Toward On-Demand Polymorphic Transitions of Organic Crystals via Side Chain and Lattice Dynamics Engineering

Luca Catalano; Rituraj Sharma; Durga Prasad Karothu; Marco Saccone; Oren Elishav; Charles Chen; Navkiran Juneja; Martina Volpi; Rémy Jouclas; Hung Yang Chen; Jie Liu; Guangfeng Liu; Elumalai Gopi; Christian Ruzié; Nicolas Klimis; Alan R. Kennedy; T. Kyle Vanderlick; Iain McCulloch; Michael T. Ruggiero; Panče Naumov; Guillaume Schweicher; Omer Yaffe; Yves H. Geerts

doi:10.1021/jacs.4c11289

Toward On-Demand Polymorphic Transitions of Organic Crystals via Side Chain and Lattice Dynamics Engineering

Luca Catalano^*, Rituraj Sharma, Durga Prasad Karothu, Marco Saccone, Oren Elishav, Charles Chen, Navkiran Juneja, Martina Volpi, Rémy Jouclas, Hung Yang Chen, Jie Liu, Guangfeng Liu, Elumalai Gopi, Christian Ruzié, Nicolas Klimis, Alan R. Kennedy, T. Kyle Vanderlick, Iain McCulloch, Michael T. Ruggiero, Panče NaumovGuillaume Schweicher, Omer Yaffe, Yves H. Geerts

^*Corresponding author for this work

Department of Chemical and Biological Physics

Research output: Contribution to journal › Article › peer-review

1 Citation (Scopus)

Abstract

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.

Original language	English
Pages (from-to)	31911-31919
Number of pages	9
Journal	Journal of the American Chemical Society
Volume	146
Issue number	46
Early online date	8 Nov 2024
DOIs	https://doi.org/10.1021/jacs.4c11289
Publication status	Published - 20 Nov 2024

Funding

L.C. thanks the University of Modena and Reggio Emilia for financial support. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 801505. R.S. acknowledges the Weizmann Institute of Science, Israel, for funding. G.L. thanks the Jiangsu Specially Appointed Professor Foundation. M.T.R. thanks the USA National Science Foundation for support (DMR-2348765). P.N. thanks New York University Abu Dhabi for financial support. This material is based upon work supported by Tamkeen under NYUAD RRC Grant No. CG011. G.S. is a Belgian National Fund for Scientific Research (FNRS) Research Associate.

All Science Journal Classification (ASJC) codes

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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Catalano, L., Sharma, R., Karothu, D. P., Saccone, M., Elishav, O., Chen, C., Juneja, N., Volpi, M., Jouclas, R., Chen, H. Y., Liu, J., Liu, G., Gopi, E., Ruzié, C., Klimis, N., Kennedy, A. R., Vanderlick, T. K., McCulloch, I., Ruggiero, M. T., ... Geerts, Y. H. (2024). Toward On-Demand Polymorphic Transitions of Organic Crystals via Side Chain and Lattice Dynamics Engineering. Journal of the American Chemical Society, 146(46), 31911-31919. https://doi.org/10.1021/jacs.4c11289

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abstract = "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.",

author = "Luca Catalano and Rituraj Sharma and Karothu, {Durga Prasad} and Marco Saccone and Oren Elishav and Charles Chen and Navkiran Juneja and Martina Volpi and R{\'e}my Jouclas and Chen, {Hung Yang} and Jie Liu and Guangfeng Liu and Elumalai Gopi and Christian Ruzi{\'e} and Nicolas Klimis and Kennedy, {Alan R.} and Vanderlick, {T. Kyle} and Iain McCulloch and Ruggiero, {Michael T.} and Pan{\v c}e Naumov and Guillaume Schweicher and Omer Yaffe and Geerts, {Yves H.}",

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Catalano, L, Sharma, R, Karothu, DP, Saccone, M, Elishav, O, Chen, C, Juneja, N, Volpi, M, Jouclas, R, Chen, HY, Liu, J, Liu, G, Gopi, E, Ruzié, C, Klimis, N, Kennedy, AR, Vanderlick, TK, McCulloch, I, Ruggiero, MT, Naumov, P, Schweicher, G, Yaffe, O & Geerts, YH 2024, 'Toward On-Demand Polymorphic Transitions of Organic Crystals via Side Chain and Lattice Dynamics Engineering', Journal of the American Chemical Society, vol. 146, no. 46, pp. 31911-31919. https://doi.org/10.1021/jacs.4c11289

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AU - Catalano, Luca

AU - Sharma, Rituraj

AU - Karothu, Durga Prasad

AU - Saccone, Marco

AU - Elishav, Oren

AU - Chen, Charles

AU - Juneja, Navkiran

AU - Volpi, Martina

AU - Jouclas, Rémy

AU - Chen, Hung Yang

AU - Liu, Jie

AU - Liu, Guangfeng

AU - Gopi, Elumalai

AU - Ruzié, Christian

AU - Klimis, Nicolas

AU - Kennedy, Alan R.

AU - Vanderlick, T. Kyle

AU - McCulloch, Iain

AU - Ruggiero, Michael T.

AU - Naumov, Panče

AU - Schweicher, Guillaume

AU - Yaffe, Omer

AU - Geerts, Yves H.

PY - 2024/11/20

Y1 - 2024/11/20

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AB - 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.

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ER -

Toward On-Demand Polymorphic Transitions of Organic Crystals via Side Chain and Lattice Dynamics Engineering

Abstract

Funding

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