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However, there have been only a few reports on the brush-printing method. Here, we report the preparation of a uniaxially oriented film of a green light-emitting conductive polymer, poly\u00ad(9,9-dioctylfluorene-alt-benzothiadiazole) (F8BT). The fluorescence polarization ratio of the oriented F8BT films was as high as 11.3, and the average orientation factor reached 0.74 \u00b1 0.06. The orientation factor and the torsion angle of F8BT were visualized by two mappings of fluorescence and Raman spectral measurements by confocal spectromicroscopy, respectively. These two x-y mapping data with many pixels (\u223c750 pixels) were evaluated by x-y-z mapping of the film thickness at a single position and were used to reveal the three-dimensional (3D) orientation mechanism from a stochastic approach. Polarized green fluorescence originates from polymer chains uniaxially oriented along the brush direction. The high orientation for a film thickness &amp;lt; 100 nm is established by shear stress, faster capillary flow, and flow-induced chain extension for a thin solution film on a substrate. The high orientation factor was also demonstrated by a high brushing speed, whereas an optimized brushing speed existed. We found that this optimization is attributed to the property of a non-Newtonian fluid. By applying this brush-printing method to the fabrication of an optoelectrical device, polarized green electroluminescence was preliminarily demonstrated by the OLED assembled from an oriented F8BT film.<\/jats:p>","DOI":"10.1021\/acsami.0c08061","type":"journal-article","created":{"date-parts":[[2020,9,28]],"date-time":"2020-09-28T09:00:39Z","timestamp":1601283639000},"page":"46598-46608","source":"Crossref","is-referenced-by-count":19,"title":["Brush\nPrinting Creates Polarized Green Fluorescence:\n3D Orientation Mapping and Stochastic Analysis of Conductive Polymer\nFilms"],"prefix":"10.1021","volume":"12","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0702-1985","authenticated-orcid":true,"given":"Toshiki","family":"Sakata","sequence":"first","affiliation":[{"name":"Hiroshima University , , 1-3-1 Kagamiyama , , ,","place":["Higashi-Hiroshima, Hiroshima, Japan, 739-8526"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0556-9357","authenticated-orcid":true,"given":"Daisuke","family":"Kajiya","sequence":"additional","affiliation":[{"name":"Hiroshima University , , 1-3-1 Kagamiyama , , ,","place":["Higashi-Hiroshima, Hiroshima, Japan, 739-8526"]},{"name":"Hiroshima University , , 1-3-1 Kagamiyama , , ,","place":["Higashi-Hiroshima, Hiroshima, Japan, 739-8526"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2405-222X","authenticated-orcid":true,"given":"Ken-ichi","family":"Saitow","sequence":"additional","affiliation":[{"name":"Hiroshima University , , 1-3-1 Kagamiyama , , ,","place":["Higashi-Hiroshima, Hiroshima, Japan, 739-8526"]},{"name":"Hiroshima University , , 1-3-1 Kagamiyama , , ,","place":["Higashi-Hiroshima, Hiroshima, Japan, 739-8526"]},{"name":"Hiroshima University , , 1-3-1 Kagamiyama , , ,","place":["Higashi-Hiroshima, Hiroshima, Japan, 739-8526"]},{"name":"Hiroshima University , , 1-3-1 Kagamiyama , , ,","place":["Higashi-Hiroshima, Hiroshima, Japan, 739-8526"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2020,9,28]]},"reference":[{"key":"2026081714074431400_cit1","doi-asserted-by":"publisher","first-page":"5997","DOI":"10.1002\/adma.201302240","article-title":"25th Anniversary\nArticle: The Evolution of Electronic Skin (E-Skin): A Brief History,\nDesign Considerations, and Recent Progress","volume":"25","author":"Hammock","year":"2013","journal-title":"Adv. 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Mater.\nInterfaces"},{"key":"2026081714074431400_cit5","doi-asserted-by":"publisher","first-page":"4556","DOI":"10.1021\/cm049473l","article-title":"Electron Transport\nMaterials for Organic Light-Emitting Diodes","volume":"16","author":"Kulkarni","year":"2004","journal-title":"Chem. Mater."