Ultrasensitive PbS‐Quantum‐Dot Photodetectors for Visible–Near‐Infrared Light Through Surface Atomic‐Ligand Exchange

A surface atomic‐ligand exchange method is applied the first time in the construction of photodetectors (PDs) based on PbS quantum dots (QDs) for ultrasensitivity. The device thus produces a high photosensitivity to visible and near‐infrared light with a photoresponsivity up to 7.5 × 10³ A W^?1 and a high stability in air. In particular, these PbS‐QD‐based PDs show the capability of following a pulse light with a frequency up to 100 kHz well at a relatively fast response time/recovery time of ≈4/40 μs, much faster than most previous QD‐based PDs. The short response time is attributed to modification for the surface of the PbS‐QDs by cetyltrimethylammonium bromide treatment, which effectively improves the contact between the QDs and the Au electrodes, leading to extracting a high carrier mobility (≈0.142 cm² V^?1 s^?1). These findings show the great potential of PbS‐QDs as high‐speed nano‐photodetectors, and, more importantly, demonstrate the importance of the surface atomic‐ligand exchange method in the construction of QD‐based devices.     

Investigation of Interfacial Charge Separation at PbS QDs/(001) TiO2 Nanosheets Heterojunction Solar Cell

In the recent years, the heterojunction solar cells based on quantum dots (QDs) have attracted attention due to strong light absorbing characteristics and the size effect on the bandgap tuning. This paper reports on the kinetics of interfacial charge separation of PbS QDs/(001) TiO₂ nanosheets heterojunction solar cells. PbS QDs are deposited using a bifunctional linker molecule on two different TiO₂ films, i.e., TiO₂ nanosheets (with 001 dominant exposed facet) and TiO₂ nanoparticles (with 101 dominant exposed facet). Upon bandgap excitation, electrons are transferred from the PbS QDs conduction band to the lower lying conduction band of TiO₂. Based on the ultrafast pump‐probe laser spectroscopy technique, the kinetics of charge separation is scrutinized at the PbS/TiO₂ interface. The interfacial charge separation at PbS/TiO₂ nanosheets films made of (001) dominant exposed facets is five times faster than that on (101) dominant exposed facets TiO₂ nanoparticles. The quantum yields for charge injection are higher for the (001) TiO₂ nanosheets than the (101) TiO₂ nanoparticles due to enhanced interfacial interaction with (001) surface compared to the (101) nanoparticles. The superior interfacial charge separation at PbS/(001) nanosheets respect to PbS/(101) nanoparticles is consistent with the higher photocurrent and enhanced power conversion efficiency in the PbS QDs/(001) TiO₂ heterojunction solar cell. The use of (001) TiO₂ nanosheets can be a better alternative to conventional mesoporous TiO₂ films in QD heterojunction solar cells and perovskites‐based heterojunction solar cells.     

Increased open‐circuit voltage of ZnO nanowire/PbS quantum dot bulk heterojunction solar cells with solution‐deposited Mg(OH)2 interlayer

An ultrathin Mg(OH)₂ layer was solution‐deposited onto the ZnO nanowires to solve the problem of interfacial charge recombination, caused by the increase of interfacial area in bulk heterojunction (BHJ) PbS colloidal quantum dot solar cells (CQDSCs). This Mg(OH)₂ interlayer efficiently passivated the surface defects of ZnO nanowires and provided tunnel barrier at ZnO/PbS interface. As a result, the charge recombination at ZnO/PbS interface was largely suppressed, proved by the significantly elongated electron lifetime and the increased open‐circuit voltage of the Mg(OH)₂‐involved BHJ CQDSCs. Careful thickness optimization of Mg(OH)₂ interlayer finally brought a ～33% increase in V_oc and ～25% improvement in power conversion efficiency.     

Light Trapping and Down‐Shifting Effect of Periodically Nanopatterned Si‐Quantum‐Dot‐Based Structures for Enhanced Photovoltaic Properties

Periodically nanopatterned Si structures have been prepared by using a nanosphere lithography technique. The formed nanopatterned structures exhibit good anti‐reflection and enhanced optical absorption characteristics. The mean surface reflectance weighted by AM1.5 solar spectrum (300–1200 nm) is as low as 5%. By depositing Si quantum dot/SiO₂ multilayers (MLs) on the nanopatterned Si substrate, the optical absorption is higher than 90%, which is significantly improved compared with the same multilayers deposited on flat Si substrate. Furthermore, the prototype n‐Si/Si quantum dot/SiO₂ MLs/p‐Si heterojunction solar cells has been fabricated, and it is found that the external quantum efficiency is obviously enhanced for nanopatterned cell in a wide spectral range compared with the flat cell. The corresponding short‐circuit current density is increased from 25.5 mA cm^?2 for flat cell to 29.0 mA cm^?2 for nano‐patterned one. The improvement of cell performance can be attributed both to the reduced light loss and the down‐shifting effect of Si quantum dots/SiO₂ MLs by forming periodically nanopatterned structures.     

