Voznyy, Oleksandr; Levina, Larissa; Fan, Feng-Jia; Walters, Grant; Fan, James Z.; Kiani, Amirreza; Ip, Alexander H.; Thon, Susanna M.; Proppe, Andrew H.; Liu, Mengxia; Sargent, Edward H.(Nano Letters, American Chemical Society (ACS), 2017-10-27)[Article]
Stokes shift, an energy difference between the excitonic absorption and emission, is a property of colloidal quantum dots (CQDs) typically ascribed to splitting between dark and bright excitons. In some materials, e.g., PbS, CuInS2, CdHgTe, a Stokes shift of up to 200 meV is observed, substantially larger than the estimates of dark-bright state splitting or vibronic relaxations. The shift origin remains highly debated, as contradictory signatures of both surface and bulk character were reported for the Stokes-shifted electronic state. Here we show that the energy transfer among CQDs in a polydispersed ensemble in solution suffices to explain the excess Stokes shift. This energy transfer is primarily due to CQD aggregation, and can be substantially eliminated by extreme dilution, higher-viscosity solvent, or better-dispersed colloids. Our findings highlight that ensemble polydispersity remains the primary source of the Stokes shift in CQDs in solution, propagating into the Stokes shift in films and the open-circuit voltage deficit in CQD solar cells. Improved synthetic control can bring notable advancements in CQD photovoltaics, and the Stokes shift continues to provide a sensitive and significant metric to monitor ensemble size distribution.
Yang, Zhenyu; Voznyy, Oleksandr; Liu, Mengxia; Yuan, Mingjian; Ip, Alexander H.; Ahmed, Osman S.; Levina, Larissa; Kinge, Sachin; Hoogland, Sjoerd; Sargent, Edward H.(ACS Nano, American Chemical Society (ACS), 2015-12-22)[Article]
Yang, Zhenyu; Yassitepe, Emre; Voznyy, Oleksandr; Janmohamed, Alyf; Lan, Xinzheng; Levina, Larissa; Comin, Riccardo; Sargent, Edward H.(Journal of the American Chemical Society, American Chemical Society (ACS), 2015-12-02)[Article]
Koleilat, Ghada I.; Wang, Xihua; Labelle, Andre J.; Ip, Alexander H.; Carey, Graham H.; Fischer, Armin; Levina, Larissa; Brzozowski, Lukasz; Sargent, Edward H.(Nano Letters, American Chemical Society (ACS), 2011-12-14)[Article]
Nootz, Gero; Padilha, Lazaro A.; Olszak, Peter D.; Webster, Scott; Hagan, David J.; Van Stryland, Eric W.; Levina, Larissa; Sukhovatkin, Vlad; Brzozowski, Lukasz; Sargent, Edward H.(Nano Letters, American Chemical Society (ACS), 2010-09-08)[Article]
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