Toward On-Demand Polymorphic Transitions of Organic Crystals via Side Chain and Lattice Dynamics Engineering
Controlling polymorphism, namely, the occurrence of multiple crystal forms for a given compound, is still an open technological challenge that needs to be addressed for the reliable manufacturing of crystalline functional materials. Here, we devised a series of 13 organic crystals engineered to embody molecular fragments undergoing specific nanoscale motion anticipated to drive cooperative order-disorder phase transitions. By combining polarized optical microscopy coupled with a heating/cooling stage, differential scanning calorimetry, X-ray diffraction, low-frequency Raman spectroscopy, and calculations (density functional theory and molecular dynamics), we proved the occurrence of cooperative transitions in all the crystalline systems, and we demonstrated how both the molecular structure and lattice dynamics play crucial roles in these peculiar solid-to-solid transformations. These results introduce an efficient strategy to design polymorphic molecular crystalline materials endowed with specific molecular-scale lattice and macroscopic dynamics.
Authors
- Pancě Naumov (ORCID: https://orcid.org/0000-0003-2416-6569)
- Oren Elishav (ORCID: https://orcid.org/0000-0002-3062-9673)
- Durga Prasad Karothu (ORCID: https://orcid.org/0000-0001-5956-6496)
- Martina Volpi (ORCID: https://orcid.org/0009-0002-4020-9856)
- Rémy Jouclas (ORCID: https://orcid.org/0000-0002-1346-6817)
- Omer Yaffe (ORCID: https://orcid.org/0000-0003-4114-7968)
- Guillaume Schweicher (ORCID: https://orcid.org/0000-0002-6501-0790)
- Guangfeng Liu (ORCID: https://orcid.org/0000-0001-5029-3794)
- Navkiran Juneja (ORCID: https://orcid.org/0000-0003-2920-2733)
- Marco Saccone (ORCID: https://orcid.org/0000-0002-1768-0028)
- Iain McCulloch (ORCID: https://orcid.org/0000-0002-6340-7217)
- Luca Catalano (ORCID: https://orcid.org/0000-0002-1003-6512)
- Alan R. Kennedy (ORCID: https://orcid.org/0000-0003-3652-6015)
- Yves Henri Geerts (ORCID: https://orcid.org/0000-0002-2660-5767)
- Michael T. Ruggiero (ORCID: https://orcid.org/0000-0003-1848-2565)
- Rituraj Sharma (ORCID: https://orcid.org/0000-0002-7692-0108)
- Jie Liu (ORCID: https://orcid.org/0000-0002-1301-057X)
- T. Kyle Vanderlick (ORCID: https://orcid.org/0009-0001-8882-9694)
- Charles Chen (ORCID: https://orcid.org/0000-0002-2203-0433)
- Elumalai Gopi (ORCID: https://orcid.org/0000-0003-1860-4673)
- Hung‐Yang Chen (ORCID: https://orcid.org/0000-0001-8426-4254)
- Christian Ruzié
- Nicolas Klimis
Institutions
- University of Modena and Reggio Emilia (IT)
- Università degli Studi del Piemonte Orientale “Amedeo Avogadro” (IT)
- Université Libre de Bruxelles (BE)
- Macedonian Academy of Sciences and Arts (MK)
- University of Strathclyde (GB)
- Princeton University (US)
- Yale University (US)
- University of Warwick (GB)
- University of Oxford (GB)
- IPS Academy (IN)
- PlasticsEurope (BE)
- Changzhou University (CN)
- Plastic Electronics (Netherlands) (NL)
- International Solvay Institutes (BE)
- Imperial College London (GB)
- University of Rochester (US)
- Weizmann Institute of Science (IL)
- New York University (US)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2024-11-08
- DOI
- https://doi.org/10.1021/jacs.4c11289
- Citations
- 24
- Primary Topic
- Molecular Junctions and Nanostructures
- Type
- article
- Field-Weighted Citation Impact
- 5.01
Funders
- National Science Foundation
- Università Degli Studi di Modena e Reggio Emila
- New York University Abu Dhabi
- York University
- European Commission
- Weizmann Institute of Science
- Fonds De La Recherche Scientifique - FNRS
- Tamkeen
- Division of Materials Research
- H2020 European Research Council
- H2020 Marie Skłodowska-Curie Actions