{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,2,20]],"date-time":"2026-02-20T05:03:09Z","timestamp":1771563789918,"version":"3.50.1"},"reference-count":34,"publisher":"Springer Science and Business Media LLC","issue":"1","license":[{"start":{"date-parts":[[2022,12,28]],"date-time":"2022-12-28T00:00:00Z","timestamp":1672185600000},"content-version":"tdm","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0"},{"start":{"date-parts":[[2022,12,28]],"date-time":"2022-12-28T00:00:00Z","timestamp":1672185600000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0"}],"funder":[{"DOI":"10.13039\/501100004329","name":"Javna Agencija za Raziskovalno Dejavnost RS","doi-asserted-by":"publisher","award":["P1-0125"],"award-info":[{"award-number":["P1-0125"]}],"id":[{"id":"10.13039\/501100004329","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001871","name":"Funda\u00e7\u00e3o para a Ci\u00eancia e a Tecnologia","doi-asserted-by":"publisher","award":["UID\/CTM\/04540\/2019"],"award-info":[{"award-number":["UID\/CTM\/04540\/2019"]}],"id":[{"id":"10.13039\/501100001871","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001871","name":"Funda\u00e7\u00e3o para a Ci\u00eancia e a Tecnologia","doi-asserted-by":"publisher","award":["PTDC\/CTM-REF\/30529\/2017"],"award-info":[{"award-number":["PTDC\/CTM-REF\/30529\/2017"]}],"id":[{"id":"10.13039\/501100001871","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":["link.springer.com"],"crossmark-restriction":false},"short-container-title":["Sci Rep"],"abstract":"<jats:title>Abstract<\/jats:title><jats:p>Local molecular ordering in liquids has attracted a lot of interest from researchers investigating crystallization, but is still poorly understood on the molecular scale. Classical nucleation theory (CNT), a macroscopic thermodynamic description of condensation, has shortcomings when dealing with clusters consisting of tens of molecules. Cluster formation and local order fluctuations in liquid media are difficult to study due to the limited spatial resolution of electron- and photon-imaging methods. We used NMR relaxometry to demonstrate the existence of dynamic clusters with short-range orientational order in nominally isotropic liquids consisting of elongated molecules. We observed clusters in liquids where the local ordering is driven by polar, steric, and hydrogen-bond interactions between the molecules. In the case of a liquid crystal, measuring the local orientational order fluctuations allowed us to observe the size of these clusters diverging when approaching the phase transition from the isotropic to the nematic phase. These fluctuations are described in terms of rotational elasticity as a consequence of the correlated reorientations of the neighbouring molecules. Our quantitative observations of the dynamic clusters in liquids, numbering about ten or fewer molecules, indicate that this is a general phenomenon in various types of liquids.<\/jats:p>","DOI":"10.1038\/s41598-022-27187-7","type":"journal-article","created":{"date-parts":[[2022,12,28]],"date-time":"2022-12-28T18:05:06Z","timestamp":1672250706000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Observing short-range orientational order in small-molecule liquids"],"prefix":"10.1038","volume":"12","author":[{"given":"Anton","family":"Gradi\u0161ek","sequence":"first","affiliation":[]},{"given":"Toma\u017e","family":"Apih","sequence":"additional","affiliation":[]},{"given":"Maria J.","family":"Beira","sequence":"additional","affiliation":[]},{"given":"Carlos","family":"Cruz","sequence":"additional","affiliation":[]},{"given":"Susete