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Their structures and functions are highly dependent on the organization and dynamics of the surrounding solvent environment. Ionic liquids (ILs) act as excellent media for storing GQs by modifying their hydration patterns and dynamics. However, systematic studies on the solvation behavior of GQs remain scarce. Attempts have been made in this study to explore how aqueous solutions containing nucleobase (purine and pyrimidine) ionic liquids (NBILs) alter the time scale of dynamic heterogeneity within the GQ solvation shell. The calculations revealed that the solvent (water) and the cosolvent (NBIL) have markedly nonuniform spatial density distributions around the GQ, with the cations and anions exhibiting more heterogeneous distributions than water due to their stronger and more specific interactions with the GQ. It is found that the GQ can trap water within its confined pockets, thereby leading to nonuniform water residence times around it. Our analyses demonstrated that both water and IL around the GQ exhibit highly retarded heterogeneous translational and rotational motions. Among the two components, water molecules experience a comparatively greater degree of restriction in mobility due to their wide range of interaction strengths and the excluded-volume effect of the GQ. Interestingly, the relative increase in dynamic heterogeneity at the GQ interface in aqueous medium with respect to pure bulk water has been found to be noticeably greater as compared to the corresponding increase in dynamic heterogeneity at the interface in aqueous NBIL solutions with respect to their respective bulk states. Further, heterogeneity in translational motions of solvent components has been found to be much higher in purine-based IL solutions than in pyrimidine-based ones, though no such effect was observed for the rotational motions of the solvent components.<\/jats:p>","DOI":"10.1021\/acs.jpcb.6c03655","type":"journal-article","created":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T03:01:59Z","timestamp":1788922919000},"page":"9826-9842","source":"Crossref","is-referenced-by-count":0,"title":["Dynamically Heterogeneous\nSolvation Environment around\na G-Quadruplex in Aqueous Solutions Containing Nucleobase Ionic\nLiquids"],"prefix":"10.1021","volume":"130","author":[{"given":"Dipayan","family":"Sarder","sequence":"first","affiliation":[{"name":"Indian Institute of Technology Kharagpur , , ,","place":["Kharagpur, India, 721302"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3267-6326","authenticated-orcid":true,"given":"Sanjoy","family":"Bandyopadhyay","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Kharagpur , , ,","place":["Kharagpur, India, 721302"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,8]]},"reference":[{"key":"2026092408092005100_cit1","doi-asserted-by":"publisher","first-page":"123","DOI":"10.1002\/1097-0282(2000\/2001)56:3&lt;123::AID-BIP10010&gt;3.0.CO;2-3","article-title":"Quadruplex\nStructures in Nucleic Acids","volume":"56","author":"Keniry","year":"2000","journal-title":"Biopolymers"},{"key":"2026092408092005100_cit2","doi-asserted-by":"publisher","first-page":"123","DOI":"10.1016\/j.trechm.2019.07.002","article-title":"The Structure\nand Function of DNA\nG-Quadruplexes","volume":"2","author":"Spiegel","year":"2020","journal-title":"Trends Chem"},{"key":"2026092408092005100_cit3","doi-asserted-by":"publisher","first-page":"718","DOI":"10.1038\/350718a0","article-title":"Inhibition of Telomerase\nby G-Quartet DNA Structures","volume":"350","author":"Zahler","year":"1991","journal-title":"Nature"},{"key":"2026092408092005100_cit4","doi-asserted-by":"publisher","first-page":"9640","DOI":"10.1021\/ja404868t","article-title":"G-Quadruplex\nDNA as a Molecular Target for Induced Synthetic Lethality in Cancer\nCells","volume":"135","author":"McLuckie","year":"2013","journal-title":"J. Am. Chem. Soc"},{"key":"2026092408092005100_cit5","doi-asserted-by":"publisher","first-page":"769","DOI":"10.3390\/ph14080769","article-title":"G-Quadruplexes and\nTheir Ligands: Biophysical Methods to Unravel G-Quadruplex\/Ligand\nInteractions","volume":"14","author":"Santos","year":"2021","journal-title":"Pharmaceuticals"},{"key":"2026092408092005100_cit6","doi-asserted-by":"publisher","first-page":"1","DOI":"10.1016\/j.aca.2009.12.007","article-title":"Ionic Liquids\nin Analytical Chemistry","volume":"661","author":"Sun","year":"2010","journal-title":"Anal. Chim. Acta"},{"key":"2026092408092005100_cit7","doi-asserted-by":"publisher","first-page":"598662","DOI":"10.3389\/fchem.2020.598662","article-title":"Use of Ionic Liquids\nin Protein and DNA Chemistry","volume":"8","author":"Shukla","year":"2020","journal-title":"Front. 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Soc"},{"key":"2026092408092005100_cit30","doi-asserted-by":"publisher","first-page":"9824","DOI":"10.1021\/ja200786q","article-title":"Structure of Human\nTelomeric DNA in Crowded Solution","volume":"133","author":"Heddi","year":"2011","journal-title":"J. Am. Chem.\nSoc"},{"key":"2026092408092005100_cit31","doi-asserted-by":"publisher","first-page":"028702","DOI":"10.1088\/1674-1056\/ac7452","article-title":"Heterogeneous\nHydration Patterns of G-Quadruplex DNA","volume":"32","author":"Ji","year":"2023","journal-title":"Chin.