ABSTRACT
Self-assembled monolayers (SAMs) as the hole-selective contact have achieved remarkable success in iodine-based perovskite solar cells (PSCs), while their impact on bromine-based PSCs is limited due to the poor perovskite crystallization behavior and mismatched energy level alignment. Here, a highly efficient SAM of (2-(3,6-diiodo-9H-carbazol-9-yl)ethyl)phosphonic acid (I-2PACz) is employed to address these challenges in FAPbBr3-based PSCs. The incorporation of I atoms into I-2PACz not only releases tensile stress within FAPbBr3 perovskite, promoting oriented crystallization and minimizing defects through halogen-halogen bond, but also optimizes the energy levels alignment at hole-selective interface for enhanced hole extraction. Ultimately, a power conversion efficiency (PCE) of 11.14% is achieved, which stands among the highest reported value for FAPbBr3 PSCs. Furthermore, the semitransparent devices/modules exhibit impressive PCEs of 8.19% and 6.23% with average visible transmittance of 41.98% and 38.99%. Remarkably, after operating at maximum power point for 1000 h, the encapsulated device maintains 93% of its initial PCE. These results demonstrate an effective strategy for achieving high-performance bromine-based PSCs toward further applications.
ABSTRACT
Mixed Br/Cl perovskite nanocrystals (PeNCs) exhibit bright pure-blue emission benefiting for fulfilling the Rec. 2100 standard. However, phase segregation remains a significant challenge that severely affects the stability and emission spectrum of perovskite light-emitting diodes (PeLEDs). Here, we demonstrate the optimization of the spacing between polydentate functional groups of polymer ligands to match the surface pattern of CsPbBr1.8Cl1.2 PeNCs, resulting in effective synergistic passivation effect and significant improvements in PeLED performances. The block and alternating copolymers with different inter-functional group spacing are facilely synthesized as ligands for PeNCs. Surprisingly, block copolymers with a higher functional group density do not match PeNCs, while alternating copolymers enable efficient PeNCs with the high photoluminescence intensity, low non-radiative recombination rate and high exciton binding energy. Density functional theory calculations clearly confirm the almost perfect match between alternating copolymers and PeNCs. Finally, pure-blue PeLEDs are achieved with the emission at 467â nm and Commission Internationale de l'Eclairage (CIE) coordinates of (0.131, 0.071), high external quantum efficiency (9.1 %) and record spectral and operational stabilities (~80â mins) in mixed-halide PeLEDs. Overall, this study contributes to designing the polymer ligands and promoting the development of high-performance and stable pure-color PeLEDs towards display applications.
ABSTRACT
Metal halide perovskite solar cells (PSCs) show significant advancements in power conversion efficiency (PCE). However, the open-circuit voltage (VOC) of PSCs is limited by interfacial factors such as defect-induced recombination, energy band mismatch, and non-intimate interface contact. Here, an exciplex interface is first developed based on the strategically designed and synthesized two spirobifluorene phosphonate molecules to mitigate VOC loss in PSCs. The exciplex interface constructed by the intimate contact between the multi-functional molecules and hole transport layer takes the roles to promote the hole extraction by donor-acceptor interaction, passivate coordination-unsaturated Pb2+ defects by equipped phosphonate groups, and optimize the energy level alignment. As a result, a record VOC of 1.26 V with a perovskite bandgap of 1.61 eV is achieved, representing over 95% of theoretical limit. This advancement leads to an increase in PCE from 21.29% to 24.12% and improved stability. The exciplex interface paves the way for addressing the long-standing challenge of VOC loss and promotes the wider application of PSCs.