},{"key":"2026081714074431400_cit6","doi-asserted-by":"publisher","first-page":"4928","DOI":"10.1021\/am509047g","article-title":"Single-Junction Polymer Solar Cells\nwith Over 10% Efficiency by a Novel Two-Dimensional Donor-Acceptor\nConjugated Copolymer","volume":"7","author":"Liu","year":"2015","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"2026081714074431400_cit7","doi-asserted-by":"publisher","first-page":"18020","DOI":"10.1038\/natrevmats.2018.20","article-title":"All-Organic Thermally\nActivated Delayed Fluorescence Materials for Organic Light-Emitting\nDiodes","volume":"3","author":"Liu","year":"2018","journal-title":"Nat. Rev. Mater."},{"key":"2026081714074431400_cit8","doi-asserted-by":"publisher","first-page":"64","DOI":"10.1039\/C8TA09383K","article-title":"Conjugated\nMaterials Containing Dithieno\u00ad[3,2-b:2\u2032,3\u2032-d]\u00adpyrrole\nand Its Derivatives for Organic and Hybrid Solar Cell Applications","volume":"7","author":"Geng","year":"2019","journal-title":"J. Mater. Chem. A"},{"key":"2026081714074431400_cit9","doi-asserted-by":"publisher","first-page":"23","DOI":"10.1016\/j.jphotochem.2010.04.015","article-title":"Synthesis and Characterization of\nSquaric Acid Based\nNIR Dyes for Their Application Towards Dye-Sensitized Solar Cells","volume":"213","author":"Inoue","year":"2010","journal-title":"J. Photochem. Photobiol. A"},{"key":"2026081714074431400_cit10","doi-asserted-by":"publisher","first-page":"1802","DOI":"10.1021\/jz400723u","article-title":"Organic Solar\nCells beyond One Pair of Donor-Acceptor:\nTernary Blends and More","volume":"4","author":"Yang","year":"2013","journal-title":"J. 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Phys.\nLett."},{"key":"2026081714074431400_cit22","doi-asserted-by":"publisher","first-page":"6926","DOI":"10.1021\/ma049051x","article-title":"Formation of Single-Crystal-like Poly\u00ad(9,9-dioctylfluorene) Thin Film\nby the Friction-Transfer Technique with Subsequent Thermal Treatments","volume":"37","author":"Misaki","year":"2004","journal-title":"Macromolecules"},{"key":"2026081714074431400_cit23","doi-asserted-by":"publisher","first-page":"243503","DOI":"10.1063\/1.2142082","article-title":"Highly Polarized\nPolymer\nLight-Emitting Diodes Utilizing Friction-Transferred Poly\u00ad(9,9-dioctylfluorene)\nThin Films","volume":"87","author":"Misaki","year":"2005","journal-title":"Appl. Phys. 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Lett."},{"key":"2026081714074431400_cit32","doi-asserted-by":"publisher","first-page":"780","DOI":"10.1021\/nn800574f","article-title":"Controlling\nthe Orientation of Terraced Nanoscale \u201cRibbons\u201d\nof a Poly\u00ad(thiophene) Semiconductor","volume":"3","author":"DeLongchamp","year":"2009","journal-title":"ACS Nano"},{"key":"2026081714074431400_cit33","doi-asserted-by":"publisher","first-page":"16070","DOI":"10.1038\/ncomms16070","article-title":"Dynamic-Template-Directed Multiscale Assembly for Large-Area Coating\nof Highly-Aligned Conjugated Polymer Thin Films","volume":"8","author":"Mohammadi","year":"2017","journal-title":"Nat. Commun."},{"key":"2026081714074431400_cit34","doi-asserted-by":"publisher","first-page":"8394","DOI":"10.1038\/ncomms9394","article-title":"Macroscopic and High-Throughput Printing\nof Aligned\nNanostructured Polymer Semiconductors for MHz Large-area Electronics","volume":"6","author":"Bucella","year":"2015","journal-title":"Nat. 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Soc."},{"key":"2026081714074431400_cit48","doi-asserted-by":"publisher","first-page":"14493","DOI":"10.1021\/am5037862","article-title":"Regulating Charge Injection in Ambipolar\nOrganic Field-Effect\nTransistors by Mixed Self-Assembled Monolayers","volume":"6","author":"Xu","year":"2014","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"2026081714074431400_cit49","doi-asserted-by":"publisher","first-page":"1171","DOI":"10.1002\/adma.201103513","article-title":"Control of Efficiency,\nBrightness, and Recombination\nZone in Light-Emitting Field Effect Transistors","volume":"24","author":"Hsu","year":"2012","journal-title":"Adv. Mater."