首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 718 毫秒
1.
A solution‐processed nanoarchitecture based on PbS quantum dots (QDs) and multi‐walled carbon nanotubes (MWCNTs) is synthesized by simply mixing the pre‐synthesized high‐quality PbS QDs and oleylamine (OLA) pre‐functionalized MWCNTs. Pre‐functionalization of MWCNTs with OLA is crucial for the attachment of PbS QDs and the coverage of QDs on the surface of MWCNTs can be tuned by varying the ratio of PbS QDs to MWCNTs. The apparent photoluminescence (steady‐state emission and fluorescence lifetime) “quenching” effect indicates efficient charge transfer from photo‐excited PbS QDs to MWCNTs. The as‐synthesized PbS‐QD/MWCNT nanoarchitecture is further incorporated into a hole‐conducting polymer poly(3‐hexylthiophene)‐(P3HT), forming the P3HT:PbS‐QD/MWCNT nanohybrid, in which the PbS QDs act as a light harvester for absorbing irradiation over a wide wavelength range of the solar spectrum up to near infrared (NIR, ≈1430 nm) range; whereas, the one‐dimensional MWCNTs and P3HT are used to collect and transport photoexcited electrons and holes to the cathode and anode, respectively. Even without performing the often required “ligand exchange” to remove the long‐chained OLA ligands, the built nanohybrid photovoltaic (PV) device exhibits a largely enhanced power conversion efficiency (PCE) of 3.03% as compared to 2.57% for the standard bulk hetero‐junction PV cell made with P3HT and [6,6]‐Phenyl‐C61‐Butyric Acid Methyl Ester (PCBM) mixtures. The improved performance of P3HT:PbS‐QD/MWCNT nanohybrid PV device is attributed to the significantly extended absorption up to NIR by PbS QDs as well as the effectively enhanced charge separation and transportation due to the integrated MWCNTs and P3HT. Our research results suggest that properly integrating QDs, MWCNTs, and polymers into nanohybrid structures is a promising approach for the development of highly efficient PV devices.  相似文献   

2.
Trap states in colloidal quantum dot (QD) solids significantly affect the performance of QD solar cells, because they limit the open‐circuit voltage and short circuit current. The {100} facets of PbS QDs are important origins of trap states due to their weak or missing passivation. However, previous investigations focused on synthesis, ligand exchange, or passivation approaches and ignored the control of {100} facets for a given dot size. Herein, trap states are suppressed from the source via facet control of PbS QDs. The {100} facets of ≈3 nm PbS QDs are minimized by tuning the balance between the growth kinetics and thermodynamics in the synthesis. The PbS QDs synthesized at a relatively low temperature with a high oversaturation follow a kinetics‐dominated growth, producing nearly octahedral nanoparticles terminated mostly by {111} facets. In contrast, the PbS QDs synthesized at a relatively high temperature follow a thermodynamics‐dominated growth. Thus, a spherical shape is preferred, producing truncated octahedral nanoparticles with more {100} facets. Compared to PbS QDs from thermodynamics‐dominated growth, the PbS QDs with less {100} facets show fewer trap states in the QD solids, leading to a better photovoltaic device performance with a power conversion efficiency of 11.5%.  相似文献   

3.
Quasi type‐II PbSe/PbS quantum dots (QDs) are employed in a solid state high efficiency QD/TiO2 heterojunction solar cell. The QDs are deposited using layer‐by‐layer deposition on a half‐micrometer‐thick anatase TiO2 nanosheet film with (001) exposed facets. Theoretical calculations show that the carriers in PbSe/PbS quasi type‐II QDs are delocalized over the entire core/shell structure, which results in better QD film conductivity compared to PbSe QDs. Moreover, PbS shell permits better stability and facile electron injection from the QDs to the TiO2 nanosheets. To complete the electrical circuit of the solar cell, a Au film is evaporated as a back contact on top of the QDs. This PbSe/PbS QD/TiO2 heterojunction solar cell produces a light to electric power conversion efficiency (η) of 4% with short circuit photocurrent (Jsc) of 17.3 mA/cm2. This report demonstrates highly efficient core/shell near infrared QDs in a QD/TiO2 heterojunction solar cell.  相似文献   

