Synchronously Polishing the Lead-Rich Surface and Passivating Surface Defects of CsPb(Br/I)3 Quantum Dots for High-Performance Pure-Red PeLEDs.

Mixed-halide CsPb(Br/I)3 perovskite quantum dots (QDs) are regarded as one of the most promising candidates for pure-red perovskite light-emitting diodes (PeLEDs) due to their precise spectral tuning property. However, the lead-rich surface of these QDs usually results in halide ion migration and nonradiative recombination loss, which remains a great challenge for high-performance PeLEDs. To solve the above issues, we employ a chelating agent of 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid hydrate (DOTA) to polish the lead-rich surface of the QDs and meanwhile introduce a new ligand of 2,3-dimercaptosuccinic acid (DMSA) to passivate surface defects of the QDs. This synchronous post-treatment strategy results in high-quality CsPb(Br/I)3 QDs with suppressed halide ion migration and an improved photoluminescence quantum yield, which enables us to fabricate spectrally stable pure-red PeLEDs with a peak external quantum efficiency of 23.2%, representing one of the best performance pure-red PeLEDs based on mixed-halide CsPb(Br/I)3 QDs reported to date.

Ligand-Induced Cation-π Interactions Enable High-Efficiency, Bright, and Spectrally Stable Rec. 2020 Pure-Red Perovskite Light-Emitting Diodes.

Achieving high-performance perovskite light-emitting diodes (PeLEDs) with pure-red electroluminescence for practical applications remains a critical challenge because of the problematic luminescence property and spectral instability of existing emitters. Herein, high-efficiency Rec. 2020 pure-red PeLEDs, simultaneously exhibiting exceptional brightness and spectral stability, based on CsPb(Br/I)3 perovskite nanocrystals (NCs) capping with aromatic amino acid ligands featuring cation-π interactions, are reported. It is proven that strong cation-π interactions between the PbI6 -octahedra of perovskite units and the electron-rich indole ring of tryptophan (TRP) molecules not only chemically polish the imperfect surface sites, but also markedly increase the binding affinity of the ligand molecules, leading to high photoluminescence quantum yields and greatly enhanced spectral stability of the CsPb(Br/I)3 NCs. Moreover, the incorporation of small-size aromatic TRP ligands ensures superior charge-transport properties of the assembled emissive layers. The resultant devices emitting at around 635 nm demonstrate a champion external quantum efficiency of 22.8%, a max luminance of 12 910 cd m-2 , and outstanding spectral stability, representing one of the best-performing Rec. 2020 pure-red PeLEDs achieved so far.

A Simple and Effective Phosphine-Doping Technique for Solution-Processed Nanocrystal Solar Cells.

Solution-processed cadmium telluride (CdTe) nanocrystal (NC) solar cells offer the advantages of low cost, low consumption of materials and large-scale production via a roll-to-roll manufacture process. Undecorated CdTe NC solar cells, however, tend to show inferior performance due to the abundant crystal boundaries within the active CdTe NC layer. The introduction of hole transport layer (HTL) is effective for promoting the performance of CdTe NC solar cells. Although high-performance CdTe NC solar cells have been realized by adopting organic HTLs, the contact resistance between active layer and the electrode is still a large problem due to the parasitic resistance of HTLs. Here, we developed a simple phosphine-doping technique via a solution process under ambient conditions using triphenylphosphine (TPP) as a phosphine source. This doping technique effectively promoted the power conversion efficiency (PCE) of devices to 5.41% and enabled the device to have extraordinary stability, showing a superior performance compared with the control device. Characterizations suggested that the introduction of the phosphine dopant led to higher carrier concentration, hole mobility and a longer lifetime of the carriers. Our work presents a new and simple phosphine-doping strategy for further improving the performance of CdTe NC solar cells.

A Multifunctional "Halide-Equivalent" Anion Enabling Efficient CsPb(Br/I)3 Nanocrystals Pure-Red Light-Emitting Diodes with External Quantum Efficiency Exceeding 23.

