Photostability of colloidal single photon emitter in near-infrared regime at room temperature

The photostability of a colloidal single photon emitter in near-infrared regime at room temperature is investigated.The fluorescence lifetime,blinking phenomenon,and anti-bunching effect of a single CdTeSe/ZnS quantum dot with an emission wavelength of 800 nm at room temperature are studied.The second-order correlation function at zero delay time is much smaller than 0.1,which proves that the emission from single quantum dots at 800 nm is a highly pure single-photon source.The effects of the irradiation duration on the fluorescence from single quantum dots are analyzed.The experimental results can be explained by a recombination model including a multi-nonradiative recombination center model and a multi-charged model.

A Furan-Substituted Polymeric Hole-Transporting Material for Energy Level Regulation and Less Planarity in Colloidal Quantum Dot Solar Cells

For efficient colloidal quantum dot(CQD)solar cells(CQD-SCs),thiol-passivated p-type CQDs are generally used as a hole-transporting material(HTM);however,there are issues with the control of optoelectrical properties,low thiol passivation rate,and poor morphology with a power conversion efficiency(PCE)of approximately 11%.Although polymeric HTMs have been introduced to address these issues,maximizing efficiency and achieving green-solvent processability and thermal stability for commercialization is necessary.Here,we synthesize a novel benzodifuran(BDF)-based HTM(asy-ranPBTBDF)showing an electron-deficient state,low steric hindrance,and low planarity compared to those of a typical benzodithiophene(BDT)-based HTM(asy-ranPBTBDT).BDF properties lead to deep high occupied molecular orbital(HOMO)levels,closeπ-πstacking,excellent solubility,and amorphous properties related to efficiency,green-solvent processability,and thermal stability.With these benefits,the asy-ranPBTBDF-based CQD-SC showed enhanced open-circuit voltage(Voc)(0.65 V)and PCE(13.29%)compared to those of the asy-ranPBTBDT-based device(0.63 V and 12.22%)in toxic processes with chlorobenzene.The asy-ranPBTBDF-based CQD-SC showed a PCE of 12.51%in a green-solvent process with 2-methylanisole and improved thermal stability at 80℃(83.8%retaining after 24 h)owing to less lateral crystallization than the asy-ranPBTBDT-based device(60.8%retaining after 24 h).

Review of roll-to-roll fabrication techniques for colloidal quantum dot solar cells

Colloidal quantum dots(CQDs)are of great interest to photovoltaic(PV)technologies as they possess the benefits of solution-processability,size-tunability,and roll-to-roll manufacturability,as well as unique capabilities to harvest near-infrared(NIR)radiation.During the last decade,lab-scale CQD solar cells have achieved rapid improvement in the power conversion efficiency(PCE)from~1%to 18%,which will potentially exceed 20%in the next few years and approach the performance of other PV technologies,such as perovskite solar cells and organic solar cells.In the meanwhile,CQD solar cells exhibit long lifetimes either under shelf storage or continuous operation,making them highly attractive to industry.However,in order to meet the industrial requirements,mass production techniques are necessary to scale up the fabrication of those lab devices into large-area PV modules,such as roll-to-toll coating.This paper reviews the recent developments of large-area CQD solar cells with a focus on various fabrication methods and their principles.It covers the progress of typical large-area coating techniques,including spray coating,blade coating,dip coating,and slot-die coating.It also discusses next steps and new strategies to accomplish the ultimate goal of the low-cost large-area fabrication of CQD solar cells and emphasizes how artificial intelligence or machine learning could facilitate the developments of CQD solar cell research.

Recent progress of colloidal quantum dot based solar cells

Colloidal quantum dot （CQD） solar cells have attracted great interest due to their low cost and superior photo-electric properties. Remarkable improvements in cell performances of both quantum dot sensitized solar cells （QDSCs） and FbX （X = S, Se） based CQD solar cells have been achieved in recent years, and the power conversion efficiencies （PCEs） ex- ceeding 12% were reported so far. In this review, we will focus on the recent progress in CQD solar cells. We firstly summarize the advance of CQD sensitizer materials and the strategies for enhancing carrier collection efficiency in QD- SCs, including developing multi-component alloyed CQDs and core-shell structured CQDs, as well as various methods to suppress interfacial carrier recombination. Then, we discuss the device architecture development of PbX CQD based solar cells and surface/interface passivation methods to increase light absorption and carrier extraction efficiencies. Finally, a short summary, challenge, and perspective are given.