4.
Here, highly efficient and stable monolithic (2-terminal (2T)) perovskite/PbS quantum dots (QDs) tandem solar cells are reported, where the perovskite solar cell (PSC) acts as the front cell and the PbS QDs device with a narrow bandgap acts as the back cell. Specifically, ZnO nanowires (NWs) passivated by SnO2 are employed as an electron transporting layer for PSC front cell, leading to a single cell PSC with maximum power conversion efficiency (PCE) of 22.15%, which is the most efficient NWs-based PSCs in the literature. By surface passivation of PbS QDs by CdCl2, QD devices with an improved open-circuit voltage and a PCE of 8.46% (bandgap of QDs: 0.92 eV) are achieved. After proper optimization, 2T and 4T tandem devices with stabilized PCEs of 17.1% and 21.1% are achieved, respectively, where the 2T tandem device shows the highest efficiency reported in the literature for this design. Interestingly, the 2T tandem cell shows excellent operational stability over 500 h under continuous illumination with only 6% PCE loss. More importantly, this device without any packaging depicts impressive ambient stability (almost no change) after 70 days in an environment with controlled 65% relative humidity, thanks to the superior air stability of the PbS QDs.  相似文献   

5.
The major impediment to the high photovoltaic performance of organic solar cells (OSCs) involves deficient photon harvesting and ineffective charge transfer from the photoactive layer to the electrodes. To improve these constraints, in this study, a new OSC device architecture is demonstrated by incorporating PbS colloidal quantum dots (QDs) between the organic photoactive layer and the top electrode. PbS QDs were spin-coated on top of an organic blend via a layer-by-layer deposition process, which formed a separate PbS QD layer with high density and uniformity. The PbS QD layer reinforced the optical property of the OSC by harvesting photons that were not absorbed by the underlying organic photoactive layer. In addition, the OSC employing the QD layer showed the enhanced charge transfer and suppressed recombination loss through the hybrid organic-inorganic interfacial contacts. Thus, a significant increase in the efficiency was achieved compared with the OSC with no PbS QD layer (10.12 vs 8.84%). Accompanied with the improved optoelectronic properties, a superior stability of the proposed architecture advances the practical viability of OSCs in various applications.  相似文献   

6.
Hybrid organic‐inorganic halide perovskites are actively pursued for optoelectronic technologies, but the poor stability is the Achilles’ heel of these materials that hinders their applications. Very recently, it has been shown that lead sulfide (PbS) quantum dots (QDs) can form epitaxial interfaces with the perovskite matrix and enhance the overall stability. In this work, it is demonstrated that embedding QDs can significantly modify the transport property of pristine perovskite single crystals, endowing them with new functionalities besides being structurally robust and free from grain boundaries. Resistive switching memory devices are constructed using solution‐processed CH3NH3PbBr3 (MAPbBr3) perovskite single crystals and the QD‐embedded counterparts. It is found that QDs could significantly enhance the charge transport and reduce the current–voltage hysteresis. The pristine singe crystal device exhibits negative differential resistance, while the QD‐embedded crystals are featured with filament‐type switching behavior and much improved device stability. This study underscores the potential of QD‐embedded hybrid perovskites as a new media for advanced electronic devices.  相似文献   

7.
Lead chalcogenide quantum dot (QD) infrared (IR) solar cells are promising devices for breaking through the theoretical efficiency limit of single-junction solar cells by harvesting the low-energy IR photons that cannot be utilized by common devices. However, the device performance of QD IR photovoltaic is limited by the restrictive relation between open-circuit voltages (VOC) and short circuit current densities (JSC), caused by the contradiction between surface passivation and electronic coupling of QD solids. Here, a strategy is developed to decouple this restriction via epitaxially coating a thin PbS shell over the PbSe QDs (PbSe/PbS QDs) combined with in situ halide passivation. The strong electronic coupling from the PbSe core gives rise to significant carrier delocalization, which guarantees effective carrier transport. Benefited from the protection of PbS shell and in situ halide passivation, excellent trap-state control of QDs is eventually achieved after the ligand exchange. By a fine control of the PbS shell thickness, outstanding IR JSC of 6.38 mA cm−2 and IR VOC of 0.347 V are simultaneously achieved under the 1100 nm-filtered solar illumination, providing a new route to unfreeze the trade-off between VOC and JSC limited by the photoactive layer with a given bandgap.  相似文献   

