The COSY webinars will be organized every three months (each webinar will consist of one lecture):
- March 25th, 2024
- September 18th, 2024
The 1st Webinar:
Moderator: Kaido Sillar (University of Tartu)
Speaker: María Pilar de Lara-Castells (Spanish National Research Council)
Speaker: María Pilar de Lara-Castells (AbinitFot Group, IFF-CSIC, Madrid)
An ab initio journey towards the molecular-level understanding of subnanometric metal clusters
Current advances in synthesizing and characterizing atomically precise monodisperse metal clusters (AMCs) at the subnanometer (Angstrom) scale have opened fascinating possibilities in new quantum materials research. Their quantized ‘molecule-like’ electronic structure showcases unique stability and physical and chemical properties different from those of nanoparticles and bulk materials. When integrated into materials that interact with environmental molecules and sunlight, AMCs may exhibit enhanced (photo)catalytic activity, electronic properties, and even optical behavior. Their tiny size (below 1 nm) makes free AMCs amenable to atomic-scale modelling using either density functional theory (DFT)-based approaches or methods at a higher level of ab initio theory, even including nonadiabatic (e.g., Jahn-Teller) effects. Surfacesupported AMCs can routinely be modelled using DFT-based single-reference methods, enabling real-time molecular dynamics simulations on the nanoseconds scale. The study of their optical properties is also possible using timedependent DFT or reduced density matrix theory. All these computational and theoretical efforts aim to achieve a molecular-level understanding of the stability and properties of AMCs as function of their chemical composition, size, and structural fluxionality in different thermodynamical conditions (temperature and pressure). These efforts bear the potential of guiding experiments to control AMCs functionalities for applications. In this webinar, the potential of state-of-the-art ab initio (DFT and beyond DFT) modelling will be emphasized through an illustrative overview of recent studies of free and surface-supported AMCs, including a comparison with experimental measurements [1-17]. Possible directions for methodological enhancements on the ab initio modelling of hybrid AMCs-materials systems will also be discussed with a focus on AMCs-support intermolecular interactions, including excited states.
References:
1. M. P. de Lara-Castells, J. Colloid Interface Sci. (2022), 612, 737.
2. M. P de Lara-Castells, C. Puzzarini, V. Bonačić-Koutecký, M. A. López-Quintela, S. Vajda, Editorial for the Themed Collection “Stability and properties of new-generation metal and metal-oxide clusters down to subnanometer scale” in Phys. Chem. Chem. Phys. (2023), 25, 15081.
3. B. Fernández, M. Pi, M. P. de Lara-Castells, Phys. Chem. Chem. Phys. (2023), 25, 16699.
4. A. O. Mitrushchenkov, M. P. de Lara-Castells, ChemPhysChem (2023), 24, e202300317
5. J. Garrido-Aldea, M. P. de Lara-Castells, Phys. Chem. Chem. Phys. (2022), 24, 24810.
6. B. Fernández, M. P. de Lara-Castells, Phys. Chem. Chem. Phys. (2022), 24, 26992.
7. L. L. Carroll, L. Moskaleva, M. P. de Lara-Castells, Phys. Chem. Chem. Phys. (2023), 25, 15729.
8. D. Buceta, S. Huseyinova, M. Cuerva, H. Lozano, L. J. Giovanetti, J. M. Ramallo-López, P. López-Caballero, A. Zanchet, A. O. Mitrushchenkov, A. W. Hauser, G. Barone, C. HuckIriart, C. Escudero, J. C. Hernández-Garrido, J. J. Calvino, M. López-Haro, M. P. de Lara-Castells, F. G. Requejo, M. Arturo López-Quintela. Chem. A European J. (2023), 29, e202301517.
9. M. P. de Lara-Castells, A. W. Hauser, J. M. Ramallo-López, D. Buceta, L. J. Giovanetti, M. A. López-Quintela, F. G. Requejo, J. Mater. Chem. A (2019), 7, 7489.
10. P. López-Caballero, J. M. Ramallo-López, L. J. Giovanetti, D. Buceta, S. Miret-Artés, M. A. López-Quintela, F. G. Requejo, J. Mater. Chem. A (2020), 8, 6842.
11. P. López-Caballero, A. W. Hauser, M. P. de Lara-Castells, J. Phys. Chem. C (2019), 123, 23064.
12. M. P. de Lara-Castells, S. Miret-Artés, Europhys. News (2022), 53, 7-9.
13. A. O. Mitrushchenkov, A. Zanchet, A. W. Hauser, J. Phys. Chem A (2021), 125,9143.
14. P. López-Caballero, R. Garsed, M. P. de Lara-Castells, ACS Omega (2021), 24, 16165
15. P. López-Caballero, S. Miret-Artés, A. O. Mitrushchenkov, M. P. de Lara-Castells, J. Chem. Phys. (2020), 153, 164702.
16. A. Zanchet, P. López-Caballero, A. O. Mitrushchenkov, D. Buceta, M. A. LópezQuintela, A. W. Hauser, M. P. de Lara-Castells, J. Phys. Chem. C (2019), 123, 27064.
17. M. P. de Lara-Castells, C. Cabrillo, D. A. Micha, A. O. Mitrushchenkov, T. Vazhapilly, Phys. Chem. Chem. Phys. (2018), 29, 19110.
