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THz mobility and polarizability: impact of transformation and dephasing on the spectral response of excitons in a 2D semiconductor

Quick, Michael T.; Ayari, Sabrine; Owschimikow, Nina; Jaziri, Sihem; Achtstein, Alexander W.

We introduce a response theory based transformation for excitonic polarizability into mobility, which allows an in-depth analysis of optical pump–THz probe conductivity experiments, and compare the results with those of a conventional oscillator model. THz spectroscopy is of high interest e.g. for investigations in high bandwidth and low noise nanoelectronics or solar energy harvesting nanomaterials. In contrast to simple ω scaling of estimated static polarizability, suggested in the literature, an appropriate transformation of the spectral response into mobility can be achieved in principle forward and backward due to the presence of dephasing, as we show for the exemplary system of CdSe nanoplatelets. Common analysis approaches capture the excitonic properties only under specific conditions, and do not apply in many cases. We demonstrate that a thermal distribution of excitons and transitions between higher states in general have to be considered and that dephasing has to be taken into account for a proper transformation at all temperatures. The presented in-depth understanding of the exciton mobility in nanoparticles can help improve e.g. solar hydrogen generation, charge extraction efficiencies of solar cells, or light emission performance of LEDs.
Published in: Physical Chemistry Chemical Physics, 10.1039/d2cp03584g, Royal Society of Chemistry (RSC)