8.
Infrared solar cells that utilize low‐bandgap colloidal quantum dots (QDs) are promising devices to enhance the utilization of solar energy by expanding the harvested photons of common photovoltaics into the infrared region. However, the present synthesis of PbS QDs cannot produce highly efficient infrared solar cells. Here, a general synthesis is developed for low‐bandgap PbS QDs (0.65–1 eV) via cation exchange from ZnS nanorods (NRs). First, ZnS NRs are converted to superlattices with segregated PbS domains within each rod. Then, sulfur precursors are released via the dissolution of the ZnS NRs during the cation exchange, which promotes size focusing of PbS QDs. PbS QDs synthesized through this new method have the advantages of high monodispersity, ease‐of‐size control, in situ passivation of chloride, high stability, and a “clean” surface. Infrared solar cells based on these PbS QDs with different bandgaps are fabricated, using conventional ligand exchange and device structure. All of the devices produced in this manner show excellent performance, showcasing the high quality of the PbS QDs. The highest performance of infrared solar cells is achieved using ≈0.95 eV PbS QDs, exhibiting an efficiency of 10.0% under AM 1.5 solar illumination, a perovskite‐filtered efficiency of 4.2%, and a silicon‐filtered efficiency of 1.1%.  相似文献   

9.
Colloidal lead sulfide (PbS) quantum dots (QDs), which possess quantum confinement effect and processing compatibility with perovskite, are regarded as an excellent material for optimizing perovskite solar cells (PSCs). However, the existing PSCs optimized by PbS QDs are still facing the challenges of poor performance of the charge transport layers, low utilization in the near-infrared (NIR) region, and unsuitable energy level alignment, which limit the improvement of power conversion efficiency (PCE). Herein, a synchronous optimization strategy is realized via simultaneously introducing PbS QDs into SnO2 electron transport layer and employing rare-earth-doped PbS QDs (Eu:PbS QDs) film with hydrophobic chain ligands as the NIR light-absorping layer and hole transport layer (HTL) of devices. PbS QDs effectively decrease the density of trap states by passivating defects. Eu:PbS QDs film with adjustable bandgap is employed as an absorption layer to broaden the NIR spectral absorption. The well-matched energy level between Eu:PbS QDs layer and perovskite layer implies efficient hole transfer at the interface. The successful synchronous optimization greatly elevates all photovoltaic parameters, reaching a maximum PCE of 23.27%. This PCE is the highest for PSCs utilizing PbS QDs material in recent years. The optimized PSCs retain long-term moisture and light stability.  相似文献   

10.
Light harvesting from large size of semiconductor PbS quantum dots (QDs) with a bandgap of less than 1 eV is one of the greatest challenges precluding the development of PbS QD‐based solar cells because the interfacial charge transfer (CT) from such QDs to the most commonly used electron acceptor materials is very inefficient, if it occurs at all. Thus, an alternative electron‐accepting unit with a new driving force for CT is urgently needed to harvest the light from large‐sized PbS QDs. Here, a cationic porphyrin is utilized as a new electron acceptor unit with unique features that bring the donor–acceptor components into close molecular proximity, allowing ultrafast and efficient electron transfer for QDs of all sizes, as inferred from the drastic photoluminescence quenching and the ultrafast formation of the porphyrin anionic species. The time‐resolved results clearly demonstrate the possibility of modulating the electron transfer process between PbS QDs and porphyrin moieties not only by the size quantization effect but also by the interfacial electrostatic interaction between the positively charged porphyrin and the negatively charged QDs. This approach provides a new pathway for engineering QD‐based solar cells that make the best use of the diverse photons making up the Sun's broad irradiance spectrum.  相似文献   