Surface-Modified Graphene Oxide/Lead Sulfide Hybrid Film-Forming Ink for High-Efficiency Bulk Nano-Heterojunction Colloidal Quantum Dot Solar Cells

Solution-processed colloidal quantum dot solar cells(CQDSCs) is a promising candidate for new generation solar cells.To obtain stable and high performance lead sulfide(PbS)-based CQDSCs,high carrier mobility and low non-radiative recombination center density in the PbS CQDs active layer are required.In order to effectively improve the carrier mobility in PbS CQDs layer of CQDSCs,butylamine(BTA)-modified graphene oxide(BTA@GO) is first utilized in PbS-PbX2(X=I-,Br-) CQDs ink to deposit the active layer of CQDSCs through one-step spin-coating method.Such surface treatment of GO dramatically upholds the intrinsic superior hole transfer peculiarity of GO and attenuates the hydrophilicity of GO in order to allow for its good dispersibility in ink solvent.The introduction of B TA@GO in CQDs layer can build up a bulk nano-heterojunction architecture,which provides a smooth charge carrier transport channel in turn improves the carrier mobility and conductivity,extends the carriers lifetime and reduces the trap density of PbS-PbX2 CQDs film.Finally,the BTA@GO/PbS-PbX2 hybrid CQDs film-based relatively large-area(0.35 cm2) CQDSCs shows a champion power conversion efficiency of 11.7% which is increased by 23.1% compared with the control device.

Modification of the spontaneous emission of quantum dots near the surface of a three-dimensional colloidal photonic crystal

This paper demonstrates experimentally and numerically that a significant modification of spontaneous emission rate can be achieved near the surface of a three-dimensional photonic crystal. In experiments, semiconductor coreshell quantum dots are intentionally confined in a thin polymer film on which a three-dimensional colloidal photonic crystal is fabricated. The spontaneous emission rate of quantum dots is characterised by conventional and time-resolved photoluminescence （PL） measurements. The modification of the spontaneous emission rate, which is reflected in the change of spectral shape and PL lifetime, is clearly observed. While an obvious increase in the PL lifetime is found at most wavelengths in the band gap, a significant reduction in the PL lifetime by one order of magnitude is observed at the short-wavelength band edge. Numerical simulation reveals a periodic modulation of spontaneous emission rate with decreasing modulation strength when an emitter is moved away from the surface of the photonic crystal. It is supported by the fact that the modification of spontaneous emission rate is not pronounced for quantum dots distributed in a thick polymer film where both enhancement and suppression are present simultaneously. This finding provides a simple and effective way for improving the performance of light emitting devices.

Recent progress of infrared photodetectors based on lead chalcogenide colloidal quantum dots

Commercial photodetectors based on silicon are extensively applied in numerous fields. Except for their high performance, their maximum absorption wavelength is not over than 1100 nm and incident light with longer wavelengths cannot be detected; in addition, their cost is high and their manufacturing process is complex. Therefore, it is meaningful and significant to extend absorption wavelength, to decrease cost, and to simplify the manufacturing process while maintaining high performance for photodetectors. Due to the properties of size-dependent bandgap tunability, low cost, facile processing,and substrate compatibility, solution–processed colloidal quantum dots(CQDs) have recently gained significant attention and become one of the most competitive and promising candidates for optoelectronic devices. Among these CQDs, lead chalcogenide CQDs are getting very prominent and are widely investigated. In this paper, the recent progress of infrared(IR) photodetectors based on lead sulfide(PbS), lead selenide(PbSe), and ternary PbS_x Se_(1-x) CQDs, and their underlying concepts, breakthroughs, and remaining challenges are reviewed, thus providing guidance for designing high-performance quantum-dot IR photodetectors.