ABSTRACT
Continuous-wave (CW) lasing in quasi-two-dimensional (2D) perovskite-based distributed feedback cavities has been achieved at room temperature; however, CW microcavity lasers comprising distributed Bragg reflectors (DBRs) have rarely been prepared using solution-processed quasi-2D perovskite films because the roughness of perovskite films significantly increases intersurface scattering loss in the microcavity. Herein, high-quality spin-coated quasi-2D perovskite gain films were prepared using an antisolvent to reduce roughness. The highly reflective top DBR mirrors were deposited via room-temperature e-beam evaporation to protect the perovskite gain layer. Lasing emission of the prepared quasi-2D perovskite microcavity lasers under CW optical pumping was clearly observed at room temperature, featuring a low threshold of â¼1.4 W cm-2 and beam divergence of â¼3.5°. It was concluded that these lasers originated from weakly coupled excitons. These results elucidate the importance of controlling the roughness of quasi-2D films to achieve CW lasing, thus facilitating the design of electrically pumped perovskite microcavity lasers.
ABSTRACT
The introduction of additives has become an important method for enhancing the device performance of quasi-two-dimensional perovskite light-emitting diodes. In this work, we systematically studied the electronic and spatial effects of molecular additives on defect passivation abilities using the methyl, hydrogen, and hydroxyl groups substituted three diphenyl phosphine oxygen additives. The electron-donating conjugation effect of the hydroxyl group on diphenylphosphinic acid (OH-DPPO) leads to a more electron-rich region in OH-DPPO, and the hydroxyl group has a moderate steric hindrance. All these factors endow it with best passivation ability than the other two additives. Furthermore, ion migration was suppressed due to hydrogen bonding between the hydroxyl group and Br. Ultimately, the OH-DPPO passivated devices achieved an external quantum efficiency of 22.44% and a 6-fold improvement in lifetime. These findings provide guidance for developing multifunctional additives in the field of perovskite optoelectronics.
ABSTRACT
Quasi-2D perovskites have demonstrated great application potential in light-emitting diodes (LEDs). Defect passivation with chemicals plays a critical role to achieve high efficiency. However, there are still challenges in comprehensively passivating the defects distributed at surface, bulk, and buried interface of quasi-2D perovskite emitting films, hindering the further improvement of device performance. Herein, 9,9-substituted fluorene derivatives with different terminal functional groups are developed tactfully to realize comprehensive passivation, which greatly contributes to reducing nonradiative recombination at surface, suppressing ion migration in bulk, and filling interfacial charge traps at buried interface, respectively. Eventually, quasi-2D perovskite LEDs have an increased external quantum efficiency from 18.2% to 23.2%, improved operation lifetime by more than six times and lower turn-on voltage simultaneously. Here the importance of comprehensive passivation is highlighted and guidelines for the design and application of passivators for perovskite optoelectronics are provided.
ABSTRACT
Emission thermal quenching is commonly observed in quasi-2D perovskite emitters, which causes the severe drop in luminescence efficiency for the quasi-2D perovskite light-emitting diodes (PeLEDs) during practical operations. However, this issue is often neglected and rarely studied, and the root cause of the thermal quenching has not been completely revealed now. Here, we develop a passivation strategy via the 2,7-dibromo-9,9-bis (3'-diethoxylphosphorylpropyl)-fluorene to investigate and suppress the thermal quenching. The agent can effectively passivate coordination-unsaturated Pb2+ defects of both surface and bulk of the film without affecting the perovskite crystallization, which helps to more truly demonstrate the important role of defects in thermal quenching. And our results reveal the root cause that the quenching will be strengthened by the defect-promoted exciton-phonon coupling. Ultimately, the PeLEDs with defect passivation achieve an improved external quantum efficiency (EQE) over 22% and doubled operation lifetime at room temperature, and can maintain about 85% of the initial EQE at 85 °C, much higher than 17% of the control device. These findings provide an important basis for fabricating practical PeLEDs for lighting and displays.
ABSTRACT
Additives play a critical role for efficient perovskite light-emitting diodes (PeLEDs). Here, we report a novel phosphonate/phosphine oxide dyad molecular additive (PE-TPPO), with unique dual roles of passivating defects and enhancing carrier radiative recombination, to boost the device efficiency of metal-halide perovskites. In addition to the defect passivation effect of the phosphine oxide group to enhance the photoluminescence intensity and homogeneity of perovskite film, the phosphonate group with strong electron affinity can capture the injected electrons to increase local carrier concentration and accelerate the carrier radiative recombination in the electroluminescence process. Owing to their synergistic enhancement on device efficiency, quasi-two-dimensional green PeLEDs modified by this dyad additive exhibit a maximum external quantum efficiency, current efficiency, and power efficiency of 25.1 %, 100.5â cd A-1 , and 98.7â lm W-1 , respectively, which are among the reported state-of-the-art efficiencies.