N.","family":"Fernandes","sequence":"additional","affiliation":[]},{"given":"Helena M.","family":"Godinho","sequence":"additional","affiliation":[]},{"given":"Pedro J.","family":"Sebasti\u00e3o","sequence":"additional","affiliation":[]}],"member":"297","published-online":{"date-parts":[[2022,12,28]]},"reference":[{"issue":"11","key":"27187_CR1","doi-asserted-by":"publisher","first-page":"6663","DOI":"10.1021\/acs.cgd.6b00794","volume":"16","author":"S Karthika","year":"2016","unstructured":"Karthika, S., Radhakrishnan, T. K. & Kalaichelvi, P. A review of classical and nonclassical nucleation theories. Cryst. Growth Des. 16(11), 6663\u20136681 (2016).","journal-title":"Cryst. Growth Des."},{"issue":"12","key":"27187_CR2","doi-asserted-by":"publisher","first-page":"5007","DOI":"10.1021\/cg1011633","volume":"10","author":"PG Vekilov","year":"2010","unstructured":"Vekilov, P. G. Nucleation. Cryst. Growth Des. 10(12), 5007\u20135019 (2010).","journal-title":"Cryst. Growth Des."},{"issue":"1","key":"27187_CR3","doi-asserted-by":"publisher","first-page":"1","DOI":"10.1038\/ncomms6598","volume":"5","author":"M Sleutel","year":"2014","unstructured":"Sleutel, M., Lutsko, J., Van Driessche, A. E., Dur\u00e1n-Olivencia, M. A. & Maes, D. Observing classical nucleation theory at work by monitoring phase transitions with molecular precision. Nat. Commun. 5(1), 1\u20138 (2014).","journal-title":"Nat. Commun."},{"issue":"44","key":"27187_CR4","first-page":"443002","volume":"29","author":"F Zhang","year":"2017","unstructured":"Zhang, F. Nonclassical nucleation pathways in protein crystallization. J. Phys.: Condens. Matter 29(44), 443002 (2017).","journal-title":"J. Phys.: Condens. Matter"},{"issue":"5334","key":"27187_CR5","doi-asserted-by":"publisher","first-page":"1975","DOI":"10.1126\/science.277.5334.1975","volume":"277","author":"PRT Wolde","year":"1997","unstructured":"Wolde, P. R. T. & Frenkel, D. Enhancement of protein crystal nucleation by critical density fluctuations. Science 277(5334), 1975\u20131978 (1997).","journal-title":"Science"},{"issue":"4","key":"27187_CR6","doi-asserted-by":"publisher","first-page":"450","DOI":"10.1038\/s41563-019-0514-1","volume":"19","author":"Z Ou","year":"2020","unstructured":"Ou, Z., Wang, Z., Luo, B., Luijten, E. & Chen, Q. Kinetic pathways of crystallization at the nanoscale. Nat. Mater. 19(4), 450\u2013455 (2020).","journal-title":"Nat. Mater."},{"issue":"5","key":"27187_CR7","doi-asserted-by":"publisher","first-page":"621","DOI":"10.1021\/ar800217x","volume":"42","author":"D Erdemir","year":"2009","unstructured":"Erdemir, D., Lee, A. Y. & Myerson, A. S. Nucleation of crystals from solution: Classical and two-step models. Acc. Chem. Res. 42(5), 621\u2013629 (2009).","journal-title":"Acc. Chem. Res."},{"issue":"2","key":"27187_CR8","doi-asserted-by":"publisher","first-page":"763","DOI":"10.1021\/jacs.8b11972","volume":"141","author":"J Yang","year":"2019","unstructured":"Yang, J. et al. Amorphous-phase-mediated crystallization of Ni nanocrystals revealed by high-resolution liquid-phase electron microscopy. J. Am. Chem. Soc. 141(2), 763\u2013768 (2019).","journal-title":"J. Am. Chem. Soc."},{"key":"27187_CR9","doi-asserted-by":"crossref","DOI":"10.1093\/oso\/9780198520245.001.0001","volume-title":"The Physics of Liquid Crystals","author":"PG de Gennes","year":"1993","unstructured":"de Gennes, P. G. & Prost, J. The Physics of Liquid Crystals (Oxford University Press, 1993)."