{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,7,27]],"date-time":"2026-07-27T14:04:09Z","timestamp":1785161049771,"version":"3.55.0"},"reference-count":53,"publisher":"American Chemical Society (ACS)","issue":"7","license":[{"start":{"date-parts":[[2026,7,15]],"date-time":"2026-07-15T00:00:00Z","timestamp":1784073600000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by-nc-nd\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100000781","name":"European Research Council","doi-asserted-by":"publisher","award":["101021081"],"award-info":[{"award-number":["101021081"]}],"id":[{"id":"10.13039\/501100000781","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100003130","name":"Fonds Wetenschappelijk Onderzoek","doi-asserted-by":"publisher","award":["G0C6623N"],"award-info":[{"award-number":["G0C6623N"]}],"id":[{"id":"10.13039\/501100003130","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100003130","name":"Fonds Wetenschappelijk Onderzoek","doi-asserted-by":"publisher","award":["I006920N"],"award-info":[{"award-number":["I006920N"]}],"id":[{"id":"10.13039\/501100003130","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/na","name":"Bijzonder Onderzoeksfonds","doi-asserted-by":"publisher","award":["BOF.BAS. 2022.0023.01"],"award-info":[{"award-number":["BOF.BAS. 2022.0023.01"]}],"id":[{"id":"10.13039\/na","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,7,27]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Liquid crystals (LCs) are a class of materials that combine molecular order and fluidity, making them crucial for technologies from displays to sensors. However, polymeric LC materials typically lack molecular precision, limiting systematic control over their phase behavior. Here, we report a modular synthetic strategy to prepare amphiphilic columnar liquid crystals based on hydrophobic di- and trialkylated galloyl cores attached to a sequence-defined polar oligomer grown by a thiolactone-based iterative protocol. This approach enables independent variation of (i) polar monomer type (e.g., hydroxyethyl acrylate and N,N-dimethylacrylamide), (ii) oligomer length (from 1-mer to tetramer), and (iii) core topology (two or three C18 chains). Differential scanning calorimetry, polarized optical microscopy, and X-ray scattering show that the number of hydrophobic C18 chains on the aromatic core is the dominant parameter governing mesophase stability. Derivatives with three C18 chains exhibit higher melting and isotropization temperatures and more pronounced transitions from lamellar crystals to hexagonally packed columnar mesophases than their two C18 analogues. The chemistry and length of the sequence-defined polar block further tune crystallization and mesophase behavior, i.e. hydrogen-bonding heads increase thermal stability, whereas bulkier PEG-like heads reduce crystallinity and can destabilize mesophases. Increasing oligomer length reduces crystallization enthalpies and can introduce competing liquid-crystalline states. These results demonstrate that the liquid crystalline behavior can be encoded at the molecular level, providing a basis for designing responsive and sequence-programmed LC materials.<\/jats:p>","DOI":"10.1021\/jacsau.6c00469","type":"journal-article","created":{"date-parts":[[2026,7,15]],"date-time":"2026-07-15T16:06:17Z","timestamp":1784131577000},"page":"3914-3926","source":"Crossref","is-referenced-by-count":0,"title":["Tunable Thermotropic\nLiquid Crystals Using Amphiphilic\nSequence-Defined Macromolecules"],"prefix":"10.1021","volume":"6","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9921-6853","authenticated-orcid":true,"given":"Irene","family":"De Franceschi","sequence":"first","affiliation":[{"name":"Ghent University , , Krijgslaan 291 (S4) , ,","place":["Ghent, Belgium, 9000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2751-5691","authenticated-orcid":true,"given":"Valentin