11.
《Organic Electronics》2014,15(2):391-398
We present two novel techniques for improving the efficiency of PbS quantum dot (QD) solar cells. First, plasma was applied to QD film with the aim of removing surface organic ligands, and then the chemical and optical properties of the QDs were investigated. Second, a thin layer of conjugated polymer was then deposited on top of the plasma-treated PbS QD film as a transportation layer for holes. The charge separation and subsequent transfer dynamics were examined, as were the resultant photovoltaic characteristics, according to the kind of polymer used. The developed device, which comprises a bilayer heterojunction of plasma-treated PbS QDs and poly[2,6-(4,4′-bis(2-ethylhexyl)dithieno[3,2-b:2′,3′-d]silole)-alt-4,7(2,1,3-benzothiadiazole)] (PSBTBT), showed not only broad-range absorption of the solar spectrum, but also high charge transfer efficiency prior to recombination. This results in a largely increased power conversion efficiency (PCE) of 1.76%, compared to the 0.7% value of a PbS QD-only device not subjected to plasma treatment. This indicates that the proposed techniques are very useful for improving the efficiency of inorganic QD-based solar cells.  相似文献   

12.
The pulsed laser deposition (PLD) technique is used for the direct fabrication of nanohybrid heterojunctions (NH‐HJs) solar cells exhibiting high PCE and excellent stability in air without any encapsulation and/or resorting to any surface treatment, ligand engineering and/or post‐synthesis processing. The NH‐HJs are achieved through the PLD‐based decoration of hydrothermally‐grown one‐dimensional TiO2 nanorods (TiO2‐NRs) by PbS quantum dots (PbS‐QDs). By optimizing both the amount of PbS‐QDs (via the number of laser ablation pulses) and the length of the TiO2‐NRs, it is possible to achieve optimal NH‐HJs based PV devices with high power conversion efficiency (PCE) of 4.85%. This high PCE is found to occur for an optimal length of the NRs (≈290 nm) which coincides with the average penetration depth of PbS‐QDs into the porous TiO2‐NRs matrix, leading thereby to the formation of the largest extent of NH‐HJs. Most importantly, the PCE of these novel devices is found to be fairly stable for several months under ambient air. The addition of single‐wall carbon nanotubes (SWCNTs) onto the TiO2‐NRs prior to their decoration by PbS‐QDs is shown to further enhance their PCE to a value as high as 5.3%, because of additional light absorption and improved charge collection ensured by SWCNTs.  相似文献   

13.
Solution‐processed core/multishell semiconductor quantum dots (QDs) could be tailored to facilitate the carrier separation, promotion, and recombination mechanisms necessary to implement photon upconversion. In contrast to other upconversion schemes, upconverting QDs combine the stability of an inorganic crystalline structure with the spectral tunability afforded by quantum confinement. Nevertheless, their upconversion quantum yield (UCQY) is fairly low. Here, design rules are uncovered that enable to significantly enhance the performance of double QD upconversion systems, and these findings are leveraged to fabricate upconverting QDs with increased photon upconversion efficiency and reduced saturation intensities under pulsed excitation. The role of the intra‐QD band alignment is exemplified by comparing the upconversion process in PbS/CdS/ZnSe QDs with that of PbS/CdS/CdSe ones with variable CdSe shell thicknesses. It is shown that electron delocalization into the shell leads to a longer‐lived intermediate state in the QDs, facilitating further absorption of photons, and enhancing the upconversion process. The performance of these upconversion QDs under pulsed excitation versus continuous pumping is also compared; the reasons for the significant differences between these two regimes are discussed. The results show how one can overcome some of the limitations of previous upconverting QDs, with potential applications in biophotonics and infrared detection.  相似文献   

14.
Lead sulfide (PbS) and cadmium sulfide (CdS) quantum dots (QDs) are prepared over mesoporous TiO2 films by a successive ionic layer adsorption and reaction (SILAR) process. These QDs are exploited as a sensitizer in solid‐state solar cells with 2,2′,7,7′‐tetrakis(N,N‐di‐p‐methoxyphenylamine)‐9,9′‐spirobifluorene (spiro‐OMeTAD) as a hole conductor. High‐resolution transmission electron microscopy (TEM) images reveal that PbS QDs of around 3 nm in size are distributed homogeneously over the TiO2 surface and are well separated from each other if prepared under common SILAR deposition conditions. The pore size of the TiO2 films and the deposition medium are found to be very critical in determining the overall performance of the solid‐state QD cells. By incorporating promising inorganic QDs (PbS) and an organic hole conductor spiro‐OMeTAD into the solid‐state cells, it is possible to attain an efficiency of over 1% for PbS‐sensitized solid‐state cells after some optimizations. The optimized deposition cycle of the SILAR process for PbS QDs has also been confirmed by transient spectroscopic studies on the hole generation of spiro‐OMeTAD. In addition, it is established that the PbS QD layer plays a role in mediating the interfacial recombination between the spiro‐OMeTAD+ cation and the TiO2 conduction band electron, and that the lifetime of these species can change by around 2 orders of magnitude by varying the number of SILAR cycles used. When a near infrared (NIR)‐absorbing zinc carboxyphthalocyanine dye (TT1) is added on top of the PbS‐sensitized electrode to obtain a panchromatic response, two signals from each component are observed, which results in an improved efficiency. In particular, when a CdS‐sensitized electrode is first prepared, and then co‐sensitized with a squarine dye (SQ1), the resulting color change is clearly an addition of each component and the overall efficiencies are also added in a more synergistic way than those in PbS/TT1‐modified cells because of favorable charge‐transfer energetics.  相似文献   

