@article{doi:10.1021/jacs.4c03174,
  author = {Mudryk, Karen and Lee, Chin and Tomaník, Lukáš and Malerz, Sebastian and Trinter, Florian and Hergenhahn, Uwe and Neumark, Daniel M. and Slavíček, Petr and Bradforth, Stephen and Winter, Bernd},
  title = {How Does Mg2+(aq) Interact with ATP(aq)? Biomolecular Structure through the Lens of Liquid-Jet Photoemission Spectroscopy},
  journal = {Journal of the American Chemical Society},
  volume = {146},
  number = {23},
  pages = {16062-16075},
  year = {2024},
  doi = {10.1021/jacs.4c03174},
  note ={PMID: 38802319},
  URL = {https://doi.org/10.1021/jacs.4c03174},
  eprint = { https://doi.org/10.1021/jacs.4c031},
  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 (Mg2+(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 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 [Mg2ATP](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 Mg2+(aq) 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. },
  bibbase_note={<img src="https://pubs.acs.org/cms/10.1021/jacs.4c03174/asset/images/medium/ja4c03174_0009.gif">}
}

{"_id":"yCEYvM2ALEmLroQxb","bibbaseid":"mudryk-lee-tomank-malerz-trinter-hergenhahn-neumark-slavek-etal-howdoesmg2aqinteractwithatpaqbiomolecularstructurethroughthelensofliquidjetphotoemissionspectroscopy-2024","author_short":["Mudryk, K.","Lee, C.","Tomaník, L.","Malerz, S.","Trinter, F.","Hergenhahn, U.","Neumark, D. M.","Slavíček, P.","Bradforth, S.","Winter, B."],"bibdata":{"bibtype":"article","type":"article","author":[{"propositions":[],"lastnames":["Mudryk"],"firstnames":["Karen"],"suffixes":[]},{"propositions":[],"lastnames":["Lee"],"firstnames":["Chin"],"suffixes":[]},{"propositions":[],"lastnames":["Tomaník"],"firstnames":["Lukáš"],"suffixes":[]},{"propositions":[],"lastnames":["Malerz"],"firstnames":["Sebastian"],"suffixes":[]},{"propositions":[],"lastnames":["Trinter"],"firstnames":["Florian"],"suffixes":[]},{"propositions":[],"lastnames":["Hergenhahn"],"firstnames":["Uwe"],"suffixes":[]},{"propositions":[],"lastnames":["Neumark"],"firstnames":["Daniel","M."],"suffixes":[]},{"propositions":[],"lastnames":["Slavíček"],"firstnames":["Petr"],"suffixes":[]},{"propositions":[],"lastnames":["Bradforth"],"firstnames":["Stephen"],"suffixes":[]},{"propositions":[],"lastnames":["Winter"],"firstnames":["Bernd"],"suffixes":[]}],"title":"How Does Mg2+(aq) Interact with ATP(aq)? Biomolecular Structure through the Lens of Liquid-Jet Photoemission Spectroscopy","journal":"Journal of the American Chemical Society","volume":"146","number":"23","pages":"16062-16075","year":"2024","doi":"10.1021/jacs.4c03174","note":"PMID: 38802319","url":"https://doi.org/10.1021/jacs.4c03174","eprint":"https://doi.org/10.1021/jacs.4c031","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 (Mg2+(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 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 [Mg2ATP](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 Mg2+(aq) 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. ","bibbase_note":"<img src=\"https://pubs.acs.org/cms/10.1021/jacs.4c03174/asset/images/medium/ja4c03174_0009.gif\">","bibtex":"@article{doi:10.1021/jacs.4c03174,\n author = {Mudryk, Karen and Lee, Chin and Tomaník, Lukáš and Malerz, Sebastian and Trinter, Florian and Hergenhahn, Uwe and Neumark, Daniel M. and Slavíček, Petr and Bradforth, Stephen and Winter, Bernd},\n title = {How Does Mg2+(aq) Interact with ATP(aq)? Biomolecular Structure through the Lens of Liquid-Jet Photoemission Spectroscopy},\n journal = {Journal of the American Chemical Society},\n volume = {146},\n number = {23},\n pages = {16062-16075},\n year = {2024},\n doi = {10.1021/jacs.4c03174},\n note ={PMID: 38802319},\n URL = {https://doi.org/10.1021/jacs.4c03174},\n eprint = { https://doi.org/10.1021/jacs.4c031},\n 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 (Mg2+(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 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 [Mg2ATP](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 Mg2+(aq) 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. },\n bibbase_note={<img src=\"https://pubs.acs.org/cms/10.1021/jacs.4c03174/asset/images/medium/ja4c03174_0009.gif\">}\n}","author_short":["Mudryk, K.","Lee, C.","Tomaník, L.","Malerz, S.","Trinter, F.","Hergenhahn, U.","Neumark, D. 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