Near-Infrared Colloidal Quantum Dots for Efficient and Durable Photoelectrochemical Solar-Driven Hydrogen Production.
Ontology highlight
ABSTRACT:
SUBMITTER: Jin L
PROVIDER: S-EPMC5021169 | biostudies-literature |
REPOSITORIES: biostudies-literature
Similar Datasets
Project description:Colloidal heterostructured quantum dots (QDs) are promising candidates for next-generation optoelectronic devices. In particular, "giant" core/shell QDs (g-QDs) can be engineered to exhibit outstanding optical properties and high chemical/photostability for the fabrication of high-performance optoelectronic devices. Here, the synthesis of heterostructured CuInSe x S2-x (CISeS)/CdSeS/CdS g-QDs with pyramidal shape by using a facile two-step method is reported. The CdSeS/CdS shell is demonstrated to have a pure zinc blend phase other than typical wurtzite phase. The as-obtained heterostructured g-QDs exhibit near-infrared photoluminescence (PL) emission (≈830 nm) and very long PL lifetime (in the microsecond range). The pyramidal g-QDs exhibit a quasi-type II band structure with spatial separation of electron-hole wave function, suggesting an efficient exciton extraction and transport, which is consistent with theoretical calculations. These heterostructured g-QDs are used as light harvesters to fabricate a photoelectrochemical cell, exhibiting a saturated photocurrent density as high as ≈5.5 mA cm-2 and good stability under 1 sun illumination (AM 1.5 G, 100 mW cm-2). These results are an important step toward using heterostructured pyramidal g-QDs for prospective applications in solar technologies.
| S-EPMC6097093 | biostudies-literature
Project description:We review the concept and the evolution of bandgap and wavefunction engineering, the seminal contributions of Dr. Chemla to the understanding of the rich phenomena displayed in epitaxially grown quantum confined systems, and demonstrate the application of these concepts to the colloidal synthesis of high quality type-II CdTe/CdSe quantum dots using successive ion layer adsorption and reaction chemistry. Transmission electron microscopy reveals that CdTe/CdSe can be synthesized layer by layer, yielding particles of narrow size distribution. Photoluminescence emission and excitation spectra reveal discrete type-II transitions, which correspond to energy lower than the type-I bandgap. The increase in the spatial separation between photoexcited electrons and holes as a function of successive addition of CdSe monolayers was monitored by photoluminescence lifetime measurements. Systematic increase in lifetimes demonstrates the high level of wavefunction engineering and control in these systems.
| S-EPMC3409670 | biostudies-literature
Project description:A structural change between amorphous and crystalline phase provides a basis for reliable and modular photonic and electronic devices, such as nonvolatile memory, beam steerers, solid-state reflective displays, or mid-IR antennas. In this paper, we leverage the benefits of liquid-based synthesis to access phase-change memory tellurides in the form of colloidally stable quantum dots. We report a library of ternary MxGe1-xTe colloids (where M is Sn, Bi, Pb, In, Co, Ag) and then showcase the phase, composition, and size tunability for Sn-Ge-Te quantum dots. Full chemical control of Sn-Ge-Te quantum dots permits a systematic study of structural and optical properties of this phase-change nanomaterial. Specifically, we report composition-dependent crystallization temperature for Sn-Ge-Te quantum dots, which is notably higher compared to bulk thin films. This gives the synergistic benefit of tailoring dopant and material dimension to combine the superior aging properties and ultrafast crystallization kinetics of bulk Sn-Ge-Te, while improving memory data retention due to nanoscale size effects. Furthermore, we discover a large reflectivity contrast between amorphous and crystalline Sn-Ge-Te thin films, exceeding 0.7 in the near-IR spectrum region. We utilize these excellent phase-change optical properties of Sn-Ge-Te quantum dots along with liquid-based processability for nonvolatile multicolor images and electro-optical phase-change devices. Our colloidal approach for phase-change applications offers higher customizability of materials, simpler fabrication, and further miniaturization to the sub-10 nm phase-change devices.
