Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 31
Filtrar
Mais filtros

Base de dados
Tipo de documento
Intervalo de ano de publicação
1.
Small ; 20(37): e2402531, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38727180

RESUMO

The efficacy of electron transport layers (ETLs) is pivotal for optimizing the device performance of perovskite photovoltaic applications. However, colloidal dispersions of SnO2 are prone to aggregation and possess structural defects, such as terminal-hydroxyls (OHT) and oxygen vacancies (VOs), which can degrade the quality of ETLs, impede charge extraction and transport, and affect the nucleation and growth processes of the perovskite layer. In this study, the Sb(OH)4 - ions hydrolyzed from SbCl3 in colloidal dispersion can bind to defect sites and effectively stabilize the SnO2 nanocrystals are demonstrated. Upon oxidative annealing, a Sb2O5@SnO2 composite film is formed, in which the Sb2O5 not only mitigates the aforementioned defects but also broadens the energy range of unoccupied states through its dispersed conduction band. The increased electron affinity (EA) facilitates more efficient capture of photoexcited electrons from the perovskite layer, thus augmenting electron extraction and minimizing electron-hole recombination. As a result, a significant improvement in power conversion efficiency (PCE) from 22.60% to 24.54% is achieved, with an open circuit voltage (VOC) of up to 1.195 V, along with excellent stability of unsealed devices under various conditions. This study provides valuable insights for the understanding and design of ETLs in perovskite photovoltaic applications.

2.
Small ; 20(38): e2402385, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38742952

RESUMO

Non-radiative recombination losses limit the property of perovskite solar cells (PSCs). Here, a synergistic strategy of SnSe2QDs doping into SnO2 and chlorhexidine acetate (CA) coating on the surface of perovskite is proposed. The introduction of 2D SnSe2QDs reduces the oxygen vacancy defects and increases the carrier mobility of SnO2. The optimized SnO2 as a buried interface obviously improves the crystallization quality of perovskite. The CA containing abundant active sites of ─NH2/─NH─, ─C═N, CO, ─Cl groups passivate the defects on the surface and grain boundary of perovskite. The alkyl chain of CA also improves the hydrophobicity of perovskite. Moreover, the synergism of SnSe2QDs and CA releases the residual stress and regulates the energy level arrangement at the top and bottom interface of perovskite. Benefiting from these advantages, the bulk and interface non-radiative recombination loss is greatly suppressed and thereby increases the carrier transport and extraction in devices. As a result, the best power conversion efficiency (PCE) of 23.41% for rigid PSCs and the best PCE of 21.84% for flexible PSCs are reached. The rigid PSC maintains 89% of initial efficiency after storing nitrogen for 3100 h. The flexible PSCs retain 87% of the initial PCE after 5000 bending cycles at a bending radius of 5 mm.

3.
Small ; 20(28): e2310742, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38329192

RESUMO

Targeted treatment of the interface between electron transport layers (ETL) and perovskite layers is highly desirable for achieving passivating effects and suppressing carrier nonradiative recombination, leading to high performance and long-term stability in perovskite solar cells (PSCs). In this study, a series of non-fullerene acceptors (NFAs, Y-H, Y-F, and Y-Cl) are introduced to optimize the properties of the perovskite/ETL interface. This optimization involves passivating Pb2+ defects, releasing stress, and modulating carrier dynamics through interactions with the perovskite. Remarkably, after modifying with NFAs, the absorption range of perovskite films into the near-infrared region is extended. As expected, Y-F, with the largest electrostatic potential, facilitates the strongest interaction between the perovskite and its functional groups. Consequently, champion power conversion efficiencies of 21.17%, 22.21%, 23.25%, and 22.31% are achieved for control, Y-H-, Y-F-, and Y-Cl-based FA0.88Cs0.12PbI2.64Br0.36 (FACs) devices, respectively. This treatment also enhances the heat stability and air stability of the corresponding devices. Additionally, these modifier layers are applied to enhance the efficiency of Cs0.05(FA0.95MA0.05)0.95PbI2.64Br0.36 (FAMA) devices. Notably, a champion PCE exceeding 24% is achieved in the Y-F-based FAMA device. Therefore, this study provides a facile and effective approach to target the interface, thereby improving the efficiency and stability of PSCs.