Novel Hybrid Ligands for Passivating Pb S Colloidal Quantum Dots to Enhance the Performance of Solar Cells

We developed novel hybrid ligands to passivate Pb S colloidal quantum dots(CQDs),and two kinds of solar cells based on as-synthesized CQDs were fabricated to verify the passivation effects of the ligands.It was found that the ligands strongly affected the optical and electrical properties of CQDs,and the performances of solar cells were enhanced strongly.The optimized hybrid ligands,oleic amine/octyl-phosphine acid/Cd Cl2improved power conversion efficiency(PCE)to much higher of 3.72%for Schottky diode cell and 5.04%for p–n junction cell.These results may be beneficial to design passivation strategy for low-cost and high-performance CQDs solar cells.

Colloidal quantum dot lasers and hybrid integrations

Colloidal quantum dots (CQDs) are semiconductor nanocrystalswith diameters about 2 to 20 nm. At such nanoscales,the CQDs exhibit obvious quantum and dielectric confinementeffects[1]. The CQDs are usually composed of II–VI, III–V,and IV–VI semiconductors fabricated by the low-cost wet chemicalsynthetic methods. The emission wavelengths of CQDs,which can be easily tuned by the sizes, shapes, and compositions,have already covered the whole range of the visible andnear-infrared (NIR) spectra (from 440 to 1530 nm). Owing tothe low-cost fabrications, high quantum yields (QYs^100%), tunableemission wavelengths, and outstanding stability, the solution-processable CQDs can act as the nanoscale buildingblocks with large gains, and they have attracted enormous attentionin the lasing applications in the past decade.

Unraveling the efficiency losses and improving methods in quantum dot-based infrared up-conversion photodetectors

Quantum dot-based up-conversion photodetector,in which an infrared photodiode(PD)and a quantum dot light-emitting diode(QLED)are back-to-back connected,is a promising candidate for low-cost infrared imaging.However,the huge efficiency losses caused by integrating the PD and QLED together hasn’t been studied sufficiently.This work revealed at least three origins for the efficiency losses.First,the PD unit and QLED unit usually didn’t work under optimal conditions at the same time.Second,the potential barriers and traps at the interconnection between PD and QLED units induced unfavorable carrier recombination.Third,much emitted visible light was lost due to the strong visible absorption in the PD unit.Based on the understandings on the loss mechanisms,the infrared up-conversion photodetectors were optimized and achieved a breakthrough photon-to-photon conversion efficiency of 6.9%.This study provided valuable guidance on how to optimize the way of integration for up-conversion photodetectors.

Double-ended passivator enables dark-current-suppressed colloidal quantum dot photodiodes for CMOS-integrated infrared imagers

Lead sulfide(PbS)colloidal quantum dot(CQD)photodiodes integrated with silicon-based readout integrated circuits(ROICs)offer a promising solution for the next-generation short-wave infrared(SWIR)imaging technology.Despite their potential,large-size CQD photodiodes pose a challenge due to high dark currents resulting from surface states on nonpassivated(100)facets and trap states generated by CQD fusion.In this work,we present a novel approach to address this issue by introducing double-ended ligands that supplementally passivate(100)facets of halidecapped large-size CQDs,leading to suppressed bandtail states and reduced defect concentration.Our results demonstrate that the dark current density is highly suppressed by about an order of magnitude to 9.6 nA cm^(2) at -10 mV,which is among the lowest reported for PbS CQD photodiodes.Furthermore,the performance of the photodiodes is exemplary,yielding an external quantum efficiency of 50.8%(which corresponds to a responsivity of 0.532 A W^(-1))and a specific detectivity of 2.5×10^(12) Jones at 1300 nm.By integrating CQD photodiodes with CMOS ROICs,the CQD imager provides high-resolution(640×512)SWIR imaging for infrared penetration and material discrimination.