| S-EPMC10100560 | biostudies-literature
Project description:Colloidal quantum dots (CQDs) are promising materials for novel light sources and solar energy conversion. However, trap states associated with the CQD surface can produce non-radiative charge recombination that significantly reduces device performance. Here a facile post-synthetic treatment of CdTe CQDs is demonstrated that uses chloride ions to achieve near-complete suppression of surface trapping, resulting in an increase of photoluminescence (PL) quantum yield (QY) from ca. 5% to up to 97.2 ± 2.5%. The effect of the treatment is characterised by absorption and PL spectroscopy, PL decay, scanning transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. This process also dramatically improves the air-stability of the CQDs: before treatment the PL is largely quenched after 1 hour of air-exposure, whilst the treated samples showed a PL QY of nearly 50% after more than 12 hours.
| S-EPMC4409856 | biostudies-literature
Project description:Photonic quantum information requires high-purity, easily accessible, and scalable single-photon sources. Here, we report an electrically driven single-photon source based on colloidal quantum dots. Our solution-processed devices consist of isolated CdSe/CdS core/shell quantum dots sparsely buried in an insulating layer that is sandwiched between electron-transport and hole-transport layers. The devices generate single photons with near-optimal antibunching at room temperature, i.e., with a second-order temporal correlation function at zero delay (g (2)(0)) being <0.05 for the best devices without any spectral filtering or background correction. The optimal g (2)(0) from single-dot electroluminescence breaks the lower g (2)(0) limit of the corresponding single-dot photoluminescence. Such highly suppressed multi-photon-emission probability is attributed to both novel device design and carrier injection/recombination dynamics. The device structure prevents background electroluminescence while offering efficient single-dot electroluminescence. A quantitative model is developed to illustrate the carrier injection/recombination dynamics of single-dot electroluminescence.
| S-EPMC5656660 | biostudies-literature
Project description:Colloidal quantum wells are two-dimensional materials grown with atomically-precise thickness that dictates their electronic structure. Although intersubband absorption in epitaxial quantum wells is well-known, analogous observations in non-epitaxial two-dimensional materials are sparse. Here we show that CdSe nanoplatelet quantum wells have narrow (30-200 meV), polarized intersubband absorption features when photoexcited or under applied bias, which can be tuned by thickness across the near-infrared (NIR) spectral window (900-1600 nm) inclusive of important telecommunications wavelengths. By examination of the optical absorption and polarization-resolved measurements, the NIR absorptions are assigned to electron intersubband transitions. Under photoexcitation, the intersubband features display hot carrier and Auger recombination effects similar to excitonic absorptions. Sequenced two-color photoexcitation permits the sub-picosecond modulation of the carrier temperature in such colloidal quantum wells. This work suggests that colloidal quantum wells may be promising building blocks for NIR technologies.
| S-EPMC6778118 | biostudies-literature
Project description:Pairs of coupled quantum dots with controlled coupling between the two potential wells serve as an extremely rich system, exhibiting a plethora of optical phenomena that do not exist in each of the isolated constituent dots. Over the past decade, coupled quantum systems have been under extensive study in the context of epitaxially grown quantum dots (QDs), but only a handful of examples have been reported with colloidal QDs. This is mostly due to the difficulties in controllably growing nanoparticles that encapsulate within them two dots separated by an energetic barrier via colloidal synthesis methods. Recent advances in colloidal synthesis methods have enabled the first clear demonstrations of colloidal double quantum dots and allowed for the first exploratory studies into their optical properties. Nevertheless, colloidal double QDs can offer an extended level of structural manipulation that allows not only for a broader range of materials to be used as compared with epitaxially grown counterparts but also for more complex control over the coupling mechanisms and coupling strength between two spatially separated quantum dots. The photophysics of these nanostructures is governed by the balance between two coupling mechanisms. The first is via dipole-dipole interactions between the two constituent components, leading to energy transfer between them. The second is associated with overlap of excited carrier wave functions, leading to charge transfer and multicarrier interactions between the two components. The magnitude of the coupling between the two subcomponents is determined by the detailed potential landscape within the nanocrystals (NCs). One of the hallmarks of double QDs is the observation of dual-color emission from a single nanoparticle, which allows for detailed spectroscopy of their properties down to the single particle level. Furthermore, rational design of the two coupled subsystems enables one to tune the emission statistics from single photon emission to classical emission. Dual emission also provides these NCs with more advanced functionalities than the isolated components. The ability to better tailor the emission spectrum can be advantageous for color designed LEDs in lighting and display applications. The different response of the two emission colors to external stimuli enables ratiometric sensing. Control over hot carrier dynamics within such structures allows for photoluminescence upconversion. This Account first provides a description of the main hurdles toward the synthesis of colloidal double QDs and an overview of the growing library of synthetic pathways toward constructing them. The main discoveries regarding their photophysical properties are then described in detail, followed by an overview of potential applications taking advantage of the double-dot structure. Finally, a perspective and outlook for their future development is provided.