4.
Small ; 20(27): e2307807, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38342673

RESUMO

Sodium (Na) doping is a well-established technique employed in chalcopyrite and kesterite solar cells. While various improvements can be achieved in crystalline quality, electrical properties, or defect passivation of the absorber materials by incorporating Na, a comprehensive demonstration of the desired Na distribution in CZTSSe is still lacking. Herein, a straightforward Na doping approach by dissolving NaCl into the CZTS precursor solution is proposed. It is demonstrated that a favorable Na ion distribution should comprise a precisely controlled Na+ concentration at the front surface and an enhanced distribution within the bottom region of the absorber layer. These findings demonstrated that Na ions play several positive roles within the device, leading to an overall power conversion efficiency of 12.51%.

5.
Angew Chem Int Ed Engl ; 63(30): e202406153, 2024 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-38730419

RESUMO

Innovative molecule design strategy holds promise for the development of next-generation acceptor materials for efficient organic solar cells with low non-radiative energy loss (ΔEnr). In this study, we designed and prepared three novel acceptors, namely BTP-Biso, BTP-Bme and BTP-B, with sterically structured triisopropylbenzene, trimethylbenzene and benzene as side chains inserted into the shoulder of the central core. The progressively enlarged steric hindrance from BTP-B to BTP-Bme and BTP-Biso induces suppressed intramolecular rotation and altered the molecule packing mode in their aggregation states, leading to significant changes in absorption spectra and energy levels. By regulating the intermolecular π-π interactions, BTP-Bme possesses relatively reduced non-radiative recombination rate and extended exciton diffusion lengths. The binary device based on PB2 : BTP-Bme exhibits an impressive power conversion efficiency (PCE) of 18.5 % with a low ΔEnr of 0.19 eV. Furthermore, the ternary device comprising PB2 : PBDB-TF : BTP-Bme achieves an outstanding PCE of 19.3 %. The molecule design strategy in this study proposed new perspectives for developing high-performance acceptors with low ΔEnr in OSCs.

6.
Small ; 19(11): e2205336, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36581559

RESUMO

Functional passivators are conventionally utilized in modifying the crystallization properties of perovskites to minimize the non-radiative recombination losses in perovskite light-emitting diodes (PeLEDs). However, the weak anchor ability of some commonly adopted molecules has limited passivation ability to perovskites and even may desorb from the passivated defects in a short period of time, which bring about plenty of challenges for further development of high-performance PeLEDs. Here, a multidentate molecule, formamidine sulfinic acid (FSA), is introduced as a novel passivator to perovskites. FSA has multifunctional groups (S≐O, C≐N and NH2 ) where the S≐O and C≐N groups enable coordination with the lead ions and the NH2 interacts with the bromide ions, thus providing the most effective chemical passivation for defects and in turn the formation of highly stable perovskite emitters. Moreover, the interaction between the FSA and octahedral [PbBr6 ]4- can inhibit the formation of unfavorable low-n domains to further minimize the inefficient energy transfer inside the perovskite emitters. Therefore, the FSA passivated green-emitting PeLED exhibits a high external quantum efficiency (EQE) of 26.5% with fourfold enhancement in operating lifetime as compared to the control device, consolidating that the multidentate molecule is a promising strategy to effectively and sustainably passivate the perovskites.

7.
Angew Chem Int Ed Engl ; 62(35): e202304931, 2023 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-37431837

RESUMO

Reducing non-radiative recombination energy loss (ΔE3 ) is one key to boosting the efficiency of organic solar cells. Although the recent studies have indicated that the Y-series asymmetric acceptors-based devices featured relatively low ΔE3 , the understanding of the energy loss mechanism derived from molecular structure change is still lagging behind. Herein, two asymmetric acceptors named BTP-Cl and BTP-2Cl with different terminals were synthesized to make a clear comparative study with the symmetric acceptor BTP-0Cl. Our results suggest that asymmetric acceptors exhibit a larger difference of electrostatic potential (ESP) in terminals and semi-molecular dipole moment, which contributes to form a stronger π-π interaction. Besides, the experimental and theoretical studies reveal that a lower ESP-induced intermolecular interaction can reduce the distribution of PM6 near the interface to enhance the built-in potential and decrease the charge transfer state ratio for asymmetric acceptors. Therefore, the devices achieve a higher exciton dissociation efficiency and lower ΔE3 . This work establishes a structure-performance relationship and provides a new perspective to understand the state-of-the-art asymmetric acceptors.

