Extracting quantitative dielectric properties from pump-probe spectroscopy.

Autor: Ashoka A; Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, CB3 0HE, Cambridge, UK., Tamming RR; Robinson Research Institute, Faculty of Engineering, Victoria University of Wellington, Wellington, 6012, New Zealand.; School of Chemical and Physical Sciences, Victoria University of Wellington, Wellington, 6012, New Zealand.; MacDiarmid Institute for Advanced Materials and Nanotechnology, Wellington, 6012, New Zealand., Girija AV; Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, CB3 0HE, Cambridge, UK., Bretscher H; Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, CB3 0HE, Cambridge, UK., Verma SD; Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, CB3 0HE, Cambridge, UK.; Department of Chemistry, Indian Institute of Science Education and Research Bhopal, Bhopal Bypass Road, Bhopal, 462066, Madhya Pradesh, India., Yang SD; Institute of Photonics Technologies, National Tsing Hua University, Hsinchu, 30013, Taiwan., Lu CH; Institute of Photonics Technologies, National Tsing Hua University, Hsinchu, 30013, Taiwan., Hodgkiss JM; School of Chemical and Physical Sciences, Victoria University of Wellington, Wellington, 6012, New Zealand.; MacDiarmid Institute for Advanced Materials and Nanotechnology, Wellington, 6012, New Zealand., Ritchie D; Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, CB3 0HE, Cambridge, UK., Chen C; Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, CB3 0HE, Cambridge, UK., Smith CG; Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, CB3 0HE, Cambridge, UK., Schnedermann C; Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, CB3 0HE, Cambridge, UK., Price MB; School of Chemical and Physical Sciences, Victoria University of Wellington, Wellington, 6012, New Zealand.; MacDiarmid Institute for Advanced Materials and Nanotechnology, Wellington, 6012, New Zealand., Chen K; Robinson Research Institute, Faculty of Engineering, Victoria University of Wellington, Wellington, 6012, New Zealand.; MacDiarmid Institute for Advanced Materials and Nanotechnology, Wellington, 6012, New Zealand.; The Dodd-Walls Centre for Photonic and Quantum Technologies, Dunedin, 9016, New Zealand., Rao A; Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, CB3 0HE, Cambridge, UK. ar525@cam.ac.uk.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2022 Mar 17; Vol. 13 (1), pp. 1437. Date of Electronic Publication: 2022 Mar 17.
DOI: 10.1038/s41467-022-29112-y
Abstrakt: 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.
(© 2022. The Author(s).)
Databáze: MEDLINE
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