Femtosecond proton transfer in urea solutions probed by X-ray spectroscopy

Zhong Yin (), Yi-Ping Chang, Tadas Balčiūnas, Yashoj Shakya, Aleksa Djorović, Geoffrey Gaulier, Giuseppe Fazio, Robin Santra, Ludger Inhester (), Jean-Pierre Wolf () and Hans Jakob Wörner ()
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Zhong Yin: ETH Zürich
Yi-Ping Chang: Université de Genève
Tadas Balčiūnas: ETH Zürich
Yashoj Shakya: Deutsches Elektronen-Synchrotron DESY
Aleksa Djorović: Université de Genève
Geoffrey Gaulier: Université de Genève
Giuseppe Fazio: ETH Zürich
Robin Santra: Deutsches Elektronen-Synchrotron DESY
Ludger Inhester: Deutsches Elektronen-Synchrotron DESY
Jean-Pierre Wolf: Université de Genève
Hans Jakob Wörner: ETH Zürich

Nature, 2023, vol. 619, issue 7971, 749-754

Abstract: Abstract Proton transfer is one of the most fundamental events in aqueous-phase chemistry and an emblematic case of coupled ultrafast electronic and structural dynamics1,2. Disentangling electronic and nuclear dynamics on the femtosecond timescales remains a formidable challenge, especially in the liquid phase, the natural environment of biochemical processes. Here we exploit the unique features of table-top water-window X-ray absorption spectroscopy3–6 to reveal femtosecond proton-transfer dynamics in ionized urea dimers in aqueous solution. Harnessing the element specificity and the site selectivity of X-ray absorption spectroscopy with the aid of ab initio quantum-mechanical and molecular-mechanics calculations, we show how, in addition to the proton transfer, the subsequent rearrangement of the urea dimer and the associated change of the electronic structure can be identified with site selectivity. These results establish the considerable potential of flat-jet, table-top X-ray absorption spectroscopy7,8 in elucidating solution-phase ultrafast dynamics in biomolecular systems.

Date: 2023
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DOI: 10.1038/s41586-023-06182-6

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