15.
In this article, we will focus on the carrier relaxation time in quantum dots (QDs), its probable mechanism, and the implications for the performance characteristics of directly modulated QD lasers and other QD devices. The electron and hole bound states and general predictions of carrier capture time into them will be presented, followed by a discussion of intersubband carrier relaxation in QDs. The modulation characteristics of QD lasers as a function of temperature will be described, and these modulation results will be discussed in terms of the temperature, composition, and size dependence of the relaxation time in QDs, including possible methods for designing QDs to overcome this relaxation time barrier. Also, the performance characteristics of other possible QD devices, such as intersubband lasers and detectors, will be examined in terms of our current understanding of the relaxation time in QDs  相似文献   

16.
This study demonstrated the feasibility of fabricating a highly stacked vertically aligned InGaAs/GaAs(Sb) quantum dot (QD) structure with an AlGaAsSb spacer layer for improving the device performance of QD intermediate‐band solar cell (QD‐IBSC) devices. The power‐dependent photoluminescence measurements of the proposed structure revealed a blueshift in the QD ground‐state emissions when the excitation power was increased, indicating the formation of an intermediate band inside the QD structure. Capping the InGaAs QDs with a GaAsSb layer prevented the QDs from collapsing because there was less In–Ga intermixing between the QDs and GaAsSb layer. In addition to maintaining the QD structure, the carrier lifetime was extended by tuning the energy band alignment of the InGaAs/GaAsSb QD structure. Inserting the AlGaAsSb layer into the spacer layer increased the band gap, which in turn increased the open‐circuit voltage of the QD‐IBSC. The QD‐IBSC in this work shows an extension of external‐quantum efficiency by up to 1200 nm (compared with a GaAs reference cell) through the absorption by QDs and increased the open‐circuit voltage from 0.67 to 0.70 V by adopting the AlGaAsSb spacer layer. These results confirm that adopting a columnar InGaAs/GaAs(Sb) QD structure with a AlGaAsSb spacer layer can enhance the performance of QD‐IBSC devices. Copyright © 2016 John Wiley & Sons, Ltd.  相似文献   

17.
Indium phosphide-based colloidal quantum dot (QD) light-emitting diodes represent a promising technology for various lighting applications. To promote this innovative technology closer to an industrialized production environment, the fabrication methods should be adapted. Hence it is necessary to replace the common spin-coating process under an inert atmosphere, by a more cost-efficient inkjet-printing process at ambient conditions. However, in our case, this transfer results in devices with limited performance and parasitic emission channels besides the desired QD emission. In this paper, we identify the physical origin of these parasitic emission channels for three different device layouts depending on the QD material as well as the number of inkjet-printed layers. For the first type of devices, a recombination process on the dopant of the electron transporting layer (ETL) as well as an exciplex formation at the interface between QDs and ETL was identified. For the next device layout, the introduction of a hole-conducting matrix embedding the QDs leads to a shift of the parasitic emission with contributions from the matrix material. Finally, the integration of a hole injection layer leads to a reduction of the undesired emission processes. For all three kinds of devices, the spacial separation of the dopant in the ETL from the QDs is a critical factor, since it directly influences the parasitic emission channels.  相似文献   

