC) lipid matrix. The penetration of oleic, linoleic, lauric and capric acids into human skin was studied by time-of-flight secondary ion mass spectrometry (TOF-SIMS) imaging and related to fatty acids enhancing effect o...
Article
Argon cluster ion sources for sputtering and secondary ion mass spectrometry use projectiles consisting of several hundreds of atoms, accelerated to 10-20 keV, and deposit their kinetic energy within the top few nanometers of the surface. For organic materials, the sputtering yield is high removing material to similar depth. Consequently, the expos...
Chapter
Mass spectrometry imaging (MSI) is now becoming a method of choice to study the spatial distribution of various compounds at the surface of a tissue sample, with in situ detection of various intact molecular ions and fragments. Secondary ion mass spectrometry, by using a time-of-flight analyser and a cluster primary ion source is a method which can...