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.
Kim, Younghoon; Bicanic, Kristopher; Tan, Hairen; Ouellette, Olivier; Sutherland, Brandon R.; García de Arquer, F. Pelayo; Jo, Jea Woong; Liu, Mengxia; Sun, Bin; Liu, Min; Hoogland, Sjoerd; Sargent, Edward H.(Nano Letters, American Chemical Society (ACS), 2017-03-13)[Article]
Colloidal quantum dot (CQD) materials are of interest in thin-film solar cells due to their size-tunable bandgap and low-cost solution-processing. However, CQD solar cells suffer from inefficient charge extraction over the film thicknesses required for complete absorption of solar light. Here we show a new strategy to enhance light absorption in CQD solar cells by nanostructuring the CQD film itself at the back interface. We use two-dimensional finite-difference time-domain (FDTD) simulations to study quantitatively the light absorption enhancement in nanostructured back interfaces in CQD solar cells. We implement this experimentally by demonstrating a nanoimprint-transfer-patterning (NTP) process for the fabrication of nanostructured CQD solids with highly ordered patterns. We show that this approach enables a boost in the power conversion efficiency in CQD solar cells primarily due to an increase in short-circuit current density as a result of enhanced absorption through light-trapping.
Kim, Gi-Hwan; García de Arquer, F. Pelayo; Yoon, Yung Jin; Lan, Xinzheng; Liu, Mengxia; Voznyy, Oleksandr; Yang, Zhenyu; Fan, Fengjia; Ip, Alexander H.; Kanjanaboos, Pongsakorn; Hoogland, Sjoerd; Kim, Jin Young; Sargent, Edward H.(Nano Letters, American Chemical Society (ACS), 2015-11-11)[Article]
Paz-Soldan, Daniel; Lee, Anna; Thon, Susanna M.; Adachi, Michael M.; Dong, Haopeng; Maraghechi, Pouya; Yuan, Mingjian; Labelle, André J.; Hoogland, Sjoerd; Liu, Kun; Kumacheva, Eugenia; Sargent, Edward H.(Nano Letters, American Chemical Society (ACS), 2013-04-10)[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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