},{"key":"27187_CR10","doi-asserted-by":"publisher","first-page":"969","DOI":"10.1103\/PhysRevLett.23.969","volume":"23","author":"R Blinc","year":"1969","unstructured":"Blinc, R., Hogenboom, D. L., O\u2019Reilly, D. E. & Peterson, E. M. Spin relaxation and self-diffusion in liquid crystals. Phys. Rev. Lett. 23, 969 (1969).","journal-title":"Phys. Rev. Lett."},{"key":"27187_CR11","doi-asserted-by":"publisher","first-page":"638","DOI":"10.1103\/PhysRevLett.29.638","volume":"29","author":"SK Ghosh","year":"1972","unstructured":"Ghosh, S. K., Tettamanti, E. & Indovina, P. L. Dynamical behavior of a nematic liquid crystal just above the nematic-isotropic transition from spin-lattice relaxation. Phys. Rev. Lett. 29, 638 (1972).","journal-title":"Phys. Rev. Lett."},{"key":"27187_CR12","doi-asserted-by":"publisher","first-page":"610","DOI":"10.1139\/p75-077","volume":"53","author":"RY Dong","year":"1975","unstructured":"Dong, R. Y., Tomchuk, E. & Bock, E. Proton spin relaxation study of order fluctuations above the nematic-isotropic transition in the liquid crystal MBBA: II. Coherent and incoherent scattering. Can. J. Phys. 53, 610\u2013616 (1975).","journal-title":"Can. J. Phys."},{"key":"27187_CR13","doi-asserted-by":"publisher","first-page":"91","DOI":"10.1103\/PhysRevLett.25.91","volume":"25","author":"B Cabane","year":"1970","unstructured":"Cabane, B. & Clark, W. G. Effects of order and fluctuations on the N 14 NMR in a liquid crystal. Phys. Rev. Lett. 25, 91 (1970).","journal-title":"Phys. Rev. Lett."},{"key":"27187_CR14","doi-asserted-by":"publisher","first-page":"2282","DOI":"10.1139\/p76-272","volume":"54","author":"JJ Visintainer","year":"1976","unstructured":"Visintainer, J. J., Bock, E., Dong, R. Y. & Tomchuk, E. A proton FFT study of the aromatic and alkyl motions in the liquid crystal CBOOA: Orientational order fluctuations in the isotropic phase. Can. J. Phys. 54, 2282\u20132286 (1976).","journal-title":"Can. J. Phys."},{"key":"27187_CR15","doi-asserted-by":"publisher","first-page":"139","DOI":"10.1070\/PU1994v037n02ABEH000007","volume":"37","author":"AY Val\u2019kov","year":"1994","unstructured":"Val\u2019kov, A. Y., Romanov, V. P. & Shalaginov, A. N. Fluctuations and light scattering in liquid crystals. Phys. Usp. 37, 139\u2013183 (1994).","journal-title":"Phys. Usp."},{"key":"27187_CR16","doi-asserted-by":"publisher","first-page":"101","DOI":"10.1080\/15421407608083875","volume":"33","author":"RY Dong","year":"1976","unstructured":"Dong, R. Y., Tomchuk, E., Visintainer, J. J. & Bock, E. 14N NMR study of order fluctuations in the isotropic phase of liquid crystals. Mol. Cryst. Liq. Cryst. 33, 101\u2013111 (1976).","journal-title":"Mol. Cryst. Liq. Cryst."},{"key":"27187_CR17","doi-asserted-by":"publisher","first-page":"503","DOI":"10.1103\/PhysRevLett.25.503","volume":"25","author":"TW Stinson","year":"1970","unstructured":"Stinson, T. W. & Litster, J. D. Pretransitional phenomena in the isotropic phase of a nematic liquid crystal. Phys. Rev. Lett. 25, 503 (1970).","journal-title":"Phys. Rev. Lett."},{"key":"27187_CR18","doi-asserted-by":"publisher","first-page":"688","DOI":"10.1103\/PhysRevLett.30.688","volume":"30","author":"TW Stinson","year":"1973","unstructured":"Stinson, T. W. & Litster, J. D. Correlation range of fluctuations of short-range order in the isotropic phase of a liquid crystal. Phys. Rev. Lett. 30, 688 (1973).","journal-title":"Phys. Rev. Lett."