Hybrid polymer/inorganic nanoparticle blended ternary solar cells

Hybrid polymer/inorganic nanoparticle blended ternary solar cells are reported. These solar cells have an active layer consisting of PbS colloidal quantum dots (CQDs), poly (3‐hexylthiophene) (P3HT), and [6,6]‐phenyl‐C61‐butyric acid methyl ester (PCBM). Power conversion efficiency (PCE) was improved by incorporating PbS CQDs in the active layer of P3HT:PCBM‐based organic solar cells. As the concentration of PbS CQDs in the hybrid solar cells was increased, PCE was also increased. This improvement resulted from improved charge transfer and also extended light absorption into the near‐infrared. The PCE of the hybrid solar cells was 47% higher than that for reference organic solar cells on average under air mass 1.5 global illumination. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

The synthesis of MDMO-PPV capped PbS nanorods and their application in solar cells

Poly[2-methoxy-5-(3′,7′-dimethyloctyloxy)-1,4-phenylenevinylene] (MDMO-PPV) capped PbS nanorods about 100 nm in diameter and 400 nm in length were synthesized via a hydrothermal route in toluene and dimethylsulfoxide solution. By blending the PbS nanorods with the MDMO-PPV as the active layer, bulk heterojunction solar cells with an indium tin oxide (ITO)/polyethylenedioxythiophene/polystyrenesulphonate (PEDOT: PSS)/MDMO-PPV: PbS nanorods/Al structure were fabricated in a N₂ filled glove box. Current density–voltage characterization of the devices showed that the solar cells with PbS nanorods hybrid with MDMO-PPV as active layer were better in performance than the devices with the polymer only.     

Near‐field optical enhancement by lead‐sulfide quantum dots and metallic nanoparticles for SERS

There is a growing interest in using quantum dots (QDs) and metallic nanoparticles (NPs), both for luminescence enhancement and surface‐enhanced Raman scattering (SERS). Here, we study the electromagnetic‐field enhancement that can be generated by lead‐sulfide (PbS) QDs using three‐dimensional finite‐element simulations. We investigate the field enhancement associated with combinations of PbS QDs with metallic NPs and substrates. The results show that high field enhancement can be achieved by combining PbS QDs with metallic NPs of larger sizes. The ideal size for Ag NPs is 25 nm, providing a SERS enhancement factor of ~5*10⁸ for light polarization parallel to the NP dimer axis and a gap of 0.6 nm. For Au NPs, the bigger the size, the higher is the field for the studied diameters, up to 50 nm. The near‐field values for PbS QDs above metallic substrates were found to be lower compared to the case of PbS QD‐metal NP dimers. This study provides the understanding for the design and application of QDs for the enhancement of near‐field phenomena. Copyright © 2013 John Wiley & Sons, Ltd.     

Effectiveness of full spectrum light soaking on solar cell degradation analysis

This study examined the effect of UV-spectrum light soaking on solar cell degradation tests. An indoor light soaking test was evaluated over three different spectral ranges: “UV only”, “UV blocked” and “Full spectrum”. a-Si:H and poly-crystalline silicon solar cell technologies were studied by light soaking tests with the same optical filter configurations.The I–V measurement results demonstrated that “UV only” irradiated solar cells exhibited the smallest output power degradation, which was only half of a percent variation compared with the full spectrum light soaking case. Using a filter that excluded the effect of the UV spectral range on light soaking, the “UV blocked” case also exhibited a significant output power degradation of the solar cells. A comparative analysis of the solar cell response, based on the I–V characteristics and the diode ideality factor under these different light soaking spectra, demonstrated the importance of the full spectrum light soaking test in the evaluation of the long-term performance of solar cells.     

表面配体和器件结构对PbS胶体量子点电池性能的影响

利用吸收光谱、傅里叶变换红外光谱和循环伏安等表征技术,分析了利用四丁基碘化铵(TBAI)和1,2-乙二硫醇(EDT)配体钝化处理的PbS胶体量子点的光学性质、表面化学及其能级结构,并在此基础上分别以PbS-TBAI薄膜、PbS-EDT薄膜和PbS-TBAI/PbS-EDT薄膜作为有源层制备了PbS胶体量子点/Zn O纳米粒子异质结太阳能电池,以比较研究表面配体和器件结构对器件光伏性能及其稳定性的影响。结果表明,TBAI和EDT均能与PbS胶体量子点表面原有的油酸配体实现良好置换,但是配体置换之后量子点表面均残留少量油酸分子; PbS-TBAI薄膜的导带底为-5.12 eV,价带顶为-3. 86 eV,而PbS-EDT薄膜的导带底为-4. 99 eV,价带顶为-3. 74 eV,后者相对前者出现了明显的能带上移; PbS-TBAI/PbS-EDT双配体器件的光伏性能最优,能量转化效率达到4. 43%;随着空气暴露时间的增加,PbS-TBAI/PbS-EDT双配体器件和PbS-TBAI单配体器件表现出相似的性能变化趋势,于3 d后达到最优光伏性能,而PbS-EDT单配体器件的空气稳定性差,3 d后的能量转换效率下降至初始效率的1/4。本工作的研究结果将不仅有助于加深对PbS胶体量子点电池性能变化规律的认识,而且有望促进该类电池制备技术的进一步优化。     

