Theoretical insights for the design of transition metal emitters and lanthanide single-molecule magnets

Abstract:

This talk presents recent examples on joint experimental/theoretical studies about lanthanide single molecule magnets and copper(I) TADF emitters developed in our group. In the topic of lanthanide magnetism, out group has developed several methods to predict tunnelling demagnetization times,[1] determine the most relevant demagnetization mechanism [2,3] and to interpret magnetic anisotropy [4]. We discuss how these tools help to comprehend molecular demagnetization processes in detail and allow to obtain critical information to design new systems with tailored properties.
The second part of the talk deals with photophysical properties of copper(I) complexes exhibiting thermally activated delayed fluorescence (TADF). We highlight two recent studies performed in collaboration with IMDEA researchers, where the photophysical properties of a family of six structurally related copper(I) complexes was determined by time resolved photoluminescence spectroscopy in a broad temperature range (1.5-300K). Structural, spectroscopic and theoretical results allowed us to identify the key structural parameters contributing to TADF.[5] Furthermore an experimental protocol to disentangle radiative and non-radiative decay is proposed.[6]

References
[1] Aravena D, J. Phys. Chem. Lett. 9, 5327−5333 (2018)
[2] Castro-Alvarez A, Gil Y, Llanos L, Aravena D, Inorg. Chem. Front., 7, 2478 – 2486 (2020).
[3] Y, Quesada-Moreno MM, Palacios MA, Gómez-Coca S, Colacio E, Ruiz E, Aravena D, Inorg. Chem. Front. 12, 2856 - 2871 (2025)
[4] Gil Y, Aravena D, Dalton Trans., 53, 2207 - 2217 (2024)
[5] Sun C, Llanos L, Arce P, Oliver A, Wannemacher R, Cabanillas-Gonzalez J, Lemus L, Aravena D, Chem. Mater., 33, 6383–6393 (2021)
[6] Llanos L, Staforelli S, Oliver AG, Moscoso FG, Wannemacher R, Cabanillas-Gonzalez J, Lemus L, Aravena D, Angew. Chem. Int. Ed. (2025) DOI: 10.1002/anie.202501407