Often, experimental techniques cannot dissect such processes at the nanoscale, which hinders a rational design of new devices with better performances. Thus, the application of computational modeling tools with atomistic resolution represents an ongoing revolution in materials design and device development.

In this context, this contribution will display how cutting edge DFT-based approaches allow to unveil the charge transfer mechanisms in several different electrochemical environments: (i) at hybrid interfaces considering promising Cu-based molecular redox couples in dye sensitized solar cell photoanodes [1,2], (ii) at heterogeneous interface in last generation perovskite solar cells [3] and (iii) ion-electrode interfaces in the context of nanostructured electrodes in sodium-ion batteries [4,5,6].

The results will provide new insights on the structure-property-functional relationships of different functional materials/interfaces and will pave the basis of new design principles for further improvements of the corresponding devices.

[1] AB Muñoz-García, I Benesperi , G. Boschloo, JJ Concepcion, JH Delcamp, EA Gibson, GJ Meyer, M Pavone, H Pettersson, A Hagfeldt, M Freitag

Dye-sensitized Solar Cells strike back

2021 Chemical Society Reviews 50, 12450-12550

[2] I Benesperi, H Michaels, T Edvinsson, M Pavone, MR Probert, P Waddel, AB Muñoz-García*, M Freitag

Dynamic dimer copper coordination redox shuttles

2022 Chem 8, 439-449 (Cover Article)

[3] A Pecoraro, A De Maria, P Delli Veneri, M Pavone, AB Muñoz-García*

Interfacial electronic features in methyl-ammonium lead iodide and p-type oxide heterostructures: new insights for inverted perovskite solar cells

2020 Physical Chemistry Chemical Physics 22, 28401-28413

[4] A Massaro, AB Muñoz-García, PP Prosini, C Gerbaldi, M Pavone

Unveiling Oxygen Redox Activity in P2-Type Na_xNi_0.25Mn_0.68O₂ High-Energy Cathode for Na-Ion Batteries

2021 ACS Energy Letters 6, 2470-2480

[5] A Massaro, A. Langella, AB Muñoz-García, M Pavone

First-principles insights on anion redox activity in Na_xFe_1/8Ni_1/8Mn_3/4O₂: Towards efficient high-energy cathodes for Na-ion batteries

2022 Journal of American Ceramic Society https://doi.org/10.1111/jace.18494

[6] A Massaro, AB Muñoz-García, P Maddalena, F Bella, G Meligrana, C Gerbaldi, M Pavone

First-principles study of Na insertion at TiO₂ anatase surfaces: new hints for Na-ion battery design

2020 Nanoscale Advances 2, 2745-2751