Colloidal quantum dot for infrared-absorbing solar cells:State-oftheart and prospects

Colloidal quantum dot(CQD)shows great potential for application in infrared solar cells due to the simple synthesis techniques,tunable infrared absorption spectrum,and high stability and solution-processability.Thanks to significant efforts made on the surface chemistry of CQDs,device structure optimization,and device physics of CQD solar cells(CQDSCs),remarkable breakthroughs are achieved to boost the infrared photovoltaic performance and stability of CQDSCs.In particular,the CQDSC with a high power conversion efficiency of~14%and good stability is reported,which is very promising for infrared-absorbing solar cells.In this review,we highlight the unique optoelectronic properties of CQDs for the development of infrared-absorbing solar cells.Meanwhile,the latest advances in finely controlling surface properties of CQDs are comprehensively summarized and discussed.Moreover,the device operation of CQDSCs is discussed in-depth to highlight the impact of the device structure optimization of CQDSCs on their photovoltaic performance,and the emerging novel types of CQDSCs,such as semitransparent,flexible,and lightweight CQDSCs,are also demonstrated.The device stability of CQDSCs is also highlighted from the viewpoint of practical applications.Finally,the conclusions and possible challenges and opportunities are presented to promote the development steps of the CQDSCs with higher infrared photovoltaic performance and robust stability.

Ligand engineering of colloid quantum dots and their application in all-inorganic tandem solar cells

How to effectively utilize the energy of the broad spectrum of sunlight is one of the basic problems in the research of tandem solar cells. Due to their size effect, quantum confinement effect and coupling effect, colloidal quantum dots(QDs) exhibit new physical properties that bulk materials don’t possess.CdX(X = Se, S, etc.) and Pb X(X = Se, S, etc.) QDs prepared by hot-injection methods have been widely studied in the areas of photovolitaic devices. However, the surfactants surrounding QDs seriously hinder the charge transport of QDs based solar cells. Therefore, how to fabricate high-performance tandem solar cells via ligands engineering has become a major challenge. In this paper, the latest progress of colloidal QDs in the research of all-inorganic tandem solar cells was summarized. Firstly, the improvement of QDs surface ligands and the optimization of ligands engineering were discussed, and the control of the physical properties of QDs films were realized. From the aspects of colloidal QDs, ligand engineering, and solar cell preparation, the future development direction of colloidal QDs solar cells was proposed, providing technical guidances for the preparation of low-cost and high-efficiency nanocrystalline solar cells.

Magnetotransport properties of graphene layers decorated with colloid quantum dots

The hybrid graphene-quantum dot devices can potentially be used to tailor the electronic, optical, and chemical properties of graphene. Here, the low temperature electronic transport properties of bilayer graphene decorated with PbS colloid quantum dots(CQDs) have been investigated in the weak or strong magnetic fields. The presence of the CQDs introduces additional scattering potentials that alter the magnetotransport properties of the graphene layers, leading to the observation of a new set of magnetoconductance oscillations near zero magnetic field as well as the high-field quantum Hall regime.The results bring about a new strategy for exploring the quantum interference effects in two-dimensional materials which are sensitive to the surrounding electrostatic environment, and open up a new gateway for exploring the graphene sensing with quantum interference effects.

硫化铅胶体量子点的溶剂工程及光电器件性能研究

量子点光电器件以近红外吸收的硫化铅(PbS)胶体量子点(CQDs)为代表,因其带隙可调、吸收系数高、具备多激子效应和可溶液化加工等优点而受到广泛关注。然而,囿于胶体稳定性,PbS CQDs光电器件大规模制备困难、商业化进度迟缓。为解决该问题,本工作首先通过配体交换制备了溶液稳定性良好的量子点,进而开发了新型正丁胺/氯苯混合溶剂。以正丁胺为溶剂的量子点在空气条件下最多保存3 d,而以正丁胺/氯苯为溶剂的量子点可以保存至少15 d。紫外可见吸收光谱和荧光光谱结果显示混合溶剂中的量子点表现出优异的尺寸均一性。最终,通过该溶剂工程制备的PbS CQDs太阳能电池器件光电转换效率达到了5.18%,光电探测器的响应度和探测率分别为0.18 A·W^(-1)和1.05×10^(12)Jones。

Infrared-harvesting colloidal quantum dot inks for efficient photovoltaics: Impact of surface chemistry and device engineering

