Light Induced Charge Transfer from Transition-metal Doped Aluminium Clusters to Carbon Dioxide

Journal Of Physical Chemistry A 125,27, 5878 - 5885 (2021)

Light Induced Charge Transfer from Transition-metal Doped Aluminium Clusters to Carbon Dioxide

Alexandra Göbel, Angel Rubio, Johannes Lischner

Charge transfer between molecules and catalysts plays a critical role in determining the efficiency and yield of photo-chemical catalytic processes. In this paper, we study light-induced electron transfer between transition metal doped aluminium clusters and CO2 molecules using first-principles time-dependent density-functional theory. Specifically, we carry out calculations for a range of dopants (Zr, Mn, Fe, Ru, Co, Ni and Cu) and find that the resulting systems fall into two categories: Cu- and Fe-doped clusters exhibit no ground state charge transfer, weak CO2 adsorption and light-induced electron transfer into the CO2. In all other systems, we observe ground state electron transfer into the CO2 resulting in strong adsorption and predominantly light-induced electron back-transfer from the CO2 into the cluster. These findings pave the way towards a rational design of atomically precise aluminium photo-catalysts.

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http://dx.doi.org/https://doi.org/10.1021/acs.jpca.1c02621
arxiv
http://arxiv.org/abs/2103.14405.pdf
Notes
This work was supported by the European Research Council (ERC-2015-AdG694097), the Cluster of Excellence ‘Advanced Imaging of Matter’ (AIM), Grupos Consolidados (IT1249- 19), SFB925 ”Light induced dynamics and control of correlated quantum systems” and by the Deutsche Forschungsgemeinschaft (DFG) through the Research Training Group -Quantum Mechanical Materials Modelling - GRK 2247. The Flatiron Institute is a division of the Simons Foundation.

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