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Richard Stones

Publications and source records attributed to Richard Stones.

2 recordsLinked to original sources

On the perfomance of a photosystem II reaction centre-based photocell

The photosystem II reaction centre is the photosynthetic complex responsible for oxygen production on Earth. Its water splitting function is particularly favoured by the formation of a stable charge separated state via a pathway that starts at an accessory chlorophyll. Here we envision a photovoltaic device that places one of these complexes between electrodes and investigate how the mean current and its fluctuations depend on the microscopic interactions underlying charge separation in the pathway considered. Our results indicate that coupling to well resolved vibrational modes does not necessarily offer an advantage in terms of power output but can lead to photo-currents with suppressed noise levels characterizing a multi-step ordered transport process. Besides giving insight into the suitability of these complexes for molecular-scale photovoltaics, our work suggests a new possible biological function for the vibrational environment of photosynthetic reaction centres, namely, to reduce the intrinsic current noise for regulatory processes.

physics.bio-ph

Non-Perturbative Electron Counting Statistics

The theory of full counting statistics allows complete characterization of charge transport processes through nanoscale systems. The majority of existing theoretical treatments used to obtain the current cumulants rely on perturbative approximations with respect to either the system-bath coupling or the electronic tunnelling coupling within the system. This is not generally well suited to electron transfer through organic molecules where these couplings can be on the same order of magnitude. Here we present a non-perturbative approach that uses the formalism of the hierarchical equations of motion to describe the system-bath dynamics while retaining a weak coupling with respect to source and drain leads. The scope of this new framework is demonstrated by comparisons with a perturbative approach for a dimer system coupled to a thermal bath. The inadequacy of the perturbative approach to describe current fluctuations in a variety of regimes is shown.

cond-mat.mes-hall