8.
Angew Chem Int Ed Engl ; 61(34): e202207300, 2022 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-35761506

RESUMO

To enhance the fluorescence efficiency of semiconductor nanocrystal quantum dots (QDs), strategies via enhancing photo-absorption and eliminating non-radiative relaxation have been proposed. In this study, we demonstrate that fluorescence efficiency of molybdenum disulfide quantum dots (MoS2 QDs) can be enhanced by single-atom metal (Au, Ag, Pt, Cu) modification. Four-fold enhancement of the fluorescence emission of MoS2 QDs is observed with single-atom Au modification. The underlying mechanism is ascribed to the passivation of non-radiative surface states owing to the new defect energy level of Au in the forbidden band that can trap excess electrons in n-type MoS2 , increasing the recombination probability of conduction band electrons with valence band holes of MoS2 . Our results open an avenue for enhancing the fluorescence efficiency of QDs via the modification of atomically dispersed metals, and extend their scopes and potentials in a fundamental way for economic efficiency and stability of single-atom metals.

9.
Angew Chem Int Ed Engl ; 60(13): 7227-7233, 2021 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-33369830

RESUMO

Currently, the performance improvement for inverted perovskite solar cells (PVSCs) is mainly limited by the high open circuit voltage (VOC ) loss caused by detrimental non-radiative recombination (NRR) processes. Herein, we report a simple and efficient way to simultaneously reduce the NRR processes inside perovskites and at the interface by rationally designing a new pyridine-based polymer hole-transporting material (HTM), PPY2, which exhibits suitable energy levels with perovskites, high hole mobility, effective passivation of the uncoordinated Pb2+ and iodide defects, as well as the capability of promoting the formation of high-quality polycrystalline perovskite films. In absence of any dopants, the inverted PVSCs using PPY2 as the HTM deliver an encouraging PCE up to 22.41 % with a small VOC loss (0.40 V), among the best device performances for inverted PVSCs reported so far. Furthermore, PPY2-based unencapsulated devices show an excellent long-term photostability, and over 97 % of its initial PCE can be maintained after one sun constant illumination for 500 h.

10.
Angew Chem Int Ed Engl ; 59(10): 4099-4105, 2020 Mar 02.
Artigo em Inglês | MEDLINE | ID: mdl-31872927

RESUMO

Defect passivation has been demonstrated to be effective in improving the radiative recombination of charge carriers in perovskites, and consequently, the device performance of the resultant perovskite light-emitting diodes (LEDs). State-of-the-art useful passivation agents in perovskite LEDs are mostly organic chelating molecules that, however, simultaneously sacrifice the charge-transport properties and thermal stability of the resultant perovskite emissive layers, thereby deteriorating performance, and especially the operational stability of the devices. We demonstrate that lithium halides can efficiently passivate the defects generated by halide vacancies and reduce trap state density, thereby suppressing ion migration in perovskite films. Efficient green perovskite LEDs based on all-inorganic CsPbBr3 perovskite with a peak external quantum efficiency of 16.2 %, as well as a high maximum brightness of 50 270 cd m-2 , are achieved. Moreover, the device shows decent stability even under a brightness of 104  cd m-2 . We highlight the universal applicability of defect passivation using lithium halides, which enabled us to improve the efficiency of blue and red perovskite LEDs.

11.
Sci Technol Adv Mater ; 20(1): 786-795, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31447957

RESUMO

The possibility to manufacture perovskite solar cells (PSCs) at low temperatures paves the way to flexible and lightweight photovoltaic (PV) devices manufactured via high-throughput roll-to-roll processes. In order to achieve higher power conversion efficiencies, it is necessary to approach the radiative limit via suppression of non-radiative recombination losses. Herein, we performed a systematic voltage loss analysis for a typical low-temperature processed, flexible PSC in n-i-p configuration using vacuum deposited C60 as electron transport layer (ETL) and two-step hybrid vacuum-solution deposition for CH3NH3PbI3 perovskite absorber. We identified the ETL/absorber interface as a bottleneck in relation to non-radiative recombination losses, the quasi-Fermi level splitting (QFLS) decreases from ~1.23 eV for the bare absorber, just ~90 meV below the radiative limit, to ~1.10 eV when C60 is used as ETL. To effectively mitigate these voltage losses, we investigated different interfacial modifications via vacuum deposited interlayers (BCP, B4PyMPM, 3TPYMB, and LiF). An improvement in QFLS of ~30-40 meV is observed after interlayer deposition and confirmed by comparable improvements in the open-circuit voltage after implementation of these interfacial modifications in flexible PSCs. Further investigations on absorber/hole transport layer (HTL) interface point out the detrimental role of dopants in Spiro-OMeTAD film (widely employed HTL in the community) as recombination centers upon oxidation and light exposure.