P.","family":"Beyer","sequence":"additional","affiliation":[{"name":"University of Warwick , , ,","place":["Coventry, U.K., CV4 7AL"]},{"name":"Aston University , , ,","place":["Birmingham, U.K., B4 7ET"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Steve","family":"Huband","sequence":"additional","affiliation":[{"name":"University of Warwick , , ,","place":["Coventry, U.K., CV4 7AL"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4220-571X","authenticated-orcid":true,"given":"Nezha","family":"Badi","sequence":"additional","affiliation":[{"name":"Ghent University , , Krijgslaan 291 (S4) , ,","place":["Ghent, Belgium, 9000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Se\u0301bastien","family":"Perrier","sequence":"additional","affiliation":[{"name":"University of Warwick , , ,","place":["Coventry, U.K., CV4 7AL"]},{"name":"University of Warwick , , ,","place":["Coventry, U.K., CV4 7AL"]},{"name":"Monash University , , , ,","place":["Parkville, Victoria, Australia, 3052"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Filip E.","family":"Du Prez","sequence":"additional","affiliation":[{"name":"Ghent University , , Krijgslaan 291 (S4) , ,","place":["Ghent, Belgium, 9000"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,15]]},"reference":[{"key":"2026072709074357100_cit1","doi-asserted-by":"publisher","first-page":"19","DOI":"10.1039\/df9582500019","article-title":"Liquid\ncrystals. 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Mater."},{"key":"2026072709074357100_cit4","doi-asserted-by":"publisher","first-page":"4887","DOI":"10.1021\/acs.chemrev.1c00761","article-title":"Liquid crystals: versatile\nself-organized smart soft materials","volume":"122","author":"Bisoyi","year":"2022","journal-title":"Chem. Rev."},{"key":"2026072709074357100_cit5","doi-asserted-by":"publisher","first-page":"38","DOI":"10.1002\/anie.200501384","article-title":"Functional liquid-crystalline assemblies:\nself-organized soft materials","volume":"45","author":"Kato","year":"2006","journal-title":"Angew. Chem.,\nInt. 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Cryst."},{"key":"2026072709074357100_cit26","doi-asserted-by":"publisher","first-page":"1294","DOI":"10.1021\/ja8087778","article-title":"Self-Assembly\nof Dendritic Crowns into Chiral Supramolecular Spheres","volume":"131","author":"Percec","year":"2009","journal-title":"J. Am. Chem. Soc."},{"key":"2026072709074357100_cit27","doi-asserted-by":"publisher","first-page":"9941","DOI":"10.1021\/ja071012o","article-title":"Liquid\u2013Crystalline Janus-Type\nFullerodendrimers Displaying Tunable Smectic\u2013Columnar Mesomorphism","volume":"129","author":"Lenoble","year":"2007","journal-title":"J. Am. Chem. Soc."},{"key":"2026072709074357100_cit28","doi-asserted-by":"publisher","first-page":"1208","DOI":"10.1126\/science.1078849","article-title":"Giant Supramolecular\nLiquid Crystal Lattice","volume":"299","author":"Ungar","year":"2003","journal-title":"Science"},{"key":"2026072709074357100_cit29","doi-asserted-by":"publisher","first-page":"1070","DOI":"10.1002\/(SICI)1521-3765(19990301)5:3&lt;1070:AID-CHEM1070&gt;3.0.CO;2-9","article-title":"Coassembly\nof a Hexagonal Columnar Liquid Crystalline Superlattice from Polymer(s)\nCoated with a Three-Cylindrical Bundle Supramolecular Dendrimer","volume":"5","author":"Percec","year":"1999","journal-title":"Chem.\u2500Eur. J."},{"key":"2026072709074357100_cit30","doi-asserted-by":"publisher","first-page":"2495","DOI":"10.1021\/ol049555f","article-title":"Bisfunctionalized\nJanus molecules","volume":"6","author":"Ropponen","year":"2004","journal-title":"Org. Lett."},{"key":"2026072709074357100_cit31","doi-asserted-by":"publisher","first-page":"4739","DOI":"10.1002\/anie.200501254","article-title":"Self-assembly of\nsemifluorinated\njanus-dendritic benzamides into bilayered pyramidal columns","volume":"44","author":"Percec","year":"2005","journal-title":"Angew. Chem., Int. Ed."