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While the role of nucleotides as a stabilizer and biological hydrotrope is well-established, their interaction with biological assembly is inherently paradoxical. Furthermore, the interaction of nucleotides with the transient intermediates of self-assembly of proteins and peptides remains largely unexplored. Here, l-phenylalanine (Phe) is employed as a minimal model to investigate nucleotide-mediated regulation in both native and metal-stabilized assemblies. In native Phe assemblies, ATP and ADP exhibit a concentration-dependent disruption of fibrillar morphology, whereas AMP offers a minimal influence. In contrast, within cation-mediated metastable assemblies, nucleotides actively redirect the assembly pathways. Phosphate multiplicity dictates structural outcomes: ATP and ADP stabilize compact spherical-like architectures, while AMP promotes fibrillar aggregates. Mechanistic analysis, supported by imaging techniques and zeta potential, reveals synergistic contributions from multivalent phosphate interaction and nucleoside-mediated interactions.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c01729","type":"journal-article","created":{"date-parts":[[2026,7,20]],"date-time":"2026-07-20T11:03:48Z","timestamp":1784545428000},"page":"8606-8615","source":"Crossref","is-referenced-by-count":0,"title":["Diverse Roles of Nucleotides in Tuning Metal-Ion-Stabilized\nIntermediates of Amino Acid Aggregate via Phosphate Multiplicity and\nSalt-Triggered Fusion"],"prefix":"10.1021","volume":"17","author":[{"given":"Suman","family":"Choudhury","sequence":"first","affiliation":[{"name":"Indian Institute of Technology Indore , , , ,","place":["Indore, Madhya Pradesh, India, 453552"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Priyanka","family":"Nath","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Indore , , , ,","place":["Indore, Madhya Pradesh, India, 453552"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huma","family":"Tabassum","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Indore , , , ,","place":["Indore, Madhya Pradesh, India, 453552"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Naveen","family":"Kumar","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Indore , , , ,","place":["Indore, Madhya Pradesh, India, 453552"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Avijit","family":"Maity","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Indore , , , ,","place":["Indore, Madhya Pradesh, India, 453552"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Debanjan","family":"Bagchi","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Indore , , , ,","place":["Indore, Madhya Pradesh, India, 453552"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5564-0679","authenticated-orcid":true,"given":"Anjan","family":"Chakraborty","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Indore , , , ,","place":["Indore, Madhya Pradesh, India, 453552"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,20]]},"reference":[{"issue":"1","key":"2026073009075556100_cit1","doi-asserted-by":"publisher","first-page":"13","DOI":"10.1038\/nmat4474","article-title":"Supramolecular Biomaterials","volume":"15","author":"Webber","year":"2016","journal-title":"Nat. Mater."},{"issue":"34","key":"2026073009075556100_cit2","doi-asserted-by":"publisher","first-page":"11252","DOI":"10.1039\/D1SC03545B","article-title":"Supramolecular Chemistry\nin Lipid Bilayer Membranes","volume":"12","author":"Bickerton","year":"2021","journal-title":"Chem. Sci."},{"issue":"6","key":"2026073009075556100_cit3","doi-asserted-by":"publisher","first-page":"10715","DOI":"10.1021\/acsomega.9b00047","article-title":"Self-Assembly\nof Diphenylalanine\u2013Peptide\nNucleic Acid Conjugates","volume":"4","author":"Datta","year":"2019","journal-title":"ACS Omega"},{"issue":"14","key":"2026073009075556100_cit4","doi-asserted-by":"publisher","first-page":"9196","DOI":"10.1073\/pnas.142459399","article-title":"The Protofilament Structure of Insulin Amyloid Fibrils","volume":"99","author":"Jime\u0301nez","year":"2002","journal-title":"Proc. Natl. Acad. Sci. U.S.A."