Role of a‐Si:H bulk in surface passivation of c‐Si wafers

The low thermal stability of hydrogenated amorphous silicon (a‐Si:H) thin films limits their widespread use for surface passivation of c‐Si wafers on the rear side of solar cells. We show that the thermal stability of a‐Si:H surface passivation is increased significantly by a hydrogen rich a‐Si:H bulk, which acts as a hydrogen reservoir for the a‐Si:H/c‐Si interface. Based on this mechanism, an excellent lifetime of 5.1 ms (at injection level of 10¹⁵ cm^–3) is achieved after annealing at 450 °C for 10 min. (© 2010 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

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 PbX(X = S, Se) based CQD solar cells have been achieved in recent years, and the power conversion efficiencies(PCEs) exceeding 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 QDSCs, 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.     

Fullerene solubility–current density relationship in polymer solar cells

During the last decade polymer solar cells have undergone a steady increase in overall device efficiency. To date, essential efficiency improvements of polymer–fullerene solar cells require the development of new materials. Whilst most research efforts aim at an improved or spectrally extended absorption of the donor polymer, not so much attention has been paid to the fullerene properties themselves. We have investigated a number of structurally related fullerenes, in order to study the relationship between chemical structure and resulting polymer–fullerene bulk heterojunction photovoltaic properties. Our study reveals a clear connection between the fullerene solubility as material property on one hand and the solar cells short circuit photocurrent on the other hand. The tendency of the less soluble fullerene derivates to aggregate was accounted for smaller current densities in the respective solar cells. Once a minimum solubility of approx. 25 mg/ml in chlorobenzene was overcome by the fullerene derivative, the short circuit current density reached a plateau, of about 8–10 mA/cm². Thus the solubility of the fullerene derivative directly influences the blend morphology and displays an important parameter for efficient polymer–fullerene bulk heterojunction solar cell operation. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

n‐type silicon solar cells with surface‐passivated screen‐printed aluminium‐alloyed rear emitter

Aluminium‐doped p‐type (Al‐p⁺) silicon emitters fabricated by means of a simple screen‐printing process are effectively passivated by plasma‐enhanced chemical‐vapour deposited amorphous silicon (a‐Si). We measure an emitter saturation current density of only 246 fA/cm², which is the lowest value achieved so far for a simple screen‐printed Al‐p⁺ emitter on silicon. In order to demonstrate the applicability of this easy‐to‐fabricate p⁺ emitter to high‐efficiency silicon solar cells, we implement our passivated p⁺ emitter into an n⁺np⁺ solar cell structure. An independently confirmed conversion efficiency of 19.7% is achieved using n‐type phosphorus‐doped Czochralski‐grown silicon as bulk material, clearly demonstrating the high‐efficiency potential of the newly developed a‐Si passivated Al‐p⁺ emitter. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Synthesis of the wheat-like CdSe/CdTe thin film heterojunction and their photovoltaic applications

We report on the fabrication of wheat-like CdSe/CdTe thin film heterojunction solar cells made using a simple electrochemical deposition method and close-spaced sublimation technology on indium tin oxide (ITO) substrates. Structural, optical, and electrical properties of the wheat-like CdSe/CdTe thin film junctions were characterized by X-ray diffraction (XRD), field emission scanning electron microscope (FESEM), energy dispersive spectrometry (EDS), ultraviolet–visible (UV–vis) absorption spectrum and Keithley 2400 analysis. A significant red-shift of the absorption edge is observed in this heterojunction. The heterostructure is composed of the wheat-like CdSe array and CdTe thin film, showing optical properties typical of type II heterostructures that are suited for photovoltaic applications. A photocurrent density of 8.34 mA/cm² has been obtained under visible light illumination of 100 mW/cm². This study demonstrates that the electrochemical deposition and the close-spaced sublimation technology, which are easily adapted to other chemical systems, are promising techniques for large-scale fabrication of low-cost heterojunction solar cells.     

