Interplay of structural and electronic properties and their impact on thin films of metal-free organic radicals (Prolongation).
Experimental Condensed Matter Physics
Final Report Abstract
The project and its extension concentrate on radical thin films. I have identified and refined the growth protocols for various radicals and multi-radicals, enabling their evaporation while preserving their radical nature. Additionally, I have explored the influence of different functional groups on thin film properties. During these years, I have addressed a variety of aspects, demonstrating the feasibility of using radicals in fields ranging from quantum technologies to spintronics. By using primarily X-ray-based techniques, including at synchrotron facilities, I have linked structural, electronic, and magnetic properties. I have also examined how the interaction strength between the (multi-)radicals and the substrate affects the interface formation, growth modes, and film processes of the radical thin films. Furthermore, I have focused on evaluating film stability, which is crucial for understanding their chemistry when exposed to air prior to performing electron spin resonance (ESR) spectroscopy—a traditional (ex-situ) technique used for radicals—and for determining film stability in environments simulating working devices. I have developed a protocol to study the effects of air exposure on radical thin films and utilized this method. Finally, I have conducted and interpreted X-ray magnetic circular dichroism (XMCD) investigations, revealing the interplay between structure and magnetic behavior in radical thin films.
Link to the final report
https://chemrxiv.org/engage/chemrxiv/article-details/67c062fdfa469535b9297fcd
Publications
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Interfacing a Potential Purely Organic Molecular Quantum Bit with a Real-Life Surface. ACS Applied Materials & Interfaces, 11(1), 1571-1578.
Ciccullo, Francesca; Calzolari, Arrigo; Bader, Katharina; Neugebauer, Petr; Gallagher, Nolan M.; Rajca, Andrzej; van Slageren, Joris & Casu, Maria Benedetta
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Thermally and Magnetically Robust Triplet Ground State Diradical. Journal of the American Chemical Society, 141(11), 4764-4774.
Gallagher, Nolan; Zhang, Hui; Junghoefer, Tobias; Giangrisostomi, Erika; Ovsyannikov, Ruslan; Pink, Maren; Rajca, Suchada; Casu, Maria Benedetta & Rajca, Andrzej
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Exploiting the versatile alkyne-based chemistry for expanding the applications of a stable triphenylmethyl organic radical on surfaces. Chemical Science, 11(2), 516-524.
de Sousa, J. Alejandro; Bejarano, Francesc; Gutiérrez, Diego; Leroux, Yann R.; Nowik-Boltyk, Ewa Malgorzata; Junghoefer, Tobias; Giangrisostomi, Erika; Ovsyannikov, Ruslan; Casu, Maria Benedetta; Veciana, Jaume; Mas-Torrent, Marta; Fabre, Bruno; Rovira, Concepció & Crivillers, Núria
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Stability of radical-functionalized gold surfaces by self-assembly and on-surface chemistry. Chemical Science, 11(34), 9162-9172.
Junghoefer, Tobias; Nowik-Boltyk, Ewa Malgorzata; de Sousa, J. Alejandro; Giangrisostomi, Erika; Ovsyannikov, Ruslan; Chassé, Thomas; Veciana, Jaume; Mas-Torrent, Marta; Rovira, Concepció; Crivillers, Núria & Casu, Maria Benedetta
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Challenges in Controlled Thermal Deposition of Organic Diradicals. Chemistry of Materials, 33(6), 2019-2028.
Junghoefer, Tobias; Gallagher, Nolan M.; Kolanji, Kubandiran; Giangrisostomi, Erika; Ovsyannikov, Ruslan; Chassé, Thomas; Baumgarten, Martin; Rajca, Andrzej; Calzolari, Arrigo & Casu, Maria Benedetta
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From radical to triradical thin film processes: the Blatter radical derivatives. Journal of Materials Chemistry C, 9(33), 10787-10793.
Calzolari, Arrigo; Rajca, Andrzej & Casu, Maria Benedetta
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Metal-free radicals show magnetic behaviour
Maria Benedetta Casu
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Overcoming the challenges in controlled thermal deposition of organic diradicals
Maria Benedetta Casu
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Synthesis and Thin Films of Thermally Robust Quartet (S = 3/2) Ground State Triradical. Journal of the American Chemical Society, 143(14), 5508-5518.
Shu, Chan; Pink, Maren; Junghoefer, Tobias; Nadler, Elke; Rajca, Suchada; Casu, Maria Benedetta & Rajca, Andrzej
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X-ray analysis points way to flexible and transparent magnets
Maria Benedetta Casu
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High-Spin ( S = 1) Blatter-Based Diradical with Robust Stability and Electrical Conductivity. Journal of the American Chemical Society, 144(13), 6059-6070.
Zhang, Shuyang; Pink, Maren; Junghoefer, Tobias; Zhao, Wenchao; Hsu, Sheng-Ning; Rajca, Suchada; Calzolari, Arrigo; Boudouris, Bryan W.; Casu, Maria Benedetta & Rajca, Andrzej
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Magnetic behavior in metal-free radical thin films. Chem, 8(3), 801-814.
Junghoefer, Tobias; Calzolari, Arrigo; Baev, Ivan; Glaser, Mathias; Ciccullo, Francesca; Giangrisostomi, Erika; Ovsyannikov, Ruslan; Kielgast, Fridtjof; Nissen, Matz; Schwarz, Julius; Gallagher, Nolan M.; Rajca, Andrzej; Martins, Michael & Casu, Maria Benedetta
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The magnetic behavior of metal-free organic materials. Science X
Maria Benedetta Casu
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Long-Term Degradation Mechanisms in Application-Implemented Radical Thin Films. ACS Applied Materials & Interfaces, 15(25), 30935-30943.
Nowik-Boltyk, Ewa Malgorzata; Junghoefer, Tobias; Glaser, Mathias; Giangrisostomi, Erika; Ovsyannikov, Ruslan; Zhang, Shuyang; Shu, Chan; Rajca, Andrzej; Calzolari, Arrigo & Casu, M. Benedetta
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Thermally Ultrarobust S = 1/2 Tetrazolinyl Radicals: Synthesis, Electronic Structure, Magnetism, and Nanoneedle Assemblies on Silicon Surface. Journal of the American Chemical Society, 145(24), 13335-13346.
Yang, Zhimin; Pink, Maren; Nowik-Boltyk, Ewa Malgorzata; Lu, Shutian; Junghoefer, Tobias; Rajca, Suchada; Stoll, Stefan; Casu, Maria Benedetta & Rajca, Andrzej
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First step in radical spintronics
Maria Benedetta Casu
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Radical‐Induced Changes in Transition Metal Interfacial Magnetic Properties: A Blatter Derivative on Polycrystalline Cobalt. Angewandte Chemie International Edition.
Nowik‐Boltyk, Ewa Malgorzata; Junghoefer, Tobias; Giangrisostomi, Erika; Ovsyannikov, Ruslan; Shu, Chan; Rajca, Andrzej; Droghetti, Andrea & Casu, M. Benedetta
