Linear-scaling approaches to charge- and energy-transfer in (extended) photo-electro-chemical interfaces

DIPC Seminars

Gilberto Teobaldi, University of Liverpool, UK
Donostia International Physics Center (DIPC).Paseo Manuel de Lardizabal, 4 (nearby the Facultad de Quimica), Donostia
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Linear-scaling approaches to charge- and energy-transfer in (extended) photo-electro-chemical interfaces **Linear-scaling approaches to charge- and energy-transfer in (extended) photo-electro-chemical interfaces** Gilberto Teobaldi, _a_ David D. O'Regan, _b_ Nicholas D. M. Hine, _c,d_ Arash A. Mostofi _d_ _a_ _Stephenson Institute for Renewable Energy, Department of Chemistry, University of Liverpool, L69 7ZD Liverpool, UK._ _ _ _b_ _Theory and Simulation of Materials, École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland._ _c_ _Cavendish Laboratory, University of Cambridge, J. J. Thomson Avenue, Cambridge CB3 0HE, UK_ _._ _d_ _The Thomas Young Centre and the Department of Materials, Imperial College London, London SW7 2AZ, UK_ _._ In the pursuit of a more sustainable energy-economy, great efforts are being directed towards improved, industrially viable photocatalytic, photovoltaics, electrochemical energy conversion (fuel cells) and storage (batteries) devices. Atomic-scale understanding of the different materials and interfaces constituting such devices is crucial for the development of novel solutions. This, in turn, requires the possibility of accessing the atomic-scale parameters governing the thermodynamics and kinetics of charge (energy) transfer processes at the device interfaces. Recently, very encouraging results have appeared regarding the potential of constrained Density Functional Theory (cDFT) for the study of charge (energy) transfer and chemical reactivity [1]. Here we present the implementation of cDFT in the ONETEP program [2], based on the existing framework of tensorial invariance and self-consistency for non-orthogonal projectors [3,4]. The linear-scaling (LS) nature of the cDFT implementation and its compatibility with the LS-DFT+U functionality in ONETEP [5] open up for cDFT(+U) simulation of systems up to a few thousands of atoms on academically available hardware. This should make the method useful for the study of the extended photo- and electro-chemical interfaces present in photocatalysts, solar cells, fuel cells, and batteries. **References** 1 B. Kaduk _et. al._ _Chem._ _Rev._ **112** , 321 (2012). 2 C.-K. Skylaris _et al._ , _J. Chem._ _Phys._ , 2005, **122** , 084119 (2005). 3 D. D. O'Regan _et al._ , _Phys._ _Rev. B_ , 2010, **82** , 081102(R) (2010). 4 D. D. O'Regan _et al._ , _Phys._ _Rev. B_ , 2011, **83** , 245124 (2011). 5 D. D. O'Regan _et al._ , _Phys._ _Rev. B_ , 2011, **85** , 085107 (2011).