Nonequilibrium Dynamics of Excitons and Charges in Semiconductor Nanomaterials
William Tisdale a
a Massachusetts Institute of Technology (MIT), Massachusetts Avenue, 77, Cambridge, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting19 (NFM19)
#CharDy19. Charge Carrier Dynamics
Berlin, Germany, 2019 November 3rd - 8th
Organizers: Mahshid Ahmadi, Efrat Lifshitz, Cristiane Morais Smith, Marcus Scheele, Roel van de Krol, Pablo P. Boix, Erwin Reisner, Stefan Weber, Germà Garcia-Belmonte, Doron Naveh and Maksym Yarema
Keynote, William Tisdale, presentation 089
DOI: https://doi.org/10.29363/nanoge.nfm.2019.089
Publication date: 18th July 2019

Structure, surface chemistry, and energetic disorder can dramatically affect excited state dynamics in low-dimensional systems. Using a combination of ultrafast laser spectroscopy, time-resolved optical microscopy, and kinetic modeling, I will show how these effects manifest in assemblies of colloidal quantum dots (QD) and atomically thin 2D semiconductors, which are promising components of next-generation photovoltaic and lighting technologies. In particular, I will demonstrate the counterintuitive role of entropy in the nonequilibrium population dynamics of excitons and charge carriers in nanoscale systems.

In semiconductors, increasing mobility with decreasing temperature is a signature of charge carrier transport through delocalized bands. Here, we show that this behavior can also occur in nanocrystal solids due to temperature-dependent structural transformations. Using a combination of broadband infrared transient absorption spectroscopy and numerical modeling, we investigate the temperature-dependent charge transport properties of well-ordered PbS quantum dot (QD) solids. Contrary to expectations, we observe that the QD-to-QD charge tunneling rate increases with decreasing temperature, while simultaneously exhibiting thermally activated nearest-neighbor hopping behavior. Using synchrotron grazing-incidence small-angle X-ray scattering (GISAXS), we show that this trend is driven by a temperature-dependent reduction in nearest-neighbor separation that is quantitatively consistent with the measured tunneling rate.[1]

This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Award Number DE-SC0010538.

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