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@ARTICLE{Mudryk:610905,
author = {Mudryk, Karen and Lee, Chin and Tomaník, Lukáš and
Malerz, Sebastian and Trinter, Florian and Hergenhahn, Uwe
and Neumark, Daniel M. and Slavicek, Petr and Bradforth,
Stephen and Winter, Bernd},
title = {{H}ow {D}oes ${M}g^{2+}_{(aq)}$ {I}nteract with
${ATP}_{(aq)}$? {B}iomolecular {S}tructure through the
{L}ens of {L}iquid-{J}et {P}hotoemission {S}pectroscopy},
journal = {Journal of the American Chemical Society},
volume = {146},
number = {23},
issn = {0002-7863},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {PUBDB-2024-04728},
pages = {16062-16075},
year = {2024},
note = {Open Access},
abstract = {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$^{2+}$$_{(aq)}$),
highlighting the synergy brought about by the simultaneous
analysis of different regions in the photoelectron spectrum.
In particular, we demonstrate intermolecular Coulombic decay
(ICD) spectroscopy as a new and powerful addition to the
arsenal of techniques for biomolecular structure
investigation. We apply LJ-PES assisted by
electronic-structure calculations to study ATP$_{(aq)}$
solutions with and without dissolved Mg$^{2+}$. Valence
photoelectron data reveal spectral changes in the phosphate
and adenine features of ATP$_{(aq)}$ due to interactions
with the divalent cation. Chemical shifts in Mg
$\small2$$p$, Mg $\small2$$s$, P $\small2$$p$, and P
$\small2$$s$ core-level spectra as a function of the
Mg$^{2+}$/ATP concentration ratio are correlated to the
formation of [Mg(ATP) $_{2}$$]$$^{6-}$$_{(aq)}$,
[MgATP]$^{2-}$$_{(aq)}$, and [Mg$_{2}$ATP]$_{(aq)}$
complexes, demonstrating the element sensitivity of the
technique to Mg$^{2+}$–phosphate interactions. The most
direct probe of the intermolecular interactions between
ATP$_{(aq)}$ and Mg$^{2+}$$_{(aq)}$ is delivered by the
emerging ICD electrons following ionization of Mg
$\small1$$s$ electrons. ICD spectra are shown to sensitively
probe ligand exchange in the Mg$^{2+}$–ATP$_{(aq)}$
coordination environment. In addition, we report and compare
P $\small2$$s$ 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 Mg$^{2+}$–ATP$_{(aq)}$ complexes relevant
to phosphorylation and dephosphorylation reactions that are
central to bioenergetics in living organisms.},
cin = {DOOR ; HAS-User / FS-PET-S},
ddc = {540},
cid = {I:(DE-H253)HAS-User-20120731 /
I:(DE-H253)FS-PET-S-20190712},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3) / AQUACHIRAL - Chiral
aqueous-phase chemistry (883759) / DFG project
G:(GEPRIS)509471550 - Dynamik photoionisations-induzierter
Prozesse in laser-präparierten Molekülen in der Gasphase
und der wässrigen Phase (509471550) / FS-Proposal:
II-20180012 (II-20180012) / FS-Proposal: I-20200682
(I-20200682)},
pid = {G:(DE-HGF)POF4-6G3 / G:(EU-Grant)883759 /
G:(GEPRIS)509471550 / G:(DE-H253)II-20180012 /
G:(DE-H253)I-20200682},
experiment = {EXP:(DE-H253)P-P04-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:38802319},
UT = {WOS:001234460800001},
doi = {10.1021/jacs.4c03174},
url = {https://bib-pubdb1.desy.de/record/610905},
}