Pure-red perovskite LEDs (PeLEDs) based on CsPb(Br/I)3 nanocrystals (NCs) usually suffer from a compromise in emission efficiency and spectral stability on account of the surface halide vacancies-induced nonradiative recombination loss, halide phase segregation, and self-doping effect. Herein, a "halide-equivalent" anion of benzenesulfonate (BS- ) is introduced into CsPb(Br/I)3 NCs as multifunctional additive to simultaneously address the above challenging issues. Joint experiment-theory characterizations reveal that the BS- can not only passivate the uncoordinated Pb2+ -related defects at the surface of NCs, but also increase the formation energy of halide vacancies. Moreover, because of the strong electron-withdrawing property of sulfonate group, electrons are expected to transfer from the CsPb(Br/I)3 NC to BS- for reducing the self-doping effect and altering the n-type behavior of CsPb(Br/I)3 NCs to near ambipolarity. Eventually, synergistic boost in device performance is achieved for pure-red PeLEDs with CIE coordinates of (0.70, 0.30) and a champion external quantum efficiency of 23.5%, which is one of the best value among the ever-reported red PeLEDs approaching to the Rec. 2020 red primary color. Moreover, the BS- -modified PeLED exhibits negligible wavelength shift under different operating voltages. This strategy paves an efficient way for improving the efficiency and stability of pure-red PeLEDs.

A Demulsification-Crystallization Model for High-Quality Perovskite Nanocrystals.

A room-temperature technique with all-nonpolar-solvent, which circumvents the sensitivity of ionic perovskite to polar solvent, has become attractive for the synthesis of metal halide perovskite nanocrystals (PNCs). However, the lack of understanding of the inner mechanism, especially for the state of the precursor and the crystallization process of the PNCs, hinders further development of this technique. Here, through systematic study of the Pb precursor and in situ characterization of the PNCs, it is revealed that the reverse micelle nature of the Pb precursor exactly creates a novel demulsification-crystallization (D-C) model, namely, a two-stage nucleation is divided by a demulsification process for the PNCs. On this basis, a top efficiency for green light-emitting diodes based on PNCs is obtained with a maximum external quantum efficiency of 22.5% through tailoring the D-C model using a multiple-acid-anion synergistic assisted strategy to obtain high-quality PNCs. Beyond the high efficiency, the work paves the way for diverse ideas in PNC synthesis.

Complete Solution-Processed Semitransparent and Flexible Organic Solar Cells: A Success of Polyimide/Ag-Nanowires- and PH1000-Based Electrodes with Plasmonic Enhanced Light Absorption.

Organic solar cells (OSCs) have been widely studied due to the advantages of easy fabrication, low cost, light weight, good flexibility and sufficient transparency. In this work, flexible and semitransparent OSCs were successfully fabricated with the adoption of both polyimide/silver nanowires (PI/AgNW) and a conducting polymer PEDOT:PSS named PH1000 as the transparent conductive electrodes (TCEs). It is demonstrated that PI/AgNW is more suitable as a cathode rather than an anode in the viewpoint of its work function, photovoltaic performance, and simulations of optical properties. It is also found that the light incidence from PH1000 TCE can produce more plasmonic-enhanced photon absorption than the PI/AgNW electrode does, resulting in more high power conversion efficiency. Moreover, a high light transmittance of 33.8% and a decent efficiency of 3.88% are achieved for the whole all-flexible semitransparent device with only 9% decrease of resistance in PI/AgNW after 3000 bending cycles. This work illustrates that PI/AgNW has great potential and bright prospect in large-area OSC applications in the future.

Promoting Energy Transfer Between Quasi-2D Perovskite Layers Toward Highly Efficient Red Light-Emitting Diodes.

