scispace - formally typeset
Search or ask a question
Journal ArticleDOI

Structural, Optical and Electrical Properties of Self-Assembled Films of PbSe Nanocrystals Treated with 1,2-Ethanedithiol

31 Jan 2008-ACS Nano (American Chemical Society)-Vol. 2, Iss: 2, pp 271-280
TL;DR: The LbL process described here is a general strategy for producing uniform, conductive nanocrystal films for applications in optoelectronics and solar energy conversion.
Abstract: We describe the structural, optical, and electrical properties of high-quality films of PbSe nanocrystals fabricated by a layer-by-layer (LbL) dip-coating method that utilizes 1,2-ethanedithiol (EDT) as an insolubilizing agent. Comparative characterization of nanocrystal films made by spin-coating and by the LbL process shows that EDT quantitatively displaces oleic acid on the PbSe surface, causing a large volume loss that electronically couples the nanocrystals while severely degrading their positional and crystallographic order of the films. Field-effect transistors based on EDT-treated films are moderately conductive and ambipolar in the dark, becoming p-type and 30–60 times more conductive under 300 mW cm−2 broadband illumination. The nanocrystal films oxidize rapidly in air to yield, after short air exposures, highly conductive p-type solids. The LbL process described here is a general strategy for producing uniform, conductive nanocrystal films for applications in optoelectronics and solar energy co...
Citations
More filters
Journal ArticleDOI
TL;DR: Nanocrystals (NCs) discussed in this Review are tiny crystals of metals, semiconductors, and magnetic material consisting of hundreds to a few thousand atoms each that are among the hottest research topics of the last decades.
Abstract: Nanocrystals (NCs) discussed in this Review are tiny crystals of metals, semiconductors, and magnetic material consisting of hundreds to a few thousand atoms each. Their size ranges from 2-3 to about 20 nm. What is special about this size regime that placed NCs among the hottest research topics of the last decades? The quantum mechanical coupling * To whom correspondence should be addressed. E-mail: dvtalapin@uchicago.edu. † The University of Chicago. ‡ Argonne National Lab. Chem. Rev. 2010, 110, 389–458 389

3,720 citations

Journal ArticleDOI
TL;DR: The simple mesoscopic CH(3)NH( 3)PbI(3)/TiO(2) heterojunction solar cell shows impressive photovoltaic performance, with short-circuit photocurrent J(sc)= 16.1 mA/cm(2), open-circuits photovvoltage V(oc) = 0.631 V, and a fill factor FF =0.57.
Abstract: We report for the first time on a hole conductor-free mesoscopic methylammonium lead iodide (CH3NH3PbI3) perovskite/TiO2 heterojunction solar cell, produced by deposition of perovskite nanoparticles from a solution of CH3NH3I and PbI2 in γ-butyrolactone on a 400 nm thick film of TiO2 (anatase) nanosheets exposing (001) facets. A gold film was evaporated on top of the CH3NH3PbI3 as a back contact. Importantly, the CH3NH3PbI3 nanoparticles assume here simultaneously the roles of both light harvester and hole conductor, rendering superfluous the use of an additional hole transporting material. The simple mesoscopic CH3NH3PbI3/TiO2 heterojunction solar cell shows impressive photovoltaic performance, with short-circuit photocurrent Jsc= 16.1 mA/cm2, open-circuit photovoltage Voc = 0.631 V, and a fill factor FF = 0.57, corresponding to a light to electric power conversion efficiency (PCE) of 5.5% under standard AM 1.5 solar light of 1000 W/m2 intensity. At a lower light intensity of 100W/m2, a PCE of 7.3% was m...

1,799 citations

Journal ArticleDOI
16 Dec 2011-Science
TL;DR: It is demonstrated that MEG charge carriers can be collected in suitably designed QD solar cells, providing ample incentive to better understand MEG within isolated and coupled QDs as a research path to enhancing the efficiency of solar light harvesting technologies.
Abstract: Multiple exciton generation (MEG) is a process that can occur in semiconductor nanocrystals, or quantum dots (QDs), whereby absorption of a photon bearing at least twice the bandgap energy produces two or more electron-hole pairs. Here, we report on photocurrent enhancement arising from MEG in lead selenide (PbSe) QD-based solar cells, as manifested by an external quantum efficiency (the spectrally resolved ratio of collected charge carriers to incident photons) that peaked at 114 ± 1% in the best device measured. The associated internal quantum efficiency (corrected for reflection and absorption losses) was 130%. We compare our results with transient absorption measurements of MEG in isolated PbSe QDs and find reasonable agreement. Our findings demonstrate that MEG charge carriers can be collected in suitably designed QD solar cells, providing ample incentive to better understand MEG within isolated and coupled QDs as a research path to enhancing the efficiency of solar light harvesting technologies.