},{"key":"2026081714074431400_cit50","doi-asserted-by":"publisher","first-page":"2728","DOI":"10.1002\/adma.201104602","article-title":"Highly Efficient\nSingle-Layer Polymer Ambipolar Light-emitting Field-Effect Transistors","volume":"24","author":"Gwinner","year":"2012","journal-title":"Adv. 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Interfaces"},{"key":"2026081714074431400_cit54","doi-asserted-by":"publisher","first-page":"201102","DOI":"10.1063\/1.4921415","article-title":"White-Blue Electroluminescence from\na Si Quantum Dot Hybrid Light-Emitting Diode","volume":"106","author":"Xin","year":"2015","journal-title":"Appl. Phys. Lett."},{"key":"2026081714074431400_cit55","doi-asserted-by":"publisher","first-page":"15780","DOI":"10.1039\/C5NR02361K","article-title":"Si-nanocrystal\/P3HT\nHybrid Films with a 50- and 12-Fold\nEnhancement of Hole Mobility and Density: Films Prepared by Successive\nDrop Casting","volume":"7","author":"Kajiya","year":"2015","journal-title":"Nanoscale"},{"key":"2026081714074431400_cit56","doi-asserted-by":"publisher","first-page":"127130","DOI":"10.1063\/1.4939135","article-title":"Hole Mobility Enhancement of MEH-PPV\nFilm by Heat Treatment at Tg","volume":"5","author":"Kajiya","year":"2015","journal-title":"AIP Adv."},{"key":"2026081714074431400_cit57","doi-asserted-by":"publisher","first-page":"6881","DOI":"10.1021\/acsaem.8b01260","article-title":"Ultrapure Films of\nPolythiophene Derivatives are Born\non a Substrate by Liquid Flow","volume":"1","author":"Kajiya","year":"2018","journal-title":"ACS Appl. Energy\nMater."},{"key":"2026081714074431400_cit58","doi-asserted-by":"publisher","first-page":"22215","DOI":"10.1039\/C8NR05650A","article-title":"Field Enhancement of\nMoS2: Visualization\nof the Enhancement and Effect of the Number of Layers","volume":"10","author":"Sakamoto","year":"2018","journal-title":"Nanoscale"},{"key":"2026081714074431400_cit59","doi-asserted-by":"publisher","first-page":"437","DOI":"10.1021\/acsaelm.9b00673","article-title":"Spectral\nVisualization of Near-Infrared\nEnhancement in 2D Layered WS2","volume":"2","author":"Sakamoto","year":"2020","journal-title":"ACS\nAppl. Electron. Mater."},{"key":"2026081714074431400_cit60","doi-asserted-by":"publisher","first-page":"115338","DOI":"10.1103\/PhysRevB.77.115338","article-title":"Polarization Anisotropy\nDynamics for Thin Films of a Conjugated Polymer Aligned by Nanoimprinting","volume":"77","author":"Schmid","year":"2008","journal-title":"Phys. Rev. B"},{"key":"2026081714074431400_cit61","unstructured":"In\ngeneral, orientation\nfactor, Sa(=R\u22121R+1), obtained from absorption spectra can range\nfrom +1 to \u22121, where +1 and \u22121 correspond to R\u00a0(=A\u2225A\u22a5) = \u221e and 0, respectively. The former\nand latter situations are established as A\u22a5 = 0 and A\u2225 = 0, respectively.\nHere, the fluorescence polarization was treated as the orientation\nfactor Sf(=I\u2225\u2212I\u22a5I\u2225+I\u22a5). In general, Sf can\nalso range from +1 to \u22121. The former and latter situations\nare established as I\u22a5 = 0 and I\u2225 = 0, respectively, whose situation\nis the same as the orientation factor of Sa."},{"key":"2026081714074431400_cit62","unstructured":"To consider the alignment\nof polymer molecules that do not involve crystalline aggregates of\nF8BT, Sf was evaluated from the fluorescence\nspectra using a shorter wavelength (500\u2013525 nm). This is because\nthe component of the fluorescence spectra in a longer wavelength has\nbeen characterized as a component of crystalline aggregates for \u03c0-conjugated\npolymers in refs.\n                     63,64\n                   In fact, fluorene polymers show\nred-shifted PL by forming aggregates, e.g., refs.\n                     65,66\n                   The fluorescence spectra of F8BT have spectral components at longer\nwavelengths, which might be due to aggregate species. However, the\nspecies of longer wavelength have not been attributed to date, to\nthe best of our knowledge."