First principle calculations; Lattice modes; Low-frequency Raman; Mechanistics; Normal modes; Order/disorder phase transition; Pentacenes; Raman measurements; Raman peak; Temperature dependent; Materials Science (all); Physical and Theoretical Chemistry; General Materials Science
Abstract :
[en] We combine temperature-dependent low-frequency Raman measurements and first-principles calculations to obtain a mechanistic understanding of the order-disorder phase transition of 2,7-di-tert-butylbenzo[b]benzo[4,5]thieno[2,3-d]thiophene (ditBu-BTBT) and 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS-pentacene) semiconducting amphidynamic crystals. We identify the lattice normal modes associated with the phase transition by following the position and width of the Raman peaks with temperature and identifying peaks that exhibit nonlinear dependence toward the phase transition temperature. Our findings are interpreted according to the "hardcore mode" model previously used to describe order-disorder phase transitions in inorganic and hybrid crystals with a Brownian sublattice. Within the framework of this model, ditBu-BTBT exhibits an ideal behavior where only one lattice mode is associated with the phase transition. TIPS-pentacene deviates strongly from the model due to strong interactions between lattice modes. We discuss the origin of the different behaviors and suggest side-chain engineering as a tool to control polymorphism in amphidynamic crystals.
Disciplines :
Chemistry
Author, co-author :
Asher, Maor ; Department of Chemical and Biological Physics, Weizmann Institute of Science, Rehovot76100, Israel
Bardini, Marco ; Université de Mons - UMONS > Faculté des Science > Service de Chimie des matériaux nouveaux
Catalano, Luca; Laboratoire de Chimie des Polymères, Université Libre de Bruxelles (ULB), 1050Brussels, Belgium
Jouclas, Rémy; Laboratoire de Chimie des Polymères, Université Libre de Bruxelles (ULB), 1050Brussels, Belgium
Schweicher, Guillaume ; Laboratoire de Chimie des Polymères, Université Libre de Bruxelles (ULB), 1050Brussels, Belgium
Liu, Jie ; Laboratoire de Chimie des Polymères, Université Libre de Bruxelles (ULB), 1050Brussels, Belgium
Korobko, Roman ; Department of Chemical and Biological Physics, Weizmann Institute of Science, Rehovot76100, Israel
Cohen, Adi; Department of Chemical and Biological Physics, Weizmann Institute of Science, Rehovot76100, Israel
Geerts, Yves ; Université de Mons - UMONS ; Laboratoire de Chimie des Polymères, Université Libre de Bruxelles (ULB), 1050Brussels, Belgium ; International Solvay Institutes for Physics and Chemistry, 1050Brussels, Belgium
Beljonne, David ; Université de Mons - UMONS > Faculté des Science > Service de Chimie des matériaux nouveaux
Yaffe, Omer ; Department of Chemical and Biological Physics, Weizmann Institute of Science, Rehovot76100, Israel
Language :
English
Title :
Mechanistic View on the Order-Disorder Phase Transition in Amphidynamic Crystals.
R400 - Institut de Recherche en Science et Ingénierie des Matériaux Complexys
Funders :
Fédération Wallonie-Bruxelles H2020 Marie Sklodowska-Curie Actions Fondation Francqui - Stichting Fonds De La Recherche Scientifique - FNRS H2020 European Research Council
Funding text :
We thank Lior Segev for software development. O.Y. acknowledges funding from the European Research Counsel (850041-ANHARMONIC). Y.G. is thankful to the Belgian National Fund for Scientific Research (FNRS) for financial support through research projects Pi-Fast (No T.0072.18), Pi-Chir (No T.0094.22), DIFFRA (No U.G001.19), 2D to 3D (No O.005018F), and CHISUB (No O.00322). Financial support from the French Community of Belgian (ARC No. 20061) is also acknowledged. L.C. thanks the H2020 MSCA COFUND IF@ULB program for financial support (Grant Agreement 801505). G.S. is a FNRS Research Associate and acknowledges financial support from the Francqui Foundation (Francqui Start-Up Grant). D.B. is a FNRS research director. The work in Mons has been supported by the Consortium des Équipements de Calcul Intensif (CÉCI), funded by the Fonds de la Recherche Scientifique de Belgique (F.R.S.-FNRS) under Grant No. 2.5020.11. This project has received funding from the European Union’s Horizon 2020 research and innovation program under Marie Skodowska-Curie Grant Agreements No. 811284 (UHMob) and No. 801505.
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