},{"key":"2026072709074357100_cit32","doi-asserted-by":"publisher","first-page":"921","DOI":"10.1002\/chem.200390114","article-title":"Hierarchical Self-Assembly Coassembly, and Self-Organization\nof Novel Liquid Crystalline Lattices and Superlattices from a Twin-Tapered\nDendritic Benzamide and Its Four-Cylinder-Bundle Supramolecular Polymer","volume":"9","author":"Percec","year":"2003","journal-title":"Chem.\u2500Eur. J."},{"issue":"DOI","key":"2026072709074357100_cit33","doi-asserted-by":"publisher","first-page":"4767","DOI":"10.1039\/c2sm07332c","article-title":"Phase\nbehaviour and Janus hierarchical supramolecular structures based on\nasymmetric tapered bisamide","volume":"8","author":"Sun","year":"2012","journal-title":"Soft Matter."},{"key":"2026072709074357100_cit34","doi-asserted-by":"publisher","first-page":"9797","DOI":"10.1021\/la061849h","article-title":"Water-Soluble\nPegylated Quantum Dots: From a Composite Hexagonal Phase to Isolated\nMicelles","volume":"22","author":"Boulmedais","year":"2006","journal-title":"Langmuir"},{"key":"2026072709074357100_cit35","doi-asserted-by":"publisher","first-page":"1246","DOI":"10.1039\/C0CC03753B","article-title":"Stable functionalized\nPEGylated quantum dots micelles with a controlled stoichiometry","volume":"47","author":"Amela-Cortes","year":"2011","journal-title":"Chem. Commun."},{"key":"2026072709074357100_cit36","doi-asserted-by":"publisher","first-page":"9670","DOI":"10.1021\/ja0266868","article-title":"Conjugated Polymer\nLiquid Crystal Solutions: Control\nof Conformation and Alignment","volume":"124","author":"Zhu","year":"2002","journal-title":"J. Am. Chem.\nSoc."},{"key":"2026072709074357100_cit37","doi-asserted-by":"publisher","first-page":"6569","DOI":"10.1021\/cm7028189","article-title":"Tunable Columnar Organization\nby Twisted Stacking of End-Capped Aromatic Rods","volume":"19","author":"Huang","year":"2007","journal-title":"Chem. Mater."},{"key":"2026072709074357100_cit38","doi-asserted-by":"publisher","first-page":"7562","DOI":"10.1021\/j100359a011","article-title":"Stability\nof lyotropic phases with curved interfaces","volume":"93","author":"Gruner","year":"1989","journal-title":"J. Phys. Chem."},{"key":"2026072709074357100_cit39","doi-asserted-by":"publisher","DOI":"10.1017\/CBO9780511616044","volume-title":"Liquid Crystalline Polymers","author":"Donald","year":"2006"},{"issue":"DOI","key":"2026072709074357100_cit40","doi-asserted-by":"publisher","first-page":"7316","DOI":"10.1039\/C7PY01576C","article-title":"Control of the alignment\nof liquid crystal molecules on a sequence-polymerized film by surface\nmigration and polarized light irradiation","volume":"8","author":"Cai","year":"2017","journal-title":"Polym.\nChem."},{"key":"2026072709074357100_cit41","doi-asserted-by":"publisher","first-page":"6209","DOI":"10.1021\/acs.macromol.8b01585","article-title":"Assessing the Sequence Specificity\nin Thermal and Polarized Optical Order of Multiple Sequence-Determined\nLiquid Crystal Polymers","volume":"51","author":"Han","year":"2018","journal-title":"Macromolecules"},{"key":"2026072709074357100_cit42","doi-asserted-by":"publisher","first-page":"11514","DOI":"10.1021\/acs.langmuir.2c01768","article-title":"Liquid-Crystalline\nPolymers: Molecular Engineering, Hierarchical\nStructures, and Applications","volume":"38","author":"Wei","year":"2022","journal-title":"Langmuir"},{"key":"2026072709074357100_cit43","doi-asserted-by":"publisher","first-page":"7701","DOI":"10.1021\/ma970783h","article-title":"Monodisperse Linear\nLiquid Crystalline Polyethers via\na Repetitive 2n Geometric Growth Algorithm","volume":"30","author":"Percec","year":"1997","journal-title":"Macromolecules"},{"key":"2026072709074357100_cit44","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adw5327","article-title":"Supramolecular bending\nand twisting in the hierarchical self-assembly of monodisperse mesogenic\noligomers","volume":"11","author":"Chan","year":"2025","journal-title":"Sci. Adv."