| S-EPMC4879659 | biostudies-other
Project description:Thanks to their broadly tunable bandgap and strong absorption, colloidal lead chalcogenide quantum dots (QDs) are highly appealing as solution-processable active layers for third-generation solar cells. However, the modest reproducibility of this kind of solar cell is a pertinent issue, which inhibits the exploitation of this material class in optoelectronics. This issue is not necessarily imputable to the active layer but may originate from different constituents of the device structure. Herein, the deposition of TiO2 electron transport layer is focused on. Atomic layer deposition (ALD) greatly improves the reproducibility of PbS QD solar cells compared with the previously optimized sol-gel (SG) approach. Power conversion efficiency (PCE) of the solar cells using atomic layer-deposited TiO2 lies in the range between 5.5% and 7.2%, whereas solar cells with SG TiO2 have PCE ranging from 0.5% to 6.9% with a large portion of short-circuited devices. Investigations of TiO2 layers by atomic force microscopy and scanning electron microscopy reveal that these films have very different surface morphologies. Whereas the TiO2 films prepared by SG synthesis and deposited by spin coating are very smooth, TiO2 films made by ALD repeat the surface texture of the fluorine-doped tin oxide (FTO) substrate underneath.
| S-EPMC7006825 | biostudies-literature
Project description:Optical sensing in the mid- and long-wave infrared (MWIR, LWIR) is of paramount importance for a large spectrum of applications including environmental monitoring, gas sensing, hazard detection, food and product manufacturing inspection, and so forth. Yet, such applications to date are served by costly and complex epitaxially grown HgCdTe quantum-well and quantum-dot infrared photodetectors. The possibility of exploiting low-energy intraband transitions make colloidal quantum dots (CQD) an attractive low-cost alternative to expensive low bandgap materials for infrared applications. Unfortunately, fabrication of quantum dots exhibiting intraband absorption is technologically constrained by the requirement of controlled heavy doping, which has limited, so far, MWIR and LWIR CQD detectors to mercury-based materials. Here, we demonstrate intraband absorption and photodetection in heavily doped PbS colloidal quantum dots in the 5-9 ?m range, beyond the PbS bulk band gap, with responsivities on the order of 10-4 A/W at 80 K. We have further developed a model based on quantum transport equations to understand the impact of electron population of the conduction band in the performance of intraband photodetectors and offer guidelines toward further performance improvement.
| S-EPMC7020105 | biostudies-literature
Project description:We present the synthesis of InAs quantum dots (QDs) with a ZnCdS shell with bright and stable emission in the near-infrared (NIR, 700-900 nm) region for biological imaging applications. We demonstrate how NIR QDs can image tumor vasculature in vivo at significantly deeper penetration depths and with higher contrast than visible emitting CdSe(CdS) QDs. Targeted cellular labeling is also presented and may enable multiplexed and low autofluorescence cellular imaging.
| S-EPMC2862004 | biostudies-literature