},{"issue":"7","key":"2026073009075556100_cit5","doi-asserted-by":"publisher","first-page":"2162","DOI":"10.1021\/ja0565673","article-title":"Cytochrome Display\non Amyloid Fibrils","volume":"128","author":"Baldwin","year":"2006","journal-title":"J. Am. Chem. Soc."},{"issue":"10","key":"2026073009075556100_cit6","doi-asserted-by":"publisher","first-page":"750","DOI":"10.1038\/s41578-025-00793-3","article-title":"Design and Sustainability\nof Polypeptide Material Systems","volume":"10","author":"Yorke","year":"2025","journal-title":"Nat. Rev. Mater."},{"key":"2026073009075556100_cit7","doi-asserted-by":"publisher","DOI":"10.1016\/j.ijbiomac.2023.128944","article-title":"Self-Assembling Peptides: Perspectives Regarding Biotechnological\nApplications and Vaccine Development","volume":"259","author":"Reyes","year":"2024","journal-title":"Int. J.\nBiol. Macromol."},{"issue":"3","key":"2026073009075556100_cit8","doi-asserted-by":"publisher","first-page":"289","DOI":"10.1021\/acs.accounts.3c00592","article-title":"Peptide Self-Assembly:\nFrom Ordered to Disordered","volume":"57","author":"Chang","year":"2024","journal-title":"Acc. Chem. Res."},{"issue":"6365","key":"2026073009075556100_cit9","doi-asserted-by":"publisher","DOI":"10.1126\/science.aam9756","article-title":"Self-Assembling Peptide\nSemiconductors","volume":"358","author":"Tao","year":"2017","journal-title":"Science"},{"issue":"14","key":"2026073009075556100_cit10","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202318365","article-title":"Designing\nMultifunctional Biomaterials\nvia Protein Self-Assembly","volume":"63","author":"Solomonov","year":"2024","journal-title":"Angew. 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Phys.\nChem. B"},{"issue":"44","key":"2026073009075556100_cit26","doi-asserted-by":"publisher","first-page":"10409","DOI":"10.1021\/acs.jpclett.2c02882","article-title":"Metal-Ion-Induced\nEvolution of Phenylalanine Self-Assembly: Structural Polymorphism\nof Novel Metastable Intermediates","volume":"13","author":"Bagchi","year":"2022","journal-title":"J. Phys.\nChem. Lett."},{"issue":"16","key":"2026073009075556100_cit27","doi-asserted-by":"publisher","first-page":"4468","DOI":"10.1021\/acs.jpclett.4c00444","article-title":"Metal Ion-Induced\nUnusual Stability\nof the Metastable Vesicle-like Intermediates Evolving during the Self-Assembly\nof Phenylalanine: Prominent Role of Surface Charge Inversion","volume":"15","author":"Bagchi","year":"2024","journal-title":"J. Phys. Chem. Lett."},{"issue":"22","key":"2026073009075556100_cit28","doi-asserted-by":"publisher","first-page":"5531","DOI":"10.1021\/acs.jpclett.5c01228","article-title":"Interaction\nof Metal Ion Stabilized\nOligomeric Dipeptide with Lipid Membrane: Concurrent Observations\nof Supported Lipid Membrane, Wetting, and Uptake","volume":"16","author":"Nath","year":"2025","journal-title":"J. Phys. Chem. Lett."},{"issue":"40","key":"2026073009075556100_cit29","doi-asserted-by":"publisher","first-page":"21915","DOI":"10.1021\/jacs.3c06287","article-title":"An Analysis of Nucleotide\u2013Amyloid\nInteractions Reveals Selective Binding to Codon-Sized RNA","volume":"145","author":"Rout","year":"2023","journal-title":"J. Am. Chem. Soc."},{"issue":"1","key":"2026073009075556100_cit30","doi-asserted-by":"publisher","first-page":"86","DOI":"10.1021\/acs.jpcb.3c05996","article-title":"Suitability of Adenosine Derivatives\nin Improving the Activity and Stability of Cytochrome c under Stress:\nInsights into the Effect of Phosphate Groups","volume":"128","author":"Bharadwaj","year":"2024","journal-title":"J. Phys. Chem. B"},{"issue":"2","key":"2026073009075556100_cit31","doi-asserted-by":"publisher","first-page":"1326","DOI":"10.1021\/jacs.3c09134","article-title":"Adenosine Triphosphate\nMediates Phase\nSeparation of Disordered Basic Proteins by Bridging Intermolecular\nInteraction Networks","volume":"146","author":"Kota","year":"2024","journal-title":"J. Am. Chem. Soc."},{"issue":"6","key":"2026073009075556100_cit32","doi-asserted-by":"publisher","first-page":"2740","DOI":"10.1002\/anie.202006614","article-title":"ATP-Driven Synthetic Supramolecular\nAssemblies: From ATP as a Template to Fuel","volume":"60","author":"Mishra","year":"2021","journal-title":"Angew. Chem., Int. Ed."