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In this work, in situ linear absorption and single-shot transient absorption measurements are used to characterize the molecular aggregation of copper phthalocyanine (CuPc) during film deposition, revealing an intermediate stage during deposition when the molecules have formed H-aggregates but have yet to agglomerate into a herringbone structure. Experiments with supersaturated solutions of CuPc showed that the steps of aggregation can be separated, with H-aggregates first forming in solution followed by columns of H-aggregates, of unknown length, coming together to form nanoribbons. Films cast from solutions of supersaturated CuPc have a more crystalline structure and fits to transient absorption spectra showed that exciton\u2013exciton annihilation becomes more rapid compared to regular films. In addition to presenting a method to control exciton diffusion lengths in films that tend to adopt a herringbone packing structure, this study also provides a framework for how in situ spectroscopies can be used to design new aggregate structures and control exciton dynamics.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c01584","type":"journal-article","created":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T16:02:49Z","timestamp":1786377769000},"page":"9523-9529","source":"Crossref","is-referenced-by-count":0,"title":["Tuning the Crystallinity\nof the Herringbone Packing\nStructure in Phthalocyanine Nanoribbons Using in Situ Spectroscopies"],"prefix":"10.1021","volume":"17","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-6993-4584","authenticated-orcid":true,"given":"Alyssa Y.","family":"Paulson","sequence":"first","affiliation":[{"name":"University of Oregon , , , ,","place":["Eugene, Oregon, United States, 97403"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3368-9978","authenticated-orcid":true,"given":"Zachary S.","family":"Walbrun","sequence":"additional","affiliation":[{"name":"University of Oregon , , , ,","place":["Eugene, Oregon, United States, 97403"]},{"name":"University of Wisconsin\u2500River Falls , , , ,","place":["River Falls, Wisconsin, United States, 54022"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weston L.","family":"Bodle","sequence":"additional","affiliation":[{"name":"University of Oregon , , , ,","place":["Eugene, Oregon, United States, 97403"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nicholas M.","family":"Frainey","sequence":"additional","affiliation":[{"name":"University of Oregon , , , ,","place":["Eugene, Oregon, United States, 97403"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6867-1968","authenticated-orcid":true,"given":"Cathy Y.","family":"Wong","sequence":"additional","affiliation":[{"name":"University of Oregon , , , ,","place":["Eugene, Oregon, United States, 97403"]},{"name":"University of Oregon , , , ,","place":["Eugene, Oregon, United States, 97403"]},{"name":"University of Oregon , , , ,","place":["Eugene, Oregon, United States, 97403"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,10]]},"reference":[{"issue":"17","key":"2026082008264635500_cit1","doi-asserted-by":"publisher","first-page":"6548","DOI":"10.1021\/acs.chemmater.8b05293","article-title":"Large Crystalline\nDomains and an Enhanced Exciton Diffusion Length Enable Efficient\nOrganic Solar Cells","volume":"31","author":"Zhang","year":"2019","journal-title":"Chem. 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