Although tremendous progress has recently been made in quasi-2D perovskite light-emitting diodes (PeLEDs), the performance of red PeLEDs emitting at ≈650-660 nm, which have wide prospects for application in photodynamic therapy, is still limited by an inefficient energy transfer process between the quasi-2D perovskite layers. Herein, a symmetric molecule of 3,3'-(9H-fluorene-9,9-diyl)dipropanamide (FDPA) is designed and developed with two functional acylamino groups and incorporated into the quasi-2D perovskites as the additive for achieving high-performance red PeLEDs. It is demonstrated that the agent can simultaneously diminish the van der Waals gaps between individual perovskite layers and passivate uncoordinated Pb2+ related defects at the surface and grain boundaries of the quasi-2D perovskites, which truly results in an efficient energy transfer in the quasi-2D perovskite films. Consequently, the red PeLEDs emitting at 653 nm with a peak external quantum efficiency of 18.5% and a maximum luminance of 2545 cd m-2 are achieved, which is among the best performing red quasi-2D PeLEDs emitting at ≈650-660 nm. This work opens a way to further improve the electroluminescence performance of red PeLEDs.

Efficient Nanocrystal Photovoltaics with PTAA as Hole Transport Layer.

The power conversion efficiency (PCE) of solution-processed CdTe nanocrystals (NCs) solar cells has been significantly promoted in recent years due to the optimization of device design by advanced interface engineering techniques. However, further development of CdTe NC solar cells is still limited by the low open-circuit voltage (Voc) (mostly in range of 0.5-0.7 V), which is mainly attributed to the charge recombination at the CdTe/electrode interface. Herein, we demonstrate a high-efficiency CdTe NCs solar cell by using organic polymer poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) as the hole transport layer (HTL) to decrease the interface recombination and enhance the Voc. The solar cell with the architecture of ITO/ZnO/CdS/CdSe/CdTe/PTAA/Au was fabricated via a layer-by-layer solution process. Experimental results show that PTAA offers better back contact for reducing interface resistance than the device without HTL. It is found that a dipole layer is produced between the CdTe NC thin film and the back contact electrode; thus the built-in electric field (Vbi) is reinforced, allowing more efficient carrier separation. By introducing the PTAA HTL in the device, the open-circuit voltage, short-circuit current density and the fill factor are simultaneously improved, leading to a high PCE of 6.95%, which is increased by 30% compared to that of the control device without HTL (5.3%). This work suggests that the widely used PTAA is preferred as the excellent HTL for achieving highly efficient CdTe NC solar cells.

Spacer Cation Alloying in Ruddlesden-Popper Perovskites for Efficient Red Light-Emitting Diodes with Precisely Tunable Wavelengths.

Perovskite light-emitting diodes (PeLEDs) have recently shown significant progress with external quantum efficiencies (EQEs) exceeding 20%. However, PeLEDs with pure-red (620-660 nm) light emission, an essential part for full-color displays, remain a great challenge. Herein, a general approach of spacer cation alloying is employed in Ruddlesden-Popper perovskites (RPPs) for efficient red PeLEDs with precisely tunable wavelengths. By simply tuning the alloying ratio of dual spacer cations, the thickness distribution of quantum wells in the RPP films can be precisely modulated without deteriorating their charge-transport ability and energy funneling processes. Consequently, efficient PeLEDs with tunable emissions between pure red (626 nm) and deep red (671 nm) are achieved with peak EQEs up to 11.5%, representing the highest values among RPP-based pure-red PeLEDs. This work opens a new route for color tuning, which will spur future developments of pure-red or even pure-blue PeLEDs with high performance.

Perovskite Light-Emitting Diodes with EQE Exceeding 28% through a Synergetic Dual-Additive Strategy for Defect Passivation and Nanostructure Regulation.

Quasi-2D perovskites have long been considered to have favorable "energy funnel/cascade" structures and excellent optical properties compared with their 3D counterparts. However, most quasi-2D perovskite light-emitting diodes (PeLEDs) exhibit high external quantum efficiency (EQE) but unsatisfactory operating stability due to Auger recombination induced by high current density. Herein, a synergetic dual-additive strategy is adopted to prepare perovskite films with low defect density and high environmental stability by using 18-crown-6 and poly(ethylene glycol) methyl ether acrylate (MPEG-MAA) as the additives. The dual additives containing COC bonds can not only effectively reduce the perovskite defects but also destroy the self-aggregation of organic ligands, inducing the formation of perovskite nanocrystals with quasi-core/shell structure. After thermal annealing, the MPEG-MAA with its CC bond can be polymerized to obtain a comb-like polymer, further protecting the passivated perovskite nanocrystals against water and oxygen. Finally, state-of-the-art green PeLEDs with a normal EQE of 25.2% and a maximum EQE of 28.1% are achieved, and the operating lifetime (T50 ) of the device in air environment is over ten times increased, providing a novel and effective strategy to make high efficiency and long operating lifetime PeLEDs.