ABSTRACT
Solution-processed quasi-two-dimensional (quasi-2D) perovskites with self-assembled multiple quantum well (QW) structures exhibit enhanced exciton binding energy, which is ideal for use as light emitters. Here, we have found that postannealing is important to promoting the QWs' composition transfer, and we explored the correlation among the annealing time, the external quantum efficiency (EQE), and the operational stability of the device. During thermal annealing, the low-n QWs will gradually convert to high-n phases, accompanied by an increase in grain size. The EQE and working stability of the device exhibit different annealing-time dependences; that is, with the extension of the annealing time, the EQE gradually decreases while the working stability improves. By introducing trimethylolpropane trimethacrylate (TPTA) to passivate the emitting-region defects, the annealing-time dependence of the EQE was effectively eliminated due to the reduction of the nonradiative recombination rate, wherefore high efficiency and stability can be achieved simultaneously. Our research provides an effective way to develop highly efficiency and stable perovskite light-emitting diodes.
ABSTRACT
Organic-inorganic lead halide quasi-two-dimensional (2D) perovskites are promising gain media for lasing applications because of their low cost, tunable colour, excellent stability and solution processability1-3. Optically pumped continuous-wave (CW) lasing is highly desired for practical applications in high-density integrated optoelectronics devices and constitutes a key step towards electrically pumped lasers4-6. However, CW lasing has not yet been realized at room temperature because of the 'lasing death' phenomenon (the abrupt termination of lasing under CW optical pumping), the cause of which remains unknown. Here we study lead halide-based quasi-2D perovskite films with different organic cations and observe that long-lived triplet excitons considerably impede population inversion during amplified spontaneous emission and optically pumped pulsed and CW lasing. Our results indicate that singlet-triplet exciton annihilation is a possible intrinsic mechanism causing lasing death. By using a distributed-feedback cavity with a high quality factor and applying triplet management strategies, we achieve stable green quasi-2D perovskite lasers under CW optical pumping in air at room temperature. We expect that our findings will pave the way to the realization of future current-injection perovskite lasers.
ABSTRACT
TiO2 has been widely used in ultraviolet (UV) photodetectors, but due to the large number of structural defects and strong band-to-band recombination of the exciton in TiO2, the devices usually have large dark current (I d) and low light current (I l), which seriously reduces the sensitivity and responsivity (R) of the TiO2 based devices. In this work, carbon (C) quantum dots (QDs) are introduced into TiO2 film to ameliorate these issues. Due to the difference of work function between TiO2 nanoparticles and C QDs, the built-in electric field (E bi) can be formed, which effectively facilitates the photogenerated exciton dissociation in the TiO2 film under UV illumination. Meanwhile, the constructed depletion region in dark reduces the majority carrier density, thus decreasing the I d of the photodetector. Moreover, the E bi and depletion region will also contribute to the faster charge collection under UV illumination and recombination of the electron in dark, which is beneficial for the improved response/recovery speed of the device.
ABSTRACT
Increasing evidences have suggested that deregulated miRNAs may involve in drug chemoresistance in a lot of human cancers. However, the role of miR-613 in drug chemoresistance of GC cell is still unknown. The expression of miR-613 and Sex-determining region Y (SRY)-box 9 (SOX9) in GC tissues and cell lines was detected by using qRT-PCR. Cell migration and viability were measured by the wound healing assay and CCK-8 assays. Western blot and dual-luciferase reporter were done to identify the target gene of miR-613. We showed that miR-613 expression was downregulated in GC tissues and cell lines. Ectopic expression of miR-613 increased the sensitivity of GC cells to cisplatin. Overexpression of miR-613 suppressed GC cell proliferation, cycle and migration. In addition, we identified SOX9 was a direct target gene of miR-613 in GC cell. We showed that SOX9 expression was upregulated in gastric cancer samples. Moreover, the expression of SOX9 was negatively correlated with miR-613 expression in GC tissues. Furthermore, elevated expression of miR-613 increased the sensitivity of GC cells to cisplatin and suppressed GC cell proliferation and migration by targeting SOX9. These data suggested that miR-613 might function as a chemoresistant suppressor in GC.
