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

Abstract

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.

arXiv comment10 pages, 4 figures. Accepted version

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Cited by in corpus (3)

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• Observation and control of potential-dependent surface state formation at a semiconductor-electrolyte interface via the optical anisotropy
• The relevance of structural variability in the time-domain for computational reflection anisotropy spectroscopy at solid-liquid interfaces