12.
Adv Mater ; : e2410669, 2024 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-39328030

RESUMO

An effective defect passivation strategy is crucial for enhancing the performance of antimony selenosulfide (Sb2(S,Se)3) solar cells, as it significantly influences charge transport and extraction efficiency. Herein, a convenient and novel in situ passivation (ISP) technique is successfully introduced to enhance the performance of Sb2(S,Se)3 solar cells, achieving a champion efficiency of 10.81%, which is among the highest recorded for Sb2(S,Se)3 solar cells to date. The first principles calculations and the experimental data reveal that incorporating sodium selenosulfate in the ISP strategy effectively functions as an in situ selenization, effectively passivating deep-level cation antisite SbSe defect within the Sb2(S,Se)3 films and significantly suppressing non-radiative recombination in the devices. Space-charge-limited current (SCLC), photoluminescence (PL), and transient absorption spectroscopy (TAS) measurements verify the high quality of the passivated films, showing fewer traps and defects. Moreover, the ISP strategy improved the overall quality of the Sb2(S,Se)3 films, and fine-tuned the energy levels, thereby facilitating enhanced carrier transport. This study thus provides a straightforward and effective method for passivating deep-level defects in Sb2(S,Se)3 solar cells.

13.
Adv Mater ; 36(26): e2401319, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38531370

RESUMO

Tailoring multifunctional additives for performing interfacial modifications, improving crystallization, and passivating defects is instrumental for the fabrication of efficient and stable perovskite solar cells (PSCs). Here, a Schiff base derivative, (chloromethylene) dimethyliminium chloride (CDCl), is introduced as an additive to modify the interface between the mesoporous TiO2 electron transport layer and the MAPbI3 light absorber during the annealing process. CDCl chemically links to TiO2 and MAPbI3 through coordination and hydrogen bonding, respectively, and results in the construction of fast electron extraction channels. CDCl also optimizes the energy-level alignment of the TiO2/MAPbI3 heterojunction and improves the pore-filling and crystallization of MAPbI3 in the mesoscopic scaffold, which inhibits nonradiative recombination and eliminates open-circuit voltage losses. As a result, an impressive power conversion efficiency of 19.74%, which is the best one ever reported, is obtained for printable carbon-based hole-conductor-free PSCs based on MAPbI3.

14.
Adv Mater ; 36(13): e2310962, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38111378

RESUMO

Perovskite solar cells (PSCs) have attracted extensive attention due to their higher power conversion efficiency (PCE) and simple fabrication process. However, the open-circuit voltage (VOC) loss remains a significant impediment to enhance device performance. Here, a facile strategy to boost the VOC to 95.5% of the Shockley-Queisser (S-Q) limit through the introduction of a universal multifunctional polymer additive is demonstrated. This additive effectively passivates the cation and anion defects simultaneously, thereby leading to the transformation from the strong n-type to weak n-type of perovskite films. Benefitting from the energy level alignment and the suppression of bulk non-radiative recombination, the quasi-Fermi level splitting (QFLS) is enhanced.  Consequently, the champion devices with 1.59 eV-based perovskite reach the highest VOC value of 1.24 V and a PCE of 23.86%. Furthermore, this strategy boosts the VOC by at least 0.07 V across five different perovskite systems, a PCE of 25.04% is achieved for 1.57 eV-based PSCs, and the corresponding module (14 cm2) also obtained a high PCE of 21.95%. This work provides an effective and universal strategy to promote the VOC approach to the detailed balance theoretical limit.

15.
Sci Rep ; 14(1): 24254, 2024 Oct 16.
Artigo em Inglês | MEDLINE | ID: mdl-39414975

RESUMO

The study of charge transfer in thin film solar cells made of several layers is of high importance since they may lose their energy via the recombination process at the interfaces, specifically at the interface of the electron transport layer (ETL) and perovskite. Titanium dioxide (TiO2) is mostly used as an ETL in perovskite solar cells due to its many advantages. However, TiO2 has some disadvantages, such as low electron mobility compared to the perovskite layer and electron trap states on its top at the interface. These effects cause the accumulation of carriers at the ETL/perovskite interface then the non-radiative recombination will be enhanced, which is considered as one of the significant losses in the Perovskite Solar Cells (PSCs). In this work, a new technique is taken for more optimal ETL doping. We fabricated the ETL layers with graded doping of platinum quantum dots (Pt QDs), in which Pt QDs concentration is high at the ETL/Perovskite interface and zero at the FTO/ETL interface. This strategy not only suppresses the recombination at the ETL/perovskite interface and subsequently enhances the device efficiency from 12.92 to 14.36% but also improves the stability of the PSCs.

