Since to achieve high solar energy conversion efficiencies one has to optimize/maximize the interfacial light absorption, charge separation and surface redox reactions, the “interface design problem” requires fundamental understanding of (1) photo-excitation; (2) interfacial electron transfer (IET) and charge separation; (3) charge transport; (4) catalytic cycles mechanism. Clearly, characterization of all these processes necessitates interplaying of different disciplines: synthesis, quantum chemistry, solid-state physics, material chemistry, electrochemistry, and spectroscopy. Gathering together the most active experts in method development and predictive simulation of photo-induced catalytic processes on one side, and the leading experimentalists operating in the WOX field on the other side, we will discuss current methodological limitations and open issues toward a quantitative modelling of interfacial processes from first principles with the ambitious purpose of defining precise short-to-medium term goals toward higher device efficiencies.
A list of specific points and open issues we will address during the workshop follows:
• What are the methods enabling the description of interfacial ET allowing to propose solutions to suppress fast reverse electron transfer?
• Is it possible to combine experimental (spectroscopic) and theoretical approaches to elucidate IET kinetics?
• Do current methods enable a realistic description of the interface both in terms of morphology and electronic structure? How to optimally combine quantum and classical approaches for describing interface phenomena in WO?
• What and how can we learn from biological systems? What are the new methods enabling the description of spin and excited states of natural and bio-mimetic systems?
• Is there an efficient way of coupling state of the art wavefunction methods with a realistic model of the environment?
• Is it possible to reliably model the sequence of elementary steps involved in water oxidation, beyond the well-known approach of Norskov&Rossmeisl? Non-concerted PCETs and charged intermediates.
• What is the influence of the structure of the double layer at the electrode/electrolyte interface on the kinetics of water oxidation?
• What is the accuracy of available theoretical approaches to model thermodynamics and kinetics of water oxidation?
• What are the main limitation of current theoretical approaches (the treatment of dispersion effects, reaction barrier heights, and the underlying issue of self-interaction error)?
• Is it possible to efficiently combine electronic structure calculations with chemoinformatic approaches in view of a reliable and predictive computational screening of novel materials?
We remark that the workshop is focused on interfacial processes in the context of photo-induced water splitting, but very similar challenges are shared by (and limiting) many other technologies, such as the synthesis of chemicals and fuels, or the degradation of environmental pollutants assisted by solar energy. Although well focused on an important and active scientific field, the discussion and knowledge arising in this workshop can have a lasting impact also on broader areas of physics and chemistry.
How to apply: go the "Apply" page, in the section "Your Message" please provide a title and abstract of your work, specifying whether you prefer an oral or a poster contribution. We will notify the accepted participants by June 30th.