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1.
Nat Commun ; 15(1): 513, 2024 Jan 13.
Article in English | MEDLINE | ID: mdl-38218871

ABSTRACT

Among today's nonvolatile memories, ferroelectric-based capacitors, tunnel junctions and field-effect transistors (FET) are already industrially integrated and/or intensively investigated to improve their performances. Concurrently, because of the tremendous development of artificial intelligence and big-data issues, there is an urgent need to realize high-density crossbar arrays, a prerequisite for the future of memories and emerging computing algorithms. Here, a two-terminal ferroelectric fin diode (FFD) in which a ferroelectric capacitor and a fin-like semiconductor channel are combined to share both top and bottom electrodes is designed. Such a device not only shows both digital and analog memory functionalities but is also robust and universal as it works using two very different ferroelectric materials. When compared to all current nonvolatile memories, it cumulatively demonstrates an endurance up to 1010 cycles, an ON/OFF ratio of ~102, a feature size of 30 nm, an operating energy of ~20 fJ and an operation speed of 100 ns. Beyond these superior performances, the simple two-terminal structure and their self-rectifying ratio of ~ 104 permit to consider them as new electronic building blocks for designing passive crossbar arrays which are crucial for the future in-memory computing.

2.
Adv Mater ; 36(9): e2307646, 2024 Mar.
Article in English | MEDLINE | ID: mdl-37812198

ABSTRACT

Herein, a binary cathode interface layer (CIL) strategy based on the industrial solvent fractionated LignoBoost kraft lignin (KL) is adopted for fabrication of organic solar cells (OSCs). The uniformly distributed phenol moieties in KL enable it to easily form hydrogen bonds with commonly used CIL materials, i.e., bathocuproine (BCP) and PFN-Br, resulting in binary CILs with tunable work function (WF). This work shows that the binary CILs work well in OSCs with large KL ratio compatibility, exhibiting equivalent or even higher efficiency to the traditional CILs in state of art OSCs. In addition, the combination of KL and BCP significantly enhanced OSC stability, owing to KL blocking the reaction between BCP and nonfullerene acceptors (NFAs). This work provides a simple and effective way to achieve high-efficient OSCs with better stability and sustainability by using wood-based materials.

3.
Adv Mater ; 36(13): e2309991, 2024 Mar.
Article in English | MEDLINE | ID: mdl-38154115

ABSTRACT

Constructing 3D/2D perovskite heterojunction is a promising approach to integrate the benefits of high efficiency and superior stability in perovskite solar cells (PSCs). However, in contrast to n-i-p architectural PSCs, the p-i-n PSCs with 3D/2D heterojunction have serious limitations in achieving high-performance as they suffer from a large energetic mismatch and electron extraction energy barrier from a 3D perovskite layer to a 2D perovskite layer, and serious nonradiative recombination at the heterojunction. Here a strategy of incorporating a thin passivating dipole layer (PDL) onto 3D perovskite and then depositing 2D perovskite without dissolving the underlying layer to form an efficient 3D/PDL/2D heterojunction is developed. It is revealed that PDL regulates the energy level alignment with the appearance of interfacial dipole and strongly interacts with 3D perovskite through covalent bonds, which eliminate the energetic mismatch, reduce the surface defects, suppress the nonradiative recombination, and thus accelerate the charge extraction at such electron-selective contact. As a result, it is reported that the 3D/PDL/2D junction p-i-n PSCs present a power conversion efficiency of 24.85% with robust stability, which is comparable to the state-of-the-art efficiency of the 3D/2D junction n-i-p devices.