},{"issue":"42","key":"2026073009075556100_cit33","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202002629","article-title":"ATP-Responsive and\nATP-Fueled Self-Assembling Systems\nand Materials","volume":"32","author":"Deng","year":"2020","journal-title":"Adv. Mater."},{"issue":"6339","key":"2026073009075556100_cit34","doi-asserted-by":"publisher","first-page":"753","DOI":"10.1126\/science.aaf6846","article-title":"ATP as a Biological Hydrotrope","volume":"356","author":"Patel","year":"2017","journal-title":"Science"},{"issue":"2","key":"2026073009075556100_cit35","doi-asserted-by":"publisher","DOI":"10.1016\/j.xcrp.2021.100343","article-title":"Hofmeister versus Neuberg:\nIs ATP Really a Biological Hydrotrope?","volume":"2","author":"Mehringer","year":"2021","journal-title":"Cell\nRep. Phys. Sci."},{"issue":"1","key":"2026073009075556100_cit36","doi-asserted-by":"publisher","first-page":"1155","DOI":"10.1038\/s41467-019-09107-y","article-title":"Proteome-Wide Solubility and Thermal Stability Profiling\nReveals Distinct Regulatory Roles for ATP","volume":"10","author":"Sridharan","year":"2019","journal-title":"Nat.\nCommun."},{"issue":"10","key":"2026073009075556100_cit37","doi-asserted-by":"publisher","first-page":"1766","DOI":"10.1021\/jacsau.1c00316","article-title":"ATP Can Efficiently Stabilize Protein through a Unique Mechanism","volume":"1","author":"Ou","year":"2021","journal-title":"JACS Au"},{"issue":"2","key":"2026073009075556100_cit38","doi-asserted-by":"publisher","first-page":"929","DOI":"10.1021\/jacs.2c09615","article-title":"Nonspecific\nBinding of Adenosine Tripolyphosphate and\nTripolyphosphate Modulates the Phase Behavior of Lysozyme","volume":"145","author":"Zalar","year":"2023","journal-title":"J. Am. Chem. Soc."},{"issue":"7","key":"2026073009075556100_cit39","doi-asserted-by":"publisher","first-page":"5406","DOI":"10.1039\/D2CP05160E","article-title":"Influence of Salt and\nTemperature on the Self-Assembly of Cyclic\nPeptides in Water: A Molecular Dynamics Study","volume":"25","author":"Moral","year":"2023","journal-title":"Phys. Chem. Chem. Phys."},{"issue":"50","key":"2026073009075556100_cit40","doi-asserted-by":"publisher","first-page":"15494","DOI":"10.1021\/acs.langmuir.2c01394","article-title":"Anion Effects on\nthe Supramolecular Self-Assembly of Cationic Phenylalanine Derivatives","volume":"38","author":"Abraham","year":"2022","journal-title":"Langmuir"},{"issue":"1","key":"2026073009075556100_cit41","doi-asserted-by":"publisher","first-page":"210","DOI":"10.1021\/acs.jpcb.9b10175","article-title":"ATP Controls the Aggregation\nof A\u03b216\u201322 Peptides","volume":"124","author":"Pal","year":"2020","journal-title":"J. Phys. Chem. B"},{"issue":"14","key":"2026073009075556100_cit42","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.101.148101","article-title":"Reentrant\nCondensation of Proteins\nin Solution Induced by Multivalent Counterions","volume":"101","author":"Zhang","year":"2008","journal-title":"Phys. Rev. Lett."},{"issue":"3","key":"2026073009075556100_cit43","doi-asserted-by":"publisher","first-page":"593","DOI":"10.1021\/acs.jpcb.8b10868","article-title":"Controlling Phase\nSeparation of Lysozyme with Polyvalent\nAnions","volume":"123","author":"Bye","year":"2019","journal-title":"J. Phys. Chem. B"},{"issue":"3","key":"2026073009075556100_cit44","doi-asserted-by":"publisher","first-page":"798","DOI":"10.1006\/bbrc.1997.7052","article-title":"Effects of\nNucleotides on the Denaturation\nof F Actin: A Differential Scanning Calorimetry and FTIR Spectroscopy\nStudy","volume":"236","author":"Bombardier","year":"1997","journal-title":"Biochem. Biophys. Res. Commun."