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Herein, we report the formation of the simplest coupled system, the Chl\u2005a dimer, tagged with a quaternary ammonium ion by electrospray ionization. Based on action spectroscopic studies in\u2005vacuo, the dimer complexes were found to absorb 50\u201370\u2005meV to the red of the monomers under the same conditions. First\u2010principles calculations predict shifts that somewhat depend on the relative orientation of the two Chl units, namely 50 and 30\u2005meV for structures where the Chl rings are stacked and unstacked, respectively. Our work demonstrates that Chl association alone can produce a large portion of the color shift observed in photosynthetic macromolecular assemblies.<\/jats:p>","DOI":"10.1002\/anie.201601979","type":"journal-article","created":{"date-parts":[[2016,4,13]],"date-time":"2016-04-13T11:31:45Z","timestamp":1460547105000},"page":"6248-6251","source":"Crossref","is-referenced-by-count":20,"title":["On the Exciton Coupling between Two Chlorophyll Pigments in the Absence of a Protein Environment: Intrinsic Effects Revealed by Theory and Experiment"],"prefix":"10.1002","volume":"55","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5522-4808","authenticated-orcid":false,"given":"Bruce F.","family":"Milne","sequence":"first","affiliation":[{"name":"CFisUC, Department of Physics University of Coimbra  Rua Larga 3004-516 Coimbra Portugal"}]},{"given":"Christina","family":"Kj\u00e6r","sequence":"additional","affiliation":[{"name":"Department of Physics and Astronomy Aarhus University  Ny Munkegade DK-8000 Aarhus C Denmark"}]},{"given":"J\u00f8rgen","family":"Houm\u00f8ller","sequence":"additional","affiliation":[{"name":"Department of Physics and Astronomy Aarhus University  Ny Munkegade DK-8000 Aarhus C Denmark"}]},{"given":"Mark H.","family":"Stockett","sequence":"additional","affiliation":[{"name":"Department of Physics and Astronomy Aarhus University  Ny Munkegade DK-8000 Aarhus C Denmark"}]},{"given":"Yoni","family":"Toker","sequence":"additional","affiliation":[{"name":"Institute of Nanotechnology and Advanced Materials Bar-Ilan University  Ramat-Gan 5290002 Israel"}]},{"given":"Angel","family":"Rubio","sequence":"additional","affiliation":[{"name":"Max Planck Institute for the Structure and Dynamics of Matter  Luruper Chaussee 149 22761 Hamburg Germany"},{"name":"Nano-Bio Spectroscopy Group and ETSF Universidad del Pa\u00eds Vasco, CFM CSIC-UPV\/EHU-MPC &amp; DIPC  20018 San Sebasti\u00e1n Spain"}]},{"given":"Steen Br\u00f8ndsted","family":"Nielsen","sequence":"additional","affiliation":[{"name":"Department of Physics and Astronomy Aarhus University  Ny Munkegade DK-8000 Aarhus C Denmark"}]}],"member":"311","published-online":{"date-parts":[[2016,4,13]]},"reference":[{"key":"e_1_2_2_1_1","doi-asserted-by":"publisher","DOI":"10.1039\/c2ee23013e"},{"key":"e_1_2_2_2_1","doi-asserted-by":"publisher","DOI":"10.1039\/C1FD00078K"},{"key":"e_1_2_2_3_1","doi-asserted-by":"publisher","DOI":"10.1146\/annurev.physchem.040808.090259"},{"key":"e_1_2_2_4_1","doi-asserted-by":"publisher","DOI":"10.1007\/978-1-4615-2033-7"},{"key":"e_1_2_2_5_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5CP03392F"},{"key":"e_1_2_2_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja072818r"},{"key":"e_1_2_2_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/jz500478w"},{"key":"e_1_2_2_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200905061"},{"key":"e_1_2_2_8_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.200905061"},{"key":"e_1_2_2_9_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5CP05063D"},{"key":"e_1_2_2_10_1","doi-asserted-by":"publisher","DOI":"10.1039\/c3cp44362k"},{"key":"e_1_2_2_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpca.5b04835"},{"key":"e_1_2_2_12_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5CP03611A"},{"key":"e_1_2_2_13_1","doi-asserted-by":"publisher","DOI":"10.1063\/1.3637048"},{"key":"e_1_2_2_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201410899"},{"key":"e_1_2_2_14_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201410899"},{"key":"e_1_2_2_15_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5CP01513H"},{"key":"e_1_2_2_16_1","doi-asserted-by":"publisher","DOI":"10.1085\/jgp.24.5.565"},{"key":"e_1_2_2_17_1","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.75.5.2301"},{"key":"e_1_2_2_18_1","doi-asserted-by":"publisher","DOI":"10.1016\/0003-9861(83)90396-X"},{"key":"e_1_2_2_19_1","doi-asserted-by":"publisher","DOI":"10.1111\/j.1432-1033.1979.tb04250.x"},{"key":"e_1_2_2_20_1","doi-asserted-by":"publisher","DOI":"10.1039\/C6CP00104A"},{"key":"e_1_2_2_21_1","doi-asserted-by":"publisher","DOI":"10.1021\/jp110120c"},{"key":"e_1_2_2_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201206213"},{"key":"e_1_2_2_22_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201206213"},{"key":"e_1_2_2_23_1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.52.997"},{"key":"e_1_2_2_24_1","doi-asserted-by":"publisher","DOI":"10.1063\/1.2831900"},{"key":"e_1_2_2_25_1","doi-asserted-by":"publisher","DOI":"10.1039\/b822941d"},{"key":"e_1_2_2_26_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja311400t"},{"key":"e_1_2_2_27_1","doi-asserted-by":"publisher","DOI":"10.1104\/pp.65.5.814"},{"key":"e_1_2_2_28_1","doi-asserted-by":"publisher","DOI":"10.1007\/s00775-006-0164-z"},{"key":"e_1_2_2_29_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature02373"},{"key":"e_1_2_2_30_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature02200"}],"container-title":["Angewandte Chemie International Edition"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/api.wiley.com\/onlinelibrary\/tdm\/v1\/articles\/10.1002%2Fanie.201601979","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/api.wiley.com\/onlinelibrary\/tdm\/v1\/articles\/10.1002%2Fanie.201601979","content-type":"unspecified","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.201601979","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2023,9,16]],"date-time":"2023-09-16T01:46:10Z","timestamp":1694828770000},"score":1,"resource":{"primary":{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/10.1002\/anie.201601979"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2016,4,13]]},"references-count":33,"journal-issue":{"issue":"21","published-print":{"date-parts":[[2016,5,17]]}},"alternative-id":["10.1002\/anie.201601979"],"URL":"https:\/\/doi.org\/10.1002\/anie.201601979","archive":["Portico"],"relation":{},"ISSN":["1433-7851","1521-3773"],"issn-type":[{"type":"print","value":"1433-7851"},{"type":"electronic","value":"1521-3773"}],"subject":[],"published":{"date-parts":[[2016,4,13]]}}}