Shohei Shimizu, Jess M Clough, Christoph Weder, Yoshimitsu Sagara
{"title":"基于[2.2]副环环烷的铰链状机械致色团。","authors":"Shohei Shimizu, Jess M Clough, Christoph Weder, Yoshimitsu Sagara","doi":"10.1002/anie.202510114","DOIUrl":null,"url":null,"abstract":"<p><p>A hinge-like supramolecular mechanophore based on a [2.2]paracyclophane core and two excimer-forming 1,6-bis(phenylethynyl)pyrene luminophores is presented. Each luminophore shares one phenyl group with the [2.2]paracyclophane, resulting in a rigid and strained structure that forces the two luminophores into close proximity. As a consequence, the photoluminescence of the mechanophore in THF solution and in solid films of a polyurethane containing the new motif is dominated by excimer emission. Stretching the polymer films causes an easily discernible change from bright yellow excimer to blue-green monomer-dominated emission. The ratio of excimer to monomer emission intensities traces the nonlinear stress-strain curves of the polymer well and is a good indicator for the macroscopically applied force. The reversibility of the mechanoresponse, theoretical analyses, and reference experiments with a similar mechanophore in which the emitters and the [2.2]paracyclophane core are connected by flexible linkers support the conclusion that the mechanoactivation is caused by distorting the molecule into a bent, more open conformation and not the scission of covalent bonds. The operating principle was further confirmed by investigating a second hinge-like mechanophore based on a [2.2]paracyclophane core and 1,4-bis(phenylethynyl)benzene emitters.</p>","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202510114"},"PeriodicalIF":0.0000,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Hinge-Like Mechanochromic Mechanophores Based on [2.2]Paracyclophane.\",\"authors\":\"Shohei Shimizu, Jess M Clough, Christoph Weder, Yoshimitsu Sagara\",\"doi\":\"10.1002/anie.202510114\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>A hinge-like supramolecular mechanophore based on a [2.2]paracyclophane core and two excimer-forming 1,6-bis(phenylethynyl)pyrene luminophores is presented. Each luminophore shares one phenyl group with the [2.2]paracyclophane, resulting in a rigid and strained structure that forces the two luminophores into close proximity. As a consequence, the photoluminescence of the mechanophore in THF solution and in solid films of a polyurethane containing the new motif is dominated by excimer emission. Stretching the polymer films causes an easily discernible change from bright yellow excimer to blue-green monomer-dominated emission. The ratio of excimer to monomer emission intensities traces the nonlinear stress-strain curves of the polymer well and is a good indicator for the macroscopically applied force. The reversibility of the mechanoresponse, theoretical analyses, and reference experiments with a similar mechanophore in which the emitters and the [2.2]paracyclophane core are connected by flexible linkers support the conclusion that the mechanoactivation is caused by distorting the molecule into a bent, more open conformation and not the scission of covalent bonds. The operating principle was further confirmed by investigating a second hinge-like mechanophore based on a [2.2]paracyclophane core and 1,4-bis(phenylethynyl)benzene emitters.</p>\",\"PeriodicalId\":520556,\"journal\":{\"name\":\"Angewandte Chemie (International ed. in English)\",\"volume\":\" \",\"pages\":\"e202510114\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2025-06-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Angewandte Chemie (International ed. in English)\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1002/anie.202510114\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Angewandte Chemie (International ed. in English)","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1002/anie.202510114","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Hinge-Like Mechanochromic Mechanophores Based on [2.2]Paracyclophane.
A hinge-like supramolecular mechanophore based on a [2.2]paracyclophane core and two excimer-forming 1,6-bis(phenylethynyl)pyrene luminophores is presented. Each luminophore shares one phenyl group with the [2.2]paracyclophane, resulting in a rigid and strained structure that forces the two luminophores into close proximity. As a consequence, the photoluminescence of the mechanophore in THF solution and in solid films of a polyurethane containing the new motif is dominated by excimer emission. Stretching the polymer films causes an easily discernible change from bright yellow excimer to blue-green monomer-dominated emission. The ratio of excimer to monomer emission intensities traces the nonlinear stress-strain curves of the polymer well and is a good indicator for the macroscopically applied force. The reversibility of the mechanoresponse, theoretical analyses, and reference experiments with a similar mechanophore in which the emitters and the [2.2]paracyclophane core are connected by flexible linkers support the conclusion that the mechanoactivation is caused by distorting the molecule into a bent, more open conformation and not the scission of covalent bonds. The operating principle was further confirmed by investigating a second hinge-like mechanophore based on a [2.2]paracyclophane core and 1,4-bis(phenylethynyl)benzene emitters.