18.
Over the past decade, near‐infrared (NIR)‐emitting nanoparticles have increasingly been investigated in biomedical research for use as fluorescent imaging probes. Here, high‐quality water‐dispersible core/shell/shell PbS/CdS/ZnS quantum dots (hereafter QDs) as NIR imaging probes fabricated through a rapid, cost‐effective microwave‐assisted cation exchange procedure are reported. These QDs have proven to be water dispersible, stable, and are expected to be nontoxic, resulting from the growth of an outer ZnS shell and the simultaneous surface functionalization with mercaptopropionic acid ligands. Care is taken to design the emission wavelength of the QDs probe lying within the second biological window (1000–1350 nm), which leads to higher penetration depths because of the low extinction coefficient of biological tissues in this spectral range. Furthermore, their intense fluorescence emission enables to follow the real‐time evolution of QD biodistribution among different organs of living mice, after low‐dose intravenous administration. In this paper, QD platform has proven to be capable (ex vivo and in vitro) of high‐resolution thermal sensing in the physiological temperature range. The investigation, together with the lack of noticeable toxicity from these PbS/CdS/ZnS QDs after preliminary studies, paves the way for their use as outstanding multifunctional probes both for in vitro and in vivo applications in biomedicine.  相似文献   

19.
We report on interplay of epitaxial growth phenomena and device performance in quantum dot (QD) and quantum wire (QWW) lasers based on self-organized nanostructures. InAs QDs are the most explored model system for basic understanding of "near-ideal" QD devices. Vertically-coupled growth of QDs and activated phase separation allow ultimate QD wavefunction engineering enabling GaAs lasers beyond 1400 nm and polarization-insensitive optical amplification. A feasibility of QD semiconductor optical amplifiers at terabit frequencies using InAs QDs is manifested at 1300 and 1500 nm. 1250-1300 nm QD GaAs edge emitters and VCSELs operate beyond 10 Gb/s with ultimate temperature robustness. Furthermore, temperature-insensitive operation without current or modulation voltage adjustment at >20 Gb/s is demonstrated up to ~90 degC. Light-emitting devices based on InGaN-QDs cover ultraviolet (UV) and visible blue-green spectral ranges. In these applications, InN-rich nanodomains prevent diffusion of nonequilibrium carries towards crystal defects and result in advanced degradation robustness of the devices. All the features characteristic to QDs are unambiguously confirmed for InGaN structures. For the red spectral range InGaAlP lasers are used. Growth on misoriented surfaces, characteristic to these devices, leads to nano-periodi- cally-step-bunched epitaxial surfaces resulting in two principal effects: 1) step-bunch-assisted alloy phase separation, leading to a spontaneous formation of ordered natural super lattices; 2) formation of quantum wire-like structures in the active region of the device. A high degree of polarization is revealed in the luminescence recorded from the top surface of the structures, in agreement with the QWW nature of the gain medium. QD and QWW lasers are remaining at the frontier of the modern optoelectronics penetrating into the mainstream applications in key industries.  相似文献   

20.
Low‐dimensional III–V semiconductors have many advantages over other semiconductors; however, they are not particularly stable under physiological conditions. Hybridizing biocompatible organic molecules with advanced optical and electronic semiconductor devices based on quantum dots (QDs) and quantum wires could provide an efficient solution to realize stress‐free and nontoxic interfaces to attach larger functional biomolecules. Monitoring the modifications of the optical properties of the hybrid molecule–QD systems by grafting various types of air‐stable diazonium salts onto the QD structures surfaces provides a direct approach to prove the above concepts. The InAs/GaAs QD structures used in this work consist of a layer of surface InAs QDs and a layer of buried InAs QDs embedded in a wider‐bandgap GaAs matrix. An enhancement in photoluminescence intensity by a factor of 3.3 from the buried QDs is achieved owing to the efficient elimination of the dangling bonds on the surface of the structures and to the decrease in non‐radiative recombination caused by their surface states. Furthermore, a narrow photoluminescence band peaking at 1620 nm with a linewidth of 49 meV corresponding to the eigenstates interband transition of the surface InAs QDs is for the first time clearly observed at room temperature, which is something that has rarely been achieved without the use of such engineered surfaces. The experimental results demonstrate that the hybrid molecule–QD systems possess a high stability, and both the surface and buried QDs are very sensitive to changes in their surficial conditions, indicating that they are excellent candidates as basic sensing elements for novel biosensor applications.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号