ABSTRACT
PURPOSE: Oxidative stress was significantly associated with the development of malignancies. The purpose of this study was to evaluate the significance of serum total oxidant/antioxidant status in operable advanced gastric cancer patients. MATERIALS AND METHODS: A total of 284 patients who underwent curative resection for primary stage III gastric cancer were enrolled. Total oxidant status, total antioxidant status, and oxidative stress index (OSI) were evaluated within 24 hours before surgery, and compared with 120 healthy donors. The correlation between the OSI and survival outcome was analyzed by the Kaplan-Meier method with log-rank test and Cox's regression methods, respectively. RESULTS: Mean OSI of gastric cancer patients was higher than healthy controls (1.41±0.96 vs 0.78±0.42, P<0.001). All patients were stratified into two groups using the optimal cutoff value (1.42) of OSI using a sensitivity of 94.1% and a specificity of 64.0% as optimal conditions from receiver operating curve analysis. Patients with an OSI ≥1.42 had poorer mean overall survival (45.6 vs 29.8 months, P=0.022) and mean recurrence-free survival (43.3 vs 28.1 months, P=0.011) than patients with an OSI <1.42 in univariate analysis, and OSI was also confirmed as an independent predictor for survival for gastric cancer in multivariate analysis (hazard ratio, 0.541; 95% CI: 0.127-1.102; P=0.01). CONCLUSION: Preoperative OSI can be considered as an independent prognostic factor for operable and advanced gastric cancer.
ABSTRACT
A visible-blind ultraviolet (UV) photodetector (PD) based on TiO2/polyvinyl carbazole doped with poly {[2,7-(9-(20-ethylhexyl)-9-hexyl-fluorene])-alt-[5,50-(40,70-di-2-thienyl-20,10,30-benzothid-iazole)]} (PFTBT) was successfully fabricated. The introduced PFTBT exhibits high absorbance in the UV region and high conductivity which increases the device absorbance and the efficiency of carrier mobility. Besides, PFTBT acts as traps which can increase the concentration of the majority carrier. Therefore, the doped device exhibits high responsivity and high specific detectivity with the value of 0.22 A W-1 and 1.78 × 1012 Jones which respectively has a 3.6 and 2.6 times greater enhancement than the device without doping. The response time is also improved from 27 ms to 22 ms. Owing to the different absorbances that the materials have, the PD has a narrow detection range from 320 nm to 340 nm which is helpful to the study of the specific wavelength. In other words, the research provides a potential way to fabricate practical high-performance UVPDs.
ABSTRACT
Applications of ZnO in photodetectors are limited by the great quantity of extrinsic majority carriers due to structural defects and difficult exciton dissociation due to the large exciton binding energy; these generally lead to a higher dark current (Id) and lower light current (Il), severely degrading the responsivity and detectivity. C dots are incorporated into an annealing-free ZnO layer to innovatively construct a local built-in electric field (Ebi) using the difference in the work functions; this simultaneously overcomes the drawbacks of the pristine ZnO photosensitive layer. In dark, the extrinsic majority carrier of ZnO is depleted around the incorporated C dots due to the self-depleting effect; thus, the Id decreases. Under UV illumination, the photogenerated exciton driven by the local Ebi is easily dissociated into a free charge carrier, contributing to the improved Il. This study paves a universal way to effectively improve the detection characteristics of photoconductive devices by incorporating the local Ebi.