Colloidal quantum dots(CQDs)are promising semiconducting materials,which can be used as a photoactive layer in various optoelectronic applications,because of their size-tunable bandgap energy,solution processability,and excellent optical and optoelectronic properties.In particular,these features have generated great interest in the development of CQD solar cells and led to a rapid increase in their power conversion efficiency.These improvements were enabled by many innovative approaches in terms of CQD’s surface chemistry and device architecture optimizations.In this review,a critical overview of the research progress in CQD solar cells is presented with a focus on the strategies adopted for achieving record efficiency in CQD solar cells.These strategies include the use of organic/inorganic surface ligands,pre-and post-treatment of CQDs,and solid-state/solution-phase ligand exchange.Additionally,we provide an understanding of the research history to inspire the rational design of next-generation CQD optoelectronic devices,such as solar cells,light-emitting diodes,and photodetectors.Recent research on the development of infrared CQD solar cells as complementary platforms to other solar cell technologies is also critically discussed to provide another perspective on CQD technologies.

Electrochemical biosensor employing PbS colloidal quantum dots/Au nanospheres-modified electrode for ultrasensitive glucose detection

Rapid and accurate detection of glucose is of great significance for diabetic management.Highly sensitive glucose sensors promise to achieve noninvasive detection technology,enabling more convenient and efficient means for large-scale screening and long-term dynamic monitoring of diabetes patients.In this work,we demonstrate a sensitive glucose electrochemical biosensor through the synergetic labelling strategy utilizing PbS colloidal quantum dots(CQDs)and Au nanospheres(AuNSs).The PbS CQDs/AuNSs/glucose oxidase(GOx)mixture could be stably immobilized on the carbon electrode surface via the onestep dip-coating method.The electrochemical biosensor employing PbS CQDs/AuNSs/GOx-modified electrode integrates the functions of specific molecule recognition,signal transduction as well as signal amplification.The sensor is capable of transducing the glucose enzyme-catalyzed reaction into significant current signals,exhibiting a good linear response in the glucose concentration range of 0.1μM-10 mM with the limit of detection being 1.432 nM.

Stable PbS colloidal quantum dot inks enable blade‑coating infrared solar cells

Infrared solar cells are more efective than normal bandgap solar cells at reducing the spectral loss in the near-infrared region,thus also at broadening the absorption spectra and improving power conversion efciency.PbS colloidal quantum dots(QDs)with tunable bandgap are ideal infrared photovoltaic materials.However,QD solar cell production sufers from small-areabased spin-coating fabrication methods and unstable QD ink.Herein,the QD ink stability mechanism was fully investigated according to Lewis acid–base theory and colloid stability theory.We further studied a mixed solvent system using dimethylformamide and butylamine,compatible with the scalable manufacture of method-blade coating.Based on the ink system,100 cm2 of uniform and dense near-infrared PbS QDs(~0.96 eV)flm was successfully prepared by blade coating.The average efciencies of above absorber-based devices reached 11.14%under AM1.5G illumination,and the 800 nm-fltered efciency achieved 4.28%.Both were the top values among blade coating method based devices.The newly developed ink showed excellent stability,and the device performance based on the ink stored for 7 h was similar to that of fresh ink.The matched solvent system for stable PbS QD ink represents a crucial step toward large area blade coating photoelectric devices.

Tuning energy transfer efficiency in quantum dots mixture by controling donor/acceptor ratio

Improving the emission performance of colloidal quantum dots(QDs)is of paramount importance for their applications on light-emitting diodes(LEDs),displays and lasers.A highly promising approach is to tune the carrier recombination channels and lifetime by exploiting the energy transfer process.However,to achieve this precise emission optimization,quantitative modulation on energy transfer efficiency is highly desirable but still challenging.Here,we demonstrate a convenient approach to realize tunable energy transfer efficiency by forming QDs mixture with controllable donor/acceptor(D/A)ratio.With the mixing ratio ranging from 16/1 to 1/16,the energy transfer efficiency could be effectively tuned from near zero to~70%.For the high mixing ratio of 16/1,acceptors obtain adequate energy supplied by closely surrounding donors,leading to~2.4-fold PL enhancement.While for the low mixing ratio,the ultrafast and efficient energy extraction process directly suppresses the multi-exciton and Auger recombination in the donor,bringing about a higher threshold.The facile modulation of emission performance by controllably designed mixing ratio and quantitatively tunable energy transfer efficiency will facilitate QD-based optoelectronic and photovoltaic applications.