1,537 citations

Journal ArticleDOI
TL;DR: An atomic ligand strategy is established that makes use of monovalent halide anions to enhance electronic transport and successfully passivate surface defects in PbS CQD films that shows up to 6% solar AM1.5G power-conversion efficiency.
Abstract: Colloidal-quantum-dot (CQD) optoelectronics offer a compelling combination of solution processing and spectral tunability through quantum size effects. So far, CQD solar cells have relied on the use of organic ligands to passivate the surface of the semiconductor nanoparticles. Although inorganic metal chalcogenide ligands have led to record electronic transport parameters in CQD films, no photovoltaic device has been reported based on such compounds. Here we establish an atomic ligand strategy that makes use of monovalent halide anions to enhance electronic transport and successfully passivate surface defects in PbS CQD films. Both time-resolved infrared spectroscopy and transient device characterization indicate that the scheme leads to a shallower trap state distribution than the best organic ligands. Solar cells fabricated following this strategy show up to 6% solar AM1.5G power-conversion efficiency. The CQD films are deposited at room temperature and under ambient atmosphere, rendering the process amenable to low-cost, roll-by-roll fabrication.

1,435 citations


Cites background from "Structural, Optical and Electrical ..."

  • ...S3 ), combined with the effect of the increased dielectric constan...

    [...]

Journal ArticleDOI
TL;DR: The role of surface ligands in tuning and rationally designing properties of functional nanomaterials and their importance for biomedical and optoelectronic applications is focused on and an assessment of application-targeted surface engineering is concluded.
Abstract: All nanomaterials share a common feature of large surface-to-volume ratio, making their surfaces the dominant player in many physical and chemical processes. Surface ligands - molecules that bind to the surface - are an essential component of nanomaterial synthesis, processing and application. Understanding the structure and properties of nanoscale interfaces requires an intricate mix of concepts and techniques borrowed from surface science and coordination chemistry. Our Review elaborates these connections and discusses the bonding, electronic structure and chemical transformations at nanomaterial surfaces. We specifically focus on the role of surface ligands in tuning and rationally designing properties of functional nanomaterials. Given their importance for biomedical (imaging, diagnostics and therapeutics) and optoelectronic (light-emitting devices, transistors, solar cells) applications, we end with an assessment of application-targeted surface engineering.

1,247 citations

References
More filters
Journal ArticleDOI
14 Oct 1999-Nature
TL;DR: In this article, the authors used thin-film, field effect transistor structures to probe the transport properties of the ordered microcrystalline domains in the conjugated polymer poly(3-hexylthiophene), P3HT.
Abstract: Self-organization in many solution-processed, semiconducting conjugated polymers results in complex microstructures, in which ordered microcrystalline domains are embedded in an amorphous matrix1. This has important consequences for electrical properties of these materials: charge transport is usually limited by the most difficult hopping processes and is therefore dominated by the disordered matrix, resulting in low charge-carrier mobilities2 (⩽10-5 cm2 V-1 s-1). Here we use thin-film, field-effect transistor structures to probe the transport properties of the ordered microcrystalline domains in the conjugated polymer poly(3-hexylthiophene), P3HT. Self-organization in P3HT results in a lamella structure with two-dimensional conjugated sheets formed by interchain stacking. We find that, depending on processing conditions, the lamellae can adopt two different orientations—parallel and normal to the substrate—the mobilities of which differ by more than a factor of 100, and can reach values as high as 0.1 cm2 V-1 s-1 (refs 3, 4). Optical spectroscopy of the field-induced charge, combined with the mobility anisotropy, reveals the two-dimensional interchain character of the polaronic charge carriers, which exhibit lower relaxation energies than the corresponding radical cations on isolated one-dimensional chains. The possibility of achieving high mobilities via two-dimensional transport in self-organized conjugated lamellae is important for applications of polymer transistors in logic circuits5 and active-matrix displays4,6.

