Extracting quantitative dielectric properties from pump-probe spectroscopy

Arjun Ashoka, Ronnie R. Tamming, Aswathy V. Girija, Hope Bretscher, Sachin Dev Verma, Shang-Da Yang, Chih-Hsuan Lu, Justin M. Hodgkiss, David Ritchie, Chong Chen, Charles G. Smith, Christoph Schnedermann, Michael B. Price, Kai Chen and Akshay Rao ()
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Arjun Ashoka: University of Cambridge
Ronnie R. Tamming: Victoria University of Wellington
Aswathy V. Girija: University of Cambridge
Hope Bretscher: University of Cambridge
Sachin Dev Verma: University of Cambridge
Shang-Da Yang: National Tsing Hua University
Chih-Hsuan Lu: National Tsing Hua University
Justin M. Hodgkiss: Victoria University of Wellington
David Ritchie: University of Cambridge
Chong Chen: University of Cambridge
Charles G. Smith: University of Cambridge
Christoph Schnedermann: University of Cambridge
Michael B. Price: Victoria University of Wellington
Kai Chen: Victoria University of Wellington
Akshay Rao: University of Cambridge

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract 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.

Date: 2022
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DOI: 10.1038/s41467-022-29112-y

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