Synthesis of Group II-VI Semiconductor Nanocrystals via Phosphine Free Method and Their Application in Solution Processed Photovoltaic Devices.

Solution-processed CdTe semiconductor nanocrystals (NCs) have exhibited astonishing potential in fabricating low-cost, low materials consumption and highly efficient photovoltaic devices. However, most of the conventional CdTe NCs reported are synthesized through high temperature microemulsion method with high toxic trioctylphosphine tellurite (TOP-Te) or tributylphosphine tellurite (TBP-Te) as tellurium precursor. These hazardous substances used in the fabrication process of CdTe NCs are drawing them back from further application. Herein, we report a phosphine-free method for synthesizing group II-VI semiconductor NCs with alkyl amine and alkyl acid as ligands. Based on various characterizations like UV-vis absorption (UV), transmission electron microscope (TEM), and X-ray diffraction (XRD), among others, the properties of the as-synthesized CdS, CdSe, and CdTe NCs are determined. High-quality semiconductor NCs with easily controlled size and morphology could be fabricated through this phosphine-free method. To further investigate its potential to industrial application, NCs solar cells with device configuration of ITO/ZnO/CdSe/CdTe/Au and ITO/ZnO/CdS/CdTe/Au are fabricated based on NCs synthesized by this method. By optimizing the device fabrication conditions, the champion device exhibited power conversion efficiency (PCE) of 2.28%. This research paves the way for industrial production of low-cost and environmentally friendly NCs photovoltaic devices.

13.4 % Efficiency from All-Small-Molecule Organic Solar Cells Based on a Crystalline Donor with Chlorine and Trialkylsilyl Substitutions.

How to simultaneously achieve both high open-circuit voltage (Voc ) and high short-circuit current density (Jsc ) is a big challenge for realising high power conversion efficiency (PCE) in all-small-molecule organic solar cells (all-SM OSCs). Herein, a novel small molecule (SM)-donor, namely FYSM-SiCl, with trialkylsilyl and chlorine substitutions was designed and synthesized. Compared to the original SM-donor FYSM-H, FYSM-Si with trialkylsilyl substitution showed a decreased crystallinity and lower highest occupied molecular orbital (HOMO) level, while FYSM-SiCl had an improved crystallinity, more ordered packing arrangement, significantly lower HOMO level, and predominant "face-on" orientation. Matched with a SM-acceptor Y6, the FYSM-SiCl-based all-SM OSCs exhibited both high Voc of 0.85 V and high Jsc of 23.7 mA cm-2 , which is rare for all-SM OSCs and could be attributed to the low HOMO level of FYSM-SiCl donor and the delicate balance between high crystallinity and suitable blend morphology. As a result, FYSM-SiCl achieved a high PCE of 13.4 % in all-SM OSCs, which was much higher than those of the FYSM-H- (10.9 %) and FYSM-Si-based devices (12.2 %). This work demonstrated a promising method for the design of efficient SM-donors by a side-chain engineering strategy via the introduction of trialkylsilyl and chlorine substitutions.

Highly Luminescent and Stable CsPbI3 Perovskite Nanocrystals with Sodium Dodecyl Sulfate Ligand Passivation for Red-Light-Emitting Diodes.

CsPbI3 perovskite nanocrystals (NCs) have recently emerged as promising materials for optoelectronic devices because of their superior properties. However, the poor stability of the CsPbI3 NCs induced by easy ligand desorption represents a key issue limiting their practical applications. Herein, we report stable and highly luminescent black-phase CsPbI3 NCs passivated by novel ligands of sodium dodecyl sulfate (SDS). Theoretical calculation results reveal a stronger adsorption energy of SDS molecules at the CsPbI3 surface than that of commonly used oleic acid. As a result, the defect formation caused by the ligand loss during the purification process is greatly suppressed. The optimized SDS-CsPbI3 NCs exhibit significantly reduced surface defects, much enhanced stability, and superior photoluminescence efficiency. The red perovskite light-emitting diodes based on the SDS-CsPbI3 NCs demonstrate an external quantum efficiency of 8.4%, which shows a 4-fold improvement compared to the devices based on the oleic acid-modified CsPbI3 NCs.