4,306 citations

Journal ArticleDOI
04 Aug 1994-Nature
TL;DR: In this article, a hybrid organic/inorganic electroluminescent device was constructed based on the recombination of holes injected into a layer of semiconducting p-paraphenylene vinylene (PPV) with electrons injected into the multilayer film of cadmium selenide nanocrystals.
Abstract: ELECTROLUMINESCENT devices have been developed recently that are based on new materials such as porous silicon1 and semiconducting polymers2,3. By taking advantage of developments in the preparation and characterization of direct-gap semiconductor nanocrystals4–6, and of electroluminescent polymers7, we have now constructed a hybrid organic/inorganic electroluminescent device. Light emission arises from the recombination of holes injected into a layer of semiconducting p-paraphenylene vinylene (PPV)8–10 with electrons injected into a multilayer film of cadmium selenide nanocrystals. Close matching of the emitting layer of nanocrystals with the work function of the metal contact leads to an operating voltage11 of only 4V. At low voltages emission from the CdSe layer occurs. Because of the quantum size effect19–24 the colour of this emission can be varied from red to yellow by changing the nanocrystal size. At higher voltages green emission from the polymer layer predominates. Thus this device has a degree of voltage tunability of colour.

3,783 citations

Journal Article
TL;DR: In this article, a hybrid organic/inorganic electroluminescent device was constructed based on the recombination of holes injected into a layer of semiconducting p-paraphenylene vinylene (PPV) with electrons injected into the multilayer film of cadmium selenide nanocrystals.
Abstract: ELECTROLUMINESCENT devices have been developed recently that are based on new materials such as porous silicon' and semiconducting polymers 2,3 . By taking advantage of developments in the preparation and characterization of direct-gap semiconductor nanocrystals 4-6 , and of electroluminescent polymers7, we have now constructed a hybrid organic/inorganic electroluminescent device. Light emission arises from the recombination of holes injected into a layer of semiconducting p-paraphenylene vinylene (PPV) 2-10 with electrons injected into a multilayer film of cadmium selenide nanocrystals. Close matching of the emitting layer of nanocrystals with the work function of the metal contact leads to an operating voltage" of only 4 V. At low voltages emission from the CdSe layer occurs. Because of the quantum size effect 19-24 the colour of this emission can be varied from red to yellow by changing the nanocrystal size. At higher voltages green emission from the polymer layer predominates. Thus this device has a degree of voltage tunability of colour.

3,285 citations

Journal ArticleDOI
19 Dec 2002-Nature
TL;DR: A hybrid light-emitting diode (LED) that combines the ease of processability of organic materials with the narrow-band, efficient luminescence of colloidal quantum dots (QDs) is demonstrated and a 25-fold improvement in luminescent efficiency is observed.
Abstract: The integration of organic and inorganic materials at the nanometre scale into hybrid optoelectronic structures enables active devices that combine the diversity of organic materials with the high-performance electronic and optical properties of inorganic nanocrystals. The optimization of such hybrid devices ultimately depends upon the precise positioning of the functionally distinct materials. Previous studies have already emphasized that this is a challenge, owing to the lack of well-developed nanometre-scale fabrication techniques. Here we demonstrate a hybrid light-emitting diode (LED) that combines the ease of processability of organic materials with the narrow-band, efficient luminescence of colloidal quantum dots (QDs). To isolate the luminescence processes from charge conduction, we fabricate a quantum-dot LED (QD-LED) that contains only a single monolayer of QDs, sandwiched between two organic thin films. This is achieved by a method that uses material phase segregation between the QD aliphatic capping groups and the aromatic organic materials. In our devices, where QDs function exclusively as lumophores, we observe a 25-fold improvement in luminescence efficiency (1.6 cd A(-1) at 2,000 cd m(-2)) over the best previous QD-LED results. The reproducibility and precision of our phase-segregation approach suggests that this technique could be widely applicable to the fabrication of other hybrid organic/inorganic devices.

2,438 citations

Journal ArticleDOI
TL;DR: In this article, three QD solar cell configurations are described: (1) photoelectrodes comprising QD arrays, (2) QD-sensitized nanocrystalline TiO 2, and (3) QDs dispersed in a blend of electron- and hole-conducting polymers.
Abstract: Quantum dot (QD) solar cells have the potential to increase the maximum attainable thermodynamic conversion efficiency of solar photon conversion up to about 66% by utilizing hot photogenerated carriers to produce higher photovoltages or higher photocurrents. The former effect is based on miniband transport and collection of hot carriers in QD array photoelectrodes before they relax to the band edges through phonon emission. The latter effect is based on utilizing hot carriers in QD solar cells to generate and collect additional electron–hole pairs through enhanced impact ionization processes. Three QD solar cell configurations are described: (1) photoelectrodes comprising QD arrays, (2) QD-sensitized nanocrystalline TiO 2 , and (3) QDs dispersed in a blend of electron- and hole-conducting polymers. These high-efficiency configurations require slow hot carrier cooling times, and we discuss initial results on slowed hot electron cooling in InP QDs.

2,405 citations