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Here we show a crystalline phase (CP) of adamantyl\u2010substituted pyrene that exhibits one\u2010dimensional, translationally aligned columnar \u03c0\u2010stacks enabled by dispersion\u2010assisted adamantyl \u201cclamps\u201d. Single\u2010crystal x\u2010ray diffraction reveals an exceptionally short interplanar separation of 3.297(3) \u00c5 at 100 K. Energy\u2010decomposition analysis shows that the adamantyl substituents provide larger dispersion stabilization relative to their Pauli penalty, rationalizing the formation of the zero\u2010offset \u03c0\u2010columns. The solution\u2010to\u2010crystal color shift is exceptionally large (\u0394\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>obs<\/jats:sub>\n                    = \u22120.761\u00a0eV), which exceeds exciton coupling contributions and is dominated by intermolecular orbital interactions captured by a frontier crystal orbital (FCO) model. To the best of our knowledge, both the translationally zero\u2010offset \u03c0\u2010columns and the large crystallization\u2010induced red shift are unprecedented for ambient\u2010pressure CPs of neutral, closed\u2010shell hydrocarbon PAHs.\n                  <\/jats:p>","DOI":"10.1002\/anie.1681939","type":"journal-article","created":{"date-parts":[[2026,8,22]],"date-time":"2026-08-22T09:05:12Z","timestamp":1787389512000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Dispersion\u2010Clamped Crystalline Supramolecular Columnar \u03c0\u2010Stacks of Adamantyl\u2010Substituted Pyrenes"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0937-4431","authenticated-orcid":false,"given":"Kazutaka","family":"Shoyama","sequence":"first","affiliation":[{"name":"Institut f\u00fcr Organische Chemie Universit\u00e4t W\u00fcrzburg W\u00fcrzburg Germany"},{"name":"Center for Nanosystems Chemistry (CNC) Universit\u00e4t W\u00fcrzburg W\u00fcrzburg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,8,22]]},"reference":[{"key":"e_1_2_6_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr040084k"},{"key":"e_1_2_6_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.9b00320"},{"key":"e_1_2_6_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/adom.202002251"},{"key":"e_1_2_6_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201002307"},{"key":"e_1_2_6_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.7b00581"},{"key":"e_1_2_6_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.5b00190"},{"key":"e_1_2_6_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr990322p"},{"key":"e_1_2_6_9_1","doi-asserted-by":"publisher","DOI":"10.1039\/D4CS00804A"},{"key":"e_1_2_6_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.199523111"},{"key":"e_1_2_6_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr030070z"},{"key":"e_1_2_6_12_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586\u2010024\u201008299\u20108"},{"key":"e_1_2_6_13_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41557\u2010021\u201000861\u20105"},{"key":"e_1_2_6_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010019\u201011098\u20109"},{"key":"e_1_2_6_15_1","doi-asserted-by":"publisher","DOI":"10.1107\/S0108768189003794"},{"key":"e_1_2_6_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202300094"},{"key":"e_1_2_6_17_1","doi-asserted-by":"publisher","DOI":"10.1039\/D0SC02667K"},{"key":"e_1_2_6_18_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c03169"},{"key":"e_1_2_6_19_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.6c03371"},{"key":"e_1_2_6_20_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja00170a016"},{"key":"e_1_2_6_21_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c13291"},{"key":"e_1_2_6_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/chem.201804139"},{"key":"e_1_2_6_23_1","doi-asserted-by":"publisher","DOI":"10.1021\/cg401637a"},{"key":"e_1_2_6_24_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja0383118"},{"key":"e_1_2_6_25_1","doi-asserted-by":"publisher","DOI":"10.1021\/jp0573689"},{"key":"e_1_2_6_26_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.organomet.6b00781"},{"key":"e_1_2_6_27_1","doi-asserted-by":"publisher","DOI":"10.1142\/S1088424617500705"},{"key":"e_1_2_6_28_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010021\u201027324\u20102"},{"key":"e_1_2_6_29_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature10367"},{"key":"e_1_2_6_30_1","doi-asserted-by":"publisher","DOI":"10.1002\/chem.70949"},{"key":"e_1_2_6_31_1","unstructured":"Deposition Numbers 2544930\u20132544941 contain the supplementary crystallographic data for this paper. 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