},{"issue":"8","key":"2026073009075556100_cit45","doi-asserted-by":"publisher","first-page":"5321","DOI":"10.1021\/acs.biomac.4c00738","article-title":"Minimal Peptide\nSequences That Undergo Liquid\u2013Liquid Phase Separation via Self-Coacervation\nor Complex Coacervation with ATP","volume":"25","author":"Castelletto","year":"2024","journal-title":"Biomacromolecules"},{"issue":"2","key":"2026073009075556100_cit46","doi-asserted-by":"publisher","first-page":"181","DOI":"10.1016\/0045-2068(77)90019-0","article-title":"Equilibrium Constants for Association of Guanidinium and Ammonium\nIons with Oxyanions: The Effect of Changing Basicity of the Oxyanion","volume":"6","author":"Springs","year":"1977","journal-title":"Bioorganic Chemistry"},{"issue":"36","key":"2026073009075556100_cit47","doi-asserted-by":"publisher","first-page":"11934","DOI":"10.1021\/jp1054342","article-title":"Effect of\nAssociation with Sulfate on the Electrophoretic Mobility of Polyarginine\nand Polylysine","volume":"114","author":"Wernersson","year":"2010","journal-title":"J. Phys. Chem. B"},{"issue":"17","key":"2026073009075556100_cit48","doi-asserted-by":"publisher","first-page":"16890","DOI":"10.1021\/acsnano.5c02235","article-title":"Salt-Bridge-Mediated\nCoacervate-to-Vesicle\nTransformation in Arginine-Rich Coacervates","volume":"19","author":"Seo","year":"2025","journal-title":"ACS Nano"},{"issue":"6","key":"2026073009075556100_cit49","doi-asserted-by":"publisher","first-page":"658","DOI":"10.1016\/j.cbpa.2006.09.020","article-title":"Interactions between Macromolecules and Ions: The Hofmeister\nSeries","volume":"10","author":"Zhang","year":"2006","journal-title":"Curr. Opin Chem. Biol."},{"issue":"20","key":"2026073009075556100_cit50","doi-asserted-by":"publisher","first-page":"14307","DOI":"10.1021\/jacs.4c04036","article-title":"Ionic Effect on the\nMicroenvironment of Biomolecular Condensates","volume":"146","author":"Zhu","year":"2024","journal-title":"J. Am. Chem. Soc."},{"issue":"40","key":"2026073009075556100_cit51","doi-asserted-by":"publisher","first-page":"11700","DOI":"10.1021\/jp074404q","article-title":"Electrostatic Self-Assembly of Neutral\nand Polyelectrolyte Block Copolymers and Oppositely Charged Surfactant","volume":"111","author":"Annaka","year":"2007","journal-title":"J. Phys. Chem. B"},{"issue":"84","key":"2026073009075556100_cit52","doi-asserted-by":"publisher","first-page":"12688","DOI":"10.1039\/C4CC05406G","article-title":"Visualized Discrimination of ATP\nfrom ADP and AMP through Collapse of Supramolecular Gels","volume":"50","author":"Yang","year":"2014","journal-title":"Chem. Commun."},{"issue":"33","key":"2026073009075556100_cit53","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2506491122","article-title":"Structural\nbasis and affinity improvement for an ATP-binding DNA aptamer","volume":"122","author":"Jiang","year":"2025","journal-title":"Proc. Natl. Acad. Sci. U.S.A."},{"issue":"19","key":"2026073009075556100_cit54","doi-asserted-by":"publisher","first-page":"7698","DOI":"10.1021\/acs.jcim.4c01389","article-title":"Mechanism of Dual-Site Recognition\nin a Classic DNA Aptamer","volume":"64","author":"Wang","year":"2024","journal-title":"J. Chem. Inf. Model."},{"issue":"9","key":"2026073009075556100_cit55","doi-asserted-by":"publisher","first-page":"1883","DOI":"10.1039\/c1nj20393b","article-title":"Binding and Recognition of AMP, ADP, ATP and Related\nInorganic Phosphate Anions by a Tren-Based Ligand Containing a Pyrimidine\nFunctionality","volume":"35","author":"Arranz-Mascaro\u0301s","year":"2011","journal-title":"New J. Chem."}],"container-title":["The Journal of Physical Chemistry Letters"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/acs.jpclett.6c01729","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jpclcd\/article-pdf\/17\/30\/8606\/66049780\/acs.jpclett.6c01729.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jpclcd\/article-pdf\/17\/30\/8606\/66049780\/acs.jpclett.6c01729.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,7,30]],"date-time":"2026-07-30T13:13:44Z","timestamp":1785417224000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jpclcd\/article\/17\/30\/8606\/5218354\/Diverse-Roles-of-Nucleotides-in-Tuning-Metal-Ion"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,7,20]]},"references-count":55,"journal-issue":{"issue":"30","published-online":{"date-parts":[[2026,7,20]]},"published-print":{"date-parts":[[2026,7,30]]}},"URL":"https:\/\/doi.org\/10.1021\/acs.jpclett.6c01729","relation":{},"ISSN":["1948-7185"],"issn-type":[{"value":"1948-7185","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,7,20]]}}}