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Liquid-jet photoemission spectroscopy as a structural tool: site-specific acid–base chemistry of vitamin C

MPS-Authors
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Pugini,  Michele       
Molecular Physics, Fritz Haber Institute, Max Planck Society;

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Mudryk,  Karen       
Molecular Physics, Fritz Haber Institute, Max Planck Society;

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Stemer,  Dominik       
Molecular Physics, Fritz Haber Institute, Max Planck Society;

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Credidio,  Bruno       
Molecular Physics, Fritz Haber Institute, Max Planck Society;

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Trinter,  Florian       
Molecular Physics, Fritz Haber Institute, Max Planck Society;

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Winter,  Bernd       
Molecular Physics, Fritz Haber Institute, Max Planck Society;

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Citation

Tomanik, L., Pugini, M., Mudryk, K., Thürmer, S., Stemer, D., Credidio, B., et al. (2024). Liquid-jet photoemission spectroscopy as a structural tool: site-specific acid–base chemistry of vitamin C. Physical Chemistry Chemical Physics, 26(29), 19673-19684. doi:10.1039/d4cp01521e.


Cite as: https://hdl.handle.net/21.11116/0000-000F-8D1F-1
Abstract
Liquid-jet photoemission spectroscopy (LJ-PES) directly probes the electronic structure of solutes and solvents. It also emerges as a novel tool to explore chemical structure in aqueous solutions, yet the scope of the approach has to be examined. Here, we present a pH-dependent liquid-jet photoelectron spectroscopic investigation of ascorbic acid (vitamin C). We combine core-level photoelectron spectroscopy and ab initio calculations, allowing us to site-specifically explore the acid–base chemistry of the biomolecule. For the first time, we demonstrate the capability of the method to simultaneously assign two deprotonation sites within the molecule. We show that a large change in chemical shift appears even for atoms distant several bonds from the chemically modified group. Furthermore, we present a highly efficient and accurate computational protocol based on a single structure using the maximum-overlap method for modeling core-level photoelectron spectra in aqueous environments. This work poses a broader question: to what extent can LJ-PES complement established structural techniques such as nuclear magnetic resonance? Answering this question is highly relevant in view of the large number of incorrect molecular structures published.