},{"key":"2026081714074431400_cit63","doi-asserted-by":"publisher","first-page":"1038","DOI":"10.1038\/nmat3722","article-title":"A General Relationship\nBetween Disorder, Aggregation, and Charge Transport in Conjugated\npolymers","volume":"12","author":"Noriega","year":"2013","journal-title":"Nat. Mater."},{"key":"2026081714074431400_cit64","doi-asserted-by":"publisher","first-page":"114","DOI":"10.1021\/acs.jpclett.6b01641","article-title":"Temperature Induced Order-Disorder\nTransition in Solution of Conjugated Polymer Probed by Optical Spectroscopy","volume":"8","author":"Panzer","year":"2017","journal-title":"J. Phys. Chem. Lett."},{"key":"2026081714074431400_cit65","doi-asserted-by":"publisher","first-page":"439","DOI":"10.1002\/(SICI)1521-4044(199808)49:8&lt;439::AID-APOL439&gt;3.0.CO;2-A","article-title":"Chain Geometry,\nSolution\nAggregation and Enhanced Dichroism in the Liquid-Crystalline Conjugated\nPolymer Poly\u00ad(9,9-dioctylfluorene)","volume":"49","author":"Grell","year":"1998","journal-title":"Acta Polym."},{"key":"2026081714074431400_cit66","doi-asserted-by":"publisher","first-page":"961","DOI":"10.1002\/cphc.202000118","article-title":"Control of\nInterchain Morphology in the Formation of Polyfluorene Aggregates\non the Single-Molecule Level","volume":"21","author":"Wilhelm","year":"2020","journal-title":"ChemPhysChem"},{"key":"2026081714074431400_cit67","doi-asserted-by":"publisher","first-page":"12890","DOI":"10.1021\/ja051891j","article-title":"Effects\nof Packing Structure on the\nOptoelectronic and Charge Transport Properties in Poly\u00ad(9,9-di-n-octylfluorene-alt-benzothiadiazole)","volume":"127","author":"Donley","year":"2005","journal-title":"J. Am. Chem. Soc."},{"key":"2026081714074431400_cit68","first-page":"51","volume-title":"Fluid\nMechanics: Fundamentals and Applications, Second Edition","author":"C\u0327engel","year":"2010"},{"key":"2026081714074431400_cit69","doi-asserted-by":"publisher","first-page":"1334","DOI":"10.1021\/jp0118322","article-title":"Evaporation of a\nSessile Droplet on a substrate","volume":"106","author":"Hu","year":"2002","journal-title":"J. Phys. Chem.\nB."},{"key":"2026081714074431400_cit70","doi-asserted-by":"publisher","first-page":"308","DOI":"10.1038\/nature10344","article-title":"Suppression of the\nCoffee-Ring Effect by Shape-Dependent Capillary Interactions","volume":"476","author":"Yunker","year":"2011","journal-title":"Nature"},{"key":"2026081714074431400_cit71","doi-asserted-by":"publisher","first-page":"3963","DOI":"10.1021\/la047528s","article-title":"Analysis of the\nMicrofluid Flow in an Evaporating Sessile\nDroplet","volume":"21","author":"Hu","year":"2005","journal-title":"Langmuir"},{"key":"2026081714074431400_cit72","doi-asserted-by":"publisher","first-page":"417","DOI":"10.1016\/0095-8522(65)90022-X","article-title":"Rheology\nof Non-Newtonian Fluids: A New Flow Equation for Pseudoplastic Systems","volume":"20","author":"Cross","year":"1965","journal-title":"J. Colloid Sci."}],"container-title":["ACS Applied Materials &amp; Interfaces"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/acsami.0c08061","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/aamick\/article-pdf\/12\/41\/46598\/9291004\/am0c08061.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/aamick\/article-pdf\/12\/41\/46598\/9291004\/am0c08061.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,8,17]],"date-time":"2026-08-17T18:51:49Z","timestamp":1786992709000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/aamick\/article\/12\/41\/46598\/869448\/Brush-Printing-Creates-Polarized-Green"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2020,9,28]]},"references-count":72,"journal-issue":{"issue":"41","published-online":{"date-parts":[[2020,9,28]]},"published-print":{"date-parts":[[2020,10,14]]}},"URL":"https:\/\/doi.org\/10.1021\/acsami.0c08061","relation":{},"ISSN":["1944-8244","1944-8252"],"issn-type":[{"value":"1944-8244","type":"print"},{"value":"1944-8252","type":"electronic"}],"subject":[],"published":{"date-parts":[[2020,9,28]]}}}