},{"key":"27187_CR19","doi-asserted-by":"publisher","first-page":"2214","DOI":"10.1021\/jp111408n","volume":"115","author":"J Zhang","year":"2011","unstructured":"Zhang, J., Su, J. & Guo, H. An atomistic simulation for 4-Cyano-4\u2019-pentylbiphenyl and its homologue with a reoptimized force field. J. Phys. Chem. B 115, 2214\u20132227 (2011).","journal-title":"J. Phys. Chem. B"},{"key":"27187_CR20","doi-asserted-by":"publisher","first-page":"204901","DOI":"10.1063\/1.4804270","volume":"138","author":"MF Palermo","year":"2013","unstructured":"Palermo, M. F., Pizzirusso, A., Muccioli, L. & Zannoni, C. An atomistic description of the nematic and smectic phases of 4-n-octyl-4\u2019 cyanobiphenyl (8CB). J. Chem. Phys. 138, 204901 (2013).","journal-title":"J. Chem. Phys."},{"key":"27187_CR21","doi-asserted-by":"publisher","first-page":"1573","DOI":"10.1080\/026782900750037149","volume":"27","author":"MJ Cook","year":"2000","unstructured":"Cook, M. J. & Wilson, M. R. Simulation studies of dipole correlation in the isotropic liquid phase. Liq. Cryst. 27, 1573\u20131583 (2000).","journal-title":"Liq. Cryst."},{"key":"27187_CR22","doi-asserted-by":"publisher","first-page":"625","DOI":"10.1039\/c3fd00111c","volume":"167","author":"CA Angell","year":"2014","unstructured":"Angell, C. A. & Zhao, Z. Fluctuations, clusters, and phase transitions in liquids, solutions, and glasses: From metastable water to phase change memory materials. Faraday Discuss. 167, 625\u2013641 (2014).","journal-title":"Faraday Discuss."},{"issue":"1","key":"27187_CR23","doi-asserted-by":"publisher","first-page":"1","DOI":"10.1038\/s41598-019-50077-4","volume":"9","author":"AV Malm","year":"2019","unstructured":"Malm, A. V. & Corbett, J. C. Improved dynamic light scattering using an adaptive and statistically driven time resolved treatment of correlation data. Sci. Rep. 9(1), 1\u201311 (2019).","journal-title":"Sci. Rep."},{"issue":"11","key":"27187_CR24","doi-asserted-by":"publisher","first-page":"695","DOI":"10.1038\/nnano.2011.161","volume":"6","author":"N De Jonge","year":"2011","unstructured":"De Jonge, N. & Ross, F. M. Electron microscopy of specimens in liquid. Nat. Nanotechnol. 6(11), 695\u2013704 (2011).","journal-title":"Nat. Nanotechnol."},{"key":"27187_CR25","doi-asserted-by":"publisher","DOI":"10.1007\/978-1-4612-1954-5","volume-title":"Nuclear Magnetic Resonance of Liquid Crystals","author":"RY Dong","year":"1997","unstructured":"Dong, R. Y. Nuclear Magnetic Resonance of Liquid Crystals (Springer, 1997)."},{"key":"27187_CR26","volume-title":"The Principles of Nuclear Magnetism","author":"A Abragam","year":"1961","unstructured":"Abragam, A. The Principles of Nuclear Magnetism (Oxford University Press, 1961)."},{"key":"27187_CR27","doi-asserted-by":"publisher","first-page":"358","DOI":"10.1039\/9781788012966","volume-title":"Field-Cycling NMR Relaxometry: Instrumentation, Model Theories and Applications","author":"R Kimmich","year":"2018","unstructured":"Kimmich, R. Field-Cycling NMR Relaxometry: Instrumentation, Model Theories and Applications 358\u2013384 (Royal Society of Chemistry, 2018)."},{"key":"27187_CR28","doi-asserted-by":"publisher","first-page":"14348","DOI":"10.1021\/jp206429j","volume":"115","author":"PJ Sebasti\u00e3o","year":"2011","unstructured":"Sebasti\u00e3o, P. J. et al. Fast field-cycling NMR relaxometry study of chiral and nonchiral nematic liquid crystals. J. Phys. Chem. B 115, 14348\u201314358 (2011).","journal-title":"J. Phys. Chem. B"},{"key":"27187_CR29","doi-asserted-by":"publisher","first-page":"5600","DOI":"10.1021\/jp502542q","volume":"118","author":"A Gradi\u0161ek","year":"2014","unstructured":"Gradi\u0161ek, A. et al. 1H\u20132H cross-relaxation study in a partially deuterated nematic liquid crystal. J. Phys. Chem. B 118, 5600\u20135607 (2014).","journal-title":"J. Phys. Chem. B"},{"key":"27187_CR30","doi-asserted-by":"publisher","first-page":"1175","DOI":"10.1051\/jphys:019810042080117500","volume":"42","author":"JD Bunning","year":"1981","unstructured":"Bunning, J. D., Faber, T. E. & Sherrell, P. L. The Frank constants of nematic 5CB at atmospheric pressure. J. Phys. 42, 1175\u20131182 (1981).","journal-title":"J. Phys."