Efficient PbS Quantum Dot Solar Cells with Both Mg-Doped ZnO Window Layer and ZnO Nanocrystal Interface Passivation Layer.

In this paper, a Mg-doped ZnO (MZO) thin film is prepared by a simple solution process under ambient conditions and is used as the window layer for PbS solar cells due to a wide n-type bandgap. Moreover, a thin layer of ZnO nanocrystals (NCs) was deposited on the MZO to reduce carrier recombination at the interface for inverted PbS quantum dot solar cells with the configuration Indium Tin Oxides (ITO)/MZO/ZnO NC (w/o)/PbS/Au. The effect of film thickness and annealing temperature of MZO and ZnO NC on the performance of PbS quantum dot solar cells was investigated in detail. It was found that without the ZnO NC thin layer, the highest power conversion efficiency(PCE) of 5.52% was obtained in the case of a device with an MZO thickness of 50 nm. When a thin layer of ZnO NC was introduced between MZO and PbS quantum dot film, the PCE of the champion device was greatly improved to 7.06% due to the decreased interface recombination. The usage of the MZO buffer layer along with the ZnO NC interface passivation technique is expected to further improve the performance of quantum dot solar cells.

Nonconjugated Terpolymer Acceptors with Two Different Fused-Ring Electron-Deficient Building Blocks for Efficient All-Polymer Solar Cells.

The ternary polymerization strategy of incorporating different donor and acceptor units forming terpolymers as photovoltaic materials has been proven advantageous in improving power conversion efficiencies (PCEs) of polymer solar cells (PSCs). Herein, a series of low band gap nonconjugated terpolymer acceptors based on two different fused-ring electron-deficient building blocks (IDIC16 and ITIC) with adjustable photoelectric properties were developed. As the third component, ITIC building blocks with a larger π-conjugation structure, shorter solubilizing side chains, and red-shifted absorption spectrum were incorporated into an IDIC16-based nonconjugated copolymer acceptor PF1-TS4, which built up the terpolymers with two conjugated building blocks linked by flexible thioalkyl chain-thiophene segments. With the increasing ITIC content, terpolymers show gradually broadened absorption spectra and slightly down-shifted lowest unoccupied molecular orbital levels. The active layer based on terpolymer PF1-TS4-60 with a 60% ITIC unit presents more balanced hole and electron mobilities, higher photoluminescence quenching efficiency, and improved morphology compared to those based on PF1-TS4. In all-polymer solar cells (all-PSCs), PF1-TS4-60, matched with a wide band gap polymer donor PM6, achieved a similar open-circuit voltage (Voc) of 0.99 V, a dramatically increased short-circuit current density (Jsc) of 15.30 mA cm-2, and fill factor (FF) of 61.4% compared to PF1-TS4 (Voc = 0.99 V, Jsc = 11.21 mA cm-2, and FF = 55.6%). As a result, the PF1-TS4-60-based all-PSCs achieved a PCE of 9.31%, which is ∼50% higher than the PF1-TS4-based ones (6.17%). The results demonstrate a promising approach to develop high-performance nonconjugated terpolymer acceptors for efficient all-PSCs by means of ternary polymerization using two different A-D-A-structured fused-ring electron-deficient building blocks.

Optimized Active Layer Morphologies via Ternary Copolymerization of Polymer Donors for 17.6 % Efficiency Organic Solar Cells with Enhanced Fill Factor.

