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Direct Imaging of Long-Range Exciton Transport in Quantum Dot Superlattices by Ultrafast Microscopy

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Radiation Laboratory, University of Notre Dame, Notre Dame, Indiana 46556, United States
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States
§ Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States
Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, United States
Cite this: ACS Nano 2016, 10, 7, 7208–7215
Publication Date (Web):July 7, 2016
https://doi.org/10.1021/acsnano.6b03700
Copyright © 2016 American Chemical Society

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    Long-range charge and exciton transport in quantum dot (QD) solids is a crucial challenge in utilizing QDs for optoelectronic applications. Here, we present a direct visualization of exciton diffusion in highly ordered CdSe QDs superlattices by mapping exciton population using ultrafast transient absorption microscopy. A temporal resolution of ∼200 fs and a spatial precision of ∼50 nm of this technique provide a direct assessment of the upper limit for exciton transport in QD solids. An exciton diffusion length of ∼125 nm has been visualized in the 3 ns experimental time window and an exciton diffusion coefficient of (2.5 ± 0.2) × 10–2 cm2 s–1 has been measured for superlattices constructed from 3.6 nm CdSe QDs with center-to-center distance of 6.7 nm. The measured exciton diffusion constant is in good agreement with Förster resonance energy transfer theory. We have found that exciton diffusion is greatly enhanced in the superlattices over the disordered films with an order of magnitude higher diffusion coefficient, pointing toward the role of disorder in limiting transport. This study provides important understandings on energy transport mechanisms in both the spatial and temporal domains in QD solids.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.6b03700.

    • Preparation of CdSe QDs and QD superlattice, material and photophysical characterization methods. Additional structural analysis of CdSe QD superlattices, TAM configuration and resolution, transition dipole calculation for CdSe QDs, and time-resolved transient absorption/PL spectra are also provided. (PDF)

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