},{"key":"2026072709074357100_cit45","doi-asserted-by":"publisher","first-page":"1700582","DOI":"10.1002\/marc.201700582","article-title":"Defining\nthe Field of Sequence-Controlled Polymers","volume":"38","author":"Lutz","year":"2017","journal-title":"Macromol.\nRapid Commun."},{"key":"2026072709074357100_cit46","doi-asserted-by":"publisher","first-page":"14182","DOI":"10.1021\/jacs.6b07120","article-title":"Automated\nSynthesis of Monodisperse Oligomers, Featuring Sequence Control and\nTailored Functionalization","volume":"138","author":"Martens","year":"2016","journal-title":"J. Am. Chem. Soc."},{"issue":"DOI","key":"2026072709074357100_cit47","doi-asserted-by":"publisher","first-page":"5616","DOI":"10.1039\/D2PY00883A","article-title":"Uniform soluble\nsupport for the large-scale synthesis of sequence-defined macromolecules","volume":"13","author":"De Franceschi","year":"2022","journal-title":"Polym. Chem."},{"key":"2026072709074357100_cit48","doi-asserted-by":"publisher","first-page":"2805","DOI":"10.1039\/D3SC04820A","article-title":"Telechelic sequence-defined\noligoamides: their step-economical synthesis, depolymerization and\nuse in polymer networks","volume":"15","author":"De Franceschi","year":"2024","journal-title":"Chem. Sci."},{"key":"2026072709074357100_cit49","doi-asserted-by":"publisher","first-page":"4193","DOI":"10.1039\/D1PY00662B","article-title":"Sequence-defined\noligoampholytes using hydrolytically stable vinyl sulfonamides: design\nand UCST behaviour11Electronic supplementary information (ESI) available","volume":"12","author":"Mertens","year":"2021","journal-title":"See Polym. Chem."},{"issue":"DOI","key":"2026072709074357100_cit50","doi-asserted-by":"publisher","first-page":"4271","DOI":"10.1039\/D0PY00645A","article-title":"Stereocontrolled,\nmulti-functional sequence-defined oligomers through automated synthesis","volume":"11","author":"Mertens","year":"2020","journal-title":"Polym. Chem."},{"key":"2026072709074357100_cit51","doi-asserted-by":"publisher","first-page":"7236","DOI":"10.1021\/jacs.2c00145","article-title":"Sequence-Defined\nMikto-Arm Star-Shaped Macromolecules","volume":"144","author":"Reith","year":"2022","journal-title":"J. Am.\nChem. Soc."},{"key":"2026072709074357100_cit52","doi-asserted-by":"publisher","first-page":"429","DOI":"10.3390\/molecules26020429","article-title":"Pretransitional Effects of the Isotropic\nLiquid\u2013Plastic Crystal Transition","volume":"26","author":"Drozd-Rzoska","year":"2021","journal-title":"Molecules"},{"key":"2026072709074357100_cit53","doi-asserted-by":"publisher","first-page":"450","DOI":"10.1021\/acsmaterialsau.3c00030","article-title":"Room-Temperature\nColumnar Liquid Crystals from Twisted and Macrocyclic 9,9\u2032-Bifluorenylidene\nMesogen with Ambipolar Carrier Transport Properties","volume":"3","author":"Xu","year":"2023","journal-title":"ACS Mater. Au"}],"container-title":["JACS Au"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/jacsau.6c00469","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jaaucr\/article-pdf\/6\/7\/3914\/65965412\/jacsau.6c00469.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jaaucr\/article-pdf\/6\/7\/3914\/65965412\/jacsau.6c00469.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,7,27]],"date-time":"2026-07-27T13:11:38Z","timestamp":1785157898000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jaaucr\/article\/6\/7\/3914\/5211299\/Tunable-Thermotropic-Liquid-Crystals-Using"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,7,15]]},"references-count":53,"journal-issue":{"issue":"7","published-online":{"date-parts":[[2026,7,15]]},"published-print":{"date-parts":[[2026,7,27]]}},"URL":"https:\/\/doi.org\/10.1021\/jacsau.6c00469","relation":{},"ISSN":["2691-3704"],"issn-type":[{"value":"2691-3704","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,7,15]]}}}