Interrogating the CISS effect in chiral and paramagnetic organic radicals: the impact of the molecular spin over the total spin polarization De Sousa, J. Alejandro Mayorga-Burrezo, Paula Míguez Lago, Sandra Catalán-Toledo, José Ramos-Tomás, Raúl Ortuño Guzmán, Ana María A. Zotti, linda Palacios, Juan José G. Campaña, Araceli Veciana, Jaume Crivillers, Núria Continuous research on new chiral molecular materials brings new exciting properties to the field of molecular electronics. The discovery of the chirality-induced spin selectivity (CISS) effect has expanded the list of applications for chiral structures, opening promising avenues for their exploitation in molecular spintronics. In this work, the persistent propeller-like organic perchlorotriphenylmethyl (PTM) radical is investigated as a potential spin filter combining chirality and paramagnetism. In particular, two different PTM derivatives, mono- and bis-functionalized, with one or two terminal alkyne groups have been used for the preparation of enantioenriched solid-state assemblies. The analysis of their chiroptical properties reveals that the functionalization does not play a crucial role in their final conformational stability and highlights the dissimilarities of the racemization barriers in solution and solid states. Spindependent electrochemical and charge transport measurements of enantioenriched PTM-based selfassembled monolayers did not reveal the existence of the CISS effect. Density functional theory quantum transport calculations show that the most dominant contribution to the spin polarization would not be CISS-related polarization, but the one intrinsically associated with the radical spin. Nevertheless, at room temperature this contribution is affected by thermal fluctuations averaging to a net zero spin polarization. 2024-07-29T10:14:37Z 2024-07-29T10:14:37Z 2024-06-18 journal article De Sousa, J.A. et. al. J. Mater. Chem. C, 2024. [https://doi.org/10.1039/d4tc01389a] https://hdl.handle.net/10481/93550 10.1039/d4tc01389a eng http://creativecommons.org/licenses/by-nc/4.0/ open access Atribución-NoComercial 4.0 Internacional Royal Society of Chemistry