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      Solid‐State Ligand‐Exchange Fabrication of CH 3NH 3PbI 3 Capped PbS Quantum Dot Solar Cells

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          Abstract

          CH 3NH 3PbI 3 capped PbS colloidal quantum dots have been successfully fabricated by solid‐state ligand exchange from oleate and oleylamine capped PbS. The optimal solar cells made by layer‐by‐layer solution deposition give a high power conversion efficiency of 4.25% with an impressive short‐circuit photocurrent density of 24.83 mA cm −2.

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          Most cited references16

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          Highly efficient multiple exciton generation in colloidal PbSe and PbS quantum dots.

          We report ultra-efficient multiple exciton generation (MEG) for single photon absorption in colloidal PbSe and PbS quantum dots (QDs). We employ transient absorption spectroscopy and present measurement data acquired for both intraband as well as interband probe energies. Quantum yields of 300% indicate the creation, on average, of three excitons per absorbed photon for PbSe QDs at photon energies that are four times the QD energy gap. Results indicate that the threshold photon energy for MEG in QDs is twice the lowest exciton absorption energy. We find that the biexciton effect, which shifts the transition energy for absorption of a second photon, influences the early time transient absorption data and may contribute to a modulation observed when probing near the lowest interband transition. We present experimental and theoretical values of the size-dependent interband transition energies for PbSe QDs. We present experimental and theoretical values of the size-dependent interband transition energies for PbSe QDs, and we also introduce a new model for MEG based on the coherent superposition of multiple excitonic states.
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            Depleted-heterojunction colloidal quantum dot solar cells.

            Colloidal quantum dot (CQD) photovoltaics combine low-cost solution processability with quantum size-effect tunability to match absorption with the solar spectrum. Rapid recent advances in CQD photovoltaics have led to impressive 3.6% AM1.5 solar power conversion efficiencies. Two distinct device architectures and operating mechanisms have been advanced. The first-the Schottky device-was optimized and explained in terms of a depletion region driving electron-hole pair separation on the semiconductor side of a junction between an opaque low-work-function metal and a p-type CQD film. The second-the excitonic device-employed a CQD layer atop a transparent conductive oxide (TCO) and was explained in terms of diffusive exciton transport via energy transfer followed by exciton separation at the type-II heterointerface between the CQD film and the TCO. Here we fabricate CQD photovoltaic devices on TCOs and show that our devices rely on the establishment of a depletion region for field-driven charge transport and separation, and that they also exploit the large bandgap of the TCO to improve rectification and block undesired hole extraction. The resultant depleted-heterojunction solar cells provide a 5.1% AM1.5 power conversion efficiency. The devices employ infrared-bandgap size-effect-tuned PbS CQDs, enabling broadband harvesting of the solar spectrum. We report the highest open-circuit voltages observed in solid-state CQD solar cells to date, as well as fill factors approaching 60%, through the combination of efficient hole blocking (heterojunction) and very small minority carrier density (depletion) in the large-bandgap moiety.
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              Charge Carriers in Planar and Meso-Structured Organic-Inorganic Perovskites: Mobilities, Lifetimes, and Concentrations of Trap States.

              Efficient solar cells have been obtained using thin films of solution-processed organic-inorganic perovskites. However, there remains limited knowledge about the relationship between preparation route and optoelectronic properties. We use complementary time-resolved microwave conductivity (TRMC) and photoluminescence (PL) measurements to investigate the charge carrier dynamics in thin planar films of CH3NH3PbI(3-x)Cl(x), CH3NH3PbI3, and their meso-structured analogues. High mobilities close to 30 cm(2)/(V s) and microsecond-long lifetimes are found in thin films of CH3NH3PbI(3-x)Cl(x), compared to lifetimes of only a few hundred nanoseconds in CH3NH3PbI3 and meso-structured perovskites. We describe our TRMC and PL experiments with a global kinetic model, using one set of kinetic parameters characteristic for each sample. We find that the trap density is less than 5 × 10(14) cm(-3) in CH3NH3PbI(3-x)Cl(x), 6 × 10(16) cm(-3) in the CH3NH3PbI3 thin film and ca. 10(15) cm(-3) in both meso-structured perovskites. Furthermore, our results imply that band-to-band recombination is enhanced by the presence of dark carriers resulting from unintentional doping of the perovskites. Finally, our general approach to determine concentrations of trap states and dark carriers is also highly relevant to other semiconductor materials.
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                Author and article information

                Journal
                Adv Sci (Weinh)
                Adv Sci (Weinh)
                10.1002/(ISSN)2198-3844
                ADVS
                Advanced Science
                John Wiley and Sons Inc. (Hoboken )
                2198-3844
                18 February 2016
                June 2016
                : 3
                : 6 ( doiID: 10.1002/advs.v3.6 )
                : 1500432
                Affiliations
                [ 1 ] Department of Materials ScienceFudan University Shanghai 200433P.R. China
                [ 2 ] Department of ChemistryFudan University Shanghai 200433P.R. China
                Author notes
                Article
                ADVS117
                10.1002/advs.201500432
                5067684
                c6f0d13e-71f1-4926-a8fd-741b508e61e7
                © 2016 The Authors. Published by WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim

                This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.

                History
                : 23 December 2015
                Page count
                Pages: 6
                Categories
                Communication
                Communications
                Custom metadata
                2.0
                advs117
                June 2016
                Converter:WILEY_ML3GV2_TO_NLMPMC version:4.9.5 mode:remove_FC converted:18.10.2016

                ch3nh3pbi3 perovskites,layer‐by‐layer method,ligand exchange,pbs quantum dots,photovoltaics

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