Combining experimental and computational methods to unravel the dynamical structure of photoelectrosynthetic interfaces

At photoelectrosynthetic interfaces, an electrochemical reaction is driven by excited charge-carriers from a semiconducting photoabsorber. Structure and composition of this interface determine both the electronic and electrochemical performance of devices, yet this structure is often highly dynamic both in the time-domain and upon applied potentials. We discuss the arising challenges from this dynamical nature and review recent approaches to gain an atomistic understanding of the involved processes, which increasingly involves a combination of experimental and computational methods. Bearing a similarity to solid-electrolyte interphase formation in batteries, their apprehension could help to develop functional passivation layers for high-performance photoelectrosynthetic devices.

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