Regulating molecular structure to optimize the active layer morphology is of considerable significance for improving the power conversion efficiencies (PCEs) in organic solar cells (OSCs). Herein, we demonstrated a simple ternary copolymerization approach to develop a terpolymer donor PM6-Tz20 by incorporating the 5,5'-dithienyl-2,2'-bithiazole (DTBTz, 20 mol%) unit into the backbone of PM6 (PM6-Tz00). This method can effectively tailor the molecular orientation and aggregation of the polymer, and then optimize the active layer morphology and the corresponding physical processes of devices, ultimately boosting FF and then PCE. Hence, the PM6-Tz20: Y6-based OSCs achieved a PCE of up to 17.1% with a significantly enhanced FF of 0.77. Using Ag (220 nm) instead of Al (100 nm) as cathode, the champion PCE was further improved to 17.6%. This work provides a simple and effective molecular design strategy to optimize the active layer morphology of OSCs for improving photovoltaic performance.

Hole Transfer Layer Engineering for CdTe Nanocrystal Photovoltaics with Improved Efficiency.

Interface engineering has led to significant progress in solution-processed CdTe nanocrystal (NC) solar cells in recent years. High performance solar cells can be fabricated by introducing a hole transfer layer (HTL) between CdTe and a back contact electrode to reduce carrier recombination by forming interfacial dipole effect at the interface. Here, we report the usage of a commercial product 2,2',7,7'-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene (Spiro) as a hole transfer layer to facilitate the hole collecting for CdTe nanocrystal solar cells. It is found that heat treatment on the hole transfer layer has significant influence on the NC solar cells performance. The Jsc, Voc, and power conversion efficiency (PCE) of NC solar cells are simultaneously increased due to the decreased contact resistance and enhanced built-in electric field. We demonstrate solar cells that achieve a high PCE of 8.34% for solution-processed CdTe NC solar cells with an inverted structure by further optimizing the HTL annealing temperature, which is among the highest value in CdTe NC solar cells with the inverted structure.

A Non-Conjugated Polymer Acceptor for Efficient and Thermally Stable All-Polymer Solar Cells.

A non-conjugated polymer acceptor PF1-TS4 was firstly synthesized by embedding a thioalkyl segment in the mainchain, which shows excellent photophysical properties on par with a fully conjugated polymer, with a low optical band gap of 1.58 eV and a high absorption coefficient >105  cm-1 , a high LUMO level of -3.89 eV, and suitable crystallinity. Matched with the polymer donor PM6, the PF1-TS4-based all-PSC achieved a power conversion efficiency (PCE) of 8.63 %, which is ≈45 % higher than that of a device based on the small molecule acceptor counterpart IDIC16. Moreover, the PF1-TS4-based all-PSC has good thermal stability with ≈70 % of its initial PCE retained after being stored at 85 °C for 180 h, while the IDIC16-based device only retained ≈50 % of its initial PCE when stored at 85 °C for only 18 h. Our work provides a new strategy to develop efficient polymer acceptor materials by linkage of conjugated units with non-conjugated thioalkyl segments.

Efficient Low-Cost All-Flexible Microcavity Semitransparent Polymer Solar Cells Enabled by Polymer Flexible One-Dimensional Photonic Crystals.

High-efficiency low-cost all-flexible microcavity semitransparent polymer solar cells (STPSCs) are comparatively studied in both fullerene- and nonfullerene-based systems with the structure strategy, employing polymer flexible one-dimensional photonic crystals (F-1DPCs), as well as indium tin oxide-free UV/ozone plasma-treated polymer/ultrathin metal and PEDOT:PSS transparent electrodes. Based on the reasonable optimization of electrical and optical characteristics in the device, the maximum power conversion efficiency with the use of polymer F-1DPCs can be greatly improved by 24-27% compared to the respective control devices. The improvement in JSC is comprehensively discussed, which is mainly ascribed to the enhancement of effective photon absorption in the device. Although color tunability of fullerene and nonfullerene all-flexible STPSCs can be easily achieved with the use of different photonic band gaps of polymer F-1DPCs, the CIE coordinates of nonfullerene STPSCs differ a lot from the original light source compared to the fullerene ones because of a high absorption coefficient in a narrow wavelength region. This work presents an easy and effective microcavity device strategy incorporated with different elements and demonstrates a new sketch of structure-absorption-performance relationships for fullerene- versus nonfullerene-based all-flexible STPSCs, which is compatible with low-cost roll-to-roll manufacturing and surely has a diversity of potential applications to better meet specific needs.