4.
J Phys Chem Lett ; 14(35): 7953-7959, 2023 Sep 07.
Article in English | MEDLINE | ID: mdl-37646609

ABSTRACT

The suboptimal carrier dynamics at the heterointerface between the perovskite and charge transport layer severely limit further performance enhancement of the state-of-the-art perovskite solar cells (PSCs). Herein, we completely map charge carrier extraction and recombination kinetics over a broad time range at buried electron-selective heterointerfaces via ultrafast transient technologies. It is revealed that the heterointerfaces carefully contain the electronic processes of free charge generation in perovskite within ∼2.8 ps, relaxation process of trap-state induced electron capturing less than ∼10.0 ps, electron extraction from perovskite to SnO2 within ∼194 ps, trap-assisted recombination within ∼2047 ps, and recombination between back-injected electrons and remaining holes within ∼8.4 ns. Moreover, we further demonstrate that the inserted poly(vinyl alcohol) (PVA) thin layer can effectively enhance the electron extraction from perovskite to SnO2, block the undesired electron back injection, and significantly suppress the nonradiative recombination, contributing to the improved device parameters of photovoltage and fill factor. This work sheds light on charge-transfer limitations at the perovskite buried heterointerface and provides an effective guide of ideal heterointerface design for promoting charge transfer and improving PSC performance.

5.
J Allergy Clin Immunol ; 152(5): 1153-1166.e12, 2023 11.
Article in English | MEDLINE | ID: mdl-37437744

ABSTRACT

BACKGROUND: Immune regulation in chronic rhinosinusitis with nasal polyps (CRSwNP) with a neutrophilic endotype remains unclear. Mucosal-associated invariant T (MAIT) cells are tissue-resident innate T lymphocytes that respond quickly to pathogens and promote chronic mucosal inflammation. OBJECTIVE: We aimed to investigate the roles of MAIT cells in neutrophilic CRSwNP. METHODS: Nasal tissues were obtained from 113 patients with CRSwNP and 29 control subjects. Peripheral and tissue MAIT cells and their subsets were analyzed by flow cytometry. Polyp-derived MAIT cells were analyzed by RNA sequencing to study their effects on neutrophils. RESULTS: Endotypes of CRSwNP were classified as paucigranulocytic (n = 21), eosinophilic (n = 29), neutrophilic (n = 39), and mixed granulocytic (n = 24). Frequencies of MAIT cells were significantly higher in neutrophilic (3.62%) and mixed granulocytic (3.60%) polyps than in control mucosa (1.78%). MAIT cell percentages positively correlated with local neutrophil counts. MAIT cells were more enriched in tissues than in matched PBMCs. The frequencies of MAIT1 subset or IFN-γ+ MAIT cells were comparable among control tissues and CRSwNP subtypes. The proportions of MAIT17 subset or IL-17A+ MAIT cells were significantly increased in neutrophilic or mixed granulocytic polyps compared with controls. RNA sequencing revealed type 17 and pro-neutrophil profiles in neutrophilic polyp-derived MAIT cells. In patients with neutrophilic CRSwNP, the proportions of MAIT and MAIT17 cells were positively correlated with local proinflammatory cytokines and symptom severity. In vitro experiments demonstrated that neutrophilic polyp-derived MAIT cells promoted neutrophil migration, survival, and activation. CONCLUSIONS: MAIT cells from neutrophilic CRSwNP demonstrate type 17 functional properties and promote neutrophil infiltration in nasal mucosa.


Subject(s)
Mucosal-Associated Invariant T Cells , Nasal Polyps , Rhinitis , Sinusitis , Humans , Inflammation/complications , Cytokines , Chronic Disease
6.
Adv Sci (Weinh) ; 9(30): e2203681, 2022 Oct.
Article in English | MEDLINE | ID: mdl-36031391

ABSTRACT

Perovskite solar cells (PSCs) suffer from significant nonradiative recombination at perovskite/charge transport layer heterojunction, seriously limiting their power conversion efficiencies. Herein, solution-processed chromium multioxide (CrOx ) is judiciously selected to construct a MAPbI3 /CrOx /Spiro-OMeTAD hole-selective heterojunction. It is demonstrated that the inserted CrOx not only effectively reduces defect sites via redox shuttle at perovskite contact, but also decreases valence band maximum (VBM)-HOMO offset between perovskite and Spiro-OMeTAD. This will diminish thermionic losses for collecting holes and thus promote charge transport across the heterojunction, suppressing both defect-assisted recombination and interface carrier recombination. As a result, a remarkable improvement of 21.21% efficiency with excellent device stability is achieved compared to 18.46% of the control device, which is among the highest efficiencies for polycrystalline MAPbI3 based n-i-p planar PSCs reported to date. These findings of this work provide new insights into novel charge-selective heterojunctions for further enhancing efficiency and stability of PSCs.