16.
Nanomicro Lett ; 16(1): 178, 2024 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-38656466

RESUMO

This study presents experimental evidence of the dependence of non-radiative recombination processes on the electron-phonon coupling of perovskite in perovskite solar cells (PSCs). Via A-site cation engineering, a weaker electron-phonon coupling in perovskite has been achieved by introducing the structurally soft cyclohexane methylamine (CMA+) cation, which could serve as a damper to alleviate the mechanical stress caused by lattice oscillations, compared to the rigid phenethyl methylamine (PEA+) analog. It demonstrates a significantly lower non-radiative recombination rate, even though the two types of bulky cations have similar chemical passivation effects on perovskite, which might be explained by the suppressed carrier capture process and improved lattice geometry relaxation. The resulting PSCs achieve an exceptional power conversion efficiency (PCE) of 25.5% with a record-high open-circuit voltage (VOC) of 1.20 V for narrow bandgap perovskite (FAPbI3). The established correlations between electron-phonon coupling and non-radiative decay provide design and screening criteria for more effective passivators for highly efficient PSCs approaching the Shockley-Queisser limit.

17.
Nanomaterials (Basel) ; 14(20)2024 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-39452985

RESUMO

CsGeI2Br-based perovskites, with their favorable band gap and high absorption coefficient, are promising candidates for the development of efficient lead-free perovskite solar cells (PSCs). However, bulk and interfacial carrier non-radiative recombination losses hinder the further improvement of power conversion efficiency and stability in PSCs. To overcome this challenge, the photovoltaic potential of the device is unlocked by optimizing the optical and electronic parameters through rigorous numerical simulation, which include tuning perovskite thickness, bulk defect density, and series and shunt resistance. Additionally, to make the simulation data as realistic as possible, recombination processes, such as Auger recombination, must be considered. In this simulation, when the Auger capture coefficient is increased to 10-29 cm6 s-1, the efficiency drops from 31.62% (without taking Auger recombination into account) to 29.10%. Since Auger recombination is unavoidable in experiments, carrier losses due to Auger recombination should be included in the analysis of the efficiency limit to avoid significantly overestimating the simulated device performance. Therefore, this paper provides valuable insights for designing realistic and efficient lead-free PSCs.

18.
Micromachines (Basel) ; 14(5)2023 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-37241615

RESUMO

GaN-based micro-size light-emitting diodes (µLEDs) have a variety of attractive and distinctive advantages for display, visible-light communication (VLC), and other novel applications. The smaller size of LEDs affords them the benefits of enhanced current expansion, fewer self-heating effects, and higher current density bearing capacity. Low external quantum efficiency (EQE) resulting from non-radiative recombination and quantum confined stark effect (QCSE) is a serious barrier for application of µLEDs. In this work, the reasons for the poor EQE of µLEDs are reviewed, as are the optimization techniques for improving the EQE of µLEDs.

19.
Discov Nano ; 18(1): 48, 2023 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-37382729

RESUMO

Generally, the inductively coupled plasma-reactive ion etching (ICP-RIE) mesa technology was used to remove p-GaN/MQWs and expose n-GaN for electrical contact in a fabricated micro light-emitting diode (µLED). In this process, the exposed sidewalls were significantly damaged which result in small-sized µLED presenting a strong size-dependent influence. Lower emission intensity was observed in the µLED chip, which can be attributed to the effect of sidewall defect during etch processing. To reduce the non-radiative recombination, the ion implantation using an As+ source to substitute the ICP-RIE mesa process was introduced in this study. The ion implantation technology was used to isolate each chip to achieve the mesa process in the µLED fabrication. Finally, the As+ implant energy was optimized at 40 keV, which exhibited excellent current-voltage characteristics, including low forward voltage (3.2 V @1 mA) and low leakage current (10-9 A@- 5 V) of InGaN blue µLEDs. The gradual multi-energy implantation process from 10 to 40 keV can further improve the electrical properties (3.1 V @1 mA) of µLEDs, and the leakage current was also maintained at 10-9 A@- 5 V.

20.
Exploration (Beijing) ; 3(3): 20220027, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37933381

RESUMO

Inverted perovskite solar cells (inverted-PSCs) have exhibited advantages of longer stability, less hysteresis, and lower fabrication temperature when compared to their regular counterparts, which are important for industry commercialization. Because of the great efforts that have been conducted in the past several years, the obtained efficiency of inverted-PSCs has almost caught up with that of the regular ones, 25.0% versus 25.7%. In this perspective, the recent studies on the design of high-performance inverted-PSCs based on diverse hole transport materials, as well as device fabrication and characterization are first reviewed. After that, the authors moved on to the interface and additive engineering that were exploited to suppress the nonradiative recombination. Finally, the challenges and possible research pathways for facilitating the industrialization of inverted-PSCs were envisaged.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA