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Open Access Unveiling the Nature of Charge Carrier Interactions by Electroabsorption Spectroscopy: An Illustration with Lead-Halide Perovskites

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Unravelling the nature of the interactions between photogenerated charge carriers in solar energy conversion devices is key to enhance performance. In this perspective, we discuss electroabsorption spectroscopy (EAS), as the spectral bandshape of the electroabsorption (EA) signal directly depends on the strength of the charge carrier interactions. For instance, the electroabsorption response in molecular or confined excitonic systems can be modelled perturbatively yielding the Stark effect. In contrast, most solids exhibit weaker interactions, and a perturbative approach cannot be taken in general. For solids with negligible charge carrier interactions, one resorts to the Franz-Keldysh theory of a continuum in a field, that, in the low-field limit, simplifies to the low-field FKA effect. Alternatively, when the continuum approximation breaks down, the problem of a Wannier exciton in a field has to be solved, and numerical methods emerged as the best solution. We illustrate our discussion with two examples involving lead-halide perovskites, a new, high-stake solar cell material. In the first example, we discuss the lineshape of the electroabsorption response for thin-films of lead-iodide perovskite, that sustains the photogeneration of free carriers. In the second example, we address a confined excitonic case with lead-bromide perovskite nanoparticles, and demonstrate the presence of so-called charge-transfer excitons.
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Keywords: CHARGE CARRIER INTERACTIONS; ELECTROABSORPTION; LEAD-HALIDE PEROVSKITES; PHOTOVOLTAIC DEVICES; SPECTROSCOPY

Document Type: Research Article

Affiliations: 1: Photochemical Dynamics Group Institute of Chemical Sciences & Engineering, and Lausanne Centre for Ultrafast Science École polytechnique fédérale de Lausanne CH-1015 Lausanne;, Email: [email protected] 2: Photochemical Dynamics Group Institute of Chemical Sciences & Engineering, and Lausanne Centre for Ultrafast Science École polytechnique fédérale de Lausanne CH-1015 Lausanne

Publication date: April 1, 2017

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  • International Journal for Chemistry and Official Membership Journal of the Swiss Chemical Society (SCS) and its Divisions

    CHIMIA, a scientific journal for chemistry in the broadest sense, is published 10 times a year and covers the interests of a wide and diverse readership. Contributions from all fields of chemistry and related areas are considered for publication in the form of Review Articles and Notes. A characteristic feature of CHIMIA are the thematic issues, each devoted to an area of great current significance.

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