7.
Nanomicro Lett ; 14(1): 108, 2022 Apr 19.
Article in English | MEDLINE | ID: mdl-35441280

ABSTRACT

Surface passivation via post-treatment is an important strategy for improving power conversion efficiency and operational stability of perovskite solar cells. However, so far the interaction mechanisms between passivating additive and perovskite are not well understood. Here, we report the atomic-scale interaction of surface passivating additive 2,2-difluoroethylammonium bromine (2FEABr) on the MAPbI3. It is found that the bulky 2FEA+ cations tend to distribute at film surface, while the Br- anions diffuse from surface into bulk. A combination of 19F, 207Pb, and 2H solid-state NMR further reveal the Br- anions' partial substitution for the I- sites, the restricted motion of partial MA+ cations, and the firmed perovskite lattices, which would improve charge transport and stability of the perovskite films. Optical spectroscopy and ultraviolet photoelectron spectroscopy demonstrate that the 2FEABr induced surface passivation and energetic modification suppress the nonradiative recombination loss. These findings enable the efficiency of the p-i-n structured PSC significantly increasing from 19.44 to 21.06%, accompanied by excellent stability. Our work further establishes more knowledge link between passivating additive and PSC performance.

8.
ACS Appl Mater Interfaces ; 14(10): 12450-12460, 2022 Mar 16.
Article in English | MEDLINE | ID: mdl-35235287

ABSTRACT

Organic solar cells (OSCs) based on an inverted architecture generally have better stability compared to those based on a standard architecture. However, the photoactive area of the inverted solar cells increases under ultraviolet (UV) or solar illuminatiom because of the too-high conductivity of the UV-illuminated zinc oxide (ZnO) interlayer. This limits the potential of the inverted solar cells for industrial applications. Herein, lithium-doped ZnO (Li-ZnO) films are employed as the cathode interlayer to construct inverted OSCs. The incorporation of Li ions is found to reduce the lateral conductivity of the UV-treated ZnO films because of the presence of Li ions, preventing the high-quality-growth of ZnO nanocrystals. This addresses the problem of having too-high conductivity in the UV-treated ZnO layer, causing the increased photoactive area of inverted solar cells. The overall performance of the solar cell is shown to be higher after the incorporation of Li ions in the ZnO layer, mainly due to the increased fill factor (FF), originating from the reduced trap-assisted recombination losses. Finally, the inverted solar cells based on the Li-ZnO interlayer are demonstrated to have a much better long-term stability, as compared to those based on ZnO. This allows the ZnO-based interlayers to be used for the mass production of organic solar cell modules.

9.
ACS Appl Mater Interfaces ; 11(14): 13491-13498, 2019 Apr 10.
Article in English | MEDLINE | ID: mdl-30880387

ABSTRACT

The fast evolution of metal halide perovskite solar cells has opened a new chapter in the field of renewable energy. High-quality perovskite films as the active layers are essential for both high efficiency and long-term stability. Here, the perovskite films with enlarged crystal grain size and decreased defect density are fabricated by introducing the extremely low-cost and green polymer, ethyl cellulose (EC), into the perovskite layer. The addition of EC triggers hydrogen bonding interactions between EC and the perovskite, passivating the charge defect traps at the grain boundaries. The long chain of EC further acts as a scaffold for the perovskite structure, eliminating the annealing-induced lattice strain during the film fabrication process. The resulting devices with the EC additive exhibit a remarkably enhanced average power conversion efficiency from 17.11 to 19.27% and an improvement of all device parameters. The hysteresis index is found to decrease by three times from 0.081 to 0.027, which is attributed to suppressed ion migration and surface charge trapping. In addition, the defect passivation by EC significantly improves the environmental stability of the perovskite films, yielding devices that retain 80% of their initial efficiency after 30 days in ambient air at 45% relative humidity, whereas the pristine devices without EC fully degrade. This work provides a low-cost and green avenue for passivating defects that improves both the efficiency and operational stability of perovskite solar cells.

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