Extracting quantitative dielectric properties from pump-probe spectroscopy.
Tamming, Ronnie R
Hodgkiss, Justin M
Springer Science and Business Media LLC
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Ashoka, A., Tamming, R. R., Girija, A. V., Bretscher, H., Verma, S. D., Yang, S., Lu, C., et al. (2022). Extracting quantitative dielectric properties from pump-probe spectroscopy.. Nat Commun, 13 (1) https://doi.org/10.1038/s41467-022-29112-y
Funder: EC | Horizon 2020 Framework Programme (EU Framework Programme for Research and Innovation H2020); doi: https://doi.org/10.13039/100010661
Funder: RCUK | Engineering and Physical Sciences Research Council (EPSRC); doi: https://doi.org/10.13039/501100000266
Funder: We acknowledge financial support from the EPSRC and the Winton Program for the Physics of Sustainability. This project has received funding from the European Research Council (ERC) under the European Unions Horizon 2020 research and innovation programme (grant agreement no. 758826).
Optical pump-probe spectroscopy is a powerful tool for the study of non-equilibrium electronic dynamics and finds wide applications across a range of fields, from physics and chemistry to material science and biology. However, a shortcoming of conventional pump-probe spectroscopy is that photoinduced changes in transmission, reflection and scattering can simultaneously contribute to the measured differential spectra, leading to ambiguities in assigning the origin of spectral signatures and ruling out quantitative interpretation of the spectra. Ideally, these methods would measure the underlying dielectric function (or the complex refractive index) which would then directly provide quantitative information on the transient excited state dynamics free of these ambiguities. Here we present and test a model independent route to transform differential transmission or reflection spectra, measured via conventional optical pump-probe spectroscopy, to changes in the quantitative transient dielectric function. We benchmark this method against changes in the real refractive index measured using time-resolved Frequency Domain Interferometry in prototypical inorganic and organic semiconductor films. Our methodology can be applied to existing and future pump-probe data sets, allowing for an unambiguous and quantitative characterisation of the transient photoexcited spectra of materials. This in turn will accelerate the adoption of pump-probe spectroscopy as a facile and robust materials characterisation and screening tool.
Article, /639/301/299/946, /639/624/1107/527, /639/766/119, /639/638/439, article
Engineering and Physical Sciences Research Council (EP/M006360/1)
European Research Council (758826)
Royal Commission for the Exhibition of 1851 (RF499/2018)
External DOI: https://doi.org/10.1038/s41467-022-29112-y
This record's URL: https://www.repository.cam.ac.uk/handle/1810/335125