How Does Mg2+ (aq) Interact with ATP(aq)? Biomolecular Structure through the Lens of Liquid-Jet Photoemission Spectroscopy

Result code in IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60461373%3A22340%2F24%3A43931075" target="_blank" >RIV/60461373:22340/24:43931075 - isvavai.cz</a>

Result on the web

<a href="https://pubs.acs.org/doi/10.1021/jacs.4c03174" target="_blank" >https://pubs.acs.org/doi/10.1021/jacs.4c03174</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/jacs.4c03174" target="_blank" >10.1021/jacs.4c03174</a>

Result language

angličtina

Original language name

How Does Mg2+ (aq) Interact with ATP(aq)? Biomolecular Structure through the Lens of Liquid-Jet Photoemission Spectroscopy

Original language description

Liquid-jet photoemission spectroscopy (LJ-PES) allows for a direct probing of electronic structure in aqueous solutions. We show the applicability of the approach to biomolecules in a complex environment, exploring site-specific information on the interaction of adenosine triphosphate in the aqueous phase (ATP((aq))) with magnesium (Mg-(aq)(2+)), highlighting the synergy brought about by the simultaneous analysis of different regions in the photoelectron spectrum. In particular, we demonstrate intermolecular Coulombic decay (ICD) spectroscopy as a new and powerful addition to the arsenal of techniques for biomolecular structure investigation. We apply LJ-PES assisted by electronic-structure calculations to study ATP((aq)) solutions with and without dissolved Mg2+. Valence photoelectron data reveal spectral changes in the phosphate and adenine features of ATP((aq)) due to interactions with the divalent cation. Chemical shifts in Mg 2p, Mg 2s, P 2p, and P 2s core-level spectra as a function of the Mg2+/ATP concentration ratio are correlated to the formation of [Mg(ATP) (2)](6-)((aq)), [MgATP](2-)((aq)), and [Mg(2)ATP]((aq)) complexes, demonstrating the element sensitivity of the technique to Mg2+-phosphate interactions. The most direct probe of the intermolecular interactions between ATP((aq)) and Mg-(aq)(2+) is delivered by the emerging ICD electrons following ionization of Mg 1s electrons. ICD spectra are shown to sensitively probe ligand exchange in the Mg2+-ATP((aq)) coordination environment. In addition, we report and compare P 2s data from ATP((aq)) and adenosine mono- and diphosphate (AMP((aq)) and ADP((aq)), respectively) solutions, probing the electronic structure of the phosphate chain and the local environment of individual phosphate units in ATP((aq)). Our results provide a comprehensive view of the electronic structure of ATP((aq)) and Mg2+-ATP((aq)) complexes relevant to phosphorylation and dephosphorylation reactions that are central to bioenergetics in living organisms.

Czech name

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Czech description

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Type

J_imp - Article in a specialist periodical, which is included in the Web of Science database

CEP classification

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OECD FORD branch

10403 - Physical chemistry

Project

Result was created during the realization of more than one project. More information in the Projects tab.

Continuities

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Publication year

2024

Confidentiality

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Name of the periodical

Journal of the American Chemical Society

ISSN

0002-7863

e-ISSN

1520-5126

Volume of the periodical

146

Issue of the periodical within the volume

23

Country of publishing house

US - UNITED STATES

Number of pages

14

Pages from-to

16062-16075

UT code for WoS article

001234460800001

EID of the result in the Scopus database

2-s2.0-85194472678