ABSTRACT
Recently, long noncoding RNAs (lncRNAs) have emerged as new gene regulators and prognostic biomarkers in several cancers, including gastric cancer (GC). In this study, we investigate the role of lncRNA ZEB1 antisense1 (ZEB1-AS1) on GC progression. In the present study, we found that ZEB1-AS1 expression was upregulated in GC tissues and cell lines. High ZEB1-AS1 expression was significantly correlated with advanced TNM stage, lymph node metastasis, and poor overall survival in GC patients. ZEB1-AS1 suppression reduced GC cell proliferation and invasion in vitro. Tumor formation assay in nude mice showed that ZEB1-AS1 inhibition suppressed GC cell growth. Quantitative real-time PCR showed that miR-335-5p expression was downregulated and negatively correlated with ZEB1-AS1 expression in GC tissues. And miR-335-5p expression was directly regulated by ZEB1-AS1. Furthermore, we found that inhibition of miR-335-5p abrogated the suppression of proliferation and invasion of GC cells induced by ZEB1-AS1 depletion. Collectively, ZEB1-AS1 is critical for the proliferation and invasion of GC cells by regulating miR-335-5p. Our findings indicated that ZEB1-AS1 might offer potential novel therapeutic targets for GC patients.
Subject(s)
Cell Proliferation/genetics , Down-Regulation/genetics , MicroRNAs/genetics , Neoplasm Invasiveness/genetics , RNA, Long Noncoding/genetics , Stomach Neoplasms/genetics , Zinc Finger E-box-Binding Homeobox 1/genetics , Biomarkers, Tumor/genetics , Cell Line, Tumor , Cell Movement/genetics , Gene Expression Regulation, Neoplastic/genetics , Humans , Lymphatic Metastasis/genetics , Lymphatic Metastasis/pathology , Neoplasm Invasiveness/pathology , Stomach Neoplasms/pathology , Up-Regulation/geneticsABSTRACT
A novel paradigm in tumor biology suggests that gastric cancer progression is driven by gastric cancer stem cell-like cells (GCSCs), but molecular mechanisms regulating tumorigenic and self-renewal potential of GCSCs are still unclear. Here, we aim to investigate biological function of SLC34A2 in regulating sphere formation and tumorigenicity (both are the hallmark of CSCs) of GCSCs and its underlying mechanisms. Our findings testified that CD44+ cells which were derived from fresh primary gastric cancer samples and cell lines displayed stem cell-like features. Significantly, SLC34A2 is increased in CD44+ GCSCs compared with those in adherent counterpart from CD44+ GCSCs. On clinic, SLC34A2 is overexpressed in primary tumor tissues compared with adjacent counterparts. We showed that SLC34A2 regulated sphere formation and self-renewal properties of CD44+ GCSCs in vitro and in vivo. Mechanistic investigations revealed that Gsk3ß was the most strikingly up-regulated gene in response to SLC34A2 knockdown in GCSCs and Wnt/ß-cantenin signaling was required for SLC34A2-mediated sphere formation. Furthermore, SLC34A2 directly binds specific sites in the miR-25 promoter region and that the promoter activity is decreased after the mutation of putative SLC34A2-binding sites, indicating that SLC34A2 is required for the transcriptional induction of miR-25. Meanwhile, luciferase assays showed that miR-25 directly targeted Gsk3ß in CD44+ GCSCs. Overall, our findings define a SLC34A2-miR-25-Gsk3ß pathway in the regulation of GCSCs features and gastric cancer progression, with potential therapeutic applications in blocking their progression.
Subject(s)
Glycogen Synthase Kinase 3 beta/metabolism , MicroRNAs/metabolism , Neoplastic Stem Cells/pathology , Signal Transduction , Sodium-Phosphate Cotransporter Proteins, Type IIb/metabolism , Stomach Neoplasms/pathology , Animals , Cell Line, Tumor , Disease Progression , Female , Gene Expression Regulation, Neoplastic , Glycogen Synthase Kinase 3 beta/genetics , Humans , Mice, Inbred BALB C , Mice, Nude , MicroRNAs/genetics , Neoplastic Stem Cells/metabolism , Sodium-Phosphate Cotransporter Proteins, Type IIb/genetics , Stomach Neoplasms/genetics , Stomach Neoplasms/metabolism , Wnt Signaling PathwayABSTRACT
The original version of this article unfortunately contained a mistake. The presentation of the affiliation number was incorrect. The corrected one is given below.Zhong-zhu AI () 1.