},{"key":"27187_CR31","doi-asserted-by":"publisher","first-page":"129","DOI":"10.1142\/9789814273671_0005","volume-title":"Nuclear Magnetic Resonance Spectroscopy of Liquid Crystals","year":"2009","unstructured":"Dong, R. (ed.) Nuclear Magnetic Resonance Spectroscopy of Liquid Crystals 129\u2013167 (World Scientific Co., 2009)."},{"issue":"6","key":"27187_CR32","doi-asserted-by":"publisher","first-page":"061704","DOI":"10.1103\/PhysRevE.74.061704","volume":"74","author":"J Zhang","year":"2006","unstructured":"Zhang, J., Ferraz, A., Ribeiro, A. C., Sebasti\u01ceo, P. J. & Dong, R. Y. Deuterium nuclear-magnetic-resonance study of a chiral smectic-C* phase. Phys. Rev. E 74(6), 061704 (2006).","journal-title":"Phys. Rev. E"},{"issue":"4047","key":"27187_CR33","doi-asserted-by":"publisher","first-page":"393","DOI":"10.1126\/science.177.4047.393","volume":"177","author":"PW Anderson","year":"1972","unstructured":"Anderson, P. W. More is different: Broken symmetry and the nature of the hierarchical structure of science. Science 177(4047), 393\u2013396 (1972).","journal-title":"Science"},{"key":"27187_CR34","doi-asserted-by":"publisher","first-page":"445","DOI":"10.1007\/978-1-4613-0883-6_24","volume-title":"Self-Organizing Systems","author":"PW Anderson","year":"1987","unstructured":"Anderson, P. W. & Stein, D. L. Broken symmetry, emergent properties, dissipative structures, life. In Self-Organizing Systems 445\u2013457 (Springer, 1987)."}],"container-title":["Scientific Reports"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.nature.com\/articles\/s41598-022-27187-7.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/www.nature.com\/articles\/s41598-022-27187-7","content-type":"text\/html","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/www.nature.com\/articles\/s41598-022-27187-7.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2023,12,3]],"date-time":"2023-12-03T17:13:52Z","timestamp":1701623632000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.nature.com\/articles\/s41598-022-27187-7"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2022,12,28]]},"references-count":34,"journal-issue":{"issue":"1","published-online":{"date-parts":[[2022,12]]}},"alternative-id":["27187"],"URL":"https:\/\/doi.org\/10.1038\/s41598-022-27187-7","relation":{},"ISSN":["2045-2322"],"issn-type":[{"value":"2045-2322","type":"electronic"}],"subject":[],"published":{"date-parts":[[2022,12,28]]},"assertion":[{"value":"20 November 2022","order":1,"name":"received","label":"Received","group":{"name":"ArticleHistory","label":"Article History"}},{"value":"27 December 2022","order":2,"name":"accepted","label":"Accepted","group":{"name":"ArticleHistory","label":"Article History"}},{"value":"28 December 2022","order":3,"name":"first_online","label":"First Online","group":{"name":"ArticleHistory","label":"Article History"}},{"value":"The authors declare no competing interests.","order":1,"name":"Ethics","group":{"name":"EthicsHeading","label":"Competing interests"}}],"article-number":"22500"}}