Nanoimprint texturing of transparent flexible substrates for improved light management in thin‐film solar cells

We present a nanoimprint based approach to achieve efficient light management for solar cells on low temperature transparent polymer films. These films are particularly low‐priced, though sensitive to temperature, and therefore limiting the range of deposition temperatures of subsequent solar cell layers. By using nanoimprint technology, we successfully replicated optimized light trapping textures of etched high temperature ZnO:Al on a low temperature PET film without deterioration of optical properties of the substrate. The imprint‐textured PET substrates show excellent light scattering properties and lead to significantly improved incoupling and trapping of light in the solar cell, resulting in a current density of 12.9 mA/cm², similar to that on a glass substrate. An overall efficiency of 6.9% was achieved for a flexible thin‐film silicon solar cell on low cost PET substrate. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Optical management in high‐efficiency thin‐film silicon micromorph solar cells with a silicon oxide based intermediate reflector

In the effort to increase the stable efficiency of thin film silicon micromorph solar cells, a silicon oxide based intermediate reflector (SOIR) layer is deposited in situ between the component cells of the tandem device. The effectiveness of the SOIR layer in increasing the photo‐carrier generation in the a‐Si:H top absorber is compared for p–i–n devices deposited on different rough, highly transparent, front ZnO layers. High haze and low doping level for the front ZnO strongly enhance the current density (J_sc) in the μc‐Si:H bottom cell whereas J_sc in the top cell is influenced by the angular distribution of the transmitted light and by the reflectivity of the SOIR related to different surface roughness. A total J_sc of 26.8 mA/cm² and an initial conversion efficiency of 12.6% are achieved for 1.2 cm² cells with top and bottom cell thicknesses of 300 nm and 3 μm, and without any anti‐reflective coating on the glass. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Efficient interdigitated back‐contacted silicon heterojunction solar cells

We present back‐contacted amorphous/crystalline silicon heterojunction solar cells (IBC‐SHJ) on n‐type substrates with fill factors exceeding 78% and high current densities, the latter enabled by a SiN_x /SiO₂ passivated phosphorus‐diffused front surface field. V_oc calculations based on carrier lifetime data of reference samples indicate that for the IBC architecture and the given amorphous silicon layer qualities an emitter buffer layer is crucial to reach a high V_oc, as known for both‐side contacted silicon heterojunction solar cells. A back surface field buffer layer has a minor influence. We observe a boost in solar cell V_oc of 40 mV and a simultaneous fill factor reduction introducing the buffer layer. The aperture‐area efficiency increases from 19.8 ± 0.4% to 20.2 ± 0.4%. Both, efficiencies and fill factors constitute a significant improvement over previously reported values. (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Microwave‐Assisted Synthesis of Biocompatible Silk Fibroin‐Based Carbon Quantum Dots

A biocompatible silk fibroin‐based carbon quantum dot (SF‐CQD) is first synthesized under microwave irradiation for a short time. This fast and environmentally safe technique produce well‐defined nanosized SF‐CQDs. The SF‐CQDs have good crystallinity, a strong emission peak in the blue‐color region, high quantum yield, and the potential for modification with various functional groups on the surface. These SF‐CQDs demonstrate stable emission, good water dispersity, low toxicity, and good biocompatibility. These properties show the great potential of these SF‐CQDs for use in biomedical applications including bioimaging, biosensing, and drug delivery systems.     

A flexible blue light sensitive organic photodiode with high properties for the applications in low‐voltage‐control circuit and flexion sensors

Low‐voltage‐control circuit is one of the most important parts of the modern electrical control system due to the avoidance of operation risk and easy automation. Here, based on a C₆₀: m‐MTDATA bulk heterojunction, a blue‐light‐sensitive organic photodiode (OPD) is explored for the development of flexible low‐voltage‐control circuit. The control of circuit under 2000 V high voltage is achieved. The influences of the organic‐layer thickness, the donor/acceptor volume ratio and the matching of energy levels on the photocurrent are investigated. The maximum light/dark current ratio and current transfer ratio of 1.3 × 10⁴ and 1.3% are achieved, respectively. The highest photoresponse is up to 130 mA/W, markedly higher than some commercial inorganic photodiodes. This device could also be used as flexion and mechanical force sensors with the current density changing under different bending conditions. Therefore, this sort of OPD has a promising application in low‐voltage‐controlled, high‐voltage‐endurable hands for intelligent robots.     

Properties of nitride‐based photovoltaic cells under concentrated light illumination

We investigated the properties of nitride‐based solar cells under concentrated light illumination from 1 to 200 suns. The conversion efficiency of our solar cells increased with increasing concentration up to 200 suns. The short‐circuit cur‐ rent density, open‐circuit voltage, fill factor, and conversion efficiency were 510 mA/cm², 1.9 V, 70%, and 3.4%, respectively, under an air mass filter of 1.5G at 200 suns and room temperature. (© 2012 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)