ABSTRACT
The main purpose of this study was to investigate the active components of the Chinese medicine formula Shenqi San (SS) by high performance liquid chromatography with diode array detector and electrospray ionization-hybrid quadrupole time-of-flight mass spectrum (HPLC-DADESI- QTOF-MS), and demonstrate the anticancer mechanism of SS on human lung adenocarcinoma A549 cells by evaluating the cell proliferation and apoptosis induction. The chloroform extraction of SS (CE-SS) was extracted from SS, while HPLC-DAD-ESI-QTOF-MS assay was performed to identify components of CE-SS. MTT assay was used to quantify the proliferation of A549 cells with the treatment of CE-SS. Apoptosis analysis was carried out by detecting phosphatidylserine (PS) externalization using the Annexin V-FITC Apoptosis Detection Kit and the stained cells were analyzed with a flow cytometer. DAPI staining assay was carried out to observe morphological characteristics of apoptotic cells. Western blotting was used to detect the expression of important signaling proteins including caspase-3, -8, -9, p53, Bax and Bcl-2. Eight compounds were identified through HPLC-DAD-ESI-QTOF-MS analysis and 3-pyridine carboxylic acid, barbatin C, scutebarbatine F and barbatine D might be the main compounds responsible for the antitumor effect of CE-SS. CE-SS suppressed the proliferation of lung cancer A549 cells in a time- and dose-dependent manner. By Annexin V-FITC/PI double staining, we found that treatment with CE-SS induced apoptosis in A549 cells. After 24-h exposure to CE-SS, the expression of cleaved-caspase-9, cleaved-caspase-8 and cleaved-caspase-3 protein was activated, the expression of p53 protein increased while the ratio of Bax/Bcl-2 also increased. This study identified the eight compounds of CE-SS, and demonstrated their anticancer effect on human lung adenocarcinoma A549 cells via induction of apoptosis.
Subject(s)
Adenocarcinoma/metabolism , Antineoplastic Agents, Phytogenic/pharmacology , Drugs, Chinese Herbal/pharmacology , Lung Neoplasms/metabolism , Plant Extracts/pharmacology , A549 Cells , Adenocarcinoma/drug therapy , Adenocarcinoma of Lung , Antineoplastic Agents, Phytogenic/chemistry , Caspases/metabolism , Cell Proliferation/drug effects , Cell Survival/drug effects , Drugs, Chinese Herbal/chemistry , Gene Expression Regulation, Neoplastic/drug effects , Humans , Lung Neoplasms/drug therapy , Plant Extracts/chemistry , Proto-Oncogene Proteins c-bcl-2/metabolism , bcl-2-Associated X Protein/metabolismABSTRACT
To overcome drawbacks of the electron transport layer, such as complex surface defects and unmatched energy levels, we successfully employed a smart semiconductor-metal interfacial nanojunciton in organic solar cells by evaporating an ultrathin Al interlayer onto annealing-free ZnO electron transport layer, resulting in a high fill factor of 73.68% and power conversion efficiency of 9.81%. The construction of ZnO-Al nanojunction could effectively fill the surface defects of ZnO and reduce its work function because of the electron transfer from Al to ZnO by Fermi level equilibrium. The filling of surface defects decreased the interfacial carrier recombination in midgap trap states. The reduced surface work function of ZnO-Al remodulated the interfacial characteristics between ZnO and [6,6]-phenyl C71-butyric acid methyl ester (PC71BM), decreasing or even eliminating the interfacial barrier against the electron transport, which is beneficial to improve the electron extraction capacity. The filled surface defects and reduced interfacial barrier were realistically observed by photoluminescence measurements of ZnO film and the performance of electron injection devices, respectively. This work provides a simple and effective method to simultaneously solve the problems of surface defects and unmatched energy level for the annealing-free ZnO or other metal oxide semiconductors, paving a way for the future popularization in photovoltaic devices.