\nPhys. B"},{"key":"2026092408092005100_cit32","doi-asserted-by":"publisher","first-page":"9138","DOI":"10.1021\/acs.jpcb.5c04379","article-title":"Unraveling\nthe Effects of Purine- and Pyrimidine-Based\nIonic Liquids on G-Quadruplex","volume":"129","author":"Sarder","year":"2025","journal-title":"J. Phys. 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Chem.\nB"},{"key":"2026092408092005100_cit39","doi-asserted-by":"publisher","first-page":"1902","DOI":"10.1063\/1.472061","article-title":"Simulation of Activation Free Energies\nin Molecular Systems","volume":"105","author":"Neria","year":"1996","journal-title":"J. Chem. Phys"},{"key":"2026092408092005100_cit40","doi-asserted-by":"publisher","first-page":"926","DOI":"10.1063\/1.445869","article-title":"Comparison\nof Simple Potential Functions for Simulating Liquid Water","volume":"79","author":"Jorgensen","year":"1983","journal-title":"J. Chem. Phys"},{"key":"2026092408092005100_cit41","doi-asserted-by":"publisher","first-page":"4613","DOI":"10.1063\/1.470648","article-title":"Constant Pressure\nMolecular Dynamics Simulation: The Langevin Piston Method","volume":"103","author":"Feller","year":"1995","journal-title":"J. Chem. 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J"},{"key":"2026092408092005100_cit48","doi-asserted-by":"publisher","first-page":"363","DOI":"10.1002\/(SICI)1096-987X(199802)19:3&lt;363::AID-JCC9&gt;3.0.CO;2-R","article-title":"Effect\nof Available Volumes on Radial Distribution Functions","volume":"19","author":"Astley","year":"1998","journal-title":"J. Comput. Chem"},{"key":"2026092408092005100_cit49","doi-asserted-by":"publisher","first-page":"6762","DOI":"10.1021\/acsnano.6b02333","article-title":"Structure\nand Dynamics of Confined Alcohol\u2013Water\nMixtures","volume":"10","author":"Bampoulis","year":"2016","journal-title":"ACS Nano"},{"key":"2026092408092005100_cit50","doi-asserted-by":"publisher","first-page":"17819","DOI":"10.1021\/acs.jpcc.0c04897","article-title":"Nanoconfined Water Dynamics in Multilayer\nGraphene Nanopores","volume":"124","author":"Pan","year":"2020","journal-title":"J. Phys. Chem. C"},{"key":"2026092408092005100_cit51","doi-asserted-by":"publisher","first-page":"15950","DOI":"10.1021\/ja8046552","article-title":"Diarylethynyl\nAmides that Recognize the Parallel Conformation of Genomic Promoter\nDNA G-Quadruplexes","volume":"130","author":"Dash","year":"2008","journal-title":"J. Am. Chem. Soc"},{"key":"2026092408092005100_cit52","doi-asserted-by":"publisher","first-page":"2709","DOI":"10.1093\/nar\/gks1328","article-title":"A Dual-Site\nSimultaneous Binding Mode in the Interaction between Parallel-Stranded\nG-Quadruplex [d(TGGGGT)]4 and Cyanine Dye 2,2\u2032-Diethyl-9-methyl-selenacarbocyanine\nBromide","volume":"41","author":"Gai","year":"2013","journal-title":"Nucleic Acids Res"},{"key":"2026092408092005100_cit53","volume-title":"Computer Simulation\nof Liquids","author":"Allen","year":"1987"},{"key":"2026092408092005100_cit54","doi-asserted-by":"publisher","first-page":"7271","DOI":"10.1021\/acs.jpcb.2c03940","article-title":"Exploring the Dynamic Heterogeneity\nat the Interface of a Protein in Aqueous Ionic Liquid Solutions","volume":"126","author":"Ghanta","year":"2022","journal-title":"J. Phys. Chem. B"},{"key":"2026092408092005100_cit55","doi-asserted-by":"publisher","first-page":"20330","DOI":"10.1021\/ja304519d","article-title":"Groove Binding Mechanism\nof Ionic\nLiquids: A Key Factor in Long-Term Stability of DNA in Hydrated Ionic\nLiquids?","volume":"134","author":"Chandran","year":"2012","journal-title":"J. Am. Chem. Soc"},{"key":"2026092408092005100_cit56","doi-asserted-by":"publisher","first-page":"14835","DOI":"10.1039\/C8CP01942H","article-title":"Dynamical\nCrossover of Water Confined within the Amphiphilic\nNanocores of Aggregated Amyloid \u03b2 Peptides","volume":"20","author":"Khatua","year":"2018","journal-title":"Phys. Chem. Chem. Phys"},{"key":"2026092408092005100_cit57","doi-asserted-by":"publisher","first-page":"249","DOI":"10.1103\/PhysRev.95.249","article-title":"Correlations in Space and Time and Born Approximation Scattering\nin Systems of Interacting Particles","volume":"95","author":"Van Hove","year":"1954","journal-title":"Phys. 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Chem. Phys"},{"key":"2026092408092005100_cit61","doi-asserted-by":"publisher","first-page":"A405","DOI":"10.1103\/PhysRev.136.A405","article-title":"Correlations\nin the Motion of Atoms in Liquid Argon","volume":"136","author":"Rahman","year":"1964","journal-title":"Phys.\nRev"},{"key":"2026092408092005100_cit62","doi-asserted-by":"publisher","first-page":"061504","DOI":"10.1103\/PhysRevE.70.061504","article-title":"Temperature Dependence of Spatially Heterogeneous Dynamics\nin a Model of Viscous Silica","volume":"70","author":"Vogel","year":"2004","journal-title":"Phys. Rev. E"},{"key":"2026092408092005100_cit63","doi-asserted-by":"publisher","first-page":"15683","DOI":"10.1021\/acs.jpcb.5b08763","article-title":"Composition Dependence\nof Dynamic Heterogeneity Time-\nand Length Scales in [Omim][BF4]\/Water Binary Mixtures:\nMolecular Dynamics Simulation Study","volume":"119","author":"Pal","year":"2015","journal-title":"J. Phys.\nChem. 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