Publications

The survival of living systems relies on their ability to process complex physico-chemical information. Here, we introduce a scalable approach to design complex enzymatic reaction networks capable of reservoir computation based on recursive competition of substrates. As for the formose reservoir, Electrospray ionization-mass spectrometry allows for a real-time readout of chemical outputs, which effectively enables to demonstrate the information processing capabilities of this molecular system.

Periodic perturbations, such as modulations of reactant concentration, propagate through chemical reactions with distinct phase delays. In this project, we used ESI-MS to monitor the propagation of periodic concentrations perturbations through an organocatalytic reaction in a continuous stirred tank reactor (CSTR). The propagation patterns provide insights on reaction kinetics in solution, especially by comparing reactants bearing electron donating or withdrawing substituents. Although the reaction studied is relatively simple, we plan to extend this approach to much larger reaction networks.

With this publication, we made a cover feature for ChemistryEurope ! :)

In this project, we hypothesized that ML models could be trained based on IMS-MS measurements to classify guests based on their propensity to form inclusion or exclusion complexes with a supramolecular host. By combining CCS measurements with DFT-derived molecular descriptors, we trained a regression model that accurately predicts CCS values. The predicted values naturally separate in two groups, representing the inclusion vs exclusion topologies, and enable to determine a classification boundary of complex topologies.

Here, we investigated the impact of post-translational succination on the structure and stability of small ubiquitin-like modifier 1 (SUMO1). Combining solution, gas-phase and modelling studies reveals a complete picture of the changes induced by succination.

In this review article, I summarized recent developments on the integration between flow chemistry and mass spectrometry to achieve real-time monitoring of reaction mixtures under well-defined conditions.

Here, we investigated the gas phase structure of copolymers containing styrene, stryene alcohol and styrene-PPh2-AuCl moities.

Here, we investigated the gas phase structure of polystyrene ions with different end groups to establish how the nature and the rigidity of the monomer unit affect the charge stabilization.

Here, we report on an interface between a continuous stirred-tank reactor, in which an immobilized enzymatic network made of 12 enzymes is compartmentalized, and an ion mobility–mass spectrometer. The metabolic flux can be continuously and quantitatively monitored by ESI-IMS-MS. The real-time quantitative data were then harnessed to train a model of network kinetics, which proves sufficiently predictive to control the ERN output after a single optimally designed experiment, demonstrating the usefulness of high-throughput and highly informative analytical approaches.

In this work, we demonstrated how the formose reaction can perform several computational tasks, including nonlinear classification tasks in parallel, predicting the dynamics of other complex systems and achieving time-series forecasting. The reservoir outputs were measured by an ion mobility mass spectrometer, highlighting the importance of online analytics for achieving chemical reservoir computation.

In this collaborative work with Prof. Jiří Hanusek (University of Pardubice, Czech Republic), we combined the results from ESI-MS and various add-on methods, such as IR spectroscopy, ion mobility, or flow chemistry, to uncover the autocatalytic nature of the Eschenmoser Coupling Reaction.

In this publication, we used ion mobility-mass spectrometry to quantify the size of substituents grafted onto macrocyclic porphyrin cage compounds. The substituent size correlates well with the threading rates of chiral guests, demonstrating the role of the substituent bulkiness on kinetic enantio-recognition.

Here, we investigate the solution equilibria of labile pyridine ligands coordinated in the cavity of macrocyclic porphyrin cage complexes by ESI-MS. Using delayed reactant labeling, we could obtain rate constants and activation parameters for ligand dissociation in solution. With our approach, we gathered mechanistic evidence that are not easily obtained from traditional solution-phase techniques.

In this review article, we reflected on the synergy between IMS-MS and theoretical approaches, including computational chemistry, demonstrating the essential role they play to fully understand/interpret IMS-MS data for polymer ions.

Here, we investigated alkene epoxidation reactions mediated by two mangangese(III) porphyrin cage complexes. We monitored the formation of isomeric high-valent manganese(V)oxo complexes by ion-mobility mass spectrometry and demonstrated that the position at which the oxo ligand is formed depends on the preferential binding site of the oxidant molecule in solution.

With this publication, we made it to the cover of EJOC ! :)

In this collaboration with the group of Prof. Benjamin Elias (Université de Louvain, Belgium), we harnessed ion mobility-mass spectrometry to detect and characterize four isomeric trinuclear Ru(II) bipyridine complexes.

Here, we combined ultra-high performance liquid chromatography (UPLC) and ion mobility-mass spectrometry to characterize isomeric homopolymers and block copolymers. We demonstrated that ion mobility is only able to resolve a subset of ions with precise charge states and chain lengths.

In this collaboration with the group of Prof. Benjamin Elias (Université de Louvain, Belgium), we characterized antenna complexes using ion mobility-mass spectrometry.

In this work, we investigated the suitability of ion mobility spectrometry-mass spectrometry (IMS-MS) for the relative quantification of isomeric cyclic and linear polylactides. The results highlight intrinsic limitations when using IMS-MS in the context of relative quantification. Nonetheless, the linear-to-cyclic ratio can be roughly estimated by this method.

In this publication, We found that cationized gaseous PLA ions can be formed via various competing pathways during Electrospray Ionization. For a subset of ions, the IMS-MS response appears to be strongly correlated with the ESI release mechanism (CEM vs. CRM). The former favored extended structures, whereas the latter preferentially generated compact conformers.

This review article discusses recent computational and experimental studies that have shed light on the mechanisms whereby [M + zH]^z+ protein ions are released from charged nanodroplets during Electrospray Ionization.

In this collaboration with the group of Prof. Paolo Samorì (Université de Strasboug, France), we took advantage of ion mobility spectrometry to separate the metastable photoisomers of novel multiphotochromic compounds.

Here, we addressed critical flaws in previously published fitting models of collisional cross sections for polymer ions.

In this publication, we investigated the additional stabilization of longer metal-complexed alkylamines compared to ones with shorter alkyl chains. This publication was awarded the 2019 IJMS Best Student Paper Award.

Here, we report on a new DREDING-based force field for the atomistic modelling of peptoids.

During my scientific stay in the Konermann Lab (University of Western Ontario, Canada), I contributed to investigate the release of unfolded protein ions from charged droplet by atomistic simulations.

During my scientific stay in the Konermann Lab (University of Western Ontario, Canada), I studied the release of polyether ions from charged droplets with atomistic simulations. We found that gaseous polymer ion can be generated by competing pathways during Electrospray ionization.

In collaboration with Prof. Cyril Poriel (Université de Rennes, France), we introduced ion mobility-mass spectrometry as a direct method to distringuish positional isomers produced during the synthesis of compounds used in opto-electronics.

We proposed a new calibration based on the use of synthetic polymers for determining collisional cross sections on traveling wave ion mobility spectrometry instruments.

Here, we evaluated the feasibility of performing action-FRET on a supramolecular assembly constituted by a chromophore tagged cyclodextrin receptor and a donor chromophore tagged amyloid beta peptide fragment.

In this paper, we analyzed polylactide ions with traveling wave ion mobility and tandem drift tube ion mobility. We observed the coexistence of non-interconverting extended and compact ion populations, suggesting that the polylactide ions are ‘frozen’ in their specific conformation during the desolvation/ionization Electrospray process.